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Fuel 347 (2023) 128402

Contents lists available at ScienceDirect

Fuel
journal homepage: www.elsevier.com/locate/fuel

Full Length Article

Simulation of and multi-aspect study of a novel trigeneration process for

crude helium, liquefied natural gas, and methanol production; operation
improvement and emission reduction
Yang Xiao a, b, Shengbin Wu c, *, Hantao Xia a, Jinyuan Zhang a, Lingling Ding a, Xiaolong Bao a,
Yi Tang a, Yongjie Qi d
a
College of Energy, Chengdu University of Technology, Chengdu 610059, Sichuan, China
b
Chengdu Technology Sun Energy Technology Co. Ltd., Chengdu 610059, Sichuan, China
c
Center of Modern Educational Technology, Guizhou University of Finance and Economics, Guiyang, 550000, Guizhou, China
d
Huainan Union University, Huainan 232038, Anhui, China

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

Keywords: This study suggested a novel integrated trigeneration system for crude helium (He), liquefied natural gas, and
Trigeneration system methanol production. This proposed system consisted of a cryogenic-based helium recovery unit from natural
Crude helium gas, a syngas synthesis unit by hybrid reforming, a methanol synthesis unit, and a sour water recovery unit.
Methanol production
Comprehensive energy, exergy, environmental, and economic analyses were performed to assess the system’s
4E analysis
Emission reduction
performance. Based on the results, the crude helium, liquefied natural gas, and methanol production rates were
Performance improvement obtained to be 4105kg/h, 3594000kg/h, and 707800kg/h, respectively. These production rates provided 93.4 %
and 94.38 % overall exergy and energy efficiencies. Also, over 60 % of the total exergy destruction occurred in
reactors (R1-R4). The application of sour water recovery supplied 85.66 % of the reforming and methanol
synthesis process. Regarding environmental analysis, 94 % of the CO2 emission was due to the indirect mode, and
the rate of the CO2 emission was estimated to be 0.164 kgCO2 /kgprods . Finally, the economic analysis indicated that
the total annual production costs were about 440.16 M$ and 0.13 USD/kg. Therefore, the net present value of the
designed scheme was estimated to be 364.36 M$.

1. Introduction
Helium (He) gas is the second lightest substance with various ap­
plications in different sections such as medicine, MRI scanners, elec­
tronics, nuclear industries, aviation, etc. [1]. Natural gas (NG) and
atmospheric air are the two main reservoirs of helium in nature, where
their helium concentration is almost 7 % by volume and 5.2 ppm,
respectively [2]. In essence, the helium extraction process has three
principal steps, including NG pretreatment (containing helium),
removal of water and acid gases, and recovering heavy hydrocarbons
[3]. Among different methods of helium recovery from NG, the cryo­
genic process is the most suitable method with a purity of 50 % mol
generally [4]. This process operates at an extremely low temperature;
thus, it is vital to involve advanced cascade cryogenic cycles [5].
Overall, the cryogenic process is divided into three forms of operation,
namely, distillation- and flash-based forms and their integration, which
can be applied to assess the other products [6–8]. Some previous studies
evaluated the potential of He recovery from NG. The literature review
presented below reveals their contribution to the topic.
Pakzad et al. [9] proposed a cryogenic system, consisting of a helium
upgrader, pressure swing adsorption, and helium liquefier to produce
liquid helium, which could produce 196.5 kg/h liquid helium with a
23.4 % exergy efficiency. Likewise, Pakzad et al. [10] modified their
proposed system by adding a mixed refrigeration subprocess to evaluate
liquid hydrogen and helium and they achieved 67 % exergy efficiency.
Mehrpooya and Shafaei [11] designed a process of helium recovery from
NG using two cryogenic flash-based separation methods. They stated
that the minimum temperature of the Linde process led to decreasing the
mass flow rate of the produced helium. They also investigated the exergy
aspect of the system and predicted the major irreversibility sources of
the whole process. In a study by Ansarinasab et al. [12], the cost analysis
of a cryogenic flash separation process was accomplished for helium

* Corresponding author.
E-mail address: wushengbin@mail.gufe.edu.cn (S. Wu).

https://doi.org/10.1016/j.fuel.2023.128402
Received 3 November 2022; Received in revised form 30 March 2023; Accepted 10 April 2023
Available online 21 April 2023
0016-2361/© 2023 Elsevier Ltd. All rights reserved.
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Y. Xiao et al.
Fig. 1. Block diagram of the proposed process.
recovery from NG. They declared that the cost of the exergy destruction
rate of the compressors was avoidable while their investment cost rate
was significant. In contrast, the investment cost of heat exchangers was
insignificant in the overall case. Two cryogenic-based helium recovery
processes from NG, namely Exxon and Linde, were simulated and
comprehensively studied by Shafaei and Mehrpooya [13]. The second
one was more suitable with an exergy efficiency of 96 %. A cryogenic
helium recovery process from NG by utilizing a three-stage propane
refrigeration unit was proposed and scrutinized by Ansarinasab et al.
[14]. Three modification processes were examined as well. The scenario
in which efficient devices were replaced with conventional ones was the
most suitable way of reducing the cost rate of exergy destruction. Zaitsev
et al. [15] improved the potential of a mixed fluid cascade process for
recovering helium and generating liquified natural gas (LNG) from the
feedstock (NG) by a pre-cooling cycle (an absorption refrigeration unit).
The new process decreased the specific power consumption from 0.265
kWh/kg to 0.184 kWh/kg compared to the base process. Although the
investment cost rate of the modified process was 31.2 % higher than its
base, the cost of products of the modified one diminished by 6.3 %. A
cogeneration process capable of the simultaneous production of natural
gas liquids (NGLs) and helium from NG was designed, examined, and
optimized by Hamedi [16]. The helium extraction unit was embedded
into a nitrogen removal process using a single column and the crude
helium with a purity of 60 mol% was achievable. Al-Sobhi et al. [17]
designed three different cryogenic-based processes including single
column, double columns, and cold box, and then compared their feasi­
bility from the thermodynamic, environmental, and economic perspec­
tives. The cold box-based framework reached the highest profitability
per kilogram of generated helium which was equal to 260 $. However,
other techniques were more appropriate thermodynamically and envi­
ronmentally. McElroy et al. [18] investigated the process of helium re­
covery from NG in Australia producing helium of 913 tons/year. They
estimated the net present value of the process at 175.8 M$ with a
payback period of 2.4 years.
As an industrial primary chemical, methanol is a viable solvent or
feedstock for different purposes, e.g., generating crucial chemicals (e.g.,
acetic acid, formaldehyde, and methyl tert-butyl ether). It is possible to
employ methanol as the input fuel of the Otto cycle or integrated it with
dimethyl ether to generate quality fuel [19]. In addition, methanol is a
starting material for dimethyl terephthalate, methylamines, chloro­
methanes, and methyl methacrylate [20]. With a variety of use, this
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Fuel 347 (2023) 128402
substance is achievable through the synthesis process. The literature
review reflects the relevant recent studies in the following.
The CO2 captured from a power plant was utilized by Van-Dal and
Bouallou [21] for methanol synthesis. The process of hydrogenation,
where the hydrogen was achievable from a water electrolysis process,
was considered for this purpose. The whole process resulted in pro­
ducing methanol of 470.5 ktons/year. Kiss et al. [22] designed a hy­
drogenation process for methanol synthesis taking into account wet
hydrogen for a double positive impact. The process reached a methanol
production of 100.07 ktons/year. Considering flue gas leaving a power
plant that produced 112 MW of power, Abdelaziz et al. [23] designed
and examined a methanol synthesis unit using the CO2 content within
the flue gas, decreasing CO2 emission by 62 %. The plant could yield
methanol of 0.625 tons per tons of CO2 released to the environment.
Four different sources of biogas (i.e., sorghum, palm oil, landfill, and
corn cobs) were regarded by Santos et al. [24] for methanol synthesis.
Using palm oil, the process was the most suitable case with a methanol
production capacity of 53300 kg/h. Salman et al. [25] evaluated the
potential of either methanol or dimethyl ether production via refuse-
derived fuel in integration with a combined heat and power (CHP)
plant. They performed energy and cost assessments and employed
Monte-Carlo simulation to predict future profitability. It was found that
the CHP + methanol was more appropriate from the energy point of
view while the CHP + dimethyl ether was cost-effective. Kim et al. [26]
designed a process for the simultaneous production of electricity,
heating, and methanol by using coke oven gas. The process had a height
energy efficiency of 71 % with a minimum selling price of methanol
between 0.23 and 0.29 $/kg. Combining biomass pyrolysis, gasification,
and a methanol synthesis unit, Im-orb et al. [27] utilized the recycled
CO2 as the gasification agent and improved the methanol production
capacity and environmental aspect. The methanol production capacity
of 0.23 kmol/h with a total energy efficiency of 60.7 % was obtained
from the process. From the thermodynamic point of view, Nazerifard
et al. [28] designed and investigated a trigeneration scheme assisted by
solar energy leading to yielding power, hydrogen, and methanol. The
exergy efficiency of the process was 55.1 %. A coal-based power plant
was improved by Xin et al. [29] by employing the Allam cycle (a direct-
fired supercritical CO2 cycle) and a methanol synthesis unit. The fuel-
saving ratio of the suggested process and the increase in the power
output were 5.3 % and 29.4 %, respectively. This process produced
methanol of 24.1 kg/s, as well. Using a solar-based water electrolysis
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Y. Xiao et al. Fuel 347 (2023) 128402

Table 1 energy, exergy, economic, and environmental viewpoints by imple­

Composition of the feed natural gas [23]. menting an Aspen HYSYS code. The economic analysis consists of net
Component Molar percentage present value estimation, which presents the system’s profitability
during the operational lifetime. Further, the environmental analysis
Methane 87.86
Ethane 4.73 evaluates the CO2 emission by estimating direct and indirect emissions.
Propane 1.64 Moreover, the designed system’s energy and exergy performances are
n-butane 0.38 compared with the previous investigation to show its superiority.
Isobutane 0.34 Furthermore, a sensitivity analysis is performed to assess the variation
Nitrogen 5
Helium 0.05
effect of some parameters on the methanol production rate, energy and
exergy efficiencies, and CO2 footprint.

cycle and a CO2 capture unit, Battaglia et al. [30] devised a methanol
synthesis unit. Different conditions of the operation were examined and
the results were compared accordingly. In another study based on solar
energy and NG, Ghorbani and Amidpour [31] designed a process leading
to the simultaneous production of helium of 18.9 kmol/h, LNG of 3590
kmol/h, and methanol of 3590 kmol/h, and evaluated it from the
thermodynamic point of view. The process had an exergy efficiency of
93.8 %.
The literature review emphasized the potential of producing helium
and methanol using responsible processes designed in previous studies.
Such processes were environmentally and economically useful and
could produce further products. These advantages have motivated the
researchers of the current study to focus on a combined process designed
for the first time. This process uses NG as the feed gas and is composed of
a helium recovery unit (HRU) in a cryogenic cycle, a syngas synthesis
unit (SSU) through hybrid reforming, a methanol synthesis (MSU), and a
sour water recovery unit (WRU). The application of WRU provides the
feasibility of producing more methanol through a separation process
from vapor streams. In this way, a higher performance is achieved due to
the novel combined process. The designed system is analyzed from
2. Process overview
A trigeneration process is proposed in the present study in which a
large portion of the consumed water is recovered; thus, it has a low
water loss, and the additional methanol in the vapor streams is re-
introduced into the distillation cycle. Fig. 1 depicts a block diagram of
the proposed process. In this process, NG (Table 1) is the main feed, and
the products include crude helium, LNG, and methanol. The process
consists of an HRU in a cryogenic cycle, an SSU through hybrid
reforming, an MSU, and a sour WRU. In the HRU using a cryogenic cycle,
in addition to the separation and production of LNG, crude helium with
a concentration of 45.81 %.mol is also obtained. Gas fuel, which is
produced by separation in flash separators, is the feed for reforming and
methanol synthesis processes. In the reforming unit, to achieve high
methane conversion, in addition to steam reforming, autothermal
reforming is also employed.
The produced syngas in the reforming process reacts in the catalytic
reactor of the methanol unit, leading to the formation of methanol. In
addition, in the methanol process, some portion of the methanol is lost
through the overhead vapors of the distillation column. Using the

Fig. 2. Process flow diagram of the proposed integrated process.

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Y. Xiao et al. Fuel 347 (2023) 128402

Table 2
Thermophysical specifications of working fluids used in different sections [32].
Working Parameters
fluids
Molecular weight Triple point Normal boiling Critical temperature Critical pressure Critical density Heating value [kJ/
[g/mol] temperature [K] point [K] [K] [kPa] [mol/L] mol]

CH4 16.04 90.69 111.66 190.56 4599.2 10.14 890.63

C2H6 30.06 90.36 184.57 305.32 4872.2 6.85 1560.69
C3H8 44.09 85.52 231.03 369.89 4251.2 5 2219.17
n-C4H10 58.12 134.89 272.66 425.12 3796 3.92 2877.4
i-C4H10 58.12 113.73 261.4 407.81 3629 3.87 2868.2
N2 28.01 63.15 77.35 126.19 3395.8 11.18 0
He 4 2.17 4.22 5.19 227.6 18.13 0
H2O 18.01 273.16 373.12 647.09 22064 17.87 44.01
CO 28.01 68.16 81.64 132.86 3494 10.85 282.98
CO2 44 216.59 194.68 304.12 7377.3 10.62 0
CH4O 32.04 175.61 337.63 512.6 8103.5 8.6 764.17
H2 2.015 13.95 20.37 33.14 1296.4 15.5 285.83
O2 31.99 54.36 90.18 154.58 5043 13.63 0

scrubber tower, this loss is minimized, resulting in the recovery and
production of almost all the methanol. Sour waters obtained in
reforming and methanol units are regenerated in a unit and reused in the
production cycle to minimize the water consumption process. A
desorption column in the WRU is responsible for removing the CO2
content of the sour water and injecting the regenerated process water
into the steam reformer and methanol scrubber column. Fig. 2 illustrates
more details of the trigeneration process. Here, NG is treated in a
cryogenic cycle to recover helium at first.
The thermophysical specifications of working fluids used in different
sections of the proposed plant are presented in Table 2.
2.1. Helium recovery unit
NG treatment at low temperatures leads to the separation of methane
and other hydrocarbons as LNG. The liquefaction process occurs in heat
exchangers HE-1 and HE-2. First, the NG stream is divided into two parts
(Streams 2 and 3). More than 94 % [23] of the NG is liquefied in HE-1
(Stream 2), and the other part (Stream 3) is liquefied by exchanging
heat with cold streams 24 and 26. NG liquefaction temperature at the
constant pressure of 6000 kPa is considered at − 145 ◦ C. Both NG
streams mix, which reaches the temperature of − 145 ◦ C, and the sepa­
ration of LNG takes place in flash tanks F-1 to F-3 through three stages of
flash, in which the pressure of NG reaches 530, 190, and 130 kPa [23],
respectively. Pressure is reduced through Joule-Thomson expansion
valves V-1 to V-3.
In the helium liquefaction and recovery unit, vapor streams, which
exit from the top of separators F-1 (stream 8) and F-2 (stream 11), are
partially condensed in HE-2. Their liquid content is separated in two-
phase separators, F-4 (stream 17) and F-5 (stream 19), and is reused
as the refrigerant after expansion. These streams act as the refrigerant
and finally leave HE-1 and are compressed in compressors C-1 to C-6
[23]. The overhead vapors of separators F-4 (stream 33), F-5 (stream
32), and F-3 (stream 23) form the crude helium stream, which is com­
pressed to the pressure of 2500 kPa by compressors C-1 to C-3. The
temperatures of the obtained liquid streams in two separators F-4 and F-
5, gradually increase by heat transfer in HE-2 and HE-1 and finally reach
the pressure of 2000 kPa by compressors C-4 to C-6 to form the feed
(Fuel gas stream) for the SSU. Due to the temperature increase after each
compressor, between compressing stages water coolers (CW-1 and CW-
2) are employed. These coolers reduce the fluid temperature after each
compression stage to 25 ◦ C [23].
2.2. Syngas synthesis unit
Gas fuel, which is the by-product of helium recovery from NG, is the
feed of the SSU. This stream contains some ethane in addition to
methane; thus, a primary reforming is conducted in reactor R-1 before
steam reforming. In this reactor, all the ethane, propane, heavier hy­
drocarbons, and a portion of methane are converted to syngas. Before
the steam/hydrocarbon mixture stream enters reactor R-1, the temper­
atures of the gas fuel and water reach 500 ◦ C using heat exchangers HX-4
and HX-3, respectively. In this study, the steam-to-carbon ratio is
considered at 3, which is compatible with the surveyed papers [33]. The
WRU supplies the required water stream for reforming (stream 94) with
a flow rate of 99,600 kmol/h, and its pressure increases from 101.3 to
2000 kPa by pump P-2. In the current study, for steam methane
reforming in reactor R-2, Nickle commercial catalyst (Ni/Al2O3) is used,
which is recommended for the operating temperature of 700–1000 ◦ C
and pressure of 300–2500 kPa [25]. The general reaction that occurs in
reactor R-2 is as follows [33,34]:
CO + H2 O ↔ CO2 + H2 (1)
CH4 + H2 O ↔ CO + 3H2 (2)
The output stream of reactor R-2 (stream 48) still has some uncon­
verted methane, which should be converted, which enhances the carbon
conversion efficiency of the process. For this purpose, autothermal
reforming (reactor R-3) is used. This reactor works at a temperature of
920.5 ◦ C and its feedstocks are fuel, steam, and oxygen. Autothermal
reforming reactions are expressed as follows [26]:
CO + H2 O ↔ CO2 + H2 (3)
CH4 + H2 O ↔ CO + 3H2 (4)
CH4 + H2 O ↔ CO2 + 4H2 (5)
CH4 + 2O2 ↔ CO2 + 2H2 O (6)
Output product of the autothermal reactor (stream 52), after
exchanging heat with the entering oxygen at a temperature of 917.7 ◦ C,
enters heat exchangers HX-3 and HX-4 to heat the water and gas fuel
streams. Since it contains condensed water, it goes into the two-phase
separator F-6, where the sour water is partially separated from the
syngas and sent into the WRU. The overhead vapor of this separator
(stream 57) is again cooled down to the temperature of 25 ◦ C in the
cooler CW-7, and the sour water stream (stream 61) is separated again
using a two-phase separator F-7. Finally, syngas from the top of sepa­
rator F-7 (stream 60) is sent into the MSU.
2.3. Methanol synthesis unit
The produced syngas in the SSU with the operating conditions of
25 ◦ C, 2000 kPa, and a flow rate of 105,500 kmol/h is the main feed of
the MSU. The stoichiometric number of the syngas produced in the SSU,
according to Eq. (7), equals 2.7 [22]. F represents the molar flow rate in

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Y. Xiao et al.
Fig. 3. Simulation schematic for the proposed integrated process.
kmol/h.
ḞH2 − ḞCO2
SN = (7)
ḞCO2 + ḞCO
Syngas (stream 60), first, is compressed to the pressure of 7500 kPa
[23] by compressor C-7 and mixed with the recirculated gases from
separator F-8. This gas mixture (stream 64), using hot gases leaving the
methanol synthesis reactor, reaches the temperature of 210 ◦ C [23], and
the synthesis reaction occurs in the fixed bed catalytic reactor, which has
the following dimensions: diameter of 5.5 m, length of 10 m, and the
number of tubes of 3026 [23]. The catalyst of the reactor is of copper
commercial type [21], which works under the operating conditions of
5000–10000 kPa and operating temperature of 210–270 ◦ C [16].
Methanol synthesis reactions that occur in reactor R-4 are [35]:
CO2 + 3H2 ↔ CH3 OH + H2 O (8)
CO + 2H2 ↔ CH3 OH (9)
CO + H2 O ↔ CO2 + H2 (10)
The outlet product of the reactor, after heat transfer with the inlet
feed, experiences a slight temperature decrement and in the heat
exchanger CW-8 reaches the temperature of 25 ◦ C, so the maximum
separation of the liquid (crude methanol) and gas is achieved. The outlet
stream of cooler CW-8 (stream 67) goes into separator F-8 so that 90 %
of the separated vapor is recirculated to the methanol synthesis reactor
(R-4, stream 70) through a TEE. The remaining 10 % of the overhead
vapor of separator F-8 is used as fuel (stream Fuel). From the bottom of
separator F-8 (stream 69), crude methanol exits, mainly consisting of
water and methanol. This crude methanol stream and the outlet stream
from the bottom of scrubber column T-2 (stream 80), and the excess
water stream are preheated to 83 ◦ C in the heat exchanger HX-7 and
injected into water-methanol separation distillation column T-1.
Considering that the light gases of the crude methanol stream are not
completely separated in separator F-8 and the goal is to produce meth­
anol with a purity higher than 99 %.mol, distillation column T-1 with a
partial condenser is considered. In this column, by exiting some portion
of the product in the vapor phase, the concentration of liquid phase
methanol produced in the condenser reaches the desired value. To avoid
methanol loss in the vapor stream (which includes carbon dioxide,
methanol, water, hydrogen, and nitrogen) scrubber column T-2 is
employed. This column has 20 sieve trays with a spacing of 0.6096 m,
the column diameter is 3.92 m, and its height equals 12.19 m. In con­
tactor column T-2, a water stream (stream 92) with a flow rate of 20,000
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Fuel 347 (2023) 128402
kmol/h is poured on the overhead vapor stream of column T-1 (stream
77). Thus, more than 99 % of the methanol is recovered and enters pump
P-3 from the bottom of contactor column T-2. The liquid stream (stream
78) is pressurized to 120 kPa by pump P-3 and fed to distillation column
T-1 along with the crude methanol stream. Distillation column T-1 has
80 sieve trays and its dimensions are a diameter of 4.6 m, tray spacing of
0.6096, and height of 48.77 m. The reflux ratio of column T-1 equals 2.5,
and the simulation is performed based on the methanol concentration of
0.01 %.mol in the reboiler. Finally, in the condenser of distillation col­
umn T-1, methanol with a flow rate of 22,090 kmol/h, a pressure of 110
kPa, and a temperature of 67.67 ◦ C is obtained. In addition, from the
reboiler of this column, the wasted water (stream 76) exits, and before
going into the WRU unit, its temperature is utilized for preheating the
feed of distillation column T-1. The overhead vapor of scrubber column
T-2 (stream 79), since it contains lots of water, is cooled down to 25 ◦ C in
cooler CW-9, and the liquids (stream 84) are separated by separator F-9
to be recovered in the WRU and reused. In addition, the overhead vapors
of the mentioned separator column are considered as the feed of the unit
(stream Fuel2).
2.4. Water recovery unit
This unit is responsible for recovering the sour water streams that are
produced in SSU and MSU units. The mixture of these streams is stream
86, which has a flow rate of 102,500 kmol/h and contains 300 ppm of
carbon dioxide and 100 ppm of. First, the sour water stream is preheated
to the temperature of 93 ◦ C in heat exchanger HX-8 and the outlet
stream of this heat exchanger (stream 87) enters column T-3, which is a
stripper column. This column has a full reflux condenser, where the
desorbed gases leave from its top. Distillation column T-3 has 3 sieve
trays, a diameter of 4.56 m, a height of 6.1 m, and a reflux ratio of 0.5.
Simulation of this distillation column is performed based on the 1 ppm of
CO2 concentration in the reboiler. Regenerated water (stream process
water) with a CO2 content of 1 ppm is produced in the reboiler of the
distillation column T-3, and to decrease the energy consumption in the
reboiler, it exchanges heat with the sour water in heat exchanger HX-8.
Process water stream leaves this heat exchanger at 86.39 ◦ C (stream 88)
and is cooled down to 25 ◦ C in cooler CW-10. Fluid leaving cooler CW-10
(stream 89) is mixed with fresh water with a flow rate of 17,140 kmol/h
and feeds scrubber column T-2 and methane reformer.
3. Process simulation
Aspen HYSYS software is employed to simulate the proposed process
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Y. Xiao et al. Fuel 347 (2023) 128402

Table 3
Operating conditions for streams of the proposed process.
Stream T (◦ C) P (kPa) F (kmol/h) Stream T (◦ C) P (kPa) F (kmol/h)

Feed 27 6000 235,100 2 27 6000 222,800

3 27 6000 12,220 4 − 145 6000 222,800
5 − 145 6000 12,220 6 − 145 6000 235,100
7 − 145.2 530 235,100 8 − 145.2 530 4474
9 − 145.2 530 230,600 10 − 156.9 190 230,600
11 − 156.9 190 22,910 12 − 156.9 190 207,700
13 − 160.7 130 207,700 LNG − 160.7 130 201,700
15 − 183 190 22,910 16 − 183 530 4474
17 − 183 190 22,840 18 − 185.6 130 22,840
19 − 183 530 4296 20 − 187.9 130 4296
21 − 186 130 27,140 22 − 157 130 27,140
23 − 160.7 130 6628 24 − 157.7 130 33,160
25 − 9.4 130 33,160 26 86.03 350 33,160
27 25 350 33,160 28 123.8 900 33,160
29 25 900 33,160 30 107.9 2000 33,160
Residue gas 25 2000 33,160 32 − 183 530 177.5
33 − 183 190 68.14 34 − 184.9 190 177.5
35 − 184.5 190 245.7 36 − 147.5 197 245.7
37 19.08 190 245.7 38 162.2 500 245.7
39 28 500 245.7 40 159.3 1200 245.7
41 26 1200 245.7 42 133 2500 245.7
Crude helium 25 2500 245.7 44 25.17 2000 99,600
45 500 2000 99,600 46 500 2000 33,160
47 498.4 2000 132,800 48 860 2000 166,600
49 500 2000 141,800 50 500 2000 0
51 200 4000 3400 52 920.5 2000 178,900
53 920.5 2000 0 54 917.7 2000 178,900
55 815.3 2000 178,900 56 140.5 2000 178,900
57 140.5 2000 130,900 58 140.5 2000 47,930
59 25 2000 130,900 60 25 2000 105,500
61 25 2000 25,440 62 201.8 7500 105,500
63 210 7500 367,200 64 133.5 − 132.2 415,600
65 265 7500 322,900 66 132.8 7500 322,900
67 25 7500 322,900 68 25 7500 291,200
69 25 7500 31,720 Fuel 25 7500 29,120
70 25 7500 262,100 71 25 7500 261,800
72 26.68 120 31,720 74 76.07 120 78,720
75 83 120 78,720 76 104.8 120 46,630
77 67.67 110 10,000 Methanol 67.67 110 22,090
78 85.49 110 23,040 79 100.2 110 6956
80 85.49 120 23,040 81 85.5 120 23,040
82 25 110 6956 Fuel2 25 110 488.4
84 25 110 6467 85 80.08 120 46,630
86 77.52 110 102,500 87 93 110 102,500
88 86.39 110 102,400 89 25 110 102,400
Process water 102.1 110 102,400 To incinerator 87.17 110 78.80
90 25 110 82,430 91 25 110 20,000
92 25 110 20,000 93 25 101.3 99,570
94 25 101.3 99,600 95 140.5 2000 23,960
Fresh water 25 101.3 17,140 Excess water 140.5 2000 23,960

in the present study. In addition, the Peng Robinson equation of state is

Table 4
used to estimate the thermodynamic properties, which is defined as
Composition of important streams of the proposed process.
[36–38]:
Component Streams
RT a
Crude LNG 60 Methanol 65 Process P= − (11)
v − b v × (v + b) + b × (v − b)
Helium Water

CH4 0.025 0.908 0.004 0.000 0.014 0.000

R2 T2c
C2H6 0.000 0.055 0.000 0.000 0.000 0.000 a = 0.45724 α (12)
C3H8 0.000 0.019 0.000 0.000 0.000 0.000 pc
n-C4H10 0.000 0.004 0.000 0.000 0.000 0.000
i-C4H10 0.000 0.004 0.000 0.000 0.000 0.000 RTc
b = 0.07780 (13)
N2 0.516 0.010 0.091 0.000 0.285 0.000 Pc
He 0.458 0.000 0.000 0.000 0.000 0.000
H2O 0.000 0.000 0.002 0.000 0.028 1.000 The simulation schematic is shown in Fig. 3. The operating condi­
CO 0.000 0.000 0.125 0.000 0.000 0.000 tions of the process equipment and streams are reported in previous
CO2 0.000 0.000 0.093 0.000 0.023 0.000 sections. In Tables 3-5, accurate operating conditions for all the process
CH4O 0.000 0.000 0.000 1.000 0.071 0.000
H2 0.000 0.000 0.684 0.000 0.579 0.000
points, the composition of the vital process streams, and principal
O2 0.000 0.000 0.000 0.000 0.000 0.000 specifications for the employed unit operations in the process.

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Y. Xiao et al. Fuel 347 (2023) 128402

Table 5 on the equilibrium conversion results in the maximum conversion of

Specifications of equipment employed in the proposed process. reactants under defined operating conditions [24]. In the performed
Interstage Coolers simulation in this study, coke formation under the operating conditions
of the autothermal and primary reformer reactors is not considered. This
Component Tin (◦ C) Tout (◦ C) ΔP(kPa) heat(kW) ṁin (kg/h)
matter has also been taken into account by other researchers [24]. The
CW-1 162.2 25 0 236.5 4105 products of a reactive system based on the thermodynamic equilibrium
CW-2 159.3 25 0 235.8 4105
CW-3 133 25 0 192.3 4105
are determined using the free Gibbs energy minimization. The total free
CW-4 86.03 25 0 19,760 647,600 Gibbs energy of a reactive system with different components can be
CW-5 123.8 25 0 32,850 647,600 calculated by Eq. (14) as [24]:
CW-6 107.9 25 0 27,920 647,600
CW-7 140.5 25 0 438,400 1,687,000 ∑
N

CW-8 132.8 25 0 630,900 4,249,000 Gt = ni μi (14)

CW-9 100.2 25 0 84,560 131,800 i=1

CW-10 86.39 25 0 136,300 1,845,000

In Eq. (11), ni is the mole number of component i and μi is the
E-1 27 − 145 0 812,400
chemical potential of component i. For gas mixture, standard fugacity
equals 1atm, and the fugacity of gas phase for component i can be
Compressors
computed by Eq. (15) as follows [24]:
Component Adiabatic Power ΔP(kPa) P ratio Outlet
efficiency (kW) pressure f gi = yi ∅∧i P (15)
(%) (kPa)
In Eq. (12), yi is the mole fraction of component i, is the fugacity
∅∧i
C-1 75 251.4 310 2.632 500
coefficient of component i, and P is the operating pressure of the system.
C-2 75 230.8 700 2.4 1200
C-3 75 187.8 1300 2.083 2500 In addition, the total free Gibbs energy of the system based on liquid and
C-4 75 30,130 220 2.692 350 vapor phases can be calculated by Eq. (16) [24]:
C-5 75 32,120 550 2.571 900
C-6 75 26,480 1100 2.222 2000 ∑
N
( ))
C-7 75 156,600 5500 3.75 7500
Gt = ni (G0fi + RTln yi ∅∧i P (16)
i=1

Pump Accordingly, for simulating the steam reformer and methanol syn­
thesis reactors, the plug model through Aspen HYSYS is employed. Other
Component Adiabatic Power ΔP(kPa) P ratio Outlet
efficiency (kW) pressure
researchers used this method for simulating methane steam reformer
(%) (kPa) [40,41] and methanol synthesis [22,23,41], and accurate results were
obtained. As previously mentioned, the methane steam reformer (R-2)
P-2 75 1253 1899 19.4 2000
P-3 75 2.484 10 1.091 120 uses a Nickel catalyst, and two reactions given in Eqs. (1) and (2) are
defined for the reactor. These reactions are modeled as heterogeneous
Heat Exchangers
catalytic reactions, and the kinetics of the reactions are given in Eqs.
(17) and (18) [34]. Methane conversion in reactor R-2 is calculated by
Component LMTD Heat duty Min. UA
Eq. (16) where k is the reaction constant, f represents fugacity, K denotes
–
(◦ C) (kW) approach (kJ/h◦ C)
(◦ C) the equilibrium constant, and Y is the molar flow rate.
( )
HE-1 14.66 44,560 6.327 10,940,000 3 3
k1 fCH4 fH2O − fH2 fH2 /Kp, SMR
HE-2 5.129 62,710 2.333 44,020,000 rSMR = ( (
2.5
) )2 /fH2 (17)
− 1
HX-3 164 1,686,000 115.336 37,000,000 1 + KCO fCO + KH2 fH2 + KCH4 fCH4 + KH2O fH2O fH2
HX-4 569.9 191,900 417.711 1,210,000
( )/
HX-5 803.4 5184 720.452 23,200 k2 fCO fH2O − fH2 fCO2 /Kp, fH2
(18)
WGS
HX-6 49.18 4,156,000 55 30,400,000 rWGS =
HX-7 10.19 25,230 4 8,920,000
(1 + KCO fCO + KH2 fH2 + KCH4 fCH4 + KH2O (fH2O fH2 ) )2
HX-8 7.723 35,350 8.873 16,500,000
CH44 Conversion = (Yin − Yout ) × Y−in1 (19)
Reactor For the kinetic values, interested readers can refer to the paper by
Component Length ΔP(kPa) Diameter Number of Void Park et al. [34]. The methanol synthesis reactor is simulated with the
(m) (m) tubes fraction sizing license of Lurgi. Dimensions of this reactor were mentioned
R-2 13 0 2 6000 0.5 earlier. This reactor is modeled based on heterogeneous reactions for
R-4 10 0 5.5 3026 0.39 carbon dioxide hydrogenation (Eq. (8) [23]), carbon monoxide hydro­
genation (Eq. (9) [41]), and water–gas shift (Eq. (10)). The diameter of
Columns catalyst particles is 0.00574 m, and its density equals 1775 kg/m3 [34].
Component Stages Diameter Reflux Reboiler Condenser Kinetic equations [23,41,42] for reactions in the methanol reactor are as
(m) ratio duty (kW) duty (kW) follows:
( )
T-1 80 4.6 2.5 1,182,000 1,066,000 P P 3 OH
T-2 20 4.56 – – – k3 PCO2 PH2 1 − K1eq1 HP23O PCH
H2 CO2
T-3 3 4.56 0.5 20,660 461.8 rCO2 Hydrogenation = ( PH 2 O
) (20)
0.5
1 + k4 PH + k5 PH2 + k6 PH2 O
2

3.1. Reactors modeling ( ( )− 1 )

1/2
k7 KCO f CO f 1.5
H2 − f CH4O Kp,7 f H2
In this study, primary reformer and autothermal reformer reactors rCO Hydrogenation = [ ] (21)
1/2 1/2
are modeled using the Gibbs reactor type in Aspen HYSYS. Ersoz et al. [1 + KCO f CO ] 1 + KH2 f H2 + KH2O f H2O
[39] used the Gibbs reactor model to simulate the reformer reactor for
biomass gasification products in Aspen HYSYS. The Gibbs method based

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Y. Xiao et al. Fuel 347 (2023) 128402

Table 6 4. Model validation

Comparison of the simulation results.
Parameter Xref [18] Xsim
⃒ ⃒
⃒Xref − Xsim ⃒ The helium recovery process was presented by Ansarinasab et al.
Xref [12], and it is also used in the present study for producing LNG, crude
helium, and fuel stream as the feedstock of the SSU. Some of the oper­
Helium concentration (mole frac) in crude 0.4581 0.4581 0
helium stream ating parameters presented in Ref. [12] are compared with the results of
Nitrogen concentration (mole frac) in 0.5165 0.5165 0 the present study. These parameters include flow rate, product con­
crude helium stream centrations, and power consumption of the equipment, which are
Methane concentration (mole frac) in 0.0254 0.0254 0 compared in Table 6, and finally, validation is conducted according to
crude helium stream
Flow rate of crude helium stream (kg/s) 1.14 1.14 0
Eq. (19). Based on the calculations, the deviation of the simulation re­
Methane concentration (mole frac) in LNG 0.9076 0.9076 0 sults of the HRU process is less than 1 %, and it is calculated accurately
stream at 0.141 %.
Nitrogen concentration (mole frac) in LNG 0.0098 0.0098 0 [ ∑ ⃒⃒ ⃒]
stream 1 Xref − Xsim ⃒
Flow rate of the LNG stream (kg/s) 998.44 998.4 0.00004 AARD[%] = 100 × (22)
m Xref
Ethane concentration (mole frac) in LNG 0.0551 0.0551 0
stream
Flow rate of fuel gas stream (kg/s) 179.83 179.9 0.00039 5. Process analyses
Power consumption of C-1 (kW) 256.37 251.4 0.019
Power consumption of C-2 (kW) 230.72 230.8 0.00035 5.1. Exergy analysis
Power consumption of C-3 (kW) 187.7 187.8 0.00053
Power consumption of C-4 (kW) 30122.62 30,130 0.000245
Power consumption of C-5 (kW) 32109.42 32,120 0.00033 One of the most important analyses in the performance evaluation
Power consumption of C-6 (kW) 26473.24 26,480 0.00026 and comparison with other similar technologies is the exergy analysis. In
the present study, a comprehensive assessment of the whole process, and
its different units regarding exergy destruction and exergy efficiency for
Table 7
Equations for exergy destruction and total exergy efficiency of the proposed
process.
Equipment Exergy destruction

Pumps [27] ĖD = Ėin − Ėout + Ẇ

Flash drums [46] ĖD = Ėin − Ėout,L − Ėout,V
Compressors [46] ĖD = Ėin − Ėout + Ẇ
Turbine [46] ĖD = Ėin − Ėout − Ẇ
Expansion valve ĖD = Ėin − Ėout
[27]
Reactors [35] ĖD = Ėin − Ėout ± ExQ
Interstage Coolers ĖD = Ėin − Ėout
[46]
∑ ∑
Heat Exchangers ĖD = Ėin − Ėout
[47]
∑ ∑
Columns [48] ĖD = Ėin − Ė +
( ) out ( )
T0 T0 T2 − T1
Q̇reb 1 − − Q̇cond 1 − TLMTD =
TLMTD TLMTD T2
ln
T1
∑
Process [47] ∑ ∑ ĖD
ĖD = Ėin − Ėout ηex = 1 − ∑
Ėin

Fig. 5. Inlet and outlet exergies in different units of the proposed integrated.

Fig. 4. Comparison between exergy destructions in different units of the proposed integrated process.

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Y. Xiao et al. Fuel 347 (2023) 128402

Fig. 6. Values of inlet and outlet exergies for the equipment types employed in the proposed process.

Fig. 7. Contributions of employed equipment to the exergy destruction of the proposed process.

Table 8 Table 9
Comparing the Exergy efficiency with previous studies. Results of energy efficiency for units of the proposed process and the whole
Reference System type Products Exergy
cycle.
∑ ∑
efficiency (%) Energy input(kW) Energy output (kW) ηenergy
Ref. [28] Trigeneration Methanol, hydrogen, 55.1 HRU 53,990,011 53,902,120 99.84 %
and power SSU 7,322,015 5,989,911 81.81 %
Ref. [49] Cogeneration Bio-methane/bio- 60.03 MSU 6,972,025 3,914,527 56.15 %
methanol WRU 20,660 324 1.57 %
Ref. [50] Polygeneration power and methanol 70 Total Process 55,704,161 52,574,685 94.38 %
Ref. [51] Integrated CCHP system Methanol, power, 76.41
cooling and liquid
fuels
equipment and the whole process is conducted. The total exergy of each
Ref. [52] Polygeneration Methanol production 54.86
and power generation
stream consists of physical and chemical exergies which are calculated
Ref. [53] Cogeneration Dimethyl-ether and 32.54 by Eqs. (23) and (24), respectively [42,43]:
electricity
Ref. [54] Integrated CHP system Methanol and 32.7 eph
i = h − h0 − T0 (s − s0 ) (23)
incorporating solar energy hydrogen
∑ ∑
Ref. [55] Cogeneration/SOFC Power and hydrogen 28.19 ech xi e0i + RT0 xi lnxi γi (24)
i =
Ref. [56] Cogeneration Hydrogen and 90
methanol
This Trigeneration Crude Helium, LNG, 93.4 where e0i , h0 , and s0 denote the specific chemical exergy of component i,
Study and Methanol the enthalpy at standard conditions, and the entropy at standard con­
ditions, respectively. Further, xi and γi represent the molar fraction of
component i in the mixture and the activity coefficient of component i,
respectively. The chemical exergies of the existing components in the
proposed process are adopted from Ref. [44]. The total exergy balance of

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Y. Xiao et al. Fuel 347 (2023) 128402

Table 10 exergy destruction occurs in heat exchanger HX-8 (87.88 %). In the SSU,
Comparison of energy efficiency with previous papers. the maximum exergy destruction belongs to reactor R-1 (40.97 %). In
Reference System type Products Energy addition, in the HRU, heat exchanger E-1, which is the substitute for the
efficiency (%) cryogenic refrigeration of NG, has the largest exergy destruction (80.49
Ref. [28] Trigeneration Methanol, hydrogen, 66.84 %). Also, the inlet exergy to different units and outlet exergy from
and power various units are shown in Fig. 5. As shown, from the 242868 kW of inlet
Ref. [49] Cogeneration Bio-methane/bio- 30.69 exergy to the WRU, 195829 kW is destructed, which implies an exergy
methanol efficiency of 19.36 % for this unit.
Ref. [51] Integrated CCHP system Methanol, power, 74.21
cooling and liquid
As mentioned earlier, the exergy efficiency of a process is a
fuels competitive characteristic of the thermodynamic performance. The
Ref. [52] Polygeneration Methanol production 56.09 exergy efficiencies of the four constituent units of the proposed process
and the power are calculated and it is demonstrated that HRU, SSU, MSU, and WRU
generation
have exergy efficiencies of 94 %, 93 %, 94.2 %, and 19 %, respectively,
Ref. [53] Cogeneration Dimethyl-ether and 28.75
electricity while the total exergy efficiency of the proposed process is determined at
Ref. [54] Integrated CHP system Methanol and 48.8 93.4 %. This value shows that the proposed integrated process with
incorporating solar hydrogen three products has high efficiency. Although the unit has low efficiency,
energy from the whole process point of view, it does not significantly affect the
Ref. [55] Cogeneration/SOFC Power and hydrogen 23.31
Ref. [58] Carbon dioxide and Methanol 28.18
total efficiency. By rising the feed temperature of heat exchanger HX-8,
solar energy the exergy destructions of this heat exchanger and cooler CW-10
Ref. [27] Integrated Methanol 60.7 decrease, leading to an increase in the efficiency of the WRU. Another
biomass pyrolysis, analysis of exergy is illustrated in Figs. 6 and 7, showing that reactors
gasification
with a total exergy destruction of 2116447 kW have the largest contri­
This Trigeneration Crude helium, LNG, 94.38
Study and methanol butions to exergy destruction (60 %) compared to other the equipment.
Nonetheless, it should be noted that the reactors of the SSU are the main
reason for increasing the exergy destruction of reactors because a large
equipment is written as Eq. (25) [45]: amount of exergy is released through thermal energy in the methanol
reactor. However, reformers R-1 and R-2, due to their high energy
Exi + ExQi = Exo + ExQo + Wsh + I (25)
consumption, result in occurring the maximum exergy destruction of the
where Exi is the inlet stream exergy, Exo is the outlet material stream process in reactors.
exergy, Wsh represents the shaft work, and ExQi and ExQo denote the inlet Among the heat exchangers, E-1 has the highest exergy destruction.
According to the results in Table A.1 and Fig. 7, among the three sepa­
and outlet exergies by energy streams. In addition, it represents the
ration columns, distillation column T-1 has the largest exergy destruc­
irreversibility of the system. Based on Eq. (25), the equation of exergy
tion (94.11 %). Similarly, among the expansion valves, expansion valve
destruction for each piece of equipment is given in Table 7.
V-1 with exergy destruction of 30430 kW, exhibits a 67.8 % contribution
To calculate the values of inlet and outlet exergies for each piece of
to exergy destruction.
equipment, operating conditions and thermodynamic properties of each
Among compressors C-1 to C-7 (Fig. 6 and Table A.1), the syngas
material stream are required, which are obtained from Aspen HYSYS.
compressor (C-7) with a 58.63 % contribution has the largest exergy
Therefore, the results of exergy calculations for the proposed scheme
destruction. Finally, the exergy efficiencies of the process proposed in
(Fig. 3) are summarized in Table A.1 of the appendix. According to
this paper and previous studies are compared in Table 8. The results
Fig. 4, the MSU has the largest and the WRU has the smallest exergy
show that energy integration in the process (Fig. 3) has a high impact so
destruction. In the MSU, the methanol synthesis reactor is responsible
it results in a higher exergy efficiency compared to the other
for 70.8 % of exergy destruction. While in the WRU, the maximum

Fig. 8. CO2 emission intensity from the equipment and comparison between CO2 emission contributions.

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Y. Xiao et al. Fuel 347 (2023) 128402

Table 11
Equipment capital cost [23].
Equipment Equations (Installed cost)

Compressor, pump M&S 0.82

× 517.5 × Ẇp&c (bhp) × Fc The compressor type is
280
determined by knowing its capacity.
According to the capacities, all the compressors present in
the proposed process are to be of centrifugal type.
Centrifugal pumps are like giant electric fans and involve
only rotary motion. They are cheaper than reciprocating
pumps, require less frequent maintenance, and do not
require lubrication. Their single drawback is that they are
limited to pressures of about 250 bar. Fc here is a
correction factor based on design and type of pumps and
can be found in the book of Douglas

Heat exchanger (shell & M&S

× 101.3 × A0.65 2
HEX (ft ) × (2.29 +Fc )Fc = Fm × Fig. 10. The effect of return gas ratio on the energy and exergy efficiencies, and
tube) (280 ) CO2 footprint.
Fd +Fp The Fd factor is based on the design type of the
heat exchanger, while Fp is a function of the pressure and
Fm is dependent on the material of construction. factor Fc
is calculated using tables provided in the aforementioned
textbooks. 200 < A < 5000.

pressure vessels, M&S ( )

× 101.9 × D1.066 × H0.82 × (2.18 + Fc ) D:
reactors, and columns 280
diameter of the column in ft
H: column height in ft

Trays M&S
× 4.7 × D1.55 × H × Fc Fc = FS + Fr + Fm The
280
correction factors Fs, Fr and Fm are related to tray
spacing, tray type and material of construction,
respectively and again can be found in the book by
Douglas.
Fig. 11. The effect of return gas ratio on the total cost f products.

Table 12 significantly affects the increase in the total exergy efficiency.

Results of economic evaluation of the proposed scheme.
Parameters Value
5.2. Energy analysis
Capital cost (dollars) 196,872,979
Electricity cost (dollars per year) 120,901,982
Fuel cost (dollars per year) 228,322,250 The main objective of energy analysis is to calculate the energy ef­
Cooling water cost (dollars per year) 25,317,604 ficiencies of each unit and the whole process. To derive the equations of
The total cost of energy (dollars per year) 374,541,836 energy efficiency for HRU, SSU, MSU, and WRU, first, the general mass
Total Annual cost of the proposed process ($/year) 440,166,162
annual income Cash Flow ($/year) 65,624,326
and balance equations are written and then based on these equations,
Net present value ($) 364,361,928 energy efficiency equations for each unit and the whole proposed pro­
Methanol total product cost (USD/kg) 0.013 cess are obtained. Total mass and energy equations are as follows [57]:
∑ ∑
ṁin = ṁout (26)
∑ ∑
ṁin hin + Q̇in + Ẇin = ṁout hout + Q̇out + Ẇout (27)

where ṁ is the mass flow rate at the equipment inlet and outlet, Q̇
represents the required or released heat rate of the equipment, Ẇ is the
required or produced work of equipment, and h denotes the specific
enthalpy of the inlet and outlet streams of each piece of equipment.
According to Eqs. (23) and (24), energy efficiency for a process is
calculated according to Eq. (28) [57] as:
∑
Energy input
ηenergy = 100 × ∑ (28)
Energy output
In the HRU, input energy includes the chemical energy of the NG and
power consumption in compressors C-1 to C-6, and the output energy is
Fig. 9. The effect of return gas ratio on the methanol production rate.
the sum of the chemical energies of LNG, crude helium, and fuel gas
streams (Eq. (29)) as follows[57]:
technologies. This significant superiority is because of utilizing the heat ∑
exchanger network in HRU, SSU, MSU, and WRU. On the other hand, ηHRU
mo LHVo
(29)
energy = 100 ×
recovering methanol from the overhead vapors of the scrubber column mNG LHVNG + Ẇin
leads to an increase in the chemical exergy of the products, which
Similarly, in the SSU, total input energy consists of the chemical

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Y. Xiao et al. Fuel 347 (2023) 128402

Fig. 12. The effect of the distillation tower’s solvent water flow rat on the methanol production rate.

The sum of the chemical energy of the fuel stream and the released
energy of reactor R-4 are determined, and its difference with the duty of
the reboiler of distillation column T-1 is considered as the required en­
ergy of the reboiler in the energy efficiency equation (Eq. (31)). The
produced energy of the MSU only includes the chemical energy of the
methanol stream produced in the condenser of distillation column T-1
[57]:
mmethanol LHVmethanol
ηMSU
energy = 100 ×
( ) (31)
∑
m60 LHV60 + Ẇin + Q̇reb − Q̇R4 − mFuel LHVFuel

The WRU only has a distillation column that consumes energy. In this
unit, the produced energy includes the chemical energy of the vapors
sent into the incinerator (To the incinerator stream), and consumed
energy equals the duty of the reboiler of distillation column T-3.
Therefore, the equation for the energy efficiency of this unit is as
Fig. 13. The effect of the distillation tower’s solvent water flow rate on the follows.
energy and exergy efficiencies, and CO2 footprint. In Table A.2, heating values (LHV) of products and streams
mentioned in Eqs. (29) to (32) are given. In Table 9, a summary of the
results of the energy analysis is presented [57].
mvap LHVvap
ηWRU
energy = 100 × (32)
Q̇reb
To calculate the total efficiency of the proposed process (Fig. 3), the
total input energy includes the chemical energy of NG, the required
energy for heating the reboilers and reformers R-1 and R-2, and power
consumed by the pump and compressors. The output energy consists of
the chemical energy of products helium, LNG and methanol. Eq. (30) is
written for computing the total energy efficiency. In Eq. (30), the value
of Q̇req is determined by Eq. (34) as [57]:
∑
mo LHVo
ηtotal
energy = 100 × ∑ (33)
mi LHVi + Ẇin + Q̇req
Fig. 14. The effect of the distillation tower’s solvent water flow rate on the ∑ ∑
total cost of products. Q̇req = Q̇rebs + Q̇refs − mFuel LHVFuel − mFuel2 LHVFuel2 − Q̇R4 (34)

According to Table 9, among the constituent units of the proposed

energy of the fuel gas stream (output of the HRU) and energy con­
process, the WRU has the lowest energy efficiency. In the MSU, pro­
sumption in reformers R-1 and R-2. In addition, produced energy only
ducing the fuel streams from the top of separators F-9 and F-8 along with
includes the chemical energy of the syngas stream (stream 60), and the
released energy from reactor R-4, almost supplies the required energy of
energy efficiency is calculated based on Eq. (30) as [57]:
distillation column T-1, and the energy efficiency of this unit reaches
ηSSU
m60 LHV60
(30) above 56 %. In the SSU, one of the reasons for high energy efficiency is
energy = 100 × ∑
mFuel LHVFuel + Q̇in employing heat exchangers HX-3 and HX-4, which generally recovered
1877900 kW of energy. This energy, which is transferred from Reformed
The total input energy of the MSU includes the chemical energy of
gases to fuel gas and water streams, eliminates the need for any addi­
the syngas stream (stream 60), power consumptions in compressor C-7
tional utility consumption for preheating these two streams, and on the
and pump P-3, and the required energy for the reboiler of distillation
other hand, the required energy for heating the reformers R-1 and R-2
column T-1. To calculate the required energy of the reboiler the
also decreases. Finally, according to the conducted analysis, the total
following procedure is followed:

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Y. Xiao et al. Fuel 347 (2023) 128402

Table A.1 Table A.1 (continued )

The exergy analysis of the proposed system’s sections. Helium Recovery Section
Helium Recovery Section
Equipment Ėin (kW) Ėout (kW) ĖD (kW)
Equipment Ėin (kW) Ėout (kW) ĖD (kW)
Water Recovery
C4 36,475 30,023 6452
Equipment Ėin (kW) Ėout (kW) ĖD (kW)
C5 60,345 54,129 6216
C6 76,075 70,768 5307 HX-8 199,685 27,582 172,103
CW-4 30,023 28,225 1798 CW-10 12,387 5 12,385
CW-5 54,129 49,595 4534 T-3 30,796 19,455 11,341
CW-6 70,768 67,440 3328 Total 242,868 – 195,829
C1 358 313 45
C2 501 459 42
C3 606 570 36 ηwaterrec
ex 0.19
CW-1 313 270 43
CW-2 459 418 41
CW-3 570 542 38 Total Process
E-1 1,417,044 1,005,132 411,912
Total irreversibility (kW) 3,551,190
HE-1 68,956 61,590 7366
Total Exergy input (kW) 53,899,286
V1 1,060,321 1,029,891 30,430
Overall Exergy Efficiency 0.934
V2 1,019,230 1,009,537 9693
V3 971,131 969,999 1132
F-1 1,029,891 1,027,640 2251
F-2 1,009,537 1,000,406 9131
F-3 969,999 967,876 2123
Table A.2
HE-2 187,834 178,594 9240 The Low heating value of the feed streams and products.
V4 125,151 125,151 0.0 Stream Heating value (kJ/kg)
V5 23,559 23,463 96
V6 381 259 122 Methanol 19,910
F-4 125,352 125,260 92 Overhead vapor of column T-3 556
F-5 24,228 23,940 288 Syngas (stream 60) 17,560
Total 8,363,236 – 511,756 Fuel stream 14,660
Natural gas stream 45,700
Product LNG 48,740
ηHeliumRec
ex
0.94 Product helium 1220
Fuel gas stream 29,140

Reforming Section

Equipment
energy efficiency of the proposed process is 94.38 %, which in com­
Ėin (kW) Ėout (kW) ĖD (kW)
parison with previous papers (Table 10) exhibits superiority.
P-2 1253 1116 137
HE-4 136,989 130,911 6078
HE-3 1,161,821 952,227 209,594 5.3. Environmental analysis
R-1 1,299,109 722,425 576,684
R-2 8,012,051 7,606,457 405,594
HE-5 1,315,205 1,312,068 3137 The goal of environmental analysis is to calculate the CO2 emission
CW-7 305,769 218,748 87,021 intensity for the proposed process according to Eq. (35) [57]:
R-3 7,619,847 7,502,349 117,498
F-7 218,748 216,930 1818 ( ) total CO2 emission
CO2 emission intensity kgCO2 /kgprods = ∑ (35)
F-6 325,323 325,243 80 ṁprods
Total 20,396,115 – 1,407,641
The total CO2 emission of the proposed process (Fig. 3) is due to the
0.93
heat and electricity utilities (indirect emission) and through the process
ηReforming
streams (direct emission). Therefore, Eq. (35) is rewritten as Eq. (36) for
ex

the integrated scheme proposed in this paper. To calculate the CO2

Methanol Section emission two emission factors are used which for electricity utility is
Equipment Ėin (kW) Ėout (kW) ĖD (kW)
1MWh = 596kgCO2 and for heat utility is 1MMBtu = 205.3 lbCO2 [59].

C7 373,240 347,592 25,648 ( ) CO2direct + CO2indirect

CO2 emission intensity kgCO2 /kgprods = (36)
HE-6 2,242,646 2,209,008 33,638 ṁLNG + ṁCrude He + ṁMeOH
CW-8 989,781 884,736 105,045
R-4 19,432,091 18,415,420 1,016,671 In Fig. 8, a comprehensive analysis of CO2 emission and emission
F-8 884,736 868,745 15,991 contributions in the proposed process is shown. The total CO2 emission
V7 3474 64 3410 of the proposed process equals 0.164 kgCO2 /kgprods , and according to the
HX-7 18,447 17,716 731
performed analysis, 73 % of total emission is due to the emission related
T-1 913,157 695,786 217,371
T-2 20,866 18,598 2268 to the required heating of reactors R-1 and R-2 and the reboiler of the
P-3 3382 3382 0 methanol separation distillation column (T-1). In addition, assessments
CW-9 15,219 28 15,191 show that indirect emission has the highest contribution (94 %) to the
F-9 28 28 0
total CO2 emission of the proposed process.
Total 24,897,067 – 1,435,964

ηMethanol
ex
0.942 5.4. Economic analysis

Determining the total annualized cost of the proposed scheme and

the total product cost of methanol is the goal of economic analysis. For
this purpose, Eqs. (37) [60] and (35) [61] are used:

13
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Y. Xiao et al. Fuel 347 (2023) 128402

Table A.3 and Swift (M&S) and is updated monthly by Chemical Engineering [23].
The components’ installation costs. Cost of energy includes fuel cost (5 dollars per gigajoule) required in
Component Investment Cost [USD] reformers R-1 and R-2, reboiler thermal energy (5 dollars per gigajoule
[64] for NG under the conditions of 446 kPa and 25 ◦ C), electricity
C2 970,200
HX-7 661,000 consumption in compressors and pumps (0.06 dollars per kWh [64]),
F-9 180,200 and cooling water (0.354 dollars per gigajoule [64]). In addition, in
F-1 1,970,100 Table 12, results of economic calculations are given and the components
R-4 1,458,741 installation costs are listed in Table A.3. Based on the performed anal­
F-8 745,841
T-2 2,385,400
ysis, the total product cost of methanol through CO2 hydrogenation has
C6 12,961,400 been 0.27 dollars [23], which is higher than the total product cost of
E-1 458,743 methanol in this paper. This comparison shows that multi-generation
C7 31,371,900 systems have the capability to produce methanol with a lower product
CW-9 1,667,900
cost. In addition, comparing the total product cost with Ref. [61] dem­
F-4 471,200
HE-2 479,514 onstrates that the total product cost of methanol by the proposed method
CW-6 2,016,000 (Fig. 3) is lower by 95.19 %. Moreover, a comparison of the total product
CW-10 3,993,800 cost with that of Ref. [47] illustrates that the methanol production by
CW-2 74,400 the process proposed in this paper exhibits a 77.19 % decrease compared
CW-3 76,000
HE-5 525,415
to methanol production from coke oven gas.
CW-7 7,591,100
CW-1 75,200
HE-3 695,748 5.5. Parametric study
F-3 1,567,500
C3 972,900
A portion of the non-reacted gasses is returned to the methanol
F-6 1,077,400
T-3 425,700 reactor through the separator of F-8. Hence, the gas return ratio is
P-2 739,400 assumed as an independent parameter and the effect of this parameter
C4 1,698,125 on the system’s performance is probed in this section. The increment of
F-2 1,628,100 return gas ratio enhances the CO2 change value in R-4, leading to
CW-4 2,560,200
HE-6 16,045,100
increasing the methanol production rate, which is shown in Fig. 9. The
C1 950,500 methanol production rate’s enhancement improves the energy and
T-1 42,129,700 exergy efficiencies and declines the CO2 footprint in the designed tri­
CW-8 25,597,200 generation, as shown in Fig. 10. Accordingly, increasing the methanol
HE-1 598,412
production rate affects the system’s total product cost in which this
HE-4 395,125
C5 23,226,700 index faces with and descending trend, which is plotted in Fig. 11.
P-3 113,300 The second effective parameter on the thermodynamic performance
F-7 680,500 indexes is the flow rate of the distillation tower’s solvent water.
F-5 276,800 Increasing the distillation tower’s solvent flow rate enhances the
R-1 585,265
R-2 1,420,150
methanol production rate, which is the consequence of the methanol
CW-5 1,727,400 recovery from vapors (see Fig. 12). But this parameter increments up to
R-3 505,652 20,000 kmol/h recovers all methanol and the higher flow rates do not
HX-8 1,627,700 affect the methanol production. Besides, this increment raises the
reboiler duty in the T-1, which is not desired. Due to enhancing the
∑ methanol production rate, the thermodynamic efficiencies increase and
total capitla cost( Ci )
TAC = + Energy cost, where payback period 3 years the CO2 footprint declines, which is illustrated in Fig. 13. Also, the total
payback period
product cost’s trend versus the flow rate of the distillation tower’s sol­
(37)
vent water is shown in Fig. 14 in which this economic index due to the
TAC methanol production’s trend, continually reduces continually.
methanol total product cost (USD/kg) = (38)
annual product
6. Conclusion
By assuming term payback period of about 3 years, the annual in­
come cash flow (CF) is obtained as [62]: In this paper, a process for the production of helium, LNG, and
∑
Ci methanol is proposed, which has high thermodynamic efficiency, low
Payback period = (39) methanol loss, and also low CO2 emission. The proposed scheme consists
CF
of helium recovery synthesis gas through NG reforming, and methanol
As an economic performance index, the net present value (NPV) is synthesis. The main feed of the designed scheme is the natural gas in
estimated as the following [62]: which after the separation of helium and producing LNG, the waste gas
∑ (1 + n)d − 1 is reformed and due to producing the synthesis gas, methanol is ob­
NPV = − Ci + CF (40) tained. The designed system is analyzed from energy, exergy, economic,
n(1 + n)d
and environmental viewpoints and the obtained results are compared
Where n is the interest rate and d depicts the system’s lifetime, which are with some previous investigations to show its advantages. In this way,
0.1 and 20 years, respectively [63]. Equipment Installation costs, which the following conclusions are made:
in total form the total investment cost, are calculated based on the
equations in Table 11 [23]. The costs are further corrected with • The proposed system provides 4105 kg/h crude helium, 3,594,000
Chemical Engineering’s Plant Cost Index. Economic evaluations in this kg/h LNG, and 707,800 kg/h methanol, leading to achieving 94.38 %
study are based on the correlations given by Douglas. One of the most energy and 93.4 % exergy efficiencies.
commonly used cost indices for cost scaling up is published by Marshall • The application of a distillation tower all methanol content of the
vapor flows is absorbed and the methanol production rate increases.

14
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Y. Xiao et al.
• The exergy analysis indicates that the total exergy destruction rate is
about 3551190 kW in which the methanol synthesis unit by
1435964 kW has a portion of 40.44 %. Also, the WRU has the lowest
exergy performance.
• Over 90 % of the CO2 emission is carried out by the indirect mode,
which is performed through the power and heat utilities. Also, the
CO2 footprint is obtained at about 0.16 kgCO2 /kgprods .
• The return gas ratio and the distillation tower’s solvent flow rate are
the main effective parameters of the thermodynamic performance of
the system. Increasing these parameters improve energy and exergy
efficiencies, and reduces the CO2 footprint.
• The system’s annual and product costs rate are obtained at about
364.36 M$ and 0.013 USD/kg, which led to achieving 440.16 M$ net
present value in the system’s lifetime.
Conceptual design and modeling of novel-integrated process con­
figurations for helium extraction, natural gas liquefaction, and methanol
is investigated. Aspen HYSYS was used for the simulations and techno-
economic analysis to evaluate the potential of hybrid plant for the
direct recovery helium from natural gas. Detailed energy and exergy
analyses were considered to identify and allocate the source of ther­
modynamic inefficiencies within the considered separation and recov­
ery system. However, advanced exergy and economic analyses are
missing in the current study. It is recommended to consider the
advanced exergy and exergoeconomic analyses of the novel hybrid
system in the future studies.
CRediT authorship contribution statement
Yang Xiao: Conceptualization, Methodology, Validation, Writing –
review & editing, Writing – original draft. Shengbin Wu: Formal
analysis, Methodology, Validation, Investigation, Supervision, Funding
acquisition. Hantao Xia: Validation, Formal analysis, Investigation.
Jinyuan Zhang: Data curation, Software, Conceptualization, Writing –
review & editing. Lingling Ding: Conceptualization, Writing – review &
editing. Xiaolong Bao: Conceptualization, Methodology, Writing – re­
view & editing. Yi Tang: Conceptualization, Methodology, Writing –
review & editing. Yongjie Qi: Visualization, Writing – review & editing.
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.
Acknowledgment
This work was supported by the Natural Science Foundation of
Sichuan Province, grant number 2023NSFSC0426.
Appendix
This appendix chapter consists of the proposed system’s exergy
analysis, specified component by component, the low heating value of
the feed streams and products, and components’ installation costs, ob­
tained from economic analysis, which is reported in Tables A.1, A.2, and
A.3.
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Fuel 347 (2023) 128402
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