Article

Cite This: Ind. Eng. Chem. Res. 2018, 57, 7188−7200 pubs.acs.org/IECR

Automatic Design and Optimization of Column Sequences and

Column Stacking Using a Process Simulation Automation Server
Yuan-Wei Ni and Jeffrey D. Ward*
Dept. of Chemical Engineering, National Taiwan University, Taipei 106-07, Taiwan
*
S Supporting Information

ABSTRACT: Simulation−optimization is applied to determine

nearly optimal process designs in column sequencing and
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stacking problems using a simulated annealing algorithm (SAA)

in the client (MATLAB) and a single distillation column in the
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server (Aspen Plus). Each column in every sequence is optimized

separately, and the total cost of each sequence is calculated. This
method benefits from both the rigor of column modeling in a
process simulator and the flexibility of implementing sequential
procedures and derivative-free optimization in a procedural
programming language. Using this method, a single column can be optimized within 6 min of computer time. Furthermore, when
stacking rules and available utilities are specified, a nearly optimal heat-integrated distillation column sequence can be designed
automatically. Results are illustrated using two case studies of column sequencing problems.

1. INTRODUCTION In distillation column sequences, it is possible that the

Optimization is the selection of the best set of variables from
numerous alternatives. Chemical engineering process design
optimization problems are often complicated, time-consuming,
discrete, and nonconvex. If a near-optimal conceptual design can
be obtained automatically and efficiently for further detailed
study, a great deal of time and effort on the part of process
designers can be saved.
Synthesis of the separation systems is one of the most
important tasks in chemical process design. An important issue in
the synthesis of the separation system is the choice of distillation
column sequence (DCS). The problems can be defined as follows:
given a known feed stream and desired product compositions,
determine the column sequence that minimizes the total annual
cost (TAC). Many researchers1−6 have proposed different
methods for solving this problem.
Optimization algorithms, including the simulated annealing
algorithm (hydrodealkylation process,7,8 process synthesis,9−11
heat exchanger network,12 pressure swing distillation,13 and
reactive distillation14), genetic algorithm (dividing wall col-
umns15 and process synthesis16−18), and tabu search (hydro-
dealkylation process7 and synthesis of reaction/separation
systems19), have successfully been used in process design and
optimization problems.
Simulation−optimization20−23 is a new type of optimization
technique that replaces deterministic mathematical formulations
(usually based on simplified process models) with the use of
simulation. Simulation−optimization has been applied to chem-
ical engineering processes such as a turbo-expander process,24
pressure swing distillation,13 reactive distillation process,14
dividing wall columns,15 distillation of ternary mixtures, and
extractive distillation.18
condenser of one column provides some or all of heat duty to the
reboiler operating at a lower temperature in the other column.25
The heat-integrated distillation synthesis problems can be defined
as follows: Given available utilities and a distillation column
sequence, determine whether column stacking is feasible and if so
what heat-exchange connections should be made between
columns and how much money can be saved by stacking. This
problem has been studied by a number of authors.10,18,26−32
Although the problems of column sequencing and stacking
have been studied by many researchers, all existing methods have
certain limitations. Approaches that rely on shortcut column
design methods are limited by the accuracy of those methods,
and approaches that use rigorous process models but rely on
heuristics for column sequencing and stacking may fail to find the
best process design. In the present work, simulation−optimization
is applied to column sequencing and stacking problems. The simu-
lated annealing algorithm (SAA) is applied to obtain the optimum
design of each column using a rigorous column model in Aspen
Plus and a process simulation automation server.
2. COLUMN MODELING, SEQUENCING, AND
STACKING
2.1. Single-Column Simulation. Simple distillation col-
umns are those with a single feed stream and two product
streams. Sharp separation is separation in which no component is
distributed (i.e., present in a significant amount) in both product
streams. Therefore, for simple sharp distillation, separation of an
Received: September 25, 2017
Revised: March 13, 2018
Accepted: May 2, 2018
Published: May 2, 2018

© 2018 American Chemical Society 7188 DOI: 10.1021/acs.iecr.7b03943

Ind. Eng. Chem. Res. 2018, 57, 7188−7200
Industrial & Engineering Chemistry Research
n-component mixture requires n − 1 columns. Thompson and
King33 developed an equation for the number of sequences (Sn)
for simple sharp separation of n components:
[2(n − 1)]!
Sn =
n! (n − 1)!
The number of column sequences increases dramatically as the
number of components increases. Therefore, it becomes difficult
to obtain overall column sequence conditions and optimization
results.
In this research, we make an assumption to simplify column
sequencing and stacking problems. Figure 1 shows the concept
Figure 1. Concept and illustration of using a single column to simulate
entire systems.
and illustration. Each column is assumed to have only the com-
ponents that must be separated. The pure or key components
that are separated in previous columns do not appear in the later
columns. With this assumption, a process simulator flowsheet
containing only a single distillation column can be used to
simulate all possible column sequences. With simple arrange-
ments and combinations, all column sequences can be modeled.
This saves a great deal of time compared to constructing a
separate flowsheet simulation for every column sequence. In the
single column, we can specify the inlet conditions, set column
specifications or change any other variable from an external
application, and use the single column to model each column in
every sequence separately.
2.2. Column-Sequencing Procedure. Using the single-
column simulation discussed previously, the flowsheet is shown
in Figure 2. The feed is specified to be saturated liquid at the
Figure 2. Single-column simulation flowsheet.
pressure of the previous column. If the column is the first
column, the feed pressure is set to be 1 bar. The pump duty is
determined by comparing the inlet flow pressure and feed stage
pressure. The column condenser pressure is 1 bar. After feed
properties and pump duty are specified, the simulated annealing
algorithm is applied to minimize the total annual cost (TAC).
Article
The design variables in this work are number of trays (NT) and
feed stages (NF) for each column. All the above procedures are
completed with Aspen Plus ActiveX automation server. The
complete procedure is as follows:
Step 1. Determine the feed stream pressure. The feed
(1)
stream pressure of the first column is set to be 1 bar. For all
other columns, the feed pressure is the pressure at the top
or bottom of the previous column (whichever is the feed to
the present column).
Step 2. If the feed stream pressure is less than the column
feed stage pressure, a pump is added to raise the pressure
as necessary.
Step 3. Proceed with SAA to obtain the optimization.
Step 4. Proceed to the next column until all columns are
optimized.
2.3. Column-Stacking Procedure. Separation of chemicals
by distillation consumes a great deal of energy, and reducing this
energy demand is often a priority in separation system design.
If two or more distillation columns are present in a process, and the
condenser temperature in one column is higher than the reboiler
temperature in the other column, then the higher-temperature
condenser can be used to power the lower-temperature reboiler.
Furthermore, it is possible to adjust column pressures to match
temperatures in order to achieve heat integration. The basic idea
was proposed by King,39 and the conceptual process design
was implemented by Andrecovich and Westerberg et al.27
The approach is also called column stacking heat integration.
Hence, given the available utilities, columns can be stacked by
adjusting their pressures to appropriate values.
Figure 3 shows the flowchart for column stacking with SAA
used in this work. First, the average of condenser and reboiler
temperatures is calculated for each column. Then columns are
arranged and numbered in order of ascending average temper-
ature. Next, for the column with the lowest average temperature
(i = 1), the condenser pressure corresponding to saturated liquid
at a temperature 10 K higher than cooling water temperature
is determined using a flash module in Aspen Plus. After the
condenser pressure is determined, the column is designed using
the SAA. The algorithm then determines the condenser pressure
for the second column so that liquid in the condenser will be
saturated at a temperature 10 K higher than the reboiler of the
first column. The procedure is repeated until no more stacking is
possible. All the above statements are completed with the Aspen
Plus ActiveX automation server.
3. SIMULATED ANNEALING ALGORITHM
Many methods have been proposed and developed to solve
optimization problems. Many process design optimization prob-
lems are nonconvex and discrete. Derivative-free methods may
perform better than derivative-based methods for such problems.
Derivative-free, stochastic algorithms such as genetic algorithm
(GA), simulated annealing algorithm, and tabu search (TS) are
commonly applied to such problems. SAA is a probabilistic
algorithm for estimating the global optimum. The concept of
simulated annealing was first proposed by Metropolis et al.34
Kirkpatrick et al.35 applied the concept of simulated annealing to
the optimization problem and successfully solved the traveling
salesman problem. SAA has the advantages that it involves fewer
loops than a sequential optimization procedure and is relatively
easy to program.
The concept of simulated annealing is analogous to metal-
lurgical annealing, in which metals are cooled in such a manner as
7189 DOI: 10.1021/acs.iecr.7b03943
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Figure 3. Column stacking flowchart.

to reduce crystal defects. At first, molecules are disordered at high Otherwise, the original energy state is retained.
temperature and gradually adopt a lower-energy, ordered con- From the above statements, we can see that the system is more
figuration as the metal is cooled. Therefore, they can be regarded likely to accept a high-energy state as current solution at higher
as being in thermodynamic equilibrium at each moment and at temperature and less likely to do so at lower temperature.
each temperature. If the system is in thermodynamic equilibrium Therefore, SAA can avoid becoming trapped in local minima
at a given temperature (T), the probability of the system because it may accept higher-energy states over lower-energy
adopting an energy state (E) is given by the Boltzmann energy states, especially at the beginning, and still achieves a low-energy
distribution: state at the end. The complete procedure is described below, and
⎛ E ⎞ a flowchart for the SAA used in this work is shown in Figure 4.
1
P{E} = exp⎜ − ⎟ Step 1. Generate a set of variables dnew, which is near
Z (t ) ⎝ KbT ⎠ (2) original design variables d.
where Kb is the Boltzmann’s constant and 1/Z(t) is a Step 2. Execute process simulator, and calculate ΔE (ΔE =
normalization factor. Note that molecules are allowed to move E(dnew)− E(d)) from external application.
randomly from original energy state to new energy state Step 3.
depending on the current temperature and energy state. (a) If ΔE < 0, accept dnew as the new solution
Therefore, we can calculate the ratio of the probability between (b) If ΔE > 0 and exp(−ΔE/T) > U(0, 1), accept dnew as
a possible new energy state and the old (current) energy states the new solution. U(0, 1) represents uniformly
according to Boltzmann energy distribution and define it as the distributed random numbers on the interval
acceptance probability: between 0 and 1.
⎛ E − Eold ⎞ (c) Otherwise, set d new = d. (The solution is
P{Enew } ⎛ ΔE ⎞
Paccept = = exp⎜ − new ⎟ = exp⎜ − ⎟ unchanged.)
P{Eold} ⎝ KbT ⎠ ⎝ T ⎠ Step 4. Return to step 1 and continue until thermody-
(3) namic equilibrium at the current temperature is achieved.
where ΔE is the normalized energy difference between the new Step 5. Reduce the system temperature based on the
and old energy states. Based on the Metropolis criterion, the new temperature decrement or cooling schedule.
energy state is accepted if one of the following two statements is Step 6. Return to step 1 and continue until the freezing
true: temperature (Tf) or the termination criterion is achieved.
(1) If the new energy state is less than the old energy state, the There are some annealing schedule parameters in SAA pro-
system accepts the new state. cedures, such as initial temperature (T0), freezing temperature,
(2) If the new energy state is greater than the old energy state temperature decrement, and equilibrium detection. Parameter set-
but the acceptance probability, exp(−ΔE/T), is greater tings have an important impact on the convergence of the algorithm
than a value generated from uniformly distributed random and CPU execution time. Aarts and Vanlaarhoven,36 Patel et al.,37
numbers, the system accepts the new state. Painton and Diwekar,38 and Cheng et al.14 have discussed parameter
7190 DOI: 10.1021/acs.iecr.7b03943
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Figure 4. SAA flowchart.

Table 1. Five-Components Column Sequence

initiation first column second column third column fourth column label
C/DE → D/E (1)
B/CDE →
CD/E → C/D (2)
A/BCDE → BC/DE → B/C and D/E (3)
B/CD → C/D (4)
BCD/E →
BC/D → B/C (5)
A/B and C/DE → D/E (6)
AB/CDE →
A/B and CD/E → C/D (7)
ABCDE a
→
A/BC and D/E → B/C (8)
ABC/DE →
AB/C and D/E → A/B (9)
B/CD → C/D (10)
A/BCD →
BC/D → B/C (11)
ABCD/E → AB/CD → A/B and C/D (12)
A/BC → B/C (13)
ABC/D →
AB/C → A/B (14)
a
A, ethanol; B, isopropanol; C, n-propanol; D, isobutanol; E, n-butanol.

Table 2. Alcohol Case Study Optimization Results of NT, NF, and TAC
separation column NT NF TACa separation column NT NF TACa
A/BCDE 1 138 81 5.2893 BC/D (from 8) 18 54 26 2.3664
AB/CDE 2 37 20 2.0394 C/DE (from 2) 19 56 31 2.2566
ABC/DE 3 44 19 2.7727 C/DE (from 7) 20 56 31 2.2545
ABCD/E 4 42 15 2.5039 CD/E (from 2) 21 51 23 1.9951
A/BCD 5 139 80 5.3113 CD/E (from 7) 22 51 23 1.9930
ABC/D 6 47 19 2.6398 A/B (from 2) 23 151 74 5.2637
B/CDE 7 41 20 1.4477 A/B (from 9) 24 152 74 5.2636
BCD/E 8 48 20 2.1348 A/B (from 14) 25 152 74 5.2636
AB/CD 9 38 20 1.9816 B/C (from 10) 26 45 21 1.3391
BC/DE 10 52 27 2.4113 B/C (from 12) 27 45 21 1.3180
A/BC (from 3) 11 143 80 5.3227 B/C (from 18) 28 45 21 1.3391
A/BC (from 6) 12 144 81 5.3224 C/D (from 9) 29 59 31 2.1415
AB/C (from 3) 13 41 21 1.9222 C/D (from 16) 30 59 31 2.1393
AB/C (from 6) 14 41 21 1.9222 C/D (from 22) 31 59 31 2.1569
B/CD (from 5) 15 43 20 1.3913 D/E (from 3) 32 67 32 1.3056
B/CD (from 8) 16 44 21 1.4172 D/E (from 10) 33 67 32 1.3046
BC/D (from 5) 17 54 26 2.3043 D/E (from 20) 34 67 32 1.3042
a
TAC unit, ×106$.
settings for SAA. The definition of parameters and the move 3.1. Move Generator. A move generator is the generation of
generator are discussed in the following sections. new design variables. The next design variables depend on the
7191 DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research Article

step sizes defined by users. A move generator can be categorized Table 3. TAC for 14 Distillation Column Sequencesa
into two sections: integer variables and continuous variables.
sequence run 1 TAC run 2 TAC run 3 TAC
(a) Integer variables: dnew = d + INT{[2 × U(0, 1) −1]Nstep}, 1 10.296 10.296 10.296
where Value_LB ≤ dnew ≤ Value_UB 2 10.887 10.887 10.887
(b) Continuous variables: dnew = d + {[2 × U(0, 1) − 1]Nstep}, 3 10.344 10.344 10.344
4 10.980 10.980 10.980
where Value_LB ≤ dnew ≤ Value_UB
5 11.130 11.130 11.130
d and dnew represent the original and new set of variables, 6 10.864 10.864 10.861
respectively. Value_LB and Value_UB are the lower and upper 7 11.455 11.455 11.452
bound of dnew. INT means the value is rounded to the nearest 8 10.719 10.719 10.719
integer; U(0, 1) is a uniformly distributed random number on the 9 11.264 11.264 11.262
interval between 0 and 1, and Nstep is the step size for each move. 10 11.346 11.347 11.347
In this work, Nstep is set to 1. 11 11.459 11.460 11.460
3.2. Initial Temperature (T0). Initial temperature is the 12 11.891 11.888 11.901
starting point of the system temperature. The purpose of initial 13 11.784 11.785 11.784
temperature is to ensure that there is a high enough acceptance 14 12.329 12.329 12.327
ratio at the start of SAA. If the acceptance ratio at the beginning a
TAC unit, ×106$.
of the simulation is too low, the system may not escape a local
minimum. The initial temperature should be great enough to
ensure that the algorithm has the possibility of finding the global
optimum. However, a very large CPU execution time will be
required if the initial temperature is too high. In this work, an
arbitrary value is specified and several hundred moves are made.
If the acceptance is greater than 80%, we set that value as initial
temperature for the system. Otherwise, the initial temperature is
doubled and the procedure is repeated until an acceptance ratio
greater than 80% is achieved.
3.3. Freezing Temperature. The freezing temperature, also
called the final temperature, is the termination point of the SAA.
If the freezing temperature is close to the initial temperature, the
result may not be correct because only a few executions may Figure 5. Fourteen column sequences’ TAC.
occur. However, if the freezing temperature is too small in
comparison with the initial temperature, computation time will
be unnecessarily large. In this work, the total number of simula-
tion executions is fixed, and the freezing temperature is
determined by the calculation given the other parameters (i.e.,
initial temperature, temperature decrement, and equilibrium
detection criterion). The algorithm terminates when the system
temperature reaches the given value.
3.4. Temperature Decrement. The temperature decre-
ment affects the convergence and execution performance of SAA.
If the system temperature is reduced too quickly, the energy state
may not escape from a local minimum. If the system temperature
is reduced too slowly, CPU execution time will be longer than
necessary. In this work, the expression of temperature decrement
is as follows: Tn+1 = αTn, where 0.8 ≤ α ≤ 0.9 (α is temperature
decrement factor, and n is the counter).
3.5. Equilibrium Detection. Equilibrium detection is a
quasi-equilibrium at a given temperature throughout the SAA.
System temperature decreases when equilibrium is detected.
NE should be large enough to ensure that the algorithm explores
the neighborhood of a given set of variables in all directions at a
given temperature. If there are n optimization variables and each
variable can remain the same, increase, or decrease, the equi-
librium detection variable could be set equal to 3n. In this work, Figure 6. SAA results for direct sequence: (a) A/BCDE, (b) B/CDE,
the equilibrium detection parameter is set to be 15 to ensure that (c) C/DE, and (d) D/E.
equilibrium is achieved at each temperature.
3.6. Recovery after Special Cases. While the simulated point is not counted toward the equilibrium detection. To handle
annealing is running, there are two special cases that must be the case where Aspen Plus crashes, a second instance of Matlab is
handled. One is that the Aspen Plus flowsheet fails to converge, run in the background. If it is found that Aspen Plus has not
and the other is that the Aspen Plus program crashes. If the responded after a certain amount of time (about 15 seconds), the
Aspen Plus flowsheet fails to converge, that point is discarded Aspen Plus task is killed (using the Windows command taskkill),
and the algorithm proceeds to try another point. The discarded Aspen Plus is restarted, the simulation file is reloaded, and the
7192 DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research Article

Table 4. Column Stacking Optimization Results for 14

Arrangements
sequence NT NF P (bar) sequence NT NF P (bar)
1 33 17 0.2595 2 33 17 0.2595
149 89 1.7741 149 89 1.7741
68 39 3.7349 73 41 3.7349
98 45 6.2940 76 33 7.0785
3 38 18 0.2595 4 36 18 0.2595
150 90 1.5672 144 87 1.6379
63 34 4.1465 71 39 3.5175
100 46 6.8244 74 30 7.8223
5 38 18 0.2595 6 116 52 0.3221
146 85 1.5672 40 22 1.7540
68 35 4.1015 68 39 3.2564
76 30 8.8149 95 44 5.6340
7 115 52 0.3221 8 38 18 0.2595
40 22 1.7441 152 86 1.5672
72 40 3.2417 53 24 4.1486
75 33 6.2975 100 46 6.7579
9 116 52 0.3221 10 36 18 0.2595
45 23 1.7523 149 88 1.6379
53 24 3.9458 56 20 4.2272
98 45 6.4793 82 45 10.7723
11 38 18 0.2595 12 116 52 0.3221
150 86 1.5672 42 22 1.7531
65 33 3.7161 54 19 3.8911
68 23 9.5750 83 46 10.0383
13 38 18 0.2595 14 116 52 0.3221
156 87 1.5672 45 23 1.7523
60 27 4.1844 59 26 3.9414
69 23 10.4672 69 23 9.9542

Table 5. Column Stacking TACa

sequence column sequence column stacking save (%)
1 10.296 8.1531 20.81
2 10.887 8.3524 23.28
3 10.344 7.8840 23.78
4 10.980 8.4597 22.95
5 11.130 8.1383 26.88
6 10.864 6.9184 36.32
7 11.455 7.0608 38.36
8 10.719 8.0375 25.01
9 11.264 7.6822 31.80
10 11.346 8.6557 23.71
Figure 7. Alcohol column stacking T−Q diagram. 11 11.459 8.4663 26.12
12 11.891 7.7882 34.50
optimization resumes from the point at which Aspen Plus 13 11.784 8.4117 28.62
became unresponsive. 14 12.329 8.0899 34.38
a
TAC unit, ×106$.
4. CASE STUDIES
4.1. Alcohol Case Study. The case study used in this rate is 500 koml/h, and component compositions are 0.25/0.15/
example is taken from King.39 Boozarjomehry et al.16,17 proposed 0.35/0.10/0.15, respectively. The feed is saturated liquid at 1 bar.
a genetic algorithm to obtain an optimal column sequence using The purity of key components in each column is specified to be
short-cut column models. Andrecovich and Westerberg27,28 have 0.98. UNIFAC property methods are used in Aspen Plus
discussed the heat-integrated distillation using both constant simulations. TAC calculations are taken from Luyben,40 and the
QΔT and nonconstant QΔT approaches to calculate minimum detailed information is shown in appendix.
utility use within utility bound. In this work, the procedure Table 1 shows the 14 possible column sequences for a five-
described previously is applied to determine an optimal column component separation problem. Table 2 shows optimization
sequence and column stacking configuration. Five components results including the optimal number of stages and feed stage for
are considered in this study: ethanol, isopropanol, n-propanol, each column. The execution time is about 5−6 min per column.
isobutanol, and n-butanol. Those are labeled A, B, C, D, and E, Therefore, it takes about 3 h to determine the optimal design of
respectively, according to their relative volatilities. The total flow all 34 columns in all 14 column sequences. After every column
7193 DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research Article

Figure 8. Column stacking flowchart with split.

Table 6. Further Column Stacking TACa

column stacking further column stacking additional savings
sequence TAC TAC (%)
1 8.1531 7.4264 8.91
2 8.3524 7.5286 9.86
3 7.8840 7.0633 10.41
a
TAC unit, ×106$.

Table 7. Four-Component Column Sequence

first second third
initiation column column column label
B/CD → C/D (1)
A/BCD →
BC/D → B/C (2)
ABCDa → AB/CD → A/B and C/D (3)
A/BC → B/C (4)
ABC/D →
AB/C → A/B (5)
a
A, benzene; B, toluene; C, ethylbenzene; D, styrene.

Table 8. Styrene Case Study Optimization Results of NT, NF,

and TACa
separationb column NT NF TACc
A/BCD 1 44 18 0.9883
AB/CD 2 66 31 1.6918
ABC/D 3 159 90 4.5134
A/BC 4 44 19 0.8704
AB/C 5 61 35 1.4508
B/CD 6 66 25 1.4053
BC/D 7 166 93 4.1967
Figure 9. Further column stacking T−Q diagram for sequences 1−3. A/B (from 2) 8 41 21 0.7309
A/B (from 5) 9 41 21 0.7309
is optimized, the TAC for all 14 column sequences can be B/C (from 4) 10 58 29 1.1212
determined by summation. Table 3 shows the TAC for the 14 B/C (from 7) 11 58 29 1.1394
column sequences, and Figure 5 shows the sequence TAC results C/D (from 2) 12 155 78 3.6861
in the form of a bar chart. Sequence 1, which is the direct C/D (from 6) 13 156 79 3.6871
sequence, has the lowest total annual cost ($10.296 × 106). a
Condenser pressure = 1 bar. Elapsed time: 0.08−0.1 h per column.
b
Figure 6 shows SAA results for the four columns in the direct A, benzene; B, toluene; C, ethylbenzene; D, styrene. cTAC unit,
sequence (sequence 1). As was discussed previously, SAA may ×106$.
accept solutions with a higher TAC at the beginning to avoid
being trapped at extremes but should converge to a solution with lowest cost. Therefore, the curve fluctuates significantly at the
a lower TAC at the end to ensure that the answer is near the beginning but becomes flat by the end. For each column, the
7194 DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research Article

Figure 10. Styrene SAA results.

optimization is repeated three times using different initial Table 9. TAC for Five Distillation Column Sequencesa
conditions and SAA parameter values, and similar results were
sequence run 1 TAC run 2 TAC run 3 TAC
found for each run.
Figure 7 shows the column stacking T−Q diagram for 14 1 6.0807 6.0809 6.0807
2 6.3244 6.3245 6.3252
sequences, and Table 4 shows the optimization results for
3 6.1088 6.1088 6.1101
number of trays and feed stage for each column in each stacked
4 6.5050 6.5050 6.5051
sequence. The operating pressure of each column is also shown
5 6.6950 6.6950 6.6952
in the table. The procedure stacks the columns in order by the a
TAC unit, ×106$.
average column temperature at the optimal pressure for that
column. While this is likely to be the optimal stacking given temperature allows for heat integration and reduces
configuration, the possibility that a better configuration exists energy consumption. However, it may increase capital costs and
is not checked by the algorithm. Increasing pressure to achieve a energy costs because of operation at higher pressure or with
7195 DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research Article

Some sequences have enough space (temperature driving

force between the hot utility and the hottest reboiler) that further
stacking can be accomplished by dividing one of the columns into
two columns operated at different pressures (double-effect
distillation). Therefore, the previous column stacking procedure
is modified to permit such splitting. Figure 8 shows the flowchart
allowing column splitting if possible. A criterion is applied to
determine whether column splitting can be implemented. If the
high-pressure steam temperature minus the highest reboiler
temperature (Tavail) is greater than the temperature difference
between condenser and reboiler of the highest heat duty column
(Tdifference) plus the driving force temperature difference
Figure 11. Five column sequences’ TAC. (ΔTdriving force), further stacking by column splitting is possible.
In that case, the column with the highest duty is split into two
Table 10. Deviation between Entire System and Single columns and the stacking procedure is repeated. This process is
Column repeated until Tavail is less than Tdifference, at which point the
column 1 column 2 column 3 TAC deviation
algorithm is terminated.
optimization (NT, NF) (NT, NF) (NT, NF) (×106$) (%) Figure 9 shows the results of further column sequence for
single (44, 18) (66, 25) (156, 79) 6.0807 − sequences 1−3. Table 6 shows the comparison between column
column stacking without splitting and column stacking with column
entire (44, 18) (69, 27) (156, 79) 6.0979 0.2821 splitting. Column splitting can further reduce the TAC by about
system (45, 19) (69, 27) (157, 80) 6.0984 0.2902 8−10%.
(45, 19) (68, 27) (155, 79) 6.0968 0.2641 4.2. Styrene Case Study. Vasudevan et al.41 have proposed
several process design and control structures for the styrene
higher-grade utility. Therefore, column stacking is not guar- process using integrated configurations. Luyben42 has provided
anteed to reduce total cost. different process designs for the styrene process and developed
Therefore, for each column sequence, the total cost of the the plantwide optimization and control structure. In this work,
stacked sequence is compared with the total cost of the unstacked the procedure described previously is applied to determine an
sequence in Table 5. Because of the reasons mentioned above, optimal column sequence and column stacking configuration.
the percentage savings is quite different for different sequences, Four components are used in this study: benzene, toluene,
from 20 to 38%. ethylbenzene, and styrene. Those are labeled A, B, C, and D,

Figure 12. Styrene column stacking T−Q diagram.

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Industrial & Engineering Chemistry Research Article

Table 11. Column Stacking Optimization Results for Five column sequences can be determined by summation. Table 9 and
Arrangements Figure 11 show the TAC results for all five column sequences.
Sequence 1, the direct sequence, again has the lowest total annual
sequence NT NF P (bar) sequence NT NF P (bar)
cost ($6.0807 × 106).
1 39 16 0.3945 2 40 16 0.3945 To verify the results, the entire direct sequence was
70 28 1.3708 60 29 1.3837 constructed in Aspen Plus, and the SAA was used to perform
184 95 2.5684 205 121 3.0936 optimization. In this case, SAA changes six variables simulta-
3 35 18 0.3945 4 41 16 0.3945
neously (the number of trays and feed tray for each column).
72 34 1.4613 59 30 1.1857
Table 10 shows the results and deviations between the simulation
183 95 2.7041 207 122 4.2974
of the entire sequence and column-by-column simulations. The
5 35 18 0.3945
errors (less than about 0.3%) are quite small if the purity
65 36 1.4615
specifications are high. The flowsheets for the individual columns
216 128 4.9976
and the combined column sequence are shown in Figure S1 in
Table 12. Column Stacking TACa the Supporting Information.
Column stacking was also studied for the styrene example.
sequence column sequence column stacking save (%) Figure 12 shows column stacking T−Q diagrams for five
1 6.0807 4.9161 19.1524 sequences, and Table 11 shows the optimization results of
2 6.3244 5.6578 10.5401 number of trays and feed stage. The operating pressure at a given
3 6.1088 4.9378 19.1691 temperature is also shown in the table. The number of trays
4 6.5050 6.2900 3.3051 required in a given column increase as pressure increases because
5 6.6950 6.4601 3.5086 of the difficulty of separation increases. Table 12 shows TAC
a
TAC unit = [ × 106$] comparison between column sequences with and without stacking.
The percentage savings varies from 3 to 20%. The best stacked
respectively, according to their relative volatilities. It is assumed sequence, the direct sequence, is the same as the best unstacked
that total flow rate is 400 kmol/h and each component has the sequence.
same molar flow rate. The feed is assumed to be saturated liquid From Figure 12, we can see that the separation of ethylbenzene
at 1 bar. The desired purity of key components in each column is and styrene dominates the majority of utility consumption as a
set to be 0.999. Peng−Robinson physical properties are used in result of the difficult separation. Furthermore, the separation of
the Aspen Plus simulations. TAC calculations are taken from ethylbenzene and styrene could be conducted under vacuum to
Luyben,40 and additional details are given in the appendix. prevent styrene polymerization if there are no inhibitors.42
Column sequences and labels are shown in Table 7. Table 8 Therefore, the stacking procedure is modified so that the
shows the optimization results: the optimal number of trays and ethylbenzene/styrene separation occurs at the lowest pressure.
feed stage for each column and the minimum TAC. The The new stacking flowchart is shown in Figure 13. It is almost the
computer time required is again about 5−6 min per column. same flowchart as the previous stacking flowchart except that the
Therefore, 1−1.5 h was required to determine the minimum cost stacking sequence is modified. Figure 14 shows T−Q diagram
for all 13 columns in all five column sequences. Figure 10 shows results for five sequences. The third column cannot be stacked
SAA results for all 13 columns. With this data, the TAC of all five upon the second column because of the greater temperature

Figure 13. Flowchart of column stacking with SAA (ethylbenzene/styrene stacks first).

7197 DOI: 10.1021/acs.iecr.7b03943

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Industrial & Engineering Chemistry Research
Figure 14. Styrene column stacking T−Q diagram with C/D separation first.
Figure 15. Flowchart of further column stacking with SAA (ethylbenzene/styrene stacks first).
range in the first two columns. However, the second and third
columns can both be stacked upon the first column. Therefore,
the flowchart is modified again to achieve this goal. The further
modified stacking flowchart is shown in Figure 15. The condenser
temperature of columns 2 and 3 are set to be 10 K higher than the
reboiler of column 1. Figure 16 shows further T−Q diagram results
7198
Article
for five sequences, and Table 13 shows TAC and comparison of
two methods for stacking ethylbenzene/styrene first. When the
second and third columns are stacked upon the first column, the
reboiler and condenser duty is reduced but the energy cost of the
third column is increased because of the use of higher-grade
utility. The cost savings on a percentage basis vary from 5 to 13%.
DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research Article

Figure 16. Styrene further column stacking T−Q diagram with C/D separation first.

Table 13. Column Stacking with Ethylbenzene/Styrene the unstacked sequences. Because a rigorous column model is
Separation Firsta employed, the results are more accurate than results based on
shortcut column design methods. Furthermore, the simulated
column stacking column stacking (ethylbenzene/
(ethylbenzene/ styrene first) (stack upon the annealing algorithm is more likely to achieve a result closer to the
sequence styrene first) first column) save (%) global minimum than either a heuristic-based method or a
sequential optimization method.

■
1 6.2135 5.3986 13.1150
2 6.4329 6.1004 5.1687
3 6.1236 5.5309 9.6789 ASSOCIATED CONTENT
4 6.3989 5.8370 8.7812 *
S Supporting Information
5 6.5169 6.0614 6.9895 The Supporting Information is available free of charge on the
a
TAC unit, ×106$. ACS Publications website at DOI: 10.1021/acs.iecr.7b03943.
TAC caluculation, optimal flowsheets for the styrene
separation process, additional data tables (PDF)

■
5. CONCLUSION
Simulation−optimization is a useful optimization technique that AUTHOR INFORMATION
replaces deterministic mathematical formulations with the use of Corresponding Author
simulation. In this work, simulation−optimization is applied to *E-mail: jeffward@ntu.edu.tw.
the problems of column sequencing and stacking. A simulated
ORCID
annealing algorithm written in Matlab interfaces with a flowsheet
simulator, Aspen Plus, with a model of a single distillation Jeffrey D. Ward: 0000-0003-0727-7689
column. The flowsheet is used to model and optimize every Notes
The authors declare no competing financial interest.

■
column in every sequence, after which the total cost (TAC) of
each sequence can be determined. The results demonstrate that
the optimal sequence can be obtained quickly, with each column NOMENCLATURE
being optimized within 5−6 min. For both case studies NT = Number of trays
considered, the direct sequence was found to have the lowest NF = Feed stage
cost. A column stacking algorithm is also implemented. Given P = Pressure
utility temperatures, heat integration between columns can be T = Temperature
achieved by adjusting the operating pressure of each column. Q = Heat duty
Overall cost savings of 20−30% can be achieved compared to Kb = Boltzmann’s constant
7199 DOI: 10.1021/acs.iecr.7b03943
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Industrial & Engineering Chemistry Research
E = Energy state
T0 = Initial temperature
Tf = Frozen temperature
Nstep = Step size
d = Design variables
dnew = New design variables
ΔTdriving force = Driving force temperature
INT = Rounded to the nearest integer
TAC = Total annual cost
SAA = Simulated annealing algorithm
■
GREEK SYMBOLS
α = Temperature decrement factor
■
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