Bubbly Flow PDF

WASHINGTON UNIVERSITY
SEVER INSTITUTE
DEPARTMENT OF ENERGY, ENVIRONMENTAL AND CHEMICAL
ENGINEERING
___________________________________________________________________
Bubble and Slurry Bubble Column Reactors: Mixing, Flow Regime Transition and
Scaleup
by
Ashfaq Shaikh
Prepared under the direction of
Professor Muthanna H. Al-Dahhan
___________________________________________________________________
A dissertation presented to the Sever Institute of Washington University
in partial fulfillment of the requirements for the degree of
DOCTOR OF SCIENCE
August 2007
Saint Louis, Missouri, USA
WASHINGTON UNIVERSITY
SEVER INSTITUTE
DEPARTMENT OF ENERGY, ENVIRONMENTAL AND CHEMICAL ENGINEERING
_________________________________________________________________________
ABSTRACT
_____________________________________________________________
Bubble and Slurry Bubble Column Reactors: Mixing, Flow Regime Transition and
Scaleup
by
Ashfaq Shaikh
ADVISOR: Professor Muthanna H. Al-Dahhan
_____________________________________________________________
August 2007
Saint Louis, Missouri, USA
_____________________________________________________________
Bubble and slurry bubble column reactors are used for a wide range of applications in the
chemical, petrochemical, and biochemical industries. A thorough understanding of their
complex flow structure is crucial for design and scale-up of these reactors.
This study used a multi-pronged approach to advance the state of knowledge of the
hydrodynamics of high pressure bubble and slurry bubble column reactors. First, the
effect of liquid phase physical properties and solids loading on the flow structure of
slurry bubble column reactors was studied, with particular emphasis on the churnturbulent flow regime. This study was performed in a system using a liquid phase which
at room temperature mimics Fischer-Tropsch (FT) wax at FT synthesis conditions and a
gas at a pressure that mimics syngas density. Computer Automated Radioactive Particle
Tracking (CARPT) and single source -ray Computed Tomography (CT) were utilized to
compute the time-averaged solids velocity fields, turbulent parameters profiles, and
time-averaged solids and gas holdup profiles.
The second part of this study included the development of non-invasive techniques, such
as CT and Nuclear Gauge Densitometry (NGD), for delineation of flow regimes in
bubble column reactors. The capability of these techniques to identify flow regime
transition was evaluated and compared against conventional methods of flow regime
demarcations, such as the change in the slope of the gas holdup curve and the drift flux
plot. Special attention was given to NGD to develop a non-invasive and online flow
regime measurement and monitoring technique. Hence, the guidelines and rules were set
up for these techniques (CT and NGD) by developing its flow regime identifiers. Both
of these techniques are active, i.e., involve penetration of -rays through the column,
and therefore are expected to represent the prevailing hydrodynamics with fidelity, even
in industrial scale columns.
The last part tackled the challenging task of extrapolating small diameter behavior to
large diameters, a task that essentially needs criteria for hydrodynamic similarity. Based
on a comprehensive review of the reported scaleup procedures, this work proposed a new
hypothesis for hydrodynamic similarity and subsequently for scale-up of bubble column
reactors operating in the regime of industrial interest, i.e., the churn-turbulent regime.
This task was performed in two stages: first, the proposed hypothesis was experimentally
evaluated for hydrodynamic similarity using existing CT and CARPT; second, for a
priori prediction of hydrodynamic parameters to maintain such similarity, state-of-the-art
correlations were developed using an Artificial Neural Network (ANN). The current
study showed that the similarity of overall gas holdup and its radial profile is pertinent for
similar recirculation and mixing in two systems. The similarity based only on global
hydrodynamics should be exercised with prudence.
The work accomplished in this study, and in particular the concepts developed in last two
parts, are, in retrospect, generic for multiphase reactors with bubble columns as an
example. Hence it presents promising avenues to explore them in other configurations of
multiphase reactors.
To
my Ammiji, Abbaji, and Didi
Copyright by
Ashfaq Shaikh
2007
Contents
1.
2.
3.
Tables .
Figures ...
Nomenclature
Acknowledgements ...
Page No.
ix
x
xix
xxiv
Introduction
1.1 Motivation .
1.2 Objectives .
10
1.3 Thesis Organization .
12
Literature Review
15
2.1 Mixing of liquid/slurry phase .
15
2.2 Flow Regime Transition .
18
2.2.1 Flow Regime Types and Characteristics
19
2.2.2 Methods for Flow Regime Identification ..
21
2.2.3 Prediction of Flow Regime Transition ..
26
2.2.4 Remarks .
26
2.3 Scaleup of Bubble Column Reactors
28
2.3.1 Reported status of scaleup in literature ..
28
2.3.2 Reported status of scaleup in industry
37
Experimental Investigation of the Hydrodynamics of Slurry

Bubble Column: Phase Holdups Distribution via Computed
Tomography .
39
3.1 Choice of Phases ..
40
3.2 Experimental Details
42
3.3 Single Source Computed Tomography (CT)
45
3.4 Results and Discussion.
4.
47
3.4.1 Overall gas holdup ...
47
3.4.2 Drift Flux Model ..
49
3.4.3 Cross-sectional Distribution of Gas Holdup
51
3.4.4 Time averaged gas and solids holdup radial profile
53
3.4.5 Effect of liquid phase physical properties on gas and solids

holdup radial profile
.
55
3.4.6 Effect of solids loading on gas and solids holdup radial

profile .
63
3.4.8 Normalized gas holdup radial profile .
67
3.4.9 Normalized solids holdup radial profile .
67
3.4.7 Comparison with predictions of Sedimentation-Dispersion

Model (SDM)
..
68
3.5 Remarks
70
Experimental Investigation of the Hydrodynamics of Slurry

Bubble Column: Solids Flow Pattern via CARPT
73
4.1 Experimental .
73
4.2 Computer Automated Radioactive Particle Tracking (CARPT) ..
74
4.3 Results and Discussion .
75
4.3.1 Time averaged solids velocities ..
75
4.3.2 Turbulent stresses and kinetic energy ..
81
4.3.3 Effect of liquid phase physical properties on solids axial

velocity and turbulent parameters parameters.
84
4.3.4 Effect of solids loading on solids axial velocity and turbulent

parameters ..
89
vi
5.
6.
4.3.5 Cross-sectional averaged turbulent stresses .
93
4.3.6 Turbulent eddy viscosity
93
4.3.7 Eddy diffusivities .
93
4.4 Remarks
94
Flow Regime Transition ...
95
5.1 Flow Regime Transition using CT ...
95
5.1.1 Experimental setup and conditions
96
5.1.2 Results and Discussion ...
96
5.1.3 Evaluation of the empirical correlations .
103
5.2 Flow Regime Transition using NGD
105
5.2.1 Nuclear Gauge Densitometry (NGD)
106
5.2.2 Results and Discussion ...
109
5.2.3 Evaluation of the flow regime identifiers developed for

NGD ...
130
5.2.4 Evaluation of literature correlations
142
5.3 Remarks
144
Scaleup of Bubble Column Reactors ...
147
6.1 Hypothesis for hydrodynamic similarity ..
147
6.2 Experimental conditions ...
149
6.3 Results ...
151
6.3a Discussion
162
6.4 Development of correlations for a priori prediction of

hydrodynamic parameters
166
vii
6.5 Remarks
167
Summary and Recommendations ...
168
7.1 Summary and Conclusions ...
168
7.2 Recommendations .
172
Appendix-A. Phase Distribution in Three Dynamic Phase Systems via

Combination of Computed Tomography (CT) and Electrical
Capacitance Tomography (ECT) .
175
Appendix -B. Experimental Investigation of Hydrodynamics of Slurry

Bubble Column Reactors via CT
186
Appendix -C. Experimental Investigation of Hydrodynamics of Slurry

Bubble Column Reactors via CARPT.
203
7.
Appendix -D. Sedimentation-Dispersion Model 231

Appendix -E. Material Safety Data Sheet for Therminol LT . 236
Appendix F. Development of Artificial Neural Network (ANN)
Correlations for Hydrodynamic Parameters . 244
References 269
Vita 279
viii
Tables
3-1
Physical properties of Sasol wax and Therminol LT
40
3-2
Experimental conditions employed in this study
45
3-3
The values of drift flux parameters at the studied experimental

conditions
50
4-1
CARPT experimental conditions
73
5-1
Comparison of experimental and predicted transition velocities

from the available correlations in an air-Therminol LT system
at various operating pressures
105
5-2
Characteristics frequencies in bubble column (Drahos et al.,

1991)
109
5-3
Slope of power spectra at studied operating conditions
128
5-4
Experimental conditions for evaluation of flow regime

identifiers
131
5-5
Statistical comparisons of prediction of correlations with

experimental data
144
6-1
List of similarity conditions in a 6 diameter stainless steel

column
151
6-2
List of experimental conditions of mismatch gas holdup radial

profile in a 6 diameter stainless steel column
152
ix
Figures
1-1
Schematic diagram of bubble/slurry bubble column
1-2
Projected US energy and oil production and consumption [Source:

National Energy Policy, White House Report, 2001]
1-3
US vulnerability to oil disruption (Williams and AlHajji, 2003)
1-4
a) M. King Hubbert at 1956 API Spring Meeting proposing peak

theory b) Popular Hubbert-peak curve.
1-5
Relationship between fuel economy and urban air benefits (Koelmel,

2005)
1-6
CAPEX cost for GTL (Rahmim, 2003)
1-7
Projected economies of scale for GTL-FT process (Brown, 2003)
2-1
Various flow regimes in bubble column reactors
20
2-2
Flow regime map for air-water system at ambient pressure a) Shah et

al., 1982 and b) Zhang et al., 1997
21
2-3
Photographs of bubbly and churn-turbulent flow in 2-D column
22
2-4
Typical overall gas holdup curve a) Shaikh and Al-Dahhan, 2005; and
b) Rados, 2003
23
2-5
Typical drift flux plot using Wallis (1969) approach (Deckwer et al.,
1981)
24
2-6
Average bubble-swarm velocity in air-ethanol-Co (van Baten et al.,

2003)
35
3-1
Bubble column reactor of 6 diameter used for CARPT/CT

measurements. CT1, CT2, and CT3 represent the scan levels used in
this investigation.
44
3-2
Configuration of the CT experimental setup (Kumar, 1994)
46
3-3
Effect of solids loading on a) overall gas holdup curve and b) drift

flux plot in air-Therminol LT-glass beads system at ambient
conditions in 6 steel column
48
3-4
Effect of operating pressure on overall gas holdup at various solids

loading in air-Therminol LT glass beads system in 6 steel column
49
3-5
Cross-sectional distribution of gas holdup in 6 diameter stainless

steel column using air-Therminol LT-glass beads system at different
superficial gas velocities, solids loading of 9.1 % vol. and P = a) 0.1,
and b) 1 MPa.
51
3-6
Cross-sectional distribution of gas holdup in 6 diameter stainless

steel column using air-Therminol LT-glass beads system at superficial
gas velocity of 30 cm/s, operating pressure of 1 MPa, and solids
loading of a) 9.1 and b) 25 % volume.
52
3-7
a)Gas holdup and b) solids holdup radial profile in air-Therminol LTglass beads system using 9.1 % vol. solids loading at superficial gas
velocity of 8 cm/s and ambient pressure
54
3-8
a) Gas holdup and b) solids holdup radial profile in air-Therminol LTglass beads system using 25 % vol. solids loading at superficial gas
velocity of 30 cm/s and operating pressure of 1 MPa
54
3-9
Overall gas holdup curve using air-water-glass beads (Rados, 2003)

and air-Therminol LT-glass beads system at ambient conditions,
solids loading of 9.1 % vol. in a 6 diameter column.
55
3-10
Effect of physical properties on a) gas holdup, and b) solids holdup

radial profile at P = 0.1 MPa, z/D = 5.5, solids loading of 9.1 % vol.
and Ug = a) 8, b) 14, and c) 30 cm/s in 6 diameter steel column
58
3-11
Overall gas holdup curve using air-water-glass beads (Rados, 2003)

and air-Therminol LT-glass beads system at operating pressure of 1
MPa, solids loading of 9.1 % vol. in a 6 diameter column..
60
3-12
Effect of physical properties on a) gas holdup, and b) solids holdup

radial profile at P = 1 MPa, z/D = 5.5 and solids loading of 9.1 % vol.
at Ug = a) 8, b) 14, and c) 30 cm/s in 6 diameter steel column
61
3-13
Effect of solids loading on gas and solids holdup radial profile in airTherminol LT-glass beads system at ambient pressure at Ug = a) 20
and b) 30 cm/s 6 diameter steel column
64
3-14
Effect of solids loading on gas and solids holdup radial profile in airTherminol LT-glass beads system at Ug = a) 20 and b) 30 cm/s and P
= 1 MPa in 6 steel column
66
xi
3-15
Predictions of the SDM in air-Therminol LT-glass beads system at

ambient pressure and solids loading of a) 9.1 and b) 25 % vol. in 6
diameter column
68
3-16
Comparison of the SDM predictions with experimental data in airTherminol LT-glass beads system at ambient pressure, solids loading
of 9.1 % vol., and Ug = a) 8 and b) 30 cm/s in 6 diameter column
69
3-17
Comparison of the SDM predictions with experimental data in airTherminol LT-glass beads system at ambient pressure. a) effect of
superficial gas velocity at solids loading of 25 % vol. and b) effect of
solids loading at Ug = 30 cm/s in 6 diameter column
70
4-1
Configuration of the CARPT experimental setup (Degaleesan, 1997)
75
4-2
Time and azimuthally averaged solids velocity in air-Therminol LTglass beads system at Ug = 30 cm/s, P = 0.1 MPa, and solids loading =
9.1 % volume a) uz-ur vector map, b) axial, and c) radial velocity
components
77
4-3
Radial profile of solids a) axial, b) radial, and c) tangential velocity in

air-Therminol LT-glass beads system at Ug = 30 cm/s, P = 0.1 MPa,
and solids loading = 9.1 % volume
77
4-4
Probability distribution function of solids axial velocities at L/D = 2.5

at various dimensional radius positions of r/R = 0.063, 0.44, and 0.96
at Ug = 30 cm/s, P = 0.1 MPa, and solids loading of 9.1 % volume
78
4-5
Probability distribution function of solids axial velocities at L/D = 2.5,

5.5, and 9 along the column radius at r/R = 0.063, 0.44, 0.69, and 0.96
at Ug = 30 cm/s, P = 0.1 MPa, and solids loading of 9.1 % volume
79
4-6
Probability distribution function of solids axial velocities in fully

developed flow in the column center and near the wall at a) 30 cm/s,
9.1 % vol., and 0.1 MPa, b) 30 cm/s, 9.1 % vol., and 1.0 MPa, and c)
30 cm/s, 25 % vol., and 1.0 MP in 6 diameter stainless steel column.
80
4-7
Radial profile of solids a) turbulent kinetic energy, and b) axial, b)

radial, and c) tangential normal stresses in air-Therminol LT-glass
beads system at Ug = 30 cm/s, P = 0.1 MPa, and solids loading = 9.1
% volume.
82
4-8
Radial profile of solids shear stress components in an air-Therminol

LT-glass beads system at Ug = 30 cm/s, P = 0.1 MPa, and solids
loading = 9.1 % volume
84
xii
4-9
Comparison of radial profile of a) gas holdup, b) solids axial velocity

c) solids TKE, and d) solids shear stress in air-waterglass beads and
air-Therminol LT-glass beads system at Ug = 30 cm/s, P = 0.1 MPa,
and solids loading of 9.1 % vol.
86
4-10
Comparison of radial profile of a) gas holdup, b) solids axial velocity

c) solids TKE, and d) solids shear stress in air-water-glass beads and
air-Therminol LT-glass beads system at Ug = 30 cm/s, P = 1 MPa, and
solids loading of 9.1 % vol.
87
4-11
Effect of solids loading on radial profile of solids a) axial velocity, b)

turbulent kinetic energy, c) axial normal stress, and d) shear stress in
air-Therminol LT-glass beads system at Ug = 20 cm/s, and P = 0.1
MPa.
89
4-12

air-Therminol LT-glass beads system at Ug = 30 cm/s, and P = 0.1
MPa
90
4-13

air-Therminol LT-glass beads system at Ug = 20 cm/s, and P = 1 MPa
91
4-14

air-Therminol LT-glass beads system at Ug = 30 cm/s, and P = 1 MPa.
92
5-1
Gas holdup radial profile at various superficial gas velocities in an airTherminol LT system at ambient condition in a 0.162 m steel column.
97
5-2
a) Cross-sectional averaged gas holdup versus superficial gas velocity

and b) Drift flux plot based on cross-sectional averaged gas holdup in
an air-Therminol LT system at ambient conditions in a 0.162 m steel
column.
99
5-3
Evolution of steepness parameter with superficial gas velocity in an

air-Therminol LT system at ambient conditions in a 0.162 m steel
column.
100
5-4
Gas holdup radial profile at various superficial gas velocities in an airTherminol LT system at operating pressure of 0.4 MPa in a 0.162 m
steel column.
100
5-5
a) Gas holdup curve based on cross-sectional averaged gas holdup and

b) Flux plot based on cross-sectional averaged gas holdup in an air-
101
xiii
Therminol LT system at operating pressure of 0.4 MPa in a 0.162 m

steel column.
5-6
a) Gas holdup curve based on cross-sectional averaged gas holdup and

b) Drift flux plot based on cross-sectional averaged gas holdup in an
air-Therminol LT system at operating pressure of 1.0 MPa in a 0.162
m steel column.
102
5-7
Evolution of steepness parameter with superficial gas velocity in an

air-Therminol LT system at operating pressures of 0.4 and 1 MPa in a
0.162 m steel column
103
5-8
Experimental setup of Nuclear Gauge Densitometry (NGD)
108
5-9
Overall gas holdup curve using an air-water system at ambient

conditions in 0.1012 m diameter column
110
5-10
Drift flux plot using an air-water system at ambient conditions in

0.1012 m diameter column
110
5-11
Time-series of photon count fluctuations in 0.1012 m diameter column

in a) empty column and b) water (no gas flow).
111
5-12
Time-series of photon count fluctuations in 0.1012 m diameter column

using air-water system at superficial gas velocity of in a) 1, b) 3, c) 7,
and d) 11 cm/s at ambient conditions.
112
5-13
Variation of variance of photon counts fluctuations with superficial

gas velocity in 0.1012 m diameter column using air-water system at
ambient conditions.
114
5-14
Variation of variance of pressure drop fluctuations with superficial gas

velocity in 0.1012 m diameter column using air-water system at
ambient conditions (Reproduced from Lin et al., 1999).
115
5-15
The coefficient of departure from Poisson distribution versus

superficial gas velocity in 0.1012 m diameter column using an airwater system at ambient conditions.
117
5-16
Autocorrelation curve at superficial gas velocities of a) 1, b) 3, and c)

4 cm/s using an air-water system in 0.1012 m diameter column at
ambient conditions.
118
5-17
Autocorrelation curve at superficial gas velocities of a) 7, b) 9, and c)

11 cm/s using an air-water system in 0.1012 m diameter column at
ambient conditions.
119
xiv
5-18
Typical log-log plot of normalized psdf at superficial gas velocities of

a) 1, b) 3, c) 4, d) 6, e) 9, and f) 11 cm/s using an air-water system in
0.1012 m diameter column at ambient conditions.
122
5-19
Power spectra of liquid velocity fluctuations in a bubble column by

Zarzewski et al. (1981).
124
5-20
LDA axial velocity signal power spectra a) D = 15 cm, Ug = 2.7 cm/s,

z/D = 5.5, b) D = 23 cm, Ug = 1.2 cm/s, z/D = 6, and c) D = 40 cm,
Ug = 5.5 cm/s, z/D = 5 (Groen, 2004)
125
5-21
Log-log plot of normalized psdf of photon counts history obtained in

a) empty column and b) water (with no gas flow).
127
5-22
Log-log plot of normalized psdf with fitted slope line at superficial

gas velocities of a) 4, b) 6, c) 9, and d) 11 cm/s using an air-water
system in 0.1012 m diameter column at ambient conditions
127
5-23
a) Overall gas holdup curve and b) drift flux plot in an air-water

system at ambient pressure in 6 diameter stainless steel column
132
5-24
Variation of coefficient of departure, Dp with superficial gas velocity

in an air-water system at ambient pressure in 6 diameter stainless
steel column
132
5-25
Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at ambient pressure using an air-water
system.
133
5-26
Psdf plot at superficial gas velocity of a) 2 cm/s, b) 7 cm/s, and c) 20

cm/s and ambient pressure using an air-water system in 6 diameter
stainless steel column.
133
5-27
a) Overall gas holdup curve and b) drift flux plot in an air-water

system at operating pressure of 1 MPa in 6 diameter stainless steel
column
134
5-28
Variation of coefficient of departure, Dp, with superficial gas velocity

in an air-water system at operating pressure of 1 MPa in 6 diameter
stainless steel column
135
5-29
Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at operating pressure of 1 MPa using an
air-water system.
135
xv
5-30

cm/s and operating pressure of 1 MPa using an air-water system in 6
diameter stainless steel column.
135
5-31
a) Overall gas holdup curve and b) drift flux plot in an air-C9-C11

system at operating pressure of 0.1 MPa in 6 diameter stainless steel
column
136
5-32
Variation of coefficient of departure, Dp, with superficial gas velocity

using an air-C9-C11 system at operating pressure of 0.1 MPa in 6
diameter stainless steel column
137
5-33
Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at ambient pressure using an air-C9-C11
system.
137
5-34

cm/s and ambient pressure using an air- C9-C11 system in 6 diameter
138
5-35
a) Overall gas holdup curve and b) drift flux plot in an air-C9-C11

system at operating pressure of 1 MPa in 6 diameter stainless steel
column
138
5-36
Variation of coefficient of departure, Dp with superficial gas velocity

using an air-C9-C11 system at operating pressure of 1 MPa in 6
139
5-37
Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at operating pressure of 1 MPa using an
air-C9-C11 system.
139
5-38

cm/s and operating pressure of 1 MPa using an air- C9-C11 system in
6 diameter stainless steel column.
140
5-39
Comparison of reported correlations with transition velocities

obtained based on variation in Dp of photon counts history in a) an
air-water system b) an air- C9-C11 system at ambient and high
pressure.
143
6-1
Comparison of gas holdup radial profile in 6 column using an airwater system at two different operating conditions [D6U12P7Water: 7
bar, 12 cm/s, air-water (Kemoun et al., 2001); D6U60P1Water: 1 bar,
60 cm/s, and air-water (Ong, 2003)] with similar overall gas holdup (~
0.41).
148
xvi
6-2
a) Gas holdup and b) Axial liquid velocity radial profile in 6 diameter

stainless steel column using an air-water system [D6P4U45: 6 inch
diameter, 4 bar, and 45 cm/s (Ong, 2003), D6P10U30: 6 inch
diameter, 10 bar and 30 cm/s] (Overall gas holdup ~ 0.41).
152
6-3
Variation of AARD in liquid axial velocities between similarity

conditions [D6P4U45Water (Ong, 2003) and D6P10U30Water] along
the column radius in 6 diameter stainless steel column using an airwater system.
153
6-4
TKE profile in 6 diameter stainless steel column using an air-wate

system [D6P4U45: 6 inch diameter column, 4 bar and 45 cm/s (Ong
2003), D6P10U30: 6 inch diameter column, 10 bar and 30 cm/s
(Overall gas holdup ~ 0.41).
153
6-5

stainless steel column using an air-water system (D6P1U45Water: 6
inch diameter column, 1 bar and 45 cm/s, D6P4U30Water: 6 inch
diameter column, 4 bar and 30 cm/s) [Overall gas holdup ~ 0.35].
154
6-6

conditions (D6P1U45water and D6P4U30water) along the column
radius in 6 diameter stainless steel column using an air-water system.
155
6-7
TKE radial profile in 6 diameter stainless steel column using an airwater system (D6P1U45Water: 6 inch diameter column, 1 bar and 45
cm/s, D6P4U30Water: 6 inch diameter column, 4 bar and 30 cm/s)
[Overall gas holdup ~ 0.35].
155
6-8

stainless steel column [D6P1U30 C9-C11: 6 inch diameter column, 1
bar, 30 cm/s (Han, 2006), and air- C9-C11 fluid system,
D6P4U30water: 6 inch diameter column, 4 bar, 30 cm/s, and an airwater system] [Overall gas holdup ~ 0.35].
156
6-9

conditions [D6P1U30C9-C11 (Han, 2006) and D6P4U30water] along
the column radius in 6 diameter stainless steel column.
157
6-10
TKE radial profile in 6 diameter stainless steel column (D6P1U30

C9-C11: 6 inch diameter column, 1 bar, 30 cm/s, and air- C9-C11 fluid
system, D6P4U30water: 6 inch diameter column, 4 bar, 30 cm/s, and
an air-water system) [Overall gas holdup ~ 0.35].
157
6-11
159
xvii
stainless steel column (D6P4U30water: 6 inch diameter column, 4 bar

and 30 cm/s, air-water; D6P4U16C9-C11: 6 inch diameter column, 4
bar and 16 cm/s, air- C9-C11) [Overall gas holdup ~ 0.35].
6-12

conditions (D6P4U30water and D6P4U16C9-C11) along the column
radius in 6 diameter stainless steel column.
159
6-13
TKE radial profile in 6 diameter stainless steel column

(D6P4U30water: 6 inch diameter column, 4 bar and 30 cm/s, an airwater; D6P4U16C9-C11: 6 inch diameter column, 4 bar and 16 cm/s,
air- C9-C11) [Overall gas holdup ~ 0.35].
160
6-14

stainless steel column (D6P4U30water: 6 inch diameter column, 4 bar
and 30 cm/s, an air-water; D6P10U8C9-C11: 6 inch diameter column,
10 bar and 8 cm/s, air- C9-C11) [Overall gas holdup ~ 0.35].
161
6-15

conditions (D6P4U30water and D6P10U8C9-C11) along the column
radius in 6 diameter stainless steel column.
161
6-16
TKE radial profile in 6 diameter stainless steel column

(D6P4U30water: 6 inch diameter column, 4 bar and 30 cm/s, an airwater; D6P10U8C9-C11: 6 inch diameter column, 10 bar and 8 cm/s,
air- C9-C11) [Overall gas holdup ~ 0.35].
162
6-17
Gas holdup radial profile in 6 diameter stainless steel column

(D6U2P1water: 1 bar and 2 cm/s, an air-water; D6U3P1TherminolLT:
1 bar and 3 cm/s, air- Therminol LT) [Overall gas holdup ~ 0.1].
165
6-18
Gas holdup radial profile in 6 diameter stainless steel column

(D6U5P4TherminolLT: 4 bar and 5 cm/s, air-Therminol LT;
D6U3.5P10Therminol: 10 bar and 3.5 cm/s, air- Therminol LT)
[Overall gas holdup ~ 0.22].
165
xviii
Nomenclature
BO
Bodenstein number, dimensionless
Wall holdup parameter (equation 3-2), dimensionless
Wall holdup parameter (equation 3-4), dimensionless
C0
Distribution parameter in drift flux model, dimensionless
C1
Weighted average drift velocity, m.s-1
CD
Drag coefficient, dimensionless
CV
Volumetric solids loading (equation 2-3), dimensionless
Cxx
Autocorrelation function, dimensionless
Column diameter, m
dB
Bubble diameter, cm
dB
Dimensionless bubble diameter, dimensionless
DG
Gas dispersion coefficient, m2.s-1
DL
Liquid dispersion coefficient, m2.s-1
DP
Coefficient of departure from Poisson distribution, dimensionless
Drr
Radial eddy diffusivity, m2.s-1
DR
Ratio of gas and liquid phase densities, dimensionless
Dzz
Axial eddy diffusivity, m2.s-1
Permittivity, F.m-1
Eo
Etovos number, dimensionless
Frequency, Hz
F(x)
Fourier transform of x
Frg
Gas Froude number, dimensionless
xix
Gravity constant, m.s-2
Hd
Dynamic height, m
HS
Static height, m
Number of input nodes
drift flux, m.s-1
Number of hidden layers
k0
Pseudo-first order rate constant, s-1
kLa
Volumetric mass transfer coefficient, s-1
Turbulent kinetic energy, cm2.s-2

Number of output nodes
Column length, m
Mo
Morton number, dimensionless
Slope of gas holdup curve (equation 2-1), dimensionless

Steepness parameter of gas holdup radial profile (equation 3-2), dimensionless
Steepness parameter of solids holdup radial profile (equation 3-4), dimensionless
Length of time series, dimensionless
Radial location in the column, m
rk
Relative permittivity, dimensionless
Cross-correlation coefficient
Relative volumetric attenuation coefficient
Re
Reynolds number, dimensionless
Sk
Normalized output variable
length of time series, min
ui
ub0
Fluctuation velocity in ith direction (i = r, , z)

Terminal velocity of an isolated bubble, m.s-1
xx
UB
Terminal bubble rise velocity, m.s-1
UG
Superficial gas velocity, m.s-1
UGtrans Superficial gas velocity at flow regime transition, m.s-1

Ui
Normalized input variable
UL
Superficial liquid velocity, m.s-1
Ulb
Large bubble rise velocity, m.s-1
umax
Rise velocity of maximum stable bubble size, m.s-1
ur
Solids radial velocity, m.s-1
u rec
Liquid recirculation velocity, m.s-1
Usb
Small bubble rise velocity, m.s-1
uslip
Slip velocity, m.s-1
uz
Solids/liquid axial velocity, m.s-1
Solids azimuthal velocity, m.s-1
Vb0
Bubble rise velocity at vanishingly small velocity, m.s-1
wij,wjk ANN fitting parameters
Greek Letters
Cross-sectionally averaged gas holdup, dimensionless
Overall gas hold up at transition point, dimensionless
Overall gas hold up, dimensionless
trans
Cross-sectionally averaged solids holdup, dimensionless
Overall solids hold up, dimensionless

xxi
SL
Solids loading, dimensionless
Constant (equation 2-17), dimensionless
eff
Effective turbulent eddy viscosity, cm2.s-1
BIT
Turbulent eddy viscosity due to bubble-induced turbulence, cm2.s-1
SIT
Turbulent eddy viscosity due to shear-induced turbulence, cm2.s-1
Molecular viscosity, cm2.s-1
Solids loading, (% vol/ %vol), dimensionless
SC
Critical solids loading, (% vol/ %vol), dimensionless
Mean of a time-series, dimension of time-series
Phase angle of cross-spectral density function, rad
Standard deviation of a time series, dimension of time-series

Surface tension, dyne.cm-1
Time lag, sec
Drag interaction parameter, dimensionless
Particle to liquid density ratio, dimensionless
Drag interaction parameter, dimensionless
Gas phase density, kg m-3
Liquid phase density, kg m-3
Solids phase density, kg m-3
SL
Slurry phase density, kg m-3
Liquid surface tension, N m-1
Liquid viscosity, kg m-1 s-1
xx
Power spectral density function
Correction factor, dimensionless
xxii
Time lag, sec
Abbrevations
AARD
Average Absolute Relative Difference
AARE
Average Absolute Relative Error
ANN
Artificial Neural Network
ARD
Absolute Relative Difference
CARPT
Computer Automated Radioactive Particle Tracking
CFD
Computational Fluid Dynamics
CT
Computed Tomography
DGD
Dynamic Gas Disengagement
ECT
Electrical Capacitance Tomography
FT
Fischer-Tropsch
GTL
Gas-to-Liquids
LDV
Laser Doppler Velocimetry
PBM
Population Balance Model
PDF
Probability Density Function
PIV
Particle Image Velocimetry
PSDF
Power Spectral Density Function
SDM
Sedimentation Dispersion Model
xxiii
Acknowledgements
First and foremost, thanks are due to the One God for His kindness and blessings, for
they sailed me through the ups and downs, and ecstasies and agonies during this time. It
is divinity we tend to believe in during such times, however, per JFKs famous quote
...here on earth, God's work must truly be our own, for better or worse we tend to rely
on people around us. As I am writing this acknowledgement, I see a fine ray of hope of
getting some name to the work and efforts of these peak years of my youth and also feel a
sense of gratitude to all those who have influenced it in some or other way during these
years.
I express a deep sense of gratitude to my advisor, Prof. M. H. Al-Dahhan, for giving me

an opportunity to work on this project. I wish to thank him for his encouragement and
support throughout my doctoral work which helped me overcome many obstacles. The
load of enthusiasm and intensity he brings to the work is simply amazing. The times
spent helping him on different reports, presentations, and short courses on bubble
columns were unforgettable.
I would like to thank Prof. M. P. Dudukovic for his comments on some parts of my work
and for being on my committee. It was indeed an experience to see him working so
closely which was and will be useful in future. I am thankful to my committee members,
Prof. P. A. Ramachandran, Prof. John Kardos, Prof. R. A. Gardner, and Dr. Jiangping
Zhang (Chevron) for investing their time and providing valuable comments. I also want
to thank my thesis committee members Prof. Ramesh Agarwal and Dr. Ralph Goodwin
(ConocoPhillips, USA) for agreeing to be on my committee and investing their valuable
time on relatively short notice. Thanks to Prof. Ramachandran for teaching me as well as
discussing facets of multiphase reactor modeling and to Prof. Kardos for being supportive
during different stages.
I would like to acknowledge the financial support of the High Pressure Slurry Bubble
Column Reactor Consortium (HPSBRC) [ConocoPhillips, USA; EniTech, Italy; Sasol,
xxiv
South Africa; Statoil, Norway] and the U.S. Department of Energy-University Coal
Research (DOE-UCR) grant (DE-FG26-99FT40594) that made this work possible. The
interactions with scientists and engineers from these industries during bi-annual review
meetings were a rewarding experience. The discussions with Drs. Alex Vogel and
Bremann Berthold of Sasol and Christina Marretto of EniTech provided me much needed
industrial perspective on parts of my research. During these years, I worked on various
bubble column related projects of Syntroleum Corporation and Snamprogetti that
certainly helped in looking at things from different angles. For the sake of my fancy of
undergraduate days, I had gone through Fischer-Tropsch (FT) synthesis and in general
Gas-to-Liquid (GTL) literature, most of it made sense after those long discussions with
Dr. Steve LeViness from Schlumberger. The discussions with him were invaluable and
further enhanced my interest in the field of energy. Thanks to Dr. Kym Arcuri from
Syntroleum for those valuable suggestions and advice, they were timely and will
certainly be useful.
I wish to acknowledge Professor K. Krishnaiah of the Indian Institute of Technology

(IIT), Madras for encouraging me to pursue doctoral studies. His reaction engineering
classes and surprise tests were certainly an enjoyable and memorable experience during
IIT-days. I am also thankful to my masters research advisors Drs. Abhijit Deshpande and
Susy Varughese of IIT, Madras.
Apart from CRELs abundant and high quality literature on bubble column reactors, I
immensely benefited from the works of Prof. J. B. Joshi of MUICT, Prof. R. Krishna of
University of Amsterdam, and Prof. L. S. Fan of OSU.
Prof. Krishnas creative
descriptions of complex phenomena have been always a pleasure to read.
I am thankful to Mr. Pat Harkins, Mr. Jim Linders, and Mr. John Krietler for helping me
in various technical issues and fabrication of equipments. The experience of Mr. Steve
Picker was useful, particularly during crunch times. Mr. Edward Lau and Mrs. Susan
Tucker (MIT Nuclear Reactor) were extremely helpful during irradiation of tracer
radioactive particles.
xxv
Numerous people at CREL were of immense help during these years. I thank Dr. Novica
Rados, with whom I started my research day-1 at CREL. He introduced me to CARPT,
CT, and experimental issues related to radioactive materials and bubble columns. I am
thankful to Dr. Muhammad Rafique for discussions on general research in multiphase
flows and also on different topics in my initial days. I am also thankful to Drs. Peter
Spicka and Stoyan Nedeltchev, who helped me understand various aspects of bubble
columns in the first year. The several useful discussions with Stoyan on regime transition
and chaos theory along with my own literature survey on regime transition convinced me
to work on flow regime transition in my thesis (although not using pressure fluctuations).
The long conversations with Dr. W. Warsito (OSU) on tomography were enlightening
and extremely useful. I wish to acknowledge Mr. Klass Koop for those daily insightful
discussions on hydrodynamics and mass transfer in bubble columns while we were
sharing an office. I am thankful to Mr. Lu Han and Mr. Chengtian Wu for helping me
during CARPT and other experimental work. Working together on the consortium project
with Novica, Lu, and Chengtian was an experience to remember. I am also thankful Dr.
Liu, a visiting scholar from China, and Mr. Saurabh Agarwala for being a timely help on
countless occasions when I was working late nights on CARPT/CT with Therminol LT. I
wish to acknowledge the help I received from Mr. Rajneesh Varma with a new CT setup
and experiments during joint work with OSU. I am thankful to Dr. Satish Bhusarapu for
his timely help at numerous occasions during my experimental work. The help I received
from Mr. Z. Kuzeljevic and Mr. S. Nayak during CT and CARPT experiments is highly
appreciated.
I wish to acknowledge the help of the secretaries of the Department of Chemical

Engineering in numerous administrative issues. I wish to thank Dr. Y. Yamashita for his
prompt help in computer and network related issues. The discussions on chaos theory,
symbolic dynamics, and S-statistics with Dr. Miryan Cassanello from University of
Buenous Aires were helpful in improving my knowledge regarding time-series analysis.
Thanks to Mr. Jim Ballard from the Engineering Technical Writing Center for going
through the manuscripts and helping to improve their language. Discussions with him on
nuances of technical English to various topics were amazing. I must also thank the
xxvi
personnel of InterLibraryLoan (ILL) services for providing the needed references on

time. Thanks to all those unknown faces behind Google and Wikipedia, for without them
my research life would not have been complete. However, I must mention that these were
not used as the scholarly references during this work.
During these years, I have made numerous friends who were of immense help time and
time and also made my stay enjoyable. Thanks to Dr. R. Ramaswamy for all those
agreements and disagreements over wide ranging issues during Sub-way lunches. I
assume they will continue. I wish to acknowledge all my roommates over these years
namely, Dennis Thomas, Keshav Ruthiya, Wisam Khudayar, and Ahmed Youssef. The
discussions with Keshav, ranging from the economy of chemical industries to economy
of India, to fancy business plans certainly diversified my interests. Thanks, Ahmed for
being a co-operative roommate during my last few months. Time spent with Ahmed and
Keshav was indeed a learning experience for me. I am thankful to many other people who
made a difference in one way or other: Shaibal, Pubs, Kartik, Subu, Karim, Mehul,,
Salim, Huping, Rajneesh, Radmila, Kaps, Saurabh, RC, DG, Ert, Nicola, Prashant.
Thanks to Abdul Rehman, Rehan, and Jaani for Eid dinners and to Chachi and Dr. Zakir
Sabry for making the environment during fasting far lighter and fun. I am thankful to
Jaani and Vikram for those weekend movie and biryani times in last years. Thanks to Mr.
Farhan Majid for discussing those lofty and fancy ideas related to economics.
I express a deep sense of gratitude to my parents and my younger sister for unconditional
support, patience, and belief in me. My father is my strength, and I forever appreciate the
courage of my mother in allowing her only son to go to the other side of the globe for
further education. In school days, out of guilt, I would pretend studying seeing my
younger sister studying so hard. I guess those times helped me when I actually started
studying. Words are just not enough to thank them. I owe everything that I have achieved
to them. I am thankful to my grandfathers and grandmothers, who, out of their affection
for my parents, wanted me to have some education. I wish to thank my Mumaani and
Mamu and also my other relatives for being a moral support to my family during these
years.
xxvii
Robert Frost ended his poem Stopping by Woods on Snowy Evening as,
The woods are lovely, dark and deep,
But I have promises to keep,
And miles to go before I sleep,
And miles to go before I sleep.
As I end my walk through this portion of the woods and hope to enter a new one, I thank,
from the bottom of my heart, all those who directly and indirectly helped me over the
years during this journey.
Ashfaq Shaikh
Washington University, St. Louis
xxviii
Chapter 1.
Introduction
Bubble columns are two-phase gas-liquid systems in which a gas is dispersed through a
sparger and bubbles through a liquid in a vertical cylindrical column (Figure 1-1), with or
without internals. When suspended fine solids are present in liquid, they form a slurry
phase. Accordingly, they can be called either two-phase or three-phase (slurry) bubble
column. The liquid/slurry phase flow can be either co-current, counter-current, or in
batch mode with respect to the gas flow. The size of the solid particles ranges from 5 to
150 m, with solids loading up to 50 % volume (Krishna et al., 1997). The gas phase
contains one or more reactants, while the liquid phase usually contains product and/or
reactants (or is sometimes inert). The solid particles are typically catalyst. In these
reactors, momentum is transferred from the faster, upward moving gas phase to the
slower liquid/slurry phase. Generally, the operating liquid superficial velocity (in the
range of 0 to 2 cm/s) is an order of magnitude smaller than the superficial gas velocity (1
to 50 cm/s). Hence, the hydrodynamics of such reactors are controlled mainly by the gas
flow.
Bubble columns offer numerous advantages such as good heat and mass transfer
characteristics, no moving parts and thus reduced wear and tear, higher catalyst
durability, ease of operation, and low operating and maintenance cost. One of the main
disadvantages of bubble column reactors is significant back-mixing, which can reduce
product conversion. The excessive back-mixing can be overcome by modifying the
design of bubble column reactors. Such modifications include the addition of internals,
baffles (Deckwer, 1991), or sieve plates (Maretto and Krishna, 2001). Bubble column
reactors have been used in chemical, petrochemical, biochemical, and pharmaceutical
industries for various processes (Carra and Morbidelli, 1987; Deckwer, 1992; Fan, 1989).
Gas Outlet
Liquid
.
Solids
Liquid
... . . .
Sparger
Gas Inlet
Figure 1-1: Schematic diagram of bubble/slurry bubble column

Examples of such chemical and petrochemical processes are the partial oxidation of
ethylene to acetaldehyde, wet-air oxidation (Deckwer, 1992), liquid phase methanol
synthesis
(LPMeOH),
Fischer-Tropsch
(FT)
synthesis
(Wender,
1996),
and
hydrogenation of maleic acid (MAC). In biochemical industries, bubble columns are used
for cultivation of bacteria, cultivation of mold fungi, production of single cell proteins,
animal cell culture (Lehmann et al., 1978), and treatment of sewage (Diesterweg, 1978).
In metallurgical industries, they can be used for leaching of ores. The most popular
3
present day application of bubble columns is for energy conversion process where
stranded gas is converted to liquids. The popularity of such a conversion is a response
to the postulated future energy crisis.
Albert Einstein once wrote, I never think of the future, it comes soon enough. Einsteins
convenient approach to the future is a luxury that is denied to governments and energy
companies. These days of global economy and increased energy demands, coupled with
complex international relationships and interdependence, demand an understanding of the
probable trends and the drivers for future energy use. Figure 1-2 shows the projected gap
between oil production and consumption in USA. Currently, North America imports 65
% of their crude oil. With the economic growth of China, India, and other developing
countries, the demand for oil in these countries has risen significantly. Currently, Asia
imports approximately 65 % of their crude oil, while Western Europe imports 55 % of its
crude oil (Koelmel, 2005). These countries depend on the oil producing countries to meet
their energy demands. With current scenarios, it is clear that such dependence possibly
makes an existence of their own and subsequently of other nations vulnerable.
Figure 1-2: Projected US energy and oil production and consumption [Source: National
Energy Policy, White House Report, 2001]
Figure 1-3 shows the vulnerability of the US to oil supply disruption. The percentage of
the vulnerability depends on the oil supply from secure and nonsecure sources.
4
Presently, US vulnerability is at its peak, and is higher than during the first and second
energy shocks (Williams and Alhajji, 2003). Such scenarios are the motivation to come
up with a solution to meet the future energy challenges. The energy business is
characterized by large-scale, long-term investment and there is an urgent need to
understand potential future energy solutions. Because the latter half of Albert Einsteins
approach is not a luxury but a universal fact. It is said that the single biggest shift in
global demand for oil over the past decade has not been the rise of China but the rise of
SUVs (Zakaria, 2006). Hence, the solution to problems regarding energy demands a
multidimensional approach that involves politicians, policy makers, scientists,
technologists, and consumers of energy.
Figure 1-3: US vulnerability to oil disruption (Williams and AlHajji, 2003)

Shell geologist M. King Hubbert analyzed oil production utilizing the concept used by
population biologists to examine population growth. Hubbert (1956) predicted that US oil
production would peak in the early 1970s (Figure 1-4), which proved correct. He
predicted in 1969 that world oil production would peak around the year 2000, which is
supposedly also coming true (Deffeyes, 2004). In addition, the assessment of Simmons
(2005) of key oil fields in the world calls for heavy investment in alternative energy
5
strategies. Such strategies should give priority to proven technologies rather than those
still in initial stages.
(a)
(b)
Figure 1-4: a) M. King Hubbert at the 1956 API Spring Meeting where he proposed the
peak theory b) Popular Hubbert-peak curve.
The development of Gas-to-Liquid (GTL) conversion provides one piece of a more
complex solution. The development of GTL worldwide today suggests that it has the
potential to supply 10 % of the global diesel fuel market within the next 15 years. The use
of GTL fuel, in addition to utilizing flared and stranded gas, can aid energy conservation.
US economies are dominated by petrol fuels and thus, spark ignition engines, which are
less efficient than diesel engines. As shown in Figure 1-5, compared to the conventional
refinery fuels, GTL fuel can improve transportation fuel economy and carbon dioxide
efficiency while also augmenting urban air quality benefits. Hence, the combination of
efficient engines and clean fuels allows economies to reduce fuel consumption, reduce
greenhouse emissions, and improve air quality (Koelmel, 2005).
While GTL is a marginally commercial proposition today, it is a proven technology
compared to most other alternative energy technologies such as hydrogen and biomass.
Figure 1-5: Relationship between fuel economy and urban air benefits (Koelmel, 2005)
Since Franz Fischer and Hans Tropsch developed the process to convert CO/H2 mixture
into hydrocarbons and oxygenated compounds back in 1922, the obvious question is why
was its potential not un-locked before now? The answer lies in the Capital Expenditure
cost (CAPEX) of the GTL process, which has remained above $ 20,000/per specific
barrel of installed GTL capacity. The early pioneers of this process, specifically Sasol,
built plants at more like $ 120,000/bpd. As shown in Figure 1-6, the current CAPEX
remains close to $ 25,000/bpd (Brown, 2003). However below $ 20,000/bpd, one can
reach a watershed where GTL becomes attractive. At this cost, the resource holders have
enough margin to compete with refinery products.
Figure 1-6: CAPEX cost for GTL (Rahmim, 2003).
7
An improvement in efficiency of the GTL industry can be realized through economies of
scale, reduced costs from technology improvements in all areas of the processes, and
process efficiency gains from de-bottlenecking (Koelmel, 2005). As far as multiphase
reaction engineering domain is concerned, the solution lies in improving catalyst
efficiency and economies of scale. Espinoza et al. (1999) recommended that an ideal
catalyst, apart from its high selectivity, should have the activity of cobalt and robustness
of iron towards changing conditions. As shown in Figure 1-7, an economy of scale
suggests that GTL can become economically viable if high capacity plants are built.
Figure 1-7: Projected economies of scale for GTL-FT process (Brown, 2003).
Based on Figure 1-7, it is clear that to reach below the $ 20,000/bpd mark from the
current level, the plant capacity need to be increased by at least double. The high capacity
plants will need efficient catalysts and, more importantly, larger reactors. The different
reactor configurations utilized for FT processes are divided into two types, depending
upon the types and quantities of FT products required.
1. High temperature FT (HTFT): This process, with an iron based catalyst and
temperature in a range of 300 3500 C, is used for production of gasoline and low
molecular weight olefin (C3 C11). The reactors are circulating fluidized beds (CFBs)
and fixed fluidized beds (FFBs).
8
2. Low temperature FT (LTFT): This process, with either an iron or cobalt based
catalyst and temperature in a range of 200 2400 C, is used for the production of high
molecular weight linear waxes (> C20). The reactors are fixed beds and slurry bubble
columns.
The design of bubble columns has been considered for low temperature FT processes
since Kolbels pioneering work in 1950s. According to Krishna and Sie (2000), with the
present state of knowledge, it can be expected that a bubble column reactor may achieve
productivity a thousand times higher than that of the classical FT reactors (such as fixed
beds and multibed reactors) used in industry. However, there are considerable reactor
design and scale-up problems associated with such energy conversion processes
involving bubble columns. In order to achieve economically high space-time yields, a
high slurry concentration (typically 30 50 % vol) needs to be employed. To suspend
such a large amount of catalyst, a high energy input is needed, which can be provided by
high superficial gas velocities. The process operates under high-pressure conditions
(typically 10 80 bar). The high exothermic heat of reaction requires an efficient means
of heat removal that can operate in the churn-turbulent flow regime. Finally, the large gas
throughputs necessitate the use of large diameter reactors (typically 5 8 m), and to
obtain high conversion levels, large reactor heights, typically 20 30 m tall, are required.
Successful commercialization of bubble column reactors is crucially dependent on proper
understanding of their hydrodynamics and scale-up principles.
1-1 Motivation
Although bubble column reactors are simple in construction, proper design and scale-up
of such reactors require a thorough understanding of the prevailing hydrodynamic and
mixing characteristics at conditions similar to the targeted process. The hydrodynamics of
such reactors affect the mixing intensity and gas-liquid interfacial area, which affect the
transport coefficients, and hence the conversion and selectivity of the reactor.
Hydrodynamic behavior in a bubble column reactor is complex, since the fluid phases
involved are characterized by very different masses, and one is more compressible than
9
the other. Various design parameters (e.g., reactor geometry, internals, sparger design,
etc.) and operating variables (e.g., reactor pressure and temperature, gas and liquid/slurry
flow rates, catalyst size and loading, etc.) along with phase properties and kinetics, affect
the reactor hydrodynamic and transport rates in bubble/slurry bubble column reactors.
These, in turn, impact the reactor performance, operation, and its design and scale-up.
However, due to the complex interaction among the various phases, the flow field and
hydrodynamics of these reactors have not yet been well understood. In slurry bubble
column reactors, the ability to achieve complete catalyst suspension and the desired flow
pattern of the liquid/solid phase is critical to the targeted reactor performance.
Accordingly, in order to accomplish the desired flow pattern, an improved understanding
and quantification of the key hydrodynamic phenomena are required.
As mentioned earlier, industrial processes such as FT synthesis and liquid phase
methanol synthesis need to be carried out at high superficial gas velocity, high pressure,
high temperature, high catalyst loading, and in large diameter reactors. The literature
studies performed under such conditions are limited to global parameters such as overall
gas holdup and overall mass transfer coefficient (Wilkinson, 1991, Letzel, 1997).
Detailed studies of hydrodynamic parameters, such as phase holdup distribution and
velocity and turbulent parameter profiles, have been performed at high superficial gas
velocity and pressure only in air-water (Ong, 2003) and air-water-glass beads systems
(Rados, 2003) via advanced diagnostic techniques such as CT and CARPT. They found
that the effect of the sparger on hydrodynamics at high superficial gas velocities is
relatively insignificant. The pressure tends to increase the gas holdup and flatten gas
holdup radial profile. It was observed that an increase in pressure increases liquid
recirculation and reduces turbulent kinetic energy. In the literature, no work has been
reported regarding detailed hydrodynamic studies of slurry bubble columns at the
conditions of industrial interest. Such studies can be performed either by using a real
system or by mimicking the system of interest at laboratory operating conditions.
Therefore, the lack of hydrodynamic studies at the conditions of industrial interest
motivates the present work, which seeks to fill this gap by investigating the
hydrodynamics of a slurry bubble column using a liquid phase that at room temperature
10
mimics the FT synthetic wax at low temperature FT reaction conditions. In addition, such
work will be useful in gaining insight into the effect of physical properties on the flow
dynamics by comparing the findings with those obtained using air-water-glass beads
(Rados, 2003). The work will further extend the benchmark data for evaluation and
validation of Computational Fluid Dynamics (CFD) models and closures predictions.
The demarcation of the flow regime in bubble columns is an important task because
different hydrodynamic characteristics exist in different flow regimes, and result in
different mixing and heat and mass transfer. It is very possible that the laboratory column
may operate in a heterogeneous regime, while industrial columns, due to their high
operating pressure and temperature and large diameters, may operate in a homogeneous
regime under similar conditions. The current state of empirical correlations, semianalytical models, and analytical models to predict transition in bubble columns is not yet
complete (Shaikh and Al-Dahhan, 2007a). The experimental techniques used to measure
flow regime transition are either visual or probe based. Apart from being intrusive,
probing techniques provide only point information or hydrodynamic information at the
wall. In large diameter industrial scale columns, such hydrodynamic information
transmitted from large distances can be questionable. Also, the implementation of a
probing technique for flow regime transition requires modification of existing reactors
and/or shut-down of the operation. Therefore, this work attempts to develop and
demonstrate non-invasive techniques for flow regime transition identification and its
objective flow regime identifiers that can be implemented on industrial scale bubble
columns without disturbing the operation to pinpoint the flow regime at the reactor
operating conditions. Noninvasive techniques such as -ray CT and Nuclear Gauge
Densitometry (NGD) will be considered for this purpose. NGD is commercially available
and used widely in industries for liquid/slurry level monitoring and control. Hence, the
successful development and demonstration of these techniques can be utilized for online
flow regime monitoring in commercial as well as laboratory applications.
Extrapolating the behavior of laboratory scale columns to industrial scale columns is
always a difficult and challenging task. Because the dispersion and interfacial heat and
11
mass transfer fluxes, which often limit the chemical reaction rates (and in turn
conversion, selectivity, and yield), are closely related to hydrodynamics of the system
through the gas-liquid contact area and the turbulence properties of the flow, the scaleup
criteria need a reliable hydrodynamic similarity rule. The available scale up
methodologies for bubble columns depend on the similarity of overall gas holdup in the
two systems. It will be shown later that such an approach could be exclusively applicable
in bubbly flow, where gas holdup radial profiles are flat, but it cannot be extended to the
churn-turbulent regime, where parabolic profiles are present. Hence, the development of
a hydrodynamic similarity hypothesis in the regime of industrial interest motivates this
work to propose and evaluate a new methodology for scale up of bubble columns
operated in the churn-turbulent flow regime, with the aid of existing CT, CARPT, and
state-of-the-art modeling tool. An ideal choice of modeling tool for scaleup would be
CFD. However, due to the lack of universal closures, CFD has not yet been developed for
scaleup purposes. Hence, in this work, we have resorted to Artificial Neural Network
(ANN) correlations.
In summary, this work aims at advancing the state of knowledge of key hydrodynamic
parameters of bubble and slurry bubble column reactors at mimic industrial conditions. It
develops an experimental technique and flow regime identifiers for flow pattern
delineation that can be useful for online monitoring. Also, it proposes and demonstrates a
new scaleup methodology with the aid of state-of-the-art experimental and modeling
tools.
12
1-2 Objectives
The primary objective of the work is to improve the fundamental understanding of the
hydrodynamics of bubble/slurry bubble column reactors at industrially relevant
conditions. The specific goals of the work are as follows:
1-2.1 Hydrodynamic Parameters
Study the hydrodynamic characteristics of a slurry bubble column reactor using a

liquid, which, at room temperature, mimics FT wax at FT reaction conditions.
Investigate the effects of liquid phase physical properties and solids loading on the
phase distribution via a single source -ray CT.
Investigate the effects of liquid phase physical properties and solids loading on solids
axial velocity and turbulent parameters radial profile via CARPT.
1-2.2 Flow Regime Transition

This part of work includes the evaluation of single source -ray CT and NGD for
identification of regime transition. It comprises the following:
Evaluate CT for flow regime delineation and propose its flow regime identifiers.
Develop NGD for flow regime identification by analyzing obtained photon counts
history via various signal processing methods such as statistical analysis,
autocorrelation function analysis, and spectral analysis. The emphasis will be to study
the deviation of system behavior from a Poisson distribution and to develop flow
regime identifiers. This exercise will be useful for generalization of the proposed
flow regime identifiers. A successful development and demonstration should lead to
the implementation of Nuclear Gauge Densitometry (NGD) as a tool for online flow
13
regime identification in industrial scale bubble/slurry bubble column reactors in
particular and multiphase flow systems in general.
1-2.3 Scale-up and hydrodynamic similarity
Develop a scale-up methodology for bubble columns by proposing a hypothesis that

to be hydrodynamically similar, the two reactors should have the same overall gas
holdup and its radial profile or cross-sectional distribution. The development of the
scaleup methodology consists of two steps:
I. Experimental evaluation of the proposed hypothesis, using CT and CARPT.
II. Development of state-of-the-art correlations based on ANN for prediction of
the overall gas holdup, the radial profiles of the gas holdup and liquid axial
velocity, and the center-line liquid velocity using available database and
including the findings of this work. Development of such correlations will
facilitate implementation of the developed scaleup methodology by a priori
prediction of the needed hydrodynamic parameters.
1-3 Thesis Organization

A general review of mixing of liquid/solids phase, flow regime transition studies, and
available scaleup methodologies is provided in Chapter 2. The experimental studies
regarding flow behavior of slurry bubble column reactors are divided into two chapters
(Chapters 3 and 4). Chapter 3 provides the discussion on choice of fluid, experimental
setup, techniques used, and results related to the effect of operating parameters on phase
distribution. Chapter 4 discusses the effect of operating parameters on the solids axial
velocity and turbulent parameters at operating conditions similar to the studies in Chapter
3. The development of flow regime monitoring techniques and its flow regime identifiers
will be discussed in Chapter 5, while Chapter 6 presents the development of the new
scaleup methodology for hydrodynamic similarity and its experimental evaluation using
14
CT and CARPT. ANN correlations of the needed hydrodynamic parameters that can be
useful in implementing the developed scaleup methodology are presented in Appendix-F.
Chapter 7 provides the conclusions and recommendations, and outlines possible future
efforts.
15
Chapter 2.
Literature Review
In this chapter, a literature review pertinent to this thesis is presented. It is divided into
three parts as per the structure of thesis mentioned in Chapter 1. In the first part, mixing
of liquid/slurry phase is briefly reviewed. The second part reviews flow regime transition
studies in bubble column. The detailed review on this subject has been submitted for
publication [Shaikh and Al-Dahhan (2007a). A Review on Flow Regime Transition in
Bubble Columns. Accepted in International Journal of Chemical Reactor Engineering].
The third part deals with scaleup studies in bubble column reactors. The detailed review
on this part [Shaikh and Al-Dahhan. (2007b) Scaleup of Bubble Column Reactors: A
Review of Current State of the Art] is being prepared and will be submitted for
publication.
2.1 Mixing and velocity profiles of liquid/slurry phase
Mixing and velocity profiles in two- and three-phase bubble columns have been reviewed
in detail by Ong (2003) and Rados (2003). In addition, Joshi et al. (1998) and Wild et al.
(2004) discussed mixing and velocity profiles in bubble columns in great detail, and
hence, these will not be repeated here.
Several studies have examined the hydrodynamics of bubble column reactors (Franz,
1984; Devanathan 1991; Yao, 1991; Degaleesan, 1997). These studies have been
performed at atmospheric pressure and/or at superficial gas velocities up to 15 cm/s.
Though high pressure operations are preferred operating conditions, very little is known
about the flow structure of bubble and slurry bubble columns at high pressure.
Information available at high pressure is limited mainly to global parameters such as
overall gas holdup, and overall mass transfer coefficient. There have been few efforts to
study mixing in bubble columns at high pressure.
16
Yang and Fan (2003) measured the axial dispersion coefficient in bubble columns using
the thermal dispersion technique at operating pressures up to 10.3 MPa and superficial
gas velocities upto 40 cm/s. The axial dispersion coefficient increases with an increase in
superficial gas velocity and decreases with an increase in pressure. Axial dispersion was
found to increase with liquid velocity due to enhanced liquid phase turbulence. The
scaleup effect on liquid mixing reduces as the operating pressure increases. Wei et al.
(2003) investigated local bubble behavior using an optical fiber probe in different column
diameters (20, 40, and 80 cm). They confirmed the presence of a coherent gross
circulation structure spanning the entire column diameter in the larger column rather than
a pair of symmetrical circulation cells.
Cui and Fan (2004) applied Laser Doppler Velocimetry (LDV) and Particle Image
Velocimetry (PIV) techniques to measure turbulent properties in two- and three-phase
bubble columns and fluidized beds. They have performed experiments up to 7.5 cm/s of
superficial gas velocity. Bubble induced turbulence was found to be dominant in
turbulence generation under the studied operating conditions. They found that the effect
of solids on the turbulence in the liquid phase is complex and depends upon the solids
properties and superficial gas velocity. They proposed a criterion based on, local gas
velocity/minimum fluidization velocity, to account for the effect of solid particles on
turbulence in the liquid phase in three-phase fluidized beds.
Pohorecki et al. (2001) performed experimental studies in a nitrogen-cyclohexane system
to investigate the hydrodynamics in a pilot plant bubble column at high pressure (up to
1.1 MPa) and high temperature (up to 1600 C). They found that the current state of
prediction of hydrodynamics gives highly divergent results when applied to conditions of
industrial interest.
The only studies that have investigated detailed hydrodynamics at high superficial gas
velocity and operating pressure, in terms of instantaneous and time averaged velocity,
turbulent parameters profiles, and time averaged phase holdup distributions have been
performed by Ong (2003) and Rados (2003). They utilized advanced diagnostic
17
techniques such as CARPT and CT to study the effect of superficial gas velocity,
operating pressure, and sparger design on the bubble column hydrodynamics using airwater and air-water-150 m glass beads. In general, some of their significant findings are:
i)
At atmospheric pressure, the effect of distributor was observed even at

superficial gas velocity of 14 cm/s, although the flow is generally be
considered in churn-turbulent flow at this gas velocity.
ii)
Gas holdup in churn-turbulent flow increases with an increase in pressure and

radial profile of gas holdup becomes flatter with an increase in pressure.
iii)
The strength of axial liquid recirculation increases with both increase in

superficial gas velocity and pressure which is directly related to gas holdup
and its radial profile which increases with these parameters.
iv)
At ambient pressure, the liquid recirculation was independent of type of

distributor at Ug = 30 cm/s. However, differences were observed in turbulent
quantities with cross-sparger exhibiting higher turbulent kinetic energy
compared perforated plate distributors.
v)
At P = 0.4 MPa, the effect of distributor on liquid recirculation was found to

be insignificant.
vi)
While liquid recirulcation increases with an increase in pressure, turbulent

kinetic energy and eddy diffusivities were found to decrease.
vii)
The contribution of bubble induced turbulence to eddy viscosity was found to

be less than 10 %.
viii)
An addition of solids, in general, tends to decrease gas holdup. However, an

addition of solids from 0 to 9.1 % vol. does not appear to have significant
effect on gas holdup and liquid axial velocity profile.
There is little known about the turbulent characteristics in three phase systems. Except for
Rados (2003) and Cui and Fan (2004), no studies have investigated the turbulent
characteristics of three dynamic phase flow. Cui and Fan (2004) performed their studies
in a two dimensional bubble column and at low superficial gas velocities up to 7.5 cm/s.
Although Rados (2003) has studied the turbulent behavior of slurry bubble columns at
18
high superficial gas velocity and high pressure, his studies are limited only to water as the
liquid phase. Hence, it is necessary to study the effect of physical properties on the
detailed flow behavior in such systems as the industrial systems consists of liquid phases
that has properties vastly different than water. It is important to know whether using the
liquid other than water will affect the trend and/or the magnitude of flow behavior.
In addition, Rados (2003) studies were conducted at relatively low solids loading (9.1 %
vol.) and have not investigated the effect of solids loading on hydrodynamic
characteristics of slurry bubble columns. The effect of solids loading is of particular
interest because the flow behavior of solids that are used as catalyst in industrial
processes will have significant effect on the performance of slurry bubble column
reactors. Such investigations will be extremely useful in determining the optimum
amount of catalyst for maximum reactor performance. Hence the brief review shows that,
there is a need to study the effect of physical properties and solids loading on
hydrodynamic characteristics of bubble/slurry bubble column reactors.
Also, as shown by Pohorecki et al. (2001) hydrodynamics at conditions of industrial
interest may show different behavior than at laboratory conditions. Therefore, one needs
to know in detail the fluid dynamics and mixing characteristics at the conditions of
industrial interest. This can be achieved either by performing experiments at the
industrial conditions using the real system or by mimicking the industrial system at
laboratory operating conditions. With the limitations encountered in laboratory studies,
the later option is more attractive. Such an option needs to be utilized to study the
hydrodynamic behavior of bubble column reactors.
2.2 Flow Regime Transition

Due to varied flow behavior, the demarcation of hydrodynamic flow regimes is an
important task in the design and scaleup of bubble column reactors. This section reviews
the studies performed for flow regime identification in bubble columns. The detailed
review article dealing with flow regime transition studies in bubble column has been
accepted for publication [Shaikh and Al-Dahhan (2007a). A Review on Flow Regime
19
Transition in Bubble Columns. accepted International Journal of Chemical Reactor
Engineering]. Hence, it is briefly reviewed in the following sections.
2.2.1 Flow Regime Types and Characteristics

In bubble columns, four types of flow patterns have been observed, viz., homogeneous
(bubbly), heterogeneous (churn-turbulent), slug, and annular flow. Researchers have
reported the occurrence of a slug flow regime only in small diameter columns. In these
different flow regimes, the interaction of the dispersed gas phase with the continuous
liquid phase varies considerably. Figure 2-1 shows the various flow regimes in bubble
columns. However, bubbly and churn-turbulent flow regimes are most frequently
encountered. Depending upon the operating conditions, these two regimes can be
separated by a transition regime.
The homogeneous flow regime generally occurs at low to moderate superficial gas
velocities. It is characterized by uniformly sized small bubbles traveling vertically with
minor transverse and axial oscillations. There is practically no coalescence and break-up,
hence there is a narrow bubble size distribution. The gas holdup distribution is radially
uniform; therefore bulk liquid circulation is insignificant. The size of the bubbles depends
mainly on the nature of the gas distribution and the physical properties of the liquid.
Heterogeneous flow occurs at high gas superficial velocities. Due to intense coalescence
and break-up, small as well large bubbles appear in this regime, leading to wide bubble
size distribution. The large bubbles churn through the liquid, and thus, it is called as
churn-turbulent flow. The non-uniform gas holdup distribution across the radial direction
causes bulk liquid circulation in this flow regime.
20
Figure 2-1: Various flow regimes in bubble column reactors

As one can see, homogeneous and heterogeneous flow regimes have entirely different
hydrodynamic characteristics. Such different hydrodynamic characteristics result in
different mixing as well as heat and mass transfer rates in these flow regimes. Therefore,
the demarcation of flow regimes becomes an important task in the design and scale up of
such reactors and has led to considerable research efforts which have resulted into
various experimental methods and empirical, semi-empirical, and mechanistic models to
identify flow regime transition.
The flow regime transition from bubbly to churn-turbulent flow or from churn-turbulent
to slug flow depends simultaneously on parameters such as superficial gas velocity,
column diameter, liquid and gas phase properties, and distributor design (Urseanu, 2000).
No flow regime map is available that covers a wide range of industrial conditions. Figure
2-2a shows one of the few approximate flow regime maps of transition velocity versus
column diameter that distinguishes among bubbly, transition, churn-turbulent, and slug
flow (Shah et al., 1982). However, it is limited to low viscosity systems at ambient
conditions. Figure 2-2b shows another flow regime map of superficial gas velocity versus
superficial liquid velocity which distinguishes discrete bubble, dispersed bubble, slug,
churn, bridging, and annular flow (Zhang et al., 1997). This map was proposed based on
data collected using air-water system at ambient conditions in a small diameter column
(0.0826 m).
21
(a)
(b)
Figure 2-2: Flow regime map for air-water system at ambient pressure a) Shah et al.,
1982 and b) Zhang et al., 1997.
2.2.2 Methods for Flow Regime Identification

The experimental methods used for regime transition identification can be broadly
classified in the following groups:
Visual observation
Evolution of global hydrodynamic parameter
Temporal signatures of quantity related to hydrodynamics
Advanced measurement techniques
22
Visual Observation
Visual observation is the simplest method to study the flow pattern in bubble columns.
The slow, vertically rising bubbles can be observed in the homogeneous regime.
However, in the heterogeneous regime there is an intense interaction of bubbles, leading
to gross circulation (Figure 2-3). It is difficult to pinpoint the exact transition velocity by
visual observation. Moreover, this method can be useful only when the column is
transparent.
Figure 2-3: Photographs of bubbly and churn-turbulent flow in 2-D column
Evolution of global hydrodynamic parameter

Because the global hydrodynamic parameters are manifestations of the prevailing flow
patterns, they vary with the regimes. This fact has generally been utilized to identify flow
regime transition point. Typically, the global hydrodynamics have been quantified based
on overall gas holdup. The relationship between overall gas holdup and superficial gas
velocity can be expressed as
G U Gn .
(2-1)
The overall gas holdup increases with an increase in superficial gas velocity. As can be
seen in Figure 2-4a (Shaikh and Al-Dahhan, 2005), the relationship between overall gas
holdup and superficial gas velocity varies over a range of velocities. The relationship is
almost linear (n ~ 0.8-1) at low gas velocities, but with an intense non-linear interaction
of bubbles at high gas velocities, the relationship between overall gas holdup and
superficial gas velocity deviates from linearity. The value of n is less than 1 (n ~ 0.4
0.6). Hence, the change in slope of the gas holdup curve can be identified as a regime
23
transition point. Sometimes, gas holdup shows an S-shaped curve, depending upon
operating and design conditions (Figure2-4b) [Rados, 2003]. In such cases, the superficial
gas velocity at which maximum gas holdup has been attained is identified as the
transition velocity.
0.5
Cross-sectional gas holdup
0.4
0.3
0.2
0.1
10
20
30
Superficial gas velocity (cm/s)
(a)
(b)
Figure 2-4: Typical overall gas holdup curve a) Shaikh and Al-Dahhan, 2005; and b)
Rados, 2003.
However, when the change in slope is gradual or the gas holdup curve does not show a
maximum in gas holdup, it is difficult to identify the transition point. In such cases, the
drift flux method proposed by Wallis (1969) has been used extensively.
In this method, the drift flux, jGL (the volumetric flux of either phase relative to a surface
moving at the volumetric average velocity) is plotted against the superficial gas velocity,
UG. The drift flux velocity is given by:
jGL = U G (1 G ) U L G ,
(2-2)
where G is gas holdup and UL is superficial liquid velocity. The positive or negative sign
indicates counter-current or co-current flow of liquid relative to the gas phase,
respectively. Figure 2-5 shows a typical plot of the drift flux versus gas holdup. The
change in the slope of the curve represents the transition from homogeneous to
24
heterogeneous flow. The change in slope of the drift flux plot is generally sharper than
the change in slope of gas holdup curve.
Figure 2-5: Typical drift flux plot using Wallis (1969) apporach (Deckwer et al., 1981)
Temporal signatures of quantity related to hydrodynamics

The global parameters represent macroscopic phenomena that are result of prevailing
microscopic phenomena. Several attempts have been made to capture the instantaneous
flow behavior through an energetic parameter.
The following temporal signatures have been utilized for flow regime transition:
-
Pressure fluctuations [Nishikawa, 1969; Matsui, 1984; Drahos et al., 1991; Letzel
et al., 1997; Vial et al., 2001, Park and Kim, 2003]
Local holdup fluctuations using resistive or optical probes [Bakshi et al., 1995;
Briens et al., 1997]
Temperature fluctuations using a heat transfer probe [Thimmapuram et al., 1991]
Local bubble frequency measured using an optical transmittance probe [Kikuchi

et al., 1997]
Conductivity probe [Zhang et al., 1997]
Sound fluctuations using an acoustic probe [Holler et al., 2003; Al-Masry, 2004]
25
Various time-series analyses have been used to interpret the fluctuations of these
parameters and to identify flow regimes and their transition. The commonly used timeseries analyses are statistical analysis, autocorrelation analysis, stochastic modeling,
spectral analysis, chaos analysis, and wavelet analysis.
Amongst these techniques, pressure fluctuations are supposed to be an attractive option.
However, the relationship between pressure and flow structure is not straightforward.
Although in gas-solid flows pressure fluctuations are mainly due to bubbles, in gas-liquid
flows more complex phenomena exist as shown by Drahos et al. (1991) and Letzel et al.
(1997). Hence, these fluctuations need careful analysis when applying novel time-series
techniques to interpret the data.
Advanced measurement techniques

With advances in measurement techniques, various imaging and velocimetric techniques
have been used in flow regime transition studies.
-
Particle Image Velocimetry (PIV) [Chen et al., 1994; Lin et al., 1996]
Electrical Capacitance Tomography (ECT) [Bennett et al., 1999]
Electrical Resistance Tomography (ERT) [Dong et al., 2001; Murugaian et al.,

2005]
Laser Doppler Anemometry (LDA) [Olmos et al., 2003]
Computer Automated Radioactive Particle Tracking (CARPT) [Cassanello et al.,

2001; Nedeltchev et al., 2003]
Although the implementation of advanced measurement techniques is relatively difficult,

they provide detailed flow information and are useful in understanding prevailing
phenomena.
Table summarizing most of the flow regime transition studies along with operating and
design conditions and significant remarks is provided in Shaikh and Al-Dahhan (2007a).
26
The details of few important studies as well as the effects of operating and design
parameters can be found in Shaikh and Al-Dahhan (2007a).
2.2.3 Prediction of Flow Regime Transition

The objectives of the experimental studies, apart from achieving a fundamental
understanding of the prevailing phenomena, are to evaluate theoretical criteria. To design
bubble column reactors, one needs to know a priori the prevailing flow regime at the
design and operating conditions. Predictions of flow regime transition have been
achieved by the development of various models and approaches that include pure
empirical correlations, semi- empirical and phenomenological (or mechanistic) models,
linear stability theory, and Computational Fluid Dynamics (CFD). The brief discussion
on this topic can be found in Shaikh and Al-Dahhan (2007a).
2.2.4 Remarks
The methods to determine regime transition have progressed from visual observation, to
the measurement of time-averaged global hydrodynamic parameters, to more quantitative
analysis based on examination of temporal signatures related to hydrodynamics. Various
linear and non-linear time-series techniques have been applied to the temporal signatures.
The simpler techniques, such as statistical analysis, spectral analysis, do identify the flow
regime transition point. Advanced non-linear techniques such as chaos analysis,
stochastic modeling, and multiresolution analyses provide tools to extract additional
features of the flow, apart from regime transition. However, these techniques can be
computationally intensive. Hence, the choice of time-series techniques appears to be a
compromise between what and how fast the information is needed. In this regard, the
comments made by Drahos (2003) need consideration.
Shaikh and Al-Dahhan (2007a) showed that empirical correlations exhibit large
discrepancies in their predictions at the same operating and design conditions. All of
these studies calculated transition velocities from the gas holdup curve, however, the
method of treatment to predict transition point from gas holdup curve differs in each case.
27
The prediction of transition using stability theory and CFD still needs substantial
improvement.
Energy conversion processes such as Fischer-Tropsch synthesis and methanol synthesis
operate in large diameter columns at high temperature, pressure, and solids loading.
Increased diameter, pressure, temperature (and thereby reduced viscosity) increases the
transition velocity, while solids loading reduces the transition velocity. Therefore,
experiments performed in lab scale columns and operating conditions (i.e., using airwater system or conditions of no interest to industry) may be very much in the
heterogeneous regime, but quite possibly that in the homogeneous regime in industrial
columns. The state-of-the-art of empirical correlation, stability theory and CFD is not yet
sophisticated enough to a priori predict transition velocities in real systems. Hence, the
only option remains is to measure the transition velocity using a reliable experimental
technique. As discussed above, the available experimental techniques are based on either
visual observation or are probe based. Visual observation is often not possible due to the
opaque nature of the flows in bubble columns while probe based techniques are intrusive
and can provide unreliable hydrodynamic information in large diameter industrial scale
columns. By using probes flush to the wall, some researchers claim the probing
techniques to be non-invasive. However, in large diameter columns, one can not be sure
that fluctuations transmitted over great distances up to the wall can represent the
underlying hydrodynamics with fidelity. In addition, the probe-based techniques provide
point information that may not necessarily describe hydrodynamic information across
that cross-section. Also, Ellis et al. (2004) have shown that the probe dimensions can
influence the obtained hydrodynamic information and subsequently its interpretation. To
diagnose the flow in an industrial reactor which is in operation, probing techniques
require modification in the reactor and also shut-down of the operation to implement it,
which is not economical. Therefore, there is a need to develop a technique that is
noninvasive, can be easily implemented on an industrial scale without disturbing the
operation, and can provide hydrodynamic information that is reliable in lab scale and
industrial scale reactors.
28
2.3 Scaleup of Bubble Column Reactors
The following is a brief review of the current state of the scale up of bubble column
reactors reported in literature. The detailed review regarding this topic [Shaikh and AlDahhan. (2007b) Scaleup of Bubble Column Reactors: A Review of Current State of the
Art] will be submitted for publication and hence is briefly reviewed here.
2.3.1 Reported status of scaleup in literature
Wilkinson et al. (1992)

Wilkinson et al. (1992) performed experiments for scaleup purposes in two different
column diameters (15 and 23 cm) at operating pressures varying between 0.1 to 2 MPa
using three different liquids. Based on these experimental observations, they proposed
criteria for scaleup of high pressure bubble column reactors. It was argued that, the gas
holdup is virtually independent of the column dimensions and the sparger layout (for low
as well as high pressures) provided following criteria are fulfilled:
1) The column diameter has to be larger than 15 cm.
2) The column height to diameter ratio has to be in excess of 5.
3) The hole diameter of the sparger has to be larger than 1-2 mm.A correlation was
proposed based on their own and literature data that accounts the effect of gas density
and incorporates the flow regime transition.
A correlation was proposed for overall gas holdup based on their own and literature data
that accounts the effect of gas density and incorporates the flow regime transition.
Wilkinson et al. (1991) recommended using this correlation for scaleup purposes.
29
Degaleesan (1997)
Degaleesan (1997) proposed a scaleup method that was based on the assumption that any
gas-liquid/slurry would exhibit the similar hydrodynamic behavior as air-water system if
both the systems have the same overall gas holdup. The procedure involves measuring (or
evaluating based on the suitable correlation) the overall gas holdup in scaled up unit at its
operating conditions and then calculating the equivalent superficial gas velocity, uGe that
results in the same overall gas holdup in an atmospheric air-water system as in the scaled
up unit. Hence, it was suggested that hydrodynamics and mixing at the equivalent
superficial gas velocity, uGe in an atmospheric air-water system would represent the
hydrodynamics and mixing in scaled up unit. The value of uGe can then be used to predict
recirculation velocity and other turbulent parameters using correlations proposed based
on CARPT data in an air-water system. The liquid velocity profile has been estimated
using a 1-D model (Kumar, 1994), with a known mean recirculation velocity and gas
holdup radial profile.
Degaleesan (1997) developed a two-dimensional convection-diffusion model for liquid
mixing to interpret the tracer response in 18-inch diameter slurry bubble column reactor
for liquid phase methanol synthesis at La Porte, Texas. The convection-diffusion model
needs knowledge of liquid axial velocity profile, eddy diffusivities profile, and gas
holdup profile to predict the tracer responses. The available fluid dynamic measurements
in industrial unit were gas holdup radial profile measured using Nuclear Gauge
Densitometry (NGD). The liquid axial velocity profile and eddy diffusivities profile were
not available in industrial scale unit at reaction conditions. The experimental
measurements of these fluid dynamic parameters were available only in laboratory scale
bubble column (diameter = 14, 19, 44 cm) at ambient conditions in air-water system.
Degaleesan (1997) developed scaling rules to extrapolate available laboratory scale data
to industrial unit, to predict the needed fluid dynamic parameters,
It provides a systematic approach to characterize recirculation and mixing in an industrial
scale bubble column using an atmospheric air-water data. However, similarity based on
30
only overall gas holdup may not be sufficient. This method needs a priori knowledge of
gas holdup and its distribution.
Inga and Morsi (1998)

Inga and Morsi (1998) have demonstrated their scaleup/scaledown methodology for FT
synthesis where it was shown that how the experimental results obtained in laboratory
scale stirred tank reactor could be extrapolated to design industrial scale slurry bubble
column. It is based on similarity of the relative importance of mass transfer resistance in
the overall reaction resistances, defined in terms of a dimensionless parameter, i which
represents the balance between kLa (mass transfer coefficient) and k0 (rate of
consumption, pseudo kinetic constant for first order). Accordingly, maintaining the same
in two reactors will result in the same reactant concentration and catalyst activity and
thereby the conversion and selectivity in two reactors.
Inga and Morsi (1998) demonstrated their proposed method for FT synthesis using a
laboratory scale 4-litre stirred tank reactor operating at 20 Hz and 5 % wt which was
simulated to a conceptual industrial scale slurry bubble column reactor. The conceptual
slurry bubble column reactor with 7 m diameter and 30 m height operating at 30 bars,
523 K and 20 cm/s was modeled using Axial Dispersion Model (ADM). The simulations
were performed to maintain similar i as in stirred tank reactor. The authors found the
same productivity in both the reactors when the values of i were the same.
The method proposed by these authors shows that, maintaining relative contribution of
transport parameter the same in two systems results into the same performance even if
one system is impeller-agitated (CSTR) and the other one is gas-agitated (slurry bubble
column). Although Inga and Morsi (1998) procedure combines transport and reaction
kinetics, the use of overall mass transfer coefficient is not enough to describe the mixing
as it represents global transport parameter. The authors described phase mixing using
ADM that needs reliable prediction of axial dispersion coefficient in both gas and slurry
phase.
31
Fan et al. (1999)
Fan et al. (1999) proposed a criterion for hydrodynamic similarity in bubble and slurry
bubble columns based on the overall gas holdup. Using the vast range of data collected
from literature and their own data, an empirical correlation was proposed to estimate the
gas holdup in terms of three dimensionless numbers,
uG4 G G
) ( )
G
Lg
L
=
0.054 0.41
(1 G ) [cosh( MoSL )]
2.9(
(2-3)
where,
0.0079
0.011
= 0.21MoSL
; = 0.096 MoSL
MoSL =
g ( SL G )( L ) 4
2
SL
L3
ln( ) = 4.6CV {5.7CV0.58 sinh[0.71exp(5.8CV ) ln Mo 0.22 ] + 1}

It was argued that maintaining these numbers the same in two systems would lead to
similar overall gas holdup and hence mixing and hydrodynamics. However, this proposed
similarity rule has not been evaluated experimentally. The suggested dimensionless
numbers does not account the effect of column diameter on gas holdup. The reason for
not accounting column diameter lies in the reported studies which found that, above 15
cm, column diameter has negligible effect on overall gas holdup. However, such studies
were performed mostly but not exclusively in air-water system. Recently, van Baten and
Krishna (2004) reported that, in concentrated slurries such an observation does not quiet
hold. Additionally, similarity criteria based only on overall gas holdup may not be
sufficient in churn-turbulent flow regime.
32
Safonuik et al. (1999) and Macchi et al. (2001)
Safonuik et al. (1999) presented a scale-up method for three phase fluidized beds with the
aid of the Buckingham pi theorem, which yielded five dimensionless numbers that have a
profound effect on overall gas holdup. These dimensionless groups are Morton number,
Mo; Etovos number, Eo; Reynolds number, Re; Density ratio; Superficial gas and liquid
velocity ratio.The methodology was evaluated by maintaining these dimensionless groups
the same in 0.91 m (hydrogen-kerosene-ceramic particles) and 0.0826 m (air-magnesium
sulphate solution-cylindrical alumina particles) diameter columns. Whenever the
dimensionless numbers were close in these systems, the dimensionless hydrodynamic
parameter, viz., overall gas holdup was found to be close to each other.
Later, Macchi et al. (2001) have tested the scaling approach of Safounik et al. (1999) in
three phase fluidized beds where the liquid phase was an aqueous solution of glycerol (a
liquid mixture) in one column and silicone oil (a pure liquid) in the other. The
experiments were performed in an acrylic column of 0.127 m diameter and 2.58 m long.
It was observed that, whenever five dimensionless numbers were the same in these
systems, the overall gas holdups were within 11 % of root mean standard deviations.
Hence, it provided a reasonable basis for hydrodynamic similarity in two systems.
However, the pressure fluctuations studies revealed that the power spectra in the two
systems are different. Macchi et al. (2001) concluded that, the mismatch is likely due to
the difference between coalescence in monocomponent and multicomponent liquid that
results into different bubble distribution. Hence, they suggested that more than five
dimensionless groups are needed to fully characterize the system.
Krishna et al. (2001)
Krishna et al. (2001) developed a strategy for scaling laboratory reactors to commercial
ones based on the fundamental understanding of hydrodynamics. The developed
understanding in terms of correlations of various hydrodynamic parameters was
33
incorporated into Computational Fluid Dynamics (CFD) to design commercial size
bubble column reactor.
Based on Dynamic Gas Disengagement (DGD) experiments in different systems and
different column diameters, they proposed correlations to predict bubble diameter, rise
velocity, and small and large bubble holdups. These models have been incorporated into
a fundamental model based on CFD in an Eulerian framework. The overall gas holdup
and velocity profiles predicted from CFD were compared to experimental values for three
different column diameters and found to be in a good agreement. Based on this
confirmation, they studied hydrodynamics in a 6 m diameter bubble column using CFD.
However, no comparison of CFD predictions with experimental data was shown at these
conditions.
The correlations for prediction of bubble diameter, rise velocity, and holdups were
developed based on Dynamic Gas Disengagement (DGD) studies. These reported studies
suggest that, the small bubble holdup remains constant in heterogeneous flow regime.
However, Jordan et al. (2003) performed DGD experiments at atmospheric as well as
high pressure and analyzed the obtained results using independent disengagement,
sequential disengagement, and constant slip velocity assumptions. In contradiction to
previous findings, they observed that, the small bubble holdup increases with an increase
in superficial gas velocity. In addition, Xue (2004) studied bubble dynamics in air-water
system at atmospheric and high pressure using newly developed four point optical probe
and found that small bubble holdup increases with an increase in superficial gas velocity.
In addition, Lee et al. (1999) studied the assumptions of DGD technique in twodimensional bubble column and slurry bubble column with the help of Particle Image
Velocimetry (PIV). They found that the assumptions in DGD that there is no bubblebubble coalescence and breakup during disengagement and disengagement of bubble
classes are not affected by each other are not valid particularly in heterogeneous regime.
However, such limitations shown by Lee et al. (1999) have to be checked in threedimensional bubble column.
34
van Baten et al. (2003)
van Baten et al. (2003) proposed a new method for scale up of bubble columns where
they have demonstrated how the hydrodynamic behavior in 1 m. diameter column can be
estimated using the experimental data in 5.1 cm diameter column. They developed a
procedure to study the flow behavior in commercial scale bubble columns based on CFD
in Eulerian framework by considering only momentum exchange term. A method was
devised to replace the need for closure equation that may mar the predictions of CFD.
The drag coefficient and bubble diameter were calculated utilizing only overall gas
holdup data in small diameter column (5.1 cm).
van Baten et al. (2003) developed a CFD model in Eulerian framework for three phase
system (16.4 % wt. solids loading) assuming pseudo-homogeneity. Based on the work of
Sanyal et al. (1999) and Sokolichin and Eigenberger (1999), the added mass and lift force
terms were neglected. The momentum exchange term was written following the work of
Pan et al. (1999) as,
M L ,G = [
3 CD
L ] G L (u G u L ) u G u L
4 db
(2-4)
For a bubble swarm rising in a gravitational field, drag force balances the difference
between weight and buoyancy so that the bracketed term in equation 2-4 can be
substituted as,
3 CD
1
L = ( L G )g 2
4 db
Vb, 0
(2-5)
where, Vb,0 is the rise velocity of bubble swarms at low superficial gas velocities.
Equation 2-5 clearly shows that, the knowledge of the bubble rise velocity in infinite
volume of liquid is the only unknown parameter in the model. The authors proposed a
following method to calculate bubble rise velocity
35
i)
Perform overall gas holdup experiments in small diameter column (5.1 cm, in
current case).
ii)
Calculate average bubble swarm velocity, Vb as

Vb = uG / G
iii)
..(2-6)
Plot average bubble swarm velocity, Vb versus superficial gas velocity (Figure 26).
iv)
Extrapolate Vb data to low superficial gas velocity as shown in Figure 2-6.
v)
The value of bubble swarm velocity at vanishingly small superficial gas velocity
is Vb,0. Substitute this value in equation 2-5.
This way, one does not need to know the bubble size in the momentum exchange term to
predict drag coefficient. The overall gas holdups predicted from CFD along with the
developed approach was compared to the one obtained from experiments and were found
to be in a good agreement. Based on this comparison, van Baten et al. (2003) estimated
the behavior of 1 m diameter bubble column.
The authors proposed an elegant approach and it appears to be promising and robust to
study and design the flow behavior in large diameter bubble columns, as it does not
require a priori knowledge of bubble diameter and also it does not need drag force
coefficient closure. The only knowledge needed is simple overall gas holdup
Figure 2-6: Average bubble-swarm velocity in air-ethanol-Co (van Baten et al., 2003)
36
experimental data in laboratory scale column. However, the validation of CFD simulation
results with experiments in large diameter columns need to be established. This method
can be applicable in cases where the bubble size does not increase significantly with
superficial gas velocity. Vermeer and Krishna (1981) showed that, ratio of kLa / G is
constant (~ 0.5) in churn-turbulent flow regime in air-Turpentine 5 system. Godbole et al.
(1984) reached the similar conclusions in air-water and air-Soltrol -130 systems. Vandu
and Krishna (2004) also found the similar results in three different diameter columns (10,
15, and 38 cm) using air-water system and concluded that the constant value of ratio of
kLa / G is due to the fact that the effective bubble diameter is independent of superficial
gas velocity. Based on these findings, van Baten and Krishna (2004) rationalized the
application of the developed approach for scaleup of bubble columns. Recently, Chaumat
et al. (2005) developed a gas tracer technique to study Residence Time Distribution
(RTD) and mass transfer in 0.2 m diameter and 1.6 m long bubble column. Various gases
(nitrogen, carbon dioxide) and liquids (water, cyclohexane) were used at ambient
pressure. However, they concluded that, the relation between mass transfer and
hydrodynamics appears to be more complex than simplified linear relation. In the light of
conflicting results, such an approach may need to be revisited.
Zhang and Zhao (2006)
Recently, Zhang and Zhao (2006) proposed a scale up strategy for low temperature
methanol synthesis in a continuous slurry bubble column reactor. It involved studying
hydrodynamics in cold flow units, catalyst performance evaluation in an autoclave, and
process investigation in pilot-scale continuous slurry bubble column reactor.Overall the
study was performed in following three steps,
1) Hydrodynamics in a cold flow unit with different column structure using the
different three-phase systems
2) Catalyst preparation and performance evaluation in an autoclave
3) Process exploration in continuous slurry bubble column reactor with a capacity of
2 tons per year.
37
The authors provided a comprehensive roadmap for development of the low-temperature
methanol synthesis in circulating slurry bubble column reactor. The strategy tied flow
behavior and catalysis studies with that of process engineering. However, neither any
guidelines were provided regarding hydrodynamic similarity in cold and hot unit nor any
results with successful scaleup were shown.
2.3.2 Reported status of scaleup in industry
The status of scaleup of bubble column reactors in industry is not widely reported in
literature. Tarmy and Coulaloglou (1992) discussed fundamental development and
scaleup issues and related them through example of coal liquefaction process and
mentioned that understanding of hydrodynamics and related issues to be the most critical
element in development and scaleup of these reactors. The industrial example of scaleup
demonstrated by them involves hydrodynamic studies based on overall phase holdups
and liquid backmixing in terms of Peclet number measured using pressure transducers
and radioactive tracers, respectively. The highest superficial gas velocity in the pilot
reactor at process conditions was 8 cm/s. Based on Tarmy et al. (1984) studies; this
condition appears to be in bubbly flow.
Espinoza et al. (1999) discussed gas holdup prediction and scaleup for Sasol slurry phase
reactor. Espinoza et al. (1999) modified gas distribution theory proposed by Toomey and
Johnstone (1952) for slurry bubble column reactors where it was divided into dense and
dilute phases. The minimum fluidization velocity was replaced by transition velocity
from homogeneous to heterogeneous flow regime. Using the modified two-phase theory,
they developed an approach similar to the one proposed by Krishna and Ellenberger
(1992). Espinoza et al. (1999) mentioned that during scaleup of 1 m diameter FT reactor
to 5 m diameter one, such an approach was not used. However, an importance of gas and
slurry mixing characteristics in a slurry bubble column was emphasized.
The reported scaleup procedures so far utilize the similarity of global parameter such as
overall gas holdup in two columns for hydrodynamic similarity. Such similarity based on
38
global parameters is not surprising because over the years bubble column hydrodynamics
have been quantified mostly based on the global parameters such as overall gas holdup
and mass transfer coefficient. Based on the studies reported by Macchi et al. (2001), it is
clear that the close overall gas holdup in two systems does not necessarily result in
similar local hydrodynamics. Hence, there is a need to evaluate and update the
generalization of hydrodynamic similarity based on global parameter such as overall gas
holdup and a new approach needs to be sought.
39
Chapter 3.
Experimental Investigation of the Hydrodynamics of
Slurry Bubble Column: Phase Holdups Distribution via
Computed Tomography
As mentioned in Chapter 2, although there have been numerous efforts to study the
hydrodynamics of bubble/slurry bubble column reactors, most of these studies provide
information regarding global hydrodynamics. The only investigations to study the
detailed hydrodynamics of bubble and slurry bubble column reactors at high superficial
gas velocities and/or pressures of industrial interest were performed using air-water and
air-water-150 m glass beads systems (Kumar, 1994; Degaleesan, 1997; Ong, 2003;
Rados, 2003). No work has been reported that studies the detailed hydrodynamics (the
radial profiles of axial velocity, turbulent kinetic energy, normal stress, shear stress, and
eddy diffusivities) of slurry bubble column reactors at high superficial gas velocity and
pressure using a liquid other than water. That motivates us to study the detailed fluid
dynamics and mixing characteristics at the operating conditions of pressure and
superficial gas velocity using a gas-liquid-solids system of industrial interest. There are
two ways to proceed: either perform experiments using real industrial conditions or
mimic a industrial system and operating conditions in the laboratory. Due to the general
limitations encountered in laboratory studies, we have chosen the second option. As
mentioned earlier, one of the most popular applications of slurry bubble column reactors
in the present day is the conversion of syngas to liquid fuels called as Fischer-Tropsch
(FT) synthesis. Based on this, one of the primary objectives of this chapter is to
investigate and study the effect of operating parameters on the flow behavior of slurry
bubble columns using a liquid that at room temperature mimics FT wax at FT reaction
conditions. This study will thus provide an idea about how the change in liquid phase
would affect the qualitative and quantitative behavior of these flows. In addition to
providing detailed insights into the flow microstructure of slurry bubble columns, this
40
study will extend a database that can be utilized as a benchmarking tool for CFD and
phenomenological modeling.
This study of the flow behavior of slurry bubble columns is divided into two chapters.
This chapter discusses the choice of phases employed, experimental setup, and
techniques, and then presents results, acquired via CT, related to the effect of operating
parameters on phase distribution in the selected system. Chapter 4 discusses the effect of
these operating parameters on the solids axial velocity and turbulent parameters at similar
conditions.
3.1 Choice of Phases
3.1.1
Choice of Liquid Phase
The physical properties of various liquids at ambient conditions were compared with
those of Sasol FT wax at FT reaction conditions, i.e., P = 3.1 MPa and T = 2400 C. The
physical properties of Sasol wax were measured at the Multiphase Flow and Powder
Reaction Laboratory, The Ohio State University, Columbus, utilizing a technique
developed for insitu measurement of fluid properties at high pressure and high
temperature. Based on the comparison, a heat transfer fluid popularly known as
Therminol LT was identified (the Material Safety Data Sheet is provided in Appendix-E),
which has the properties close to those of Sasol wax. Table 3-1 shows the physical
properties of Sasol wax and Theminol LT.
Table 3-1: Physical properties of Sasol wax and Therminol LT
Fluid
Pressure
Temperature
Density
Viscosity
Surface Tension
Sasol Wax
(MPa)
3.1
(0C)
240
(g/cc)
0.69
(cP)
0.81
(dyne/cm)
16.6
Therminol LT
0.1
25
0.866
0.88
17
41
The viscosity and surface tension of Sasol wax and Therminol LT are similar, while there
is a difference in their density values. Based on previous studies, it is known that the
effecst of viscosity and surface tension on flow behavior are dominant over that of fluid
density (Wilkinson, 1991). Hence, Therminol LT was used as the FT mimic liquid due to
its relatively close values of viscosity and surface tension.
3.1.2
Choice of Gas Phase
Air was used as the gas phase in this study. At an operating pressure of 1 MPa, the
density of air (12 kg.m-3) is close to the density of syngas at FT synthesis conditions.
Hence, the experimental investigations were planned at 1 MPa, in addition to an ambient
pressure to study the effect of pressure (i.e., gas density). The experimental conditions at
high pressure and ambient temperature enabled us to mimic gas and liquid phases at FT
synthesis conditions.
3.1.3 Choice of Solids Phase

FT catalyst/carrier would have been an ideal choice to mimic FT conditions. However,
glass beads with an average diameter of 150 m and particle density of 2500 kg/m3 were
selected as the solids phase, for two reasons. The first reason is related to the limitations
on the radioactive tracer particle used in CARPT experiments. A 150 m radioactive
particle has previously been successfully manufactured and irradiated and safely used in a
slurry bubble column using an air-water-glass beads system (Rados, 2003). Furthermore,
due to the limitations of the MIT Nuclear Reactor used for irradiation, it was not possible
or economical to irradiate a particle smaller than 150 m. The second reason is to
complement Rados (2003) studies and provide proper experimental comparison to study
the effect of physical properties on the flow structure of slurry bubble column reactors
using a radioactive particle that matched properly in size and density of the solids used.
Moreover, the glass beads (range: 125 to 175 m, with 85 % and above in the range of
145-155 m) used in Rados (2003) and the current studies have a density of 2.5 gm.cc-1.
This value is close to the apparent density (density of solids filled with liquid in its pores)
42
of FT catalyst, i.e., 2.2 gm.cc-1, which has a mean size of 70-90 m, with 45 % of the
solids 90 m and above. These glass beads present an opportunity to study the effect of
non-porous solids that can provide a benchmark for future studies on porous FT catalyst.
3.2 Experimental Details
3.2.1 Experimental Setup

The experiments were carried out in a stainless steel column with an inner diameter of
0.162 m and a height of 2.5 m. Figure 3-1 is a schematic of the high pressure stainless
steel column without ports used for noninvasive measurements. The column with ports
and staggered windows was used for overall gas holdup measurements and is shown in
Figure B-1. Both columns are designed to support a maximum operating pressure of 300
psi. The air as a gas phase was supplied from two compressors connected in parallel, with
a working pressure of 1.45 MPa and a maximum corresponding rated flow rate of 8.8
m3/min. The compressed atmospheric air was purified by passing it through a dryer and
several air filter units. The air flow rate was regulated by a pressure regulator and
rotameter setup, which consisted of four rotameters of increasing range connected in
parallel. Air exited the column through a demister, passed through a back pressure
regulator that controlled the column operating pressure, and was vented to the
atmosphere. The column design enabled easy removal of the distributor chamber and
replacement of the sparger. The sparger used in this study has a porosity of 1.09 %. It
consists of 163 holes of 1.32 mm diameter with triangular pitch of 1 cm. Ong (2003)
studied the effect of the distributor on the hydrodynamics of bubble columns and showed
that the effect of the distributor is insignificant, particularly in the churn-turbulent flow
regime. Hence, only one type of sparger was employed in this study (Figure B-2). In all
experiments, the dynamic height of slurry was maintained at 1.8 m (z/D ~ 11) from the
distributor by varying the initial static height of the slurry based on the operating
condition.
43
3.2.2 Experimental Conditions
The selection of experimental conditions enabled a systematic comparison with Rados
(2003) studies. In the literature, no studies regarding detailed flow behavior are reported
at the high solids loading typically employed in industrial processes. Hence, the effect of
solids loading is studied using both low (similar to Rados, 2003), and high solids loading.
Additionally, CT experiments were performed without solids. Table 3-2 lists the
experimental conditions employed in this work. It covers the study of the effect of
parameters of interest, superficial gas velocity, operating pressure, and solids loading. In
addition, the comparison of the performed experiments with those of Rados (2003)
provides information regarding the effect of liquid phase physical properties on the
hydrodynamics of such systems.
44
Top
Cover
6 3/8
Demister
4 3/4
Gas
Outlet
28 1/2
CT 3
21 1/2
90
CT 2
21 1/2
CT 1
Batch
Drain
1
Probe
8 3/4
4 1/2
8
Gas
Inlet
Bottom
Liquid
Drain
13
Figure 3-1: Bubble/slurry bubble column reactor of 6 diameter used for CARPT/CT
measurements. CT1, CT2, and CT3 represent the scan levels used in this investigation.
45
Table 3-2: Experimental conditions employed in this study
Run
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
Superficial gas
velocity
(cm/s)
8
14
20
30
8
14
20
30
20
30
20
30
20
30
20
30
Operating
pressure
(MPa)
0.1
0.1
0.1
0.1
1
1
1
1
0.1
0.1
1
1
0.1
0.1
1
1
Solids loading
(% vol.)
9.1
9.1
9.1
9.1
9.1
9.1
9.1
9.1
25
25
25
25
0
0
0
0
3.3 Single Source Computed Tomography (CT)

CT has been extensively implemented on various multiphase flow systems at the CREL,
Washington University (Kumar, 1994; Roy, 2001; Rados, 2003; Ong, 2003). Software
and hardware details of the single source -ray CT have been explained elsewhere in
detail (Kumar, 1994). Hence only a brief description is provided here. The CT setup
(Figure 3-2) consists of an array of detectors with an opposing source, which rotate
together around the object to be scanned. The scanner uses a Cesium (Cs-137)
encapsulated ray source with activity of ~ 85 mCi. The array of detectors and the
source are mounted on a gantry which can be rotated 3600 around the object to be
scanned, using a step motor. Also, the source-detector setup can be moved up and down
to scan cross-sections at any axial position of the column. In the present study, 5 NaI
scintillation detectors were used that cover the reactor diameter. Each detector consists of
a cylindrical 2 2 inch NaI crystal, a photo multiplier (PM), and electronics, forming a
46
0.054 0.26 m cylindrical assembly. In each view, every detector acquires 7 projections
covering the total angular span of 2.72o of the detector face. The total 99 views were
acquired with 3.6o of angular shift after every view. Hence, 3645 (5 x 7 x 9) projections
were used to reconstruct the phase holdup distribution at each cross-sectional plane. The
entire system is completely automated to acquire the data needed for the reconstruction of
the phase distribution in a given cross-section. After detailed analysis of various
algorithms, Kumar (1994) implemented the Estimation-Maximization (EM) Algorithm
for image reconstruction. It is based on maximum likelihood principles and takes into
account the stochastic nature of the -ray beam projection measurements.
Figure 3-2: Configuration of the CT experimental setup (Kumar, 1994).

While single source CT is used to reconstruct two-phase and three-phase (with stationary
solids phase) holdup distributions, the dynamic three-phase system under investigation
requires additional information to completely resolve phase holdup profiles. In the
absence of a dual energy/source CT technique, Rados (2003) proposed a methodology,
viz., CT/Overall gas holdup, to calculate phase holdup profiles in a slurry system using a
single -ray source. The details of this methodology are available elsewhere (Rados,
2003; Rados et al., 2005). This methodology utilized the following two assumptions,
which are sound at the range of employed operating conditions,
47
a) Axially invariant gas holdup.
b) Uniform cross-sectional solids loading (solids concentration). That is, the ratio of the
volume of solids to the volume of slurry (liquid+solids), [ Vs /(Vs + VL ) ] is constant
along the cross-section of the column.
Although the method facilitates reconstruction of three dynamic phases using single
source CT, it needs a prior knowledge of the overall gas holdup of the system under
study.
This work also initiated an effort to evaluate these assumptions and their range of
validity by combining two single modal tomographic techniques, viz., CT and Electrical
Capacitance Tomography (ECT). CT measurements were performed at Washington
University, while ECT measurements were to be performed at The Ohio State University
at identical operating and design conditions. The CT experiments and the development
of an algorithm for combination were completed at Washington University. The details
of this work can be referred to Appendix-A.
3.4 Results and Discussion
3.4.1
Overall gas holdup
Overall gas holdup measurements were performed at the conditions of interest. The
overall gas holdup was obtained by measuring the change in liquid/slurry height. The
experiments were performed using different solids loadings, viz. 9.1, 18, 25 vol.% over
the range of superficial gas velocities, and two pressures, 0.1 and 1 MPa. The
experiments were repeated three times and were found to be reproducible within 2 % of
relative error.
Figure 3-3a shows the effect of solids loading on the overall gas holdup in the airTherminol LT-glass beads system. With an increase in solids loading, overall gas holdup
decreases, which is consistent with the previous literature findings (Krishna et al., 1997).
48
An increase in solids loading increases pseudo-viscosity, which promotes coalescence of
large bubbles (Crabtree and Bridgewater, 1971), whereas the bubble break-up rate
decreases due to dampening of instabilities at interface. As a result more large bubbles
form in the system with an addition of solids, resulting in a decrease in transition
velocity. These large bubbles have high rise velocity, which results in lower gas holdup.
It can be observed that the point at which the change in the slope of the gas holdup curve
occurs shifts towards lower superficial gas velocity with an addition of solids. This can
be confirmed by plotting the drift flux (equation 2-2) against the overall gas holdup as
shown in Figure 3-3b. The drift flux plot also indicates an advance of the flow regime
transition to a lower superficial gas velocity with an increase in the solids loading, due to
the relatively early appearance of large bubble at increased solids loading. Hence, these
observations confirm that most of the planned experimental conditions appear to be in the
churn-turbulent flow regime.
Figure 3-4 shows the effect of operating pressure on overall gas holdup at various solids
loadings in the air-Therminol LT-glass beads system. An increase in pressure results in
(a)
(b)
Figure 3-3: Effect of solids loading on a) overall gas holdup curve and b) drift flux plot in
the air-Therminol LT-glass beads system at ambient conditions in a 6 diameter steel
column
an increase in overall gas holdup at the same superficial gas velocity. Increased gas
density at high pressure promotes bubble break-up, which counteracts the formation of
49
Figure 3-4: Effect of operating pressure on overall gas holdup at various solids loading in
air-Therminol LT glass beads system in a 6 diameter steel column
larger bubbles due to coalescence (Wilkinson et al., 1993). The higher number of
relatively smaller bubbles at high pressure results in higher overall gas holdup.
3.4.2 Drift Flux Model

The drift flux is defined as the volumetric flux of either phase relative to a surface
moving at the volumetric average velocity. Zuber and Findlay (1964) presented the
detailed derivation for the drift-flux model based on an argument that gas holdup in twophase flow depends on two phenomena: the gas rises locally relative to liquid due to
phase density differences, and the gas holdup and velocity distribution across the column
diameter cause gas to concentrate in a faster or slower region of flow, thereby affecting
the average gas holdup. Their model has been represented as follows,
UG
= C 0 (U G U L ) + C1 ,
(3-1)
where,
C0 =
G (U G U L )
G (U G U L )
(3-1a)
and
C1 =
jGL
(3-1b)
50
The symbol
represents averaging over the column cross-sectional area. In equation
(3-1), C0 is a distribution parameter and is a measure of the interaction of the holdup and
velocity distribution. The value of C0 is close to unity for flatter phase holdup profiles
and increases as the phase holdup profiles become steeper. C1 is the weighted average
drift velocity, accounting for the local slip. Generally, it is assumed to be similar to the
rise velocity of a bubble in an infinite medium.
Table 3-3: The values of drift flux parameters at the studied experimental conditions
Operating
Solids loading
Pressure
(% vol.)
C0
C1
R-squared
value
(MPa)
0.1
1.9
0.26
0.9910
0.1
9.1
1.8
0.36
0.9963
0.1
18
2.2
0.39
0.9837
0.1
25
0.44
0.9946
9.1
1.6
0.22
0.99
18
1.7
0.25
0.9893
25
1.9
0.36
0.9914
The overall gas holdup data was analyzed using equation 3-1. In the current study the
system is in batch mode, hence, UL = 0. Hence, equation 3-1 can be written as,
UG
= C0 (U G ) + C1 .
(3-1c)
Table 3-3 shows the values of C0 and C1 for different solids loading and operating
pressures. It can be observed that an increase in pressure decreases the value of C0, while
an increase in solids loading increases the value of C0. This result indicates that an
increase in pressure results in relatively flat profiles, while an addition of solids results in
51
steeper phase holdup profiles. The value of C1 decreases with an increase in pressure,
indicating that the value of bubble rise velocity decreases with pressure. An increase in
pressure reduces the mean bubble size due to an increase in the break-up rate and a
decrease in the coalescence rate, which results in a decrease in bubble rise velocity. An
increase in solids loading increases C1, resulting in higher bubble rise velocity with an
increase in solids loading. Increased solids loading produces larger bubbles that have
relatively higher rise velocities.
3.4.3 Cross-sectional distribution of gas holdup
Figure 3-5 shows the cross-sectional distribution of gas holdup at different superficial gas
velocities, solids loading of 9.1 % volume, and operating pressures of 0.1 and 1 MPa. The
red color shows higher gas holdup, while the blue indicates lower gas holdup. In general,
it can be observed that gas holdup is higher in the center and lower near the wall. At
lower superficial gas velocity, relatively uniform distribution of gas holdup can be
observed. Increases in superficial gas velocity and operating pressure tend to increase the
magnitude of gas holdup, while an increase in solids loading decreases gas holdup.
Generally, the cross-sectional distribution gives a qualitative picture of the way gas is
distributed across the column. The cross-sectional distribution of gas holdup observed in
this study is qualitatively similar to the one obtained in an air-water-glass beads system
(Rados, 2003), with differences in its magnitude that will be explained in the succeeding
section. The differences in magnitude and the trend observed in this study due to the
change in the liquid phase are pertinent to a fundamental understanding of the flow
behavior in a FT system.
52
a) P = 0.1 MPa
b) P = 1 MPa
Figure 3-5: Cross-sectional distribution of gas holdup in 6 diameter stainless steel

column using air-Therminol LT-glass beads system at different superficial gas velocities,
solids loading of 9.1 % vol., and P = a) 0.1, and b) 1 MPa.
a) 9.1 % volume
b) 25 % volume
Figure 3-6: Cross-sectional distribution of gas holdup in 6 diameter stainless steel

column using air-Therminol LT-glass beads system at superficial gas velocity of 30 cm/s,
operating pressure of 1 MPa, and solids loading of a) 9.1, and b) 25 % volume.
53
They show symmetry in gas holdup distribution using air-Therminol LT-glass beads
systems similar to the air-water and air-water-glass beads systems, as observed
previously by Kumar (1994), Chen et al. (1999), Ong (2003), and Rados (2003). Such
symmetry exists at high pressure and even at high solids loading, as is evident from
Figure 3-6. However, for quantitative analysis, azimuthally averaged gas holdup along
the column radius has been studied and will be discussed in the remaining part of the
chapter. Selected experimental conditions were repeated, and the reproducibility of phase
holdup profiles was found to be reasonable. The results are presented in Appendix B
(Section B-2).
3.4.4
Time-averaged gas and solids holdup radial profile
Figures 3-7 and 3-8 show the gas and solids holdup radial profile obtained using the
CT/Overall gas holdup methodology at all axial locations (2.1D, 5.5D, and 9D) in airTherminol LT-glass beads at 8 cm/s, 0.1 MPa, and 9.1 % vol. and 30 cm/s, 1 MPa, and
25 % vol., respectively. The gas holdup profiles in the slurry systems look much like the
ones obtained in gas-liquid systems (Kemoun et al., 2001; Ong 2003). There are
insignificant differences between gas holdup profiles at various axial levels, which is due
to the assumption of axially invariant gas holdup stated earlier. The solids holdups are
higher at the wall than the center due to presence of high gas holdup in the center region
of the column. These findings are consistent with those reported in the literature (Rados
et al., 2005). The solids holdup profile along the radius shows two zones, one where it
remains almost uniform (0 r/R 0.6) and a second where there is a relatively sharp
increase in solids holdup towards the wall. A decrease in cross-sectionally averaged
solids holdup was found along the length of the column. At operating conditions of 8
cm/s, 0.1 MPa, and 9.1 % vol., the cross-sectionally averaged solids holdups at axial
locations of 2.1D, 5.5D, and 9D are close to 0.12, 0.074, and 0.044, respectively.
54
(a)
(b)
Figure 3-7: a) Gas holdup and b) solids holdup radial profile in an air-Therminol LTglass beads system using 9.1 % vol. solids loading at a superficial gas velocity of 8 cm/s
and ambient pressure.
(a)
(b)
Figure 3-8: a) Gas holdup and b) solids holdup radial profile in an air-Therminol LTglass beads system using 25 % vol. solids loading at a superficial gas velocity of 30 cm/s
and operating pressure of 1 MPa.
This corresponds to solids loadings of 13.6, 8.9, and 4.5 % vol. at these axial locations.
The axial average of these estimated solids loadings at the three axial locations is 9 %
vol., which is close to the employed solids loading at this condition (i.e., 9.1 % vol.). At
operating conditions of 30 cm/s, 1 MPa, and 25 % vol., the cross-sectionally averaged
solids holdups are 0.24, 0.17, and 0.11, which correspond to solids loadings of 34.9, 24.5,
and 15.8, respectively. The axially averaged estimated solids loading at this condition is
25.4 % vol., which is close to the employed solids loading of 25 % vol.
55
3.4.5 Effect of liquid phase physical properties on gas and solids holdup radial
profiles
The effect of liquid phase physical properties were studied by comparing the gas and
solids holdup radial profile in an air-Therminol LT-glass beads system obtained in this
work with that of an air-water-glass beads system using 9.1 % vol. solids loading (Rados,
20030). The experiments were performed with all other conditions the same, except the
employed liquid. Figure 3-9 shows the overall gas holdup curve in air-water-glass beads
and air-Therminol LT-glass beads systems at ambient conditions and solids loading of
9.1 % vol. in 0.1615 m diameter column.
Figure 3-9: Overall gas holdup curve using air-water-glass beads (Rados, 2003) and airTherminol LT-glass beads system at ambient conditions and solids loading of 9.1 % vol.
in a 6 diameter column.
The overall gas holdup curve in air-water-glass beads shows a familiar S-shaped curve in
transition regime that starts around 5 cm/s and is extended up to 12 cm/s. It is worth
mentioning that the S-shaped curve is not unique characteristic of air-water systems.
Based on the reported studies, it appears to be a strong function of the type of distributor
and operating conditions. The maximum gas holdup value was found at a superficial gas
velocity of 8 cm/s. No such S-shaped behavior was observed in an air-Therminol LTglass beads system. The increase in gas holdup with superficial gas velocity is gradual in
Therminol LT. Thimmapuram and Saxena (1992) provided the following explanation for
such different behavior in water and oil systems. They performed overall gas holdup and
heat transfer studies in nitrogen-water and nitrogen-Therminol 66 systems. They
56
observed S-shaped behavior in water, but not in Therminol 66. Based on the studies of
Saxena and Rao (1991), they concluded that for water systems, bubble size almost
remains constant in the bubbly flow regime, while in Therminol systems, it keeps
growing steadily. Hence, the increase in gas holdup with superficial gas velocity in water
is higher in this regime. In the transition and churn-turbulent flow regimes, bubble
coalescence sets in abruptly, resulting in rapid growth of coalesced bubbles, which
initially decreases the gas holdup, then keeps its magnitude constant in the churnturbulent flow regime. In Therminol 66, bubble coalescence occurs in the transition and
churn-turbulent flow regime, but the number of bubbles also increases with an increase in
superficial gas velocity. Hence, variation in gas holdup with superficial gas velocity is
different in these two systems. In addition, various authors (e.g., Yamashita and Inoue,
1975; Maruyama et al. 1986) explained the peak in gas holdup as being based on
structure collapse near transition.
The comparison of overall gas holdup in water and Therminol LT shows that in the
bubbly flow regime, overall gas holdup in water is higher than in Therminol LT, while in
churn-turbulent flow regime, it is higher in the Therminol LT. In the transition regime (513 cm/s), gas holdup in water is higher than in the Therminol LT system. The higher gas
holdup in water in the bubbly flow regime and also near the transition regime due to Sshaped behavior has been discussed above. The higher gas holdup in Therminol LT
-3
-1
(viscosity, L = 0.88 cP, density, L = 886 kg.m , surface tension, L = 17 dyne.cm )

-3
compared to water ((viscosity, L = 1 cP, density, L = 998 kg.m , surface tension, L =

-1
72 dyne.cm ) in churn-turbulent flow can be attributed to the physical properties.

Therminol LT has lower viscosity and surface tension than water. When the surface
tension decreases, the bubble breakup rate increases and the coalescence rate decreases,
resulting in a relatively large number of small bubbles (Walter and Blanch, 1986). Also,
the lower viscosity promotes bubble break-up (because of the instabilities at the bubble
interface) and decreases bubble coalescence rate (Wilkinson, 1991), increasing the small
bubble population. Hence, the combination of lower viscosity and surface tension results
57
in relatively lower occurrences of larger bubbles in Therminol LT, which reduces bubble
rise velocity and thereby increases overall gas holdup.
The overall gas holdups at superficial gas velocities of 8, 14, and 30 cm/s at ambient
pressure and solids loading of 9.1 % vol. in the water system are 0.23, 0.22, and 0.27,
while in the Therminol LT system, they are 0.16, 0.23, and 0.33, respectively. The
absolute relative differences in gas holdup values at 8, 14, and 20 cm/s are 29, 5, and 19
%, respectively. Hence, it is obvious that the magnitude of gas holdup profiles in water
will be higher at Ug = 8 cm/s, while it will be higher in Therminol LT at Ug = 30 cm/s.
Also, the magnitude of the gas holdup profiles will be closer at Ug = 14 cm/s.
Figure 3-10 shows the comparison of gas and solids holdup radial profiles in air-waterglass beads and air-Therminol LT-glass beads systems at ambient pressure and solids
loading of 9.1 % vol. in a 6 diameter column. At Ug = 8 cm/s, as discussed earlier,
overall gas holdup is higher in water than in Therminol LT, which results in a higher
magnitude of the gas holdup radial profile in water. The higher gas holdup in water
results in a lower magnitude of the solids holdup radial profile in water. The solids
holdup profile is higher in Therminol LT due to lower gas holdup in this system.
However, in both the systems, the solids holdup profiles are relatively flat. At Ug = 14
cm/s, the overall gas holdup values are close to each other. Hence, the magnitude of gas
holdup radial profiles is similar in both the systems. The holdup profiles in both the
systems almost match. The similar gas holdup profiles in water and Therminol LT results
in close solids holdup radial profiles in these systems. As discussed earlier, at Ug = 30
cm/s, the magnitude of gas holdup in Therminol LT was found to be higher than in water,
and hence higher magnitude of gas holdup radial profiles were observed in Therminol
LT. The higher gas holdup radial profiles result in slightly lower solids holdup radial
profiles
58
(a)
(b)
0.1
0.7
P = 0.1 MPa
Solids holdup (-)
P = 0.1 MPa
0.6
Gas holdup (-)
0.5
0.4
0.3
air-water-glass beads
air-Therminol LT-glass beads
0.2
0.05
0.1
0
0
0.2
0.4
0.6
0.8
Dimensionless radius (-)
0.2
0.4
0.6
0.8
(c)
Figure 3-10: Effect of physical properties on a) gas holdup, and b) solids holdup radial
profile at P = 0.1 MPa, z/D = 5.5, solids loading of 9.1 % vol., and Ug = a) 8, b) 14, and
c) 30 cm/s in 6 diameter steel column
in Therminol LT. The close observation of gas holdup radial profiles in these systems
shows that the shape of the profile is relatively flatter in Therminol LT, which is due to
the presence of more small bubbles than in water. Also, the lower viscosity and surface
tension in Therminol LT tend to delay flow regime transition to the churn-turbulent flow
regime.
59
Figure 3-10 also shows the effect of superficial gas velocity on the radial profiles of gas
and solids holdup in an air-Therminol LT-glass beads system at ambient pressure and
solids loading of 9.1 % vol. in a 6 diameter column. An increase in superficial gas
velocity from 8 to 30 cm/s increases overall gas holdup from 0.16 to 0.33, and hence the
magnitude of gas holdup radial profile increases. With an increase in superficial gas
velocity, the system tends to be in the churn-turbulent flow regime. An increase in
superficial gas velocity results in more large bubbles that give rise to a wider bubble size
distribution. This subsequently results in a steeper gas holdup radial profile. An increase
in superficial gas velocity from 8 to 14 cm/s increases overall gas holdup by 28 %, while
increases in superficial gas velocity from 14 to 20 cm/s and from 20 to 30 cm/s increase
overall gas holdup by 17 and 15 %. As discussed in Section 3.4.1, the transition velocity
at this condition is around 5-6 cm/s. Accordingly, Ug = 8 cm/s which, is close to bubbly
flow and/or in the transition region, while other operating conditions fall in churnturbulent flow regime. Hence, a relatively larger change in overall gas holdup was
observed when superficial gas velocity was increased from 8 to 14 cm/s. As the system
enters the churn-turbulent flow regime, the rate of increase in gas holdup reduces with an
increase in superficial gas velocity, due to non-linear and intense interaction between
bubbles. An increase in superficial gas velocity at a given operating pressure and solids
loading does not seem to have a noticeable effect on gas holdup near the wall.
It can be observed that with an increase in superficial gas velocity, the magnitude of the
solids holdup profile decreases due to an increase in gas holdup. The solids holdup
profile tends to become steeper with an increase in superficial gas velocity as the system
tends to be in the churn-turbulent flow regime, which results in increased solids mixing.
This was reflected when Ug increased from 14 to 20 cm/s and 20 to 30 cm/s. At Ug = 8
cm/s, the solids holdup profile is relatively flatter, and gradually becomes steeper with an
increase in superficial gas velocity. The effect of superficial gas velocity on the gas
holdup profile is stronger than on the solids holdup profile. The effect of superficial gas
velocity on the solids holdup profile decreases with an increase in superficial gas
velocity. The stronger effect of superficial gas velocity on the solids holdup was found
when Ug was changed from 8 to 14 cm/s. The change in Ug from 8 to 14 cm/s reduces
60
the averaged solids holdup from by 8 %, while changes in Ug from 14 to 20 cm/s and 20
to 30 cm/s reduced the averaged solids holdup by 6.5 and 5 %, respectively.
Figure 3-11: Overall gas holdup curve using air-water-glass beads (Rados, 2003) and airTherminol LT-glass beads system at operating pressure of 1 MPa, and solids loading of
9.1 % vol. in a 6 diameter column.
Figure 3-11 shows the variation of overall gas holdup with superficial gas velocity at an
operating pressure of 1 MPa and solids loading of 9.1 % vol. in a 6 diameter column. At
high operating pressure, no S-shaped curve was observed in air-water-glass beads
systems, as was observed at ambient pressure. This observation is in line with the results
of Wilkinson (1991) and Letzel et al. (1997) who observed a gradual change in the
overall gas holdup at high pressure, as opposed to the S-shaped curve observed at
ambient pressure. Hence at high pressure, overall gas holdup in Therminol LT is
consistently higher than in water. The reason for this lies in the lower viscosity and
surface tension of Therminol LT. The combination of lower viscosity and surface tension
reduces the coalescence rate and increases the breakup rate, leading to more small
bubbles and a higher overall gas holdup in Therminol LT.
Figure 3-12 shows the effect of liquid phase physical properties on the gas and solids
holdup radial profiles at an operating pressure of 1 MPa and solids loading of 9.1 % vol.
at superficial gas velocities of 8, 14, and 30 cm/s. As explained above, based on the
61
(a)
(b)
0.7
0.1
P = 1 MPa
P = 1 MPa
0.6
Solids holdup (-)
Gas holdup (-)
0.5
0.4
0.3
0.2
0.05
0.1
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
0.2
0.4
0.6
0.8
(c)
Figure 3-12: Effect of physical properties on a) gas holdup, and b) solids holdup radial
profile at P = 1 MPa, z/D = 5.5 and solids loading of 9.1 % vol. at Ug = a) 8, b) 14, and c)
30 cm/s in a 6 diameter steel column
overall gas holdup curve at high pressure, the overall gas holdup is consistently higher in
Therminol LT than water at all the studied superficial gas velocities at high pressure. Due
to high overall gas holdup in Therminol LT system, the magnitude of the gas holdup
radial profiles is higher in Therminol LT. Similar to the ambient conditions, an increase
in gas holdup profile in Therminol LT resulted in a subsequent decrease in the solids
holdup radial profile. At high operating pressure, the gas holdup radial profiles at Ug = 8
62
cm/s look qualitatively similar in shape, while at Ug = 14 and 30 cm/s, the shapes of the
gas holdup radial profiles in Therminol LT are relatively flatter. The probable reason for
the similar shape at Ug = 8 cm/s can be due to existence of either the bubbly or transition
flow at these conditions. The comparison of gas holdup radial profiles in Therminol LT at
ambient and high pressure shows that an increased in pressure increases overall gas
holdup (Letzel et al., 1997; Kemoun et al., 2001) and hence the magnitude of the gas
holdup radial profile. An increase in pressure at the same superficial gas velocity
increased the gas density, which increased the rate of bubble break-up especially for large
bubbles. Such higher bubble break-up counters the formation of larger bubbles by
coalescence and generates small bubbles. The higher small bubble population in the
system results in an increase in overall gas holdup and therefore, the magnitude of the gas
holdup radial profile. An increase in pressure from 0.1 to 1 MPa at Ug = 8, 14, 20, and 30
cm/s increased gas holdup from 0.16 to 0.25, 0.22 to 0.33, 0.28 to 0.4 and 0.33 to 0.45,
almost relative increase of 36, 33, 30 and 27 % for solids loading of 9.1 % vol.,
respectively. The effect of pressure tends to decrease with an increase in superficial gas
velocity, which adds larger bubbles to the system with an increase superficial gas velocity
that counters the formation of smaller bubbles due to higher pressure. However, the effect
of operating pressure on gas holdup appears to be stronger than that of superficial gas
velocity. For example, at solids loading of 9.1 % vol., an increase in superficial gas
velocity from 14 to 20 and 20 to 30 cm/s increases gas holdup by 21 and 14 %,
respectively while an increase in operating pressure from 0.1 to 1 MPa at Ug = 14, 20,
and 30 cm/s increases gas holdup by 33, 30 and 27 %, respectively.
Due to generation of smaller bubbles at increased pressure, the shape of the gas holdup
radial profile becomes relatively flatter. An increase in pressure, in general, increases the
gas holdup in the center as well as close to the wall. An increase in gas holdup at higher
pressure results in reduction of solids holdup with an increase in operating pressure. In
addition, close observation of the solids holdup profile shows a relatively flatter profile at
higher operating pressure. The effect of pressure on the solids holdup profile is not as
strong as its effect on the gas holdup profile.
63
At ambient pressure and Ug = 30 cm/s, the gas holdup in Therminol LT was 0.33, while
in water it was 0.28, almost an increase of 19 %. At high pressure, the gas holdup in
Therminol LT was 0.44 while in water it was 0.39, almost an increase of 13 %. The
difference in liquid appears to have stronger effect at ambient pressure. In water, gas
holdup increased by 33 %, while in Therminol LT it increased by 28 % with the change
in operating pressure from 0.1 to 1 MPa.
The effect of physical properties on the solids holdup profile was observed to be less
significant than on the gas holdup radial profile. At Ug = 8 cm/s, the cross-sectional
averaged solids holdup in Therminol LT increased by 12 %, while gas holdup in
Therminol LT was reduced by 29 %. At Ug = 14 cm/s, the changes in cross-sectional
solids and gas holdups were 2.5 and 5 %, respectively. At Ug = 30 cm/s, the change in
cross-sectional solids and gas holdup is 6.5 and 18 %, respectively, while at P = 1 MPa,
the solids holdup was reduced by about 3.6 %. It should be noted that the reduction in
cross-sectional averaged solids holdup is higher at atmospheric pressure, and the increase
in gas holdup is also higher at ambient pressure.
3.4.6 Effect of solids loading on gas and solids holdup radial profiles
The effect of solids loading on gas and solids holdup radial profiles at ambient pressure
and Ug = 20 and 30 cm/s is illustrated in Figure 3-13. An increased solids loading
reduces gas holdup and hence the magnitude of gas holdup radial profile. With an
addition of solids loading, the coalescence rate increases, while the break-up rate
decreases, which generates larger bubbles. The large bubbles have a high bubble rise
velocity that results in lower gas holdup at increased solids loading. An increase in solids
loading from 0 to 9.1 % vol. decreased the magnitude of the gas holdup radial profile.
However, the effect of addition of solids from 0 to 9.1 % vol. was weaker than the
addition of solids from 9.1 to 25 % vol. This observation is in line with the previous
studies of Rados (2003) who observed a weak effect of the addition of solids on the gas
holdup radial profile by changing the solids loading from 0 to 9.1 % vol. in air-water- 150
m glass beads system. This weak effect is evident from the change in overall gas holdup
with an addition of solids. Increasing solids loading from 0 to 9.1 % vol, reduced overall
64
gas holdup by close to 9 % at Ug = 20 and 30 cm/s, while increasing solids loading from
9.1 to 25 % vol. reduced overall gas holdup by close to 34 % at Ug = 20 and 30 cm/s.
Similar trend was observed by Behkish (2005) in a He-Isopar M-alumina system at Ug =
15.4 cm/s and T = 400 K in a 0.3 m diameter column. An increase in solids loading from
0 to 10 % vol. reduced gas holdup by 10 %, while increasing solids loading from 10 to 20
% vol. reduced gas holdup by 60 %.
As mentioned earlier, the addition of solids increased the large bubble population in the
system. An increased larger bubble population, along with trapped small bubbles,
concentrates at the center of the column, pushing small bubbles towards the wall. The
bubble size distribution becomes wider with the addition of solids to the system. The
(a)
(b)
Figure 3-13: Effect of solids loading on gas and solids holdup radial profile in airTherminol LT-glass beads system at ambient pressure at Ug = a) 20, and b) 30 cm/s 6
diameter steel column
reasoning is in line with the study of Lau (2004) who, based on 2-point optical probe
studies, observed wide bubble size distribution with an addition of solids. Due to this
reason, the gas holdup radial profile becomes relatively steeper at higher solids loading.
65
The system tends towards the churn-turbulent flow regime at higher solids loading when
operating at the same superficial gas velocity. The transition velocity calculated based on
the overall gas holdup curve and the drift flux plot also shows that an addition of solids
advances the flow regime transition. Additionally, gas holdup close to the wall is found to
be higher in the gas-liquid system compared to the slurry system. Also, it was found that
gas holdup close to the wall reduces as solids loading increases.
Obviously, an increase in solids loading increases the solids holdup at all axial locations.
The effect of superficial gas velocity and operating pressure on the solids holdup profile
was weaker than on the gas holdup profile. However, solids loading has a stronger effect
on the solids holdup profile than on the gas holdup profile. At Ug = 20 and 30 cm/s, an
increase in solids loading from 9.1 to 25 % vol. (change of 63.6 %) increased the crosssectional solids holdup by 68 and 66 % at ambient pressure.
Figure 3-14 shows the effect of solids loading on the gas and solids holdup radial profile
at superficial gas velocities of 20 and 30 cm/s and an operating pressure of 1 MPa.
Similar to the ambient pressure, increased solids loading decreased the magnitude of the
gas holdup radial profile. Similar to ambient pressure, the effect of addition of solids
from 0 to 9.1 % vol. was weaker (10 %) compared to an addition of solids from 9.1 to 25
% vol. At Ug = 20 and 30 cm/s, the gas holdup was reduced by 31 and 29 % at an
operating pressure of 1 MPa. The shape of the gas holdup radial profile became steeper
with an addition of solids. It is worth mentioning here that, although an increase in
operating pressure results in relatively flatter profiles, it cannot necessarily hold in the
case of high solids loading. As shown in Figure 3-14, at low solids loading and high
operating pressure, the profiles are relatively flat until r/R = 0.7, and then show a steep
decrease in gas holdup value in the region near the wall. However, at high solids loading
and high operating pressure, such behavior was not observed, and the gas holdup profiles
were found to be consistently steeper across the column radius. Although the shape of the
profile is steeper, it does show two different regions. However, both of these regions
show relatively steep behavior. The observation of such steep profiles at high operating
pressure (as opposed to flat ones at low solids loading and high pressure) is important for
66
FT reactor design, as these processes are generally operated at high pressure and high
solids loading. The importance of this finding is significant since the gas holdup profiles
studied at high pressure but low solids loading could be misleading. One should note here
that pressure and solids loading tend to have the favorable effect on FT reaction kinetics.
An increase in pressure increases the solubility of reactant gases in the liquid, while an
addition of solids increases the number of active sites in the reactor.
(a)
(b)
Figure 3-14: Effect of solids loading on gas and solids holdup radial profile in an airTherminol LT-glass beads system at Ug = a) 20, and b) 30 cm/s and P = 1 MPa in a 6
steel column
Hence, the knowledge of true behavior of the gas holdup profile at high pressure and
solids loading is pertinent in designing such reactors. An increase in solids loading from
9.1 to 25 % vol. (change of 63.6 %) increased solids holdup in the system by 70 and 71 %
at Ug = 20 and 30 cm/s, respectively.
67
The effect of solids loading on the gas holdup profile was stronger than the effect of
superficial gas velocity. At a superficial gas velocity of 20 cm/s, an increase in solids
loading from 9.1 to 25 % vol. at P = 0.1 and 1 MPa changed gas holdup by 35 and 30 %,
respectively. While the change in operating pressure from P = 0.1 to 1 MPa at solids
loading of 9.1 and 25 % vol. shows the change in gas holdup by 30 and 35 %,
respectively. At superficial gas velocity of 30 cm/s, an increase in solids loading from 9.1
to 25 % vol. at P = 0.1 and 1 MPa changes gas holdup by 34 and 30 %, respectively.
While the change in operating pressure from P = 0.1 to 1 MPa at solids loading of 9.1 and
25 % vol. shows the change in gas holdup by 28 and 32 %, respectively. This shows that,
pressure affects more at high solids loading while the solids loading has relatively more
effect at low pressure. However, the effect of solids loading at lower pressure is stronger
than the effect of pressure at higher solids loading.
3.4.7 Normalized gas holdup radial profile

The normalized gas holdup radial profile is the ratio of gas holdup at a certain radial
location to the cross-sectional averaged gas holdup. The analysis detailed discussion of
the normalized gas holdup radial profile is included in Appendix B (Section B-6).
3.4.8
Normalized solids holdup radial profile
The normalized solids holdup radial profile is the ratio of solids holdup at a certain radial
location to the cross-sectional averaged solids holdup. The analysis detailed discussion of
the normalized solids holdup radial profile is included in Appendix B (Section B-7).
3.4.9
Comparison with predictions of Sedimentation-Dispersion Model (SDM)
The solids holdup axial gradient obtained in the current experimental studies was
compared with Sedimentation-Dispersion Model (SDM). SDM is currently the only
model available to predict the solids distribution over the column length in a batch slurry
68
reactor,. SDM predicts the exponential solids distribution profile in the following form
(for details, see Appendix-D),
z
]
L ,
S = S Bo S
1 exp [ BoS ]
exp [ BoS
(3-5)
where BoS is a Bodenstein number.
(a)
(b)
Figure 3-15: Predictions of the SDM in air-Therminol LT-glass beads system at ambient
pressure and solids loading of a) 9.1 and b) 25 % vol. in 6 diameter column
Figures 3-15a and b show the SDM predictions in air-Therminol LT-glass beads at P =
0.1 MPa and solids loading of 9.1 and 25 % vol., respectively. As expected, there is an
exponential solids distribution over the column length. At a given solids loading, the
SDM predicts more uniform solids distribution at higher superficial gas velocities. At
lower superficial gas velocities, it shows a higher solids holdup gradient and at lower
solids loading, it shows the relatively steeper solids distribution over the column length.
The correlations used to predict the solids axial dispersion coefficient do not account for
the effect of gas density, hence the comparison of the SDM predictions with the
experimental data was restricted to ambient pressure.
Figures 3-16a and b show the comparison of the SDM predictions with the experimental
data obtained in this study at superficial gas velocities of 8 and 30 cm/s, respectively. At
a superficial gas velocity of 8 cm/s, the experimental data is close to the SDM
predictions, while at a superficial gas velocity of 30 cm/s, the experimental data do not
69
match with the SDM predictions. However, the experimental data and SDM predictions
at z/D = 5.5 match well. The differences can be found only at z/D = 2.1 and 9. At Ug =
30 cm/s, the % average absolute errors between the experimental data and the SDM
prediction at z/D = 2.1 and 9 are 18 and 28 %, respectively.
(a)
(b)
Figure 3-16: Comparison of the SDM predictions with experimental data in airTherminol LT-glass beads system at ambient pressure, solids loading of 9.1 % vol., and
Ug = a) 8 and b) 30 cm/s in 6 diameter column
Figure 3-17a shows the SDM predictions with the experimental data at superficial gas
velocities of 20 and 30 cm/s. The experimental data shows a higher normalized solids
holdup gradient at higher superficial gas velocity. This is in contradiction to the SDM
predictions, as shown in Figure 3-15. However, at high superficial gas velocities such as
20 and 30 cm/s, the solids holdup gradient appears to be linear, rather than exponential as
predicted by the SDM. The experimental data at these conditions also do not match with
the SDM predictions at z/D = 2.1 and 9, while at z/D = 5.5, the SDM and experimental
data match well.
Figure 3-17b compares the effect of solids loading on solids distribution using the SDM
predictions and experimental data at a superficial gas velocity of 30 cm/s and ambient
pressure. The predictions of the SDM do not match with the experimental data obtained
70
(a)
(b)
Figure 3-17: Comparison of the SDM predictions with experimental data in airTherminol LT-glass beads system at ambient pressure. a) effect of superficial gas
velocity at solids loading of 25 % vol. and b) effect of solids loading at Ug = 30 cm/s in
6 diameter column
in this study. At a solids loading of 9.1 % vol., the average absolute errors between the
SDM prediction and experimental data are 18 and 28 %, while at a solids loading of 25 %
vol., the differences are 24 and 33 % at z/D = 2.1 and 9, respectively. However the trend
of the effect of solids loading predicted using the SDM is similar to the experimental
observation.
3.5
Remarks
The significant findings of this study are as follows.

1)
At ambient pressure, the comparison of gas and solids radial profiles in air-
Therminol LT-glass beads and air-water-glass beads reveals that in bubbly flow the
magnitude of the gas holdup profile is higher in water; in churn turbulent flow, it is
higher in Therminol LT. In transition flow, the close gas holdup radial profiles were
observed in water and Therminol LT. The increased gas holdup in water in bubbly flow
71
accords with the S-shaped behavior of the overall gas holdup curve at the studied
conditions. An opposite effect of superficial gas velocity was observed on the solids
holdup radial profile.
2)
At high operating pressure (1 MPa), the Therminol LT liquid phase consistently
increased the magnitude of the gas holdup radial profile due to an increased bubble
breakup rate and decreased coalescence rate that together produce more small bubbles.
This results in a relatively flatter profile in Therminol LT. The solids holdup radial
profile decreased with an increase in superficial gas velocity.
3)
An addition of solids in the slurry reduced the magnitude of the gas holdup radial
profile due to a higher coalescence rate that produces more large bubbles in the system.
The higher population of large bubbles concentrated at the center and resulted in a steeper
profile at increased solids loading, and thereby advancing flow regime transition. An
addition of solids linearly increased the solids holdup profile at both pressures. At high
operating pressure and high solids loading, the gas holdup radial profile showed a
consistently steeper profile. The shape of the profile at this condition is qualitatively
similar to the one observed at low solids loading and ambient pressure.
4)
Within the studied experimental conditions, the effect of superficial gas velocity
on overall gas holdup is weaker than that of operating pressure and solids loading.
5)
Changes in the studied operating parameters consistently affected the gas holdup
radial profile more than they affected the solids holdup profile.
6)
The cross-sectional averaged solids holdup increased with solids loading, but
decreased with superficial gas velocity and operating pressure.

7)
The normalized solids holdup profiles at all the axial locations show a similar
shape and fall on each other for a given operating condition. The normalized solids
holdup at low superficial gas velocities show a similar shape and also fall on each other,
while the normalized solids holdup at higher superficial gas velocities show a similar and
relatively steeper shape and fall on each other within a band of relative error of 10 %.
8)
The normalized solids holdup radial profile in water and Therminol LT shows
similar shapes and fall on each other at all the studied conditions except in bubbly flow at
ambient pressure. This shows that the solids flow behavior in these systems is
72
qualitatively similar. However, the differences are due to the different liquid phase
physical properties.
73
Chapter 4.
Experimental Investigation of the Hydrodynamics of
Slurry Bubble Column: Solids Flow Pattern via CARPT
This second part of the experimental investigation of the hydrodynamics of a slurry
bubble column focused on the effect of various operating parameters on the solids axial
velocity and turbulent parameters [turbulent kinetic energy, normal and shear stresses,
and eddy diffusivities] profiles using a liquid that at room temperature mimics FT wax at
FT reaction conditions. This chapter discusses the experimental setup, technique, and
results related to the solids axial velocity and turbulent parameters profiles.
4.1 Experimental
The choice of fluid and experimental setups is discussed in Chapter 3 and will not be
repeated here. Table 4-1 shows the CARPT experimental conditions used in this study.
Due to difficulties in performing CARPT experiments at severe conditions such as high
superficial gas velocity, high operating pressure, and solids loading along, with an
aromatic liquid, the experiments were planned only in fully churn-turbulent flow.
Table 4-1: CARPT Experimental conditions

Run
1
2
3
4
5
6
7
8
Superficial gas
velocity
(cm/s)
20
30
20
30
20
30
20
30
Operating
pressure
(MPa)
0.1
0.1
1
1
0.1
0.1
1
1
Solids loading
(% vol.)
9.1
9.1
9.1
9.1
25
25
25
25
74
4.2 Computer Automated Radioactive Particle Tracking (CARPT)
The computer Automated Radioactive Particle Tracking (CARPT) technique was first used
by Kondukov et al. (1964) to study particle motion in a fluidized bed. This technique has
been used extensively at Washington University in the CREL to measure the flow pattern
and turbulent parameters of different multiphase flow reactors in a non-invasive manner. A
CARPT experiment comprises two steps:
a) CARPT calibration (a static experiment),
b) CARPT experiment (a dynamic experiment).
The dynamic experiment involves tracking of a single radioactive tracer particle by

detecting the intensity distribution of emitted -rays. The -ray intensity distribution is
detected using an array of NaI scintillating detectors strategically placed around the studied
region of the column (Figure 4-1). In the static experiment, the photon count rate obtained
at each detector is related to the distance between the source and the detector. The
instantaneous position of the tracer is then accurately calculated from the distances using an
optimized regression scheme. The time differentiation of the displacement yields local
velocities. The ensemble averaged velocity profiles and turbulent parameters can then be
computed with the aid of an improved particle reconstruction algorithm proposed by Rados
(2003).
Due to various advantages, Scandium 46 with an activity of about 200 300 Ci was used
in this work (Rados, 2003). The objective was to compute solids instantaneous velocities,
the radial profile of the axial solids velocity, and turbulent parameters. Therefore a
radioactive particle of the same size and density as the solids was essential to monitor the
motion of the solids. A tracer scandium Sc46 particle of the required diameter was protected
with a thin coating of Parylene N. The resulting radioactive scandium Sc46 particle (with a
strength of up to 300 Ci and a half-life of 83 days) had a total diameter of 150 m, which
was equal to the average particle size of the glass beads used in this study. The density of
Paralyne N is 1.11 g/cm3, so the application of a 7 m coating lowered the overall particle
density from 2.99 g/cm3 (of pure scandium) to about 2.5 g/cm3.
75
The detailed experimental setup and calculation procedure for the CARPT experiments is
given in Degaleesan (1997) and Rados (2003). In-situ calibration of detectors was
performed under the desired operating conditions at high pressure. CARPT data (tracer
particle position in time) was acquired over a sufficiently long time to ensure enough
particle occurrences in each column cell and good time/ensemble averaging and was used
for calculation of the time averaged solids
a) velocities
b) Reynolds stresses
c) turbulent kinetic energy, and
d) eddy diffusivities
Figure 4-1: Configuration of the CARPT experimental setup (Degaleesan, 1997)
4.3 Results and Discussion
4.3.1
Time-averaged solids velocities
Before elaborating on the effect of liquid phase physical properties and solids loading, the
sample CARPT results at a superficial gas velocity of 30 cm/s, a solids loading of 9.1 %
vol,. and ambient pressure will be discussed (Figure 4-2). It should be noted that similar
qualitative flow behavior was observed at all the studied conditions. Based on CT studies
performed in the same system, it is known that the gas holdup is high in the center and
low at the wall, leading to buoyancy driven gross recirculation, which results in slurry
76
flowing up in the center (positive axial velocity) and down in the annular region, near the
column wall (negative axial velocity). Figure 4-2a is a two-dimensional vector plot at a
superficial gas velocity of 30 cm/s, solids loading of 9.1 % vol., and ambient pressure. It
is clear from the vector plot that there exists only one slurry recirculation cell in the timeaveraged sense, with slurry upflow in the center and downflow near the wall. The fully
developed flow extends axially between approximately 2D (0.32 m) and HD-D (1.63 m)
(2D < z < HD-D), where HD is the dynamic height and z is the total column height from
the distributor. From the plot, it is evident that everywhere in the column the time
averaged solids radial velocity is lower than the axial solids velocity. The highest upward
and downward axial velocities were found to be 140 and 135 cm/s. The highest value of
radial velocity was found be around 1.5 cm/s.
The axial and radial velocity components across the radius of the column are presented at
three axial locations, i.e., z = 2.5D, 5.5D, and 9D in Figure 4-2b and c. The averaged
velocity in these figures is averaged axially from z = 2D to HD D, which represents the
fully developed flow region. One can see that the solids axial velocities at all axial
locations are similar to the averaged velocity.
As mentioned earlier, this familiar
recirculation pattern has been observed earlier by many investigators: in bubble columns
(Franz, 1984; Devanathan, 1990; Degaleesan, 1997), in slurry bubble columns (Rados,
2003), and in liquid fluidized beds (Limtrakul, 1996). The inversion point where the
solids velocity becomes zero was found to be around a dimensionless radius (r/R =) 0.7
for all the studied experimental conditions. In CT studies, close inspection of the solids
holdup radial profile revealed two zones with different slopes. One region was from 0
r/R 0.6 0.7 and other was close to wall region and characterized by a larger slope. In
the core region (0 r/R 0.6 0.7) where the slope was relatively uniform, the solids are
moving up while in the higher slope region, as well as in high solids holdup region near
the wall, they move downward. Figure 4-3 shows the radial profiles of time- and
azimuthally- averaged axial, radial, and tangential solids velocities at these operating
conditions, with error bars. The error bars in these figures represent one standard
deviation from the averaged velocities along the axial coordinate at every radial location.
77
9
(b)
z/D
2
0
0.2 0.4 0.6 0.8

r/R
(a)
(c)
Figure 4-2: Time and azimuthally averaged solids velocity in air-Therminol LT-glass
beads system at Ug = 30 cm/s, P = 0.1 MPa, and solids loading = 9.1 % volume a) uz-ur
vector map, b) axial, and c) radial velocity components
(a)
(b)
(c)
Figure 4-3: Radial profile of solids a) axial, b) radial, and c) tangential velocity in airTherminol LT-glass beads system at Ug = 30 cm/s, P = 0.1 MPa, and solids loading = 9.1
% volume
78
Clearly, the radial and tangential solids velocities are much lower than axial velocities
indicating advectionless radial and tangential flow.
Figure 4-4 shows a PDF plot of the axial solids velocity at three different radial positions
(r/R = 0.063, 0.44, and 0.96) at an axial level of L/D = 2.5 at Ug = 30 cm/s, P = 0.1 MPa,
and a solids loading of 9.1 % vol. The alternating vortices appear to dominate the PDF of
solids axial velocity. As expected, the resultant solids axial velocity in the center is
positive, while near the wall, it is negative. Although the mean of the PDF in the center is
positive, it shows a few negative velocities. Figure 4-5 shows the PDF plot of solids axial
velocity at three different radial positions (r/R = 0.063, 0.44, 0.69, and 0.94) and at three
axial levels (L/D = 2.5, 5.5, and 9). Very small axial variation in PDFs was observed in
the studied region. As one moves from the column center to the column wall, the
contribution of negative velocities starts increasing. The mean of solids axial velocities at
r/R = 0.063, 0.44, and 0.69 are positive while at r/R = 0.94, it is negative. The negative
Figure 4-4: Probability distribution function of solids axial velocities at L/D = 2.5 at
various dimensional radius positions of r/R = 0.063, 0.44, and 0.96 at Ug = 30 cm/s, P =
0.1 MPa, and solids loading of 9.1 % volume.
solids velocities in the center are possibly due to downward moving small bubbles in the
wake of large bubbles. This fact can be corroborated based on the experimental studies
performed by Chen et al. (1994). Based on Particle Image Velocimetry (PIV), Chen et al.
(1994) showed that a significant number of small bubbles are trapped with large bubbles
moving in the center of the column. As seen from Figure 4.5, the presence of positive
79
L/D
p
d
f
Column Center
Axial solids velocity (cm/s)
Column Wall
Figure 4-5: Probability distribution function of solids axial velocities at L/D = 2.5, 5.5,
and 9 along the column radius at r/R = 0.063, 0.44, 0.69, and 0.96 at Ug = 30 cm/s, P =
0.1 MPa, and solids loading of 9.1 % volume.
and negative velocities at all the radial locations indicates high fluctuations and the
dynamic nature of flow in the column. In addition, it can be observed that at a radial
location of r/R = 0.69, the contribution of both positive and negative velocities is equal.
Such comparable positive and negative velocities can possibly generate larger, and
vigorous fluctuations in the vortical region.
Figure 4-6 shows the effect of pressure as well as solids loading on the PDF of solids
axial velocity. The comparison of 4-6 a and b shows the effect of operating pressure at a
superficial gas velocity of 30 cm/s and 9.1 % vol. solids loading, while comparison of
Figures 4-6 b and c show the effect of solids loading at a superficial gas velocity of 30
80
r/R = 0.063
r/R = 0.96
(a)
(b)
(c)
Figure 4-6: Probability distribution function of solids axial velocities in fully developed
flow in the column center and near the wall at a) 30 cm/s, 9.1 % vol., and 0.1 MPa, b) 30
cm/s, 9.1 % vol., and 1.0 MPa, and c) 30 cm/s, 25 % vol., and 1.0 MP in 6 diameter
cm/s and an operating pressure of 1 MPa. It can be observed that an increase in pressure
results in a narrow PDF, while increasing the mean of the PDF both in the center and at
the wall. An addition of solids broadens the PDF and decreases its magnitude. However,
the general qualitative behavior at all the studied operating conditions is similar. It shows
averaged positive velocity in the center, with few negative velocities, and the contribution
of negative velocities increases as one move towards the wall.
81
4.3.2 Turbulent stresses and kinetic energy
When a gas is bubbled through slurry, large scale eddies are created. The turbulent
interaction between these eddies can be characterized by studying the auto-/crosscorrelation of the fluctuating velocity components (Degaleesan, 1997). The second order
velocity correlations, ui' u 'j , represent the turbulent momentum transport along ith direction
due to the instantaneous flow in the jth direction. The turbulent stress tensors can be
defined by the following symmetric matrix in a cylindrical system,
ur' ur'
= s u' ur'
u z' ur'
ur' u'
u' u'
u z' u'
ur' u z'
u' u z' ,
u z' u z'
(4-1)
where, ui' u 'j = u 'j ui' .
The above tensor consists of following quantities,

Normal stress in the axial direction = s u z' u z'
(4-2a)
Normal stress in the radial direction = s ur' ur'
(4-2b)
Normal stress in the tangential direction = s u' u'
(4-2c)
' '
Shear stress = s ur u z
(4-2d)
The solids phase turbulence can also be characterized in terms of turbulent kinetic
energy, which is defined as
1
2
2
k = S [u ' r + u ' + u ' 2z ] .
2
(4-3)
There is considerable evidence that the time averaged turbulence in bubble columns is
not isotropic (Franz et al., 1984; Chen et al., 1994; Degaleesan, 1997; Mudde et al.,
1997). The normal stresses in the axial direction are much larger than in the radial and
82
tangential direction. Hence, the characteristic length scale in the axial direction is
significantly larger than in the other two directions.
Figure 4-6a, b, c, d shows the radial profile of the solids turbulent kinetic energy, and of
the axial, radial, and tangential normal stresses at Ug = 30 cm/s and P = 0.1 MPa at a
solids loading of 9.1 % vol. using the air-Therminol LT-glass beads system. It is evident
that as in bubble column reactors, the solids axial normal stress is much higher in
magnitude than the radial and tangential normal stresses. Hence, it is not quite surprising
that the radial profile of the solids turbulent kinetic energy follows the behavior of the
solids axial normal stress.
(a)
(c)
(b)
(d)
Figure 4-7: Radial profile of solids a) turbulent kinetic energy, and b) axial, b) radial, and
c) tangential normal stresses in air-Therminol LT-glass beads system Ug = 30 cm/s, P =
0.1 MPa, and solids loading = 9.1 % volume.
Compared to the axial normal stress, the radial and tangential normal stresses are uniform
along the column radius. The magnitude of the radial and tangential stresses is
83
approximately 1/3rd of the axial normal stress. Although the axial velocities are higher in
the center, the axial normal stress shows a peak closer to the vortical region. Based on
Figure 4-5, it is clear that in the vortical region, both positive and negative velocities are
comparable. Hence the flow dynamically changes from upward to downward in this
region, based on the location of the central large bubble stream and its swirling motion.
The flow in this region, therefore, experiences larger and more vigorous fluctuations
leading to a peak in axial normal stress closer to the vortical region rather than in the
center, where flow is mostly upward.
The nature of the turbulence developed in a bubble column can be deduced from the
nature of these normal stresses. An isotropic turbulence, frequently used in modeling
such flows, does not exist in a slurry bubble column as the normal stresses in three
directions are of different magnitudes.
Figure 4-8a, b, c shows the radial profile of the solids shear stresses in an air-Therminol
LT-glass beads system at Ug = 30 cm/s, P = 0.1 MPa, and a solids loading of 9.1 % vol.
It is evident that the shear stresses are less than the normal stresses. A similar
phenomenon was observed in bubble columns, where the magnitude of the liquid shear
stress is much lower than that of normal stresses (Degaleesan, 1997; Ong 2003). This
implies that the cross-correlations (shear stresses) between the solids velocities are not as
strong as the auto-correlations (normal stresses). Between various shear stresses, the
value of rz is the most significant, hence will be used in further analysis. The radial
profile of rz shows the minimum value in the center and near the wall. It exhibits a
maximum value at r/R = 0.4 - 0.6. The peak in shear stress can be related to the inversion
point in the axial solids velocity near this region. In addition, the radial profile of
normalized solids holdup shows a change in its slope in this region as shown in
Appendix-B.
In the following analysis, only the axial normal stress and the shear stress in the axial and
radial directions are presented, since they are frequently used in the modeling of slurry
bubble columns. The effect of operating parameters on axial and radial eddy diffusivities
84
is provided in Appendix-C. The data pertinent to study the effect of operating parameters
is presented here, and the remaining data is provided in Appendix-C.
Now the effect of various operating parameters on the radial profiles of solids velocities
and of turbulent parameters will be studied.
rz
(a)
r
(b)
(c)
Figure 4-8: Radial profiles of solids shear stress components in an air-Therminol LTglass beads system Ug = 30 cm/s, P = 0.1 MPa, and solids loading = 9.1 % volume
4.3.3
Effect of liquid phase physical properties on the solids axial velocity and
turbulent parameters
Figure 4-9 compares the solids axial velocity and turbulent parameters in an airTherminol LT-glass beads and air-water-glass beads system at a superficial gas velocity
of 30 cm/s, ambient pressure, and a solids loading of 9.1 % vol. Due to low surface
tension and viscosity, the gas holdup radial profile in air-Therminol LT-glass beads is
higher than that of the air-water-glass beads system. The higher gas holdup radial profile
results in a higher solids axial velocity in the air-Therminol LT-glass beads system. The
center line velocity, as well as negative wall velocity, are higher in Therminol LT than in
water. Although, the solids axial velocity is higher in the air-Therminol LT-glass beads
system, the turbulent kinetic energy and normal stresses were found to be lower than
those of the air-water-glass beads system. The combination of low surface tension and
viscosity in the Therminol LT system generates more small bubbles that impart a low
level of fluctuations to the solids phase and result in the lower TKE and normal stresses.
On the other hand, due to higher radial gradient of solids axial velocity, the shear stresses
are higher in the air-Therminol LT-glass beads system. The change in physical properties
85
of the liquid phase does not alter the location of the inversion point and maximum in
shear stress. Figure 4-10 shows the effect of change in liquid phase at a superficial gas
velocity of 30 cm/s, P = 1 MPa, and solids loading of 9.1 % vol. From the CT studies it is
known that, at a high operating pressure, the gas holdup profiles are higher in Therminol
LT. Such higher gas holdup profiles give rise to a higher solids axial velocity profile in
Therminol LT, even at high operating pressure. As with ambient pressure in Therminol
LT, the TKE is lower while the solids shear stress is higher.
With the change in operating pressure from 0.1 to 1 MPa, the centerline velocity
increased by 50 % in the water system, while it increased by 35 % in the Therminol LT
system. One should note here that a similar change in pressure resulted in 34 and 28 %
increase in overall gas holdup in water and Therminol LT, respectively. The comparison
between water and Therminol LT at ambient and high pressure shows that at ambient
pressure the center-line velocity is higher in Therminol LT by 33 %, ande at 1 MPa, it is
higher by 19 %. The change in center-line velocity between water and Therminol LT
appears to be higher at ambient pressure. It should be recalled here that the change in
liquid phase at ambient pressure increased overall gas holdup in Therminol LT by 19 %,
while at high pressure, it increased by 12 %. Thus the behavior of the solids velocity is in
accordance with the behavior of the gas holdup and its radial profile.
The change in liquid phase, i.e. physical properties does not appear to have any effect on
the location of the inversion point and maximum in shear stress. These two systems show
only quantitative differences in solids axial velocity and turbulent parameters. The
qualitative flow behavior in these systems remains the same indicating the same,
hydrodynamics in the two systems, differing only in magnitude due to the change in
86
(a)
(b)
(c)
(d)
Figure 4-9: Comparison of radial profile of a) gas holdup, b) solids axial velocity c)
solids TKE, and d) solids shear stress in air-waterglass beads and air-Therminol LTglass beads system at Ug = 30 cm/s, P = 0.1 MPa, and solids loading of 9.1 % vol.
The comparison of solids axial velocity profiles in Therminol LT in Figure 4-9 and
Figure 4-10 also shows the effect of operating pressure on solids axial velocity and
turbulent parameters at Ug = 30 cm/s and solids loading of 9.1 % vol. An increase in
operating pressure at the same superficial gas velocity results in an increased magnitude
of the gas holdup profile. Because the gas holdup profile drives the solids circulation in
slurry columns, higher pressure results in higher solids axial velocity due to increased gas
holdup. The reason for this behavior can be rationalized by drawing an analogy to bubble
dynamics studies performed in a two-phase bubble column. Xue (2004) developed a fourpoint optical probe for bubble velocity, bubble size, and interfacial area measurement in
bubble columns. The experiments were conducted in an air-water system at atmospheric
87
0.7
100
P = 1 MPa
0.6
Solids axial velocity (cm/s)
Gas holdup (-)
0.5
0.4
0.3
0.2
0.1
80
60
40
20
0
-20
-40
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
0.8
0.9
-60
0.2
0.4
0.6
0.8
(a)
(b)
3500
400
3000
300
2000
Trz (cm /s )
TKE (cm /s )
2500
1500
200
1000
100
500
0.2
0.4
0.6
0.8
0.2
0.4
0.6
0.8
(c)
(d)
Figure 4-10: Comparison of radial profile of a) gas holdup, b) solids axial velocity c)
solids TKE, and d) solids shear stress in air-water-glass beads and air-Therminol LTglass beads system at Ug = 30 cm/s, P = 1 MPa, and solids loading of 9.1 % vol.
and high pressure (0.4 and 1 MPa). It was observed that in the center the percentage of
bubbles moving downwards was reduced, while near the wall the percentage of bubbles
moving downwards increased greatly. Xue (2004) also noticed that in the center the mean
velocity of bubbles moving upwards increased, while downward movement was
enhanced near the wall due to an increase in negative velocity of the downward moving
bubbles. In addition, Xue (2004) observed that the bubble frequency increases greatly
with an increase in operating pressure. This results in higher solids/slurry recirculation
with an enhancement in pressure, as the solids/ slurry moves along with the bubbles. An
increase in pressure from 0.1 to 1 MPa at Ug = 30 cm/s increased the gas holdup by 27
%, and the centerline velocity increases from 60 to 90 cm/s, almost by 34 % while at
88
superficial gas velocity of 20 cm/s, gas holdup and centerline velocity increased by 30
and 35 %. At higher pressure, the negative velocity also increased from 28 to 35 cm/s
at Ug = 30 cm/s and from -23 to -27 cm/s at Ug = 20 cm/s, thereby increasing the
recirculation in the system. The effect of operating pressure at the remaining superficial
gas velocities is shown in Appendix-C.
The effect of pressure observed in this study is in line with previous studies in bubble
columns (Ong, 2003) and slurry bubble columns (Rados, 2003). However, Lee et al.
(2001) performed Laser Doppler Velocimetry (LDV) studies using nitrogen-water and
nitrogen-Paratherm NF and found that an increase in pressure resulted in reduced liquid
axial velocity. It is worth mentioning here that the experimental conditions of Lee et al.
(2001) appear to be in the bubbly flow regime (particularly at high pressure), while those
of Ong (2003) and Rados (2003) were in the churn-turbulent flow regime, similar to the
current study.
Although operating pressure increased solids axial velocity, the effect of pressure on
TKE was the opposite. It showed reduced turbulence in the system at higher operating
pressure. An increase in operating pressure increased the gas density and destabilized the
large bubbles. The maximum stable bubble size was reduced with an increase operating
pressure (Wilikinson, 1991; Lin et al., 1998; Xue, 2005). The high pressure resulted in a
narrow bubble size distribution with a smaller mean bubble size. Although at elevated
pressure the gas phase momentum is higher, due to the small mean bubble size, the
fluctuations of the solids/slurry phase are dampened out. As the population of the large
bubbles decreased with pressure, it results in relatively reduced swirling motion caused
by such structures. The lower intensity of fluctuations of smaller bubbles therefore leads
to a lower level of turbulence at high pressure. An increase in pressure reduces TKE by
close to 20 % at 20 and 30 cm/s.
The effect of pressure on the radial-axial shear stress is similar to its effect on the solids
axial velocity. An increase in operating pressure increases the shear stress due to the
89
higher radial gradient of solids axial velocity. The shear stress increased by 19 and 22 %
with an increase in pressure from 0.1 to 1 MPa at Ug = 20 and 30 cm/s, respectively.
4.3.4
Effect of solids loading on solids axial velocity and turbulent parameters
The effect of solids loading on the solids axial velocity and turbulence parameter at
ambient pressure in the air-Therminol LT-glass beads system at superficial gas velocities
of 20 and 30 cm/s is shown in Figures 4-11 and 4-12. The addition of solids reduced the
gas holdup and hence solids axial velocity. The reduction of gas holdup radial profile at
higher solids loading is translated into the lower solids axial velocity profile. An increase
in solids loading reduces centerline as well as negative velocity near the wall. The
centerline velocity decreased by 16 and 14 % at Ug = 20 and 30 cm/s, respectively. The
negative velocities changed from -27 to -21 cm/s at Ug = 30 cm/s, while at Ug = 20 cm/s,
it changed from -22 to -18 cm/s at ambient pressure.
(a)
(c)
(b)
(d)
Figure 4-11: Effect of solids loading on the radial profile of solids a) axial velocity, b)
turbulent kinetic energy, c) axial normal stress, and d) shear stress in air-Therminol LTglass beads system at Ug = 20 cm/s and P = 0.1 MPa.
90
3500
70
Vs = 9.1 % vol
Vs = 25 % vol
60
Vs = 9.1 % vol
Vs = 25 % vol
3000
40
2500
30
TKE (cm /s )
20
50
10
0
-10
2000
1500
1000
-20
500
-30
-40
0.2
0.4
0.6
0.8
0.2
0.4
0.6
(a)
400
Vs = 9.1 % vol
data2
Vs = 9.1 % vol
Vs = 25 % vol
350
3000
300
250
Trz (cm /s )
(b)
4000
Axial normal stress (cm /s )
0.8
2000
1000
200
150
100
50
0.2
0.4
0.6
0.8
0.2
0.4
0.6
0.8
(c)
(d)
turbulent kinetic energy, c) axial normal stress, and d) shear stress in air-Therminol LTglass beads system at Ug = 30 cm/s, and P = 0.1 MPa
Figures 4-13 and 4-14 illustrate the effect of solids loading on the solids axial velocity
and turbulence parameters in the air-Therminol LT-glass beads system at high pressure
and superficial gas velocities of 20 and 30 cm/s, respectively. The addition of solids at
high pressure resulted in a decrease in gas holdup and subsequently in the solids axial
velocity and its profile. The addition of solids at higher pressure decreased gas holdup by
close to 30 %, while the centerline velocity decreased by 13 and 10 % at Ug = 20 and 30
cm/s.
91
(a)
(c )
(b)
(d)
turbulent kinetic energy, c) axial normal stress, and d) shear stress in air-Therminol LTglass beads system at Ug = 20 cm/s and P = 1 MPa
At both ambient and high pressure, the addition of solids resulted in an increase in TKE
and axial normal stress. At superficial gas velocities of 20 and 30 cm/s, the addition of
solids increased TKE by 22 and 18 % at ambient pressure, and by 20 and 15 % at P = 1
MPa, respectively. The addition of solids increased the pseudo-viscosity of the slurry,
thereby results in a stable interface that promoted coalescence and reduced bubble
breakup. The combination of these phenomena generated more large bubbles. Based on a
2- point optical probe, Lau (2003) also observed that an addition of particles led to
significantly larger bubble sizes in the system. Based on PIV studies, Chen et al. (1994)
92
showed that the large bubbles that accumulate at the center move in a rocking spiral
manner in the churn- turbulent flow regime. Hence the fluctuations of the solid/slurry
100
3000
Vs = 9.1 % vol
Vs = 25 % vol
Vs = 9.1 % vol
Vs = 25 % vol
60
2000
TKE (cm /s )
40
80
20
1000
-20
-40
0.2
0.4
0.6
0.8
0.2
0.4
(a)
450
Vs = 9.1 % vol
Vs = 25 % vol
Vs = 9.1 % vol
Vs = 25 % vol
400
3000
350
0.8
(b)
4000
0.6
Trz (cm /s )
300
2000
250
200
150
1000
100
50
0
0.2
0.4
0.6
0.8
0.2
0.4
0.6
0.8
(c )
(d)
Figure 4-14: Effect of solids loading on radial profile of solids a) axial velocity, b)
turbulent kinetic energy, c) axial normal stress, and d) shear stress in air-Therminol LTglass beads system at Ug = 30 cm/s, and P = 1 MPa
phase induced by gas phase become higher at increased solids loading due to the higher
large bubble population. The observation of increased turbulence at higher solids loading
is in line with the recent findings by Cui and Fan (2005). Their studies were performed in
a 2-D column using low solids loading (4 % vol.) at superficial gas velocities ranging
from 0.025 to 7.5 cm/s, covering bubbly and churn-turbulent flow. In general, Cui and
Fan (2005) observed enhancement in turbulence with an addition of particles, however
the effect of solids loading on the turbulence was found to be function of the solids
properties and the operating flow regime.
93
As shear stress is a radial gradient of the solids axial velocity, an addition of solids results
in reduction in the radial gradient of axial velocity; hence, axial-radial shear stress is
reduced at high solids loading. The reduction of shear stress at ambient pressure is 15 %,
while, at high pressure it is close to 12 %.
In Chapter 3, it was observed that pressure affects overall gas holdup more at high solids
loading, while solids loading affects overall gas holdup relatively more at low pressure. A
similar trend in the effect of the combination of solids loading and operating pressure was
observed on the solids axial velocity and turbulent parameters.
4.3.5 Cross-sectional averaged turbulent stresses
The values of the cross-sectional average of the turbulent stresses were obtained from
CARPT data. The effects of the studied parameters on the cross-sectional average of the
turbulent stresses are provided in Appendix-C.
4.3.6 Turbulent eddy viscosity
In this section, turbulent eddy viscosity, which signifies the turbulent transfer of
momentum by eddies giving rise to an internal fluid friction, is calculated from the
CARPT experimental data. Next the turbulent eddy viscosity is predicted using the
approach proposed by Ohnuki and Akimoto (2001) in gas-liquid systems and is compared
with the experimental values. In the next section, the available correlations for turbulent
viscosity are presented. The predictions of these correlations are also compared with the
ones obtained from CARPT data. The details are provided in Appendix-C.
4.3.7 Eddy diffusivities
In this section, eddy diffusivity, which is the exchange coefficient for the diffusion of a
conservative property by eddies in a turbulent flow, is calculated, and the effects of the
94
liquid phase physical properties and solids loading are discussed. The details of this part
are provided in Appendix-C.
4.4 Remarks
The significant findings of this part are as follows:
1) As found in air-water and air-water-glass beads systems, this work also exhibits a
single circulation cell in fully developed flow in a time-averaged sense. The solids
move upward at the center and downward near the wall. The pdf of the solids
axial velocity reveals that although the net flow in the center is upward, there are
few negative velocities, net flow near the wall is downward, and there are few
positive velocities. Near the vortical region, comparable positive and negative
velocities are present, causing vigorous fluctuations. The axial solids velocity
shows an inversion point around a dimensionless radius of 0.7 while shear stress
shows maximum in the center of the column radius.
2) Comparison with an air-water-glass beads systems shows an increased solids axial
velocity and shear stresses in the air-Therminol LT-glass beads system. However,
due to the presence of smaller bubbles in the air-Therminol LT-glass beads, it
shows less TKE and normal stresses. The qualitative flow behavior in both
systems is similar; the quantitative differences exist due to differences in physical
properties.
3) An addition of solids reduces the solids axial velocity and shear stress, due to a
decrease in gas holdup, while TKE and normal stresses are higher at high solids
loading, due to an increased large bubble population.
4) The effect of superficial gas velocity is not as strong as the effect of operating
pressure. The operating pressure has a significant effect at high solids loading,
while the solids loading exhibits more effect at ambient conditions.
95
Chapter 5.
Flow Regime Transition
As discussed in Chapter 2, for lab scale and industrial scale reactors, there is a need to
develop a technique for flow regime diagnosis that is noninvasive, that can be easily
implemented on an industrial scale without disturbing the operation, and that provides
reliable information regarding the prevailing flow regime. The primary objective of this
chapter is to develop and demonstrate a non-invasive technique for online flow regime
demarcation and its corresponding flow regime identifiers. The developed technique
will then be utilized to study the effect of operating parameters on flow regime transition.
Stitt et al. (2003) summarized various tomographic systems and concluded that -ray
based techniques meet all essential requirements for field use. For this purpose, the
available non-invasive techniques, such as -ray CT and Nuclear Gauge Densitometry
(NGD), were evaluated for flow regime identification. This chapter is divided into two
parts. The first part evaluates CT for flow regime demarcation, while the second part
deals with the more robust NGD.
5.1 Flow Regime Transition using CT

Darwood et al. (2003) discussed in detail the commercial practicability of -ray CT
system as a process diagnostic tool. They developed a proprietary method to deliver an
economic, portable, and commercial product that can measure tomograms of equipment
at manufacturing sites.
Based on this development, in the first part of this work the following tasks were focused
on:
i)
Explore the potential of CT for delineation of hydrodynamic flow regime
ii)
Develop flow regime identifiers for CT
iii)
Study the effect of operating pressure on flow regime transition
96
As we know, single source -ray CT has been used for phase holdup reconstruction in two
phase systems. Based on the published studies on gas holdup radial profiles, it is well
known that the homogeneous regime is characterized by a close to flat holdup profile,
while the heterogeneous regime has a parabolic profile. Therefore, the actual measurement
of either the holdup profiles or/and the liquid flow pattern across the column should
conclusively indicate the prevailing flow regime (Joshi et al., 1998).
5.1.1 Experimental setup and conditions
The details of the experimental setup and CT used in this part of the work were given in
Chapter 3. Air was used as a gas phase, while Therminol LT was the liquid phase. The
obtained experimental data was processed using the EM algorithm implemented by Kumar
(1994). As mentioned earlier, the available studies show that the shape of gas holdup radial
profiles is different in both regimes. Therefore, based on the obtained results, the parameter
that defines the shape of the gas holdup radial profile will be studied for identification of
flow regime transition. The behavior of such a parameter will be explored in the context of
the knowledge of flow regime transition obtained from the gas holdup curve and Drift Flux
plot, based on the cross-sectional averaged gas holdup calculated from the obtained radial
profiles. Systematic experiments were performed where the superficial gas velocities were
varied from 1 to 20 cm/s with an interval of 1 cm/s and at 30 cm/s. The operating pressures
were 0.1, 0.4, and 1 MPa.
5.1.2 Results and Discussion

Figure 5-1 shows the plot of the gas holdup radial profile at superficial gas velocities
ranging from 1 to 20 and 30 cm/s with an interval of 1 cm/s, at ambient conditions using an
air-Therminol LT system. With an increase in superficial gas velocity, the magnitude of the
gas holdup profile increases. In addition, one can observe that an increase in superficial gas
velocity results in a change in the shape of the gas holdup radial profile, from flatter at low
superficial gas velocities to steeper, i.e. parabolic, at high superficial gas velocities.
Particularly, there is a distinct change in the shape of the gas holdup radial profile around
97
superficial gas velocities of 6 7 cm/s. To evaluate whether this is due to change in the
flow regime, the evolution of the cross-sectional averaged gas holdup with superficial gas
velocity was assessed.
Figure 5-1: Gas holdup radial profile at various superficial gas velocities in an airTherminol LT system at ambient conditions in a 0.162 m steel column.
Once the gas holdup radial profile was obtained by azimuthally averaging the crosssectional gas holdup distribution, the cross-sectional averaged gas holdup was then
estimated as follows,
G = 2 G ( )d ,
(5-1)
where = r/R.
The fact that bubbly and churn-turbulent flow exhibit different slopes in the gas holdup
curve will be utilized to identify the transition point. The commonly used drift flux
method proposed by Wallis was also used to determine the regime transition point. The
drift flux can be written as (Wallis, 1969)
jGL = U G (1 G ) U L G ,
(5-2)
98
where the positive or negative sign indicates counter-current or co-current flow of liquid
relative to the gas phase, respectively. The change in the slope of the drift flux curve (jGL
v/s G) represents the transition from homogeneous to heterogeneous flow. The change in
slope in the drift flux plot is generally sharper than the change in slope in the gas holdup
curve.
For the batch liquid, equation (5-2) will become
jGL = U G (1 G ) .
(5-2a)
Figure 5-2a shows the evolution of the cross-sectional averaged gas holdup with superficial
gas velocity in an air-Therminol LT system at ambient conditions. The gas holdup curve
shows a change in slope around superficial gas velocities of 6 7 cm/s, indicating a regime
transition point.
In addition, the drift flux based on the cross-sectional gas holdup was plotted and is shown
in Figure 5-2b. The drift flux was calculated from equation (5-2a). The drift flux plot also
shows a sharp change in slope around 6 7 cm/s, confirming the regime transition point
around these velocities.
The shape of the obtained gas holdup radial profile data was analyzed further to identify the
flow regime transition. From traditional analysis (gas holdup curve and drift flux plot), it is
clear that regime transition occurs around 6 7 cm/s. This is consistent with Figure 5-1,
which shows a noticeable change in the shape of the profile around superficial gas
velocities of 6 7 cm/s. Therefore, the shape parameter of the profile and its evolution over
the studied superficial gas velocities can reveal information regarding the flow regime
transition.
To include the possibility of finite gas holdup close to the wall, Luo and Svendsen (1991)
modified the proposed form of Nassos and Bankoff (1967) for the gas holdup radial profile
as follows:
99
=(
r
n+2
)[1 c( ) n ] ,
R
n + 2 2c
(5-3)
where G is the cross-sectional averaged gas holdup and r/R is the dimensionless radial
position. The exponent n is a parameter that indicates the steepness of the gas holdup radial
profile. The value of n is large for a flat profile (as observed in bubbly flow) and
(a)
(b)
Figure 5-2: a) Cross-sectional averaged gas holdup versus superficial gas velocity and b)
Drift flux plot based on cross-sectional averaged gas holdup in an air-Therminol LT
system at ambient conditions in a 0.162 m steel column.
small for a steep profile (as observed in churn-turbulent flow). In the above equation, the
parameter c indicates the value of gas holdup near the wall. If c = 1, there is zero holdup
close to the wall, while for c = 0, the holdup is constant with changing r/R.
The obtained gas holdup radial profile has been fitted to the equation proposed by Luo and
Svendsen (1991) to calculate the steepness parameter. Figure 5-3 shows the evolution of
the steepness parameter, n, against superficial gas velocity. A break-point in the steepness
parameter curve has been observed around 6 7 cm/s, which matches with the one
obtained in the drift flux plot. Hence, the break-point in the steepness parameter curve
100
Figure 5-3: Evolution of steepness parameter with superficial gas velocity in an airTherminol LT system at ambient conditions in a 0.162 m steel column.
can be utilized as the regime transition identifier. Using this identifier, the effect of
operating pressure on the flow regime transition was further studied.
Figures 5-4a and b show the gas holdup radial profile at superficial gas velocities of 1 to 20
cm/s, with an interval of 1 cm/s, and at 30 cm/s in an air-Therminol LT system at operating
(a)
(b)
Figure 5-4: Gas holdup radial profile at various superficial gas velocities in an airTherminol LT system at operating pressure of 0.4 MPa in a 0.162 m steel column.
101
pressures of 0.4 and 1 MPa, respectively. The behavior of the profiles is similar to that at
ambient conditions, but the shape of the profiles is much flatter than at the ambient
conditions, which is consistent with the earlier literature findings (Kemoun et al., 2001;
Ong, 2003). This flatter profile is due to an increase in breakup rate and a decrease in the
coalescence rate at higher pressure. The distinct change in the shape of the profile observed
at ambient conditions was not observed at higher pressures. From the obtained gas holdup
radial profiles, cross-sectional gas holdups were estimated from equation 5-1. The gas
holdup curve and drift flux plot based on the estimated cross-sectional gas holdups are
shown in Figures 5-5a and b for an operating pressure of 0.4 MPa, while Figures 5-6a and b
show the gas holdup curve and drift flux plot at operating pressure of 1 MPa. The change of
slope in the gas holdup curve and drift flux starts at 7 cm/s for an operating pressure of 0.4
MPa, and at 9 cm/s for 1 MPa. To quantify the observed phenomena based on the obtained
gas holdup radial profiles, the steepness parameter n was plotted against superficial gas
velocities at operating pressures of 0.4 and 1 MPa (Figure 5-7). A gradual change, contrary
0.5
20
0.3
Drift-flux, j
0.4
0.2
10
0.1
10
20
30
(a)
0.2
0.4
(b)
Figure 5-5: a) Gas holdup curve based on cross-sectional averaged gas holdup and b)
Flux plot based on cross-sectional averaged gas holdup in an air-Therminol LT system at
operating pressure of 0.4 MPa in a 0.162 m steel column.
0.6
15
0.4
10
Drift-flux, j
102
0.2
10
20
30
(a)
0.2
0.4
(b)
Figure 5-6: a) Gas holdup curve based on cross-sectional averaged gas holdup and b) Flux
plot based on cross-sectional averaged gas holdup in an air-Therminol LT system at
operating pressure of 1.0 MPa in a 0.162 m steel column.
to the distinct one observed at ambient conditions, was observed in the steepness parameter
curve at increased pressure. Figure 5-7 shows that at an operating pressure of 0.4 MPa, a
noticeable change in the steepness parameter occurs at a superficial gas velocity of 7 8
cm/s. Also, at 1 MPa the change in the steepness parameter can be observed around 8 9
cm/s. Such a noticeable change in the steepness parameter curve has been observed at a
velocity similar to the transition velocity point obtained from the gas holdup curve and drift
flux plot based on cross-sectional gas holdup, thereby confirming the utilization of the
break-point in the steepness parameter for regime transition identification. In addition,
one can observe that, at increased pressure, the change in the steepness parameter near the
break-point is gradual, rather than distinct as observed at atmospheric pressure. In
general, the steepness parameter, n, decreases with an increase in superficial gas velocity
and reaches a constant value close to 2.
At atmospheric pressure, the change in the steepness parameter that starts at a superficial
gas velocity of 6 cm/s becomes smaller around 8 cm/s. At 0.4 MPa, the change in the
steepness parameter starts around 7 cm/s and extends up to 11 cm/s, while at 1 MPa, such
a change starts around 8 cm/s and extends up to 13 cm/s. In general, the break-point in
steepness parameter curve, which is similar to the transition velocity, increases with an
103
increase in operating pressure. Although the change in the steepness parameter curve is
sudden at ambient conditions, it extends over the region of superficial gas velocities at
Figure 5-7: Evolution of steepness parameter with superficial gas velocity in an airTherminol LT system at operating pressures of 0.4 and 1 MPa in a 0.162 m steel column.
higher pressures. The extension of such a zone depends upon the operating pressure, and it
increases with an increase in pressure. Based on Deterministic Chaos Analysis of pressure
fluctuations, Letzel et al. (1997) found a sharp dip in Kolomogorov entropy at the transition
point, while at higher pressure, such a dip has not been observed. They observed a region
of low Kolomogorov entropy at higher pressure, and the length of the region increased with
an increase in pressure, similar to the observations made in this work. The increased
pressure delays the formation of larger bubbles and thereby postpones the break-point
velocity. The presence of an extended transition zone at higher pressure has been linked to
the appearance of swirl and large bubbles at different superficial gas velocities, whereas
at atmospheric pressure these two phenomena coincide (van den Bleek et al., 2002).
5.1.3 Evaluation of the empirical correlations
In the literature, the following two correlations have been utilized to predict transition
velocity,:
104
i) Wilkinson (1991)
Wilkinson (1991) developed a model for gas holdup prediction that is similar to but slightly
different from the one proposed by Krishna et al. (1991). They incorporated their own
experimental data along with the literature data in their model and proposed the following
correlation for prediction of regime transition velocity.
U s ,b L
3 L 0.273 L 0.03
= 2.23[
]
[ ]
G
g L4
U trans
= trans = 0.5 exp( 193 G0.61 L0.5 0.11 )
U s ,b
(5-4)
(5-5)
ii) Reilly et al. (1994)

Reilly et al. conducted experiments in 15 cm diameter column using water and nonaqueous liquids. They used helium, nitrogen, air, argon and CO2 to study the effect of gas
density on regime transition. Using their own experimental data, they proposed the
following correlation based on the change in gas phase momentum,
trans = 0.59( B)1.5 [ G0.96 0.12 / L ]0.5

U trans =
1
1
0.12 trans (1 trans )
0.04
2.84 G
(5-6)
(5-7)
where B = 3.85.
Table 5-1 shows the predicted transition velocities using the above correlations in
comparison with the experimental transition velocities at various operating pressures.
Quite surprisingly, both correlations show maximum relative error at atmospheric
pressure. Within the studied range of operating conditions, Wilkinson (1991) correlation
105
tends to underpredict the transition velocities compared to the correlation of Reilly et al.
(1991). The average relative errors using the correlations of Wilkinson and Reilly et al.
are 70 and 49 %, respectively. Clearly, the state of prediction of flow regime transition
velocities based on the correlations needs to be further improved.
Table 5-1: Comparison of experimental and predicted transition velocities from the
available correlations in an air-Therminol LT system at various operating pressures.
Operating
Pressure
(MPa)
Experimental
Wilkinson (1991)
Utrans
Utrans(cm/s) % Relative
(cm/s)
Error
0.1
0.4
1
6-7
7 - 11
9 - 14
0.4
2.4
4.3
93
66
52
Reilly et al. (1994)

Utrans(cm/s)
% Relative
Error
2.5
4
4.8
58
43
47
5.2 Flow Regime Transition using Nuclear Gauge Densitometry (NGD)

The objective of this part of the chapter is to develop NGD for demarcation of
hydrodynamic flow regimes in bubble column reactors. The -ray CT was first attempted
because it provides a detailed time averaged cross-sectional distribution of underlying
hydrodynamics. However, NGD appeared to be more robust from an experimental point
of view, both on the laboratory as well as the industrial scale. Of particular industrial
interest is the fact that NGD can be implemented without disturbing the running
operation. Also, it is being currently used in industry for liquid/slurry level monitoring
and control.
Based on this development, this part of the work focused on the following tasks:
i)
Explore the potential of NGD for demarcation of hydrodynamic flow regime
ii)
Propose flow regime identifiers for NGD
iii)
Evaluate the applicability of the proposed identifiers in different systems and at

high operating pressure.
106
5.2.1 Nuclear Gauge Densitometry (NGD)
Nuclear gauge densitometry (NGD) consists of a sealed source in a source holder and a
scintillation detector in front of the source. The source holder is mounted on one side of a
column, with the detector on the opposite side. A focused beam of radiation is transmitted
from the source, through the column and process material, to the detector. As the density
of the material in the column changes, the amount of radiation reaching the detector
changes. It is generally believed that the amount of radiation that reaches the detector
through the process material is reflective of its flow behavior and properties. Figure 5-8
shows the schematics of NGD with a source and a detector in front of it.
NGD is used extensively in industry for such applications as level control, density
measurement, interface identification, and weight measurements in conveyors. It is
widely used in the following industries: chemicals, petrochemicals, off shore oil and gas,
pharmaceuticals, cement, quarrying, solids handling, paper and food. The major
advantages of NGD that make it attractive in everyday industrial use are
(www.vegacontrols.com),
i)
Totally non-contact: Because the sources and detectors are mounted externally
from the column or process, they are completely unaffected by the conditions
inside, however extreme, providing reliable solutions when other technologies
fail. They can be easily accessed, installed or removed without the process
being affected or interrupted.
ii)
High integrity: A non-invasive system mounted outside the vessel means no

exposure or wear by corrosive or abrasive products, and no need for
construction to resist high pressure, high temperature process conditions. This
means less risk of leaks or emissions, protecting processes, people and the
environment.
iii)
High reliability and low maintenance: NGD measurements offer reliability

and long term performance. In addition, source checking is routine, simple
and can be planned well in advance.
107
iv)
Low installation costs: NGD can often be installed and commissioned without
process shutdown. Also, on most applications, no alterations to the
reactors/columns are needed, which means no expensive design changes for
such implementation of NGD.
5.2.1a Experimental Setup
The experimental setup consists of a laboratory scale plexi-glass column (diameter = a

0.1012 m, height = 1.2 m) as shown in Figure 5-8. Air from the in-house utility line was
fed through a sparger located at the bottom of the column. The gas flow rate was
measured and adjusted by a rotameter (Dwyer Intruments Inc., model Rate Master). The
sparger used in this study consists of 64 holes of 0.052 diameter with an open area (%
OA) of 1.09. This sparger is equivalent to the one used in the 6 stainless steel column
for slurry bubble column hydrodynamics experiments. The equivalent sparger was
designed such that the hole size and % OA remain the same in the two spargers, therefore
the number of holes differ in these spargers. In this study, an existing CT setup was
converted to NGD (Figure 5-8) by placing a detector in front of an encapsulated -ray Cs137 source (~ 100 mCi). The source and detector were mounted on a plate that can move
in axial direction. The detector consists of a cylindrical 2 2 inch NaI crystal, a photo
multiplicator (PM), and electronics, forming a 0.054 0.26 m cylindrical assembly. The
collimator (1/16 X 3/16) was placed in front of the detector. The photon count rate that
was converted from the output voltage was collected through an automated data
acquisition system. The superficial gas velocity was varied from 1 to 12 cm/s, with an
interval of 0.5 cm/s, near the transition region. Air was used as the gas phase, while water
( = 1 cP, = 998 kg.m-3, = 72 dyne.cm-1) was the liquid phase.
108
35
-ray Source
0.62
Detector
35
35
3.6
"
Figure 5-8: Experimental setup for Nuclear Gauge Densitometry (NGD)
Drahos et al. (1991) systematically examined the effect of various operating parameters
on axial and radial profiles of the basic characteristics of pressure fluctuations. The signal
measured in the bubble column is a complex function of the effects connected with
formation, coalescence and passage of bubbles and their mutual interactions with the
liquid phase eddies of various scales. Based on the cross-spectral studies, they showed
that the characteristic frequencies are different, depending on the source as shown in
Table 5-2. Drahos et al. (1991) found that the interesting frequencies range from 0 to 20
109
Hz for bubble columns. Hence, the photon counts history was obtained at an acquisition
frequency of 50 Hz. In order to minimize statistical error in the various time-series
analysis, a time-series with a total number of points, N = 15,000, was collected (Smith,
1999, van Ommen, 2001). This requires a total acquisition time of 5 minutes. To check
the consistency of the obtained data, the experiments were repeated three times.
Table 5-2: Characteristic frequencies in bubble column (Drahos et al., 1991)
Source
Order of characteristic frequencies (Hz)
Formation of bubbles
> 101
Passage of bubbles
100 101
Coalescence of bubbles
100
Large-scale eddies
10-1
Medium-size eddies
100
Liquid level fluctuations
10-2 10-1
5.2.2 Results and Discussion

5.2.2a Traditional analysis of flow regime transition
The flow regimes were first defined using traditional methods such as the change in the
slope of the gas holdup curve and the change in the slope of the drift flux plot. The
overall gas holdup was calculated by measuring the change in dynamic liquid height.
Figure 5-9 shows the evolution of overall gas holdup with superficial gas velocity. The
overall gas holdup curve shows a change in slope around 3-4 cm/s, indicating flow
regime transition.
Figure 5-10 shows the drift flux plot in an air-water system at ambient conditions in a a
0.1012 m diameter column. The drift flux curve also exhibits a change in the slope
around 3 4 cm/s, confirming it to be the transition velocity.
110
Figure 5-9: Overall gas holdup curve using an air-water system at ambient conditions in a
0.1012 m diameter column
8
Drift Flux
0
0
0.1
0.2
Gas holdup
Figure 5-10: Drift flux plot using an air-water system at ambient conditions in a 0.1012 m
diameter column
Once the flow regime boundaries were defined using conventional methods, the obtained
photon counts history was analyzed to propose new flow regime identifiers for NGD.
The characteristic behavior of photon counts history and also the derived information
from the obtained time-series around the transition velocities, i.e., 3-4 cm/s will be
utilized to propose such identifiers.
111
5.2.2b Analysis of photon counts history
Figure 5-11 shows the photon counts history over 20 sec. of acquisition length for: a) an
empty column (air) and b) water (without gas flow). The photon emission inherently
shows Poisson distribution, where the mean and the variance of the obtained photon
counts is the same. The photon counts history obtained in air and water (without gas
flow) in the current study also shows Poisson distribution. In case of an empty column,
the mean the variance = 265 while in water (no gas flow), the mean the variance =
130.
Figure 5-12 shows the photon counts history received by the detector at various
superficial gas velocities, a) 1, b) 3, c) 7, and d) 11 cm/s using air-water system at
ambient conditions in a 0.1012 m diameter column. It clearly shows an increase in
amplitude as well as oscillations in photon counts with an increase in superficial gas
velocity. The photon counts fluctuations at low superficial gas velocities are relatively
uniform, while at higher velocities, intense fluctuations can be observed, due to wide
bubble size distribution. At higher velocities, large peaks can also be observed which are
due to the presence of large bubbles in the path of -rays. The photon counts history
appears to show the signature of the prevailing flow regime.
(a)
(b)
Figure 5-11: Time-series of photon count fluctuations in a 0.1012 m diameter column in
a) empty column and b) water (no gas flow).
112
(a)
(b)
(c)
(d)
Figure 5-12: Time-series of photon count fluctuations in a 0.1012 m diameter column
using air-water system at superficial gas velocities of a) 1, b) 3, c) 7, and d) 11 cm/s at
ambient conditions.
The obtained photon counts history was subjected to various time-series analyses.
i)
Statistical analysis
Statistical analysis is one of the obvious methods to study a time-series. The mean, is
given by
N
x
i =1
(5-8)
113
The average deviation of a signal can be then written as
N
Average deviation =
x
i =1
(5-9)
Although it is straightforward, the average deviation is almost never used in statistical

analysis. The important parameter is not average deviation but the power represented by
deviation from mean, called as the standard deviation, , or the the variance, 2, and
given as
N
2 =
( xi )
i =1
( N 1)
(5-10)
Figure 5-13 shows the change in the second moment (i.e. the variance) of the photon
counts history with superficial gas velocity. An increase in superficial gas velocity
increases the variance of photon counts fluctuations. Around a superficial gas velocity of
34 cm/s, a noticeable increase in the variance with superficial gas velocity was
observed. The variance versus superficial gas velocity relationship shows two distinct
slopes. The change in the slope of the variance of the photons counts history was
observed at 3-4 cm/s. Based on the conventional methods, the transition from
homogeneous to heterogeneous flow also occurs at the same superficial gas velocities.
Hence, a change in slope of the variance of photon counts history can be used to identify
flow regime transition.
In the bubbly flow regime, the value of the slope of the variance is less, while in churnturbulent flow a rapid increase in the variance with superficial gas velocity was observed.
Apart from a Poisson distribution, the fluctuations in photon counts history are imparted
by the passage of bubbles in the system. The value of the variance is low in bubbly flow,
as small non-interacting bubbles with uniform sizes are present that result into lower
photon counts fluctuations and less the variance. However in churn-turbulent flow, both
small and large bubbles are present, resulting in a wide bubble size distribution. In
addition, there is an intense bubble-bubble interaction in this regime. In churn-turbulent
114
flow, the -rays are frequently intercepted by bubbles of different sizes and intensity
giving rise to higher fluctuations that result in higher value of the variance of the photon
counts history. The two distinct slopes in the variance are mainly due to the different
nature of bubble interactions and bubble size distribution in the two flow regimes. Hence,
the change in the variance indicates the flow regime transition point.
Lin et al. (1999) performed flow regime transition studies using pressure drop fluctuation
measurements. Figure 5-14 shows the transition velocity obtained in Lin et al. (1999) at
the same operating and design conditions used in the present work, based on the standard
deviation of the pressure fluctuation measurements. They performed experiments in a
0.1012 m diameter plexi-glass column using an air-water system to corroborate the
transition velocity obtained by pressure drop fluctuations with those of visual observation
and conventional methods such as the drift flux plot. Based on such evaluation, they
further implemented pressure drop fluctuations measurements for regime transition
identification at high pressure and temperature. The transition velocity obtained from the
change in the slope of the standard deviation of the pressure fluctuations (3.5 cm/s) is
close to the one obtained in the current study (3-4 cm/s).
Figure 5-13: Variation of the variance of photon counts fluctuations with superficial gas
velocity in a 0.1012 m diameter column using air-water system at ambient conditions.
115
Figure 5-14: Variation of the variance of pressure drop fluctuations with superficial gas
velocity in a 0.1012 m diameter column using air-water system at ambient conditions
(Reproduced from Lin et al., 1999).
ii) Deviation from Poisson distribution

-rays inherently show Poisson distribution (i.e. the mean = the variance) in empty
column as well as in water (no gas flow). Due to the introduction of gas in static water,
the photon counts history deviates from a Poisson distribution because the photon counts
obtained in a dynamic system have additional information characterizing the flow
behavior. Hence, the deviation from Poisson distribution might be able to decipher
information regarding the flow behavior and subsequently about the underlying flow
regime. It was observed that with an increase in superficial gas velocity, the mean and the
variance increase. In addition, the difference between the mean and the variance also
appears to increase with an increase in superficial gas velocity. To account for such a
deviation of the time-series from a Poisson distribution, a new coefficient was proposed,
called the coefficient of departure from Poisson distribution, DP, and defined as
DP =
(Variance) i
(Variance) pd
(5-11)
where (variance)i is the variance of the obtained photon counts history at a certain
superficial gas velocity, and (variance)pd is the variance of the obtained photon counts
history at that velocity, if it had been a Poisson distribution, i.e., the mean.
116
This reduces equation (5-11) to
DP =
(Variance) i
.
( Mean) i
(5-12)
Hence, it is the ratio of the variance and the mean of the obtained photon counts history at
a certain superficial gas velocity.
The value of DP in an empty scan and in water (no gas flow) was found to be, as
expected, unity. With an increase in superficial gas velocity, the value of DP departs from
unity. Figure 5-15 shows the change in the coefficient of departure from a Poisson
distribution with superficial gas velocity in a 0.1012 m diameter column using an airwater system. The value of DP increases with an increase in superficial gas velocity. The
rate of change in the value of DP is less at low superficial gas velocities, but at higher
superficial gas velocities it increases significantly with the change in superficial gas
velocity. Only small bubbles are present in the system at low superficial gas velocities (in
bubbly flow) that imparts fewer fluctuations around the mean, and hence the deviation
with respect to the mean is less. However, in churn-turbulent flow, both small and large
bubbles come in the path of -rays, which imparts intense fluctuations around the mean.
Hence, the deviation of photon counts from the mean is significant at high superficial gas
velocities.
It was observed that for superficial gas velocities above 3 cm/s, the value of DP is greater
than 1.4. Based on the conventional methods, the transition velocity was found to be
around 3 4 cm/s; hence the behavior of the departure coefficient can be generalized
based on the flow regime. It was found that in the churn-turbulent flow regime the value
of DP was greater than 1.4. It should be noted that, although the coefficient of departure
from Poisson distribution has been defined based on the physics of -rays, its value for
flow regime demarcation is purely empirical.
117
Figure 5-15: The coefficient of departure from Poisson distribution versus superficial gas
velocity in a 0.1012 m diameter column using an air-water system at ambient conditions.
The proposed coefficient facilitates identification of the underlying flow regime at the
operating superficial gas velocity and promises to be a robust flow regime identifier in
bubble columns.
i)
Autocorrelation Analysis
The autocorrelation function expresses the linear relationship between signal values at
two different times and can be mathematically written as
C xx ( ) =
1
T
x(t ) x(t ).dt ,
(5-13)
where is time lag, and and are the first and second moments of the distribution.
The autocorrelation function is used to estimate how well future values of a signal can be
predicted from knowledge of the signal history. It provides information regarding the
repetitiveness of a given signal. As long term processes do not appear in autocorrelation
curves, they are generally evaluated over the time lag of 0-2 sec without loss of any
important information (Smith, 1999).
118
The obtained photon counts histories were subjected to autocorrelation analysis. Figure 516 shows the autocorrelation curve, i.e., the autocorrelation coefficient versus time lag in
bubbly flow at superficial gas velocities of a) 1, b) 3, and c) 4 cm/s. The autocorrelation
curves in bubbly flow exhibit the behavior of a typically random process and show a
shape close to an exponential curve. In homogeneous flow, as the name suggests, due to
the presence of uniform bubble sizes, the system is virtually similar everywhere. The
events evolving over the time are similar in nature in bubbly flow. Hence, the time-series
obtained in this regime is well correlated, as reflected in the autocorrelation curve.
(a)
(b)
(c)
Figure 5-16: Autocorrelation curve at superficial gas velocities of a) 1, b) 3, and c) 4 cm/s

using an air-water system in a 0.1012 m diameter column at ambient conditions.
119
Figure 5-17 shows the autocorrelation curve in churn turbulent flows at superficial gas
velocities of a) 7, b) 9, and c) 11 cm/s. As the system enters into heterogeneous flow, the
coalescence of small bubbles results in the appearance of larger bubbles, which in turn
results into wider bubble size distribution. Hence, -rays encounter both small and large
bubbles. Due to interception by bubbles of different sizes and characteristics, the
probability of the same events evolving over time is relatively less, and hence the
obtained series is not well correlated. This reflects in a characteristic anti-correlation
superimposed on the exponential behavior in the autocorrelation curve in the churnturbulent flow regime.
(a)
(b)
(c)
Figure 5-17: Autocorrelation curve at superficial gas velocities of a) 7, b) 9, and c) 11

cm/s using an air-water system in a 0.1012 m diameter column at ambient conditions.
The autocorrelation curve shows close to exponential behavior in bubbly flows, while in
churn-turbulent flows it exhibits characteristic anti-correlation behavior where cosine
120
behavior is superimposed on an exponential curve. The visibly different behavior of the
autocorrelation curves in the two regimes provides a means to demarcate them based on
the shape of the autocorrelation curve at the operating condition.
The behavior of the autocorrelation curves is a reflection of the nature of the time-series,
irrespective of its operating and design conditions. Based on the inherent nature of the
flow, the bubbly regime should exhibit correlated curve, while the churn-turbulent regime
should exhibit an uncorrelated curve. This fact can be utilized for online flow regime
identification in industrial reactors.
iv) Spectral Analysis

The goal of spectral analysis is to describe the distribution of the power contained in a
signal over a frequency, based on a finite set of data. It converts information available in
the time-domain into the frequency-domain.
Spectral analysis is performed using Fourier transform, which is named after the French
mathematician and physicist Jean Baptiste Joseph Fourier. Fourier presented a paper in
1807 to the Institut de France on the use of sinusoids to represent temperature
distributions. The paper contained the (then) controversial claim that any continuous
periodic signal could be represented as the sum of properly chosen sinusoidal waves.
Among the reviewers were two of history's most famous mathematicians, Joseph Louis
Lagrange and Pierre Simon de Laplace.
While Laplace and the other reviewers voted to publish the paper, Lagrange adamantly
protested. For nearly decades, Lagrange had insisted that such an approach could not be
used to represent signals with corners, i.e., discontinuous slopes, such as in square waves.
The Institut de France bowed to the prestige of Lagrange, and rejected Fourier's work.
Luckily, Fourier had other things to keep him busy: political activities, expeditions to
Egypt with Napolean, and trying to avoid the guillotine after the French revolution. It
121
was only after Lagrange died that the paper was finally published (Smith, 1999).
Afterwards, it has been used abundantly to analyze time-series in various fields.
Fourier transform, F, of a time series x(t) can be given as
+
F ( x) =
x(t ) exp( j 2f .t )dt ,
(5-15)
where, f, is frequency.
The power spectral density (PSD), xx , is the square of the magnitude of the continuous
Fourier transform
xx = F ( x).F * ( x) ,
(5-16)
where F*(x) is the complex conjugate of Fourier transform.

Figure 5-18 shows the log-log normalized psdf plots at superficial gas velocities of a) 1,
b) 3, c) 4, d) 6, e) 9, and f) 11 cm/s. The normalized psdf is calculated by substracting the
original time-series from its mean. At 1 and 3 cm/s, i.e., in bubbly flow, the psdf plot did
not show any power law fall off, while at higher superficial gas velocities, i.e., in the
transition and churn-turbulent flow regimes, a distinct the power-law fall off was
observed. An analogy can be drawn between power-law fall off observed in the current
study with that observed in single phase turbulent flow.
The general picture of energy distribution in a single phase turbulent flow can be
explained as follows (Hinze, 1975). There exist large primary eddies, which originate
during the formation of the flow or as a result of disturbances. These eddies cause large
fluctuations of low frequency. Their size is comparable to the characteristic geometrical
dimension of the flow system.
122
(a)
(b)
(c)
(d)
(e)
(f)
Figure 5-18: Typical log-log plot of normalized psdf at superficial gas velocities of a) 1,
b) 3, c) 4, d) 6, e) 9, and f) 11 cm/s, using an air-water system in a 0.1012 m diameter
column at ambient conditions.
123
The eddies in the range of the peak in spectral energy can be regarded as large. They
contain most of the energy and contribute little to energy dissipation by internal friction.
These eddies dissipate energy through fine-scale eddies. The process, by which energy
travels from large to fine scale in an energy cascade, is one-way street where counterflow
of energy from small to large scale has previously considered insignificant compared to
energy transfer in the opposite direction. It is now better understood that the energy flow
in both directions is significant, with just a net excess of energy moving to the fine scale
to be dissipated. The flow of energy transfers from large scale to fine scale through
vortex stretching and folding, and transfers from fine scale to large when vortices
compress, recombine, or reconnect into larger vortices. Energy dissipation by friction
occurs in the small eddies of high frequency.
Hence, one can divide the flow into three scales: the mesoscale, macroscale, and
microscale. Mesoscale eddies fluctuate at low frequency and have a size comparable to
the diameter of the column. Macroscale eddies contain most of the energy, microscale
eddies dissipates energy at the finer scale.
The famous Russian mathematician Kolmogorov pioneered a scale analysis that has had a
profound influence on the way in which the energy spectrum in turbulence is understood.
The general picture of energy transfer explained above in a single phase turbulent flow
forms the basis of the theory of isotropic turbulence. This theory is based on the
following two assumptions.
1) While the stirring force (i.e. the mechanism causing turbulence production) that
creates turbulence varies from flow to flow and affects the turbulence characteristics,
the small-scale motions at which dissipation takes place develop a common form for
all flows. For sufficiently great Reynolds numbers, the turbulence is in a universal
equilibrium that is entirely determined by the kinematic viscosity and the rate of
energy dissipation per unit mass.
124
2) In the so-called inertial subrange, the energy spectrum becomes independent of
viscosity and is solely determined by energy dissipation per unit mass. The following
distribution law of Kolomogorov applies:
E k-5/3,
(5-17)
where, k is the wavenumber and is proportional to frequency.

In the bubble column literature, attempts have been made to apply the theory of isotropic
turbulence. The ideas of Kolmogorov have proved to be of great value, and the past
experimental studies suggest and to some extent justify the applicability of this theory to
bubble columns. However, it should be noted here that the current study attempts neither
to justify/evaluate the applicability of Kolmogorovs law for bubble columns nor to gain
insights into such flows based on its applicability.
Zakrzewski et al. (1981) performed constant temperature film anemometer experiments
to measure liquid velocity in a 0.14 m diameter and 2.69 m high column. The liquid
phase was water and 1% Methanol. Two spargers were employed, viz., a sintered plate
(pore diameter of 5 m) and a perforated plate (home diameter = 1 and 3 mm). They
measured the turbulent intensities and determined the energy distribution spectra.
Figure 5-19: Power spectra of liquid velocity fluctuations in a bubble column, by

Zarzewski et al. (1981).
125
Zakrzewski et al. (1981) found the slope of the log-log energy distribution plot to be 2
in the inertial subrange, as shown in Figure 5-19. They concluded that Kolomogrovs
law for single phase turbulence with 5/3 slope was derived for grid turbulence, whereas
for the case of the bubble swarm turbulence in bubble columns, a slope of 2 is to be
expected.
Lance and Bataille (1991) performed Laser Doppler Anemometry (LDA) and hot-film
anemometry experiments in an air-water bubble column. The test section used in the
study was a 2 m long square channel (0.45 X 0.45 m) operated at ambient conditions. The
experimental conditions were such that the void fraction was varied between 0 to 3 %.
Lance and Bataille (1991) found that the classical 5/3 power law describing the behavior
of the spectra in the high wavenumber range was progressively replaced by another
power law of exponent equal to 8/3.
Recently, Groen (2004) performed LDA studies in an air-water system in three different
column diameters, i.e., 15, 23, and 40 cm. Groen (2004) found the value of the slope to
be in the range of 3/2 and 5/3. The close observation of psdf plots provided in Groen
(2004) thesis shows that the frequency range where such a power law fall-off was
observed depends on the radial location of the measurement. As one moves inwards to
the column center, the power spectra also appear to shift inwards, as shown in Figure 518. The power-law fall-off seems to exist in the inertial subrange for measurement
(a)
(b)
126
(c)
Figure 5-20: LDA axial velocity signal power spectra a) D = 15 cm, Ug = 2.7 cm/s, z/D =
5.5, b) D = 23 cm, Ug = 1.2 cm/s, z/D = 6, and c) D = 40 cm, Ug = 5.5 cm/s, z/D = 5
(Groen, 2004)
locations close to the wall. However, such a slope was observed in far smaller frequency
ranges for measurement locations towards the column center. The power spectra at a few
measurement locations show a power-law fall off in the frequency range observed in the
current work.
It is worth mentioning that in earlier studies, experiments were apparently performed in
the bubbly flow regime. The power-law fall off was observed in homogeneous flow in
these studies. In the current study, no such exponent was observed in bubbly flow. Based
on this, further quantitative analysis was performed for observed power-law fall off in the
psdf plot of photon counts history at higher superficial gas velocities in the current study.
The psdf plot of photon counts history obtained in an empty column (air) and water (with
no gas flow) is shown in Figure 5-21a and b. As mentioned earlier, a Poisson distribution
was observed during scans in air and water (with no gas flow). The log-log normalized
psdf plot does not show any variation in the power. This is expected, as the photon counts
obtained in air and water indicate characteristic noise inherent to gamma-rays. This rules
out the possibility of occurrence of meaningful power spectra and its slope, due to the
contribution of, or being an artifact of, a Poisson distribution.
127
(a)
(b)
Figure 5-21: Log-log plot of normalized psdf of photon counts history obtained in a)
empty column and b) water (with no gas flow).
(a)
(c)
(b)
(d)
Figure 5-22: Log-log plot of normalized psdf with fitted slope line at superficial gas
velocities of a) 4, b) 6, c) 9, and d) 11 cm/s using an air-water system in a 0.1012 m
diameter column at ambient conditions.
128
Next, the operating conditions where the psdf plot showed a power-law fall off were
analyzed. In general, the power-law fall off was observed in the frequency range of 5
15 Hz, and the data points in this range were regressed to obtain the best fit. The fitted
equations are shown in Figure 5-22a, b, c, and d along with the R-squared value. The Rsquared values were found to be equal to or greater than 0.85 in all the cases. At high
superficial gas velocities, the R-squared values were close to 0.96.
The distinct slope in the psdf plot started to appear at a superficial gas velocity of 4 cm/s
where the transition regime exists (Figure 5-22a). The slope increases with an increase in
superficial gas velocity. At a superficial gas velocity of 6 cm/s, the slope is close to 1
(Figure 5-22b). Above superficial gas velocities of 6 cm/s, the slope gradually increases
and remains close to 1.7 in fully churn-turbulent flow. Figures 5-22c and d show the
log-log plot of the normalized psdf at superficial gas velocities of 9 and 11 cm/s with an
exponent close to 1.7. Table 5-3 shows the slopes of the power spectra at studied
operating conditions. It is clear that Kolomogorovs 5/3 law appears to be applicable in
Table 5-3: Slope of power spectra at studied operating conditions
Superficial gas
velocity
(cm/s)
1
2
3
4
5
6
7
8
9
10
11
12
Slope of power
spectra
- 0.7
- 0.7
- 1.02
-1.6
- 1.62
- 1.65
- 1.67
- 1.69
-1.7
the two phase churn-turbulent flow, as in a single phase turbulent flow, indicating that the
mechanism of energy dissipation in two-phase flow is similar to that observed in single
129
phase turbulent flows. However the power-law fall off was observed at relatively low
frequencies during these studies.
In the current study, the exponent was observed in either transition or churn-turbulent
flow regimes. The close observation of power spectra obtained in this study shows that
the values of the power in water (with no gas flow) and the values in bubbly flows are
close to each other, indicating that a Poisson distribution might be still dominant at these
conditions. The value of the coefficient of a Poisson distribution also varies up to 1.2
1.3. At high superficial gas velocities the appearance of large bubbles increases the
fluctuations in the system, adding significant flow dynamics information to a Poisson
distribution. This might be a possible reason for the absence of the slope in power spectra
in bubbly flow using NGD.
Apart from its analogy to a single phase turbulent flow, the observed slope can be utilized
for the main objective of this study, i.e., to demarcate the underlying flow regime. It is
worth mentioning that although the literature studies exhibit power law fall off in bubbly
flow, such behavior was not observed in the current study. The current study observed
power law fall-off in transition flow (-0.7), which gradually increased to 1.7 in churnturbulent flow. The previous studies were performed using either LDA or a hot film
anemometer. No experiments were performed during those studies in churn-turbulent
flow.
Based on the available information and the current study, it can be concluded that no
power law fall off in bubbly flow and power law fall off in the churn-turbulent flow can
be exclusive characteristics of photon counts time-series obtained using NGD. The main
goal of this study was not to analyze the power spectra or its utility in understanding the
flow in bubble column. However, such an observation is helpful in developing a flow
regime identifier for NGD, which is the main objective of the current study.
In conclusion, the following flow regime identifiers were developed for NGD using an
air-water system:
130
1)
The coefficient of departure is greater than 1.4 in the churn-turbulent flow.
2)
The autocorrelation curve exhibits different behavior in bubbly and churn-
turbulent flows. In bubbly flow, it exhibits a near exponential curve, while churnturbulent flow exhibits anti-correlation behavior superimposed on an exponential curve.
3)
The normalized logarithmic psdf plot shows no slope in bubbly flow, while a
distinct slope was observed in churn-turbulent flow.

The development of NGD, along with its identifiers, presents an opportunity to identify
the prevailing flow regime without disturbing the process operation. As mentioned
earlier, NGD can be mounted externally, and analyzing the obtained time-series at
process conditions in the context of the developed identifiers can provide information
regarding the prevailing flow regime. The developed method negates the need to observe
the evolution of a secondary parameter over the range of superficial gas velocities for
flow regime identification, and hence it can be applied without changing the process
conditions.
These flow regime identifiers were developed based on the experiments performed in
an air-water system at ambient pressure using a plexi-glass column that enables visual
observation of the flow. The next section deals with the evaluation of the developed flow
regime identifiers at various operating and design conditions.
5.2.3 Evaluation of the flow regime identifiers developed for NGD

In this part, the flow regime identifiers developed for NGD are evaluated at high
pressure and in different systems. For this purpose, the experiments were performed in a
6 diameter stainless steel column. The details of this experimental and the CT setup are
provided in Chapter 3, and will not be repeated here. During these experiments, an
existing CT was converted to densitometry by placing the central detector in front of the
radioactive source. One should recall here that the experimental setup used for these
experiments is made of stainless steel. In this way we demonstrate the applicability of the
developed technique and its flow regime identifiers in different systems, as well as in a
131
steel column. This is important when we consider applying NGD for flow regime
monitoring in industrial columns. The overall gas holdup experiments were performed
using the column with windows (Figure B-1), while the densitometry experiments were
performed using the experimental setup shown in Figure 3-1. Table 5-4 shows the
operating conditions and the systems used. Air was used as the gas phase, while the
liquid phases were water and C9 C11 mixture. The composition of C9 C11 mixture was:
C8 3.3 %, C9 36.3 %, C10 34.5 %, C11 23.8 %, and C12 1.9 %. The physical
properties of this mixture are different from water [density = 0.726 gm.cc-1; viscosity =
0.85 mPa s; surface tension = 23.2 mN.m-1].
The dynamic liquid height in all the
experiments was the same, i.e., L/D ~ 10. The acquisition frequency of the photon counts
history was 50 Hz. The time-series, with the number of data points, N = 15000 was
collected at superficial gas velocities of 1 to 20 cm/s with intervals of 1 cm/s and at 30
cm/s.
Table 5-4: Experimental conditions for the evaluation of flow regime identifiers
System
Operating
pressure
(MPa)
Air-water
0.1
Air-water
1.0
Air-C9-C11
0.1
Air-C9-C11
1.0
First the transition velocities were determined based on the overall gas holdup and the
drift flux plot, which enable us to tag conditions based on the prevailing flow regime. The
transition velocity obtained using the traditional methods were compared with the one
obtained using the variation of Dp with superficial gas velocity. Then the photon counts
history obtained in different flow regimes were analyzed using autocorrelation analysis
and spectral analysis to evaluate the applicability of the developed flow regime
identifiers. The identifiers were found to be satisfactory.
132
5.2.3a Air-water system, P = 0.1 MPa
Figures 5-23a and b show the overall gas holdup curve and the drift flux plot for an airwater system in a 6 diameter column at ambient pressure. Based on the change in the
slope of the gas holdup curve and the drift flux plot, the transition velocity at this
condition is 5 cm/s. Hence, the developed criteria were evaluated for data collected in the
identified different flow regimes.
30
0.3
D rift flu x , j
O ve rall g as h old up (- )
0.4
0.2
20
10
0.1
0
0
10
20
30
0.1
0.2
0.3
0.4
Overall gas holdup (-)
(a)
(b)
Figure 5-23: a) Overall gas holdup curve and b) drift flux plot in an air-water system at
ambient pressure in a 6 diameter stainless steel column
Figure 5-24: Variation of coefficient of departure, Dp with superficial gas velocity in an

air-water system at ambient pressure in a 6 diameter stainless steel column
Autocorrelation function (-)
1
0.8
0.6
0.4
0.2
0
0
-0.2
Autocorrelation coefficient (-)
133
1
0.8
0.6
0.4
0.2
0
0
-0.2
Time lag (sec)
Time lag (sec)
(a)
(b)
Figure 5-25: Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at ambient pressure using an air-water system.
(a)
`(b)
(c)
Figure 5-26: Psdf plot at superficial gas velocities of a) 2 cm/s, b) 7 cm/s, and c) 20 cm/s
and ambient pressure using an air-water system in a 6 diameter stainless steel column.
134
Figure 5-24 shows the variation of the coefficient of departure from a Poisson
distribution with superficial gas velocity. It can be observed that the value of Dp is
greater than 1.4 for superficial gas velocities above 5 cm/s. Figure 5-25a shows the
autocorrelation curve in the bubbly flow (Ug = 2 cm/s), while Figure 5-25b shows the
autocorrelation curve in the churn-turbulent flow (Ug = 20 cm/s). The autocorrelation
curve in the bubbly flow shows the exponential behavior, while the one in the churnturbulent flow shows characteristic anti-correlation, indicating the prevailing flow
regime. Figure 5-26 shows the psdf plot at superficial gas velocities of 2, 7, and 20 cm/s.
In the bubbly flow no power-law fall off was observed, while at the conditions above
transition velocity, i.e., 5 cm/s, a distinct power-law fall off was observed. At Ug = 7
cm/s, the slope was close to 1, while at Ug = 20 cm/s, it was -1.7. It showed a gradual
increase in the value of the slope with an increase in superficial gas velocity. However,
the value of the slope levels off at high superficial gas velocities. At Ug =30 cm/s, the
value of slope was -1.71.
5.2.3b Air-water system, P = 1.0 MPa

20
15
0.4
Drift flux, j
0.6
10
0.2
0
0
10
20
Superficial gas velocity (cm/s)`
(a)
30
0.2
0.4
(b)
Figure 5-27: a) Overall gas holdup curve and b) drift flux plot in an air-water system at
an operating pressure of 1 MPa in a 6 diameter stainless steel column
Based on the overall gas holdup curve (Figure 5-27a) and drift flux plot (Figure 5-27b),
the regime transition velocity is around 8 9 cm/s at an operating pressure of 1 MPa in
an an air-water system. Figure 5-28 shows that for superficial gas velocities greater than
135
Figure 5-28: Variation of coefficient of departure, Dp, with superficial gas velocity in an
air-water system at an operating pressure of 1 MPa in a 6 diameter stainless steel
1.2
column
0.8
0.6
0.4
0.2
0
0
0.5
-0.2
Time lag (sec)
1.5
1
0.8
0.6
0.4
0.2
0
-0.2
0.5
1.5
Time lag (sec)
(a)
(b)
Figure 5-29: Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at an operating pressure of 1 MPa using an air-water
system.
(a)
(b)
136
(c )
and an operating pressure of 1 MPa, using an air-water system in a 6 diameter stainless
steel column.
8 cm/s the value of Dp is higher than 1.4. In addition, the autocorrelation curves in
bubbly flow (Ug = 2 cm/s) and churn-turbulent flow (Ug = 20 cm/s) show distinctly
different behavior (Figure 5-29). The logarithmic psdf plot reveals that there is no power
law fall off in the bubbly flow (Ug = 2 cm/s), while above the transition velocities, a
distinct power law fall off was observed (Figure 5-30). The value of the slope of varies
from 1 at Ug = 10 cm/s to 1.6 at Ug = 20 cm/s, while it is 1.65 at Ug = 30 cm/s.
5.2.3c An air-C9-C11 system, P = 0.1 MPa
40
0.5
0.4
0.3
Drift flux
Gas holdup (-)
30
0.2
20
10
0.1
0
0
10
20
30
0
0
0.2
0.4
0.6
Gas holdup
(a)
(b)
Figure 5-31: a) Overall gas holdup curve and b) drift flux plot in an air-C9-C11 system at
an operating pressure of 0.1 MPa in a 6 diameter stainless steel column
137
Based on the overall gas holdup curve and the drift flux plot (Figure 5-31), the transition
velocity in an air-C9-C11 system at an operating pressure of 0.1 MPa was around 8 cm/s.
Figure 5-32 shows that for superficial gas velocities less than 8 cm/s the value of Dp is
less than 1.4. The autocorrelation curves in the bubbly (Ug = 2 cm/s) and the churnturbulent (Ug = 20 cm/s) flows show distinctly different behavior (Figure 5-33). The
logarithmic psdf plot shows power law fall off at superficial gas velocities greater than
the transition velocity (Figure 5-34).
Figure 5-32: Variation of coefficient of departure, Dp, with superficial gas velocity using
an air-C9-C11 system at operating pressure of 0.1 MPa in 6 diameter stainless steel
column
1.2
0.8
0.6
0.4
0.2
0
0
-0.2
1
0.8
0.6
0.4
0.2
0
0
0.5
1.5
-0.2
Time lag (sec)
(a)
Time lag (sec)
(b)
Figure 5-33: Autocorrelation curve in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at ambient pressure using an air-C9-C11 system.
138
log(Y) = -1 log(X) + 2
R^2 = 0 8
(a)
(b)
log(Y) = -1.7
log(X) + 2 2
(c )
and an ambient pressure using an air- C9-C11 system in a 6 diameter stainless steel
column.
5.2.3d An air-C9-C11 system, P = 1.0 MPa

0.7
20
15
0.5
Drift flux, j
0.6
0.4
0.3
10
0.2
5
0.1
0
0
10
20
30
0
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
(a)
(b)
Figure 5-35: a) Overall gas holdup curve and b) drift flux plot in an air-C9-C11 system at
an operating pressure of 1 MPa in a 6 diameter stainless steel column
139
The overall gas holdup curve and the drift flux plot (Figure 5-35) in an air-C9-C11
system at operating pressure of 1 MPa reveal that the transition velocity is around 12
cm/s. The variation of Dp with superficial gas velocity (Figure 5-36) at this condition
shows that below the transition velocity, the value of Dp is less than 1.4. Figure 5-37
shows the autocorrelation curve that exhibits different behavior in the bubbly (Ug = 2
cm/s) and the churn-turbulent (Ug = 20 cm/s) flows. The logarithmic psdf plot (Figure 538) shows power law fall-off at superficial gas velocities greater than the transition
velocity while no such power law fall-off was observed for velocities less than the
transition velocity.
Figure 5-36: Variation of coefficient of departure, Dp, with superficial gas velocity using
an air-C9-C11 system at an operating pressure of 1 MPa in a 6 diameter stainless steel
column
1
0.8
0.6
0.4
0.2
0
0
0.5
-0.2
Time lag (sec)
(a)
1.5
A utoc orrelation c oeffic ient (-)
0.8
0.6
0.4
0.2
0
0
0.5
1.5
-0.2
Time lag (sec)
(b)
Figure 5-37: Autocorrelation curves in a) bubbly flow (Ug = 2 cm/s) and b) churnturbulent flow (Ug = 20 cm/s) at an operating pressure of 1 MPa using an air-C9-C11
system.
140
(a)
(b)
(c )
and an operating pressure of 1 MPa using an air- C9-C11 system in a 6 diameter stainless
steel column.
In the above section, the applicability of NGD for flow regime demarcation was
evaluated in different systems and at high operating pressure. The transition velocity
obtained from the overall gas holdup curve and the drift flux plot matches the one
revealed by variation in Dp. It was also observed that the flow regime identifiers
developed for NGD [listed in Section 5.2.2c] using an air-water system in a 4 diameter
column are applicable in different systems, at high operating pressure, and more
importantly in stainless steel columns. It is evident that the developed flow regime
identifiers are functions of the nature of the obtained photon counts history rather than the
operating and design conditions. The nature of the photon counts history, in turn, is a
function of the prevailing flow behavior.
141
5.2.3e Observed effects of operating and design parameters on flow regime
transition
i)
Effect of operating pressure
In the current study, two operating pressures were studied in two different systems. An
increase in operating pressure from 0.1 to 1 MPa increased the transition velocity from 5
to 8 cm/s in an air-water system, while it increased from 8 to 12 cm/s in an air- C9-C11
system. An increase in pressure increased the breakup rate, reduced the coalescence rate,
and delayed the appearance of large bubble and thereby the flow regime transition. The
effect of operating pressure observed in this study is in line with the previous findings by
Krishna et al. (1991), Wilkinson et al. (1991), Reilly et al. (1994), Lin et al., (1999), and
Lin et al. (2001).
ii)
Effect of physical properties
The change in the liquid from water to C9-C11 increased the transition velocity from 5 to 8
cm/s at ambient pressure, while it increased from 8 to 12 cm/s at an operating pressure of
1 MPa. The mixture of C9-C11 has a lower viscosity and surface tension than water. The
reduction in viscosity and surface tension appear to have qualitatively similar effects on
the flow regime transition. The decrease in viscosity resulted in an unstable interface that
in turn resulted into a higher bubble break up rate and a lower coalescence rate, and
delayed the appearance of large bubble. The reduction in surface tension also shows a
similar effect. Urseanu (2000) studied the effect of surface tension by adding various
percentages of ethanol in water. Based on dynamic gas disengagement (DGD) studies,
she found that an addition of alcohol tends to suppress the coalescing tendencies of small
bubbles and thereby delays flow regime transition. Hence, the combined effect of low
viscosity and surface tension results in an increase in the transition velocity in C9-C11 at
both ambient and high pressures.
142
iii) Effect of column diameter
The reported effect of column diameter on the flow regime transition remains conflicting.
Based on their own data and the literature data in an air-water systems, Sarrafi et al.
(1999) found that transition velocity increases with an increase in column diameter,
which becomes independent of column diameter beyond 0.15 m. Earlier, Ohki and Inoue
(1970) found that transition velocity increases with an increase column diameter in the
range of 0.04 0.16 m. Urseanu (2000) found a general trend of an increase in transition
holdup with an increase in column diameter in an air-water and an air-Tellus oil systems.
However, Ruzicka et al. (2001) utilized their own gas holdup data from three different
column diameters (0.14, 0.29, and 0.4 m) to calculate the transition velocity. At different
liquid static heights they found that an increase in column diameter reduced the transition
velocity. Their results are in line with the observations of Zahradnik et al. (1997).
The current study provides a comparison of the transition velocity obtained in 4 (a
0.1012 m) and 6 (0.1615) diameter columns using an air-water system at ambient
pressure. In both cases, the dynamic liquid height was maintained the same (L/D ~ 10).
The transition velocity in a 4 column was 3 cm/s, while in a 6 column it was 5 cm/s.
Thus the current study observed an increase in the transition velocity with an increase in
column diameter, similar to the findings of Ohki and Inoue (1970) and Sarrafi et al.
(1999). In addition, transition gas holdup in a 4 column was 0.11, while in a 6 column
it was 0.2. Hence, an increase in column diameter increased the transition gas holdup,
similar to the findings of Urseanu (2000).
5.2.4 Evaluation of literature correlations

In this section, the transition velocities predicted using reported correlations are
compared with the ones obtained in this study. These correlations are provided in section
5.1.3.
143
Figures 5-39a and b show the comparison of the predictions of these correlations with
that of the experimental data obtained in 4 and 6 inch diameter columns. In general, both
correlations show vast differences between the prediction and experimental data. Table
5-5 shows the % relative error between predicted and experimental data. The observed
percent relative errors are higher than the permissible engineering errors. Surprisingly,
both correlations show higher percent relative errors at ambient pressure.
However, the correlation of Reilly et al. (1992) predicts the transition velocity in a 4 (a
0.1012 m) diameter column at ambient pressure using an air-water system within 2 % of
relative error. One should note here that Reilly et al. (1992) correlation was developed
based on the experimental data in a 0.15 m diameter column. Hence care should be taken
regarding such a comparison.
(a)
(b)
Figure 5-39: Comparison of reported correlations with transition velocities obtained

based on variation in Dp of the photon counts history in a) an air-water system b) an airC9-C11 system at ambient and high pressure.
144
Table 5-5 Statistical comparisons of prediction of correlations with experimental data
System
Pressure
Column
Experimental
(MPa)
diameter
Utrans
(m)
(m/s)
% absolute relative error

Reilly et al.
(1992)
1.7
Wilkinson et al.
(1991)
98
Air-water
0.1
0.1012
0.03
Air-water
0.1
0.1615
0.05
39
96
Air-water
1.0
0.1615
0.08
29
31
Air-C9-C11
0.1
0.1615
0.08
64
95
Air-C9-C11
1.0
0.1615
0.12
58
51
5.3 Remarks
The goal set for this chapter was to develop and demonstrate non-invasive techniques
such as CT and NGD for flow regime demarcation and to explore their use as flow
regime identifiers.
In the first part, experiments were performed using a single source -ray CT in a high
pressure bubble column. The obtained gas holdup radial profiles were studied for flow
pattern identification. Based on the cross-sectional averaged gas holdup estimated from
the obtained radial gas holdup profiles, the regime transition velocity was calculated
using both the gas holdup curve and the drift flux plot. The evolution of the steepness
parameter with superficial gas velocity was analyzed, and the break-point in the
steepness parameter curve was found to reveal information regarding transition velocity.
The transition velocity obtained from the steepness parameter curve was evaluated with
traditional methods and found to be in good agreement. The effect of operating pressure
on the flow regime transition was studied using the developed methodology. The
transition velocity was found to increase with an increase in operating pressure. Also, it
was observed that the change in the flow regime is noticeable at ambient conditions,
while at higher pressure, a gradual change occurs over a region of superficial gas
145
velocities. The obtained transition velocities were compared with the predicted transition
velocities of Wilkinson (1991) and Reilly et al. (1994) correlations. Both correlations
noticeably underpredict the experimental transition velocities; hence, the state of current
correlations needs to be further improved.
In the second part, the feasibility of NGD for flow regime demarcation in bubble column
reactors was explored. The well-known air-water system was utilized for such feasibility
studies, as well as to propose promising flow regime identifiers. Experiments were
performed in a laboratory scale column (diameter = a 0.1012 m, height = 1.2 m) at
ambient conditions. Superficial gas velocities were varied from 1 to 12 cm/s, with an
interval of 0.5 cm/s near transition region. The flow regime boundaries were determined
based on conventional methods such as the change in slope of gas holdup curve and the
drift flux plot.
The photon counts history obtained using NGD was subjected to statistical analysis,
autocorrelation analysis, and spectral analysis. Based on the comparison of such timeseries analyses with those of conventional methods, promising flow regime identifiers for
NGD were proposed. In general, the photon counts history revealed the signatures of the
underlying flow regime. Based on the inherent nature of gamma-ray emission, a new
parameter, called the coefficient of departure from Poisson distribution, was proposed
and found to be greater than 1.4 for churn-turbulent flow regimes. Autocorrelation
analysis exhibited different behavior in bubbly and churn-turbulent flow regimes.
Spectral analysis showed a distinct power-law fall off in the churn turbulent flow regime,
with its slope close to 5/3, similar to the slope observed in a single phase turbulent
flow. The proposed flow regime identifiers for NGD can be helpful in demarcating
underlying flow regimes in laboratory as well as in industrial scale columns, and can be
utilized for online flow regime diagnostics. The flow regime identifiers developed in
this work were evaluated for their applicability in different systems and at high operating
pressure, and were found to identify prevailing flow regimes satisfactorily.
146
In addition, the effects of operating and design parameters on the flow regime transition
observed during this study were discussed. The current state of correlation prediction was
also evaluated. It was found that the current state of prediction could not predict
transition velocities at the performed experimental conditions with statistical confidence.
147
Chapter 6.
Scaleup of Bubble Column Reactors
This chapter focuses on proposing and evaluating a new methodology for hydrodynamic
similarity and subsequently for scaleup of bubble column reactors. The available scaleup
procedures for bubble column reactors have summarized and critically reviewed by
Shaikh and Al-Dahhan (2007b), soon to be published. The findings were briefly
presented in Chapter 2. This part of the work develops and proposes a new hypothesis for
hydrodynamic similarity in bubble columns, based on the conclusions of the above
mentioned review and the understanding developed through abundant hydrodynamic
studies performed at the CREL over the years. The new hypothesis proposed in this work
was also evaluated using existing advanced diagnostic techniques such as CT and
CARPT.
In this chapter, the hydrodynamic similarity hypothesis is discussed in the first section,
followed by a description of the experimental conditions needed to evaluate the proposed
hypothesis. The next section presents the experimental results obtained under similarity
and mismatch conditions, followed by a discussion.
6.1 Hypothesis for hydrodynamic similarity
As mentioned in Chapter 2, the scaleup procedures reported so far utilize the similarity of
global parameters, such as overall gas holdup, for hydrodynamic similarity in two
columns. Such similarity based on global parameters is not surprising, because over the
years bubble column hydrodynamics have been quantified mostly by global parameters
such as overall gas holdup and mass transfer coefficient. However, while hydrodynamic
similarity based on overall hydrodynamics may be applicable in bubbly flow, in the
churn-turbulent flow regime, such criteria may possibly lead to a different gas holdup
distribution across the column cross-section. Figure 6-1 shows the gas holdup radial
148
profile obtained using CT in an air-water system (Ong, 2003; Kemoun et al., 2001) at
different operating conditions with the overall gas holdup of 0.41.
0.8
D6U60P1Water
D6U12P7Water
Gas Holdup
0.6
0.4
0.2
0.2
0.4
0.6
0.8
r/R
Figure 6-1: Comparison of gas holdup radial profile in a 6 column using an air-water
system at two different operating conditions [D6U12P7Water: 7 bar, 12 cm/s, an airwater (Kemoun et al., 2001); D6U60P1Water: 1 bar, 60 cm/s, and an air-water (Ong,
2003)] with similar overall gas holdups (~ 0.41).
Although these systems have similar overall gas holdups, the existence of different gas
holdup radial profiles possibly leads to different flow patterns and mixing intensities. The
conclusions of Macchi et al. (2001) [Section 2.3] and Figure 6-1 suggests that the two
systems can have similar overall gas holdups but different flow patterns and mixing
intensities. This indicates that two systems can be globally similar in nature, but have
different local hydrodynamics. Hence, similarity based only on overall gas holdup does
not appear sufficient.
Based on this, we propose a new methodology based on the hypothesis that
Overall gas holdup and its radial profile or cross-sectional distribution should be the
same for two reactors to be dynamically similar.
149
This work attempts to evaluate the proposed methodology utilizing advanced diagnostic
techniques such as CT and CARPT. Based on the combination of similarity and mismatch
experiments, we will show whether similar overall gas holdups and similar gas holdup
radial profiles indicate similar hydrodynamic performance in two reactors.
6.2 Experimental conditions
The first step in the experimental evaluation was to identify the needed operating
conditions. The experimental conditions were identified that have the same overall gas
holdup and gas holdup radial profile. These conditions are called similarity conditions.
Additionally, experimental conditions were identified such that had same overall gas
holdup, but mismatched radial profiles. These conditions are called as mismatch
conditions.
The mismatch conditions were identified to further demonstrate that
similarity of gas holdup and its radial profile is essential to maintain similar
hydrodynamic performance.
The procedure for experimental evaluation of the proposed methodology is as follows,
1) Identify experimental conditions that have similar overall gas holdup. The overall gas
holdup is obtained by measuring the change in liquid height [ G =
Hd HS
] (where
Hd
Hd and HS are the dynamic and static liquid heights, respectively). In all these
experiments, the dynamic height was kept around 1.8 m (L/D ~ 11).
2) Perform CT experiments to identify similarity conditions.
3) Perform CT experiments to identify mismatch conditions.
4) Perform CARPT experiments at the identified similarity/mismatch conditions to
measure the detailed hydrodynamics (the radial profiles of liquid velocity and
turbulent parameters) in order to assess the proposed methodology for the
hydrodynamic similarity hypothesis.
150
Table 6-1 shows the similarity conditions, while Table 6-2 shows the mismatch
conditions identified during this study. The gas holdup radial profiles at the conditions of
similar overall gas holdup have been measured using CT at the desired conditions. A few
experimental conditions in this study are extracted from the CREL database (references
mentioned in Tables 6-1 and 6-2), in addition to the performed experiments. Although
CT and CARPT experiments in an air-water system were performed earlier in the CREL,
most of these experiments were repeated in this study. Unless it is otherwise referenced,
the experiments were performed as part of this study.
Table 6-1: Similarity conditions in a 6 diameter stainless steel column

Set
System
Pressure
(MPa)
Superficial gas
velocity
(cm/s)
Overall gas
holdup
0.1
0.4
1.0
0.4
0.4
0.1
45
30
30
45
30
30
0.35
An air-water
An air-water
An air-water
An air-water (Ong, 2003)
An air-water
Air-C9- C11 (Han, 2006)
2
3
0.41
0.35
Table 6-2: Experimental conditions for mismatch gas holdup radial profiles in a 6
Set
1
2
System
Pressure
(MPa)
An air-water
Air-C9- C11
An air-water
Air-C9- C11
0.4
0.4
0.4
1.0
Superficial
gas velocity
(cm/s)
30
16
30
8
Overall gas
holdup
0.35
0.35
The emphasis here is to show that if one maintains similar overall gas holdups and gas
holdup radial profiles, the hydrodynamic characteristics of these two systems will be the
151
same. Such a hydrodynamic similarity is the ultimate goal of any scaleup procedure to
maintain the desired conversion and process performance.
6.3 Results
The gas holdup radial profiles, axial liquid velocity profiles, and TKE radial profiles shown
in this section are time- and azimuthally averaged. The statistical difference between
hydrodynamic parameter (gas holdup and liquid axial velocity) profiles are represented in
terms of the average absolute relative difference, is defined as follows,
AARD =
1 N x( r ) y ( r )
x( r ) ,
N 1
(6-1)
where x and y can either be gas holdup, axial liquid velocity, or TKE at the corresponding
radial location.
The strength of liquid recirculation at similarity/mismatch conditions is described in

terms of mean liquid recirculation velocity. The liquid recirculation velocity is defined as
*
u rec =
( ) [1 G ( )] d
[1
(6-2)
( )] d
where * is the radial position of flow inversion.
Figure 6-2a shows the gas holdup radial profiles at experimental conditions of 45 cm/s, and
4 bar (Ong, 2003), and 30 cm/s and 10 bar in an air-water system. The gas holdup radial
profiles are close to each other, with an AARD of 5.5 %. The similar gas holdup radial
profiles in these cases result in close liquid axial velocity profiles (Figure 6-2b) with an
AARD of 14 %. Figure 6-3 shows the variation of an absolute relative difference (ARD) at
these conditions. Except at the inversion point, an ARD appears to be close to 10 %. The
relatively higher AARD can be attributed to such a large difference at the inversion point.
152
(a)
(b)
Figure 6-2: a) Gas holdup and b) Axial liquid velocity radial profile in a 6 diameter
stainless steel column using an air-water system [D6P4U45: 6 inch diameter, 4 bar, and
45 cm/s (Ong, 2003), D6P10U30: 6 inch diameter, 10 bar and 30 cm/s] (Overall gas
holdup ~ 0.41).
Figure 6-3: Variation of AARD in liquid axial velocities between similarity conditions
[D6P4U45Water (Ong, 2003) and D6P10U30Water] along the column radius in a 6
diameter stainless steel column using an air-water system.
153
Figure 6-4: TKE profile in a 6 diameter stainless steel column using an air-water system
[D6P4U45: 6 inch diameter column, 4 bar and 45 cm/s (Ong, 2003), D6P10U30: 6 inch
diameter column, 10 bar and 30 cm/s] (Overall gas holdup ~ 0.41).
At all the studied conditions, an ARD was found to be maximum close to the inversion
point. A possible reason is that the values of the velocities are low (i.e., -6 and -13 cm/s) in
this region (sometimes one condition has a positive value, and other has a negative value)
and the relative differences between these values gets amplified and subsequently increases
the AARD.
Additionally, mean liquid recirculation was calculated at these conditions using equation 62. The mean recirculation velocity at 30 cm and 10 bar is 52 cm/s, while at 45 cm/s and 4
bar, it is 55 cm/s. The relative difference between mean recirculation velocities at these
conditions is 5.5 %. The mixing intensity at these conditions is expressed in terms of the
TKE of the system at those conditions. Figure 6-4 compares the radial distribution of TKE
at these similarity conditions. The AARD in TKE at these conditions was found to be close
to 11 %. This shows that the similar gas holdup radial profiles resulted in close axial
velocity and TKE radial profiles, and thereby the close recirculation rates and mixing
intensities.
Figure 6-5a shows gas radial profiles at operating conditions of 30 cm/s and 4 bar and 45
cm/s and 1 bar in an air-water system. The overall gas holdup in these cases is 0.35. The
154
AARD in gas holdup radial profiles was found to be 4.5 %. Such close gas radial profiles
result in close liquid axial velocity profiles (Figure 6-5b). The AARD in liquid axial
velocity profiles is 17 %. The variation of ARD along the column radius is shown in Figure
(a)
(b)
stainless steel column using an air-water system (D6P1U45Water: 6 inch diameter column,
1 bar and 45 cm/s, D6P4U30Water: 6 inch diameter column, 4 bar and 30 cm/s) [Overall
gas holdup ~ 0.35].
(D6P1U45water and D6P4U30water) along the column radius in a 6 diameter stainless
steel column using an air-water system.
155
6-6. In this case also, the ARD appears to be higher near the inversion point, as explained
above. The mean recirculation velocity at 30 cm/s and 4bar is 42 cm/s, while at 45 cm/s
and 1 bar, it is 39.5. The relative difference between mean recirculation velocities is close
to 6 %, indicating similar liquid recirculation patterns and its strength at these conditions.
Figure 6-7 shows a comparison between TKE at these conditions. The AARD in TKE was
found to be within 9 %, indicating similar mixing intensity and liquid recirculation at these
conditions.
Figure 6-7: TKE radial profile in a 6 diameter stainless steel column using an air-water
system (D6P1U45Water: 6 inch diameter column, 1 bar and 45 cm/s, D6P4U30Water: 6
inch diameter column, 4 bar and 30 cm/s) [Overall gas holdup ~ 0.35].
Figure 6-8a shows the gas holdup radial profiles at 30 cm/s and 1 bar in an air-C9C11
system (Han, 2006) and 30 cm/s and 4 bar in an air-water system. In this set of
experiments, one experimental condition uses a pure liquid (water), while the other uses a
mixture of n-paraffin liquid. The mixture of paraffinic liquid is predominantly C9 C11
cut. The compositions of the various n-paraffins are C8 3.3 %, C9 36.3 %, C10 34.5 %,
C11 23.8 %, and C12 1.9 %. The physical properties of this mixture are also vastly
different from water [density = 0.726 gm.cc-1; viscosity = 0.85 mPa s; surface tension =
23.2 mN.m-1]. The experiments with such different liquids were motivated by the findings
of Macchi et al. (2001). Macchi et al. (2001) used one system with a pure liquid and an
other with a mixture of liquids, and found that although the overall gas holdup in these two
systems matched within allowable statistical difference (11 %), the power spectra in these
156
systems were different. Thus, even though the systems were globally similar, their local
behavior differed. The current work sought to evaluate whether maintaining the hypothesis
proposed in this work would provide similar hydrodynamic performance, even if one
system had a pure liquid and the other one had a mixture of liquids.
Figure 6-8a shows close gas holdup radial profiles in this case, except close to the center of
the column. An AARD in gas holdup radial profiles is within 4 %. Figure 6-8b shows the
(a)
(b)
stainless steel column [D6P1U30 C9-C11: 6 inch diameter column, 1 bar, 30 cm/s (Han,
2006), and air- C9-C11 fluid system, D6P4U30water: 6 inch diameter column, 4 bar, 30
cm/s, and an air-water system] [Overall gas holdup ~ 0.35].
[D6P1U30C9-C11 (Han, 2006) and D6P4U30water] along the column radius in a 6
diameter stainless steel column.
157
Figure 6-10: TKE radial profile in a 6 diameter stainless steel column (D6P1U30 C9-C11: 6
inch diameter column, 1 bar, 30 cm/s, and air- C9-C11 fluid system, D6P4U30water: 6 inch
diameter column, 4 bar, 30 cm/s, and an air-water system) [Overall gas holdup ~ 0.35].
liquid axial velocities in these cases. An AARD in the liquid axial velocity profile was
found to be close, within 14 %. As in other cases, the maximum ARD (120 %) was found
at the inversion point. The values of the velocities at this point are 0.93 and 3.85 cm/s.
The positive and negative values of liquid velocity led to a higher ARD at the inversion
point. The mean liquid recirculation velocity in an air-water system was 42 cm/s, while in
an air-C9C11 system it was 41 cm/s. The relative difference of mean recirculation
velocities in this set is 3 %, indicating similar liquid recirculation in these systems. Figure
6-10 shows the radial profile of TKE with an AARD of 8.5 %, reflecting similar
distributions of TKE at these conditions that indicate a similar mixing intensity in these
systems.
Based on this set of experimental conditions, we have demonstrated that maintaining the
hypothesis proposed in the current work results in similar liquid recirculation and mixing
intensity, even if one system has pure liquid and other one has a mixture of liquids. It
shows that bulk liquid physical properties are sufficient to describe the liquid phase only
when the gas holdup radial profiles are matched in two systems.
Using the identified sets of similarity experiments, we demonstrate that overall gas holdup
and gas holdup radial profiles in two systems need to be similar for similar hydrodynamic
158
performance. Additionally, to demonstrate the essence of similarity of both of these
parameters, the experiments were performed at mismatch conditions. The reason to
perform these experiments is to further buttress the proposed hypothesis.
Figure 6-11a shows a set of experimental conditions where the overall gas holdup is the
same, i.e., 0.35. Although the overall gas holdup is the same, the gas holdup radial profiles
in these cases are mismatched. AARD, of gas holdup radial profile between 30 cm/s and 4
bar in an air-water system and 16 cm/s and 4 bar in an air-C9C11 system, is 13 %. The
mismatched gas holdup radial profiles result in different liquid axial velocities (Figure 611b). An AARD in liquid axial velocities is 35 %. Figure 6-12 shows that, similar to earlier
sets of experiments, the maximum ARD is near the inversion point (r/R = 0.8); moreover,
the ARD in axial velocities at the remaining radial locations was consistently above 20 %.
The mean recirculation velocity at 30 cm/s and 4 bar in an air-water system was 42 cm/s,
while at 16 cm/s and 4 bar, it was 30 cm/s. The relative difference between mean liquid
(a)
(b)
stainless steel column (D6P4U30water: 6 inch diameter column, 4 bar and 30 cm/s, an airwater; D6P4U16C9-C11: 6 inch diameter column, 4 bar and 16 cm/s, air- C9-C11) [Overall
gas holdup ~ 0.35].
159
(D6P4U30water and D6P4U16C9-C11) along the column radius in a 6 diameter stainless
steel column.
Figure 6-13: TKE radial profile in a 6 diameter stainless steel column (D6P4U30water: 6
inch diameter column, 4 bar and 30 cm/s, an air-water; D6P4U16C9-C11: 6 inch diameter
column, 4 bar and 16 cm/s, air- C9-C11) [Overall gas holdup ~ 0.35].
recirculation velocities was 28 %. The radial profile of TKE at these conditions was
compared to evaluate how the mismatched gas holdup radial profiles affect mixing
intensity. Although the qualitative distribution of TKE appears to be similar at these
160
conditions, there exists a significant quantitative difference in their magnitudes. An
AARD in the radial profile of TKE was found to be around 27 %, as shown in Figure 613.
Figure 6-14 shows one more set of mismatch experimental conditions (30 cm/s and 4 bar in
an air-water system, and 8 cm/s and 10 bar in an air-C9C11 system). The overall gas
holdup at these conditions is 0.35; however, an AARD in gas holdup radial profiles is 25
%. The mismatched radial profiles result in entirely different liquid recirculation velocities,
with an AARD in velocities close to 48 %. In this case also, the ARD of liquid axial
velocities (Figure 6-15) is consistently above 40 %. The mean recirculation velocity at 30
cm/s and 4 bar in an air-water system is 42 cm/s, while at 8 cm/s and 10 bar, it is 22 cm/s.
The relative difference between mean liquid recirculation velocities is 47 %. Figure 6-16
shows the radial distribution of
(a)
(b)
stainless steel column (D6P4U30water: 6 inch diameter column, 4 bar and 30 cm/s, an airwater; D6P10U8C9-C11: 6 inch diameter column, 10 bar and 8 cm/s, air- C9-C11) [Overall
gas holdup ~ 0.35].
161
(D6P4U30water and D6P10U8C9-C11) along the column radius in a 6 diameter stainless
steel column.
Figure 6-16: TKE radial profile in a 6 diameter stainless steel column (D6P4U30water: 6
inch diameter column, 4 bar and 30 cm/s, an air-water; D6P10U8C9-C11: 6 inch diameter
column, 10 bar and 8 cm/s, air- C9-C11) [Overall gas holdup ~ 0.35].
TKE at these conditions. An AARD in the radial profile of TKE is around 45 %. One
should note here that in this case there exist both qualitative and quantitative differences in
TKE. The distribution of TKE at 8 cm/s and 10 bars appears to be uniform, possibly
because of the relatively uniform gas holdup radial profile.
162
6.3a Discussion
Based on the sets of mismatch experiments, two points are worth mentioning:
a) The radial or cross-sectional distribution of gas holdup indicates that the second set
of mismatch experiments has one condition (30 cm/s, 4bar, an air-water) operating
in the churn-turbulent flow regime, while the other condition (8 cm/s, 10 bar, airC9-C11) appears close to bubbly or transition flow although they have similar overall
gas holdups. It shows that to be hydrodynamically similar it is necessary that both
the systems, apart from having similar global hydrodynamics, should operate in the
same flow regime. Operation in the same flow regime ensures that bubble
interaction and dynamics in these systems are similar.
b) It is clear from the radial or cross-sectional distribution of gas holdup in the first set
of mismatch experiments that both the systems operate in the churn-turbulent flow
regime. However due to mismatched gas holdup radial profiles, these systems show
different liquid recirculations and mixing intensities. Hence the combination of two
sets of mismatch experiments shows that the condition that two systems must
operate in the same flow regime to be hydrodynamically similar is necessary but
not sufficient. It shows the importance of matching gas holdup radial profiles or
cross-sectional distributions in two systems, even if both systems operate in the
same flow regime.
The current work combines the set of similarity and mismatch experiments and
demonstrates that to be hydrodynamically similar, it is necessary to have similarity of both
overall gas holdup and gas holdup radial profile. The similarity conditions showed that
similar overall gas holdup and gas holdup radial profiles resulted in close liquid
recirculation and mixing intensity in both systems. The mismatch experiments had similar
overall gas holdups but mismatched profiles, and resulted in varied liquid recirculation and
mixing intensity. This clearly shows that maintaining similar overall gas holdup alone can
lead to different recirculation and mixing, if gas holdup radial profiles are not matched.
Although overall gas holdup determines the magnitude of macroscopic hydrodynamics, the
163
microscopic flow dynamics are controlled by gas phase motion due to the gradient of
buoyancy forces between the column center and the wall region. In churn-turbulent flow
regime, there exists an unequal distribution of gas holdup along the column cross-section,
with higher gas holdup in the center and lower holdup in the wall region. A similarity based
solely on overall gas holdup masks such distribution and lumps it into one global
parameter. This simplistic approach lead to different mixing and flow patterns, as the
momentum transferred by the gas phase motion is responsible for the liquid recirculation in
such flows.
In bubbly flow, the distribution of bubble size is narrow and uniform along the column
cross-section, resulting in relatively flat gas holdup radial profiles. Due to the absence of
nonuniform microscopic flow behavior; the determining factor in bubbly flow is the
magnitude of the macroscopic hydrodynamics. Hence, the similarity of global parameters
can be specifically applicable if both the systems operate in bubbly flow, and it may result
in similar liquid recirculation and mixing intensity. To corroborate this fact, experiments
with different operating conditions with the same overall gas holdup in bubbly flow were
identified to evaluate whether these conditions inherently have similar gas holdup radial
profiles. Two sets of such conditions extracted from the CREL database are reported here.
Figure 6-17 shows a set of experimental conditions with an overall gas holdup close to 0.1.
One condition is at 2 cm/s and 1 bar in an air-water system (Ong, 2003), while other one is
at 3 cm/s and 1 bar in an air-Therminol LT system (Shaikh and Al-Dahhan, 2005). Based
on overall gas holdup studies performed in the respective studies, it is clear that both these
conditions are in bubbly flow. The gas holdup radial profiles were close to each other, with
AARD of 6 %. Figure 6-18 shows another set of conditions operating in the bubbly flow
regime with an overall gas holdup of 0.22. In this set, one conditions is at 5 cm/s and 4 bar
in an air-Therminol LT system (Shaikh and Al-Dahhan, 2005), while other one is at 3.5
cm/s and 10 bar in an air-Therminol LT system (Shaikh and Al-Dahhan, 2005). The gas
holdup radial profiles at these conditions were found to be close, with an AARD of 4.5 %.
These results show that when both operating conditions fall in bubbly flow, the similarity
of overall gas holdup necessarily results in similar gas holdup radial profiles. As shown
164
earlier, such close gas holdup radial profiles would subsequently result in similar liquid
recirculation and mixing intensity. From the above comparisons, it is evident that similarity
based on global parameters can be generalized only when both the conditions are in bubbly
flow, because the magnitude of macroscopic hydrodynamics is the controlling
hydrodynamic parameter in the presence of uniform holdup distribution across the column
cross-section.
Figure 6-17: Gas holdup radial profile in a 6 diameter stainless steel column
(D6U2P1water: 1 bar and 2 cm/s, an air-water; D6U3P1TherminolLT: 1 bar and 3 cm/s,
air- Therminol LT) [Overall gas holdup ~ 0.1].
Figure 6-18: Gas holdup radial profile in a 6 diameter stainless steel column
(D6U5P4TherminolLT: 4 bar and 5 cm/s, air-Therminol LT; D6U3.5P10Therminol: 10 bar
and 3.5 cm/s, air- Therminol LT) [Overall gas holdup ~ 0.22].
165
The current work cautions against the generalization of similarity criteria based only on
global parameter. It was demonstrated that similarity of global parameters does not
necessarily ensure similar hydrodynamic performance, particularly in the churn-turbulent
flow regime. The similarity of gas holdup and its distribution along the cross-section are
pertinent in obtaining similar recirculation and mixing intensity in two systems.
6.4 Development of correlations for a priori prediction of hydrodynamic parameters
In a nutshell, this work has proposed a hypothesis for hydrodynamic similarity and
successfully evaluated utilizing CT and CARPT. However to facilitate the proposed
methodology for scaleup/scaledown purposes, it needs modeling tools to a priori predict
the needed hydrodynamic parameters. An ideal choice for such a task would be
fundamentally based Computational Fluid Dynamics (CFD) models. However, Rafique et
al. (2005) showed that interfacial closures are still an unresolved issue, and tuning the
coefficients to a known field is still a state-of-the-art practice. Additionally, available
closures do not account for the effect of turbulence. Chen (2005) implemented the
Population Balance approach where the bubble population balance equation was solved
simultaneously with solution of the flow field. In the churn-turbulent flow regime, Chen
(2005) model predicted a coalescence rate an order of magnitude higher than that of a
break-up rate. Therefore bubble diameter does not reach equilibrium, which is in contrast
with experimental observations. Hence, Chen (2005) enhanced the breakup rate to be 10
times the predicted one, in order to match experimental flow field results. He then found a
good agreement between model predictions and experimental data in different air-liquid
systems. This shows that even after incorporating detailed science, there are still unresolved
issues. Hence CFD, although certainly a promising tool, is not yet ready for use in the
design and scaleup of bubble columns.
In the absence of fully resolved CFD, the current work resorted to a state-of-the-art
modeling tool, the Artificial Neural Network (ANN). Correlations for the following
hydrodynamic parameters were developed:
i)
Overall gas holdup
166
ii)
Gas holdup radial profile
iii)
Liquid axial velocity radial profile
iv)
Center-line liquid velocity
A brief introduction to ANN and the development of the correlations using ANN for the
hydrodynamic parameters mentioned above is discussed in Appendix-F.
6.5 Remarks
Based on a comprehensive review of reported scaleup procedures in literature and industry,

the current work proposes a new hypothesis for hydrodynamic similarity and subsequently
for scale-up of bubble column reactors. The hypothesis requires the similarity of overall gas
holdup as well as of gas holdup radial profile. It was evaluated using single source -ray CT
and CARPT. The conditions of similarity where overall gas holdup and radial gas holdup
profiles were the same, and mismatch where overall gas holdup was the same but gas
holdup radial profiles were different, have been identified. The combination of similarity
and mismatch experiments shows the importance of maintaining the gas holdup radial
profiles the same, not just the overall gas holdup. Such similarity exhibited the similar
liquid circulation and mixing intensity in two systems.
This work also showed that the condition that two systems must operate in the same flow
regime to be hydrodynamically similar is necessary but not sufficient. It showed the
importance of matching gas holdup radial profiles or cross-sectional distributions in two
systems, even if both the systems operate in the same flow regime. Hence, the traditionally
used criterion for hydrodynamic similarity, based only on global parameters, can be fatal
and needs to be exercised with prudence.
The hypothesis proposed in this work has been evaluated in different systems and
operating conditions. However it needs to be evaluated at two different scales. Industrial
167
reactors often consist of internals such as sieve trays and heat exchangers, hence the
applicability of the proposed hypothesis needs to be checked in such systems.
168
Chapter 7
Summary and Recommendations
The main objectives set for this work are to advance the state of knowledge of key
hydrodynamic parameters of bubble and slurry bubble column reactors at mimic
industrial conditions in the context of FT synthesis, using existing noninvasive techniques
such as CARPT and CT. This work was also planned to develop experimental techniques
and their flow regime identifiers for flow pattern delineation that can be useful for online
monitoring in the laboratory as well as in industrial scale reactors. With the aid of stateof-the-art experimental and modeling tools, this work proposed and evaluated a new
hypothesis for hydrodynamic similarity and subsequently for scaleup of bubble column
reactors.
7.1 Summary and Conclusions

The key findings in this work are as follows:
1. The effect of liquid phase physical properties was studied by comparing the phase
holdup profiles obtained in an air-Therminol LT-glass beads with that of an air-waterglass beads system in bubbly and churn-turbulent flow at ambient and high pressure
(1 MPa). At ambient pressure, the comparison of the gas and solids holdup radial
profile in an air-Therminol LT-glass beads and an air-water-glass beads revealed that
in bubbly flow the magnitude of the gas holdup profile is higher in water, while in
churn turbulent flow; it is higher in Therminol LT. In transition flow, closely similar
gas holdup radial profiles were observed in water and Therminol LT. An increased
gas holdup in water in bubbly flow was due to the S-shaped behavior of the overall
gas holdup curve at the studied condition. An opposite effect of the superficial gas
velocity was observed on the solids holdup radial profile. At high operating pressure
(1 MPa), the change in the liquid phase to Therminol LT consistently increased the
169
magnitude of the gas holdup radial profile due to an increased bubble breakup rate
and decreased coalescence rate that produced more small bubbles. This effect resulted
in a relatively flatter profile in Therminol LT. The solids holdup radial profile
decreased with an increase in superficial gas velocity.
2. An addition of solids in slurry reduces the magnitude of the gas holdup radial profile
due to a higher coalescence rate that produces more large bubbles in the system. The
higher population of large bubbles concentrated at the center and resulted in a steeper
profile at increased solids loading, it thereby advanced flow regime transition. An
addition of solids linearly increased the solids holdup profile at both pressures. At
high operating pressure and high solids loading, the gas holdup radial profile showed
a consistently steeper profile. The shape of the profile at this condition is qualitatively
similar to the one observed at low solids loading and ambient pressure.
3. Within the studied experimental conditions, the effect of superficial gas velocity on
the overall gas holdup was weaker than that of operating pressure and solids loading.
The effect of the studied operating parameters on the solids holdup profile was less
significant than on the gas holdup radial profile.
4. The solids holdup profiles at all the axial locations showed the similar shapes, and fell
on each other at a given operating condition. The normalized solids holdup at low
superficial gas velocities showed similar shape and fell on each other, while the
normalized solids holdup at higher superficial gas velocities showed similar and
relatively steeper shapes and fell on each other within a band of relative error of 10
%. The normalized solids holdup radial profile in water and Therminol LT showed
the similar shapes and fell on each other at all the studied conditions, except in bubbly
flow at ambient pressure. This shows that the solids flow behavior in these systems
was qualitatively similar. However, the differences were to the different liquid phase
5. In general, a slurry bubble column exhibited a single circulation cell in fully
developed flow in a time-averaged sense. The solids moved upward at the center, and
moved downward near the wall. The pdf of solids axial velocity revealed that
although the net flow in the center is upward, a few negative velocities existed.
Correspondingly, the net flow near the wall is downward, a few positive velocities
170
were noted. Near the vortical region, comparable positive and negative velocities
were present, causing vigorous fluctuations. The axial solids velocity showed the
inversion point around a dimensionless radius of 0.7, while the shear stress showed a
maximum in the center of the column radius.
6. Comparison with an air-water-glass beads system shows an increased solids axial
velocity and shear stresses in an air-Therminol LT-glass beads system. However, due
to the presence of smaller bubbles in an air-Therminol LT-glass beads system, there
was less TKE and normal stresses. The qualitative flow behavior in both the systems
was similar, the quantitative differences exist due to different liquid phases.
7. An addition of solids tended to decrease the solids axial velocity, due to decrease in
the gas holdup. However, an addition of solids results in enhanced turbulence in the
system, due to an increased large bubble population.
8. The existing CT was evaluated for flow regime identification in bubble column
reactors. The evolution of the steepness of the gas holdup radial profile with
superficial gas velocity was analyzed, and the break-point in the steepness
parameter curve was found to reveal information regarding transition velocity. The
transition velocity obtained from the steepness parameter curve was evaluated with
traditional methods such as the change in the gas holdup curve and the drift flux plot
and found to be in good agreement. The effect of operating pressure on the flow
regime transition was studied using the developed methodology. The transition
velocity was found to increase with an increase in operating pressure. Also, it was
observed that the change in the flow regime was noticeable at ambient conditions,
while at higher pressure a gradual change occurred over a region of superficial gas
velocities. The obtained transition velocities were compared with the predicted
transition velocities using the correlations of Wilkinson (1991) and Reilly et al.
(1994). Both correlations noticeably underpredict the experimental transition
velocities, hence the state of current correlations needs to be further improved.
9. The feasibility of NGD for flow regime demarcation in bubble column reactors was
explored. The well-known air-water system was utilized to propose promising flow
regime identifiers. The flow regime boundaries were determined based on
conventional methods such as the change in the slope of the gas holdup curve and the
171
drift flux plot. The photon counts history obtained using NGD was subjected to
statistical analysis, autocorrelation analysis, and spectral analysis. Based on the
comparison of such time-series analyses with those of conventional methods,
promising flow regime identifiers for NGD were proposed. In general, the photon
counts history revealed the signatures of the underlying flow regime. Based on the
inherent nature of gamma-ray emission, a new parameter called the coefficient of
departure from a Poisson distribution was proposed and found to be greater than 1.4
for churn-turbulent flow regimes. The autocorrelation analysis exhibited different
behavior in bubbly and churn-turbulent flow regime. Spectral analysis showed a
distinct power-law fall off in the transition and the churn turbulent flow regime, while
no such power law fall-off was observed in the bubbly flow. The proposed flow
regime identifiers for NGD provide a promising method for online flow regimes
monitoring in laboratory as well as industrial scale reactors. Furthermore, the
developed flow regime identifiers were evaluated in different systems (air-water and
air-C9-C11) at different pressures (0.1 and 1 MPa) in a stainless steel column and
found to be consistent.
10. A new hypothesis was proposed for hydrodynamic similarity and subsequently for the
scale-up of bubble column reactors. It emphasizes the similarity of the overall gas
holdup as well as the gas holdup radial profile. A combination of similarity and
mismatch experiments showed the importance of maintaining the gas holdup radial
profiles the same, in addition to the overall gas holdup. Such similarity exhibited the
similar liquid circulation and mixing intensity in two systems. We showed that the
traditionally used criteria for hydrodynamic similarity based only on global parameters
can be fatal and advised that it be exercised with prudence. In addition, ANN based
correlations were developed for a priori prediction of the needed hydrodynamic
parameters.
7.2 Recommendations
The work accomplished in the last two parts of current study is, in retrospect, generic to
multiphase reactors, with bubble columns as an example. Hence, it provides promising
172
avenues to implement similar concepts in different configurations of multiphase reactors.
The few suggestions for possible extension of the work performed in different parts are
listed below:
1. Most hydrodynamic studies reported in the literature deal with systems where the
aspect ratio (L/D) was maintained equal to or above 5. The reason for performing
such studies lies in the general observation that if L/D > 5, the effect of column height
on hydrodynamics is not significant. However the demands of high throughput
necessitate industrial reactors to have a larger column diameter, often equal to or
greater than 5 m. In these cases, the column height is often restricted due to the
limitations on the weight of reactor allowable for transportation. Hence these reactors
have L/D lower than commonly studied in the literature. Very few studies have been
performed in this regard, and they are limited to overall gas holdup and mass transfer
coefficient. Detailed studies regarding low L/D and its effect on the hydrodynamics,
using CARPT and CT, will be beneficial for the design of industrial reactors.
2. This work evaluated the capability of CT for flow regime identification based on the
steepness of the gas holdup radial profiles. The systematic data obtained for the flow
regime transition studies using CT can be further analyzed using chaos analysis,
symbolic dynamic analysis, and S-statistics.
3. This work developed a new technique utilizing NGD for online flow regime
identification in bubble column reactors. The same technique can be extended for
flow monitoring in other multiphase reactors. The possibility of applying NGD for
flow regime monitoring in packed beds, fluidized beds, circulating fluidized beds, and
spouted beds should be considered. The applicability of flow regime identifiers
developed using NGD for bubble column reactors can be evaluated for other
configurations, and if needed, new flow regime identifiers specific to those
configurations can be proposed.
173
4. Due to the requirement of using the time-series techniques that are simpler, faster,
robust, and easily used by non-experts in the plant, a basic time-series analysis was
performed on photon counts history obtained using NGD. However one can use
sophisticated time-series techniques such as chaos analysis for flow regime
delineation. In addition, one can apply symbolic dynamic analysis, 2- analysis, and
S-statistics to evaluate their feasibility for flow regime monitoring in bubble columns.
5. There has always been considerable interest in demarcating as well as understanding

the flow regime transition. Towards this, there were attempts to describe flow regimes
and, in particular, flow during transition. However, the descriptions provided by Ohki
and Inoue (1979) and Olmos et al. (2003) are in contradiction with each other and
also with the one explained by Nedeltchev et al. (2003), which was based on the
quality of mixedness. As a preliminary evaluation of these explanations by various
authors, one can perform 4-point optical probe experiments within the flow regime
transition region at specific axial locations. High-speed camera images along with
these experiments would certainly aid in enhancing our fundamental understanding.
6. This work successfully evaluated the proposed hypothesis for hydrodynamic

similarity of bubble column reactors. Before investing efforts to extend it to different
diameter columns using CT and CARPT, as a first step the hypothesis was evaluated
in the same column at widely different operating conditions and using different
liquids. The successful evaluation of the proposed hypothesis provides an opportunity
to evaluate the proposed hypothesis at different scales.
7. The proposed hypothesis for dynamic similarity and subsequently, for scaleup needs
modeling tools for design engineers. In this work, combination of ANN based tools
for different hydrodynamic parameters were developed based on the reported
database available over wide range of operating and design conditions. However the
reactor scale models based on first principle needs to be evaluated for this purpose.
Based on CFD studies of Chen (2005), the improved breakup closures need to be
implemented during such an exercise.
174
8. The scaleup methodology developed in this work can be evaluated in other

multiphase reactors such as fluidized beds, spouted beds, and CFBs. In the literature,
there have been attempts to study the scaleup of these reactors. However, these
methods also rely on the similarity of global parameters for dynamic similarity in two
systems. The scaleup hypothesis proposed for bubble columns during this work, in
retrospect, is generic for multiphase reactors. Hence the scaleup rules proposed for
these reactors should be revisited in the light of the hypothesis developed in this
work.
175
APPENDIX A.
Phase Distribution in Three Dynamic Phase Systems via
Combination of Computed Tomography (CT) and
Electrical Capacitance Tomography (ECT)
A-1 Background
Although many tomographic techniques have been developed over the past 5-10 years
(Williams and Beck, 1995), few are readily applicable to three-phase systems. In threephase systems, the requisite sensed signal contains information that is a function of more
than one parameter in the object space. Most tomographic techniques are single modal
systems that can not be applied for multiple sensing in three phase flows. Approaches
adopted by the researchers to tackle this problem have been classified in the following
three categories:
I)
combining two single-modal systems
II) using an inherently multi-modal system

III) modifying reconstruction techniques of single-modal system to accommodate three
dynamic phases.
The example of combination of two single modal systems in medical field is the
combination of X-ray CT (which illustrates bone structures but remains insensitive to soft
tissues) with magnetic resonance imaging (MRI) (which distinguishes between diseased
and healthy tissues but remains insensitive to bony structures). Such measurement can
provide surgeon with the position of the diseased tissue relative to the bone structure
(Beck, 1995). In multiphase reactors research there have been considerable efforts
towards developing multi-modal systems for three dynamic phase flow imaging.
A-1.1 Approach I: Combining two single-modal techniques

Table A-1 summarizes the reported investigations that use approach I.
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Table A-1: Summary of the studies combining two single-modal systems

Author
Combination
Comments
Seo and
Gidaspow
(1987)
Johansen et
al. (1996)
X-ray densitometry
and -ray densitometry
(GDT)
Electrical Capacitance
Tomography (ECT)
and GDT
-ray densitometry
with two different
sources
Measured volume fraction of particles and of

the gas in fluidized bed involving particles of
two sizes.
Studied the gas phase distribution in threecomponent flows of gas, oil, and water.
Bukur et al.
(1996)
George et al.
(2001)
Grassler and
Wirth (2001)
Failed in implementation in slurry bubble

columns. Suggested using sources with widely
different energy levels such as, Cs 137 and
Am.
Electrical Resistance
Three phase system was chosen such that GDT
Tomography (ERT)
was used to measure gas fraction while ERT to
and GDT
measure solids fraction.
Dual energy X-ray Applied in slurry bubble column. Not
tomography
applicable at high pressure due to excessive
attenuation.
A-1.2 Approach II: Using an inherently multi-modal system

Using the second approach, Warsito et al. (1995) implemented a dual-frequency
ultrasonic method, and Warsito et al. (1999) developed an ultrasonic tomographic (UT)
technique with two-parameter sensing, i.e., energy attenuation and sound speech to
measure simultaneously the three dynamic phase holdups. Vatankul et al. (2004)
correlated the fluctuations of sound waves, in terms of variance of transmission time and
amplitude ratio, with gas and solids holdup. Warsito et al. (1997) and Soong et al. (1995)
showed that the speed of ultrasound is independent of gas holdups, while Macchi et al.
(2001a) and Vatankul (2003) showed that gas bubbles do affect sound velocity due to the
distortion of ultrasound around bubbles. There remains a discrepancy regarding the key
177
assumption in reconstructing phase holdups using UT. In addition, due to its high signal
non-linearity the technique is limited to bubbly flow and very low solids holdup.
A-1.3 Approch III: Modifying reconstruction technique of single- modal system

Table A-2 summarizes the reported investigations that use approach III.
Table A-2: Studies that modified the reconstruction technique of single-modal techniques
Authors
Technique
Nooralahiyan
and Hoyle
(1997)
Electrical
Capacitance
Tomography
(ECT)
Warsito and
Fan (2001,
2003)
Rados et al.
(2004)
Comments on Reconstruction Technique
Feedforward neural network (NN) with double

sigmoid function used to image three dynamic
phase flows. Reconstruction is fast once training
has been done but network training is the major
disadvantage for real applications.
Electrical
Hopfield neural network with multicriterion
Capacitance
optimization technique. Does not need prior
Tomography
training. Uniform solids loading assumption
(ECT)
applied for three dynamic phase imaging.
Single source - Combines CT with overall gas holdup
ray Tomography measurements,
along
with
two
sound
assumptions[uniform solids loading and overall gas
holdup equal to cross-sectional gas holdup].
Applied in different systems at low as well as high
pressure.
Approach III is an attractive option for phase holdup measurement in three-phase systems
as it is easy to construct and implement. However, the obtained results need to be
evaluated and the validity of the improved reconstruction technique and the assumptions
used therein need to be defined. As discussed above, with the current state of imaging
techniques, while Approach III remains to be in development stage, Approach I can be
used for such evaluation. This makes it necessary to demonstrate the possibility of
coupling two single-modal tomographic techniques and evaluate the assumptions
incorporated in Approach III (Table A-2).
A-2 Combination of CT/ECT
178
Based on this, the focus is to establish and implement the possibility of the combination of
two single-modal tomographic techniques, viz., single source -ray CT and Electrical
Capacitance Tomography (ECT). This study consists of two parts:
i) Development of the CT/ECT algorithm.
ii) Execution of the CT/ECT experiments.
A-2.1 Development of the CT/ECT algorithm
As this methodology combines two single modal systems, the development of a system of
equations to resolve three dynamic phase holdups consists of combining CT and ECT
equations. The single source -ray CT equation will be coupled with Two-Region Three
Phase Capacitance Model proposed by Warsito and Fan (2003), which is modified for the
current case. Such a coupling yields a system with a similar number of non-linear algebraic
equations as the unknowns, i.e., the phase holdups.
Based on the ECT data, the permittivity distribution will be estimated at Ohio State
University using Neural Network Multi Objective Iterative Reconstruction Technique
(NNMOIRT). The CT experiments were conducted under the similar experimental
conditions and the attenuation distribution was estimated using the EM algorithm
implemented by Kumar (1994). The CT/ECT algorithm developed in the current work
couples the attenuation and permittivity distribution to evaluate three dynamic phase
holdups. A user friendly compact software is developed for CT/ECT combination using
HYBRD subroutine.
This part essentially involves combining CT and ECT equations to form a system of
equations that can resolve three dynamic phase holdups. The needed ECT equation has
been derived from the three-phase two-compartment model proposed by Warsito and Fan
(2003), which has been modified to accommodate the current case.
179
According to Warsito and Fan (2003), the system is divided into two compartments, viz.,
gas and liquid-solid emulsion. The series and parallel combinations of these two
compartments can be represented, respectively, as
1
eGLS , s
G
eG
(1 G )
e LS
e GLS , p = G e G + (1 G )e LS
(A-1)
(A-2)
where eLS is the permittivity of the solid-liquid emulsion phase.

Further, the liquid-solids emulsion has been divided into two compartments, viz., liquid
and solid. These two compartments has also been arranged in parallel and series
combinations as
(1 SE )
1
= SE +
e LS , s
eS
eL
(A-3)
e LS , p = SE e S + (1 SE )e L
(A-4)
where, eS and eL are the dielectric constants of the solid and liquid phase. While SE is
solids loading which is defined as,
SE =
S
1 G
(A-5)
The gas holdup in three phase system can be calculated by the possible series and parallel
combinations between liquid and solids phase within the emulsion and between the gas
and emulsion phases as follows
G = ss G ,ss + sp G ,sp + ps ps + pp G , pp
(A-6)
ss + sp + ps + pp = 1
(A-7)
where, is a constant between 0 and 1. The subscripts s and p denote series and parallel
capacitance connections between the liquid and solid in the emulsion phase for the first
180
subscript and between the gas and the emulsion phase for the second subscript. In the
present case, constant was equally weighted.
Relative permittivity, rk for phase k can be defined as,
rk = ek / eG
(A-8)
where k can be L (liquid), S (solid), LS (liquid-solid), or GLS (slurry experiment).

The resultant permittivity will be the equal contribution of above mentioned
combinations. The combination of these equations yields following ECT equation.
1
rGLS , ss + rGLS , sp + rGLS , ps + rGLS , pp
4
rGLS =
rS rL
rS SE + rL (1 SE )
1
+
4 rS rL G + (1 G )[rL SE + rS (1 SE )] G {rS SE + rL (1 SE )} + (1 G )
+ 2 G +
rS rL (1 G )
+ (1 G ){rS SE + rL (1 SE )}
rL SE + rS (1 SE )
(A-9)
For three dynamic phase systems the resultant CT equation can be written as (Rados et
al., 2005),
RGS ,ij
G ,ij =
S ,ij
+ RL ,ij 1 S ,ij RGLS ,ij
0
S
RL ,ij
The above equation can be rearranged as,
RGLS = (1 G ) RGS SE + RL (1 SE )
S0
(A-10)
As defined in equation (5) solids holdup can be calculated as,
S = SE (1 G )
(A-11)
181
The above system of equations has three non-linear algebraic equations i.e. (A-9), (A-10),
and (A-11) with three unknowns i.e. G , S , and SE . These equations need to be solved
simultaneously to compute gas holdup, solids holdup, and solids loading in each pixel
using Newton-Raphson Method. The pixel size being used in ECT data processing will
be 32x32; hence, during the CT data processing pixel size was reduced to 32 x 32.
A-2.2 Execution of CT/ECT experiments
The experimental part of this study needs to execute the CT and ECT experiments using the
similar operating and design conditions. Therefore, the experiments were performed at
Washington University (WU) using CT and at Ohio State University (OSU) using ECT at
the similar operating and design conditions. A plexi-glass column of the same dimensions
(diameter = 10.12 cm, height = 120 cm, Figure 5-12) as OSU has been constructed at
Washington University. Air was used as the gas phase, while Norpar15 ( = 2.53 cP, =
773 kg.m-3, = 26.4 dyne.cm-1) was used as the liquid phase. Glass beads with an average
diameter of 200 m and particle density of 2500 kg.m-3 constituted the solids phase. Table
A-1 shows the experimental conditions for this part of the work.
Sparger Solids loading Superficial gas velocity (cm/s) Axial location

(% volume)
(L/D)
S1
40
5, 10,15
2, 5.5
S2
9.1, 25
5, 15
2.5, 5.5
CT/ECT
Table
A-1
Experimenta
l conditions
for
the
coupling of
182
S1: Single hole of size 5 mm, S2: 64 holes of 1 mm size, % OA = 1.09, triangular pitch
A-3 Results
As mentioned earlier, the main goal of this work is to combine attenuation distribution
obtained using CT with the permittivity distribution obtained using ECT. The data
processing of CT data was completed while that of ECT is still in progress. Hence in this
section the cross-sectional attenuation distribution (cm-1) obtained using CT is presented
in 32 X 32 pixel form.
z/D = 2
z/D = 5.5
(a)
z/D = 2
z/D = 5.5
183
(b)
Figure A-1: Cross-sectional attenuation distribution (cm-1) of a) 200 m glass beads (with
voids) and b) Norpar 15.
z/D = 2
z/D = 5.5
(a)
z/D = 2
z/D = 5.5
184
(b)
z/D = 2
z/D = 5.5
(c)
Figure A-2: Cross-sectional attenuation distribution (cm-1) using air-Norpar 15-(200 m
glass beads in 4 diameter column at ambient conditions, two axial locations, and solids
loading of 40 % volume at Ug = a) 5, b) 10, and c) 15 cm/s with a single nozzle sparger.
185
Ug = 5 cm/s
Ug = 15 cm/s
(a)
(b)
Figure A-3: Cross-sectional attenuation distribution (cm-1) using air-Norpar 15-(200 m
glass beads in 4 diameter column at ambient conditions, z/D = 5.5, two superficial gas
velocities and solids loading = a) 9.1, b) 25 % volume with a uniform sparger.
186
Once ECT data processing is completed, the combination of permittivity and attenuation
distribution can provide phase holdups distribution in three dynamic phase systems
without any assumptions.
186
APPENDIX B
Experimental Investigation of Hydrodynamics of Slurry
Bubble Column Reactor via CT
B-1: Experimental setup and employed sparger
Top
Cover
6 3/8
Gas
Outlet
Demister
4 3/4
12
View Port
(6 staggered, 3 on
each
radially opposite side,
16 1/2
CT 3
DP
1
Probe
21 1/2
CT 2
90
DP
21 1/2
CT 1
DP
8 3/4
Batch
Drain
4 1/2
8
Liquid
Gas
Drain
Inlet
Bottom Support
13
Figure B-1: High pressure bubble column with ports used for overall gas holdup
measurement
187
Figure B-2: Sparger employed in the current studies in 6 diameter steel column
B-2 Reproducibility of CT scans

To address the issue of reproducibility of the experimental data, the conditions of Ug =
30 cm/s and P = 0.1 and 1 MPa at 9.1 % vol. solids loading was repeated with fresh batch
of liquid and glass beads. Figures B-3a and b show the gas holdup radial profile data at
z/D = 5.5 using superficial gas velocity of 30 cm/s, solids loading of 9.1 % vol. at
ambient pressure and high pressure, respectively.
Both figures indicate very good agreement between gas holdup radial profiles at ambient
and high pressure. At ambient pressure, the gas holdup radial profiles are within 2 %
while near the wall, it is 4 %. At operating pressure of 1 MPa, the gas holdup radial
profiles are within 3 % while near the wall, the differences are around 5 %. In conclusion,
the reproducibility of gas holdup radial profiles is very good. Also, the reproducibility of
solids holdup radial profile at both the pressures was found to be within 1.5 %.
188
0.7
Batch 1
Batch 2
0.6
0.6
0.5
Gas holdup (-)
Gas hol dup (-)
0.5
0.4
0.3
0.2
Batch1
0.3
Batch2
0.2
0.1
0.4
0.1
0
0.2
0.4
0.6
r/R (-)
(a)
0.8
0.2
0.4
0.6
0.8
r/R (-)
(b)
Figure B-3: Reproducibility of gas holdup radial profiles at superficial gas velocity of 30
cm/s, solids loading of 9.1 % vol., axial location of z/D = 5.5 and operating pressure of a)
0.1 MPa and b) 1 MPa using two fresh batches of air-Therminol LT-glass beads system
B-3 Effect of superficial gas velocity on gas and solids holdup radial profile
(a)
(b)
Figure B-4: Effect of superficial gas velocity on a) gas holdup, and b) solids holdup radial
profile in air-Therminol LT-9.1 % vol. glass beads system at ambient pressure in 6 steel
column
189
(a)
(b)
profile in air-Therminol LT-9.1 % vol. glass beads system at P = 1 MPa in 6 steel
column.
(a)
(b)
profile in air-Therminol LT-25 % vol. glass beads at ambient pressure in 6 steel column.
190
(a)
(b)
profile in air-Therminol LT-25 % vol. glass beads at operating pressure of 1 MPa in 6
steel column.
B-4 Effect of operating pressure on gas and solids holdup radial profile
(a)
(b)
191
(c)
(d)
Figure B-8: Effect of operating pressure on gas and solids holdup radial profile in airTherminol LT-9.1 % vol. glass beads system at Ug = a) 8, b) 14, c) 20, and d) 30 cm/s in
6 steel column
(a)
192
(b)
Figure B-9: Effect of operating pressure on gas and solids holdup radial profile in airTherminol LT-25 % vol. glass beads system at Ug = a) 20 and b) 30 cm/s in 6 steel
column
B-5 Axial variation of cross-sectional averaged phases holdup
In this section, the effect of superficial gas velocity, operating pressure, and solids
loading on axial variation of cross-sectional phases holdup will be briefly discussed. As
mentioned earlier, to reconstruct three dynamic phases using single source -ray CT, few
assumptions were incorporated. One of the assumptions is that, cross-sectional averaged
gas holdup is equal to overall gas holdup. Hence, an axial variation of cross-sectional gas
holdup has not been discussed, as the reconstructed cross-sectional averaged gas holdup
is the same as overall gas holdup within 5 % of relative error. In this section, an axial
variation of cross-sectional solids holdup is discussed.
The cross-sectional averaged solids holdup was calculated from radial profile of solids
holdup as,
s = 2 s ( )d
(B-1)
where = r/R.
Figures B-10, B-11, and B-12 illustrate the effect of operating parameters on axial
variation of cross-sectional averaged solids holdup. Solids holdup tends to decrease along
193
the column length. An increase in superficial gas velocity and operating pressure
decreases cross-sectional averaged solids holdup due to an increase in gas holdup. An
increase in solids holdup was observed with an increase in solids loading.
(a)
(b)
(c)
(d)
Figure B-10: Effect of superficial gas velocity on cross-sectional averaged solids holdup
in air-Therminol LT-glass beads system at a) solids loading = 9.1 % vol. and P = 0.1
MPa, b) solids loading = 9.1 % vol. and P = 1 MPa, c) solids loading = 25 % vol. and P
= 0.1 MPa, and d) solids loading = 25 % vol. and P = 1 MPa in 6 steel column
194
(a)
(c)
(e)
(b)
(d)
(f)
Figure B-11: Effect of operating pressure on cross-sectional averaged solids holdup in

air-Therminol LT-glass beads system at a) Vs=9.1 % vol., Ug=8 cm/s, b) Vs=9.1 % vol.,
Ug=14 cm/s, c) Vs=9.1 % vol., Ug=20 cm/s, d) Vs=9.1 % vol., Ug=30 cm/s, e) Vs=25 %
vol., Ug=20 cm/s, and f) Vs=25 % vol., Ug=30 cm/s in 6 steel column
195
(a)
(b)
(c)
(d)
Figure B-12: Effect of solids loading on cross-sectional averaged solids holdup in airTherminol LT-glass beads system at a) Ug = 20 cm/s, P = 0.1 MPa, b) Ug = 30 cm/s, P =
0.1 MPa, c) Ug = 20 cm/s, P = 1 MPa, and d) Ug = 30 cm/s, P = 1 MPa in 6 steel
column
B-6 Normalized gas holdup radial profile

In this section, the normalized gas holdup radial profile at the studied operating
conditions has been analyzed. The normalized gas holdup radial profile is the ratio of gas
holdup at certain radial location and cross-sectional averaged gas holdup. The normalized
196
gas holdup radial profiles at the studied conditions were fitted to the following empirical
form proposed by Luo and Svendsen (1992),
( G / G ) = (
n+2
)[1 c(r / R) n ]
n + 2 2c
(B-2)
where n indicates steepness of holdup profile. When n is large the profile is flat, while for
small n profile is steep. The steepness of holdup profile is reflected in the intensity of
liquid circulation. Also, c is wall holdup parameter that indicates the value of gas holdup
near the wall. If c = 1 there is zero hold up close to the wall, if c = 0 hold up is constant
with changing r/R.
Table B-1 shows the values of steepness parameter at the studied experimental
conditions. It can be observed that, in general, an increase in superficial gas velocity
decreases the value of steepness parameter and thereby changing flatter gas holdup
profiles into parabolic ones. At the same superficial gas velocity and solids loading, an
increase in pressure clearly increases the value of steepness parameter that results into
relatively flatter profiles at increased pressure. As discussed earlier, such flatter profiles
are result of an increase in small bubble population in the system at higher pressure. At
the same superficial gas velocity and operating pressure, an increase in solids loading
results into decrease in the value of steepness parameter thereby resulting into steeper
profile. As mentioned above, an addition of solids increases large bubble population that
gives rise to wide bubble size distribution and steep gas holdup radial profile with lower
gas holdup.
The careful observation of the values of steepness parameters show that the effect of
operating pressure and solids loading on normalized gas holdup radial profiles is stronger
than that of superficial gas velocity.
197
Table B-1: Values of steepness parameter, n
Superficial
gas velocity
(cm/s)
8
Pressure
(MPa)
Solids loading
(% vol.)
n
(-)
0.1
9.1
3.8
14
0.1
9.1
2.9
20
0.1
9.1
2.24
30
0.1
9.1
2.4
9.1
4.2
14
9.1
3.13
20
9.1
2.94
30
9.1
2.8
20
0.1
25
1.64
30
0.1
25
1.53
20
25
2.5
30
25
2.22
(a)
(b)
Figure B-13: Normalized gas holdup radial profile a) at different superficial gas
velocities, ambient pressure, and solids loading of 9.1 % vol. and b) at Ug = 20 cm/s and
different operating pressure and solids loading in 6 diameter steel column.
198
Figure B-13a shows the effect of superficial gas velocity on normalized gas holdup radial
profile at ambient pressure and solids loading of 9.1 % vol. in 6 diameter steel column.
An increase in superficial gas velocity, as discussed earlier, increases magnitude and
steepness of the normalized gas holdup radial profile. This clearly reflects in its steepness
parameter values. However, the effect of superficial gas velocity does not appear to have
significant effect on normalized profiles. Figure B-13b shows the normalized gas holdup
radial profiles at superficial gas velocity of 20 cm/s at low and high operating pressure as
well as solids loading in 6 diameter steel column. It can be observed that, an increase
solids loading results in steeper profile at both ambient and high pressure. An increase in
operating pressure results in flatter profile at low solids loading while the flatness of
normalized gas holdup profile due to an increased pressure is not as evident at high solids
loading. One can observe that the shapes of the normalized profiles at low solids loading
and pressure (9.1 % vol. and 0.1 MPa) and at high solids loading and pressure (25 % vol.
and 1 MPa) are close to each other.
B-7 Normalized solids holdup radial profile

In this section, the normalized solids holdup radial profile has been analyzed. The
normalized solids holdup profile is the ratio of solids holdup at any radial location and
cross-sectional averaged solids holdup.
Figures B-14a and b show the normalized solids holdup profile in air-Therminol LT-glass
beads system at Ug = 30 cm/s, P = 1 MPa, and solids loading of 9.1 % vol. and Ug = 30
cm/s, P = 1 MPa, and solids loading of 25 % vol. It can be seen that, normalized solids
holdup radial profile at all axial locations (z/D = 2.1, 5.5, 9) closely fall on each other.
Although the magnitude of solids holdup radial profile is different at various axial
locations, they follow the same qualitative behavior at a given operating condition. The
similar behavior was observed at all the performed experimental conditions.
Figures B-15a and b show the effect of studied parameters on the normalized solids
holdup radial profile at z/D = 5.5 at low and high superficial gas velocities. The
199
normalized solids holdup radial profile in Figure B-15a appears to be close and fall on
each other. Figure B-15b shows normalized solids holdup radial profile at high
superficial gas velocities where all the conditions lie in deep churn-turbulent flow regime.
The normalized solids holdup radial profiles at high superficial gas velocities are not as
close as in case of low superficial gas velocity. However, they fall on
(a)
(b)
Figure B-14: Normalized solids holdup radial profile using air-Therminol LT-glass beads
system at a) Ug = 30 cm/s, P = 1 MPa, solids loading = 9.1 % vol. and b) Ug = 30 cm/s, P
= 1 MPa, solids loading = 25 % vol. in 6 stainless steel column.
(a)
(b)
Figure B-15: Normalized solids holdup radial profile in air-Therminol LT-glass beads
system at z/D = 5.5 in 6 stainless steel column.
each other within a range of 10 % from the averaged normalized solids holdup profile.
The averaged normalized solids profile is the average of normalized solids holdup
200
profiles at all these experimental conditions. The solids holdup radial profile shows
different behavior at higher and lower superficial gas velocities as evident from Figures
B-15 a and b.
Additionally, the solids holdup radial profile can be fitted to the following form for
inverse parabola,
~
s = s (
n '+ 2
r
)[1 + c '( ) n ' ]
n '+ 2 + 2c '
R
(B-3)
where, s is cross-sectional averaged solids holdup, while n is a steepness parameter

while c is wall holdup parameter. Table B-2 shows the effect of operating parameters on
values of n and c. An increase in superficial gas velocity and solids loading reduces the
value of n while operating pressure increases the value of n. The effect of these
operating parameters on the value of c is not clear.
Earlier it was shown that the normalized solids holdup radial profiles fall on each other
within 10 % of averaged normalized solids holdup radial profile. However, based on
Table B-2, it is clear that there are significant differences in its steepness values. The
change in superficial gas velocity does not appear to have significant effect on the
steepness parameter of normalized solids holdup profile. At high superficial gas
velocities (20 and 30 cm/s), the change in operating pressure from 0.1 to 1 MPa changes
steepness parameter by 50 and 44 % at solids loading of 9.1 and 25 % vol., respectively.
An addition of solids changes steepness parameter by 8 and 11 % at 0.1 and 1 MPa,
respectively. Also, based on the significant changes in the steepness parameter, the
acceptability of 10 % as an allowable engineering tolerance for normalized solids
holdup profiles remain to be explored.
Figure B-16a shows the normalized solids holdup radial profile at Ug = 8 cm/s, P = 0.1
MPa, and solids loading = 9.1 % vol. while Figure B-16b shows the normalized solids
holdup radial profile at Ug = 30 cm/s, P = 1 MPa, and solids loading = 9.1 % vol. along
with two distinct slopes observed in the profile. However, the difference between these
201
two slopes at given condition is higher at higher superficial gas velocities. One distinct
slope lies in the region from 0 r/R 0.6 and other one is close to wall region. The slope
in the core of column is either uniform or less steep while the wall region is characterized
by relatively larger slope.
(a)
(b)
Figure B-16: Normalized solids holdup radial profile in air-Therminol LT-glass beads
system at a) Ug = 8 cm/s, P = 0.1 MPa, solids loading = 9.1 % vol., b) Ug = 30 cm/s, P =
1 MPa, solids loading = 9.1 % vol. in 6 stainless steel column with two characteristics
slope.
202
Table B-2: Steepness of solids holdup radial profile
Ug (cm/s)
P (MPa)
0.1
Solids
loading (%
vol.)
9.1
0.074
3.58
0.15
14
0.1
9.1
0.07
3.6
0.3
20
0.1
9.1
0.067
2.28
0.74
30
0.1
9.1
0.061
2.21
0.59
9.1
0.07
6.78
0.3
14
9.1
0.063
5.5
0.75
20
9.1
0.051
4.4
0.76
30
9.1
0.056
4.3
0.77
20
0.1
25
0.21
2.2
0.17
30
0.1
25
0.19
2.13
0.2
20
25
0.18
0.57
30
25
0.17
3.92
0.85
203
APPENDIX C
Experimental Investigation of Hydrodynamics of Slurry
Bubble Column Reactor via CARPT
C-1 Effect of superficial gas velocity on solids axial velocity and turbulent
parameters profile
(a)
(c)
(b)
(d)
Figure C-1: Effect of superficial gas velocity on radial profile of solids a) axial velocity,
b) turbulent kinetic energy, c) axial normal stress, and d) shear stress in air-Therminol
LT-glass beads system at P = 0.1 MPa, and solids loading = 9.1 % volume
204
100
2500
Ug = 20 cm/s
Ug = 30 cm/s
Ug = 20 cm/s
Ug = 30 cm/s
2000
60
2
TKE (cm /s )
40
1500
80
20
1000
500
-20
-40
0.2
0.4
0.6
0.8
0.2
0.4
(a)
450
Ug = 20 cm/s
Ug = 30 cm/s
Ug = 20 cm/s
Ug = 30 cm/s
400
350
2000
300
Trz (cm /s )
0.8
(b)
3000
0.6
1000
250
200
150
100
50
0.2
0.4
0.6
(c)
0.8
0.2
0.4
0.6
0.8
(d)
LT-glass beads system at P = 1 MPa, and solids loading = 9.1 % volume
205
60
3500
Ug = 20 cm/s
Ug = 30 cm/s
3000
40
2500
TKE (cm /s )
20
Ug = 20 cm/s
Ug = 30 cm/s
2000
1500
1000
-20
500
-40
0.2
0.4
0.6
0.8
0.2
0.4
0.6
0.8
(a)
(b)
300
4000
Ug = 20 cm/s
Ug = 30 cm/s
Ug = 20 cm/s
Ug = 30 cm/s
250
200
Trz (cm2/s2)
Axial normal stress (-)
3000
2000
150
100
1000
50
0
0.2
0.4
0.6
0.8
0
0
0.2
0.4
0.6
0.8
(c)
(d)
LT-glass beads system at P = 0.1 MPa, and solids loading = 25 % volume
206
(a)
(b)
(c)
(d)
LT-glass beads system at P = 1 MPa, and solids loading = 25 % volume
207
C-2 Effect of operating pressure on solids axial velocity and turbulent parameters
profile
(a)
(c)
(b)
(d)
Figure C-5: Effect of pressure on radial profile of solids a) axial velocity, b) turbulent
kinetic energy, c) axial normal stress, and d) shear stress in air-Therminol LT-glass beads
system at Ug = 20 cm/s, and solids loading = 9.1 % volume
208
100
3000
P = 0.1 MPa
P = 1 MPa
P = 0.1 MPa
P = 1 MPa
2500
60
2000
TKE (cm /s )
40
80
20
1500
1000
500
-20
-40
0.2
0.4
0.6
0.8
0.2
0.4
(a)
400
P = 0.1 MPa
P = 1 MPa
P = 0.1 MPa
P = 1 MPa
3000
300
2500
2
Trz (cm /s )
2000
0.8
(b)
3500
0.6
1500
1000
200
100
500
0.2
0.4
0.6
0.8
0.2
0.4
0.6
0.8
(c)
(d)
system at Ug = 30 cm/s, and solids loading = 9.1 % volume.
209
(a)
(c)
(b)
(d )
system at Ug = 20 cm/s, and solids loading = 25 % volume
210
(a)
(b)
(c)
(d )
FigureC-8: Effect of pressure on radial profile of solids a) axial velocity, b) turbulent

system at Ug = 20 cm/s, and solids loading = 25 % volume
C-3 Cross-sectional averaged turbulent stresses
The cross-sectional average of the turbulent stresses, that are important in modeling of
bubble/slurry bubble column reactors, obtained from CARPT was calculated as follows,
1
ij = 2 ij ( )d
0
(C-1)
211
where, i, j = r , , z and = dimensionless radius, r/R
Table C-1 shows the cross-sectionally averaged turbulent stresses at the studied
experimental conditions. An increase in superficial gas velocity increases all the turbulent
stresses. At the same superficial gas velocity and solids loading, an increase in operating
pressure decreases all the turbulent stresses except shear stress. While at the same
superficial gas velocity and operating pressure, an increase in solids loading increases all
the turbulent stresses except shear stress. The behavior of shear stress follows the
behavior of solids axial velocity while in case of normal stresses; mean bubble size
appears to be a controlling factor within the studied experimental conditions.
Table C-1: Cross-sectional averaged values of turbulent stresses at the studied operating
conditions
Solids
TKE
Tzz
T
rz
Loading
(%vol.) (dyne/cm2) (dyne/cm2) (dyne/cm2) (dyne/cm2)
9.1
2904
1737
1063
153
Ug
(cm/s)
20
(MPa)
0.1
30
0.1
9.1
3490
2149
1406
187
20
9.1
2317
1419
810
204
30
9.1
2782
1819
1170
232
20
0.1
25
3761
2144
1262
150
30
0.1
25
4243
2514
1622
160
20
25
2924
1670
956
176
30
25
3295
2023
1245
205
212
C-4 Turbulent Eddy Viscosity
In this section, turbulent eddy viscosity which signifies the turbulent transfer of
momentum by eddies giving rise to an internal fluid friction, is first evaluated from the
CARTPT experimental data. Next the turbulent eddy viscosity was predicted using the
approach proposed by Ohnuki and Akimoto (2001) in gas-liquid systems and is compared
with the experimental values.
C-4.1Experimental Evaluation of Turbulent Eddy Viscosity
The relationship between solids shear stress and the gradient of mean solids axial velocity
based on Boussinesqs hypothesis is given as follows,
S ,rz = S u r' u z' = S
eff du z
R d
(C-2)
where, = dimensionless radius.
The effective turbulent eddy viscosity is estimated from the CARPT data neglecting
molecular viscosity from equation (C-2). The radial-axial shear stress and radial gradient
of solids axial velocity is obtained from the CARPT measurements. The turbulent eddy
viscosity profile of the form given in equation (C-3) was assumed,
t ( ) = t 0 (1 k )
(C-3)
where, t0, k, and are the fitted parameters.
For each operating condition, the fitted parameters were optimized to the relationship
presented in the equation (C-2). The cross-sectional averaged turbulent eddy viscosities
are then estimated using the following equation,
1
t ,CSA = t d = t 0 (1
0
2k
)
+2
(C-4)
213
The values of fitted parameters of eddy viscosity profiles and averaged eddy viscosity at
the performed experimental conditions is provided in Table C-2. One can observe the
effect of superficial gas velocity, operating pressure, and solids loading. An increase in
superficial gas velocity and operating pressure decreases averaged turbulent eddy
viscosity while an increase in solids loading increases turbulent eddy viscosity. However,
based on earlier discussion, the magnitude of axial velocity gradient has opposite effect
of these parameters. Since the increase in axial velocity gradient is higher than that of
turbulent eddy viscosity, the shear stress profile follows the behavior of axial velocity
gradient.
Table C-2: Optimized parameters of the eddy viscosity profile

Superficial Operating
Solids
t0
gas
Pressure
loading
(cm2/s)
velocity
(MPa)
(% volume)
(cm/s)
20
0.1
9.1
35.7
30
0.1
9.1
37.5
20
1
9.1
49.8
30
1
9.1
24.9
20
0.1
25
79.2
30
0.1
25
34
20
1
25
69
30
1
25
30.5
k
(-)
(-)
1.17
0.82
0.77
0.65
0.8
14.3
0.9
0.91
1.85
0.53
0.022
0.24
0.1
0.52
0.61
0.29
t,CSA
(cm2/s)
14
13
12.1
10.4
18.9
14.8
15.2
11.6
C-4.2 Prediction of Turbulent Eddy Viscosity
The effective kinematic viscosity is the sum of the contributions of shear-induced

turbulent viscosity (SIT), and bubble-induced turbulent viscosity (BIT) (Deen et al.,
2001; Ohnuki and Akimoto, 2001) as follows,
eff = SIT + BIT
(C-5)
In the following sections, the procedure adopted to predict turbulent eddy viscosity due to
shear induced and bubble induced turbulence is discussed.
214
C-4.2a Eddy viscosity due to bubble induced turbulence
The turbulent eddy viscosity due to bubble induced turbulence is represented by the form
proposed by Sato and Sekoguchi (1975),
BIT = C , BIT G d b u slip
(C-6)
where, C,BIT = 0.6.
The calculation of eddy viscosity using equation (C-6) needs an estimation of bubble rise
velocity and bubble size. The following correlations were utilized to predict the needed
parameters.
The slip velocity is then calculated using Richardson-Zaki correlation given as,
u slip = U b, (1 G ) n1
(C-7)
where, Ub, is bubble terminal rise velocity. The bubble terminal rise velocity is obtained
from the following correlation of Fan and Tsuchiya (1990).
u b' = U b , (
sl 1 / 4
Mo 1 / 4 5 / 4 2 n 2c
d '
) = {[
( ) d 'b ] + [
+ ( ) b ] n / 2 }1 / n
Kb
d 'b
g
sl
sl 2
(C-8)
where, the dimensionless bubble diameter is given by, d ' b = d b ( sl g / )1 / 2

.
Three empirical parameters, n, c, and Kb needed to estimate terminal bubble rise velocity
reflect three specific factors governing the rate of bubble rise. They relate to the
contamination level of the liquid phase, to varying dynamic effects of the surface tension,
and to the viscous nature of the surrounding medium. The suggested values of these
parameters are,
0.8 for conta min ated liquids
n=
1.6 for purified liquids
(C-8a)
1.2 for monocomponent liquids

c=
1.4 for multicomponent liquids
(C-8b)
and
215
K b = max( K b 0 Mo 0.038 ,12)
(C-8c)
where,
14.7 for aqueous solutions
K b0 =
10.2 for organic solvents / mixtures
(C-8d)
These equations were developed exclusively for gas-liquid system and also at ambient
conditions. The effect of solids was accounted by using pseudo-homogeneous approach.
The effective slurry density was calculated as the linear combination of phase densities as
sl = s s + l (1 s )
(C-9)
To estimate the effective viscosity of slurry, the following relationship proposed by

Tsuchiya et al. (1997) was used,
sl
Kv s
= exp[
]
l
1 (v s / v sc )
(C-10)
with two parameters correlated by Luo et al. (1997):
K=
3.1 1.4 tanh [0.3(10 10 2 u t )]
(C-11)
v sc = {1.3 0.1 tanh[0.5(10 10 2 u t )]} s0
(C-12)
and
where ut is in m/s.
Equation (C-6) also needs an estimation of the bubble size. The number of correlations
were proposed for the estimation of bubble size in gas-liquid systems. However, none of
them were proposed for slurry bubble column reactors and weakly capture the effect of
operating pressure. In this work, the bubble size equation proposed by Wilikinson (1991)
is used as it was based on a wide range of the liquid phase properties.
d b = 3 g 0.44 0.34 l
where, db is in m.
0.22
l 0.45 g 0.11 U G 0.02
(C-13)
216
C-4.2b Eddy viscosity due to shear-induced turbulence
The eddy viscosity due to shear-induced turbulence can be represented similar to the
single-phase isotropic turbulence (Ohnuki and Akimoto, 2001),
SIT = C
2
k SIT
(C-14)
where, C = 0.09.
In the equation (C-14), kSIT is the turbulent kinetic energy due to shear-induced
turbulence while is the energy dissipation rate per unit mass of liquid. The energy
dissipation is estimated as the product of g (gravity constant) and Ug (superficial gas
velocity) [Deckwer and Schumpe, 1987; Camacho et al., 2001].
The turbulent kinetic energy is decomposed into contributions due to shear-induced and
bubble-induced turbulence using the approach proposed by Ohnuki and Akimoto (2001).
k tot = k SIT + k BIT
(C-15)
2
where, k BIT = G u slip . The slip velocity was calculated using Rischardson-Zaki
correlation mentioned above. The contribution of turbulent kinetic energy due to shearinduced turbulence, kSIT can be calculated by subtracting kBIT from the total turbulent
kinetic energy.
The estimation of turbulent kinetic energy due to shear-induced
turbulence, kSIT then enables to predict turbulent eddy viscosity due to shear-induced
turbulence using equation (C-14).
C-4.3 Comparison of Experimental and Predicted Turbulent Eddy Viscosity
Table C-3 presents the values of turbulent kinetic energy and eddy viscosity components
at the studied operating conditions using the analysis explained earlier. The predicted
turbulent eddy viscosity was compared with the one obtained from CARPT data. Based
on the available state of prediction of bubble size and slip velocity, it can be observed
that the contribution of turbulent kinetic energy due to bubble-induced turbulence is less
217
significant than that of the contribution due to shear-induced turbulence. The relative
contribution of bubble-induced turbulence to that of total turbulent kinetic energy is close
to 7-8 %. This indicates that the turbulence generation due to shearing action of slurry is
far more dominant compared to the one induced by bubbles. However, the comparison of
prediction of turbulent eddy viscosity using above procedure with that of experimental
data shows an average relative error of 63%. Such a discrepancy in the current work
might possibly due to following reasons,
In this work, Wilkinson (1991) correlation was used for bubble size estimation.
This correlation was developed for gas-liquid flows. It was utilized, as no
correlation is available for bubble size estimation in the slurry systems and it was
developed using a wide range of liquid phase properties including highly viscous
liquid.
The approach explained above was typically developed for gas-liquid flows. It
was extended to gas-liquid-solids system by assuming pseudo-homogeneous
properties. In the past, few studies (Krishna et al., 2001) compared the gas holdup
measured in gas-liquid-solid system to that of gas-liquid system by using a liquid
that has similar pseudo-homogeneous properties as that of slurry. The overall gas
holdup found in these two cases was close although slurry viscosities were
estimated based on Einstenian equation developed for dilute particles. However,
further studies are required to evaluate whether it is appropriate to assign a
constant resultant slurry viscosity based on pseudo-homogenous approach. A
more elaborate analysis is needed to account for the effect of bubble size on
interactions of the bubbles based either on non-Newtonian approach or
heterogeneous approach.
218
Table C-3: Eddy viscosity analysis

Superficial
gas
velocity
(cm/s)
20
30
20
30
20
30
20
30
% error =
Operating Solids
Pressure
loading
(MPa)
(%
volume)
0.1
9.1
0.1
9.1
1
9.1
1
9.1
0.1
25
0.1
25
1
25
1
25
tCSA total
total
Gas
db
holdup (cm)
(-)
kBIT
kSIT
Ub
SIT
2 2
2 2
(cm/s) (cm /s ) (cm /s )
BIT
total
%
Error
0.28
0.33
0.4
0.45
0.16
0.2
0.27
0.3
15.4
15.4
14.2
14.2
14.3
14.27
13
13
38
37
24.3
23.4
64.3
54.5
34
33
38.45
37.47
24.65
23.75
64.6
54.84
34.28
33.3
64
65
51
56
70
73
56
65
0.27
0.27
0.2
0.2
0.28
0.28
0.21
0.21
27
26
20
19.5
20
22
18.8
18.4
2877
3464
2297
2764
3740
4221
2905
3276
0.45
0.47
0.35
0.35
0.3
0.34
0.28
0.3
219
C-5 Turbulent Viscosity Correlations
In this section, the cross-sectional averaged turbulent viscosity calculated using CARPT
data in Section C-4.1 is compared with the predictions of the available correlations.
These correlations are commonly utilized as closures in modeling velocity profiles in
bubble columns assuming constant turbulent viscosity. Table C-4 lists the available
correlations for turbulent viscosity while Table C-5 shows % relative error between
experimental and predicted turbulent viscosities using the last three correlations in Table
C-5. The first two correlations were not considered as they assume turbulent viscosity to
be function only of column diameter. Clearly, none of the available correlations predict
turbulent eddy viscosity with consistent statistical confidence.
Table C-4: Correlations for turbulent viscosity
Researcher
Miyauchi and Shyu (1970)
Correlation
Ueyama and Miyauchi (1979)
0.0322 DT1.7
Miyauchi et al. (1981)
0.0345U G1 / 6 DT3 / 2
Riquarts (1981)
( DT U G / 90.9) Re1 / 8 Fr 1 / 3
Kawase and Moo-Young

(1989)
(1 / 43)
0.0199 DT1.8
DT2 g G
V L ( 0)
220
Table C-5: % relative error of literature correlations for turbulent viscosity from CARPT
data
Superficial Operating
Solids
gas
Pressure
loading
velocity
(MPa)
(% vol )
(cm/s)
20
0.1
9.1
30
0.1
9.1
20
1
9.1
30
1
9.1
20
0.1
25
30
0.1
25
20
1
25
30
1
25
% relative error *
Miyauchi Riquarts Kawase and Moo
et al.(1981)
(1981) Young (1989)
22.3
40.9
41.6
76.2
9.4
23.8
12.7
57.9
72.9
49.9
68.7
37.4
80
56
75.1
43.8
145
158
157
181
190
182
179
198
C-6 Eddy Diffusivities
Turbulent eddy diffusivities are important parameters in modeling of liquid/solids mixing

in bubble/slurry bubble column reactors. As CARPT provides lagrangian data, an
estimation of these quantities is unique to this technique. As the flow is anisotropic with
radial non-homogeneity, the radial gradient of solids axial velocity was considered in the
evaluation of axial eddy diffusivity. Degaleesan (1997) defined eddy diffusivities as
follows,
The radial eddy diffusivity is,

t
Drr (t ) =
1 d 2
yr (t ) = ur '(t ')ur '( )d
2 dt
0
(C-16)
The axial eddy diffusivity is,
Dzz (t ) =
1 d 2
yz '(t ) = yz (t )u z '(t )
2 dt
% relative error =
t , CSA t , correlation
t , CSA
(C-17)
221
First, various correlation coefficients were calculated from CARPT experimental data
which was then used to compute these eddy diffusivities.
C-6.1 Effect of liquid phase physical properties on eddy diffusivities
Figure C-9a shows the comparison of axial and radial diffusivities in air-water-glass
beads and air-Therminol LT-glass beads system at superficial gas velocity of 30 cm/s and
solids loading of 9.1 % vol. In general, diffusivities were low in air-Therminol LT-glass
beads system. However, the effect on radial eddy diffusivity is stronger than on the axial
eddy diffusivity at ambient pressure. Figure C-9b shows the comparison of axial and
radial diffusivities in these two systems at operating pressure of 1 MPa. At higher
pressure, both axial and radial eddy diffusivities were significantly reduced in airTherminol LT-glass beads system. Such reduction in eddy diffusivities in Therminol LT
systems can be related to the change in physical properties that results into generation of
higher population of small bubbles/eddies. The similar effect due to change in liquid was
observed in case of TKE and normal stresses.
(a)
222
(b)
Figure C-9: Comparison of axial and radial eddy diffusivities in air-water-glass beads and
air-Therminol LT-glass beads system at and superficial gas velocity 30 cm/s, solids
loading of 9.1 % vol. and operating pressure of a) 0.1 MPa, and b) 1 MPa.
C-6.2 Effect of solids loading on eddy diffusivities
Figures C-10 and C-11 show the effect of solids loading on axial and radial eddy
diffusivities in air-Therminol LT-glass beads system at ambient pressure and superficial
gas velocities of 20 and 30 cm/s. An addition of solids in the system tends to increase
bubble coalescence rate and decrease bubble breakup rate that results into higher
population of large bubbles/eddies in the system. Hence, at increased solids loading
higher values of axial and radial diffusivities were observed. The maximum in both the
diffusivities was not affected by an addition of solids. The similar qualitative effect of
solids loading was observed at higher pressure as shown in Figures C-12 and C-13.
223
Figure C-10: Effect of operating pressure on axial and radial eddy diffusivities in airTherminol LT-glass beads system at solids loading of 9.1 % vol. and superficial gas
velocity of 20 cm/s.
Figure C-11: Effect of solids loading on axial and radial eddy diffusivities in airTherminol LT-glass beads system at ambient pressure and superficial gas velocity of 30
cm/s.
224
Figure C-12: Effect of solids loading on axial and radial eddy diffusivities in airTherminol LT-glass beads system at operating pressure of 1 MPa and superficial gas
Figure C-13: Effect of solids loading on axial and radial eddy diffusivities in airTherminol LT-glass beads system at operating pressure of 1 MPa and superficial gas
velocity of a) 20 cm/s, and b) 30 cm/s.
C-6.3 Effect of superficial gas velocity on eddy diffusivities
Figures C-14 and C-15 show the effect of superficial gas velocity on axial and radial
eddy diffusivities in air-Therminol LT-glass beads system at Ug = 30 cm/s, solids loading
225
of 9.1 % vol and operating pressure of 0.1 MPa. An increase in superficial gas velocity
increases axial and radial eddy diffusivities. The maximum values of axial diffusivities
are observed at dimensionless radius of about 0.7, while maximum radial eddy
(a)
(b)
Figure C-14: Effect of superficial gas velocity on a) axial and b) radial eddy diffusivities
in air-Therminol LT-glass beads system at ambient pressure and solids loading of 9.1 %
vol.
(a)
(b)
in air-Therminol LT-glass beads system at operating pressure of 1 MPa and solids
loading of 9.1 % vol.
diffusivities are observed at dimensionless radius of about 0.5. The locations of these
maximum values can be explained on the basis of inversion point in axial solids velocity
226
and the maximum values of solids shear stresses. The similar effect of eddy diffusivities
was observed at high solids loading (Figures C-16 and C-17).
(a)
(b)
in air-Therminol LT-glass beads system at ambient pressure and solids loading of 25 %
vol.
(a)
(b)
in air-Therminol LT-glass beads system at operating pressure of 1 MPa and solids
loading of 25 % vol.
227
C-6.4 Effect of operating pressure on eddy diffusivities
Figures C-18 and C-19 show the effect of operating pressure on axial and radial eddy
diffusivities in air-Therminol LT-glass beads system using solids loading of 9.1 % vol.
and superficial gas velocity of 20 and 30 cm/s, respectively. Similar to the effect of
pressure on turbulent kinetic energy and other normal stresses, axial and radial eddy
diffusivities were found to decrease with an increase in pressure. As mentioned earlier,
an increase in pressure increases bubble breakup rate while decreases coalescence rate.
This results into relatively higher population of small bubbles/eddies at increased
pressure and thereby reduced diffusivities.
Figures C-20 and C-21 show the effect of operating pressure at solids loading of 25 %
vol. and superficial gas velocity of20 and 30 cm/s. The similar qualitative effect of
operating pressure was observed at high solids loading.
228
Figure C-20: Effect of operating pressure on axial and radial eddy diffusivities in airTherminol LT-glass beads system at solids loading of 25 % vol. and superficial gas
229
Figure C-21: Effect of operating pressure on axial and radial eddy diffusivities in airTherminol LT-glass beads system at solids loading of 25 % vol. and superficial gas
C-6.5 Cross-sectional averaged eddy diffusivities
The cross-sectional average of the eddy diffusivities obtained from CARPT was
calculated as follows,
1
Dii = 2 Dii ( )d
0
(C-18)
where, i = r , z and = dimensionless radius, r/R.
Table C-6 shows the cross-sectionally averaged axial and radial eddy diffusivities at the
studied experimental conditions.
230
Table C-6: Cross-sectional averaged values of axial and radial diffusivities at the studied
operating conditions in air-Therminol LT-glass beads system
Ug
Dzz
Drr
(MPa)
0.1
Solids
Loading
(%vol.)
9.1
(cm/s)
20
(cm2/s)
535
(cm2/s)
31
30
0.1
9.1
570
35
20
9.1
450
22
30
9.1
482
25
20
0.1
25
644
42
30
0.1
25
721
46
20
25
548
29
30
25
585
32
In general, an increase in superficial gas velocity increases eddy diffusivities. At the same
superficial gas velocity and solids loading, an increase in operating pressure reduces eddy
diffusivities. While at the same superficial gas velocity and operating pressure, an
increase in solids loading increases eddy diffusivities.
An increase in operating pressure from 0.1 to 1 MPa decreases axial eddy diffusivity by
15 and 20 % at solids loading of 9.1 and 25 % vol., respectively. While an increase in
solids loading from 9.1 to 25 % vol. increases axial diffusivity by 20 and 23 % at
operating pressures of 0.1 and 1 MPa, respectively. The radial eddy diffusivities exhibit
the same qualitative but slightly different quantitative behavior.
231
APPENDIX D
Sedimentation-Dispersion Model
An axial distribution of solid/catalyst particles is an important parameter for design and
scaleup of slurry bubble column reactors. The axial solids distribution influences
residence time distribution of solid particles that in turn affects the conversion rates and
the heat and mass transfer inside the reactor. Catalyst concentration in the reactor is a
function of catalyst concentration in feed, direction and magnitude of the liquid/slurry
velocity, mixing characteristics of the system, axial location in the reactor, and physical
properties of slurry (Cova, 1966). The solids axial distribution is quantitatively described
using Sedimentation-Dispersion Model (SDM). It is the popular and only predictive
model available. SDM was originally proposed by Cova (1966) and Suganuma and
Yamanishi (1966). In this model, the solids flux is obtained by the superposition of a
Fickian type solids dispersion flux and a solids settling (sedimentation) flux on the
convective slurry flux.
The following assumptions were used in formulating the model:

i)
All the solids particles have identical terminal velocity.
ii)
Solids phase dispersion coefficient is constant along the column axis.
iii)
The gas holdup is constant along the column axis.
iv)
The settling velocity of solids particles is constant along the column axis.
v)
All solids particles are completely suspended in liquid.
vi)
No radial gradients in the concentration of solids particles.
If one considers a horizontal cross-sectional element of slurry bubble column reactor with
thickness z. A mass balance in the vertical z-direction with respect to solid particle can
be written as
Rate of accumulation within volume element = rate of mass (in-out) due to dispersion +
rate of mass (in-out) due to convective
232
slurry flow + rate of mass (in-out) due to
settling of solids .. (D-1)
Equation (D-1) can be written as,

c
D z s = DT2 [n d
t
2
T
u
u
n d z + z ] + D [( sl C S ) ( sl C S )
1 G
1 G
] + DT2 [(u t C S ) z + ( u t C S ) z + z ]
2
T
z + z
.(D-2)
Dividing equation (D-2) by DT2 z and taking limit as z tends to zero yields
c s nd u sl
=
(
C S ) + ut C S
t
z z 1 G
z
.(D-3)
The dispersion flux, nd of solid particles is given as,
nd = E S
c s
z
.(D-4)
The substitution of equation (D-4) into (D-3) along with steady state assumption gives
following simplified general form,
d 2 cs
u
dC S
ES
( sl u t )
=0
2
dz
1 G
dz
(D-5)
To obtain the solids axial distribution, the equation (D-5) needs to be integrated twice and
needs two boundary conditions.
For semi-batch operation (as employed in the current work), equation (D-5) can be
written as
ES
d 2 cs
dCS
u
+
=0
t
dz
dz 2
The general solution of this differential equation is
.(D-6)
233
C S = C1 + C 2 exp [
ut
z]
ES
..(D-7)
The first boundary condition is
C S = 0 as z C1 = 0
Therefore equation (D-7) becomes
C S = C 2 exp [
ut
z]
ES
.(D-8)
The second constant can be obtained from the knowledge of nominal solids mass in the
column. Let m be the initial mass of particles, V be the total slurry volume while S and L
are cross-sectional column area and slurry height. Hence
V
m = C S dV
(D-9)
Substitution of equation (D-9) into equation (D-8) yields

L
m = C 2 exp (
0
ut
z ) S dz
ES
(D-10)
Integration of equation (D-10) will give the value of second constant. The substitution of
second constant in equation (D-8) will result into the following equation
ut
z]
mu t
ES
CS =
u
SE S
1 exp [ t L]
ES
exp [
(D-11)
The nominal solids concentration is
m = CS V
.(D-12)
Hence the final form for semi-batch operation is
z
]
L
C S = C S BoS
1 exp [ BoS ]
exp [ BoS
where, BoS = ut L / E S
.(D-13a)
234
The final form of SDM can be written in terms of solids loading (equation D-13b) and
solids holdup (equation D-13c) as follows
z
]
L
v S = v S BoS
1 exp [ BoS ]
.(D-13b)
z
]
L
S = S BoS
1 exp [ Bo S ]
.(D-13c)
exp [ BoS
exp [ BoS
To predict solids axial profile using SDM, one need to predict two parameters, i.e.,
terminal velocity and solids axial dispersion coefficient. Various correlations are
available to predict these parameters. In this work, the most commonly used correlations
in literature were utilized.
Solids axial dispersion coefficient
The solid phase Peclet number is calculated in terms of Froude number as follows
Pe S =
13Fr H D
1 + 8Fr 0.85 D
Fr =
UG
(D-14)
(D-15)
gD C
where, Pe S =
UGL
.
ES
Particle terminal velocity
The terminal velocity of particles, ut calculated from the single particle settling velocity in
a quiescent liquid (uts) using a following set of correlations (Kato et al., 1972).
U
u t = 1.2uTS G
u ts
1/ 4
1 vS 0
1 v*
S
5/ 2
(D-16)
235
u ts =
ReP L
LdP
(D-17)
Ar / 18
for Re P 0.5
Re P =
0.7
for Re P > 0.5
(Ar / 13.9)
Ar =
v *S =
( S L ) L gd 3P
L2
0.1
(D-18)
(D-19)
(D-20)
236
APPENDIX E
Material Safety Data Sheet for Therminol LT
1.
PRODUCT AND COMPANY IDENTIFICATION
Product name: THERMINOL LT Heat transfer fluid

Reference Number: 000000000208 Date: 12/03/2004
Company Information:
United States:
Solutia Inc.
575 Maryville Center Drive,
St. Louis, MO 63166-6760
Emergency :1-800-424-9300
Non-Emergency: 1-314-674-6661
Canada:
Solutia Canada Inc.
P.O. Box 66760 6800 St. Patrick Street
LaSalle, PQ H8N 2H3
Emergency: 1-613-996-6666
Mexico:
Solutia MEXICO, S. DE R.L. DE C.V.
Paseo de la Reforma No. 2654 Piso 3-A
Col. Lomas Altas, CP 11950 Mexico DF
Brazil:
Solutia Brazil Ltd.
Avenue Carlos Marcondes, 1200
CEP: 12241-420-So Jos dos Campos/SPBrazil
Emergency: 55 12 3932 7100 (PABX)
Non-Emergency: 55 11 3365 1800 (PABX)
Emergency: 01-800-002-1400
2.
HAZARDS IDENTIFICATION
EMERGENCY OVERVIEW
Form: liquid
Colour: clear to colourless
Odour: strong odour, aromatic, hydrocarbon
WARNING STATEMENTS
WARNING!
Flammable liquid and vapour
Contains material which can cause nervous system damage
May cause skin irritation
May cause respiratory tract irritation
POTENTIAL HEALTH EFFECTS
Likely routes of exposure:
237
eye and skin contact, inhalation
Eye contact: Slightly irritating to eyes.
Skin contact: Moderately irritating to skin.
Prolonged or repeated skin contact may result in irritant dermatitis.
Can be absorbed rapidly through the skin.
No more than slightly toxic if absorbed.
Inhalation:
Moderately irritating if inhaled.
No more than slightly toxic if inhaled.
Significant adverse health effects are not expected to develop under
normal conditions of exposure.
Ingestion:
No more than slightly toxic if swallowed.
Significant adverse health effects are not expected to develop if only small
amounts (less than a mouthful) are swallowed.
Signs and symptoms of overexposure:
headache
dizziness/incoordination
nausea/vomiting
loss of consciousness
vertigo
confusion
anxiety
laboured breathing
drowsiness
Target organs/systems: May cause nerve damage
Based on animal data excessive exposure may cause bluish
discoloration of tissue and urine.
Refer to Section 11 for toxicological information.
3. COMPOSITION/INFORMATION ON INGREDIENTS
Components
diethylbenzene
CAS No.
25340-17-4
Average conc. Concentration range

100.0
4. FIRST AID MEASURES

If in eyes: Immediate first aid is not likely to be required.
This material can be removed with water.
If on skin: Immediately flush the area with plenty of water.
Remove contaminated clothing.
Get medical attention if irritation persists.
Wash clothing before reuse.
Units
%
238
If inhaled: Remove patient to fresh air.
If not breathing, give artificial respiration.
If breathing is difficult give oxygen.
Remove material from eyes, skin and clothing.
If swallowed: Immediate first aid is not likely to be required.
A physician or Poison Control Center can be contacted for advice.
Wash heavily contaminated clothing before reuse.
5. FIRE FIGHTING MEASURES
Hazardous products of combustion:
carbon monoxide (CO); carbon dioxide
Extinguishing media:
Water spray, foam, dry chemical, or carbon dioxide
Unusual fire and explosion hazards:
Residual vapours may explode on ignition.
Fire fighting equipment:
Firefighters, and others exposed, wear self-contained breathing apparatus.
Equipment should be thoroughly decontaminated after use.
Miscellaneous advice: This product is not classified as a fire-resistant heat transfer fluid.
Precautions to avoid sources of ignitions should be taken.
6. ACCIDENTAL RELEASE MEASURES
Personal precautions:
Remove any sources of sparks, flame, or hot surfaces.
Ensure adequate ventilation.
Use personal protection recommended in section 8.
Environmental precautions:
Keep out of drains and water courses.
Methods for cleaning up:
Contain large spills with dikes and transfer the material to appropriate containers for
reclamation or disposal. Absorb remaining material or small spills with an inert material
and then place in a chemical waste container. Flush spill area with water.
Refer to Section 13 for disposal information and Sections 14 and 15 for reportable uantity
information.
239
7. HANDLING AND STORAGE

Handling:
Keep away from heat, sparks, and flame.
Avoid contact with eyes, skin and clothing.
Avoid breathing vapour or mist.
Keep container closed.
Use with adequate ventilation.
Wash thoroughly after handling.
Heat transfer fluids are intended for INDIRECT heating purposes ONLY.
This product has not been approved for food grade use.
Container hazardous when empty:
Emptied containers retain vapour and product residue. Follow labeled warnings even
after container is emptied. Residual vapours may explode on ignition. Do not cut, drill,
grind or weld on or near this container. Improper disposal or reuse of this container may
be dangerous and/or illegal. The reuse of this material's container for non industrial
purposes is prohibited and any reuse must be in consideration of the data provided in this
material safety data sheet.
Storage
General: Stable under normal conditions of handling and storage.
8. EXPOSURE CONTROLS/PERSONAL PROTECTION
Airborne exposure limits: (ml/m3 = ppm)
THERMINOL LT
No specific occupational exposure limit has been established.
Eye protection: Does not cause significant eye irritation or eye toxicity requiring special
protection.
Use good industrial practice to avoid eye contact.
Hand protection: Wear chemical resistant gloves.
Consult the glove/clothing manufacturer to determine the appropriate
type glove/clothing for a given application.
Body protection: Wear suitable protective clothing.
Consult the glove/clothing manufacturer to determine the appropriate
type glove/clothing for a given application.
Wear full protective clothing if exposed to splashes.
Wash contaminated skin promptly.
Launder contaminated clothing and clean protective equipment before
reuse.
240
Wash thoroughly after handling.
Respiratory protection: Avoid breathing vapour or mist.
Use approved respiratory protection equipment when airborne
exposure is excessive.
Consult the respirator manufacturer to determine the appropriate
type of equipment for a given application.
Observe respirator use limitations specified by the manufacturer.
Ventilation: Provide natural or mechanical ventilation to minimize exposure.
If practical, use local mechanical exhaust ventilation at sources of air
contamination such as processing equipment.
Components referred to herein may be regulated by specific Canadian provincial
legislation. Please refer to exposure limits legislated for the province in which the
substance will be used.
9. PHYSICAL AND CHEMICAL PROPERTIES
Flash point: 57 0C Pensky-Martens closed tester
Autoignition temperature: 429 0C ASTM D-2155
Specific gravity: 0.864 @ 25 0C
Density: 8.62 g/cm3 @ 25 0C
Boiling point : 181 0C @ 1,013 hPa
Freezing point -75 0C
Vapour pressure: 1 hPa @ 20 0C
Water solubility: 14 mg/l @ 25 0C
Kinematic viscosity: 0.81 mm2/s @ 40 0C
VOC Content: 100 % ;
NOTE: These physical data are typical values based on material tested but may vary from
sample to sample. Typical values should not be construed as a guaranteed analysis of any
specific lot or as specifications for the product.
10. STABILITY AND REACTIVITY
Conditions to avoid: All sources of ignition.
Materials to avoid: Contact with oxidizing agents.
Hazardous reactions: Hazardous polymerization does not occur.
Hazardous decomposition products: None known
11. TOXICOLOGICAL INFORMATION
Human experience:
Prolonged or repeated skin contact may result in irritant dermatitis.
Accidental inhalation during ingestion or vomiting may cause lung injury leading to
241
death. This product has been tested for toxicity. Results from Solutia sponsored studies or
from the available public literature are described below.
Acute animal toxicity data
Oral:
LD50 , rat, 2,050 mg/kg , Slightly toxic following oral administration.
Dermal:
LD50 , rabbit, > 5,000 mg/kg , Practically nontoxic after skin application
in animal studies.
Inhalation:
LC50 , mouse, > 27.4 mg/l , , No mortality or signs of toxicity at the

highest level achievable.
Eye irritation: rabbit , Slightly irritating to eyes (rabbit)., 24 h

Skin irritation: rabbit , Moderately irritating to skin., 24 h
Repeat dose toxicity: rat, subchronic, Repeated administration produced discoloration of
fur, organs and urine. Target organs affected liver, kidneys
Neurotoxicity: rat, Exposure produced weakness in hind limbs and gait disturbances
which progressed to complete paralysis in some cases.
Developmental toxicity: rat, gavage, , No birth defects were noted in rats given the active
ingredient orally during pregnancy.
Carcinogenicity: mouse, dermal, chronic, Produced tumours at the site of application.
Mutagenicity: No genetic effects were observed in standard tests using bacterial and
animal cells.
12. ECOLOGICAL INFORMATION
Environmental Toxicity:
Invertebrates 48 h, EC50 Water flea (Daphnia magna) 9.42 mg/l
Fish: 96 h, LC50 Fathead minnow (Pimephales promelas) > 1.0 mg/l
Algae: 96 h, EC50 Algae (Selenastrum capricornutum) > 20 mg/l
EC50/LC50 greater than water solubility.
Environmental fate
Biodegradation theoretical CO2 evolution 8 % 28 d
Not readily biodegradable.
13. DISPOSAL CONSIDERATIONS
US EPA RCRA Status: This material when discarded is a hazardous waste as that term is
defined by the Resource, Conservation and Recovery Act
(RCRA),40 CFR 261. See disposal considerations below for U.S.
242
EPA disposal requirements. Consult regulatory officials for
performance standards.
US EPA RCRA hazardous waste number: D001
Compound/Characteristic: Ignitability
Disposal considerations:
Incineration
Recycle
Miscellaneous advice:
This product meets the criteria for a synthetic used oil under the U.S. EPA Standards for
the Management of Used Oil (40 CFR 279). Those standards govern recycling and
disposal in lieu of 40 CFR 260 -272 of the Federal hazardous waste program in states that
have adopted these used oil regulations. Consult your attorney or appropriate regulatory
official to be sure these standards have been adopted in your state. Recycle or burn in
accordance with the applicable standards. Solutia operates a used fluid return program for
certain fluids under these used oil standards. Contact your Sales Representative for
details. This product should not be dumped, spilled, rinsed or washed into sewers or
public waterways.
14. TRANSPORT INFORMATION
The data provided in this section is for information only. Please apply the appropriate
regulations to properly classify your shipment for transportation.
US DOT
Proper shipping name: DIETHYLBENZENE
Hazard Class: 3
Hazard Identification number: UN2049
Packing Group: Packing Group III
Transport label: Flammable liquid.
Canadian TDG
Proper shipping name: DIETHYLBENZENE
Other: See DOT Information
Hazard Class: 3
Hazard Identification number: UN2049
Packing Group: Packing Group III
Transport label: Flammable liquid.
ICAO/IATA Class
Other: See DOT Information
243
15. REGULATORY INFORMATION
All components are in compliance with the following inventories:
U.S. TSCA, EU EINECS, Canadian DSL, Australian AICS, Korean, Japanese ENCS,
Phillipine PICCS, Chinese
Canadian WHMIS classification:
B3 - Combustible Liquids
D2(B) - Materials Causing Other Toxic Effects
SARA Hazard Notification:
Hazard Categories Under Title III Rules (40 CFR 370):
Immediate
Delayed
Fire
Section 302 Extremely Hazardous Substances:
Not applicable
Section 313 Toxic Chemical(s):
Not applicable
CERCLA Reportable Quantity:
Not applicable
This product has been classified in accordance with the hazard criteria of the Canadian
Controlled Products Regulation and the MSDS contains all the information required by
the Canadian Controlled Products Regulation. Refer to Section 11 for OSHA/HPA
Hazardous Chemical(s) and Section 13 for RCRA classification. Safety data sheet also
created in accordance with Brazilian law NBR 14725
16. OTHER INFORMATION
Product use: Heat transferring agents
Reason for revision: New ANSI Standard
Suggested NFPA Rating

Suggested HMIS Rating:
Health
2
2
Fire
2
2
Reactivity Additional Information

0
0
G
Prepared by the Solutia Hazard Communication Group. Please consult Solutia @ 314674-6661 if further information is needed.
244
Appendix F
Development of Artificial Neural Network (ANN)

Correlations for Hydrodynamic Parameters
As discussed in Chapter 6, the objective of this chapter of Appendix is to develop stateof-the-art correlations for a priori prediction of hydrodynamic parameters that will aid
the proposed methodology for hydrodynamic similarity. The specific focus is to develop
unified correlations for overall gas holdup, radial profile of gas holdup and liquid axial
velocity in bubble columns that can be useful for design engineers. To develop such
correlations, an approach that combines both an Artificial Neural Network (ANN) and
Dimensional Analysis has been used. These correlations were derived from a broad
experimental data bank collected from the open literature.
In the first part, a brief introduction to ANN is provided. The detailed information can be
referred to Shaikh and Al-Dahhan (2003). The next section deals with the general
procedure for the development of these correlations in the context of overall gas holdup.
The similar procedure is being adopted to develop the correlations for radial profile of
gas holdup and liquid axial velocity. The general structure of ANN correlations for radial
profile of gas holdup and liquid axial velocity and centerline velocity is presented.
F-1 Artificial Neural Networks
Neural Networks are computer algorithms inspired by the way information is processed
in the nervous system. An Artificial Neural Network is a massively parallel distributed
processor that has a natural propensity for storing experimental knowledge and making it
available (Ripley, 1996).
245
In this work, a multilayer neural network has been used, as it is effective in finding
complex non-linear relationships. It has been reported that multilayer ANN models with
only one hidden layer are universal approximators (Hornik et al., 1989). Hence, a threelayer feedforward neural network is chosen as a regression model. The weighting
coefficients of the neural network are calculated using the special-purpose software
NNFit (Cloutier et al.,1996). NNFit is a non-linear regression software that discloses
relationships between a set of normalized input variables, Ui, and a set of normalized
output variable, Sk. Figure F-1 shows the transformation S = f (U) using a neural network
with a single hidden layer. The transformation of actual variables (X, Y) to normalized
variables (U, S) is given by (Cloutier et al., 1996),
Ui =
log( X i / X min )
log( X max / X min )
Sk =
log(Yk / Ymin )
log(Ymax / Ymin )
(F-1)
(F-2)
where, Xi and Yk are raw input and output variables. The basic structure of this type of
neural network is described by the following set of equations. The various layers are
interconnected to each other by a sigmoid function through the fitted parameters wij, wjk
in the following manner,
Sk =
1
J +1
1 + exp[ w jk H j ]
j =1
(F-3)
and
Hj =
1
I +1
1 + exp[ wijU i ]
i =1
(F-4)
where I,J,K indicate the input, hidden and output nodes of the ANN structure,
respectively. HJ+1 and UI+1 (Figure 7-1) are the bias constants which are set equal to one.
246
wij and wjk are weighting parameters which are fitted by the NNFit regression model,
using a quadratic criterion as a minimization algorithm, a quasi-Newton method of the
BGFS type (Broyden-Fletcher-Goldfrab-Shanno) (Cloutier et al., 1996).
Figure F-1: Architecture of the three-layered feedforward neural network with a single
hidden layer
F-2 Development of the ANN based correlation for Overall Gas Holdup
Over the years, overall gas holdup has been studied extensively with various
measurement techniques, ranging from measuring the change in dynamic height or
measuring conventional pressure drop to CT. In the literature, numerous correlations
have been proposed for overall gas holdup. Some of the important correlations can be
referred to Shaikh and Al-Dahhan (2003). Kemoun et al. (2001) compared gas holdup
predicted by various correlations with the cross-sectional averaged gas holdup measured
using CT in the fully developed region at atmospheric to high pressure and at low to high
superficial gas velocities. The comparison between their experimental data and predicted
gas holdups from various correlations at atmospheric and high pressure (0.7 MPa) can be
summarized as follows,
At atmospheric pressure, the correlation of Idogawa et al. (1985) gives the best
agreement with the CT experimental data, except at UG = 5 cm/s.
247
At higher pressures and over the entire superficial gas velocity range studied, the
correlation of Hammer et al. (1984) gives better prediction, followed by Wilkinson et
al. (1992) and Idogawa et al. (1987).
At higher pressures and higher superficial gas velocity (UG = 10 cm/s), the correlation
of Krishna et al. (1996) and Luo et al. (1999) also provides reasonable prediction of
gas holdup.
While several correlations give reasonable predictions at different conditions, Kemoun et

al. (2001) did not find any correlation that consistently predicted their experimental data
at the studied operating conditions. To facilitate the scale-up of bubble columns, there is a
need for a correlation that can predict overall gas holdup over a range of operating
conditions, physical properties, and column dimensions.
The development of the ANN-based correlation began with the collection of a large
databank. The physical parameters were then subjected to force analysis in order to
maintain dimensional homogeneity. The last step was to perform a neural regression, and
to validate it statistically.
F-2.1 Collection of data
As mentioned earlier, over the years researchers have amply quantified the
hydrodynamics of bubble column reactors based on the overall gas holdup. In this work,
about 3500 experimental points have been collected from 60 sources spanning the years
1965 to 2000. This wide range of database includes experimental information from
different physical systems to provide a unified correlation for overall gas holdup. Table
F-1 suggests the wide range of the collected databank for gas holdup. Most of the
hydrodynamic studies on bubble columns were performed using air-water systems.
Hence, the majority of the current database (around 45%) comprises overall gas holdup
data from air-water studies.
248
Table F-1: Range of column dimensions, physical properties, operating pressures and
type of spargers included in the collected databank
Column Diameter
0.045 - 5.5 m
Liquid Density
681 - 2965 kg.m-3
Liquid Viscosity
0.41 - 2.95 cP
Surface Tension
20 - 72 mN.m-1
Gas Density
0.083 - 1.2 kg.m-3
Pressure
0.1 - 2 MPa
Superficial Gas Velocity
0.005 0.75 m/s
Superficial Liquid Velocity
0 (batch liquid)
Overall gas holdup
0.05 0.685
Gases: air, N2, CO2 , He, Ar, mixture of N2 and H2

Liquids: water, tetradecane, paraffin oil (A, B), soltrol-130, isopropanol, monoethylene
glycol, n-heptane, isopar-G etc.
Sparger types: perforated plates with different no. of holes, geometry and hole sizes,
single nozzle sparger, cross-sparger, sintered plate etc.
Number of Sources: 60 (1965 2000)
Number of data points: 3500
Most of the hydrodynamic studies on bubble columns were performed using air-water
systems. Hence, the majority of the current database (around 45%) comprises overall gas
holdup data from air-water studies. To assess the impact of physical properties such as
density, surface tension, and viscosity, several other gas-liquid systems were included in
the database. However, in this work we have included only pure liquids systems
(approximately 30 different liquids). Bubble columns are generally operated with low
liquid velocities, which have been reported to have little or no effect on overall gas
holdup (Kelkar et al., 1983, Shetty et al., 1992). Hence, in this work we have considered
data only for columns with liquid in batch mode and gas in continuous mode. As
industrial conditions of interest are at high pressure, we have added experimental studies
at high pressures up to 2 MPa. Since reactor scale-up extends small diameter behavior to
large diameters, and in order to make the developed correlation industrially useful, we
249
have included data obtained up to 5.5 m column diameter, the largest diameter described
in the open literature. All the data was collected for cylindrical columns, as they are the
favored geometry in a majority of industrial applications. There are different spargers
used in various studies. We have mentioned only the most commonly used spargers in
Table F-1. However, in the most literature studies the mentioned spargers have been used
with some modifications in geometry or by changing number of holes or hole sizes. Since
the data was collected from wide range of sources, there is no uniformity in the
measurement techniques of gas holdup. The techniques range from measurement by level
change, or pressure drop up to densitometry and computed tomography.
F-2.2 Force Analysis
The force analysis checked whether the physical parameters in the database can be
formulated in a dimensionally homogeneous manner or not. It consists of two steps
i)
All physical parameters that influence overall gas holdup are put in a so called
wish-list.
ii)
The dimensional homogeneity of the physical parameters was checked by

transforming them into various forces.
Based on the extensive literature review, the input variables that have been found to affect
gas holdup are superficial gas velocity, column diameter, operating pressure, liquid phase
physical properties, and sparger design. However, the effect of sparger is significant only
in bubbly flow.
Once the crucial identification of raw variables has been performed, the input variables
were then converted into various physical forces. Some of the important forces are
a)
gas inertial force: G uG2
b)
gas viscous force: G uG / d
250
c)
liquid gravitational force: L gd
d)
gas gravitational force: G gd
e)
capillary force: L / d
Dimensionless numbers were then formed by taking ratios of various physical forces
which are determined from the input variables. In addition to this, the various
dimensionless groups used in the gas holdup correlations reported in literature were
considered. Then, on the basis of the observed effect of some parameters on the overall
gas holdup, some of the dimensionless groups such as ratios of densities, etc., were
added.
The main advantage of performing dimensional analysis is to reduce the number of input
parameters, i.e., there are fewer dimensionless input groups than the raw parameters. The
other advantage of dimensional analysis lies in the scale-invariant property of a
dimensionless frame. The scale-invariance makes dimensional analysis a primary step
in scale-up of reactors (Zlokarnik, 1998).
F-2.3 Neural Regression
Force analysis is used to produce dimensionless groups in this case, but it alone cannot
determine which groups are relevant and should be used as input. Therefore, we used the
following methodology to select the most pertinent inputs (Bensetiti et al., 1997).
Out of the number of dimensionless groups derived, we used ANN regression to establish
the best set of chosen dimensionless groups, which describes overall gas holdup
(Bensetiti et al., 1997, Larachi et al., 1998). The following criteria guide the choice of the
set of input dimensionless groups:
The dimensionless groups should be as few as possible,
Each group should be highly cross-correlated to the output parameter,
These input groups should be weakly cross-correlated to each other,
251
-
The selected input set should give the best output prediction, which is checked by
using statistical analysis [e.g., average absolute relative error (AARE), standard
deviation, cross-correlation coefficient].
There should be minimum complexity in neural network architecture, i.e., a

minimum number of hidden layers J.
While choosing the most expressive dimensionless groups, there is a compromise

between the number of dimensionless groups and prediction. The main concern with the
number of dimensionless groups is due to two reasons: first, there should be fewer
expressive groups than raw parameters, and second for feasible scale-up we may need a
minimum number of dimensionless groups.
The cross-correlation analysis which signifies the strength of the linear relation between
input and output is then used to find the dependence between input and output groups. A
number of inputs can be highly cross-correlated to output, but there should not be any
dependency between these groups; otherwise, it just adds to the complexity of the
structure rather than contributing significantly to improve the quality of the network. One
should be careful here: although the cross-correlation analysis reveals the dependence
between inputs and outputs, it also hides non-monotonic relationships. This can result
into losing an important dimensionless group. Therefore in this study, several sets of
input groups were made and tested via rigorous trial-and-error on the Artificial Neural
Network. The above mentioned criteria were then used to identify the most pertinent set
of input groups.
The statistical analysis of prediction is based on the following criteria:
The average absolute relative error (AARE) should be minimum.
AARE =
1 N y predicted yexp erimental
N 1
yexp erimental
The standard deviation should be minimum.
252
y predictedl (i ) y exp erimental (i )

y exp erimental (i )
N 1
i =1
AARE ) 2
The cross-correlation coefficient, R between input and output should be around

unity
N
R=
(y
i =1
exp erimental ( i )
(y
i =1
exp erimental ( i )
y exp erimental ( mean ) )( y predicted ( i ) y predicted ( mean ) )
y exp erimental ( mean ) ) 2
(y
i =1
predicted ( i )
y predicted ( mean ) ) 2
Neural networks often encounter the well known overfitting problem, which can make
use of the ANN unreliable. To avoid overfitting and make the ANN more useful, the
following approach was used. The whole database was split into two parts, learning and
generalization. The first part, called the learning file, was used to perform minimization
using the ANN. The remaining part, called the generalization file, was used to validate
the model. Following the common practice, the learning file was made by randomly
selecting about 70% of the database to train the network. The remaining 30% of data was
then used to check the generalization capability of the model. The hidden layers, J, and
fitting parameters wij and wjk are a priori unknown. The number of hidden layers was
varied and chosen empirically according to the above criteria. The weighting parameters
were then determined by non-linear least-square regression over known random
inputs/outputs (70% of the data, which was picked randomly). The remaining 30% of the
database was utilized for validation of predicted weighting parameters. The chosen set of
inputs must show the best prediction during training and generalization, i.e., show the
least error on both learning and generalization files.
F-2.4 Results
After collecting the large databank, we subjected it to dimensional analysis, which

resulted into hundreds of dimensionless groups. As a matter of fact, using all these groups
253
is not feasible. Hence, to make the use of the developed model feasible, after forming a
number of sets of dimensionless groups, cross-correlation analysis was performed. As the
cross-correlation analysis can hide non-monotonic relationships, rigorous trial-and-error
testing with the aid of ANN was also performed. The criteria mentioned above led to four
pertinent input dimensionless groups: Reg, Frg, Eo/Mo, and g / L . The ratio of the
densities of the gas and liquid was added to account for the effect of high pressure. This
particular set of dimensionless groups showed consistent performance on both the
learning and generalization file. The sets of dimensionless groups which did not show
consistent performance were omitted, despite their remarkable performance on the
learning file.
Figure F-2 shows the parity plot of the experimental and predicted overall gas holdup
using the ANN correlation on the whole database. The ANN predicts the overall gas
holdup with an AARE of 15%. For comparison, Figure F-3 is the parity plot of the
experimental and predicted overall gas holdup, based on the whole database and using
selected literature correlations along with the ANN correlation. In this case, the
correlations were selected based on the conclusions of Kemoun et al., (2001). From the
figure, it is clear that the ANN correlation predicts overall gas holdup better than these
two correlations. Moreover, the comparison of additional important correlations in
literature on the basis of statistical analysis is shown in Table F-3, and confirms that the
ANN performs better than they do.
254
0.7
Predicted gasholdu
0.6
0.5
0.4
0.3
0.2
0.1
0
0
0.1
0.2
0.3
0.4
0.5
0.6
0.7
Experimental gasholdup
Figure F-2: Parity plot for ANN correlation using the whole databank (AARE = 15 %)
0.7
Predicted gasholdu
0.6
0.5
Luo et al. (1999)
0.4
Hammer et al. (1984)
0.3
ANN (current w ork)
0.2
0.1
0
0
0.2
0.4
0.6
Experimental gasholdup
Figure F-3: Parity plot for ANN and selected literature correlations
255
256
Table F-2: Set of equations and fitting parameters for the neural network correlation (I = 4, J = 10)
L d 2 L
EO / M O =
L4
2
Frg =
ug
Re g =
gd
du g ( L g )
DR =
g
L
Dimensional
Group
Range
S1 =
log( G / 0.002)
2.64
EO/MO
7.5E5 1.14E16
U1 =
log(( E o / M o ) / 1.97 E 7)
10.2
Reg
5.7 7.1E5
Frg
U3 =
2.3E-7 7.35E-1
Hj =
U2 =
U4 =
log(Re g / 5.71)
6.5
log(( g / L ) / 8.3E 5)
2.46
5.1
1
I +1
1 + exp[ wijU i ]
S1 =
i =1
g/ L
log( Frg ) / 2.3E 7)
1
J +1
1 + exp[ w jk H j ]
log( G / 0.002)
2.64
j =1
8.35E-5 2.40E-2
Overall Gas holdup (G)

Wij
1
2
3
4
1 3.44E+01 -9.81E+00 -5.78E+01 1.36E+02
2 -3.18E+01 -4.26E+01 -3.35E+01 -1.03E+02
3 2.25E+01 -3.18E+01 2.56E+01 7.55E+01
4 -1.37E+01 -6.86E+00 -4.88E+01 -8.64E+01
5 5.01E+00 -1.65E+01 6.48E+01 -1.33E+01
Wjk
1
1
2
1.37E+01 -1.05E+00
3
3.35E+00
5
6
7
8
9
10
1.46E+01 -4.25E+01 -2.00E+00 -2.64E+01 6.07E+01 1.74E-01
1.77E+01 8.36E+01 3.57E+00 6.71E+01 5.32E+01 -8.98E-02
3.54E+01 4.58E+01 9.27E-01 -1.19E+02 -3.81E+01 1.79E+00
1.52E+01 3.23E+01 -9.38E-01 1.03E+02 5.00E+01 2.08E+00
1.46E+01 -2.07E+01 1.82E+00 -1.62E+00 -7.11E+01 -4.72E+00
4
5
6
2.49E-01 -2.89E+01 -2.40E+00
7
1.32E+01
8
1.99E-01
9
3.19E+00
10
1.44E+01
11
11
1.56E+00
257
Table F-3: Comparison of ANN and previous literature correlations
Correlation
Akita and Yoshida (1973)

Hikita et al. (1981)
Hammer et al. (1984)
Idogawa et al. (1985)
Reilly et al. (1986)
Dharwadkar et al. (1987)
Idogawa et al. (1987)
Wilkinson et al. (1992)
Krishna et al. (1996)
Kojima et al. (1997)
Joshi et al. (1998)
Luo et al. (1999)
Jordan et al. (2001)
ANN (This Work)
AARE
(%)
27
25
37
24
28
47
54
25
29
48
30
25
24
15
Standard Deviation
(%)
32
20
26
24
47
45
10
20
23
49
24
25
19
14
The developed ANN correlation showed an improved prediction of overall gas holdup
over the wide range of database. However, to evaluate the consistency of the developed
correlation, the predictions of ANN correlation in different liquids, at different pressures,
in different column diameters were checked and found to be satisfactory. In addition, the
trends of the effect of various operating and design parameters were checked. It was
observed that, the developed correlation captures the trend reported in the literature. The
details of this part can be found in Shaikh and Al-Dahhan (2003).
F-3 ANN correlations for gas holdup and liquid axial velocity radial profile
The correlations were developed for prediction of gas holdup and liquid axial velocity
radial profiles using ANN as described above. The database for gas holdup radial profile
consists of 110 data points while for liquid axial velocity profile consists of 55 data
points.
258
F-3.1 Gas holdup radial profile
As discussed in Chapter 6, the radial profile of gas holdup is an important hydrodynamic

parameter. The similarity of gas holdup profile is pertinent for hydrodynamic similarity
criteria. In absence of reliable first principle models, we have resorted to ANN
correlation for prediction of gas holdup radial profile.
The number of empirical forms has been proposed over the years to fit the experimental
gas holdup radial profile. Nassos and Bankoff (1967) were the first one suggest following
empirical form,
n+2
)[1 (r / R) n ]
(F-5a)
n
where, ~G is the radial chordal averaged gas holdup, the exponent n is steepness
~
G = G (
parameter, and r/R is dimensionless radius. As mentioned in Chapter 2 and Chapter 5, the
value of n is large for flat profiles while it is small for steep profiles.
Ueyama and Miyauchi (1979) modified the above equation to accommodate the
possibility of finite gas holdup at the wall. They presented the following empirical form,
G = G (
n+2
)[1 c(r / R) n ]
n
(F-5b)
where, c is the wall holdup parameter. If c = 1, wall hold up is zero while c = 0 for
constant holdup with changing r/R.
Later, Luo and Svendsen (1991) was modified this form as,
G = G (
n+2
)[1 c(r / R) n ]
n + 2 2c
(F-5c)
where, G is the cross-sectional averaged gas holdup.

It is clear from above empirical forms that steepness parameter, n and wall holdup
parameter, c are necessary to predict radial profile of gas holdup. Hence, it was decided
259
to correlate these parameters with operating and design conditions. The procedure to
develop overall gas holdup correlation was also employed in this case. The operating and
design conditions were represented in terms of dimensionless numbers as per the force
analysis described in F-2.2. Table F-4 provides the range of operating and design
parameters in the collected data bank. One should note here that, gas holdup radial
profiles in air-water system constituted close to 60 % of databank. In addition, the data
was collected using different experimental techniques ranging from optical probe to
various tomographic techniques. Amongst this databank, few experimental datasets were
not used for training and validation of neural network. These datasets were utilized to
compare the predictions the developed ANN correlation.
Table F-4: Range of operating and design parameters in the collected databank for gas
holdup radial profile
Column Diameter
0.05 0.8 m
Liquid Density
866 - 1000 kg.m-3
Liquid Viscosity
0.88 - 1 cP
Surface Tension
17 - 72 mN.m-1
Gas Density
1.2 - 24 kg.m-3
0.01 0.6 m/s
0 (batch liquid)
After rigorous trial-and-error, dimensional analysis, and cross-correlation analysis, n and

c were correlated in terms of the following dimensionless numbers that were found to
have profound effect on these parameters,
n = f {Mo, Re, Fr, ( G / G )}
(F-6)
c = f {Mo, Re, ( G / G )}
(F-7)
The table of normalized inputs and weighting parameters is provided in Table F-5a and b.
260
Table F-5a: Set of equations for ANN correlation of steepness parameter, n
U1 =
U4 =
Hj =
lo g ( R e g / 2 5 0 )
2 .6 5
U2 =
log( Frg / 3.5 E 5)
U3 =
3.81
log( DR / 0.001)
1.14
log( M o / 2 E 11)
7.47
S1 =
1
I +1
1 + exp[ wijU i ]
1
J +1
1 + exp[ w jk H j ]
log(n /1.2)
1.24
j =1
i =1
Steepness parameter (n)
Table F-5b: Set of equations for ANN correlation of wall holdup parameter, c
U1 =
U4 =
Hj =
lo g ( R e g / 2 5 0 )
2 .6 5
log( M o / 2 E 11)
7.47
U2 =
log( Frg / 3.5 E 5)
U5 =
3.81
I +1
1 + exp[ wijU i ]
i =1
log( DR / 0.001)
1.14
log( Eo / 250)
2.54
S1 =
U3 =
1
J +1
1 + exp[ w jk H j ]
log(c / 0.005)
2.3
j =1
Wall holdup parameter (c)
The parity plot for n and c with the final ANN model is shown in Figures F-4a and b,
respectively. In case of steepness parameter, n, AARE, standard deviation, and crosscorrelation coefficient (between experimental and predicted output) were 9.5 %, 12.5 %,
and 0.98, respectively. In the case of wall holdup parameter, c, AARE, standard
261
deviation, and cross-correlation coefficient were 12.5 %, 13 %, and 0.85, respectively.
The trends of the effect of operating and design parameters on gas holdup radial profile
predicted using ANN correlation were found to be consistent with the literature findings.
20
Predicted 'n'
15
10
0
0
10
15
20
Experimental 'n'
(a)
1
Predicted 'c'
0.8
0.6
0.4
0.2
0
0
0.2
0.4
0.6
0.8
Experimental 'c'
(b)
Figure F-4: Parity plot of a) steepness parameter, n and b) wall holdup parameter, c.
262
F-3.2 Axial velocity radial profile
This part deals with the development of a correlation to predict liquid axial velocity
profile. We have adopted the procedure similar to the one utilized in above mentioned
correlations. In literature, various empirical forms have been proposed to fit observed
axial velocity profile. However, the following empirical form proposed by Kawase and
Moo-Young (1986) and Tobajas and Garcia-Calvo (1996) is commonly used in the
literature.
VL = VL 0 [1 2 N / 2 (r / R) N ]
(F-8)
where, N is parameter that defines the strength of the circulation.
Kawase and Moo-Young (1986) proposed to use the value of N to be 2 while Tobajas and
Garcia-Calvo (1996) proposed it to be 2.3. We have shown in Chapter 6 that, the
magnitude of gas holdup and its radial profile are responsible for liquid recirculation in
bubble columns. Hence, we have decided to relate the axial velocity profile with gas
holdup radial profile. For this purpose, the value of exponent N was correlated as
N = f ( n, c )
(F-9)
Table F-6 shows the range of operating and design parameters in the databank collected
for liquid axial velocity profile. The collected database was fitted to the above mentioned
empirical form to obtain the values of N. The values of n and c were calculated using the
correlations developed in F-3.1. ANN was used to correlate the values of n and c as
inputs with the corresponding values of N as output. The table of normalized inputs and
weighting parameters is provided in Table F-7.
263
Table F-6: Range of operating and design parameters in the collected databank for liquid
axial velocity profile
Column Diameter
0.1 0.6 m
Liquid Density
724 - 1000 kg.m-3
Liquid Viscosity
1 - 30 cP
Surface Tension
24 - 72 mN.m-1
Gas Density
1.2 - 12 kg.m-3
0.006 0.45 m/s
0 (batch liquid)
Table F-7: Set of equations and fitting parameters for ANN correlation of circulation
strength, N
U1 =
Hj =
log(n /1.2)
1.24
U2 =
log(c / 0.005)
2.3
S1 =
1
I +1
1 + exp[ wijU i ]
i =1
1
J +1
1 + exp[ w jk H j ]
log( N / 0.02)
2
j =1
Recirculation strength parameter (N)
Figure F-5 shows the parity plot of the exponent, N using the final ANN model. AARE,
standard deviation, and cross-correlation coefficient (between experimental and predicted
output) were found to be 9 % %, 7 %, and 0.92, respectively. The trends of the effect of
operating and design parameters on liquid axial velocity profile predicted using ANN
correlation were found to be consistent with the literature findings.
264
P redicted 'N '
0
0
Experimental 'N'
Figure F-5: Parity plot of exponent of velocity profile, N.
F-3.3 Center-line axial velocity
The prediction of center-line velocity is crucial in design and scaleup of bubble column
reactors as it determines the magnitude of liquid axial velocity profile. Hence, the
database collected for liquid axial velocity profile was utilized to develop a correlation
for center-line velocity. First, we have evaluated the reported center-line velocity
correlations with collected experimental center-line velocities. Table F-8 shows the
reported correlations along with the authors. Figure F-6 compares the predictions of these
correlations with experimental data while Table F-9 shows the statistical analysis of these
correlations. It is clear that, none of the reported correlations predict center-line velocity
with statistical confidence. Hence, a correlation was developed for center-line velocity
with the using ANN. Based on the ANN, dimensional analysis, and cross-correlation
analysis, the center-line axial velocity was correlated in terms of the following
dimensionless numbers,
VL (0) = f {Eo, Mo, Re, Fr, ( G / G )}
(7-10)
The table of structure of model and weighting parameters is provided in Table F-10.
265
Table F-8: Literature correlations for center-line velocity
Author
Ohki and Inoue
(1970)
Center-line velocity correlation
1.9U G0.6
Riquarts (1981)
0.21 D g (
U G L 1/ 8
)
L g
0.73 ( g U G D)1 / 3
Nottenkamper
(1983)
Ulbrecht et al.
(1985)
U L + 0.66 D 0.69 +1.11U G
Predicted center-line velocity (m/s)
Zehner (1982)
3.34 g 0.23 U G0.46 D 0.15 ( L / L ) 0.08
2.5
Ohki and Inoue (1970)
Riquarts (1982)
2
Zehner (1983)
Nottenkamper (1983)
Ulbrecht et al. (1985)
1.5
Experimental
1
0.5
0
0
0.2
0.4
0.6
0.8
Experimental center-line velocity (m/s)
Figure F-6: Parity plot for literature correlations using the whole database.
266
Table
F-9:
Comparison
of
prediction
of
literature
correlations
with
experimental databank.
Author
AARE
Ohki and Inoue

(1970)
Riquarts (1981)
Zehner (1982)
Nottenkamper
(1983)
Ulbrecht et al.
(1985)
This work
(%)
49
Standard
Deviation
(%)
45
27
19
22
25
20
10
0.82
0.89
0.71
43
30
0.65
11
10
0.96
Crosscorrelation
coefficient
0.48
Table F-10: Set of equations for ANN correlation of center-line axial velocity, VL0
U1 =
U4 =
Hj =
lo g ( R e g / 2 5 0 )
5 .4 8
log( M o / 2 E 11)
7.47
U2 =
U5 =
log( Frg /1E 5)

4.36
I +1
1 + exp[ wijU i ]
i =1
log( DR / 0.001)
1.22
log( Eo /1000)
3.65
S1 =
U3 =
1
J +1
1 + exp[ w jk H j ]
log(VL 0 / 0.02)
2
j =1
Center-line velocity (VL0)
the
267
Figure F-7 shows the parity plot of center-line liquid velocity using the developed ANN
correlation. AARE, standard deviation, and cross-correlation coefficient was found to be
11 %, 10 %, 0.96, respectively. The trends of the effect of operating and design
parameters on center-line liquid velocity predicted using ANN correlation was found to
be consistent with the literature findings.
Predicted center-line velocity (m/s)
0.8
0.6
0.4
0.2
0
0
0.2
0.4
0.6
0.8
Experimental center-line velocity (m/s)
Figure F-7: Parity plot for ANN correlation using whole database.
F-4 Remarks
This chapter deals with the development of ANN based correlations for a priori
prediction of needed hydrodynamic parameters. As an example, the correlation to predict
overall gas holdup is demonstrated. The correlation is developed by collecting
experimental results from open literature (3500 measurements) with the aid of Artificial
Neural Network and Dimensional Analysis. Neural Network correlation shows noticeable
improvement in the prediction of overall gas holdup compared to selected literature
correlations. The neural network correlation yields AARE of 15 % with standard
deviation of 14 %, which is better than those obtained for the selected literature
correlations. This work identified Reg, Frg, Eo/Mo, g / L as expressive dimensional
groups to overall gas holdup. Also, there is improved prediction for variety of liquids,
wide range of operating pressures and column diameters, which can be useful in the
268
scale-up of bubble column reactors. The simulations have been performed using
developed ANN correlation and found to give the trends reported in literature.
The ANN correlations were developed for additional hydrodynamic parameters such as
radial profile gas holdup and liquid axial velocity and center-line liquid velocity. The
developed correlations were found to be statistically consistent with the databank.
However, it is worth mentioning that databank available for radial profile gas holdup and
liquid axial velocity and center-line liquid velocity is limited and mostly comprises the
databank in air-water system. Hence, the performance of these developed correlations
outside its range cannot be guaranteed. However, in absence of reliable predictions of
models based on first principles, it presents a preliminary predictive platform that may
provide an initial guideline towards scaleup and design of these reactors.
269
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Vita
Date of Birth
July 5, 1975
Place of Birth
Mangalvedha (Maharashtra), India
Degrees
Bachelor of Technology in Petrochemical Engineering, 1992- 1996
Dr. B. A. Technological University, Lonere (MS), India
Master of Technology in Chemical Engineering, 1998- 2000
Indian Institute of Technology (IIT), Madras, India
Doctor of Science in Chemical Engineering, 2001-2007
Washington University, St. Louis, MO
Industrial Experience
Summer Intern at Amar Dyechem Ltd., Mahad, India, (1993)
Summer Intern at Vinati Organics Ltd., Mahad, India, (1994)
Summer Intern at Hikal Chemicals Ltd., Mahad, India (1995)
Process Engineer, Kesar PetroProducts Ltd. Lote Parashuram, India,
(1996-1998)
Professional Societies
American Institute of Chemical Engineering (AIChE)
International Association for Energy Economics (IAEE)
Publications
Shaikh A. and Al-Dahhan, M. H.; A New Methodology for Online Flow Regime
Monitoring in Bubble Column Reactors to be submitted.
Shaikh, A.; and Al-Dahhan, M. H., A New Methodology for Scaleup of Bubble Column
Reactors to be submitted.
Shaikh, A.; and Al-Dahhan, M. H.; Scaleup of Bubble Column Reactors: A Review of
Current-State-of-the-Art, submitted.
280
Nedeltechev, S.; Shaikh, A.; and Al-Dahhan, M. H.; (2007). Prediction of the
Kolmogorov Entropy Derived from CT Data in an Atmospheric Bubble Column
Operated in Transition Regime accepted Chemical Engineering and Technology.
Shaikh, A.; and Al-Dahhan, M. H.; (2007). A Review on Flow Regime Transition in
Bubble Columns, accepted International Journal of Chemical Reactor Engineering
Nedeltechev, S.; Shaikh, A.; and Al-Dahhan, M. H.; (2006). Identification of Flow
Regimes in a Bubble Column Based on Chaos Analysis of -ray Computed Tomography
Data. Chemical Engineering and Technology, 29 (9), 1 (Special Issue dedicated to 65th
Anniversary of Prof. W. D. Deckwer).
Rados, N.; Shaikh, A.; and Al-Dahhan, M. H.; (2005). Solids Flow Visualization in High
Pressure Slurry Bubble Column, Chem. Eng. Sci., 60 (22), 6067 (Special Issue on GasLiquid and Gas-Liquid-Solid Reactor Engineering).
Shaikh, A.; and Al-Dahhan, M. H.; (2005). Characterization of Hydrodynamic Flow
Regime in Bubble Columns via Computed Tomography, Flow Measurement and
Instrumentation, 16(2-3), 91 (Special Issue on Tomographic Techniques for Multiphase
Flow Measurements).
Rados, N.; Shaikh, A.; Al-Dahhan, M. H.; (2004). Phase Distribution in a High Pressure
Slurry Bubble Column via Single Source Computed Tomography, Can. J. Chem. Eng., 83
(1), 104 (Special Issue on Industrial Process Tomography).
Shaikh, A.: and Al-Dahhan, M. H.; (2003). Development of an Artificial Neural Network
Correlation for Prediction of Overall Gas Holdup in Bubble Column Reactors, Chem.
Eng. Proc., 42, 599 (Special Issue on Application of Neural Networks to Multiphase
Reactors).
Presentations
Shaikh A. and Al-Dahhan, M. H.; (2007). A New Methodology for Online Flow Regime
Monitoring in Bubble Column Reactors. accepted Oral Presentation 5th world Congress
on Industrial Tomography, Bergen, Norway.
Al-Dahhan, M. H. and Shaikh A.; (2006). Advances in Reactor Technology for FischerTropsch Synthesis with Biomass as a Feedstock: A New Methodology for Scale-up of
Bubble Column Reactors. Plenary Lecture at BTLtec06, Munich, Germany.
Shaikh A. and Al-Dahhan, M. H.; (2005). A New Methodology for Scale-up of Bubble
Column Reactors. North American Mixing Forum, AIChE Annual Meeting, Cincinati,
OH, USA.
281
Shaikh A. and Al-Dahhan, M. H.; (2005). A New Methodology for Scale-up of Bubble
Column Reactors. Plenary Talk at 5th International Chemical Engineering Conference,
Amman, Jordan.
Shaikh, A.and Al-Dahhan, M. H.; (2004). Characterization of Hydrodynamic Flow
Regime in Bubble Columns via Computed Tomography, Oral Presentation, North
American Mixing Forum, AIChE Annual Meeting, Austin, USA.
Rados, N.; Shaikh, A.; Al-Dahhan, M. H.; (2003). Phase Distribution in a High Pressure
Slurry Bubble Column via Single Source Computed Tomography, Keynote Presentation
at 3rd world Congress on Industrial Tomography, Banff, Canada.
Rados, N.; Kemoun, A.; Shaikh, A.; Al-Dahhan, M. H.; Dudukovic, M. P.; (2002).
Implementation of Radioactive Particle Tracking and Tomography in Flow Visualization
of High Pressure Slurry Bubble Column Reactors, Oral Presentation, 4th Symposium on
High Pressure Technology and Chemical Engineering, Venice, Italy.
Shaikh, A.; Al-Dahhan, M. H.; (2001). Development of Neural Network based
Correlation for Overall Gas Holdup in Bubble Column, Poster Presentation, AIChE
Annual Meeting, Reno, USA.
August 2007.

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WASHINGTON UNIVERSITY

1.3 Thesis Organization .

2.1 Mixing of liquid/slurry phase .

2.2 Flow Regime Transition .

2.2.1 Flow Regime Types and Characteristics

2.2.2 Methods for Flow Regime Identification ..

2.2.3 Prediction of Flow Regime Transition ..

2.3 Scaleup of Bubble Column Reactors

2.3.1 Reported status of scaleup in literature ..

2.3.2 Reported status of scaleup in industry

Experimental Investigation of the Hydrodynamics of Slurry

3.1 Choice of Phases ..

3.2 Experimental Details

3.3 Single Source Computed Tomography (CT)

3.4 Results and Discussion.

3.4.1 Overall gas holdup ...

3.4.2 Drift Flux Model ..

3.4.3 Cross-sectional Distribution of Gas Holdup

3.4.4 Time averaged gas and solids holdup radial profile

3.4.5 Effect of liquid phase physical properties on gas and solids

3.4.6 Effect of solids loading on gas and solids holdup radial

3.4.8 Normalized gas holdup radial profile .

3.4.9 Normalized solids holdup radial profile .

3.4.7 Comparison with predictions of Sedimentation-Dispersion

Experimental Investigation of the Hydrodynamics of Slurry

4.2 Computer Automated Radioactive Particle Tracking (CARPT) ..

4.3 Results and Discussion .

4.3.1 Time averaged solids velocities ..

4.3.2 Turbulent stresses and kinetic energy ..

4.3.3 Effect of liquid phase physical properties on solids axial

4.3.4 Effect of solids loading on solids axial velocity and turbulent

4.3.5 Cross-sectional averaged turbulent stresses .

4.3.6 Turbulent eddy viscosity

4.3.7 Eddy diffusivities .

Flow Regime Transition ...

5.1 Flow Regime Transition using CT ...

5.1.1 Experimental setup and conditions

5.1.2 Results and Discussion ...

5.1.3 Evaluation of the empirical correlations .

5.2 Flow Regime Transition using NGD

5.2.1 Nuclear Gauge Densitometry (NGD)

5.2.2 Results and Discussion ...

5.2.3 Evaluation of the flow regime identifiers developed for

5.2.4 Evaluation of literature correlations

Scaleup of Bubble Column Reactors ...

6.1 Hypothesis for hydrodynamic similarity ..

6.2 Experimental conditions ...

6.3 Results ...

6.4 Development of correlations for a priori prediction of

Summary and Recommendations ...

7.1 Summary and Conclusions ...

Appendix-A. Phase Distribution in Three Dynamic Phase Systems via

Appendix -B. Experimental Investigation of Hydrodynamics of Slurry

Appendix -C. Experimental Investigation of Hydrodynamics of Slurry

Appendix -D. Sedimentation-Dispersion Model 231

Physical properties of Sasol wax and Therminol LT

Experimental conditions employed in this study

The values of drift flux parameters at the studied experimental

CARPT experimental conditions

Comparison of experimental and predicted transition velocities

Characteristics frequencies in bubble column (Drahos et al.,

Slope of power spectra at studied operating conditions

Experimental conditions for evaluation of flow regime