Energy Conversion and Management 276 (2023) 116549

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Energy Conversion and Management

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

Energetic, GHG, and economic analyses of electrified steam methane

reforming using conventional reformer tubes
Dino Mehanovic a ,∗, Alexandre Al-Haiek b , Philippe Leclerc b , David Rancourt a , Luc Fréchette a ,
Mathieu Picard a
a
Department of Mechanical Engineering, Universite de Sherbrooke, 2500 Boul. de l’Universite, Sherbrooke, J1K 2R1, QC, Canada
b LAh Services G.P., Montreal, QC, Canada

ARTICLE INFO ABSTRACT

Keywords: A concept for electrified Steam Methane Reforming (eSMR) based on reformer tubes is proposed as a pathway
Hydrogen for hydrogen decarbonization. The proposed concept applies radiant heating elements to a conventional
Steam methane reforming gas-fired reformer. A thermochemical model and a techno-economic framework are developed to evaluate
Decarbonization
process performance at various conditions and the economic potential of the proposed concept. A baseline
Electric
scenario with feedstock and electricity priced respectively at $4/MMBtu and $0.04/kWh, and assuming 2%
Techno-economic
of fugitive methane emissions and 50 gCO2 eq/kWh, results in an LCOH of $1.53/kgH2 and a decarbonization
cost of $38/tonCO2 . The techno-economic results demonstrate that the proposed eSMR process leads to lower
LCOH than mainstream alternatives over a wide range of energy prices. The study shows that reformer
tube electrification is both economically viable and technically feasible, and therefore has the potential to
decarbonize hydrogen production at a low cost.

1. Introduction The overall reaction (Eq. (3)) is endothermic. It requires an energy

The global hydrogen market exceeds $135G in annual sales (90
GtonsH2 ), serving essential economic sectors such as fertilizer pro-
duction, methanol synthesis, steel production, and oil refining [1].
Emerging sectors such as domestic heating and transportation are also
targeting hydrogen as a clean energy carrier [2–4]. Some of the well-
established sectors are likely to see a decline in demand with the energy
transition (e.g., refining), but industrial hydrogen needs will generally
remain significant and are most likely to grow [5]. Currently, more than
95% of hydrogen production is based on fossil fuels [6].
Steam Methane Reforming (SMR) has the largest market share
among fossil fuel-based production pathways. SMR is an endothermic
process stripping hydrogen from methane and water molecules by oxi-
dizing the carbon atom in methane (Eq. (1)). The reaction is normally
followed by the exothermic water–gas-shift (WGS) reaction (Eq. (2)),
which produces an additional H2 molecule by further oxidizing the
carbon atom found in the initial methane molecule.
CH4 + H2 O ←↽
←←←←←⇀
←←←←←← CO + 3H2 𝛥Hr ◦ = 206 kJ∕mol
CO + H2 O ←↽
←←←←←⇀
←←←←←← CO2 + H2 𝛥Hr ◦ = −41 kJ∕mol
CH4 + 2H2 O ←←↽
←←←←⇀
←←←←←← CO2 + 4H2 𝛥Hr ◦ = 165 kJ∕mol
input of 247 kJ/molCH4 , which accounts for the overall heat of reaction
and the heat of vaporization of water. This energy is usually provided
by burning up to 45% of the methane feedstock [7]. The resulting
combustion-CO2 and reaction-CO2 add up to approximately 10.5 kgCO2
emitted per kgH2 produced [8].
While technologies such as electrolysis and photocatalytic water
splitting entirely avoid fossil fuels in hydrogen production, fossil fuel-
based processes remain ubiquitous due to their more favourable eco-
nomics — grid-powered water electrolysis has a cost of decarbonization
of approximately $200/tonCO2 in the best cases [9]. Cleaner alterna-
tives are mostly made viable in small-scale applications like power
plant cooling, or electronics manufacturing, where high-purity hydro-
gen is essential [2,10,11]. However, a recent push in decarbonization
policies for the adoption of electrolysis points towards significant cost
improvements by 2030 and onward [1].
The use of renewable natural gas (RNG) is seen as a means to fast-
(1) track the decarbonization of SMR. This approach leverages existing
infrastructure for both feedstock distribution and feedstock conversion
(2) to hydrogen. The worldwide potential of RNG is estimated at around
12,000 TWh, enough to produce four times the amount of current
(3) hydrogen consumption [12]. Such large-scale adoption of RNG for SMR

∗ Corresponding author.
E-mail address: dino.mehanovic@usherbrooke.ca (D. Mehanovic).

https://doi.org/10.1016/j.enconman.2022.116549
Received 16 August 2022; Received in revised form 30 November 2022; Accepted 1 December 2022
Available online 13 December 2022
0196-8904/© 2022 Elsevier Ltd. All rights reserved.
D. Mehanovic et al. Energy Conversion and Management 276 (2023) 116549

due to its potential for higher CO2 capture rates than existing SMR
Abbrevations
plants, which may only allow pre-combustion CCS [25].
ATR Autothermal Reforming A sizable reduction in the carbon footprint of SMR is also achiev-
ASU Air Separation Unit able by substituting natural gas combustion with a renewable energy
CAPEX Capital Expenditures source, which can even be combined with CCS for near-zero direct CO2
CCoA CO2 Cost of abatement emissions. The renewable energy source replacing combustion can be
CCGT Combined Cycle Gas Turbine either direct solar heating, electrical heating connected to the grid, or
a combination of both sources of energy (solar and electrical) [26–30].
CCS CO2 Capture & Sequestration
The low capacity factor and high capital investments of sun-heated SMR
eSMR Electric Steam Methane Reforming
systems is however an obstacle towards its commercialization [9,31].
HTS High Temperature Shift
Previous work on electric SMR (eSMR) is also limited, with only a
LCOH Levelized Cost of Hydrogen
few recent attempts towards electrification of the process. While Joule
LHV Lower Heating Value (resistive) heating is the most common pathway for heat generation,
LMP Larson–Miller Parameter recent implementations of eSMR rely on various combinations of re-
LTS Low Temperature Shift actor and catalyst designs: (1) electric heaters used as the substrate
O&M Operation and Maintenance for a washcoat catalyst [32], (2) small-scale tubes washcoated with
OPEX Operational Expenditures catalyst and using Joule heating with electrodes fixed directly on
PFD Process Flow Diagram the structure of the reactor [29], (3) contact-less radiative heating
POX Partial Oxidation of micro-reactors [33], (4) microwave-heated catalyst bed [34], and
PSA Pressure Swing Adsorption (5) induction heating of the catalytic zone in a hybrid solar-electric
RNG Renewable Natural Gas tube reactor [30]. Long-term operation of electric SMR has not yet
SMR Steam Methane Reforming been demonstrated in any of these implementations, and recent techno-
TWT Tuba Wall Temperature economic analyses predict higher LCOH than gas-fired SMR even in
relatively favourable economic scenarios [9,35]. Although these new
WGS Water–gas-shift
technologies could have potential for optimization of the process in
the future, there is a need to investigate low-risk eSMR solutions that
combine industrially available technologies that could be adopted in
will however remain inhibited by the high cost of RNG, with prospec- the short term to cut emissions.
tive RNG projects in the US estimated to range between $7/MMBtu This paper presents a preliminary design for conventional reformer
and $20/MMBtu the best cases — the majority of projects lead to costs electrification, which builds on well-established reactor and catalyst
above $20/MMBtu, or more than five times current US prices of natural experience to provide a hydrogen decarbonization pathway with low
gas [13,14]. capital and operational expenditures (CAPEX and OPEX). The objective
CO2 capture & sequestration (CCS) has alternatively been consid- of the proposed electrified SMR implementation is also to offer a so-
ered as a realistic solution for the reduction of the carbon footprint lution that re-purposes existing infrastructure through retro-fitting, re-
of fossil fuel-based processes, and specifically SMR [15–19]. While ducing capital investments in new long-lasting equipment that relies on
CCS ensures relatively low H2 production cost, it does not avoid CO2 fossil fuels. The broader objective of this approach is to simultaneously
production and only few practical demonstrations have been made after reduce dependence on fossil fuels and reduce CO2 generation.
decades of development [7]. CCS operation also requires energy, which A techno-economic study is applied on the proposed eSMR concept
is normally provided by fossil fuels such as natural gas. Given that to assess its commercial viability. The techno-economic study in this
methane leaks have been identified as a highly damaging factor for article adds to the currently limited knowledge on target operating
global warming and are often higher than expected [7,20,21], using conditions and economic potential of eSMR, previously studied by
even more natural gas is not necessarily in line with the long-term Ambrosetti et al. [36] and Song et al. [35] through reactors based on
objectives of the energy transition. The warming potential of methane
structured catalysts. The numerical analysis from Ambrosetti et al. [36]
is effectively around 84 times higher than that CO2 over a 20-year
notably identifies low inlet pressure at the reformer as an ideal target
period [22].
for process conditions. This conclusion results from the use of a struc-
Methane pyrolysis has been proposed as a cleaner alternative for
tured catalyst, which enables a minimal pressure drop in the reactor.
hydrogen production [6,23]. This process avoids the majority of direct
The use of conventional reforming tubes and pelletized catalysts as a
process CO2 emissions of SMR, but it also increases reliance on fossil
basis for electrified SMR, as proposed in this article, implies physical
fuels by doubling the necessary quantity of natural gas per unit of
hydrogen produced (Eq. (4)). The problem of methane leakage in characteristics that greatly differ from those considered in the litera-
the natural gas supply chain ultimately reduces the decarbonization ture. Therefore, the process conditions identified in the literature for
potential of pyrolysis. eSMR operation cannot directly inform a techno-economic analysis of
eSMR using a conventional reformer architecture. This article uses a
CH4 ←←↽
←←←←⇀
←←←←←← C𝑠 + 2H2 𝛥Hr ◦ = 75.6 kJ∕mol (4) techno-economic analysis to identify the optimal process conditions for
an eSMR process using reformer tubes and pelletized catalysts.
An alternative chemical process that also relies on natural gas as
the primary feedstock is autothermal reforming (ATR), which combines This article contributes to the literature by demonstrating with a
partial oxidation of methane (POX) and reforming reactions [24]. The rigorous analysis that eSMR deployment through conventional reformer
combustion and reforming reactions take place at high temperature in tubes, catalysts and high-temperature heating equipment is feasible,
a compact refractory lined vessel to produce syngas. In a hydrogen and presents highly favourable economics. The remainder of the ar-
production context, an ATR reactor is typically followed by WGS to ticle details the tasks accomplished to enable that contribution: (1)
produce additional hydrogen from CO oxidation. An air separation development of a conceptual electrified SMR process and a conceptual
unit (ASU) is also integrated before the ATR reactor to provide a electrified reformer tube array, (2) definition of process and reforming
stream of O2 for the POX reactions. ATR can have a slightly lower CO2 reactor models, (3) development of techno-economic framework for
footprint than SMR, notably when the ASU unit is powered by low- eSMR, and (4) comparison between eSMR and conventional gas-fired
carbon electricity. ATR is generally seen as a decarbonization pathway SMR, water electrolysis, and methane pyrolysis.

2
D. Mehanovic et al.
Fig. 1. (a) Gas-fired SMR process flow diagram, adapted from Kumar et al. [37] and (b) electric SMR process flow diagram.
2. Gas-fired SMR
This section presents on overview of the conventional gas-fired
SMR process, and the implementation of gas-fired reformer tubes. The
objective of the section is to present a reference for comparison with
eSMR, and explain the limitations of existing SMR plants.
2.1. Gas-fired SMR process
The process flow diagram (PFD) of a conventional gas-fired SMR
plant is shown in Fig. 1a. The process includes several heat exchangers
and steam generators, in addition to three core units: a reformer, a shift
reactor (high-temperature shift), and a pressure swing adsorption (PSA)
unit for hydrogen separation. The natural gas feed is split between the
process feed and the furnace burners, in which it is used as fuel (1).
The reformer operates at temperatures above 800 ◦ C, and at rel-
atively high pressure (i.e., 30 bars [8]). Feedstock conversion in the
reformer is thermodynamically favoured at lower pressure, but PSA
units normally operate between 20 bars and 30 bars for effective
hydrogen separation. Process economics are ultimately favoured by
high pressure operation — although it leads to reduced conversion
in the reformer (i.e., <0.8 [37]), it also avoids the integration of a
compression step before PSA. This is mainly enabled by the possibility
to re-purpose all the unconverted and unrecovered species (4) as fuel
(i.e., CH4 , CO, H2 ). In addition to hydrogen, export steam (2) is also
generated by recuperating sensible heat in the flue gas exiting (4)
the reformer furnace. Although export steam increases the overall
efficiency of the process, it does not lead to the production of hydrogen,
3
Energy Conversion and Management 276 (2023) 116549
which is the desired end-product. The process efficiency for gas-fired
SMR is normally defined as [37]
𝐸𝐻2
𝜂𝑠 = (5)
𝐸𝑁𝐺 − 𝑄steam
where 𝜂𝑠 is the overall process efficiency of gas-fired SMR, 𝐸𝐻2 is
the LHV of hydrogen, 𝐸𝑁𝐺 is the LHV of natural gas, and 𝑄steam is
heat stored in export steam. Based on this definition, the efficiency of
optimized large scale plants that can export steam reaches values as
high as 0.77 [37]. In small-scale plants, which are usually part of less
integrated processes, steam export is not an option and efficiency is
normally reduced to values around ∼0.63.
2.2. Gas-fired reformer heating
Reformers heated by natural gas combustion come in several differ-
ent forms, with possible burner placement on the top, side, or bottom
of the furnace. For example, in a top-fired reformer furnace, the tubes
are arranged in linear arrays, which are then separated by flue gas exits
at the bottom of the furnace, and burners at the top.
The heat flux profile experienced by the tubes in a top-fired re-
former allows to rapidly reach and maintain a tube wall temperature
(TWT) near the maximum desired value, maximizing feedstock conver-
sion [38]. In practice, the maximum wall temperature of individual
tubes in a full system varies significantly. This variability has been
addressed by solutions such as real-time control of mass flow at burn-
ers [37], or improved designs of flue gas exits to ensure a more
uniform flue gas flow [39]. Temperature differences of up to 50 ◦ C,
or 5% [8,40], remain between the various tubes, ultimately causing
D. Mehanovic et al.
productivity losses from operation at process conditions that are kept
by precaution well below tube material limits.
Process conditions are limited by creep failure, as the tubes are
subjected to a high pressure and high temperature environment. The
Larson–Miller Parameter (LMP) is normally used as a creep failure crite-
rion, linking the maximum TWT with a given combination of operating
pressure and a desired minimum tube life (e.g., 100,000 h is a standard
value). As the LMP of the tube material is obtained under static loading,
a safety factor between 0.75 and 0.85 is applied to account for plant
startup and shutdown dynamics. For example, defining a safety factor
of 0.8, a microalloy tube (i.e., 35Ni/25Cr + additions) with the same
physical dimensions as in Kumar et al. [8] and operated at 30 bars, will
remain operational for at least 100,000 h if its maximum temperature
remains below 960 ◦ C [41]. In practice, the average temperature of the
tubes in a furnace is lower than 900 ◦ C, to ensure that all the tubes in
the furnace remain below the temperature imposed by the creep failure
limit [37,42]. Tighter control on the maximum TWT among tubes of an
array could therefore have a major impact on productivity, as a higher
operating temperature increases feedstock conversion [43].
Individual tube heating has the potential to greatly reduce TWT
variability and its negative impact on plant productivity. Section 3
presents a design for such individual tube heating, using radiant electric
heating elements. The top-fired plant from Latham et al. [44] and
Kumar et al. [37] is used as a model for the remainder of the paper.
3. Electrified SMR
The electrification of an existing hydrogen plant based on SMR
involves changes at the process level and inside the reformer furnace.
This section presents process changes needed for an electrically heated
SMR process, and proposes a specific approach for the electrification of
an array of reformer tubes.
3.1. Electrified SMR process
In contrast to gas-fired SMR, an electrified SMR process must target
near-complete feedstock conversion to maximize value, while mini-
mizing carbon footprint, because unconverted species cannot be used
as fuel. In case of significant feedstock traces in the PSA off-gas,
unconverted species must be recirculated, leading to non-negligible
costs for gas separation and re-compression. Alternatively, if only a
small molar fraction of unconverted feedstock is present, flaring can
be integrated with a final CO2 sequestration step. Fig. 1b shows the
PFD of an electrified SMR process designed for minimal CO2 footprint,
without the integration of a specific system for the management of PSA
off-gas.
Comparatively to the PFD shown in Fig. 1a, this process is devoid
of heat exchangers for heat recuperation from flues gas, and is instead
equipped with four additional processing units: (1) an electric pre-
heater, (2) a low-temperature shift (LTS) reactor, (3) a downstream
compressor, and (4) a smaller PSA unit that recovers H2 from the off-
gas of a main PSA unit. The pre-heater is a necessary component due to
the absence of flue gas, which provides additional heat for the incoming
process gas in conventional SMR. The LTS reactor converts additional
CO, maximizing H2 yield from the reforming process. A compressor
is added to attain the necessary pressure for PSA — as shown further
(Sections 5 & 6), lower pressure is necessary to enable high feedstock
conversion. A second PSA unit is included to maximize H2 recovery.
The electricity conversion (electrical-to-chemical) efficiency of this
process is defined as
𝐻out,25 ◦C − 𝐻in,25 ◦C
𝜂𝑒 = (6)
𝑄𝑒
where 𝜂𝑒 is electric energy conversion efficiency, 𝐻in,25 ◦ C and
𝐻out,25 ◦ C are respectively the enthalpy of the reactants entering the
reformer and products exiting WGS at 25o C, and 𝑄𝑒 is the total
4
Energy Conversion and Management 276 (2023) 116549
electricity consumption. 𝑄𝑒 accounts for the electricity used in both
gas compression and heating (reactants pre-heating and reforming
reaction). This efficiency term is useful to quantify the ability of the
process to store electric energy in the form of chemical bonds, but does
not necessarily penalize a process converting less feedstock. Similarly to
the efficiency definition for conventional gas-fired SMR, the efficiency
of electric SMR can be defined as
𝐸𝐻2
𝜂𝑝 = (7)
𝐸𝑁𝐺 + 𝑄𝑒
where 𝜂𝑝 is the overall efficiency of an electric SMR process. Compar-
atively to the denominator in Eq. (5), where a term quantifying the
energy re-purposed through export steam is subtracted, the denomi-
nator of Eq. (7) includes the contribution of electricity to energetic
cost.
3.2. Reformer tube array electrification
The proposed electrified reformer tube concept is presented in
Fig. 2. This design uses individual radiant heaters and insulation com-
ponents for each tube. Insulation avoids significant radiative heat losses
from the reformer tubes, ensuring that a maximum quantity of the heat
generated electrically is absorbed by the reforming reaction. Forced
convection from cooling fans is used to evacuate the heat that cannot be
absorbed by the reforming reaction, and therefore avoid overheating of
electrical connections on the outside of the insulation. This forced con-
vection cooling is ultimately a source of heat loss in the process energy
balance, and is considered through an efficiency term (Section 4).
The radiant heating element is a contact-less coiled wire, physically
supported by the insulation. Such radiant heaters are normally used
in diffusion furnaces in the micro-electronics industry [45]. Maximum
heat flux is determined by (1) the reforming process temperature, (2)
maximum temperature of the radiant heating wire, and (3) the ratio of
coil diameter to inner tube diameter (𝑑coil ∕𝑑tube,in ). In an new plant, a
custom reformer tube array arrangement could allow a relatively high
𝑑coil ∕𝑑tube,in , but a potential trade-off arises to ensure minimum LCOH
— maximizing heat flux leads to a higher 𝑑coil ∕𝑑tube,in , and therefore
more coil surface area to be insulated in order to minimize thermal
losses. The coil diameter is therefore an important design variable,
but in a retro-fitting scenario it is limited by the distance between
subsequent reformer tubes — heat flux values between 90 kW/m2 and
100 kW/m2 can be reached, with the inner side of the reformer tube
as the reference surface area. Although these values are lower than the
heat flux attained in gas-fired reformers (up to ∼130 kW/m2 [46]), it is
sufficient to reach high feedstock conversion and the same H2 output
as a gas-fired reformer. Along the length of the tube, gradual variation
of the heat flux can be accomplished with a variable pitch coil. The
necessity for such precise longitudinal control of heat flux is assessed
in Section 5. Heat flux variability on the perimeter of the reformer tube
can be neglected, given that the sub-centimeter pitch and low angle of
the coil are on the scale of reforming catalyst particles.
4. Process and reformer modelling
The performance of the proposed eSMR process is evaluated using a
steady-state process balance on mass, energy, and momentum, as well
as a 1D thermochemical model of the reformer. This section presents
both the process balance and reformer model.
4.1. Process balance
The mass balance of the process is divided between a detailed
modelling for the reforming reactor (Section 4.2), and a 0D analysis
for WGS conversion and PSA recovery. The model assumes that the
CO exiting the reformer is reduced to a molar fraction of 0.5%, after
passing through the HTS and LTS reactors [47]. H2 recovery from PSA
D. Mehanovic et al. Energy Conversion and Management 276 (2023) 116549

Fig. 2. 3D representation of the proposed electrified reformer concept, with dimensions based on a model plant [8]. Two rows of 16 tubes are shown with cooling fans in between.
A detailed section view illustrates the integration of a coiled radiant heating element around a reforming tube. Manifolding and secondary structural and electrical components
are not shown.

Table 1
Flow conditions at reformer inlet [44].
Symbol Value
𝑇 inlet 611 ◦ C
𝑃 inlet Section 5
𝑥H2O 0.7462
𝑥CO2 0.0047
𝑥H2 0.0004
𝑥CO 0
𝑥CH4 0.2421

is assumed to be 90% [48] – with the second PSA unit recovering

90% of the off-gas from the first PSA unit, a total recovery of 99% is
assumed.
The energy balance of the process is defined as
( ) Fig. 3. Diagram of the inputs and outputs of the process balance and reformer model.
𝑞̇ sens, ref in + 𝑞̇ steam = 𝜂𝐻𝑋 𝑞̇ sens, ref out + 𝑞̇ 𝑊 𝐺𝑆 + 𝜂𝑃 𝐻 𝑞̇ pre-heating (8) The block identified as energy sum uses results from the model and process balance
to calculate the total energy consumption per unit of hydrogen produced.
where 𝑞̇ sens, ref in and 𝑞̇ sens, ref out are respectively the sensible heat in
the gases entering and exiting the reformer, 𝑞̇ 𝑊 𝐺𝑆 is the heat of reaction
recuperated from the shift reaction, 𝑞̇ steam gen. is the energy needed for
steam generation, 𝑞̇ pre-heating is the additional pre-heating needed for where 𝑃compressor is the compressor shaft power requirement (kW), 𝑄
energetic balance, 𝜂𝐻𝑋 is the overall process heat exchanger efficiency, is the mass flow (kg/s), 𝑍 is the compressibility factor of the gas, 𝑇 is
taken as 90% [37], and 𝜂𝑃 𝐻 is the thermal efficiency of the electric pre-
the inlet temperature (K), 𝑅 is the universal constant of ideal gases, 𝑀
heater. 𝑞̇ sens, ref in and 𝑞̇ steam gen. are fixed values, as the inlet mass flow
is the molar mass of the gas, 𝜂𝑖 is the compressor efficiency, 𝑁 is the
ans gas temperature at reformer inlet are kept constant. Table 1 shows
number of compressor stages, 𝛾 is the ratio of specific heats, 𝑃out is the
reformer inlet flow conditions.
outlet pressure and 𝑃in is the inlet pressure. An ideal gas assumption is
The pressure drop from reformer inlet to compressor inlet accounts
made, and the 𝑍 variable is equal to 1. An efficiency term 𝜂𝑐 is added
for the pressure losses in the reformer and HTS reactor, neglecting the
contribution of other components. Both pressure drop terms (reformer on top of the shaft power requirement to account for the electric motor
and HTS) are obtained using the Ergun equation for pressure drop in driving the compressor.
fluid flow through packed beds (see Eq. (13)). The physical parameters The heat required for the SMR reactor is obtained with the 1D
of the packed beds that are needed to apply the Ergun equation are thermochemical model presented in Section 4.2. Fig. 3 shows the flow
shown in Sections 7 and 6. Calculating these pressure drops allows to of information from the reformer model to the process balance, and
size the compressor unit necessary to reach the PSA inlet pressure. The the respective results needed from each to evaluate the total energy
compression power is obtained with an ideal gas model [49] consumed to produce a unit of hydrogen. The reformer model calculates
the heat for reforming, while the process balance feeds the energy sum
⎛( ) 𝛾−1 ⎞
𝑍𝑇 𝑅 𝑁𝛾 ⎜ 𝑃out 𝑁𝛾
𝑃compressor =𝑄 − 1⎟ (9) with: (1) H2 molar fraction at PSA outlet, (2) pre-heating requirement,
𝑀𝜂𝑖 𝛾 − 1 ⎜ 𝑃in ⎟ and (3) pressure at compressor inlet.
⎝ ⎠

5
D. Mehanovic et al. Energy Conversion and Management 276 (2023) 116549

Energy balance at section 𝑖 is defined as

∑ 𝑇𝑖 ( )
𝑛̇ 𝑗,𝑖,in 𝐶𝑝,𝑗 𝑑𝑇 + ℎ𝑡𝑔 2𝜋𝑟in 𝛥𝑦𝑖 𝑇𝑖,in wall − 𝑇𝑖
𝑗
∫𝑇𝑖,in
∑ (12)
− 𝜋𝑟2in 𝛥𝑦𝑖 𝜌cat 𝜂 𝑓𝑝𝑟𝑥|𝑘<2 𝑟𝑘 𝛥𝐻𝑘 = 0
𝑘

where 𝐶𝑝,𝑗 is specific heat at constant pressure of species 𝑗, ℎ𝑡𝑔 is the

convection heat transfer coefficient between tube wall and process gas,
𝑟in is the inner radius of the tube, and 𝛥𝐻𝑘 is the enthalpy of reforming
reaction 𝑘.
Momentum balance at section 𝑖 is
[ ]
𝜌𝑖 𝑣2𝑖 1−𝜙 150 (1 − 𝜙)
𝑃𝑖,in − 𝑃𝑖 − 𝑓 𝛥𝑦𝑖 = 0; 𝑓 = 1.75 + (13)
𝐷𝑝 𝜙3 𝑅𝑒
where 𝜌𝑖 is process gas density, 𝑣𝑖 is process superficial gas velocity,
𝐷𝑝 is catalyst particle diameter, 𝜙 is porosity of the catalyst bed, and
Fig. 4. 1D thermochemical model variables.
Source: Figure adapted from Kumar et al. [8].
𝑅𝑒 is the Reynolds number. This corresponds to the Ergun equation for
pressure drop associated to fluid flow in a packed bed [51].
The heat of reforming reactions is calculated using the Kirchhoff
equation
4.2. Reformer tube thermochemical model
( ) ∑ 𝑇𝑖
𝛥𝐻𝑘 𝑇𝑖 = 𝛥𝐻𝑘 (298 K) + 𝛾𝑗,𝑘 𝐶𝑝,𝑗 𝑑𝑇 , 𝑘 𝜖 {1, 2, 3} (14)
A thermochemical model of a reformer tube is used to predict 𝑗
∫298
hydrogen output and energy consumption for the proposed electric
The convection coefficient ℎ𝑡𝑔 in Eq. (12) is obtained from a general
SMR process. The model is based on work from Latham et al. [44],
heat transfer correlation for smooth spherical particles [52], defined as
and certain elements from Kumar et al. [8,37]. Model parameters were
fitted on experimental data of full-scale industrial SMR reactors. The ( )
𝑘gas 𝐷𝑝
implementation of the model in this study was validated using specific ℎ𝑡𝑔 = 𝑓ℎ𝑡𝑔 0.813 exp −3 𝑅𝑒0.9 (15)
data points from Latham et al. [44]. 2𝑟in 𝑟in
A single reformer tube is discretized longitudinally, with the model where 𝑓ℎ𝑡𝑔 is a fitting parameter taken from Latham et al. [44], and
variables of a tube section 𝑖 shown in Fig. 4: 𝑛̇ 𝑗,𝑖,in and 𝑛̇ 𝑗,𝑖 are re- 𝑘gas is the thermal conductivity of the process gas. This correlation is
spectively the incoming and exiting molar flows of species 𝑗, 𝑃𝑖,in and satisfactory for ratios of 𝐷𝑝 ∕𝐷tube,in varying from approximately 0.05
𝑇𝑖,in are pressure and temperature of the incoming flow, 𝑃𝑖 and 𝑇𝑖 are to 0.3. For the catalyst tube in this study, 𝐷𝑝 ∕𝐷tube,in is equal to 0.045.
pressure and temperature at section 𝑖, 𝑇𝑖,in wall and 𝑇𝑖,out wall are the Heat flux balance at the tube wall is
( )
inner and outer temperature of the tube wall, 𝛥𝑦𝑖 is the height of section 2𝜋𝑘tube 𝛥𝑦𝑖 𝑇𝑖,out wall − 𝑇𝑖,in wall ( )
𝑖, and 𝑞𝑖,rad is the radiative heat flux. ( ) = ℎ𝑡𝑔 2𝜋𝑟in 𝛥𝑦𝑖 𝑇𝑖,in wall − 𝑇𝑖 (16)
𝑟
The full model developed by Latham et al. [44] captures the com- ln 𝑟out
in
plex physics of radiative heating from combustion at a furnace level. where 𝑘tube is the thermal conductivity of the tube, and 𝑟out is the outer
Given the design of the proposed electric reformer tube array, radiative radius of the tube. The left hand side corresponds to the conduction
heating physics are constrained to individual tubes, and there are heat flux through the tube wall, and the right hand side corresponds
no complex interactions between arrays of tubes and with refractory to the convection heat transfer to the process gas. The incoming heat
furnace walls that need to be modelled. The heat flux profile of each flux itself equals the imposed radiative heat flux 𝑞𝑖,rad . A baseline value
tube can be controlled in a relatively accurate way, allowing radiative of 0.95 is assumed for reformer heating efficiency in further analyses
heating to be simply represented as an imposed heat flux along the (Sections 5 & 6), which is a design standard for electric furnaces
length of individual tubes. The hydrogen output and energy consump- using the radiant heaters considered [45]. The exact thermal losses
tion of the complete tube array is therefore the multiplication of the are however unknown, and Section 6 presents a sensitivity analysis
total number of tubes by the hydrogen output and energy consumption quantifying the impact of variations in reformer heating efficiency on
of a single tube. This allows to rapidly run several simulations and LCOH.
assess performance over a wide range of operating conditions (see Given the flexibility of the proposed electric heating implementa-
Section 5). To complete a simulation, the balance equations for mass, tion, the heat flux prescribed can be adjusted to near-optimal values. An
energy, and momentum are solved for each discretized tube section optimal heating profile for an electrified system is one that maximizes
using the Newton–Raphson method feedstock conversion, in order to minimize the carbon footprint of the
( ) process. The minimization problem that arises is defined as [38]
𝑥⃗𝑘+1 = −𝐽 −1 ⋅ 𝑓⃗ 𝑥⃗𝑘 + 𝑥⃗𝑘 (10)
min 𝑥CH4 (𝐿)
where 𝑥⃗𝑘+1 is the vector of model unknowns at step 𝑘 + 1, −𝐽 −1 is the 𝑞̇ rad (𝑧)
Jacobian matrix, 𝑓⃗ is the vector of model equations, and 𝑥⃗𝑘 is the vector s.t. 𝑇out wall (𝑧) ≤ 𝑇max (17)
of model unknowns at step 𝑘.
𝑞̇ rad (𝑧) ≤ 𝑞̇ max
Mass balance at section 𝑖 is defined as
∑ where 𝑧 is the vertical/longitudinal coordinate of the tube, 𝑥CH4 is
𝑛̇ 𝑗,𝑖,in − 𝑛̇ 𝑗,𝑖 + 𝜋𝑟2in 𝛥𝑦𝑖 𝜌cat 𝜂 𝛾𝑗,𝑘 𝑓𝑝𝑟𝑥|𝑘<2 𝑟𝑘 = 0 (11) the molar fraction of natural gas in the process gas at tube outlet,
𝑘
𝑇max is the maximum allowable tube wall temperature, and 𝑞̇ max is
where 𝜌cat is catalyst density (kg/m3 ), 𝜂 is catalyst effectiveness, 𝛾𝑗,𝑘 the maximum attainable radiative heat flux. Therefore, after setting
is the coefficient of species 𝑗 in reforming reaction 𝑘, 𝑓𝑝𝑟𝑥 is a fitting process gas conditions at tube inlet (molar flow, temperature, pressure),
parameter taken from Latham et al. [44], and 𝑟𝑘 is the reaction rate an iterative optimization algorithm based on Eq. (17) can be used
of reaction 𝑘. Reaction rates are defined using equations from Xu to determine the optimal heating distribution along the tube, given
et al. [50] for SMR and WGS kinetics on a nickel-based catalyst. constraints on 𝑇max and 𝑞̇ max . The objective of Eq. (17) is redundant

6
D. Mehanovic et al.
Table 2
Parameter values used in the reformer thermochemical model [8,44].
Symbol Description Value
𝐿 Reformer tube length 12.5 m
𝑟in Inner tube radius 6 cm
𝑟out Outer tube radius 7.5 cm
𝜌cat Catalyst density 1100 kg/m3tube
𝑓prx Fitted parameter 1.0
𝑓htg Fitted parameter 1.67
𝜙 Bed porosity 0.605
𝐷𝑝 Catalyst particle diameter 5.4 mm
𝜂 Catalyst effectiveness 0.1
𝑘tube Tube wall thermal conductivity 29.58 W/mK
in the case of a continuous heating profile, as either 𝑇max or 𝑞̇ max are
always maximized locally. The objective is however not redundant in
the case of a discretized heating profile, which involves heating profile
sections that consist of 𝑇max and 𝑞̇ max values both below their respective
maxima.
5. Process performance with optimal and discretized reformer
heating
Simulations of the reformer and process models enable the calcula-
tion of overall energy consumption and molar fractions at PSA outlet,
allowing the selection of optimal operating conditions for electrified
eSMR. Table 2 presents the physical parameters used in the model.
This section first presents the key reformer model results for specific
operating conditions, for both continuous and discretized heat flux
profiles. The remainder of the section is an evaluation of the impact
of different combinations of 𝑃in and 𝑇max on feedstock conversion and
process efficiency. All the simulations are conducted with a mass flow
35% below the nominal mass flow in the model reformer from Latham
et al. [44], with the objective to have approximately the same H2 yield
at process outlet at a feedstock conversion of 0.95.
5.1. Reformer heat flux profile
Fig. 5 presents the optimal heat flux profile, and corresponding
temperature distribution, pressure drop, and molar fractions along
reformer tube length, for 𝑃in = 21 bars and 𝑇max = 970 ◦ C – this is
the design point selected for the techno-economic analysis. The top
and bottom left graphs in Fig. 5 show that heat flux is maintained at
peak value until maximum TWT is reached, and then rapidly decays
to ensure that TWT does not exceed the maximum allowable value.
Given the practically null heat flux at reformer outlet, TWT (in and out)
are virtually the same as the process gas temperature. Although inlet
pressure is significantly lower than in the model reformer (21 bars vs.
30 bars [44]), pressure drop is comparable (∼1 bar) due to the lower
mass flow. The graph of molar fractions shows however shows that
most of the feedstock conversion is completed at around 8 m down the
tube length.
This last graph demonstrates the potential for process intensification
with the process conditions allowed by electrified reforming, and that
although near-optimal heating can be targeted with electric heating,
there remains a high degree of robustness to a non-optimal heat flux
profile. This is notably illustrated by comparing the attainable feedstock
conversion of a reformer operated under a continuous heat flux profile
and a reformer operated under a discretized heat flux profile, with both
cases targeting an optimal heating policy in which feedstock conversion
is maximized. Fig. 6 illustrates the continuous heat flux profile and
corresponding 𝑇𝑖,out wall , along discretized heat flux profile and corre-
sponding 𝑇𝑖,out wall for 5 and 10 discrete heating sections. Results show
that, as the number of heating sections decreases, the initial reactor
length subject to peak heat flux decreases, leading to a sharper drop
in temperature. For the case of 5 heating sections, 𝑇𝑖,out wall drops
7
Energy Conversion and Management 276 (2023) 116549
Table 3
Process conditions and performance of the model gas-fired SMR plant [8,44] and the
proposed electrified version of the plant.
Parameter Gas-fired SMR eSMR
𝑇max (◦ C) 860 970
𝑃𝑖𝑛 (bars) 30.06 21
CH4 conversion <0.8 0.97
𝜂𝑝 ∼0.63 0.81
by nearly 6%, but the impact on feedstock conversion is minimal —
the average 𝑇𝑖,out wall is decreased by less than 10 ◦ C relatively to
continuous heating, and conversion at tube outlet is reduced by less
than 0.7%, from 0.97 to 0.964.
Given the minimal impact from heat flux profile discretization on
process performance, the parameter study presented in the remainder
of this section assumes a continuous heat flux profile.
5.2. Parameter study
Fig. 7 presents feedstock conversion at reformer outlet as a function
of 𝑃in and 𝑇max . As expected, conversion increases with decreasing 𝑃in
and increasing 𝑇max . Reproducing the same conditions as in the model
gas-fired process (𝑃in = 30 bars and 𝑇max = 860 ◦ C), conversion is near
0.8, far below an acceptable value for an electrified SMR process (see
Section 3). At 𝑃in = 30 bars, the necessary temperature to attain a
feedstock conversion of 0.95 is above the limit imposed by the creep
failure criterion (i.e., 100,000 h tube life). This shows that 𝑃in must be
minimized if conversion alone is a decision parameter.
Electrical-to-chemical efficiency (Eq. (6)) is shown in Fig. 8 as a
function of 𝑃in and 𝑇max . In contrast to feedstock conversion, electrical-
to-chemical efficiency is maximized at higher pressure (𝑃in = 26 bars).
This results from compression energy adding up to the denominator
of Eq. (6) as 𝑃in is reduced, in order to reach the prescribed pressure at
PSA inlet (25 bars). If pressure is increased beyond ∼26 bars, sensible
heat is needlessly lost through unconverted feedstock, as heat energy
is added without additional hydrogen production. By increasing 𝑇max
beyond 1030 ◦ C, the reverse WGS reaction is favoured, leading to an
increase in energy demand and a decrease in hydrogen output.
Overall process efficiency, as defined by Eq. (7), is also assessed for
various combinations of 𝑃in and 𝑇max and shown in Fig. 9, along with
the tube creep limit. Results show an optimal point at 𝑃in = 21 bars
and 𝑇max = 1040 ◦ C, above the tube creep limit, and corresponding
to a feedstock conversion of 0.99. Because Eq. (7) imposes a penalty
on unconverted feedstock, through the inclusion of feedstock LHV
in the denominator, the set of optimal process conditions is located
between the conditions for maximum feedstock conversion and those
for minimum electricity consumption. For almost the full graph region
below the creep limit of the tube material, process efficiency is favoured
at lower 𝑃in (exception above 𝑇max = 1000 ◦ C). This shows that if a set of
operating conditions leading to high feedstock conversion is targeted,
the proposed electric SMR process is more efficient than existing gas-
fired SMR processes in converting feedstock and thermal energy into
hydrogen. However, the exact set of operating conditions to target is
ultimately dictated by the economics of the process, which involve
capital expenditures and equipment replacement costs that are not
taken into account in this purely energetic analysis.
Table 3 presents a summary of the operating conditions and process
performance of the model gas-fired SMR plant (Section 2) and the
proposed electrified version of the plant.
6. Techno-economic model
The proposed eSMR process is compared with gas-fired SMR on a
levelized cost basis (LCOH) and with CO2 cost of abatement (CCoA), a
decarbonization metric defined as
𝐿𝐶𝑂𝐻 − 𝐿𝐶𝑂𝐻𝑅𝐸𝐹
𝐶𝐶𝑜𝐴 = (18)
𝛥𝐶𝑂2
D. Mehanovic et al. Energy Conversion and Management 276 (2023) 116549

Fig. 5. Heat flux profile, and corresponding temperature, pressure, and molar fractions distributions along reactor length for an optimal heating distribution profile, with 𝑃in = 21
bar and 𝑇𝑚𝑎𝑥 = 970◦ C.

Fig. 6. Continuous and discrete (5 and 10 equal sections) axial heat flux with corresponding outer tube wall temperature(𝑇out wall ).

where 𝐶𝐶𝑜𝐴 is the CO2 cost of abatement ($/tonCO2 ), 𝐿𝐶𝑂𝐻𝑅𝐸𝐹 is the is the levelized cost of hydrogen of a decarbonizing process ($/kgH2 ),
levelized cost of hydrogen of the reference process ($/kgH2 ), 𝐿𝐶𝑂𝐻 and 𝛥CO2 is the difference in CO2 emissions between the two processes

8
D. Mehanovic et al.
Fig. 7. Feedstock conversion at reformer outlet as a function of 𝑃in and 𝑇max . Tube creep life limit shown with a dashed white line [41]. The identified design point corresponds
to the baseline process conditions selected for the techno-economic analysis in Section 7.
Fig. 8. Electrical-to-chemical conversion efficiency as a function of 𝑃in and 𝑇max . Tube creep life limit shown with a dashed white line [41]. The identified design point corresponds
to the baseline process conditions selected for the techno-economic analysis in Section 7.
(tonsCO2 /kgH2 ). Gas-fired SMR is defined as the reference, having a
total CO2 footprint of 17.1 kgCO2eq /kgH2 , that breaks down into direct
emissions (process and combustion) of 10.58 kgCO2 /kgH2 [37] and
indirect emissions of 6.52 kgCO2eq /kgH2 from methane leakage in the
natural gas supply chain (see Table 4).
For combustion-based SMR, LCOH over a wide range of production
has been defined by [53] as
𝐿𝐶𝑂𝐻𝑆𝑀𝑅 = 𝐶𝐺,𝐹 𝑆 𝑃 + 𝐶𝐺,𝐶𝐴𝑃 + 𝐶𝐺,𝑂𝑀 (19)
where 𝐿𝐶𝑂𝐻𝑆𝑀𝑅 is the levelized cost of hydrogen from SMR ($/kgH2 ),
𝐶𝐺,𝐹 𝑆 is a coefficient representing feedstock expenses for a gas-fired
SMR process (0.19), 𝑃 is natural gas price ($/MMBtu), and 𝐶𝐺,𝐶𝐴𝑃
and 𝐶𝐺,𝑂𝑀 are respectively the CAPEX (0.34) and fixed operation and
maintenance (O&M) expenses (0.16) for a gas-fired SMR plant. All
terms have been adjusted with the M&S index using 2021 as the basis
year.
9
Energy Conversion and Management 276 (2023) 116549
Subtracting the portion of the multiplication coefficient in Eq. (19)
attributable to feedstock expenses, and adding a lumped term for
overall capital and operational expenses for electrification, the LCOH
of electrified SMR can be defined as
𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 = 𝐶𝐸,𝐹 𝑆 𝑃 + 𝐶𝐸 𝐸 + 𝐶𝐸,𝐶𝐴𝑃 + 𝐶𝐸,𝑂𝑀 (20)
where 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 is the LCOH of eSMR, 𝐶𝐸,𝐹 𝑆 and 𝐶𝐸 are coeffi-
cients representing feedstock and electric energy consumption for an
electrified SMR process, 𝐸 is electric energy price ($/kWh), 𝐶𝐸,𝐶𝐴𝑃
and 𝐶𝐸,𝑂𝑀 are CAPEX and OPEX for an electrified SMR plant. The
main techno-economic parameters allowing to these coefficients and
constants are shown in Table 4. At the selected eSMR process conditions
in Section 7, 𝐶𝐸,𝐹 𝑆 , 𝐶𝐸 , 𝐶𝐸,𝐶𝐴𝑃 , and 𝐶𝐸,𝑂𝑀 are respectively 0.11
MMBtu/kgH2 , 12.12 kWh//kgH2 , $0.416/kgH2 , and $0.192/kgH2 .
Economic parameters are the same, or closely aligned with, values
from other studies on hydrogen production alternatives [6,10,31]. The
natural gas price of $4/MMBtu approximates the average pricing trend
D. Mehanovic et al.
Fig. 9. Process efficiency as a function of 𝑃in and 𝑇max . Tube creep life limit shown with a dashed white line [41]. The identified design point corresponds to the baseline process
conditions selected for the techno-economic analysis in Section 7.
Table 4
Main techno-economic parameters.
Economic parameters Value
Equipment lifetime 20 years
Nominal discount rate 10%
Inflation rate 2%
$ basis year 2021
Grid parameters Value
Natural gas price (𝑃 ) $4/MMBtu
Electricity price (𝐸) $0.04/kWh
Natural gas indirect emissions 32.4 kgCO2 eq/MMBtu
Electricity carbon footprint 50 gCO2 eq/kWh
from the three previous years in the US [14,54]. The use of natural gas
as feedstock also implies indirect carbon emissions through methane
leakage in the natural gas supply chain (extraction, processing, dis-
tribution). The methane leakage as a percentage of total natural gas
production is estimated to range between approximately 1% and 3.5
% [7,25,55]. The upper bound corresponds to leakage at production
sites primarily dedicated to oil extraction, in which natural gas is a
by-product [55], while extraction sites strictly dedicated to natural
gas production show much less leakage. A comprehensive field study
by Alvarez et al. estimates that methane leakage in the U.S. oil and
gas industry is equivalent to 2.3% of domestic natural gas production.
A figure of 2% is used for the purposes of carbon footprint analysis
in this study, making the assumption that some reduction in supply
chain leakage is readily achievable with improved maintenance [20].
This leakage value corresponds to indirect emissions of approximately
32.4 kgCO2 eq/MMBtu, assuming that the global warming potential
of methane is 84 times that of CO2 [22]. The electricity price of
$0.04/kWh is currently a best-case scenario found in Quebec [56], but
it is also in the near-term reach of several renewable energy harvesting
pathways [57]. The CO2 footprint considered for electricity is taken
as an above-average value of the range of emissions associated with
hydro, wind, and PV electricity. These emissions range from less than
10 gCO2 eq/kWh to ∼70 gCO2 eq/kWh [58]. The total emissions per
unit of hydrogen produced are assessed for various process operating
conditions in Section 7.
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Energy Conversion and Management 276 (2023) 116549
Table 5
Lang factor breakdown and yearly OPEX as a function of total purchased equipment
cost.
Factors for added capital investment Value
Equipment installation 0.47
Electrical systems (installed) 0.11
Indirect costs 1.4
Total Lang factor 3
OPEX parameters Value (%)
O&M 3
Electric heating replacement 20a
a Applied only on electrical heating system cost.
The total capital cost incurred from the process electrification equip-
ment is obtained by applying a Lang factor of 3 to equipment cost [59].
The different sources of costs considered for the Lang factor defini-
tion are presented in Table 5. Operational expenses, other than those
associated to feedstock and electricity costs, are also defined as a
function of capital investment (Table 5). Insurance and labour costs are
already considered by other terms in Eq. (19), and are not directly af-
fected by electrification. The defined OPEX of 20% for electric heating
replacement is equivalent to an equipment life of 5 years.
The cost of process electrification equipment is presented in Table 6.
The costs of the furnace electrification system, the electric feedstock
pre-heater, and the PSA unit are obtained from manufacturer quotes.
The furnace electrification system includes radiant heating elements
and insulation — the cost of cooling fans is negligible. LTS reactor
cost is a function of its dimensions, assumed conservatively to be the
same as the dimensions of the HTS reactor (7.7 m length, 3.8 m diame-
ter [37]). Compressor cost is a function of its shaft power (Eq. (9)) [59].
7. Techno-economics results and discussion
Fig. 10a presents the change in 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 relatively to 𝐿𝐶𝑂𝐻𝑆𝑀𝑅
in the baseline economic scenario.
Results show that cost parity cannot be attained even with process
parameters above the tube creep limit. Variation in 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 is
mostly caused by a change in 𝑇max , especially above the 22% isoline,
D. Mehanovic et al. Energy Conversion and Management 276 (2023) 116549

Fig. 10. (a) Relative 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 variation relatively to 𝐿𝐶𝑂𝐻𝑆𝑀𝑅 in the baseline economic scenario and (b) CO2 avoided as a function of 𝑃in and 𝑇max .

minimize LCOH. The results also show a minimum 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 at oper-

Table 6
Equipment cost.
ating conditions different from the ones observed in Fig. 9, illustrating
Component Value
overall process efficiency (Eq. (7)). The minimum 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 value
is obtained at a higher inlet pressure, comparatively to the optimal
Furnace electrification system $2.5 k/m of reformer tube
Electric feedstock pre-heater $150 k/MW pressure inlet from maximum process efficiency, close the point of
LTS reactor $5 k/tonH2 /day minimum 𝜂𝑒 . This is caused by the inclusion of capital expenses in
Compressor $800 k/MW the calculation of LCOH, and increased post-reforming compressor cost
PSA unit $500/N m3 /h
when inlet pressure at the reformer is lower. The variation of LCOH
is however relatively low (below ∼3%) over the graph portion where
conversion is above 0.95.
As decarbonization is the main objective with electrification, CO2
which is relatively flat from approximately 17 bars to 26 bars. This abatement is presented in Fig. 10b as a function of maximum TWT
demonstrates the importance of precise control over maximum TWT to and reformer inlet pressure. Unlike LCOH, CO2 abatement is optimized

11
D. Mehanovic et al.
Fig. 11. LCOH of eSMR as a function of feedstock and electricity prices at design-point operating conditions (𝑃𝑖𝑛 = 21 bars and 𝑇max = 970 ◦ C). Graph zones where the LCOH of
water electrolysis and methane pyrolysis are lower than 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 are highlighted.
at the lowest inlet pressure considered (15 bars). This shows that the
carbon footprint of eSMR in a low-carbon electric grid is minimized at
high feedstock conversion (low 𝑃𝑖𝑛 ), rather than high process efficiency
(high 𝑃𝑖𝑛 ). There is however a significant shift with increasing CO2
footprint of the electric grid. At approximately 400 gCO2 eq/kWh, the
point after which eSMR becomes more carbon intensive than gas-fired
SMR (𝛥CO2 < 0), minimum CO2 footprint is achieved at 𝑃𝑖𝑛 = 23.5
bars. For reference, a Combined Cycle Gas Turbine (CCGT) power plant
has a CO2 footprint of 500 gCO2 eq/kWh [60]. If the input electricity of
eSMR is indeed coming from a CCGT power plant, the proposed process
will ultimately lead to more CO2 emissions than an equivalent gas-
fired SMR, which is itself based on natural gas combustion, but without
an additional energy conversion step that generates electricity before
process heat generation.
Fig. 10a and b also show that optimizing process parameters based
on the best values for either H2 production cost or CO2 abatement is not
an option, with both criteria leading to 𝑃𝑖𝑛 and 𝑇max values above the
tube creep limit. For the remainder of the analysis, a set of operating
conditions is instead selected by (1) placing a requirement for high
feedstock conversion (0.97), and by (2) assuming that a relatively low
temperature margin (20 ◦ C) is sufficient for continuous operation away
from the tube creep limit, given the precise control on TWT allowed by
electric heating. As shown on Fig. 7, this corresponds to 𝑃𝑖𝑛 = 21 bars
and 𝑇max = 970 ◦ C, where process efficiency is 0.816 (see Fig. 9). At
this point, LCOHeSMR is equal to $1.53/kgH2 .
Fig. 11 shows 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 as a function of feedstock and electricity
prices, using 𝑃𝑖𝑛 = 21 bars and 𝑇max = 970 ◦ C as process conditions.
Graph zones where price combinations lead to LCOH supremacy for
either water electrolysis [9] or methane pyrolysis are also identified.
The LCOH of electrolysis is modelled as a linear function of electricity
price, with a constant term for CAPEX and an energy requirement
of 50 kWh/kgH2 [9]. Pyrolysis is not yet a well-established hydrogen
production pathway, and several distinctive technologies have been
proposed [23]. The results from a specific techno-economic assessment
of pyrolysis, powered by natural gas combustion, are used to define
the LCOH of pyrolysis as a direct function of natural gas price [6].
The free region in the graph represents a funnel in which feedstock
and electricity price combinations allow the proposed eSMR pathway
to have the lowest LCOH.
Results show that 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 remains relatively low (<$2/kgH2 )
over a wide range of feedstock and electricity prices. The orientation
12
Energy Conversion and Management 276 (2023) 116549
of the isolines further shows that the sensibility of LCOH to every
variation of $1/MMBtu in feedstock price is practically the same as
a variation of $0.01/kWh in electricity price. This comes from the
fact 𝐶𝐸,𝐹 𝑆 and 𝐶𝐸 in Eq. (20) have comparable values at the selected
process design point. This makes eSMR more robust to market vari-
ability when compared to gas-fired SMR or methane pyrolysis, and
purely electric pathways such as electrolysis, as the OPEX portion in its
LCOH is equally split between natural gas and electricity expenses. The
free region in Fig. 11 represents this with a funnel in which feedstock
and electricity price combinations allow the proposed eSMR pathway
to have the lowest LCOH among other potential H2 decarbonization
pathways. At a fixed electricity price, electrolysis becomes more eco-
nomically advantageous than eSMR when a threshold natural gas price.
Similarly, at a fixed natural gas price, pyrolysis has a lower LCOH than
eSMR as a threshold electricity price is reached. The selected eSMR
design point, combined with the baseline techno-economic scenario,
results in an LCOH at the intersection with methane pyrolysis. eSMR
has a lower LCOH than pyrolysis for any higher natural gas price or
lower electricity price.
Fig. 12 directly compares the cost of decarbonization of eSMR with
gas-fired SMR through the CCoA metric. The baseline scenario corre-
sponds to a CCoA of $38/tonCO2 , in line with the carbon tax in certain
jurisdictions [61]. Results show that negative CCoA values are also
well within reach, notably given natural gas price volatility in certain
regions of the world (e.g., European natural gas prices have surpassed
$30/MMBtu in 2021 [62]). Negative values result from 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅
being lower than 𝐿𝐶𝑂𝐻𝑆𝑀𝑅 , indicating that electrification leads to
both lower cost and lower carbon emissions.
The CCoA of eSMR also compares favourably with that of water
electrolysis, which is at approximately $120/tonCO2 . In the baseline
scenario, taking into account direct process emissions and indirect
emissions from the natural gas supply chain, the carbon footprint of
methane pyrolysis is 8.55 kgCO2eq /kgH2 , corresponding to a CCoA of
approximately $10/tonCO2 . Although this makes pyrolysis the hydrogen
production pathway with the lowest decarbonization cost, it does not
show its increased reliance on fossil fuels. For example, due to major
disruptions in the energy supply chain, U.S. natural gas prices have
surpassed $8.5/MMBtu in May 2022 [14]. For combustion-powered
methane pyrolysis, a gas price of $8.5/MMBtu leads to an LCOH of
approximately $2.50/kgH2 and a CCoA of ∼$48/tonCO2 . This contrasts
with electrolysis which, assuming no disruption in the baseline price of
D. Mehanovic et al. Energy Conversion and Management 276 (2023) 116549

Fig. 12. CCoA as a function of electricity and feedstock price at design-point operating conditions (𝑃𝑖𝑛 = 21 bars and 𝑇max = 970 ◦ C).

Table 7 7.2. Alternative studies of eSMR

Absolute and relative LCOH sensitivity to variations in key techno-economic
parameters.
There is currently only a limited amount of knowledge available on
Parameters Baseline Range LCOH Rel. Var. (%) eSMR, especially regarding the techno-economic aspects of the process.
Tube elec. system cost $2.5 k/m [1; 4] [1.49; 1.57] ±2.5 Given that interest for the process is relatively new, recent work has
Tube elec. system life 5 years [3; 10] [1.52; 1.55] ±1.1 rather focused on the demonstration of SMR electrification through
Furnace eff. (grid 1)a 0.95 [0.9; 0.99] [1.52; 1.56] ±1.4
various approaches (e.g., microwave-based heating, induction-based
Furnace eff. (grid 2)b 0.95 [0.9; 0.99] [1.47; 1.54] ±1.8
PSA recovery rate 0.9 [0.85; 0.95] [1.53; 1.55] ±0.7 heating, reactors using structured catalysts, micro-reactors) [29,30,32–
34].
a Baseline electricity price ($0.04/kWh).
b
A recent study from Song et al. [35] however sheds light on the
Off-base electricity price ($0.06/kWh).
techno-economics on two eSMR process versions. The study is based
on reactors incorporating a structured catalyst [32] and assumes that
unconverted species (CH4 , CO) can be recirculated until complete con-
version is attained. The first version (V1) of the process uses resistive
low-carbon electricity, would see its CCoA decrease to ∼$60/tonCO2 . In
heating to pre-heat reactants up to the necessary reformer inlet temper-
the case of eSMR, LCOH would be $2/kgH2 , corresponding to a negative
CCoA value of −$14/tonCO2 . ature, similarly to the present study (Fig. 1b). A second process version
(V2) increases thermal efficiency by integrating a high-temperature
7.1. Sensitivity analysis heat pump and a steam compressor instead of resistive heating. The
LCOH for both process versions is presented with and without CCS,
The techno-economic analysis presented relies on certain assump- which is considered through a CCoA metric ($22/tonsCO2 ). At a natural
tions for both cost and performance parameters. A sensitivity analysis gas price of $10.56/MMBtu and an electricity price of $0.06/kWh,
(Table 7) was therefore completed to quantify the impact of variations the LCOH of the V1 process without CCS is $2.65/kgH2 . At the same
in these key parameters. energy grid cost parameters, the LCOH of the eSMR implementation
Given that only a preliminary design of the eSMR concept is pro- in the present study is $2.50/kgH2 . Both LCOH values are in the same
posed, there is potential for significant variations in tube electrification order of magnitude, but it can be observed that cost sources differ.
expenses (e.g., additional structural or insulation equipment). A relative Results from Song et al. indicate a CAPEX of ∼$0.14/kgH2 , and an
variation of ±60% is considered in the sensitivity analysis. The result is OPEX of ∼$0.85/kgH2 for expenses not related to natural gas and
an almost negligible impact on LCOH, with a variation of ±2.5%. This electricity consumption, compared respectively to $0.416/kgH2 and
shows that major optimization on the integration of the electrification $0.192/kgH2 for the proposed eSMR implementation. This indicates
system would not bear significant cost gains. It also shows that the that Song et al. could be underestimating CAPEX, especially considering
broad conclusions regarding the economic viability of the solution are that their study models a small-scale reformer with an approximate
robust to substantial variations in electrification cost. Variations in the output of 5 tonsH2 /day.
durability of the electrification system have even less impact on LCOH Although the predicted LCOH values are comparable, it should be
(±1.1%), as its useful life is varied from 3 years to 10 years. noted that this study includes more conservative assumptions: (1) pro-
Similarly, variations in the thermal efficiency of electrified reformer cess modelling does not include re-circulation of unconverted species
heating have a small effect on LCOH, even with an efficiency as low that would predict lower LCOH and CO2 footprint, (2) process pressure
as 0.90. After increasing the baseline electricity price to $0.06/kWh, is set above 22 bars to achieve the prescribed recovery rate per refer-
LCOH variation remains below ±2%. The impact of PSA recovery rate is ence from Shi et al. [63], (3) Scope 2 emissions from methane leaks in
also assessed, as it may vary with a change in molar ratios. The change the natural gas supply chain and from electricity generation are con-
in LCOH is below ±1% over the considered range of values. As for the sidered, and (4) process efficiency includes a realistic effectiveness for
cost and durability of the tube electrification system, this shows that heat exchangers. Under these same realistic assumptions, it is expected
the conclusions on the economics of eSMR apply over a broad range that electrified reformer tubes would achieve lower CCoA and LCOH
values in these key input parameters. values than other proposed technologies such as structured catalysts.

13
D. Mehanovic et al.
8. Summary and conclusions
Steam Methane Reforming (SMR) is still the most prominent hy-
drogen production pathway in essential economics sectors, yet existing
SMR plants generate more than ∼10.5 kgCO2 /kgH2 in direct CO2 emis-
sions. The availability and low cost of fossil fuels has led to the com-
modification of hydrogen. Renewable alternatives such as electrolysis
have an H2 production cost of ∼$3/kgH2 in the best cases, significantly
above the $1.26/kgH2 of SMR with feedstock priced at an average
value of spot prices between 2018 and 2020 (i.e., $4/MMBtu). This
is equivalent to a CO2 cost of abatement (CCoA) above $120/tonCO2 ,
assuming that electrolysis is powered by a low-cost and low-carbon
electric grid ($0.04/kWh and 50 gCO2 eq/kWh). Mass adoption of
such cleaner hydrogen production pathways necessitates a substantially
lower decarbonization cost. Methane pyrolysis is considered as a po-
tential solution, reaching relatively low LCOH values, but this pathway
relies even more on carbon-based feedstock to generate hydrogen.
The use of renewable energy as a source of heat for SMR represents
a promising pathway for low-cost partial decarbonization of hydrogen
production. Previous embodiments of the concept have relied on novel
reactor or catalyst designs, which lead to significant technological risk
or increased LCOH.
This work was aimed at assessing a concept for electrified SMR
(eSMR), combining conventional reformer tubes with radiant heating
elements normally applied in high-temperature heating for the micro-
electronics industry. A thermochemical model of the proposed eSMR
system and a techno-economic framework were developed. The study
was based on a model SMR plant of 336 reformer tubes, and used a
retro-fitting approach rather than the design of an entirely new plant.
Process conditions were identified and a rigorous parameter study
was applied to predict potential hydrogen production costs in several
different operation scenarios. The results of the techno-economic model
were ultimately compared with the LCOH of gas-fired SMR, water
electrolysis, and methane pyrolysis.
Results show that operation at lower pressure, which allows high
feedstock conversion, leads to similar costs as high pressure operation
— this allows additional decarbonization without significant added
cost. Specifically, 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 at process design conditions, in the
baseline scenario, is $1.53/kgH2 , corresponding to a CO2 cost of abate-
ment (CCoA) of $38/tonCO2 . The parameter study further identifies the
combinations of energy grid cost parameters (natural gas and electricity
prices) that make 𝐿𝐶𝑂𝐻𝑒𝑆𝑀𝑅 lower than the LCOH of both water elec-
trolysis and methane pyrolysis. A sensitivity analysis demonstrates the
robustness of these conclusions to significant variations in key techno-
economic parameters (e.g., electrification system cost and durability,
electric heating efficiency, etc.).
Future work will be necessary to develop a more detailed design for
reformer tube electrification. A detailed design will also enable a more
accurate prediction of aspects such as retro-fit installation time, which
may affect significantly the short-term economics of the solution. On
the long term, the proposed eSMR process is shown to be a viable path-
way for low-cost decarbonization of hydrogen production, especially in
energy grids where either natural gas or electricity prices are relatively
high. The possibility to retro-fit existing assets also makes eSMR a
highly desirable solution for the energy transition. The electrification
of conventional reformers should therefore be considered as a serious
option in future strategies for hydrogen decarbonization and the energy
transition.
CRediT authorship contribution statement
Dino Mehanovic: Conceptualization, Methodology, Formal analy-
sis, Visualization, Writing – original draft. Alexandre Al-Haiek: Re-
viewing and editing. Philippe Leclerc: Reviewing and editing. David
Rancourt: Supervision. Luc Fréchette: Reviewing. Mathieu Picard:
Conceptualization, Supervision.
14
Energy Conversion and Management 276 (2023) 116549
Declaration of competing interest
The authors declare the following financial interests/personal rela-
tionships which may be considered as potential competing interests:
Dino Mehanovic reports financial support was provided by Natural
Sciences and Engineering Research Council of Canada.
Data availability
Data will be made available on request.
Acknowledgements
This work was supported by the Natural Sciences and Engineering
Research Council of Canada.
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