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Dynamics and Predictive Control of Gas Phase Propylene Polymerization in

Fluidized Bed Reactors

Data · November 2013

DOI: 10.13140/RG.2.1.4298.3128

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PROCESS SYSTEMS ENGINEERING AND PROCESS SAFETY
Chinese Journal of Chemical Engineering, 21(9) 1015—1029 (2013)
DOI: 10.1016/S1004-9541(13)60565-0

Dynamics and Predictive Control of Gas Phase Propylene

Polymerization in Fluidized Bed Reactors*

Ahmad Shamiri1,2,**, Mohamed azlan Hussain1,3, Farouq sabri Mjalli4, Navid Mostoufi5 and
Seyedahmad Hajimolana1
1
Department of Chemical Engineering, University of Malaya, Kuala Lumpur 50603, Malaysia
2
Training Center, Razi Petrochemical Company, Bandar Imam 161, Iran
3
UM Power Energy Dedicated Advanced Centre (UMPEDAC), University of Malaya, Kuala Lumpur 50603, Malaysia
4
Petroleum and Chemical Engineering Department, Sultan Qaboos University, Muscat 123, Oman
5
Process Design and Simulation Research Center, School of Chemical Engineering, College of Engineering, Uni-
versity of Tehran, Tehran 11155/4563, Iran

Abstract A two-phase dynamic model, describing gas phase propylene polymerization in a fluidized bed reactor,
was used to explore the dynamic behavior and process control of the polypropylene production rate and reactor
temperature. The open loop analysis revealed the nonlinear behavior of the polypropylene fluidized bed reactor, jus-
tifying the use of an advanced control algorithm for efficient control of the process variables. In this case, a central-
ized model predictive control (MPC) technique was implemented to control the polypropylene production rate and
reactor temperature by manipulating the catalyst feed rate and cooling water flow rate respectively. The corre-
sponding MPC controller was able to track changes in the setpoint smoothly for the reactor temperature and pro-
duction rate while the setpoint tracking of the conventional proportional-integral (PI) controller was oscillatory with
overshoots and obvious interaction between the reactor temperature and production rate loops. The MPC was able
to produce controller moves which not only were well within the specified input constraints for both control vari-
ables, but also non-aggressive and sufficiently smooth for practical implementations. Furthermore, the closed loop
dynamic simulations indicated that the speed of rejecting the process disturbances for the MPC controller were also
acceptable for both controlled variables.
Keywords model predictive control, fluidized bed reactor, propylene polymerization, Ziegler-Natta catalyst

1 INTRODUCTION is highly exothermic. To maintain acceptable polymer

Modeling and control of polymerization process
in fluidized bed reactors such as polypropylene pro-
duction are challenging issues in process control en-
gineering. This is due to many factors such as the high
non-linearity of the process dynamics involving com-
plicated reaction mechanisms, complex flow character-
istics of gas and solids, various heat and mass transfer
mechanisms and the interaction between the process
control loops. Many studies were reported on the mod-
eling and control of ethylene polymerization processes
using various types of algorithms [1-6]. However, there
is little work on the modeling and control of gas phase
propylene polymerization in fluidized bed reactors.
The schematic of an industrial gas-phase fluid-
ized bed polypropylene reactor with control design is
shown in Fig. 1. The feed gas stream provides mono-
mer, hydrogen and nitrogen, and at the same time agi-
tates and fluidizes the bed through the distributor and
also removes the heat of polymerization reaction. Po-
lymerization occurs in the fluidized bed in the pres-
ence of Ziegler-Natta catalyst and triethyl aluminum
co-catalyst. The unreacted gas exits the top of the reactor
and is then compressed and cooled before being fed
back into the bottom of the fluidized bed. The polymer
production rate in this system is limited by heat removal
from the circulating gas since the polymerization reaction
production rate, which is an important goal for indus-
try, it is necessary to keep the bed temperature above
the dew point of the reactants to avoid gas condensation
and below the melting point of the polymer to prevent
particle melting, agglomeration and consequent reactor
shut down. For these reasons, process stabilization for
propylene polymerization in a fluidized bed reactor is
a challenging problem to be addressed through an ef-
ficient control system design.
Most of the reactor design and control problems
are associated with achieving adequate production rate
and heat removal from the reactor. The steady-state
and dynamic behavior of the reactor is influenced by
many process variables such as the superficial gas
velocity, feed gas temperature, monomer concentration,
catalyst activity and catalyst feed rate. Choi and Ray
[1] used a dynamic model considering bubble and
emulsion phases in the bed in the first attempt to de-
scribe the dynamics of polypropylene production. They
showed that a PI feedback control scheme can be used
to control the process transients, but it was limited by
the recycle gas cooling capacity. Dadebo et al. [2]
showed that for the temperature control of industrial
gas phase polyethylene reactors, the nonlinear error
trajectory controller (ETC) exhibited significantly supe-
rior responses in terms of speed, damping and robust-
ness compared with an optimally-tuned proportional

Received 2012-02-17, accepted 2013-01-12.

* Supported by the Research Grants of the Research Council of Malaya.
** To whom correspondence should be addressed. E-mail: a.shamiri@um.edu.my
1016 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013
Figure 1 Simplified schematic of an industrial gas-phase fluidized bed polypropylene reactor with a model predictive con-
trol (MPC) design
TI—temperature transmitter; FT—mass flow transmitter
integral derivative (PID) controller over a wide range
of operating conditions. Ali et al. [3] proposed a
non-linear process model based control (modified ge-
neric model control) for the control of liquid propylene
polymerization. The controller manipulated the hy-
drogen flow rate and cooling water flow to follow the
setpoints for cumulative melt index and reaction con-
version. They showed that the proposed controller has
good setpoint tracking and disturbance rejection prop-
erties and it was superior to the conventional generic
model control and proportional-integral (PI) control
algorithms. Ibrehem et al. [4] modeled the process in
four phases namely: bubble, cloud, emulsion and solid
phases with polymerization reactions occurring in the
emulsion and solid phases to describe the olefin po-
lymerization in fluidized bed reactor. They imple-
mented neural-networks based predictive controller
(NNMPC) to control the system and showed that the
performance of the NNMPC was superior to the PID
controller in terms of the setpoint tracking. Summary
of relevant studies in olefin polymerization and its
control are listed in Table 1. The summary shows that
most of the control studies are related to polyethylene
and only three of them are related to polypropylene.
Due to nonlinearities in the process dynamics and
difficulties involved in the control of the gas phase
propylene polymerization fluidized bed reactor, an
efficient process control scheme is vital for stable and
efficient operation of the process. The most commonly
used controllers in industrial applications are propor-
tional-integral (PI) controllers [23]. A more intelligent
and efficient process control scheme, model predictive
control (MPC) algorithm, is gradually becoming
popular in the process industries due to their ability to
handle process interactions, constraints on manipulated
and output variables and time delays as well as their
ability to control nonlinear processes [25]. The unified
framework of MPC and its capacity to incorporate
various practical control objectives and requirements
have found extensive acceptance in the chemical
process industries. However, linear model predictive
control (LMPC) algorithms are incapable to handle
the complexities encountered in nonlinear processes.
Nonlinear model predictive control (NMPC) has good
capability in improving control and operation of nonlin-
ear processes such as these polymerization processes.
The basic principle of NMPC is the same as LMPC
with the exception that the model describing the proc-
ess dynamics is nonlinear [12, 14]. Successful applica-
tions of NMPC on polymerization reactors have been
reported, which is also capable of dealing with unan-
ticipated changes in the process dynamics through the
state estimator. Summary of relevant studies in olefin
polymerization and its control are listed in Table 1.
Based on our knowledge it is the first time that a
multiple-input, multiple output (MIMO) model pre-
dictive control (MPC) strategy as a centralized MPC
technique is used to control the polypropylene produc-
tion rate and reactor temperature for setpoint tracking
and disturbance rejection. Furthermore, a two-phase
model with comprehensive kinetics for propylene
 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013 1017

Table 1 Summary of control studies in olefin polymerization

Reactor type Model Control algorithm Variables controlled Reference
fluidized bed polyethylene two phase PID feed concentration [7]
pressure
temperature
bed level
continues stirred bed polypropylene CSTR (well mixed) PID temperature [8]
bed level
pressure
fluidized bed polyethylene CSTR (well mixed) NMPC feed flow rates [9]
LMPC temperature
PI bleed flow and pressure
fluidized bed polyethylene CSTR (well mixed) ETC temperature [2]

fluidized bed polyethylene CSTR (well mixed) PID melt index and density [10]

fluidized bed polypropylene and two phase PI temperature [1]

polyethylene
hollow shaft liquid-pool CSTR (well mixed) GMC melt index [3]
polypropylene monomer conversion
fluidized bed polyethylene CSTR (well mixed) IMC melt index [11]
density
fluidized bed polyethylene two phase MPC (INCA) melt index [12]
density
temperature
production rate
fluidized bed polyethylene four phase NNMPC molecular weight [4]
temperature
fluidized bed polyethylene two phase and CSTR (well mixed) PID temperature [13]
pressure
bed level
polyethylene CSTR CSTR (well mixed) NMPC partial pressures of the [14]
gas phase compositions
production rate
fluidized bed polyethylene two phase PI temperature [15]
monomer concentration
fluidized bed polyethylene two phase PI temperature [16]
NMPC monomer concentration
fluidized bed polyethylene CSTR (well mixed) NMPC molecular weight distribution [17]

fluidized bed polyethylene two phase PID bed level [18]

fluidized bed polyethylene CSTR (well mixed) PI temperature [19]

pressure
bed level
density
melt flow index
production rate
fluidized bed polyethylene CSTR (well mixed) PID density and melt flow index [20]
optimal servo system
fluidized bed polyethylene CSTR (well mixed) PID temperature [21]

slurry polypropylene CSTR (well mixed) NMPC melt flow index [22]
amount of unreacted monomer
fluidized bed polyethylene two phase PI temperature [23]

fluidized bed polyethylene CSTR (well mixed) fuzzy logic temperature [24]

homo-polymerization in a fluidized bed reactor that excess gas in the emulsion phase with polymerization
considers the presence of particles in the bubbles and reaction in both phases is also considered [26-29].
1018 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013

2 MATHEMATICAL MODEL OF PROPYLENE
POLYMERIZATION
2.1 Reactor model
In the present study, the kinetic model of propyl-
ene homo-polymerization over a Ziegler-Natta cata-
lyst (based on the kinetic model developed by Shamiri
et al. [30]) and the dynamic two-phase flow structure
proposed by Cui et al. [27, 28] were combined and im-
plemented to provide a more realistic understanding of
the phenomena encountered in the reactor hydrody-
namics.
The two-phase model presented in this work
assumes that all particles have the same mean diame-
ter of 500×10−6 m [1, 2, 4, 13, 26]. Polypropylene parti-
cles of such size are Geldart B, thus, the constants of
this type of particles were chosen and shown in Table
2. It is worth noting that the same approach was
adopted in similar modeling attempts [13, 31] and pro-
vided good prediction of the reactor performance.
The correlations required for estimating bubble
volume fraction in the bed, voidage of emulsion and
bubble phases, gas velocities in emulsion and bubble
phases and mass and heat transfer coefficients for the
improved two-phase model are summarized in Table 2.
Fluidized bed reactors are able to produce a broad
range of polypropylene.

Table 2 Correlations and equations used in the two-phase model

Parameter Formula Reference
2 1/ 2
minimum fluidization velocity Remf = [(29.5) + 0.357 Ar ] − 29.5 [32]
bubble velocity U b = U 0 − U e + ubr [33]
1/ 2
bubble rise velocity ubr = 0.711( gd b ) [34]

U0 − δU b
emulsion velocity Ue = [34]
1−δ

bubble diameter d b = d b0 [1 + 27(U 0 − U e )]1 / 3 (1 + 6.84 H ) [35]

d b0 = 0.0085 (for Geldart B)
−1
⎛ 1 1 ⎞
mass transfer coefficient K be = ⎜ + ⎟ [33]
⎝ K bc K ce ⎠
1/ 2 1/ 4
Ue Dg g
K bc = 4.5 + 5.85
db d b5 / 4

Dgε eubr
K ce = 6.77
db
−1
⎛ 1 1 ⎞
heat transfer coefficient H be = ⎜ + ⎟ [33]
H
⎝ bc H ce ⎠

( kg ρgCpg )
1/ 2
U e ρg Cpg g1 / 4
H bc = 4.5 + 5.85 5/ 4
db d b

1/ 2
⎛ ε eubr ⎞
H ce = 6.77 ( ρg Cpg kg )
1/ 2
⎜ d3 ⎟
⎝ b ⎠

⎡ ⎛ U 0 − U mf ⎞⎤
bubble phase fraction δ = 0.534 ⎢1 − exp ⎜ − ⎟⎥ [27]
⎣ ⎝ 0.413 ⎠⎦

⎛ U 0 − U mf ⎞
emulsion phase porosity ε e = ε mf + 0.2 − 0.059 exp ⎜ − ⎟ [27]
⎝ 0.429 ⎠

⎛ U 0 − U mf ⎞
bubble phase porosity ε b = 1 − 0.146 exp ⎜ − ⎟ [27]
⎝ 4.439 ⎠

volume of polymer phase in the emulsion phase VPe = AH (1 − ε e ) (1 − δ ) [26]

volume of polymer phase in the bubble phase VPb = AH (1 − ε b ) δ [26]
volume of the emulsion phase Ve = A(1 − δ ) H [26]
volume of the bubble phase Vb = Aδ H [26]
 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013 1019

The UNIPOL Polypropylene Technology is a the superficial gas velocity increases in a fluidized bed
simple and delicate processing system, comprising of due to more solid particles entering bubbles and more
either one or two gas-phase fluidized-bed reactors. To gas entering the emulsion phase [13, 18, 27, 28, 31].
produce homopolymers and random copolymers, a (3) The bubbles are assumed to be spherical with
single reactor is used [36]. In this work a single reactor uniform size and rise up through the bed in plug flow
is used to produce propylene homopolymers. Charac- at constant velocity.
terization of polymer properties was modeled using the (4) Mass and heat transfer resistances between
population balance and the method of moments [30, 37]. gas and solids in the emulsion and bubble phases are
Assuming that the only significant consumption negligible (i.e., low to moderate catalyst activity) [40].
of monomer is by the propagation reaction and hy- (5) Radial concentration and temperature gradi-
drogen by transfer to hydrogen, the following expres- ents in the reactor are negligible due to the agitation
sions for the consumption rate of component (mono- produced by the up-flowing gas.
mer and hydrogen) can be obtained: (6) Elutriation of solids at the top of the bed is
For monomer: negligible.
Ns (7) Constant particle size exists throughout the
Ri = ∑ [ M i ]Y (0, j )kp ( j ) , i =1 (1) bed [1, 2, 4, 13, 26].
j =1 (8) The direction of mass transfer was assumed to
For hydrogen: be from bubble to emulsion phase.
Based on these assumptions, the following dynamic
Ns material balances were derived for all the components
Ri = ∑ [ M i ]Y (0, j )kfh ( j ) , i=2 (2) in the bed.
j =1 For bubbles:
The total polymer production rate for each phase [ M i ]b,in U b Ab − [ M i ]b U b Ab − Rvε b [ M i ]b −
can be then calculated from
Ab
K be ([ M i ]b − [ M i ]e )Vb − (1 − ε b )
VPFR ∫
2 Ri ,b dz =
Rp = ∑ M w,i Ri (3)
i =1 d
in which Ri is the instantaneous rate of reaction for
(Vbε b [M i ]b ) (4)
dt
monomer and hydrogen. The reaction rate constants
were taken from literature and are listed in Table 3. For emulsion:
The assumptions made in developing the equa- [ M i ]e,in U e Ae − [ M i ]e U e Ae − Rvε e [ M i ]e +
tions of the improved two phase model are summa-
⎛ δ ⎞
rized below: K be ([ M i ]b − [ M i ]e )Ve ⎜ ⎟ − (1 − ε e ) Ri ,e =
(1)The polymerization reactions occur in both ⎝1−δ ⎠
bubble and emulsion phases. d
(2) The emulsion phase is considered to be per- (Veε e [M i ]e ) (5)
fectly mixed, and it may contain more gas at higher dt
gas velocities than at the minimum fluidization condi- The energy balances can be expressed as
tion. A better mixing between two phases occurs when For bubbles:

Table 3 Reactions rate constants

Reaction rate constant
Formation Initiation Propagation Activation energy
−1 −1 −1 −1 −1 −1 −1 −1 −1
kf(j)/s ki(j)/L·mol ·s kh(j)/L·mol ·s Khr/L·mol ·s kp(j)/L·mol ·s E/J·mol−1
site type 1 1 22.88 0.1 20 208.6 30124.8
site type 2 1 54.93 0.1 20 22.8849 30124.8
Ref. [38] [39] [38] [38] [39] [39]
Reaction rate constant
Transfer Deactivation
−1 −1 −1 −1 −1 −1 −1 −1
kfm(j)/L·mol ·s kfh(j)/L·mol ·s kfr(j)/L·mol ·s kfs(j)/L·mol ·s kds(j)/s−1
site type 1 0.0462 7.54 0.024 0.0001 0.00034
site type 2 0.2535 7.54 0.12 0.0001 0.00034
Ref. [39] [39] [38] [38] [39]
1020 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013

m simulation of the heat removal system [2] given as

U b Ab (Tb,in − Tref ) ∑ [ M i ]b,in C pi −
dq qss − q
i =1 = (12)
m dt τ
U b Ab (Tb − Tref ) ∑ [ M i ]b C pi − where q is the dynamic heat removal rate, and qss is
i =1 the steady state heat removal rate given as
⎛ m ⎞ qss = Fg C pg (Te − Tin )
Rv (Tb − Tref ) ⎜ ∑ ε b C pi [ M i ]b + (1 − ε b ) ρ polC p ,pol ⎟ + (13)
⎝ i =1 ⎠ where Fg is the gas flow rate, Cpg is the gas heat ca-
Ab ΔH R pacity and Te is the temperature of the gas entering the
(1 − ε b ) Rpb dz + H be (Te − Tb )Vb −
VPFR ∫ heat exchanger, which is also the reactor temperature.
m
Tin is the outlet temperature of the gas from heat ex-
d changer, which is also the temperature of the gas en-
Vbε b (Tb − Tref ) ∑ C pi ([M i ]b ) =
i =1 dt tering the reactor, given as
⎛ ⎛ m ⎞⎞ d Twi [1 − exp(γ )] − T (1 − η )
⎜⎜ Vb ⎜ ε b ∑ C pi [ M i ]b + (1 − ε b ) ρ pol C p ,pol ⎟ ⎟⎟ (Tb − Tref ) Tin = (14)
η − exp(γ )
⎝ ⎝ i =1 ⎠ ⎠ dt
(6) with
For emulsion: ⎡ 1 1 ⎤
γ = AexU ex ⎢ + ⎥ (15)
m ⎣ Fg C pg Fcw C pw ⎦
U e Ae (Te,in − Tref ) ∑ [ M i ]e,in C pi −
i =1
and
m Fg C pg
U e Ae (Te − Tref ) ∑ [ M i ]e C pi − η= (16)
i =1
Fcw C pw
⎛ m ⎞ Twi is the temperature of cooling water entering the
Rv (Te − Tref ) ⎜ ∑ ε e C pi [ M i ]e + (1 − ε e ) ρ polC p ,pol ⎟ − heat exchanger, Aex is the contact area and Uex is a
⎝ i =1 ⎠ heat transfer coefficient. Fcw and Cpw are the flow rate
δ ⎞
(1 − ε e ) Rpe ΔH R − H beVe ⎛⎜
and heat capacity of the cooling water, respectively.
⎟ (Te − Tb ) −
⎝1− δ ⎠
m
d 3 MULTIPLE-INPUT, MULTIPLE OUTPUT
Veε e (Te − Tref ) ∑ C pi ([M i ]e ) = (MIMO) MODEL PREDICTIVE CONTROL
i =1 dt STRATEGY
⎛ ⎛ m ⎞⎞ d
⎜⎜ Ve ⎜ ε e ∑ C pi [ M i ]e + (1 − ε e ) ρ pol C p ,pol ⎟ ⎟⎟ (Te − Tref ) MPC is an optimization-based control strategy
⎝ ⎝ i =1 ⎠ ⎠ dt which is well suited for constrained, multivariable
(7) processes. The model predictive controller predicts the
The initial conditions for solution of the model future behavior of the actual system over a time inter-
equations are as follows: val defined by the prediction horizon. The simplified
diagram of the MPC algorithm shown in Fig. 2 indi-
[ M i ]b,t =0 = [ M i ]in (8) cates that a process model is used in MPC in order to
predict the controlled variable and in this system the
Tb (t = 0) = Tin (9) process model is used in parallel to the plant. The pre-
dicted controlled variable is fed back to the controller
[ M i ]e,t =0 = [ M i ]in (10) where it is used in an on-line optimization procedure,
which minimizes an appropriate cost function to de-
Te (t = 0) = Tin (11) termine the optimal input to the plant acting as the
manipulated variable. The optimization problem is
2.2 Heat exchanger model solved subject to constraints on input and output vari-
ables and also constraints imposed by the nonlinear
model equations. The controller output is implemented
As shown in Fig. 1, the external gas cooler is a in real time and then at the next sampling time. The
countercurrent single-pass shell and tube heat exchanger difference between the plant measurement yp and the
with the recycle gas on the tube side and cooling water process model output ym is also fed to the controller to
on the shell side. A linear first-order dynamic model eliminate steady state offset and compensate modeling
obtained by imposing first order dynamics on the heat uncertainties. The cost function usually is specified as
removal rate with a corresponding time constant, τ, to a sum of quadratic future errors between the reference
yield a linear dynamic model was considered for trajectory and predicted plant output, and the predicted
 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013 1021

Figure 2 Model predictive control system

Table 4 Operating conditions and physical parameters considered in this work for
modeling fluidized bed polypropylene reactors
Operating conditions Physical parameters
Propylene Hydrogen Catalyst
H Dt V Tref Tin P
concentration concentration feed rate μ/Pa·s ρg/kg·m−3 ρs/kg·m−3 dp/m εmf
/m /m /m3 /K /K /MPa /mol·L−1 /mol·L−1 /g·s−1
7.08 3 50 353.15 328.15 2.5 0.9 0.015 0.3 1.14×10−4 23.45 910 500×10−6 0.45

control effort along the prediction horizon.

Due to its ability and simplicity the Model Pre-
dictive Control (MPC) algorithm is implemented to
control the gas phase propylene polymerization process
in this fluidized bed reactor. The MIMO based MPC
controller used in this work takes into account both
the output and manipulated variables and minimizes
the following cost functions V(k) as given by [41, 42]
P ny
{ }
2
V (k ) = ∑∑ w yj ⎡⎣ yi (k + i ) − rj (k + i ) ⎤⎦
i =1 j =1
M nmv
∑∑ {wΔj u Δu j (k + i − 1)}
2
i =1 j =1
where k is the current sampling interval, k + i is a
future sampling interval (within the prediction horizon),
P is the prediction horizon, ny is the number of plant
outputs, w yj is the weight for output j, [ y j (k + i ) −
rj (k + i )] is the predicted deviation at future instant
k + i , M is the control horizon, nmv is the number of
manipulated variables (inputs), Δu j (k + i − 1) is the
predicted adjustment (i.e., move) in manipulated
variable j at future (or current) sampling interval
(k + i − 1) , and wΔj u is the weight for input j.
The cost function is also subjected to inequality
constraints of the manipulated and output variables
given below:
Manipulated variable constraint is given as:
umax (k ) ≥ u (k + i − 1) ≥ umin (k )
Manipulated variable rate constraint is given as
Δumax (k ) ≥ u (k + i − 1) ≥ Δumin (k )
Output variable constraint is given as:
ymax (k ) ≥ y (k + i − 1) ≥ ymin (k ) (20)
Depending on the problem formulation, parame-
ters such as the control horizon, prediction horizon
and weighting matrices in the optimization formula-
tion has to be finalized to obtain the best performance
for the predicted output.
In this study, a MIMO system is controlled by the
centralized MPC techniques. This system takes the
+ reactor temperature (Te) and production rate (Rp) as
controlled variables, with the catalyst feed rate (Fcat)
and cooling water flow rate (Fcw) as manipulated
(17) variables , and the hydrogen concentration (CH) , pro-
pylene concentration (CM) and superficial gas velocity
(U0) as measured disturbances. The improved two
phase model is written in MATLAB and implemented
in S-functions in order to be accessed by Simulink.
4 RESULTS AND DISCUSSION
4.1 Open loop analysis of the propylene polym-
erization fluidized bed reactor
To demonstrate the non-linearity of the reactor,
the process was simulated at the operating conditions
given in Table 4 to explore the effect of step change in
the superficial gas velocity, catalyst feed rate, cooling
water flow rate and hydrogen and propylene concen-
trations on the emulsion phase temperature and poly-
propylene production rate. The results of the open-loop
(18) simulations are shown in Figs. 3 to 7.
As shown in Fig. 3 (a) and 3 (b), the superficial
gas velocity was changed from the nominal value (0.4
m·s−1) using increments of 0.05 m·s−1 in both positive
(19)
and negative directions. The superficial gas velocity has
a significant effect on the emulsion phase temperature
1022 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013
(a)
Figure 3 Effect of step change in U0 on (a) the emulsion phase temperature and (b) production rate (Fcat = 0. 3 g·s−1, CM =
0.9 mol·L−1 and CH = 0.015 mol·L−1)
U0/m·s−1: a—0.4; b—0.25; c—0.3; d—0.35; e—0.45; f—0.5; g—0.55
(a)
Figure 4 Effect of step change in the catalyst feed rate on (a) the emulsion phase temperature and (b) production rate
(U0 = 0.45 m·s−1, CM = 0.9 mol·L−1 and CH = 0.015 mol·L−1)
Fcat/g·s−1: a—0.3; b—0.6; c—0.5; d—0.4; e—0.2; f—0.1
and production rate even for small changes in the su-
perficial gas velocity which indicates that it is an im-
portant parameter for the heat removal and conse-
quently the control of reactor temperature and produc-
tion rate. Although one can manipulate the fluidizing
gas velocity to control the reactor temperature and
production rate but changes in fluidization character-
istics (e.g. solids entrainment) may occur when the
gas velocity is varied [1] which is also difficult to con-
trol in practice and thus the fluidizing gas velocity is
not used as the manipulated variable.
This test clearly shows that the negative steps in
superficial gas velocity have more significant effect
than the corresponding positive steps for both output
variables (emulsion phase temperature and production
rate) and produce non-symmetrical responses. The
variation of the emulsion phase temperature and poly-
propylene production rate as the superficial gas veloc-
ity change deviates from the linear behavior. For such
nonlinear relationships, the use of conventional con-
trollers tends to produce poor control of the process
variables, thus justifying the use of a more efficient
control scheme to properly regulate the effect of super-
ficial gas velocity on the process variables.
The effect of step changes in the catalyst feed
rate on the emulsion phase temperature and production
(b)
(b)
rate is depicted in Fig. 4 (a) and 4 (b). Once the emul-
sion phase temperature and polypropylene production
rate reached steady state conditions at catalyst feed
rate of 0.3 g·s−1, the catalyst feed rate was changed to
show the effect of manipulating this variable on the
process dynamics. Small step changes in the catalyst
feed rate result in significant changes in the reactor
temperature and polymer production rates. The slightly
symmetrical nature of these profiles due to the sys-
tematic positive and negative variations in the catalyst
flow rate indicates the slightly nonlinear relationships.
In this case, using a conventional controller can be
acceptable provided that the effect of disturbances,
measurement noise, modeling uncertainty and process
interaction are not pronounced.
In the industry, the properties of polypropylene
are controlled by varying the monomer and hydrogen
feed rates. Increasing the hydrogen to propylene ratio
in the reactor leads to increased chain transfer and to
lower molecular weight. Changes in monomer and
hydrogen feed rates also act as disturbances to the
reactor temperature and polymer production rate. To
explore these effects, positive and negative steps were
introduced in the hydrogen and propylene feed con-
centrations by 0.005 mol·L−1 and 0.1 mol·L−1 respec-
tively. The effect of a step change in the hydrogen
 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013 1023

(a) (b)
Figure 5 Effect of step change in the hydrogen feed concentration on (a) emulsion phase temperature and (b) production
rate (U0 = 0.45 m·s−1, Fcat = 0. 3g·s−1 and CM = 0.9 mol·L−1)
CH/mol·L−1: a—0.015; b—0; c—0.005; d—0.01; e—0.02; f—0.025; g—0.3

(a) (b)
Figure 6 Effect of step change in the propylene feed concentration on (a) the emulsion phase temperature and (b) produc-
tion rate (Fcat = 0. 3 g·s−1, U0 = 0.45 m·s−1 and CH = 0.015 mol·L−1)
CM/mol·L−1: a—0.7; b—1; c—0.9; d—0.8; e—0.6; f—0.5; g—0.4

concentration in the feed on the emulsion phase tem- in terms of the control algorithm used.
perature and production rate predicted by the model is Figure 7 illustrates the effect of step changes in
shown in Fig. 5 (a) and 5 (b). The initial hydrogen the cooling water flow rate on the emulsion phase
feed concentration was set at 0.015 mol·L−1 and step temperature. By changing the cooling water flow rate
changes was introduced from the steady state condi- from an initial value of 3×105 g·s−1, the emulsion
tions. As can be seen, hydrogen concentration has highly
nonlinear relationship with the reactor temperature
and polymer production rate. Increasing the hydrogen
concentration leads to enhancing the chain transfer
reaction rate and consequently lowers the degree of
polymerization due to the shorter polymer chain length.
The effect of varying the feed propylene concen-
tration on the emulsion phase temperature and produc-
tion rate is shown in Fig. 6 (a) and 6 (b). The propyl-
ene concentration was changed from the nominal
value of 0.7 mol·L−1. By increasing the feed propylene
concentration, the emulsion phase temperature and
production rate increases. Increasing the propylene
concentration leads to enhancing the reaction rate and
consequently the degree of polymerization. This ob- Figure 7 Effect of step change in the cooling water flow
servation, in addition to the ones discussed previously, rate on the emulsion phase temperature (Fcat = 0. 3 g·s−1,
U0 = 0.45 m·s−1, CM = 0.9 mol·L−1 and CH = 0.015 mol·L−1)
show nonlinear behavior as inferred from the produced
dynamic profiles. Such observations indicate that the Fcw/g·s−1: a—3×105; b—1.5×105; c—2×105; d—2.5×105; e—
process model under investigation needs special attention 3.5×105; f—4×105; g—4.5×105
1024 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013
Figure 8 A simplified schematic of the process sub-models and control system of the gas phase propylene polymerization
fluidized bed reactor
phase temperature changes significantly and shows
strong dependency. This indicates that it has an im-
portant role on the heat removal and on the control of
the fluidized bed polymerization rector temperature.
4.2 Closed loop performance of the model predic-
tive controller scheme
A simplified schematic of the process sub-models
and control system of the gas phase propylene polym-
erization fluidized bed reactor is shown in Fig. 8.
4.2.1 MPC controller design
The results presented in the previous section
show the nonlinear behavior of the system as inferred
from the produced dynamic profiles. Such observa-
tions imply that the process model under investigation
needs special attention in terms of the control algo-
rithm to be used for this process. Despite the fact that
the superficial gas velocity, catalyst feed rate and hy-
drogen and propylene concentrations have significant
effect on the output variables, based on actual process
experience, not all of them are suitable to be selected
as manipulated variables. In the industrial fluid-
ized-bed olefin polymerization reactor, the tempera-
ture is usually controlled by manipulating the cooling
water flow rate of an upstream heat exchanger which
is used to remove the heat of the exothermic polym-
erization reaction from the recycle gas stream [2], and
changes to the catalyst feed rate can be used to control
the polymer production rate [11]. Based on this approach,
Fcat and Fcw were selected as manipulated variables
and Rp and Te were used as control variables to design
the centralized MPC in this work (see Fig. 1). In this
case, superficial gas velocity (U0), propylene concen-
tration (CM), and hydrogen concentration (CH) were
classified as the disturbance variables.
To ensure good performance of the MPC con-
troller, the tuning parameters must be appropriately
tuned. The tuned parameters suggested by Shridhar
and Cooper [43] were used as the starting values but
the exact values used in this work were the result of
further fine tuning based on actual control perform-
ance. In addition to the selection of controller tuning
parameters, appropriate values were chosen for the
input/output variables constraints and imposed on the
system based on practical experience. The values of
the upper and lower limits of the constraints for the
Fcat − Rp profile are: 0≤Fcat≤100%, −20%≤ΔFcat≤
20% and for the Fcw − Te profile are: 0≤Fcw≤100%,
−20%≤ΔFcw≤20%. The control system has a sam-
pling time of 15 s, a prediction horizon of 20, a con-
trol horizon of 2, an output variables weight of 0.005
for Rp and 0.0005 for Te. The manipulated variables
weights selected were 0.1 for Fcat and 0.1 for Fcw.
4.2.2 Setpoint tracking
It is interesting to see how the nonlinear poly-
propylene fluidized bed reactor behaves under advanced
and conventional control algorithms. Hence the closed
loop performance of the MPC scheme in tracking a
series of setpoint changes for emulsion phase tempera-
ture and production rate in the polymerization reactor
was evaluated. For this purpose, a series of setpoint
changes in opposite directions were introduced for the
controlled variables. The magnitude of the setpoints
introduced for these variables were typical of the re-
spective nominal operating ranges. The commonly
used conventional controllers in industrial applications
are proportional integral (PI) controllers due to their
relative simple design, simple control structure and
moderate cost [23]. Therefore, for comparison purposes,
a conventional PI controller, tuned using the standard
Ziegler-Nichols (Z-N) [44] open loop tuning method,
was included in this simulation work. The PI control-
ler tuning parameters were calculated based on an
analysis of the open loop process reaction curve for a
particular operational region of the process, where the
open loop response was approximated by a first order
plus dead time (FOPDT) dynamic model [K = −0.3
(process gain), τ = 890 s (process time constant) and
 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013
(a)
MPC; setpoint
Figure 9 Comparison of the performance between the MPC and the PI controller (Kc = 7, τI = 46.6666, τD = 0) in tracking
series of setpoint changes in the Rp loop
(a)
MPC; setpoint
Figure 10 Comparison of the performance between the MPC and the PI controller (Kc = −34, τI = 271.5654, τD = 0) in track-
ing series of setpoint changes in the Te loop
α = 80 (process dead time) for the Te profile, and
K = 42.5 (process gain), τ = 988 s (process time con-
stant) and α = 5 (process dead time) for the Rp profile].
The parameters tuned using Ziegler and Nichols
[44] method were used as starting values but the exact
values used in this work were the result of further fine
tuning.
Figures 9 and 10 show the performance of the
MPC as compared to the PI controller in tracking the
series of setpoint changes for Rp and Te profiles, re-
spectively. The MPC controller is able to track the
changes in the setpoints for both profiles. The quality
of the setpoint tracking as demonstrated by the MPC
in terms of its ability to attain minimal overshoot and
minimize the effect of process variables interaction is
acceptable. In contrast, the PI controller produced
noticeable overshoots for both loops, in addition to the
obvious effect of process variables interaction for the
Te loop. This illustrates the failure of the decentralized
PI controller to track the setpoints for both loops due
to loop interactions as well as the process nonlinearity.
The controller moves for MPC and PI controllers
in tracking these series of setpoint changes for the Rp
and the Te profiles are shown in Figs. 11 and 12,
1025
(b)
PI; setpoint
(b)
PI; setpoint
respectively. It can be seen that the PI controller
moves are vigorous for the Rp profile. Although the
controller moves observed for the Te profile (Fig. 12)
are less vigorous and physically realizable, such con-
troller moves typically are not desired during practical
implementations due to possible ‘wear and tear’ which
can severely shorten the life span of the actuator. In
general, the MPC is able to not only produce control-
ler moves which are well within the specified input
constraints, but also the controller moves produced are
non-aggressive and smooth for practical implementa-
tions. The high quality control performance of the
MPC is attributed to its ability to handle constraints in
the inputs, of which the conventional PI controller was
unable to achieve due to the high degree of interaction
between these process variables. To summarize, Table 5
shows the integral absolute error (IAE) for the two
controllers in tracking the series of setpoint changes
for both controlled variables and the performance of
the MPC is also superior.
4.2.3 Disturbance rejection
The results thus far have demonstrated the good
performance of the MPC in handling the servo process
1026 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013

(a) (b)
Figure 11 Comparison of the corresponding controller moves between the MPC and the PI controller for the Rp profile
MPC; PI

(a) (b)
Figure 12 Comparison of the corresponding controller moves between the MPC and the PI controller for the Te profile
MPC; PI

Table 5 Integral absolute error (IAE) for the MPC and mol·L−1) at the time of 13000 s. Figs. 13 to 15 show
the PI controller in tracking series of setpoint changes for the performance of the MPC in rejecting the effect of
the production rate (Rp) and the emulsion phase such changes on the Rp and Te profiles. Generally, the
temperature (Te) profiles MPC controller was able to reject these disturbances
Controller IAE for Rp profile IAE for Te profile in an efficient manner. As a general observation, the
4 superficial gas velocity had the largest effect on both
MPC 4.31×10 2.22×103
the Rp and Te profiles. On the contrary, hydrogen and
5
PI controller 1.84×10 4.3×103 propylene concentrations have negligible effect on
both of the profiles.

control problem for the polymerization reactor as 5 CONCLUSIONS

compared to the conventional controller. However, for
a particular controller to be practically useful in the
process industry, the controller must additionally be
able to handle regulatory problems effectively. In this
case, three variables i.e., hydrogen concentration (CH),
superficial gas velocity (U0) and propylene concentra-
tion (CM) were identified as the measured disturbance
variables. The disturbance variables were introduced
one at a time to observe their individual effect on the
Rp and Te profiles. Each disturbance variable was in-
creased by 15% of its nominal value (superficial gas
velocity from 0.4 m·s−1 to 0.46 m·s−1, hydrogen con-
centration from 0.01 mol·L−1 to 0.0115 mol·L−1 and
propylene concentration from 0.8 mol·L−1 to 0.92
A two-phase dynamic model describing the gas
phase propylene polymerization in a fluidized bed
reactor was used to investigate the dynamic behavior
and control on the polypropylene production rate and
reactor temperature. The hydrodynamics of the fluid-
ized bed reactor of polypropylene production was based
on the dynamic two-phase concept of fluidization.
Results of the open loop analysis revealed that the
catalyst feed rate and gas superficial velocity have
significant effect on the transient behavior of the
polypropylene fluidized bed reactor and the process
shows nonlinear behavior, especially by the variation
of the superficial gas velocity.
 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013 1027

(a) (b)
Figure 13 Performance of the MPC controller in rejecting the effect of superficial gas velocity (U0) on the Rp and Te profiles
(a 15% increase in the superficial gas velocity was introduced at time = 13000)

(a) (b)
Figure 14 Performance of the MPC controller in rejecting the effect of hydrogen concentration (CH) on the Rp and Te pro-
files (a 15% increase in hydrogen concentration was introduced at time = 13000 s)

(a) (b)
Figure 15 Performance of the MPC controller in rejecting the effect of propylene concentration (CM) on the Rp and Te pro-
files (a 15% increase in the propylene concentration was introduced at time = 13000 s)

Two control algorithms namely, the conventional
PI and MPC were tested for the stabilization of the
process during setpoint and disturbances changes. The
closed-loop simulations for setpoint changes revealed
that the MPC is able to track the changes in the setpoint
effectively with minimal overshoot while the PI con-
troller produces oscillatory response for the reactor
temperature and production profiles. The PI controller
produces overshoots for both Rp and Te loops, in addi-
tion to the obvious effect of loop interaction for both
loops while the MPC moves were shown to be
non-aggressive and sufficiently smooth for practical
implementations. By introducing changes in the dis-
turbance variables, where each disturbance variable
was increased by 15% of its nominal value, the closed
loop dynamic simulations indicated that the speed of
disturbance rejection for the MPC controller was ac-
ceptable for both the Rp and Te profiles. In conclusion,
the results demonstrated excellent performance of the
MPC in handling servo and regulatory process control
1028 Chin. J. Chem. Eng., Vol. 21, No. 9, September 2013

problems for this polymerization reactor. Remf Reynolds number at minimum fluidization velocity, Remf =
U mf ρg d p / μg
Rp production rate, kg·s−1
NOMENCLATURE
Rpb bubble phase production rate, kg·s−1
Rpe emulsion phase production rate, kg·s−1
A cross sectional area of the reactor, m2 Rv volumetric polymer phase outflow rate from the reactor, m3·s−1
Aex heat transfer area of the heat exchanger, m2 t time, s
Ar Archimedes number, d p3 ρg ( ρs − ρg ) g / μ 2 T temperature of the gas entering the exchanger, K
CH hydrogen concentration, kmol·m−3 Tin temperature of the inlet gaseous stream, K
CM propylene concentration, kmol·m−3 Twi temperature of the cooling water entering the heat exchanger, K
Cpi specific heat capacity of component i, J·kg−1·K−1 U0 superficial gas velocity, m·s−1
Cpg specific heat capacity of gaseous stream, J·kg−1·K−1 Ub bubble velocity, m·s−1
Cp,pol specific heat capacity of solid product, J·kg−1·K−1 Ue emulsion gas velocity, m·s−1
Cpw specific heat capacity of the cooling water, J·kg−1·K−1 Uex overall heat transfer coefficient of the heat exchanger, J·K−1·s−1·m−2
Dg gas diffusion coefficient, m2·s−1 Umf minimum fluidization velocity, m·s−1
Dt reactor diameter, m V reactor volume, m3
db bubble diameter, m Vb volume of the bubble phase, m3
dp particle diameter, m Ve volume of the emulsion phase, m3
Fg gas flow rate, kg·s−1 Vp volume of polymer phase in the reactor, m3
Fcat catalyst feed rate, kg·s−1 Vpb volume of polymer phase in the bubble phase, m3
Fcw cooling water flow rate, kg·s−1 Vpe volume of polymer phase in the emulsion phase, m3
H height of the reactor, m VPFR volume of PFR, m3
Hbe bubble to emulsion heat transfer coefficient, W·m−3·K−1 Y(n,j) nth moment of chain length distribution for living polymer pro-
Hbc bubble to cloud heat transfer coefficient, W·m3·K−1 duced at a site of type j
Hce cloud to emulsion heat transfer coefficient, W·m3·K−1 γ dimensionless variable defined in Eq. (14)
ΔHR heat of reaction, J·kg−1 δ volume fraction of bubbles in the bed
j active site type εb void fraction of bubble for Geldart B particles
kds(j) spontaneous deactivation rate constant for a site of type j εe void fraction of emulsion for Geldart B particles
kf(j) formation rate constant for a site of type j εmf void fraction of the bed at minimum fluidization
kfh(j) transfer rate constant for a site of type j with terminal monomer η dimensionless variable defined in Eq. (14)
M reacting with hydrogen μ gas viscosity, Pa·s
kfm(j) transfer rate constant for a site of type j with terminal monomer ρ density, kg·m−3
M reacting with monomer M ρg gas density, kg·m−3
kfr(j) transfer rate constant for a site of type j with terminal monomer ρpol polymer density, kg·m−3
M reacting with AlEt3 Subscripts
kfs(j) spontaneous transfer rate constant for a site of type j with ter- 1 propylene
minal monomer M 2 hydrogen
kh(j) rate constant for reinitiating of a site of type j by monomer M b bubble phase
khr(j) rate constant for reinitiating of a site of type j by cocatalyst e emulsion phase
ki(j) rate constant for initiation of a site of type j by monomer M g gas mixture property
kp(j) propagation rate constant for a site of type j with terminal i component type number
monomer M reacting with monomer M in inlet
kg gas thermal conductivity, W·m−1·K−1 j active site type number
kp(j) propagation rate constant for a site of type j with terminal mf minimum fluidization
monomer M reacting with monomer M pol polymer
Kbc bubble to cloud mass transfer coefficient, s−1 PP polypropylene
Kbe bubble to emulsion mass transfer coefficient, s−1 ref reference condition
Kce cloud to emulsion mass transfer coefficient, s−1
M monomer (propylene)
[Mi] concentration of component i in the reactor, kmol·m−3
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