Journal of Energy Storage 100 (2024) 113519

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Journal of Energy Storage

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Review article

Recent advances in sustainable and efficient hydrogen

storage nanomaterials
Nour F. Attia a,* , Sally E.A. Elashery b,*, Mohamed A. Nour a , Alfonso Policicchio c,d,e,
Raffaele G. Agostino c,d,e, Marwa Abd-Ellah f,g, Saihua Jiang h , Hyunchul Oh i,*
a
Gas Analysis and Fire Safety Laboratory, Chemistry Division, National Institute for Standards, 136, Giza 12211, Egypt
b
Chemistry Department, Faculty of Science, Cairo University, Gamaa Str., 12613 Giza, Egypt
c
Department of Physics, University of Calabria, Via Ponte P. Bucci, Cubo 31C, 87036 Arcavacata di Rende, CS, Italy
d
CNISM - National Interuniversity Consortium for the Physical Sciences of Matter, Via della Vasca Navale, 84, 00146 Roma, Italy
e
CNR-Nanotec, c/o University of Calabria, Via Ponte P. Bucci, Cubo 31C, 87036 Arcavacata di Rende, CS, Italy
f
Department of Chemistry, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates
g
Center for Catalysis and Separations, Khalifa University of Science and Technology, Abu Dhabi 127788, United Arab Emirates
h
Institute of Safety Science and Engineering, School of Mechanical and Automotive Engineering, South China University of Technology, Wushan Road 381, Guangzhou
510641, PR China
i
Department of Chemistry, Graduate School of Carbon Neutrality, Ulsan National Institute of Science and Technology, UNIST, South Korea

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

Keywords: The enormous depletion of fossil fuel reserves has been attributed to the rapid expansion in the usage of fossil
Hydrogen storage fuels, which currently serve as the dominant energy source on a worldwide scale. Thus, environmental pollution
Solid-state storage nanomaterials and energy crisis are anticipated to occur as a result of the significant emission of greenhouse gases specifically
Physisorption
carbon dioxide (CO2), produced by the combustion of fossil fuels. Therefore, the replacement of fossil fuels re­
Sustainable fuel
Nanoporous materials
quires the implementation of alternative renewable and environmentally friendly energy sources. The exploi­
tation of hydrogen (H2) as an alternative fuel for automobiles holds significant promise owing to its
environmentally sustainable combustion process, renewable characteristics, and noteworthy gravimetric energy
density. Unfortunately, the inherent gaseous state of hydrogen presents a substantial barrier to its secure, suit­
able, and competent storage, hence hindering the advancement of hydrogen-powered automobiles in the com­
mercial market. Therefore, the need to tackle the anticipated energy problem requires the development of H2 as
an ecologically sustainable fuel alternative. Hence, development, design, engineering, and synthesis of intelli­
gent, innovative, highly efficient, and secure nanomaterials for solid-based hydrogen media will be imperative in
order to effectively harness hydrogen as a sustainable and environmentally friendly fuel source. Therefore, this
state-of-art provides an overview of several technologies utilized in the storage of hydrogen. More precisely,
focuses on sustainable solid-state hydrogen nanomaterials and their various methods of interaction with
hydrogen. Furthermore, this study examines many aspects of hydrogen storage utilizing nanomaterials, specif­
ically focusing on the physisorption uptake and the necessary engineering required to enhance storage capacity
under practical conditions. Furthermore, new prospects for the advancement of an economically, efficient, and
sustainable hydrogen storing materials in order to meet the necessary technical requirements for
commercialization.

1. Introduction commercialization of hydrogen fuel. This is due to hydrogen's notable

advantages as a clean, safe, and abundant fuel that is environmentally
The pressing demand for a clean and sustainable energy source, benign [16,17]. When hydrogen is burned, it produces energy and water
driven by the severe environmental problems associated with current vapor (H2O), without emitting any carbon compounds [18,19]. Addi­
fuel usage [1–15], compels society to expedite the transition towards the tionally, hydrogen, being a renewable and sustainable energy carrier, is

* Corresponding authors.
E-mail addresses: [email protected] (N.F. Attia), [email protected] (S.E.A. Elashery), [email protected] (H. Oh).

https://doi.org/10.1016/j.est.2024.113519
Received 29 April 2024; Received in revised form 21 August 2024; Accepted 23 August 2024
Available online 29 August 2024
2352-152X/© 2024 Elsevier Ltd. All rights are reserved, including those for text and data mining, AI training, and similar technologies.
N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

superior than petroleum, natural gas, and coal in terms of being non- solid materials i) physisorption process and ii) chemisorption process as
toxic and environmentally benign. Interestingly, hydrogen gas pro­ shown in Fig. 1.
duced by both forms of renewable energy. Many forms of renewable
energy can be harnessed, including water, wind, waves, sun, biomass, 2. Solid-state storage approach of H2
and geothermal heat. In contrast, coal, natural gas, and nuclear energy
are examples of non-renewable energy forms used for hydrogen gener­ Physisorption is the process of storing hydrogen by adsorbing mo­
ation. Furthermore, it has been determined that 1 kg of H2 exhibits an lecular hydrogen onto material surfaces via week interactions. Phys­
energy capacity of approximately 120 MJ surpassing the energy content isorption mainly occur on surface pores of high SSA materials such as
of most traditional fossil fuels by more than double [20]. Hydrogen MOFs, fibers, fullerenes, ACs, zeolites, and organic nanoporous poly­
storage is crucial for facilitating technological progress in numerous mers. This procedure necessitates the input of energy to propel it into the
applications, including fuel cells-powered vehicles, batteries and ca­ surface and subsequently release it as hydrogen molecule as indicated in
pacitors [21–23], and so on. Therefore, in order to utilize this energy Fig. 2. Despite their desirable reversibility and rapid kinetics, they
carrier in many industries, it is necessary to have effective and reliable exhibit inferior H2 uptake capacity at RT and require cryogenic tem­
storage methods [24]. There are three primary technologies for storing peratures to achieve higher uptake. These technical limitations severely
hydrogen: high-compressed pressure gas form storage, cryogenic tem­ restrict their practical application [33]. This is because the thermal
perature liquid form storage, and solid form storage [25,26]. For gas- motion of H2 gas molecules at RT over the surface of adsorbents over­
state H2 storage, involves storing H2 gas at high pressure inside a comes the weak interaction bonds between H2 molecules and pore walls.
specialized container. It is appropriate for situations that are both huge Thus, the inclusion of nanomaterials (spherical nanoparticles, two-
in scale and involve long distances. However, the concerns for this H2 dimension nanosheets and nanotubes doped with high density active
storage system, is that this technique involve high compressed pressure sites) in addition to ultramicropores will offer a superior heat of
gas cylinders to accommodate H2 gas at a higher density, both in terms
of weight and volume. Therefore, global industry has set a new objective
for the cylinder, which is to achieve a pressure of 70 MPa while weighing
110 kg. This affords gravimetric and volumetric densities of 5.06 % by
mass and 30 kg/m, respectively which involves high expensive pro­
cessing, in addition to safety issues [20,27]. In contrast for liquid-sate H2
storage, the storage procedure involves compressing hydrogen, cooling
it to a temperature of 21 K and subsequently storing it in a specialized
vacuum container, such as cryo-tanks, at 21.2 K and at 1 bar. The benefit
of this technology, it offers high density (volumetric), which reach to
70.8 kg/m3, surpassing solid-based storage technology; however, it is
not realistic for light-duty vehicle applications [28]. Interestingly, the
solid-based hydrogen storage technology offers a substantial storage
capacity, ensures safe transportation, and provides favourable economic
benefits. This technology has several commendable attributes, including
its high level of safety, effectiveness, affordability, lightweight nature,
and compact design. Previous studies indicate that both high pressure
hydrogen gas and liquid hydrogen storage systems necessitate substan­
tial space, large storage infrastructure, and present safety hazards, in Fig. 2. Schematic representation of current approaches to store hydrogen with
addition to being expensive and inefficient [29–32]. The solid-based materials.
storage process of H2 involve two main routes of uptake hydrogen in Reproduced with permission [30]. Copyright 2018, Elsevier.

Fig. 1. Presentation displaying the main routes of storing hydrogen in solid-based materials.

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

adsorption via improving the binding interaction between H2 molecules

and pore walls. Which significantly transitioning to reversible storing of
hydrogen at near room temperature as described below.
Chemisorption process involves the formation of strong chemical
bonds between the H atoms and storage media surface. This is in
contrast to physisorption process, when molecules are anchored to a
surface through weaker interactions. Chemisorption involves sharing or
transfer of electrons between the adsorbent and adsorbate molecules,
leading to the formation of chemical bonds that can be either covalent or
ionic. This process requires a higher activation energy to overcome the
barrier for bond formation [34,35]. The process is also influenced by the
existence of surface reactive sites on the adsorbent, which limits the
number of molecules that can be adsorbed. An augmented quantity of
reactive positions will lead to a corresponding increase in the quantity of
bonding sites where the H2 molecule can be situated [20]. Recently,
development of new solid materials for hydrogen storage applications is
hot topic. These materials have gained attention because of their
exceptional ability to chemically absorb hydrogen, making them safe
and efficient. Additionally, they have a high hydrogen density and can
absorb hydrogen at very low pressures. They have been identified and
categorized to three groups; first group denoted as metal hydrides and
refer to compounds formed by the combination of metals with hydrogen Fig. 3. (a), Schematic of hydrogen storage composite material: high-capacity
[36]. Secondly, light metal-based hydrides are materials which involves Mg NCs are encapsulated by a selectively gas-permeable polymer and (b) syn­
of metal hydrides and complex hydrides which possess remarkably high thetic approach to formation of Mg NCs/PMMA nanocomposites.
hydrogen densities in both forms, making them highly attractive for Reproduced with permission [40]. Copyright 2011, Springer nature.
vehicles applications compared to other chemisorption-based materials
[37,38]. Thirdly, complex hydrides which involve the ability of the al­
Table 1
kali and alkaline earth metals such as lithium, magnesium, boron, and
US. DOE hydrogen storage technical challenges for on board vehicle application.
aluminum, to produce a diverse array of metal‑hydrogen complexes.
These materials are fascinating due to they have a low weight and often Hydrogen storage technical item 2025 Ultimate target

include two hydrogen atoms for every metal atom. Basically, the dif­ Gravimetric capacity: kg− 1 H2 kg system (wt 0.055 (5.5 wt 0.065 (6.5 wt
ference between complex hydrides and metallic hydrides was ascribed %) %) %)
Volumetric capacity: kg/L H2 0.04 0.05
to the change of metals into ionic or covalent compounds upon hydrogen
Storage system cost: $ Kg− 1 H2 300 266
absorption [39]. Unfortunately, these materials have some kinetic and Operation temperature: ◦ C − 40/60 − 40/60
thermodynamics limitations which restrict their commercialization. Charging temperature (min/max): ◦ C − 40/85 − 40/85
Thus, extensive research has been carried out in the area of hydrogen Charging pressure (min/max): bar 5/12 5/12
storage using hydride systems via design and fabrication new based Cyclability(uptake/release): min 1500 1500
System charging time (4–10 kg): min 3–5 3–5
nanoscale materials, such as nanoconfinement of high capacity hydrides
and reactive hydride nanocomposites to address thermodynamics chal­
lenges and achieve rapid reaction kinetics [40–43]. This obviously, class of materials own interesting features such as outstanding physi­
noted as reported, metallic Mg nanocrystals affords the storage of a high cochemical properties, high specific surface area, good electrical con­
density of hydrogen with fast kinetics via nanoconfinement feature as ductivity and interesting electronic properties rather than their bulk
shown in Fig. 3 [40]. structure due to their molecular size and morphological structure
Regrettably, the gaseous nature of hydrogen poses a hindrance to its [51,52]. Therefore, there are some factors regulates the storing process
secure, convenient, and effective storage, hence impeding the progress of hydrogen in solid-state nanomaterials such as elemental composition,
of commercializing cars powered by hydrogen [29,44,45]. Therefore, structure and morphology [53]. Thus, exploitation of nanoscale mate­
goals for solid-based H2 storage systems for onboard applications has rials and tailoring the engineering process for their structure,
been undertaken by the United States Department of Energy (US-DOE) morphology, textural properties and composition open new avenues for
with regular updates being made to these targets [46–49]. Thus, the set production of new generation of hydrogen storage materials overcoming
gravimetric and volumetric capacities for the year 2020 were estab­ the existing limitations and affords storage at near room temperature
lished to be 4.5 % per mass and 0.03 kg/L H2, respectively [48,49]. conditions. The nanomaterials can be classified based on their dimen­
Furthermore, the objectives for 2025 include achieving a gravimetric sion and chemical composition. For dimension classification, nano­
and volumetric capacities of 5.5 wt% and 0.04 kg/L H2 based in system materials are divided in to four types as depicted in Fig. 4; Zero-
[48,49]. This is in addition to other key technical requirements which is dimension nanomaterials (0-D) when the materials are in nanoscale
considered as technical challenges for commercialization for hydrogen dimension (1–100 nm) from all directions, such spherical nanoparticles
as fuel for light-duty onboard vehicle based on system as summarized in and quantum dots. One dimensional nanomaterial (1-D), when the
Table 1 [29,50]. materials are in nanoscale only diameter and length in microscale such
It is noteworthy that the phenomenon of physisorption by porous as nanotubes, nanofibers and nanowires, two-dimension nanomaterials
solids has efficacy solely under conditions of exceedingly low temper­ (2-D), when the materials are in nanoscale in two dimension such gra­
atures, whereas chemisorption in chemical hydrides is characterized by phene nanosheets and nanocoatings and three-dimension (3-D) are
restricted reversibility and sluggish reaction speeds. Hence, the ability to nanomaterials that are over the nanoscale dimension in any directions,
store H2 at ambient temperature remains a substantial technological but are fabricated from individual nanoscale materials nanometer scale
constraint. Hence, it is imperative to develop a hydrogen storage system (1–100 nm) [54]. However, based on chemical composition, the nano­
that is both cost-effective and efficient, utilizing materials. Thus, there materials can be classified in to 1) organic nanomaterials which
are various nanomaterials have been examined for hydrogen storage composed from organic materials (ONMs) such as organic nanoparticles,
applications. On the other hand, the nanoscale materials afford new

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

2.1. Zero-dimensional based hydrogen storage nanomaterials

Actually, nanoparticles-based hydrogen storage materials including

nanoparticles alone or nanoparticles decorated composite were used for
enhancing the storage capacity. For storing hydrogen molecules in
nanoparticles alone as storage media, nanoporous silica nanoparticle
derived from rice husk and had an average diameter of 50 nm, SSA of
226 m2/g, mesopore size of 2.6 nm and TPV of 0.39 cm3/g was first
reported as hydrogen storage media offering H2 uptake capacity of 0.34
wt% at 77 K and 19 bars [55]. However, when utilized as template for
production of mesoporous carbon, the H2 uptake capacity was signifi­
cantly improved under similar conditions and was found to be 1.61 wt%
(Table 2) [55]. This higher storage capacity was ascribed to the higher
porosity properties in attained porous carbon recording almost four-fold
SSA and TPV [55]. In another attempt, organic polypyrrole nano­
particles (PPY-NPs; 193 nm) were exploited for storing hydrogen mol­
ecules at 77 K and 80 bar and record hydrogen storage capacity of 2.75
wt% [56]. This storage capacity was stemmed from attractive sites for
hydrogen molecules adsorption in PPY-NPs backbone surface of delo­
calized bi-electron [57]. This attributed to improved intermolecular
interactions forces between H2 molecules and the conjugated PPY-NPs
backbone and this attributed to the fact that aromatic rings have been
found to exhibit enhanced hydrogen adsorption capabilities [58,59].
This was the reason for storing good hydrogen uptake capacity in
nanoporous polypyrrole recording storage capacity of 2.2 wt% at 77 K
and 9 MPa (Table 2) with SSA of less than 100 m2/g [60]. On the other
hand, spherical metal nanoparticles were decorated on the surface of
various substrate to improve the binding interaction with hydrogen
Fig. 4. Schematic diagram displaying classification of nanomaterials based on molecule and in turn improves hydrogen storage capacity. In this regard,
dimension and chemical composition. spherical Ni nanoparticles (NPs) of an average size of 5.5 nm were doped
on the surface of mesopores of porous carbon structures affording
polyaniline nanofibers, 2) inorganic nanomaterials (INMs) which are porous composites [61]. The adsorption data displayed that the H2 up­
composed form inorganic materials, 3) hybrid nanomaterials which are take was expressively increased for Ni-NPs doped porous composite
composed from organic and inorganic materials such as hybrid com­ compared to Ni-NPs free one recording 4.29 and 1.44 wt%, under
posites and 2D MOF nanosheets (HNMs) and 4) carbon nanomaterials, cryogenic temperature and 5 bars, respectively [61]. Interestingly
which are composed from carbon materials such as carbon nanotubes, similar hydrogen storage capacity trend was noticed at room tempera­
carbon nanofibers and nanoparticles as depicted in Fig. 4. ture adsorption @ 5 bar achieving uptake capacity of 1.69 wt% for Ni-
Hence, in this review, zero, one- and two-dimensional nanomaterials NPs doped porous composite compared to 0.44 wt% for undoped one
in addition to nanoporous materials have been reviewed and discussed (Table 2) [61]. The superior H2 uptake capacity was ascribed to H2
for physisorption hydrogen storage application because it affords easier spillover phenomena which involve two-step process; the first one is
reversibility to H2 molecule once pressure release without destructive dissociation of H2 molecules on metal nanoparticle surface, then sec­
issue to storage materials as indicated in Fig. 5. ondly, allowing hydrogen atoms adsorption in neighbouring porous
carbon surface and this approach was working for other metal

Fig. 5. Schematic diagram displaying the different types hydrogen storage nanomaterials based on physisorption process.

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Table 2 reduction of energy barrier which is required for dissociation process of

State of art of hydrogen storage materials (HSMs) performance of nanomaterials- H2 and in turn affords superior hydrogen uptake.
based adsorbents. This spillover hydrogen storage trend was further reported with
Material Adsorption Adsorption H2 uptake Ref. different metal nanoparticles decorated on activated carbons (AC) of Ni,
temperature (K) pressure (bar) capacity (wt Pd, Pt, Rh and Cu [65–67]. The data displayed that, the spillover
%) hydrogen storage process is strongly dependent on temperature,
Zero-dimensional HSMs based nanomaterials dispersion and type of metal nanoparticles decorated on porous ACs
RH-SNP 77 19 0.34 [55] [61,65]. Recently, AC with high SSA of 3155 m2/g which was derived
MCs 77 19 1.42 [55]
from Mosa Bamboo and subsequently doped with nitrogen (N) and Pt
MCg 77 19 1.61 [56]
PPY-NPs 77 80 2.75 [56] nanoparticles individually and then used for hydrogen uptake as dis­
PPYsvp2h 77 90 2.2 [60] played in Fig. 6 [68].
HPCM 77 5 1.44 [61] The data found that SSA was decrease once Pt nanoparticles were
Ni-HPCM 77 5 4.29 [61] decorated on the surface of AC, and this was ascribed to pore blocking
HPCM 298 5 0.44 [61]
Ni-HPCM 298 5 1.69 [61]
effect, also, the N doping leads to uniform dispersion of smaller size of
AC 77 1 2.74 [68] Pt-NPs and the developed Pt-NPs size was found to be in the range of 1.9
NAC 77 1 2.91 [68] to 4.7 nm. The hydrogen adsorption capacity for AC and N doped AC was
AC 298 40 0.409 [68] found to be 2.74 and 2.91 wt% at 1 bar and 77 K (Fig. 6a) reflecting
NAC 298 40 0.429 [68]
insignificant increase in hydrogen storage due to N doping. This trend
NACPT20 298 40 0.745 [68]
was also noticed at cryogenic condition when Pt-NPs was doped dis­
playing reduction in hydrogen uptake which ascribed to inferior of SSA
One-dimensional HSMs based nanomaterials
and microporosity occurred due to blocking of pores (Fig. 7a) [68]. In
P-CNTs 298 80 0.65 [69]
F-CNTs 298 80 0.89 [69] contrast, the H2 uptake capacity under RT and 40 bar pressure was
Ni-MWCNTs 298 20 0.298 [71] significantly increased in AC doped with Pt-NPs recording reversible H2
TiO2/COOH- 253 70 1.35 [72] uptake capacity of 0.745 wt% compared to 0.409 and 0.425 wt% for AC
MWNCNTs
and N doped AC, respectively as shown in Fig. 7b (Table 2). This su­
Co-oxide- 298 23 0.8 [73]
MWCNTs
perior hydrogen storage capacity could be attributed to spillover
Cu-oxide- 298 23 0.9 [73] hydrogen storage process [68].
MWCNTs Although, the inclusion of spherical metal nanoparticles on the sur­
MWCNTs 298 40 0.26 [74] face of porous materials leads to raising the binding forces between
Mn3O4- 298 40 0.8 [74]
hydrogen atoms and adsorbents and overcome the adsorption at room
MWCNTs
Ni-doped-ACNF 298 100 1.39 [75] temperature, however, rational engineering for porous adsorbents,
HCl-PANI-NFs 298 80 0.46 [76] nanoparticles size, decoration and distribution still required to achieve
HCl-PANI-NF- 298 80 0.91 [76] the hydrogen storage capacity for practical conditions.
PPY20-2h
HCl-PANI-NF- 298 80 0.12 [76]
PdNP 2.2. One-dimensional based hydrogen storage nanomaterials
HCl-PANI-NF- 298 80 0.47 [76]
PdNP-PPY20- One-dimensional nanomaterials are interesting class of nano­
2h
HNTs 298 5 0.019 [78]
materials including nanotubes (inorganic and carbon nanotubes), car­
PANI 298 5 0.05 [78] bon nanofibers and organic nanofibers such as polyaniline nanofibers
HNT-PANI-0.5 298 5 0.78 [78] and nanorods. For carbon nanotubes (CNTs) as a familiar one-
dimensional nanomaterial, their unique features such as nanotubes
Two-dimensional HSMs based nanomaterials walls, lumens and interstitial spaces afford good adsorption sites for
GO 298 80 1.9 [79] hydrogen molecules via physisorption mechanism. However, due to
rGO 298 80 1.34 [87] their inferior SSA and TPV their hydrogen storage capacity is con­
GO 298 90 0.21 [88]
strained to a maximum of 1 wt% at ambient temperature and 100
N-doped- 298 90 1.5 [88]
graphene pressure [48]. Nevertheless, when exposed to cryogenic temperatures,
Preheated self- 298 20 2.5 [85] carbon nanotubes demonstrate a substantial adsorption of H2 [44].
aligned-GO However, functionalized carbon nanotubes (F-CNTs) exhibited a greater
Ni-graphene 298 60 1.18 [91]
Mn-V-graphene 298 40 1.81 [93]
Pd/F/HEG 298 40 3 [62]
SG 298 40 0.68 [96]
N-SG 298 40 1.1 [96]
Pd/N-SG 298 40 4.3 [96]
rGO/PD06-Pt 298 100 3.19 [98]
Pd-doped- 303 40 0.42 [101]
graphene
sheets

nanoparticles such as Pt and Pd [62,63]. Therefore, hydrogen molecules

dissociated at Ni-NPs surface and then attained hydrogen atoms were
adsorbed inside pores of porous carbon [57,64]. The reported results
found that this approach is responsible for raising hydrogen storage
capacity for porous carbons. This corroborated the significant role of
nanoparticles for improving the hydrogen storage capacity. However, Fig. 6. Schematic procedure of the platinum nanoparticles decorated nitrogen
the uniform dispersion of smaller size and spherical shape of metal doped ACs.
nanoparticles on the surface of porous carbons played a pivotal role for Reproduced from reference [68]. Copyright 2019, Elsevier.

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 7. (a) Hydrogen isotherms at 77 K up to 1 bar and (b) Hydrogen isotherms at 298 K up to 4 MPa: adsorption (solid dots)-desorption (void dots).
Reproduced with permission [68]. Copyright 2019, Elsevier.

H2 uptake capacity of 0.89 wt% compared to pristine CNTs of 0.65 wt% desirable for uptake of hydrogen molecules as indicated in Fig. 8 and
under conditions of 298 K and 8 MPa as presented in Fig. 8 [69]. The Table 2 [69].
higher hydrogen uptake of F-CNTs can be ascribed to the increase of Thus, to afford higher adsorption capacity in CNTs, it is desirable to
surface oxygen species which afford more surface sites and the existence employ surface modifications and composite production involving
of open-end caps, in addition abundance of defective surfaces which are spherical metals or metal-oxides nanoparticles, which affords strong

Fig. 8. (a) Bright field TEM images of P-CNTs (a and its insert) and image (b–f) is F-CNTs. Scale bar of figure (a) insert is 50 nm. In image (b), black arrow indicate
the side wall of F-CNTs has been damage and image (c) is showing the open the end cap of F-CNTs Image (d) showing defect on surface and white arrow line in image
(e) is showing the edge of graphene. Image (f) is showing edge of graphene layer is partially destroyed. (b) Hydrogen uptakes by P-CNTs and F-CNT at 80 bars and (c)
Different storage sites of carbon nanotubes.
Reproduced with permission [69]. Copyright 2018, Elsevier.

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

binding interaction between the substrate and hydrogen molecule [70]. under 100 bar and RT conditions (Fig. 9b). This superior hydrogen up­
Hence, Ni-decorated MWCNTs was fabricated and hydrogen storage take was ascribed to dual modes of spillover and physisorption hydrogen
properties were investigated under varying pressures and at RT [71]. storage process [75].
Thus, at a pressure of 20 bars, highest uptake of H2 was detected to be Hence, the integration of evenly distributed spherical metal and
0.298 wt% which stored via physisorption mode and uptake capacity metal oxide nanoparticles offers a viable approach for producing
was linked directly with pressure [71]. Further design of TiO2/COOH- nanomaterials suitable for storing H2 molecules at RT. Nevertheless, it is
MWCNTs-based hydrogen storage media was developed and exhibited important to acknowledge certain limitations of the synthesized mate­
an H2 uptake efficiency of 1.35 wt% under conditions of 253 K and 7 rial, including its relatively low hydrogen storage capacity in compari­
MPa [72], this superior H2 uptake was ascribed to synergistic effect of son to the desired aim set by USDOE, as well as the potential for carbon
oxygenated species, micropores and role of TiO2. Additionally, com­ nanotubes/nanofibers aggregation and fracture when exposed to high
posites consisting of Co-oxide-MWCNTs and Cu-oxide-MWCNTs, which levels of metal/metal oxide doping. Thus, further research is required to
had specific surface area values of 147 and 237 m2/g, respectively. enhance the synthesis factors, investigate other incorporation or surface
These composites also had H2 uptake values of 0.8 and 0.9 wt%, engineering, and assess the material's storage capacity performance
respectively, at RT and 23 bar [73]. This significant uptake of H2 was under RT and practical needs. Interestingly, organic nanofibers espe­
accomplished due to improved binding forces of H2 molecules and cially polyaniline nanofibers (PANI-NFs) and their composites was
surface Co and Cu oxides, hence, raise uptake at RT [73]. Adhering to found to `be desirable for hydrogen uptake capacity at RT [76,77]. Thus,
the same trend, the uptake of H2 by Mn3O4 nanoparticles decorated with hydrogen storage capacity of PANI-NFs of an average size of 50 nm and
MWCNTs was found to be three times higher compared to pristine one. its composites with PPY was scrutinized at RT and 80 bar (Fig. 10a). The
This can be due to the spillover process facilitated by decoration of hydrogen uptake capacity of PANI-NFs integrated with surface PPY layer
Mn3O4 nanoparticles (Table 2) [74]. Moreover, the porous carbon record 0.91 wt% compared to 0.46 wt% for PANI-NFs alone (Fig. 10b). It
nanofibers of an average diameter of 200 nm with SSA and TPV of 750 was found that the hydrogen uptake mechanism of PANI-NF is signifi­
m2/g and 0.515 cm3/g respectively, derived from polyacrylonitrile cantly influenced by the inclusion of a dopant. Also, it is noted that, the
(PAN) and petroleum pitch as carbon precursors and subsequently diameter of the counterions were also determined to have a pivotal role
decorated with spherical Ni-NPs (Fig. 9a) record H2 uptake of 1.39 wt% in the process of H2 uptake process (Fig. 10). Therefore, the H2 sorption
capacity of the PANI-NFs is improved when the counterions are smaller
in size due to negligible steric hindrance surrounding the adsorption
centres, as opposed to larger counterions [76]. Furthermore, surface
decorated PANI-NFs with spherical Pd nanoparticles (NPs) with an
average size ranging from 4 to 5 nm, for the purpose of hydrogen storage
under similar conditions also tested [76]. The H2 uptake capacity of
PANI-NF-PdNPs was found to be 0.12 wt%, which was inferior than the
storage capacity of Pd-NPs free PANI-NFs as seen in Fig. 10b (Table 2).
However, the H2 storage capacity of PANI-NF-PdNP-PPY20-2 h which
was covered with PPY layer was found to be 0.47 wt% [76]. This
attributed that, additional engineering process of PANI-NFs with
different dopant molecules is required to afford higher storage capacity
at practical applications. Additionally, cost-effective, naturally occur­
ring halloysite nanotubes (HNTs) were utilized in conjunction with
polyaniline nanorods for construction of hydrogen storage nano­
composite at ambient temperature. The optimal nanocomposite exhibits
a significantly higher H2 uptake capacity of 0.78 wt%, in comparison to
pristine HNTs of less than 0.019 wt% and the 0.05 wt% of PANI at RT
and 5 bars (Table 2) [78]. The significant rise in hydrogen uptake is
ascribed to the chemically sorption of H2, which was increased by the
sorption centres formed during the mechanical milling of polyaniline
with the nanotubes. Furthermore, the hydrogen adsorption process is
enhanced by the regulated lumen size, which is optimized to achieve
optimal hydrogen adsorption and affords good binding forces between
regulated HNTs lumen and H2 molecules. This is achieved by incorpo­
rating polyaniline chains into the nanotubes [78]. Thus, further tuning
and regulation of lumen cavity of the cost-effective and sustainable
HNTs with reactive materials such PANI and or PPY could afford new
engineered nanocomposites with various active sites facilitates inter­
action with H2 molecules.

2.3. Two-dimensional based hydrogen storage nanomaterials

Graphene is a prominent carbon allotrope and popular two-

dimensional nanostructure that exhibits favourable electrical and me­
chanical characteristics, making it suitable for a wide range of applica­
tions. The graphene has garnered significant attention due to its
exceptional physical features, including quantum electronic transport,
high elasticity, high mobility, and a configurable band-gap [79–83].
Interestingly, graphene sheets present novel opportunities for hydrogen
Fig. 9. (a) (a,b) TEM images and (c,d) high-resolution TEM images of ACNF-3 storage [84]. Thus, numerous researches have been implemented on
and (b) hydrogen adsorption isotherms of ACNFs at 298 K [75]. materials-based graphene for the purpose of hydrogen storage

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 10. (a) Schematic illustration of the preparation of the conducting composite network PANI-NF-PPY and the sandwich structure PANI-NF-PdNP-PPY, in which
polyaniline nanofibers (PANI-NF), palladium nanoparticles (PdNP), and polypyrrole (PPY) are involved and (b) Hydrogen storage isotherms of PANI-NFs and their
composites.
Reproduced with permission [76]. Copyright 2013, Wiley.

applications. Also, graphene oxide (GO) has been the subject of much shown in Fig. 11a [85]. Their findings revealed that the H2 hydrogen
research and can be facilely synthesized from graphite using several adsorption capacity values recorded were 1.5 wt%@ 25 ◦ C, 2.0 wt%@
techniques [85,86]. H2 uptake characteristics of GO, and reduced gra­ 250 ◦ C, and 2.5 wt%@ 450 ◦ C. Thus, process of preheating graphene
phene oxide (rGO) were tested and uptake capacities were found to be of oxide sample has the potential to modify the interlayer gap, hence
1.90 and 1.34 wt% for GO and rGO, respectively, @ RT and 80 bar increasing the binding capacity for hydrogen molecules as presented in
(Table 2) [87]. It was found that the oxygen groups found in GO and rGO Fig. 11b [85].
play a crucial role in occupying the interlayer space, resulting in The hydrogen adsorption and desorption were further investigated
increased hydrogen binding inside the nanosheets [87]. Interestingly, using semi-empirical kinetic analysis. Hence, the data revealed that in­
H2 uptake capacity of nitrogen-doped graphene was detected to be 1.5 crease in interlayer spacing increases the reversibility and desorption
wt% compared to 0.21 wt% for graphitic oxide under RT and 90 bar rate, while the oxygen moieties greatly improves the nanoparticle
conditions [88]. This, higher H2 uptake capacity was proposed that the anchoring [91]. Also, a significant hydrogen adsorption occurred as a
inclusion of nitrogen elements on graphene amend the inherent catalytic result of the adsorption of hydrogen molecules between the graphene
properties of graphene for boosting the hydrogen molecules dissociation layers [92,93]. Nevertheless, the limitations of inferior hydrogen uptake
[88]. Moreover, the H2 uptake capacity was investigated theoretically at RT in graphene-based materials are ascribed to low binding energy
via density functional theory calculation in Al-doped graphene and the problem of graphene sheets with hydrogen molecules. This problem
capacity was found to be 3.84 wt% at 300 K and 100 MPa which ascribed could be solved via surface functionalization, bandgap management,
to physisorption and chemisorption hydrogen uptake process and to metal/alkali metal doping, and other synthesis techniques, which will
regulation of interlayer distance [89]. Notably, new graphene-based all produce additional active sites on adsorbent surface [89,94]. Thus,
alkali metal nanocomposite was studied grand canonical Monte Carlo based on this finding, TiO2 nanoparticle decorating on GO increases H2
simulations and the H2 uptake capacity of Li-doped graphene is unex­ uptake by 230 % and produces convenient reversibility of near to 80 %
pectedly high, reaching up to 6.5 wt% under conditions of RT and 20 bar [91]. Hence, the volumetric H2 uptake for GO and rGO decorated Ti
[90]. Furthermore, the H2 adsorption properties of preheated graphene yielding Ti-GO r(Ti-GO) composites at RT was carried out as shown in
oxide at variable temperatures were investigated at RT and 20 bars and Fig. 12. The results indicate that Ti-GO demonstrates a significant

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

graphene has been fabricated and tested for hydrogen adsorption. The
findings demonstrated a H2 uptake capacity of 1.18 wt% under RT and 6
MPa, with total desorption occurring at 250 ◦ C (Table 2) [95]. Other
separate study documented that graphene decorated with Mn–V
exhibited a H2 uptake of 1.81 wt% at a pressure of 4 MPa, a value that is
notably greater than that of unmodified graphene (0.25 wt%) [93]. This
superior of hydrogen uptake could be ascribed to exploitation of
inherent catalytic feature of nanoparticles on graphene hydrogen
adsorption. Interestingly, a notable increase in hydrogen uptake ca­
pacity, was attained (3 wt%), in graphene doped with 20 wt% Pd under
a pressure of 40 bar (Table 2) and higher uptake was stemmed from
spillover action [62]. However, nitrogen-doped graphene exhibits a H2
uptake of 1.1 wt% at 20 bars [96]. While, the fabricated Pd-N-graphene
composite yields H2 uptake capacity of 4.3 wt% at pressures of 40 bar,
respectively compared to 0.68 wt% for undoped graphene sheets [96].
This higher uptake capacity was ascribed to catalytic feature of Pd-NPs
boost the hydrogen molecule dissociation process yields hydrogen atoms
and subsequently diffusion of attained hydrogen atoms over graphene
layers surface in the via physisorption process and are chemisorbed at
the nitrogen doped sites [96,97]. Nevertheless, the use of graphene foam
adorned with Pt nanoparticles has been found to result in a noteworthy
hydrogen uptake of 3.19 wt% [98]. The study revealed that polydop­
amine is useful for functionalizing graphene substrates as it maintains
the desired surface area, distribution of dopants, and amount of doping
[98], thus was responsible for affording this superior H2 uptake. Addi­
tionally, Ni-doped graphdiyne, a two-dimensional carbon allotrope, was
assessed theoretically for hydrogen storage utilizing Density Functional
Fig. 11. (a) Hydrogen storage recorded at room temperature by preheated GO
sample (at various temperatures). (b) Variation in interlayer spacing of pre­
Theory (DFT). The study demonstrates that boron doping has been
heated GO (preheated at 25, 250, and 400 ◦ C, respectively) and corresponding employed to enhance the binding of Ni atoms to graphdiyne, resulting in
adsorption of hydrogen molecules. a substantial increase in Ni bonding with graphdiyne. The findings
Reproduced with permission [85]. Copyright 2020, Elsevier. suggest that the incorporation of boron doping leads to a reduction in
the adsorption energy, and in turn an enhancement in the desorption
volumetric adsorption capacity of 5.5 g/L, comparable to that of the condition within the temperature range of 300–500 K and hydrogen
pristine sample, with a reversibility rate of 80 %. In a similar vein, r(Ti- uptake recorded was 1.2 wt% [99].
GO) demonstrates a notable volumetric adsorption capacity of 5.5 g/L Furthermore, the graphene-based adsorbent doped with nickel and
however, with inferior reversibility rate of only 42 % [91]. aluminum consist of nickel, aluminum and carbon phases, exhibit a
Further, graphene based composite material consisting of nickel and significant capacity for storing hydrogen and possess exceptional

Fig. 12. Hydrogen adsorption and desorption capacity of (a) pristine GO, (b) GO+Ti composite, and (c) r(GO+Ti) composite samples.
Reproduced with permission [91]. Copyright 2020, Elsevier.

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

stability in terms of hydriding and dehydriding [100]. The composites of high SSA, micropores and TPV are much desirable for H2 molecules
have a maximum H2 uptake capacity of 5.7 wt% at a temperature of 473 adsorption.
K [100]. Additionally, the dehydriding efficiency is notably high, MOFs are considered as one the of the famous NPMs utilized for
ranging from 96 % to 97 % at a dehydriding temperature of 380 K. The hydrogen storage applications due to their interesting features such as
regulation of H2 adsorption and desorption rates in graphene composites functionals, tunable pore size and high SSA and TPV. Basically, they are
doped with nickel and aluminum is achieved through the nucleation and formed via reaction of metal ions clusters and organic ligands, yielding
two-dimensional growth mechanisms (Fig. 13). Importantly, graphene crystalline porous materials [111–113]. There are two types of MOFs
sheets and their decorated system with Pd-NPs were constructed using based on their design and dimensions such as two-dimensional nano­
green approach affording superior hydrogen storage capacity of 0.42 wt sheets (2D) and three-dimensional (3D) MOFs [114,115]. The first MOFs
% at 30 ◦ C and 40 bars (Table 2) compared to Pd-NPs free adsorbent tested for hydrogen storage was reported two decades ago [116]. MOF-5
(Fig. 14) [101]. was attained based on reaction of zinc ions with 1,4-benzenedicarbox­
Also, various graphene and GO based materials were recently ylic acid (BDC) and H2 uptake capacity was found to be 4.5 and 1.0
fabricated and their hydrogen storage properties were tested such as wt% at 78 K and RT, respectively, under a pressure of 20 bar (Table 3)
zeolite-graphene composite [102], GO doped with copper ferrite [116]. Nevertheless, their prospective use was restricted due to subpar
(CuFe2O4) [103]. Recently, new theoretical and validated experimental performance and susceptibility to moisture instability. Interestingly,
approach was introduced for design of non-dissociative chemisorption superior porosity of 4600 m2/g and in turn higher H2 uptake of 7.5 wt%
materials for storage of hydrogen molecules in nanoscale carbon mate­ at 77 K and 70 bar were attained when 1,3,5-benzen etribenzoate (BTB)
rials to afford the required practical storage capacity [104]. The was used as linker [117,118]. Moreover, adjustment the synthesis pro­
approach was mainly depending on the efficient of engineered materials cess of MOF via insertion of other groups in MOF-5 results in the for­
and can be achieved through the exploitation of heteroatom-doped mation of a framework had superior SSA of 6143 m2/g and consequently
graphene adorned Ca atom carbon-based materials. It has been sug­ recording H2 uptake of 10.0 wt% at 77 K and 56 bars [119–121].
gested to establish a connection between the inherent characteristics of Interestingly, the additional modifications made during the synthesis of
dopants and the ability of carbon-based adsorbent to store hydrogen. MOFs result in the production of MOFs with a higher SSA. Specifically,
Thus, the predictive capability of the generalized design principle allows NU-110 has an SSA of 7140 m2/g, while MOF-399 has an SSA of 7157
the identification of optimal doping process of graphene-based adsor­ m2/g. As a result, these MOFs demonstrate a high capacity for hydrogen
bent for hydrogen storage. Thus, the hydrogen storage capability of uptake, with NU-110 able to store 8.82 wt% of hydrogen and MOF-399
dual-doped materials is significantly superior than that of sole-doped able to store 9.02 wt% of hydrogen at 77 K and 45 bars as shown in
materials [104]. However, still much nanostructure engineering is Table 3 [122]. This higher H2 uptake was ascribed to superior properties
required for production of promising nanomaterials achieving hydrogen attained. Deep learning has recently provided an intelligent method for
storage capacity for practical working conditions. screening and investigating the most promising MOFs for hydrogen
storage, with the aim of conducting further experimental investigations
[123]. Thus, several MOFs have been screened as depicted in Fig. 16a.
2.4. Nanoporous based hydrogen storage nanomaterials However, IRMOF-20 and MOF-5 affords higher volumetric H2 uptake
capacities rather than other MOFs tested [123]. In contrast, the gravi­
Actually, nanoporous materials (NPMs) are a distinct class of nano­ metric H2 uptake of the other three MOFs is shown to be greater
materials characterized by their exceptional structure and morphology reaching 35.5 g H2/L, compared to the benchmark MOFs which exhibit
containing pores in nanoscale dimension [105]. These materials are near to 33.4 g H2/g as depicted in Fig. 16b. The research presented a
distinguished by their distinctive pore structure. It is noteworthy that negative association between the usable H2 storage capacities in these
NPMs are categorized according to their pore sizes and their chemical MOFs and the volumetric SSA and density, which contradicts previous
composition. Therefore, the classification of NPMs is determined by findings. On the other hand, Chahine's rule states that the uptake of H2 is
their pore size and can be microporous materials of pore sizes smaller greatly influenced by SSA of the sorbent material. Thus, based to this
than 2 nm, mesoporous materials of pore sizes ranging from 2 to 50 nm, rule, 1 wt% of H2 is adsorbed for every 500 m2/g [124,125]. Conse­
and finally macroporous materials of pore sizes higher than 50 nm, as quently, it is simple to forecast the effectiveness of H2 adsorption in
depicted in Fig. 15 [106]. Additionally, NPMs can be classified based on different MOFs. Also, it was found that, the porosity of MOFs strongly
their chemical composition to organic NPMs like porous polymers influenced by manipulating the reactants species [126]. Hence, engi­
[107], inorganic NPMs like zeolites, silica, and nanoporous carbons neered MOFs are better suited for H2 storage application under cryo­
[48,110,111], and hybrid NPMs like metal-organic frameworks (MOFs) genic conditions and demonstrate a significant storage capacity
[110] (Fig. 15). Therefore, the characteristic features of NPMs in terms limitation at RT. Thus, MOF-210 demonstrates a notable capacity for H2
uptake, with a value of 17.6 wt% at cryogenic temperature and 8 MPa,
which drops to 2.7 wt% at RT and similar pressure [127]. Thus, in order
to maintain the stability of H2 on MOFs surfaces at room temperature, it
is essential to have a high value of isosteric heat of adsorption (Qst)
ranging from 15 to 20 kJ/mol [128]. Therefore, incorporating active
metal sites, tunable pores, and surface functions is universally
acknowledged as a highly effective strategy for raising hydrogen uptake
at RT [129]. Therefore, there are still obstacles to enhance the capa­
bilities of nanoporous MOFs for H2 uptake at RT by increasing the
gravimetric adsorption, TPV, microporosity, reactive active sites and
SSA.
Furthermore, a variety of organic nanoporous organic polymers,
including covalent organic frameworks (COFs) [130], hypercrosslinked
polymers (HCPs) [131], conjugated microporous polymers (CMPs)
[132], and polymers with intrinsic microporosity (PIMs) [133], have
Fig. 13. Schematic diagram of the hydrogen adsorption mechanism for Ni/Al/ been extensively employed in the field of H2 storage to enhance uptake
graphene composites. capacity. Interestingly, Yaghi's research team presented the first porous
Reproduced with permission [100]. Copyright 2019, Elsevier. COFs as materials for storing H2 [134]. COF-5, demonstrates the highest

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 14. Schematic diagram of dry ball milling exfoliation and facile post-synthesis modification of palladium-decorated graphene-like materials dedicated to room
temperature H2 adsorption.
Reproduced with permission [101]. Copyright 2024, Wiley.

Table 3
State of art of hydrogen storage materials (HSMs) performance of nanoporous-
based adsorbents.
Material Adsorption Adsorption H2 uptake Ref.
temperature pressure (bar) capacity
(K) (wt%)

MOF-5 78 20 4.5 [116]

MOF-5 298 20 1 [116]
NU-110 77 45 8.82 [122]
MOF-399 77 45 9.02 [122]
MOF-210 77 80 17.6 [127]
MOF-210 298 80 2.7 [127]
COF-5 77 80 3.5 [134]
Hypercrosslinked 77 1.2 1.5 [107]
polymer
Microporous 77 15 3.04 [146]
hypercrosslinked
polymer
PIM-1 77 10 1.44 [154]
AMC-750-5 77 20 4.77 [162]
SBL-PNP-0.5-2-800 77 20 4.5 [159]
SBL-PNP-0.5-2-800 298 20 0.15 [159]
PS 77 20 1.29 [160]
BC-3 77 1 3.04 [163]
BC-3 298 50 0.85 [163]
SF-4600 77 20 8.1 (total) [165]
SF-4600 77 30 10.4 (total) [165]
SF-4600 77 40 11.2 (total) [165]
CA-4700 77 30 8.9 (total) [167]
CA-4700 298 30 1.2 (total) [167]
C60-CC-PNP 77 20 4 [108]
C60-CC-PNP 298 20 0.173 [108]
M-C-KOH-4-800 77 25 6.1 (total) [161]
M-C-KOH-4-800 298 25 0.45 (total) [161]

family derived from COF-102 [138]. This engineering modification

leads to a significant increase in the uptake of H2, reaching up to 26.7
and 6.5 wt% at temperatures of 77 and 300 K, and a pressure of 100 bar
Fig. 15. Schematic flow chart displaying the classes of NPMs based on their respectively, as shown in Fig. 17. The boost in H2 uptake is attributed to
pore diameter and chemical composition. the significant increase in SSA, pore volume, and heat of adsorption.
These factors combined facilitate the process of physisorption of
SSA of 1590 m2/g and a storage capacity of 3.5 wt% H2 at 77 K and 8 hydrogen molecules in nanopores of COFs and strengthen the interac­
MPa (Table 3) [134] this storage capacity was attributed to porosity. tion with nanopores walls [138]. While COFs demonstrate substantial
Subsequently, 3D-COFs family, were developed with a greater SSA H2 uptake capacity under high pressure, the storage capacity of COFs
compared to 2D COF-5 [135]. Thus, COF-105 was predicted to exhibit significantly decreases when the adsorption temperature is raised. Thus,
superior H2 uptake of 10 wt% at 77 K and 100 bars [136,137]. However, in order to counteract these technical limitations, metal-doped COFs
COF-102 predicated to achieve a remarkable volumetric capacity of were developed that have enhanced H2 holding capabilities at high
40.4 g/L [136]. It is noteworthy that several engineering alterations temperatures [139–141]. Thus, multiple theoretical and experimental
were implemented in COF-102 resulting in the formation of new COF investigations have carried out and displayed improved storage of H2 in

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 16. (a) Crystal structures of MOFs whose hydrogen uptake was assessed experimentally following their identification by computational screening. a PCN-610/
NU-100, b SNU-70, c ZELROZ, and d UMCM-9 (C: gray, H: white, O: red, Cu: orange and Zn: blue) and (b) H2 adsorption isotherms. Measured total (a) volumetric and
(b) gravimetric H2 adsorption isotherms of NU-100, SNU-70, and UMCM-9 at 77 K. For comparison, isotherms for the two benchmark MOFs, MOF-5 and IRMOF-20,
are also shown. Inset plots illustrate capacities at low pressure [123]. (For interpretation of the references to color in this figure legend, the reader is referred to the
web version of this article.)

metal-doped COFs [138,142–144]. microporosity [152,153]. PIM-1 was initially introduced based on
On the other hand, alternative economically viable porous polymers cyclotricatechylene (CTC), achieving an SSA of 760 m2/g and an H2
were tested for hydrogen storage performance such as HCPs, CMPs, and uptake capacity of 1.4 wt% at 77 K and 10 bar (Table 3) [154]. Notably,
PIMs, which provide a flexible structure, convenient functionalization, the process of thermal annealing of PIM-1 resulted in superior hydrogen
adjustable porosity, low density, and excellent processability. Hyper­ uptake by 100 % [154]. Thus, in order to meet the current storage ca­
crosslinked polymer of SSA of 1930 m2/g was developed and record H2 pacity goals, set by the US Department of Energy (USDOE) for practical
uptake of 1.5 wt% @ 77 K and 1.2 bar (Table 3) [107]. Thus, engineering H2 storage materials, extensive engineering of nanoporous materials and
was implemented to improve microporosity [145]. Other HCPs had SSA research is necessary, particularly in relation to achieving storage ca­
of 2090 m2/g exhibited a significant H2 uptake of 3.04 wt% under 77 K pacity at room temperature (RT).
and 15 bar [146] higher H2 adsorption value was stemmed from supe­ On the other hand, nanoporous carbon materials presents potential
rior microporosity and SSA. Recently, a series of HCPs were developed cost-effective and sustainable hydrogen storage materials
and the synthesized HCPs have outstanding textural characteristics [109–111,155,156], because of their high textural properties, custom­
recording SSA reach to 1132 m2/g with superior microporosity [147]. It izable pore construction, chemical stability, plenty and economical
is found the augmentation of crosslinking significantly amplifies mi­ synthesis procedures [109–111,155–157]. Thus, the activated carbons
cropores and mesopores volume. In addition, conjugated microporous (ACs) of higher SSA and pore volume are widely used form of nano­
polymers (CMP) are polymers that include pores and are characterized porous carbon for storing hydrogen. Therefore, it has been determined
by conjugated structures. The poly(aryleneethynylene) of SSA 1018 m2/ that the ideal pore diameter for effective hydrogen storage in activated
g was initially employed for H2 storage recording storage capacity of 1.4 carbons (ACs) is between 0.6 and 0.7 nm [158]. It is worth noting that
wt% under 77 K and 1.0 bar conditions [148]. As a result, the imple­ the presence of elements with high electron density, such as oxygen,
mentation of structural modifications and the addition of heteroatom/ nitrogen, and sulfur, on the surface of activated carbons (ACs) enhances
metal doping led to the creation of several CMPs that could achieve good the strength of the binding interactions between hydrogen molecules
storage capacity [149–151]. Polymers with intrinsic microporosity and the adsorbents. As a result, this leads to an increased capacity for
(PIMs) are another class of polymers consisting of a large, flat backbone storing hydrogen gas [105,109–111,159–161]. Thus, N-doped AC of SSA
and separate ring spacers. These components integrate a distorted 2378 m2/g and micropores features affording storing of hydrogen
structure and increase the interior volume, resulting in inherent molecules by 4.8 wt% at 20 bar and cryogenic conditions which ascribed

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 17. (a) The different organic moieties that have been used for the construction of the COF materials. By using the same topology as COF-102 and the same
connectivity and alternating the organic moieties there have been constructed a series of periodic COF cells ranging from COF-102 to COF-102-5. Carbon, oxygen,
boron, and hydrogen atoms are shown as gray, red, pink, and white colors, respectively and (b)Predicted total gravimetric and volumetric adsorption isotherms at 77
and 300 K for COF-102, COF-102-2, COF-102-3, COF-102-4, and COF-102-5. (For interpretation of the references to color in this figure legend, the reader is referred
to the web version of this article.)
Reproduced with permission [138]. Copyright 2010, the royal Society of Chemistry 2010.

to high microporosity and high nitrogen doping boost (Table 3) [162]. It This process offers both environmental and economic advantages.
is noteworthy that bio-wastes, such as by-products of fruits and other Additionally, it results in the incorporation of valuable precious metals
biomass and agricultural wastes, can be used as sustainable carbon and heteroatoms into the generated porous carbon, which greatly en­
precursors for the synthesis of sustainable nanoporous carbon materials. hances its ability to adsorb H2 [68,109,159–161]. Therefore, the

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

nanoporous carbon derived from peanut shell as agricultural by prod­ developed from cellulose acetate affords a superior total capacity of H2
ucts achieved H2 uptake of 1.29 wt% at 20 bar (Table 3) this uptake is recoding 8.1 wt% @ 77 K and 20 MPa. This higher uptake is ascribed to
ascribed to microporosity and presence of precious elements naturally their exceptional SSA of 3800 m2/g, and TPV of 1.8 cm3/g, in addition to
doped [160]. A noteworthy development involved the production of a oxygen-rich surface. Additionally, the total H2 uptake capacity at RT was
sustainable nanoporous carbon with a high surface area, nitrogen, and found to be 1.2 wt% at 30 bar (Table 3) [167]. It is important to mention
oxygen doping [159]. This was achieved by recycling sugar beet leaves that the amount of H2 molecules on the surface decreases significantly at
into graphite flakes and subsequently incorporating polymer nano­ high temperatures compared to very low temperatures, and the increase
particles. This process resulted in the production of a highly porous in H2 adsorption due to improved porosity is limited. Thus, it is strongly
activated carbon, which was further enhanced with spherical porous advised to alter ACs by including heteroatoms or producing composites.
carbon nanoparticles recording SSA and TPV of 2777 m2/g and 1.86 Hence, carbon-based composite was developed consisting of nanoscale
cm3/g through chemical activation, as illustrated in Fig. 18 [159]. The carbon shells containing encapsulated V-doping Mg nanoparticles
attained H2 uptake capacity of 4.5 and 0.15 wt% at temperatures of 77 [168]. This composite material demonstrates remarkable hydrogen
and 298 K and 20 bar, as shown in Table 3 [159], can be attributed to the storage capabilities, with storage capacity of 6.6 wt% at temperatures of
elevated values of SSA, TPV, microporosity, and the increased doping of 473/573 K and 40 bar [168]. Recently, ultrahigh specific surface area
nitrogen and oxygen functional groups. AC was developed by chemically activating a polymer based on mel­
Other sustainable nanoporous AC was developed from recycling of amine. The AC achieved a SSA of 3463 m2/g, demonstrating a distinct
biomass by utilizing Bark and Camellia shell, recording high SSA of 2473 and uniform distribution of heteroatoms and a well-defined hierarchical
m2/g and achieving exceptional hydrogen storage uptake of 3.01 wt% at microporous structure. The advanced carbon material demonstrated a
77 K and 1 bar and 0.85 wt% at RT and 5 MPa (Table 3) [163]. favourable hydrogen adsorption capability of 5.2 wt% at a temperature
Furthermore, the obtained hydrogen storage capacity was corroborated of 77 K and a pressure of 50 bar [169]. The storage capacity originated
via calculation the Qst at77–87 K and which was found to be 8.0 kJ/mol. from the exceptional microporosity and the introduction of heteroatoms
Also, the value of Qst BC-control is ascribed to the excellent adsorption through doping [169]. Interestingly, in recent times, activated carbon
sites provided by oxygen functions on the carbon surface [163]. Addi­ fabric (cloth) has emerged as a highly effective hydrogen adsorbent due
tionally, sustainable hierarchically nanoporous carbons were derived to its chemical stability and flexibility [170]. The exploitation of flexible
from Neolamarckia cadamba as carbon source and demonstrate notable activated porous carbon fabric is more convenient compared to powder
SSA reaching up 3462 m2/g, and substantial TPV of 1.67 cm3/g, which one, as it affords smooth and harmless handling. This is particularly
afford H2 uptake capacity of 2.81 wt% under 1 bar and 77 K [164]. In beneficial when constructing hydrogen storage tank that are more
line with the current trend of producing sustainable ACs from recycling convenient and efficient, this in conjunction to easier adsorption kinetics
bio-wastes, an AC has been developed using recycled smoked cigarette and mass transfer [171–173]. Thus, recently, a versatile N doped acti­
filters. This AC developed has a very high SSA of 4300 m2/g, with a TPV vated porous carbon cloth (ACC) was fabricated. The flexible ACC had
of 2.09 cm3/g. Additionally, it is naturally enriched with oxygen func­ higher SSA and TPV of 2000 m2/g and 0.85 cm3/g, respectively, with
tionals [165]. The research results showed that the surplus capacity of significant N content, in addition to flexibility [108]. The attained ACC
H2 was determined to be with a total adsorption of 8.1, 10.4 and 11.2 wt achieved H2 uptake capacity of 4.0 and 0.173 wt% at 77 K and RT
%, at temperatures of 77 K and pressures of 20, 30, and 40 bars, (Table 3), respectively, under a pressure of 20 bar as seen in Fig. 19. The
respectively (Table 3), which was ascribed to outstanding SSA, TPV, high storage capacity was ascribed to microporosity and nitrogen doping
microporosity and oxygenated species [165]. Moreover, other AC was which enhance hydrogen molecules interaction with ACC surface.
developed from polyaniline yields polyaniline-derived activated carbon In another attempt for production of sustainable nanoporous carbon
(PDAC) and attained PDAC had SSA and TPV of 2200 m2/g and 1 cm3/g, from bio-waste, high porosity AC was derived from mandarin peels as
respectively [166]. The H2 uptake capacity was examined at various by-products of fruit production which offer a financially feasible and
temperature and 1 bar recording uptake values of 2.5 wt% @77 K, 1.6 wt sustainable carbon source. The developed AC has notable SSA (2500 m2/
% @ 90 K, and 1.1 wt%@ 100 K. However, at RT and higher pressure g) and TPV (1.04 cm3/g) in addition to naturally doped with sulfur. The
(80 bar), PDAC achieved hydrogen uptake capacity of 0.6 wt% [166], AC achieved higher total H2 uptake of 6.1 and 0.45 wt% under 77 and
which displayed low uptake capacity at practical conditions. Hence, it is 298 K and 25 bar as presented in Fig. 20a [161]. Thus, this mandarin
imperative to allocate further resources towards augmenting the storage peel derived AC presents sustainable, effective and economically
capabilities of hydrogen at ambient temperature. Therefore, AC hydrogen storage adsorbents as depicted in Fig. 20b.

Fig. 18. Schematic diagram of the synthesis of renewable nanoporous carbon materials based on sugar beet leaves.
Reproduced from reference [159].

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N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 19. (a) Schematic diagram describing the innovative approach for the synthesis of CC-PNP and the two dual activation methods (chemically or physically
activated CC-PNP) and (b) The H2 adsorption (closed symbols)–desorption (open symbols) isotherms for CC-PNP and activated CC-PNP at (a) 77 K and (b) 298 K at
20 bar.
Reproduced with permission [108] Copyright 2020, Elsevier.

Artificial intelligence has been used to investigate and forecast po­ 1. Incorporation of artificial intelligence, specifically machine
tential solid-state hydrogen storage materials and other types of clean learning techniques for understanding and predication of H2
and renewable energy sources [174–176]. Therefore, machine learning storage capacity.
techniques, for example, provide a more convenient method for inves­ 2. Design and engineering of carbon-based materials with ultra-
tigating and comprehending the process of H2 storage. Additionally, micropore size of 0.6–0.7 nm for hydrogen storage systems.
they allow for the evaluation of different materials capacity to store 3. Fabrication of hierarchical porous (meso-microporous) carbon
hydrogen [175–177]. Therefore, it is important to consider many as­ materials to affords good storage capacity @ RT at convenient
pects that have a major impact on the absorption of H2, such as specific pressure.
surface area, total pore volume, the presence and amount of hetero­ 4. Surface engineering the porous surface of carbon material with
atoms, and the type of species. Additionally, the ultramicropore volume high electron density elements such N, O and S.
and micropore size should also be considered as shown in Fig. 21 [124]. 5. It is crucial to have a high isosteric heat of adsorption (Qst) value
Therefore, it can provide novel perspectives for the design and devel­ within the range of 15–20 kJ/mol to afford convenient storage at
opment of innovative hydrogen storage nanomaterials, which can RT.
overcome the technological constraints associated with storing 6. Expand the exploitation of bio-wastes as sustainable carbon
hydrogen at room temperature. This, in turn, can expedite the process of precursor for production of sustainable high SSA porous carbon
making hydrogen economy commercially viable. naturally doped with precious metals.
7. Precise doping the developed hierarchical porous carbon with
3. Future perspective and research directions small metal nanoparticles for enhancing the binding energy with
H2 molecules and in turn increase storage capacity @ RT.
The delayed commercialization of hydrogen (H2) as a clean fuel for 8. Fabrication of hierarchical porous carbon cloth naturally doped
operating light-duty vehicles is the primary cause of the significant with O and N elements to afford fast kinetic for adsorption-
carbon dioxide emissions produced by cars globally. Hence, by con­ desorption and processable flexible hydrogen storage media for
ducting thorough research and applying advanced engineering tech­ tank applications.
niques to nanoporous materials, particularly sustainable nanoporous 9. Tailoring the carbon contents relative to heteroatoms contents for
carbon, in combination with artificial intelligence, it is possible to make the nanoporous carbon adsorbents.
significant progress in the development of hydrogen storage adsorbents 10. Tailoring the micropore volume and its share in total pore
that meet the necessary technical storage capacity and operational re­ volume.
quirements. Therefore, future study should consider the following 11. Expand the exploitation of nanoscale-based materials for fabri­
criteria as outlined in Fig. 22. cation of hydrogen storage media for their outstanding role.

15
N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Fig. 20. (a) H2 adsorption isotherms for the renewable developed nanoporous carbons@ 77 K (b) H2 adsorption isotherms of M-C-KOH-4-800, M-C-APS-4-800 and
M-C-4-800 @ 298 K and (b) schematic presentation displaying the valuable usage of activated porous carbon derived from mandarin peels as sustainable hydrogen
materials.
Reproduced with permission [161]. Copyright 2020, Elsevier.

Fig. 21. Schematic diagram displaying the key factors should be considering for designing and synthesis of promising hydrogen storage nanoporous carbon ma­
terials.
Reproduced from reference [124].

4. Conclusion usage of hydrogen as clean fuel for light-duty vehicle is the safe and
convenient solid-state storage media. Therefore, the ultimate objective
The bottleneck step of commercialization of hydrogen economy and of energy storage systems is to easier store and release hydrogen in solid-

16
N.F. Attia et al. Journal of Energy Storage 100 (2024) 113519

Declaration of competing interest

The authors declare that they have no known competing financial

interests or personal relationships that could have appeared to influence
the work reported in this paper.

Data availability

Data will be made available on request.

Acknowledgements

This paper is based upon work supported by the Science, Technology

& Innovation Funding Authority (STDF) under grant No. 46262.

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