Energy Conversion and Management 254 (2022) 115245

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Energy Conversion and Management

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

Comparative assessment of blue hydrogen from steam methane reforming,

autothermal reforming, and natural gas decomposition technologies for
natural gas-producing regions
A.O. Oni, K. Anaya, T. Giwa, G. Di Lullo, A. Kumar *
Department of Mechanical Engineering, 10-263 Donadeo Innovation Centre for Engineering, University of Alberta, Edmonton, Alberta T6G 1H9, Canada

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

Keywords: Interest in blue hydrogen production technologies is growing. Some researchers have evaluated the environ­
Blue hydrogen cost mental and/or economic feasibility of producing blue hydrogen, but a holistic assessment is still needed. Many
Carbon capture and storage aspects of hydrogen production have not been investigated. There is very limited information in the literature on
Steam methane reforming
the impact of plant size on production and the extent of carbon capture on the cost and life cycle greenhouse gas
Autothermal reforming
Natural gas decomposition
(GHG) emissions of blue hydrogen production through various production pathways. Detailed uncertainty and
GHG emissions sensitivity analyses have not been included in most of the earlier studies. This study conducts a holistic
comparative cost and life cycle GHG emissions’ footprint assessment of three natural gas-based blue hydrogen
production technologies – steam methane reforming (SMR), autothermal reforming (ATR), and natural gas
decomposition (NGD) to address these research gaps. A hydrogen production plant capacity of 607 tonnes per
day was considered. For SMR, based on the percentage of carbon capture and capture points, we considered two
scenarios, SMR-52% (indicates 52% carbon capture) and SMR-85% (indicates 85% carbon capture). A scale
factor was developed for each technology to understand the hydrogen production cost with a change in pro­
duction plant size. Hydrogen cost is 1.22, 1.23, 2.12, 1.69, 2.36, 1.66, and 2.55 $/kg H2 for SMR, ATR, NGD,
SMR-52%, SMR-85%, ATR with carbon capture and sequestration (ATR-CCS), and NGD with carbon capture and
sequestration (NGD-CCS), respectively. The results indicate that when uncertainty is considered, SMR-52% and
ATR are economically preferable to NGD and SMR-85%. SMR-52% could outperform ATR-CCS when the natural
gas price decreases and the rate of return increases. SMR-85% is the least attractive pathway; however, it could
outperform NGD economically when CO2 transportation cost and natural gas price decrease. Hydrogen storage
cost significantly impacts the hydrogen production cost. SMR-52%, SMR-85%, ATR-CCS, and NGD-CCS have
scale factors of 0.67, 0.68, 0.54, and 0.65, respectively. The hydrogen cost variation with capacity shows that
operating SMR-52% and ATR-CCS above hydrogen capacity of 200 tonnes/day is economically attractive. Blue
hydrogen from autothermal reforming has the lowest life cycle GHG emissions of 3.91 kgCO2eq/kg H2, followed
by blue hydrogen from NGD (4.54 kgCO2eq/kg H2), SMR-85% (6.66 kgCO2eq/kg H2), and SMR-52% (8.20
kgCO2eq/kg H2). The findings of this study are useful for decision-making at various levels.

1. Introduction
With the need for a transition to a low-carbon economy and to reach
net-zero emissions by 2050, the demand for hydrogen production
globally is expected to increase. Global demand for hydrogen is expected
to reach almost $12 trillion by 2050 [1]. This demand will create op­
portunities for countries with large natural gas reserves to export clean
hydrogen. The production of hydrogen for export and use provides an
opportunity for these countries to transition to a low-carbon economy.
Given global energy use and the need to lower GHG emissions, it is

Abbreviations: ATR, Autothermal reforming; ASU, Air separation unit; CAPEX, Capital expenditure; CAD, Canadian dollar; CC, Carbon capture; CCS, Carbon
capture and sequestration; CER, Canada Energy Regulator; CO2, Carbon dioxide; DCFA, Discounted cash flow analysis; FBR, Fluidized bed reactor; GHG, Greenhouse
gas; IRR, Internal rate of return; NGD, Natural gas decarbonisation; OPEX, Operating expenditure; PSA, Pressure swing adsorption; TRL, Technology readiness level;
SMR, Steam methane reforming; WGS, Water-gas shift.
* Corresponding author.
E-mail address: amit.kumar@ualberta.ca (A. Kumar).

https://doi.org/10.1016/j.enconman.2022.115245
Received 20 October 2021; Received in revised form 9 January 2022; Accepted 10 January 2022
Available online 24 January 2022
0196-8904/© 2022 The Authors. Published by Elsevier Ltd. This is an open access article under the CC BY-NC-ND license
(http://creativecommons.org/licenses/by-nc-nd/4.0/).
A.O. Oni et al.
expected that hydrogen will play a key role in the future of energy
systems and the world economy. Hydrogen is an alternative fuel to
traditional fossil fuels like natural gas. It has a relatively high power
density and low carbon emissions when consumed over its life cycle
depending on the production pathways. It can also be blended with
natural gas to meet the fuel demand of various energy systems [2].
However, hydrogen production needs to be environmentally and
economically competitive, and this need has ignited significant research
and development activities. Two studies investigated the economic
feasibility and emissions associated with green hydrogen (hydrogen
from a renewable energy source) production [3,4]. The studies showed
that the emissions from green hydrogen production are relatively low,
but the production cost is not attractive. Another study focuses on green
hydrogen, and a stepwise deployment of green hydrogen technologies is
recommended until they are cost-competitive [5].
There is increasing interest in blue hydrogen. Blue hydrogen is pro­
duced from fossil fuels such that some or nearly all the CO2 emissions
associated with its production are captured and sequestered. There are
many proposed alternative technologies to produce blue hydrogen. But
to produce blue hydrogen with these technologies depends on factors
such as feedstock availability, technology readiness level, and economic
feasibility. These factors are important because they guarantee the
sustainability of blue hydrogen. For example, the availability of feed­
stock in a region to meet market demand is key to sustainable hydrogen
production. Feedstock such as natural gas has been widely explored for
the production of grey hydrogen (hydrogen produced without capturing
and sequestering the CO2 emitted during operation). Natural gas has a
high percentage volume of methane, which is a reliable source of
hydrogen. Its availability poses little or no challenges to hydrogen
production in the jurisdictions around the world where it is in abun­
dance including the USA and Canada. The production of natural gas in
these countries significantly impacts global use [6]. Together the two
countries had 512 trillion cubic feet (Tcf) of proven reserves of natural
gas at the beginning of 2019 [6], and they are well positioned to lead
blue hydrogen production globally. In Alberta (a western province in
Canada), the production of natural gas continues to increase. An average
of 280 million cubic feet was produced per day between 2019 and 2020
[7].
In terms of technology readiness level, the production of hydrogen
from natural gas is not new. Steam methane reforming (SMR) is a mature
technology that has been used for hydrogen production for decades. This
technology uses natural gas and steam to produce grey hydrogen and is
responsible for 48% of the hydrogen produced globally [8,9]. SMR can
handle large capacities in the range of 130,000–300,000 tonnes/year
and these capacities are commercially available [10]. Furthermore,
50%-92% of CO2 in a SMR plant can be captured [11,12].
Interest in autothermal reforming (ATR) and natural gas decarbon­
ization (NGD) for blue hydrogen production is also growing. These
technologies may become part of the future energy portfolio of hydrogen
production technologies. The concept behind these technologies is not
new. Their applications are found in some industrial processes [13]. For
ATR, the most notable commercial applications are oxygen-blown units
for methanol production and air-blown units for ammonia production
using natural gas. Hydrogen is produced along with syngas from these
processes. The produced syngas composition is favorable for hydrogen
production. NGD, on the other hand, has been known to produce carbon
black as early as the 1920s. Hydrocarbon such as natural gas is thermally
decomposed into carbon and hydrogen. The produced gases, which
contain hydrogen, are combusted to supply heat for the process [14].
The success of NGD is its reactor, other process units involved are well
established. The main challenge with the thermal decomposition process
is related to the removal of the carbon produced. Reactor fouling and
clogging have been reported [15,16], and catalyst deactivation is the
major challenge in the catalytic approach [17,18]. Pocock et al. pro­
posed a low-cost iron ore catalyst in a fluidized bed to circumvent these
challenges [19]. Although the technology readiness level of NGD is
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Energy Conversion and Management 254 (2022) 115245
lower than that of ATR and SMR, some studies have suggested that it can
significantly reduce carbon emissions.
Countries such as Canada have the resources to both explore this
opportunity and meet their greenhouse gas (GHG) emissions targets. For
Canada to meet its 2050 net-zero emissions target, clean hydrogen must
make up about 31% of its energy sector demand [20]. This demand is
equivalent to 20 Mt of hydrogen per year in 2050 [20]. For these rea­
sons, the Canadian government is looking to produce clean hydrogen on
a large scale. Canada produces about 3 million tonnes of hydrogen
yearly through the steam methane reforming of natural gas (without
carbon capture and sequestration [CCS]) [21]. Most of Canada’s
hydrogen is produced and consumed in western Canada. Alberta, a
province in western Canada, consumes the largest share of the hydrogen
produced in Canada, about 61% [22]. Currently, Alberta’s hydrogen is
mostly used for industrial processes such as oil refining, upgraders,
ammonia production, and other industrial sectors. The demand for
hydrogen in Alberta is expected to grow dramatically because of the
province’s ability to transform its energy sector into a low-carbon one.
More importantly, Alberta is a low-cost producer of natural gas (the
most common feedstock for hydrogen production) and is strategically
positioned to use its globally recognized experience in natural gas
extraction and transmission, hydrogen production, and CCS to achieve
the required economies of scale for low-carbon hydrogen production.
Alberta has the resources, technologies, and infrastructure to capture,
transport, and sequester CO2 produced in natural gas-based hydrogen
production pathways. The Alberta Carbon Trunk Line, for example, is
designed to capture, transport, and sequester 14.6 million tonnes of CO2
per year [23]. Alberta also has the capacity and infrastructure to export
blue hydrogen to different jurisdictions around the world [24]. For these
reasons, in this study, Alberta is used as a case study.
Carbon capture and sequestration is critical for the production of
blue hydrogen. Although the feasibility of CCS has been proven, its
integration into industrial processes is yet to be widely accepted. Only a
few CCS plants have been implemented around the world. In 2013, the
Global CCS Institute reported that eight large-scale CCS projects were in
operation globally and nine were under construction [25,26]. Recently,
Alberta invested in two commercial-scale CCS plants capable of reducing
GHG emissions in the oil sands and fertilizer sectors by 2.76 million
tonnes per year [27]. The existing CCS plants and geographical location
make Alberta an attractive jurisdiction for blue hydrogen. Despite these
signs of progress, there are economic concerns that need to be addressed
before integrating CCS to produce blue hydrogen at a large scale to meet
current or future demand. It is important to note that CCS is relatively
capital-intensive and requires energy for operations [28]. For large ca­
pacities, hydrogen storage is an important factor to realize the full po­
tential of hydrogen production and is expensive [29]. Therefore,
determining the optimum plant capacity for blue hydrogen production is
essential. These aspects of the economic evaluation have been ignored in
the literature. This study aims to address these gaps.
Many studies have provided useful information comparing various
types of hydrogen technology based on cost or/and life cycle GHG
emissions. Okonkwo et al. reviewed the potential for carbon-free
hydrogen production, use, and exportation based on technical, eco­
nomic, and environmental criteria [30]. Their findings revealed that the
production and exportation of blue ammonia is the preferred pathway,
and green hydrogen is expected to become as competitive as blue
ammonia in the mid-future. Haider et al. assessed the economic feasi­
bility of blue hydrogen from steam methane reforming. Their results
showed that hydrogen production costs are dominated by natural gas
and the extra capital required for carbon capture and storage [31].
Simbeck and Chang assessed the economic feasibility of fossil fuel- and
renewable-based hydrogen technologies [32]. They showed that SMR
produces less expensive hydrogen than other fossil fuel- and renewable-
based technologies. They also suggested that mandating CO2 trading or
capturing it for enhanced oil recovery could improve the blue hydrogen
economy. In a similar study, Lenger et al. evaluated the economic
A.O. Oni et al.
feasibility of hydrogen produced from SMR, coal and biomass gasifica­
tion, and water electrolysis [33]. The SMR technology is the most
competitive, with an estimated hydrogen cost of 1.3 and 1.5 $/kg H2,
with and without a carbon capture (CC), respectively. However,
compared to some other blue hydrogen technologies, blue hydrogen
from SMR may be less attractive in terms of cost and emissions. Salkuyeh
et al., for example, compared the costs and life cycle GHG emissions of
four natural gas-based hydrogen technologies: SMR, ATR, syngas
chemical looping, and chemical looping reforming [34]. The authors
showed that adding CC decreases the efficiency of the SMR and ATR
processes by 18% and 2%, respectively, while increasing the corre­
sponding hydrogen cost by 1.10 and 0.44 $/kg H2. In contrast to the
findings by Simbeck and Chang and Lenger et al., adding CC to a SMR
plant is not economically competitive. Timmerberg et al. compared the
GHG emissions and economic performance of hydrogen produced from
methane decomposition in three configurations (plasma, molten metal,
and thermal gas) with SMR with and without CC [35]. Their results
showed that the methane decomposition systems lower GHG emissions
compared to SMR, but emissions are similar when a CC is added to SMR.
However, the cost of hydrogen from the methane decomposition systems
(1.6 to 2.2 €/kg H2) is higher than from SMR (1.0 to 1.2 €/kg H2). Keipi
et al. compared only the economic feasibility of hydrogen produced by
the thermal decomposition of methane with SMR with and without CC
[14]. The results showed that the methane decomposition system is
economically competitive with SMR when the price of product carbon is
at least 280–310 €/tonne.
Howarth and Jacobson [36] compared SMR blue hydrogen to natural
gas and concluded that blue hydrogen had larger emissions than natural
gas. However, their work only investigated current SMR facilities with
relatively low CC rates and assumed higher than average fugitive
methane emissions. The authors claim that fugitive emissions have been
underestimated, which aligns with recent studies suggesting methane
emissions are 1.5 to 2.2x higher than current Canadian and US estimates
[37–40]. However, methane regulations have reduced emissions by 9%
(2014 to 2019) in Canada [41], and 2020 regulations aim to reduce
methane fugitives by 45% by 2025 [42]. In addition, the global warming
potential considered is debatable, as the assumed values show one
extreme and result in higher GHG emissions from blue hydrogen. The
present study aims to address these gaps.
While many studies have provided significant insights into blue
hydrogen production, several crucial aspects have been ignored, such as
the variabilities in economic parameters, the impact of carbon pricing
on cost, determining optimum plant size, and the impact of storage ca­
pacity on hydrogen cost. Several of these aspects have not been inves­
tigated. For instance, economic data are usually based on several
assumptions with wide variability. Therefore, using point estimates
when comparing the cost-effectiveness of projects can be misleading.
One way to examine the impact of variations on plant performance is to
conduct a comprehensive uncertainty analysis. Comparing the uncer­
tainty in the desired outputs helps to determine the most preferable
alternative.
Another issue is the limited focus on the impact of carbon price on
hydrogen production cost. Investigating the impact of carbon price
provides insights into the benefits of decarbonization options, the eco­
nomic impact of carbon reduction options, and the potential gaps in
carbon price policies. For these reasons, a carbon price estimate is
relevant for assessing the external costs reducing emissions and as a tool
for economic decision making and policy formulation. Salkuyeh et al.
examined the impact of carbon prices on grey hydrogen using blue
hydrogen as a benchmark [34]. The impact of carbon pricing on the
direct emissions from blue hydrogen technologies was not considered.
Since the direct GHG emissions from blue hydrogen technologies may
differ, the impact of carbon price on emission should be investigated.
But thus far no study has considered the holistic economic and GHG
emissions impacts of blue hydrogen production including these crucial
points.
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Energy Conversion and Management 254 (2022) 115245
A robust comparative assessment should include the entire life cycle
stages of products/technologies. Most of the system boundaries
considered in the blue hydrogen studies do not include hydrogen storage
nor, in some cases, CO2 transportation and sequestration. Hydrogen
storage is an important enabler for the advancement of large-scale
hydrogen production. For this reason, it is important to understand
how storage cost impacts the hydrogen production cost. Such informa­
tion is crucial for the hydrogen supply chain, including transportation,
distribution, and uses/meeting demands. More importantly, under­
standing how the added emissions, because of hydrogen compressions,
impact the overall life cycle GHG emissions is crucial to compare these
technologies. Lastly, none of these studies developed a scale factor for
blue hydrogen production technologies, which is critical for determining
the optimum scale of the production plant. The scale factor helps to
identify the link between the size of a production plant and the variation
in the capital cost. The inclusion of hydrogen storage (which has long
been ignored in previous work) in the evaluation of scale factors for blue
hydrogen technologies provides information on the benefits of econo­
mies of scale and enables business decisions on plant size.
Determining a sustainable hydrogen production technology is crit­
ical to the growing interest in blue hydrogen. Factors such as compre­
hensive analyses on the economic variabilities, the impact of carbon
pricing, optimum plant size, and storage cost are crucial to under­
standing the environmental and economic sustainability of the potential
blue hydrogen technology. These factors are the missing links in the
earlier works, and their inclusion in a comparative assessment of blue
hydrogen technologies will help identify the most favorable. More
importantly, there has been no large-scale development or commer­
cialization of hydrogen production from NGD. Despite the benefits
associated with the breakdown of hydrocarbons into solid carbon and
hydrogen, the fuel required for thermal decomposition and the rela­
tively large volume of feedstock (natural gas) needed for large-scale
production could pose major challenges for NGD. Therefore, a
comprehensive comparative analysis of blue hydrogen from NGD, SMR,
and ATR is needed. These technologies have begun to gain research,
investors, and government interest because of their potential to mitigate
emissions. Hence, any research thrust that would fill these gaps is in high
demand.
In this study, we conducted holistic techno-economic and GHG
emissions analyses of SMR-CCS, ATR-CCS, and NGD-CCS to address the
gap in the literature. To the best of our knowledge, this is the first
comparative assessment that examines the economic and GHG impacts
of SMR-CCS, ATR-CCS, and NGD-CCS technologies.
The specific objectives of this study are to:
• Develop process models focussed on mass and energy balances for
SMR-CCS, ATR-CCS, and NGD-CCS technologies;
• Develop techno-economic models for SMR-CCS, ATR-CCS, and NGD-
CCS technologies to determine hydrogen production costs;
• Evaluate the life cycle GHG emissions (kg of CO2 emitted/kg of H2
produced) of hydrogen production from each technology;
• Develop a scale factor for each technology to understand the impact
of plant size on the cost of hydrogen;
• Conduct sensitivity and uncertainty analyses of various input pa­
rameters to determine their effect on the cost of production of
hydrogen;
• Conduct a case study for Alberta, a western province in Canada, and
an example of jurisdiction with an abundance of natural gas and CCS
opportunities.
2. Methods
2.1. Process description
In this section, we describe the operation of SMR, ATR, and NGD.
Fig. 1 shows an overview of the hydrogen production processes. Each
A.O. Oni et al.
Natural gas-
based
technology
84 km CO2
pipeline
transport
CO2
sequestration
Fig. 1. An overview of hydrogen-based technology.
process includes hydrogen production units, carbon capture, CO2
transportation, sequestration, and hydrogen storage. Upstream material
and energy are also included to indicate sources of feedstock, fuel, and
electricity. The production capacity of each technology is 607 tonnes of
hydrogen per day. This capacity is typical of existing large-scale SMR
plants at bitumen upgraders in Alberta, Canada [10]. In each technol­
ogy, CCS is coupled to points where CO2 emissions are released to the
environment. For the ATR and NGD configurations, one CO2 capture
point is considered. In SMR, GHG emissions from the reformer’s furnace
and the CO2 emissions leaving the amine unit are captured.
2.1.1. Steam methane reforming
The process flow diagram (Fig. 2) shows a reforming reactor, water
shift reactors (WGS, high-temperature (HT) and low-temperature (LT)),
syngas purification, CO2 compression, transportation, sequestration,
and hydrogen storage. First, we discuss the case with carbon capture and
Fig. 2. Simplified process flow diagram of steam methane reforming with carbon capture and storage (SMR-CCS).
4
Energy Conversion and Management 254 (2022) 115245
Storage
storage. In the reforming reactor, natural gas reacts with steam at high
pressure to produce syngas (a mixture of hydrogen and carbon monox­
ide). The reaction takes place in the presence of nickel-based catalysts,
thus producing carbon monoxide and hydrogen-rich syngas. The syngas
is cooled and fed into the water–gas shift (WGS) reactors, where the
carbon monoxide is converted to carbon dioxide and hydrogen through
the addition of steam. The HT and LT WGS reactors are arranged in
series with Fe2O3-Cr2O3 and CuO/ZnO/Al2O3 catalysts, respectively.
The hydrogen produced is purified in the syngas purification unit (amine
unit). It is then pressurized and stored in the storage tanks. CO2 emis­
sions from the syngas purification unit are compressed and transported
through a pipeline to an underground cavern. For the case without CCS,
the syngas from the WGS reactors is directly sent to the syngas purifi­
cation/pressure swing adsorption (PSA) unit after cooling. CO2 pro­
duced is released directly into the atmosphere.
A.O. Oni et al.
2.1.2. Autothermal reforming of methane
The process flow diagram in Fig. 3 shows an autothermal reactor, HT
and LT WGS reactors, syngas purification, CO2 compression, trans­
portation, sequestration, hydrogen storage, and an air separation unit
(ASU). First, we discuss the case with carbon capture and storage. Ox­
ygen (produced in the ASU), steam, and methane react over a nickel
catalyst in an ATR reactor to produce syngas. The reactions of these feed
streams cause reforming and oxidation to occur simultaneously. The
partial oxidation reaction provides the heat needed for the endothermic
reforming reaction. The steam and methane are preheated and then
heated again in a furnace on entering the ATR reactor. The produced
syngas contains hydrogen, carbon dioxide, steam, and some trace gases.
It is cooled to the temperature required for water-gas shift reactions to
occur. In the water-gas shift reactors, carbon oxide reacts with steam
over an iron and chromium catalyst to produce hydrogen and carbon
dioxide. The shifted gas is sent to the syngas purification (amine unit),
where carbon oxide is separated from the hydrogen-rich gas. The
separated carbon oxide is compressed and stored while the hydrogen-
rich gas, containing unconverted carbon oxide, argon, and some trace
gases, is sent to the pressure swing adsorption unit (PSA). In the PSA,
90% of the hydrogen is assumed to be recovered at a purity of 99.9%,
while the remaining gases (fuel gases) are used as fuel in the boiler/
furnace. For the case without CCS, the effluents from the WGS reactors
are sent directly to the PSA unit after cooling and water separation. The
CO2 produced is released directly into the atmosphere.
2.1.3. Natural gas decomposition
Fig. 4 is the process diagram that defines the scope and boundary of
our modeling for the NGD pathway. As shown, natural gas is fed into the
thermal decomposition unit, where it decomposes into hydrogen and
carbon. The thermal decomposition reaction is endothermic and,
without catalysis, the reaction requires a high temperature (above
1000 ◦ C) to achieve reasonable reaction rates [15,43]. At such a tem­
perature, metallurgical limitations are likely to increase costs. The use of
catalysts allows the process to operate at temperatures around 800 ◦ C.
Various catalysts in metallic or carbonaceous forms can be used [44]. An
iron ore catalyst was assumed in our process modeling. It has been re­
ported that iron ore can catalyze the process and produce graphitic
carbon as by-product carbon [19]. A fluidized bed reactor (FBR) with an
internal cyclone is used; it helps separate the solid carbon from the
Fig. 3. Simplified process flow diagram of autothermal reforming with a carbon capture and storage (ATR-CCS) plant.
5
Energy Conversion and Management 254 (2022) 115245
produced hydrogen and unconverted natural gas. When the carbon is
removed, the hydrogen and natural gas exiting the cyclones and filters
are pressurized and cooled to ambient temperature before entering a
PSA unit, where the unconverted natural gas is trapped and pure
hydrogen is produced. In the PSA, 90% of the hydrogen is assumed to be
recovered at a purity of 99.9%, while the remaining gases are recycled to
the fluidized bed reactor. The heat required by the thermal decompo­
sition process is supplied by burning natural gas. The CO2 emissions
from the burning of natural gas are captured through the carbon capture
unit. The captured CO2 is later transported and stored underground.
2.2. Process simulation
Process simulations of the natural gas-based hydrogen technologies
considered in this study were developed in Aspen HYSYS [45]. Peng-
Robinson, ASME steam, and acid gas chemical solvents equations of
state were used to predict thermodynamic performances of hydrocar­
bons and syngas, steam, and amine solvent, respectively. The reactors in
each technology were modeled using the Aspen HYSYS equilibrium
reactor. The chemical reactions that occur in each reactor and their
corresponding kinetic parameters were taken from the literature. There
are many reactions involving natural gas in the steam-methane
reformer, autothermal reactor, and NGD. These reactions are pre­
sented in Equations S1-S11 in the supplementary information (SI).
2.3. Evaluation of energy consumption
We developed a detailed process model using Aspen HYSYS [45] to
obtain material and energy balances for each unit operation involved in
the production process. We used the resulting energy and material
balances to determine the energy consumed and equipment sizes. The
energy inputs for electrical devices were obtained from the simulation
models using the appropriate efficiencies. The fuel consumed by the
heaters was evaluated using Equations (1) and (2).
Q̇stream = ṁstream Δh (1)
Δh is the enthalpy change in the stream:
Q̇stream
ṁfuel = (2)
LHV × ηb
A.O. Oni et al. Energy Conversion and Management 254 (2022) 115245

Transportation CO2
CO2
capture
sequestration
Flue gas Feedstock:
Natural gas
Heat Heat
recovery recovery
Natural gas

Recycled

Syngas
Flue gas gases

Cyclones Pressure swing

Fluidized bed
Catalyst reactor adsorption
Fuel Syngas

Hydrogen
Fuel: Carbon & catalyst
Natural gas

Hydrogen
storage

Fig. 4. Simplified process flow diagram of the thermal decomposition of natural gas in a carbon capture and storage (NGD-CCS) plant.

applying economic factors to account for the costs associated with

where ṁfuel is the mass flow of the fuel, Q̇stream (kW) is the heat duty of the
bringing the equipment into service. Peters et al. [52] suggested that a
process stream, LHV is the lower heating value of the fuel (kJ/kg), and ηb
302% overall installation factor is more appropriate than software-
is the thermal efficiency of the heaters.
derived installation factors. The method used to estimate the capital
cost, as used by Peters et al. [52] and Swanson et al. [53], is given in
2.4. Evaluation of GHG emissions Table 1. The total purchased equipment costs (TPEC) are estimated from
Aspen Icarus, and the total installed cost (TIC) and indirect costs (IC)
Life cycle GHG emissions were evaluated through a life cycle were determined using installation factors of 302% and 89%, respec­
assessment (LCA) framework according to the International Organiza­ tively. The total indirect costs (TDIC) were then estimated. Project
tion for Standardization (ISO) recommendations [46,47]. One kg of the contingency is included as 20% of the direct and indirect cost, which is
produced hydrogen is considered the functional unit to which the GHG the sum of the TIC and the IC. A location factor of 10% was included in
footprint as kilograms of CO2-equivalent gas emitted (kg CO2e) is the capital cost estimate.
normalized. For natural gas, we considered both combustion and up­ OPEX consists of utilities, raw material, labor, maintenance, and
stream emissions. The 5-year average of Alberta natural gas recovery, general and administrative costs. For the economic analysis, plant life
processing, transmission, and distribution emissions is 8.88 kg-CO2eq/ and capacity use were assumed to be 25 years and 90%. All other
GJ of natural gas produced [48,49]. The natural gas combustion emis­ assumed values for the economic analysis are listed in Table 1,
sions factor was taken as 55.78 kgCO2eq/GJ [50]. Electricity is assumed Table 2, and Table 3.
to be from the Alberta electricity grid. The Alberta grid electricity GHG All costs were adjusted to the 2020 Canadian dollar (CAD). For each
emission factor was taken as 544 g CO2eq/kWh based on the modeling technology, a common set of assumptions was made regarding the cost
done by Davis et al. [50]. of energy resources and GHG emissions factors. The Alberta reference
price of natural gas was considered to be $1.96/GJ (2016-20 Canada
2.5. Techno-economic assessment
Table 1
The cost of equipment such as pumps, compressors, heat exchangers, Assumptions for the calculation of the total capital cost.
and so on was evaluated using the developed process model. The cost of
CAPEX component Factor
the reformers, WGS, fluidized bed reactor (FBR), and PSA was estimated
from work by Mohajerani et al. using an appropriate economic model Total purchase equipment cost (TPEC) Obtained from equipment sizing
Total installed cost (TIC) 302 % of TPEC
and scale factor [51]. The hydrogen cost for all the technologies assessed
Indirect cost (IC) 89% of TPEC
was estimated using a discounted cash flow analysis (DCFA) model and Total indirect cost (TDIC) TIC + IC
based on an internal rate of return. The DCFA model takes input from Contingency 20% of TDIC
three categories: capital expenditure (CAPEX), operating expenditure Fixed capital investment (FCI) TDIC + contingency
(OPEX), and economic and other technical assumptions. Estimating Location factor (LF) 10% of FCI
Total capital investment FCI + LF
CAPEX involves determining the equipment purchase costs and then

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Table 2
Assumptions used to calculate the operating cost.
Operating cost Specification

Fixed costs
Labor cost Based on the number and nature of pieces of
equipment in the flowsheet.
Non-fuel operating and 4% of TPC [30]
maintenance
Insurance 2% of TPC [31]
Administrative and support 25% of labor cost [31]
labor

Variable cost
Utility cost Based on the electricity, fuel, steam, and cooling
water consumption.
Raw material cost Based on the feedstock materials and make-up
requirements.

Table 3
Assumptions for the economic model.
Parameter Specification

Base year and currency 2020 CAD

Capacity use 90%
Internal rate of return (IRR) 10%-15%
Plant lifetime 25 years

Construction payment years 3

• Year 1 10%
• Year 2 55%
• Year 3 35%

Energy Regulator [CER] price averages) and electricity prices were

considered to be $16.14/GJ (2016-20 CER price averages) [54].

2.5.1. Evaluation of CO2 transportation, sequestration, and hydrogen

storage cost
A case study for Alberta, a western province in Canada, was con­
ducted. Alberta is a major natural gas-producing region in North
America. The distance for CO2 transport to the sequestration site was
assumed to be approximately 84 km in the natural gas-based pathways
requiring the integration of CCS. The 84 km was chosen simply to have a
consistent assumption for each technology for a reasonable comparison
and is also the approximate transportation distance between the
hydrogen production plant in Fort Saskatchewan and sequestration in
Thorhild, Alberta. Fig. 5 shows these locations. This distance is not fixed;
it is used to provide a value considered as a likely distance.
We calculated the capital cost of the CO2 pipeline and sequestration
based on the estimate by Olateju and Kumar [55]. In their study, 4406
tonnes of CO2 per day was assumed to be transported through an 84 km
pipeline from Fort Saskatchewan to Thorhild. Olateju and Kumar re­
ported C$69 million each for the capital costs of the CO2 pipeline and
CO2 sequestration. These costs were corrected in time using the chem­
ical engineering plant cost index (CEPCI) from the base year 2013 to the
year 2020. Using a capacity factor cost exponent of 0.6 and CO2 ca­
pacity, we estimated the capital cost required for each hydrogen pro­
duction pathway. The cost of compressors and pumps needed for
transportation were estimated using Aspen Icarus.
Hydrogen needs to be stored to deal with fluctuations in demand and
supply. Hydrogen can be stored in aboveground tanks or belowground
salt caverns. Aboveground tank capital costs are between $135 and
$345/kg of H2 capacity [56], while underground salt caverns only cost
$2 to $13/kg of H2 capacity [56,57]. Therefore, we assumed that only
0.5 days of hydrogen is stored in aboveground tanks on-site, while
cheaper salt caverns are used for longer term storage. The salt caverns
can be located off-site and may be shared between several production
facilities. Aboveground storage tank capital cost, S, was calculated using
the following correlation derived from Tzimas et al. [56]:
Fig. 5. An overview map of the compressed CO2 transportation to the
sequestration site.
S = 10− 0.2581*(log10 C)+6.0391
*A*I*C (3)
C is the hydrogen storage capacity in tonnes, C is equal to the plant
capacity in tonnes per day, multiplied by the storage days. A is the
conversion of USD to CAD, 1.32. I is the inflation from 2004 to 2020,
1.3036 [58]. The tank capital costs include the purchase of the tank but
not the installation. An installation factor of 0.65 is assumed. While
underground salt cavern storage is cheaper, caverns can only be built in
areas with appropriate geology. Additionally, large-scale storage in salt
caverns is part of the transportation and distribution system, which is
shared by several producers and consumers. The 0.5-day on-site storage
allows the production facility to test the product purity before export
and handle small fluctuations in production volumes.
2.5.2. Sensitivity and uncertainty
We investigated input parameters that could impact the cost of blue
hydrogen from SMR, ATR-CCS, and NGD-CCS using the Morris method.
The Morris method assesses the elementary effects produced by changes
in the input parameters at various sample points. The Morris standard
deviation is plotted against the Morris mean to identify influential and
non-influential inputs. In the Morris plot (standard deviation against
mean), less sensitive parameters fall in the lower left corner, and sen­
sitive parameters are in the upper right corner. Furthermore, an increase
in Morris’s standard deviation and mean may indicate parameters are
influential and interactive. In this study, the Regression, Uncertainty,
and Sensitivity Tool (RUST) was used to conduct sensitivity and un­
certainty analyses [59]. The details on these methods can be found in an
earlier publication [44]. The parameters considered for sensitivity
analysis and their upper and lower limits are presented in Table 4.

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Table 4 Table 5
Range of parameters used in the sensitivity analysis. Natural gas and electricity consumption in hydrogen production from different
Parameter Minimum Maximum
technologies at a plant capacity of 607 tonnes/day.
Grey hydrogen Blue hydrogen
Electricity price ($/GJ) 15 40
Natural gas price ($/GJ) 1 10 Items SMR ATR NGD SMR- SMR- ATR- NGD-
Labor cost ($) − 30% +30% 52% 85% CCS CCS
Capacity use (%) 80% 100%
Internal rate of return (%) 5% 20% NG feedstock 0.12 0.15 0.18 0.12 0.12 0.15 0.18
H2 storage duration (days) 0 7 (GJ/kg H2)
Capital-intensive units ($) − 30% +30% NG fuel (GJ/ 0.06 0.00 0.03 0.10 0.13 0.00 0.03
CO2 capture cost ($) − 30% +30% kg H2)
CO2 transportation length (km) 25 225 Electricity 0.96 2.35 2.23 1.32 4.42 3.59 3.07
CO2 sequestration cost ($) − 30% +30% (kWh/kg
PSA, reformer, ASU, FBR ($) − 30% +30% H2)
NG as 65.46 94.85 82.68 53.44 45.24 92.35 81.59
feedstock
(%)
3. Results and discussion
NG as fuel 32.73 0.01 13.78 44.53 49.01 0.01 13.60
(%)
We considered cases without CCS to provide insight into energy use, Electricity 1.81 5.14 3.54 2.03 5.76 7.64 4.81
production cost, and life cycle GHG emissions of blue hydrogen tech­ (%)
nologies. In a typical SMR, CO2 can be captured from shifted syngas, PSA *NG: Natural gas.
tail gas, and SMR flue gas [60,61]. When the PSA tail gas is sent to the
reforming furnace for combustion, CO2 emissions can be captured from pattern for each technology. Natural gas and electricity are the main
two possible locations: from the purification unit (the CO2 due to the sources of energy for the technologies, both with and without CCS.
chemical reactions occurring in the reactors) and the reforming furnace When these energy use data are converted to a similar base unit of GJ,
(the CO2 released because of combustion). To capture a significant the percentage of electricity used is less than 8% in all technologies.
portion of the CO2 emissions from SMR, two carbon units may be Natural gas is consumed as feedstock and fuel. Its percentage con­
required: one at the reactor (purification unit) and the other at the sumption as feedstock is over 50% except in SMR-85%, where 49% is
reforming furnace. The variation in carbon capture rate depends on used as fuel (Table 5).
many factors, such as heat integrations of the process, the efficiency of SMR-85% consumes the most natural gas per kg of H2 produced. It
the capture unit, the regenerator of the capture unit also requires heat also consumes more natural gas as fuel than the other technologies per
for reboiling, which adds to the overall emissions. Note that the kg of H2 produced. The consumption is high because more natural gas is
reforming furnace can provide heat for the amine re-boiler (re­ needed to generate low-pressure steam for the amine regenerators. It is
generators). For SMR, capturing the CO2 emissions through the amine important to note that in a situation where low-grade heat is available to
unit leads to a 52% capture rate. We refer to this case as SMR-52%. generate steam, both the natural gas consumption and the associated
When the CO2 emissions from the reformer’s flue gas are included, the GHG emissions can be reduced. For example, in refineries and bitumen
overall capture rate increases to 85%. We refer to this case as SMR-85%. upgraders, it is common practice to recover and use low-grade heat
Collodi et al. demonstrated SMR capture rates ranging from 53% to 90% where they are needed. NGD consumes a high amount of natural gas as
[60]. Their results are in close agreement with the findings of this study. feedstock per unit of H2 produced but uses relatively little as fuel. The
Capturing CO2 emissions from the ATR leads to a 91% capture rate, and high natural gas consumption as feedstock is expected because NGD
capturing CO2 emissions from the NGD leads to a 61% capture rate. For sources hydrogen only from the gas, thus leading to high natural gas
NGD, this includes only the GHG emissions and not the solid carbon consumption. SMR and ATR source hydrogen from both steam and
portion. The rate of carbon capture depends on many factors such as the natural gas, which allows them to lower the amount of natural gas
efficiency of the capture unit, natural gas composition, process condi­ consumed as feedstock per unit of H2 produced. In SMR without CCS,
tions, plant configuration, and other factors. These factors can lead to recovered gases from the PSA unit are used as fuel in the reformer’s
the differences in carbon capture rate found in studies. In this study, the furnace. These gases, a mixture of hydrogen, hydrocarbons, CO2, and
grey hydrogen technologies are SMR, ATR, and NGD, and the blue other gases, help lower natural gas consumption. ATR consumes the
hydrogen technologies are SMR-52%, SMR-85%, ATR-CCS, and NGD- least fuel (natural gas) per unit of H2 produced. The heat recovered from
CCS. the autothermal reactor significantly lowers fuel requirements. But ATR
requires more natural gas as feedstock than SMR per unit of H2 produced
because it has a relatively lower hydrogen-to-carbon ratio. One advan­
3.1. Energy analysis
tage of ATR is that the heat of combustion in the reactor raises the
temperature and quality of the heat produced for recovery and
The steam-to-natural gas ratio is an important input parameter in
reforming reactions. Since most CO2 emissions are from the reactors and
both SMR and ATR. In ATR, oxygen flow is another parameter necessary
released through the purification unit, using a single CCS unit is suffi­
for the combined partial oxidation and reforming. The reactions
cient to capture a significant amount of emissions. SMR, on the other
improve heat and temperature management. These parameters deter­
hand, requires at least two CCS units, which capture up to 90% of the
mine material input, fuel consumed by the processes, and the yield of
overall on-site emissions. The volumes of flue gas and CO2 gases from
hydrogen produced. Steam-to-natural gas molar ratios of 5 and 1.7 are
the reformer’s furnace and purification unit, respectively, are relatively
required to produce 607 tonnes/day of hydrogen through SMR and ATR
large. NGD requires a relatively small CCS unit; however, the unused
(with and without CCS), respectively. An oxygen-to-natural gas molar
solid carbon must be sequestered.
ratio of 0.59 is required in the autothermal reactor. A typical SMR plant
With respect to electricity use by these technologies, cases without
can operate with a steam-to-natural gas ratio of 3–6 [62] and an ATR
CCS consume less electrical energy than those with CCS. SMR without
plant with 1.1–3 [63]. Table A4 (in the SI) presents material inputs for
CCS consumes the least electricity and SMR-85% the most. Of the total
each process. The process conditions for the units in each technology are
electrical energy used by the two CCS units in SMR-85%, the second CCS
presented in Tables A5-A7. The energy analyses of the natural gas-based
unit (coupled to the reformer’s furnace) accounts for over 70%. Elec­
hydrogen technologies provide useful information on the type of energy
tricity consumption is high because a large volume of flue gases leaving
used and its consumption. Table 5 presents the energy consumption

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the reformer’s furnace is compressed at a high compression ratio. A
three-stage compression with 2.66 kWh/kg H2 is needed to compress
flue gases from 0.12 MPa to 3.6 MPa. The compression ratio of flue gas in
NGD-CCS is also high, from 0.12 MPa to 3.6 MPa. However, electricity
consumption is low because the volume flow of flue gases is much lower.
The situation is different for ATR-CCS and SMR-52%. Electricity con­
sumption is lower because the compression ratio of syngas from the WGS
units and separators to the amine unit is less than 2. The reactors in both
systems (ATR and SMR) operate at high pressure, so less compression
power is needed to transport syngas to the amine unit. For cases without
CCS, the electrical energy consumed in ATR and NGD is higher than in
SMR by 57.1% and 59.1%, respectively. In SMR and NGD without CCS,
syngas compression to the PSA unit and hydrogen compression to the
storage account for 88% and 95% of the overall electrical energy use,
respectively. In ATR without CCS, electricity consumed by the ASU
(compression of air) accounts for 62% of the overall use.
3.2. GHG emissions
The GHG emissions for each technology are listed in Table 6. The
highest and lowest emissions are from SMR without CCS and ATR with
CCS, respectively. On-site emissions are due to the combustion of nat­
ural gas as fuel. For cases without CCS, on-site emissions from SMR,
ATR, and NGD account for 80.8%, 76.2%, and 37.6% of the overall
carbon emissions, respectively. NGD lowers on-site emissions substan­
tially compared to the others. The NGD technology produces 1804
tonnes of carbon to lower its overall emissions significantly. If part of the
product carbon (558.4 tonnes of carbon) generates heat in the NGD
reactor, the on-site emissions will increase by 1.53 kgCO2/kg H2 (about
83.1% increase). NGD’s overall emissions will still be lower than other
technology (without CCS) using the carbon product as a fuel source. The
high electricity emissions in ATR are partly due to its consumption in the
ASU. The ASU uses cryogenic air separation technology to produce ox­
ygen. This separation method is energy-intensive, with electricity being
the major energy input. On the other hand, the high electricity emissions
in NGD can partly be explained by the high compression required to
transport syngas to PSA. The NGD reactor produces hydrogen at rela­
tively low pressure (101 kPa). Compressing these gases is energy-
intensive. Estimates are about ~2.2 kWh/kg H2 for compression to
3.0 MPa, which leads to about ~1.2 kgCO2eq/kg H2.
The application of CCS lowers on-site emissions, but it also raises the
upstream emissions associated with electricity and natural gas required
to generate steam for the amine regenerator. Although CCS is effective,
some on-site emissions still occur because of inefficiencies in the capture
unit and emission points that are not integrated into CCS. For SMR-85%,
Table 6
GHG emissions results for blue and gray hydrogen production.
Grey hydrogen Blue hydrogen
where on-site emissions are lowered by 85%, upstream emissions from
electricity and natural gas (feedstock and combustion) are more signif­
icant; they account for about 70% of the overall emissions. A large
portion of ATR’s on-site emissions is released to the environment
through the amine regenerator. When captured, on-site emissions are
significantly reduced, but the upstream emissions from electricity and
natural gas (feedstock and combustion) dominate. The upstream emis­
sions account for 84% of the overall emissions after carbon capture. In
NGD, on-site emissions from the process account for 38% to 20% with
the application of CCS. These on-site emissions stem from the combus­
tion of natural gas for process heat, which is primarily for the thermal
decomposition reaction. The remaining emissions are from upstream
natural gas processing and on-site electricity consumption. There is no
significant reduction in the overall GHG emissions of the NGD process in
the case without CCS compared to that with CCS. This is because the
process inherently has low direct emissions. A reduction in direct
emissions increases both electricity consumption (by the CO2 capture
compression unit) and the regenerator reboiler duty. This increase off­
sets the possible gains from the direct emission reduction. Hence, a CO2
capture rate of 61% was deemed a reasonable maximum for the process.
Overall, the percentage of carbon capture is 89%, which includes solid
carbon (1804 tonnes/day) and gaseous CO2 emissions resulting from
combustion.
To practically reduce emissions associated with carbon capture and
sequestration and with the feedstock’s upstream emissions, the use of
electricity with a low carbon emission source and of low carbon-
intensive feedstocks are alternatives, respectively. In this study, the
electricity source is assumed to be from the Alberta electricity grid.
Alberta electricity grid has a relatively high emission factor. The use of
electricity from a combined power plant or renewable power source will
help lower electricity-based emissions. Regarding low carbon-intensive
feedstocks, using a blend of natural gas with renewable methane
(from biomass/biogas) can help to replace fossil-based CO2 with
biomass emissions. Biomass emissions are part of a natural cycle in
which forest growth balances the carbon emitted. The portion of
renewable methane converted to CO2 can be released directly into the
atmosphere, thus reducing the electrical loads on the compression of
CO2. Furthermore, the use of CO2 is an immediate solution to the
accumulation of CO2. Carbon dioxide can be used to develop various
products such as renewable low-carbon fuels and high-value products.
Carbon pricing has a significant impact on the economic perfor­
mance of CCS integrated into these hydrogen production technologies.
Understanding carbon pricing in the hydrogen economy provides a
practical guide to determining the optimal balance between emissions
reduction and CCS application. Fig. 6, Fig. 7, and Fig. 8 show the plots of
carbon price vs the cost of hydrogen. In each case, the cost of hydrogen
increases as the price of carbon increases. Fig. 6 shows that a carbon

Parameter SMR ATR NGD SMR- SMR- ATR- NGD-

52% 85% CCS CCS

On-site 9.17 8.39 1.84 5.52 1.98 0.62 0.9

emission (kg
CO2 eq./kg
H2)
Electricity 0.52 1.28 1.21 0.72 2.4 1.95 1.74
emission (kg
CO2 eq./kg
H2)
Upstream NG 1.65 1.34 1.84 1.96 2.28 1.34 1.9
emission (kg
CO2 eq./kg
H2)
Total GHG 11.35 11.01 4.89 8.20 6.66 3.91 4.54
emissions (kg
CO2 eq./kg
Fig. 6. The effect of carbon prices on the cost of hydrogen from SMR with and
H2)
without CCS.

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Table 7
4.0
Cost breakdown of natural gas-based technologies at a plant capacity of 607
tonnes/day.
3.5
Parameter Grey hydrogen Blue hydrogen
Hydrogen cost ($/kg H2)

3.0 SMR ATR NGD SMR- SMR- ATR- NGD-

52% 85% CCS CCS
2.5
Capital costs 764 1090 1143 1063 1347 1536 1363
2.0 ($M)
Operating costs 121 75 165 167 254 91 201
Without CCS ($M/year)
1.5
Hydrogen cost 1.22 1.23 2.12 1.69 2.36 1.66 2.55
With CCS ($/kg H2)
1.0

0.5
0 50 100 150
Carbon price ($/tonne)
Fig. 7. The effect of a carbon price on the cost of hydrogen from ATR with and
without CCS.
Without CCS
With CCS
Carbon price ($/tonne CO2)
Fig. 8. The effect of a carbon price on the cost of hydrogen from NGD with and
without CCS.
price of $125 or more is needed to justify SMR-52% considering grey
hydrogen production using SMR as the baseline. SMR-85% needs a
carbon price of $130 to compete with grey hydrogen produced using
SMR as the baseline. For NGD (Fig. 8), even at a CO2 carbon price of
$200/tonne, the hydrogen production cost is not competitive with grey
hydrogen produced through NGD. This is because NGD without CCS is
inherently a less emissions-intensive process. Because of the low volume
of CO2 generated, the cost penalty is not sufficient for the case with CCS
to compete with the case without CCS. ATR-CCS needs a carbon price of
$60 to be competitive with the no-CCS scenario. ATR-CCS offers a
relatively low carbon price requirement compared to SMR-CCS and
NGD-CCS.
3.3. Techno-economic analysis
3.3.1. Economic assessment of hydrogen technologies
In this section, we examine how capital and operating costs impact
hydrogen production cost and, more importantly, how the integration of
CCS influences production cost. Table 7 presents the cost breakdown of
grey and blue hydrogen technologies. Details on the capital and oper­
ating costs are included in Table 8, Table 9, and Table 10. Hydrogen cost
is evaluated at a 10% IRR for both grey and blue hydrogen produced
from SMR and ATR. Both technologies have a high TRL. A 15% discount
rate is assumed for grey and blue hydrogen produced from NGD to ac­
200
count for the added risks; its TRL is low.
The cost of grey hydrogen produced from NGD is high. As mentioned
earlier, an economic analysis of NGD was conducted with an IRR of 15%.
However, at an IRR of 10%, NGD’s hydrogen cost is still high at $2.10/
kg H2. The NGD-based hydrogen production cost is about 42.0% higher
than the hydrogen production costs from both SMR and ATR. The SMR-
based hydrogen cost is slightly higher than the cost of ATR-based
hydrogen by about 1.0%, both at an IRR of 10%. This price difference
is not significant. A slight change in how these technologies are accepted
based on their readiness level can lead to a different conclusion. For
example, assuming an IRR of 14%, the ATR-based hydrogen cost in­
creases to $1.53/kg H2, 25.4% more than the cost of SMR-based
hydrogen. Although ATR is a well-established technology, its limited
application, specifically for hydrogen production so far, justifies a
higher IRR value.
The percentage contribution of the operating cost of the technologies
is presented in Table 8. SMR and NGD’s operating costs have more
impact on hydrogen cost than ATR. ATR’s low utility cost helps lower its
hydrogen cost. ATR has a lower utility cost than the other technologies
because its hot and cold process streams are sufficient to reduce fuel and
cooling utilities, respectively. For SMR and NGD, utility costs account
for 24% and 27% of the total operating cost, respectively (see Table 8).
Table 8 also shows the percentage contribution of raw material, utilities,
maintenance, etc., to the total operating cost.
The percentage contribution of the plant process units to the overall
capital investment of grey hydrogen is presented in Table 9. For SMR
and ATR, hydrogen storage accounted for the largest share of capital
cost, about 48% and 34%, respectively. For NGD, the PSA unit accounts
for the largest share of the capital cost, about 36%. The PSA unit requires
large compressors, which contribute significantly to its cost. Hydrogen
storage is also a significant cost contributor, at about 32%. It is impor­
tant to point out that the storage capacity is for half-day hydrogen
production (305 tonnes/day of hydrogen). Storage is a necessary
infrastructure for large-scale production to cut production costs and
improve transportation and distribution to end users. However, large-
scale aboveground hydrogen storage is expensive because of safety
concerns and the material required to handle the high storage pressure
vessels. Underground storage is cheaper because its infrastructure is
inexpensive but often comes with some challenges such as hydrogen
interaction with subsurface minerals and hydrogen-consuming mi­
crobes, hydrogen loss due to geochemical reactions, potential leakage,
and geomechanical response to changes of stress, pressure, and tem­
perature [64].
The integration of CCS reduces carbon emissions, but it increases
hydrogen costs for all the technologies (see Table 7). The increase in
hydrogen cost depends on syngas/flue gas source, volume, composition,
and compressor inlet pressure. These factors increase the number of
units, equipment sizes, and utility demand. Table 10 shows the per­
centage contribution of the process units to the overall capital invest­
ment. The results obtained are similar to cases without CCS, with
hydrogen storage and PSA unit having a significant share. However, the

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Table 8
Operating cost breakdown.
Categories SMR ATR NGD

Cost ($M/year) Percent. contribution Cost ($M/year) Percent. contribution Cost ($M/year) Percent. contribution

Operation and maintenance 30 25% 25 33% 45 27%

Utilities 39 32% 11 14% 40 24%
Raw materials 48 40% 33 44% 78 47%
Labor 2 2% 4 5% 2 1%
Supervision and administration 1 1% 3 4% 2 1%
Total operating cost 121 75 165

Table 9
Capital cost breakdown (without CCS)
Categories SMR ATR NGD

Cost ($M) Percent. contribution Cost ($M) Percent. contribution Cost ($M) Percent. contribution

Reformer* 183 24% 109 10% – –

FBR* – – – – 312 27%
ASU – – 196 18% – –
WGS 23 3% 76 7% – –
PSA 176 23% 327 30% 409 36%
H2 compression 15 2% 11 1% 54 5%
H2 storage 367 48% 371 34% 369 32%
Total capital cost 764 1090 1143
*
Includes heat supply system.

Table 10
Capital cost breakdown (with CCS).
Categories SMR-52% SMR-85% ATR-91% NGD-61%

Cost ($M) Percent. contribution Cost ($M) Percent. contribution Cost ($M) Percent. contribution Cost ($M) Percent. contribution

Reformer* 182 17.1% 182 13.5% 108 7.0% – –

FBR* – – – – – – 311 22.8%
ASU – – – – 198 12.9% – –
WGS 22 2.1% 23 1.7% 61 4.0% – –
CO2 capture 74 7.0% 248 18.4% 230 15.0% 125 9.2%
PSA 155 14.6% 156 11.6% 246 16.0% 407 29.9%
H2 compression 20 1.9% 20 1.5% 15 1.0% 54 3.9%
H2 storage 368 34.6% 368 27.3% 366 23.9% 367 26.9%
CO2 compression 12 1.1% 15 1.1% 31 2.0% 23 1.7%
CO2 storage 2 0.2% 4 0.3% 4 0.3% 2 0.1%
CO2 pipeline 114 10.7% 166 12.3% 138 9.0% 38 2.8%
CO2 sequestration 114 10.7% 166 12.3% 138 9.0% 38 2.8%
Total capital cost 1063 1347 1536 1363
*
Includes heat supply system.

integration of the CCS units, CO2 capture unit (amine unit), storage,
transportation, and sequestration, contribute significantly to the overall
capital cost. For NGD-CCS and ATR-CCS, the integration of CCS in­
creases hydrogen by ~$0.43/kg H2, a 20% and 35% increase compared
to the case without CCS, respectively. Assuming an IRR of 14%, ATR-
CCS’s hydrogen cost increases to $1.96/kg H2, a 16% increase compared
to SMR-52%. When CCS is integrated to SMR-52%, the hydrogen cost
increases by $0.47/kg H2. The increase in hydrogen cost is more sig­
nificant in SMR-85% because two large-capacity CCS units are needed to
achieve 85% carbon capture. Of the CCS units in SMR-85%, the second
unit, which captures carbon emissions from the reformers’ furnace, is
more expensive. Its annual operating cost is higher than SMR-52%’s and
NGD-CCS’s and significantly higher than ATR-CCS’s. The cost of
hydrogen from SMR-85% is 40% higher than from SMR-52%. The results
obtained by Collodi et al. for 206 tonnes of hydrogen per day suggest
that by capturing around 90% of the CO2 emitted by the SMR plant
(compared to a conventional 53–60% capture rate), the cost of hydrogen
production through SMR-CCS increases by approximately 46% [60].
Collodi et al.’s results align with the findings in this work. In all cases,
the cost of CCS is dominated by the electricity used for the compression
and liquefaction of CO2. The remaining costs, such as cooling water,
maintenance, labor, etc., have less impact on the hydrogen cost.
A direct comparison of blue hydrogen costs from the considered
technologies is a challenging task. The costs of hydrogen vary across the
literature because of key economic inputs like plant size (the effect of
economies of scale), the lifetime of the facility, the expected internal rate
of return (IRR) on investment of the project, the equivalent capacity
factors, the cost of feedstock (natural gas), etc. In this study, we
considered a large-scale hydrogen plant and obtain hydrogen costs of
$1.69/kg H2 and $2.36/kg H2 for 52% and 85% CCS, respectively.
Olateju and Kumar considered a similar hydrogen capacity with a 61%
SMR-CCS and reported hydrogen supply cost in the range of 2.5-$3.01/
kg H2 [55]. On the other hand, Salkuyeh et al. reported $2.16/kgH2 for a
90% SMR-CCS without hydrogen storage. For a 90% ATR-CCS, Salkuyeh
et al. reported a hydrogen price of $1.58/kg H2 [34], while in our study,
we estimated $1.66/kg H2 for 91% ATR-CCS.
There are a few techno-economic assessments of hydrogen produc­
tion from natural gas decomposition. Because it is an emerging tech­
nology, the studies report different conceptual designs of the NGD-CCS
process. An early study calculated hydrogen supply cost to be $2.28/kg
H2 at a natural gas price of $4.84/GJ [65]; our study assumed a natural
gas price of $1.96/GJ. The authors of the earlier study considered credit

11
A.O. Oni et al.
from the sale of the produced carbon at the rate of $0.64/kg H2, which
was not considered in our base case. A more recent study by Keipi et al.,
using a regenerative heat exchanger reactor, derived a hydrogen supply
cost of $3.86/kg H2 at a natural gas price of $8.5/GJ [14]. Their higher
hydrogen supply cost may be attributed to the higher price of natural gas
and the small scale of 2.2 tonnes/day plant capacity. Using a molten
metal reactor, Parkinson et al. derived a cost of $1.99/kg H2 at a natural
gas price of $5.2/GJ [66]
3.3.2. Sensitivity and uncertainty analysis of the blue hydrogen technologies
With the point estimates, we obtained hydrogen production costs
using current and most likely (assumed) economic parameters during
the study period. However, economic parameters fluctuate and do not
always follow a predictable trend. For example, the IRR value was
chosen subjectively. Its effect on hydrogen cost could influence decision-
making. Moreover, some of these parameters may not be the optimum
value for a project and thus may introduce a level of uncertainty in the
output results. In addition, there is a wide range of results in the liter­
ature, primarily due to the differences and assumptions in input pa­
rameters. The differences in the output results in the literature also make
it difficult to draw a reasonable conclusion from them. Because of the
degree of uncertainty in input parameters, we conducted sensitivity and
uncertainty analyses to account for the variability in hydrogen pro­
duction cost. Fig. 9 (a–d) presents the Morris sensitivity plots for SMR-
52%, SMR-85%, ATR-CCS, and NGD-CCS, respectively. Each point on a
plot represents a set of input parameter. Points with a large standard
deviation indicate non-linearity and/or interaction between input pa­
rameters. Points with a large mean value indicate that the variation in
the effect of the input parameter on the output (hydrogen production
cost) is large. Parameters in the bottom left corner of the plots (in the
SMR-52% (a)
ATR (c)
Fig. 9. The influence of economic parameters on the hydrogen cost from (a) SMR-52%, (b) SMR-85% (c) ATR, and (d) NGD.
12
Energy Conversion and Management 254 (2022) 115245
green box) have a negligible effect on hydrogen production cost and so
are not considered in the uncertainty analyses. Parameters in the top
right corner of the plots (in the red box) indicate that hydrogen pro­
duction cost is highly sensitive to changes in these parameters. The
parameters between the two boxes are semi-sensitive, and it is difficult
to fully understand how they impact output uncertainty. The decision to
include them in the uncertainty analysis is subjective when Morris plots
are used. Fig. 9 shows that hydrogen storage and IRR are highly sensitive
in all the technologies. Natural gas is highly sensitive in SMR-85% and
semi-sensitive to other technologies. An increase in these highly sensi­
tive inputs leads to an increase in hydrogen cost. In the uncertainty
analysis, with the Monte Carlo simulation, Sobol’s method was used to
evaluate the contribution of the uncertain parameters. Sobol indices are
useful for determining how the output variance (hydrogen cost) is
impacted by the input variance. Further details on Sobol indices are
given by Koziel et al. [67]. The results indicate that many of these input
parameters had a negligible effect on the variabilities in the output
model. Fig. 10 presents the box plot of the uncertainty results for each
technology. The box plot depicts how the variation in input parameters
impacts hydrogen production cost. For SMR-52%, ATR-CCS, and NGD-
CCS, hydrogen storage, and IRR have a significant impact on the pro­
duction cost of hydrogen from these technologies and contribute up to
92.4%, 94.5%, and 86.8% to the total variability, respectively. In each
case, hydrogen storage contributes more than 55%, making it the most
sensitive parameter. The contribution of the other input parameters in
all cases is less than 14%. SMR-85% has a wide range of variation
because of hydrogen storage, IRR, and natural gas price, which
contribute 34.9%, 30.1%, and 26.3% to the total variability, respec­
tively. Capacity use, CO2 transportation, and electricity, less influential
parameters, contribute 8.7%. In every technology, the base case results
SMR-85% (b)
NGD (d)
A.O. Oni et al.
Hydrogen cost ($/kgH2)
SMR-52% SMR-85% ATR-CCS NGD-CCS
Fig. 10. Uncertainty in cost results of blue hydrogen production technologies.
are much lower than the mean values. They are closer to the lower
bounds of the output model because of the asymmetric nature of the
range of the inputs used and the non-linear model responses. Using a
triangular distribution instead of a uniform distribution reduces the
mean values by less than 2%. Details on triangular and uniform distri­
butions can be found in the e-Handbook of Statistical Methods [68]. This
reduction is negligible, and it illustrates that the parameter distribution
selection has little or no effect on the output distribution.
Comparative analysis sometimes goes beyond identifying sensitive
inputs and conducting traditional uncertainty analysis when output re­
sults overlap. In Fig. 10, the overlaps among the uncertainty ranges of
the four technologies complicate comparison. It is difficult to state that
one technology is better than or equal to another. For comparison pur­
poses, Henriksson et al. recommended a four-step approach to outcomes
useful for decision-making [69]. The four steps are quantifying and
characterizing input parameters (step 1), quantifying output un­
certainties using propagation methods like Monte Carlo (step 2), sta­
tistical testing (step 3), and communicating results (step 4). However,
Bromssen and Roos cautioned against inappropriately using Monte
Carlo for comparative analysis [70]. They discouraged comparing
Fig. 11. Comparative analysis of cost production for blue hydrogen technologies.
13
Energy Conversion and Management 254 (2022) 115245
simulation results of many inputs to avoid undermining output vari­
ability and misleading conclusions. To conduct steps 2 and 3, we
modeled the difference between two technologies using shared input
distributions for dependent inputs. This concept allows for an accurate
comparison between technologies. The data considered for this analysis
are dependent, so each technology uses the same sampled parameter. A
Monte Carlo simulation was run for the sampled parameters. We then
evaluated the differences in each Monte Carlo simulation by subtracting
the results of one technology from another. It is worth noting that the
differences in the results obtained, as presented in Fig. 11, follow a
normal distribution. In Fig. 11, each technology is compared with
another. Each box plot represents the differences between the probable
outcomes in two technologies. Differences between technologies are
entirely in the positive region (Fig. 11), except for SMR-52% and ATR-
CCS and NGD-CCS and SMR-85%, with differences in P5 (the bottom
error in Fig. 11) of − 0.04 $/kg H2 and − 0.05 $/kg H2, respectively. The
positive values indicate that the technology with a low hydrogen cost is
subtracted from those with high costs. Subtracting the output of ATR-
CCS from SMR-85% or NGD-CCS leads to a positive outcome consid­
ering a 90% confidence interval. For these cases, ATR-CCS produces a
lower hydrogen cost, and it is economically preferable. On average, the
differences between SMR-52% and ATR-CCS are positive, but some
scenarios are negative at P5. These negative scenarios present a possi­
bility for SMR-52% to outperform ATR-CCS when natural gas price de­
creases and IRR increases. Fig. 12(a) shows that natural gas price and
IRR are responsible for about 89% of the total variability in SMR-52%
and ATR-CCS. These results also indicate that the negative scenarios are
driven by both input parameters. Similarly, NGD-CCS is preferable to
SMR-85% within the positive region. However, it is possible for SMR-
85% to outperform NGD-CCS at P5 when CO2 transportation cost and
natural gas price decrease. The influence of both parameters is evident,
and they are shown in Fig. 12(b). Furthermore, the differences in other
technologies (shown in Fig. 11) clearly indicate that SMR-52% is pref­
erable to NGD and SMR-85%. SMR-85% is less attractive economically.
It has a larger mean hydrogen production cost than the other
technologies.
3.3.3. Development of a scale factor and the effect of plant capacity on blue
hydrogen cost
To evaluate the scale factor of each blue hydrogen technology, we
A.O. Oni et al. Energy Conversion and Management 254 (2022) 115245

Fig. 12. Sobol results for the differences between (a) SMR-52% and ATR-CCS and (b) SMR-85%-NGD-CCS.

investigated plant capacities of 50 to 1000 tonnes/day of hydrogen
production. We estimated the capital cost for each hydrogen production
capacity to determine the plant scale factor. Fig. 13 shows the plots of
capital cost vs plant capacity for the hydrogen technologies. The scale
factors were developed using the process simulation models for each
technology. The capital cost of each component of the hydrogen pro­
duction plants was developed at various capacities. These were then
used to develop the scale factor of the whole plant. The scale factors
obtained for SMR-52%, SMR-85%, ATR-CCS, and NGD-CCS are 0.67,
0.68, 0.54, and 0.58, respectively. For all the cases considered, the scale
factor value indicates that to lower the hydrogen cost, plant capacity
needs to be increased. Fig. 14 presents the economic feasibility of
increasing plant capacity. The cost of hydrogen decreases as the plant
capacity increases. It is worth mentioning that the decrease in the pro­
duction cost of ATR-CCS hydrogen is steeper because of its lower
operating costs. ATR-CCS and NGD-CCS are more attractive economi­
cally for large-scale hydrogen production. The lowest hydrogen costs
obtained at a plant capacity of 1000 tonnes/day are $1.55/kg H2, $1.7/
kg H2, $1.28/kg H2, and $1.28/kg H2 for SMR-52%, SMR-85%, ATR-
CCS, and NGD-CCS, respectively. Because economies of scale exist for
all blue hydrogen technologies, operating the plants at a higher capacity
will be beneficial.
The costs of large-scale blue hydrogen plants are expected to be
attractive compared to the costs of hydrogen from renewable feedstock,

Fig. 13. Capital costs at different plant capacities for the four blue hydrogen technologies.

14
A.O. Oni et al.
Fig. 14. Hydrogen costs at different plant capacities (tonnes/day) for the four blue hydrogen technologies.
electrolysis plants, or small-scale hydrogen plants. It will be interesting
to compare the cost of hydrogen from Fig. 13 and Fig. 14 with prior
works. However, most of these works did not consider the cost of
hydrogen storage, and, in some cases, the source of electricity is
different (electricity is generated within the plant premises or from the
grid). Besides, there are disparities in economic parameters (capital
factors, cost of natural gas, plant life, internal rate of return, etc.), which
also create uncertainties in hydrogen cost. For example, when we apply
Fig. 13 and Fig. 14 to Salkuyeh et al.’s work [34], the capital and
hydrogen costs obtained were $M 1,125 and $2.4/kg H2, respectively,
Salkuyeh et al. obtained M$ 831 and $2.16/kg H2. When these values
were adjusted for inflation, from 2016 to 2020, we obtained M$ 914 and
$2.4/kg H2. The differences in these values and the ones obtained by our
models are because of the source of electricity, economic assumptions,
and hydrogen storage.
4. Conclusion
In this study, comparative techno-economic and greenhouse gas
(GHG) emissions assessments were carried out for natural gas-based
blue hydrogen production technologies: steam methane reforming
(SMR), autothermal reforming (ATR), and natural gas decomposition
(NGD). For steam methane reforming, based on the percentage of carbon
capture and capture points, we considered two scenarios: SMR-52% and
SMR-85%. From an energy perspective, SMR-85% consumes the most
natural gas (as fuel and feedstock) and ATR-CCS the least. However,
SMR-85%, SMR-52%, and ATR-CCS source hydrogen from both steam
and natural gas, so they consume less natural gas as feedstock than NGD-
CCS. ATR-CCS uses less fuel than SMR-85% and NGD-CCS.
For 607 tonnes of hydrogen production per day, blue hydrogen from
autothermal reforming has the lowest life cycle GHG emissions, 3.91
kgCO2eq/kg H2, followed by NGD (4.54 kgCO2eq/kg H2), SMR-85%
(6.66 kgCO2eq/kg H2), and SMR-52% (8.20 kgCO2eq/kg H2). The
hydrogen costs are 1.22, 1.23, 2.12, 1.69, 2.36, 1.66, and 2.55 $/kg H2
for SMR, ATR, NGD, SMR-52%, SMR-85%, ATR-CCS, and NGD-CCS,
respectively. For blue hydrogen production, ATR-CCS and NGD-CCS
produce hydrogen with the lowest and highest cost, respectively.
15
Energy Conversion and Management 254 (2022) 115245
Detailed sensitivity and uncertainty analyses were conducted mainly to
compare, and better understand the parameters impacting hydrogen
cost. Sensitivity analysis showed that hydrogen storage and internal rate
of return (IRR) have a significant impact on the costs of blue hydrogen
produced by SMR-52%, ATR-CCS, and NGD-CCS. For SMR-85%,
hydrogen cost is significantly influenced by hydrogen storage, IRR, and
natural gas price. We modeled the differences between two technologies
using shared input distributions for dependent inputs. SMR-52% and
ATR-CCS have lower blue hydrogen production costs and are econom­
ically preferable to NGD-CCS and SMR-85%. SMR-52% may outperform
ATR-CCS when natural gas prices decrease and IRR increases. Similarly,
NGD-CCS may outperform SMR-85% economically when CO2 trans­
portation costs and natural gas prices decrease. SMR-85% is less
attractive economically; it has a higher mean blue hydrogen production
cost than other technologies. The scale factors obtained for SMR-52%,
SMR-85%, ATR-CCS, and NGD are 0.67, 0.68, 0.54, and 0.65, respec­
tively. The blue hydrogen production cost versus capacity profile shows
there are economies of scale for all the blue hydrogen production
technologies, and operating at a higher capacity will be economically
beneficial.
The findings of this study show that no matter what goal is set for
blue hydrogen technology, it must be ranked alongside energy use,
upstream feedstock, electricity GHG emissions, and key economic pa­
rameters to provide robust and meaningful information for decision-
making.
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Acknowledgements
The authors are grateful to the Alberta Department of Energy
(ADOE), Natural Resources Canada (NRCan), and the British Consulate-
General, Calgary for the financial support to carry out this project, as
A.O. Oni et al.
well as their expert feedback on the assumptions and results. The au­
thors would also like to thank the representatives from the Ministry of
Alberta Environment and Parks, the Ministry of Jobs, Economy and
Innovation, and the Ministry of Treasury Board and Finance who have
provided input and feedback during the project. The authors are grateful
to the NSERC/Cenovus/Alberta Innovates Associate Industrial Research
Chair Program in Energy and Environmental Systems Engineering and
the Cenovus Energy Endowed Chair Program. As a part of the University
of Alberta’s Future Energy Systems (FES) this research was made
possible in part thanks to funding from the Canada First Research
Excellence Fund. We are thankful to Astrid Blodgett for editing this
paper and also acknowledge Ayodeji Okunlola, Matthew Davis, Eskinder
Gemechu and Minza Haider from the University of Alberta for providing
valuable input and feedback during the study.
Appendix A. Supplementary data
Supplementary data to this article can be found online at https://doi.
org/10.1016/j.enconman.2022.115245.
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