Review and Comparison of Various Hydrogen Production Methods Based On Costs and Life Cycle Impact Assessment Indicators

i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 8 6 1 2 e3 8 6 3 5
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Review Article
Review and comparison of various hydrogen

production methods based on costs and life cycle
impact assessment indicators
Mengdi Ji a, Jianlong Wang a,b,*

a
Laboratory of Environmental Technology, INET, Tsinghua University, Beijing, 100084, PR China
b
Beijing Key Laboratory of Radioactive Waste Treatment, INET, Tsinghua University, Beijing, 100084, PR China
highlights graphical abstract
Various H2 production methods

from renewable/non-renewable
resources were reviewed.
H2 production methods were
compared in terms of cost and life
cycle assessment.
The current mainstream approach
is to obtain hydrogen from natural
gas and coal.
Electrolysis and thermochemical
cycle using new clean energy are
more sustainable.
article info abstract
Article history: Hydrogen is a clean, renewable secondary energy source. The development of hydrogen
Received 22 June 2021 energy is a common goal pursued by many countries to combat the current global warming
Received in revised form trend. This paper provides an overview of various technologies for hydrogen production
12 September 2021 from renewable and non-renewable resources, including fossil fuel or biomass-based
Accepted 16 September 2021 hydrogen production, microbial hydrogen production, electrolysis and thermolysis of
Available online 7 October 2021 water and thermochemical cycles. The current status of development, recent advances and
challenges of different hydrogen production technologies are also reviewed. Finally, we
Keywords: compared different hydrogen production methods in terms of cost and life cycle envi-
Hydrogen ronmental impact assessment. The current mainstream approach is to obtain hydrogen
Hydrogen production from natural gas and coal, although their environmental impact is significant. Electrolysis
Environmental impact and thermochemical cycle methods coupled with new energy sources show considerable
potential for development in terms of economics and environmental friendliness.
© 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
* Corresponding author. Energy Science Building, INET, Tsinghua University, Beijing, 100084, PR China.
E-mail address: wangjl@tsinghua.edu.cn (J. Wang).
https://doi.org/10.1016/j.ijhydene.2021.09.142
0360-3199/© 2021 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.
i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 8 6 1 2 e3 8 6 3 5 38613
Contents
Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38613
Hydrogen production from fossil fuels . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38615
Steam methane reforming (SMR) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38615
Partial oxidation of methane (POM) and autothermal reforming (ATR) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38616
Coal gasification (CG) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38617
Partial oxidation (POX) of oil products . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38618
Hydrogen production from biomass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38618
Biomass gasification . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38618
Steam gasification of biomass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38618
Supercritical water gasification (SCWG) of biomass . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38619
Biological conversion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38619
Biophotolysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38619
Photo fermentation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38620
Dark fermentation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38620
Dark-photo co-fermentation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38621
Water electrolysis-based hydrogen production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38621
Conventional water electrolysis methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38621
High-temperature electrolysis/solid oxide electrolysis (SOEL) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38622
Anion exchange membrane (AEM) electrolysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38623
Clean electricity and electrolysis for hydrogen production . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38623
Water thermolysis and thermochemical cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38624
One-step water thermolysis . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38624
Thermochemical cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38624
Sulfur-iodine (SeI) cycle . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38624
Copper-chlorine (CueCl) cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38625
Two-step metal oxide cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38625
Costs and life cycle environmental impacts of hydrogen production methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38626
Costs of different methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38626
Environmental impact comparison . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38626
Conclusion and recommendation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38628
Declaration of competing interest . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38629
Acknowledgements . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38629
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 38629
than 40 years, natural gas for less than 60 years and coal for
Introduction less than 250 years [2,7].
Also, the environmental impacts from fossil fuel use have
The growing global economy, rapidly increasing population also attracted people's attention, such as the massive emis-
and accelerated urbanization have greatly increased the de- sions of greenhouse gases (GHG), mainly carbon dioxide, and
mand for energy [1e4]. Now the main energy sources are fossil their significant contribution to global warming [4,6,8]. Fossil
fuels including coal, oil and natural gas. According to the fuels contain nitrogen, sulfur and other heteroatoms, which
statistical data from International Energy Agency (IEA), in may form atmospheric pollutants such as nitrogen oxides and
2018, fossil fuel accounted for over 80% of global total energy sulfur oxides during the utilization process and cause a
supply. As for the total final consumption, about 67% was in number of ensuing environmental problems such as acid rain,
the form of fossil fuels. Electricity and heat respectively soil acidification and eutrophication of surface water bodies.
accounted for 19.31% and 3.03% as shown in Fig. 1. However, a In order to address the global warming trend, the Inter-
considerable part of electricity or heat is obtained relying on governmental Panel on Climate Change (IPCC) has proposed to
fossil fuels as the primary energy sources [5]. limit warming to no more than 1.5 C compared to pre-
The fossil fuel reserves are limited, and non-renewable in industrial levels and expects to reach net zero CO2 emis-
short time period with uneven distribution in different regions sions by 2050 [9]. An important initiative to achieve this goal is
[1]. Existing reserves may not be in stable supply to meet to minimize GHG generated from human activities.
future energy needs. Consequent problems include energy Although fossil fuels still have an unassailable position in
price increasing and even political conflict [3,6]. It is estimated global energy supply so far, their poor sustainability and
that the currently discovered reserves can supply oil for less apparent environmental disadvantages have led to a search
38614 i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 8 6 1 2 e3 8 6 3 5
[3,8]. In fact, it has the most heat content per unit mass among
all fuels we have used and has a very high potential to be an
energy carrier [2]. Nevertheless, hydrogen has a much lower
bulk density than these conventional fuels, so the comparison
in terms of heat content per unit volume has no significant
advantage [10]. As a result, hydrogen compression and storage
technologies are also receiving more attention [8]. Table 1
summarizes the heat values of several fuels [11].
Currently, most hydrogen product is used as a kind of raw
material for industrial production. If its potential as an energy
carrier can be fully realized, it will have the possibility to play a
role in more areas [12]. The idea of using hydrogen as vehicle
fuel came up in the early 19th century. In the 1970s, interest in
hydrogen was raised again because of the energy crisis. With
many institutions’ attention and technological progress,
related researches have been making considerable break-
throughs since then [8,13e15]. The global fuel cell electric
vehicle (FCEV) sales are ,12350 at the end of 2019, and this
number is more than twice that of 2018. There were 470
operational hydrogen refueling stations worldwide. Devel-
oping hydrogen economy and ensuring energy security has
become a common goal pursued by many countries [16].
Hydrogen is considered as a clean and non-toxic energy
source because in theory water is the only product of the
process of using hydrogen [17e19]. However, hydrogen pro-
duction processes are not absolutely environmentally
friendly. The feedstocks, energy inputs and waste emissions
during hydrogen's whole life cycle will affect how clean it is.
Hydrogen is classified into three different colors: green, blue
and grey, to describe its environmental friendliness. The
classification mainly bases on primary energy sources used to
generate hydrogen and production technologies [1,20]. Green
hydrogen is considered to be clean, which relies primarily on
renewable energy to produce. Grey hydrogen from fossil fuels
can place a significant burden on the environment during its
production. The environmental impact of blue hydrogen is
between green and grey hydrogen. Some hydrogen made from
fossil fuels is called “blue” because it adds the process of
capturing and sequestering CO2 to reduce carbon emissions,
thus distinguishing it from grey hydrogen [21].
Hydrogen can be obtained through a variety of production
Fig. 1 e Global total energy supply, total final consumption methods and technologies. All methods require feed stocks
and electricity generation by source. and energy, including non-renewable fossil fuels and renew-
able biomass, wind and solar energy, and so on (Fig. 2).
There is no doubt that it is particularly desirable to obtain
for an alternative energy source. The new energy source is hydrogen from renewable energy sources. From the point of
expected to be clean enough and renewable to ensure a stable, waste emissions, light-based hydrogen production technolo-
continuous supply, with sufficient security and low difficulties gies are more environmentally benign than many other
for production and storage. We hope that it has the potential methods [3]. But these technologies lose their superior
to replace fossil fuels in the future.
Hydrogen is the first chemical element in the periodic table
of elements. It is the most abundant element in the universe
and the tenth most abundant in the Earth's crust. Hydrogen Table 1 e Heat values of several fuels.
monomers are scarce in nature and we find almost no HHV (MJ/kg) LHV (MJ/kg)
hydrogen in the atmosphere [2]. Instead, the vast majority of
Hydrogen (g) 141.9 119.9
hydrogen atoms are found in compounds. Therefore, Methane (g) 55.5 50
hydrogen gas that can be used as an energy carrier needs Ethane (g) 51.9 47.8
artificial production. As a kind of fuel, the low heat value of Gasoline (l) 47.5 44.5
hydrogen is about 120 MJ/kg, much higher than methane Diesel (l) 44.8 42.5
(50.0 MJ/kg), gasoline (44.5 MJ/kg), diesel (42.5 MJ/kg) and so on Methanol (l) 20 18.1
Fig. 2 e Primary energy sources, feed stocks and routes for hydrogen production.
competitiveness when costs and efficiencies are taken into Microbiological processes could achieve the dual purpose
account. The total global demand for hydrogen is about 70 Mt of organic waste utilization and hydrogen production via
per year, but it is mainly produced by fossil fuels [22]. biochemical action but they are still limited to laboratory-
The most widely used hydrogen production technology in scale research. Because the amount of hydrogen produced
recent years is natural gas steam reforming and contributes by microorganisms is low so cannot be put into industrial
more than 45% of hydrogen products, followed by oil production for the time being [11,20,23].
reforming and coal gasification as shown in Fig. 3 [3,13,23,24]. More detailed information about hydrogen production
In short, a large amount of hydrogen still comes from fossil methods will be shown in the following parts. We will present
fuels rather than renewable energy. Using biomass to the characteristics and research progress of various hydrogen
generate hydrogen has also found some application but faces production technologies, try to analyze their economic costs,
some technological and economic challenges [25]. Electrolysis and compare their environmental impacts from the perspec-
and thermolysis methods are constantly developing, both of tive of carbon emissions, etc.
which are based on the decomposition of water to obtain
hydrogen gas. They manifest more advantageous in small-
scale applications [6,13,26]. Hydrogen production from fossil fuels
Steam methane reforming (SMR)
Steam methane reforming, or natural gas steam reforming, is

currently the most widely used method of hydrogen produc-
tion, with nearly half of the world's hydrogen coming from
this source [27]. SMR is generally carried out with precious
metals or nickel-based materials as catalysts at high tem-
peratures of about 800 C [28,29]. Reforming is achieved
through three main processes. Firstly, methane and water
vapor undergo reforming reaction to obtain syngas with main
components of H2 and CO, followed by CO conversion through
water gas shift (WGS) reaction. Finally, CO2 is removed from
the gas mixture by CO2 adsorption device to improve the pu-
rity of hydrogen gas. The reaction equations for the first two
Fig. 3 e Current hydrogen gas product sources [3,13,23,24]. processes are shown in (1) and (2), respectively:
CH4 þ H2O / CO þ 3H2 (1) for about 65% of the total. Most catalysts are obtained by
modifying nickel-based materials due to the proven advan-
CO þ H2O / CO2 þ H2 (2) tages of nickel materials, such as precious metal infusion [38]
or the use of TiO2 [39] as a support. Angeli et al. experimentally
Natural gas contains about 95% methane and 3.5% other found that the choice of support also has effect on the per-
hydrocarbons [30]. Other alkanes can also perform a reaction formance of catalysts and confirmed the catalytic function of
that is similar to reaction (1), which can be expressed as non-nickel materials [40].
follows: Another research focus is the combination of carbon cap-
The enthalpy change of reaction (1) is þ206.1 kJ/mol, and ture and storage (CCS) with SMR technologies. Increasing the
the enthalpy change in Eq. (3) is also greater than zero, which capture rate of CO2 is beneficial to both the high purity of
means reforming reaction is a heat-absorbing process and hydrogen and the reduction of GHG emission. Since SMR
therefore requires a certain amount of external heat [3]. It is technology is essentially the conversion of fossil fuels into
generally obtained through the combustion of natural gas [31]. hydrogen, the CO2 emissions during the process are signifi-
The final gas mixture contains 70e75% hydrogen, with other cant and do not perfectly meet the expected pursuit of “low
components including 7e10% CO, 6e14% CO2, and a small carbon” or “clean”. However, SMR is economically less
amount of methane (2e6%). Factors affecting SMR technology expensive and suitable for large-scale production. If effective
include the quality of feed stocks, the choice of fuel and means can be adopted to control carbon emissions from the
catalyst, the type of reactor, and so on [32]. production process, this technology will have a broader and
SMR technology itself is well developed. The current issues more promising development prospect, which can provide an
of greater concern are how to increase the conversion of alternative until the absolute transition to a renewable energy
natural gas and hydrogen production capacity, and how to phase for hydrogen production [41].
reduce the temperature required for the reaction to make the In addition to natural gas, a number of other substances
technology become a more desirable production mode. Low containing alkane gases can be used as feed stocks, such as
temperature steam reforming technology is used to produce biogas, to achieve the reforming process similar to the one
syngas at 400e550 C. Its advantage over high temperature described above. Although they are not currently used on the
reactions is that the lower temperature requirement reduces same scale as natural gas, their potential to produce high
the energy required for preheating and allows for rapid start- purity hydrogen has been demonstrated on a laboratory scale
up without CO shift reactor. Also, there is a wider choice of [42].
materials for the reactor, without limiting it to high-
temperature resistant alloys. These advantages can signifi- Partial oxidation of methane (POM) and autothermal
cantly reduce the construction and operating costs of SMR reforming (ATR)
hydrogen production plants. However, certain measures must
be taken to eliminate the negative effects of low reaction The feature that SMR technology needs external heat input
temperatures on methane conversions [33]. has limited its development to some extent, and other tech-
The membrane reactor allows the hydrogen produced by nologies have emerged to overcome the drawback of high
the reaction to be transferred outside the reaction system energy demand. Partial oxidation of methane (POM) is another
through hydrogen-selective membrane, thus shifting the re- method of hydrogen production by natural gas that has been
action equilibrium to the right and greatly improving the applied commercially. Incomplete oxidation of methane gives
conversion of natural gas. The properties of the membrane are a mixture of H2 and CO by the input of oxygen at less than
of interest. High permeability facilitates the rapid exit of stoichiometric ratio:
hydrogen from the reaction zone, while the high selectivity
makes it difficult for other gases to pass through thus ensuring CH4 þ 0.5O2 / CO þ 2H2 (3)
the purity of hydrogen. Palladium is an ideal membrane ma-
terial [34,35]. Anzelmo et al. experimented with a palladium- The reaction above is exothermic and the oxidation
gold composite membrane reactor that permeates hydrogen (combustion) of methane provides heat for the system, so it is
with 100% purity at low temperature and low pressure no longer dependent on external heat sources [30]. This is
(350e400 C, 300 kPa), which can maintain stability over the followed by WGS reaction shown in Eq. (2). As the reaction in
long period of time tested [36]. Eq. (3), partial oxidation process requires the participation of
On the other hand, the use of catalysts is very important to pure oxygen, so the purchase of oxygen needs to be added to
the operation of membrane reactors. Because the hydrogen the production costs. Nevertheless, use of air instead of pure
permeation rate is fast with a right membrane material, the oxygen is not very desirable, since the presence of large
catalyst activity largely determines the size of the final amounts of nitrogen increases the cost of separation process
hydrogen product stream [34,37]. Certainly, conventional high later [33,43]. Partial oxidation reaction can be performed
temperature steam reforming reaction also requires the under catalyst-free conditions and it has better tolerance to
involvement of catalysts. Therefore, the development of high- impurities of sulfur in fossil fuels [3,17]. Currently, the
efficiency catalysts has become a popular direction with the hydrogen yield of POM method is not yet comparable to that of
development of SMR technology. We searched for “steam SMR [44].
methane reforming” as the topic on the “web of science” Autothermal reforming (ATR) can be seen as a combination
website and got a total of 8825 results. Then we entered of favorable features of both steam reforming and partial
“catalyst” to refined results and got 5740 results, accounting oxidation processes. It allows the production for hydrogen via
connecting the devices of two processes in series. The heat steam is introduced and the air input is stopped. The water
required for ATR comes from the partial oxidation of natural vapor will be converted into water gas as Eq. (5). When the
gas and the exotherm of the oxidation process is used to heat of the fuel layer is consumed to a certain level, air is
achieve steam reforming [43]. This series of reactions will reintroduced. These two reactions are cycled in turn, and the
perform continuously as the system reaches an overall ther- product obtained is water gas [49]. Most of the coal gasification
mal equilibrium through exothermic and endothermic re- to hydrogen is done by the above method, and a few takes
actions. Because of the existence of partial oxidation reaction, external indirect heat supply so that reaction (6) can occur
ATR also requires the provision of pure oxygen as a reactant to without reaction (5). This method does not require oxygen to
achieve, and the cost of oxygen production is also included in be supplied to the system, which simplifies the process and
the holistic cost calculation. ATR technology is not yet reduces the production of CO2. The key point is to ensure a
commercially available on a large scale [3,23]. stable and continuous supply of heat to the reaction unit [50].
Since expectations for high reaction rates, mild reaction The gas mixture generated consumes CO and produces H2 via
environments, low production costs and less pollutant emis- the WGS reaction. Finally, CO2 is removed from the mixture in
sions are present in both technologies, researchers have had the pressure swing adsorption (PSA) unit, which generally
to seek effective ways to accomplish these pursuits. In recent combines calcium oxide (CaO) with CO2 to form calcium car-
years, research on catalysts for POM and ATR technologies has bonate (CaCO3), and high purity hydrogen is then obtained.
attracted more attention, although for the former the cata- Due to the high sulfur content of feed stocks, the absorbed
lysts are not indispensable [44e46]. For comparison purposes, sulfur can be recovered for re-production [26,51].
we have briefly listed the characteristics of the three methods At the current state of art, CG method is already available
of hydrogen production via natural gas, as shown in Table 2. for commercial production and provides 18% of the world's
hydrogen production. Since its lower efficiency (60e75%) than
Coal gasification (CG) the SMR method (70e85%) [52], it is not as widely used as the
latter. However, in countries and regions where coal reserves
Among the three major fossil fuels, coal is the most abundant are relatively abundant or natural gas prices are not friendly,
in terms of reserves, providing a viable option for hydrogen such as China, CG is also the mainstream hydrogen produc-
production. The conversion from coal to hydrogen is accom- tion process [24,31,32]. With the shortage of natural gas re-
plished mainly through the coal gasification (CG) process. serves and rising natural gas prices, the economic advantages
According to whether the coal is mined before gasification, of CG in large-scale production are expected to make it a better
coal gasification can be divided into surface coal gasification choice in more regions in the foreseeable future [6].
(SCG) and underground coal gasification (UCG) [47]. The One obvious drawback of CG for hydrogen production is its
former is a mature method of hydrogen production, while significant environmental impact. According to reports in the
UCG is a newly developed technology in recent years, and literature, CG has approximately twice the carbon emissions
there are still many unknowns in its fields. So we will not of SMR when both mainstream fossil fuel hydrogen produc-
introduce it in detail in this paper. tion technologies are evaluated from a full life cycle perspec-
SCG operates in a specific equipment known as gasifier. tive. In fact, coal gasification has the highest global warming
Depending on the contact mode between reactants and potential (GWP) of all existing hydrogen production methods,
gasifier, the gasifiers can be subdivided into various types, and has an appreciable acidification potential (AP), probably
among which the entrained flow gasifier is the cleanest and related to the higher sulfur content in coal [26,53,54].
most efficient type [48]. Their basic mechanism is the same: In order to control the detrimental environmental impact
the coal is dried and ground and then fed into a gasifier, where CO2 emission causes, effective measures must be taken to
it successively reacts with oxygen and steam under high reduce it from the production process. Researchers have tried
temperature conditions to produce gas mixture containing H2, to incorporate CCS technology to achieve this goal. Li et al.
CO and CO2. The reaction equation is shown below. used ash agglomeration fluidized bed gasification to evaluate
the GHG emissions from CG with and without CCS, and the
C þ O2 / CO2 (4) results showed that the use of CCS could reduce the GHG
emissions by 81.72%, while the primary fossil energy con-
C þ H2O / CO þ H2 (5) sumption only increased by 2.32% [55]. Burmistrz et al.
designed three scenarios by selecting different feedstock coals
This production process is intermittent. Firstly, air is and gasification units from two companies, GE Energy/Texaco
introduced into the gasifier, which oxidizes part of the fuel and Shell, and calculated CO2 emissions respectively. With the
based on Eq. (4) and stores the heat in the fuel layer. Then sequestration of CO2, carbon emissions were reduced by
Table 2 e Comparison of three methods for hydrogen production from natural gas.
Material and energy requirements Efficiency Temperature ( C)
External heat Catalysts Pure oxidation
steam methane reforming (SMR) ✓ ✓ 70e85% 800e1100
partial oxidation of methane (POM) ✓ 55e75% 950e1500
auto-thermal reforming (ATR) ✓ ✓ 60e75% 700e1000
69e78% for these different scenarios [56]. These data showed production [61]. At present, the efficiency of hydrogen pro-
the effectiveness of CCS in GHG emission reduction, so the duction from biomass gasification is around 50%, and there is
development of CCS technology and its combined use with CG still room for development and application prospects [63,64].
is effective and very necessary. The gasification agents that can be used for this method
include steam, oxygen and air. Steam (H2O) can facilitate
Partial oxidation (POX) of oil products reforming reactions, resulting in gasification products with
the highest H2/CO ratio and fewer impurities, and is therefore
Partial oxidation (POX), which can also be called “gasification”, considered the most suitable gasification agent [60,65]. The
is the most suitable method to produce hydrogen from feed steam gasification reaction can be simply expressed by the
stocks with high carbon-to-hydrogen ratios such as heavy oil following equation.
and naphtha. Similar to the mechanism of POM, the process
requires an input of pure oxygen to proceed. Oxygen below the Biomass þ H2O / H2 þ CH4 þ CO þ CO2 þ Tar þ Char (7)
stoichiometric ratio of complete oxidation reacts with the feed
stocks to produce a mixture of CO and H2 at a temperature of Biomass steam gasification is an endothermic process that
1200e1350 C [11,57]. occurs at temperatures of 700e1200 C [66]. In fact, the
transformations that occur in gasifiers are very complex.
CnHm þ 0.5nO2/ nCO þ 0.5mH2 (6) Specific chemical reactions that have been identified include
pyrolysis of biomass, tar cracking, combustion of methane,
Canadian company Proton Technologies and the Univer- dry reforming and steam reforming, as well as WGS reactions.
sity of Calgary have collaborated to develop a new technology. The main components of the final gas mixture obtained from
That is, oxygen is injected into the ground containing heavy steam gasification are H2 and CO2, which are then processed
oil, which will spontaneously undergo oxidation at over in a PSA unit to obtain higher purity hydrogen [65].
350 C. The hydrogen produced is brought back to the surface In theory, hydrogen production by gasification can be ach-
and the other products will remain underground and be ieved from various biomass feed stocks, such as sugarcane
sequestered directly to avoid emissions [20]. press-mud [67], bark, vineyard pruning [68], sorghum [69], algal
biomass [70], oil palm [71], and rice husk [72]. According to the
components and properties of different categories of biomass,
Hydrogen production from biomass mixing them in a certain ratio before gasification can effectively
improve the production efficiency. By changing the raw mate-
Considering that fossil fuels are unsustainable, there is an rials and mixing ratio, the composition of the product gas can
urgent need to develop technologies of generating hydrogen be controlled. This method is suitable for feed stocks that are
using renewable energy sources, even though they currently difficult to gasify individually, such as sewage sludge and
contribute only a small fraction of global hydrogen produc- glycerol [73]. Anniwaer et al. used a mixture of banana peel,
tion. Among renewable energy sources, biomass is the earliest Japanese cedar wood and rice husk to produce hydrogen-rich
energy carrier to be used by humans and is still used today gas. Banana peels contain high levels of alkali and alkaline
[58]. Biomass comes from a wide range of sources, including earth metals, which can play a catalytic role in the gasification
wood, grass, agricultural products, crop residues, plant and process. This experiment also confirmed the effect of mixing
animal wastes, municipal solid wastes, food scraps and algae, ratio and temperature on gas yield and that the biomass with
and is seen as an alternative to fossil fuels [58e60]. high silica content of would hinder gasification [74].
Depending on the way of gas generation, direct hydrogen Although hydrogen is produced through a similar ther-
production from biomass can be achieved by two routes: mochemical process, hydrogen production from biomass
thermochemical methods and biochemical processes of mi- gasification is considered to have less adverse environmental
croorganisms. The former include gasification, pyrolysis and impact than that based on fossil fuels because the CO2
liquefaction [23]. Among them, biomass gasification is a rela- released comes from CO2 absorbed while the organisms are
tively mature technology and has been shown to hold great still alive and no excess carbon is entered into the atmosphere
potential for the future. Hydrogen production from biochemical [13,23]. However, biomass gasification also faces its own
processes is currently mainly studied at the laboratory level. problems, namely the high number of impurities in the
In addition to direct methods, it is possible to convert product due to the complex composition of biomass mate-
biomass into storable intermediates firstly and then obtain rials, especially the formation of tar, which can cause clog-
hydrogen from these biomass-derived products [61]. Xu et al. ging, wear and tear of the equipment and failure of the
summarized the progress of research related to the use of catalyst. Only at high temperatures above 1250 C and a resi-
biomass-derived polyols for hydrogen and other chemicals dence time of at least 0.5s the most stable tar can be decom-
production [62]. We will discuss the thermochemical and posed [66,75].
biochemical routes to hydrogen production in detail. To avoid these harmful situations as much as possible,
Guan et al. designed a two-region catalytic gasification unit. In
Biomass gasification the facility, feed stocks pass through the gasification reactor
and the product is transported to the upper catalytic reactor,
Steam gasification of biomass where the tar is catalytically decomposed [76]. Plasma-
Biomass gasification is a typical thermochemical pathway and assisted biomass gasification technology has come up, in
considered an economical method of renewable hydrogen order to promote the tar cracking reaction and reduce tar
residue. On the other hand, it helps to improve reaction ki- lower temperatures than biomass steam gasification, the very
netics. Plasma gasification requires the feed stocks expose to high pressures and demanding pumping capability it requires
extreme high temperature above 2000 C to produce syngas in greatly increase the cost of industrial production [65,81].
the presence of oxidant [77]. Therefore, technology optimization is a necessary process to
achieve commercialization. Some studies have been reported
Supercritical water gasification (SCWG) of biomass on the effects of operating parameters of SCWG technology.
A supercritical fluid is the fluid whose temperature and pres- These factors include operating temperature, pressure, resi-
sure exceed its critical point. For water, the conditions of this dence time, biomass constituents, reactant concentration,
critical point are a temperature of 374 C and a pressure of catalysts and mineral salts [79,82]. The specific impact effects
22.1 MPa. Biomass can be gasified in a special environment that they produce are summarized in Table 3 [78e80].
beyond this critical point, where water acts as both a reaction
medium and a reactant. Water in the supercritical state has a Biological conversion
low dielectric constant, a low number of hydrogen bonds as
well as the high solubility, reactivity and diffusivity. These Certain enzymes contained in microorganisms such as
features mean that organics and gases can be easily miscible to microalgae and cyanobacteria allow them to synthesize
become homogenous phase under this condition, which facil- hydrogen by biochemical action. Biotransformation can be
itates the conversion of reactants [65,78,79]. Supercritical water divided into biophotolysis, photo fermentation and dark
gasification (SCWG) of biomass does not require drying pre- fermentation [83,84]. Unlike all technologies mentioned
treatment of raw materials. So it is suitable for biomass with above, microbial hydrogen production does not require high
high moisture content such as algae and sewage sludge [66]. temperatures and can usually perform at room temperature
Biomass in supercritical water will undergo complex re- and atmospheric pressure. And there is no need to add addi-
actions such as pyrolysis, hydrolysis, condensation, and tional catalysts, because the biological enzymes assume the
dehydrogenation [80]. The main conversion pathways are catalytic function [65]. For dark fermentation, it also enables
shown in Fig. 4. The large molecules such as cellulose, hemi- the reuse of organic wastes simultaneously. Despite these
cellulose and lignin are hydrolyzed into small organic mole- distinctive advantages of bioconversion methods, what
cules such as sugars, which are then catalytically degraded fundamentally prevents them from scaling up production is
into smaller acids, alcohols, phenols, etc., and finally the low hydrogen yield [60].
completely degraded into water gas. After that, hydrogen is
obtained by the WGS reaction [79]. The simplified overall re- Biophotolysis
action is given by the following equation. Biophotolysis can be divided into two forms: direct bio-
photolysis and indirect biophotolysis. For direct bio-
CHxOy þ (2-y)H2O / CO2 þ (2 - y þ 0.5 x)H2 (8) photolysis, microorganisms use light for water
decomposition reactions to produce hydrogen, converting
SCWG technology has been studied at the laboratory level, light energy into storable chemical energy. It occurs in mi-
but commercial applications are lacking. Although SCWG has croorganisms that can perform photosynthesis, such as
high energy conversion efficiency and can be accomplished at algae that contain chlorophyll, and requires sufficient light
Fig. 4 e Schematic diagram of biomass supercritical water gasification [80].

Table 3 e Impact effects of operating parameters in SCWG.

Operating parameters Effects
Temperature At low temperature, the hydrogen yield and gasification rate are low, and then increase
dramatically with the increase of temperature. It is mainly because the dielectric constant of
supercritical water decreases with increasing temperature, which enhances the dissolution of
organic components and favors the free radical reaction. High temperature promotes the
endothermic reforming reaction and facilitates the generation of gas products.
Pressure The effect of reaction pressure on the SCWG process is relatively low but complex. Different
studies have shown inconsistent results. As the pressure increases, the dielectric constant of
supercritical water increases, which is not favorable for hydrogen production. However, high
pressures cause the coking and polymerization to restrain, while favoring the reforming and
WGS reactions.
Feed stocks characteristics In general, the higher heating value of a fuel would make a higher chemical exergy for the fuel
but a lower exergy efficiency.
Reactant concentration Increasing reactant concentrations usually have a negative impact on the gasification process.
Excessive biomass feedstock concentrations lead to a decrease in the water content percent,
which will hinder the steam reforming reaction and the WGS reaction. High reactant
concentrations can also lead to an increase in intermediates such as coke, causing clogging
problems of the reactor.
Resident time In the case of limited reaction rate, prolonging the reaction time is beneficial for completing
reaction and possible to obtain a higher conversion. Note that there exists a critical residence
time, corresponding to the highest conversion. When the reaction time continues to be
extended, the exergy efficiency may decrease due to the methanation reaction.
Catalysts The use of catalyst increases the exergy efficiency for hydrogen production and higher catalyst
concentration means better results. Different types of catalysts also produce different effects.
Alkali and alkali metal salts are significantly more effective. On the one hand, it accelerates the
WGS reaction, on the other hand it inhibits the formation of tar and coke.
intensity to complete the process. Indirect biophotolysis is a CH2O þ H2O /2H2 þ CO2 (11)
two-step process. Firstly, CO2 is fixed as carbohydrates,
which are then broken down by the action of the hydroge- External conditions have significant impacts on the
nase enzyme to produce hydrogen [85]. biochemical process, so the culture environment for bacteria
and light conditions need to be strictly controlled in order to
12H2O þ 6CO2 þ light / C6H12O6 þ 6O2 (9) ensure smooth hydrogen production [91]. It has been reported
that the suitable temperature and light wavelengths were
C6H12O6 þ 12H2O þ light / 12H2 þ 6CO2 (10) 30e36 C and 400e1000 nm, respectively, and the light should
be spatially uniformly distributed among the bioreactor. In
A great challenge it faces is that hydrogenase is highly addition, a strictly anaerobic environment and a near-neutral
sensitive to oxygen. As the hydrolysis reaction, biophotolysis pH (6.8e7.5) are also necessary conditions [90e92]. The opti-
produces both hydrogen and oxygen. However, with the mum environmental conditions vary slightly depending on
increasing oxygen concentration, the activity of hydrogenase the substrate, bacteria species and strain [93,94], while con-
is inhibited and reactions becomes slower [86,87]. Researchers ditions such as substrate concentration and enzyme loading
have already explored ways to avoid excessive oxygen accu- may also affect the results. However, there are still a lot of
mulation. By providing cells with an intermittent sulfur- unsolved problems with photo fermentation, such as low
deficient environment, oxygen can be partially inactivated to energy conversion efficiency and high price of bioreactors [92].
promote hydrogen production [88,89].
In terms of reaction process, biophotolysis represents Dark fermentation
zero pollution, it consumes only water as raw material and Some anaerobic bacteria and microalgae degrade complex
has no additional carbon emissions. Photo fermentation and organic matters into small molecules under anaerobic con-
dark fermentation are considered to be superior methods ditions while producing hydrogen. This process does not
because they simultaneously generate hydrogen and require the provision of light source so it is called dark
consume wastes. fermentation. Dark fermentation can utilize a variety of
carbon sources, including biomass wastes. Large molecules
Photo fermentation of organic matters are first decomposed into soluble carbo-
Photo fermentation for hydrogen production is a process in hydrates and so on, then further hydrolyzed into smaller
which microorganisms use light energy to convert organic matters like monosaccharides. Finally, they would be
substrates into hydrogen and CO2. A typical example is the degraded into small molecules including organic acids and
purple non-sulfur (PNS) bacteria, which primarily relies on alcohols, and H2 and CO2 are produced. Organic products
nitrogenase to catalyze the following reactions in a nitrogen- such as acetic acid and butyric acid can be produced as by-
deficient environment [85,90]. products of the process [95].
If only hydrogen production is considered, the energy Water electrolysis needs to be carried out in an electro-
conversion efficiency of dark fermentation is very low because lyzer. Based on the different types of electrolytes, electrolysis
only a small portion of energy in the substrate is transferred to techniques can be classified into these types: alkaline elec-
hydrogen, while most of it is transferred to other metabolites trolysis (AEL), polymer electrolyte membrane (PEM) electrol-
and remains in the fermentation effluent. This means that ysis, solid oxide electrolysis (SOEL) and alkaline anion
making full use of these by-products can improve the exchange membrane (AEM) electrolysis [24,101e103].
affordability of dark fermentation [96]. However, some of the
intermediates or by-products are inhibitory to biohydrogen Conventional water electrolysis methods
production because they interfere with the normal physio-
logical and metabolic processes of microorganisms. The pos- AEL and PEM electrolysis are performed at temperatures of
sibility of modifying microorganisms at the genetic level is several tens of degrees Celsius. The two types are the most
also being explored to solve the problem [97]. mature electrolysis technologies and commonly used by
hydrogen production plants for commercial purpose [23]. In
Dark-photo co-fermentation AEL device, two electrodes are immersed in a high-
In recent years, coupled dark-photo fermentation technology concentrate alkaline solution, typically KOH or NaOH. Nega-
has emerged, which combines both photo and dark microbial tively charged hydroxide ions act as charge carriers and can
fermentation for hydrogen production, thus complementing cross an anion-selective porous diaphragm, transfer from the
each other. Small organic molecules that cannot be further cathode to the anode in solution, and then generate water
decomposed by dark-fermenting microorganisms can be uti- with the hydrogen ions produced at the anode [104,105].
lized by photo-fermenting microorganisms, while the latter
cannot directly utilize large molecules of complex organic Cathode: 4H2O þ 4e / 2H2 þ 4OH (13)
matters. Fully exploiting the advantages of both and creating a
coupled system can improve the hydrogen production effi- Anode: 2H2O / O2 þ 4Hþ þ 4e (14)
ciency of the overall system and expand the range of available
substrates. The porous diaphragm assumes a very important role,
Dark-photo co-fermentation can be divided into microbial separating the hydrogen and oxygen produced. It must be
co-culture and two-step hydrogen production. Co-culture is durable and highly wettable in alkaline electrolytes, other-
culturing two or more microorganism species in a single wise gas bubbles would be produced and increase resistance
reactor. The availability of this method has been demon- and affect the purity of the gas product. The long-time-used
strated at the laboratory level [98,99]. Pachapur et al. sum- diaphragm material is chrysotile asbestos, but it is not
marized and discussed the relevant studies on co-culture for resistant to alkaline solutions above 80 C and is has been
biohydrogen production in detail [100]. Nevertheless, the banned from commercial use in the EU due to its carcino-
limitations of co-culture are obvious: it is clearly impractical genicity [106].
to inoculate microorganisms with widely different growth An alternative, Zirfon, is a new porous separator material
habits in one system and efficiently produce hydrogen. A that was proposed at the end of 20th century [107,108]. It is
two-step hydrogen production with alternating dark and synthesized from zirconium oxide nanoparticles and poly-
photo fermentation is much easier to achieve. sulfone [109,110]. Zirfon showed great superiority in the tests,
such as low resistance (about 0.1e0.3 U/cm2) and low
hydrogen permeability, which means that only little hydrogen
Water electrolysis-based hydrogen production will mix near the anode. By adjusting and modifying the ma-
terial, such as changing the ratio of raw materials used for
The first time human synthesized hydrogen was by electrol- synthesis, its performance can be further enhanced [110e112].
ysis of water [1,13]. Although the advent of more economical Burnat et al. tested a new composite membrane of mineral
SMR and CG methods made them the predominant source of filler and polysulfone and found that it yielded higher purity
hydrogen contribution, the energy crisis of the 1970s rekin- hydrogen than the commercially used Zirfon membrane [113].
dled interest in electrolysis. Water electrolysis is currently Several new polymeric materials with high stability in alka-
used in some small-scale industrial hydrogen production, line liquids are also being tested at the laboratory level [114].
supplying 4% of the global hydrogen production. The basic mechanism of PEM electrolysis is similar to
With the drive of direct current, water undergoes decom- that of AEL. It follows the same electrochemical reaction,
position reaction, also the inverse reaction of the hydrogen but occurs in an acidic environment. Because it uses an
fuel cell, and produces hydrogen and oxygen. The two kinds of acidic polymer membrane as a solid electrolyte, the charge
gases are produced at the cathode and anode respectively, so carriers in the electrolyte are hydrogen ions (protons), which
they can be easily separated to obtain pure hydrogen and pure is the biggest difference from AEL [115]. The two types of
oxygen. Generating hydrogen from water means that the electrolyzers are shown in Fig. 5 [13]. PEM electrolysis allows
process can be applied over a wider area without regard to for a compact system design, rapid response and higher
local reserves of fossil fuels or biomass. current density [116,117]. In terms of reaction dynamics, it is
a superior technology to AEL and its energy efficiency is a
2H2O / 2H2 þ O2 (12) little higher than AEL. However, PEM electrolyzer requires
noble metals as electrodes, such as iridium, ruthenium and At a temperature of 500e1000 C, water (steam) is decom-
platinum, while AEL can use nickel-based or iron-based posed into hydrogen and oxygen [13,23,101]. The electrolyte is
electrodes [102]. In addition, the service life of PEM elec- generally ZrO2 stabilized with a small amount of Y2O3 (YSZ)
trolysis equipment is shorter due to the degradation of its [127,129]. It is O2 that acts as a charge carrier in this system,
electrolyte during operation, which means that AEL has the so the electrode reaction of SOEL is different from AEL and
advantage in terms of economy and flexibility, unless PEM PEM electrolysis. O2 generated at the cathode moves to the
electrolysis has a significant cost reduction in the short term anode and is then oxidized to oxygen.
[116,118].
In order to make PEM electrolysis technology more Cathode: 2H2O þ 4e / 2H2 þ 2O2 (15)
commercially competitive, researchers are working on
developing new materials as polymer membranes, catalysts Anode: 2O2 / O2 þ 4e (16)
and electrode plates to reduce equipment construction and
operating costs. Non-noble metal materials are economical Basic information and characteristics of AEL, PEM elec-
alternatives. Besides, researchers have tried to apply nano- trolysis and SOEL are shown in Table 4 [13,127,129e132].
fiber membranes in electrode assemblies [119,120]. A major technical challenge comes from the severe de-
For catalysts, molybdenum disulfide (MoS2) and related mands for the electrolyzer material by the operating condi-
compounds represent outstanding catalytic activity tions. Due to the exposure to high temperature and high
[121,122]. Mo et al. found that the combination of first-row humidity, the electrolyzer material must be sufficiently stable
transition metal elements with MoS2 can improve the cat- to ensure the system long-term operation. The anode usually
alytic activity of monolayer MoS2, especially Co-sMoS2, uses strontium-doped lanthanum manganite, which can be
which is able to compete with the Pt-based catalysts used in produced by some inexpensive methods. This material has a
industry [123]. The effectiveness of the cobalt chelate and porous structure and its microstructure is able to remain un-
cobalt oxide based catalysts was also demonstrated. At changed for thousands of hours during testing [130]. The
specific operating voltages, 47 wt% Co3O4-based catalysts cathode material is generally Ni/YSZ cermet, which has been
can outperform even Pt-black [124,125]. Phosphides and used for more than 30 years. However, the agglomeration of
carbides of transition metals are also effective alternative nickel particles has called its stability into question, as evi-
options [126]. denced by the rapid decrease in initial conductivity [131].
Subsequently, some new alternative cathode materials are
High-temperature electrolysis/solid oxide electrolysis (SOEL) reported, including Titanate-based and lanthanide metal-
based composites [130].
SOEL has higher operating power and energy efficiency than A current research trend is to use SOEL in combination
the two room-temperature electrolysis technologies with other technologies to obtain multiple benefits or opti-
mentioned above [127]. In the solid oxide electrolyzer, elec- mize its performance. One example is the combination of
tricity and heat are used together to drive the water decom- SOEL and POM. When the input gas is a mixture of methane
position reaction. In other words, the heat takes over part of and steam, the methane is oxidized on the anode side. The
the energy supply, so the system uses less electricity. SOEL is a overall hydrogen production rate is 2.6 times higher than
late starter in research and is not yet commercially available when steam is fed alone [130].
for hydrogen production, but its inverse process capability Another novel and attractive design is CO2/steam co-
(solid oxide fuel cells, SOFC) and low estimated cost (by 2050) electrolysis by SOEL. It is a low-energy-consumption process
bode well for its future potential [116,128]. compared to electrolysing the two substances separately, and
Fig. 5 e AEL (left) and PEM electrolysis (right) devices [13].

Table 4 e Comparison of hydrogen production technologies by water electrolysis.

AEL PEM SOEL
Electrolyte NaOH/KOH(aq) Polymer(s) YSZ(s)
Charge carriers OH Hþ O2-
Electrode material Ni and Ni alloys Platinum group metals Cermet and doped metal composites
Temperature 60e90 C 50e90 C 500e1000 C
Pressure 2e10 bar 15e30 bar less than 30 bar
Cell voltage 1.8e2.4 V 1.8e2.2 V 0.95e1.3 V
Current density 0.2e0.5 A/cm2 1e2 A/cm2 0.3e1 A/cm2
Efficiency 62e82% 67e84% 81e86%
Stack lifetime (maximum) 90000 h 40000 h 40000 h
System lifetime 20e30 yr 10e20 yr e
Hydrogen production (maximum) 760Nm3/h 30Nm3/h e
Cost (by 2050) ~$600/kWch ~$750/kWch ~$200/kWch
Annual degradation 2e4% 2e4% 17%
Need a diaphragm ✓
Commercial or not ✓ ✓
Advantages Long lifetime Higher current density High energy efficiency

Low cost Compact system design Less electricity consumption
High maturity Rapid response Feasible reversible operation
Large stack size Dynamic advantages Low expected cost
Combination with other technologies
Disadvantages Low current density Need noble metal materials Severe environment
Corrosive electrolyte Short lifetime Unstable electrodes
Mixing of gases High membrane cost Sealing issues
achieves the recycling of CO2 without complicating the electricity to the grid, nuclear reaction processes generate
equipment [133]. The product of co-electrolysis as well as the large amounts of heat that can be utilized. Therefore, elec-
combination is syngas (H2 and CO) instead of pure hydrogen. trolysis of water, high-temperature electrolysis and thermo-
So we will not describe it in detail. chemical methods for hydrogen production can all use
nuclear energy as an energy source supply. Karaca et al.
Anion exchange membrane (AEM) electrolysis evaluated nuclear energy-based hydrogen production
methods, including conventional electrolysis, high-
In AEM electrolysis system, the electrolyte is a low- temperature electrolysis and some thermochemical cycles,
concentration alkaline solution or water, rather than the in terms of their environmental impacts. The results showed
high-concentration of KOH used in AEL [102]. The AEM that high-temperature electrolysis is cleaner than the normal
concept was introduced at the beginning of the 21st century, electrolysis method [136]. For high-temperature electrolysis
and this technology is still in early development [134]. In terms coupled to nuclear power, the heat transfer process is very
of principle, AEM electrolysis is relatively similar to PEM critical, so the development of efficient heat exchangers is
electrolysis, with the main difference being the charge car- expected [137].
riers. However, the equipment cost of AEM electrolysis is The coupling system of photovoltaic electrolysis (PV-EL)
lower [104,135]. Once this technology comes to maturity, it proved to be very clean, yet very costly. It is also not sufficiently
may have a higher commercial value. energy efficient due to the level of development of photovoltaic
materials [3]. Therefore, it is not a really attractive option
Clean electricity and electrolysis for hydrogen production presently [13], unless the carbon emissions of hydrogen pro-
duction by fossil fuel thermochemical technology are not
Electricity and heat, as secondary energy sources, need to be acceptable and the economic cost of carbon reduction is greater
generated from primary energy sources. According to the data than that of photovoltaic electrolysis [138].
from IEA, more than 60% of the world's total electricity in 2018 The challenge with wind-powered hydrogen production is
came from fossil fuels [5]. An obvious fact is that electricity the instability of the wind energy supply, as the wind is
based on new energy sources is more environmentally dependent on local climatic condition variations. Therefore, it
friendly than electricity from fossil fuels. For the purpose of is necessary to consider alternative power supply options if
obtaining truly clean hydrogen, water electrolysis hydrogen the plant tries to use wind power as an energy supply for the
production systems are desired to be coupled with new energy electrolysis process. Currently, wind power to hydrogen is
electricity generation systems, the most interesting of which being evaluated for feasibility or has been established as a
are nuclear, wind and solar photovoltaic power generation. pilot in many regions, including Yazd province (Iran), Berlin
Nuclear power plants have been built and operated in and Brandenburg (Germany), Hebei province (China), Turkey,
many countries around the world. In addition to supplying Chile and Argentina [139e143].
Currently 2000e3000 thermochemical cycles have been stud-

Water thermolysis and thermochemical cycles ied, of which only about 10% are available for large-scale
hydrogen production [2]. Thermochemical cycles are usually
As with electrolysis, the pyrolysis of water follows the general combined with solar or nuclear reactors in an integrated
reaction Eq. (12). The thermal decomposition reaction done in system to obtain heat and electricity [19].
one step is called “water thermolysis” [144]. Circulating mul-
tiple reaction steps with the help of other substances can Sulfur-iodine (SeI) cycle
reduce the temperature requirements. During the multi-step Of all the thermochemical cycles that have been applied, the
process, only water is decomposed into hydrogen and oxy- SeI cycle developed by General Atomics is considered to have
gen. Other substances are both reactants of some reaction and the highest efficiency prospect [4,151]. The United States and
products of another reaction and are continuously recycled in Japan have carried out a lot of work in the technological
these reactions. This multi-reaction cycle are called “ther- development of SeI cycle, expecting it to be the primary
mochemical cycle". choice for clean energy hydrogen production in the future. In
China, the Nuclear Institute of Nuclear and New Energy
One-step water thermolysis Technology, Tsinghua University has started the research of
SeI cycle hydrogen production since 2005, and the SeI cycle
One-step thermolysis reaction follows a very simple chemical
equipment with a hydrogen production scale of 60 NL/h was
principle. However, the decomposition of water requires a
put into trial operation in 2014 [19,152].
large amount energy, which is provided by heat, so the reac-
This cycle contains three reactions. In the first reaction,
tion system has a very high operating temperature. It is re-
water, I2 and SO2 react to form H2SO4 and HI. The other two are
ported that water can be decomposed at a temperature
the decomposition of HI to produce hydrogen and I2, and the
>1700 C, and to achieve complete decomposition requires a
decomposition of H2SO4 to produce oxygen, water and SO2.
high temperature of over 4000 C [23,145]. Baykara et al.
The I2 and SO2 produced in the latter two reactions can be
evaluated the cost of hydrogen production via water ther-
reused in the first reaction. The equations are as follows.
molysis based on solar energy and the cost was as high as $68/
GJ for a small-scale operation (172 GJ/yr) [146]. Even if this
2H2O þ SO2 þ I2 / H2SO4 þ 2HI (17)
assessment was based on the technology level in 1980s, this
value is exorbitant. According to a 2004 literature report, the
2HI / H2 þ I2 (18)
cost is 12.5 times of that via CG hydrogen production or 3.3
times of that via commercial water electrolysis [147]. Bidard
H2SO4 / H2O þ SO2 þ 0.5O2 (19)
et al. compared water electrolysis and thermolysis processes
under nuclear power supply and demonstrated that ther-
The SeI cycle process is shown in Fig. 6.
molysis is not competitive in terms of efficiency and avail-
The first reaction, named Bunsen, is an exothermic reac-
ability for the time being [148].
tion that can occur at room temperature. The decomposition
Thermal energy can also be provided by biomass and
of H2SO4 requires an environment of 850 C. It consists of two
geothermal heat [149]. However, under such extreme condi-
consecutive parts, i.e., it is first decomposed to water and SO3
tions, the thermal energy sources may not support the system
at a relatively low temperature, and then SO3 continues to be
to operate continuously [11]. On the other hand, it is difficult to
decomposed into SO2 and oxygen at a higher temperature
find suitable high-temperature resistant materials to build
[153]. Obviously, the only substance that really changes
such installations while controlling the cost.
throughout SeI cycle is water, accompanied by the production
Another problem is that hydrogen and oxygen cannot be
of hydrogen and oxygen.
produced on two different plates, as in electrolysis. The
In theory, there are no redundant reactions in SeI cycle and
product obtained by water thermolysis is a mixture of two
all substances involved are raw materials, end products or
gases, which are easily recombined into water, not easily
recyclable substances [144]. However, the products of the
separated and explosive. Quenching can prevent the recom-
Bunsen reaction, H2SO4 and HI, may continue to react in side
bination of hydrogen and oxygen, but only at low tempera-
reactions to form sulfur or hydrogen sulfide, which can lead to
tures, where the temperature must drop sharply by 1500e2000
clogging of the equipment [4]. Therefore, the hydriodic phase
K in a few milliseconds. Some membrane reactors, centrifu-
(HIx) and sulfuric acid phase need to be purified to prevent
gation and supersonic jets allow the separation of gases in
side reactions.
situ, but are still limited by technology [27,150]. Therefore,
Many studies have focused on the optimization of Bunsen
water thermolysis is not currently attempting to enter com-
reaction conditions, since process parameters and operation
mercial or industrial production. These limitations lead to the
mode can affect purification and side reactions. For example,
rise of thermochemical cycles.
both an increase of solution temperature and an increase of
iodine concentration favor the removal of H2SO4 from HIx. In
Thermochemical cycles
fact, the reaction (18) is often carried out under conditions of an
excess of I2 that eight times higher than the stoichiometric
Compared to one-step thermolysis, hydrogen production
value [154e156]. Under conditions below atmospheric pressure,
from thermochemical cycles requires lower temperature and
purification of H2SO4 promotes the conversion of HI and the
effectively solves the problem of separating hydrogen and
reaction (18). Although the purification of HIx does not promote
oxygen, as they are produced in different reaction steps.
this reaction, it facilitates the removal of H2SO4 from HIx [157].
Fig. 6 e SeI cycle process for hydrogen production.
Another challenge is that the decomposition reaction of As the number of reactions decreases, the complexity of
H2SO4 has no kinetic advantage and requires the assistance of the process and the number of reactors is reduced. Each cycle
a catalyst to advance the reaction. However, the strong has its advantages and disadvantages and a reasonable choice
corrosiveness brought by H2SO4 at high temperatures places can be made depending on the production scenario. From the
high demands on reactor materials and catalysts [152]. Both environmental impact point of view, the four-step CueCl
silicon-containing ceramic materials, such as SiC and Si3N4, cycle is less impactful than the three- and five-step cycles
and FeeSi alloys that can form a passivation layer on the because it has a lower thermal energy requirement [163].
surface have good corrosion resistance [158]. Pt-based cata-
lysts showed high activity and stability in SeI cycle. Zhang Two-step metal oxide cycles
et al. compared several catalysts and found that the material A metal oxide cycle is generally a two-step reaction. It is
synthesized by loading Pt on SiC had the highest stability usually expressed as follows (in the case of a metallic element
[159]. More economical non-noble metal catalysts have also in the reduced state as a monomer).
been investigated, but their suitability in terms of lifetime for
prolonged use in industrial production must be considered. Su M þ H2O / MO þ H2 (20)
et al. prepared copper chromite catalyst by vacuum freezing
drying, which possessed an activity close to that of platinum MO / M þ 0.5O2 (21)
catalyst and remained stable over a test time of 70 h [160].
For reaction (19), the decomposition of HI into I2 and where M represents a metal element. Of all the thermo-
hydrogen is reversible and its equilibrium conversion is very chemical cycle pathways to hydrogen production, this type
low even at high temperatures [156]. In order to promote the requires relatively high temperatures, typically above 1500 C,
reaction to the right and increase the HI conversion, it is because of the large amount of heat required for the decom-
necessary to transfer hydrogen or I2 out of the reaction system position of stable metal oxides [164]. Metal oxide cycles prefer
in time. The approach is to develop a membrane reactor with a to rely on concentrated solar energy rather than nuclear en-
hydrogen-selective permeation membrane, along the same ergy because such high temperatures are challenging for nu-
idea as in SMR technology increasing methane conversion. clear reactor heat production. Metals that have been found to
However, in the SeI cycle, the membrane also needs to cope perform this process include iron, zinc, cerium, etc.
with the strong corrosive environment caused by the presence Charvin et al. reported a two-step thermochemical cycle
of HI [161]. based on iron oxides to generate hydrogen drove by solar
energy, and the key to exploiting its potential lies in the sys-
Copper-chlorine (CueCl) cycles tem optimization and scaling up of the solar reactor [165].
The CueCl cycle is also a promising approach. Compared to SeI Steinfeld et al. used the Zn/ZnO system to perform a cycle
cycle, it has a lower reaction temperature, so it can be integrated with an energy efficiency of 29%. They pointed out that to
more easily with a wide range of energy sources [4]. Depending achieve economic feasibility, an effective means of separation
on the number of reactions contained in the cycle, CueCl cycles is needed to avoid the recombination of Zn and O2 chemistry
is divided into two-step, three-step, four-step and five-step cy- at high temperatures which would interfere with the normal
cles. The specific reactions and the principles of these cycles intra-cycle reactions [166]. Abanades et al. successively
involved are shown in Table 5 and Table 6 [162].
Table 5 e Reactions and equations for hydrogen production.

Number Reactions Equations T (K)
1 Disproportionation nH2O(l) þ 4CuCl(s) / 2Cu(s) þ 2CuCl2$nH2O(aq) 350
2 Hydrolysis H2O(g) þ 2CuCl2$mH2O(s) / CuO$CuCl2(s) þ 2HCl(g) þ mH2O(g) 650
3 H2O(g) þ 2CuCl2(s) / CuO$CuCl2(s) þ 2HCl(g) 673
4 H2O(g) þ 2CuCl2$nH2O(s) / 0.5O2(g) þ 2HCl(g) þ 2CuCl(l) þ nH2O(g) 823
5 Cl2 hydrolysis H2O(g) þ Cl2(g) / 0.5O2(g) þ 2HCl(g) 1073
6 Cu chlorination 2Cu(s) þ 2HCl(g) / H2(g) þ 2CuCl(l) 723
7 CuCl chlorination 2CuCl(s) þ 2HCl(aq) þ nH2O(l) / H2(g) þ 2CuCl2$nH2O(aq) 473
8 Oxy-chlorination 2CuCl(s)$nH2O(g) / CuO$CuCl2(s) þ 2HCl(g) þ (n-1)H2O(g) 650
9 Thermolysis CuO$CuCl2(s) / 0.5O2(g) þ 2CuCl(l) 800
10 CuCl2 thermolysis 2CuCl2$nH2O(g) / 2CuCl(l) þ Cl2(g) þ nH2O(g) 773
11 Drying (spray) 2CuCl2$nH2O(aq) / 2CuCl2$mH2O(s) þ (n-m)H2O(g) 550
Costs of different methods

Table 6 e Reactions included in different CueCl cycles for
hydrogen production.
Cost is the most important determinant of technology
Cycle Reactions included in the process
commercialization. It determines the effectiveness of the
Two-step cycle 4e7 plant and whether the users can get affordable hydrogen and
Three-step cycle a 4-6-1 related products or not. In general, now the most economi-
Three-step cycle b 7-9-8
cally advantageous are SMR and CG, which have been in use
Three-step cycle c 5-7-10
Four-step cycle a 1-6-9-8
for many years. The addition of CCS technology has led to cost
Four-step cycle b 3-7-9-11 increases of 9.1% and 21.6%, respectively. Biomass gasification
Five-step cycle 2-6-9-1-11 is also inexpensive because it can use some wastes as feed
stocks instead of already commercialized fossil fuels. Micro-
bial hydrogen production shows attractive costs, but the cost
proposed the feasibility of the CeO2/Ce2O3 and SnO2/SnO calculation is now based mainly on laboratory studies and it is
systems for hydrogen production. not yet possible to determine the capital investment for real
High temperatures pose many challenges for its applica- production.
tion, including sintering and deactivation of circulating ma- Most of the emerging technologies require advanced
terials. Some poly-metal/metal oxide composite materials equipment to work well, and the cost invested in the con-
have attracted the attention of researchers because they can struction of the facilities raises the initial cost of hydrogen
hinder sintering to some extent. e.g. nickel ferrite supported production. For example, photovoltaic electrolysis has the
on calcium-stabilized zirconia [167], first-row transition highest cost of all methods. The costs of water electrolysis
metal-doped cerium oxide [168], etc. To realize the large-scale and thermolysis are related to the sources of primary energy,
application of metal oxide cycle, future research should focus with nuclear-based processes generally having relatively low
on the selection and improvement of metal oxide raw mate- costs. The costs of high temperature electrolysis and ther-
rials, the efficient aggregation of solar energy and the effective mochemical cycles have very wide ranges of variability. It is
control of the reaction process. worth noting that their minimum values are low, implying
In addition to the above three types of thermochemical cy- they can be used as inexpensive methods under well-
cles, some other feasible cycles have been proposed, including controlled construction and operation processes. These
CaeBr cycle [169], MgeCl cycle [170], FeeCl cycle [171], ZneSeI methods may assume a larger contribution of hydrogen
cycle [4], etc. Although each cycle process has unique charac- products in the future.
teristics, they are not yet comparable to the maturity of SeI There are many works collating the costs of hydrogen
cycle, and no remarkable advantage has been found to imme- production methods, and we have selected some to show in
diately replace the SeI cycle as the preferred thermochemical Table 7.
hydrogen production scheme for the time being.
Environmental impact comparison
Costs and life cycle environmental impacts of Global warming potential (GWP), acidification potential (AP),
hydrogen production methods eutrophication potential (EP), abiotic depletion potential
(ADP) and human toxicity potential (HTP) are common in-
In order to compare the pros and cons of different hydrogen dicators used in the life cycle environmental impacts
production methods, including the various consumptions and assessment. We primarily focus on GWP, as it represents the
emissions of the whole process, much literature has quantita- GHG emissions from the whole process, which is the most
tively assessed their capital costs, operating costs and life cycle obvious environmental effect from hydrogen production.
environmental impacts. For comparison purposes the func- This is followed by AP and ADP (fossil), which represent acid
tional unit was identified as the production of 1 kg of hydrogen. substance emissions and consumption of fossil fuel re-
All data in the following are given based on this functional unit. sources, respectively.
Table 7 e Costs of various hydrogen production technologies.

Method Cost ($/kg H2) Refs.
Fossil fuels to hydrogen SMR 2.08 [11,172]
SMR with CCS 2.27
CG 1.34
CG with CCS 1.63
ATR with CCS 1.48
Biomass to Hydrogen Biomass gasification 1.77e2.77 [11,13]
Direct biophotolysis 2.13 [11,172]
Indirect biophotolysis 1.42 [11,172]
Photo fermentation 2.83 [11,172]
Dark fermentation 2.57e6.98 [11,13]
Electrolysis Grid electrolysis 5.73e8.54 [13]
PV electrolysis 5.78e23.27 [11,172]
Wind electrolysis 5.27e9.37 [11,13]
Nuclear electrolysis 3.56e7.00 [11,13]
High-temperature electrolysis (SOEL) 2.89e6.03 [4,13]
Thermolysis & thermochemical cycles Nuclear thermolysis 2.17e2.63 [11,172]
Solar thermolysis 7.98e8.40 [11,172]
SeI cycle 1.99e14.85 [4,13]
CueCl cycle 1.71e14.20 [4,13]
CaeBr cycle 7.06 [23]
MgeCl cycle 3.67 [4]
However, the results obtained from different literatures Therefore, technologies using new energy sources are often
have very different values for some indicators, especially for assessed focusing on GWP and AP instead of ADP. This leads
hydrogen production via clean energy. This may be due to the to a lack of data richness in ADP, which prevents us from
difficulty of obtaining normative parameters for methods that making more in-depth comparisons.
are not in large-scale production, so that the inventory data Biomass gasification has an intermediate GWP and AP. It
used for the evaluation are different or require more self- has less environmental impacts than fossil fuel-based
defined parameters. We will list the maximum, minimum methods but larger than electrolysis and thermochemical
and average results instead of a single value. The specific data cycles based on new energy sources. Considering the current
are shown in Table 8. Because some technologies such as state of the art, biomass gasification offers an alternative op-
microbial hydrogen production are still limited to the labora- tion during the period of transition from fossil fuels to water
tory research stage, it is not possible to make an accurate life- as the source of hydrogen.
cycle assessment, so this table does not contain the full range The GWP of hydrolysis process depends mainly on the
of hydrogen production methods. source of electrical energy, which can have a very significant
Fossil fuel-based methods, i.e. CG and reforming of some effect on the results [163]. If the grid electricity is used ac-
fuels, are seen to have the greatest negative impacts on the cording to the current electricity structure, a very large envi-
environment because of its very high GWP and AP values. In ronmental impact is obtained, with a GWP of 29.21 kg CO2 eq
particular, CG, with its GWP of 22.99 kg CO2 eq, is the second and a AP of 69.0 g SO2 eq, respectively, which exceeds even CG
highest of all hydrogen production methods, after electrolysis (22.99 kg CO2 eq, 59.7 g SO2 eq) and SMR (11.98 kg CO2 eq, 15.2 g
based on grid. As the result shows, incorporating CCS tech- SO2 eq). If the electricity is generated based on wind, solar or
nology in the fossil fuel hydrogen production process can nuclear energy, GWP and AP are significantly reduced. This
result in significant GHG reductions. It is estimated that the result means that the coupling of clean electricity with elec-
incorporation of CCS can reduce the GWP of CG by 71.7e81.7% trolysis systems is essential. As shown in Fig. 7, all new
[55,56]. For SMR, there is a 69.1% GWP reduction in the average energy-based approaches have low GWP and AP (M10-M16),
level. The specific effect depends on the efficiency of CO2 except for a moderate level of AP from biomass power
sequestration. However, CCS technology has not been pro- electrolysis.
moted in practical applications. Thermochemical cycles based on nuclear energy have a
The ADP of fossil fuel hydrogen production is also an relatively small environmental impact. Assuming a scenario
important indicator because fossil fuels are not only the where the energy supply comes from nuclear energy, the
source of energy but also feed stocks to provide hydrogen different modes of cycles are compared and SeI cycle is
atoms, implying a larger consumption. The calculations in cleaner than CueCl cycle. And the least environmental impact
literatures for primary energy consumption are of CueCl cycles comes from the four-step cycle. Similarly, if
183.2e198.4 MJ for SMR [175e177] and 213.8e333.2 MJ for CG grid power is used, the GWP and AP of the CueCl cycle are
[51,55,184], respectively, so SMR is a better choice for energy respectively 15.9 and 14.8 times higher than in the nuclear-
friendliness. Other technologies have lower ADP values based condition and the AP exceeds that of electrolysis as
because they do not require fossil fuels as feed stocks. the highest value.
[54,173,174,181]
[53,54,173e177]
References.
[136,174,182]
[136,174,183]
[53,54,179]
[53,54,180]
[51,53e56]
[174,179]
[173,174]
[174,183]
[55,56]
[176]
[178]
[136]
[163]
[53]
[53]
Minimum
11.0
14.5
76.6
8.4
0.2
2.1
3.4
2.4
2.8
AP (g SO2 eq)
Maximum
139.0
28.9
37.1
11.8
99.5
8.1
4.8
4.3
9.6
Table 8 e GWP and AP of different hydrogen production methods, including average, maximum and minimum values.
Average
15.2
59.7
32.0
17.0
22.5
69.0
29.0
91.7
4.2
5.1
4.3
6.1
4.4
3.4
6.2
Minimum
10.56
19.42
28.60
12.30
3.90
4.14
2.67
2.40
0.03
0.37
0.42
0.41
0.56
Fig. 7 e GWP and AP of different hydrogen production

methods, an average value for each method.
GWP (kg CO2 eq)
Conclusion and recommendation

Maximum
13.80
25.28
29.54
15.90
3.50
7.14
4.40
3.00
2.21
2.50
2.00
0.86
1.35
As a clean and sustainable new energy source, hydrogen is

gradually developing as an effective alternative to fossil
fuels, contributing to the control of GHG emissions and
global temperature change. Choosing the right routes for
hydrogen production is critical, and it determines the sus-
Average
11.98
22.99
12.20
17.90
29.21
14.67
tainability of hydrogen. Now, hydrogen is mainly derived

3.70
4.87
9.55
3.54
0.71
2.70
1.08
1.82
1.24
0.64
0.92
from fossil fuels, but there are many studies focusing on

hydrogen from cleaner sources. SMR will remain the domi-
nant technology in the short term because of its maturity,
and the advent of membrane reactor gives it additional ad-
High-temperature electrolysis (based on nuclear)
vantages; CG may be more applicable in some regions due to

local resource distribution.
Hydrogen production from renewable energy sources is
gradually playing a more important role and is constantly
Production method
being optimized technologically. Among them, water elec-

Electrolysis (based on biomass)
CueCl cycle (based on nuclear)

Electrolysis (based on nuclear)
trolysis is currently the most feasible for application, and

SeI cycle (based on nuclear)
Electrolysis (based on wind)
Electrolysis (based on solar)
CueCl cycle (based on grid)

Electrolysis (based on grid)
Alcoholic waste reforming
this technology is changing from AEL to the more flexible

PEM. In the past few years, EU, US and Japanese companies
Biomass gasification
Methanol reforming
have launched PEM electrolysis hydrogen production plants

Ethanol reforming
and other supporting products to promote application and to

SMR with CCS
scale up. In China, the megawatt-scale PEM technology

CG with CCS
hydrogen production project of Anhui Electric Power Cor-

poration is expected to be in operation by the end of 2021
SMR
CG
[185].
The prospect of nuclear energy in hydrogen production
industry attracts interest. High-temperature gas-cooled re-
actors are being actively developed and nuclear hydrogen
M10
M11
M12
M13
M14
M15
M16
M17
M1
M2
M3
M4
M5
M6
M7
M8
M9
production demonstration facilities are planned worldwide.

The U.S., Japan and China have piloted facilities for SeI cycle. Changjiang Scholars and Innovative Research Team in Uni-
CueCl cycle requires lower temperature and has received versity (IRTe13026).
much attention in recent years. Now, the thermochemical
cycle technology looks forward to the optimization of reaction
conditions. On the other hand, advances in nuclear technol-
references
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Review and Comparison of Various Hydrogen Production Methods Based On Costs and Life Cycle Impact Assessment Indicators

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i n t e r n a t i o n a l j o u r n a l o f h y d r o g e n e n e r g y 4 6 ( 2 0 2 1 ) 3 8 6 1 2 e3 8 6 3 5

Available online at www.sciencedirect.com

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

Review and comparison of various hydrogen

Mengdi Ji a, Jianlong Wang a,b,*

highlights graphical abstract

Various H2 production methods

article info abstract

Steam methane reforming (SMR)

Steam methane reforming, or natural gas steam reforming, is

Fig. 4 e Schematic diagram of biomass supercritical water gasification [80].

Table 3 e Impact effects of operating parameters in SCWG.

Fig. 5 e AEL (left) and PEM electrolysis (right) devices [13].

Table 4 e Comparison of hydrogen production technologies by water electrolysis.

Advantages Long lifetime Higher current density High energy efficiency

Currently 2000e3000 thermochemical cycles have been stud-

Fig. 6 e SeI cycle process for hydrogen production.

Table 5 e Reactions and equations for hydrogen production.

Costs of different methods

Table 7 e Costs of various hydrogen production technologies.

Fig. 7 e GWP and AP of different hydrogen production

Conclusion and recommendation

As a clean and sustainable new energy source, hydrogen is

tainability of hydrogen. Now, hydrogen is mainly derived

from fossil fuels, but there are many studies focusing on

vantages; CG may be more applicable in some regions due to

being optimized technologically. Among them, water elec-

CueCl cycle (based on nuclear)

trolysis is currently the most feasible for application, and

CueCl cycle (based on grid)

this technology is changing from AEL to the more flexible

have launched PEM electrolysis hydrogen production plants

and other supporting products to promote application and to

scale up. In China, the megawatt-scale PEM technology

hydrogen production project of Anhui Electric Power Cor-

production demonstration facilities are planned worldwide.

Acta 2021;369:137684. https://doi.org/10.1016/ evolving electrocatalysts. Int J Hydrogen Energy

2019. https://news.bjx.com.cn/html/20190311/967884. purification of H2SO4 and HIx phases in the iodineesulfur

[173] Suleman F, Dincer I, Agelin-Chaab M. Comparative impact Energy 2019;44:21193e203. https://doi.org/10.1016/

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