Energy Conversion and Management 272 (2022) 116364

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Energy Conversion and Management

journal homepage: www.elsevier.com/locate/enconman

Energy and economic comparison of five mixed-refrigerant natural gas

liquefaction processes
Matheus A.M. Pereira a, Lucas F. Santos a, b, José A. Caballero b, Mauro A.S.S. Ravagnani a,
Caliane B.B. Costa a, *
a
Department of Chemical Engineering, State University of Maringá, Av. Colombo 5790, CEP 87020900 Maringá, PR, Brazil
b
Department of Chemical Engineering, University of Alicante, Ap. Correos 99, Alicante 03080, Spain

A R T I C L E I N F O A B S T R A C T

Keywords: The demand for liquified natural gas grows as it is an energy resource that has more flexible means of transport
Natural gas liquefaction processes than non-liquefied natural gas, and is more eco-friendly than other fossil fuels. This paper focused on comparing
Energy efficiency five different mixed-refrigerant liquefaction processes to determine which one is the most efficient in energetic
Economic analysis
and economic terms for four different natural gas processing scales (20,000 kg/h and 2, 4, and 8 MTPA of natural
Optimization
gas feed). Simpler processes with one or two refrigerant cycles (single mixed refrigerant, propane pre-cooled
CAPCOST technique
Simulation-Optimization mixed refrigerant, and dual mixed refrigerant) and more complex processes with three cycles (mixed fluid
cascade and AP-X) were analyzed. All processes were simulated in Aspen HYSYS, and the energy consumption
was optimized by a communication between the simulator and an optimization algorithm based on Particle
Swarm Optimization coded in MATLAB. The economic analysis was performed using the CAPCOST technique
and the rule of six-tenths for upscaling. In the best-optimized scenario, the results show that the most complex
process, AP-X, consumes the lowest amount of energy (0.2367 kWh/kg-LNG) while the simplest one, the single
mixed refrigerant, consumes the highest value (0.2561 kWh/kg-LNG). In the economic analysis, the results
indicate that energetically better processes may not provide a higher economic return even on large scales.

natural gas (LNG) at atmospheric pressure. It reduces its volume 600

1. Introduction
Natural gas (NG) has been widely recognized as a clean and powerful
energy resource in recent years, due to its low carbon emission
compared to other fossil fuels. For example, when compared to coal and
oil the NG emits between 29 % and 44 % less carbon dioxide per unit of
energy [1]. The demand for eco-friendly energy resources drives NG
growth, which is predicted to be of 60 % increase from 2010 to 2030 [2],
and it is predicted to outperform coal as an energy source by about 2035
[3].
A big share of NG is found in remote locations, far from the refineries
or the consumer market, being necessary to transport it over long dis­
tances. The transportation of NG is challenging due to its high specific
volume, and flammability risk, if transported in the gas state. Pipelines
are an alternative for short and fixed routes (approximately 1500 km
[4]). For longer distances, transporting it in the liquified state is more
effective. NG is liquefied in industrial refrigeration plants, energy-
intensive processes, being cooled to − 160 ◦ C to obtain liquified
times and augments safety as a consequence of decreasing the explosion
risk. The economic viability of LNG is linked to the energy efficiency of
this cooling process as it is one of the main costs in the LNG value chain.
The NG liquefaction plants represent more than 40 % of the total cost
[5], and the energy consumption for liquefaction provides approxi­
mately 30 % of the total energy of the NG value chain [2].
The demand for LNG is growing. The European Union has been
importing more and more LNG from the United States, reaching more
than 22 billion cubic meters in 2021 [6]. Moreover, the European Union
plans to increase the near-term import of United States LNG to phase out
Russian pipeline NG imports by 2027 [7]. The LNG capacity is expected
to increase to replace Russian gas in Europe and, to be more suitable, it is
important choosing the best liquefaction technology for each applica­
tion. There are many different NG liquefaction technologies and con­
figurations of refrigeration process developed worldwide [8].
The processes may be categorized into three kinds of liquefaction
processes: mixed-refrigerant (MR), cascade, and expander-based [9].
The expander-based process utilizes a turbo-expander to refrigerate the

* Corresponding author.
E-mail address: cbbcosta@uem.br (C.B.B. Costa).

https://doi.org/10.1016/j.enconman.2022.116364
Received 13 May 2022; Received in revised form 20 September 2022; Accepted 14 October 2022
Available online 29 October 2022
0196-8904/© 2022 Elsevier Ltd. All rights reserved.
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Nomenclature FBM Bare module factor

FM Equipment material factor
Abbreviation FP Equipment pressure factor
APCI Air Products and Chemicals Inc. g Constraint vector
LNG Liquefied natural gas I Cost index
M$/y Million dollars per annum i Interest rate (%)
MCHE Main cryogenic heat exchanger ṁ Mass flow rate (kg/h)
MMBtu Million Btu n Lifetime (year)
MR Mixed refrigerant P Pressure (kPa)
MSHE Multi-stream heat exchanger Pdes Discharge pressure (kPa)
NG Natural Gas PO Operating pressure (barg)
TAC Total annualized cost Psuc Suction pressure (kPa)
pen Penalty function
Symbols Q Heat duty (kW)
A Equipment capacity r Adaptative penalty factor
c Penalty factor sLNG Liquified natural gas price ($/MMBtu)
CBM Bare module cost ($/year) SLNG Liquified natural gas revenue ($/year)
cene Electricity price ($/kW-h) t Operation time (h)
Cmt Maintenance cost ($/year) T Temperature (◦ C)
CNG Natural gas cost ($/year) U Overall heat transfer coefficient (kW/◦ C•m2)
cNG Natural gas price ($/MMBtu) UA Heat exchange area multiplied by overall heat transfer
CP Equipment purchase cost ($) coefficient (kW/◦ C)
D Tower diameter (m) W Compression power (kW)
f Objective function (kWh/kg-LNG)
F Penalized objective function (kWh/kg-LNG)

NG. It is a simple process but is less energy efficient than others. The MR
process uses a mixture of hydrocarbons and nitrogen to liquefy the NG
and is considered a good balance between energy consumption and the
number of devices. Therefore it received the most attention in the NG
field [9]. The cascade process, on the other hand, is better in energy
efficiency, however, it uses independent refrigeration cycles with pure
refrigerant at different pressure levels, and its several devices increase
the capital costs. Apart from being classified according to the refriger­
ation technology, the processes may be also categorized according to the
plant scale. Zhang et al. [8] provide an overview of the current status of
NG liquefaction processes. Based on industrial application and academic
research, the authors divided the processes into three categories:
onshore small-scale plants, which liquefy less than 1 MTPA of NG;
onshore large-scale plants, able to liquefy more than 1 MTPA of NG; and
offshore processes, which present different criteria for selection.
Lim et al. [5] described the liquefaction processes that are currently
commercially available. One of the well-known processes presented is
the single nitrogen single expander, which is based on reverse-Brayton
and Claude cycles. It utilizes nitrogen at high and low pressure to cool
the NG and is suitable for small-scale and offshore plants. The single
mixed refrigerant (SMR) was developed by Air Products and Chemicals
Inc. (APCI) and uses a single cycle of a mixture of refrigerants to liquefy
the NG. This process has fewer devices than the cascade process and is
suitable for small-scale and offshore plants. The AP-X process, which
comprises three cooling cycles, was developed by APCI and utilizes a
pure propane refrigerant for precooling, a mixed refrigerant for cooling,
and a nitrogen refrigerant for subcooling the NG. This process contains
many devices to liquefy at much higher capacities than other processes
(around 8 MTPA). In 1999, the Phillips’ Optimized Cascade was devel­
oped for the Trinidad LNG plant and utilized three different cycles of
pure refrigerants at multiple pressure levels [5]. It is more energy effi­
cient compared to other processes, however, requires high capital and
maintenance costs for all devices present in the plant, therefore, it is
suitable for large-scale plants.
Comparisons among the NG liquefaction processes are important to
define which one is the most adequate. Qyyum et al. [10] provided a
review of the optimal design of NG liquefaction processes and found
some difficulties in comparing the processes with different design con­
siderations. The processes have many parameters that have a significant
impact on the objective functions, and these parameters are different or
are not mentioned in many studies, so the authors recommend the
evaluation of competing process-optimized alternatives with similar
parameters and conditions. Moreover, since the operation costs, e.g.
energy costs, tend to be more significant than capital costs for large-scale
plants, the suitability of the different LNG processes is linked to different
conditions. For example, the single mixed refrigerant (SMR) is suitable
for small-scale plants while the AP-X is suitable for larger-scales plants
[8,11]. However, there is no consensus on what is the best process if it is
possible the choose which one will be implemented. Also, different
processes may be suitable for the same situation, e.g. SMR and single
expander (SE) process are both used for small-scale plants [8,11], but
there is no comprehensive decision on which is the more efficient pro­
cess for small-scale applications.
The major issue related to LNG plants is the high energy consump­
tion. The review of Austbø [12] showed that the main work in the LNG
study field is concentrated on dealing with process synthesis and design
to improve the LNG value chain. It is common to use energy efficiency as
a parameter to compare processes. However, normally the most energy-
efficient processes are more complex because use several refrigeration
cycles or a mixture of refrigerants, many unit operation devices, and
many streams. This complexity of the processes makes it difficult to
control and find an optimal operating condition. The review of Zhang
et al. [8] showed that the mixed-refrigerant (MR) process dominates the
LNG field, but there is competition with the expander-based process in
small-scale applications, which is simpler and less energy-efficient.
Since the NG liquefaction processes are energy-intensive and require
complex models, optimization approaches have been considered in
several studies to achieve the most effective operating conditions of the
processes, especially a condition of minimum energy consumption.
Commercial simulation software, such as Aspen HYSYS and Aspen Plus,
are commonly employed to model complex processes with rigorous
thermodynamic libraries and property calculation methods. In this
scenario, Nogal et al. [13] proposed the use of a genetic algorithm (GA)
to evaluate the optimal design of LNG processes, especially mixed-

2
M.A.M. Pereira et al.
refrigerant (MR) and cascade types, and achieved better and more
feasible solutions compared to previous proposals, increasing the coef­
ficient of performance in 16.48 %. Morin, Wahl, and Mølnvik [4] pre­
sented an optimization approach using Sequential Quadratic
Programming to minimize the energy consumption of LNG plants. They
showed the positive aspects of this technique to deal with complex LNG
processes, such as robust convergence and satisfactory results, which
were less than 5.0 % of the assumed optimal solution. Alabudulkarem
et al. [14] optimized energetically the propane pre-cooled mixed
refrigerant (C3MR) plant using a GA from the MATLAB optimization
toolbox. The total power consumption was reduced by 9.08 % compared
to a base case. Aspelund et al. [15] used a gradient-free optimization-
simulation method, based on a Tabu Search and the Nelder-Mead
Downhill Simplex method, to find a local optimum while reducing the
required number of simulations. The method proved to be more effective
than other metaheuristic methods to obtain a better solution in energetic
terms. Khan and Lee [16] applied the particle swarm paradigm algo­
rithm to optimize the single mixed refrigerant (SMR) LNG plant. The
optimization was able to reduce the compression energy requirement by
10 %, demonstrating the applicability of the method in the optimization
of natural gas liquefaction processes. Khan et al. [2] incorporated the
sequential coordinate randomization search method for optimizing two
well-established NG liquefaction processes, SMR and C3MR. Using a
simple implementation, the approach was suitable for optimizing
nonlinear LNG processes, achieving for SMR and C3MR respectively 15
% and 14 % lower specific power consumption. The SMR process was
optimized energetically by Santos et al. [17] by a surrogate-assisted
framework. The authors used the kriging-assisted model, acquisition
function, and Nelder-Mead simplex method to perform a local refine­
ment search in the penalized simulation. Later, these authors improved
their framework by embedding the surrogate optimization problem into
mathematical programming to guide the search for the optimal design of
SMR processes [18] and the multi-objective design of SMR and C3MR
processes [19]. Sun et al. [20] compared three well-known optimization
algorithms for LNG processes (PSO, GA, and BOX algorithm), and the
results demonstrated that PSO had the best performance to optimize the
specific energy consumption of four different natural gas mixed refrig­
erant liquefaction processes.
As NG liquefaction processes contain many different devices and
operations, it is difficult to estimate the investment and operating costs.
Hence, the major focus in the literature is to optimize energy con­
sumption and exergy destruction to improve the LNG value chain.
However, some authors tried directly optimizing the costs, by consid­
ering only the major devices, normally using simplified equations to
estimate the value of each device. Aslambakhsh et al. [21] performed a
global cost optimization of a mini-scale LNG plant, considering the
operating equipment, energy utilization, and capital cost. The factory
net profit was maximized by the hybrid modified coordinate descent
algorithm. The paper indicated more than a 9 % improvement in net
profit by reducing the electricity consumption by 60 % and heat
exchanger size by 37.50 %. Jin, Son, and Lim [22] compared the eco­
nomic performance of various LNG recovery schemes. The economic
analysis indicated different outcomes when the total annualized cost
(TAC) results were compared with the gross profit and payout time. The
dual mixed refrigerant (DMR) process had the highest net profit and
lowest TAC. However, SMR had the lowest capital cost and the highest
payout time. Qyyum et al. [23] proposed a dual-effect single mixed
refrigerant (DSMR) process, that is considered energy- and cost-efficient
approach, and compared with other processes. The paper compared
DSMR with the classic DMR process and evaluated the energy con­
sumption, exergy efficiency, and annualized total cost, concluding that
DSMR was less exergy efficient, however, it reduced the energy con­
sumption by 22.89 % and the TAC by 18.52 %. Furda et al. [24]
employed a robust genetic algorithm (GA/NSGA-II) to perform a multi-
objective optimization of the C3MR plant with 18 process parameter
variations. The results led to more than a 12 % reduction in LNG
3
Energy Conversion and Management 272 (2022) 116364
processing costs and a 14 % cut in CO2 emission while only six param­
eters showed significant changes throughout the optimization process.
Many well-known LNG processes have already been investigated in
the literature, some simpler and others more complex. Many studies
have been carried out to simulate and find the most energetically effi­
cient and economically viable configuration of these processes. How­
ever, there is no conclusive answer to which is the most suitable
liquefaction process, either in economic or energetic terms, for a given
LNG process specification. Lim, Choi, and Moon [5] presented an
extensive discussion of the current perspectives on cryogenic cycles and
LNG processes, addressing the growth of the natural gas market and the
main commercial natural gas liquefaction processes employed world­
wide. Some researchers have investigated which is the most suitable
liquefaction process by comparing available well-known processes. Cao
et al. [25] compared two small-scale LNG processes, to know, SMR and
an N2-CH4 expander cycle. The study consisted of comparing the results
of minimizing the specific power consumption (power consumption per
LNG unit) for both processes while complying with process constraints.
The paper showed the improvement of a pre-cooling cycle, the impor­
tance of the exergy loss caused by the temperature difference between
the pipelines in the heat exchanger (HE), and the improvement in the
use of an intercooler between compression stages. Hwang et al. [26]
studied twenty-seven liquefaction configurations of two MR cycles with
multi-stage compression for LNG floating plants. Their results showed
that the power requirement for the optimized liquefaction cycle was
decreased by 7.45 % compared with the DMR cycle. Wang et al. [27]
performed thermodynamic and economic single objective function
optimization of C3MR and DMR processes. The approach reduced total
shaft work by 44.5 % for C3MR and 48.6 % for DMR and showed that
DMR consumes the least energy. However, the DMR process was
assumed to be more costly due to the use of the MCHE in pre-cooling.
Castillo et al. [28] performed a technical comparison between
different precooling cycles of LNG processes The authors found that the
heat capacitance UA (heat exchange area multiplied by the overall heat
transfer coefficient) and power consumption requirements are better for
propane precooling, while a better distribution of power consumption
among the cooling stages is present for the mixed refrigerant cascade
process. A novel concept for the LNG supply chain was proposed by Park
et al. [29], in which liquid air is used to retain cold energy from LNG
regasification and then reduce energy consumption for LNG. The pro­
posed process exhibits lower energy requirements when compared with
SMR and C3MR. Nguyen et al. [30] compared three small-scale LNG
processes: SMR, single, and dual reverse Brayton cycles. The energy
single-objective optimization of each process showed that MR processes
feature smaller net power consumption, at the price of having a more
complex process flowsheet and larger heat exchangers. Zhang et al. [8]
provided a quantitative technical and economic overview of three LNG
process categories: onshore large-scale, onshore small-scale, and
offshore. The authors showed that among these categories there are
large ranges of specific energy consumption values, specific capital
costs, and production costs due to, among other aspects, different
complexities of the facility, capacity of the plants, and location. Son
et al. [31] studied the influence of heat exchanger types and minimum
internal temperature approach (MITA) value on three different pro­
cesses: dual expander processes, SMR, and DMR. The results showed that
the DMR has high energy efficiency at a low utility cost. However, the
energy optimization performed better for low-efficiency processes than
high-efficiency processes in terms of the resulting total annualized cost.
Although much research has been conducted on the evaluation of
different LNG processes, the studies reported in the literature are not
able to answer more comprehensively which is the best liquefaction
process, given some specific conditions, because, in some of the studies,
the comparison is not the focus, and usually only a few similar processes
(two or three) are compared. The literature lacks comparisons among
several different processes that serve as a basis for concluding which is
the most suitable one for a given condition. The present paper aims to
M.A.M. Pereira et al.
carry out a more comprehensive comparison of LNG processes by
analyzing simple and complex processes while maintaining similar pa­
rameters and operating conditions. Five well-known different processes
are simulated and optimized energetically. The energetically-optimized
processes are compared and economic analysis is performed for all
processes at different processing scales to determine their suitability for
a given condition.
Bearing the foregoing in mind, the objective of this paper is to
compare LNG processes to show the most energy efficient and the most
profitable on four different scales. Furthermore, the paper analyses two
important relationships in the behavior of liquefaction processes present
in the LNG literature: (i) more complicated liquefaction processes, i.e.
comprising different mixed refrigerants, multiple refrigeration cycles,
and complex flowsheet configurations, exhibit higher energy efficiency;
and (ii) energy-efficient processes tend to present a reduction in the total
annualized cost of their plants, as electrical energy represents one of the
main expenses in the value chain of the liquefaction processes.
2. Materials and methods
The commercial simulator Aspen HYSYS V10.0 was used to model
the natural gas liquefaction processes and MATLAB version r2020a was
used to run the optimization task and to perform the economic analysis
and upscale technique. This section provides a detailed description of
the methods employed.
2.1. Simulation of liquefaction processes
Aiming for the analysis and comparison of natural gas liquefaction
plants, different liquefaction processes described in the literature were
modeled in Aspen HYSYS. Five processes were analyzed in this work:
APCI single mixed refrigerant (SMR), APCI propane pre-cooled mixed
Fig. 1. Simplified flowsheet of the SMR.
4
Energy Conversion and Management 272 (2022) 116364
refrigerant (C3MR), Shell and APCI dual mixed refrigerant (DMR),
Statoil-Linde mixed fluid cascade (MFC), and APCI AP-X. Detailed ex­
planations about the processes and the flowsheets of modeled processes
in Aspen HYSYS are presented in the Supplementary Material (Fig. S.1 to
Fig. S.5).
One of the most robust and well-known liquefaction processes is the
SMR, which uses one MR stream to liquefy the NG. Inspired by Khan
et al. [2], the process employs a single subcooling cycle with a mixture of
refrigerants as shown in Fig. 1. The refrigerant stream is composed of a
mixture of nitrogen and hydrocarbons. The SMR is the simplest process
analyzed in this paper, as there is only one MR cycle and fewer devices
than others processes.
The C3MR (Fig. 2) is one of the most dominant processes in the LNG
plant market. The natural gas is liquified by two refrigeration cycles. A
pre-cooling cycle with pure propane refrigerant cools the NG to around
− 40 ◦ C at four different pressure levels. In the subcooling cycle, the MR
refrigerant (a mixture of nitrogen and hydrocarbons) is separated into a
vapor and liquid stream to subcool the NG to a temperature of around
− 160 ◦ C.
Based on Qyyum et al. [32], the Shell and APCI dual mixed refrig­
erant (DMR) was modeled, and a simplified flowsheet is illustrated in
Fig. 3. This process comprises two separated cycles: a heavy mixed
refrigerant pre-cooling cycle composed of methane, ethane, propane,
and butane, and a light mixed refrigerant subcooling one composed of
nitrogen, methane, ethane, and propane.
The Statoil-Linde mixed fluid cascade (MFC) process was simulated
based on Ding et al. [33]. This is a cascade process (Fig. 4) that uses three
MR refrigeration cycles instead of pure refrigerants. It has a pre-cooling
cycle with heavy refrigerant (composed of propane, butane, and
ethylene), an intermediate cooling cycle with medium-weight refrig­
erant (composed of methane, propane, and ethylene), and a subcooling
cycle with light refrigerant (composed of nitrogen, methane, and
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Fig. 2. Simplified flowsheet of the C3MR.

Fig. 3. Simplified flowsheet of the DMR.

ethylene).
The last and most complex liquefaction process analyzed was the
APCI AP-X, based on Sun et al. [11]. This process (Fig. 5) includes three
cooling cycles: a pre-cooling cycle with pure propane refrigerant, a
cooling cycle with MR (composed of methane, ethylene, and propane),
and a subcooling cycle with methane and nitrogen mixture. The main
differences between this process and the others are the use of an
expander instead of a valve in the subcooling cycle and the energy
integration with the boil-off gas from the NG that did not liquefy after
the last valve expansion. This cold vapor is used as cold stream in the
subcooling cycle.
2.2. Process specifications
Each process has different specifications based on literature consid­
erations and regional variations (e.g. ambient temperature and natural
gas composition). In this work, the same parameters and conditions
were adopted for all simulated processes to ensure a fair comparison

5
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Fig. 4. Simplified flowsheet of the MFC.

Fig. 5. Simplified flowsheet of the AP-X.

among them. These process specifications are listed in Table 1. The exchanger size, and exergy. The most common and robust method
pressure drops across MSHEs are subdivided among the heat exchangers adopted in the literature is minimizing the compression power con­
of the same cycle if there is more than one in the same cycle. sumption, because the liquefaction process is energy-intensive, and costs
related to energy consumption are reported as the most relevant part of
the expenditure in the LNG liquefaction process. The intensity of energy
2.3. Optimization approach
consumption has an impact both on capital investment and operating
costs [10].
Liquefaction plants are complex processes because they involve
The difficulty of modeling the liquefaction processes makes the use
many unit operations, rigorous thermodynamic calculations, and cryo­
of process simulators attractive, once they use state-of-the-art modeling
genic conditions. To improve liquefaction efficiency, researchers have
equations and numerical methods. Because of the use of simulated
been applying optimization tools to maximize or minimize one or more
models, the liquefaction plant optimization problem is an expensive
process metrics. The overall goal is to achieve maximum performance at
black box problem, i.e. the symbolic formulation of the functions that
a minimal cost. It is possible to determine the costs of the processes using
describe the problem is unavailable. To solve this, the metaheuristic
cost estimation techniques, and these costs can be minimized using
optimization method Particle Swarm Optimization (PSO) [34] was
optimization methods. However, this is not the most common approach
employed in MATLAB, to optimize the following constrained optimiza­
adopted in the liquefaction optimization literature. Efforts have been
tion problem:
focused on optimizing process metrics that are directly related to the
cost of the process, such as power consumption, cryogenic heat

6
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Table 1 the simulator Aspen HYSYS with MATLAB, as depicted in Fig. 6. The
Parameters of the simulation. MATLAB optimization toolbox has already implemented a PSO algo­
Item Parameter rithm, based on Kennedy and Eberhart [34] studies and using modifi­
cations suggested in Mezura-Montes and Coello Coello [35], and
Feed NG condition Mass flow (kg/h) 1.00
Temperature (◦ C) 30.0 Pedersen [36]. The algorithm generates the first swarm and sends the
Pressure (kPa) 5,000 values of the decision variables to HYSYS. The simulator calculates the
Molar composition of natural gas (%) [2] N2 0.22 thermodynamic properties, unit operations, constraints, and objective
CH4 91.33 function values, and sends them back to MATLAB, which then calculates
C2H6 5.36
C3H8 2.14
the penalty function and the penalized objective function value of each
iC4H10 0.46 particle. Then, the velocity and position of each particle are calculated
nC4H10 0.47 and the current particle best and global best are updated. MATLAB again
iC5H12 0.01 sends to HYSYS the updated values of decision variables and the pro­
nC5H12 0.01
cedure is repeated until the stop criterion is achieved. PSO was coded to
Number of compression stages 4
Thermodynamic model for fluid properties Peng-Robinson EOS run 500 iterations with 30 particles and two stop criteria (maximum
Adiabatic compressor efficiency 75 % number of iterations and tolerance for objective function value
Adiabatic expander efficiency 80 % improvement of 1.0 × 10-4) were used. The values of the PSO parameters
Pressure drop in intercoolers (kPa) 0.0 were: 1.49 for cognitive and social parameters and a range of 0.1 to 1.1
Intercooler output temperature (◦ C) 30.0
LNG condition Vapor fraction 8%
for the inertia range. In the first iteration, the inertia factor value is the
Pressure (kPa) 120.0 upper bound of the inertia range. In subsequent iterations, an adaptative
Pressure drop across MSHE (kPa) Hot stream 100.0 evolution is obeyed to update the inertia factor, based on the objective
Cold stream 10.0 function value evolution. The counter is initialized as ic = 0. At each
new iteration, if the global best does not change, the counter is increased
by one, ic = ic +1, and the value of the inertia factor remains unchanged.
minx∈D f (x)
(1) However, at each new iteration step, if the global best improves, the
s.t.g(x) ≤ 0
counter is reduced by one, ic = max(0,ic − 1), and the value of the inertia
⃒ ⃒ ⃒ ⃒
⃒Wshaft ⃒ − ⃒WExp ⃒ factor is calculated as follows: if ic < 2, the value of the inertia factor is
f (x) = (2) doubled; if ic > 5, the value of the inertia factor is halved; otherwise, the
ṁLNG
value of the inertia factor does not change. Moreover, the value of the
In Eq. (1) and (2), x is the vector of decision variables, Wshaft is the inertia factor is ensured to respect the bounds of the inertia range.
shaft power of all pumps and compressors, WExp is the expansion power
of expanders, ṁLNG is the mass flow rate of LNG that leaves the process, 2.4. Search space
and g(x) is the vector of constraint functions. The problem domain is
limited by the search space defined by the upper and lower bounds of the The decision variables of the optimization problem are the degrees of
decision variables. freedom of the process streams and unit operations that can be modified
The optimization of the NG liquefaction processes is subject to two to change the objective function and constraint values. Each process has
constraints: its decision variables, and they are limited by lower and upper bounds.
Normally a simpler process has fewer decision variables than a complex
• The minimum internal temperature approach (MITA) inside the NG one. This is relevant because the number of decision variables and the
heat exchangers must be greater than or equal to 3 ◦ C. This constraint size of the search space influence directly the convergence time of the
establishes a reasonable trade-off between power consumption and optimization method.
total heat exchanger surface area; The search space of the simulated processes was defined empirically,
• To prevent liquid inlet in compressors, the vapor fraction of the based on base cases. For the SMR, C3MR, and DMR processes, the search
stream fed to the first compression stage must be 1.0. space and decision variables of the reference papers are presented.
However, some changes were adopted in this work so that the base
To deal with the constraints of the optimization problem, penalty decision variables were insufficient to specify all degrees of freedom.
functions are used. So, a penalized objective function is optimized in an Furthermore, the tests performed with the search space of the reference
unconstrained problem, as shown in Eq. (3). papers demonstrated that unsatisfactory objective function results were
achieved, and the values of the decision variables tended to the bounds
minx∈D F(x) = f (x) + pen(x) (3)
of the search space. In this paper, the lower and upper bounds of the
F(x) is the penalized objective function and pen(x) is the penalty design variables were determined by the following methods:
function. This work adopted three different penalty functions: quadratic For SMR, C3MR, and DMR processes:
penalty (Eqs. (4) and (5)), exponential penalty (Eq. (6)), and extreme
barrier (Eq. (7)). • Decision variables that are not mentioned in the base case (i.e., the
∑
m process described in the corresponding reference paper) were heu­
(( { } ) )2
pen2 (x) = rj,k • max 0, gj (x) (4) ristically determined to specify all degrees of freedom. The values of
j=1 their bounds were determined by several optimization tests per­
formed with different limits;
rj,k = b • rj,k− 1 (5) • Temperature and pressure bounds were set to the base case values
⎧ first, but some of them were empirically modified based on optimi­
⎨ f (x), if feasible zation tests;
pene (x) = ( ∑m ) (6)
⎩ f (x) • 1 + e j=1
cj •(max{0,gj (x) } )
, if infeasible • Refrigerant flow rate bounds were set to the base case values first,
but some of them were empirically modified to expand by 10 % the
∑m ( { }) lower or upper bound if the tests demonstrated objective function
penb (x) = j=1
cj max 0, gj (x) (7) value improvement.
The optimization task was performed by a communication between
As MFC and APCI AP-X base cases do not present the search space

7
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Fig. 6. Method flow diagram.

8
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

and in the reference papers the NG feed flow rate is not 1.0 kg/h, the Table 3
following methods were adopted: C3MR base case and the selected lower and upper bounds for the design decision
variables.
• Bounds for the decision variables that are not mentioned in the base Variable Base case Selected search space
case, temperature, pressure, and split fraction were determined in a Lower Upper Lower Upper
similar way as that described for SMR, DMR, and C3MR; Pre-cooling:
• Refrigerant flow rate base case values are the optimum of the T NG2 (◦ C) 15.00 30.00 11.00 29.00
reference papers, but the molar flow rate was converted to mass flow T NG3 (◦ C) 0.00 10.00 − 2.00 10.00
T NG4 (◦ C) − 20.00 − 5.00 − 20.00 − 5.00
rate and divided by the base case NG feed mass flow rate (8 MTPA) to
T NG5 (◦ C) – – − 35.00 − 27.00
convert it to the calculation basis of 1.0 kg/h NG feed. The initial Subcooling:
search space was considered to vary between ± 30 % of these base N2 (kg/h) 0 0.30 0 0.30
case values. Moreover, the bounds were expanded by 10 % for the C1 (kg/h) 0.30 0.80 0.30 0.80
lower or upper bound if the tests demonstrated objective function C2 (kg/h) 0.50 1.30 0.50 1.30
C3 (kg/h) 0.20 0.80 0.20 0.80
value improvement.
Psuc (kPa) 800.00 1,300.00 200.00 400.00
Pdis (kPa) 5,000.00 5,500.00 4,500.00 5,500.00
Tables 2 to 6 list the optimization decision variables bounds for all T NG6(◦ C) – – − 150.00 − 125.00
base case processes and the selected search space employed in this
paper. The decision variables refer to the modeled process streams and
devices that are presented in Fig. S.1 to S.5 of the Supplementary Table 4
Material. DMR base case and the selected lower and upper bounds for the design decision
Since a wide search space for the decision variables was used, some variables.
of the simulations may not converge (i.e., one or more unit operations Variable Base case Selected search space
may be not fully computed by Aspen HYSYS), and as a result, this could Lower Upper Lower Upper
lead to algorithm failure. To handle these cases, the penalization method
Pre-cooling:
was used such that, if a non-converged simulation is returned for a C1 (kg/h) 0.01 0.35 0.00 0.35
particle, a very high value is used as the objective function value for that C2 (kg/h) 0.05 0.60 0.05 0.60
particle and the optimization run does not crash. However, situations in C3 (kg/h) 0.10 2.30 0.10 2.30
iC4 (kg/h) 0.10 1.50 0.10 1.50
which the simulation did not converge were somewhat rare and only
nC4 (kg/h) 0.10 1.00 0.00 1.00
happened at the beginning of the run, because, as the optimization Psuc (kPa) 120.00 400.00 120.00 520.00
progresses, the method converges to feasible solutions. Pdis (kPa) 1,500.00 3,500.00 1,100.00 3,500.00
T NG2 (◦ C) – – –32.00 2.00
T NG3 (◦ C) – – − 60.00 –32.00
2.5. Economic analysis approach Subcooling:
N2 (kg/h) 0.10 0.45 0.05 0.45
The economic analysis of the five energetically optimized processes C1 (kg/h) 0.25 1.00 0.19 1.00
is performed. The total annualized cost of the designed liquefaction C2 (kg/h) 0.30 1.20 0.30 1.20
C3 (kg/h) 0.80 2.70 0.00 2.70
processes is compared to check if the cost reduction due to energy use
Psuc (kPa) 325.00 1,500.00 120.00 600.00
minimization surpasses the increased investment cost of more complex Pdis (kPa) 3,500.00 6,500.00 2,900.00 6,500.00
processes.
In a liquefaction process, the total annualized cost (TAC) is estimated
as the sum of Annualized Capital Cost (ACAP) and Operating Cost (OP), Table 5
as shown in Eq. (8). MFC base case and the selected lower and upper bounds for the design decision
TAC = ACAP + OP (8) variables.
Variable ±30 % from the optimum base case Selected search space
Lower Upper Lower Upper
2.5.1. Capital cost
The characteristics of each device, such as its building material, size, Pre-cooling:
requirements for installation, and operating pressure, influence its cost PR-C3 (kg/h) 1.60 2.96 1.60 2.96
PR-nC4 (kg/h) 0.41 0.77 0.41 1.18
and must be taken into account in the cost analysis. Different correla­
PR-Ethyl (kg/h) 0.10 0.18 0.10 0.20
tions are available for the estimation of equipment cost. Psuc (kPa) 107.32 198.32 120.00 300.00
In this work, the Bare Module Cost method [37] was used to estimate Pdis (kPa) 921.47 1,711.29 1,000.00 2,100.00
the cost of the main pieces of equipment in the liquefaction processes. T NG2 (◦ C) – – –33.00 − 10.00
T NG3 (◦ C) – – − 60.00 –33.00
Cooling:
Table 2 LR-C1 (kg/h) 0.07 0.13 0.07 0.15
SMR base case and the selected lower and upper bounds for the design decision LR-C3 (kg/h) 0.20 0.38 0.20 0.41
variables. LR-Ethyl (kg/h) 0.90 1.68 0.90 1.68
Psuc (kPa) 260.68 484.12 200.00 500.00
Variable Base case Selected search space
Pdis (kPa) 1,444.02 2,681.76 1,500.00 3,500.00
Lower Upper Lower Upper
T NG4 (◦ C) – – − 105.00 − 80.00
N2 (kg/h) 0.10 0.60 0.10 0.81 Subcooling:
C1 (kg/h) 0.30 0.80 0.19 0.91 SR-C1 (kg/h) 0.25 0.47 0.22 0.47
C2 (kg/h) 0.40 1.00 0.33 1.70 SR-N2 (kg/h) 0.06 0.12 0.04 0.12
C3 (kg/h) 2.00 4.50 0.00 5.80 SR-Ethyl (kg/h) 0.13 0.25 0.13 0.25
nC4 (kg/h) – – 0.00 2.20 Psuc (kPa) 293.30 544.70 250.00 550.00
iC4 (kg/h) – – 0.00 2.20 Pdis (kPa) 2,883.06 5,354.26 2,500.00 5,100.00
Psuc (kPa) – – 120.00 550.00
Pdis (kPa) 4,500.00 5,500.00 2,700.00 5,500.00
TExp (◦ C) − 160.00 − 150.00 – –
T NG2 (◦ C) – – − 60.00 20.00

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M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Table 6 Here k1 , k2 , and k3 are parameters of the price of each piece of

APCI AP-X base case and the selected lower and upper bounds for the design equipment and A is its capacity. The value of these parameters and the
decision variables. corresponding capacity are presented in Table 7. U-tube HE is a shell and
Variable ±30 % more from the Selected search tube heat exchanger, not a multi-stream heat exchanger. However, it is
optimum base case space very difficult to obtain good correlations to estimate the costs for MSHE,
Lower Upper Lower Upper mainly for Spiral Wound heat exchangers. Therefore, it is common to use
Pre-cooling cost correlations for types of heat exchangers present in the CAPCOST
P1-C3 (kg/h) 1.59 2.96 – – technique to represent the MSHE [23,31,40,41].
T NG2 (◦ C) 6.00 25.00
– –
Regarding compressors, the intervals for the capacity reported in the
T NG3 (◦ C) – – − 8.00 6.00
T NG4 (◦ C) – – –22.00 − 8.00 CAPCOST technique do not cover the capacity of the compressors in the
T NG5 (◦ C) – – − 35.00 –22.00 considered liquefaction processes. For compressors then the correlation
TEE-101 0.60 1.00 – – of Eq. (13) [42] was used to calculate de purchase cost of centrifugal
(P4→P6) compressors in the range of 200 to 30,000 HP. The power obtained in
TEE-102 0.38 0.70
kW from Aspen HYSYS is multiplied by 1.3410.
– –
(P10→P12)
Pdes K-100 (kPa) 217.63 404.17 – –
CP = exp(7.58 + 0.80ln(A)) valid for centrifugal compressors (13)
Pdes K-101 (kPa) 407.61 756.99 – –
Pdes K-102 (kPa) 840.00 1,560.00 – – For some pieces of equipment, the Bare Module Cost Factor (FBM ) is a
Cooling:
constant value based on the equipment type and building material.
MR-C1 (kg/h) 0.13 0.23 0.09 0.23
MR-Ethyl (kg/h) 0.68 1.26 0.68 1.26 However, for towers, vessels, pumps, and heat exchangers, this factor is
MR-C3 (kg/h) 0.28 0.52 0.28 0.56 estimated as in Eq. (14).
Psuc (kPa) 303.24 563.16 240.00 600.00
Pdis (kPa) 2,106.30 3,911.70 2,000.00 4,500.00 FBM = B1 + B2 FM FP (14)
T NG6 (◦ C) – – − 130.00 − 90.00
TEE-100 (MR6→MR8) 0.66 1.0 0.65 1.00
For the pressure factor (FP ) calculation, Eq. (15) is used for heat
Subcooling: exchangers and pumps, while for vessels and towers Eq. (16) is indi­
N-C1 (kg/h) 0 0 0 0.18 cated. In these equations PO is the design pressure in barg and D is the
N-N2 (kg/h) 1.77 3.29 1.26 3.29 device diameter in meters.
Psuc (kPa) 1,332.80 2,475.20 1,000.00 2,800.00
Pdis (kPa) 4,732.00 8,788.00 4,000.00 9,500.00 log(FP ) = C1 + C2 PO + C3 P2O (15)
T NG10 (◦ C) – – 14.00 28.00
(PO +1)D
+ 0.00315
(16)
2[850− 0.6(PO +1) ]
FP =
This method uses different scaling factors for each device to determine 0.0063
the purchase cost at base condition. Then, this purchase cost is multi­ The material factor (FM ) is a constant that depends on the material
plied by a factor that depends on the direct and indirect costs of each used for building the piece of equipment. The base value for this factor is
unit, such as specific building material, pressure, equipment installation one for carbon steel, and it was assumed that all devices are built with
costs, freight, insurance, taxes, and salaries for project management carbon steel.
personnel. This method is commonly employed for estimating the cap­ All equipment capacity values were directly obtained with the pro­
ital cost of the main devices in an LNG process. Qyyum et al. [23], Son cess model in Aspen HYSYS, except for the heat exchange areas. The
et al. [31], Qadeer et al. [38], and Jin and Lim [39] are some works that simulator only returns the value of UA, the heat exchange area multi­
adopted this same approach. plied by the overall heat transfer coefficient (U). Literature values for U
The main process pieces of equipment in liquefaction processes are were considered [40,43–45]: 1700 W/(m2 ◦ C) for multi-stream heat
heat exchangers, compressors, pumps, vessels (flash separators), and exchangers,1000 W/(m2 ◦ C) for propane cycle heat exchangers, and
turbines. Except for compressors, equipment cost is estimated according 500 W/(m2 ◦ C) for intercoolers.
to the Module Costing CAPCOST technique, in which the Bare Module The surface area of each heat exchanger was determined by dividing
Cost (CBM ) for each piece of equipment is calculated by multiplying the its UA value by its U. UA values for multi-stream and propane heat ex­
Bare Module Cost Factor (FBM ) by the purchased cost (CP ), as indicated changers were obtained directly from the process model in Aspen
in Eq. (9). HYSYS. For intercoolers, UA calculated by Eq. (17) was employed using
CBM = FBM CP (9) the heat duty calculated in the process simulation and considering a cold
utility with a constant temperature of 25 ◦ C.
The Capital Cost (CAP) is calculated by multiplying the sum of Bare
Module Costs (CBM ) by a constant related to changes or unexpected ex­ UA =
Q
(17)
pansions for the installation of equipment in the industrial plant, as in ΔTln
Eq. (10).
∑ 2.5.2. Cost index
CAP = 1.18 CBM (10) The cost index is employed to update the equipment purchase cost
from the base year (Cbase ) to a new year (Cp− new ), considering the
To estimate the ACAP, the CAP is amortized over the plant’s ex­
changing economic conditions over time and accommodating inflation
pected lifetime. Based on the literature, this work adopted 20 years of
over the years. In this paper, the values of the Chemical Engineering
lifetime (n, years) and a 10 % annual interest rate (i). So, the annualized
Plant Cost Index (CEPCI) are used to escalate the capital cost.
capital cost is calculated in Eq. (11).
Turton’s and Seider’s correlations are based on prices of 2001 and
i(1 + i)n 2006, respectively. The base index (Ibase ) for those years are 397 and 500
ACAP = CAP (11)
(1 + i)n − 1 by CEPCI. The equipment purchase cost was updated considering the
average cost index for the year 2019, which, according to CEPCI, is
The purchase cost, CP , is defined in the CAPCOST technique by a
607.5 [46]. This is the most updated average annual value freely
logarithm correlation on a capacity related to it, as described in Eq. (12).
available on the Chemical Engineering website.
logCP = k1 + k2 A + k3 A2 (12)

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M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Table 7
CACOST equipment parameters.
Device HE HE HE Vessels Turbines Pumps

Type U-tube Kettle Reboiler Floating Head Vertical Tower Axial Centrifugal
k1 4.1884 4.4646 4.8306 3.4974 2.7051 3.3892
k2 − 0.2503 − 0.5277 − 0.8509 0.3161 1.4398 0.0536
k3 0.1974 0.3955 0.3187 0.1074 − 0.1776 0.1538
A, unit Area, m2 Area, m2 Area, m2 Volume, m3 Power, kW Power, kW
A range 10 – 1,000 10–100 10 – 1,000 0.3–520 100 –4,000 1–300

Inew
Cp− = Cbase (18)
new
Ibase
2.5.3. Operating cost
To estimate operating cost three main expenses are considered:
compression power consumption cost, annual maintenance cost, and
raw material cost. The latter only considers the natural gas feed price.
Annual maintenance cost is defined as a part of the annualized capital
cost and, for this work, maintenance cost (Cmt ) is set at 3 % of ACAP.
Energy cost (Cene ) is calculated by total shaft work multiplied by elec­
tricity price multiplied by annual plant operation time, as in Eq. (19).
Cene = Wshaft • cene • t (19)
Similarly, feed NG price per year (CNG ) is found by multiplying feed
natural gas mass flow rate (ṁNG ) by annual plant operation time (t) and
natural gas price (cNG ).
CNG = ṁNG • cNG • t (20)
Finally, the operating cost is calculated as in Eq. (21).
OP = Cene + CNG + Cmt (21)
The economic feasibility was measured by the difference between
the annual sale of liquefied natural gas (SLNG ) and the total annualized
cost. Revenues with the sale of LNG were estimated by Eq. (22).
SLNG = ṁLNG • sLNG • t (22)
Based on the literature, the following parameters were adopted:
• The plant’s lifetime was considered 20 years;
• Annual operation time was taken as 8,000 h;
• The price of electricity is 0.0681 $/kWh – Average price of electricity
in the year 2019 was reported by the U.S. Energy Information
Administration (EIA) [47];
• The price of pre-treated feed natural gas is 2.56 $/MMBtu – Average
price of treated natural gas price in the year 2019 was reported by
the U.S. Energy Information Administration (EIA) [48];
• The price of LNG is 6.01 $/MMBtu – Average contract-based price of
LNG in the year 2019 was reported by the Ministry of Economy,
Trade, and Industry of Japan (METI) [49].
of some device for a new capacity value, based on the cost for a base
capacity, using an exponent ex, which is usually approximated to 0.6 but
other values can be used for each device to generate a more accurate cost
estimate for the entire plant [50]. Normally the exponent value ranges
from 0.35 to 1.00. Different authors have already used Eq. (23) to es­
timate the costs of devices for LNG processes. Son et al. [31] used the
module costing technique by Turton et al. [37] to obtain a base cost at a
small capacity LNG process and applied the rule of six-tenths for
calculating the cost for a greater capacity. Son and Kim [51] used
module costing for most devices and the rule of six-tenths for small-sized
equipment. Lee and Moon [52] used only the rule of six-tenths to
calculate the costs based on the Aspen Economic Evaluation and pilot
plant experience.
( )ex
Anew
Cp,new = Cp,base (23)
Abase
The literature served as a basis for the recommended value for the
exponent for each piece of equipment evaluated in the processes. The
exponent values are 0.61 [53] for pumps, 0.78 [53] for compressors,
0.65 [50] for all heat exchangers, 0.7 [50] for flash separators, and 0.7
[50] for turbines. The plant capacity was increased to different scale
categories: 2, 4, and 8 MTPA, which are considered onshore large-scale
LNG plants [8].
To assess the parameters and properties of larger-scale plants, the NG
feed flow rate in the simulated processes was changed from 20,000 kg/h
to 2, 4, and 8 MTPA, and each refrigerant component flow rate was
increased at the same proportion and with the same intensive variable
values (pressure, temperature, and others). Aspen HYSYS calculated
new capacity values for compressors, expanders, vessels, and heat ex­
changers. Knowing the base costs and the base capacities for the lique­
faction process with 20,000 kg/h NG feed, and the new capacity value
for each device at 2, 4, and 8 MTPA, Eq. (23) was used to estimate the
cost for each device of large-scale LNG plants. Then, the annualized
capital cost was obtained following the methods described in sections
2.5.1 and 2.5.2 For the operating cost, all parameters described in sec­
tion 2.5.3 (lifetime, operating time, and energy, NG, and LNG prices)
were kept constant for upscaling. The maintenance cost was kept at 3 %
of the new ACAP while Cene , CNG and SLNG were determined by knowing
the consumption of NG and energy, and the production of LNG.

To comply with CAPCOST equipment capacity limits, the plant ca­
pacity was fixed to process 20,000 kg/h of NG and produce 18,539 kg/h
of LNG. So, the annual processing of the plants is 160,000,000 kg/year
of NG and 148,312,000 kg/year of LNG. As the calculation basis of NG
feed is 1.0 kg/h, the optimal values of decision variables that are
extensive properties are multiplied by 20,000 to maintain the objective
function value expressed in kWh/kg-LNG. These values represent a
production of 0.148 MTPA of LNG. Therefore, the plants are considered
small-scale liquefaction plants.
2.5.4. Upscale
Since it is well-known that the energy cost increases more than the
capital cost when plant capacity increases, an upscale study was per­
formed. Therefore, to analyze the costs in a large capacity plant, the rule
of six-tenths (Eq. (23)) was adopted, which estimates the purchase cost
3. Results and discussion
Each process generates results from energy optimization and eco­
nomic analysis. In this section, all results are presented and the appro­
priate comparisons and discussions are carried out.
3.1. Optimization results
The present framework was run on a Ryzen 5–3600 CPU at 3.6 GHz,
16 Gb RAM computer. To deal with the PSO, the present approach was
applied five times for each simulation and penalization method. The
evaluation time depends much more on the time needed to perform the
flowsheet calculations in the process simulator than the time to run the
code in MATLAB. To run 100 iterations for each process is necessary, on
average, 24.97, 59.97, 41.37, 45.2, and 61.45 min for the SMR, C3MR,

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M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Table 8 Table 10
Main features of each studied process in the optimal condition. Optimal values of the decision variables in the C3MR process.
Variable Unit SMR C3MR DMR MFC APCI Variable Value Variable Value
AP-X
Pre-cooling:
Total shaft work kW 0.2374 0.2362 0.2277 0.2340 0.2194 T NG2 (◦ C) 16.0415 T NG4 (◦ C) − 11.8611
Specific shaft kWh/ 0.2561 0.2548 0.2456 0.2525 0.2367 T NG3 (◦ C) 2.4509 T NG5 (◦ C) − 29.5386
work kg- Subcooling:
LNG N2 (kg/h) 0.0508 Psuc (kPa) 239.7473
Total cooling kW 0.8400 0.5639 0.7678 0.7257 0.5462 C1 (kg/h) 0.4200 Pdis (kPa) 4,502.8510
duty (HEs and C2 (kg/h) 0.7788 T NG6 (◦ C) − 135.0858
MSHEs) C3 (kg/h) 0.6354
Specific cooling kWh/ 0.9062 0.6084 0.8284 0.7829 0.5892
duty (HEs and kg-
MSHEs) LNG
Pre-cooling UA kW/◦ C – 0.0281 0.0827 0.0602 0.0241 Table 11
(HEs and Optimal values of the decision variables in the DMR process.
MSHEs)
Variable Value Variable Value
Cooling UA (HEs kW/◦ C – – – 0.0596 0.0489
and MSHEs) Pre-cooling:
Subcooling UA kW/◦ C 0.1758 0.0616 0.0755 0.0182 0.0237 C1 (kg/h) 0.0500 Psuc (kPa) 491.0995
(HEs and C2 (kg/h) 0.5222 Pdis (kPa) 1,770.4742
MSHEs) C3 (kg/h) 1.6326 T NG2 (◦ C) − 0.1048
TOTAL UA (HEs kW/◦ C 0.1758 0.0897 0.1582 0.1380 0.0967 iC4 (kg/h) 0.5293 T NG3 (◦ C) − 34.4108
and MSHEs) nC4 (kg/h) 0.6239
Subcooling:
N2 (kg/h) 0.1154 C3 (kg/h) 0.6531
DMR, MFC, and APCI AP-X, respectively. C1 (kg/h) 0.3594 Psuc (kPa) 227.9406
The main features of each process in the optimal condition are C2 (kg/h) 0.7938 Pdis (kPa) 3,620.8809
summarized in Table 8. The optimal values of the decision variables are
shown in Tables 9 to 13. The best specific energy consumption is
observed in the APCI AP-X process, which uses 0.2367 kWh/kg-LNG. Table 12
The values obtained for the objective function on each optimization run Optimal values of the decision variables in the MFC process.
are listed in Tables S.1 to S.5 of the Supplementary Material. Fig. 7 Variable Value Variable Value
presents a boxplot of the objective function value obtained in the
Pre-cooling:
different optimization runs for each process. Also in the Supplementary PR-C3 (kg/h) 1.9142 Pdis (kPa) 1,604.7723
Material, Tables S.6 and S.7 bring a compilation of interesting infor­ PR-nC4 (kg/h) 0.9369 T NG2 (◦ C) –23.5187
mation regarding each process, and in Tables S.21 to S.30 one can find PR-Ethyl (kg/h) 0.1676 T NG3 (◦ C) − 41.8580
information regarding the vapor fraction, pressure, temperature, mass Psuc (kPa) 171.9205
Cooling:
flow rate, molar flow rate, and composition of all flowsheet streams in LR-C1 (kg/h) 0.1121 Psuc (kPa) 392.2373
the optimal condition. LR-C3 (kg/h) 0.3758 Pdis (kPa) 2,338.6789
The optimized processes can be arranged in the following descending LR-Ethyl (kg/h) 1.0718 T NG4 (◦ C) − 92.5854
order regarding the value of the objective function: SMR, C3MR, MFC, Subcooling:
SR-C1 (kg/h) 0.2512 Psuc (kPa) 390.2074
DMR, and APCI AP-X. Apart from DMR and MFC, the arrangement fol­
SR-N2 (kg/h) 0.0781 Pdis (kPa) 4,060.6675
lowed as expected: more complex processes exhibit smaller objective SR-Ethyl (kg/h) 0.2404
function values. PSO was able to find an operating condition for DMR
that makes it the process with the second-lowest value for shaft work.
However, in the fifteen runs of PSO for this process, only two of them led
Table 13
to an optimum objective function value less than 0.2500 kWh/kg-LNG
Optimal values of the decision variables in the APCI AP-X process.
(Table S.3), which suggests that the process conditions that lead to such
Variable Value Variable Value
a small value of shaft work are difficult to be found. Maybe these con­
ditions represent small feasible regions in the search space, surrounded Pre-cooling:
by a large infeasible space. Moreover, to reinforce this finding, it is T NG2 (◦ C) 14.2789 T NG4 (◦ C) − 17.0793
T NG3 (◦ C) − 1.0590 T NG5 (◦ C) –33.7574
possible to observe that the greatest average value of the objective Cooling:
function in the fifteen optimization runs for each process is relative to MR-C1 (kg/h) 0.1738 Pdis (kPa) 4,098.7886
the DMR process (Fig. 7). MR-Ethyl (kg/h) 0.7304 T NG6 (◦ C) − 120.0000
It is observed in Table 8 that APCI AP-X is the best process in terms of MR-C3 (kg/h) 0.5300 TEE-100 0.9797
Psuc (kPa) 250.1884
shaft work consumption and that SMR, C3MR, and MFC did not have
Subcooling:
significant differences in objective function optimum values. The greater N-C1 (kg/h) 0.1410 Pdis (kPa) 5,534.0682
complexity of MFC and C3MR, when compared to the SMR process, N-N2 (kg/h) 1.2610 T NG10 (◦ C) 20.7034
improved the energy efficiency, but the improvement was not as Psuc (kPa) 1,541.0933

Table 9 significant as reported by the papers that address these processes [2,11].
Optimal values of the decision variables in the SMR process. C3MR and SMR simulations are based on the same paper [2] and in their
Variable Value Variable Value modeling similar parameters were used. However, in this work, SMR
presents more components in the mixed refrigerant and more phase-
N2 (kg/h) 0.2589 iC4 (kg/h) 0.0224
C1 (kg/h) 0.4432 Psuc (kPa) 322.4010 separation operations. These changes can justify the difference be­
C2 (kg/h) 1.6331 Pdis (kPa) 2,809.8481 tween the optimum of C3MR and SMR processes.
C3 (kg/h) 0 T NG2 (◦ C) –32.5792 Each process was individually optimized, however, the results pre­
nC4 (kg/h) 2.1931 sent certain relationships and similarities, such as the pressure ratio in

12
M.A.M. Pereira et al.
Fig. 7. Objective function boxplot.
the many cycles, which is in the range of 1.38 to 2.08 (Table S.6). This
analysis is relevant since papers that present optimization studies on the
natural gas liquefaction process usually use a pressure ratio constraint.
However, a pressure ratio of 2.08 is a reasonable value, obtained
without the imposition of such a constraint, indicating that this type of
constraint is unnecessary when there are four compression stages.
Regarding the composition of MR, the amount of nitrogen in the opti­
mized processes was always very small, except in APCI AP-X, with the
mass percentage varying between 2.7 (in C3MR) and 13.7 % in MFC
(Table S.7). However, this is an important component because it is
present in all liquefaction processes, mainly for the subcooling of NG.
After all, it is the component with the lowest boiling point.
Another similarity observed is that all processes required phase
separation in the pre-cooling cycle. From an energy point of view, it
brings an advantage since compressing liquids demands less energy.
However, from an economic point of view, the advantage is uncertain, as
a separation vessel and a pump are required, although a pump is cheaper
than a compressor (for the same pressure ratio) and its presence in the
cycle reduces the size of the compressor.
It can be noted that processes with propane pre-cooling cycles
(C3MR and APCI AP-X) have lower total UA and specific cooling duty for
HE and MSHEs than other processes. Although the sum of individual UA
values may be controversial because different global heat transfer co­
efficients may be valid for different pieces of equipment, it is related to
the total heat transfer area in HEs and MSHEs. The heat transfer area in
such devices was calculated for the economic analysis and, as presented
in the economic analysis results (Tables S.8 to S.12 in the Supplementary
Material), these areas are indeed lower in C3MR and APCI AP-X pro­
cesses (total area of 1.285 × 103 m2 and 1.336 × 103 m2, respectively).
Still, concerning the parameters of total area and total UA in HEs and
MSHEs, the SMR process, which has only one refrigeration cycle, pre­
sents the highest total area (2.068 × 103 m2), total UA value, and spe­
cific cooling duty in HEs and MSHEs, while DMR presents the second-
13
Energy Conversion and Management 272 (2022) 116364
highest total area (1.861 × 103 m2), total UA value, and specific cool­
ing duty.
Comparing the results in Tables 8 and S.7, it is interesting to draw
attention to the fact that the total refrigerant mass flow rate and the
specific shaft work followed contrary trends: less energy-consuming
processes required higher refrigerant flow rates. This is a piece of rele­
vant information because volumetric flow rate and compression energy
are directly proportional properties, but the different specific volume
values of the refrigerants (which had their composition optimized) in
each compression stage in the different processes led to this trend. So
even a larger mass flow rate may present a lower volumetric flow rate
and, consequently, the efficiency of the processes and the reductions of
pressure ratio were able to outweigh the increase in shaft work gener­
ated by the amount of refrigerant.
The boxplot of Fig. 7 shows APCI AP-X as the best process in terms of
shaft work consumption because besides achieving the lowest energy
consumption among all processes, it tended to lower results (the median
is below 0.2450 kWh/kg-LNG). DMR process achieved the second-
lowest objective function value, however, showed the greatest disper­
sion and largest quartiles, with objective function values varying from
about 0.2456 kWh/kg-LNG (the best result obtained) to 0.2810 (the
worst result obtained). SMR and MFC processes showed a very similar
dispersion, but the tendency of the results was different between them
because in SMR the median is near the second quartile (next to 0.2600
kWh/kg-LNG) while in MFC the median is near the third quartile (next
to 0.2650 kWh/kg-LNG). Furthermore, it is possible to observe that the
best value achieved for the objective function in the fifteen runs for
optimizing SMR, C3MR, and MFC processes are very similar among
these processes, although the C3MR process showed the lowest disper­
sion and the median showed a tendency to lower objective function
values.
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

Table 14 Furthermore, the analyses of the capital costs of the processes did not
Main items in the economic analysis of the liquefaction processes for 20,000 kg/ follow the expected relationship between energy consumption and the
h of NG ($•106/year). cost of the process, because C3MR, which is the second simplest process,
Item SMR C3MR DMR MFC APCI AP-X presents the second highest energy consumption and investment needed
CAP 14.87 18.78 16.28 17.43 19.85
to acquire the equipment (capital cost).
ACAP 1.75 2.21 1.91 2.05 2.33 The results showed that SMR is the best process, in economic terms,
Cene 2.59 2.57 2.48 2.55 2.39 and C3MR is the worst. However, it is worth noticing that the cost
Cman 0.05 0.07 0.06 0.06 0.07 analysis was limited by the CAPCOST technique capacity range. To
21.03 21.03 21.03 21.03 21.03
CNG
maintain almost all pieces of equipment within its range, it was neces­
OP 23.67 23.67 23.57 23.65 23.49
TAC 25.42 25.88 25.48 25.69 25.83 sary to adopt a processing capacity of 20,000 kg/h of NG, representing
SLNG 45.83 45.83 45.83 45.83 45.83 the production of 0.148 MTPA of LNG. The SMR process has a certain
Profit 20.41 19.96 20.35 20.14 20.01 tendency to be more profitable for small scales plants, while the others
process (C3MR, DMR, MFC, and APCI AP-X) are more suitable for me­
dium- and large-scale liquefaction plants. Therefore, this tendency can
3.2. Economic analysis
explain why SMR was the best process according to the economic
analysis.
Table 14 presents the main items of the economic analysis of each
Moreover, the operating costs related to energy consumption grow
liquefaction process operating in its optimal condition and with a ca­
faster than the TAC. So, when NG feed flow is increased, the energy-
pacity of processing 20,000 kg/h of NG. More detailed results, such as
efficient processes may be also superior in economic terms. Then, in a
the cost and capacity of each piece of equipment and cost factors are
large-scale plant or offshore plant, maybe C3MR, DMR, MFC or APCI AP-
listed in the Supplementary Material (Tables S.8 to S.12). Fig. 8 presents
X processes outperform the SMR.
a comparison of the major costs of the analyzed liquefaction processes.
The price to acquire the raw material, NG, is the most significant
Considering the present process specifications and using the imple­
annual cost for all processes in comparison with the other operating
mented methods, all natural gas liquefaction processes had a positive
costs and the capital costs, as can be seen in Fig. 8. The cost estimation of
profit with annual revenue that surpasses the cost of more than 19 M$/y
an industrial process depends a lot on the employed approach and the
(profit). The simplest and most energy-consuming process, SMR, pre­
adopted parameters, which must be determined by the researcher or the
sents the lowest TAC, 25.42 M$/y, while the most studied liquefaction
group who performs the economic analysis. Therefore, the estimation
process, C3MR, presents the highest TAC, 25.88 M$/y. The high cost of
accuracy may be subjective. However, by making comparisons with the
the C3MR process can be explained as it includes many unit operations,
same premises, as the analyses were conducted in this paper, it is
mainly in the propane pre-cooling cycle, in which there are eight heat
possible to make comparisons with more reliability. All costs presented
exchangers, four compressors, four phase-separators, and one inter­
in this paper are estimates for a liquefaction plant considering the major
cooler while saving just 0.51 % of specific shaft work compared to the
costs to construct and operate the process. These estimates do not
SMR. The APCI AP-X process presents high capital costs too and there is
consider specific situations, such as the plant location, laws, labor wage,
also a propane pre-cooling cycle in this process, but the energy reduction
taxes, or tax exemption of the region, nor other minor costs such as
is more relevant in this process compared to C3MR.

Fig. 8. Annualized major costs of liquefaction processes for 20,000 kg/h of NG.

14
M.A.M. Pereira et al. Energy Conversion and Management 272 (2022) 116364

minor expensive devices, administrative items, outsourcing, and many Table 16

others. Main features in the economic analysis of 2 MTPA plants ($•106/year).
Even adopting the scale of 20,000 kg/h NG being fed, some devices’ Item SMR C3MR DMR MFC APCI AP-X
design capacity violated the CAPCOST application range. They are listed
ACAP 10.70 12.20 11.71 12.94 13.09
in Table 15 (these devices are present in Fig. S1 to S.5 of the Supple­ Cene 29.53 29.39 28.32 29.11 27.29
mentary Material). The value of 20,000 kg/h NG was chosen because Cman 0.32 0.37 0.35 0.39 0.39
with this scale the number and degree of violations were lower than with CNG 240.11 240.11 240.11 240.11 240.11
other scales. OP 269.96 269.86 268.78 269.61 267.79
280.66 282.07 280.49 282.55 280.88
To summarize the discussion, the five liquefaction processes were
TAC
SLNG 523.22 523.22 523.22 523.22 523.22
energetically optimized and an economic analysis was performed. The Profit 242.56 241.15 242.73 240.68 242.34
results, with a base of 20,000 kg/h NG feed, were compared to verify the
validity of two important relationships generally accepted as true: (i) the
higher the process complexity the lower its energy consumption; and (ii)
Table 17
the lower the process energy consumption the lower its cost. Regarding Main features in the economic analysis of 4 MTPA plants ($•106/year).
the first of these relationships, it was noticed that not always more
Item SMR C3MR DMR MFC APCI AP-X
complex processes have lower energy expenditure. Moreover, the
analysis of the second-mentioned relationship showed that the cost ACAP 17.12 19.37 18.73 20.75 20.80
59.06 58.75 56.64 58.22 54.58
reduction related to energy consumption was not enough to justify the Cene
Cman 0.51 0.58 0.56 0.62 0.62
increase in investment related to the acquisition of more equipment for CNG 480.22 480.22 480.22 480.22 480.22
the most complex processes. Many papers take these two relationships as OP 539.78 539.55 537.40 539.04 535.40
true for their analysis and arguments, however, the efforts in this work TAC 556.89 558.92 556.13 559.79 556.21
demonstrated that they are not always true. SLNG 1046.44 1046.44 1046.44 1046.44 1046.44
Profit 489.55 487.52 490.31 486.65 490.24
The cost analysis was limited by the technique implemented to es­
timate the capital cost. The CAPCOST technique is a robust method to
determine the equipment cost and the direct and indirect costs of each
unit. However, the equipment purchase cost equation has upper and Table 18
lower bounds that must be respected. These ranges limited the NG feed Main features in the economic analysis of 8 MTPA plants ($•106/year).
flow, so the processes analyzed are considered small-scale plants. Item SMR C3MR DMR MFC APCI AP-X
Another aspect worth mentioning is that the types of heat exchangers ACAP 28.14 31.69 30.80 34.15 34.05
available in the CAPCOST technique do not include spiral-wound heat Cene 118.13 117.50 113.28 116.44 109.16
exchangers (the most common type of heat exchanger for the cryogenic Cman 0.84 0.95 0.92 1.02 1.02
960.44 960.44 960.44 960.44 960.44
cycle of NG liquefaction processes). If those situations are resolved, it is CNG
OP 1079.41 1078.89 1074.64 1077.91 1070.62
possible to make cost estimations more robust and accurate for lique­ TAC 1107.55 1110.58 1105.44 1112.06 1104.67
faction processes for rigorous cost optimization. SLNG 2092.89 2092.89 2092.89 2092.89 2092.89
Profit 985.34 982.31 987.45 980.82 988.21

3.3. Increased plant capacity

processes, the SMR, which is the process with the highest shaft work
To verify the validity of the methods and discussions raised in this consumption, presented a higher profit than other more energy-efficient
paper, the plant capacity was expanded. The new monetary results for 2, processes (MFC and C3MR). The process with the lowest energy con­
4, and 8 MTPA NG feed liquefaction plants are presented in Tables 16, sumption, APCI AP-X, presents respectively the third, second and first
17, and 18 respectively. highest profit for 2, 4 and 8 MTPA feed NG. The DMR process presented
The sequence for profit value of the processes was modified because the highest profit for 2 and 4 MTPA LNG plants. It corresponds to the
energy cost increased more than capital cost. For 2 MTPA processes the second-lowest value of energy consumption and also the second-lowest
sequence is DMR > SMR > APCI AP-X > C3MR > MFC. For a 4 MTPA annualized capital cost. Then, DMR was the process that exhibited a
scale, the profit order is DMR > APCI AP-X > SMR > C3MR > MFC, balance between the energy and capital costs for large-scale plants.
while for an 8 MTPA plant the order is APCI AP-X > DMR > SMR > Moreover, the results show that the most complex and energy-efficient
C3MR > MFC. The upscale study demonstrated that, even for large-scale process, APCI AP-X, is the best option only for very large-scale plants.
Regarding the MFC and C3MR processes, which consume less energy
Table 15
than SMR and are recommended in the literature for large-scale plants,
Devices whose capacity violated the capacity range of the CAPCOST method. all the economic analyses (20,000 kg/h, 2, 4, and 8 MTPA NG feed)
showed that they were worse than SMR. This result indicates that
Device Capacity Limit violated
energetically optimal processes may not provide higher economic
SMR: returns than simpler processes.
MSHE1 1,467.7370 m2 <1,000 m2
Finally, let us analyze again the two relationship hypotheses: (i) the
C3MR: higher the process complexity the lower its energy consumption; and (ii)
K-104 126.3753 kW >149 kW the lower the process energy consumption the lower its cost. Regarding
HE5 127.8244 m2 <100 m2 the first of these hypotheses, it was noticed that not always more com­
HE6 122.4578 m2 <100 m2 plex processes have lower energy expenditure. The results of the upscale
HE7 105.7074 m2 <100 m2
study showed that these hypotheses are partially true because the
MFC: simplest process is the best (in economic terms) for small-scale, the
E-106 5.7935 m2 >10 m2 second most energy efficient is the best for 2 and 4 MTPA plants, and the
most complex and energy-efficient is the best for 8 MTPA scale. On the
APCI AP-X:
other hand, the hypotheses are false when C3MR and MFC processes are
K-100 78.1666 kW >149 kW
HE5 112.1547 m2 <100 m2 at focus because they are economically worst than SMR on all scales,
HE6 110.0153 m2 <100 m2 although both are considered, in the literature, robust and efficient

15
M.A.M. Pereira et al.
processes for larger-scale plants, like 2 and 4 MTPA.
3.4. Sensitivity analysis
A sensitivity analysis was performed to verify the validity of the
qualitative results from the economic assessment. The values of interest
rate, the period in which the capital cost will be amortized, and the
electricity cost were varied using a two-level factorial design with the
extreme values found for them in the literature. The economic analysis
was performed for the eight ”experiments” (to an experiment corre­
sponds a set of values for the factors being varied). For the electricity
cost, the average costs of 2018 and 2020 were used. Table 19 lists the
values of the properties analyzed and Tables S.13 to S.20 of the Sup­
plementary Material present the costs of the 20,000 kg/h plants with the
new properties.
The results of the sensitivity analysis showed that the annualized
capital cost, maintenance cost, and electricity cost were modified,
however, in all eight “experiments” the same sequence for profit was
obtained: SMR > DMR > MFC > APCI AP-X > C3MR. Then, it is possible
to verify that the applied methods are valid and do not present great
disparities when the main parameters in the economic analysis have
their values modified.
4. Conclusions
In the present paper, five different liquefaction processes were
simulated in Aspen HYSYS and their energy consumption was mini­
mized by employing an algorithm based on Particle Swarm Optimization
coded in MATLAB. All processes were modeled with the same specifi­
cations and considerations to provide a fair comparison of the energy
consumption behavior as liquefaction processes get more complex, with
more unit operations and refrigeration cycles. Moreover, an economic
analysis of the energy-optimized processes was performed considering
the major costs for a small-scale natural gas liquefaction plant and an
upscaling technique was applied to access the economic aspects of
larger-scale plants. This allowed the evaluation of the economic benefits
of decreasing energy costs and increasing the required investment.
Considering a small-scale natural gas liquefaction plant, the results of
both analyses, economic and energetic, showed that SMR, the most
energy-consuming process, with 0.2561 kWh/kg-LNG, was the most
economically profitable process (20.41 M$/y), while APCI AP-X, the
most energy-efficient process, with 0.2367 kWh/kg-LNG, was the sec­
ond least profitable one (20.01 M$/y). Both energetic and economic
analyses demonstrate that there are flaws in the following two expected
relationships: the more complex the liquefaction process, the lower the
energy consumption, and energy-efficient processes exhibit lower total
annualized costs. In a large-scale plant with 2 MTPA NG feed, the DMR
process, which is the second one in terms of energy consumption, has the
highest profit (242.73 M$/y), while SMR presents the second-highest
profit (242.56 M$/y). For plants with 4 and 8 MTPA NG feed, the two
most energy-efficient processes become more profitable than SMR. For a
4 MTPA plant, the DMR process is the best in economic terms, with a
profit of 490.31 M$/y, followed by APCI AP-X with 490.24 M$/y. When
a plant of 8 MTPA is considered, APCI AP-X becomes the most profitable
process (profit of 988.21 M$/y), and DMR is the second most recom­
mended, with 987.45 M$/y of profit. Additionally, for large-scale plants,
C3MR and MFC were the two least viable processes and for small-scale,
the C3MR and the APCI AP-X were the two least viable.
The validity of the results and the raised discussions are verified as
the most energy-consuming process (SMR) presents the lowest TAC for
small-scale LNG plants and higher TAC than the two most energy-
efficient processes for 4 and 8 MTPA plants. However, the results indi­
cate that energetically optimal processes may not provide a higher
economic return, since two less energy-consuming processes (C3MR and
MFC) were less profitable than SMR, both in small- and large-scale
plants. Moreover, the methods applied to estimate the costs for
16
Energy Conversion and Management 272 (2022) 116364
Table 19
Sensitivity analysis factors and upper and lower values.
Factor Lower Center Upper
Interest rate (i) 8 % [31,54] 10 % 12 % [8,45,55]
Electricity cost 0.0667 $/kWh 0.0681 0.0692 $/kWh
(cene ) [47] $/kWh [47]
Lifetime (n) 15 years 20 years 25 years [21,56]
20,000 kg/h-NG plants are validated by sensitivity analysis. It showed
that the TAC and profit values changed when economic parameters are
modified, however, the discussion and conclusion are the same as those
already addressed.
CRediT authorship contribution statement
Matheus A.M. Pereira: Conceptualization, Methodology, Software,
Formal analysis, Writing – original draft, Writing – review & editing.
Lucas F. Santos: Conceptualization, Methodology, Software, Formal
analysis, Writing – original draft, Writing – review & editing. José A.
Caballero: Conceptualization, Writing – review & editing. Mauro A. S.
S. Ravagnani: Conceptualization, Writing – review & editing. Caliane
B. B. Costa: Conceptualization, Writing – original draft, Writing – re­
view & editing, Supervision, Project administration, Funding
acquisition.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
Acknowledgments
The authors acknowledge the National Council for Scientific and
Technological Development – CNPq (Brazil), processes 117948/2020-9,
307958/2021-3, 200305/2020-4, 148184/2019-7, 311807/2018-6,
and 428650/2018-0, and Coordination for the Improvement of Higher
Education Personnel – CAPES (Brazil) for the financial support. J.A.
Caballero wants to acknowledge the financial support of the ‘Generalitat
Valenciana’ under project PROMETEO 064/2020 and the Ministerio de
Ciencia e Innovación, under project PID2021-124139NB-C21.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.enconman.2022.116364.
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