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Article in IRANIAN JOURNAL OF CHEMISTRY & CHEMICAL ENGINEERING-INTERNATIONAL ENGLISH EDITION · September 2008
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Mirzaei, Ahmad
Iran Polymer and Petrochemical Institute, Faculty of Polymerization Engineering, Tehran, I.R. IRAN
ABSTRACT: In present paper, dynamic behavior and control of a fluidized bed reactor for
polyethylene production has been considered. A double active sites model for Ziegler-Natta
catalysts is used for simulation of polymerization reaction. Hydrodynamic behavior of the bed is
modeled using a two phase model including bubble and emulsion phases in which bubble phase has
plug flow pattern with differentially variable velocity and size through the bed and emulsion phase
has the CSTR flow pattern. The reactor model is validated using industrial data. Conventional PID
controllers with anti-windup are considered for control purposes. It has been shown that the control
system has satisfactory performances either for setpoint tracking or load rejection. To improve the
performance of the control system for load rejection the cascade control strategy has been
considered.
KEY WORDS: Fluidized bed reactor, Polyethylene, PID control, Dynamic simulation, Two phase
model.
INTRODUCTION
Nowadays polyethylene is considered to be the world Choi and Ray [1] proposed a two phase model
largest produced polymer in petrochemical plants. including bubble and emulsion phases with constant
Because of the advantages of gas-phase processes such as bubble size. McAluey et al. [2] proposed a single phase
moderate reaction operating conditions, absence of model by modifying the Ray’s model with additional
solvent and well mixing of the components, production of assumptions. In a comparison between two models, they
different grades of polyolefin in the fluidized bed reactor have shown that the single phase assumption doesn’t
(FBR) has been recognized as one of the most efficient make considerable difference in the results obtained from
processes for olefin polymerization in petrochemical the models. Hatzantonis et al. [3] in a research work
plants. Recently modeling and simulation of polyethylene developed the two phase model by considering the bubble
production in a fluidized bed reactor has received growth effect on hydrodynamic behavior of the reactor
considerable attention. and have shown that the developed model has a better
* To whom correspondence should be addressed.
+ E-mail: Shahrokhi@sharif.edu
1021-9986/08/3/87 15/$/3.50
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Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
Purge
PC
LC TC
CW Supply
Product
CW Return
CC
Catalyst CC
CC
FC FC FC
Nitrogen
Ethylene Butene Hydrogen
agreement with industrial data than single and two phase The paper has been organized as follows. First reactor
model with constant bubble size. In another work, modeling is discussed. Next reactor dynamic and its
Kiashemshaki et al. [4] developed the two phase model control have been considered. Finally the simulation
by considering the polymerization reaction not only in the results are presented and discussed.
emulsion phase but also in the bubble phase. They have
indicated that about 20 % of the polymerization reaction
occurs in bubble phase. REACTOR MODELING
In this work a two phase model including bubble and A schematic representation of a gas-phase ethylene
emulsion phases which considers the bubble growth copolymerization FBR is depicted in Fig. 1. As can be
effect is used for modeling the hydrodynamic behavior of seen from Fig. 1, a gas stream comprises four components
the reactor. The double active sites Ziegler-Natta catalyst (ethylene, 1-butene, hydrogen and nitrogen) is fed
model proposed by McAuley et al. [5] has been used for continuously to the reactor through a distributor. Catalyst
simulating the kinetic of ethylene copolymerization. particles are introduced to the reactor above the
To control the reactor at the operating conditions, six distributor. Polymer particles produced in the reactor are
feedback control loops with PID controllers, including withdrawn from middle of the reactor. Because of the
anti-windup, have been used. The advantage of the low conversion, the unreacted gas leaving the reactor is
present work over the previous ones is considering dynamic recycled to the reactor. Since the polymerization reaction
for the bubble phase in dynamic simulation of the reactor. is exothermic, an external heat exchanger is employed for
In the previous works a simple CSTR model has been cooling the recycle gas stream.
used for dynamic simulation and control, while we have The following assumptions are made for modeling the
used a comprehensive two phase model for control reaction loop:
purposes. To improve the performance of the control 1- Emulsion phase is perfectly mixed and stays in the
system for load rejection, cascade control strategy has minimum fluidization condition.
been implemented. Simulation results indicate that this 2- Polymerization reaction occurs only in the
strategy promotes the control performance considerably. emulsion phase.
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Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
3- Bubble phase has plug flow pattern and its Table 1: Ethylene 1-butene copolymerization kinetics
properties change differentially through the bed. mechanism over Ziegler-Natta catalyst.
4- No elutriation of solids occurs. Activation by cocatalyst j
S p + C ¾¾® N 0
j kf j
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Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
(
d [M N 2 ]e Ve ) n
= U e -in [M N 2 ]in (1 - din ) eA - (5) å[M i ]in Mw i Cp i U e-in (1 - d in )eA(Tin - Tref ) -
dt i =1
U e - o [M N 2 ] in (1 - do ) eA + n
å ò
0
R M i Mw i DH i Vp + Hm av (Tb - Te )dAdz +
i =1 0
where “Q” denotes the volumetric flow rate of gas and
H n
polymer mixture withdrawn from the reactor and
R M i and R H 2 are consumption rates of monomers and òå
i =1
Km i ([M i ] b - [M i ] e )Mw i Cp i dA(Tb - Tref )dz -
0
hydrogen respectively and are obtained from following Q(1 - e)rpCpp (Te - Tref ) + q catCpp (Tin - Tref ) -
equations [5]: n
s å[M i ]e Mw i Cp i Qe(Te - Tref )
R Mi = å [M i ]Y0jKp Tij i = 1,2,..., m (6) i =1
j=1
Since the temperature variation in the reactor is small,
s
its effect on the heat capacity has been neglected while
R H2 = å [H 2 ]Y0j Kth Tj (7)
the effect of composition has been taken into account.
j=1
Correlations needed to calculate the parameters used in
Yn is the nth moment of the live polymer chains and above equations are given in the Table 2.
is given by [5]: Assuming lump formulation for the external heat
m ¥ exchanger, the heat balance on tube side of the heat
Ynj = åå r n [ N rj,i ] (8) exchanger yields:
i =1 r =1
d (Tg r g Cp g -av )
The third term in equations (3)-(5) shows the total = (11)
dt
amount of mass transfer between bubble and emulsion
rec Cp g -av (Tg -in - Tg ) - U ex A ex (Tg - Tw )
m
phases. The mass balance for solid particles existing in
the bed yields [3]: Vtube
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Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
Re mf - m g
U mf = Minimum fluidization velocity
rg - d p
( 2
Re mf = 28.7 + 0.0494Ar )
0.5
- 28.7 Reynolds number
3
(
d prg rs - rg g )
Ar = Archimedes number
2
mg
æ 0.3z ö
d b = d bm - (d bm - d b 0 ) expç - ÷ Bubble diameter
è D ø
[
d bm = 0.652 A(U 0 - U mf ) ]0.4
Maximum bubble diameter
d b 0 = 0.00376(U 0 - U mf )
2
Initial bubble diameter
0.5
U b = U 0 - U mf + 0.711(gd b ) Bubble rise velocity
U mf
Ue = Emulsion gas velocity
e mf (1 - d )
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Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
In another work, Ali et al. [11] have investigated used to discretize the partial differential equations with
control of the reactor temperature and pressure in respect to reactor length. The resulting ordinary
addition to the gas partial pressures. They have compared differential equations are solved using Runge Kutta
the performances of two different multivariable control method through the MATLAB software. The flowchart
approaches. Recently Chatzidoukas et al. [12] have studied that represents the solution procedure is shown in
the optimal grade transition problem and selection of Fig. 2.
appropriate pairings for polyethylene production in a FBR.
For process safety and operability, the reactor Static simulation
temperature and pressure as well as the bed height should To check the accuracy of the model, a static simulation
be controlled at desired operating points. Regarding the has been performed. Program inputs are: rates of each
product quality, the components concentration (i.e. component makeup, pressure difference across the
ethylene, 1-butene and hydrogen concentrations) must be compressor, catalyst and production rates, purge gas and
controlled at desired values. cooling water flow rates. The corresponding figures used
To control the process variables given above, seven for simulation are given in Table 4. These data have been
manipulated variables are considered. These manipulated selected such that the feed condition entering the reactor
variables are the volumetric flow rates of makeup streams to be the same as an industrial case. The operating
(ethylene, 1-butene and hydrogen), nitrogen volumetric condition of gas entering the bed is given in Table 5.
flow rate, volumetric flow rate of purge stream, the The results of static simulation and the corresponding
cooling water makeup mass flow rate and the polymer industrial data are given in Table 6. As can be seen the
withdrawal mass flow rate. The control pairings are results of the simulation are in a good agreement with
shown in the Fig. 1 and are given in Table 3. industrial data.
For each control loops, conventional PID controllers Static simulation can be used for evaluating the effect
are used. To avoid deterioration of controller performance, of different parameters on the reactor performance. As an
the anti-windup scheme which stops integration upon example, the effect of gas superficial velocity for various
input saturation has been used [13]. Tuning of the catalyst feed rate on emulsion phase temperature and
controller parameters are accomplished based on ethylene concentration are shown in Fig 3. In this figure
maximum 10 % overshoot for each loop while the other the concentration of ethylene is denoted by C2. As can be
loops are open. To handle the loop interactions, the seen, increasing the gas superficial velocity results in a
detuning procedure proposed by Luyben [14] has been better heat removal from the reactor. Therefore the
used. Equation describing the flowrate of the gas stream catalyst feed rate can be increased for more production
control valve is given below: rate without the risk of polymer meld-down. On the other
hand, increasing the gas superficial velocity leads to
F = Kv Pup (Pup - Pdown ) (16) lower conversion of the monomer (Fig. 3). In addition, it
can increase the rate of polymer particles elutriation.
where “F” denotes the volumetric flow rate of gas passing
through the valve, “Pup” and “Pdown” denote the upstream Dynamic simulation
and downstream pressures of the gas and “Kv” denotes Through dynamic simulation, the performances of
the valve coefficient which is a function of valve different control strategies are evaluated for load rejection
opening. and set-point tracking. Table 7 shows the desired values
of the controlled variables of an industrial polyethylene
RESULTS AND DISCUSSION production unit (Tabriz petrochemical, in the north part of
In this section static and dynamic simulations using Iran).
the comprehensive model are considered. System model
contains 5 partial differential, 37 ordinary differential Load rejection
equations and many algebraic equations used for In industrial plants a common disturbance is
calculating the various model parameters. To solve fluctuation of feed stream pressure. Therefore a
this set of equations, backward difference method is disturbance is introduced into the all feed stream pressures.
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Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
Hydrogen concentration Hydrogen makeup feed rate Table 6: Simulation results and the corresponding industrial
data.
Temperature Cooling water makeup feed rate
Industrial data Two phase model
Pressure Nitrogen and bleed rates
T (oC) 76 75.6
Start
Initial conditions
ti+1 = t1 + Dt
No
Solve ODE equations t < tf
Yes
End
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Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
460
0.00059 Uo/Umf=7
Uo/Umf=5 420
[C2] (mol/cm3)
Uo/Umf=3
0.00057
T (k)
380
Uo/Umf=7
0.00055 Uo/Umf=5
340 Uo/Umf=3
0.00053 300
0.02 0.03 0.04 0.05 0.06 0.07 0.08 0.09 0.00 0.02 0.04 0.06 0.08 0.10
qcat (g/s) qcat (g/s)
Fig. 3: Variations of emulsion phase temperature and ethylene concentration versus catalyst feed rate.
0.0001495
0.000319
[C2] (mol/cm3)
[C4] (mol/cm3)
0.0001493
0.000318
0.0001491
0.000317
0.000316 0.0001489
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
0.00007505
0.000075
20.1
[H2] (mol/cm3)
0.00007495
20.06
P (bar)
0.0000749
20.02
0.00007485
0.0000748 19.98
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
349.2 1404
349.18 1403
349.16 1402
T (K)
H (cm)
349.14 1401
349.12 1400
349.1 1399
0 100 200 300 400 500 600 700 800 0 50 100 150 200 250 300 350 400
Fig. 4: Deviations of the controlled variables from their steady state values due to 5 bar increase in the
makeup stream pressures (---- single concentration loops, ── cascade loops).
94
Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
95
Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
96
Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
40
26
Ethylene makeup
30
Butene makeup
22
20
18
14 10
10 0
0 100 200 300 400 500 0 100 200 300 400 500 600 700 800
50 60
40 50
Hydrogen makeup
Nitrogen makeup
40
30
30
20
20
10
10
0 0
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
110 62
100 60
90
58
CW makeup
80
Purge
56
70
54
60
50 52
40 50
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
70
60
Production rate
50
40
30
20
10
0
0 50 100 150 200 250 300 350 400
Time (s)
Fig. 5: Variations of manipulated variables (valve opening percentages) due to 5 bar increase in the
makeup stream pressures (---- single concentration loops, ── cascade loops).
97
Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
0.00032 0.0001496
0.0003195 0.0001495
0.000319 0.0001494
[C2] (mol/cm3)
[C4] (mol/cm3)
0.0003185
0.0001493
0.000318
0.0001492
0.0003175
0.000317 0.0001491
0.0003165 0.000149
0.000316 0.0001489
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
0.0000751 20.14
0.00007505 20.12
20.1
[H2] (mol/cm3)
0.000075
20.08
0.00007495 P (bar) 20.06
0.0000749 20.04
20.02
0.00007485
20
0.0000748 19.98
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
349.2 1403
349.18 1402
349.16 1401
H (cm)
T (K)
349.14 1400
349.12 1399
349.1 1398
0 100 200 300 400 500 600 700 800 0 50 100 150 200 250 300 350 400
Fig. 6: Deviations of the controlled variables from their steady state values due to 5 bar increase in the
makeup stream pressures under fixed purge flow rate(---- single concentration loops, ── cascade loops).
[10] McAuley, K. B., McGregor, J. F., Nonlinear Product Selection of Closed Loop Controllers in a Gas Phase
Quality Control in Industrial Gas-Phase Poly- Olefin Polymerization Fluidized Bed Reactor,
ethylene Reactor, AICHE J., 39, 855 (1993). Chemical Engineering Science, 58, 3543 (2003).
[11] Ali, E., Al-Humaizi K., Ajbar, A., Multivariable [13] Bequette, W., “Process Control, Modeling, Design
Control of Simulated Industrial Gas Phase Reactor, and Simulation”, Prentice Hall, (2003).
Ind. Chem. Eng. Res., 42, 2349 (2003). [14] Luyben, W. L., Simple Method for Tuning SISO
[12] Chatzidoukas, C., Perkins, J. D., Pistikopoulos, E. Controllers in a Multivariable System, Ind, Eng.
N., Kiparissides, C., Optimal Grade Transition and Chem. Proc. Des. Dev., 25, 654 (1986).
98
Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
28 40
26 35
24
30
Butene makeup
Ethylene makeup
22
25
20
20
18
16 15
14 10
12 5
10 0
0 50 100 150 200 250 300 350 400 0 50 100 150 200 250 300 350 400
50 60
45
40 50
Hydrogen makeup
35
Nitrogen makeup
40
30
25 30
20
15 20
10
10
5
0 0
0 50 100 150 200 250 300 350 400 0 50 100 150 200 250 300 350 400
70 62
60 60
50
Production rate
58
CW makeup
40
56
30
54
20
10 52
0 50
0 50 100 150 200 250 300 350 400 0 50 100 150 200 250 300 350 400
Fig. 7: Variations of manipulated variables (valve opening percentages) due to 5 bar increase in the makeup stream pressures
under fixed purge flow rate (---- single concentration loops, ── cascade loops).
99
Iran. J. Chem. Chem. Eng. Vahidi, O., et al. Vol. 27, No.3, 2008
351.5 100
351.0 75
CW makeup
350.5
T (K)
50
350.0
24
349.5
349.0 0
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
Time (s) Time (s)
Fig. 8: Variations of the reactor temperature and cooling water makeup stream (valve opening percentage)
due to 2 °C increase in the reactor temperature setpoint.
3.170E-04 1.492E-04
[C2] (mole/cm3)
[C4] (mole/cm3)
3.165E-04 1.490E-04
3.160E-04 1.488E-04
3.155E-04 1.486E-04
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
7.50E-05 20.1
[H2] (mole/cm3)
7.48E-05 20.05
P (bar)
7.46E-05 20
7.44E-05 19.95
0 100 200 300 400 500 600 700 800 0 100 200 300 400 500 600 700 800
1402
1401
H (cm)
1400
1399
0 100 200 300 400 500 600 700 800
Time (s)
Fig. 9: Variations of other controlled variables due to 2 oC increase in the reactor temperature setpoint.
100
Iran. J. Chem. Chem. Eng. Control of a Fluidized Bed … Vol. 27, No.3, 2008
21
20.6
P (bar)
20.2
19.8
0 100 200 300 400 500 600 700
Time (s)
100 60
80
40
Nitrogen
60
Purge
40 20
20
0 0
0 100 200 300 400 500 600 700 0 100 200 300 400 500 600 700
Time (s) Time (s)
Fig. 10: Variations of the reactor pressure and the nitrogen and purge volumetric flow rates
(valve opening percentages) due to 1 bar increase in the reactor pressure setpoint.
0.000318 0.00015
[C4] (mole/cm3)
[C2] (mole/cm3)
0.000317 0.0001495
0.000316 0.000149
0.000315 0.0001485
0.000314 0.000148
0 100 200 300 400 500 600 700 0 100 200 300 400 500 600 700
0.000076 349.2
349.18
[H2] (mole/cm3)
0.0000755
349.16
T (k)
0.000075
349.14
0.0000745
349.12
0.000074 349.1
0 100 200 300 400 500 600 700 0 100 200 300 400 500 600 700
1405
1403
1401
H (cm)
1399
1397
1396
0 100 200 300 400 500 600 700
Time (s)
Fig. 11: Variations of other controlled variables due to 1 bar increase in the reactor pressure setpoint.
101