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Industrial polymer plants are composed of reactors and downstream processes such as separators,
dryers, and pelletizers. The polymer properties are delayed and changed in the downstream
processes because of process dynamics. The polymer grade is determined by the properties of
both the polymer slurry from the reactors and the polymer pellet from the pelletizer. Therefore,
the grade transition strategy must be optimized in a plantwide viewpoint, and the models of
downstream processes must be included in the optimization problem. In this study, a plantwide
optimal grade transition strategy is proposed using the models of the reactors and the
downstream processes, and the results are compared in a plantwide viewpoint. The plantwide
grade transition time using the entire set of process models is shorter than that using the reactor
model only.
in a plantwide viewpoint. The HDPE process models of individual grade transition times of y1, y2, y3, and y4.
the reactors, the separator, the dryer, and the pelletizer The plantwide grade transition time by the second policy
are used for the dynamic optimization model to include is 2ty2. The plantwide grade transition time by the
the properties of the polymer slurry and the polymer second policy is shorter than that by the first policy,
pellet in the objective function, and the results are although three individual grade transition times by the
compared with those by the reactor model only in a first policy are shorter than those by the second policy.
plantwide viewpoint. The empirical model combined Therefore, it is important in industrial grade transition
with the first principle model is used because MI cannot operations to make all properties satisfy grade specifica-
be calculated by the first principle model and the tions rather than only one of properties being used for
moment equations. Regression models are used to grade specifications.
estimate the MI value from the concentration of the
reactants in reactors.5,6 A modified hierarchical method 3. Case Study
is applied to solve the dynamic optimization problem
for the grade transition.7 3.1. Process Description. Figure 2 shows the sim-
plified schematic diagram of the slurry-phase HDPE
2. Plantwide Grade Transition process for this study. It is composed of two continuously
stirred tank reactors in series, the centrifugal separator,
Continuous polymer processes are composed of reac-
the dryer, and the pelletizer. Polymerization reaction
tors and downstream processes such as separators,
occurs in the slurry phase. Ethylene monomer is the
dryers, and pelletizers. The downstream processes
main raw material of the HDPE product, and hexane
recover the unreacted monomer and produce the poly-
adjusts the slurry concentration in the reactors. Ethyl-
mer slurry as the final product. Polymer grades are
ene, hexane, and the catalyst are continuously fed to
determined by the MIs and densities of the polymer
the reactors. Propylene or 1-butene is used as the
slurry from the reactors and the polymer pellet from
comonomer and hydrogen as the chain-transfer agent.
the pelletizers. In a plantwide viewpoint, grade transi-
The polymer slurry from the first reactor is transferred
tion operation is completed if all of the properties satisfy
to the flash tank for dropping the pressure and fed to
the ranges for the grade specification. The plantwide
the second reactor. The polymer slurry from the second
grade transition time can be defined as the time when
reactor is not the final product but the intermediate
all of the properties satisfy the ranges for the grade
product in polymer industries. The polymer slurry from
specifications. It is required in industrial HDPE plants
the second reactor is fed to the separator to recycle the
to satisfy all of the grade specifications together. Figure
unreacted materials. The polymer from the separator
1 shows the grade transition results for two different
is dried to remove the remaining solvent. The polymer
grade transition policies where four properties, y1 (MI
powder from the dryer is pelletized as the final product.
in the first reactor), y2 (MI in the second reactor), y3
The polymer pellet from the pelletizer is stored in the
(density of the final product), and y4 (MI of the final
silos.
product), determine the polymer grade. The individual
grade transition times for properties y1, y2, and y4 from Figure 3 shows the strategy for the grade transition
the first policy are shorter than those from the second of the HDPE product. The HDPE plant has measuring
policy. instruments for temperature, pressure, concentration,
MI, and density. Measurements are used for updating
1 the dynamic and steady-state models of the HDPE
ty1 < 2ty1, 1ty2 < 2ty2, 1ty4 < 2ty4 (1) process to predict polymer properties. MI and density
are the major properties of grade specification in
where ityk is the individual grade transition time of polyethylene industries. MI is controlled by the molar
property yk by the ith policy. The individual grade ratios of hydrogen to ethylene in the gas phase in the
transition time for property y3 from the first policy is reactors. Because the feed rates of ethylene are deter-
longer than that from the second policy mined by the production rate, MI must be controlled
1
by the feed rate of hydrogen to the reactors. Specifically,
ty3 > 2ty3 (2) the polymer slurry MI from the first/second reactors and
the polymer pellet MI from the pelletizer are used as
The plantwide grade transition time by the first policy the properties for grade specification in industrial
is 1ty3, which is the longest grade transition time of the HDPE processes. The density of the HDPE product is
Ind. Eng. Chem. Res., Vol. 42, No. 1, 2003 93
( MI1
) ( MI2
)
2 2
min J ) w1 1 - + w2 1 - +
uSS MI1,tg MI2,tg
( MIpellet
) ( Fpellet
)
2 2
w3 1 - + w4 1 - + CTuSS (3)
Figure 3. Strategy for grade transition in the industrial HDPE MIpellet,tg Fpellet,tg
process.
Table 1. Grade Specification for the Initial and Target Grades To Compare the Plantwide Grade Transition Time
initial grade target grade
1st reactor MI 2nd reactor MI pellet MI pellet density 1st reactor MI 2nd reactor MI pellet MI pellet density
minimum 80.0 0.39 0.5130 0.9500 784.0 0.07 0.0390 0.9535
standard 110.0 0.49 0.4830 0.9590 884.0 0.09 0.0460 0.9543
maximum 140.0 0.59 0.4530 0.9680 984.0 0.11 0.0530 0.9551
[( ) MI (t) 2
min
u(t0:tfm),tfm
J) ∫tt t w5 1 - MI11,tg
ft
0
+
( ) ( )
MI2(t) 2 MIpellet(t) 2
w6 1 - + w7 1 - +
MI2,tg MIpellet,tg
( w8 1 -
Fpellet(t) 2
Fpellet,tg )]
dt (7) Figure 4. Procedure of modified hierarchical dynamic optimiza-
tion methodology.
subject to
f(x3 (t),x(t),y(t),u(t),t) ) 0 (8)
Acknowledgment
This work was supported by the National Research
Laboratory project (2000-N-NL-01-C-18) and Brain
Korea 21 project.
(kg/m3), kdsp,i ) spontaneous deactivation rate constant Property Change Model in the Downstream
of the catalyst (h-1), Mcat,i ) amount of catalyst in the Processes. The change of the cumulative MI during
ith reactor (kg), Ṁcat,f,i ) catalyst flow rate fed into the pelletizing is modeled empirically using the density, MI,
ith reactor (kg/h), and Ṁcat,o,i ) output flow rate of the blending ratio, and amount of antioxidant. Antioxidant
catalyst from the ith reactor (kg). prevents polymer from the oxidation that makes the MI
of the polymer increase in the downstream processes.
Mass balance of hydrogen A simple time delay model is also used to represent the
dynamics in the centrifugal separator, the dryer, and
dMH2,i
the pelletizer.
) ṀH2,f,i - ṀH2,o,i - Vw,ikH2,iCH2,iCcat,i
dt
(i ) 1, 2, ..., 4) (A4) MI change in the downstream processes
where CH2,i ) hydrogen concentration in the ith reactor MIplt ) d0 + d1Fcum,2 + d2BR log MIinst,1 +
(kg/m3), kH2 ) rate constant of chain transfer to hydro- d3(1 - BR) log MIinst,2 + d4MIcum,2 + d5CAO (A9)
gen (m3/kg‚h), Ṁcat,o,i ) output hydrogen flow from the
ith reactor (kg/h), MH2,i ) amount of hydrogen in the where BR ) ratio of the ethylene feed in the first reactor
ith reactor (kg), and ṀH2,f,i ) hydrogen flow rate fed into to the ethylene feed in the second reactor [(kg/h)/(kg/
the ith reactor (kg/h). h)], CAO ) concentration of antioxidant (ppm), and MIplt
Instantaneous Polymer Properties in Reactors. ) pellet MI (g/10 min).
The instantaneous properties of the polymer are deter-
mined by the empirical equations from the reaction
Nomenclature
temperature and the concentrations of hydrogen, mono-
mer, and comonomer. C ) vector of the operating cost
J ) objective function
Instantaneous MI equation MI1 ) polymer slurry MI in the first reactor
log MIinst ) a0 + a1 log T + a2 log CH2/C2 + MI2 ) polymer slurry MI in the second reactor
MIpellet ) pellet MI of HDPE
a3MC3/C2 + a4MC4/C2 (A5) t0 ) initial time for the grade transition operation
tfm ) final manipulation time for the grade transition
where CH2/C2 ) concentration ratio of hydrogen to operation
ethylene in a reactor (mol %/mol %), MIinst ) instanta- tft ) final transition time for the grade transition operation
it ) grade transition time of property yk by the ith policy
neous MI (g/10 min), MC3/C2 ) mass ratio of propylene yk
to ethylene in a reactor (kg/kg), MC4/C2 ) mass ratio of u ) vector of control input variables
1-butene to ethylene in a reactor (kg/kg), and T ) w1-w8 ) weighting factor in the formulation of optimiza-
reaction temperature (°C). tion
x ) vector of differential state variables
Instantaneous density equation y ) vector of algebraic state variables
(8) Lee, J.; Kim, W. K.; Kim, S. H. Method of Estimating (11) Sargent, R. W. H.; Sullivan, G. R. The Development of an
Product Polymer Properties. Korea Patent Application No. 10- Efficient Optimal Control Package. In Proceedings of the 8th IFIP
2000-0049232, 2000. Conference on Optimization Technique; Stoer, J., Ed.; Springer-
(9) Lee, M. H.; Han, C.; Chang, K. S. Hierarchical Time- Verlag: Berlin, 1978.
Optimal Control of a Continuous Copolymerization Reactor during
Start-Up or Grade Change Operation Using Genetic Algorithms. Received for review March 26, 2002
Comput. Chem. Eng. 1997, S1037. Revised manuscript received October 4, 2002
(10) Lee, M. H.; Han, C.; Chang, K. S. Dynamic Optimization Accepted November 1, 2002
of a Continuous Polymer Reactor Using a Modified Differential
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