8724 Ind. Eng. Chem. Res.

2008, 47, 87248740

Optimal Design of Mixed Refrigerant Cycles

Frank Del Nogal, Jin-Kuk Kim,* Simon Perry, and Robin Smith
Centre for Process Integration, School of Chemical Engineering and Analytical Science, The UniVersity of
Manchester, PO Box 88, Manchester, M60 1QD, U.K.

A new approach for the optimal design of mixed refrigerant cycles is presented. It is based on mathematical
programming and offers significant improvements in relation to previous approaches. It includes multistage
refrigerant compression, full enforcement of the minimum temperature difference in heat exchangers,
simultaneous optimization of variables, consideration of capital costs, and the use of stochastic optimization
(genetic algorithm) to overcome local optima. The approach can be applied to either single mixed refrigerant
cycles or to systems consisting of two of these in cascade. The effectiveness of the method is illustrated by
revisiting previously published liquified natural gas case studies, for which better and feasible solutions are
produced, and which prove the importance of considering multistage compression and capital costs during
optimization. The application of genetic algorithms in the design of mixed refrigerant cycles permits a greater
confidence in the optimality of the results.

1. Introduction details of the mathematical formulation and optimization strategy

Most low temperature processes feature one or more refrig-
eration cycles with the purpose of removing heat from subam-
bient hot streams. The provision of a cryogenic cooling requires
significant power demands for compression, and it is very
important to achieve high energy efficiency in the design and
operation of refrigeration cycles, leading to low carbon emis-
sions to the environment.
In a simple system with a closed refrigeration cycle, the heat
is removed by vaporization of a low pressure refrigerant which
is then compressed and condensed at a higher pressure against
a warmer cold utility or heat sink. The condensed liquid is let
down in pressure (and temperature) by means of an expanding
device such as a throttle valve. When cooling for a wide
temperature range is required, a complex arrangement (for
example, a cascade cycle or a cycle with multilevel cooling) is
introduced to improve thermodynamic efficiency of the refrig-
eration systems.
On the other hand, using mixed refrigerant (MR) in the
refrigeration cycles provides very promising potential to yield
more efficient, yet simple and reliable systems in comparison
to pure refrigerant ones, because a mixture of refrigerants is
evaporated isobarically, not at a single but in a range of
temperatures. Although there are important natural applica-
tions for MR cycles (e.g., LNG), their optimal design has not
been the object of extensive research as in the case of pure
refrigerant systems. Therefore, to explore advantages using
mixed refrigerants in low temperature cooling, it is the aim of
this paper to develop a systematic design and synthesis
optimization framework for MR systems. The new design
methodology provides systematic investigation of design inter-
actions as well as optimal and economic design of MR systems.
First, a brief overview is made regarding the design problems
being tackled in the area of mixed refrigeration systems, which
is followed by the review of existing literature as relevant to
the optimal design of MR systems, identifying improvement
opportunities and gaps in the existing design practice. Next,
the optimal design of MR systems is presented, in which the
* To whom correspondence should be addressed. E-mail: j.kim-2@
manchester.ac.uk. Tel.: +44 (0)161 306 8755. Fax: +44 (0)161 236
7439.
10.1021/ie800515u CCC: $40.75 2008 American Chemical Society
Published on Web 10/18/2008
are provided for both single MR systems and MR systems in
cascade, including multistage compression and typical flowsheet/
equipment variations. Finally, the proposed approach is il-
lustrated with two case studies.
2. MR Systems
2.1. Pure Refrigerant and MR Cycles. A major limitation
of vapor compression cycles that make use of pure components
as refrigerants is that refrigeration is provided at a constant
temperature while the cold refrigerant is evaporating. For a
chosen refrigerant, the temperature at which cooling is provided
is a consequence of the evaporator pressure, that is, the saturation
temperature.
If the hot streams (streams that need cooling) demand the
cooling task to be carried out along a wide temperature range,
a system providing all the refrigeration at a single level is likely
to have a poor performance. This is because large temperature
differences would exist in the heat exchanger(s), moving the
system away from thermodynamic reversibility, and hence, from
thermodynamic efficiency. That being the case, a multilevel pure
refrigerant system is likely to be implemented, in an attempt to
reduce the temperature differences in the system, as seen in
Figure 1, in which three pressure levels are used to provide
refrigeration at three temperature levels. However, both heat
transfer area and complexity would increase as a consequence.
The refrigerant compressor would need as many stages as
refrigeration levels.
Multicomponent, or mixed refrigerants, unlike pure refriger-
ants, undergo isobaric phase change through a range of
temperatures contained within the dew and bubble temperatures
of the mixture. Given the right pressures and compositions, a
good match between the process and refrigerant temperature
profiles can be obtained with a simple configuration, as shown
in Figure 2. Although refrigerant compression can take place
in several compression stages with intercooling, only one stage
is shown in the illustration for simplicity. A practical maximum
pressure ratio per compression stage (usually 4-5 for industrial
applications) is likely to define the number of compression
stages, rather than the number of pressure levels, since in this
case the cold refrigerant evaporates at a unique pressure (or
through a small pressure range, if friction pressure drop is
 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8725

Figure 1. A three-level pure refrigerant cycle.

Figure 2. A MR cycle.

Figure 3. A self-cooling MR cycle.

accounted for in the evaporator). Care should be taken, however,

since the reduced average temperature difference would lead
to increased heat transfer area. A minimum temperature differ-
ence (T min) should be established for practical design purposes.
Since the benefits of using MR cycles are highlighted in
situations where refrigeration is to be provided along wide
temperature ranges, these types of cycle find a natural applica-
tion in the liquified natural gas (LNG) industry, where refrigera-
tion is required from ambient temperature to around -160 C. Figure 4. A three-stage MR cycle.
2.2. Flowsheet Variations of MR Cycles. An interesting
flowsheet variation in MR cycles is the one shown in Figure 3, external heat sink but also to itself, once expanded. In this way
where the high pressure refrigerant rejects heat not only to an the hot refrigerant is further cooled down, probably subcooled,
8726 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008
Figure 5. MR structure used by Vaidyaraman and Maranas.6
Figure 6. MR system diagram.
before expanding, allowing the cold refrigerant to reach a lower
temperature and/or a lower vapor fraction after the expansion.
Such a benefit is achieved at the expense of a higher heat transfer
area, since the total duty in the heat exchanger increases
significantly. A multistream heat exchanger can be used to
handle all hot streams and the cold stream in a single piece of
equipment. This process is known as the Pritchard cycle and is
described in more detail by Walsh.1
Repeated partial condensation and separation of the refrigerant
stream has been reported to achieve a better match between the
temperature profiles.2 However, this should not be taken as a
general rule. Figure 4 shows a MR cycle with three refrigeration

Figure 7. Temperature feasibility check.
stages, as an extension of Figure 3a. Although increasing the
number of stages may reduce the power consumption, the design
also grows in complexity and probably in capital cost. This
results in an important tradeoff for designers.
2.3. Multistage Compression. As compressors used in
industry have a practical maximum stage pressure ratio of
around 4-5, it is very common to find compression tasks
performed in multiple stages. Further, if there is an appropriate
cold utility, the partially compressed gas originating from a given
stage may be cooled down before entering the next compression
stage (intercooling). The lower temperature of the partially
compressed gas reduces the volumetric flowrate and in conse-
quence reduces the compression power of the next stage. If part
of the gas condenses, then it is necessary to remove the liquid
so that a dry vapor stream enters the next compression stage.
The liquid removed is then pumped and mixed with the fully
compressed gas and with any liquid streams from other
intercoolers at the outlet of the last compression stage at same
pressure. Condensate removal and pumping also helps in saving
power, as increasing the pressure of liquids is much cheaper in
power (and capital) than doing so with gases.
3. Literature Review
Although there are many publications on the analysis of MR
systems, only a few exist on their optimal design using
mathematical programming. The earliest attempt to optimize
these systems in a systematic manner was carried out by Ait-
Ali.3 This work tackled the optimization of an MR system with
the same configuration as a two-level pure refrigerant system.
The focus was largely on minimizing total compression power
by trying to enforce a constant temperature difference through
the cryogenic heat exchangers. Although rich in practical
considerations and insights relevant to LNG production, refrig-
erant pressures and flowrates were not the result of optimization,
but rather set heuristically. Different solution procedures were
required depending on the number of components present in
the refrigerant. Also, to handle the complexity of the problem,
only binary and tertiary mixtures were considered and the
thermodynamic accuracy had to be sacrificed by using an
equation of state based on ideal solution assumptions and
Raoults law for vapor-liquid equilibrium, which restrict the
validity of the numerical results to low pressure and warm
temperature conditions. The optimization method was limited
to a two-dimensional numerical search. Refrigerant subcooling
and separation of liquid and vapor refrigerant streams at
Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8727
intermediate temperatures were not addressed, neither was
cascading heat to a different refrigeration cycle.
Lee4 (part of this work was also published as Lee et al.5)
worked on the optimal design of multistage MR cycles. Given
a refrigeration task in the form of a hot composite curve (a
combined temperature-enthalpy profile of all hot streams) and
the number of refrigeration stages, his approach allows for the
optimization of key variables in a process flowsheet of the type
shown in Figure 4. In principle, the optimization variables are
the refrigerant composition and flowrate (at compressor inlet),
the compressor inlet and outlet pressures, and the intermediate
temperatures (at which refrigerant is separated into vapor and
liquid streams). However, the decision variables are not
optimized simultaneously. Instead, the refrigerant compositions
are optimized at fixed refrigerant flowrate and pressures using
nonlinear programming (NLP). Once the optimal composition
is obtained, the hot and cold temperature profiles are checked
for feasibility. If they do not cross, then new refrigerant flowrate
and pressures are proposed on the basis of heuristics, judgment,
or optimization. And the procedure is repeated until no further
improvementispossiblewithoutincurringtemperatureinfeasibilities.
Lee4 also used three different types of objective function.
Two of them tried to match the temperature profile of the cold
refrigerant to an ideal profile (the hot composite curve shifted
down by Tmin) by minimizing either the maximum violation
of the minimum temperature difference or the sum of such
violations along the profile. The third possible objective function
was the minimization of compressor power, but its use was not
recommended until the final part of the overall optimization.
That is because, since there is no constraint on the vapor fraction
at the inlet of the compressor, it is less likely to have wetness
at the compressor inlet toward the end of the overall optimization
due to a probable lower value of the refrigerant flowrate.
The design of MR cycles is a highly nonlinear problem with
many local optima. One of the main drawbacks of Lees
approach is that the nonsimultaneous optimization of variables
coupled with the dependence of the final solution on the initial
guess, on the nonsystematic selection of refrigerant flowrate and
pressures (especially if updated using heuristics or judgment)
and on the switching of the objective function, makes reaching
the global optimal solution (or a good near-optimal solution,
for practical purposes) very unlikely.
In Lees method, the minimum temperature difference
between the hot and cold temperature profiles is not fully
enforced, which often leads to very tight profiles, apart from
relying on human intervention at each iteration to check for
8728 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008
temperature feasibility. It is assumed that the refrigerant
compression takes place in one stage with no intercooling,
regardless of the compression ratio. No capital costs are
considered during the optimization procedure.
Lee4 also explored the synthesis of more complex systems
such as MR cycles in cascade with pure refrigerant cycles. In
his approach, although the partition temperature between the
two cycles was subject to optimization, each cycle was
optimized separately to minimize compression power for an
assumed value of partition temperature. The partition temper-
ature was then iterated manually in an outer loop until the total
power was considered optimal. Again, this nonsimultaneous,
nonsystematic optimization of variables is likely to lead to
nonoptimal solutions, as discussed before.
Another relevant precedent in the synthesis of multistage
MR cycles is that by Vaidyaraman and Maranas,6 which is
also based on NLP. The cycle topology used by them is the
one shown in Figure 5a. Although in principle it may look
very different, it is just a slight variation of the type of
structure in Figure 4, only that the liquid refrigerant stream
is not subcooled after each flash step, as shown in Figure 5b
as an alternative representation. The variables being opti-
mized in this case were the refrigerant composition (at the
stream being expanded in the last stage), the compressor inlet
and outlet pressures and the vapor fraction at flash drums 2
to N. All the design variables (each with a fixed number of
stages) were optimized simultaneously.
Two key assumptions were made by Vaidyaraman and
Maranas.6 The first one was that the hot refrigerant leaving stage
N was at its bubble point, and the second one was that the cold
refrigerant streams leaving each stage were at their dew point.
These assumptions, although not unreasonable, constrain the
solution space unnecessarily and could lead to good opportuni-
ties missed by the optimizer. Another major shortcoming of the
method proposed is that temperature feasibility is only enforced
at the ends of the heat exchangers. This opens the possibility
of not only minimum temperature difference violations but also
of temperature crossovers being overlooked during the optimi-
zation. Although the authors suggest that, if violated, feasibility
might be regained after the optimization by correcting the
refrigerant pressures, doing so could lead the solution to lose
its optimality.
As in Lee,4 Vaidyaraman and Maranas6 assumed single stage
compression without intercooling and did not consider capital
costs. However, they made a further effort in trying to overcome
local optima by performing a number of optimizations with
different starting points. The effect of refrigerant pressure drops
was not covered in their formulation.
In overall, the review of previous work on MR systems
reveals a quite significant potential for improvement. An ideal
design approach would be one that combines (a) flexibility
to handle flowsheet options such as multiple refrigeration
stages, refrigerant subcooling, and cascade systems, (b)
energy-efficient features, such as multistage compression, (c)
a systematic optimization framework powerful enough to
exploit the relevant degrees of freedom and to overcome the
challenges of a highly nonlinear problem, (d) no assumptions
on the thermodynamic state of refrigerant streams just for
the sake of a simplified calculation procedure, (e) full
feasibility enforcement, and (f) the cost consequences of the
design decisions. A design approach like this is not yet
available in the open literature, and in order to overcome
shortcomings addressed in above, a novel, systematic and
robust procedure for the optimal design of low temperature
processes is proposed in the next section.
4. Design and Optimization Frameworks
Figure 6 shows a generic multistage MR cycle and a
multistage compression system with intercooling, indicating
some of the nomenclature used in the formulation. Variables
for the hypothetical refrigeration stage 0 and compression stage
0 were included in order to simplify the formulation. Also, for
the sake of a compact formulation, some calculations are not
described explicitly. These are represented as functions of the
type f(x1,..., xN) and are mainly routine physical property
calculations (e.g., enthalpy for a given set of compositions,
temperature, and pressure) and temperature profile operations.
It is assumed that all hot streams leaving each multistream heat
exchanger are at the same temperature.
Objective Function. Equation 1 represents the objective
function as a generic function of the main process variables.
This objective function may well change from case to case
according to the purpose of the designer (e.g., minimum
compressor power, minimum capital investment, minimum total
cost, etc.) and to the economic models used.
OBJECTIVE )
OBJ(WC, QCMP, THCOMP, HHCOMP, TCCOMP, HCCOMP, ...) (1)
Stage Material and Energy Balances. Equations 2-7
establish the relationship between the total flows of the streams
around the system. Equations 2-4 describe the continuity of
vapor and liquid hot refrigerant stream flows from stage to stage.
The hot vapor refrigerant stream is made unavailable at the NRth
stage because of the inexistence of a flash drum at stage NR-1
(eq 5). All the material arriving to stage NR from stage NR -1
is put through the hot refrigerant liquid stream for formulation
purposes, although part of it might not be in the liquid state.
Equations 6 and 7 represent the material balance of the mixers.
Fn ) FVn + FLn (2)
Fn ) FVn-1 (3)
FVn ) VF(Yn-1, TIn-1, PHn-1
OUT
) n e NR - 1 (4)
FVNR ) 0 (5)
FCn ) FLn + FCn+1 n e NR - 1 (6)
FCNR ) FNR (7)
Vapor and liquid compositions are obtained from phase
equilibrium calculations at each flash drum (eq 8 and 9) although
in practice the vapor and liquid compositions are obtained
simultaneously from a single flash subroutine. The composition
of the only hot refrigerant stream in stage NR must be the same
as that of the hot vapor refrigerant at the previous stage (eq
10). Equation 11 states that the total composition of the cold
refrigerant at each stage is the same as that of the hot vapor
refrigerant at the previous stage and is derived from component
balances carried out around the first n - 1 stages as a group.
Yn ) ZVAP(Yn-1, TIn-1, PHn-1
OUT
) (8)
Xn ) ZLIQ(Yn-1, TIn-1, PHn-1
OUT
) n e NR - 1 (9)
XNR ) YNR-1 (10)
Zn ) Yn-1 (11)
The heat removed from hot refrigerant streams at each stage
is calculated in eq 12 and 13. The initial and final values of the
 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8729
IN
vector of intermediate temperatures (TI) are set to TR and at the inlet of stage NR, the inlet cold refrigerant temperature
TPOUT, respectively, for consistency with the input data (eqs is the same as the one after expansion (eq 27).
14 and 15), although TI0 and TINR are not actual intermediate
temperatures. Since the refrigeration task is assumed to be given hCnIN )
in the form of a precalculated process composite curve (PR, FLn hTP(Xn, TnEXPN, PLnIN) + FCn+1hTP(Zn+1, TCn+1
OUT
, PLnIN)
HPR), eq 16 calculates the heat removed from the process
FCn
stream(s) at each stage according to the enthalpy difference of
such a curve between the respective pair of adjacent intermediate n e NR - 1 (25)
temperatures, the exception being stage 1 (eq 17), because in
n ) ThP
TCIN Zn, hCIN n e NR - 1
IN
( n , PLn ) (26)
principle the initial process temperature (TPIN) might be different
from the initial hot refrigerant temperature (TI0 ) TRIN).
IN
TCNR ) TNR
EXPN
(27)
Equation 18 ensures that the total heat removed from the hot
Pressure, Temperature, And Enthalpy Profiles. Accurate
streams is absorbed by the cold refrigerant stream at each stage.
pressure drop predictions across heat exchangers, especially of the
As a result, the cold refrigerant outlet enthalpies and temper-
compact type, may result in a quite lengthy calculation task, since
atures can be determined as a result of an energy balance (eqs
details of the actual exchanger geometry and internals (e.g., type
19 and 20).
of fins), as well as a set of additional fluid transport properties, are
QVn ) FVn[hTP(Yn, TIn, PHOUT required for such a purpose.7 If a rigorous calculation of such kind
n ) - hTP(Yn, TIn-1, PHn-1
OUT
)] was implemented in the present formulation it would increase the
(12) mathematical complexity considerably, taking the focus away form
the main design variables. On the other hand, neglecting the
QLn ) FLn[hTP(Xn, TIn, PHOUT
n ) - hTP(Xn, TIn-1, PHn-1
OUT
)] pressure drops in the cycle could lead to overlooked infeasibilities
(13) because of an inaccurate prediction of temperature profiles and/or
to a nonoptimal and/or subdesigned system. In the present for-
TI0 ) TRIN (14) mulation, an intermediate point is adopted. The total hot refrigerant
pressure drop (PHNR OUT
-PH0OUT) has a fixed value defined by the
TINR ) TPOUT (15) user before the optimization (PHOT), which allows the estimation
of intermediate hot refrigerant pressures by approximating them
QPn ) EVAL(TPR, HPR, TIn) - as a linear function of the respective temperature, as shown in eq
EVAL(TPR, HPR, TIn-1) n g 2 (16) 28. A similar approximation is performed to obtain the intermediate
cold refrigerant pressures (eq 29). However, these are assumed as
QP1 ) EVAL(TPR, HPR, TI1) - EVAL(TPR, HPR, TPIN) a linear function of the temperature of the hot refrigerant, instead
(17) of that of the cold refrigerant for convenience in the sequential
simulation approach.
QCn ) - (QVn + QLn + QPn) (18)
TIn - TRIN
FCnhTP( Zn, TCIN IN
n, PLn ) + QCn PHOUT
n ) PHOUT
0 - PHOT (28)
hCOUT
n ) (19) TP OUT
- TR IN
FCn

TCOUT ) ThP(hCOUT IN
, PLn-1 ) (20) TIn - TRIN
n ) PL0 +
PLIN IN
n n PCOLD (29)
The enthalpy of the refrigerant after expansion is calculated TP OUT
- TR IN

in eq 21. Depending on the value of the user defined binary For a given composition and inlet and outlet temperatures, the
parameter YLEX, such an enthalpy will be set equal to either temperature-enthalpy profiles at each refrigeration stage are ob-
the inlet enthalpy (for YLEX ) 0, corresponding to Joule- tained by evaluating the stream enthalpy repeatedly at a number
Thompson valves) or to a function of the isentropic enthalpy of intermediate points, previously defined by the designer (i.e., the
of expansion and a constant isentropic efficiency (for YLEX ) number of points, not the points themselves), within the respective
1, corresponding to liquid expanders). The enthalpy of isentropic temperature range. A linear behavior of refrigerant pressure with
expansion is calculated in eq 22. The refrigerant temperature temperature is also assumed during the calculation of the
after expansion is given in eq 23. When expanders are used, eq temperature-enthalpy profiles. Cold refrigerant pressures, this time,
24 will calculate the associated power produced. Otherwise this are estimated according to the cold refrigerant temperatures and
power would be implicitly forced to zero as in such case there not those of the hot refrigerant as done previously. Extra evaluation
is no enthalpy difference. points are added at the exact dew and/or bubble points of the
mixture if found within the temperature and pressure range. The
hEXPN
n ) (1 - YLEX)hTP(Xn, TIn, PHOUT
n )+ functions TPROF and HPROF are in practice one single function
YLEX(1 - LEX)hTP(Xn, TIn, PHOUT
n ) + LEXhISLEX
n (21) being shown separately for formulation purposes. The hot vapor
refrigerant, hot liquid refrigerant, and cold refrigerant profiles are
hISLEX
n ) hsP(Xn, sTP(Xn, TIn, PHOUT
n ), PLIN
n ) (22) defined in eq 30 to 35.
TEXPN
n ) ThP(Xn, hEXPN
n , PLIN
n ) (23) THVn ) TPROF(TIn-1, TIn, PHn-1
OUT
, PHOUT
n , Yn)
WLEXn ) FLn(hEXPN
n - hTP(Xn, TIn, PHOUT
n )) (24) n e NR - 1 (30)
The inlet cold refrigerant temperature to any given stage HHVn ) HPROF( OUT
TIn-1, TIn, PHn-1 , PHOUT
n , Yn, FVn )
featuring an inlet mixer (stages 1 to NR -1) can be calculated n e NR - 1 (31)
(Equation 26) after its enthalpy is known through an energy
balance around the mixer (Equation 25). Since there is no mixer THLn ) TPROF( OUT
TIn-1, TIn, PHn-1 , PHOUT
n , Xn ) (32)
8730 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008

HHLn ) HPROF(TIn-1, TIn, PHn-1

OUT
, PHOUT
n , Xn, FLn) (33) th - TEV(HCCOMP
n , TCCOMP
n , HEV(THCOMP
n , HHCOMP
n , th)) g
TCn ) TPROF(TCIN OUT
, PLIN IN Tmin th THCOMP (46)
n , TCn n , PLn-1, Zn) (34) n

Compression. In practice, stages belonging to the same

HCn ) HPROF(TCIN OUT
n , TCn , PLIN IN
n , PLn-1, Zn, FCn) (35) compressor feature pressure ratios not too different from each
Since the overall process composite curve is given as an input other. Identical pressure ratios are therefore not an unreasonable
to the problem, the process profiles at each stage are obtained assumption. However, allowing dissimilar pressure ratios would
by just extracting the corresponding data within each respective mean more degrees of freedom during optimization, which may
range of temperatures. The overall process profile input to the bring the advantage of an even further improvement of the
problem should consider the effect of pressure drop. The process objective function value (e.g., total compression power) and/or
data extraction is performed in eq 36-39. If the process a more flexible matching with mechanical drivers. The formula-
composite curve was not an input to the problem, the process tion in this work is flexible and allows both approaches;
profiles could be constructed using a similar method as for the dissimilar compression ratios subject to optimization when full
refrigerant profiles. exploitation of the degrees of freedom is required and an
identical compression ratio approach in case a simpler optimiza-
TPn ) CROP(TPR, TIn-1, TIn) ng2 (36) tion is desired.
Equation 47 ensures that the values of stage pressure ratios
TP1 ) CROP(TPR, TPIN, TI1) (37) are consistent with the compressor inlet and outlet pressures.
The discharge pressures of each compression stage are then
HPn ) CROP(HPR, TIn-1, TIn) ng2 (38)
calculated by eq 48. Equations 49 and 50 enforce minimum
and maximum limits to the stage pressure ratios. In case the
HP1 ) CROP(HPR, TPIN, TI1) (39)
designer would like to perform the optimization assuming
Equations 40-43 combine all the hot profiles to form a single identical pressure ratios, the unique variable PR would replace
hot composite curve in each stage. Equations 44 and 45 obtain the set of variables PRi in the problem formulation. Equation
the stage cold refrigerant composite curves. 51 states that the number of stages is such that the
compression task would not be possible with one stage less.
THCOMP
n ) TCOMP(THVn, THLn, TPn, HHVn, HHLn, HPn) Although this may appear redundant with eq 47, it is
n e NR - 1 (40) necessary for the identical pressure ratio approach since in
that case the unique variable PR is not controlled by the
COMP
TH ) TCOMP(THLNR, TPNR, HHLNR, HPNR) (41) optimizer. As a consequence, there may be more that one
NR
set of NC and PR values that satisfy eqs 47, 49, and 50
HHCOMP
n ) simultaneously, and to ensure the number of stages is not
HCOMP(THVn, THLn, TPn, HHVn, HHLn, HPn) ne excessive, eq 51 has to exist in order to define the minimum
number of stages as the design criteria in that situation.
NR - 1(42)
NC

PR ) PH
COMP
HH ) HCOMP(THLNRTPNR, HHLNR, HPNR) (43) PLIN
0 j
OUT
0 (47)
NR j)1

TCCOMP ) TCOMP(TCn, HCn) (44) i

PR
n
PCMP
i ) PLIN
0 j (48)
HCCOMP
n ) HCOMP(TCn, HCn) (45) j)1

Once the hot and cold composite curves are known at each PRi e PRMAX (49)
stage, the temperature feasibility at each stage can be evaluated
by comparing the temperature of the hot composite curve to
PRi g PRMIN (50)
that of the cold one for a given enthalpy. Such comparison is
performed at each enthalpy point belonging to the hot composite NC-1
curve. If the temperature of the cold composite evaluated at a PHOUT
0 > PLIN
0 PR
j)1
j (51)
given enthalpy is greater than that of the hot composite then a
temperature cross occurs. If the temperature of the cold Equation 52 avoids any wetness in the cold refrigerant stream
composite is lower than that of the hot composite by less than from refrigeration stage 1, which is the stream entering the
Tmin then a violation of the minimum temperature difference compression train. Equations 53 and 54 make the compression
occurs. If the temperature of the cold composite is lower than nomenclature consistent with that of the remainder of the
that of the hot composite by at least Tmin then the point is cycle.
perfectly feasible. This temperature feasibility check is per-
formed by eq 46 and further illustrated in Figure 7. Checking TCOUT
1 g TDEW(Y0, PLIN
0 ) (52)
feasibility for a couple of points only will not ensure overall
feasibility for heat transfer throughout overall temperature range, PCMP
0 ) PLIN
0 (53)
whereas employing a large number of discrete points with very
YCMP
0 ) Y0 (54)
small interval will significantly increase computational time in
the optimization. Various numbers of points have been tested, Equations 55-59 establish refrigerant flowrates and composi-
and in this study, around 30 points (together with extra tions around the compression system in consistency with
evaluation points, depending on the characteristics of composite phase equilibrium and stage material balances. It is assumed
curves) were taken, which was enough to check feasibility of that all the partially compressed streams can be cooled down
heat recovery in exchangers without using excessive computa- to a temperature TRIN by an external heat sink and that any
tional resources. liquid that is formed is separated, pumped to the final
 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8731
pressure, and remixed before the final cooler, in accordance WLEXn ) FLn(hEXPN - hTP(Xn, TIn-1, PHn-1
OUT
)) (24b)
n
with Figure 6b.
THCOMP
n ) TCOMP(THVn, TPn, HHVn, HPn)
YCMP
i ) ZVAP (CMP
Yi-1 , TRIN, PCMP
i ) i e NC - 1 (55) n e NR - 1 (40b)
XCMP
i ) ZVAP Yi-1
CMP
, TRIN, PCMP
i ( ) (56) HHCOMP
n ) HCOMP(THVn, TPn, HHVn, HPn)
n e NR - 1 (42b)
FCMP
i ) Fi-1
CMP CMP
VF Yi-2 (
CMP
, TRIN, Pi-1 ) ng2 (57)
5. Solution Strategy
FCMP
1 ) F1 (58)
The optimization problem, as formulated in the previous
FPi ) FCMP
i - Fi+1
CMP
i e NC - 1 (59) section, is of the NLP type: Minimize eq 1, subject to constraints
Stage compression power is calculated in eqs 60 and 61on the 2-64 (with variations 13b, 21b, 29b, 30b, and 37b-40b, if
basis of the stage flowrate and enthalpy difference. Stage outlet appropriate).
enthalpy is calculated using a constant isentropic efficiency in However, not all the formulation has been explicit (e.g., phase
eq 62 and 63, the last one being derived from the definition of equilibrium and physical property calculations), and in practice
isentropic efficiency. Stage pumping power is calculated in a part of the calculations may take place in external subroutines
similar way by eqs 64-66 (e.g., interfacing with commercial process simulators). Also, as
stated before, the problem is nonlinear and features many local
WCi ) FCMP
i (hCMP
i - hTP Yi-1
CMP CMP
, TRIN, Pi-1 ( ) ng2 optima. Traditional deterministic optimization methods would
(60) get readily trapped in these. On the other hand, stochastic
methods (e.g., genetic algorithm, simulated annealing) may offer
WC1 ) FCMP (hCMP - hTP(YCMP , TCOUT , PCMP )) (61) more confidence on the optimality of the final solution at the
1 1 0 1 0
expense of computational time. A genetic algorithm (GA) has
hISCMP
i ) hSP Yi-1
CMP
( CMP
, sTP Yi-1 CMP
, TRIN, Pi-1 (
, PCMP
i ) ) (62) been chosen as the main optimizer in this work. Genetic
algorithms try to copy nature regarding the evolution of species.
hCMP
i ) (1 - c)hTP Yi-1
CMP
(
CMP
, TRIN, Pi-1 + chISCMP
i (63) ) They perform iterations not on a single candidate solution but
on a population of candidate solutions (individuals) instead. The
(
WPi ) FPi hPi - hTP XCMP
i (
, TRIN, PCMP
i )) i e NC - 1 path toward optimality is built by sharing information between
individuals (reproduction) and by evaluating and ranking the
(64)
resulting offspring according to their relative optimality (fitness)
in a given number of major iterations (generations). The
i (
hPi ) (1 - p)hTP XCMP , TRIN, PCMP
i + phISPi ) information defining a particular individual (chromosome)
i e NC - 1 (65) consists of a set of values of the chosen independent variables
(genes), over a discretized solution space, encoded as a string
(
hISPi ) hsP XCMP
i , sTP XCMP
i (
, TRIN, PCMP
i , PHOUT
0 ) ) (e.g., binary encoding, real encoding). Another key advantage
i e NC - 1 (66) of GA is that no initial guess is needed to start up the
Finally, eq 67 calculates the heat removed at each intercooler optimization process. Further details on how genetic algorithms
except for the one after the last compression stage, which is work can be found in books such as Goldberg8 and Stender et
calculated in eq 68 based on an energy balance around the last al.9
intercooler and all the mixers in conjunction. Pikaia,10 a genetic algorithm by the U.S. National Center for
Atmospheric Research, has been adopted in this work and
QCMP
i ) FCMP
i ( (
hTP Yi-1
CMP
, TRIN, PCMP
i - hCMP
i ) ) modified in order to improve the quality of the initial generation.
i e NC - 1 (67) Randomly generated individuals are now evaluated before being
allowed into the initial generation. They qualify as a member
CMP
QNC ) F1hTP(ZCMP
i , TRIN, PH) - of the initial generation only if excessive infeasibilities are not
incurred (e.g., average crossovers of no more than 3 C and a
NC-1
i)1
(hPi FPi ) - FNC
CMP CMP
hNC (68)
compressor inlet temperature at most 2 C below dew point),
Adaptation for Hot Liquid Refrigerant without Subco- otherwise they are rejected. This filter, although it increases the
oling. MR cycles without hot liquid refrigerant subcooling, as computational time for the first generation considerably, ensures
in Figure 5, are a particular case in the formulation above. If a departure from a better set of candidate solutions, shortening
such a cycle was to be represented, some constraints would the path to optimality. For case studies in this paper, 9095%
change: Namely, all QLs would be equal to zero; the refrigerant of candidates are rejected during the filtration step.
expansions would start at conditions TIn-1 and PHn-1 OUT
, instead Figure 8 illustrates the flow of information within the general
OUT
of TIn and PHn ; there would not be need for calculating any optimization framework. The optimizer (GA in this case)
hot liquid refrigerant profile (i.e., eqs 32, 33, 41, and 43). The proposes a series of candidate solutions and relies on the
equations to be modified are shown below as variations b of simulator for their assessment. How the optimization task
the original equations: evolves is decided by the optimizer on the basis of the
assessment of the candidate solutions. The interactions between
QLn ) 0 (13b) the GA and the simulator result in a set of the best solutions
found over a discretized solution space. Standard NLP optimiza-
hEXPN
n ) (1 - YLEX)hTP(Xn, TIn-1, PHn-1
OUT
)+ tion(s) can be carried out afterward having the best discretized
YLEX(1 - LEX)hTP(Xn, TIn-1, PHn-1
OUT
) + LEXhISLEX
n (21b) solution(s) as initial guess in order to fine-tune and finally report
the optimal solution on the basis of a continuous solution space.
hISLEX
n ) hsP(Xn, sTP(Xn, TIn-1, PHn-1
OUT
), PLIN
n ) (22b) Both the optimizer and the simulator have been implemented
8732 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008

Figure 8. Optimization strategy. Figure 9. Composite curves for the base case optimal solution.
Table 1. Temperature-Enthalpy Data of the Natural Gas Stream to Table 2. The Three Solutions for the Base Case
Be Liquefied
new method Lees method new method
temperature (C) enthalpy (MW)
Tmin (C) 5.0 1.2 1.2
25.0 20179 power (MW) 33.49 26.60 24.53
-6.0 18317 F1 (kmol/s) 3.47 3.2 3.53
-34.1 16353 PL0IN (bar) 2.40 3.7 4.84
-57.7 14468 PH0OUT (bar) 36.95 40.0 43.87
-70.1 11978 Z1 (mol %)
-74.6 10198 N2 15.32 11.0 10.08
-82.3 7114 CH4 17.79 27.3 27.12
-96.5 5690 C2H6 40.85 35.6 37.21
-115.0 3840 C3H8 0.41 5.20 0.27
-163.0 0 n-C4H10 25.62 20.9 25.31

in FORTRAN 77 and within WORK, part of the process design
software suite available from the Centre for Process Integration
at the University of Manchester. This gives the user the choice
of using either built-in thermodynamic property models or
delegating these calculations to commercial process simulators
such as HYSYS or Aspen Properties that would run in the
background.
The chosen independent variables for this application are the
refrigerant flowrate (F1) and composition (Z1), the compressor
inlet and outlet pressures (PHOUT and PLIN
0 0 ) and the intermediate
temperatures (TI1 to TINR -1) for cycles with two stages or more.
Given the values for all these variables, the simulator is
responsible for calculating the remaining variables and the
magnitude of infeasibilities (e.g., temperature profiles and
compressor inlet wetness) and evaluating the objective function.
Penalties may be applied to the objective function according to
the magnitude of the infeasibilities as a disincentive in the
ranking of solutions incurring violations. However, during
optimization, care should be taken in removing design candidates
with considerable magnitude of infeasibilities in the objective
function since infeasible solutions (especially the slightly and
moderately infeasible) may still contain features worthy to
inherit and evolve by offspring candidate solutions.
6. Case Study 1
The problem formulation and optimization strategy discussed
in the previous section are put into practice using the same LNG
case study published by Lee.4 A pretreated natural gas stream
is to be cooled from 25 C down to -163 C using a mixture
of nitrogen, methane, ethane, propane, and n-butane as refriger-
ant in a single stage cycle (as in Figure 3a) using minimum
compression power as the objective function. Subcooling of
liquid refrigerant is allowed and compression takes place in one
stage. External cold utility is available to cool hot streams down
to 30 C. The minimum temperature difference is 5 C, the
isentropic compression efficiency is 80%, and the physical
properties calculations are based on the Peng-Robinson equa-
tion of state (WORK built-in). Refrigerant expansion occurs in
Joule-Thompson valves and the refrigerant pressure drop across
the heat exchangers is neglected. The temperature-enthalpy data
of the natural gas are given in Table 1.
6.1. Base Case Solution. The application of the new
methodology results in an optimal solution with a compression
power of 33.39 MW. The composite curves for this solution
are given in Figure 9. The optimal solution reported by Lee,4
on the other hand, had a compression power of 26.60 MW,
which is 20.6% lower than the one found with the new
methodology. However, it must be considered that because the
minimum temperature difference was not fully enforced, Lees
solution ended up with an effective Tmin of approximately 1.2
C. Hence, for the comparison to be really meaningful, the base
case was reoptimized with the new methodology and Tmin of
1.2 C, finding an optimal solution that features 24.53 MW of
power, that is, 7.8% lower than in Lees solution. The three
solutions discussed are reported in Table 2. Note that a
temperature approach as tight as 1.2 C may result as impractical
as it is unlikely to handle the normal operational variations that
may occur in the plant once constructed. In practice it is unlikely
that temperature approaches of less than 3 C are considered
during design. Solving the base case involved the optimization
of seven variables and took 410 min in a Pentium IV processor
(3.0 GHz) with 512 Mb of RAM.
6.2. Effect of Multistage Compression. It is worth noting
that all three solutions presented in the previous section have a
compressor outlet temperature of no less than 140 C. A gas
undergoing compression at such temperatures certainly occupies
a relatively high specific volume and hence demands a relatively
high specific compression power. To illustrate the effect of
multistage compression, another design task was performed. This
time the maximum stage pressure ratio was set to 5 and the
minimum temperature difference back to 5 C. The resulting

Figure 10. Compression train for optimal solution with maximum stage pressure ratio of 5.
Figure 11. Tmin sensitivity for two-staged refrigeration cycles.
minimum power solution has total compression power of 27.87
MW, which is 16.8% lower than the minimum power found
when optimizing for a single compression stage (33.49 MW).
Details are shown in Figure 10. The compression train features
three stages with a pressure ratio of 2.95 each. The total
intercooler duty was also reduced from 53.67 to 48.15 MW.
Although the refrigerant composition is similar to that of the
base case optimal solution, meaningful differences are observed
in the refrigerant flowrates (2.81 against 3.47 kmol/s before)
and in the compressor inlet and outlet pressures (1.76 against
2.40 bar and 45.06 against 36.95 bar). It seems that now that
the compression process is more efficient, the system can afford
a larger total pressure ratio (25.6 against 15.4) in exchange for
a reduction in the refrigerant flowrate, the net effect being the
observed reduction in total power while still keeping good care
of temperature feasibility in the cryogenic exchanger.
If the compression ratios are not assumed identical but
allowed to vary as additional degrees of freedom during
optimization, the optimal power exhibits a slight further
reduction to 27.57 MW. In that case the compression ratios for
the three compression stages are 3.57, 2.83, and 2.30, respec-
tively, which are approximately within (20% of the 2.95 that
resulted when assumed identical.
One could be tempted to say that a multistage compression
model is not needed at the synthesis stage because the power
consumption can be reduced after optimizing the cycle for a
single compression stage by just increasing the number of
compression stages afterward. However, doing so in the case
study reduces the total power only to 30.18 MW; still 2.31 MW
above the 27.87 MW found when considering the effect of
multiple stages during optimization. One possible reason for
this is the unattractiveness of exploring high total pressure ratios
when minimizing power in a cycle with a single compression
stage, as discussed in the previous paragraph.
6.3. Two-Stage Refrigeration and Capital Cost Effect. A
two-stage MR cycle was also optimized in a sensitivity analysis
with a maximum stage pressure ratio of 5. The goal was to
Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8733
Figure 12. Composite curves for the optimal MR system with four
refrigeration stages.
picture the effect that the predefined minimum temperature
difference has on the minimum power solutions. The effect on
the total compression power can be seen in Figure 11a, where
the resulting power of each solution is plotted against the
respective value of Tmin. The monotonic trend was to be
expected. The closer the hot and cold composite curves are
allowed, the lesser the irreversibilities in the process and hence
the lesser the total compression power. Note that the optimiza-
tion for a Tmin of 5 C gave a solution with a power
consumption of 26.58 MW. This is 1.29 MW lower than the
solution reported in the previous section and due to the fact
that the refrigeration stages have been increased to two, which
in this case is helping to achieve a better match between the
composite curves in each stage.
The capital cost of the solutions appearing in Figure 11a are
plotted in Figure 11b also against the minimum temperature
difference. The capital cost considered for any given solution
includes the cost of the compressor and the cost of the cryogenic
heat exchangers. The latter are estimated using the method in
ESDU11 for aluminum-brazed plate-fin heat exchangers (PFHE),
which estimates the volume and cost of these on the basis of
the composite curves and typical heat transfer coefficients given
the type of application. This time the trend is not monotonic. A
8734 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008
Figure 13. General cascade of two MR cycles.
Figure 14. Optimization strategy for MR cycles in cascade.
minimum capital cost seems to exist somewhere between 1 and
5 C. This behavior is also not surprising. As the total power
decreases with decreasing Tmin, so does the compressor cost.
However, Tmin has the reverse effect on the volume (and cost)
of the PFHEs. The closer the composite curves are to each other,
the smaller the temperature driving forces and hence the larger
the heat transfer area, volume, and cost.
With the purpose of further investigating this compressor/
PFHE capital tradeoff, the minimum temperature difference
permitted during optimization was decreased to a negligible
amount and the objective of the optimization was changed to
minimum capital cost. In this way there would be no restrictions
on the temperature differences, apart from avoiding crossovers,
as long as the capital is minimized. The resulting solution is
also shown in Figure 11. In the point of closest approach
between hot and cold composite curves the temperature differ-
ence was 1.3 C. The total compression power is located slightly
above the power curve of minimum power solutions. However,
the capital cost is considerably below the cost curve of minimum
power solutions. The reason for this is that, apart from exploiting
the compressor/PFHE capital tradeoff, the resulting pressure
levels of the minimum capital solution are such that the
compression task can be accommodated in just two stages,
against the three needed in all of the minimum power solutions.
This reduction in the number of compression stages, albeit there
being the slightly increased total power, provided an additional
contribution toward the capital minimization due to the economy
of scale.
7. Refrigeration Systems in Cascade
In the previous case study, using two stages of refrigeration
allowed a 4.6% of reduction in the total compression power
when compared to a single refrigeration stage system with
multistage compression. In that case, a better match between
the composite curves was achieved because a favorable change
of the refrigerant flowrate and average composition occurred at
an intermediate temperature. However, this is not to be
generalized for systems with more refrigeration stages. It is not
always true that the more refrigeration stages there are in an
MR system of the type in Figure 5a, the lower is the total
compression power. In fact, when three refrigeration stages are
used in the given example, the minimum power solution requires
26.95 MW of compression power, a slight increase over the
26.58 MW of the optimal two-stage system, although still less
than the 27.87 MW of the optimal single-stage system.
Furthermore, the lowest possible compression power resulted
in 32.94 MW for an MR system with four refrigeration stages,
which is considerably more than in the case of one-, two-, and
three-stage systems.
The above behavior is because, with each additional refrig-
eration stage, an intermediate separation of the vapor and liquid
refrigerant streams is carried out, and this may introduce an
unfavorable change in the refrigerant flowrates and compositions
in the downstream refrigeration stage(s). These changes in turn
may make it difficult to achieve a good match between the
composite curves because the designer does not have a complete
control on the former. An illustration of this is shown in Figure
12, which corresponds to the optimal four-stage system. The
refrigerant flowrates and compositions in the different stages
are not completely independent from each other. They are very
much a consequence of the chosen overall refrigerant composi-
tion (the one through compression) and the intermediate
temperature between stages.
An alternative to increase the complexity within the same
refrigeration cycle to achieve a more efficient overall system is
to employ refrigeration systems in cascade. This is particularly

useful for refrigeration over wide temperature ranges and means
sharing the refrigeration duty between two or more cycles, where
the colder cycle(s) reject heat to the warmer one(s) and
eventually the warmest cycle rejects heat to an ambient utility.
The process stream(s) release heat to these cycles in decreasing
order of temperature for more efficiency. This is releasing as
much heat as possible to the warmest cycle, down to the first
so-called partition temperature, then releasing as much heat as
possible to the second warmest cycle, down to the second
partition temperature, and so on. The cycles within the cascade
do not have to be of the same nature (e.g., pure refrigerant,
MR, expander cycles). Cascaded cycles are commonly applied
in the LNG industry.
7.1. Optimal Design of MR Cycles in Cascade. A general
cascade of two MR cycles is shown in Figure 13. The process
stream(s), with an inlet temperature TPIN, release heat in the
upper (warmer) MR cycle, with NRU refrigeration stages, until
reaching the partition temperature TP, and then undergo(es)
further cooling in the lower (colder) MR cycle, with NRL
refrigeration stages, until the required final temperature TPOUT
is reached. After compression, the refrigerant in the lower cycle
rejects as much heat as possible to an external cold utility down
to the temperature TRIN before further heat rejection in the NRU
stages of the upper cycle, down to the partition temperature TP.
Then it is routed to the first of the NRL stages of the lower
cycle, where it undergoes self-cooling, phase splitting, and
expansion as in previously described noncascade MR systems.
In the upper cycle, the upper refrigerant rejects heat only to the
external cold utility down to the temperature TRIN before being
sent to the first of the NRU refrigeration stages. The upper
refrigerant is to provide cooling to the process stream(s) and to
the lower refrigerant.
The approach previously described in detail in the optimal
design of (noncascade) MR cycles can be adapted to a cascade
MR cycles without much difficulty. The basic idea of the
optimization framework in Figure 8 is still valid in this case
and an adaptation to a cascade cycle is presented in Figure 14.
The optimizer proposes a series of candidate solutions to be
evaluated by the simulator but this time the degrees of freedom
in both the upper and the lower cycles, along with the partition
temperature, are manipulated by the optimizer. The simulator
is to apply basically the same problem formulation described
previously to each cycle in order to evaluate the objective
function.
As the stage heat duties in the upper cycle depend on the
flowrate and properties of the MR stream received from the
lower cycle, the latter is simulated first. After this, the lower
MR cooling curve from TRIN to TP is computed and combined
with the process composite curve from TPIN to TP to produce
the effective process composite curve in the upper cycle. This
effective curve then defines the actual external refrigeration
duties in the upper cycle. The calculation of this lower cycle
cooling profile and of the effective process composite curve
for the upper cycle is represented by eq 69-72, which must be
added to the problem formulation in order to solve the upper
cycle. The effective composite curve data TPREF and HPREF
would replace TPR and HPR in the rest of the formulation when
applied to the upper cycle.
L 0, (PHL 0 - PLR), ZL1)
TLR ) TPROF(TIO, TP, PHOUT OUT
(69)
L 0,(PHL 0 - PLR), ZL1, FL1
HLR)HPROF(TI0, Tp, PHOUT OUT
(70)
Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8735
TPREF ) TCOMP(TPRU, TLR, HPRU, HLR) (71)
HPREF ) HCOMP(TPRU, TLR, HPRU, HLR) (72)
Other minor adjustments in the formulation include replacing
TPIN and TRIN with TP and PH0OUT with (PHOUT L 0 - PLR) in
the lower cycle model, except for the equations related to
compression, and TPOUT with TP in the upper cycle model. The
objective function remains as a unique equation and has to be
redefined as a function of the features in both the lower and the
upper cycles. The number of stages for both cycles can be treated
as integer variables, and consequently overall optimization
framework can be formulated with mixed-integer nonlinear
programming (MINLP). However, the optimization has been
carried out with nonlinear programming (NLP) with prespeci-
fying the number of stages employed in each cycle, in order to
avoid computational difficulties associated with the introduction
of integer variables.
8. Case Study 2 - MR Cycles in Cascade
The approach for the optimal design of MR cycles in cascade
will be illustrated by tackling a problem previously published
as a case study by Vaidyaraman and Maranas.6 A natural gas
stream contains 93 mol % of methane, 5 mol % ethane, 1.5
mol % propane, and 0.5 mol % n-butane and is to be chilled
from an inlet temperature of 19.85 to -58.15 C at a constant
pressure of 42 bar. A cascade of two MR cycles, with a varied
number of refrigeration stages each, provides the required
cooling. The hot liquid refrigerant streams are not subcooled
in the refrigeration stages and hence the variations b of eqs 13,
21, 22, 24, 40 and 42 must be used (eqs 32, 33, 41,and 44are
not required.). Contrary to the principles of an efficient system,
the process stream is not precooled in the upper MR cycle but
fed directly to the lower MR cycle. The former is only used for
heat rejection from the latter. As the intention of this case study
is to compare the results of the new design approach to those
from Vaidyaraman and Maranas,6 this flowsheet feature was
left untouched in order to make the comparison on the same
basis. Considering the above features, the generic flowsheet used
in this case study is shown in Figure 15. A further slight
adjustment of the problem formulation is required to model such
a process, the process stream(s) will not contribute to the
effective process composite curve in the simulation of the upper
cycle (i.e., TPRU and HPRU do not participate in eqs 71 and
72) and second, the process stream(s) enter the lower cycle at
the temperature TPIN instead of the partition temperature TP.
The refrigerants in the lower and the upper cycles contain
ethane, propane and n-butane. After compression in a single
stage, these reject heat to an external cold utility until reaching
a temperature of 36.85 C. The pressure drop of the refrigerants
through the system is neglected and the minimum temperature
difference allowed in the main heat exchangers is 2.5 C. The
Soave-Redlich-Kwong equation of state provides the basis
for physical property calculations, which for this case study are
performed by interfacing with Aspen Properties.
The objective of the optimization is to minimize the coef-
ficient of performance of the system for different combinations
in the number of lower and upper refrigeration stages. The
coefficient of performance (COP) in this case is defined as the
ratio between the total compression work and the amount of
heat released by the process stream. According to this definition,
the lower the COP the more efficient the system. If an arbitrary
flowrate for the process stream is chosen, then minimizing COP
would in practice be the same as minimizing total compression
power as the amount of heat released by the process is fixed.
8736 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008

Figure 15. Generic flowsheet for case study 2.

Table 3. Optimal COPs Obtained with the New Approach

NRU NRL ) 0 (no cascade) NRL ) 1 NRL ) 2 NRL ) 3
1 - 0.5415 0.5024 0.4566
2 0.5291 0.4485 0.4755 0.4951
3 0.5238 0.4266 0.4263 0.4805
4 0.5488 0.4790 0.4581 -

Table 4. Optimal COPs obtained by Vaidyaraman and Maranas6

NRU NRL ) 0 (no cascade) NRL ) 1 NRL ) 2 NRL ) 3
1 - 0.5890 0.4608 0.4623
2 0.5022 0.4547 0.4095 0.4298
3 0.4562 0.4144 0.3957 0.4124
4 0.4948 0.4226 0.4298 -

Table 5. Relative COP with the New Approach (100

COPNEW/COPPREV)
NRU NRL ) 0 (no cascade) NRL ) 1 NRL ) 2 NRL ) 3
1 - 91.91 109.00 98.73
2 105.33 98.61 116.08 115.17
3 114.80 102.85 107.77 116.48
4 110.88 113.31 106.55 -

The pressures of the refrigerants at the compressor inlet are

allowed to vary between 1.0 and 2.5 bar, the discharge pressures
between 4 and 10 bar, the compression ratios between 1.5 and
12 (but only a single compression stage) and the refrigerant
flowrates between 0.1 and 1.0 kmol/s, which is adequate for an
assumed 1 kmol/s of natural gas. The partition temperature is
allowed to vary between -40 and 10 C when a cascade is
present.
The optimal COPs encountered when applying the proposed
approach are presented in Table 3 for different combinations
of the number of stages in the lower cycle (NRL) and those in
the upper cycle (NRU). Details on each of these solutions can
be found in the Appendix. The COPs obtained with the previous
approach6 are shown in Table 4 for comparison purposes.
For more simplicity, Table 5 shows the relative improvements
in the system performance (COP) achieved with the new
approach. In only three cases it was possible to obtain lower
COPs, with the best saving over the previous method being
8.09%, in the case of one stage in the lower cycle and one in
the upper cycle. In most cases applying the new method resulted
in higher COPs, by up to 16.48%. However, contrary to what
one could initially think, this is evidence of the strength of the
new method rather than a weakness, as all the new solutions
Figure 16. Composite curves of the previous solution for three stages in
the lower cycle and three in the upper cycle.
are feasible ones. As discussed previously in the literature
review, the method by Vaidyaraman and Maranas6 enforced
temperature feasibility only at the ends of each refrigeration
stage. As a result, temperature violations are plentiful in the
previous results and an increase in the total power seems to be
the only way to regain feasibility.
For instance, assuming 1 kmol/s of natural gas, Figure 16
shows the composite curves of the lower and upper cycles that
correspond to the previous optimal solution for a system with
three stages in the lower cycle and three in the upper cycle.
This is the same case in which the new method yields the highest
relative COP increase as in Table 5. While the upper cycle
exhibits only a slight Tmin violation at the cold end of the
second stage, this violation is quite significant in the second
 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8737
flowrates in exchange for increased compression ratios. The net
effect is, as previously mentioned, a 16.48% of increase in the
COP (and total power) of the system but, nevertheless, a full
compliance with temperature feasibility.
The size of the problems solved in this case study ranged
between 5 and 16 variables subject to optimization, each case
taking between 77 and 295 min to solve in a Pentium IV
processor (3.0 GHz) with 512 Mb of RAM. Typical GA
parameters used in the optimization are population size )
1000, number of generations ) 600, crossover probability
) 0.85, mutation method ) one-point mutation with adjust-
able rate based on fitness, relative fitness differential ) 0.5,
steady-state-delete-worst reproduction, elitism technique is
applied.

9. Conclusions

The design of MR cycles is a challenging task. Also, local

optima are abundant. This paper has described and illustrated
the application of a new formulation and optimization strategy
for the synthesis of MR cycles. It considers multistage
refrigerant compression, full enforcement of the minimum
temperature difference along the temperature profiles, simul-
taneous optimization of variables, incorporation of capital
costs in the objective function and the use of stochastic
optimization (genetic algorithm) to overcome local optima.
The effectiveness of the method was illustrated by finding
improved and feasible solutions for two previously published
Figure 17. Composite curves of the new solution for three stages in the case studies. The incorporation of multistage compression
lower cycle (a) and three in the upper cycle (b). proved a key factor in the design of more efficient cycles
since it not only reduces the power consumption per se, but
Table 6. Comparison of Solutions for Three Stages in the Lower
Cycle and Three in the Upper Cycle also encourages the full exploration of total pressure ratios,
unlike the single stage case. Although only compressor and
previous approach new approach
PFHE capital costs were considered, the tradeoff between
TP (C) 14.59 0.32 these was illustrated, and how in practice this means that
FL1 (kmol/s) 0.499 0.396 the cost of power-related items is dominant in this type of
PLIN
L 0 (bar) 2.50 2.36
PHOUT systems. When applied to MR cycles in cascade, in some
L 0 (bar) 7.00 7.02
ZL 1 mol % cases it was possible to obtain new designs with improved
C2H6 32.80 46.62 thermodynamic performance against the results published in
C3H8 33.34 29.58 previous work. In most cases, however, the new solutions
n-C4H10 33.86 23.80
did not apparently exhibit a performance improvement but
TI L (C) -11.14, -35.01 -29.09, -51.17
nevertheless they were fully compliant with temperature
FU 1 (kmol/s) 0.552 0.4747 feasibility checks, unlike the previous work that enforced
PLUIN0 (bar) 2.50 2.50 this only at the ends of the heat exchangers and, as a
PHUOUT0 (bar) 4.20 5.22 consequence, intermediate Tmin violations and sometimes
ZU 1 mol %
C2H6 0.12 15.98 temperature crossovers occurred. Although it makes the
C3H8 12.76 6.81 solving process time-consuming and it still does not guarantee
n-C4H10 87.12 77.21 global optima, the application of a genetic algorithm opti-
TI U (C) 30.85, 16.53 18.07, 3.44 mizer to this design problem permits accepting the optimality
stage of the upper cycle. Furthermore, a slight temperature of the results with greater confidence than deterministic
crossover occurs. methods.
On the other hand, the composite curves of the optimal
solution found with the new approach are those in Figure 17, Acknowledgment
showing no crossovers or minimum temperature approach
violations. A more detailed comparison of both solutions is First author of this paper would like to thank the Centre for
presented in Table 6, with meaningful differences found in most Process Integration at the University of Manchester and the
variables, contrary to the suggestion by Vaidyaraman and Overseas Research Student Award Scheme for the financial
Maranas6 that any resulting infeasibility could be rectified with sponsorship of this project.
slight changes in pressure and still keep optimality. In general
the new solution (1) allocates a larger share of refrigeration to
the lower cycle than the previous solution (the partition Appendix
temperature is now more than 14 C lower), (2) features more Details on each of solutions found in case study 2 are listed in
methane and less propane and n-butane in the refrigerant Tables A1-A4. Refrigerant flowrates are per 1 kmol/s of natural
mixtures, and (3) is able to afford a reduction in the refrigerant gas.
8738 Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008

Table A1. Solutions with One Refrigeration Stage in the Lower Table A4. Solutions with four refrigeration stages in the lower cycle
Cycle
refrigeration stages in upper cycle
refrigeration stages in upper cycle
variable 0 (no cascade) 1 2 3
variable 0 (no cascade) 1 2 3
TP (C) - -11.67 11.55 -
TP (C) - -21.78 -16.39 -44.69 FL1 (kmol/s) 0.6337 0.5926 0.5060 -
FL1 (kmol/s) - 0.2019 0.2187 0.1834 PLIN
L 0 (bar) 2.461 2.499 2.499 -
PLIN
L 0 (bar) - 1.398 1.533 1.911 PHOUT
L 0 (bar) 9.690 4.397 7.193 -
PHOUT
L 0 (bar) - 7.064 9.588 9.069 ZL 1 mol %
ZL 1 mol % C2H6 0.3820 0.3902 0.4154 -
C2H6 - 0.5069 0.5297 0.5649 C3H8 0.1626 0.4723 0.2893 -
C3H8 - 0.1878 0.2843 0.0474 n-C4H10 0.4554 0.1375 0.2953 -
n-C4H10 - 0.3053 0.1860 0.3877 TI L (C) 10.60, -21.08, -24.20, -39.60, -12.61, -33.05, -
TI L (C) - - - -50.51 -50.86 -50.58

FU 1 (kmol/s) - 0.2381 0.3414 0.3703 FU 1 (kmol/s) - 0.3140 0.3239 -

PLUIN0 (bar) - 1.100 2.109 2.500 PLUIN0 (bar) - 1.743 2.451 -
PHUOUT0 (bar) - 8.849 6.421 8.773 PHUOUT0 (bar) - 9.042 4.845 -
ZU 1 mol % ZU 1 mol %
C2H6 - 0.0085 0.0546 0.1913 C2H6 - 0.0000 0.0322 -
C3H8 - 0.5701 0.3353 0.2599 C3H8 - 0.6131 0.1570 -
n-C4H10 - 0.4214 0.6102 0.5488 n-C4H10 - 0.3869 0.8108 -
TI U (C) - - 4.71 3.03, -26.50 TI U (C) - - 17.58 -

Nomenclature
Subscripts
Table A2. Solutions with Two Refrigeration Stages in the Lower i ) compression stage index
Cycle
L ) lower refrigeration cycle
refrigeration stages in upper cycle n ) refrigeration stage index
variable 0 (no cascade) 1 2 3 U ) upper refrigeration cycle
TP (C) - 3.29 -6.82 -5.92 Parameters
FL1 (kmol/s) 0.4138 0.3445 0.3529 0.3209
PLIN
L 0 (bar) 1.421 2.261 1.675 2.494 PCOLD ) total cold refrigerant pressure drop
PHOUT
L 0 (bar) 9.618 7.980 4.623 8.310 PHOT ) total hot refrigerant pressure drop
ZL 1 mol % PLR ) total pressure drop of the lower refrigerant though the
C2H6 0.3636 0.4244 0.3241 0.5263
C3H8 0.0870 0.3255 0.4566 0.2639
upper cycle
n-C4H10 0.5494 0.2501 0.2193 0.2098 Tmin ) minimum temperature difference or temperature approach
TI L (C) -15.45 -29.52 -37.63 -36.24 c ) isentropic efficiency of compressor
LEX ) isentropic efficiency of liquid expander
FU 1 (kmol/s) - 0.2106 0.3804 0.5236 p ) isentropic efficiency of pump
PLUIN0 (bar) - 1.243 2.499 2.477
PHUOUT0 (bar) - 4.610 7.613 5.674
HPR ) set of enthalpy flows defining the overall process composite
ZU 1 mol % curve
C2H6 - 0.0216 0.0067 0.1759 NR ) number of refrigeration stages
C3H8 - 0.0468 0.5384 0.0973 PRMAX ) maximum pressure or compression ratio
n-C4H10 - 0.9315 0.4549 0.7268 PRMIN ) minimum pressure or compression ratio
TI U (C) - - 3.60 18.73, 0.06
TPIN ) process inlet temperature to the system
TPOUT ) process outlet temperature from system
TPR ) temperatures in the overall process composite curve
Table A3. Solutions with Three Refrigeration Stages in the Lower
Cycle TRIN ) temperature of hot streams after heat rejection to air or
cooling water
refrigeration stages in upper cycle
YLEX ) binary parameter indicating the use of liquid expanders
variable 0 (no cascade) 1 2 3 (when set to 1)
TP (C) - 0.18 5.04 0.32 Functions
FL1 (kmol/s) 0.5821 0.4430 0.4504 0.3959 CROP ) extracts a set of enthalpy flows or temperatures contained
PLIN
L 0 (bar) 2.490 2.479 2.428 2.363 within a given temperature range from a larger array
PHOUT
L 0 (bar) 9.935 5.800 6.140 7.024 HCOMP ) combines stream data and returns the set of enthalpy
ZL 1 mol %
C2H6 0.3797 0.3638 0.3617 0.4662 flows defining a hot composite curve
C3H8 0.1833 0.4399 0.3942 0.2958 HEV ) returns the enthalpy flow that corresponds to a sample
n-C4H10 0.4369 0.1963 0.2441 0.2380 temperature in a composite curve
TI L (C) 3.26, -20.87, -19.40, -29.09, HPROF ) returns a set of enthalpy flows defining the composite
-30.04 -40.75 -40.91 -51.17 curve of a stream with the given flowrate and compositions and
FU 1 (kmol/s) - 0.2548 0.3493 0.4747 within the given temperature and pressure range
PLUIN0 (bar) - 2.500 2.469 2.500 hsP ) returns the enthalpy of a stream given its composition,
PHUOUT0 (bar) - 8.601 5.519 5.224 entropy and pressure
ZU 1 mol % hTP ) returns the enthalpy of a stream given its composition,
C2H6 - 0.0076 0.0259 0.1598
temperature and pressure
C3H8 - 0.5412 0.2717 0.0681
n-C4H10 - 0.4512 0.7024 0.7721 OBJ ) user-defined objective function. may change from case to
TI U (C) - - 14.18 18.03, 3.44 case, including economic and/or performance criteria

sTP ) returns the entropy of a stream given its composition,
temperature and pressure
TCOMP ) combines stream data and returns the temperatures in
a hot composite curve
TDEW ) returns the dew temperature of a stream given its
composition and pressure
TEV ) returns the temperature that corresponds to a sample
enthalpy flow in a composite curve
ThP ) returns the temperature of a stream given its composition,
enthalpy and pressure
TPROF ) returns a set of temperatures defining the composite curve
of a stream with the given flowrate and compositions and within
the given temperature and pressure range
VF ) returns the vapor fraction of a stream given its composition,
temperature and pressur
ZVAP ) returns the vapor composition of a partially vaporised
stream given its total composition, temperature and pressure
ZLIQ ) returns the liquid composition of a partially vaporised
stream given its total composition, temperature and pressure
Variables
F ) total molar flowrate of hot refrigerant entering a given
refrigeration stage
FC ) total molar flowrate of cold refrigerant entering a given
refrigeration stage
FCMP ) molar flowrate of refrigerant entering a given compression
stage
FL ) liquid molar flowrate of hot refrigerant entering a given
refrigeration stage
FP ) liquid molar flowrate of refrigerant after intercooler in a given
compression stage
FV ) vapor molar flowrate of hot refrigerant entering a given
refrigeration stage
HC ) set of enthalpy flows defining the composite curve of the
cold refrigerant in a given refrigeration stage
hCIN ) cold refrigerant enthalpy at the inlet of a given refrigeration
stage
HCCOMP ) set of enthalpy flows defining the composite curve of
the cold streams in a given refrigeration stage
hCMP ) enthalpy of refrigerant after a given compression stage
hCOUT ) cold refrigerant enthalpy at the outlet of a given
refrigeration stage
hEXPN ) enthalpy of refrigerant after expansion in valve or liquid
turbine in a given refrigeration stage
HHCOMP ) set of enthalpy flows defining the composite curve of
the hot streams in a given refrigeration stage
HHL ) set of enthalpy flows defining the composite curve of the
liquid hot refrigerant stream in a given refrigeration stage
HHV ) set of enthalpy flows defining the composite curve of the
vapor hot refrigerant stream in a given refrigeration stage
HLR ) set of enthalpies defining the composite curve of the lower
refrigerant through the upper cycle
hP ) enthalpy of refrigerant after pumping in a given compression
stage
HP ) set of enthalpy flows defining the composite curve of the
process stream(s) in a given refrigeration stage
HPREF ) set of enthalpy flows defining the effective process
composite curve in the upper cycle
hISCMP ) isentropic enthalpy of compression in a given compres-
sion stage
hISLEX ) isentropic enthalpy of expansion of cold liquid refrigerant
in a given refrigeration stage
hISP ) isentropic enthalpy of pumping in a given compression stage
NC ) number of compression stages
Ind. Eng. Chem. Res., Vol. 47, No. 22, 2008 8739
ObjectiVe
) objective function value
PLIN ) pressure of cold refrigerant at the inlet of a given
refrigeration stage
PHOUT ) pressure of hot refrigerant at the outlet of a given
refrigeration stage
PR ) pressure ratio of a given compression stage when dissimilar
values are allowed. unique stage pressure ratio otherwise
PCMP ) discharge pressure in a given compression stage
QC ) heat received by the cold refrigerant in a given refrigeration
stage
QCMP ) heat removed in intercooler after a given compression
stage
QL ) heat removed from the hot liquid refrigerant in a given
refrigeration stage
QP ) heat removed from the process stream(s) in a given
refrigeration stage
QV ) heat removed from the hot vapor refrigerant in a given
refrigeration stage
TC ) set of temperatures defining the composite curve of the cold
refrigerant in a given refrigeration stage
TCCOMP ) set of temperatures defining the composite curve of
the cold streams in a given refrigeration stage
TCIN ) cold refrigerant temperature at the inlet of a given
refrigeration stage
TCOUT ) cold refrigerant temperature at the outlet of a given
refrigeration stage
TEXPN ) temperature of refrigerant after expansion in valve or
liquid turbine in a given refrigeration stage
th ) sample temperature for feasibility evaluation
THCOMP ) set of temperatures defining the composite curve of
the hot streams in a given refrigeration stage
THL ) set of temperatures defining the composite curve of the
liquid hot refrigerant stream in a given refrigeration stage
THV ) set of temperatures defining the composite curve of the
vapor hot refrigerant stream in a given refrigeration stage
TI ) temperature of the hot streams after a given refrigeration stage
(intermediate temperature)
TLR ) set of temperatures defining the composite curve of the
lower refrigerant through the upper cycle
TP ) set of temperatures defining the composite curve of the
process stream(s) in a given refrigeration stage
TPREF ) set of temperatures defining the effective process
composite curve in the upper cycle
WLEX ) work produced in liquid turbine at a given refrigeration
stage
WC ) work required in a given compression stage
WP ) pumping work required after a given compression stage
X ) molar composition of hot liquid refrigerant in a given
refrigeration stage
XCMP ) molar composition of liquid after intercooler in a given
compression stage
Y ) molar composition of hot vapor refrigerant in a given
refrigeration stage
YCMP ) molar composition of vapor after intercooler in a given
compression stage
Z ) molar composition of cold refrigerant in a given refrigeration
stage
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ReceiVed for reView April 2, 2008
ReVised manuscript receiVed August 4, 2008
Accepted August 12, 2008
IE800515U