RESEARCH NOTE pubs.acs.

org/IECR

Heuristic Design of Reaction/Separation Processes with Two Recycles

William L. Luyben*
Department of Chemical Engineering, Lehigh University, Bethlehem, Pennsylvania 18015, United States ABSTRACT: A recent paper presented a heuristic approach to quickly estimate the optimum tradeo between reactor size and recycle ow rate during the preliminary conceptual process design of a reaction/separation process. The basic idea is to nd the minimum recycle ow rate by designing the process to meet some specied conversion/yield/selectivity criterion, using a very large reactor. A heuristic of setting the actual recycle ow rate equal to 1.2 times the minimum then is used to obtain an approximate optimum design. The process studied had relative volatilities such that only one recycle stream was needed. The purpose of this paper is to extend this work to the case where two recycle streams are required. There is a reactor and three distillation columns with two recycle streams. The desired product C is produced via the reaction A B f C. An undesired product D is also produced. Two alternative reactions (A C f D or A B f D) mean that there is a large recycle of either B or A to achieve high selectivity. The relative volatilities are assumed to be RA > RC > RB > RD, so reactant A is recycled from the overhead of the rst distillation column and reactant B is recycled from the overhead of the third column. Product C is the distillate of the second column, and product D is the bottoms of the third column. Results show that the more-complex separation section shifts the economics to favor a smaller heuristic ratio (1.05) of actual recycle to minimum recycle.

1. INTRODUCTION Heuristics are very useful at the conceptual design stage of process development, where the precision of a rigorous optimization method is not required. Common heuristics in distillation design are to set the actual number of trays equal to twice the minimum number of trays or to set the actual reux ratio equal to 1.2 times the minimum reux ratio. Other examples of important chemical engineering heuristics include selecting pressure drops over heat exchangers to achieve reasonable heat-transfer coecients, selecting pressure drops over control valves to achieve dynamic rangeability, and choosing reasonable heat-transfer coecients and temperature dierential driving forces to nd the area of heat exchangers. A recent paper1 suggested a new heuristic for establishing the optimum design of a reactor/separation process with recycle. There is a tradeo between the size of the reactor and the amount of recycle required to achieve a specied design criterion, such as conversion, yield, or selectivity in the overall process. Major capital and operating costs are often in the separation section, but the performance of the reaction section is usually critical because of the dominant economic eect of raw material costs and product values. The intent of the proposed heuristic is to provide some guidance for initial owsheet development at the conceptual process design stage. In the original paper, the process consisted of a reactor and two distillation columns. The relative volatilities were such that a single recycle stream was required. The heuristic developed proposed setting the actual recycle ow rate at 1.2 times the minimum recycle ow rate as determined by designing with a very large reactor. The purpose of this paper is to extend this work to consider a more complex separation section in which two recycles are required. Since the separation section is more complex and therefore more expensive, we expect the heuristic ratio of actual-to-minimum recycle ow rates to be smaller, which is indeed what the results of this paper show. There is no claim that this approach is applicable to all chemical kinetic reactions and reactor/separator systems. Although recycles
r 2011 American Chemical Society

are very commonly used to aect selectivity, which is the situation in this study, recycles are sometimes used for other purposes. For example, a recycle stream is used in some adiabatic reactors to moderate the temperature change through the reactor. The recycle serves as a thermal sink whose sensible heat absorbs some of the heat of reaction. This technique is applied with both exothermic and endothermic reactions. Another application of recycle is to maintain the composition of one of the reactants below some hazardous level. Oxidation reactions often require operation below a lower explosive limit, so a recycle stream is used to keep the concentration of oxygen well below this limit. However, the use of recycle to aect selectivity is very common in industrial application, so we may expect that the proposed methodology should be widely applicable. A continuous stirred tank reactor (CSTR) has been used in this study, but the same situation occurs in tubular reactors since what aects selectivity is the ratios of reactants, and these ratios impact recycle ow rates. However, we oer no rigorous mathematical proof that a limiting recycle ow rate exists for all reactor types and chemical kinetics.

2. PROCESS STUDIED Figure 1 shows the owsheet of the process considered in this paper with the more-complex separation section. The relative volatilities among the reactants A and B and the products C and D are RA > RC > RB > RD. Two fresh feed streams and two recycle streams are fed into a CSTR reactor. The reactor euent is fed to a distillation column in which the light reactant A goes overhead and is recycled back to the reactor. The second column produces product C at the top. The third column produces a distillate of mostly reactant B, which is recycled back to the reactor. Product D is the bottoms of the third column.
Received: September 14, 2010 Accepted: March 11, 2011 Revised: February 15, 2011 Published: March 22, 2011
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Figure 1. Two-recycle owsheet; Case 1 (k1 = 25 h1, selectivity = 100, $10/kg, R = 2).

Two cases are explored. In the rst, the undesired product consumes C and A, which leads to a large recycle of B and only a small recycle of A. In the second case, the undesired product consumes C and B, which leads to a large recycle of A and only a small recycle of B. The equipment sizes and conditions shown are the economic optimum for the rst case that are developed later in this paper for the base-case conditions: a selectivity specication of 100 (kmol C produced divided by kmol D produced), kinetic parameters of k1 = 25 h1 and k2 = 1 h1, relative volatilities between adjacent components of 2, and catalyst price of $10 per kg. 2.1. Reactor. The molar holdup of the CSTR reactor is 90 kmol. Two irreversible reactions occur with specific reaction rates k1 and k2: AB f C R 1 VR k1 zA zB 1

excess of B, and the concentrations of B and C must be kept small in Case 2 to achieve the desired selectivity by operating with an excess of A. Two fresh feed streams of pure A and pure B are fed to the reactor (F A0 and F B0 ), in addition to the two recycle streams from the top of the rst column (D 1 ) and from the top of the third column (D 3 ). Note that, in Case 1, D 1 is small, compared to D 3 because of the excess of component B in the reactor. Selectivity is dened as the number of moles of the desired component C produced divided by the number of moles of the undesired component D produced: selectivity number of moles of C D2 xD2 C number of moles of D B3 xB 3 D 3

Case 1: Reactant A and desired product C are consumed in an undesired reaction: AC f D R 2 VR k2 zA zC 2A

Case 2: Reactants B and desired product C are consumed in an undesired reaction: BC f D R 2 VR k2 zB zC 2B

where zj denotes the mole fraction component j in the reactor and VR is the reactor molar holdup. The desired product C is formed by the rst reaction, but it can react further to produce an undesired product D. Therefore, the concentrations of A and C must be kept small in Case 1 to achieve the desired selectivity by operating with an

where D2 is the distillate from the second column, xD2C the mole fraction of desired component C in the distillate, B3 the bottoms from the third column, and xB3D is the mole fraction of the undesired product in the bottoms. It is important to note that the design criterion selected in this study is selectivity, not conversion. Selectivity is the important performance measure in processes with desirable and undesirable products, such as those considered in this work. The high overall conversions of the reactants in the process are inherently set by the losses of the reactants in the two product streams, which are set by the specied impurity levels. Low concentrations of reactant components A and B appear in the distillate product stream from the second column, and a low concentration of reactant B appears in the bottoms product stream from the third column. These specied compositions determine the conversions of reactants A and B for the overall process. The per-pass conversion of A in Case 1 is fairly high, while the perpass conversion of B is quite small. The reverse is true in Case 2. The fresh feed of reactant A is xed at FA0 = 100 kmol/h in all cases. The fresh feed of B is calculated for each case by solving the
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Industrial & Engineering Chemistry Research 17 nonlinear simultaneous algebraic equations that describe the reactor and the three columns for the specied conditions (reactor size, desired selectivity, and kinetic parameters). The equations that describe the reactor are FA0 D1 xD1 A F1 zA R 1 R 2 FB0 D3 xD3 B F1 zB R 1 D1 xD1 C D3 xD3 C F1 zC R 1 R 2 D3 xD3 D F1 1 zA zB zC R 2 4 5 6 7

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The number of trays then is set at twice the minimum, and the required reux ratio is set at a factor of 1.1 times greater than the minimum to estimate the capital costs (column shell, condenser, and reboiler) and the energy cost (reboiler heat input at $7.78 per GJ). Standard column sizing and cost relationships are used.2,3 The capital cost of the column is based on the size of the vessel, getting the height from the number of theoretical trays with a 2-ft tray spacing and the diameter from Aspens Tray Sizing option. The equations describing the rst distillation column C1 are given below. F1 D1 B1 9 10 11 12

The composition of C in the D1 recycle is assumed to be xD1C = 0.001, which results in the composition of A being given as xD1A = 0.999, since we assume none of B or D goes overhead. The composition of D in the D3 recycle is assumed to be xD3D = 0.001. The six specied variables are FA0, VR, xD1C, xD3D, k1, and k2. The nine unknown variables in these four equations are FB0, zA, zB, zC, D1, D3, xD3C, xD3B, and F1. Note that the reactions are nonequimolar, so there is a reduction in the molar ows into and out of the reactor. Each reaction consumes two moles of reactants while making one mole of product. 2.2. Column C1. The reactor effluent is fed to a distillation column whose job is to recycle unreacted A back to the reactor and send a mixture of reactant B and products C and D downstream to the second distillation column. Constant relative volatilities are assumed with reactant A being the lightest, reactant C being the next lightest, product B being the next lightest, and product D being the heaviest component. RA > RC > RB > RD 8

F1 zA D1 xD1 A B1 xB1 A F 1 z B B1 xB 1 B F1 zC D1 xD1 C B1 xB1 C

With these phase equilibria relationships, the separation section must have two recycles. The sizing and cost analysis for each column uses the Fenske equation to determine the minimum number of trays and the Underwood equations to determine the minimum reux ratio. The separation in column C1 is between components A and C. All of components B and D are assumed to exit in the bottoms. The impurity of A in the bottoms is set at xB1A = 0.001.

The additional 3 unknown variables not in the previous list of 9 are B1, xB1B, and xB1C, bringing the total unknows to 12. Note that the variable xB1D can be calculated if the other 3 mole fractions are known (xB1A, xB1B, and xB1C). 2.3. Column C2. The bottoms B1 is fed to the second column whose job is to remove the desired product C overhead. The small amount of A that drops out the bottom of the first column also goes overhead. The separation in column C2 is between components C and B. All of component D is assumed to go out the bottom. The impurity of C in the bottoms is set at xB2C = 0.001. The impurity of B in the distillate is set at xD2B = 0.001. The equations describing the second distillation column C2 are given below. B1 D2 B2 B1 xB1 A D2 xD2 A 13 14

Figure 2. Eect of k1 and reactor size on recycle D1: Case 1.

Figure 3. Eect of k1 and reactor size on total recycles D1 and D3: Case 1.
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Industrial & Engineering Chemistry Research B1 xB1 B B2 xB2 B B1 xB1 C D2 xD2 C B2 xB2 C 15 16

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The additional 4 unknown variables not in the previous list of 12 are D2, B2, xD2A, and xB2B, bringing the total to 16. Note that xD2C can be calculated from eq 17. xD2 C 1 xD2 A xD2 B 17

from the bottom. The small amount of C that drops out the bottom of the second column also goes overhead. The separation in column C3 is between components B and D. The impurity of B in the bottoms is set at xB3B = 0.001. The impurity of D in the distillate is set at xD3D = 0.001. The equations that describe the third distillation column (column C3) are given below. B2 D3 B3 B2 xB2 B D3 xD3 B B3 xB3 B B2 xB 2 C D 3 xD 3 C 18 19 20

2.4. Column C3. The bottoms B2 is fed into the third column, whose job is to recycle B from the top and produce product D

Figure 4. Eect of k1 and reactor size on B1 and D3: Case 1.

Figure 5. Eect of k1 and reactor size on reactor composition: Case 1.

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Industrial & Engineering Chemistry Research The additional unknown variable that was not in the previous lists is B3, which brings the nal total number of unknown variables to 17. Note that xD3C can be calculated from eq 21. xD3 C 1 xD3 B xD3 D 21

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There are a total of 17 unknowns, so we need 17 equations. Equations 47, 916, and 1821 give a total of 16 equations that describe the system. We need one more equation. The nal equation is provided by using the denition of selectivity given in eq 3. The resulting 17 equations are solved using the Matlab function fsolve for a given case of specied reactor size (VR), specic reaction rates (k1 and k2), and selectivity.

3. RESULTS
3.1. Case 1 (A C f D). Figure 2 shows results from these calculations for the case in which reactant A is consumed in the undesired reaction. In all of the cases shown in this paper, the selectivity is set at 100. Results for three different kinetic parameters are shown: k1 = 15, 25, and 50 h1. The value of k2 is 1 in all cases. The ordinate is the flow rate of recycle D1 from the first column. The abscissa is the reactor molar holdup. Figure 3 shows the sum of the two recycles D1 and D3. Since a large excess of B must be used in the reactor, the D3 recycle from the top of the third column is much larger than the D1 recycle from the top of the first column. More recycle is needed to achieve a specied selectivity for a xed reactor size as the specic reaction rate k1 is reduced. Small values of k1 lead to larger concentrations of A in the reactor (zA) but smaller concentrations of C (zC) and D (zD). The key feature of these plots (and the basis for the heuristic proposed) is that the required recycle ow rate level out at

some minimum value as the reactor size is made very large. We dene the asymptotic recycle ow rate as the minimum recycle. It can be expressed as a ratio to the fresh feed of A to put it in dimensionless form. For example, for the k1 = 25 h1 case, the minimum total recycle is 409 kmol/h for a fresh feed of FA0 = 100 kmol/h. Thus, the minimum recycle ratio (Rmin) is 4.09. Figure 4 shows how the ow rate of the bottoms from the rst column B1 and the D3 recycle change as reactor size is varied. Somewhat unexpectedly, the ow rates of the bottoms of all three columns and the distillates from the second and third column change very little with reactor size. The only ow rate that really changes signicantly is the distillate of the rst column, as shown in Figure 2. These other ow rates are strong functions of the reaction rate k1, but change little with reactor size. Figure 5 shows how reactor compositions change. Notice that the reactor compositions all level out as the reactor size is increased. The largest changes are in the composition reactant A (zA), which decreases as reactor size increases while the other three composition increase. Reactor composition zA decreases as specic reaction rate k1 increases, while zC and zD increase, since the desired reaction is more favorable. The curves shown in Figures 2 and 3 are similar to those seen in the classical plots of reux ratio versus trays in distillation design. At any point on the curve, the products from the process are exactly the same, but equipment (reactor and columns) and energy (reboiler heat inputs) are dierent. So where is the optimum point on the curve? We address this question next for several dierent cases to determine if there is some simple relationship between the economic optimum recycle ow rates and the minimum. The minimum recycle ow rates can be easily determined by running a case with a very large reactor. 3.2. Case 2 (B C f D). Figure 6 gives results for the case in which reactant B is consumed in the undesired reaction. A

Figure 6. Eect of k1 and reactor size on recycles: Case 2.

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Industrial & Engineering Chemistry Research Table 1A. Sizing and Economics Results for the k1 = 15 h1 Case
parameter VR recycle D1 recycle D3 reactor catalyst value VR 140 kmol 45.3 kmol/h 661.1 kmol/h $0.1499 106 $0.5000 106 value parameter total trays reux ratio column vessel heat exchangers reboiler duty energy 32 8.210 $0.4908 10
6 6

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Table 1B. Sizing and Economics Results for k1 = 25 h1 Case

parameter value 90 kmol 30.12 kmol/h 396.5 kmol/h $0.1134 106 $0.3214 106 value parameter column C1 33 38 3.112 m 5.511 $0.8486 106 $0.5625 10 4.120 MW
6 6

recycle D1 recycle D3 reactor catalyst

column C2 18

column C3

column C1 38

column C2 18

column C3 total trays column diameter 1.794 m reux ratio 8.967 column vessel
6 6

column diameter 2.114 m

3.746 m 8.434 $1.034 10

6 6

2.928 m 0.2098 $0.4368 10 $0.6508 10 5.163 MW

2.495 m 0.4648 $0.3683 106 $0.5286 106 3.750 MW

$0.4245 106 $0.3442 10 1.938 MW

heat exchangers reboiler duty energy

$0.4263 10 2.693 MW

$0.7158 10 5.978 MW

$0.4754 106/yr $1.022 106/yr $0.9200 106/yr

$0.6608 106/yr $1.467 106/yr $1.267 106/yr Total Capital = $3.512 106 Total Energy = $2.408 106/yr TAC = $3.578 106/yr

Total Capital = $4.404 106 Total Energy = $3.394 106/yr TAC = $4.862 106/yr

Table 1C. Sizing and Economics Results for the k1 = 50 h1 Case

parameter VR recycle D1 recycle D3 reactor catalyst value 60 kmol 16.05 kmol/h 198.2 kmol/h $0.08846 106 $0.2143 106 value parameter total trays reux ratio column vessel heat exchangers reboiler duty energy 35 11.86 $0.3600 106 $0.2698 106 column C1 38 2.531 m 3.308 $0.6809 106 $0.4300 106 column C2 18 1.918 m 0.7321 $0.2783 106 $0.3766 106 column C3

column diameter 1.487 m

annual cost of energy and capital. Therefore, most chemical process are designed for very high yields (99%) and selectivities (100). The precise best values for these criteria are strongly dependent on market prices for raw materials and nished products. Both are dicult to estimate with any precision. In order to avoid these uncertainties, we take the approach that the designer will specify a reasonable criterion, such as a selectivity of 100. A plant then can be designed that meets this criterion with the minimum total annual cost (TAC). Pricing of feed streams and products is avoided. TAC is the sum of the energy cost plus the annual cost of the capital investment using a payback period. In this work, a payback period of 3 years and the installed cost of equipment are used. capital installed investment payback period

1.330 MW 2.730 MW 2.216 MW $0.3270 106/yr $0.6697 106/yr $0.5437 106/yr

TAC energy cost

22

Total Capital = $2.698 106 Total Energy = $1.540 106/yr TAC = $2.440 106/yr

large excess of A is required in the reactor to achieve the specified selectivity of 100. Therefore, the recycle D1 (from the top of the first column) is much larger than the D 3 recycle (from the top of the third column).

4. ECONOMIC OPTIMIZATION The annual cost of raw materials and the annual value of products are typically orders-of-magnitude larger than the

For the owsheet considered in Figure 1, the reactor and all three columns change from case to case for a specied selectivity. Capital investment is required for the reactor vessel, catalyst, column vessels, reboilers and condensers. The energy cost depends on the reboiler duties. Tables 1A, 1B and 1C give sizing and cost results for Case 1 with three values of k1 . Tables 2A, 2B, and 2C give results for Case 2. The selectivity is 100, the cost of catalyst is $10 per kg, and the relative volatility between all adjacent components is 2. The reactor size is varied over a range until the reactor that minimized the TAC is found.
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Industrial & Engineering Chemistry Research Table 2A. Sizing and Economics Results for the k1 = 15 h1 Case; B C = D
parameter VR recycle D1 recycle D3 reactor catalyst value 190 kmol 671.1 kmol/h 33.83 kmol/h $0.1813 10
6

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Table 2B. Sizing and Economics Results for the k1 = 25 h1 Case; B C = D

parameter VR recycle D1 recycle D3 reactor catalyst value 125 kmol 401.5 kmol/h 21.76 kmol/h $0.1397 106 $0.4465 106 value

$0.6786 106 value

parameter

column C1

column C2 38 1.925 m 1.466 $0.5077 106 $0.3012 106 1.578 MW

column C3 18 0.8635 m 1.056 $0.1189 106 $0.1331 106 0.4491 MW

column total trays reux ratio column vessel heat exchangers reboiler duty energy 38 1.377

C1 38

C2 18

C3

total trays 37 column diameter 4.036 m reux ratio column vessel heat exchangers reboiler duty energy 1.266 $1.100 106 $0.9881 106 9.815 MW

column diameter 3.198 m $0.8629 106 $0.7299 106 6.160 MW

1.870 m 1.329 $0.4920 106 $0.2902 106 1.490 MW

0.6998 m 1.100 $0.0950 106 $0.1012 106 0.295 MW

$2.408 106/yr $0.3871 106/yr $0.1102 106/yr

$1.511 106/yr $0.3656 106/yr $0.07238 106/yr

Total Capital = $4.088 106 Total Energy = $2.905 106/yr TAC = $4.242 106/yr

Total Capital = $3.157 106 Total Energy = $1.949 106/yr TAC = $3.002 106/yr

Table 2C. Sizing and Economics Results for the k1 = 50 h1 Case; B C = D

parameter VR recycle D1 recycle D3 reactor catalyst value 60 kmol 200.3 kmol/h 12.11 kmol/h $0.1058 106 $0.2857 106 value parameter total trays reux ratio column vessel reboiler duty energy 35 1.653 $0.6349 106 3.431 MW column C1 38 1.823 m 1.214 $0.4779 106 $0.2808 106 1.416 MW column C2 18 0.5294 m 1.160 $0.0755 106 $0.07054 106 0.168 MW column C3

column diameter 2.386 m

heat exchangers $0.4998 106

$0.8417 106/yr $0.2475 106/yr $0.04142 106/yr

Total Capital = $2.425 106 Total Energy = $1.231 106/yr TAC = $2.039 106/yr

flow rates (D1 D3) for the three values of k1 are 691 kmol/h for k1 = 15 h1, 409 kmol/h for k1 = 25 h1, and 202 kmol/h for k1 = 50 h1. The economic optimum total recycle ow rates are 706 kmol/ h for k1 = 15 h1, 426 kmol/h for k1 = 25 h1, and 214 kmol/h for k1 = 50 h1. The three optimum-to-minimum ratios are 1.02, 1.04, and 1.06. 4.2. Case 2 (B C f D). The optimum designs are indicated by stars in Figures 7 and 8. Notice that the minimum total recycle flow rates (D1 D3) for the three values of k1 are 686.4 kmol/h for k1 = 15 h1, 407.8 kmol/h for k1 = 25 h1, and 202.5 kmol/h for k1 = 50 h1. These are essentially the same minimum total recycle flow rates as found in Case 1, but now the D1 recycle is large and D3 is small, which is the reverse of Case 1. The economic optimum total recycle ow rates are 704.9 kmol/h for k1 = 15 h1, 423.3 kmol/h for k1 = 25 h1, and 216 kmol/h for k1 = 50 h1. The three optimum-to-minimum ratios are 1.03, 1.04, and 1.07. Figure 9 shows the eect that k1 and reactor size has on reactor composition (zA, zB, zC, and zD) in Case 2. The results from both cases suggest that a heuristic of 1.05 may be valid for preliminary conceptual design of systems with more-complex separation sections. The heuristic for a separation section with only one recycle is 1.2.

As expected, capital and energy costs decrease as the favorable specic reaction rate k1 increases because both the optimum reactor size and the optimum recycle ow rate decrease as k1 increases. 4.1. Case 1 (A C f D). The optimum designs are indicated by stars in Figures 2 and 3. Notice that the minimum total recycle

5. CONCLUSION The results of this study illustrate that a simple design heuristic can be used at the early stages of conceptual design to develop chemical processes with reaction and separation sections connected by a recycle stream.
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Figure 7. Eect of k1 and reactor size on reactor compositions: Case 2.

Figure 8. Eect of k1 and reactor size on total recycles: Case 2.

Figure 9. Eect of k1 and reactor size on reactor compositions; Case 2.

The economic optimum for owsheets with complex multicolumn separation sections occurs at a low ratio of actual to minimum recycle ow rates.

AUTHOR INFORMATION
Corresponding Author

*Tel.: 610-758-4256. Fax: 610-758-5057. E-mail: WLL0@Lehigh.edu.

REFERENCES
(1) Luyben, W. L. Heuristic Design of Reaction/Separation Processes. Ind. Eng. Chem. Res., 2010, 49, 1156411571. (2) Douglas, J. M. Conceptual Design of Chemical Processes; McGrawHill: New York, 1988. (3) Turton, R., Bailie, R. C., Whiting, W. B., Shaelwitz, J. A. Analysis, Synthesis and Design of Chemical Processes, 2nd Edition; Prentice Hall: Upper Saddle River, NJ, 2003.

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