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Received: 28 September 2018 Revised: 4 December 2018 Accepted: 5 December 2018

DOI: 10.1002/er.4367

RESEARCH ARTICLE

Cost‐competitive methane steam reforming in a membrane


reactor for H2 production: Technical and economic
evaluation with a window of a H2 selectivity

Boreum Lee | Hankwon Lim

School of Energy and Chemical


Engineering, Ulsan National Institute of
Summary
Science and Technology (UNIST), 50 Techno‐economic viability studies of employing a membrane reactor (MR)
UNIST‐gil, Eonyang‐eup, Ulju‐gun, Ulsan equipped with H2 separation membranes for methane steam reforming
44919, Republic of Korea
(MSR) were carried out for H2 production in Korea using HYSYS®, a well‐
Correspondence known chemical process simulator, including economic analysis based on
Hankwon Lim, School of Energy and
itemized cost estimation and sensitivity analysis (SA). With the reaction
Chemical Engineering, Ulsan National
Institute of Science and Technology kinetics for MSR reported by Xu and Froment, the effect of a wide range of
(UNIST), 50 UNIST‐gil, Eonyang‐eup, H2 selectivity (10‐10,000) on the performance in an MR was investigated in this
Ulju‐gun, Ulsan 44919, Republic of Korea.
study. Because of the equilibrium shift owing to the Le Chatelier's principle,
Email: hklim@unist.ac.kr
great performance of enhancement of methane conversion (XCH4 ) and H2 yield
Funding information and reaction temperature reduction was observed in an MR compared with a
Korea Institute of Energy Technology
Evaluation and Planning, Grant/Award
packed‐bed reactor (PBR). A window of a H2 selectivity from 100 to 300 is
Number: 20182020201260 proposed as a new criterion for better MR performance of MSR depending
on potential applications from in‐depth analysis of XCH4 and H2 yield
enhancements, a H2 purity, and temperature reduction. In addition, economic
analysis to evaluate the feasibility of an MR technology for MSR was carried
out focusing on a levelized cost of H2 based on itemized cost estimation of
capital and operating costs as well as SA. Techno‐economic assessment showed
36.7% cost reduction in an MR compared with a PBR and revealed that this MR
technology can be possibly opted for a cost‐competitive H2 production process
for MSR.

KEYWORDS
levelized cost of hydrogen, membrane reactor, methane steam reforming, techno‐economic
assessment

Nomenclature: MSR, Methane steam reforming; LCOH, Levelized cost of H2; NG, Natural gas; WGSR, Water gas shift reaction; PBR, Packed‐bed
reactor; PSA, Pressure swing adsorption; GHG, Greenhouse gas; MR, Membrane reactor; SA, Sensitivity analysis; PFD, Process flow diagram; PR
EOS, Peng‐Robinson equation of state; ri, Reaction rate of i (kmol kgcat−1 h−1); k1, Reaction rate constant of 1 (kmol bar0.5 kgcat−1 h−1); k2,
Reaction rate constant of 2 (kmol kgcat−1 h−1); k3, Reaction rate constant of 3 (kmol bar0.5 kgcat−1 h−1); Pi, Partial pressure of i (bar); Ki,
Equilibrium constant of i; DEN, Denominator; F i, Flow rate (mol s−1); PSA OPEX, PSA operating expenses; CEPCI, Chemical engineering plant
cost index; Ci, Purchased cost of i; Ai, Equipment capacity of i; n, Cost index; CRF, Capital recovery factor; i, Discount rate; N, Period of use; TCI,
Total capital investment

1468 © 2019 John Wiley & Sons, Ltd. wileyonlinelibrary.com/journal/er Int J Energy Res. 2019;43:1468–1478.
LEE AND LIM 1469

1 | INTRODUCTION

Hydrogen (H2) has been widely utilized in various indus-


trial fields such as chemicals, electronics, metal, food, fer-
tilizer, and electric power industries as well as H2 fueling
stations, as shown in Figure 1.1 In addition, H2 has
recently received considerable interests as a promising
alternative energy carrier since it is a clean and easy‐to‐
handle fuel with a higher energy yield (122 kJ kgH2−1)
than hydrocarbon fuels.2 In this context, it is very crucial
to find better pathways to produce H2 enough to meet
this strong demand. Methane steam reforming (MSR) is
currently being commercially used for H2 production3,4
because of its high efficiency and low levelized cost of FIGURE 2 Global H2 production methods8 [Colour figure can be
viewed at wileyonlinelibrary.com]
H2 (LCOH) compared to other methods like oil‐based
H2 production, coal gasification, and water electrolysis.5,6
Moreover, natural gas (NG) made up mostly of methane 1. use of a lot of energy due to the endothermic nature of
(CH4) has been considered as being more eco‐friendly MSR and extremely high operating temperature leading
than conventional fossil fuels.7 The MSR technology to limited selection of a suitable reformer and catalyst;
accounts for approximately 48% of global H2 production, 2. emission of CO2, a greenhouse gas (GHG) known as a
as shown in Figure 2,8,9 and is a well‐known process major contributor to global warming; and
consisting of MSR (Equations 1 and 3) and high‐ and 3. requirement of an additional H2 purification equipment
low‐temperature water gas shift reaction (WGSR; Equa- like PSA leading to significant capital and operating costs.
tion 2). Figure 3A shows a conventional reforming system
consisting of a packed‐bed reactor (PBR) for MSR, high‐ A membrane reactor (MR) concept combining a
and low‐temperature shift reactors for WGSR, and pres- reactor and a H2 separator in a single unit has been intro-
sure swing adsorption (PSA) for H2 purification. duced to solve the aforementioned problems, as shown in
Figure 3B, and some benefits of the MR concept
CH4 þ H2 O→CO þ 3H2 ΔCH0298 ¼ 206 kJ mol−1 ; (1) are depicted as follows. First, higher methane conversion
( XCH4 ) and H2 yield through equilibrium shift owing to
CO þ H2 O→CO2 þ H2 ΔH0298 ¼ −41 kJ mol−1 ; (2) the Le Chatelier's principle11 can result in the reduction
in an operating temperature for the equal amount of the
CH4 þ 2H2 O→CO2 þ 4H2 ΔH0298 ¼ 165 kJ mol−1 : (3) desired product. Second, a purified H2 without further
post‐purification equipment like PSA can be obtained.
Even though this MSR technology is a commercially
Last, a simpler design is possible because of the combina-
viable and mature process, there exist several drawbacks,
tion of a reactor and a H2 separator in one single unit lead-
as depicted below10:
ing to compact reactor design and cost savings in capital
and operating costs compared with those of a conventional
PBR. Many studies on H2 production via the improved
membrane properties for MSR in an MR have been
reported as shown in Table 1.12-17 Although an MR has
these benefits, it has also main downsides such as a
trade‐off between a H2 permeance and a H2 selectivity as
well as high costs due to the use of palladium (Pd)‐based
membranes.18,19 In order to make up for the aforemen-
tioned weak points of an MR, studies on membrane perfor-
mance have been done. Oyama and Lim20 studied the
impact of a H2 selectivity on reactant conversion and a
H2 yield enhancement for various reforming reactions in
MRs based on a one‐dimensional numerical study. In par-
ticular, they suggested that a H2 selectivity of 100 is enough
FIGURE 1 Distribution of a global H2 market1 [Colour figure to obtain reasonable performance in an MR. Ghasemzadeh
can be viewed at wileyonlinelibrary.com] et al21 also carried out numerical studies using a one‐
1470 LEE AND LIM

FIGURE 3 The schematic diagrams: A, a conventional reforming system using a packed‐bed reactor (PBR); B, a proposed reforming
system using a membrane reactor (MR) [Colour figure can be viewed at wileyonlinelibrary.com]

dimensional reactor model for methanol steam reforming 2 | METHODS


in a silica MR and investigated the effect of various operat-
ing parameters such as sweep factor, catalyst loading, reac- 2.1 | Comparative process simulation
tion pressure and temperature, and a H2 selectivity on studies of a PBR and an MR
methanol conversion and a H2 recovery. They reported
the little benefit of a H2 selectivity on both reactant conver- Process simulation is widely used to analyze chemical
sion and product yield in an MR when a H2 selectivity is processes of interest and to find optimized operating con-
higher than 100. From literature survey results, it was iden- ditions based on the process simulation results obtained
tified that although many researchers have released papers from material and energy balances of the whole system.
on effective H2 production via the enhanced membrane Currently, commercial process simulators are being used
property for MSR in an MR. In contrast, there are both as robust tools for chemical process simulation such as
previous studies by Oyama and Lim20 and Ghasemzadeh HYSYS® (AspenTech, Inc., Beford, MA, USA),22-24 Aspen
et al21 focusing on the optimized H2 selectivity only among Plus® (AspenTech, Inc., Beford, MA, USA),25-27 Unisim
membrane properties in an MR but no economic analysis Design® Suite (Honeywell, Morris Plains, NJ, USA),28-30
for comparison between a PBR and an MR. In this context, and CHEMCAD (Chemstations, Inc., Houston, TX,
it is timely to evaluate economic feasibility for H2 produc- USA).31-33 Among them, HYSYS was selected in this paper
tion by an MR because membrane is premature technology as an appropriate process simulator for a PBR and an MR
for applying to H2 production. So, here, we report eco- because it is well opted for gas processing technology.
nomic comparison between a PBR and an MR was con- Figure 4A shows a process flow diagram (PFD) of a PBR.
ducted on the basis of itemized cost estimations and First, CH4 and H2O compressed to a desired pressure are pre‐
sensitivity analysis (SA) with an optimized window of a heated using a heat exchanger before being fed to a PBR, a
H2 selectivity proposed on the basis of simulation results. catalytic reactor including active catalysts. The kinetics
LEE AND LIM 1471

TABLE 1 Literature survey on H2 production for methane steam reforming (MSR) in a membrane reactor (MR)

Author Method Comment

Iulianelli et al12 Experiment ‐ Perform the comparative experiment for MSR with or without Pd‐MR using a Ni‐based
catalyst.
‐ Obtain a 50% methane conversion and 70% COx‐free H2 recovery at 723 K, 3.0 bar, 1.6 sweep
factor in an MR.
‐ Observe a 6% methane conversion with same operating conditions in conventional MSR.
Patrascu and Experiment, ‐ Carry out an MSR at the temperature range of 713‐793 K in an MR consisting of a 175 cm2 Pd
Sheintuch13 numerical modeling membrane and foam catalyst.
‐ Indicate the experiment result as 90% methane conversion and 80% H2 recovery when CH4
input of 0.25 NL min−1, wall temperature of 798 K, pressure of 10 bar, S/C of 3, and sweep gas
flow of 0.7 NL min−1.
Marcobernardino Experiment, ‐ Find out the H2 permeability value of 5.16E−11 mol m−1 s−1 Pa−0.71 for thinner Pd‐Ag
et al14 numerical modeling membrane at 723 K.
‐ Determine the optimized temperature and pressure conditions in an MR at 873 K and 500 kPa,
respectively.
Kyriakides et al15 Experiment, ‐ Conduct an MSR experiment using an MR and clearly show that a higher pure H2 was
numerical modeling produced because of the increased methane input flow rate.
‐ Determine the optimized reaction parameters by describing numerical modeling based on
experimental data (length of 0.443 m, CH4 flow rate of 0.0262 mol min−1, sweep gas
volumetric flow rate of 8.88 m3 s−1, and membrane surface of 0.0195 m2).
Chompupun et al Experiment, 3D ‐ Investigate comparative study for MSR with or without Pd‐MR using a 10 wt% Ni/Al2O3
16
modeling catalyst.
‐ Verify the high performance in terms of CH4 conversion of 61.5% for a conventional reactor
and 87.1% for an MR, respectively.
‐ Design 3D model on the basis of experimental data and use kinetic parameters for scale‐up of
reactor.
Spallina et al17 Techno‐economic ‐ Implement a comparative TEA for fired tubular reforming (FTR), fluidized bed MR (FBMR),
analysis (TEA) and membrane‐assisted chemical looping reforming (MA‐CLR).
‐ Identify the H2 production cost of 0.28€ Nm3H2−1 for FTR, 0.22€ Nm3H2−1 for FBMR, and
0.19€ Nm3H2−1 for MA‐CLR.
‐ Provide influential factors (membrane, reactor, and natural gas) for H2 production cost via
sensitivity analysis.

reported by Xu and Froment4 with a Ni/MgAl2O4 catalyst as


 
shown in Equations 4 to 17 was incorporated into a PBR and k 3 PCH4 P2H 2 O =P3:5
H2 − P H2 P CO2 =K 1 K 2
0:5
high‐ and low‐temperature shift reactors were not included r3 ¼ ; (6)
for this analysis. After MSR in a PBR, product contains DEN 2
unreacted CH4 and H2O as well as produced CO, CO2, and
H2. Then, it is passed via a cooler to remove unreacted DEN ¼ 1 þ KCO PCOþ K H2 PH2 þ K CH4 PCH4
H2O. After water separation, gas is compressed to increase PH2 O
þ K H2 O ; (7)
the pressure before being fed into PSA to obtain the desired PH2
H2 purity. After PSA process, tail gas is used to supply the
 
required heat for the system by burning it in a boiler. −240 100
k1 ¼ 4:17 × 1015 exp ; (8)
RT
 
k 1 PCH4 PH2 O =P2:5  
H2 − P H2 P CO =K 1
0:5
67 130
r1 ¼ ; (4) k 2 ¼ 1:95 × 106 exp ; (9)
DEN 2 RT

 
k 2 ðPCO PH2 O =PH2 − PCO2 =K 2 Þ −243 900
r2 ¼ ; (5) k3 ¼ 1:00 × 10 exp
15
; (10)
DEN 2 RT
1472 LEE AND LIM

FIGURE 4 Process flow diagrams: A, a packed‐bed reactor (PBR); B, a membrane reactor (MR) [Colour figure can be viewed at
wileyonlinelibrary.com]

   
−4 38 280 −2 37 300
K CH4 ¼ 6:65 × 10 exp ; (11) K 2 ¼ 1:14 × 10 exp ; (16)
RT RT

  K 3 ¼ K 1 × K 2; (17)
−88 680
K H2 O ¼ 1:77 × 105 exp ; (12)
RT where ri is chemical reaction rate of i (i = 1, 2, and 3), Pi is
  partial pressure of i (i = CO, H2, CH4, and H2O), ki is chem-
−5 70 650 ical reaction rate constant of i (i = 1, 2, and 3), Ki is equilib-
K CO ¼ 8:25 × 10 exp ; (13)
RT rium constant of i (i = 1, 2, 3, CO, H2, CH4, and H2O), R is
  gas constant, and T is reaction temperature. As an appropri-
−9 82 900 ate fluid package required in the proposed simulation, the
K H2 ¼ 6:15 × 10 exp ; (14)
RT Peng‐Robinson equation of state (PR EOS) was employed
  and all simulation works were carried out assuming a steady
−224 000 state operation. In addition, an isothermal condition was
K 1 ¼ 4:71 × 10 exp
12
; (15)
RT assumed for fair comparison between a PBR and an MR,
LEE AND LIM 1473

and the required heat due to endothermic reaction for both 2.2 | Economic analysis: LCOH
reactors was calculated on the basis of energy balance.
Figure 4B shows a PFD of an MR for MSR with same Itemized cost estimations were conducted to compute an
configurations with a PBR except the use of H2‐selective LCOH for MSR in a PBR and an MR based on previous
membranes inside a reactor. For both PBR and MR, high‐ study results (chemical process simulation) and current
and low‐temperature shift reactors were not considered in economic status in Korea to assess economic feasibility
this study. In the MR, a H2O was used as a sweep gas to drive for MSR in a PBR and an MR. Total cost was calculated
enough PH2 , which is H2 partial pressure difference between by summing capital costs and operating costs. Capital cost
both retentate and permeate (PH2 ;retentate − PH2 ;permeate ) so that consists of equipment cost like a reactor, membrane mod-
concentration polarization is minimized. As an MR is not ules, a compressor, and a PSA and supplement cost and
in the modeling library of HYSYS®, we created a template operating cost is composed of electricity, PSA operating
for an MR being made up a series of five reactors and five expenses (PSA OPEX), labor, membrane replacement,
H2 separators in this study34,35 to reflect the function of an NG, maintenance, and other operating costs.41-43 In par-
MR properly like continuous H2 removal through mem- ticular, membrane replacement cost was classified as an
branes during MSR in a reactor. The pressure difference operating cost to consider membrane lifetime. Costs of a
between a retentate and a permeate was 2.5 bar and reaction reactor,44 a compressor,45 a PSA, and a PSA OPEX46 were
was performed under conditions of a H2 permeance36 of obtained on the basis of previously reported studies. In
3 × 10−6 mol m−2 s−1 Pa−1 and a H2O sweep gas molar this paper, a chemical engineering plant cost index
flow rate of 1 mol s−1 at 773 K. A wide range of H2 selectivity (CEPCI) as of 2016 was employed to properly take cost
(10‐10,000), which is defined as the ratio of H2 permeance variations into account in time for equipment47 and costs
over other gas in an MR expressed as Equation 18, was of equipment in different capacities were calculated on
chosen for MR studies, and the length of a membrane was the basis of a six‐tenths rule as shown in Equation 21.
set at 25 cm targeting a production of H2 (1 m3 h−1).  n
Ca Aa
¼ ; (21)
H 2 permeance Cb Ab
H 2 selectivity ¼ ; (18)
Other gas permeance
where C is equipment cost ($), A is equipment capacity
where H2 permeance is H2 molar flow rate passing from a (m3 h−1), and n is cost exponent for equipment size
retentate to a permeate (mol s−1) and Other gas permeance (n = 0.6, based on a six‐tenths rule).47 In addition, item-
is other gas molar flow rate passing from a retentate to a per- ized annual capital costs were calculated by converting
meate except for H2 (mol s−1). initial capital costs to annual capital costs via capital
In addition, a H2 flow rate passing from a retentate to a recovery factor (CRF) (Equation 22).41,47
permeate was calculated on the basis of Equation 19 instead
of using the Sievert's law,37 which is commonly used in calcu- i ð1 þ i ÞN
CRF ¼ ; (22)
lating H2 permeation related to dense Pd membrane, because ð1 þ i ÞN − 1
of recent development of a thin H2 membrane strongly
showing dependence on partial pressure difference.38,39 where i is a discounted rate of 8% as a conservative inter-
est rate and N is project period (10 y used in this paper).

F H2 ;permeate ¼ H 2 permeance × Area × PH2 ;ret − PH2 ;per ; Supplement cost was 20% of total capital investment
(19) (TCI), which is defined as the sum of equipment cost of
a reactor, membrane modules, a compressor, and a PSA.
where F H2 ;permeate is a H2 flow rate passing from a retentate to A stream factor was assumed as 1 and electricity was cal-
a permeate (mol s−1), H2 permeance is the molar flux via culated considering annual electricity consumption of
membrane per unit driving force (mol [m2 s Pa]−1), Area is compressor for reactants and pretreatment of PSA for a
membrane surface area (m2), PH2 ;ret is partial pressure of PBR with electricity price of $0.06 kWh−1.48 The US
H2 in a retentate (Pa), and PH2 ;per is partial pressure of H2 Department of Energy target price of H2 separation mem-
in a permeate (Pa). branes ($5382 m−2) was adopted to calculate operating
An enhancement of CH4 conversion and H2 yield costs for membranes.44 Annual costs for labor were calcu-
owing to the Le Chatelier's principle in an MR compared lated on the basis of labor for a part‐time worker in Korea
with a PBR was calculated using Equation 20.23,40 ($16 667 y−1). Maintenance and other operating costs
were 2% and 1% of TCI, respectively.49 Based on itemized
MR − PBR cost estimation results, an LCOH can be calculated by
Enhancement ð%Þ ¼ × 100: (20)
PBR dividing total annual costs by the amount of H2 produced.
1474 LEE AND LIM

2.3 | Economic analysis: SA flow rate of 1 mol s−1. For all MRs studied, higher XCH4
and H2 yield compared with those of a PBR were
SA is widely used to consider price fluctuations associated observed because of the equilibrium shift owing to the
with each economic parameter used in economic analy- Le Chatelier's principle. Overall trend of decreased XCH4
sis. The effect of change in economic parameter on an
LCOH in a PBR and an MR was studied via SA.23,40,47
Economic parameters adopted for SA were all economic
parameters covered in this work. By changing key eco-
nomic parameters by ±20%, the effect of each parameter
on an LCOH was represented by tornado diagrams.

3 | R E S U L T S AN D D I S C U S S I O N

3.1 | Impact of a H2 selectivity on


performance in an MR

Figure 5A presents the impact of a H2 selectivity on XCH4


and H2 yield enhancements at 773 K in an MR equipped
with H2 membranes with a H2 permeance of FIGURE 6 Impact of a H2 selectivity on temperature reduction
3 × 10−6 mol m−2 s−1 Pa−1 and a H2O sweep gas molar in a membrane reactor (MR). PBR indicates packed‐bed reactor
[Colour figure can be viewed at wileyonlinelibrary.com]

TABLE 2 Itemized cost estimations of a levelized cost of H2


(LCOH) for a packed‐bed reactor (PBR) and a membrane reactor (MR)

H2
PBR, H2 Production MR, Production
Item $ y−1 Cost, $ kgH2−1 $ y−1 Cost, $ kgH2−1

1. Capital cost 1995 1.88 790 0.75


Reactor 523 0.49 522 0.49
Membrane — — 117 0.11
module
Compressor 125 0.12 19 0.02
PSA 1015 0.96 — —
Supplement 333 0.31 132 0.12
2. Operating 2241 2.11 1892 1.79
cost
Electricity 192 0.18 23 0.02
PSA OPEX 2 0.002 — —
Labor 1667 1.57 1667 1.57
Membrane — — 23 0.02
replacement
Natural gas 46 0.04 46 0.04
Maintenance 223 0.21 88 0.08
Other 112 0.11 44 0.04
operating
costs
FIGURE 5 Impact of a H2 selectivity: A, CH4 conversion (XCH4 ) 3. Total cost 4236 4.00 2681 2.53
and H2 yield enhancements; B, a H2 purity in a permeate. PBR
Cost savings 36.7%
indicates packed‐bed reactor [Colour figure can be viewed at
wileyonlinelibrary.com] Abbreviations: PSA, pressure swing adsorption; OPEX, operating expense.
LEE AND LIM 1475

and H2 yield enhancements with an increased H2 selec- a main downside of an MR, as mentioned earlier. There-
tivity was observed in an MR. That is to say, high H2 fore, low H2 permeance results in decreased H2 yield and
selectivity means low H2 permeance because of trade‐off XCH4 because of little effect of equilibrium shift due to the
between a H2 permeance and a H2 selectivity, which is Le Chatelier's principle. In particular, a H2 selectivity

FIGURE 7 Itemized cost estimation of a levelized cost of H2 (LCOH): A, a packed‐bed reactor (PBR); B, a membrane reactor (MR). PBR
indicates packed‐bed reactor; PSA, pressure swing adsorption; OPEX, operating expense [Colour figure can be viewed at wileyonlinelibrary.com]

FIGURE 8 Sensitivity analysis: A, a conventional packed‐bed reactor (PBR); B, a membrane reactor (MR) using a tornado plot. PSA
indicates pressure swing adsorption; OPEX, operating expense [Colour figure can be viewed at wileyonlinelibrary.com]
1476 LEE AND LIM

slowed the significant impact on XCH4 enhancement at a purity, and it proves to demonstrate well the economic
lower H2 selectivity with little at a higher H2 selectivity. benefit of the MR. In addition, Figure 7 presents a visual
In contrast, little influence of a H2 selectivity was observed representation of itemized cost estimation for the PBR
for a H2 yield enhancement except some minor effects at a and the MR combining a pie chart and bar graph. This
lower H2 selectivity. Obviously, the effect of a H2 selectiv- cost reduction was mainly because of a huge reduction
ity on the performance in an MR was less dominant when in capital costs in the MR (approximately 60%) compared
a H2 selectivity is more than 100, reasonably confirming with the PBR owing to a PSA. The elimination of a PSA
previous studies.20,21 However, an in‐depth analysis of also decreased operating costs in the MR.
XCH4 and H2 yield enhancements (Figure 5A) coupled with
H2 purity (Figure 5B) provided a good window of a H2
selectivity ranging from 100 to 300, which is equivalent 3.4 | Economic analysis: SA
to 97.07% and 99.01% of a H2 purity, respectively.
Therefore, it can be concluded that a H2 selectivity of SA was conducted to observe how much an LCOH could be
300 should be chosen for a H2 purity comparable with changed according to the price fluctuation of each economic
PSA (>99%)46 with a H2 selectivity of 100 employed for parameter and to identify the key economic parameters
industrial application like a combustion engine requiring affecting an LCOH. Figure 8 depicts how an LCOH varies
a H2 purity of approximately 97%.50 From this analysis, a when SA is carried out for both a PBR and an MR using tor-
window of a H2 selectivity depending on potential applica- nado plot. The most deterministic economic parameter to
tions was well demonstrated as a new criterion for an MR. decide an LCOH was marked with the star symbol. From
SA result, the three important parameters are labor, a
PSA, and a reactor for a PBR and labor, a reactor, and
3.2 | Impact of a H2 selectivity on membrane modules for an MR in the order named. In
temperature reduction in an MR particular, the most important key economic factor is labor
for both reactors. It is believed that labor is the most influen-
Figure 6 illustrates the impact of a H2 selectivity on the
tial factor because a current MR system is a small‐scaled
reduction in reaction temperature in an MR compared
capacity and different key economic factors can be possibly
with a PBR denoted by TPBR − TMR. Because of the
obtained with increased H2 production capacities.47
improved H2 production in an MR, lowered operating
temperature can be possible in an MR for the equal
amount of H2 production as the one in a PBR. This temper-
ature reduction can lead to various advantages of numer-
4 | C ON C L U S I ON S
ous options for catalysts and reactor materials, reduced
In this study, techno‐economic viability studies for MSR
energy for overall system, and cost savings. Apparently, a
in an MR have been conducted to evaluate the economic
significant temperature reduction was obtained for an
viability of using an MR technology for H2 production
MR with a lower H2 selectivity, while the reduction was lit-
and the results are as follows.
tle when it is more than 300. Therefore, we propose here a
window of a H2 selectivity from 100 to 300 for the best per-
• Process simulation studies provided a window of a H2
formance of an MR depending on potential applications
selectivity from 100 to 300, which is the optimized range
from a thorough analysis of XCH4 and H2 yield enhance-
in terms of CH4 conversion and H2 yield enhancements,
ments, a H2 purity, and temperature reduction.
a H2 purity, and temperature reduction in the MR.
• Economic analysis focusing on an LCOH using
3.3 | Economic analysis: LCOH itemized cost estimations (H2 selectivity of 300) was
conducted and an LCOH of $4.00 and $2.53 kgH2−1
To be equivalent to the performance of a PSA, a H2 purity was obtained in a PBR and an MR, respectively, pre-
of more than 99% should be guaranteed. Therefore, a H2 senting approximately 37% cost reduction in the MR.
selectivity of 300 was chosen for economic analysis in this • SA provided three economic parameters influencing
paper to estimate an LCOH for a PBR and an MR. Table 2 an LCOH (labor, PSA, and reactor for the PBR and
presents itemized cost estimations to obtain an LCOH for labor, reactor, and membrane module for the MR).
a PBR and an MR with a H2 selectivity of 300 based on
capital and operating costs. An LCOH for MSR in a Conclusively, it is well demonstrated that an MR
PBR and an MR was $4.00 and 2.53 kgH2−1, respectively, technology, compared with a PBR, can serve as a cost‐
showing a significant cost reduction in the MR (36.7%) competitive method to produce H2 because of the
due to the elimination of a PSA to obtain the desired H2 improved H2 production leading to lowered costs.
LEE AND LIM 1477

A C K N O WL E D G E M E N T 14. Marcobernardino GD, Sosio F, Manzolini G, Campanari S. Fixed


bed membrane reactor for hydrogen production from steam
This work was supported by the Korea Institute of Energy methane reforming: experimental and modeling approach. Int
Technology Evaluation and Planning (KETEP) granted J Hydrogen Energy. 2015;40:7559‐7567.
financial resource from the Ministry of Trade, Industry 15. Kyriakides AS, Voutetakis S, Papadopoulou S, Seferlis P. Optimiza-
& Energy, Republic of Korea (No. 20182020201260). tion of an experimental membrane reactor for low‐temperature
methane steam reforming. Clean Technol Environ Policy.
2016;18:2065‐2075.
ORCID
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Boreum Lee https://orcid.org/0000-0003-3169-8520 Ramachandran PA. Experiments, modeling and scaling‐up of
Hankwon Lim https://orcid.org/0000-0002-1074-0251 membrane reactors for hydrogen production via steam methane
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