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journal homepage: www.elsevier.com/locate/compchemeng

Nguyen Van Duc Long, Moonyong Lee ∗

School of Chemical Engineering, Yeungnam University, Gyeongsan 712-749, South Korea

a r t i c l e i n f o a b s t r a c t

Article history: Designing dividing wall columns (DWC) – energy-efﬁcient separators of ternary mixtures – involves

Received 22 April 2011 multivariable problem solving. These variables interact with each other and need to be optimized

Received in revised form 28 June 2011 simultaneously to obtain the best design. In this work, a practical method employing response surface

Accepted 5 July 2011

methodology (RSM) is proposed for DWC design and optimization. The optimum DWC structure can be

Available online 18 July 2011

found in a practical manner while minimizing simulation runs. The proposed method was tested in the

design and optimization of an acetic acid puriﬁcation process. The RSM based optimization effectively

Keywords:

copes with interactions between optimizing variables and its predictions agreed well with the results of

Distillation process

Dividing wall column

rigorous simulation. The DWC system designed by the proposed method decreased total annual costs by

Structure design 44.57% compared with conventional distillation.

Response surface methodology © 2011 Elsevier Ltd. All rights reserved.

conﬁgurations could be better suited.

In the U.S., distillation accounts for about 3% of total energy Designing DWCs is much more complex than conventional

requirement and more than 90% of all product recovery and arrangements because of the greater number of degrees of free-

puriﬁcation separations. It consumes more than 95% of the dom (Amminudin, Smith, Thong, & Towler, 2001). These degrees

energy supplied to the chemical industry worldwide (Vazquez- of freedom interact with each other and need to be optimized

Castillo et al., 2009). Increasing energy costs are forcing industries simultaneously for optimal column design. A common difﬁculty

to cut utility consumption, with thermally coupled conﬁgura- associated with DWC design is estimating the number of stages

tions being incorporated into multicomponent distillation systems in each section (Dejanović, Matijašević, & Olujić, 2010). Since the

to reduce both utility consumption and capital costs (Franke, number of stages is an integer variable, column optimization is a

Górak, & Strube, 2004; Rong & Turunen, 2006; Rong, Kraslawski, mixed integer non-linear programming problem (MINLP), which

& Turunen, 2003; Segovia-Hernández, Hernández, & Jiménez, cannot be solved with commercially available process simulators.

2005). Dividing wall column (DWC, Fig. 1) can effectively reduce External optimization routines are therefore required to be cou-

energy requirement by up to 30% while also lowering engi- pled with process simulators. Furthermore, solving the MINLP does

neering and hardware costs compared with conventional direct not guarantee ﬁnding the global optimum in a non-convex prob-

and indirect distillation sequences (Diggelen, Kiss, & Heemink, lem. Triantafyllou and Smith (1992) proposed a short-cut design

2010; Errico, Tola, Rong, Demurtas, & Turunen, 2009; Hernández method for the design and optimization of fully thermally coupled

& Jiménez, 1999; Kiss & Bildea, 2011; Kiss & Rewarad, in columns. Using a three-column model, they applied the conven-

press; Long, Lee, & Lee, 2010; Segovia-Hernández, Hernández- tional Fenske-Underwood-Gilliland short-cut design technique to

Vargasa, & Márquez-Muñoz, 2007; Sotudeh & Shahraki, 2008; each column, not only for process screening, but also to provide

Tamayo-Galván, Segovia-Hernández, Hernández, Cabrera-Ruiz, & a reliable initialization for rigorous simulation. Amminudin et al.

Alcántara-Ávila, 2008; Triantafyllou & Smith, 1992). Energy efﬁ- (2001) developed a semi-rigorous method based on the concept

ciency arises because DWCs can allow reversible splits with no of equilibrium stage composition for the initial design of a DWC,

part of the separation being performed twice (Poth, Brusis, & which can be employed any established non-linear optimization

Stichlmair, 2004). It should be noted that although DWC has indeed solver.

many beneﬁts, it also has some application limitations such as Dünnebier and Pantelides (1999) proposed a rigorous design

a large temperature difference between reboiler and condenser, method based on detailed column superstructures for a given

heat transfer across the dividing wall, and the condition of high separation task, followed by mathematical optimization. A local

optimization code – CONOPT was interfaced to the gPROMS pro-

cess modeling tool. Their method can simultaneously determine

∗ Corresponding author. Tel.: +82 53 810 2512; fax: +82 53 811 3262. design parameters and perform simulations. However, like as most

E-mail address: mynlee@yu.ac.kr (M. Lee). approaches based on local optimization codes, their method do not

0098-1354/$ – see front matter © 2011 Elsevier Ltd. All rights reserved.

doi:10.1016/j.compchemeng.2011.07.006

120 N. Van Duc Long, M. Lee / Computers and Chemical Engineering 37 (2012) 119–124

Fig. 1. A dividing wall column. Fig. 3. Simpliﬁed ﬂow sheet illustrating the existing separation train of two con-

ventional columns.

Table 1

Feed mixture condition and product requirement.

Feed conditions

Methanol 0.08

Formic acid (FA) 425.36

Water 1069.76

Acetic acid (AA) 64796.71

Propionic acid (PA) 485.67

Temperature (◦ C) 167.7

Pressure (bar) 4.46

Product requirement

Formic acid (FA) <1000 ppm

Water <1000 ppm

Propionic acid (PA) <300 ppm

Table 2

Factors’ coded levels.

Factor Levels

−1 0 1

Middle section (N2) 30 40 50

Bottom section (N3) 40 50 60

Feed stripping section (N4) 10 15 20

Fig. 2. A three-column distillation system for the initial design of DWC structure.

Side product section (N5) 7 11 15

tion ﬁnding steps. Long et al. (2010) and Premkumar and Rangaiah

(2009) optimized only one variable at a time, keeping the others the developed model to optimize the conditions of the process

constant. For each chosen number of trays, feed and side tray loca- under investigation (Box & Behnken, 1960; Erbay & Icier, 2009;

tion, and dividing wall section, internal vapor and liquid ﬂow to the Mannan, Fakhru’l-Razi, & Alam, 2007). It uses quantitative data

prefractionator were varied to optimize energy consumption. Such from an appropriate experimental design to determine and simul-

a simpliﬁed approach does not allow interactions between vari- taneously solve multivariable problems. The Box–Behnken design

ables to be identiﬁed or quantiﬁed. Vazquez-Castillo et al. (2009) in RSM only has three levels (low, medium, and high, coded as

applied genetic algorithm with restrictions coupled to the Aspen −1, 0, +1) and requires few experimental or simulated runs. Its

PlusTM process simulator for the evaluation of the objective func- design is more efﬁcient and easier to arrange and interpret than

tion. However, this method is complex to implement. Thus, a more others, allowing RSM to be used routinely in optimization studies

practical and simple method of optimizing DWCs would be useful. of multivariable systems in several biotechnological and industrial

Statistical approaches are promising for process optimization processes. RSM has been used to optimize bioprocess parameters

studies. Response surface methodology (RSM) is a general tech- (Kalil, Maugeri, & Rodrigues, 2000; Mannan et al., 2007; Wang &

nique for the empirical study of relationships between measured Lu, 2005), as well as media and cultivations (Elibol, 2004; Hujanen,

responses and independent input variables (Box & Wilson, 1951). Linko, & Linko, 2001; Lai, Pan, & Tzeng, 2003).

A response surface is usually a polynomial whose coefﬁcients are This work proposes a simple and efﬁcient practical approach to

extracted by a simple least-square ﬁt to experimental data. RSM the design and optimization of DWCs using RSM. A case study for

is quite powerful since, in addition to modeling, it can also use acetic acid puriﬁcation is used to demonstrate its application.

N. Van Duc Long, M. Lee / Computers and Chemical Engineering 37 (2012) 119–124 121

Fig. 4. Three-dimensional response surface plots of interactions between main design variables N1, N2, N3, N4, and N5.

2. Design and optimization methodology column corresponds to the prefractionator section in the DWC. The

rectifying section of the second column and the stripping section

2.1. Design of the third represent the top and bottom sections of the DWC,

respectively. The stripping section of the second column and the

Initial DWC structure design involved applying a shortcut design rectifying section of the third are equivalent to the dividing wall

procedure (Amminudin et al., 2001; Lee, Shamsuzzoha, Han, Kim, section of the DWC. The bottom stream from the second column and

& Lee, 2011; Long et al., 2010) based on a conventional column the top stream from the third column correspond to the side stream

conﬁguration (Fig. 2). In this conventional conﬁguration, the ﬁrst of the DWC (Long et al., 2010). Consequently, the DWC structure can

122 N. Van Duc Long, M. Lee / Computers and Chemical Engineering 37 (2012) 119–124

mixture, the top and bottom sections above and below the dividing

wall section, and the dividing wall section.

2.2. Optimization

including the internal vapor (FV ) and liquid (FL ) ﬂows to the prefrac-

tionator, the number of trays in the top (N1), middle (N2), bottom

(N3), feed stripping (N4), and side product (N5) sections were opti-

mized. Main design variables of the DWC are also depicted in Fig. 1.

Note that the numbers of trays in each side of the dividing wall sec-

tion is equally ﬁxed as N2. After determining the preliminary ranges

of the variables through single-factor testing, a Box-Behnken design

was employed under the response surface methodology (RSM) to

analyze how the variables interacted and optimize the system in

Fig. 6. Simpliﬁed ﬂow sheet of the resulting DWC system.

terms of total annual cost saving.

Simulation run data were ﬁtted to a second-order polynomial

model and regression coefﬁcients were obtained. The generalized

Table 3

second-order polynomial model used in the response surface anal-

Equipment costs, utility costs and total annual cost saving for conventional sequence

ysis is as follows: and a DWC.

k

k Conventional column sequence DWC

Y = ˇ0 + ˇi Xi + ˇii Xi2 + ˇij Xi Xj + ε (1)

1st column 2nd column

i=1 i=1 i<j

Tray number 65 50 126

where Y is the predicted response (total annual cost saving), Xi are Column diameter (m) 4.3 2.9 3.7

Investment costs (US $) 5,989,333 3,401,068 7,809,244

the uncoded or coded values of the variables, ˇ0 is a constant, ˇi , ˇii

Condenser duty (Gcal/h) 25.33 12.99 21.71

and ˇij are the coefﬁcients of the linear, quadratic and interactive Reboiler duty (Gcal/h) 24.45 13.97 20.87

terms, respectively, and ε is the error term. MINITAB software was Reboiler saving (%) 0.00 45.67

used for response surfaces ﬁtting and optimizing the total annual TAC saving (%) 0.00 44.57

cost saving.

vapor (FV ) and liquid (FL ) ﬂows to the prefractionator were varied

3. Case study to minimize the total annual cost while still achieving the required

product purity. Fig. 4 shows the three-dimensional response sur-

3.1. Conventional distillation sequence face plots of interactions between the number of trays in the top

(N1), middle (N2), bottom (N3), feed stripping (N4), and side prod-

The proposed RSM-based method was used to design and opti- uct (N5) sections. Two parameters of each model were plotted

mize a DWC for acetic acid puriﬁcation. The existing distillation on each set of X and Y axes. Total annual cost saving was plot-

column sequence and current operating conditions are shown in ted on the Z axis. The remaining parameters were automatically

Fig. 3 and the conditions of the feed mixture and product require- set at their center point values by the software while construct-

ments are listed in Table 1. The system consists of two valve-tray ing the plots. The resulting second-order polynomial model was as

columns with diameters of 4.3 and 2.9 m and 65 and 50 trays, follows:

respectively (Long et al., 2010). Simulations were run using a com-

mercial simulator (Aspen HYSYS V7.1). The NRTL-HOC property Y = 43.345 − 0.126X1 + 5.253X2 + 0.004X3 − 1.707X4 − 0.764X5

method, which employs the Hayden–O’Connell equation of state − 0.167X12 − 5.235X22 − 0.106X32 − 1.211X42 − 1.114X52

as the vapor phase model and the NRTL equation for the liquid

phase, was used to predict the vapor–liquid equilibrium (VLE) in the +0.172X1 X2 − 0.056X1 X3 − 0.204X1 X4 + 0.290X1 X5

simulations. Dimerization affects the VLE, vapor phase properties, +0.130X2 X3 + 3.477X2 X4 + 2.512X2 X5 − 0.048X3 X4

such as enthalpy and density, and liquid phase properties such as

enthalpy. The Hayden–O’Connell equation reliably predicts the sol- +0.143X3 X5 − 1.034X4 X5 (2)

vation of polar compounds and the vapor phase dimerization that

occurs in mixtures containing carboxylic acids (Aspen Technology,

The greatest total annual cost saving was found at coded levels

2009). From the base case simulation model, it can be shown that

of the number of trays in the top, middle, bottom, feed stripping,

energy requirements in the reboilers of the two columns are 24.45

and side product sections of 0.3737, 0.5758, 0.6566, −0.1919 and

and 13.97 Gcal/h, respectively.

0.5152, respectively (Fig. 5). Under these conditions, the maximum

total annual cost saving by the DWC was predicted as 44.80%. The

3.2. Dividing wall column natural values of the valuables can be derived from the coded lev-

els. FV and FL then were optimized to maximize the total annual

A DWC conﬁguration can be employed to lower costs compared cost saving, while maintaining sufﬁcient product purity. Fig. 6

with a conventional column sequence. Its structure was initially shows a simpliﬁed ﬂow sheet illustrating the resulting DWC sys-

estimated using the shortcut design method (Lee et al., 2011), and tem. The result from rigorous simulation also revealed that the

it was then optimized by the RSM. Table 2 shows the factors and DWC can save up to 44.57% of total annual costs, which showed

levels used in this case study. 46 simulations were run to opti- good agreement with the predicted result by the RSM. Table 3 sum-

mize 5 parameters of the DWC structure. For each run, internal marizes equipment costs, utility costs and total annual cost saving

N. Van Duc Long, M. Lee / Computers and Chemical Engineering 37 (2012) 119–124 123

Fig. 7. Contour plots of interactions between N1–N3 and N2–N5 predicted by the RSM (a) and by the rigorous simulation (b).

for conventional sequence and a DWC. Note that only a 37.09% that the contour plots by the RSM are quite similar to the actual

improvement of total annual cost was achieved for the same sys- ones.

tem when the DWC variables were optimized one variable at one

time (Long et al., 2010). It should be also emphasized that the RSM 4. Conclusions

requires only 46 simulation runs to optimize the DMC structure

compared with the 916,839 simulation runs by the brute-force In this paper, a practical method of designing and optimizing

mesh search method. DWCs was developed based on the RSM. The proposed method is

Several simulation runs were carried out to validate the con- easy and efﬁcient to implement using Hysys and MINITAB. The DWC

tour plots predicted by the RSM. Fig. 7 compares the contour structure was efﬁciently optimized with a little computational

plots of interactions between N1–N3 and N2–N5 evaluated by the effort. The proposed RSM-based approach coped with interac-

RSM and by rigorous simulation. It is apparent from the ﬁgure tions between optimizing variables, effectively. To demonstrate its

124 N. Van Duc Long, M. Lee / Computers and Chemical Engineering 37 (2012) 119–124

validity, the proposed method was applied to design and optimize a Box, G. E. P., & Behnken, D. W. (1960). Some new three level designs for the study of

DWC for acetic acid puriﬁcation. The resulting DWC reduced total quantitative variables. Technometrics, 2, 455–475.

Box, G. E. P., & Wilson, K. B. (1951). On the experimental attainment of optimum

annual costs by 44.57% compared with conventional distillation. conditions. Journal of the Royal Statistical Society Series B, 13, 1–45.

The predicted results by the RSM showed a good agreement with Dejanović, I., Matijašević, Lj., & Olujić, Ž. (2010). Dividing wall column-a break-

the actual trend from rigorous simulation. These results conﬁrm through towards sustainable distilling. Chemical Engineering and Processing, 49,

559–580.

that the proposed RSM-based method provides a practical and efﬁ- Diggelen, R. C. V., Kiss, A. A., & Heemink, A. W. (2010). Comparison of control

cient way to the design and optimization of complex DWC. strategies for dividing-wall columns. Industrial & Engineering Chemistry Research,

49(2), 288–307.

Acknowledgement Dünnebier, G., & Pantelides, C. C. (1999). Optimal design of thermally coupled dis-

tillation columns. Industrial Engineering and Chemical Research, 38, 162–176.

Elibol, M. (2004). Optimization of medium composition for actinorhodin production

This research was supported by a grant from the Gas Plant R&D by Streptomyces coelicolor A3(2) with response surface methodology. Process

Center funded by the Ministry of Land, Transportation and Mar- Biochemistry, 39, 1057–1062.

itime Affairs (MLTM) of the Korean government. Erbay, Z., & Icier, F. (2009). Optimization of hot air drying of olive leaves using

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Errico, M., Tola, G., Rong, B. G., Demurtas, D., & Turunen, I. (2009). Energy saving

Appendix A. Column cost correlations and capital cost evaluation in distillation column sequences with a divided wall

column. Chemical Engineering Research and Design, 87(12), 1649–1657.

a. Sizing the column: Column diameter was determined by the Franke, M., Górak, A., & Strube, J. (2004). Auslegung und Optimierung von hybriden

column ﬂooding condition that ﬁxes the upper limit of vapor Trennverfahren. Chemie Ingenieur Technik, 76, 199–210.

Hernández, S., & Jiménez, A. (1999). Design of energy-efﬁcient petlyuk systems.

velocity. Operating velocity is normally between 70 and 90% Computers and Chemical Engineering, 23(8), 1005–1010.

of the ﬂooding velocity (Premkumar & Rangaiah, 2009; Sinnott, Hujanen, M., Linko, S., & Linko, Y. Y. (2001). Optimisation of media and cultivation

2005); in this study, 85% of the ﬂooding velocity was used. conditions for L(+)(S)-lactic acid production by Lactobacillus casei NRRL B-441.

Applied Microbiology Biotechnology, 56, 126–130.

b. Capital cost: Guthrie’s modular method was applied (Biegler, Kalil, S. J., Maugeri, F., & Rodrigues, M. I. (2000). Response surface analysis and simu-

Grossmann, & Westerberg, 1997). The investment cost for con- lation as a tool for bioprocess design and optimization. Process Biochemistry, 35,

ventional distillation is the total cost of the column and auxiliary 539–550.

Kiss, A. A. & Rewarad, R. R. Energy efﬁcient control of a BTX dividing-wall column.

equipment, such as reboiler and condenser. For the DWC it

Computers and Chemical Engineering, doi:10.1016/j.compchemeng.2011.03.024,

included the additional dividing wall cost. In this study, for cost in press.

updating, the Chemical Engineering Plant Cost Index of 575.4 Kiss, A. A., & Bildea, C. S. (2011). A control perspective on process intensiﬁcation in

dividing-wall columns. Chemical Engineering and Processing, 50(3), 281–292.

was used.

Lai, L. S. T., Pan, C. C., & Tzeng, B. K. (2003). The inﬂuence of medium design on

lovastatin production and pellet formation with a high-producing mutant of

Updated bare module cost (BMC) = UF × BC × (MPF + MF − 1)(3)

Aspergillus terreus in submerged cultures. Process Biochemistry, 38, 1317–1326.

Lee, S. H., Shamsuzzoha, M., Han, M., Kim, Y. H., & Lee, M. Y. (2011). Study of structural

where UF is the update factor:

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present cost index ment. Korean Journal of Chemical Engineering, 28, 348–356.

UF = (4) Long, N. V. D., Lee, S. H., & Lee, M. Y. (2010). Design and optimization of a dividing wall

base cost index column for debottlenecking of the acetic acid puriﬁcation. Chemical Engineering

BC is bare cost and Processing, 49(8), 825–835.

Mannan, S., Fakhru’l-Razi, A., & Alam, M. Z. (2007). Optimization of process param-

L ˛ D ˇ eters for the bioconversion of activated sludge by Penicillium corylophilum,

For vessels : BC = BC0 × × (5) using response surface methodology. Journal of Environmental Sciences, 19,

L0 D0 23–28.

S ˛ Poth, N., Brusis, D., & Stichlmair, J. (2004). Minimaler energiebedarf von trennwand-

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Q 47–60.

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UT Rong, B. G., Kraslawski, A., & Turunen, I. (2003). Synthesis of heat-integrated ther-

mally coupled distillation systems for multicomponent separations. Industrial &

where MPF is the material and pressure factor; MF is the module Engineering Chemistry Research, 42(19), 4329–4339.

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and S are diameter, length and area, respectively. neous thermal coupling and heat integration. Industrial & Engineering Chemistry

Research, 45(11), 3830–3842.

c. Operating cost (Op): Segovia-Hernández, J. G., Hernández-Vargasa, E. A., & Márquez-Muñoz, J. A. (2007).

Control properties of thermally coupled distillation sequences for different oper-

Op = Csteam + CCW (8) ating conditions. Computers and Chemical Engineering, 31(7), 867–874.

Segovia-Hernández, J. G., Hernández, S., & Jiménez, A. (2005). Analysis of dynamic

where Cstream is the cost of steam @ 150 psig (11.36 bar): properties of alternative sequences to the Petlyuk column. Computers and Chem-

880 USD/KW year (Biegler et al., 1997) and CCW is the cost of ical Engineering, 29(6), 1389–1399.

cooling water: 90 USD/KW year Sinnott, R. K. (2005). Chemical engineering design (4th edition). Coulson & Richardson’s

Chemical Engineering Series Oxford: Elsevier Butterworth Heinemann.

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(1 + i) − 1 Tamayo-Galván, V. E., Segovia-Hernández, J. G., Hernández, S., Cabrera-Ruiz, J., &

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where i is the fractional interest rate per year and n is the number plex column arrangements with thermal coupling for the separation of ternary

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