Energy Conversion and Management 279 (2023) 116758

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Energy Conversion and Management

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

Carbon-neutral hydrogen production from natural gas via electrified steam

reforming: Techno-economic-environmental perspective
Thai Ngan Do a, 1, Hweeung Kwon b, 1, Minseong Park a, Changsu Kim a, Yong Tae Kim c, 2,
Jiyong Kim a, *, 2
a
School of Chemical Engineering, Sungkyunkwan University, Suwon 16419, Republic of Korea
b
KOGAS Research Institute, Korea Gas Corporation, Daegu 41062, Republic of Korea
c
C1 Gas & Carbon Convergent Research Center, Korea Research Institute of Chemical Technology, Daejeon 34114, Republic of Korea

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

Keywords: This study proposes and evaluates a novel carbon-neutral hydrogen (H2) production process from natural gas
Electrified steam reforming through electrified steam methane reforming (e-SMR) with renewable electricity. The process model consists of
Hydrogen different unit technologies such as reforming, water–gas shift, hydrogen pressure swing adsorption, and CO2
Techno-economic evaluation
capture, along with heat recovery. Then, we evaluated the techno-economic-environmental performance of the
Process design
proposed e-SMR process by comparing it with the conventional fired-heating steam methane reforming (f-SMR).
Uncertainty analysis
By employing an electrically driven reformer using renewable energy, e-SMR outperforms f-SMR with less
natural gas consumption, higher energy efficiency of 78.7%, and lower net CO2eq emission of 5.28 kg CO2eq/kg
H2 and captured 5.58 kg CO2/kg H2; however, it has a drawback, i.e., higher H2 unit production cost (UPC) of
3.49 $/kg with a capacity of 7.06 ton/day. Sensitivity and uncertainty analyses identified the major cost drivers
of UPC, such as the prices of natural gas, renewable electricity, and interest rates, as well as economic risks and
uncertainties. The economic viability of e-SMR was determined by investigating multiple plant capacities, nat­
ural gas markets, renewable energy prices, and possible future CO2 selling prices. According to the investigation,
currently, the US and India show promise for e-SMR, with abundant and affordable natural gas and renewable
energy resources, both priced at around 3.49 $/kg of H2, respectively. Furthermore, the global 2030’s scenario
with 45 $/MWh of renewable electricity, and capture CO2 credit of 35 $/ton is observed at 3.40 $/kg H2,
compared with that of 2050 at 2.91 $/kg H2. e-SMR is well adaptable to many countries’ energy mix because it is
flexible to utilize hybrid primary energy input, conventional natural gas as feedstock, and conventional/
renewable energy for utilities.

1. Introduction
Energy security and climate change are the most crucial issues for the
sustainability of future society [1]. The world has primarily relied on
conventional energy resources, which primarily contribute to global
warming by increasing greenhouse gas/CO2 emissions [2]. In the face of
rising global energy consumption and the rapid depletion of fossil re­
sources, urgent actions are essential for energy security [3,4]. The world
is exempt from improving the technical efficiency of existing energy
systems to reduce emissions or searching for alternative technological
approaches to cleaner energy manufacturing. Hydrogen (H2) is one of
the most important energy sources, chemicals, and fuels used in in­
dustry, heating, and transportation. Currently, the majority of H2 is
produced by reforming natural gas/shale gas or gasification of coal/
biomass [5], with a small amount produced through water electrolysis
based on renewable energy for eco-friendliness enhancement [6]. As an
example of technology development for cleaner H2 production, a con­
ventional production process combined with CO2 capture and storage
(CCS) can produce H2 at lower emission, known as “blue H2” [7].
Another, “green H2” which is based on renewable energy, is an ideal
option for environmental benefits but has limits in terms of system ef­
ficiency and economic viability.

* Corresponding author.
E-mail address: jiyongkim@skku.edu (J. Kim).
1
Authors contributed equally to the manuscript.
2
The two authors have the same contribution to this study.

https://doi.org/10.1016/j.enconman.2023.116758
Received 25 October 2022; Received in revised form 18 January 2023; Accepted 29 January 2023
Available online 8 February 2023
0196-8904/© 2023 Elsevier Ltd. All rights reserved.
T.N. Do et al.
Fig. 1. Schematic of hydrogen production using (a) fired-heating furnace and (b) electrified furnace.
Despite the numerous advantages of employing an H2-based energy
system, there are still challenges that prevent its advancement, such as
technology, economic impact, and environmental impact. It is currently
challenged to replace conventional fossil fuel-based energy sources due
to their reliability [8]. To realize an H2 economy, a lot of work must be
put into overcoming challenges, conducting research, and developing
safe and affordable H2. Many studies have been conducted in recent
years to solve the problems of H2 production process development, for
example, the thermodynamic study of reforming technologies by Rob­
erto et al. [9]. Keipi et al. examined and compared the economics of
various H2 production processes, including thermal decomposition,
steam methane reforming (SMR), and water electrolysis [10], whereas
Antonini et al. analyzed the techno-economic-environmental perfor­
mance with natural gas or biomethane feedstock [11]. H2 pressure swing
adsorption (H2PSA), which is commercially and widely used for H2 re­
covery or purification from gas mixture, has been attractive with
research on different sorbent types [12], column or process configura­
tions [13–15]. Nowadays, H2 production process is usually integrated
with CO2 capture and storage (CCS) to reduce emissions by capturing
and storing almost CO2 in the purging/vent-out gas. Mota-Martinez et al.
investigated CCS with key indicator performances for absorbent selec­
tion and design [16], while other studies assessed the performance of
various amine-based solvents and process configurations [17,18].
Although equipped with CCS, H2 production via methane reforming
emits a certain amount of CO2 equivalent (CO2eq) primarily due to the
use of conventional heat and electricity in the process, so it does not
deliver significant environmental benefits compared with renewable
energy sources [19,20]. Such CO2eq emission scores depend on techno­
logical production pathways (e.g., steam/autothermal reforming and
gasification), feedstocks (e.g., natural gas, coal, and biomass), and
2
Energy Conversion and Management 279 (2023) 116758
process designs (e.g., with/without heat integration and well-optimized
balance) [21]. According to the Paris Agreement, many countries with
strict policy regulations will not permit new structures or penalize
existing manufacturing processes that exceed the CO2eq emission limit
[22,23]. This has driven governments, independent enterprises, and the
research community into using renewable energy in process synthesis to
lower emission rates.
Recently, Wismann and his colleagues proposed a novel electrically
driven steam reforming process that can use renewable electricity and
reduce CO2 emission for H2 production [24,25]. In an electrified steam
methane reformer (e-furnace or e-SMR), heat is generated through direct
resistive heating or Joule/Ohmic heating. When a current is applied to
and passed through a material, a high-temperature heat flow is created
to heat the environment, which is suggested for endothermic processes.
Here, an e-SMR reactor consists of multiple tubes, and the reforming
catalyst is mounted on the tube’s interior. Since reforming is extremely
endothermic reaction, structure catalysts, such as Ni-based or those
supported by SiC or metallic foam, can enhance thermal conductivity
within the catalytic bed, resulting in higher CH4 conversion and H2
productivity [26–28]. Wismann et al. also investigated e-SMR’s transi­
tion phenomena through computational fluid dynamics modeling and
lab-scale experiments [29]. In which the reformer is made up of
numerous Ni-based catalyst-coated FeCrAl alloy tubes, and two copper
sockets positioned on the external surface of the tubes’ ends for Ohmic
heating when a current is applied. The heating behavior and transient
temperature profile were observed along the reactor: the temperature
rapidly rises at the beginning of the reactor owing to the entire heat
supply for heating gas, then slightly drops and remains stable as a result
of an endothermic reaction in the catalytic coated zone, then rises again
before quickly falling due to heat exchange with the surrounding
T.N. Do et al. Energy Conversion and Management 279 (2023) 116758

Table 1
Major descriptions of sub-processes in H2 production processes.
Process Description Ref.

Pre-reforming Gibbs reactor [42,43]

Operating conditions: 550 ◦ C, ~20 bar
SMR Catalyst of Ni/Mg Al2O4 spinel [37]
Operating conditions: 850 ◦ C–900 ◦ C, ~20 bar
kSMR PCH4 PH2 O − P3H2 PCO /KSMR
eq,1
rSMR
1 = 12.5
PH2 (1 + KCO PCO + KH2 PH2 + KCH4 PCH4 + KH2 O PH2 O /PH2 )2
kSMR PCO PH2 O − PH2 PCO2 /KSMR
eq,2
rSMR
2 = 2
PH2 (1 + KCO PCO + KH2 PH2 + KCH4 PCH4 + KH2 O PH2 O /PH2 )2
kSMR PCH4 P2H2 O − P4H2 PCO /KSMR
eq,3
rSMR
3 = 33.5
PH2 (1 + KCO PCO + KH2 PH2 + KCH4 PCH4 + KH2 O PH2 O /PH2 )2
High-temperature water–gas shift HT-WGS: Plug flow fixed bed reactor contains a catalyst Fe2O3/Cr2O3/CuO. [38]
(HT-WGS) Operating conditions: 250 ◦ C–400 ◦ C, ~20 bar
( )
PCO2 PH2
rHTWGS = kHTWGS P0.9 P 0.31 − 0.156 − 0.05
P
CO H2 O CO2 P H2 1 −
KHTWGS
eq PCO PH2 O
Low-temperature water–gas shift Plug flow fixed bed reactor contains a catalyst Cu/ZnO/Al2O3 [39]
(LT-WGS) Operating conditions: 170 ◦ C–250 ◦ C, ~20 bar
( )
PCO2 PH2
rLTWGS = kLTWGS PCO2 PH2 O −
Keq
LTWGS

CO2 capture and storage (CCS) Absorption column and stripper: 1–1.5 bar [44]
Monoethanolamine (MEA) 30%
CO2 recovery: ~96%
H2 pressure adsorption (H2PSA) Hierarchy model for adsorption columns. [45–47]
Operating conditions: 30 ◦ C–35 ◦ C, 34 bar
H2 recovery: 91.9%

environment. Over a conventional reformer, e-SMR with Ohmic heating
allows for a rapid thermal response within minutes of start-up or shut­
down. Similarly, Ambrosetti et al. investigated a systematic model of e-
SMR using various structure catalysts, such as honeycomb monoliths
and open-cell foams [30]. e-SMR is emphasized as a compact reformer,
significantly smaller than conventional fired-heating furnaces [24], with
higher thermal efficiency and better/flexible control [29,31]. With such
advantages in design, control, and eco-friendliness, e-SMR has received
significant attention. Song et al. investigated the thermal efficiency and
economic and environmental performance of e-SMR for H2 [32]; Mion
et al. adopted e-SMR in methanol synthesis [33], demonstrating the
benefits of incorporating renewable energy [34,35].
Here, e-SMR utilizes conventional natural gas as a feedstock and
renewable energy for utilities to produce environmentally friendly H2.
In another aspect, renewable H2 via water electrolysis also performs
good environmental metrics that are entirely derived from renewable
energy resources. Nonetheless, even clean H2 has disadvantages, such as
being more expensive than conventional H2. Such competitions in terms
of practical implementation, economic feasibility, and environmental
impact should be investigated to make decisions toward a sustainable H2
economy. In this study, we proposed and evaluated an H2 production
process using an e-SMR and compared it with the convention fired-
heating steam methane reforming (f-SMR) and renewable H2 produced
via water electrolysis as reference cases. Here, e-SMR was distinguished
from others by a hybrid primary energy input of conventional (i.e.,
conventional natural gas feedstock) and renewable (i.e., utilities) energy
resources. The process synthesis and development considered well-
balanced heat recovery of matching hot and cold streams, targeting
energy saving in both processes. The techno-economic and environ­
mental performance of the proposed process was evaluated and
compared with that of conventional H2 in terms of energy efficiency
(EEF), unit production cost (UPC), and net CO2eq emission (NCE). This
work also included sensitivity analysis to identify bottleneck drivers for
lowering costs and emissions, as well as uncertainty analysis on those
key factors using Monte Carlo (MC) simulation. Finally, the techno-
economic-environmental perspective of the e-SMR was examined in
specific national contexts, such as the natural gas market and renewable
energy resources, as well as future scenarios.
2. Technology overview and analysis method
2.1. Technology overview
The process scheme of conventional fired-heating steam reforming
for H2 production from natural gas, including reforming, water–gas shift
(WGS), H2 purification, and CCS, is illustrated in Fig. 1(a). The natural
gas is first mixed with steam, preheated, and pre-reformed at a relatively
low-temperature of 400 ◦ C–550 ◦ C, where the higher hydrocarbon (C2+
hydrocarbon) is cracked into CH4, syngas, and possibly CO2 [36]. The
syngas is generated through steam reforming reactions of C2–C7 range
hydrocarbons [Eq. (1)], whereas CH4 and CO2 are created via a
methanation reaction [reverse Eq. (2)] and WGS reaction [Eq. (3)].
Then, the gas mixture is introduced into the tube side of a fired heater
that contains a catalyst. This heater provides high heat flux through the
tube wall for the highly endothermic reforming reactions at
850 ◦ C–900 ◦ C, which is supplied by gas combustion in the fired heater.
The SMR reaction consists of two steps: the production of CO and H2
through steam reforming of CH4, as expressed in Eq. (2), and the pro­
duction of CO2 and H2 through the WGS reaction, as expressed in Eq. (3).
In addition, the global SMR reaction, expressed in Eq. (4), is a sum of
CH4 steam reforming and the WGS reaction. In this work, the catalyst
Ni/Mg Al2O4 spinel was employed for SMR, and its kinetic models were
applied [37].
( m) /
Cn Hm + nH 2 O→nCO + n + H2 , ΔH298K = 498 kJ mol for n = 3 (1)
2
CH 4 + H2 O ↔ CO + 3H2 , ΔH298K = 206 kJ/mol (2)
CO + H2 O→CO2 + H2 , ΔH298K = − 41 kJ/mol (3)
CH 4 + 2H2 O ↔ CO2 + 4H2 , ΔH298K = 165 kJ/mol (4)
Furthermore, the WGS sub-process is operated to maximize H2 pro­
duction via the shift reaction Eq. (3) from generated CO and additional
steam, which includes two reactors of high-temperature WGS (HT-WGS)
using a Fe2O3/Cr2O3/CuO catalyst [38] and low-temperature WGS (LT-
WGS) using a Cu/ZnO/Al2O3 catalyst [39]. To separate hydrogen from
the gas mixture, the well-known pressure swing adsorption (PSA)
technology is used. Because the high-pressure flow is introduced in

3
T.N. Do et al. Energy Conversion and Management 279 (2023) 116758

adsorber columns, a porous sorbent captures and retains H2, while other Table 2
gas species exit the columns as PSA tail gas. Once the sorbent reaches its Plant assumption and major economic/environmental parameters.
maximum adsorption capacity, the columns are operated at lower Plant assumption Value
pressures to release high-purity H2. The PSA tail gas, which contains
Location North America
high-caloric CH4, CO, and H2, is transported to the furnace for com­ Year of analysis 2022
bustion, along with additional fuel gas to generate heat. The flue gas Plant lifetime 20 years
produced after burning contains a significant amount of CO2, which Interest rate 6%
must be caught to protect the environment; here, a monoethanolamine Depreciation Straight line
Operability 8000 h/year
(MEA) sorbent is used. The CCS sub-process includes two columns: an Maintenance cost 3% of annualized capital cost
absorber for contacting CO2 and the MEA solvent, and a stripper for Operating charges 15% of operating labor cost
regenerating the MEA solvent and releasing high-purity CO2. Although Plant overhead 25% of labor and maintenance
CCS is used (captures approximately 96% of generated CO2), the f-SMR cost
General and Administrative 6% of annual operating cost
requires additional fuel gas for combustion, resulting in some emissions.
(G&A)
As illustrated in Fig. 1(b), the proposed H2 production process via e- Material and utility assumption Unit price CO2eq factor
SMR primarily differs from the main reformer, which utilizes electricity Natural gas/Fuel gas 171.4 $/ton [50] 2.51 kg/kg*
for direct resistance heating [24]. The electrically driven reformer in­ [51]
cludes various FeCrAl alloy tubes with a coated catalyst in its interior. Process water 1 $/ton [52] –
Sorbent CoMo HDS** 11.35 $/kg [53]
Because an alternating current is applied to the copper sockets at the
–
Sorbent ZnO HDS 4.0 $/kg [53,54] –
opposite ends of the external tube surface, electrical resistance or ohmic Sorbent H2PSA 6.11 $/kg [55] –
heating is produced. Therefore, the steam reforming reaction is fully Solvent MEA 0.97 $/kg [56] –
driven by electricity, possibly from renewable/low-carbon energy, for Cooling water 0.03 $/ton [52] –
Low-pressure steam 10.5 $/ton [52] 0.19 kg/kWh
clean H2 production with fast [29], compact [24], and high-energy
[52]
efficient e-SMR [31]. This is followed by the following sub-processes Conventional electricity 0.06 $/kWh [57,58] 0.44 kg/kWh
WGS for H2 production rate enhancement, H2PSA for separation and [59]
purification, and CCS for CO2 capture from the PSA tail gas. After CCS, Renewable electricity*** 0.055 $/kWh [52] –
the remaining mixture of unreacted CH4, generated CO, and H2 are Renewable heat*** 0.05 $/kWh [41,52] –
By-product CO2 35 $/ton [41]
recycled to the electrified reformer instead of burning as in f-SMR.
–

* Estimated emission at 52.91 kg/mmBTU [51].

2.2. Analysis method
2.2.1. Process simulation
The proposed H2 production processes from natural gas were
modeled and simulated using Aspen Plus V11 [40]. The major de­
scriptions of the operating conditions or reaction kinetics for the sub-
processes, including SMR and WGS reactions, H2PSA, and CCS, are
presented in Table 1. The SMR kinetic expressions are also included, and
its thermal EEF is assumed at 90% (i.e., electricity-to-heat) for the
electrified reformer [33]. Heat recovery is considered for both processes.
In f-SMR, the waste heat from flue gas and hot raw syngas from the
reformer are used to pre-heat a fed natural gas and generate process
steams. Similarly, the high-temperature outlet of the electrified reformer
is used as a hot stream for feed pre-heating and steam generation.
However, its quantity and quality are insufficient for the whole process,
requiring additional heating sources. Here, solar-based thermal heating
is assumed to be used in the e-SMR process [41]. Hence, the two pro­
posed processes differ in terms of heat exchanger network as well as
utility sources, i.e., conventional energy for f-SMR and renewable en­
ergy for e-SMR.
2.2.2. Techno-economic and environmental analysis
In this work, the proposed hydrogen production processes were
evaluated with technical (i.e., EEF), economic (i.e., UPC), and envi­
ronmental (i.e., NCE) indicators, which are widely used in chemical
process evaluation. The EEF represents how effectively the proposed
process, as calculated in Eq. (5), can store or capture energy in produced
H2. It is a faction of the heat of the product over the total input energy,
including the heat of feed and required process utilities [48].
Pi × HHV i
EEF(%) = ∑ ∑ × 100% (5)
(Fi × HHV i ) + Uj
where Pi and Fi represent the mass flow of produced H2 and input
natural gas, respectively. HHVi denotes the higher heating value of H2/
input natural gas. Uj represents the energy flow of utility used for process
operation.
The environmental performance is evaluated using NCE, which is the
total CO2 equivalent emission (CO2eq) per unit of produced H2, as shown
** HDS: hydrodesulfurization, considered in economic estimation [60].
*** Solar-based by a parabolic dish or Stirling engine, and a parabolic trough
[41].
in Eq. (6). It includes direct CO2eq (DCE), which is obtained from the
process vent-out streams, and indirect CO2eq, which is estimated from
the consumed utilities and its CO2eq factor (provided in Table 2).
∑
di +
∑( ) ∑
Uj × cf j + (Fi × cf i )
NCE = (6)
F H2
where di represents CO2eq emission from the process vent-out stream. cfj
and cfi are the CO2eq factors of each utility type j and feedstock i used in
the process. FH2 denotes the amount of produced H2.
For the economic evaluation, UPC is used as a key indicator, which is
the cost to produce a unit of hydrogen, including capital and operating
expenses. The plant assumptions and process economic parameters for
economic evaluation are summarized in Table 2. For annualized capital
investment cost (ACI), the total capital investment cost (TCI) is first
estimated, including variable operating cost (VOC) and fixed operating
cost (FOC). The mass and energy flows were obtained from process while
equipment sizing and costing from Aspen Plus Economic Analyzers, that
further estimated for TCI using the Lang factor. For unit process with
hierarchy model (i.e., electrified reformer, PSA), the equipment cost/
capital cost was estimated with order of magnitude according to Eq. (7)
[49]. In which, the capital cost C2 of plant with capacity S2 is estimated
from the based capital cost C1 of the plant with capacity S1. The power n
is between 0.6 and 0.7 for many facilities, here n = 0.67 is assumed.
Then, ACI is calculated considering the interest rate (i) and the process
lifetime (r) as in Eq. (8). VOC is the sum of the costs for raw materials
and required utilities within the process, as expressed in Eq. (9).
Meanwhile, FOC includes labor, maintenance, plant overhead cost, etc.,
as assumed in Table 2. Finally, the UPC of H2 is calculated by dividing
the total production cost by the total amount of produced H2, as
expressed in Eq. (10). Here, the UPC of H2 is presented in terms of USD
per kilogram of H2 ($/kg of H2).

4
T.N. Do et al. Energy Conversion and Management 279 (2023) 116758

Fig. 2. Process flow diagram and major stream information of fired-heating steam reforming (f-SMR).

( )n
S2
C2 = C1 (7) ACI + VOC + FOC
S1 UPC = (10)
F H2
i × (1 + i)r Furthermore, net present value (NPV) has been calculated, as
ACI = TCI × (8)
(1 + i)r − 1 formulated in Eq. (11). In which, the net future cash flows during the
∑ ∑( plant lifetime (20 years) are converted into NPV and a time of profits
)
VOC = (Fi × ci ) + Uj × cj (9) could be determined with a certain selling price of H2 product.

Fig. 3. Process flow diagram and major stream information of electrified steam reforming (e-SMR).

5
T.N. Do et al. Energy Conversion and Management 279 (2023) 116758

Fig. 4. Heat recovery, energy requirement, and overall EEF of the proposed processes.

∑20
Revenue − (VOC + FOC) reactor outlet or flue gas. As shown in Fig. 2, natural gas feedstock
NPV = − TCI (11) (stream 1) is first compressed, heated, and fed to a pre-reformer, along
(1 + i)r
with steam, to crack the higher hydrocarbon component, mostly C2–C7
r=1

hydrocarbon, before being delivered to a fired-heating reformer. The fed

2.2.3. Sensitivity and uncertainty analysis
steam volume is adjusted for a steam/carbon ratio of 3.0 (stream 6) at
We also examined the effect of major economic parameters on H2
20 bar and 900 ◦ C, resulting in 91% of methane conversion in a
UPC through sensitivity and uncertainty analysis. The sensitivity anal­
reformer. The process stream 7 is then chilled and sent to the WGS sub-
ysis was conducted with a ± 20% change of examined parameter from
process, where the H2 production rate increases by 34% (i.e., 134 kmol/
the basis value, which determines the essential aspects for future pro­
h versus 100 kmol/h of H2), owing to the shift reaction of CO and
posal/scenario of the process’s economic improvement. Although
additional steam. The gas mixture (stream 13), which contains produced
sensitivity analysis indicates how much H2 UPC changed as a result of a
H2, generated CO2, and unreacted CH4, is treated by the H2PSA sub-
single variation, the limited parameter uncertainties prohibit the
process for high-purity H2 product (stream 18). The PSA tail gas
robustness of the economic estimation. Employing MC simulation could
(stream 14) is combined with more fuel gas and oxygen before being
overcome such a limitation by obtaining a statistical solution to the
delivered to a fired heater to generate heat for the extremely exothermic
parameter uncertainties. For uncertainty analysis, MC simulation was
reforming reaction. The combusted flue gas is used as a hot stream in
used to analyze the economic risk and uncertainty as an overall effect of
heat exchangers for pre-heating of natural gas and steam generation,
many variations, including interest rate, natural gas price, and renew­
and then, the CO2 in the exhausted gas (stream 16) is captured using the
able electricity (the most influenced factors identified in sensitivity
MEA sorbent before being released into the environment.
analysis). In particular, the interest rate at a basis value of 6% with a
As illustrated in Fig. 3, in e-SMR, natural gas (stream 1), steam
standard deviation of 0.8%, whereas both natural gas and renewable
(stream 2), and the recycled stream (stream 12) are heated up and fed
electricity fluctuated at ±10%, ±25%, and ± 50%. Therefore, H2 UPC
into the electrified reformer, which contains multiple tubes with a
probability was predicted, where the economic evaluation was repeated
coated catalyst inside. In the reactor, electricity is supplied at the
with the intervention of random variables.
external tubes’ surface, and direct resistance heating is generated, sup­
plying heat for reforming reactions [24]. Similarly, H2 is further
3. Results and discussion
generated in WGS, which increases the production rate by 32% (i.e., 159
kmol/h in stream 9 versus 120 kmol/h in stream 6). Finally, 146 kmol/h
3.1. Process simulation
of high-purity H2 (stream 14) is adsorbed through the PSA sub-process,
leaving the mixture gas of generated CO2, unreacted CH4, and remaining
The proposed processes were modeled and simulated using Aspen
H2 (stream 11). Unlike f-SMR, which burns PSA tail gas, e-SMR recycles
Plus V11, where the process flow diagrams (PFD) and major streams
it to the reformer after capturing CO2 (37 kmol/h in stream 13). Because
were obtained and summarized in Figs. 2 and 3, and major equipment
CCS favors lower-pressure operations, an additional compressor is
descriptions on Table S1–S2 in SI. The same flow rate of natural gas
required to compress the recycle stream (stream 12) from CCS to 20 bar.
feedstock was introduced in both processes; meanwhile, additional
There are some distinct points from the two process configurations to
natural gas was required for fired-heating in f-SMR, and electricity was
note:
required for resistive heating in the e-SMR reactor. In addition, heat
integration was considered for heat recovery from the high-temperature

6
T.N. Do et al.
Fig. 5. (a) NCE and captured CO2 and (b) breakdown of hydrogen UPC.
• e-SMR requires less natural gas but has a higher H2 production rate
than f-SMR. This is because the recycle stream entirely creates and
acquires H2, whereas f-SMR burns a small amount of produced H2 in
PSA tail gas.
• e-SMR may necessitate larger equipment and the installation of an
additional compressor for the recycle stream.
• f-SMR is advised for a larger CCS sub-process due to the high rate of
exhausted gas from burning PSA tail gas and additional fuel gas.
3.2. Techno-economic and environmental analysis
From the process simulation, the energy flow, including hot/cold
streams in heat exchanger network and utility consumption for each
sub-process, is obtained and summarized in Fig. 4, represented for a unit
of produced H2. Figs. S1 and S2 in SI demonstrate the actual heat load
and energy requirements of the two processes before and after heat re­
covery. Heat recovery activates savings of 40%–51% on heating and
45%–56% on cooling, resulting in process EEF of 65.6% for f-SMR and
78.8% for e-SMR. Here, e-SMR takes advantage of the effective thermal
transfer inside the electrified heating reactor [31], which contributes to
a greater total EEF than f-SMR. The electrically driven reformer uses
direct resistive (ohmic) heating, resulting in high electricity consump­
tion for e-SMR (10.7 kWh/kg of H2); meanwhile, f-SMR requires addi­
tional fuel gas for heat generation. Hence, e-SMR used less natural gas
feedstock, with 2.01 kg/h natural gas consumed for a unit of H2 gen­
eration. Because f-SMR uses more fed natural gas (2.39) and additional
fuel gas (0.94) for combustion, it generates more CO2, necessitating a
larger CCS installation and higher utility use to capture a high rate of
Fig. 6. Net present value (NPV) as H2 selling price at (a) 3.0 $/kg and (b) 3.5 $/kg.
7
Energy Conversion and Management 279 (2023) 116758
CO2. That is another disadvantage of f-SMR compared with e-SMR in
terms of EEF and further expense costs for CCS.
Fig. 5(a) depicts the NCE and the captured CO2 metrics for a unit of
H2 produced. DCE was obtained from the vent-out gas discharged into
the environment, whereas ICE/feed inventory was computed using the
conventional utility/feedstock consumptions and its unit CO2eq factor.
The proposed e-SMR process resulted in a lower NCE than f-SMR,
achieving this primarily through low/zero ICE using renewable utilities.
Since natural gas feedstock CO2 inventory (from extraction and pro­
cessing in the upstream stages) was considered, it became the main
contributor, accounting for around 49% in f-SMR and up to 96% in e-
SMR. The majority of f-SMR’s indirect emission is accounted for by fuel
gas and conventional heating utilities, with a lower direct emission rate
(See Table S3 in SI). Due to its large-generated CO2, f-SMR can capture
8.86 kgCO2eq/kg produced H2 (at 96% CO2 recovery) with a CCS
operation more than e-SMR. If conventional electricity was used, e-SMR
would produce more indirect emission (a diagonally striped box),
further higher NCE. Otherwise, the hybrid primary energy-based e-SMR,
which employs conventional natural gas feedstock and renewable
electricity/heat, can provide eco-friendly benefits of low NCE at 5.28
kgCO2eq/kg H2 and 5.58 kg captured CO2/kg H2. This suggests that e-
SMR with renewable energy utilization and CO2 captured benefit can
reduce emission to as low as the green H2 performance (via water
electrolysis driven by renewable electricity).
Fig. 5(b) shows H2 UPC and its breakdown into annualized capital
and operating cost contributions of feedstock, utilities, and fixed oper­
ating costs. The annualized capital cost of e-SMR is higher than that of f-
SMR, owing to the higher e-SMR capital cost. The e-SMR budget for the
T.N. Do et al. Energy Conversion and Management 279 (2023) 116758

Fig. 7. Sensitivity analysis on economic parameters.

Fig. 8. Frequency of H2 UPC for f-SMR (a) and e-SMR (b), and cumulative probability for f-SMR (c) and e-SMR (d). (See Figs. S4 and S5 in SI for the distribution of
random variation).

SMR sub-process, including larger equipment with additional com­
pressors for pressing up recycle stream, is significantly higher than the f-
SMR budget despite the larger CCS sub-process of f-SMR (See Fig. S3 in
SI). Moreover, e-SMR spends 2.2-times higher on utilities, with renew­
able electricity accounting for 50% of utility cost, whereas f-SMR utility
cost is smaller and primarily for heating (i.e., 29% for fired heat and 32%
for steam). Consequently, e-SMR produced H2 at a higher cost of 3.49
$/kg than f-SMR of 2.76 $/kg.
Similarly, f-SMR is more cost-effective than e-SMR, with a higher
NPV and a shorter payback time, at which project begins to get profit.
Fig. 6 presents NPV and net cashflow with the H2 selling price of 3.0 and
3.5 $/kg, respectively. It is evident that e-SMR is difficult to achieve
profit if H2 is sold at 3.0 $/kg. Other, e-SMR can turn a profit if H2 is sold
for a higher price, such as 3.5 $/kg, but with a longer payback period
(year 15th). The economic feasibility of e-SMR is a trade-off for envi­
ronmental performance, necessitating the identification of economic

8
T.N. Do et al.
Fig. 9. Hydrogen UPC as a function of (a) plant capacity and natural gas price for f-SMR and (b) e-SMR, (c) interest rate and natural gas price for f-SMR and (d) e-
SMR, (e) renewable electricity and natural gas price for e-SMR, and (f) future renewable electricity and captured CO2 selling price for e-SMR.
sensitivity, uncertainty, and application in specific scenarios.
3.3. Sensitivity and uncertainty analysis
A sensitivity study was conducted to identify the primary parameters
influencing H2 UPC, where a single economic parameter fluctuates
within a 20% range, while the others remain constant, as illustrated in
Fig. 7. Interest rate is the most sensitive factor on UPC, effecting a
change of up to 6.8 in f-SMR and 5.5% in e-SMR. Natural gas price is the
second largest influential factor in f-SMR at ±4.2%, whereas renewable
electricity price is the second influential factor in e-SMR at ±3.9%,
which correlates to their high budget in H2 UPC. Natural gas market
fluctuations have a greater impact on f-SMR’s economics than on e-SMR
economics, 4.2% versus 2.0%. In e-SMR, renewable energy resource for
cheaper electricity/heat price is more important for cheaper H2 product,
which depends on technological efficiency, weather, solar radiation, and
9
Energy Conversion and Management 279 (2023) 116758
locations.
Accordingly, uncertainty analysis based on MC simulation examines
the overall effect of these major influential factors. During MC simula­
tion, the random parameters are iteratively generated within the
boundary conditions through 10,000 attempts; 6% average with 0.8%p
standard deviation for the interest rate; the range of ±10%, ±25%, and
± 50% for the natural gas and renewable electricity price. From the
random variables (Figs. S4 and S5 in SI), the frequency and probability
of H2 UPC were identified, as shown in Fig. 8. f-SMR is economically
competitive to by-product H2 [gray box in Figs. 8(a) and (b)] [61]
whereas e-SMR remains prohibitively expensive. For f-SMR, H2 UPC
ranges of 2.41–3.14, 2.37–3.25, and 2.22–3.43 $/kg were observed for
cases ±10%, ±25%, and ± 50%, respectively, with an average of 2.76
$/kg. Otherwise, H2 UPC via e-SMR was determined in the range of
3.11–3.91 $/kg for ±10%, 2.88–3.99 $/kg for 25%, and a larger range
of 2.77–4.18 $/kg for 50%, with an average of 3.49 $/kg. H2 UPC
T.N. Do et al.
Fig. 10. (a) EEF for major steps from primary energy to hydrogen, and (b) trade-off between economic and environmental performance of hydrogen with/
without CCS.
fluctuation increases as parameter uncertainty increases. Uncertainty
analysis identified the feasibility of the processes with the cost fluctua­
tion on major parameters, where clean H2 via e-SMR is still far more
expensive than conventional H2 due to the extremely high renewable
electricity price. Therefore, for e-SMR to be commercially viable, further
research into the circumstances of particular countries or future per­
spectives on clean processes is necessary.
3.4. Extended economic analysis and scenarios
In this part, the economic performance of the H2 production pro­
cesses is further analyzed with specific plant assumptions (i.e., process
capacity and interest rate), the natural gas market in a particular
country, renewable energy resources, and the future selling price of CO2
as a by-product credit. In the proposed processes, the annualized capital
cost accounts for a high rate of 41%–48% of UPC, which may be reduced
by increasing process capacities and further lowering H2 UPC. To
determine the capital cost, the plant capacity and interest rate, along
with the ranges of natural gas price, one of the key influential factors,
were investigated, as shown in Figs. 9(a)–(d). The processes are sup­
portive economics with higher capacities and lower interest rates;
otherwise, they are prohibitive economics, corresponding to the natural
gas price, which is distinguished by the curves/lines and base case as star
marks. Taking Fig. 9(b) as an example, H2 can be produced at a lower
UPC with larger e-SMR (higher 7.06 ton/day) in a certain natural gas
market (171.4 $/ton), whereas other locations with higher natural gas
price must increase e-SMR capacity to maintain H2 UPC in the base
curve (the same price of base case, 3.49 $/kg) or shift H2 UPC in the
supportive economic zone (lower 3.49 $/kg). Such e-SMR decision-
making depends on the plant locations, along with the specific natural
gas market and the stakeholder financial strategies.
In Fig. 9(e), both renewable electricity prices and natural gas mar­
kets, as well as those of particular countries, are assessed for e-SMR. The
economic viability of e-SMR can be activated in countries with either
cheap/abundant natural gas or abundant renewable resources, such as
the US at 3.49 $/kg and India at 3.48 $/kg of H2. On the other hand,
although less expensive than renewable H2 produced through electrol­
ysis, clean H2 produced by electrified steam reforming is still signifi­
cantly more expensive in Japan and Korea, where e-SMR can count on
effective government support. Table S5 in SI provides details on each
country’s renewable electricity and natural gas prices. Although H2
produced by e-SMR is as clean as green H2 produced by renewable
sources, economic viability cannot be guaranteed for all national
10
Energy Conversion and Management 279 (2023) 116758
scenarios. As the credit from selling by-products also affects H2 UPC, the
future CO2 selling price is considered at 35 $/ton in 2030, 61.5 $/ton in
2040, and 88 $/ton in 2050 [62]. Fig. 9(f) depicts H2 UPC via e-SMR in
future scenarios of CO2 selling prices and renewable electricity prices
[52]. Lower renewable energy costs due to efficiency improvement/
technology development [63] and higher CO2 selling price can reduce
H2 UPC to 3.40, 3.16, and 2.91 $/kg in 2030, 2040, and 2050, respec­
tively. Note that additional compression cost of CO2 to 45 bar for cyl­
inder/storage tank transportation was considered.
Fig. 10(a) compares the overall EEF of three H2 production processes:
H2 produced from natural gas via f-SMR, from hybrid natural gas and
renewable energy via e-SMR, and from renewable energy via electrol­
ysis. Here, conventional electricity and heat are generated via natural
gas combined heat-power with 80% efficiency [64]; meanwhile,
renewable electricity and heat from solar/wind are assumed to be 100%
efficient [65]. Because each is assumed to start from a unit of primary
energy, the hybrid energy-based e-SMR produces more H2, followed by
water electrolysis. This again evidences the good performance of e-SMR
in terms of EEF and, in particular, suggests a potential sustainability
pathway for the renewable energy transition. Fig. 10(b) shows the trade-
off between cost and environmental performance (considering NCE and
CO2 capture benefit) of H2 via e-SMR with/without CCS, compared with
f-SMR and green H2 performance. e-SMR uses renewable electricity,
demonstrating its better environmental performance than f-SMR’s and
that it is particularly competitive to green H2 with total benefits of both
NCE and captured CO2.
While e-SMR appears promising, there are still several challenges to
industrial electrification, including limited infrastructure for electricity
supply [66], limited availability of electric equipment and constraints to
redesign processes, or industrial risk aversion [67]. Moreover, the pol­
icies and regulations on fuel switching with guidelines on recommended
fuels or lack of guidance are also other constraints. For example, ac­
cording to American Council for an Energy-Efficient Economic, fuel
switching might be prohibited in several states in the USA (i.e., Kansas,
Louisiana, Minnesota, Oklahoma, and West Virginia) by the state pol­
icies/rules [68].
4. Conclusion
This study proposed and evaluated an H2 production process using a
novel electrified steam methane reformer from a techno-economic-
environmental perspective, utilizing both conventional natural gas as
a feedstock and renewable energy as process utilities. The process
T.N. Do et al.
configuration was developed with a well-designed heat exchanger
network to use waste heat and save energy. Compared with the con­
ventional f-SMR, e-SMR requires a lower natural gas flow rate of 2.01 kg
to produce a unit of H2 and can capture 5.58 kg of CO2. The proposed e-
SMR demonstrated good EEF of 78.7% and low CO2eq emissions of 5.28
kg CO2eq/kg H2, owing to the use of a highly efficient electrified
reformer and low-carbon/renewable energy, respectively. However,
currently, clean H2 via e-SMR is more expensive (i.e., 3.49 $/kg) than
the conventional one and is mostly affected by natural gas, renewable
energy prices, and interest rates, as identified in the single-point sensi­
tivity analysis. Furthermore, the economic risk and uncertainty of e-SMR
were assessed with a predetermined boundary of those variations using
MC simulation. The economic viability of e-SMR was finally examined in
various plant capacities, different locations with varying natural gas
markets and renewable energy resources, and future scenarios of selling
captured CO2. At present, e-SMR is promising in the US and India with
supportive economics or in a larger CO2 credit and lower renewable
energy price in the future (i.e., 2030 at 3.40 $/kg and 2050 at 2.91 $/kg
of H2), which is also economically competitive to renewable H2.
Implementing e-SMR is adaptable for utilizing conventional or renew­
able electricity for clean H2 from natural gas (hybrid primary energy-
based), depending on a country’s energy mix toward a renewable en­
ergy society.
CRediT authorship contribution statement
Thai Ngan Do: Conceptualization, Software, Formal analysis,
Writing – original draft, Visualization. Hweeung Kwon: Methodology,
Visualization, Investigation, Writing – original draft. Minseong Park:
Investigation, Visualization, Validation. Changsu Kim: Investigation,
Visualization, Validation. Yong Tae Kim: Project administration, Vali­
dation, Funding acquisition, Writing – review & editing. Jiyong Kim:
Conceptualization, Resources, Supervision, Funding acquisition,
Writing – review & editing.
Declaration of Competing Interest
None.
Acknowledgments
This research was supported by the C1 Gas Refinery Program
through the National Research Foundation of Korea (NRF), funded by
the Ministry of Science, ICT & Future Planning (NRF-
2017M3D3A1A01037001) and supported by the Korea Institute of En­
ergy Technology Evaluation and Planning (KETEP) and the Ministry of
Trade, Industry & Energy (MOTIE) of the Republic of Korea (No.
20224C10300040).
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.enconman.2023.116758.
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