A Simple Synthesis Method for Studying
Thermally Integrated Distillation Sequences
Gorazd Sobdan and Peter GlaviE*
University of Maribor, Faculty of Chemistry and Chemical Engineering, Smetanova 17, 2000 Maribor, Slovenia
A
n important process design problem in the chemical industry is a
systematic synthesis of multicomponent separation sequences. It
i s concerned with the selection of a separation method and the
selection of the best sequence of separators to split a multicomponent
mixture into several products of relatively pure species.
Distillation columns are widely employed to solve separation problems
in chemical industry. Their advantage is simple operation and ability to
separate various kinds of mixtures into their components. Distillation
sequences can be specified by different methods: heuristic, evolutionary
and algorithmic (Kattan and Douglas, 1986).
In the past, many researchers were engaged with the goal to deter-
mine the best heat-integrated distillation sequences. Different methods
were developed for a simple and quick selection of better heat-integrated
distillation systems. Andrecovich et al. based their methods on the
assumption that the product of the column condenser or reboiler duty
and the temperature difference between its reboiler and condenser, $AT,
was constant for a single distillation task over a wide range of pressures
(Andrecovich and Westerberg, 1985a, b).
Thermodynamically oriented procedures are commonly applied to a
given separation scheme but many ways for reducing utility needs can
be considered simultaneously. Umeda et al. (1 979) used thermodynamic
analysis to synthesize energy-integrated distillation systems. They proposed
the procedure using a (T-TJT vs. I$ diagram, where the enclosed area
between the composite lines for the heat sources and sinks was a
measure of the available exergy losses in the heat exchange subsystem
(Smith and Linnhoff, 1988; Umeda et al., 1979).
This paper introduces an improved thermodynamic formulation for
the heat-integrated distillation train synthesis problem, where the
separation as well as the heating and cooling task constraints are taken
into consideration. We wanted to develop a procedure for fast screening
of the best heat-integrated distillation systems. Our analysis was oriented
towards reducing the number of promising schemes to a minimum. The
problems studied are difficult for mathematical analysis to be solved
without simplification. We tried to apply our approach to a system of
isolated distillation columns and to a distillation column train being part
of a chemical process, the so-called process system. We wanted to find
out if the conclusions taken from the isolated distillation columns sequence
could be applied to the entire process design.
Integrability Criterion
Separation using distillation has high energy requirements, but they are
reduced when applying heat integration. Significant differences may
exist between the best heat-integrated and non-integrated sequences.
The result of our previous research shows that the best heat-integrated
and non-integrated sequences are not always the same (Sobotan and
'Author to whoin corrc,.sporitleiice may be uddressed. E-muil address: g/nvic@
iirii-mb.si
908
In this paper an improved method for studying
processes for separation of multicornponent mixtures
is presented. A thermodynamically oriented procedure
was developed for the analysis and synthesis of the best
heat-integrated distillation system. Systematic ranking
of possible schemes was used in order to verify the
best structure of a heat-integrated distillation system.
An integrabilitycriterion was introduced for the selec-
tion of the most promising heat-integratedsequences.
Distillation columns were studied according to their
ability for heat integration. The proposed selection of
possible distillation columns sequences using rising
integrabilitycriteria gave a good approximation of the
best heat-integrated distillation column sequences
according to their total annual cost. Computational
simulation of the process and pinch analysis were used
for thermodynamic optimization of energy consump-
tion. The method is illustrated with five- and six-
component example problems.
On presente dans cet article une mCthode
amelioree destinee a etudier les procedes de separa-
tion de melanges de composants multiples. Une
methode thermodynamique a ete elaboree en vue de
I'analyse et de la synthkse du meilleur systeme de
distillation thermointegree. On a procede a un classe-
ment systhatique afin de verifier la meilleure struc-
ture d'un tel systeme. Un critere d'integrabilite a 6t.6
introduit pour la selection des sequences d'intbgration
thermique les plus prometteuses. Des colonnes de
distillation ont ete etudiees en fonction de leur capac-
it6 d'integration thermique. Le choix propose pour les
sequences de colonnes de distillation possibles
utilisant des criteres d'integrabilite ascendants donne
une bonne approximation des meilleures colonnes de
distillation thermointegree si Yon considere leur coQt
total annuel. On a eu recours a la simulation par
ordinateur et a I'analyse du pincement pour I'optimi-
sation thermodynamique de la consommation
d'energie. La mkthode est illustree a I'aide de
problemes a cinq et six composants.
Keywords: integrability criterion, distillation column
sequence, heat integration, temperature difference.
Javit, 1998). It was believed that the best non-
integrated sequences lead to the best heat-integrated
ones, but considering our simulation results this was
often not true (Sobotan and Clavit, 1999c). Therefore,
the optimal sequences with and without heat integra-
tion could be different. Because of lower utilities
The Canadian Journal of Chemical Engineering, Volume 78, October 2000
 consumption, heat-integrated sequences are cheaper than the
non-integrated ones. This is also achieved when comparing the
same sequence, but our research shows that heat integration
could lead to different promising sequences (Sobotan and
Clavit, 1998). In view of energy conservation, it is important to
establish a systematic method for reducing external energy
inputs by an effective use of heat in distillation systems.
Therefore, heat integration is a decisive factor in finding the
best distillation column sequence. The effectiveness of heat
integration led us to the idea of developing a better criterion for
ranking distillation column sequences. We tried to find the crite-
rion based on thermodynamic properties of the components
which had to be separated in the distillation column sequence.
It should give a ranking similar to the one established according
to the total annual costs.
In our investigation, we developed an integrability criterion
for fast screening of the best heat-integrateddistillation columns
sequences. The task is to design a separation sequence which
achieves the required splits with the lowest cost. The ultimate
objective in this project is to design an optimal process system
with multicomponent separation included, “optimum” being
defined as that arrangement of units which requires the lowest
annualized depreciation and operating costs of the entire process.
According to our research in the past, we supposed that the
best representation of distillation columns was in the extended
grand composite curve (CCC), temperature- enthalpy flow rate
difference (T-AI) diagram. For the sake of simplicity let us Figure 1. Investment and utility cost in the integrated columns system.
assume that reboiler and condenser heat flow rates are almost
the same. Therefore, distillation columns are presented with
(I A T rectangles. hot and the cold utilities. An additional intercolumn heat
In process design a distillation column sequence often deter- exchanger area results in savings for both utilities. As the invest-
mines the main part of the process costs with regard to the total ment in equipment increases, the utilities cost decreases. The
annual costs. The scope of every process design is to minimize difference between the savings (S) and the annualized depreci-
the total costs, which comprise total utilities and equipment ation cost (D,) represents the total savings ( S T ) resulting from
costs. Utility costs depend on the type of the utility (its price), the heat integration (Equations 1 and 2).
the duty in condensers (cold utility, (I,,,,) and reboilers (hot
utility, QC), (see Figure 1) (Sobotan and Clavit, 1998; Sobotan S = @ . c,,
and Clavit, 1999a).
In the absence of refrigeration, hot utility represents the main D,= 6 . AC
part of total utility cost. In the T-AI diagram, both utilities are
shown by straight lines. The equipment cost is proportional to
(3)
the condenser and reboiler heat flow rates and additionally to
condenser/cold utility and reboiler/hot utility temperature For our research a fixed temperature difference of 15 K was
differences. The higher the temperature difference between the taken in the heat exchangers. 20% of the installed cost was
utility and the condenser and/or the utility and the reboiler, the considered to be the annual depreciation cost of equipment.
smaller is the condenser and/or the reboiler area. It is recom-
The integrated heat flow rates (@) from 50 kW to 10 000 kW
mended to keep the temperature difference between the utilities
were taken into account. Low pressure steam and cooling water
and the condenser or the reboiler as high as possible (Figure 1).
were considered for the calculations of utilities cost (C,,).
In the heat exchanger network it is also recommended to keep
Coefficients A, 6 and C are used for estimation of investment
the area between the heat-integrated columns (intercolumn
cost. Figure 2 indicates that utilities savings cash flow is much
area) as large as possible (Malek and Clavit, 1994; Sobotan and
higher than the additional depreciation cost of the heat
Clavit, 1998). Promising sequences are those with the best hot
exchangers. The total savings ST (Figure 2) increase exponen-
and cold streams integration inside the whole separation process.
tially with the integrated heat flow rate. The lefthand scale of
Our idea was to develop an effective criterion for finding and
Figure 2 refers to savings and depreciation, whereas the right-
determining the best heat-integrated distillation columns
sequence. In order to handle the minimum possible number of hand one refers to total savings. The temperature difference of
candidates for promising schemes it should eliminate sequences 15 K represents a value taken only for this research. In the case
with non-promising possibilities for heat integration. The of lower temperature differences (for example 10 K) heat
integrability criterion measures the ability for heat integration. exchanger investment costs are higher and the total saving
If we want to understand this idea better, we have to study a curve has a lower slope (Figure 2).
problem in the T-A1 diagram (Figure 1).
The objective function is the sum of the total utility consump- Max Criterion
tion plus the total annual depreciation cost of the process. Each In the case of a multicomponent separation the predominant
heat-integrated unit presents a saving which reduces both the utilities consumption takes place in distillation columns. Every

The Canadian Journal of Chemical Engineering, Volume 78, October 2000 909

hatRar8tSILW
F i g u r e 2. Influence of utilities savings and additional depreciation cost
on total saving.
T/OC
hot utility area
cold utility area
I +
A M(k W )
Figure 3. Z($, ATe) values criterion in J-Al diagram.
unit using hot or cold utilities contributes to total costs. So the
main target in process integration is to make use of every avail-
able hot or cold stream in order to substitute utilities. The more
columns are connected to a heat flow cascade, the higher is the
profit of heat integration. Heat is transferred from a condenser
of a distillation column or from a process stream with a higher
temperature to a reboiler of another column or to a process
stream with a lower temperature. The greatest benefit is to
make the highest possible extent of condenser-reboiler matches.
Maximum heat transfer between the two columns is desired.
The cost of the intercolumn heat exchanger increases with
the increase of heat exchanger area. The higher the tempera-
ture difference A T between the columns, the smaller is the heat
exchanger area and the lower its cost. We want to reach the
highest possible heat flow rate exchange with the highest possible
temperature differences between the integrated columns.
Each pair of heat-integrated columns represents a saving
which reduces hot and cold utilities. The larger is the area
between the integrated columns, the higher is the saving of
heat integration. lntercolumn temperature differences are
marked by subscript e (ATe). The ( Q j ATe)-product between the
condenser of one column and the reboiler of the other one is a
good criterion for heat integration effectiveness (Figure 3). The
idea is to maximize the intercolumn's Z Qi -value and also to
maximize the intercolumns ATe values. The criterion Max): (QjATe)
was found to be a very good indicator of the promising heat-
910
integrated sequences (Sobotan and Clavit, 1999a). This crite-
rion actually gives good information about the ability of distilla-
tion columns for heat integration, Large T-Al area between the
integrated distillation columns stimulated the idea to develop
even a better criterion than the MaxZ (4; AT,) one.
Ability for heat integration depends on many parameters. To
have the maximum intercolumns areas in the T-Al diagram, we
want to design heat-integrated distillation columns with the
smallest possible heat flow rates of condensers and reboilers
and simultaneously with the smallest possible span of tempera-
tures in each distillation column, that is the minimum rectangle
(intracolumn) area. Smaller condenser and reboiler heat flow
rates result in lower utilities consumption. Distillation columns
with a small span of temperatures give large AT'S between the
source and the sink in the match and have good possibilities for
heat integration. Thus, the area between integrated distil\ation
columns is maximized (Sobotan and Clavit, 1999a).
Min Criterion
In our research we want to show the importance of the thermo-
dynamic properties of a multicomponent feed mixture which
has to be separated into pure components. These properties
dictate the sizes of distillation columns and the utilities required
for the desired separations. In chemical processes, other hot
and cold streams exist besides those of the distillation columns.
Therefore, it is often possible to integrate reboiler and condenser
streams with other process streams. As an effective aid the
integrability criterion (fI) was introduced. It is defined as a
product of temperature difference between the reboiler and the
condenser in the same column and its heat flow rates. It also
includes the possibility for integration of distillation columns
with other process streams. In the case of more distillation
columns the integrability criterion is defined as a sum of individ-
ual intracolumn Qt ATo products (Equation 4). lntracolumn
temperature difference is marked by subscript a (ATo). For
approximation we take an average value of the potential
condenser and the reboiler heat flow rates (Equation 5).
(4)
(5)
Some authors propose the Qf ATo values to be constant for a
single distillation task over a wide range of pressures. Our
detailed research shows that this is not always true. Qt ATo values
for a single distillation task can vary over a wide range of
pressures. Absolute I$~ ATo values can reach differences up to
150% compared to the values at atmospheric pressure. Qt ATo
values of some separations have been calculated in the range of
operating pressures from 0,l MPa to 0,8 MPa for our Case
Study 2. Graphical presentation is shown in Figure 4. Only 5
different distillation tasks (BCDEF, see box in Figure 4) were
selected to confirm our statements. Here Qt ATo values vary from
150 MW K to 450 MW K (52% to 150%) compared to the
values at the atmospheric pressure. Curves represent the change
of ATo values for different splits with regard to operating
pressure. Capital letters in the box signify the key components
which have to be separated ( B being the lightest and f the
heaviest one).
Integrability criterion represents the sum of intracolumn
areas in the T-Al diagram (see Figure 5). For simplification,
The Canadian Journal of Chemical Engineering, Volume 78, October 2000

+g1
-3-1
- 5 m
ECDF
0 1 I distillation (self standing) columns system and to a six-components
0.1 0.2 p?a 0.4 0.8
Figure 4. Comparison of ATo values in different splits for Case Study 2.
4 R1
b 6. Select sequences with the lowest sum of $, ATo values.
4
b
Al/kW
Figure 5. Integrability criterion in T-LU diagram.
condenser and reboiler heat flow rates of individualcolumns are
assumed to be equal. Thus, each column can be represented by
a T-Al rectangle. In most cases this column rectangles are in fact
trapezoids. The objective is to reduce the span of temperatures
of the column trapezoids. This will increase the possibility of
stacking more columns in series and thereby the heat recovery
between columns and thus reduce the overall utility demand.
Also, lower heat exchanger area and reduction of depreciation
cost will result from higher A T between the columns.
The smaller is the intracolumn temperature difference (ATo)
and the intracolumn heat duty ($) in the T-Al area, the smaller
ATo will be. Additionally, distillation columns with small intra-
column areas have better ability for heat integration. It means
that a distillation column can be heat-integrated with some
other distillation column or with a process stream. In practice
this usually results in a potential intercolumns condenser-
reboiler match.
The size of the column trapezoids varies with the composition,
heat capacities and flow rates in the condenserheboiler and
with the temperature difference between key components
which have to be separated. In the case of more difficult separa-
tions the temperature difference between the light-key and the
heavy-key component is small, but condenser and reboiler heat
flow rates are large.
The Canadian Journal of Chemical Engineering, Volume 78. October 2000
Design Procedure
In our investigation we have developed a short cut synthesis
method for finding the best structure of a heat-integrated distil-
lation system. Only distillation is used as a separation operation.
First, we studied a distillation column sequence only (Case Study 1)
and then an entire plant (Case Study 2). The process was studied
as a total plant, not only as a distillation column sequence. We
tried to find possible integrations between a distillation train
and a whole process system in the extended grand composite
curve. The procedure was applied to a five-components isolated
process-separation system. We can describe the process design
method with the following procedure:
1. Analyse thermal structure of the process.
2. Identify all possible splits.
3. Analyse each possible split according to $, ATo values.
4. Determine possible sequences.
5. Calculate $, ATo values for the splits of sequences.
7. Analyse the best sequences economically.
8. Select promising schemes.
The procedure developed in this work is based on the dimen-
sions of distillation columns represented in the T-Al diagram.
The goal is to integrate columns to a cascade where the heat
will be transferred from the condenser of one column to the
reboiler of another one or from a condenser to the process,
respectively. Maximum energy transfer between the two columns
is desired. This is achieved by the maximization of intercolumn
areas. It is the area between the condensers of the columns with
higher temperature and reboilers of the columns with lower
temperature. We named it the intercolumn area, because it is
placed between the integratedcolumns shown in T-Al diagram.
The larger the intercolumn area the higher the utilities saving.
Distillation columns with small span of temperatures have better
possibilities to yield large intercolumn areas.
In our previous work we developed the criterion which was
based on the MaxZ(@;AT,) products between the condenser of
one column and the reboiler of the other one (Sobotan and
Clavit, 1998). It was found to be a good criterion for effective
heat integration. It was used in the case of isolated distillation
columns, where distillation train was studied without consider-
ing any other process units, e.g., reactors or other heat sources
or sinks. In this work we wanted to use the above-described
minimization of intracolumn area sum to determine the ability
for heat integration (Equations 4 and 5). Distillation columns
with small intracolumn areas (Mine, ATo) will be more able to
be integrated with other columns or with process streams.
lntracolumn area minimization implies intercolumn maximiza-
tion and therefore, their intercolumn area (Max$, A < ) will also
be large enough to achieve utilities savings. The integrability
criterion was hoped to be a good one for the ability of exten-
sive heat integration. It upgrades the criterion from our earlier
work and is more convenient for processes where streams other
than the column ones appear.
Case Studies
Application of a Simple Synthesis Method
We studied two different case studies with the procedure
proposed. Both case studies were treated under the same
design procedure as discussed earlier. In the first step we
analyzed the thermal structure of the process (in the isolated
distillation columns system this step was left out). We separated
911
the process into a fixed and a variable part. With the fixed part we
Table 1. Feed compositions and properties for Case Study 1.
describe the part of the process which is not exposed to thermal
changes. Heat flow rates and temperatures of heaters and coolers Feed amount rll Relative volatility
are held constant because of the nature of the process. It is not Component fraction, xi ("c) (a) 4s'
necessary that this part is physically separated from the variable
part of the process. In the variable part thermal changes can A / propane 0.05 -42 2.00 5.26
occur. Further analyses refer to the variable part only. B / i-butane 0.15 -12 1.33 8.25
In the second step we identified all the possible splits in the C / n-butane 0.25 -0.5 2.40 114.55
5-and 6-components systems (Case Study 1 and Case Study 2, D / i-pentane 0.20 29 1.25 13.46
E/n-pentane 0.35 36 1.00 -
respectively). In the third step the splits identified were
simulated by using a range of operating pressures. For each split "Asterisks in Table 1 designates the coefficients of ease of
appropriate I$+ AT,-value was calculated. Determination of separation (CE3 (Nadgir and Liu, 1983). It is defined as:
possible sequences was the following step (step 4). The Qt ATo
values were calculated for the optimum pressure. The sum of C, = r Ai
the $t ATo values gave the F,-value for the sequence (step 5).
The results showed that utilities consumption usually rises where r is the ratio of the amount flow rates of products (distillate
monotonously with the rising pressure. In this case it is econom- and bottoms) F$FD or fdFBdepending on which of the two
ically more favourable to operate at higher pressures. Typical ratios is smaller than or equal to unity; and A, is either a boiling
deviations were shown in Figure 4. point difference between two components to be separated
A, = AT, or A2 = (a- 1) 100 with a being the relative volatility
Steps 6, 7 and 8 led to the promising sequences with their or separation factor of the two components to be separated
total annual cost analysis. (Rajah and Polley, 1995).

Cose Study 1
To demonstrate the effectiveness of the present method, two
complex case studies were selected. The first one (Case Study 1)
i s a self-standing distillation columns separation problem of a
five components hydrocarbon mixture. It is a well-researched
case study, also known as Rathore's Problem (Kattan and Douglas,
1986; Nadgir and Liu, 1983). The mixture with the composition
shown in Table 1 is to be separated into pure products. Feed
flow rate is 252 mol/s. This is a standard problem which is
generally used to test separation scheme synthesis algorithms.
The feed stream contains five light alkane components, avail-
able as a saturated liquid at atmospheric pressure.
The most promising heat-integrated sequences for Case
Study 1 are presented in Table 3. The numbering of sequences
is taken according to Figure 6 where all the flowsheets are shown.
The task is to develop a process which would separate each
mixture into pure components with lowest total annual cost. To
simplify the calculations, the following assumptions were used
for both case studies (also in Case Study 2, which will be
described later) (CACHE Case Study, 1984):
1. Minimum approach temperature (ATmi,) is held constant at
10 K.
2. Column feed and product streams are saturated liquids.
3. Vapour recompression, inter-reboilers and inter-condensers
are not allowed.
4. Each distillation column operates a t 98% recovery of the key
components.
5. The cost of changing the temperature and pressure of the
intermediate streams is negligible compared to the rest of
the sequence cost.
6. The reflux ratio (Rs) in distillation columns is held constant at
the value of 1.2RM,,.
7. Only total condensers and total reboilers are used.
8. Heat transfer coefficients are held constant at 568 W/(m2 K)
in all heat exchangers.
9. Sequences with the lowest minimum utility requirements are
favoured.
These simplifications are a usual procedure in many articles in
the past and reflux ratio is held constant at the value of 1.2RM,,
(Kattan and Douglas, 1986; Mizsey and Fonyo, 1990). We fixed
Table 2. Annualized utility cost (CACHE Case Study, 1984;
Rajah and Polley, 1995; Rathore and Powers, 1974).
Utility Annual Cost, C,/(USD/kW)
Cooling water T I 18°C 27.8
Cooling water 18°C 5 J 5 40°C 16.2
Steam, 138°C 76.3
Steam, 160°C 84.4
Steam, 180°C 94.2
Steam, 200°C 100.6
I
the reflux ratio and varied the pressure. Varying of reflux ratio
of course can lead to other optimal solutions. The process
simulator, ASPEN PLUS, was applied for the simulation of both
case studies (ASPEN PLUS, 1988). The ASPEN module DSTWU
was used for the simulation of distillation columns sequences. It
performs shortcut design calculations for a single-feed, two-
product distillation column with a total condenser. It uses
Winn's method to estimate the minimum number of stages,
Underwood's method to estimate the minimum reflux ratio and
Cilliland's correlation to estimate the required reflux ratio for a
specified number of stages or reverse. It assumes constant
amount overflow and constant relative volatilities (ASPEN PLUS,
1988). The ASPEN property option for nonpolar or mildly polar
mixtures (SYSOP5) was chosen (Oreski and Clavit, 1997).
The economy of different sequences was estimated by using
techniques described in literature (Hui and Ahmad, 1994, Smith
and Linnhoff, 1988; Sobotan and Clavit, 1998, Swaney, 1989).
The annual operating time of 8500 h was taken into considera-
tion. The cost of equipment was calculated by Cuthries method
(Cuthrie and Grace, 1969) using ASPEN PLUS process simulator
and 20Y0 of the installed cost was considered to be the annual
depreciation cost of equipment. Prices used for utilities cost
estimation were shown in Table 2.

912 The Canadian Journal of Chemical Engineering, Volume 78, October 2000
 Table 3. Comparison of integrability criterion and total annual cost ranking in Case Study 1.

CTA C,I'l CTp MaxZ(t$iATJ Minyt$[AT&

No. Sequence (M USD) (M USD) (M USD) (MW.K) (kW.K)

1. SEQ-2 2.289 2.51 7 0.864 160.1 710

2. SEQ-5 2.304 2.539 0.871 150.1 852
3. SEQ-1 2.324 2.549 0.858 127.2 a57
4. SEQ-9 2.573 63.8 950

"1Kattan and Douglas (1986).

14Nadgir and Liu (1 983).

results, but a better one as the classification suggested by the

heuristic method (Nadgir and Liu, 1983).
For the comparison we analyzed the heat-integratedprocess
by using heuristic rules. According to the heuristic rules in Case
Study 1, the promising heat-integrated sequence was the
sequence SEQ-1. Comparison with the literature shows that in
the Case Study 1 the best three heat-integrated sequences
(SEQ-2, SEQ-5, SEQ-1) all have the most favourable FI values
(compare the results in Table 3).
The selection of sequences with the best F, values was based
on the minimum areas of $, ATa trapezoids. The $, ATa values of
the splits in distillation columns sequences were summarized.
The sequences were classified according to the rising 9,ATa
values. Those with the minimum sum of qt AJa values were
found to be the best candidates for the promising sequences
after heat integration.
Sequences with very large Z($, AJ,) values were shown as
very cost inconvenient and should not be taken into account for
calculations after heat integration. The best heat-integrated
Figure 6.Sequences studied by using the integrability criterion in sequences were also classified according to the MaxZ($; AT,)
Case Study 1 . criterion, which was demonstrated to be an equivalent criterion
for heat integration effectiveness (see Figure 5) in Case Study 1.
The optimal process flowsheet of Case study 1 is shown in
Figure 7 (D1 - D4 = distillation columns).

,
In the detailed analysis we estimated costs separately for the
fixed and for the variable part of the process. The cost of the
fixed part was the same for all sequences. Changes occurred in
the variable part.
For the comparison we classified the sequences according to
total annual cost. For the heat integration effectiveness the
integrability criterion was found to be a very good measure for
the ranking of the most promising heat-integratedsequences.
It includes two most important factors which have a decisive
influence on the total annual cost: heat flow rates of condensers/
(DE) Qb' , split
ABCIOE
DIE
Alec
B/C
@Pa
-~
592
101
995
594

reboilers and the span of temperatures in the column. Distillation

columns with smaller span of temperatures are more appropri-
ate for heat integration.
The best heat-integrated sequences were those with the
lowest Fl values. We can establish that the ranking determined
by the integrability criterion FI [MinE($, AT,)] is similar to the
total annual cost ranking. For the comparison we classified the
sequences according to the MaxZ($, AJe) values (see Table 3).
Table 3 compares only four best sequences because they are
the only ones available in the literature (Kattan and Douglas,
1986; Nadgir and Liu, 1983). Comparing the MaxZ($; AT,)
values criterion with the MinZ(@,A J), values, both give the same Figure 7. The optimal process flowsheet for Case Study 1 .

The Canadian Journal of Chemical Engineering, Volume 78, October 2000 9 13

 In Case Study 1 the ability for heat integration given by the
integrability criterion shows its usable value. It is indicative for Table 4. Feed compositions and properties for Case Study 2.
the selection of the best sequences. The T-A1 diagram of the
best heat-integrated sequence (Figure 5) in Case Study 1 is Feed amount fraction, 1s
-
shown in Figure 8. Key components i' "C CES*

Case Study 2 A acetaldehyde 0.43 21 42.25

B ethyl acetate 0.01 77 0.79
The second case study, the so-called process system, is a separa-
C ethanol 0.34 78 6.21
tion problem of a six-products mixture resulting from acetalde- 100 4.79
D water 0.20
hyde production by ethanol dehydrogenation. The composition E n-butanol 0.01 117 0.01
of the mixture is shown in Table 4. The total feed flow rate is F acetic acid 0.01 118 -
4 kg/s, its temperature is 31 5 K and its pressure is 101.32 kPa
I
(CACHE, 1984). Actually, there is a seventh component, hydrogen,
but it is separated in an absorber (A in Figure 10).
In Case Study 2 the same short cut method as in Case
Study 1 was applied. The promising heat-integrated sequences ABCDEF ~-
WCDEF UDEF ~- DIEF EF

are shown in Figure 9. Results of the best heat-integrated

sequence were compared with the ranking resulting from the ABCDEF ~ WCDEF UDEF __- DEIF ~ DIE
integrability criterion. These are shown in Table 5.The situation
<
-. ~ .

in Case Study 2 is more complex than in Case Study 1. The ABCDEF __ EKDEF ~ CDEF 'ID
E/F

TPC STEAM STEAM

ABCDEF ~ - WCDEF ~ COW ~ CDIE GQ

n-n ABCDEF ___ BUDEF < F: : EIF

ABCDEF -- BUDEF <' "

w......q
DEIF __ DIE

EK
ABCDEF BCDEF
50

Figure 9. Sequences studied by using integrability criterion in Case

D4 Study 2.
25
> COOLING WATER
MinZ($, ATo) criterion was confirmed to be more effective than
the MUXZ($~ ATe) one in Case Study 2 (compare the results of
b
both criteria in Table 5).
AkW
5 10 15 20 In Case Study 2, operating pressures in the columns
Figure 8. T-Al diagram of the best heat-integrated sequence in Case sequences were cascaded downwards as the separation
Study 1 (see Figure 5). proceeded, approaching the ambient one. This was intended in

Table 5. Comparison of integrability criterion and total annual cost ranking in Case Study 2.

CJA MinZ@, AT,,) MaxZ($, AT,,)

C,['I CJA'
Rank Sequence (M USD) (kW.K) (kW.K) ranking ranking

1. SEQ-7 1.464 342 37.0 SEQ-6 SEQ-1

2. SEQ-6 1.487 353 21.7 SEQ-7 SEQ-2
3. SEQ-3 1.732 3 74 65.0 SEQ-8
4. SEQ-1 1.777 385 58.4 SEQ-1 SEQ-3
5. SEQ-4 1.829 428 62.9 -
*This is the ranking according to total annual cost before heat integration

"INadgir and Liu (1 983).

914 The Canadian Journal of Chemical Engineering, Volume 78, October 2000
order to keep the cost of changing stream pressures at the
minimum and to allow safer operation (if the columns were
near ambient conditions). Thus, the purchase of new compres-
sors and pumps for increasing pressures in distillation columns
was avoided. The annual operating time for the production of
acetaldehyde was 8500 h. The optimal process flowsheet of the
case study 2 is shown in figure 10 ( D = distillation column).
T-A/ diagram of the best heat-integrated sequence in Case
Study 2 is shown figure 11. For the sake of simplification,
condenser and reboiler heat flow rates are asumed to be equal.
Therefore, distillation columns are presented by T-l rectangles.
In Case Study 2 only the F, criterion classification was used. This
criterion has been proved as better and more effective than the
MaxZ(Qi AT,) one since in Case Study 2 the Max criterion did
not give optimal heat-integrated sequences. Other process
I n
r
I - J L l . . F
Figure 10. Process flowsheet for Case Study 2.
H P steam
300 { better ability for heat integration.
250 f very important for finding the best sequences and it was shown
II
- also helpful, because sequences enabled classification of alter-
200
\ natives in an economic order. The F, criterion is more appropri-
streams have influence on the heat integration in this case and,
therefore, intercolumns area is not the only important criterion
for the total annual cost classification.
In Case Study 2 the C,, coefficient for the A/BCDEF separation
is by far the highest. Therefore, we expect that all the best heat-
integrated sequences will have the A/BCDEf separation as the
first one. The optimal sequence obtained by using a simple
heuristic method (Nadgir and Liu, 1983) was the integrated
sequence 6 (SEQ-6). Our method showed this sequence to be
the second-best in the total annual cost ranking after heat
integration having the second lowest sum of the 9,ATa values.
Obeying the non-integratedheuristic rules only the second-best
sequence is SEQ-7 and the third one SEQ-8, which is only the
eighth-best after total annual cost ranking after heat integration.
Discussion and Conclusions
The method described so far is applicable to the analysis and
synthesis of heat-integratedprocessing systems. It is convenient
for process systems with distillation columns trains. The advan-
tage of the method is its simplicity, ease of use, and clarity of
thermodynamic characteristics of the particular modifications.
The limitation of the method is that it does not give the correct
results on the thermodynamic boundaries. It means that reboiler
and condenser heat duties differ very much. Wrong simulation
data can also lead to the wrong promising sequences. It does
not have the mechanism for avoiding the high temperature
heating and low temperature cooling.
The method proposed needs less information about the
process than other approaches. The desired data are condenser
and reboiler heat duties and their temperatures. Besides the
range of operating parameters this is the main information for
applying the synthesis method.
The method proposed has successfully been applied to five-
and six-component mixtures separation problems. It was found
to be an effective guide in synthesizing the most promising
heat-integratedsequences. It confirmed the importance of heat
integration and facilitated the most promising structures to be
found. Thermodynamic properties of a feed mixture are decisive
for the determination of the best heat-integrated sequences.
Distillation columns ranking has the greatest influence on the
total annual cost. Economic comparison of sequences indicates
that the most cost favourable ones are those with the lowest
L$, ATa values. These sequences have low utilities consumption,
low span of temperatures within the columns and, therefore,
The F, criterion proved its important role. Obviously, it was
to be very effective. Our ranking of sequences into groups was

-
M P Steam
ate for classification of distillation columns sequences in complex
case studies. Obviously, process dimensions of T-I rectangles
are decisive for heat integration.
D6
100 The MinZ(Qt ATa) criterion has been proved as better and

50 J I D I 3
more effective than the MaxZ(QjATe) criterion. Both criteria
gave the same ranking of the best heat-integratedsequences in
more simple case (Case Study l), but MinZQ, ATa criterion had
I Cooling water better screening properties and was more usable in complex
processes as demonstrated in Case Study 2.
2000 4000 6000 8000 10000 A ~ w The ranking of sequences in the case of the stand alone distil-
Figure 11. T-Al diagram of the best heat-integrated sequence in Case lation columns is more simple (Case Study l). Here only distil-
Study 2. lation columns, i.e., their reboiler and condenser heat flow rates,

The Canadian Journal of Chemical Englneerlng, Volume 78. October 2000 9 15

define the depreciation and utilities costs. The situation is more
complex in Case Study 2 where there are other process streams,
too. Hot or cold streams could have their supply and target
temperatures in a very wide range. In spite of all that the f,
criterion was effective in both cases.
The main advantage of the method compared to the
algorithmic and evolutionary ones is its screening value. It elimi-
nates inappropriate sequences and reduces the time needed for
finding the promising sequences. It is not completely programmed
yet and it is some kind of half-automated procedure. Therefore,
we cannot compare computational times of different approaches
but in the term of calculations by hand it is faster than other
approaches only but heuristics. The method is simple to apply
and use without any special computational knowledge but
process simulation. It gives identical optimum sequences as the
more rigorous and time-consuming computer methods and it is
more promising than heuristic ones.
It should be pointed out that no controllability or operability
evaluation was applied to the analysis. Distillation columns
could be very sensitive to changes in operating conditions and
may not be controllable. So controllability may prove to be a
major limitation in implementing such a scheme in practice.
Therefore, one of the future goals is to implement controllability
measures into our future work.
We shall try to apply this knowledge in the optimization of
other thermally integrated multicolumns processes and for
optimization process variables which have been kept fixed so far.
Acknowledgement
The authors gratefully acknowledge the Ministry of Science and
Technology of Slovenia who provided money for the research.
Nomenclature
heat exchanger area, (m2)
coefficient, (USD)
coefficient in to Equation (2)
coefficient of ease of separation, defined by Equation (1)
total annualized cost, (USD/a)
total annual utility cost, [USD/(w,a)]
depreciation cost, (USD/a)
amount flow rate of bottoms product, (mol/s)
amount flow rate of overhead (distillate) product, (mol/s)
integrability criterion, (W.K)
enthalpy flow rate, (w)
distillate to bottom amount flow rate ratio, F,,/f, or F,/F,
minimum reflux amount ratio, (mol/mol)
savings, (USD)
total saving, (USD)
boiling temperature, (“C)
Creek Symbols
a relative volatility of key component to be separated
A, AT or (a- 1) x 100
AT temperature difference, (K)
ATe intercolumn temperature difference between the condenser and
the reboiler, (K)
ATo intracolumn temperature difference between the condenser and
the reboiler, (K)
916
ATmin minimum approach temperature, (K)
$, intercolumn heat duty, ON)
intracolumn heat duty, ON)
$cu cold utility heat duty, ON)
$c condenser heat duty, ON)
$HU hot utility heat duty, ON)
$R reboiler heat duty, ocv)
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The Canadian Journal of Chemical Engineering, Volume 78, October 2000