Art - Graficos de Cilindros

Journal of Energy Storage 64 (2023) 107196
Contents lists available at ScienceDirect
Journal of Energy Storage

journal homepage: www.elsevier.com/locate/est
Review article
State-of-the-art hydrogen generation techniques and storage methods: A

critical review
Dan Tang a, Guang-Lei Tan b, *, Guo-Wei Li a, Jin-Guang Liang a, *, Shah Masood Ahmad c,
Ayesha Bahadur d, Muhammad Humayun e, Habib Ullah f, Abbas Khan g, M. Bououdina e, *
a
School of Mechanical Engineering, Yingkou Institute of Technology, Yingkou 115014, China
b
Liaoning Key Laboratory of Chemical Additive Synthesis and Separation, Yingkou Institute of Technology, Yingkou 115014, China
c
Institute of Chemical Sciences, University of Peshawar, 25120 Peshawar, Pakistan
d
Department of Chemistry, Bacha Khan University Charsadda, 24420, KP, Pakistan
e
Department of Mathematics and Sciences, College of Humanities and Sciences, Prince Sultan University, Riyadh, Saudi Arabia
f
Department of Renewable Energy, Faculty of Environment, Science and Economy, University of Exeter, Penryn Campus, Cornwall TR10 9FE, United Kingdom
g
Department of Chemistry, Abdul Wali Khan University Mardan, 23200, KP, Pakistan
A R T I C L E I N F O A B S T R A C T
Keywords: Hydrogen is a clean, versatile, and energy-dense fuel that has the potential to play a key role in a low-carbon
Fossil fuels energy future. However, realizing this potential requires the development of efficient and cost-effective
Hydrogen energy hydrogen generation and storage technologies. Hydrogen can be generated from a variety of sources,
Hydrogen storage materials
including fossil fuels, biomass, and renewable energy sources such as solar and wind. In regard to the renewable
Storage methods
energy sources, this paper presents a review of the state-of-the-art in hydrogen generation methods including
Applications
water electrolysis, gasification, dark fermentation, steam reforming, photocatalytic water splitting and water
thermolysis. Further, this paper presents a review of the various hydrogen storage methods, including
compression, liquefaction, liquid organic carriers, and solid-state storage. These technologies offer the potential
for improved efficiency, safety, and environmental performance, and may play a key role in the transition to a
hydrogen-based energy system. Finally, the advantages and challenges of hydrogen energy, and future per
spectives on the improvement of hydrogen storage methods are well emphasized. Overall, the development of
efficient and cost-effective hydrogen generation and storage technologies is essential for the widespread adoption
of hydrogen as a clean energy source. Continued research and development in this field will be critical to
advancing the state-of-the-art and realizing the full potential of hydrogen as a key element in a sustainable
energy future.
1. Introduction and rockets [7]. The hydrogen economy is an infra-structure employed

to supply the desired energy through hydrogen fuel instead of fossil fuels
In the current era, energy storage has become the most vital issue and its main goal is to produce hydrogen mostly from the readily
because of the rapid depletion of non-renewable fossil fuels energy existing sources of energy in order to substitute the fossil fuels employed
sources. Besides, the products obtained as a result of the combustion of in industry, transportation, and other sectors. Thus, hydrogen energy
fossil fuels are hazardous to the environment and human [1–3]. As an has been considered an everlasting solution to the global energy de
alternative clean and green form of renewable energy source, hydrogen mand, related environmental issues, and the depletion of non-renewable
is highly recommended to minimize or eliminate such energy and energy sources due to population growth and industrial development.
environmental issues. Interest in hydrogen energy can be traced back to Though the challenges related to the fossil fuels economy are devas
the 1800 century, but it got a keen interest in 1970 due to the severe oil tating, the hydrogen economy growth would have massive benefits for
crises [4–6]. Interestingly, the development of hydrogen energy tech the economy, environment, energy security, and consumers. The most
nologies started in 1980, because of its abundant use in balloon flights crucial constituents of the hydrogen economy include its generation,
* Corresponding authors.
E-mail addresses: tgl@yku.edu.cn (G.-L. Tan), liangjinguang@yku.edu.cn (J.-G. Liang), hu203@exeter.ac.uk (H. Ullah), mbououdina@psu.edu.sa (M. Bououdina).
https://doi.org/10.1016/j.est.2023.107196
Received 18 January 2023; Received in revised form 10 March 2023; Accepted 17 March 2023
Available online 27 March 2023
2352-152X/© 2023 Published by Elsevier Ltd.
D. Tang et al. Journal of Energy Storage 64 (2023) 107196
conversion, storage, transportation, and applications [8,9]. storage materials. Herein, the purpose of this comprehensive review is to
The rapid conversion of fossil fuels to hydrogen energy has been shed the light on sustainable energy resources with a particular focus on
hindered by extensive scientific, economic, and technological com methods of hydrogen generation, hydrogen storage materials, advan
plexities. It is highly difficult to store and transfer hydrogen energy tages and challenges, and future perspectives on the improvement of
obtained from a battery or electricity owing to its variation from other hydrogen storage. We believe that this review article will provide a road
fuels. Compared to other fossil fuels, hydrogen is not stable and its map for researchers not only working on hydrogen storage materials but
generation needs high energy. Besides, hydrogen is combustible and also working in the relevant fields.
oxidizes the storage systems like containers. Hence, to utilize it for
various applications including automotive and electrical, its physical 2. Hydrogen generation
state should be transformed [10–12]. Thus, due to the vast potential
benefits of the hydrogen economy, worldwide governments are In fact, hydrogen has been recognized as a vital gas in the atmo
spending a huge budgets on enhancing the prospects of energy systems. sphere which is the constituent of liquor, water, and hydrocarbons.
Due to the non-toxic and renewable merits of hydrogen, its burning Hydrogen generation from low-cost and clean sources is of utmost
release only water vapors into the atmosphere, and there is no leaking importance because hydrogen is usually referred to as the energy
and assembling alarms because of its quick dissipation [13]. The energy transporter, and not its source. Various techniques used for hydrogen
per mass of hydrogen is 142 MJ, which is higher than any of the hy production involve water electrolysis, gasification, dark fermentation,
drocarbon fuels. It has three times greater energy content by weight than steam reforming, photocatalytic, and water thermolysis [36]. In this
that of gasoline, and four times lower energy content by volume section, various techniques of hydrogen production will be presented
compared to that of gasoline [14]. Thus, compared to gasoline, and discussed in detail.
hydrogen burns more rapidly. Hydrogen has 3.2 times less energy
density compared to that of natural gas and almost 2700 times less en 2.1. Water electrolysis
ergy density than that of conventional gasoline. This means that
hydrogen has been regarded as an energy carrier rather than a source of Water electrolysis comprises only 4 % by volume of hydrogen gas
energy. In this regard, hydrogen can store and deliver energy in a more worldwide because of several economic barriers. However, it is an
practical form [15–17]. Naturally, hydrogen has compatibility with fuel environmentally friendly method to generate hydrogen from sustainable
cells, and its high efficiency (i.e., 60 %) than diesel (i.e., 45 %) and water and also evolve oxygen as a by-product. In this technique, water is
gasoline (i.e., 22 %) made it a potential candidate for future use [18]. utilized as a reactant which dissociates into hydrogen and oxygen by
Hydrogen steam generators have been recommended in the medical applying an electric potential. Notably, water electrolysis is an expen
sector for various applications, such as sterilization and cleaning of sive technique since the costly electricity utilized is generated from non-
medical equipment, as well as for air and surface disinfection. One of the renewable sources. Generally, this method can be categorized into four
key advantages of hydrogen steam generators is that they produce high- types including (i) alkaline water electrolysis (AWE), (ii) anions ex
quality, high-purity steam that is free of impurities and contaminants. change membranes (AEM) electrolysis, (iii) solid oxides electrolysis
This makes it ideal for use in medical facilities, where strict standards for (SOE), and (iv) proton exchange membrane (PEM) water electrolysis,
sterilization and cleanliness must be maintained [19–21]. In addition, depending on the electrolyte and ions-based agents (i.e., H+, OH− , O2− ).
hydrogen steam generators are highly efficient and can produce steam Every year, approximately 380,000 kg of H2 is produced through water
quickly and with minimal energy consumption. This makes them an electrolysis with a rate of 53.4 kWh/kg hydrogen consumption [37–39].
economical and sustainable option for medical facilities that require a Various types of water electrolyzers are described below.
reliable source of steam for their operations. Moreover, hydrogen steam
generators are also environmentally friendly, as they produce steam 2.1.1. Proton exchange membrane electrolyzer
using only water and hydrogen gas, with no harmful byproducts or In the 1960s, General Electric introduced the PEM electrolyzer.
emissions. This is important for medical facilities that are committed to PEM’s basic components include cathode, anode, and electrolytes, while
reducing their environmental impact and maintaining a clean and (Pt, Ru, Ir, and Pt) catalysts and carbon materials serve as the most
healthy environment for their patients [22–24]. common anode and cathode materials [40,41]. A Proton Exchange
In an advanced hydrogen economy, it is predicted that hydrogen can Membrane (PEM) electrolyzer uses an electric current to split water
be used both for stationary and onboard tenacities. For stationary ap (H2O) into hydrogen (H2) and oxygen (O2) gases. The electrolyzer
plications, hydrogen storage is less challenging compared to onboard contains an anode and a cathode separated by a PEM, which selectively
applications, whereby several challenges have to be resolved [25]. allows protons (H+) to pass through while blocking electrons (e− ) and
Worth noting, the weight of the storage system (i.e., gravimetric gas diffusion. During electrolysis, water is fed into the anode chamber,
hydrogen density) for stationary applications is of less concern where it is oxidized to produce oxygen and positively charged hydrogen
compared to the volume of the storage system or the volumetric ions (H+). The electrons generated by this reaction flow through an
hydrogen density. In contrast, for onboard applications, the volumetric external circuit to the cathode, where they react with the hydrogen ions
and gravimetric densities are vital. Nevertheless, the volumetric density and water to produce hydrogen gas and negatively charged hydroxide
is rather less vital for large-size vehicles. It is important to note that a ions (OH− ). The PEM allows the hydrogen ions to pass through to the
suitable amount of hydrogen is needed for onboard storage to cover a cathode, where they combine with electrons to form hydrogen gas,
rational distance without any refueling of the vehicle. Thus, a method of while blocking the passage of oxygen and other gases. The membrane
storage that gives high volumetric and gravimetric energy densities is plays a critical role in separating the anode and cathode compartments
required [26–28]. Furthermore, low enthalpy change, reasonable and enabling the selective passage of protons while preventing gas
operating conditions (temperature and pressure), as well as fast kinetics crossover. This separation allows the gases produced at the anode and
of hydrogen storage and release are mandatory. In addition, low cost, cathode to be collected separately, ensuring high purity and preventing
safety, and public reception are other critical aspects. Nowadays, the formation of explosive gas mixtures [42–44].
numerous physical and chemical methods for hydrogen storage with Generally, in a PEM electrolyzer, the electrolyte used is typically
specific features and storage capacities, are proven to be promising in deionized or distilled water, which serves as a source of protons and
the advancement of the future hydrogen economy [29,30]. hydroxide ions. The PEM electrolyzers are typically operated at a tem
Although, several review articles on hydrogen storage materials have perature range of 50–80 ◦ C. The optimum temperature range depends on
been published in the past [31–35], there still a need of further review the specific catalyst and membrane materials used in the electrolyzer.
articles that highlight the recent progress in the design of hydrogen The pressure of the reactant gases, such as hydrogen and oxygen, can
2
affect the efficiency and performance of the electrolyzer. The PEM have an effect on AWE performance. Furthermore, while an electrolyte’s
electrolyzers are typically operated at relatively low pressures, ranging temperature has no effect on hydrogen generation and lowers the
from 1 to 30 bar. The current density can affect the efficiency and necessary power, an electrolyte solution’s concentration does. As a
durability of the electrolyzer [45,46]. PEM electrolyzers typically result, the primary difference between AWE and PEM is the type of
operate at relatively high current densities, ranging from 0.5 to 3 A/cm2. electrolyte used, with PEMs employing a compact polymer membrane
The PEM membranes require a certain level of humidity to function electrolyte and AWEs employing a corrosive liquid electrolyte [52–54].
properly and the PEM electrolyzers typically require a humidification Fig. 1b presents a schematic illustration of the AWE cell [55].
system to maintain the proper level of humidity. The catalysts such as Pt
or Pt alloys are used to facilitate the electrochemical reactions in the 2.1.3. Alkaline anion exchange membrane
anode and cathode compartments. The type and amount of catalyst used The alkaline anion exchange membrane (AAEM) electrolyzer uses a
can affect the efficiency and cost of the electrolyzer [47,48]. PEM basic electrolyte and an anion exchange membrane to split water (H2O)
electrolyzer has the significant advantage of being able to deal with the into hydrogen (H2) and oxygen (O2) gases. In an AAEM electrolyzer, the
load fluctuations perfectly owing to its quick response, and its hydrogen anode, and cathode are separated by an anion exchange membrane that
generation purity can reach up to 99.99 %. To date, the main disad allows negatively charged hydroxide ions (OH− ) to pass through while
vantage and challenging aspect has been the high cost of the noble blocking other ions and gases. During electrolysis, water is fed into the
metals utilized in this electrolyzer [47–50]. Fig. 1a presents a schematic anode chamber, where it is oxidized to produce oxygen gas and hy
illustration of the PEM electrolyzer cell [51]. droxide ions. The hydroxide ions are transported across the AAEM to the
cathode compartment, where they react with incoming electrons and
2.1.2. Alkaline water electrolyzer protons to form hydrogen gas [56,57]. The basic electrolyte used in the
The AWE is an advanced type which is dependable and safe, as well AAEM electrolyzer provides the necessary hydroxide ions for the reac
as easy to manufacture on a large scale. Two electrodes are immersed in tion. The anion exchange membrane selectively allows the hydroxide
a water solution containing 20 to 40 % of the NaOH or KOH. The ions to pass through while blocking other ions and gases. The membrane
electrodes are separated by a diaphragm in the electrolyte solution, also separates the anode and cathode compartments, preventing gas
which allows hydroxide ions and H2O molecules to pass through. For crossover and ensuring the high purity of the hydrogen produced.
purity and safety, the diaphragm also separate H2 and O2. As a result, the Compared to a PEM electrolyzer, the AAEM electrolyzer operates at
purity of the hydrogen produced ranges from 99.5 to 99.9 %, with cat higher pH and lower pressure. This can reduce the cost and complexity
alytic gas purification processes increasing up to 99.99 %. Notably, the of the system, but it also requires different materials that can withstand
material type and thickness of the diaphragm, anode, and cathode all the highly basic environment [58,59]. In an AAEM electrolyzer, instead
Fig. 1. Schematic representation of PEM water electrolyzer. Reproduced with permission from ref. [51]. Copyright 2020, MDPI. (b) Schematic representation of the
AWE cell. Reproduced with permission from ref. [55]. Copyright 2020, MDPI. Schematic representation of AEM water electrolyzer cell. Reproduced with permission
from ref. [61]. Copyright 2020, Wiley. Schematic representation of SOE cell. Reproduced with permission from ref. [66]. Copyright 2019, Elsevier.
3
of 20 to 40 % NaOH and KOH solution, it combines a low-concentration could involve implementing water-saving technologies, such as low-
alkaline solution with a polymeric compact electrolyte membrane (i.e., flow fixtures, rainwater harvesting systems, and greywater reuse sys
Mg–Al layered double hydroxide). Additionally, the cathode of an tems. It may also require changes in behavior and water management
AAEM is fabricated from Ni and Ni–Fe components, while the anode is practices, such as reducing outdoor water use, promoting xeriscaping,
fabricated from Ni foams or titanium components [59,60]. Fig. 1c pre and implementing water-efficient landscaping [77–79]. Thus, the water
sents a schematic illustration of the AEM electrolyzer cell [61]. electrolysis technique has been regarded as the less attractive method
considering its cost of hydrogen generation [80]. To address these
2.1.4. Solid oxide electrolyzer challenges, governments, organizations, and communities in dry regions
Despite the fact that SOE works at high temperatures, the required may need to invest in building electricity infrastructure, such as power
electricity amount to power its electrolysis at high temperatures is grids, renewable energy systems, and energy storage solutions. This can
considerably less than that required for electrolysis at low temperatures. require significant upfront investments but can yield long-term benefits
The use of inexpensive thermal energy or waste heat results in an in in terms of economic development, improved quality of life, and
crease in system efficiency. In addition, the anode and electrolytes are reduced environmental impact.
ceramics, while cathode is fabricated from a mixture of La1-xSrxMnO3
(LSM) and Yt-stabilized ZrO2 (50/50 wt%) [62]. To produce superior 2.2. Gasification
catalysts and electrode materials, extensive research and development
are needed. The process for hydrogen generation is described below: the Gasification is another useful method for hydrogen generation. This
cathode reaction first converts steam to H2 at cathode, and the oxide method has two types; coal gasification and biomass gasification. In coal
anions formed at cathode are the pathways through which solid elec gasification, coal reacts with oxygen and steam at optimal conditions
trolytes generate O2 at anode side [63–65]. Fig. 1d presents a schematic and generates hydrogen, while evolving carbon monoxide as a by-
illustration of the SOE cell [66]. The water electrolysis reaction can be product with small constituents of nitrogen, hydrogen sulfide, carbon
expressed by Eqs. (1)–(3) as mentioned below [67,68]: dioxide, methane, hydrochloric acid, ammonia, carbonyl sulfide, oils,
tars, high molecular weight hydrocarbons, etc. In the coal gasification
(Cathode) 4H+ (aq) + 4e− →2H2 (g) (1)
technique, the coal is partly oxidized by oxygen and steam, thereby
generating the CO and H2 merged with steam and CO2 (i.e., syngas) in a
(Anode) 4OH− (aq)→2H2 O(l) + O2 (g) + 4e− (2)
reactor under high temperature and pressure. In order to enhance the
Overall reaction : 2H2 O(l)→2H2 (g) + O2 (g) E◦ = − 1.24 V (3) hydrogen yield, the syngas passes through a water gas shift reaction. To
extract the sulfur element or sulfuric acid, the gaseous product is usually
The benefits of water electrolyzers (renewable energy) include; (1) washed out [81]. Notably, a temperature in the range of 649–1480 ◦ C
the elimination or reduction of transportation as well as the storage costs and pressure in the range of 14.69–1200 psi is required in coal gasifi
and can be employed as stand-alone systems for end-user sites, (2) their cation. In this method, gasifiers are usually set up as fixed beds, move
firmness and prospect of exceptional hydrogen generation against the able beds, fluidized beds, and/or inlet flows. About, 18 % of the global
photoelectrochemical, (3) lack of the electricity infrastructure desires in hydrogen is obtained by gasification technique [48,82]. On the other
dry regions, and (4) their commercial availability [69]. In fact, the lack hand, in the biomass gasification technique, biomass is heated to
of electricity infrastructure in dry regions can present several challenges, generate hydrogen gas, while, carbon monoxide, carbon dioxide, and
including dependence on fossil fuels, limited access to basic services, water as by-products. In this technique, after filtering the gas, steam is
reduced economic opportunities, and an inability to address climate injected to turn the electricity from carbon monoxide gas into hydrogen
change. In the absence of reliable electricity infrastructure, people in dry during a reaction of water-gas-shift. Biomass gasification has an
regions may rely heavily on fossil fuels such as diesel generators, which importance over coal gasification due to its low cost and has been
can be expensive, polluting, and unsustainable. Without electricity, it regarded as one of the most powerful techniques used for hydrogen
can be difficult to access basic services such as healthcare, education, production over decades. In this technique, wood waste and rice husk
and clean water [70,71]. Lack of refrigeration can also make it chal are the commonly used feedstocks, while several feedstocks comprise
lenging to store and transport food and medicine. Without electricity, it paper waste, sugarcane waste, wood chips, food waste, sandstone
can be challenging to run businesses, create jobs, and generate income. wastewater, palm oil, polyethylene, etc. Constructing the enormous
This can limit economic opportunities and exacerbate poverty in dry biomass plants is more expensive than the coal plants because biomass
regions [72,73]. The lack of electricity infrastructure can make it diffi has less capacity per unit volume and its shipment is costly [37,83].
cult to implement clean energy solutions such as solar and wind power, Fig. 2a represents the step-wise coal gasification process. It has been
which are essential for mitigating climate change and reducing green investigated that transition metals (especially Ni) reveal excellent H2
house gas emissions [74,75]. Some existing challenges during water generation and tar cracking during biomass gasification, and their per
electrolysis include the commercialization of hydrogen production formance is due to their exceptional bonds breaking ability. For
through water electrolysis by reducing investment and operating costs. instance, Kraisornkachit et al. [84] demonstrated that during biochar
The erratic nature of energy resources and water consumption rate can gasification, the rate of carbon conversion and H2 evolution increased
present several challenges for ensuring efficient and sustainable with the increase in the content of Ni, and the 10 wt% catalyst revealed
resource use [76]. The possible considerations for investigating their excellent H2 evolution and H2/CO (Fig. 2b). Likewise, Zhang et al. [85]
efficiencies include: (i) renewable energy sources such as solar, wind, investigated that 2 % Ni content in the catalyst yield maximum amount
and hydroelectric power can be variable and intermittent, depending on of H2 as shown in Fig. 2c. Multi-functional catalysts composed of multi-
weather conditions and other factors. To investigate their efficiency, it metals have also been widely investigated in H2 generation and it was
may be necessary to analyze data on energy generation and usage over found that multi-metal composite catalysts exhibit high performance
time, identify patterns and trends and develop strategies to optimize than the single metal catalysts [86]. For instance, Zhang et al. [87]
energy use, storage, and distribution. This could involve using energy demonstrated that Fe0.64Ni0.36 catalyst produced the best H2 evolution
management systems, energy storage technologies, and demand with a 33.66 mmol H2 g− 1 biomass, and a low tar yield of 5.66 mg g− 1
response programs that help balance energy supply and demand. (ii) (Fig. 2d).
Water consumption rates can vary depending on factors such as climate,
geography, population density, and water management practices. To 2.3. Dark fermentation
investigate water efficiency, it may be necessary to analyze water usage
patterns and identify opportunities for conservation and reuse. This This technique is extensively utilized for hydrogen production from
4
Fig. 2. (a) Schematic representation of the key steps involved in coal gasification. (b) Yield of gas products and the carbon conversion. Reproduced with permission
from ref. [84]. Copyright 2018, Elsevier. (c) Yield of gas products with different mass ratio percentage of PS char/Ni. Reproduced with permission from ref. [85].
Copyright 2020, Elsevier. (d) Yield of gas products over the catalysts. Reproduced with permission from ref. [87]. Copyright 2019, Elsevier.
renewable biomass including algal biomass, agricultural residues, catalysts is an effective strategy [95]. Besides, the improvement in H2
organic waste, and lignocellulose biomass. In this technique, the meta generation efficiency of the metal catalysts could be attributed to their
bolic energy of biomass is converted into hydrogen energy in the quantum size effects and huge surface areas, that remarkably promote
absence of light. Due to their anaerobic biomass degradation aptitude, the effects of electron adsorption and enhances transfer of electron be
dark fermentative bacteria could be classified as facultative or obliga tween the hydrogenase growth and HPB [96]. For instance, Zhang et al.
tory anaerobes. The production of hydrogen in the dark fermentation [97]. Fabricated manganese doped magnetic carbon (MDMC) for
process mainly relies on the temperature, pH, inoculum, and type of improvement of the bio–H2. The results revealed that the particles of
substrate [88]. It has been demonstrated that utilizing the dark MnFe2O4, Fe2O3 and MnCO3 were attached to the activated carbon and
fermentation technique to generate hydrogen from wastewater or formed MDMC which displayed a large surface area of 110.92 m2⋅g− 1.
biomass can drastically lower its production cost to 2.7 $US/kg. For The batch fermentation method was used to investigate the effect of
acetate-type dark fermentation, the chemical Eq. (4) used in the indus various inorganic additives on the bio-H2 yield. The bio-H2 generation
trial process can be expressed as below [89]: was carried out in a bio-reactor with a working capacity of 500 ml. In
each bio-reactor, glucose and peptone with a concentration of 10 g/L
C6 H12 O6 + 2H2 O→4H2 + 2CH3 COOH + 2CO2 (4)
and 0.2 g/L, respectively were used as the substrates of dark fermenta
The H2 generation from biomass has great perceptions in comparison tion. Each bio-reactor was filled with 30 % (v/v) of the seed sludge and
to other conventional techniques of H2 production, because this method 70 % (v/v) deionized water. The optimized catalyst yield a 211 and 148
utilizes renewable biomass raw material for dark fermentation to ml H2⋅g− 1 glucose at 400 mg⋅L− 1 MDMC (at 37 ◦ C) and 600 mg⋅L− 1
generate H2 with low pollution [90]. Hence, H2 generation from biomass MDMC (at 55 ◦ C) as revealed in Fig. 3(a, b). Likewise, Zhang et al. [98]
received considerable attention. However, it always exhibit low effi employed cobalt ferrite nanoparticles in H2 generation through dark
ciency for H2 production during dark fermentation. The activity of H2 fermentation. The optimized content (i.e., 0.1–0.4 g/L) of the catalyst
generating bacteria (HPB) is usually decreased because of the massive remarkably improved the dark fermentation reaction. A significant H2
organic load, and the trace elements such as Iron (Fe), Zinc (Zn), Man yield of 205.24 mL⋅g− 1 glucose was obtained at a dosage content of 0.4
ganese (Mn), Copper (Cu), Cobalt (Co), and Nickel (Ni) deficiency as g⋅L− 1 as displayed in Fig. 3(c, d). Some catalysts used as additives for
well as deviation from optimal pH. These trace elements can be added to improving H2 generation in dark fermentation are summarized in
fermentation media in the form of mineral salts or complex nutrients to Table 1.
promote optimal growth and metabolic activity of microorganisms. The
specific requirements of trace elements may vary depending on the type 2.4. Steam reforming
of microorganism and the substrate used in the fermentation process
[91–94]. To overcome this shortfall, promoting the hydrogenases ac This is the most widely employed method for large-scale hydrogen
tivity during the metabolic pathway via the incorporation of metal production. It is estimated that about 48 % of the world’s hydrogen
5
Fig. 3. The manganese doped magnetic carbon (MDMC) concentration effect on the bio-H2 production. (a) Yield of H2 at 55 ◦ C, and (b) Yield of H2 at 37 ◦ C.
Reproduced with permission from ref. [97]. Copyright 2019, Elsevier. The CoFe2O4 concentration effect on the bio-H2 production. (c) H2 yield, and (d) rate of H2
generation. Reproduced with permission from ref. [98]. Copyright 2021, Elsevier.
demand is fulfilled by this technique. In steam reforming technique, gas are mixed to generate hydrogen, while carbon monoxide (12 %) and
research on glycerol, methane, ethanol, methanol, toluene, and acetic carbon dioxide (10 %) gases are also evolved. Actually, this reaction step
acid has been carried out, whereas steam reforming of ethanol and proceeds at 800 ◦ C and is highly endothermic. In the steam reforming
methanol has been widely investigated for hydrogen generation in the technique, hydrogen enrich syngas is generated and when the efficiency
last few decades [105]. Steam reforming of methanol is the commonly of the method is approximately 76 %, then the syngas ratio is 2.4:1.
used and economic method for hydrogen generation with natural gas as During the process, pure hydrogen is isolated from other gases with a
the feedstock. In steam reforming of methanol, methanol and steam are pressure swing absorption phenomenon [108]. Notably, in methanol
converted into synthesis gas, which is a mixture of hydrogen (H2), car steam reforming, alcohols or hydrocarbon fuels are highly reactive to
bon monoxide (CO), and carbon dioxide (CO2). The chemical reactions dimethyl ether, methanol, and oxygenated hydrocarbons at 180 ◦ C.
involved in steam reforming of methanol are expressed in Eqs. (5)–(7) Besides, a high hydrogen-to-carbon monoxide reformat ratio can be
[106,107]: produced which enhances hydrogen generation. However, carbon di
( ) oxide is also produced which is hazardous to the natural environment
CH3 OH→CO + 2H2 Endothermic reaction, ΔHr = + 90.2 kJ mol− 1 (5)
[109]. Fig. 4a represents the steam reforming system [110]. The reac
( ) tion of steam methane reforming can be represented by Eq. (8) [111]:
CO + H2 O→CO2 + H2 Exothermic reaction, ΔHr = − 41.1 kJ mol− 1 (6)
CH4 + H2 O→3H2 + CO (8)
The overall reaction of steam reforming of methanol can be repre
sented as: Steam ethanol reforming received an enormous interest for hydrogen
( ) generation due to the high yield (i.e., 6 mol H2/mol ethanol). However,
CH3 OH + H2 O→CO2 + 3H2 Overall reaction, ΔHr = + 49.1 kJ mol− 1 the high cost of steam ethanol reforming is extremely challenging for
(7) hydrogen generation and purification systems. In 2013, the actual cost
of the steam ethanol reforming technique was estimated to be 0.27 US
The steam methanol reforming process is typically carried out at high
$/kWh for 94.95 % efficiency [112]. Based on current estimates, the cost
temperatures (around 200–300 ◦ C) and high pressures (around 20–30
of producing hydrogen from ethanol using steam reforming is around
atm) in the presence of a catalyst, which enhances the reaction rate and
$1.50–2.00 per kg of hydrogen produced. This estimate includes the cost
reduces the energy required for the process. The catalyst used for steam
of feedstock (ethanol), utilities (steam, natural gas), and capital and
reforming of methanol is typically a mixture of copper, zinc, and
operating costs of the reforming process. However, it should be noted
aluminum oxides, which promotes the desired chemical reactions while
that the cost of producing hydrogen from ethanol can vary widely
minimizing undesired side reactions. The resulting synthesis gas can be
depending on the specific conditions and scale of production, and new
used as a feedstock for various chemical processes, such as the produc
developments in technology and process optimization could potentially
tion of ammonia, methanol, and synthetic fuels [107].
reduce the cost of production in the future [113]. On the other hand, the
On the other hand, in steam methane reforming, steam and methane
cost of hydrogen generation by the steam methanol reforming technique
6
was estimated in 2008 around 1.28 ($/kg) with a 3 % cost for operation
[100]
[101]
[102]
[103]
[100]
[104]
and maintenance. With this technique, 97 % pure hydrogen with an
[99]
Ref.
efficiency of 80 % can be achieved. Nowadays, hydrogen generation
through steam methanol reforming has a market value of approximately
2.9 $/kg [112,114–116]. Steam methane reforming is the foremost
Increase in H2 from 0.95 to 1.9 mol/mol-glucoseutilized (+100 %)

method for H2 generation, however, its viability for generating low
Increase in H2 from 2.07 to 2.54 mol/mol-glucose (+22.7 %)

Decrease in H2 from 1.44 to 1.39 mol/mol-glucose (− 3.5 %)
Increase in H2 from 2.33 to 2.48 mol/mol-glucose (+6.4 %)

carbon footprint H2 is usually inhibited by the high temperature (i.e.,
Increase in H2 from 20.25 to 24.73 mL/g COD (+22.1 %)

>800 ◦ C), reaction complexity, and high energy forfeits related to the
separation of H2 and CO2. To overcome this problem, Ling et al. [117]
Increase in H2 from 247 to 250 mL/g VS (+0.9 %)

Increase in H2 from 247 to 338 mL/g VS (+37 %)
developed a reactor comprising Pd–Ag membrane and Ni catalyst/
hydrotalcite sorbent. High purity H2 and CO2 were achieved with
methane conversion >99 % as well as selectivity and yield of H2 and CO2
>99 % at a temperature of 400 ◦ C and pressure of 1 bar. Further, a stable
generation of H2 and CO2 was confirmed for 6000 cyclic tests. Recently,
Yu et al. [118] fabricated CuCrO2-CeO2 catalysts and employed in steam
Activity at optimal dosage
methanol reforming to generate H2. The optimized 50CuCrO2-50CeO2

catalyst revealed superior H2 generation (i.e., 2059.65 ml STP min− 1
g⋅cat− 1) at 400 ◦ C (Fig. 4b). Furthermore, high stability was achieved.
Glycerol steam reforming with the assist of catalysts is also a feasible
method used for H2 generation [119]. For instance, Padmakar et al.
[120] reported Co dispersed SrO-ZrO2 catalyst and employed in glycerol
steam reforming for H2 generation. The optimized 15%Co dispersed
SrO-ZrO2 catalyst demonstrated excellent performance by completely
transforming glycerol into H2, CO, CH4, and CO2 products with H2 yield
Conditions for fermentation
of 73 % (Fig. 4(c, d)). The enhanced performance of the catalyst was

attributed to the existence of octahedral sites, small particles of Co, solid
solution of Sr-Zr-Co-O, basicity, and strong interaction between metal
and support. In addition, stability of the catalyst was maintained for 50
Batch 37 ◦ C
Batch 37 ◦ C
Batch 33 ◦ C
Batch 37 ◦ C
Batch 37 ◦ C
Batch 37 ◦ C
Batch 55 ◦ C
h. Table 2 summarizes the catalysts utilized in steam reforming of

pH = 5.5
pH = 5.6
pH = 5.5
pH = 7
pH = 7
pH = 7
pH = 7
ethanol, methanol and methane.
2.5. Photocatalytic water splitting

Enterobacter cloacae DH − 89
Diesel contaminated soil
In the last few years, the photocatalytic water splitting technique has
been widely utilized for hydrogen production. In this technique, a
Enterobacter cloacae
Anaerobic sludge
Anaerobic sludge
Anaerobic sludge
semiconductor photocatalyst is excited through the aid of solar light to

Sewage sludge
generate electrons and holes in a water/methanol system, where holes

are captured by methanol and the electrons react with water and
Inoculum
generate hydrogen. In this technique, an appropriate semiconductor

with proper conduction band potential (i.e., 0 V for water reduction
versus the NHE) as well as valence band potential (i.e., +1.23 V for
water oxidation versus the NHE) is required, and the incident photons
Wastewater
Substrates
energy should be greater or equal to the energy band gap of the semi
Glucose
Glucose
Glucose
Glucose
Glucose
Glucose
conductor. Under light irradiation, the electron-hole pairs are produced

which then transfer to the photocatalyst surface and take part in
reduction and oxidation reactions. It is worth noting, that the morpho
logical and electronic structures of the photocatalysts play a critical role
Optimal dosage (mg/L)
in light absorption and charge transport. In addition, high crystallinity

Catalysts used in dark fermentative hydrogen production.
and surface-active sites of the photocatalyst particles are found to have a

positive effect on the water-splitting activity [133]. The schematic
illustration of photocatalytic water-splitting reaction and the redox po
tentials of various semiconductors versus the NHE for water splitting are
2.5
5.7
2.5
100
25
60
5
depicted in Fig. 5(a, b), respectively [134]. The overall photocatalytic

water-splitting reactions can be expressed by the following Eqs. (9)–(11)
[135]:
Range (mg/L)
2.5 to 12.5
0.25 to 50
0.25 to 50
25 to 200
20 to 100
(9)
5.7 to 50
2H+ + 2e− →H2

5 to 20
/
H2 O + 2 h+ →2H+ + 1 2 O2 (10)
/
1
(11)
Cu Nanoparticles
Pd Nanoparticles
H2 O→H2 + 2 O2
Fe Nanoparticles
Fe Nanoparticles
Ni Nanoparticles
Ni Nanoparticles
Ni Nanoparticles
Due to its low cost and efficient hydrogen generation, the photo
Catalysts
catalytic water-splitting technique received tremendous attention in the

Table. 1
past few years. TiO2 is the most investigated semiconductor photo

catalyst in this technique due to its proper redox potential. However, the
7
Fig. 4. (a) Schematic representation of the steam reforming system. Reproduced with permission from ref. [110]. Copyright 2013, Elsevier. (b) Rate of H2 generation
over the 50CuCrO2-50CeO2, CuCrO2 and commercial Cu/Zn/Al catalysts during steam methanol reforming at corresponding temperatures. Reproduced with
permission from ref. [118]. Copyright 2022, Elsevier. Effect of temperature on the H2 production over 15CSZ catalysts during GSR. Time on stream studies at 700 ◦ C
for the 15CSZ11 catalyst. Reproduced with permission from ref. [120]. Copyright 2022, Elsevier.
Table. 2
Various catalysts utilized in steam reforming and their products concentrations.
Catalysts Conversion % H2 conc. % CH4 conc. % CO conc. % Ref.
Ni0.91La0.09(10)/CeO2 100 % C2H5OH 78 33 2 [121]

Cu/Zn/Al2O3 93.1 % CH3OH 72 0.6 [122]
Ni/Al2O3 99.4 % CH4 87 [123]
Ni/Ce–Al2O3 95.7 % CH4 97.3 [124]
Ni(21)/MgO 100 % C2H5OH 98 2 24 [125]
Ni0.58-Mg0.41(17)/CeO2 91 % C2H5OH 74 1 17 [126]
Cu/ZnO/Al2O3 96 % CH3OH 72 0.5 [127]
Ni0.5Co0.5(15)/g-Al2O3 100 % C2H5OH 92 2 8 [128]
Ni-Cu/La0.8Ce0.2Mn0.6Ni0.4O3 100 % C2H5OH 43.5 31.5 32.9 [129]
Pt/Al2O3 96 % CH3OH 65 1.5 [130]
Pt/Al2O3 91 % CH3OH 73.2 1.7 [131]
Ni/@Ca5Al6O14 94 % CH4 92 [132]
fast charge carrier’s recombination rate and low solar energy utilization production and inhibit the charge carrier’s recombination rate
greatly limit its practical applications [136]. Thus, the formation of [140,141]. Alternatively, Zhao et al. [142] prepared AuNPs/TiO2 com
heterostructure photocatalysts with other semiconductors with proper posite and employed it as photocatalysis for H2 generation. It was
band alignments is widely investigated [137,138] For instance, Liu et al. confirmed that the AuNPs/TiO2 composite catalyzed photocatalytic H2
[139] reported the fabrication of TiO2/rGO-Mo2C composite photo generation by 281 times faster compared to the bare TiO2 (Fig. 5e). This
catalyst and employed in water splitting to evolve H2. The composite considerably enhanced photocatalytic H2 evolution was attributed to the
produced 880 μmol h− 1 g− 1 of H2 with an apparent quantum efficiency enhanced charge transfer due to the surface plasmon resonance effect of
of 2.64 %, which was about 5.5 times higher than TiO2/rGO composite Au nanoparticles (Fig. 5f). Some narrow band gap semiconductors
and 88 times higher than bare TiO2 (Fig. 5c). This enhanced activity was which could be employed as potential photocatalysts for efficient
attributed to the fact that rGO performed as electron mediator during hydrogen generation under visible irradiation includes g-C3N4 [143],
electron transfer, while Mo2C served as active sites for H2 generation MoS2 [144], CdS [145], and CdSe [146]. Yet, photocatalysis has been
(Fig. 5d). Besides, the noble metal nanoparticles as electron mediators considered a low-efficiency solar-to‑hydrogen (STH) conversion tech
and cocatalysts are employed to reduce the energy barrier of hydrogen nique. Its STH conversion efficiency (i.e., 0.2 % reported), is
8
Fig. 5. (a) Schematic illustration of the photocatalytic water splitting via the assist of semiconductor photocatalyst. (b) Semiconductors band structures and the
redox potentials versus NHE for water splitting. Reproduced with permission from ref. [134] Copyright 2017, Wiley. (c) Photocatalytic H2 generation over the TiO2,
TiO2/rGO and TiO2/rGO-Mo2C photocatalysts. (d) Proposed mechanism for H2 evolution over the TiO2/rGO-Mo2C and Mo2C photocatalysts. Reproduced with
permission from ref. [139]. Copyright 2021, The American Chemical Society. (e) Photocatalytic H2 evolution over the TiO2, and AuNPs/TiO2 photocatalysts. (f)
Schematic mechanism for H2 evolution over the AuNPs/TiO2 composite. Reproduced with permission from ref. [142]. Copyright 2019, MDPI.
considerably lower than the other solar-driven hydrogen generation clear. In case of bulk water dissociation, thermodynamic equilibrium is
techniques [147]. Photocatalysis is an environmentally friendly tech usually not maintained or displaced because of the removal of some
nique and considered the best option among all other hydrogen pro dissociated byproducts. This technique is seldom utilized on industrial
duction technologies. It has the lowest economic status because this and commercial scales because of the constraints of the materials. The
technology is new, and substantial improvements are underway to reaction can be expressed by Eq. (12) as mentioned below [161]:
reduce its initial cost [81]. Table 3 summarizes various photocatalysts
H2 O + heat→H2 + O2 (12)
utilized in photocatalysis for water splitting, along with their apparent
quantum efficiencies (AQE). The efficiency of water thermolysis can be improved by stripping
away one of the existing byproducts or another possibility through by
tuning the chemical potential. Water thermolysis has been established
2.6. Water thermolysis
on a mixed ionic electronic conductive membrane with O2 permeability.
Since there exists any moving part or electronic circuit in a water
For water thermolysis technique, a heat source is utilized to disso
thermolysis membrane reactor, it should require less maintenance than
ciate water molecules into hydrogen and oxygen since there exist co
chemical looping or electrolysis processes. However, in future studies,
valent bonds in water molecules. Water thermolysis involves a single
life cycle and economic studies should be carried out for comparison
step process, in which the direct thermal decomposition of water occurs.
with the existing systems [162–165].
Actually, this process is reversible and the prevention of products
recombination back to form water is highly crucial. In this technique,
3. Hydrogen storage methods
the tolerable temperature for the reaction is limited to 2500 K, which
tentatively allows a dissociation level of over 4 % under atmospheric
Over the last two decades, various methods for H2 storage have been
pressure. The reactor involves components fabricated from superior
investigated. In this section, we reviewed several methods including the
refractory materials which are capable of lasting in chemically active
compression, liquification, liquid-organic carriers, and solid state
environments and high temperatures (≥1500 K) [158–160]. During the
method. These methods are schematically illustrated in Fig. 6.
experiments, water dissociation takes place when water vapors come
into contact with a hot dense surface. The reaction mechanism is still not
Table. 3
Various photocatalysts utilized in water splitting for hydrogen evolution.
Photocatalysts Junction type Light source Hydrogen evolution AQE % Ref.
P-doped g-C3N4/Ti3C2 p-n junction 300 W Xe lamp λ > 420 nm 627.1 μmol⋅h− 1⋅g− 1 8.7 % at 350 nm [148]
CdS/g-C3N4 Type II 300 W Xe lamp λ > 420 nm 3670 μmol⋅h− 1⋅g− 1 2.03 % at 420 nm [149]
Cd0.5Zn0.5S Phase junction 300 W Xe lamp λ > 430 nm 17.9 mmol⋅h− 1⋅g− 1 43 % at 425 nm [150]
Rutile TiO2/anatase TiO2 Phase junction 300 W Xe lamp UV–Visible 29.63 mmol⋅h− 1⋅g− 1 45.6 % at 365 nm [151]
NiS/g-C3N4 Other 300 W Xe lamp λ > 400 nm 3297 mmol⋅h− 1⋅g− 1 1.25 % at 420 nm [152]
P-doped Cd0.5Zn0.5S1-x Phase junction 500 W Xe lamp λ > 400 nm 32 μmol⋅h− 1⋅g− 1 0.15 % at 365 nm [153]
Al-doped SrTiO3 Facet junction 300 W Xe lamp 35.4 mmol⋅h− 1⋅g− 1 95.9 % at 360 nm [154]
GaInZnON@GaInON Core shell 300 W Xe lamp λ > 420 nm 603 μmol⋅h− 1⋅g− 1 3.5 % at 430 nm [155]
maleoyl-modified g-C3N4 Core shell 150 W Xe lamp λ > 420 nm 2013 μmol⋅h− 1⋅g− 1 3.2 % at 430 nm [156]
g-C3N4-Ternary homojunction Ternary junction 300 W Xe lamp λ > 420 nm 3806.5 μmol⋅h− 1⋅g− 1 1.76 % at 420 nm [157]
9
Fig. 6. Schematic illustration of the hydrogen storage methods.
3.1. H2 compression 450 bar, but can resist up to 700 bar. Type IV: These are comprised of
composites and similar to Type III. Type III liners are metal and con
The most common type of storage is high-pressure compressed H2. In tributes only 5 % to the mechanical strength, while Type IV liners are
addition to being a well-developed technology, this technique provides predominantly polymeric and constructed of high density polyethylene.
high rates of H2 filling as well as release. Furthermore, energy is not They store H2 up to 700 bar [168].
required for H2 to be released. However, compressing H2 to higher There is another modified version of Type IV vessel that has been
pressures, on the other hand, results in an important loss of 13–18 % of reinforced with space-filling skeletons to achieve substantially greater
its heating value, which has an impact on the overall cost of the oper volumetric and gravimetric density of H2 [169]. For instance, Barthe
ation. Fortunately, when pressure rises, the power required for lemy et al. [170] described in detail the construction elements of H2
compression only slightly rises. Because it is impossible to put spherical storage tanks (see Fig. 7). In Type III and IV vessels, H2 at 700 bar would
containers onboard, H2 is stored in cylindrical shaped containers. It is be a viable option, with a recharge time of three minutes and a driving
essential to utilize a vessel material that is not only inexpensive but also range of 500 km. At 700 psi, the energy density of H2 in a Type IV vessel
relatively lightweight and can handle high pressures. The chosen ma is 5.7 MJ L− 1. Pressurized vessels on board, on the other hand, are less
terial must be H2 diffusion-resistant besides avoiding any probable H2 common and pose a greater risk of explosion due to unanticipated and
embrittlement [166,167]. According to the aforementioned parameters, unplanned shocks. In an ideal scenario, energy could be recovered
four types of vessels are utilized to store compressed H2 gas. Type I: during the expansion phase, but this would demand a sophisticated
These are the most affordable options. The vessels are made of metallic design and added weight to the vehicle. Refueling at 700 bar offers
components and have a maximum operating pressure of 30 bar. High H2 logistical challenges as well as safety considerations at the filling sta
pressures or densities require a substantial metal wall. As a result, the tions. In addition, infrastructures for H2 fuel transportation as well as
storage vessel’s weight increases and its net H2 gravimetric energy distribution are essential. Fuel cell and compressed H2-powered vehicles
density decreases dramatically. Because the containers can only suc are increasingly being sold and driven on public highways. A single fill
cessfully store about 1 wt% of H2, they have a very low gravimetric of H2 at 350 bar allows a commercial Hyundai truck to go around 400
energy density. The two most common materials are steel and aluminum km. Infrastructure for H2 fuel is also expanding, albeit slowly world
alloys. Type II: These vessels’ cylindrical metal walls are covered with wide. Glass microspheres with diameters ranging from 5 to 500 μm can
fiber-resin composite. 30–40 % lighter than Type I, but 50 % more also be utilized to hold compressed H2 gas. The microspheres’ gravi
expensive. Type III: comprised of Aluminum, carbon fiber composites (i. metric H2 density is adequate (5.4 wt%). The H2 infrastructure is un
e., carbon fiber reinforced plastic). In this case, low thermal conductivity necessary because the microspheres could be filled with 350–700 bar H2
could be an issue due to the slow heat release rate during compression of gas off-site and supplied to the fuel stations. Given the low pressure of
H2. They are applicable for applications requiring high pressures up to bulk H2 storage, they seem to be more secure than cylinders of
Fig. 7. Schematic illustration of the type I, II, III and IV H2 compression vessels. Reproduced from ref. [170] with permission. Copyright 2016, Elsevier.
10
compressed H2. Furthermore, tanks do not need to be cylindrical or

spherical in shape to contain the glass spheres. In contrast, glass-
microspheres exhibit low volumetric energy densities and need high
temperatures of 200–300 ◦ C to liberate H2 [171]. They slowly leak H2 at
normal temperature, resulting in H2 loss during handling and trans
portation. They can also break while charging, discharging, or
transporting.
3.2. H2 liquification
The volumetric energy density of liquid H2 significantly increases

since it has a much larger density than gaseous or cryogenic H2. At
− 253 ◦ C, liquid H2 has a density of about 71 g.L− 1 and an energy density
of 8 MJ.L− 1. For liquification, H2 must be cooled to below − 240 ◦ C, its
critical melting point. Liquefying H2 to a temperature of − 253 ◦ C is
necessary if it is to remain in liquid form (the average boiling point of
H2). Like H2 compression, liquid H2 storage has been used successfully in
the past. H2 release rates from liquid H2 in a cryogenic systems are
equivalent to those from compressed H2, but with far less adiabatic
expansion energy being required. As a result of the small adiabatic
expansion energy, no harm occurs if H2 is accidentally allowed to seep
through an opening. Its density is about 1.5–2.0 times higher than
compressed H2 at high pressures, hence a smaller tank is sufficient. With Fig. 8. Schematic illustration for conceptual liquid-organic cycle.
low pressure storage, tank thickness and cost can be reduced. Cryogenic
storage containers can be fabricated from noncorrosive materials like
stainless steel or aluminum alloys since liquid H2 is noncorrosive. On the C10 H18 →C10 H16 + H2 (13)
downside, liquefaction is both costly and power-intensive. It has been The reaction involves the removal of two hydrogen atoms from the
calculated that 30 to 40 % of the net H2 heating value is lost during the decalin molecule, which results in the formation of a cyclic diene and
liquefaction process. The loss of H2 due to the boil-off phenomena, hydrogen gas. During the dehydrogenation process of methylcyclohex
which happens when energy is drawn from the environment, is another ane, hydrogen gas is released that can be used as a fuel source. The
critical problem. Daily H2 loss is between 1.5 % and 3.0 %. As a result of overall reaction for the dehydrogenation of methylcyclohexane is
the boil-off issue, there is a pressing need for more parking garage and expressed by Eq. (14) as follow [180,181]:
street parking lots. A costly double-walled vacuum tank is one way to
reduce boil-off. As a corollary, evaporation loss can be reduced by C7 H14 →C7 H12 + H2 (14)
selecting a container with a bigger capacity and a smaller surface area. The reaction involves the removal of two hydrogen atoms from the
The gravimetric energy density of the vessel may decrease if insulation methylcyclohexane molecule, which results in the formation of toluene
and other unique fabrication methods make it heavier. The development and hydrogen gas. The dehydrogenation of cyclohexane can occur via
of an appropriate infrastructure and widespread public acceptance of several different pathways, each of which involves the removal of
liquid H2 pose further difficulties. There is currently no way to use liq hydrogen atoms from the cyclohexane molecule. One of the common
uefied H2 on-board, particularly in small to medium size vehicles dehydrogenation reactions for cyclohexane is expressed by Eq. (15) as
[172–175]. Using liquefied H2 is an option when only a limited amount follow [182,183]:
of dormancy time is required. It’s utilized by private spaceships that can
afford it and don’t need a hibernation period. C6 H12 →C6 H10 + H2 (15)
In this reaction, one of the carbon-hydrogen bonds in the cyclo
3.3. Liquid organic carriers (LOCs) hexane molecule is broken, releasing a molecule of hydrogen gas and
forming a molecule of benzene (C6H6). These reactions can be catalyzed
In liquid organic H2 carriers, also known as a liquid organic hydrides, by a variety of metal catalysts, such as platinum or palladium, which
H2 is chemically sustained by interacting with an organic molecule help to facilitate the removal of the hydrogen atom from the cycloalkane
devoid of H2. In the reactor, organic hydride is dehydrogenated, molecule. These cycloalkanes have H2 storage capacity ranging from 6.2
releasing the H2 required for electricity generation in stationary power % to 7.3 % by weight. Benzene and naphthalene are the final products of
plants or vehicle applications. After the dehydrogenated product has dehydrogenation of cyclohexane and decalin, respectively. At room
been removed, the liquid-organic hydrides are supplied to the fuel sta temperature, naphthalene is solid while benzene is hazardous. As a
tions. Before delivering to the fuel stations, the de‑hydrogenated liquid product of methylcyclohexane dehydrogenation, toluene is non carci
organic hydrides are transferred to the off-site facility for hydrogena nogenic and exist in liquid form at ambient temperature. Another sub
tion. Carbon does not leave the carbon cycle or enter the atmosphere stance that is frequently handled extensively is toluene. It is much easy
[176,177]. Fig. 8 illustrates the approach of the liquid organic hydrides to begin the H2 economy-based on the methylcyclohexane as well as
cycle for stationary and on-board application purposes. At room tem toluene since toluene is readily available and can be produced in vast
perature, the reversible H2 capacity of organic hydrides ranges from 1.7 quantities [184–188]. Under normal operating conditions, decalin has
% to 7.3 % by weight. The most major benefit of adopting an organic the highest equilibrium conversion, whereas cyclohexane has the
hydride is the ability to successfully utilize the existing infrastructure for lowest. The methylcyclohexane de-hydrogenation to toluene is signifi
gasoline bulk storage and delivery. In the beginning, only cycloalkanes cantly easier than that of the cyclohexane de-hydrogenation to benzene
(liquid organic carriers) such as decalin, methylcyclohexane, and due to the presence of the methyl group. After evaluating all factors,
cyclohexane were of significant interest. During decalin dehydrogena methylcyclohexane appears to be a superior alternative to the two hy
tion, hydrogen gas is released that can be used as a fuel source. The drides mentioned previously. Similar to gasoline in terms of density and
overall reaction for the dehydrogenation of decalin is expressed by Eq. viscosity, methylcyclohexane has a normal boiling point of 100.9 ◦ C,
(13) as follow [178,179]:
11
which is approximately matching to the boiling point of water. The gases or liquids. Thus, their lattice would normally break down into
methylcyclohexane as well as toluene vapor pressures at 38 ◦ C (i.e., conventional crystals of ice or liquid water. Usually, gases with low
100 ◦ F) are 11.2 and 7.2 kPa, respectively. At same temperature, water molecular weights such as H2, O2, N2, CH4, CO2, H2S, Xe, Kr, and Ar form
has a vapor pressure of 6.6 kPa. The methylcyclohexane-toluene H2 hydrates at appropriate pressures and temperatures [204]. Besides,
storage system is well investigated for storing H2. About, 6.2 % by several hydrocarbons and freons also form hydrates under identical
weight of H2 contains 5.5 MJ.L− 1 of H2 [188,189]. Usman et al. [190] conditions. Actuality, these hydrates do not belong to the class of
simulated a model of methylcyclohexane-toluene-H2-Gas system, and chemical compounds, because the impounded molecules are not bonded
found promising results that might be employed for future applications to the lattice. Thus, their formation as well as disintegration do not
on vehicles. In a subsequent investigation, they developed a concept for involve chemical reactions but instead involve first-order phase transi
a small-volume storage tank capable of holding liquid hydride and its tions, and their mechanism on a molecular level is so far not fully un
dehydrogenation product. The problematic characteristics of cyclo derstood. Besides, the physisorption and chemical reactions, another
alkanes are their incredibly high dehydrogenation temperature and re hydrogen storage technique received tremendous attention from scien
action enthalpy (dehydrogenation/hydrogenation). At 325 ◦ C and 1 bar, tific researchers. This technique involves the gas encapsulation inside a
for instance, methylcyclohexane dehydrogenation results in a nearly solid guest structure to form a clathrate, which evolves hydrogen by
100 % equilibrium conversion and costs 205 kJ.mol− 1 methyl altering the temperature and pressure. Several natural gases including
cyclohexane or 68.3 kJ mol− 1 H2 [188]. A heteroatom can be added to carbon dioxide and methane form water clathrates and are named
the cycloalkane ring to alleviate some of these problems [191]. For clathrate hydrates [205,206]. However, according to the first report on
instance, Cui et al. [192] demonstrated this hydride’s superior ther hydrogen clathrates in 1999 [206], research on hydrogen clathrates
modynamics and kinetics. Nevertheless, it has been discovered, that N- received great interest and these materials are regarded as potential
based heterocyclic molecules can decompose and generate undesirable candidates for hydrogen storage. The hydrogen-bonded water molecules
byproducts [193]. Recent report [194] revealed that O2 containing around the guest molecules form polyhedral cages and produce solid
cycloalkanes (derivatives of diphenyl-ether) are feasible candidates for clathrate hydrates which exhibit three distinct structures. Among them,
H2 storage applications owing to their high storage capacities and low the hydrogen clathrate hydrates form sII type structure which is
vapor pressures. Recently, ammonia (NH3) has been regarded as a po composed of a well-organized stacking of pentagonal-dodecahedral and
tential liquid organic carrier for hydrogen storage and transportation. It hexakaidecahedral clusters as shown in Fig. 9 [207].
has a high hydrogen content of 17.6 % by weight and a high energy
density, making it an attractive candidate for hydrogen carriers [195]. 3.4.2. Metal hydrides
The dehydrogenation of NH3 can be achieved through a process called Metal hydrides belong to the class of hydrogen compounds which are
the ammonia decomposition reaction, which is expressed by the Eq. (16) formed as a result of the metal‑hydrogen bonds and give them special
as follow [196]: characteristic features. In metal hydrides, the host metal might be an
element, alloy, or metal complex. Thus, these materials are regarded as
2NH3 →N2 + 3H2 (16)
the essential constituents of hydrogen fuel tanks and secondary batteries
This reaction can be catalyzed by a variety of catalysts, including (energy storage), gas separation, desiccants, hydrogen purification (a
transition metals, such as ruthenium, and alkali metal salts [197–199]. physical separation process), fuel cells (energy conversion), catalysts,
The reaction typically requires high temperatures and pressures, with reducing agents, strong reductants and strong bases (chemical process
optimal conditions depending on the catalyst and reactor design. The ing), heat pumps (thermal application), shields, neutron moderators and
advantages of using ammonia as a liquid organic carrier for hydrogen reflectors (nuclear engineering) [208,209]. Thus, due to the diverse
include its high hydrogen content, low toxicity, and ease of handling. It applications of metal hydrides, these materials received a hot spot of
also has a well-established infrastructure for production and trans scientific research these days. In metal hydrides, the hydrogen density
portation, making it a potential cost-effective option for large-scale per unit volume is high, thus, these materials could offer a suitable and
hydrogen storage and transportation. However, there are also chal safe method for hydrogen storage [210]. As discovered for the first time
lenges associated with the use of ammonia as a hydrogen carrier. One of by Thomas Graham in 1866, the noble metal Pd can absorb a large
the main challenges is the need to overcome the high energy barrier for amount of hydrogen. The hydrogen absorption/desorption by Pd metal
the ammonia decomposition reaction, which requires high temperatures takes place through the two-phase cycle. The α-Pd phase is quite stable
and pressures. Another challenge is the potential for catalyst deactiva at low H2 concentrations, while the β-Pd phase is dominant at high H2
tion, which can reduce the efficiency of the process over time. Addi concentrations. The effect of particle size on hydrogen storage was
tionally, there is a risk associated with the use of ammonia as a investigated and cycling under a hydrogen environment at equilibrium
flammable and toxic gas, which requires careful handling and safety pressure required for the Pd hydrides formation was reported to alter
precautions [200–202]. with particle size [211,212]. According to Li et al. [213], the Pd particle
morphology might play a vital role in hydrogen absorption and the
3.4. Solid state method temperature is also critical for its absorption, uptake, and diffusion. The
isothermal hydrogenation profile of octahedral (red color) and cubic
In this method, H2 storage rely on the mechanical compression as (blue color) Pd at 303 K temperature and 101.325 kPa hydrogen pres
well as sorption on solid-state materials. Herein, we have reviewed sure (H2, 1.0 bar) is revealed in Fig. 10(a, b).
several materials. Considering the low cost, weight storage capacity, and reversibility,
Mg attracted great attention toward hydrogen storage [214]. Recently, α
3.4.1. Clathrate hydrates and β phases of MgH2 as hydrogen storage materials also received
As mentioned in the literature, clathrate hydrates were first reported tremendous attention from scientific researchers [215,216]. For
by Humphry Davy in 1810 [203]. He confirmed water as a primary instance, Shen et al. [217] reported the fabrication of γ-MgH2 by the
constituent of solidified chlorine. Thus, clathrate hydrates/gas clath electrochemical method which revealed a significant hydrogen absorp
rates, clathrates, gas hydrates, and hydrates are water-based crystalline tion of 29.6 %, and the full release of hydrogen from the γ-MgH2
solids that physically resemble ice. In these materials, the non-polar occurred at 200 ◦ C. It was investigated that the γ-MgH2 led to a sub
small molecules classically gases and polar molecules having large stantial reduction in the apparent activation energy (i.e., 106.2 ± 4.0 kJ
hydro-phobic parts are surrounded by hydrogen-bonded cages of the mol− 1 to 69.1 ± 2.9 kJ mol− 1) and also reduced the reaction enthalpy
frozen water molecules. Thus, in clathrate compounds, the host mole from 74.8 ± 1.0 to 57.7 ± 5.3 kJ mol− 1 H2, and led to the improvement
cules are comprised of water and the guest molecules are comprised of of hydrogen kinetics. Likewise, Xiao et al. [218] fabricated β-/γ-MgH2
12
Fig. 9. Crystal structure of sII type hydrogen clathrate hydrates (purple color denote the disorder D2 molecule, while the red color represent oxygen of water).
Reproduced with permission from ref. [207]. Copyright 2007, The American Chemical Society. (For interpretation of the references to color in this figure legend, the
reader is referred to the web version of this article.)
Fig. 10. (a) Graphical representation of the potential energy diagram of Pd octahedrons (red color) and cubes (blue color). (b) The isothermal hydrogenation profile
of the corresponding Pd octahedrons and cubes at a temperature of 303 K under a hydrogen pressure of 101.325 kPa (H2, 1.0 bar). Reproduced with permission from
ref. [213]. Copyright 2014, The American Chemical Society. (For interpretation of the references to color in this figure legend, the reader is referred to the web
version of this article.)
composite containing tetragonal phase β-MgH2 with 18 % orthorhombic 3.4.3. Complex metal hydrides
phase γ-MgH2. The resultant β-/γ-MgH2 composite desorbed hydrogen The complex metal hydrides are formed as a result of covalent
at 260 ◦ C, which is almost 140 ◦ C lower than that of the commercially bonding of hydrogen atoms to a central atom in coordination complexes
available MgH2, and revealed a hydrogen storage capacity of 6.6 wt%. like [AlH4]− 1, [AlH6]− 3, and the cations such as Mg, Zn, and Li stabilize
The activation energy for hydrogen desorption over the as-fabricated the anion. Complex metal hydrides are classified in three categories
β-/γ-MgH2 composite was 115 ± 3 kJ⋅mol− 1, which is almost 46 % including the alanates, borohydrides, and amides-imides [221,222].
lower than the commercially available MgH2. The exceptional desorp Alanates are defined by the general formula M(AlH4)n, where M rep
tion performance was attributed to the highly reactive and defective resents an alkaline metal (n = 1), alkaline-earth metal (n = 2), and group
nanostructure that resulted in the improved hydrogen diffusion and the III and IV elements. Usually, the complex anions such as [AlH4]− and
exothermic process linked to the transformation of γ- to β-MgH2, which [AlH6]3− and respective cations, which are salt-like insulating materials
resulted in the enhanced kinetics of hydrogen desorption. form the alanates. A covalent bond with strong ionic character exists
Metal hydrides such as TiFe(AB), LaNi5(AB5), and A2B7 have also between the Aluminum and hydrogen atoms and an ionic bond to the
been studied for hydrogen storage because they can absorb and desorb cation. Notably, the alanates with light cations are principally utilized
hydrogen gas at moderate temperatures and pressures, making them for hydrogen storage purposes. Sodium alanate (NaAlH4) is a proto-type
potential candidates for hydrogen fuel cells and other applications. compound composed of 7.4 % hydrogen content. A three steps (Eqs.
However, challenges remain, including low hydrogen storage capacity, (17)–(19)) reaction would occur when hydrogen is released from
slow kinetics, and high cost, which limit their widespread adoption. NaAlH4 as described below [223–225]:
Ongoing research is focused on developing new metal hydrides with
Dehydrogenation : 3NaAlH4 →Na3 AlH6 + 2Al + 3H2 (17)
improved properties for hydrogen storage [219]. Nevertheless, in the
case of metal hydrides, their real potential for storage purposes was In the first step, NaAlH4 undergoes dehydrogenation to produce
understood after the discovery of the reversible hydrogen absorption- Na3AlH6, aluminum, and hydrogen gas molecules. This reaction typi
desorption in inter-metallic compounds, such as LaNi5 and TiFe com cally occurs at temperatures between 180 and 190 ◦ C.
pounds. The idea of the hydrogen economy is based on the supposition /
Destabilization : Na3 AlH6 →3NaH + Al + 3 2 H2 (18)
that hydrogen can be generated through water splitting through the
utilization of low-cost sources of energy such as wind energy, biomass In the second step, Na3AlH6 undergoes destabilization to produce
decomposition, and solar energy [175,220]. NaH, aluminum, and molecules of hydrogen gas. This reaction typically
13
occurs at temperatures between 190 and 225 ◦ C. and it is mainly released at 310 ◦ C. The experiments revealed that the
/ decomposition products (i.e., B and LiH) remained within the pores of
Decomposition : NaH→Na + 1 2 H2 (19)
the carbon. The crystalline structures of LiBH4 alanate are depicted in
Finally, in the third step, the sodium hydride (NaH) decompose to Fig. 11(a, b) [234].
form Na and one and a half molecules of hydrogen gas. This reaction Based on the above discussion, it is concluded that metal alanates are
typically occurs at temperatures above 400 ◦ C [225]. the potential candidates for hydrogen storage owing to their low cost
Even though metal alanates exhibit high H2 content, they have not and high energy density. Yet, their slower kinetics, poor reversibility,
been extensively considered for hydrogen storage purposes owing to and high stability feature greatly restrict their practical applications.
their inferior kinetic properties during hydrogenation process as well as Nevertheless, the ongoing research in this field is expected to overcome
dehydrogenation, known as reversibility [226]. Bogdanović and these challenges and further advance the development of metal alanates
Schwickardi reported that NaAlH4 alanate could be reversibly hydro as hydrogen storage materials.
genated as well as dehydrogenated under mild conditions by appro
priate doping content of titanium-based catalysts [224]. This innovative 3.4.4. Microporous materials
approach opened up a new field of the catalysts doped alanates for Hydrogen storage in microporous materials is an important method
effective hydrogen storage. Afterward, several transition metal and rare under deliberation for onboard fuel storage for automotive application
earth metals-based catalysts such as alloys, oxides, metallic elements, purposes. These materials display a systematic inorganic/organic
hydrides, nitrides, and halides have been widely examined as doping framework that supports a steady porous structure with pores in the
precursors to enhance the kinetics of the alanates. Among these, range of 0.2–2.0 nm [235]. Microporous materials mainly include
Titanium-based, Scandium-based, and Cerium-based precursors activated carbon, carbon nanotubes, metal-organic frameworks, sili
revealed exceptional catalytic effects. Notably, considering the catalytic cates, and zeolites and exhibit type-I gas adsorption isotherm
performance and the storage capacity loss, the optimum content of the [236–240]. In such type of materials, the potential field of attraction
chlorides of Titanium, Scandium, and Cerium is in the range of 2–5 mol among the wall of the pore and the adsorbate molecules overlap and
% [227]. Besides, the co-doping strategy is found to be also effective, enhance the force of attraction that acts on the adsorbate, thereby
since the kinetics of the alanates doped with Titanium-based catalysts enhancing the hydrogen adsorption. For gas adsorbates, the pores and
and other materials like KH, HFCl4, and Zr, etc. are much superior. A channels might be enough small to render some portions of the internal
reversible hydrogen capacity (i.e., 4.77 to 4.92 wt%), which is very close volume inaccessible. Usually, this is a more serious problem for large
to the expected capacity of 5.13 wt% was realized in a short time (<20 adsorbate molecules rather than small ones like hydrogen. These ma
min) under reasonable conditions by doping 2 mol% of CeAl4 into the terials exhibit a specific surface area usually in thousands m2.g− 1 [235].
NaAlH4 alanate [227,228]. Carbon nanomaterials with high porosity exhibit the ever-best hydrogen
Borohydrides are a class of hydrogen storage materials that have storage features and the advanced carbon nanomaterials employed for
received significant attention due to their high hydrogen content and hydrogen storage purposes include carbon nanotubes and graphene.
potential for reversible hydrogen storage. Sodium borohydride (NaBH4) Graphene, a synthetic carbon nanomaterial exhibits excellent H2 storage
is one of the most widely studied borohydrides for hydrogen storage, capacity, however, it shows poor cyclic performance. Usually, in carbon
with a theoretical hydrogen storage capacity of 10.6 wt% and a low nanotubes, a very strong on-the-plane Sp2 hybridized covalent bond
toxicity. NaBH4 can release hydrogen via the hydrolysis step, where exists in carbon atoms and results in a strong structure. In carbon
NaBH4 reacts with water to produce hydrogen (H2), and water soluble nanotubes, hydrogen is stored with H–H bonds. In the case of multi-
sodium metaborate (NaBO2) as shown in the Eq. (20) [229,230]: wall carbon nanotubes, hydrogen is either stored in nanotubes or be
tween the multiple walls of nanotubes [241–243]. For instance, Li et al.
NaBH4 + 2H2 O→NaBO2 + 4H2 (20) [244] reported the fabrication of cup-shaped pristine and activated cup-
The hydrogen release and uptake reactions can be catalyzed by shaped carbon nanotubes (i.e., P-CSCNTs and A-CSCNTs) for hydrogen
various materials such as transition metals, metal hydrides, and metal storage. As revealed in Fig. 12a, the maximum capacity of P-CSCNTs for
oxides. However, the kinetics of the reaction are slow, requiring high hydrogen storage is 0.05 wt%, while that of the A-CSCNTs is 0.55 wt%
temperatures and/or high pressures to release and absorb hydrogen. (almost 10 times that of the P-CSCNTs). Nevertheless, such capacities
Therefore, the development of efficient catalysts is critical for the remain very low and needs much further improved top reach the values
practical use of borohydrides for hydrogen storage. Several strategies required for practical applications. The capacity of CSCNTs for hydrogen
have been proposed to improve the hydrogen storage properties of storage has been increased linearly with micropore volume (see
NaBH4, including the addition of other metal borohydrides or metal Fig. 12b), confirming the role of microporous structure in hydrogen
halides to form solid solutions, or the use of nanoconfinement to storage.
enhance the surface area of the material and reduce the diffusion path Besides, the metal-organic frameworks (MOFs) are a class of porous
for hydrogen. While NaBH4 has promising potential for hydrogen stor materials that have attracted considerable attention for their potential
age, several challenges remain for its practical use, including the need use in hydrogen storage due to their high surface area and tunable pore
for efficient catalysts, the high cost of synthesis, and the limited size. The adsorption of hydrogen onto MOFs occurs through physical
reversibility of the hydrogen uptake and release reactions. adsorption, where hydrogen molecules are held in the MOF’s pores
Similarly, Lithium borohydride (LiBH4) has been regarded as a through weak van der Waals forces, resulting in reversible physisorption
promising hydrogen storage material owing to its exceptional theoret [245]. The amount of hydrogen that can be stored in MOFs is dependent
ical hydrogen storage capacity (i.e., 18.5 wt%). However, LiBH4 due to on several factors, including the size and shape of the pores, the surface
its high thermodynamic stability, hydrogen evolution starts over 380 ◦ C, area of the MOF, and the strength of the interaction between the MOF
and nearly half of the hydrogen over LiBH4 could be released below and hydrogen. Several MOFs have been reported to have promising
600 ◦ C. In addition, the conditions required for the formation of LiBH4 hydrogen storage properties, including the Isoreticular (IR) MOF series
from its dehydrogenated products are very harsh (i.e., 15.5 MPa, (IRMOF-1, IRMOF-10, and IRMOF-16), MOF-5, UiO-66, MIL-101, and so
600 ◦ C). Hence, it is of great significance to develop new methods to on [246–248]. For example, the MOF-5 has a high surface area of 3000
improve the hydrogen storage capacity of LiBH4 [231,232]. Surrey et al. m2/g and a pore size of approximately 0.6 nm, which is close to the size
[233] studied the nanoconfinement effect of LiBH4 with aerogel-like of hydrogen molecules, making it an attractive material for hydrogen
porous carbon for hydrogen storage. They reported that the LiBH4 storage [249]. The MOF-5 has a hydrogen storage capacity of 2.5 wt% at
with nanoconfinement effect started to desorb hydrogen around 200 ◦ C 77 K and 100 bar [250]. According to Railey et al. [251], the hydrogen
spillover effect (Fig. 13(a, b)) could remarkably improve the hydrogen
14
Fig. 11. Crystal structures of the LiBH4 alanate (a) orthorhombic phase at 25 ◦ C and (b) hexagonal phase at elevated temperature. The red, green, and blue color
spheres respectively denote the Li, B, and H atoms. Reproduced with permission from ref. [234]. Copyright 2010, Elsevier. (For interpretation of the references to
color in this figure legend, the reader is referred to the web version of this article.)
Fig. 12. (a) Transient H2 adsorption profile for pristine and activated carbon nanotubes (i.e., P, A-CSCNTs). (b) H2 adsorption capacity versus the microporous
volume. Reproduced with permission from ref. [244]. Copyright 2019, Elsevier.
storage of the NP@MOF, where the molecule of hydrogen catalytically metal value of 1.3 without accomplishing of hydrogen to a metal value
dissociates into two atoms at the metal nanoparticle surface, achieving a of 9. In the body center cubic lattice, the hydrogen occupies tetrahedral
dense packing pattern. While MOFs have shown promising potential for sites. Fig. 14(a–d) demonstrates that in the body-centered cubic lattice
hydrogen storage, several challenges need to be addressed for their parameter of 0.30 nm for both hydrides (i.e., Mg55Co45H128 and
practical use, including the need to optimize the pore size and surface Mg2CaV3H8), the distance among two of the tetrahedral sites in the same
area for hydrogen storage, the development of efficient regeneration unit face is 0.11 nm and 0.15 nm (see Fig. 14e), which is much smaller
methods to release the stored hydrogen, and the need to address the than 0.21 nm. This means that one hydrogen could occupy one tetra
stability of MOFs under high-pressure hydrogen adsorption conditions. hedral site, while the other three tetrahedral sites in the same unit face
Nevertheless, MOFs represent a promising avenue for hydrogen storage, can’t be occupied by hydrogen. Further, the distance for identical
and ongoing research in this field is expected to further advance their tetrahedral sites in the two adjacent faces is 0.212 and 0.237 nm, slightly
development for practical applications [252,253]. larger than 0.21 nm, indicating that the occupancy of hydrogen in one
face doesn’t influence the occupancy in the adjacent face. According to
3.4.5. Metal alloys these predictions, it is clear that hydrogen occupies only ¼ of the
Nanocrystalline metastable alloys as hydrogen storage materials tetrahedral interstitial sites in the body center cubic metal lattice hy
received wide attention from scientific research due to their low cost and drides. Each body center cubic metal exhibit six tetrahedral sites, thus,
exceptional hydrogen storage capacity. According to Shao et al. [254], the maximum hydrogen to metal in the body center cubic metal lattice
Mg2Ni alloy fabricated by ball milling of the ultrafine particles of nickel hydrides with a lattice parameter of 0.30 nm is 6*¼ = 1.5 (see Fig. 14f).
and magnesium under 3 MPa hydrogen pressure at 280 ◦ C absorbed Accordingly, the Mg50Co50 and Mg55Co45 body center cubic alloys could
2.82 wt% of hydrogen at 220 ◦ C. Li et al. [255] used mechanical alloying attain a maximum hydrogen storage capacity of 2.67–3.24 wt%
technique to fabricate Mg–Co-based metastable nanoalloy with body- (hydrogen per metal = 1.28, hydrogen per Mg = 2.33) at − 15 ◦ C which
centered cubic lattice as revealed in Fig. 14. The proposed model is the lowest temperature reported so far in case of the Mg-based
demonstrated that the two fully hydrogenated hydrides with body hydrogen storage materials.
center cubic metal lattice only absorb hydrogen with hydrogen to a Mg-based amorphous alloys can also be regarded as efficient
15
Fig. 13. (a) Schematic representation of the spillover effect of hydrogen. (b) Comparison of the hydrogen atoms ratio packed to the Pd atoms collected from the
nanocubes of Pd (green line squares) and core-shell Pd@HKUST-1 composite (red line circles). Reproduced with permission from ref. [251]. Copyright 2017, Elsevier.
(For interpretation of the references to color in this figure legend, the reader is referred to the web version of this article.)
Fig. 14. (a) Body-centered cubic lattice with a = 0.30 nm. (b) Lattice displays the hydrogen-occupied tetrahedral and octahedral sites. (c) In body-centered cubic
lattices, the tetrahedral sites are favored for H2 occupancy. (d) Lattice displays only tetrahedral sites that are occupied by hydrogen. (e) In a body-centered cubic
lattice with a = 0.30 nm, the H–H bond distance is calculated among two tetrahedral sites. (f) Lattice displaying occupancy of only ¼ tetrahedral sites by hydrogen.
Reproduced from ref. [255]. Copyright 2019, Elsevier.
16
hydrogen storage materials. For instance, Spassov et al. [256] reported and plastics, leading to corrosion, embrittlement, and other hazards. It is
nanocrystalline/amorphous Mg–RE–Ni alloys with exceptional important to use materials that are compatible with hydrogen when
hydrogen absorption and desorption features in comparison to the designing and constructing hydrogen systems.
crystalline counterpart. They investigated that melt-spun Mg75Ni20Mm5 (iv) Hydrogen storage can present hazards due to the high pressures
(where, Mm = Ce and La-rich mischmetal) alloy exhibiting fast and temperatures required, as well as the potential for leaks or ruptures.
hydrogen absorption kinetics. Notably, due to the low crystallization Safe storage requires proper design and installation of storage vessels, as
temperature (i.e., 200 ◦ C) of Mg-based alloys, the amorphous alloys well as regular inspection and maintenance.
based on Mg could be simply crystallized during the process of hydro To mitigate these safety risks, a number of safety standards and
genation and dehydrogenation. To avoid crystallization, Lin et al. [233], regulations have been developed for hydrogen production and storage,
reported the fabrication of Mg–Ce–Ni amorphous alloys and evaluated including codes and standards developed by organizations such as the
their hydrogen storage properties at 120 ◦ C. They found that the International Organization for Standardization (ISO), the National Fire
amorphous Mg80Ce10Ni10 alloy could absorb hydrogen even at 120 ◦ C. Protection Association (NFPA), and the American Society of Mechanical
The amorphous Mg–Ce–Ni alloys revealed enhanced hydrogen storage Engineers (ASME). Additionally, proper training and education for
capacity in comparison to their crystalline counterparts. Thus, according personnel working with hydrogen is critical to ensure safe and effective
to the above investigations, the amorphous structure delivers more operation [263].
hydrogen storage sites.
6. Advantages and challenges of hydrogen energy
4. Blended hydrogen production, storage and challenges
6.1. Advantages
Blended hydrogen production refers to the process of producing
hydrogen from a combination of different feedstocks or energy sources, As an alternative to fossil fuels, hydrogen has been regarded as a
such as natural gas, coal, biomass, and renewable energy sources like clean and green form of energy carrier. Hydrogen has been extensively
wind and solar power. Blended hydrogen can be an effective way to utilized for various potential applications. The main advantages are
reduce the cost of hydrogen production and increase the efficiency and described below [264,265]:
sustainability of hydrogen systems. Yet, the blended hydrogen produc 1. It is used as a fuel in vehicles and replaced natural gas, coal, and
tion presents some challenges [257–260]: diesel oil in cars, trucks, buses, ships, rockets, and submarines.
(i) Compatibility: Different feedstocks or energy sources can require 2. In order to get knowledge about weather forecasts, hydrogen gas is
different processing technologies, which can complicate the production widely used in weather balloons by a meteorologist.
process and increase costs. Additionally, some feedstocks may contain 3. As a constituent of fuel cells, energy is produced from hydrogen
impurities or contaminants that can affect the quality and purity of the and oxygen meanwhile water is left as a clean by-product. Thus, the
resulting hydrogen. electrochemical fuel cells are environmentally friendly and can be uti
(ii) Storage: Hydrogen is a highly flammable gas that can be difficult lized as a source of fuel in space crafts, cars, and submarines.
to store safely and efficiently. Blended hydrogen, in particular, may 4. Hydrogen is utilized in the synthesis of various chemical com
require specialized storage technologies to accommodate different pounds, such as during the chemical synthesis of ammonia gas, a huge
compositions and characteristics. amount of hydrogen is required to be treated with nitrogen gas.
(iii) Safety: Hydrogen can be a hazardous material and requires 5. Hydrogen is widely utilized in the food and chemical industry. For
careful handling and transport. Blended hydrogen may present addi hydrogenated vegetable oil and in the chemical industry, hydrogen is
tional safety challenges, as different feedstocks may have different used for metal extraction. Likewise, in the petrochemical industry, it is
characteristics and safety requirements. employed for crude oil refinement.
(iv) Scale-up: Blended hydrogen production technologies may be 6. In various power plants, hydrogen is utilized as a fuel to generate
more complex and difficult to scale up than conventional hydrogen electricity.
production technologies, which can limit the potential for widespread
adoption. 6.2. Challenges
Despite these challenges, blended hydrogen production has the po
tential to be a cost-effective and sustainable way to produce and store Besides the abundant advantages of hydrogen, there also exist
hydrogen for a variety of applications. With ongoing research and several potential challenges that need to be addressed [265,266]:
development, it may be possible to overcome these challenges and fully 1. In order to meet the worldwide energy demand, establishing a
realize the benefits of blended hydrogen production. huge industry of hydrogen requires substantial money expenditure.
2. As the majority of the hydrogen is produced from non-renewable
5. Safety for hydrogen production and storage energy sources, it increases the level of carbon dioxide (greenhouse gas)
concentration in the atmosphere.
Safety is a critical consideration for hydrogen production and stor 3. The key difficulties are the utilization of hydrogen on-board cars,
age, as hydrogen is a highly flammable gas that requires careful where the volume, weight, and cost of hydrogen are all substantial,
handling and management to prevent accidents and ensure safe opera drastically limiting the hydrogen-powered vehicles.
tion. Some of the key safety considerations for hydrogen production and 4. The hydride’s life cycle shortens upon continuous refueling pro
storage are mentioned below [261,262]: cess and reduces efficiency.
(i) Hydrogen is highly flammable and can ignite in the presence of an 5. The lack of suitable hydrogen storage systems protocols and
ignition source, such as a spark or flame. This can result in a fire or standards is also a key disadvantage.
explosion if not handled properly. Proper design, installation, and 6. The storage and distribution to the point of use might be linked to
operation of equipment and systems is crucial to prevent such hazards. energy inefficiency because the low volumetric energy density of
(ii) Hydrogen gas can pose health risks if inhaled, particularly at high hydrogen still does not fulfill the requirements.
concentrations. Exposure to hydrogen gas can cause symptoms such as
headache, dizziness, nausea, and suffocation. Appropriate ventilation 7. Conclusions and outlook
and personal protective equipment should be used when working with
hydrogen gas. As an alternative to fossil fuels, hydrogen production and storage
(iii) Hydrogen can react with some materials, such as certain metals technology have been considered an emerging and proficient
17
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Journal of Energy Storage 64 (2023) 107196

Contents lists available at ScienceDirect

Journal of Energy Storage

State-of-the-art hydrogen generation techniques and storage methods: A

1. Introduction and rockets [7]. The hydrogen economy is an infra-structure employed

Increase in H2 from 0.95 to 1.9 mol/mol-glucoseutilized (+100 %)

Increase in H2 from 2.07 to 2.54 mol/mol-glucose (+22.7 %)

Increase in H2 from 2.33 to 2.48 mol/mol-glucose (+6.4 %)

Increase in H2 from 20.25 to 24.73 mL/g COD (+22.1 %)

Increase in H2 from 247 to 250 mL/g VS (+0.9 %)

methanol reforming to generate H2. The optimized 50CuCrO2-50CeO2

of 73 % (Fig. 4(c, d)). The enhanced performance of the catalyst was

h. Table 2 summarizes the catalysts utilized in steam reforming of

ethanol, methanol and methane.

2.5. Photocatalytic water splitting

semiconductor photocatalyst is excited through the aid of solar light to

generate electrons and holes in a water/methanol system, where holes

generate hydrogen. In this technique, an appropriate semiconductor

conductor. Under light irradiation, the electron-hole pairs are produced

in light absorption and charge transport. In addition, high crystallinity

and surface-active sites of the photocatalyst particles are found to have a

depicted in Fig. 5(a, b), respectively [134]. The overall photocatalytic

2H+ + 2e− →H2

catalytic water-splitting technique received tremendous attention in the

past few years. TiO2 is the most investigated semiconductor photo­

Ni0.91La0.09(10)/CeO2 100 % C2H5OH 78 33 2 [121]

Fig. 6. Schematic illustration of the hydrogen storage methods.

compressed H2. Furthermore, tanks do not need to be cylindrical or

The volumetric energy density of liquid H2 significantly increases

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past few years. TiO2 is the most investigated semiconductor photo