Ind. Eng. Chem. Res.

1997, 36, 4291-4298 4291

SEPARATIONS

An Efficient Initialization Procedure for Simulation and

Optimization of Large Distillation Problems
Pierre Rabeau and Rafiqul Gani*
Department of Chemical Engineering, Technical University of Denmark, DK-2800 Lyngby, Denmark

Claude Leibovici
Elf Aquitaine Production, Centre Scientifique et Technique Jean Feger, 64018 Pau Cedex, France

An efficient initialization procedure for steady-state distillation simulation problems involving

a large number of components is presented. The proposed initialization procedure employs
“lumping” and “delumping” of the components present in the mixture. The problem of
initialization is then reduced to a system of component mass balance equations for each plate.
The procedure generates good initial estimates and is not time consuming. The method initially
developed for petroleum fluids has proven to be efficient also for other hydrocarbon mixtures.
This is shown with two series of examples of distillation problems, by comparison with traditional
methods of initialization. Two optimization problems solved with a “lumped” system are also
presented and compared to the optimum solution found with the original system.

Introduction additional computations which would not be feasible

Although many computational schemes have been
reported in the past, active research is still being carried
out in developing efficient methods of solution for
simulating steady-state behavior of distillation columns.
The method of solution generally requires iterative
calculations, so the computational time depends strongly
on the initial estimates of the iterative variables. The
computational time also depends on the size of the
problem. Very large problems are generated due to a
large number of components in the mixture to be
separated and/or a large number of stages. In the
petroleum industry, systems of more than 300 compo-
nents are not uncommon since the crude oil feed to the
distillation column is usually a blend of several crudes,
each represented by 50 or more real and hypothetical
components. The computational time may become
prohibitive for such problems; hence, new time-reducing
solution schemes are required.
Wayburn and Seader (1983) proposed a mathematical
model of great generality for distillation-based (inter-
linked or noninterlinked) separation processes and a
robust method of solution. While their procedure ad-
dressed the important issues of flexibility and robust-
ness, it did not address the question of computational
time for large problems. In this paper, we address
flexibility, robustness, and computational time, with
special emphasis on large distillation simulation prob-
lems. Even in design computations, which are usually
off-line, reduction in computational time can be useful
since alternatives can be explored. Also, reductions in
computational times should be machine independent.
The goal should not be to use an inefficient solution
procedure on a fast computer to obtain rapid solutions.
Faster computers and efficient machines should provide
* Author to whom all correspondence should be addressed.
S0888-5885(97)00270-4 CCC: $14.00
otherwise.
In petroleum engineering, the usual way to reduce
the size of the problem when simulating operations with
distillation is to lump the components present in the
oil mixture. Montel and Gouel (1984) proposed a
lumping scheme based on the similarities of a few
properties of all the components. An iterative clustering
algorithm around mobile centers yields a classification
into “pseudo”components optimum with respect to the
considered equation of state. Leibovici (1993) has
established a procedure for the estimation of properties
of the pseudocomponents which is accurate and com-
pletely consistent with the thermodynamic model to be
used. Even though simulations can be performed with
this reduced system of pseudocomponents in a reason-
able time, it should be noted that the results from
simulation only deal with a simplified representation
of the fluid (the system of pseudocomponents) and no
information on the original system is provided here.
Therefore, a large knowledge gap exists between the
increasing amount of analytical data provided by mod-
ern laboratory equipments and the simplified simulation
results. It is obvious that employing a detailed descrip-
tion of the mixture in process optimization or control
will lead to more accuracy and quality of the resulting
solution. However, these calculations are not done
presently since it is impossible for reasons of either
memory storage or computational time.
When a simulation of a flash operation is performed,
the detailed results can be obtained by using a “delump-
ing” procedure, i.e., generating the detailed mixture
results from the “lumped” solution. Leibovici et al.
(1996) found a new way to “delump” a system which is
completely consistent with the thermodynamic model
to be used. The procedure is based on properties of the
equilibrium constants involved in the phase equilibrium
calculation.
The new initialization procedure for steady-state
© 1997 American Chemical Society
4292 Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997

Figure 1. Distillation column configuration and an arbitrary stage in the column.

one equation per stage for energy balance:

distillation models proposed in this present paper
employs the “lumping” and “delumping” techniques (Li + SiL)hi + (Vi + SiV)Hi - Li+1hi+1 -
which lead to a linear system of algebraic equations.
Vi-1Hi-1 - Qi ) 0 (1)
Solution of this set of equations provides the initial
estimates for the actual nonlinear problem (steady-state
N equations per stage for component
distillation). Steady-state distillation problems for mix- material balance:
tures with 20 < N < 320 components have been solved
by employing this new procedure. It has been observed
that the ratio of computational time needed for initial-
ization to the computational time needed for N compo-
(
lij 1 +
SiL
Li ) (
+ vij 1 +
SiV
Vi )
- li+1,j - vi-1,j - fij ) 0 (2)

nents rigorous distillation simulation decreases as N

N equilibrium relationships per stage:
increases. Thus, while the order of reduction of com-
putational times for N ) 20 is low (around 2-3), the Vi
corresponding order of reduction for N ) 320 is 8. vij - Kij lij ) 0 (3)
Li
Various distillation problems, with and without side
products, pumparounds, and side-strippers, have been The dependent variables Li and Vi are calculated from
considered. In all cases, significant reductions in com- the summation equations:
putational times to reach the rigorous solution of the N
distillation problem have been achieved. It has been
observed that the initial estimates obtained with the
Li ) ∑
j)1
lij
new initialization procedure were almost as precise as (4)
N
the rigorous solution of the distillation problem. The
details of the new method are presented together with Vi ) ∑
j)1
vij
the solution of industrially relevant problems. The
results were obtained with the commercial simulator Naphtali and Sandholm (1971) chose the liquid and
PRO/II (1992) as well as the in-house simulator SEPSIM vapor component flowrates (lij, vij) and the temperatures
(Andersen, 1985). (Ti) for each plate as iterative variables, thereby giving
a total of 2N + 1 variables. They found that, if the
equations and variables are grouped in terms of a stage,
Model Description the Jacobian matrix in the Newton-Raphson method
for these equations has a block tridiagonal form which
greatly simplifies the solution procedure. The method
Figure 1 represents a typical equilibrium stage of a of Naphtali and Sandholm also has the advantage of
distillation column. For each stage, equilibrium condi- great flexibility because it can handle absorption and
tions between the liquid and the vapor streams leaving distillation problems without requiring any additional
the stage are assumed and the model equations are changes. Many other algorithms have been proposed.
given by They may be classified into two categories: equation

decoupling methods and simultaneous solution methods.
The θ-method (Holland, 1975), the inside-out class of
methods originated by Boston and Sullivan (1974), and
the method of Láng et al. (1991) developed especially
for crude oil distillation fall into the former category,
whereas the method of Naphtali and Sandholm, Chris-
tiansen et al. (1979), Hofeling and Seader (1978), and
Letourneau et al. (1995) when pumparounds and/or
recycles are present and Buzzi Ferraris (1983) fall into
the second category. One point to note is that the most
general initialization that can be done for distillation
problems solved with any of these methods is to provide
initial values for lij, vij, and Ti and the corresponding
Kij, Li, and Vi.
Method of Solution
Let us consider a mixture of N components. In the
lumping procedure described by Montel and Gouel
(1984), components with similar properties (Tci, Pci, mi,
and Mwi) are grouped in clusters. In this way, one can
decide to generate M clusters (M < N), also called
pseudocomponents. The critical and other physical
properties of these pseudocomponents needed for the
thermodynamic description of the phase equilibrium are
calculated with the procedure developed by Leibovici
(1993). With the reduced list of M pseudocomponents,
a simulation is performed. Then, the first assumption
is made: the total flowrates and temperature profiles
(Li, Vi, Ti) found with this simulation are fully repre-
sentative of the original problem, i.e., Li, Vi, and Ti are
supposed to be equal in the simulation of the M
pseudocomponents and of the N original components
systems. The second assumption is that the equilibrium
constants (Kij) of the N components system can be
calculated from the ones of the M pseudocomponents
system.
Michelsen (1986) presented an efficient flash proce-
dure for systems described by cubic equations of state
with all binary interaction coefficients equal to zero. On
the basis of this simplification, Leibovici et al. (1996)
showed that the equilibrium constants lie on a geo-
metrical locus when the mixture parameters of an
equation of state can be expressed as a linear combina-
tion of pure-component parameters and molar composi-
tions. For example, for a system described by a two-
parameter cubic equation of state, the locus has the
following expression:
ln Ki ) ∆C0 + ∆C1xai + ∆C2bi (5)
where ai and bi are the equation of state pure-
component parameters.
Therefore, knowing the ∆C coefficients, the K-factors
for the original N components mixture can be deter-
mined by extrapolation and/or interpolation and use of
the temperature profile in the evaluation of ai. This
procedure, which is detailed in the appendix, was used
for the second assumption.
At this stage of the procedure, one knows the K-
factors and the internal and external total flowrates for
the original N components mixture without any time-
consuming calculations. If the K-factors are introduced
in the mass balance equations (2) through their defini-
tion in eq 3, the following equation is obtained:
Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997 4293
(
- Ki-1,j
Vi-1
Li-1) [
li-1,j + 1 +
SiL
Li
+ 1+
SiV
Vi ( Vi
) ]
Kij lij -
Li
li+1,j - fij ) 0 (6)
Since the feed (fij) and side stream flowrates (SiV, SiL)
are given in the problem definition, the problem consists
of solving for each component a linear system of p
algebraic equations in the liquid component flowrates
lij. Then, verification of the solution obtained is made.
The physical constraint concerning the positiveness of
the component flowrates is checked
lij g 0 ∀i,j (7)
and the values of lij are normalized with respect to the
total internal flowrates (Li) to verify
N
Li ) ∑
j)1
lij (8)
The vapor component flowrates vij are also available
directly from the equilibrium relationships (eq 3), and
the same verification as for lij is made. Now, the whole
set of variables is initialized for the rigorous solution of
the distillation problem.
Computational Procedure
A step-by-step solution technique has been defined
(Chart 1); it is given below and illustrated in Figure 2.
Chart 1. New Method of Initialization
Step 1. For the oil blend represented by N
components, use a lumping procedure to generate
M clusters (n + 1 < M , N), each representing
a subset of components and possessing a full
set of properties.
Step 2. Perform a steady-state distillation simulation with
the M clusters and save the results for Li, Vi, Ti, and Kij.
Step 3. From the Kij for the M clusters and Ti obtained in
step 2, calculate the Kij for the N components
of the original mixture (Leibovici et al., 1996).
Step 4. From the Kij calculated in step 3 and the Li and
Vi obtained in step 2, calculate lij by solving component
by component the system of linear equations (6).
Step 5. From lij, Vi, Li, and Kij obtained in steps 2-4,
calculate vij from eq 3.
Example Problems
In order to try the initialization procedure, several
test examples were used. Results from the ones which
best represent all the results and highlight the main
features of the initialization method are presented.
Although the method was initially developed for ap-
plications involving petroleum mixtures, petrochemical
mixtures have also been tested. The differences be-
tween these two types of mixtures are the number of
components present in the mixture and the continuity
of the mixture properties. A petrochemical mixture is
considered as a “discrete mixture” due to the high
discontinuity of its set of pure-component properties,
whereas a petroleum mixture is considered to be a
“continuous mixture”. Example 1 deals with a petro-
chemical mixture, and examples 2 and 3 deal with
petroleum mixtures. Then, two optimization problems
such as cost minimizations are presented, and the
optimum solutions obtained with lumped and original
systems are compared and discussed.
4294 Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997

Chart 2. Clustering Algorithm for Distillation

Step 1. From a shortcut distillation simulation (Smith, 1963)
or other existing data, determine the recovery ratio
for each component (Ri ) di/fi).
Step 2. From the values of Ri found in step 1, generate four
classes as follows:
1.00 g Ri g 0.98 w i ∈ C1

0.98 > Ri g 0.50 w i ∈ C2

0.50 > Ri > 0.02 w i ∈ C3

0.02 g Ri g 0.00 w i ∈ C4
Step 3. Identify dominant components in the feed of the
column and assign them as centers for new classes
Figure 2. Scheme of the new approach of initialization. (included in C1, C2, C3, C4).
Step 4. Assign each component to the “nearest” center
Table 1. Output Results for the Dominant Components according to a defined distance (the distance formulation
in Example 1 given by Montel and Gouel (1984) could be used
for example).
fluid rates, kmol/h
method, 23.3 s (2 iterations) was needed (note that only
feed liquid distillate vapor bottom liquid
2 s is used for the generation of the initial estimates).
n-pentane 29.58 29.58 0.00 The time reduction was then a factor of 2, which is low
2-methyl-2-butene 20.45 20.45 0.00
because the problem was not difficult to converge and
cyclopentene 28.88 28.87 0.01
cyclopentane 23.78 23.74 0.04 the conventional initial estimates were already close to
benzene 203.69 0.72 202.97 the solution. Particular attention was given here to the
toluene 64.78 0.00 64.78 quality of the initial estimates generated with the new
ethylbenzene 39.39 0.00 39.39 method or the deviation between these values and the
dicyclopentadiene 29.61 0.00 29.61 actual solution. The specifications for this simulation
others 103.32 62.11 41.20
problem were a mass percentage of benzene equal to
total rates, kmol/h 543.48 165.48 378.00 0.5% in the distillate and a reflux ratio equal to 3. The
temperature, K 314.45 345.86 405.53 bottom product flowrate found with the new initializa-
pressure, atm 1.0 2.5 2.8 tion method was 376.5 kmol/h, and it was 378 kmol/h
in the rigorous solution. The values of Li and Vi
Petrochemical Mixture. Data from a petrochemi- corresponding to simulations with the lumped system
cal plant operating in the region of Normandy (France) and the original components are available as supporting
are used in example 1. A 34-stage depentanizer column information. The average deviation for Li and Vi
operating at a pressure of 2.5 atm and having one feed between the two simulations is 1.29 kmol/h, and the
entering the column on stage 17 and two products is maximum deviation is 2.48 kmol/h. In Figure 3, the
considered (stages numbered from bottom to top of the temperature profiles corresponding to these two simula-
column). From chromatographic analysis, a 79-compo- tions are plotted, the average deviation is 0.38 K, and
nent mixture is considered as the feed of the column. the maximum deviation is 0.72 K. These comparisons
Eight components of the feed are in higher amounts; suggest that the calculations could be stopped after the
they represent 80.44% (molar basis) of the mixture. initialization proposed in this paper; i.e., consider the
Table 1 gives the steady-state condition in terms of initial estimates as the actual solution. A significant
pressure, temperature, and the component flowrates in time reduction will then be achieved; for this example
the feed, in the distillate product, and in the bottom the reduction is the ratio of the computational times for
product for the eight dominant components. The output a 79-component simulation and for a 10-component
results for a 79-component mixture are available as simulation (factor of 24 in this case). This suggestion
supporting information. requires that the guidelines of Chart 2 are automatized
The location of the clusters was imposed instead of in a way which guarantees a correct representation of
using the “automatic” dynamic clustering method of the mixture in the range of temperature and composi-
Montel and Gouel (1984) because numerical experiences tions considered in the distillation problem.
suggested special caution when applying this method Petroleum Mixture. Moderately Large Problems.
to distillation column simulation for “discrete” mixtures. A set of three cases involving columns with different
Since the mixture composition changes along the length configurations were treated in example 2. In each case,
of the column, lumping two key components together, a 20-tray column was considered; 132 components were
for example, will result in incorrect predictions. Thus, involved in examples 2a and 2c and 172 components in
from various experiments and engineering insights, a example 2b; no side products were withdrawn in ex-
step by step procedure for choosing the location of the amples 2a and 2b, whereas two side products were
clusters (Chart 2) was defined, used, and is recom- withdrawn in example 2c; in each example 39 clusters
mended. Following this procedure, 10 clusters were were considered in the lumping procedure (Montel and
made. The properties for each cluster were predicted Gouel, 1984). Table 2 gives the number of iterations
by the method of Leibovici (1993). and computational times for each example. These
Simulations were performed with the rigorous distil- results are presented for four simulation modes: SIM
lation algorithm of SEPSIM, which is a simultaneous A, the “normal” distillation simulation (conventional
solution method. With the conventional initial esti- initialization) with N components; SIM B, simulation
mates generated in this program, the computational with M clusters; SIM C, simulation with N components
time (IBM RS/6000) needed to reach the solution was and initial estimates (coming from SIM B) for Li, Vi, and
47.7 s (4 iterations), whereas with the new initialization Ti; SIM D, simulation with N components and initial
 Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997 4295

Figure 3. Temperature profiles for example 1.

Table 2. Computational Times and Number of Iterations

for Examples 2a-c
simulation mode
SIM A SIM B SIM C SIM D
simulator iter. timea iter. time iter. time iter. time
Example 2a
SEPSIM CMO 9 121 10 4 NA NA 3 44
SEPSIM RIG 6 372 7 14 3 127 2 85
Example 2b Figure 4. Crude oil unit of example 3.
SEPSIM CMO 11 638 10 4 NA NA 3 180
SEPSIM RIG 6 2042 6 13 3 727 2 471 For all the examples of this Petroleum Mixture
Example 2c
section, comparisons of the variables (lij, vij, Ti) between
SEPSIM CMO 12 167 12 5 NA NA 4 59 the actual solution of the problem and the initial
SEPSIM RIG 5 382 6 13 2 90 2 90 estimates calculated with the new method showed an
a
average relative deviation of between 0.5 and 1.5% and
Simulations were run under UNIX system on an IBM RS/6000.
a maximum relative deviation between 3 and 5%.
Therefore, the option to take the initial estimates as the
estimates for lij, vij, Ti, Li, and Vi generated with the actual solution of the problem appears again to be a
new initialization method. With the rigorous distilla- promising alternative. Their use in optimization/control
tion simulation option of SEPSIM (referred to here as studies is highly recommended by this paper, since these
SEPSIM RIG), the computational time reduction by results (estimates of lij, vij, Ti, Li, Vi and Kij) are obtained
applying the new method of initialization varied from without much computational effort (in example 2c for
3.7 to 4.2. With the “constant molar overflow” version instance, 13 s is necessary to calculate the initial
of the distillation algorithm of SEPSIM (SEPSIM CMO), estimates which differ by 0.5% from the rigorous solu-
the computational time reduction varied from 2.5 to 3.5. tion which was found in 382 s; the corresponding time
The same problems were also solved with PRO/II (1992) reduction is a factor of 29.38). This example shows that
(using SURE algorithm), and good improvements (be- the initialization procedure could also be used as a first
tween factors of 2 and 4) were also obtained. estimate in design-related computations. It should be
Very Large Problem Example. A special version of the noted, however, that for detailed design a final rigorous
“inside-out” column (Leibovici, 1996) able to use the simulation would be needed. Since “good” initial esti-
complete set of initial guesses for all iterative variables mates would be available, this step would be performed
has been used for the simulation of example 3 dealing at significantly reduced computational time.
with a mixture of five crude oils represented by a total Finally, we have seen that the initialization method
of 327 components (7 pure components + 320 petroleum is valid and efficient for both equation decoupling
cuts). As shown in Figure 4, a typical crude unit methods and simultaneous solution methods.
operating at atmospheric pressure, having the crude oil Optimization. The solutions of two cost minimiza-
feed and a bottom feed of steam and involving three side tion problems are reported in this section. The empha-
strippers (each with a bottom feed of steam) and three sis is given on the computational aspects of the problem
recycling pumps, was considered. In the lumping and not the actual operating cost.
procedure, the seven pure components were unchanged In both problems, a petrochemical mixture repre-
and the 320 petroleum cuts were lumped into 30 sented by 20 hydrocarbons (from C1 to C10) is considered.
pseudocomponents using the dynamic clustering method A 25-stage debutanizer column operating at a pressure
of Montel and Gouel (1984). Decant water was treated of 15 atm and having one feed entering the column on
as a third pure liquid phase in the calculations. By stage 20 is considered (stages numbered from bottom
applying the new initialization procedure, the total to top of the column). Table 3 gives the steady-state
computational time to reach the rigorous distillation condition in terms of pressure, temperature, enthalpy,
solution was reduced by a factor of 8 for this problem. molecular weight, and the component flowrates in the
The computational times for lumping and delumping feed, in the distillate product and in the bottom product
as well as for the distillation simulation of the lumped at the starting point (base case).
system of 37 components were negligible compared to The choice of the location of the clusters was done
the other computational times. “manually” by taking into account engineering insight
4296 Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997

Table 3. Output Results for the 20-Component Mixture Table 6. Results for Optimization Problems 1 and 2
Distillation (Base Case)
(a) Problem 1
fluid rates, kg‚mol/h
optimum objective function,
feed distillate bottom M‚kJ/h
computational feed tray
liquid vapor liquid
mixture time, s locationa starting final gain
1. methane 5.000 5.00 0.000
system 1 14.66 12 61.91 36.86 25.05
2. ethane 10.000 9.999 0.001
system 2 20.76 12 66.43 39.46 26.97
3. ethylene 40.000 39.999 0.001
original 135.00 12 67.13 39.29 27.84
4. propane 50.000 49.863 0.137
5. butane 260.000 238.257 21.743 (b) Problem 2
6. isobutane 250.000 241.170 8.830
7. pentane 140.000 8.018 131.982 compu- optimum optimum objective function,
8. isopentane 100.000 27.624 72.376 tational tray feed M‚kJ/h
9. hexane 100.000 0.000 100.000 mixture time, s location temperature starting final gain
10. heptane 80.000 0.000 80.000
11. octane 30.000 0.000 30.000 system 1 22.08 12 399.92 104.02 51.84 52.18
12. nonane 20.000 0.000 20.000 system 2 25.32 13 402.44 113.14 57.34 55.80
13. decane 5.000 0.000 5.000 original 161.00 12 399.40 115.27 57.99 57.28
14. 2,2-dimethylbutane 20.000 0.004 19.996 a Rounded numbers.
15. 3-methylpentane 30.000 0.000 30.000
16. cyclopentane 30.000 0.065 29.935
17. cyclohexane 20.000 0.000 20.000 In both problems considered here, small differences
18. methylcyclopentane 30.000 0.000 30.000 were noticed between the results obtained with the
19. cycloheptane 20.000 0.000 20.000 original and the lumped systems. The results are nearly
20. methylcyclohexane 20.000 0.000 20.000 fully reproduced when working with the lumped sys-
total rate, kg‚mol/h 1260.000 620.000 640.000 tems. This shows the benefit of also using the initial-
temperature, K 375.00 361.64 447.42 ization procedure in optimization. Although the two
pressure, atm 15.00 15.00 15.00 examples chosen are simple, much more complex con-
enthalpy, M‚kJ/h 21.49 16.67 23.79 figurations involving separation processes with inter-
molecular weight 70.28 55.07 85.01
linked columns can be considered. In that case, several
Table 4. Components Present in Each Cluster for lumped systems at different points of the flowsheet may
Systems 1 and 2 be necessary. This should not introduce any new
clusters components present in the cluster computationally expensive steps to the method of solu-
tion.
system 1 system 2 system 1 system 2
1 1 1-4 1-4
2 2 5 and 6 5 Conclusions
3 3 7 and 8 6
4 4 9-20 7 A rapid and safe procedure for initialization of steady-
5 8 state distillation calculations has been developed. The
6 9-20 procedure is particularly attractive for cases where the
Table 5. Details of the Cost Minimization Problems
mixture properties can be considered to be “continuous”.
The computational times needed to converge the rigor-
problem 1 2 ous distillation model for the full system can be reduced
objective function f ) Qreb f ) |Qreb| + |Qcond| by up to a factor of 8 through the initialization proce-
design variables 1 < FTRA < 25 1 < FTRA < 25 dure. Note that the corresponding reduction of the
350 < T(feed) < 450
absolute computational time (which is very high for
specifications (1) recovery of iC4 + nC4 in the bottom ) 2%
of the column (2) recovery of iC5 + nC5 in the top ) 2% these problems) is of greatest interest. Furthermore,
since the estimated values obtained with the initializa-
and the guidelines given in Chart 2. Two lumped tion procedure are very close to the actual solution, they
systems (systems 1 and 2) were considered because the can be used, in many cases, directly as the actual
specifications of the debutanizer given in the calcula- solution, thereby leading to much higher time reduc-
tions were directly related to the key components. The tions. It has been shown that the method is also
compositions of the clusters of systems 1 and 2 are applicable to smaller discrete mixtures, such as the ones
shown in Table 4. found in the petrochemical industry, but with special
For this problem, the initialization method is applied care (engineering insights related to distillation) when
in the following way: the optimization problem is solved choosing the clusters. The computational time reduc-
with the lumped system and then the optimal solution tion can be very profitable for optimization studies. The
is delumped, producing the required initialization for results show the future potential of the initialization
the final rigorous distillation. In the first optimization method in terms of design, simulation, and optimization
problem, the optimum feed tray location is investigated of complex flowsheets involving several distillation
in order to minimize the operating costs; the objective columns and recycles. It should be noted that, even
function solely depends on the reboiler heat duty. In though computation examples for simulation involves
the second optimization problem, the optimum feed tray only a simple column, the advantage of using the
location and temperature are investigated in order to proposed initialization procedure should be obvious
minimize the operating costs; the objective function when such columns are part of a flowsheet with recycle
depends on the reboiler and condenser heat duty. The loops. Also, the method is independent of computer
details of the problems are shown in Table 5 and the hardware. That is, there will be significant savings in
results in Table 6. These problems were treated with all computers. Also, the examples have shown that the
the simulator PRO/II (CHEMDIST algorithm for the results can be used for initial design and as initial
distillation columns simulations). estimates for final design. Current and future work will
 Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997 4297
address the computational aspects related to optimiza- n
tion of flowsheets with distillation trains and recycles. ln Φi ) C0 + ∑ Ckpi,k
k)1
(A1)

Acknowledgment
The authors gratefully acknowledge Elf Aquitaine
Production for providing financial support for this
project and the Engineering Research Center: Phase
equilibria and Separation Processes (IVC-SEP) of the
Chemical Engineering Department of the Technical
University of Denmark. We are also thankful to Elf
Atochem for providing petrochemical plant data.
provided that the mixture parameters [or any of their
power transforms] can be expressed as linear combina-
tions of the pure-component parameters, the weighting
factors being the component mole fractions (∀k, pk )
∑xipi,k). For example, with the two-parameter SRK
equation of state (Soave, 1972) the values of pi,1 and pi,2
are (ai)1/2 and bi when kij ) 0 (conditions for the linear
combination). At equilibrium the isofugacity criterion

Nomenclature fiL ) fiV (A2)

a, b ) mixture parameters in eq A4
ai, bi ) pure-component parameters in the equation of state has to be fulfilled for all components, and the logarithm
B ) bottom products flowrate of equilibrium constant can therefore be written as
C1, C2, C3, C4 ) first four classes used for proposed
n
clustering
di ) flowrate of component i in distillate ln(Ki) ) ∆C0 + ∑ ∆Ckpi,k
k)1
(A3)
f ) objective function in Table 5
fij ) molar feed flowrate of component j on plate i
Fi ) total molar feed flowrate to plate i where ∆Ck ) CkL - CkV. This relation shows that, in
FTRA ) feed tray location the case where no binary interaction coefficients (kij) are
hi ) liquid molar enthalpy on plate i used to represent the mixture, the coefficients ∆Ck are
Hi ) vapor molar enthalpy on plate i known analytically and the K-values of all components
Kij ) equilibrium constant of component j on plate i
which were lumped together can be easily obtained from
lij ) molar liquid flow of component j on plate i
eq A3 assuming that the phase parameters have not
changed. Binary interaction coefficients kij are small,
Li ) total liquid molar flowrate on plate i
typically zero for hydrocarbon-hydrocarbon interactions
M ) number of pseudocomponents
and in the range 0-0.15 otherwise. If they are used to
Mwi ) molecular weight of component i
describe the lumped system, then the coefficients ∆Ck
N ) number of components
can be approximated by any standard least-squares fit
n ) number of independent parameters in the equation of
method and requested K-values can be predicted from
state
eq A3. Note that in order to obtain the (n + 1)∆Ck
P ) number of plates
values the number of pseudocomponents in the lumped
Pi ) pressure on plate i
system has to be at least n + 1.
Qi ) heat flowrate to stage i
For the SRK equation of state with no binary interac-
Qreb ) reboiler heat duty
tion coefficients the analytical expressions for ∆C0, ∆C1,
Qcond ) condenser heat duty
and ∆C2 are
R ) gas constant in eq A4

( )
R ) reflux ratio
Ri ) recovery ratio vV - bV
∆C0 ) ln
Si ) side products flow from plate i vL - bL
Ti ) temperature on plate i
2xaV
( )
2xaL
( )
Tci, Pci ) critical properties of component i
bV bL
v ) molar volume in eq A4 ∆C1 ) ln 1 + V - L ln 1 + L
V
vij ) molar vapor flow of component j on plate i b RT v b RT v

( )
Vi ) total vapor molar flowrate on plate i
xiF ) molar composition of component i in the feed ZL - 1 aL bL ZV - 1
Z ) compressibility factor in eq A4 ∆C2 ) + ln 1 + - -
bL (bL)2RT vL bV
Greek Letters
ωi ) acentric factor of component i
∆C0, ∆C1, ∆C2 ) regression coefficients in eq 5
aV
V 2( )
(b ) RT
bV
ln 1 + V (A4)
v

Superscripts In practice the procedure contains the following steps:

L ) liquid phase
V ) vapor phase
Appendix
Leibovici et al. (1996) developed a method to predict
the detailed composition of the phases resulting from a
flash calculation just performed on a lumped mixture.
If one considers any equation of state P ) f(T,V)
involving n parameters, the fugacity coefficient of
component i in a mixture of N components can be
expressed simply as
Step 1. Lump a mixture of N components into M
pseudocomponents.
Step 2. Perform a flash calculation with the lumped
system in order to obtain the equilibrium constants
of the pseudocomponents.
Step 3. Determine the ∆Ck values from the lumped
system.
In the case of all kij ) 0, use eq A4.
In the case of some kij * 0, use regression (note that
the condition n + 1 e M e N has to be fulfilled).
Step 4. Calculate Ki from eq A3 for all components in
the full system.
4298 Ind. Eng. Chem. Res., Vol. 36, No. 10, 1997
This procedure will work even better if the lumping
does not affect, or only slightly affects, the phase
parameters and the phase split. If this is the case, then
the ∆Ck are the same for the lumped scheme and the
original one.
Supporting Information Available: Tables of
output results and internal flowrates for 79-component
mixture distillation (3 pages). Ordering information is
given on any current masthead page.
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Received for review April 10, 1997
Revised manuscript received July 25, 1997
Accepted July 26, 1997X
IE970270Z
X Abstract published in Advance ACS Abstracts, September
15, 1997.