Cornput. chent. Engng. Vol. 12, No. 6, pp. 531-546, 1988 0098-1354/88 93.00 +O.

OO
Printed in Gnat Britain. All rights reserved Copyright Q 1988 Pergamon Press plc

A MIXED-INTEGER NONLINEAR PROGRAMMING

FORMULATION FOR THE SYNTHESIS OF
HEAT-INTEGRATED DISTILLATION SEQUENCES

C. A. FLoUDAsj’ and G. E. PAULES IV

Department of Chemical Engineering, Princeton University, Princeton NJ 08544, U.S.A.

(Received 20 August 1987; final revision received 22 October 1987; received for publication
10 November 1987)

Abstrati-Sequences of distillation columns are widely employed in chemical plants as the main system
for the separation of various multicomponent mixtures into their components. Considerable savings in
plant operating costs can often be obtained by adjusting the operating pressures of the columns in a
separationsequenceso as to allow for heat transfer betweenthe condenserof one column and the reboiler
of another. Because of the importance of distillation sequences in the operation of the entire chemical
process and the large investment and operating costs represented by them, the synthesis of optimal
heat-integrated distillation sequences becomes an important synthesis problem.
In this paper, a systematic framework is presented for the synthesis problem of heat-integrated
distillation sequences with the column pressures treated as continuous variables for a single multi-
component feed of fixed composition. This framework consists of the mathematical formulation of the
distillation sequence superstructure as a mixed-integer nonlinear programming MINLP problem. The
mathematical formulation features as an objective function, the minimum total annual cost comprised of
investment costs for the distillation columns and heat exchangers plus the operating costs based on utility
consumption. The heat integration options are incorporated in the proposed formulation through the
assignment of integer variables representing the potential condense-&oiler matches. Solution of this
mathematical formulation, which can be obtained automatically using the computer programming
procedure APROS provides the optimal distillation sequence and heat integration matches as well as the
operating pressures required for each column. The effectiveness of this systematic framework is illustrated
with three example problems.

INTRODIJCITON (1982) developed an approach that synthesizes heat-

integrated distillation, sequences based upon a mini-
Sequences of distillation columns are probably the
mization of the loss of available energy. Linnhoff et
most widely used separation processes in chemical
al. (1983) considered the design of distillation se-
industry. Due to the significant contribution of the
quences in conjunction with the heat integration of
utilities to the venture cost of a distillation-based
the overall process, and developed insights based on
separation sequence, there is a general economic
the notion of the pinch point. Andrecovich and
incentive to synthesize sequences of distillation col-
Westerberg (1985a) developed a simple synthesis
umns that take advantage of the heat integration
method that is based upon utility bounding, as-
options.
suming that QAT, the product of the condenser or
The first systematic studies of heat-integrated dis-
reboiler heat duty and the temperature difference
tillation sequences were performed by Rathore et al.
between the reboiler and condenser, is constant for
(1974a, b), who presented an algorithm based on
each distillation column. Andrecovich and West-
dynamic programming for fixed and variable pres-
erberg (1985b) formulated the synthesis problem of
sures of the distillation columns. Sophos et al. (1978)
heat-integrated distillation sequences as a mixed-
and Morari and Faith (1980) developed branch and
integer linear programming MILP problem. This
bound approaches based upon Lagrangian theory.
formulation is based upon a superstructure that
Umeda et al. (1979) presented an evolutionary ap-
consists of distillation columns at discretized pressure
proach that utilizes heat availability diagrams to
levels. Westerberg and Andrecovich (1985) removed
improve the heat integration of a given distillation
the assumption of constancy on QAT and showed
sequence. Sophos et al. (1981) developed a two-level
that the minimum utility target can be calculated by
procedure for heat-integrated sequences and demon-
formulating it as a small linear programming prob-
strated that the heuristics of distillation sequences
lem. They also showed that even though the calcu-
without heat integration can be utilized for selecting
lated utility target may increase, the synthesized
the best candidates for heat integration. Naka et al.
sequences remain the same as the ones for constant
Q AT. Gomez-Munoz and Seader (1985) used the
thermodynamic principles oE (a) minimum reversible
tAuthor to whom all correspondence should be addressed. work of separation; and (b) seynd-law ‘analysis for
531
532 C. A. FLOUDAS and G. E. PAULES IV
irreversibility, to synthesize distillation sequences.
Isla and Cerda (1985) chose the least utility cost as
the design target and formulated the synthesis prob-
lem of heat-integrated distillation trains as a mixed-
integer programming problem that can identify the
optimal heat-integrated sequence from the utility
point of view. Meszarus and Fonyo (1986) developed
a two-level predictor-based search method that uti-
lizes the heat-cascade theory and sets lower bounds
for all feasible heat-integrated separation sequences.
They ordered the structures of distillation sequences
according to the lower bounds and optimized the heat
matches starting with the structure of the lowest
lower-bounding value. They defined as a con-
tinuously updated upper bound, the optimized total
annual cost of the best sequence and completed the
search for a better candidate at the crossing of the
lower and upper bounds.
In this paper, the synthesis problem of heat-
integrated distillation sequences that can allow for
continuous variations of the pressure of each cohunn
is addressed. A MINLP formulation is proposed that
minimizes the total annual cost of the postulated
superstructure of distillation sequences and involves
the pressure of each column as a variable. Explicit
expressions of the cost functions and heat loads as
function of pressure are determined by performing
short-cut simulation runs for each column involved in
the superstructure. The solution of the MINLP for-
mulation provides the minimum total cost heat-
integrated distillation sequence with the optimal as-
signment of pressures in each column as well as the
matches for heat exchange. The effectiveness of the
approach is demonstrated with three example prob-
lems.
PROBLEM STATEMENT
The problem to be addressed in this paper can be
stated as follows:
Given is a single multicomponent feed stream of
known conditions (i.e. composition, flowrate) that
is to be separated into its pure-component prod-
ucts using a sequence of distillation columns.
Available is also a set of hot and cold utilities at
different temperature levels. The problem is then to
synthesize the minimum total annual cost sequence
of distillation columns that are heat integrated.
The basic assumptions to be made for this syn-
thesis problem of heat-integrated distillation se-
quences are:
The thermodynamic state (e.g. saturated
liquid, saturated vapor) and pressure of the
feed stream to each column is known. In
addition, the thermodynamic state of the dis-
tillate and bottoms products are also known.
The condenser type of each column is known.
Available to each column is a set of constant
temperature hot and cold utilities. Each col-
umn may exchange heat with any number of
utilities. Each column condenser or reboiler
may also exchange heat with as many reboilers
and condensers in the superstructure as desired
as well as with the set of utilities. Different
minimum temperature approaches can be al-
lowed for process-process, hot utility-process
and process-cold utility matches.
4. All separations are considered to be sharp
splits of the light and heavy keys with no
distribution of components in both the dis-
tillate and the bottoms.
For the examples presented in this paper, the feed
streams to all columns are saturated liquids at their
bubble point at the pressure of the column and the
distillate and bottoms products are also saturated
liquids at their bubble point. These restrictions satisfy
Assumption 1. All columns have total condensers to
satisfy Assumption 3. Each column may exchange
heat with at most, one of each type of utility.
Most of the assumptions described above can be
relaxed so as to best fit the separation system being
considered. Partial condensers can be used for certain
columns if the physical properties or operating pres-
sure considerations of the separation require such.
Data concerning operation of the columns with this
type of condenser would then be required. As will be
seen, the nature of the mathematical formulation
makes discretionary restriction of heat-integration
matches and/or utility heat-exchange matches easy to
impose. By limiting each column to at most a single-
utility match of each type, the combinatorial nature
of the problem can be reduced and a more realistic
heat-exchange scheme can be identified.
OUTLINE OF SYNTHESIS STRATEGY
In Fig. 1, an outline of the steps involved in the
synthesis of optima1 heat-integrated distillation se-
quences is presented. These steps are as follows:
Step 1. A superstructure of distillation tasks is
derived that involves all distinct separation tasks
comprising the possible separation sequences. In
addition, all possibilities for heat integration be-
tween column condensers and reboilers as well as
possible utility matches are imposed on this super-
structure. An example of ‘the postulated ‘super-
structure for a three-component example is shown
in Fig. 2.
Step 2. In the second step, data concerning column
operating parameters and costs are obtained by
performing shortcut simulations ‘for each dis-
tillation task. These data include: condenser and
reboiler temperatures, condenser and reboiler du-
ties and total column costs. Simulations are per-
formed for a range of pressures that span the
allowable range determined by the critical proper-
ties of the components involved in the separation
or those dictated by the hottest and coldest avail-
 A mixed-integer programming formulation 533

Step 3. The overall superstructure is then formu-

I Superstructure
I
lated as a MINLP problem that can be solved
through APROS (Paules and Floudas, 1987) that
provides automated implementations of the Equal-
ity Relaxation algorithm (Kocis and Grossmann,
Dora
1987) or the Generalized Renders Decomposition
algorithm (Geoffrion, 1972).
+ Step 4. The solution of the MINLP in Step 3 will
Mixed-integer nonlinear provide the optimal heat-integrated distillation
programming sequence featuring minimum investment and
(MINLP) operating costs subject to the chosen minimum
formulation
temperature approach values.

1
MATHEMATICAL FORMULATION
1 *utorn;:btion 1
The basic ideas in the mathematical formulation of
the synthesis problem of heat-integrated distillation
sequences are: (a) representation of the discrete na-

-1 ture of the problem; and (b) implicit incorporation

the pressure of each column as a continuous variable
in the set of constraints and objective function. The
of

discrete nature of the problem is introduced by

Fig. 1. Outline of synthesis strategy.
able utilities. Using regression techniques, these
data can be fitted to linear or nonlinear expressions
as functions of the condenser and reboiler tem-
peratures of each column.
assigning to each column in the superstructure an
integer variable that will take the value of one in the
optimal solution if the column exists and will be set
to zero if the column does not exist. In addition to
this set of integer variables, a second set of integer
variables is introduced whose zero-one assignment in

\ \

tlz
I - Q
l----k’
cw ,=g cw

a
A

Fig. 2. Superstructure for three-component separation.

534 C. A. FWUDAS and G. E. PAIJLES IV
the optimal solution indicates the existence of heat
integration between any condenser and reboiler or
matches of condenser and reboiler with needed hot or
cold utilities. The pressure of each column is incorpo-
rated as a continuous variable through its condenser
temperature. This relationship is equivalent because
either one may be obtained from the other through
an equilibrium calculation of the distillate com-
position given a specified thermodynamic state. The
condenser temperature of each column determines
condenser and reboiler duties that are also included
as continuous variables and participate in column
energy balances and the objective function. The
condenser temperature levels also play key roles in
determining allowable heat-exchange matches based
on the given minimum temperature approach.
To derive the mathematical formulation of the
MINLP problem, the following index sets will be
defined to characterize the topology of the super-
structure. First, the set of all columns will be denoted
by the index set: CO = {i}. The set of hot utilities will
be denoted by the index set: HU = {h} and the set of
cold utilities by the index set: CU = {c}. Since every
column does not appear in every sequence, the index
set: CR’= {_I’) will denote the set of columns j that
can exchange heat with column i (i.e. heat integration
between the condenser of column j with the reboiler
of column i). Because it is desired to identify the
optimal sequence, this set is determined by the col-
umns that appear in the same sequence of the super-
structure. Within the superstructure, there are pro-
duced intermediate products that will undergo
further processing in other columns. This set of
intermediate products will be denoted: IP = {M}. The
index set: Pm = {i }, will denote the set of columns i
that produce intermediate product rn. The index set:
Fm = {i } will represent the set of columns that have
as feed intermediate product m. Finally, the index set
TL = (i} will denote the set of leading columns that
perform the initial split of the multicomponent feed.
Each column i has associated with it a set of
continuous and integer variables. The associated
integer variables are: (a) yC”, that denote the exis-
tence of the column i in the optimal flowsheet; (b)
JJ~, that denote heat integration between the con-
denser of column i and the reboiler of column i; (c)
yc”, that denotes the existence of a match between
hot utility h and the reboiler of column i; and (d) YE”,
that indicate the existence. of a match between the
condenser of column i and cold utility c. The con-
tinuous variables associated with each column i are
the following: (a) &, the flowrate to the column; (b)
TF, the condenser temperature of the column; (c) TF,
the reboiler temperature of the column; (d) QF, QF.
the condenser duty and reboiler duties of column i;
(e) Qz”, the amount of heat transferred from the
condenser of column i to cold utility c; (f) LMTD,,
the log mean temperature difference involved in the
cold utility match; (g) QE”, the amount of heat
transferred from hot utility h to the reboiler of
column i; and (h) QF, the amount of heat trans-
ferred from the condenser of column i to the reboiler
of column j.
Having defined the main index sets and variables
that describe the distillation superstructure, the ob-
jective function and constraints of the MINLP for-
mulation can be presented as follows:
THE MINLP OBJECTIVE FUNCTION
The objective function of the MINLP formulation
involves the investment costs for the distillation
columns and heat exchangers as well as the operating
costs for the utilities. If the operating pressure of each
column is not specified but treated as a continuous
variable, then the investment cost should be formu-
lated so as to take into account the variation of
pressure. This pressure variation is introduced in the
investment cost of each column expressed in the form
of the temperature of the condenser. Then, the in-
vestment cost for each distillation column i is repre-
sented by a nonlinear fixed charge expression of the
form:
COSTi = a?~? +f(fi)k;, (1)
where a” is the fixed charge associated with column
i and f(c) is a function of the column condenser
temperature. In this study, a linear function of the
form:
f(c)=a,+bi(fi-,TCp), (2)
was used in the regression analysis for column, cost
data. TCT is a constant representing the minimum
allowable condenser temperature for the separation
of task i. Combination of (1) and (2) yields the final
nonlinear fixed charge expression that is of the form:
COST, = aF”yco + j?yO(TF - TCp)&., (3)
where /I” is the variable charge coefficient for
column i. Note that as a result of the regression
analysis, the term resulting from the product of the
determined coefficient cziand 4 vanishes as ai was
found to be zero for all cases. It should also be noted
that in the fixed charge expression (3), UC”could also
have been expressed as a function of c. In this
paper, aF” is treated as constant for two main
reasons. Firstly, on the grounds that the regression
analysis revealed that equation (3), with a$ constant,
provided a very good fit of the cost data. Secondly,
because this results in a special structure MINLP
formulation that features linearity and separability
of the integer varizbles, which can be solved with
the Equality Relaxation algorithm (Kocis and
Grossmann, 1987).
Nonlinear fixed-charge cost models were also used
for heat-exchanger investment costs. The postulated
superstructure has embedded all possibilities for heat
integration and utility exchange. If a heat match
exists in the optimal solution, the associated integer
variable is activated and will introduce the fixed
 A mixed-integer programming formulation 535

charge portion of the investment cost. The variable denser. The defining expressions for the set of vari-
costs are introduced by nonlinear expressions that ables, LMTD,c, will be given as constraints of the
determine the heat exchange area required based model with the variables appearing in this set of
upon the heat duty of the match and the log mean fixed-charge cost models in the objective as:
temperature difference. The form of the fixed charge CU
model utilized for the heat exchangers is: Q,
COST HXCU = aHXyEU + /JHx 9 (8)
1 &c (LMTD,,) 1
COST HX = aHXy + ,!FA, (4)
where U, is the overall heat transfer coeflicient for
where aHX is the fixed charge associated with the process-cold utility heat transfer. The possibility of
purchase of a heat exchanger; bH” is the variable nonconstant temperature hot utilities could also be
charge coefficient associated with the cost of a heat included in the model by adding terms similar to
exchanger based on total heat transfer area; and A is equation (8) with hot utility teniperatures being used
the heat exchange area for that match. In the objec- to define a hot utility log mean tempetature
tive function, the variable A is replaced by nonlinear difference.
expressions relating A to the heat duties and log mean The objective function is chosen so as to represent
temperature differences. The general form of this an annualized cost for the proposed design, therefore
relation is given by: the total contribution to the objective by the in-
vestment costs is divided by the payout time in years,
A=
Q
r. The operating costs includeq in the objective
U(LMTD)
function are the costs of the hot and cold utilities vd
There are three different types of heat exchange that by the process. These costs are multiplied by a
can occur in the superstructure and each has a correction factor, 9, to adjust for income taxes. Then
different form of expression for A. The first of these the entire MINLP objective function may now be
is heat exchange between two process streams by heat expressed in mathematical form:
integration of the columns. If heats of mixing are
assumed negligible for streams containing more than Z =; c [a”“y” +b”(fi - TCp)FJ
one component, the condensing hot stream and the &CD
reboiling cold streams of these matches are both
exchanging only latent heat at constant temperature,
therefore, the log mean temperature difference is
simply the temperature difference of the hot and cold
stream, in this case, the temperature of the condenser
HU
ofcolumn i minus the reboiler temperature of column Qh,
+p
j. The fixed charge cost expressions for this type of {
U,,(T;” - TP)
exchange appear as:
+ 1 C aHxyEu
COST HXCR = aHXyy + 8” iECOCCC”
(@
QS”
+BHX
where VP,is the overall heat transfer coefficient for
1 UK (LMTD, ) 11
process-process heat transfer.
The second type of exchange occurs between hot
+ tl c c CF”Q:”
utilities and reboilers. Again the log mean tem- ( &COECU
perature difference can be expressed as the difference
of two constant temperature streams. The difference + c 1 C?“QhHi” , (Ml)
h<IfL,EC0 1
in this case is that the hot utility temperatures are not
variables but are known values. The flxed charge where CF” is the cost coefficient for the cold utility
model for this case appears as: c and C,“” is the cost coefficient for hot utility h.

QY
COSTHXHU = aHXyE”+/?HX (7) CONSTRAINTS OF THE MINLP
iJ,,(T;'-T:)
I'
In the previous section, the objective function of
where U,, is the overall heat transfer coefficient for
the MINLP formulation was presented. This objec-
hot utility-process heat transfer and Tfh” is the
tive function is minimized subject to the following set
known constant temperature of hot utility h.
of constraints:
The third type of exchange occurs between hot
process streams from the condensers and the cold 1. Heat duty and temperature definitions
utilities. The cold utility is no longer a constant
The constraints that relate the duty of the con-
temperature stream and therefore the log mean tem-
denser of column i to the temperature of the con-
perature difference must be expressed as a function of
denser have the following linear form:
the known inlet and outlet temperatures of the cold
utility and the unknown temperature of the con- Qc=,~D+kF,“~~fl~D-S2~D isC0. WV
536 C. A. FLOIJIJASand G. E. PAULESIV

The coefficients kED and k:lD are obtained from where T$rN and T$om are the,inlet and outlet tem-
regression analysis of the simulation data taken at peratures of cold utility c+ respectively. These
different pressures. Appearing in this set of con- definitions can either be treated as constraints or
straints are an additional set of continuous variables, substituted directly into the cold utility heat transfer
SIFD and S2FD, that are introduced to act as artificial area terms of the objective function.
slack variables. These variables are introduced to
prevent infeasibilities arising from the equality con- 4. Material balances
straints whenever column i does not participate in the These constraints provide the logical linking of the
activated sequence. If column i does not exist in the columns in the superstructure through the flow of
flowsheet, the condenser duty of that column must be intermediate products and have the following form:
set to zero to satisfy energy balance constraints.
Then, the artificial slack variables will eliminate the i$/i- c &=f’ meZP i&e.=FEED (M7)
potential infeasibilities. A set of logical constraints IEF
sets these artificial slack variables to zero if the where &,,,is the split fraction for intermediate product
column exists in the flowsheet and allows them to m from column i and FEED is the known total
take on positive values and prevent infeasibilities if multicomponent feed flowrate to the distillation
the column does not exist in the flowsheet. A similar superstructure. The first set of constraints sends the
set of linear constraints are included relating reboiler combined flowrates from all columns producing
duties to reboiler temperatures and have the form: intermediate product m to the set of all columns
Q~=k~D+k$oT~+Sl~D-S2~ iEC0, that further process that intermediate product. The
(MS)
second constraint requires that the total multi-
where kED, k:r’ are the coefficients for reboiler duty component feed flowrate be sent to all the leading
vs reboiler temperature fits obtained by regression columns of the superstructure that will perform the
analysis of simulation data. Another set of linear initial split.
constraints is included to relate the reboiler tem-
perature of a column to its condenser temperature. 5. Critical or imposed temperature bowto3
These constraints are of the form:
These constraints are included to permit the setting
TF=kT,+kT,TF+Sl:-S2: icC0, (M4) of lower and upper bounds on the temperatures for
each distillation task and have the following form:
where kz., kz are coefficients for reboiler temperature
vs condenser temperature fits obtained through re- 7-C FAIN
a -2%Q(l -J$~:o)<o ioco, (M8)
. ,
gression analysis of the simulation data. In both Tf‘- TRy’Ix<O iEC0,
cases, the S l”, S2” and Sir, S2: represent
artificial slack variables introduced to prevent in- where TCyIN is the minimum condenser temperature
feasibilities when column i does not exist in the for column i. TRf- is the maximum allowable
flowsheet. reboiler temp&ature for column i; and f2 is an
arbitrarily large upper bound to be used in logical
2. Energy balances constraints of this form. The first set of constraints
imposes lower bounds TCyIN, on the condenser
Qr=,TR,QzK+ 1 QE’-’ iEC0,
E eEC” temperatures. Such laker bounds are imposed to
(M5) avoid an optimal solution that may select a condenser
Qp= c QSK+h~UQ~u iEC0. temperature such that operation under a vacuum is
,ECR required. This can occur when a cold utility is
This set of linear constraints provide the energy available at a temperature below the condenser tem-
balance restrictions on the superstructure for each perature that corresponds to a bubble pressure of
column’s condenser and reboiler. All cooling required 1 atm. If the normal boiling point of the overhead
by a condenser of column i must be transferred either composition is below the coldest cold utility tem-
to a reboiler of another column in the chosen se- perature, then the minimum condenser temperature
quence or to a cold utility. Likewise, all heating should be the temperature of that utility plus the
required by a reboiler must be provided by either the minimum temperature approach for process-cold
condenser of another column in the chosen sequence utility heat exchange, ATE,, with the minimum col-
or by hot utilities. umn pressure being determined by the bubble point
pressure at that temperature. If the column does not
3. LMTD dejnitions exist in the flowsheet, the imposed restriction is
These constraints define the variables, LMTD,, for relaxed by the zeroone status of the integer variable
the heat exchanger contributions to the objective. and the upper bound R. The second set of constraints
imposes upper limits on the reboiler temperatures of
LMTD,= = iEC0 csCU, (M6) each column. These can arise due to the critical
temperatures and pressures of the bottoms com-
positions. If critical conditions are not approached by
 A mixed-integer programmiag formulation 531

the temperature of the hottest hot utility, then the AT&. The constraint is written so as to enforce this
upper bound, TRym, will be the temperature of the condition if the associated integer variable, yz”, is
hottest hot utility minus the hot utility minimum activated and to relax this condition if it is not. It
temperature approach, AT:&. Because these con- should be noted that constraints of this type for
straints act only as upper bounds on T,“, they need process-cold utility matches are not needed due to
not be relaxed based upon the existence of the column the set of imposed lower bound constraints on the
in the flowsheet. If needed, a similar set of constraints condenser temperatures shown in constraint set 5.
can be included to set upper bounds on the condenser
temperatures to bound them away from the critical 7. Logical constraints
conditions of the overhead compositions.
The following logical constraints control the levels
6. Minimum temperature approach constraints of certain continuous variables based on the zero-one
status of the integer variables.
Process-process.
Material balances. These constraints set the
(TF-fl)+A~&-Q(i -yF)~o flowrates to the distillation columns to zero if the
column does not exist in the flowsheet.
ioC0 jECR’. (M9a)
&-0ymgO iEC0, (MlOa)
This set of constraints requires a minimum tem-
perature approach of AT& between any two process Heat integration duties. These constraints set the
streams exchanging heat as part of the heat- values of the heat integration duties to zero if the
integration scheme. Note that this constraint is writ- corresponding heat-integration integer variable is not
ten for all allowable matches of condenser and re- activated.
boiler. For example, if column 1 and column 2 appear
Q$” - C?yp < 0 isC0 jeCR’. (MlOb)
in the same sequence, then there is the possibility of
heat integration between the condenser of column 1 Hot utility-rebotler duties. These constraints set the
and the reboiler of column 2 as well as the possibility values of the hot utility to reboiler duty exchanges to
of exchange between the condenser of column 2 and zero if the corresponding integer variable is not
the reboiler of column 1. Because a driving tem- activated.
perature difference must exist between a condenser
Q~“-fZy~u~O iEC0 ~EHU. (MlOc)
and a reboiler, at most, one of these is possible.
Therefore, if heat integration is to occur between the Condenser duty-cold utility. These constraints set
condenser of column 1 and the reboiler of column 2, the values of the cold utility to condenser duty
the integer variable, yy’:, is set to one and the integer exchanges to zero if the corresponding integer vari-
variable corresponding to the heat integration of the able is not activated.
condenser of column 2 and the reboiler of column 1,
Q$” -fiyf” GO iEC0 CECU. (MlOd)
yg:, must be zero. This assignment of integer vari-
ables in the two associated constraints will cause the Reboiler and condenser heat duties. These con-
first (indicating heat exchange between the condenser straints set the total condenser and reboiler duties of
of column 1 and the reboiler of column 2) to appear columns to zero if the column does not exist in the
as: flowsheet.
Tf-TfgATE,;, QF+QF-f2y”<O ieC0. (MlOe)

and the second associated constraint (indicating heat Artificial slack variables. These constraints set the
exchange between the condenser of column 2 and the values of the artificial slack variables that appear in
reboiler of column 1) should be relaxed and will have the duty and temperature definition constraints to
the form: zero if the associated column does exist in the
flowsheet. This causes the definition constraints to be
E-T~~AT~,--Q
active if the column exists and relaxed if the column
that will allow G and Ty to take whatever values are does not exist.
determined by the active part of the model without sl~“+s2~“-n(l-y”)fO
causing infeasibilities.
Hot utility-process SlRD+S2,~-fJ(l -yp)CO iEC0

(TR- TP)+AT&-n(l -J+‘)<O sl~+s2~-n(l-y”)<O (Ml of)

icC0 heHU. (M9b)

This set of constraints acts in a similar manner as the
process-process temperature approach constraints. If
a hot utility exchanges heat with a n&oiler, the
temperature of the hot utility must be greater than
the temperature of the reboiler by a difference of
8. Pure integer constraints
These sets of constraints involve only the integer
variables and create logical conditions on the allow-
able combinations of integer variables in the optimal
solution.
538 C. A. FLOUDASand G. E. PAULESIV
Utility limits. These constraints require that each
condenser or reboiler match with at most one utility
of each type (e.g. one hot utility and one cold utility).
(Mlla)
Single direction of heat integration. This set of
constraints prevent the mutual heat integration of
two columns in both directions. The temperature
approach constraints would make this occurrence
infeasible, but the pure integer constraint is included
to speed the enumerative procedure of the branch-
and-bound algorithm by reducing the number of
possible integer combinations.
yz” + yz” < 1 &CO jcCR’ (Mllb)
Sequence constraints. These constraints limit the
possible combinations of integer variables represent-
ing the distillation columns to a single separation
sequence.
&Y:O= 1. (Ml lc)
It is important to note that while this restriction on
the formulation can be relaxed, the number of ele-
ments in the index set CR’= {j} will increase dras-
tically along with the number of integer variables
indicating these matches. This is because without the
restriction to a sequence, the possibility of every
column in the superstructure heat integrating with
every other column in the superstructure must be
considered.
Pure integer logical cuts. Restriction of the branch-
and-bound enumeration tree is very important in the
solution of this mathematical formulation. Two sets
of pure integer logical cuts can be derived to dras-
tically restrict the search tree of the MILP master
problems. The first such constraint is based on the
existence or nonexistence of any distillation column
in the superstructure. If a column integer variable,
Y?O’“. is not activated, then all heat-exchange integer
variables associated with that column must also be set
to zero. These constraints will then appear as:
g0 isC0 (Mlld)
where w is an upper bound parameter whose value
should be chosen such that it is larger than the largest
possible value of the indicated summations.
A second set of pure integer logical constraints can
be derived based on the existence or nonexistence of
entire sequences. Since it is known which columns
participate in each sequence of the superstructure,
two new index sets can be defined to express this
information: SQ = {s} will indicate the set of all
sequences in the superstructure and CS’ = {i} will
indicate the set of columns i that participate in
sequence s. Whenever an entire sequence is activated
during the enumeration procedure, then all integer
variables not associated with that sequence. should be
set to zero. This set of constraints has the form:
seSQ. (Ml le)
where SPLT is a model parameter equal to the
number of distillation columns in any sequence of the
superstructure.
The objective function (Ml ) subject to the set of
constraints (M2)-( Ml 1) represent the general math-
ematical formulation whose solution will identify the
optimal heat-integrated distillation sequence. This
model corresponds to a MINLP problem since it
involves continuous and integer variables, a linear set
of constraints and a nonlinear objective function.
The properties and techniques for solution of this
mathematical formulation are presented in the next
section,
REMARRS ON THE MATHEMATICAL FORMULATION
The proposed MINLP formulation has several
characteristics that determine the required methods
and possible algorithms for its solution. Kocis and
Grossmann (1987) proposed an efficient algorithm
for the solution of special structure MINLP problems
in which all integer variables appear linearly and
separably from the continuous variables that can
appear linearly and/or nonlinearly in the model. The
proposed mathematical formulation belongs to this
special class of MINLP problems, and the basic
algorithmic steps consist of solving a finite alternating
sequence of NLP subproblems and mixed-integer
linear programming MILP master problems. The
MILP master problem selects a new combination of
integer variables that are then temporarily held fixed
to yield a new NLP subproblem corresponding to the
optimization of a specific flowsheet. For mini-
mization problems, the NLP subproblems provide
upper bounds on the objective function and the
MILP master problems provide lower bounds. Ter-
mination of the algorithm is indicated by the failure
of the MILP master problem to find a feasible integer
combination subject to these upper and lower
bounds. The optimal solution is given by the smallest
upper bound found by any NLP subproblem.
An important question that arises on the proposed
MINLP formulation is whether the properties of the
objective function and constraints allow for a global
solution to be obtained. The feasible region consists
 A mixed-integer programming formulation 539

of a linear and therefore convex set of constraints. The logarithmic expression for the log-mean tem-
The objective function however, involves non- perature difference of the cooling water matches
linearities that are expressed in the form of bi- cannot be convexified as with the other two types of
linearities of the same sign and fractional terms of the matches. Several approximations can be employed to
same sign. The bilinearities in the objective function avoid over-estimation of the objective function value
are introduced by the chosen form of nonlinear in the MILP master problems. One point is to
fixed-charge cost expressions for the distillation substitute the log-mean temperature difference with
columns: an arithmetic mean temperature difference and use a
COSTi= tc”j~” + j”(c - TCf’lN)Ff iEC0. similar transformation to those shown above for the
resulting ratio terms. Another option is to replace the
The column condenser temperatures, fi and feed
LMTD with a constant term equal to an empirically
flowrates, Fi, in these expressions form the bilinear
determined value of 2-3 times AT,,, which results in
pairs for each column in the superstructure. These
a linear participation of QE” in the objective func-
nonconvex expressions do not present difficulties for
tion.
guarantee of global optima for the following reason.
Another aspect of this formulation that should be
For any fixed combination of integer variables, the
noted is that as the number of components and
resulting NLP problem has a unique value of F,
therefore sequences increase, the number of integer
determined by the linear material balance constraints.
variables in the formulation can increase rapidly.
Therefore, the bilinearities are effectively reduced to
Model size statistics for three-, four- and
linear expressions in terms of TF for solution of each
five-component problems can be found in the tables
NLP problem.
of the example problems. Even though large numbers
The ratio terms of the objective function result
of integer variables can be involved for problems with
from the heat transfer area expressons given by
many components, the computational effort required
equation (5). Depending on the type of heat match,
to solve the MILP master problems does not increase
LMTD can have one of three forms in the objective
as drastically as the number of integers may suggest.
function. For heat-integration matches, LMTD is
This can be attributed to two main factors. The first
replaced by the difference of condenser and reboiler
is that the proposed model aims to identify the
temperatures taking part in the match as shown in
optimal sequence. This greatly eliminates the number
equation (6). For hot utility matches, LMTD is
of possible combinations of integer variables repre-
replaced by the difference of a constant parameter
senting the existence of distillation columns in the
and a variable reboiler temperature as shown in
superstructure. The second factor is that strong in-
equation (7). For cold utility matches, heat transfer
teger cuts, based on the existence or nonexistence of
does not occur at a constant temperature on the cold
individual distillation columns and entire sequences,
side and LMTD is replaced by the definition of the
drastically reduce the branch-and-bound enumer-
log mean temperature difference shown in equation
ation tree. Despite the effectiveness of the above
(M6). In the first two cases, the nonconvexities can
mentioned factors, it is in principle possible that the
be removed through convexification techniques of
mathematical formulation of an entire superstructure
geometric programming. By making the proper vari-
may become too large to solve efficiently. Several
able transformations, the nonconvex terms can be
approaches are available to deal with this problem
convexified. For the case of the heat-integration
should it arise.
matches, the following exponential transformations
A first approach for making the solution of large
are made:
problems more computationally tractable is based on
QP = exp(u,,) the observation that the overall superstructure can be
I ~20 jeCR’. (9)
TF - Ty = exp(t+) decomposed into smaller substructures. This ap_
preach would involve fixing the existence of one or
The ratio terms of the objective function then appear more leading columns in the original superstructure
as the convexified term: and letting the solution of the restricted MINLP
exp(n,, - i@ provide the optimal heat-integrated sequence from
/tea= (10) among the restricted set. For instance, the four-
{ UP, 1, component problem can be decomposed into two
A similar transformation is made for the case of the two-sequence problems and a one-sequence problem.
hot utility matches: This procedure could be used until all sequences have
been considered as part of a subproblem of the entire
Q? = exphd hEHlJ ieC0, 01) superstructure and the overall optimal sequence
Tf” - TF = exp(u,,,) found by comparison of the 6ptimal sol,ution’ from
that will transform the corresponding terms of the each of the subproblem analyses,
objective function into: A second approach is based upon a modification of
the formulation that reduces the actual number of
A HU-_ exp(ulhi - &hi)
integer variables in the formulation without altering
(12)
GIP the overall objective of the optimization model. The
540 C. A. F~oun~s and G. E. PAULESIV

motivation for this reformulation of the mode1 comes
from the observation that because the mode1
identifies a specific sequence, at most, one set of
heat-exchange integer variables need be considered at
any point in the MILP solution enumeration scheme.
By defining an arbitrary position for each distillation
task participating in each sequence of the super-
structure, a single set of “dummy” integer variables
can be used as the heat-exchange integer variables for
all possible sequences. Each unique distillation task
retains an individual integer variable in the model,
but the matches that occur for heat integration and
with the hot and cold utilities can be reduced to a
single set of integers indicating matching only of
generic positions in the sequence involved. By doing
so, the required integer variables for the three-, four-
and five-component problems involving two hot util-
ities and one cold utility can be reduced from 20 to
12, 70 to 25 and 212 to 44, respectively. This formu-
lation requires, however, more complex mappings of
the distillation columns and their positioning in each
sequence in which they participate. This results in an
increase of the number of continuous variables and
constraints due to the decomposition of the super-
structure into a more sequence-oriented problem
requiring more artificial slack variables and logical
constraints to control their behavior. It has been
observed that the trade-off in the computational
effort between the proposed formulation and the
re-formulation with the “dummy” integer variables is
problem dependent.
AUTOMATIC IMPLEMENTATION-APROS
iteration. The user chooses an initial combination of
the binary variables and includes this assignment as
part of the input to APROS. Once the input file is
prepared, the remainder of the procedure is auto-
matic. GAMS is executed and performs a com-
pilation of the input data and models. Once the
compilation is complete, the first NLP subproblem is
modeled and the input for the nonlinear pro-
gramming solver, MINOSS. 1, is created. MINOSS. 1
is then executed from within GAMS. The solution
results are returned to GAMS where the information
is used in determining the form of the MILP master
problem. GAMS models the MILP master problem
and prepares the input for the mixed-integer linear
programming solver, MPSX or ZOOM/XMP.
MPSX or ZOOMjXMP is then executed from within
GAMS. The solution results, with the new proposed
combination of binary variables, are returned to
GAMS for processing. At this point, a stopping
criterion for optimality is introduced, and GAMS
tests the desired stopping criterion. If the stopping
criterion is met, the program stops with an output
that displays the optima1 solution as well as the
intermediate work. If the criterion in not met, GAMS
uses the information from the MILP master problem
to restructure the NLP subproblem according to the
new binary combination proposed and execution
continues.
Solution of MINLP problems is a nontrivial task
and often, the characteristics and peculiarities of the
individual model must be taken into account during
solution procedures. Because APROS operates en-
tirely through the GAMS modeling language, the

The solution of the proposed MINLP formulation

was obtained automatically through the program
APROS. APROS-Automatic Process Synthesizer
(Paules and Floudas, 1987) is a computer package for
I
the automatic solution of genera1 MINLP problems.
APROS combines the Genera1 Algebraic Modeling
ti Yf
System, GAMS (Bisschop and Meeraus, 1982;
Kendrick and Meeraus, 1987), the nonlinear
programming solver MINOS5.1 (Murtagh and
Saunders, 1986) and either MPSX (IBM, 1979) or
ZOOM/XMP (Marsten, 1986) mixed-integer linear
programming solvers to provide an automated imple-
mentation of the Benders Decomposition algorithm
(Benders, 1962), Generalized Benders Decomposition
algorithm (Geoffrion, 1972), the Outer Approxi-
mation algorithm (Duran and Grossmann, 1986)
and Equality Relaxation algorithm (Kocis and
Grossmann, 1987).
A flow diagram of the computer package APROS
is shown in Fig. 3. A process model whose solution
requires an implementation of any of the three algo-
rithms mentioned represents the input data. The user
enters a general framework for the NLP subproblem
and the MILP master problem using the GAMS
modeling language, along with appropriate com-
mands to transfer data from one to the other for each Fig. 3. Flow diagram for APROS.
 A mixed-integer programming
user is afforded considerable flexibility in his exact
approach to solution of the MINLP and has a choice
of several different algorithms from which to select
the algorithm that suits best the particuar model.
To illustrate the use of APROS for the automatic
synthesis of heat-integrated distillation sequences
that allow for treatment of the pressure of each
column as a continuous variable, three example
problems will be considered.
EXAMPLE PROBLEM I
This is a three-component separation intended to
demonstrate the solution of a small example as a
complete superstructure. The three components in-
volved are given by A = hexane, B = benzene,
C = heptane. The problem data is given in Table 1.
A superstructure featuring the two possible sequences
is derived. The superstructure for this problem with
the possible sequences and allowable utility and
heat-integration matches is shown in Fig. 2. Material
balances were then performed assuming the columns
to be sharp splitters. This provides information re-
garding the composition of the overhead and bot-
toms in each column of the superstructure. These
compositions are used to determine the critical condi-
tions of the condensers and reboilers that will in turn
determine the upper and lower bounds on their
temperatures. As explained in the section on the
imposed temperature bound constraints, these
bounds are either determined by the critical tem-
peratures and associated pressures or hottest and
coldest utility temperatures if the critical conditions
lie outside these bounds. For this example, the latter
was found to be the case with the critical conditions
lying outside the utility bounds. Once the allowable
pressure/temperature range is known, a number of
pressures within the range are selected for the simu-
lation runs. A simulation of the separation for each
particular distillation task in the superstructure is
performed for the selected pessures in its range. All
simulations for this study were done using the PRO-
CESS flowsheeting system (Simulation Sciences,
1985). Sizing data from the simulations is used to
perform costing of the columns at each of the con-
denser temperatures (pressures) selected. The method
of Guthrie (1986) was used to perform the costing.
The cost data and other data from the simulations
(e.g. heat duty vs condenser temperature, reboiler
temperature vs condenser temperature, etc.) are used
Table 1. Data for Example Problem 1
A B
Feed composition 0.80 0.10
Multicomoonent feed Rowrate = 396.0 kzmol h-’
Available’utilities:
Cooling water @ 305.0 K (20 K rise); cost = $0.159. 106kJ-’
Low-pressure steam @ 421.0 K; cost = $3.11. 106k.-’
Exhaust steam @ 373.0 K; cost = $1.14. IO6kJ-’
Minimum temperature approach = 10 K
formulation 541
in regression analysis to provide the various fits
needed to construct the cost models and constraints.
The entire superstructure was then formulated as a
MINLP problem. The Equality Relaxation algorithm
was implemented with APROS running GAMS
~2.04, interfaced with MINOS5.1 and ZOOM/XMP
to solve the MINLP problem. Statistics concerning
the resulting model sizes of the NLP subproblem and
MILP master problem are given in Table 2. The
constraint statistics for the MILP models reflect first
iteration sizes. At each iteration, additional linear-
izations are added to the problem for the LMTD
definition constraints and the objective function.
Solution of the MINLP by the Equality Relaxation
algorithm required 3 iterations. VaxStation IT/GPX,
IBM 3081 and IBM PC/AT total CPU times for the
NLP subproblems and MILP master problems are
given in Table 3.
The solution, shown in Fig. 4, features a heat-
integrated scheme involving the upper sequence that
separates A first, (Column 1) and then B from C
(Column 2). The condenser temperature and corre-
sponding column pressure of Column 2 is raised to a
level high enough to permit the transfer of heat from
its condenser to the reboiler of Column 1. Low
pressure steam provides the heat for Column 2
because the column temperature is high enough to
disallow use of exhaust steam. Makeup hot utility for
Column 1 is provided by the exhaust steam utility,
and cold utility is required only for the condenser of
Column 1. The total annual cost for this design was
found to be %1,096,770.0.’
It is interesting to note that the costs associated
with an increase in column pressure outweigh the
costs for heat transfer area in this example.‘This is
indicated by the fact that the condenser temperature
of Column 2 in the optimal solution is exactly AT&
above the reboiler temperature of Column 1. Column
1 is set to operate at atmospheric,pressure, which is
the lowest pressure permitted by this model. Because
of the explicit nature of the heat exchange area
expressions, the model could choose to increase the
condenser temperature of the column contributing
the heat in a heat-integration match to a level greater
than AT& above the reboiler temperature of the
Table 2. Model statistics for Example Problem I
Continuous tnteger
Constraints variables variables
Full superstructure
NLP 32 21
MILP 94 65 20
C
0.10
Table 3. CPU times for Example Problem 1
Total time NLP submoblems fs) MILP masters Is)
Full superstructure
IBM PC/AT 54.0 672.0
VAX Station II/GPX 9.9 96.7
IBM 3081 0.6 7.6
542 C. A. FLOIJDAS
and G. E. PAULESIV

Fig. 4. Optimal solution-Example Problem 1.

other column if a savings in heat-transfer area costs and lower bounds for some separations leaves a
is indicated. narrow range of allowable column .pressures and
condenser temperatures. The flexibility of the math-
EXAMPLE PROBLEM 2
ematical model makes these conditions easy to imple-
ment. With the superstructure intact and the allow-
Example problem 2 is a four-component sepa- able pressure ranges for each separation determined,
ration involving a mulitcomponent feed of: A = simulations were performed to obtain the needed
ho-butane, B = n-butane, C = iso-pentane and D = column cost and operating data for the regression
n-pentane. It is desired to design an optimally heat- analyses. All the fits were performed using least
integrated distillation sequence of sharp splitters squares regression. The superstructure was then
that will provide four pure product streams at a modeled as a MINLP problem using the proposed
minimum total annual cost. Data for this problem is formulation.
given in Table 4. In this example, a third hot utility Solution of this example was performed using three
has been made available at a higher temperature. A different approaches that provided the same optimal
four-component distillation superstructure was de- solution. The first approach employed was to solve
rived featuring 10 distinct separation tasks and 5 the model of the entire superstructure. The second
possible separation sequences. The mass balances for approach was to decompose the overall super-
this superstructure were performed to calculate dis- structure into two two-sequence problems and a
tillate and bottoms compositions. It was found that one-sequence problem. The third approach used was
for certain columns in the superstructure, the bot-
toms compositions approach critical conditions near
the temperature of the hottest hot utility. These Table 4. Date for Example Problem 2
reboiler temperatures were therefore bounded away
A B C D
from the hottest hot utility temperature. Because of Peed comwsition 0.157 0.263 0.210 0.368
the volatile nature of the lighter components, the Multicomponent feed flowrate = 865.0 kgmol h-’
1 atm. boiling point of the distillate from some Available utilities:
columns is well below the temperature of the cold Cooling water @ 305.0 K (20 K rise); cost = $0.159. 10” W-l
Medium-pressure steam @ 459.0 K, cost = $3.98. lb kJ-’
utility. To effect total condensation, the lowest allow- Low-pressure steam @ 418.0K; cost = $2.71. IObkJ-’
able pressure of these columns is determined by the Exhaust steam @ 389.0 K; cost = $1.65. 106kJ-’
Minimum temperature approach = 10 K
cold utility temperature. The combination of upper
 A mixed-integer programming formulation 543

Table 5. Model statisticsfor Exanmle Problem 2 the expressions for the log-mean temperature
Continuous Integer differences of the cooling-water exchanges were re-
Constraints variables variables placed by constant terms. Model size statistics for
Full superstructure each type of substructure and for the full super-
NLP 58 37 - structure formulation are given in Table 5. Note that
MILP 289 197 80
in each case, the number of constraints and variables
Two sequencesubstructure
NLP 58 37 for the NLP subproblems are always the same. This
MILP 129 95 36 is due to the fact that any proposed combination of
Singlese~uence the integer variables corresponds to a subproblem
NLP 58 37 -
optimization of a single distillation sequence. As in
MILP 61 37 18
Table 2, MILP model size statistics reflect first iter-
ation sizes. Solution of the MINLP formulations
Table 6. CPU times for Example Problem 2 were performed using APROS.
NLP MILP Solution of the entire superstructure as a single
Total time subproblems(s) masters(s)
model required a total of 6 iterations to reach the
Full superstructure stopping criterion. Individual sequences required 2-3
VAX Station II/GPX 17.8 5521.4
IBM 3081 1.2 339.1 iterations and two sequence substructure problems
IBM 3090 0.7 187.2 required 3 iterations. These problems were solved on
TWO sequencesubstructure(ave) four different computers for comparison. Processing
VAX Station II/GPX 8.7 483.6 times are provided for the different formulations and
IBM 3081 0.5 21.5
different computers in Table 6. The optimal solution
Single-sequence
(ave)
IBM PC/AT 118.4 1598.4 found is shown in Fig. 5. The sequence chosen
VAX Station II/GPX 5.9 223.8 separates A from B (iso- and n-butane) from C and
IBM 3081 0.5 10.3 D (iso- and n-pentane) first (Column 1). The re-
sulting binary mixtures are then separated in their
to decompose the overall superstructure into five own columns (Columns 2 and 3, respectively). The
one-sequence problems that were solved individually. heat-integration scheme has the condensers of Col-
In all cases, the ratio terms of the objective function umns 1 and 2 transferring heat to the reboiler of
were convexified by exponential transformation and Column 3. Low pressure steam is used in Column 1

335.0 K

Fig. 5. Optimal solution-Example Problem 2.

544 C. A. FLOIJDASand G. E. PAULESIV

to provide the reboiler duty. Exhaust steam provides
all the reboiler duty of Column 2 as well as makeup
duty for the reboiler of Column 3. Cooling utility is
only needed for Column 3. The resulting total annual
cost for this design was found to be $2,448,814.0. A
detailed cost calculation for the optimal heat-
integrated sequence found in this example was per-
formed and the cost was $2,438,898.0. Therefore, it
can be seen that the proposed approach provides a
very good approximation of the actual cost solution.
EXAMPLE PROBLEM 3
Example Problem 3 is a five-component separation
that has been investigated by other researchers in
their approaches to the heat-integrated distillation
sequence design problem (Rathore et al., 1974a, b;
Sophos et al., 1978; Andrecovich and Westerberg,
1985b). The multicomponent feed contains the same
components as the four-component feed of Example
Problem 2 with the added fifth component, propane.
Components are identified in the following manner:
A = propane, B = bo -butane, C = n-butane, D =
iso-pentane and E = n-pentane. Data for this exam-
ple problem is given in Table 7. The derived super-
structure for this distillation system contains 14
possible sequences consisting of 20 distinct separation
tasks. Data for the sizing and operation of the
columns were obtained from simulation runs over the
range of pressures allowed for each task. Following
the regression analysis, the entire superstructure as
well as individual sequences were modeled as a
mixed-integer nonlinear programming MINLP prob-
lem. Model-size statistics for the entire superstructure
representation of the problem are given in Table 8
along with the corresponding statistics for a single
sequence of the decomposed superstructure.
Solution of the problem was performed in a man-

Table 7. Data for Example Problem 3

‘fable 8. Model statistics for Example Problem 3
C D E
COmitlUOUS Integer
Comvosition 0;s 0.?5 0.25 0.20 0.35
Constraints variables variables
Multicomponent feed flowrate = 910.0 kgmol h-’ Full superstructure
Available utilities
NLP 85 53
Cooling water @ 305.0 K (20 K rise); cost = 80.159. IO’W-
MILP 139 444 2n
Medium-pressure steam @ 459.0 K; cost = $3.98. 106k.-’
Low-pressure steam @ 418.0K; cost = $2.71. IO6 k.-’ Single-sequence
Exhaust steam @ 389.0K; cost = $1.65. IO6 kJ-’ NLP 85 53
Minimum temperature approach = 10 K MILP 97 53 28

353.6 K

d-06
353.6 K

7 366.6 K

Fig. 6. Optimal solution-Example Problem 3.

 A mixed-integer programming formulation 545

Table 9. CPU times for Example Problem 3 NOMENCLATURE

NLP MILP
Total time subproblems (s) masters (s)
K, = Coefficient for column cost vs condenser
temperature fits
Single-sequence (ave) A = Heat transfer area
IBM PC/AT 158.6 22776.0 bi = Coefficient for column cost vs condenser
VAX Station II/GPX 8.2 729.6
IBM 3081
temperature fits
0.53 48.6
c = Index for cold utilities
Cy = Annualized cost coefficient for cold utility c
ner similar to that of Example 2. The optimal solu- Cp” = Annualized cost coeflicient for hot utility h
CO = Index set of columns i in superstructure
tion found is shown in Fig. 6. The optimal sequence
COST, = Cost of column i
separates component A from BCDE first, in Column COST HX”” = Cost of a hot utility match heat exchanger
1. BCDE is then split between C and D (Column 2) COST HXCR = Cost of a heat-integration match heat ex-
with the two resulting binary mixtures (BC and DE) changer
being sent to two more columns for separation COST HXC” = Cost of a cold utility match heat exchanger
CR’ = Index set of columns j that appear in the
(Columns 3 and 4). Heat integration occurs between
same sequence as column i
all the columns. Columns 1, 2 and 3 provide heat to CS” = Index set of columns i that appear in
the reboiler of Column 4 to satisfy the large reboiler sequence s
duty needed for that separation. Medium-pressure CU = Index set of cold utilities c
steam must be used to provide the reboiler duty of F, = Flowrate to column i
FM = Index set of columns i that have inter-
Column 1 because of the large ATREwoN in this mediate product tn as feed
column. Low pressure steam provides the reboiler FEED = Total multicomponent flowrate to super-
duty of Column 2 and exhaust steam is used to structure
provide reboiler heat for Column 3 as well as the h = Index for hot utilities
makeup duty required in Column 4. Cold utility is HlJ = Index set of hot utilities h
i = index for columns in superstructure
needed only for the condenser of Column 4. In- IP = Index set of intermediate products m
spection reveals that the optimal solution of the j = Index for columns that can heat integrate
five-component problem features first a separation of with other columns in the same sequence
the lightest component yielding a four-component kEDD, kz” = Coefficients for condenser duty vs con-
denser temperature fits
separation identical to that of Example 2. The same
ky, ky = Coefficients for reboikr duty vs reboiler
scheme is chosen for the remainder of the separation temperature fits
sequence as well as basically the same heat- k:,, k; = Coefficients for reboiler temperature vs
integration scheme with the condenser of Column 1 condenser temperature fits
also contributing heat to Column 4. The solution LMTD, = Log-mean temperature difference for cold
utility match ic
found is in line with a heuristic approach to the m = Index for intermediate products in super-
problem that would identify the only logical se- structure
quences for separation as the two which do not Pm = Index set of columns i that produce inter-
attempt to split the two close-boiling components: mediate product m
QF = Condenser duty of column i
iso -in -butane and iso /n -pentane. The mathematical
Qr = Reboiler duty of column i
formulation of the model makes it easy to restrict the QP = Amount of heat exchanged in hcat-
solution to identify second and third best solutions integration match ij
based on either the total heat integrated Qz” = Amount of heat exchanged in cold utility
configuration (all integer decisions) or on sequence match ic
QC” = Amount of heat exchanged in hot utility
alone (column integer variables). By forcing selection match hi
of the alternate sequence identified by heuristics, a s = Index for superstructure separation se-
solution whose heat integration scheme is determined quences
by the MINLP formulation is found and whose S IF”, S2FD = Artificial slack variables for condenser duty
objective function value that is within 5% of the definition constraints
Slf”, S2y = Artificial slack variables for reboiler duty
optimal sequence. The final decision as to which definition constraints
sequence to use would then be made on operability Sl:, S2T = Artificial slack variables for condenser/
considerations. Average total processing times for the reboiler temperature definitions
NLP subproblem and MILP master of a single SPLT = Number of columns in a sequence of the
superstructure
sequence are given in Table 9. The total annual cost
SQ = Index set of superstructure sequences s
for this design was found to be %2,716,980.0. A TF = Condenser temperature of column i
comparison with results of other researchers in this Tr = Reboiler temperature of column i
example would be desirable. Such a comparison r,“” = The temperature of hot utility h
however was not attempted since different costing FIN = The inlet temperature of cold utility c
pouT = The outlet temperature of cold utility c
methods are employed in each approach. Td”I” = Minimum condenser temperature of col-
umn i
Acknowledgement-The authors would like to acknowledge TL = Index set of leading columns i of super-
financial support from the National Science Foundation structure
under Grant DMC-8617239. TRyAx = Maximum reboiler temperature of column i
546 C. A. FLOWAS and G. E. PAULES IV

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