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Chemical Enclineerim d Science, Vol. 53, No. 3, pp. 495 5(13, 1998
1998 Published by Elsevier Science Ltd. All rights reserved
Printed in Great Britain
0oo9 250998 $19.00 ~-o.l~)
PII: b01109-2509197)00320-5
INTRODUCTION
495
C. H. E. Nielsen et al.
496
o
o
t~
6
e-q
8
N
.=_
r,2
4
-6
eq
'.~
,2
.=_
E
Gilliland and Sherwood (1934) found that the gasphase mass transfer coefficient is pressure-independent in the investigated range from 0,145 to 3.06 atm,
but dependent on R % . The liquid flow was kept
constant (Re L ~ 1000) and so the dependency of Sh e
on Ret~ was not investigated. Using the Reynolds
number calculated relative to the column wall, R % ,
rather than the Reynolds number relative to the liquid
film surface, Rear, they found it feasible to correlate
both countercurrent and cocurrent mass transfer data
with just one correlation. Kafesjian et al. (1961), on
the basis of their own measurements and data from
the literature, including those of Gilliland and Sherwood (1934), determined a dimensionless correlation
for Sh G with a dependency on both Re a and Re L. The
dependency on S % was not investigated and no experimental temperature was provided in the paper,
preventing recalculation of the correlation with Sc 5
G '
which is the correct dependency on S % as reported
recently by Dudukovi6 et al. (1996). They showed that
the relative errors of the Gilliland and Sherwood
(1934) and Barnet and Kobe (1941) data are reduced
when the theoretical Schmidt number exponent of 0.5
for gas/liquid mass transport is used rather than the
theoretical exponent of 0.33 for gas/solid mass transport or an experimental value for the exponent of 0.44
found by Gilliland and Sherwood (1934). Braun and
Hiby (1970) studied the effect of humidity, H, on Sh G.
They found Sh e to be independent of H for H > 80%,
but dependent on the column height, L, and R% and
Re L. However, the correlation is only valid for
L i d i < 35, making it unsuitable for use on pilot- and
industrial-scale columns. Thus, published correlations
for She are valid at low liquid-phase Reynolds numbers only. There seems to be no correlations available
for the design of columns employing liquid-phase
Reynolds numbers of 5000 or higher. It is one of the
aims of this work to determine an empirical correlation for She, valid at industrially relevant flow conditions (i.e. high Reynolds numbers).
d~ X
Physical liquid-phase mass transfer coefficient, k
~+
[-.,
5
II
II
e~
II
-~
g
'~
=o
.~
.=
.-=
0
0
"7-
~
~X ~
r"-
II
497
"7-
x
t~
"~ +
II
e,
O
e-,
<
C. H. E. Nielsen et al.
498
A dimensional analysis (Bird et al., 1960) was conducted on the setup to predict the dimensionless
groups in terms of which Sh a and Shl~ may be correlated. It was assumed in the analysis that the liquid
film is plane. The analysis showed that, theoretically,
S h L depends on Re~. and SCL, whereas Sh G depends on
R % and Sc~ for L/di>>l. The latter criterion was
found to be valid for all measurement positions in the
applied column. The dimensional analysis does not,
however, provide any information on the functional
relationship of the dimensionless groups. It will be
shown later that experimental data suggest that Sh~
also depends on Re L and Shr. on Rea. The reason for
this is probably the formation of waves or ripples on
the liquid film at high Reynolds numbers which alter
the interracial area and cause more turbulent fluid
(1)
SETUP
499
" 'SO~_
Heat
' HzO
Film distributor
Atr m
Gas probe
Compressor
Liquid probe\
Wetted-wall column
Gas
Gas analyzer
Hold tank
/
Flow loop for
measuring pH ect.
N2
Hosepump
Gas inlet
1
Gas probe
Liquid probe
Liquid out
cone
Oxygen electrode
Volt signal to PC
Wetted-wall column
Absorber tube
L-pipe
Liquid inlet
m
Gas to sample train
C. H. E. Nielsen et
500
In(CG'')
26L)RAL
\CG,out/
(2)
( di - 26L~R A.
ac = \
di ]
Q G l n ( C~'in ~ = kGacL.
(4)
Cl~,i - HO.
3.6-101/min
20~4001/min
50~C
1 atm
5, 110, 180 #m
5, 10, 20, 30 wt%
5.0 m
3.26 cm
\CG,ouJ
Liquid flow, QL
Gas flow, Qc,, at 50C and 1 atm
Temperature, T
Pressure, P
Particle mean diameter, dp
Solid concentrations, 4,,
Height of column, L
Inner diameter of column, d~
(3)
~di
al.
(6)
The S 0 2 / N a O H system
To obtain data for k~, a system in which lean SO 2
( ~ 1000 ppmv) was absorbed into a strong N a O H
solution (pH > 11.9) was used. In this system, the
liquid-phase mass transfer resistance can be con-
988.04 kg/m a
1.0928 kg/m 3
546.8 x l0 -6 kg/ms
19.6x10 6kg/ms .
1.22 x 10- s mZ/s
Water density, p*
Dry air density, p*
Water viscosity, p~
Air viscosity,/~
Diffusion coefficient for
SO2 in air, Ds*o2
Diffusion coefficient for
02 in water, D~o:
Henry constant for 02, H *
3.93 x 10 9 m2/s
32.94 x 10- 3 atm l/mg
k~Pso 2 <<,kLCNaOH
(7)
--<<1.
Hk6
(8)
5s
45
--
Sh~; = O.O0031Re~SRe2TSc 5.
Sh L = O.Ol613Re664Re"*Z6Sc s.
(10)
1
x ReL=12000
a ReL= 9500
ReL= 7000
o ReL= 4700
//."
(9)
501
15
7000
x:
9000
11000
Reo
13000
15000
700
* R%= 18300
600 ~_ Re~-=12200.
o R%= 9900
Re~= 7600
500
,,
*j
*
i*
- - Y~," /
400
o
O']
300
200
100
3000
I!
5000
7 0 0 0 9000
ReL
11000 13000
experiment and setups are almost identical. No explanation for this inconsistency could be found. Figs 4
and 5 both show that the effect of increasing Re~ is to
enhance the rate of mass transfer. This is probably due
to more gas-phase turbulence and/or an increased
interfacial area. It is apparent that k~ac has a stronger
dependency on Ret. at high values of Re~ than at low
values. In Fig. 6, eq. (10) is compared with the correlation given by Henstock and Hanratty (1979). It can be
seen that the correlation of Henstock and Hanratty
(1979) predicts a physical liquid-phase mass transfer
coefficient significantly higher than eq. (10) at all
values of Ret. and has a stronger dependency on Rea.
The Henstock and Hanratty correlation suffers from
the disadvantage of having a strong dependency on
the falling liquid film thickness. An increase in the
liquid film thickness of as little as 0.2 m m reduces the
C. H. E. Nielsen et al.
502
CONCLUSIONS
1500
--
Present work
....
Henstock and
Hanratty (1979)
Rec,= 18000
1300
1 IOO
0
j
900
/ ~, ~"
/t'
/.J
.-~
700
R%= 7500
5OO
000
300
R%= 7500
100
3000
,
5000
7000
9 0 0 0 11000 13000
Re L
Fig. 6. Comparison of fitted correlation eq. (10), with the
dimensionless correlation of Henstock and Hanratty (1979).
The gas- and liquid-phase mass transfer coefficients, koa,. and ka~, were measured for a broad
range of gas- and liquid-phase Reynolds numbers in
a pilot-scale wetted-wall column at atmospheric pressure and 50~C. Two empirical dimensionless correlations which describe the experimental data with mean
deviations of 2.7 and 12.1% were found. The correlations are valid at high Reynolds numbers, conditions
of industrial relevance. It was shown that the increased interracial area and turbulence, due to waves
on the liquid film, are of significant importance. The
effect of inert (sand) particles present in the liquidphase on kGac was investigated at solid concentrations
ranging from 0 to 30 wt%. At high solid concentrations, the effect was seen as a reduction in koa,. of up to
15%. The data obtained at low solid concentrations,
however, were too scattered for the results to be
correlated. More work needs to be done to clarify and
correlate the effect of inert particles on the mass transfer coefficients in wetted-wall columns.
Acknowledgements
This work was carried out as a part of the CHEC (Combustion and Harmful Emission Control) research programme.
NOTATION
ac
RA(di - 2;)L)/di
di
dp
D
F
Inert particles
The effect of inert particles present in the liquid
phase on the rate of gas-phase mass transport was
investigated. The particle type used was sand with
three different mean diameters, 5, 110 and 180pm.
The applied solid concentrations were 0, 5, 10, 20 and
30wt%; the initial liquid volume in the system
was kept constant at 30 1. Also, the gas and slurry
flows were kept constant at Rea = 11,000 and
QL = 7.9 l/rain. The results showed a reduction of
about 15% in koa,. at the high solid concentrations. At
low solid concentrations, however, both reduction
and enhancement of koa,. was observed, preventing
correlation of the data. No explanation could be
found for the scatter of the data, and the above conclusions are strictly qualitative. A number of investigators (e.g. Joosten et al., 1977; Oztiirk and Schumpe,
1987) have examined the effect in bubble-column
slurry reactors. Their results are somewhat similar to
ours, with enhancements of ka at low solid concentrations and reductions at high. It is thought that the
change in k~ a~ is due to a dilution and/or stabilization
of the liquid film by the solid particles. However, more
work needs to be done in this important field before
the data can be correlated.
9
H
H
kG
k
k~-k4
L
m
p
Q
RA
ReG
Rear
(~L/~G)(P~/PL) s
gravity, 9.82 m/s 2
humidity
Henry's constant, atm m3/mol
gas-phase mass transfer coefficient, m/s
physical liquid-phase mass transfer coefficient, m/s
dimensionless empirical constants
height of column tube, m
dimensionless liquid film thickness,
(0.4203Re~/2s + 2.796Re~'2s) 4
partial pressure, atm
volumetric flow, m~/h
ratio of the interfacial area in the presence of
waves to the plane interfacial area
gas-phase Reynolds number, 4Q~p6/gdi#G
relative gas-phase Reynolds number,
4Qarpc,/7~diPG
ReL
ScG
ScL
Shc,
ShL
T
X
Greek letters
6L
c,,
I~
q)
1.8X'33Re
0"0625
density, kg/m 3
Subscripts
G
i
in
L
out
r
gas phase
interface
inlet
liquid phase
outlet
relative to the liquid surface
REFERENCES
503