2023 (Ghritalahre Et Al) - Next Generation Bio-Derived 3d-Hierarchical Porous Material For

Journal of Power Sources 587 (2023) 233648
Contents lists available at ScienceDirect
Journal of Power Sources

journal homepage: www.elsevier.com/locate/jpowsour
Review article
Next generation bio-derived 3D-hierarchical porous material for

remarkable hydrogen storage – A brief critical review
Bhupendra Ghritalahre a, b, *, Vinod Kumar Bhargav a, Sandeep Gangil a, Parmanand Sahu a,
Ravi Kumar Sahu a, b
a
ICAR-Central Institute of Agricultural Engineering, Bhopal, Madhya Pradesh, 462038, India
b
The Graduate School, IARI, India
H I G H L I G H T S G R A P H I C A L A B S T R A C T
• Carbon based material production with

properties best suited for hydrogen
storage.
• Next generation material and conven
tional method used for hydrogen
storage.
• Literature results on bio-derived carbon-
based hydrogen storage are cited.
A R T I C L E I N F O A B S T R A C T
Keywords: Today’s scientific professionals face the challenge of meeting the ever-growing demand for hydrogen fuel.
H2 Hydrogen stands as a sustainable and eco-friendly alternative. This fuel is inherently lightweight and gaseous
H2 storage Which present challenges in its production, transportation, and storage. Hydrogen fuel can be stored using
Template
different storage methods which have merits and demerits. Hydrogen can be stored by conventional methods and
Hierarchical carbon
Surface area
also using the next generation materials, i.e., pressurized gas, liquid nitrogen at cryogenic temperature, chemical
Pore volume method storage in the metal hydride, and adsorption on carbon material. According to various researches, carbon
material has been stated as a novel, emerging and next-generation material for storing hydrogen. Hierarchical
carbon having modified 3-dimensional structure and multimodal pore can be prepared from different chemically
or catalytically activation processes. The best-suited carbon material for hydrogen storage has a high specific
surface area of 2000–3000 m2/g and also high interconnectivity of pore. In this review paper, the various
hydrogen storage methods and performance of carbon materials for hydrogen storage at different pressure and
* Corresponding author. ICAR-Central Institute of Agricultural Engineering, Bhopal, Madhya Pradesh, 462038, India.
E-mail address: [email protected] (B. Ghritalahre).
https://doi.org/10.1016/j.jpowsour.2023.233648
Received 19 June 2023; Received in revised form 12 September 2023; Accepted 17 September 2023
Available online 14 October 2023
0378-7753/© 2023 Elsevier B.V. All rights reserved.
B. Ghritalahre et al. Journal of Power Sources 587 (2023) 233648
temperature are reviewed. The utilization of carbon for hydrogen storage represents a prominent technology in
addressing the obstacles linked with the use of hydrogen.
1. Introduction Fig. 1 illustrates the research articles published from 1992 to 2021,
showcasing the significant amount of research being conducted in the
The population growth is a serious concern and fulfilling the energy realm of hydrogen storage. The observed trend signifies an increasing
demand for an increased population is a major issue in the future. The level of interest within the scientific community in this domain, indi
increasing population needs some alternative energy sources and the cating a promising outlook for the advancement of hydrogen storage
replacement of fossil fuels [1]. The simultaneous rise in global energy technology. Significantly, there has been a consistent rise in the annual
demand and the depletion of fossil fuel sources like petroleum, coal, and count of research publications on hydrogen storage, with a particular
natural gas present significant challenges to energy security, climate emphasis on their application in the field of energy storage. This upward
change, as well as societal and political stability [2]. Thus, it is necessary trajectory is depicted in Fig. 1.
to adopt a new idea and alternative to address this challenge. Energy Material-based hydrogen storage specially stored in 3D hierarchical
from sources like the sun, wind, earth, water, or biomass should be porous carbon is a prominent technology and next-generation material
considered a viable solution [3]. In India, a diverse range of crops is for the future. They fulfill the alternative demand of hydrogen storage
cultivated in various regions, contributing to the country’s status as an possessing several advantages over conventional storage methods. In
agricultural-based nation. Each year, approximately 611 metric tons of conventional methods, i.e., compressed gas storage, liquid hydrogen
agricultural crop residue are produced through additional processing of storage showed some merits. Low storage capacity at high pressure [23,
crops by which 25% is available for energy generation [4]. The data 24], safety problems [24], and expansive cylinders [25] are major issues
illustrates that a significant and substantial amount of agricultural waste associated with compressed form storage. Safety issue, low temperature
is generated annually [4] and farmers used to burn crop residue in the requirement [23,25], large consumption of energy and time [25], initial
field around 120 Mt [5], and also left in open field for disposal [6] as cost [23,24] are mostly encountered demerits with liquid storage. Apart
waste management methods, which resulted in the wastage of valuable from the aforementioned methods, heavy nature [23], timely degrada
crop residues [5]. The reason behind the wastage of crop residue is the tion [23], absorbing impurities [25], and low-quality efficiency [24] are
lacuna of the waste management system. Researchers are currently some of the drawbacks faced while dealing with hydrogen storage in
paying attention to the conversion and storage of renewable energy from metal hydride materials. Overcoming these drawbacks, hierarchical
these sources, however, there are ongoing studies in the field of energy porous carbon draws the attention of researchers towards the use of
generation from crop residues, focusing on exploring various methods porous carbon for hydrogen storage and it provides several benefits such
and technologies. In the context of generation and storage of energy as it has high storage capacity [25,26], low cost [23], light material, and
from agricultural crop residues, carbon-based materials prepared from ease of production [23,26]. The utilization of porous carbon offers a dual
residues and its use as hydrogen storage material is one of the benefit. Firstly, it enables the utilization of waste materials for carbon
best-emerging technologies. production, thereby helping to mitigate waste management issues.
In general, hydrogen is stored in the form of gas, liquid, and solid [1, Secondly, this carbon production process also offers a potential solution
7]. Hydrogen storage can be achieved through various methods such as for future advancements in hydrogen storage materials.
high-pressure compression, liquefaction in a high-pressure tank, storage The hydrogen storage around 2.43–2.92 wt% was observed on beer
in solid-state hydrides, or storage in porous materials [8]. Storing lee-derived porous carbon [27]. Hydrogen uptake capacity of 1.2 wt% at
hydrogen in a solid state is considered the safest method, and it has been 30 ◦ C and 40 bars in jute fiber-derived porous carbon [1] has been re
observed that solid-state storage is a more suitable option for addressing ported. Hydrogen uptake capacity from 1 wt% to over 5 wt% in cryo
challenges related to hydrogen storage and transportation [7]. Several genic condition in Posidonia Oceanica and Wood chips derived carbon
research reported that activated carbon produced from different [10] were obtained. All the research articles and population demand
biomass is good adsorbent material for hydrogen [7,9–11]. The draw the attention of researchers toward searching the novel material or
biomass-derived activated carbon shows high surface area [10,12–14], enhancing the properties of existing materials for better hydrogen
high pore volume [13], and also good adsorbent characteristics [10,13]. storage. The review paper consists of the different hydrogen storage
The hydrogen storage ability can be increased by increasing the different technology along with the methodology adopted for the production of
properties of activated carbon produced from different biomass. The activated carbon, 3D hierarchical carbon, and their performance related
hydrogen uptake performance of activated carbons depends on and to hydrogen storage.
exhibits a linear relationship with pore-textural [15,16] and surface
characteristics, including factors such as the size and distribution of 2. Hydrogen storage material/methods
micropores and specific surface area [15]. The porosity of activated
carbons, primarily originating from micropores, is significantly influ Hydrogen storage is one of the possible ways to fulfil the upcoming
enced by activation parameters such as temperature, activating agent, energy demand and alternative way to harness the renewable source.
and other related factors [17]. Hydrogen storage capacity mainly varies from material to material.
Keeping in mind the several advantages of hydrogen storage on Advanced hydrogen storage methods offer the potential for achieving
carbon material, several kinds of research has been already carried out higher energy density. A wide range of physical and chemical hydrogen
and are under progress. The result of the previously done research work storage techniques, each with its unique characteristics and storage
concludes that carbon material is the prominent next-generation mate capacity, show promise in advancing the development of a future
rial for hydrogen storage. In the field of hydrogen storage, various hydrogen economy [28]. The Fig. 2 shows various hydrogen storage
carbon-based materials like carbon nanotubes [12], hierarchical porous methods. The hydrogen can be stored using following methods, i.e.,
carbon [18], activated carbon [19,20], carbon nanofiber [21], graphene Compressed hydrogen [21,28,29], Liquefied hydrogen [21,28,29],
[12], carbon aerogels [12], etc. were used for observing the behaviour Cryo-compressed hydrogen [21,28,29], Physically adsorbed hydrogen
and performance in relation to hydrogen storage. [21,28,29], Metal hydrides [21,28,29], Complex hydrides [21,28,29],
According to the author [22], the total count of publications based on Liquid organic hydrogen carriers (LOHC) [28,29], and Liquid organic
Scopus data on hydrogen storage between 1992 and 2021 can be sum hydrides [21,28,29].
marized as follows: The aforementioned hydrogen storage techniques will be described
2
in detail, with an emphasis on their distinguishing qualities, in the in such a manner that tank withstand the cryogenic temperature and
following subsections. internal pressure. The concept of the Cryo-compressed storage system
revolves around the design of a high-pressure vessel (approximately 350
2.1. Compressed gas bar) that operates at low temperatures (below 20 K) [38]. The storage
pressure ranges from 250 to 350 atm [28,39]. As compared to cryogenic
Compressed gas is most common method for hydrogen storage [30, hydrogen storage, cryo-compressed storage provides high storage den
31]. Typically, storage of hydrogen in compressed form required high sity 80 g/L which is about 10 g/L more. Cryo-compressed storage has
pressure tank (350–700 bar tank pressure) [32], and around 150–200 efficient and quick refuelling and high safety level due to the existence of
atmospheric pressure [33]. Cylindrical vessels are used instead of vacuumed enclosure over cryogenic storage [40,41].
spherical vessels for hydrogen storage. Cylindrical vessel has several
advantages as compared to spherical vessels and for hydrogen storage, 2.4. Metal hydrides
an ideal requirement is a lightweight and cost-effective vessel material
capable of withstanding high pressure. The chosen material should The storage of hydrogen on metal occurs when metal converts in
possess the ability to withstand hydrogen diffusion and mitigate the metal hydrides. Hydrogen interacts with many elements to form binary
potential embrittlement caused by the stored hydrogen [28]. Table 1 hydrides. The author [33] reported that there are three type of bonding
provide the summery of Four types of vessels having individual property between hydrogen and metal I) ionic (saline), II) covalent and III)
which is generally used for the storage of hydrogen in compressed gas metallic. Ionic hydride are formed by alkaline and alkali earth metals
form [28,29,34,35]. (groups IA and IIA) and covalent hydrides are formed using elements
from IIIA-VA group. Metallic hydride are formed by reacting with the
2.2. Liquide hydrogen rare earth and actinide elements, transition metal which are readily
available. The interstitial site is occupied in case of formation of metal
To store hydrogen in a liquid state, cryogenic temperatures are hydrides [33]. The storage of hydrogen in the metal is through ab
necessary as its boiling point of − 252.8 ◦ C at atmospheric pressure [32]. sorption phenomenon. The simple hydrogen storage model on metal is
Liquid storage offers a higher density compared to other storage shown in Fig. 3.
methods. At its normal boiling point of 20 K, liquid hydrogen has a Among various hydrogen storing metals, Magnesium hydride [42] is
density of approximately 71 g/L, which is roughly 1.8 times denser than most attractive material because of its affordability and abundance [29].
hydrogen pressurized up to 70 MPa at 288 K [36]. To prevent from the Electrochemical dissociation of water molecule and direct reaction of
heat leakage of stored hydrogen, special double walled vessels with the hydrogen with metal is two process by which metal hydride is
insulation is preferred. Cryogenic pressure vessels used for liquid formed [28].
hydrogen storage offer better safety advantages as compared to com
pressed hydrogen vessels due to their compact and lightweight nature Mechanism 1: Direct hydrogen reaction [66]: M + (x/2) H2 ↔ MHx
[36]. Hydrogen density in liquid form is nearly 1.5–2 time the density of
Mechanism 2: Electrochemical dissociation of water: M + (x/2) H2O + (x/2) e‒
gas compressed hydrogen at high pressure. Low pressure storage allows
↔ MHx + (x/2) OH−
for the use of relatively thin and affordable storage tanks. Slush
hydrogen is another widely used name for liquid hydrogen and at 20 K where, M represents a metal or alloy.
temperature, the liquid hydrogen is non-corrosive and colourless. Liquid Metal hydrides are capable of holding 5–7 wt% of hydrogen, but only
hydrogen tanks have a higher storage capacity, capable of storing 0.070 when heated to 2500 ◦ C or above. High temperatures of between 120
kg/L of liquid hydrogen, compared to compressed gas tanks which and 200 ◦ C are required to liberate the hydrogen content of metal hy
typically store around 0.030 kg/L [37]. drides because of their propensity to bond hydrogen firmly. Low reac
tivity (high safety) and high hydrogen storage densities are provided by
2.3. Cryo-compressed hydrogen the hydrides used for storage applications [37]. Magnesium hydrides
had an energy density of 7.6 wt% and 13.22 MJ/L, with a density of
Cryo-compressed hydrogen is combination of liquid nitrogen storage 1.45 g/cm3 [29]. Table 2 shows the lists of chosen metal hydrides and
and compressed gas storage method [28,29]. The storage tank is design alloys along with their hydrogen storage capabilities [28,36,38].
Fig. 1. Articles published between the year 1992–2021 on the field of hydrogen storage.
3
National Thermal Power Corporation Limited stated that Metal hydrides Table 1
store hydrogen in a solid form, offering a high degree of safety, revers Four types of vessel for compressed H2 storage.
ibility, high volumetric densities, and low energy requirements, making Type Material Description Pressure Cost Gravimetric
them suitable for practical applications. (bar) ($/kg) density (wt
%)
I Metallic Cheapest 30 83 1
2.5. Physically adsorbed hydrogen
Option, Low 300 1.7
gravimetric
In the physical adsorption of hydrogen, H2 molecule is stored on the density, most
adsorption principle. The hydrogen molecule is attached at surface commonly Steel
physically. The hydrogen molecule is attached with surface of material and Aluminium
is used.
through dispersive forces or van der Waals forces [14,28,43,44]. Very
II Metallic wall 30–40% less 200 86 2.1
weak interaction was observed and heat of adsorption was as low as 6–8 is wrapped weight as
kJ mol− 1 in nonporous carbons in report referenced at [45]. Porous with fiber compared to
materials, including carbon materials [46], fullerenes [30,34], Nano resin, type I
Mostly
tubes [46], graphene [46]), zeolites [34], metal organic frameworks
metal,
(MOFs) [34], covalent organic frameworks (COFs), micro porous metal composite
coordination materials (MMOMs), clathrates [37] are among the most overwrap in
commonly studied materials for hydrogen storage. The interaction en the hoop
ergy between hydrogen molecule and material is calculated by using the direction
III Carbon fiber For lining mostly 450-700, 700 4.2
formula given below [46].
composite aluminium is 700
materials preferred, strong
E = (αH2 α6substrate)/R
lined with and light weight,
metal low thermal
Where, α is the polarizability and R is the interaction distance.
Metal liner, conductivity
Moradi et al. [40] highlighted the common problems during full
hydrogen storage in two categories, i.e., issues raised during Hydrogen composite
handling and an issue arising through material properties. Hydrogen overwrap
leakage, Temperature variation, Compression process, Pressure fluctu IV All Liner is mostly 700 633 5.7
composite polymeric
ations in pipelines, and Contamination issue come under the hydrogen materials
handling. In the Impact of hydrogen on materials, liner blistering in
pressure vessels, issue of material properties giving the resistance of
storage vessels to fire and high temperatures, as well as the under cellulose, hemicellulose and lignin percentage. The properties of
standing of damage mechanisms associated with carbon fiber are biomass differ biomass to biomass. The hydrogen storage capacity of
covered. Table 3 manifest the various hydrogen storage methods with carbon materials primarily relies on surface area, which is influenced by
their capacities [29,41,47–53]. Due to the distinct characteristics of the distribution of micropore sizes, particularly the presence of narrow
each storage method, making a direct comparison becomes challenging micropores [7]. The most commonly used primary materials for
[29], and drawing a specific conclusion for single storage method extracting activated carbon include coal, coconut shell, wood, and
become difficult. various industrial wastes [6]. Posidonia Oceanica is sea plant mostly
collected from sea coast and before processing, the plant is washed
3. Biomass material for hierarchical carbon production thoroughly using normal water and distilled water to remove the salt
[10]. The size of wood chips and sea plants is reduced and further
Lignocellulosic biomass is mostly used for production of activated processing is done [10]. Several researchers reported that various pre
carbon. Different type of Biomass contains different proportion of cursor such as Coffee beam waste [15], Corncob [54], Lotus stalk [54],
Fig. 2. Classification of hydrogen material and methods for hydrogen storage.
4
Fig. 3. Simplified hydrogen storage model on metals.
pyrolysis temperature is recognized as the primary parameter that

Table 2
significantly influences the surface area and porosity of biochar [76].
List of Metal hydride and alloys for hydrogen storage.
Carbonization can be categorized into slow pyrolysis and fast pyrolysis
Material Metal Weight percent of Desorption depending on the heating rate [77] and residence time [58,73]. The fast
Hydride/ hydrogen stored [wt. temperature (◦ C)
pyrolysis results the higher production of bio-oil whereas slow pyrolysis
Alloys %]
produces higher quantum of char [73]. Apart from this carbonization
MgH2 Hydride 7.6 >300
method, microwave assisted pyrolysis [78], plasma pyrolysis [79], ul
Mg2NiH4 Hydride 3.59 >280
Mg2FeH6 Hydride 5.5 >300 trasonic assisted pyrolysis [80] is the emerging technique used for
FeTiH2 Hydride 1.89 >30 carbonization and activation and further research is going on.
LaNi5H6 Hydride 1.4 >100
MgH2–LiAlH4 Hydride 9.4
5. Methods of hierarchical carbon production
>250
(1:1 M)
MgH2–NaAlH4 Hydride 7.6 >175
(1:1 M) Activated carbon is non-hazardous, high carbon containing (up to
MgH2–LiBH4 Hydride 11.4 >350 90% [81]) material derived from pyrolysis of biomass having high
LiNi5 Metal/Alloy 1.49 –
surface area and high pore volume. The activated carbon mainly used for
ZrMn2 Metal/Alloy 1.77 –
TiMn1.5 Metal/Alloy 1.86 –
water purification and desalination, wastewater treatment and air pu
TiMn1.4 V0.6 Metal/Alloy 2.15 – rification [81], for capturing the impurities. Many of the research was
hcp-Ti, bcc-V Metal/Alloy 3.70 – previously done on the production of activated carbon and their utili
TiFe Metal/Alloy 1.86 – zation and authors of the work either used two-step process (carbon
Mg2Ni Metal/Alloy 3.60
ization and activation) [58] or three step process (synthesis,
–
carbonization and activation) [43]. The [82,83] reported two activation

sword bean shells [55], Palm kernel shell [56] were good precursor for method, i.e., physical activation and chemical activation and the
biochar production. The biomass characterization plays important role [84–86] reported three activation method, i.e., template free (chemical
for differentiating the biomass using elemental composition ultimate or physical activation), hard template method and soft template method.
analysis [57–59], using proximate analysis [57–59]. The result per The physical a chemical method comes under template free method
taining proximate and ultimate analysis data is shown in graph (Figs. 4 [84].
and 5) [60–71]. Thermogravimetric analyses are also done to find out
the thermal degrading behaviour of biomass and TG curves, which can
5.1. Template method
reveal the carbonization and activation processes [10,55].
5.1.1. Hard template method

4. Methods of carbon production (pyrolysis/carbonization)
Nano casting is another term used in place of hard template [84].
Porous carbons can also be generated using templating methods, which
Thermo-chemical conversion of biomass results the production of
utilize non-reactive porogenic substances (templates). One such method
char and other products. Pyrolysis is a process that involves the thermal
is the hard template approach, where the carbon precursor is infiltrated
decomposition of organic materials under conditions where oxygen is
into a porous matrix [87]. The hard templating mostly involves the three
either absent or minimal [58]. In the pyrolysis process, the complex and
major steps namely 1) use of rigid skeleton structure of molecular sieves,
polymeric constituents of biomass, such as lignin, cellulose, fats, and
porous alumina films and mesoporous silica as template, 2) filling the
starches, undergo through thermal degradation, resulting in the for
pore space with water soluble carbon precursors like furfural, sucrose
mation of three distinct fractions: bio-oil, char, and gases [72,73]. The
and phenolic resin, etc., and 3) Template removal after high temperature
proportion of production of these three products is depends on feedstock
carbonization [84]. However, production of porous carbon from hard
type, pyrolysis condition, temperature and heating rate [74,75]. The
templating method possess several drawbacks such as generation of lot
5
Table 3
Comparison between different hydrogen storage methods.
Method of H2 Pressure, H2 storage Gravimetric Energy Volumetric Energy Remark
storage Temperature capacity Density (wt %) Density (MJ/L)
% wt H2
Compressed 1 bar, 298 K 100 – 0.01 Volumetric capacity was 24 g/L at 350 bar, 20 K and 40 g/L at 700 bar,
350 bar, 298 K 100 – 2.94 20 K. Mainly used for industrial and vehicular or mobile applications,
700 bar, 298 K 100 – 4.97 High-pressure requirements.
700 bar, 293–298 5.7 – 4.9
K IV type
Liquid 1 bar, 20 K – 7.5 6.4 volumetric capacity was 70 g/L at 1 bar and 20 K, Boil-off hydrogen is a
1 bar, 20 K 100 – 8.5 major disadvantage
1 bar, 20 K (tank 14 – 6.12
incl.)
Cryo-compressed 350 bar, 20 K 100 9.6 volumetric capacity was 87 g/L at 240 bar and 20 K, The Cost associated
300 bar, 40–80 K – 5.4 4.0 is a major problem.
MOF 20–100 bar, 78 K – 4.5 7.2 Remarkable density was observed at very low temperature.
80 bar, 77 K 79 – 3.1
Metal hydrides 20 bar, 260–425 K – 7.6 13.2 A thermal management system is required.
Complex hydride – 7.5 – 9.6 Reversibility of hydrogen is a major problem.
Carbon 100 bar, 298 K – 2.0 5.0 Reasonable at cryogenic temperature and high pressure.
nanostructures 30–60 bar, 77 K 5 – 2.4
(AC)
40 bar, 77 K 2.55 – 2.4
(Zeolite)
K- Kelvin, AC - Activated Carbon, MOF- Metal organic framework, H2- Hydrogen.
Fig. 4. Proximate analysis of different biomass material.
of toxic pollutant during carbon production [84], generation of harmful crystal [96] are utilized to make a certain structure, and the structure is
corrosive product like concentrated NaOH, hydrofluoric acid and chlo combined with hydrogen bond, electrostatic bond and hydrophobic
rine [87], and massive use of templating agents [88]. Due to the above interaction. At the last step the surfactant is removed by pyrolysis for
reasons, the method is tedious, complicated [85,89] and expensive [85]. producing porous structure [84]. The morphological properties of
To overcome the drawback of the hard template method soft template porous carbon produced from hard and soft templating method is
method is proposed [84]. diverse, and due to high cost of production and complexity it is difficult
to industrialise the carbon production. Fig. 6 depicts the production of
5.1.2. Soft template method porous carbon prepared from endo-templating method.
The soft template method utilizes the block copolymers with ther
mosetting resin or metal-organic framework for production of porous 5.1.3. Template free method
carbon [90]. Soft templating is popularly known by endo-templating
method [87]. In the soft templating method, the surfactant like mi 5.1.3.1. Physical activation. The process of increasing porosity through
celles [91], vesicles [92], yeast [93,94], microemulsion [95] and liquid the application of high temperatures in an oxidative environment is
6
Fig. 5. Ultimate analysis of various biomass.
Fig. 6. Schematic illustration of the endo-templating (soft templating) method.
referred to as physical activation or thermal activation [97,98]. or several drawbacks, including the potential for apparatus corrosion
gaseous activation [76,77]. Several studies have been done previously caused by chemicals, challenges in recovering the chemicals used, and
on the physical activation and author stated that physical activation the high cost associated with acquiring the necessary chemicals [77].
involve oxidizing agent such as steam [76,77,81,82,99], carbon dioxide The chemicals reported for activation were alkali metals (KOH [1,13,76,
[76,77,81,82,99], ozone or air mixture [76,77,81,82,99], CO2 and ni 100], K2CO3 [90], NaOH [1], Na2CO3), metal salts (AlCl3, FeCl3, ZnCl2
trogen [81]. The temperature range kept during physical activation was [1,58,101]) and acids (H3PO4 [1,76], HCl [101], H2SO4 HNO3) [82].
800–1100 ◦ C [81,99], 350–1000 ◦ C [76], 600–1200 ◦ C [82] and above
700 ◦ C [77].
5.2. Effect of hierarchical carbon production methods on hydrogen
5.1.3.2. Chemical activation. Chemical activation involves doping the storage
char with a chemical agent, which leads to the formation of micropores
through subsequent dehydration and oxidation processes [77]. Chemi Hierarchical porous carbon materials are widely studied and utilized
cal activation methods are preferred over the physical method because as potential candidates for hydrogen storage due to their relatively high
chemical method gives higher surface area, pore volume, surface func surface area, and tunable porosity. The fabrication method adopted for
tionality [82]. Despite its advantages, chemical activation also has carbon production can directly alter the porosity and specific surface
area of produced porous carbon affecting the hydrogen storage. In their
7
study, Komatsu et al. employed KOH chemical activation to produce and macropores (diameter >50 nm) [110]. Pores within porous carbon
porous carbon from rice husks. They observed a hydrogen storage ca play distinct roles i.e. micropores primarily serve for adsorption, mac
pacity of 7.2 wt% at 77K, corresponding to a surface area of 1978 m2/g ropores act as carriers, and mesopores play a contributing role in the
[44]. Similarly, hydrogen storage capacity 6 wt% and 1.22 wt% at adsorption process [111]. Micropores provide high-capacity storage,
− 196 ◦ C and 25 ◦ C, respectively, having 1296 m2/g surface area and while mesopores enhance the kinetics of hydrogen adsorption and
0.61 cm3/g pore volume were observed at 200 bar when olive pomace desorption, making porous carbon a promising material for hydrogen
KOH derived activated carbon was utilized [102]. Table 4 compares the storage applications.
hydrogen storage capacity of various hierarchical porous carbon fabri Liu et al. stated that the activation process resulted the formation of
cated from different biomass. Based on the findings, it can be inferred meso- and micro-pores by decomposing the bio-polymers and presence
that the chemical method of producing porous carbon holds an advan of meso-as well as micro-pore in the as-prepared carbons could be
tage over other methods. The reason behind adoption of chemical regarded as hierarchical porous structure [112]. Similarly, structure of
method is production of carbon materials with higher surface areas and activated carbon might collapse while removing templates from hier
better-defined pore structures leading to superior hydrogen storage ca archical carbon resulting in the formation of interconnected network of
pacity. Other methods are selected based on the specific requirements of pores [113] and thus, the as prepared carbon could be regarded as
the situation. Tailoring the fabrication process to optimize surface area, 3D-hierarchical porous carbon [112,114]. The specific combination of
pore size distribution, and interaction strength can lead to improved these pore types could be tailored to optimize hydrogen storage per
hydrogen storage capacity, making carbon-based materials more formance for different operating conditions.
promising for future hydrogen storage applications. Hierarchical porous carbon is effectively prepared by various tem
plating methods [45,115–117]. The morphological properties like sur
6. Hierarchical carbon as hydrogen storage face area and pore size distribution can be precisely controlled using
these methods [118]. Size and microstructure of the template used for
6.1. Impact of template on quality of hierarchical carbon production of porous carbon greatly influence the pore structure of
fabricated porous carbon resulting in change in BET surface area [119].
Hierarchical carbon is prepared using different method, i.e., hard Typically, the sponge-like morphology was observed having large pore
template, soft template and template free method. Porous carbon pro size (>5 nm) when NaCl particle was used as template. The ultra-thin
duced from each method possess unique property. The produced porous carbon wall separated the large voids present in the carbon
carbon is containing mesopore, micropore and macro pore structure. morphology and in these cases 500 m2/g BET surface area was observed
Hierarchical porous carbon is characterized by its pore size distribution, which is consider as poor texture [87]. In a study Zue et al. observed the
which includes both meso- and micro-pores. The IUPAC has categorized surface area with the mixture of NaCl as template, urea (7% N) and
the pores existing on the surface of porous carbon into three groups: different concentration of Na2SiO3. The significant difference in
micropores (diameters <2 nm), mesopores (2 nm < diameter <50 nm), meso-pore was observed with increase in BET surface area from 450
m2/g with 0% Na2SiO3 to 900 m2/g with 2% Na2SiO3 [120]. High sur
face area (1660 m2/g) has observed in produced micro-mesoporous
Table 4
Comparison between the performance of various porous carbon synthesis
carbon by Chen et al. using lignin-resorcinol-formaldehyde polymer
methods using biomass precursors. synthesized in a NaCl hypersaline solution. Carbonization of mixture of
NaCl (controlled amount) and dried egg white produce porous carbon
Biomass Method adopted Surface area Performance of Ref.
precursor (m2/g), hydrogen storage
having surface area 1750 m2/g. The structure of yielded porous carbon
Pore is 3D honeycomb-like network having 100–200 nm void size with inner
volume cubic mesopore of 20–50 nm [121]. Combination of sucrose, NaCl and
(cm3/g) diluted of H2SO4 gave hierarchical micro-mesopore structure having 1.8
Corn cob Chemically 3012, 2.0 wt% at 77 K,1 [54] cm3/g pore volume and 1700 m2/g BET surface area [122]. Solubility
activated using 1.7 atm and 0.6 wt% feature of the NaCl template provide solution for removal of NaCl using
KOH, K2CO3, or at 298 K,5 MPa.
deionized water [123].
NaOH
Coffee bean Chemically 2070 4.0 wt% at 77 K [15]
Similarly, like NaCl as a template various other template can also be
waste activated using and 0.6 wt% at utilized to alter and adjust the BET surface area of hierarchical porous
KOH 298 K. carbon. Zeolite having template size 10–15 nm are utilized to produce
Posidonia Chemically 2835, 6.40 wt% at 77 K [10] porous carbon with high BET surface area around 2280 m2/g [124].
Oceanica activated using 0.73 and 0.55 wt% at
Zhao et al. observed the BET surface area 850 m2/g while synthesising
and Wood KOH 298 K.
chips porous carbon using Nano-CaCO3 nanoparticle as a template having size
Melaleuca Chemically 3170 4.08 wt% at 77 K, [103] ~50 nm [125]. Porous carbon containing very low BET surface area
bark activated using 10 bars 32.8 m2/g was prepared using NaCl particle as template size ~5 μm
KOH [126]. The surface area of porous carbon can be altered using small
Pine wood Calcium citrate 1688 0.73–1.80 wt% at [104]
pellets tetrahydrate as 77 K, 0.1 Mpa
changes in template. ZnO template was also used to prepare ZnO
CaO template nanowire and ZnO nanocones [127]. Less than 50 nm size of ZnO tem
Tamarind Chemically 1785, 4.73 wt% at 303 [105] plate is commercially available and advantage associated with these
seeds activated using 0.94 K,4 Mpa template lead to produce highly porous carbon [87]. At high tempera
KOH
ture (750–800 ◦ C) ZnO become metallic zinc [128] and this reduction of
Olive pomace H3PO4 as 1192, 2.39 wt% at 77 K, [106]
activating agent 0.50 40 bars metallic zinc help in enhancing the micropores and mesopores. Other
Olive bagasse. Physical 1185, 3.34 wt % at [107] advantage is the removal of metallic zinc after porous carbon produc
activation using 0.52 cryogenic tion. The boiling point of zinc is high (907 ◦ C), and when it is carbonized
CO2 and steam temperature. at these temperatures the porous carbon with zinc is prepared and it is
Activated Physical 1585, 1.23 wt% at 77 K, [108]
Carbon activation using 1.44 1 bar
obviating the finale refinement [129]. ZnO nanoparticle is mixed with
CO2 sucrose and carbonized at 800 ◦ C, then the produced porous carbon
Amorphous Physical 1910 1.3 wt% at 298 K, [109] show BET surface area 819 m2/g and pore volume 3.8 cm3/g. The
carbon activation using 20 MPa process need purification with the help of dilute hydrochloric acid (HCl)
nanofibers CO2
while second process does not need purification when carbonized at
8
950 ◦ C. The porous carbon reduced from second process (950 ◦ C) show Table 6
BET surface area 1757 m2/g and 3.7 cm3/g pore volume [87]. The pore Iodine value and methylene blue number of various porous carbon derived from
volume and surface area of carbon precursors with various template is different biomass.
shown in Table 5. Precursors MB (mg/g) Precursors Iodine number (mg/g)
Tea waste 402.25 Peanut hull 813.11

6.2. Surface morphology Palm shells 163.00 Coconut coir pith 203.00
Sorghum residues 386.10 Bagasse 626.00
Oil palm fibre 312.50 Sorghum 667.00
The biomass in its natural form exhibits very less specific surface Date pits 259.20 Millet straws 593.00
area. Biomass can be transformed into other forms with good surface Cotton stalk 193.50 Tobacco stem 1264.51
morphological properties suitable for different applications. Carbon
ization and thermal treatment with different activating agents like KOH,
HNO3 etc, is the best way to enhance the surface properties of raw Similar type of results was also obtained by Gadiou et al. while
biomass. Jackfruit peel and Cow Dung were used to produce highly examining the nanostructured carbon prepared by templating methods.
porous carbon with phosphoric acid as activating agent. Among the They noticed a correlation between the capacity for hydrogen adsorp
various treatment, the highest surface area was found at 1585 m2/g in tion at 77 K and the extent of micro porosity. They observed the
jack fruit peel and 2450 m2/g in cow dung-derived porous carbon [135]. hydrogen adsorption capacity as a function of the microporous volume
Hardwood alkali lignin (HPAC-H), sodium lignosulfonate (HPAC-L), and and direct correlation between material characteristic and storage ca
softwood alkali lignin with KOH treatment at 800 ◦ C was used to pro pacity [141].
duce microporous carbon. Among the samples tested, HPAC-H exhibits Hierarchical three-dimensional porous carbon contains meso, micro,
the highest surface area (2852 m2/g), total pore volume (1.50 cm3/g), and macropores all over the surface, and also connectivity of the pore in
and oxygen content (10.61 at%). In comparison, HAPC-L demonstrates two ways. The interconnectivity of the pore structure emphasizes the
slightly lower values (2397 m2/g, 1.37 cm3/g, and 9.13 at%), while hydrogen storage on the carbon surface. Garlic peel was used to produce
HAPC-S shows intermediate values (2518 m2/g, 1.41 cm3/g, and 9.59 at 3D hierarchical porous carbons (PCs) with ultrasonic-assisted impreg
%). Apart from that 1671.66 mg/g, 1182.84 mg/g, and 1409.32 mg/g nation and a change in specific surface area from 2548 m2/g to 3887 m2/
were methylene-blue (MB) adsorption capacity respectively [136]. The g was observed [80]. Similarly, 3-dimensional hierarchical carbon was
author observed considerable change while converting porous carbon derived from corn cob via template-free method and KOH activation
material prepared from Posidonia Oceanica and wood chips have shown showed a specific surface area of 2288 m2/g [142].
significant improvements in hydrogen storage capabilities. These im A pyrolysis vapors with calcium citrate template method has been
provements include increased weight percentages of hydrogen storage, developed for preparing porous carbon material from raw biomass.
ranging from 58 to 69 wt% to 93–96 wt%, expanded surface areas from Porous carbon from biomass was prepared and subjected to physi
41 to 425 m2/g to 2810–2835 m2/g, and enhanced H2 adsorption in ochemical characterization and hydrogen adsorption experiments. The
cryogenic conditions, rising from 0.1 wt% to over 5 wt% [10]. Hemp developed carbon had the largest specific surface area (1703 m2/g) and
bast fiber was hydrothermally treated with two-step process (Hot water pore volume (0.51 cm3/g) with micro porosity of 24.17%. Apart from
processing and activation with KOH and NaOH). The resulting porous the surface properties, at atmospheric pressure and 77 K temperature,
carbon achieved a remarkable surface area of 2425 m2/g [137]. Table 8 the carbon material exhibited a hydrogen adsorption capacity of 170.12
shows the various hydrogen storage capacity of bio-derived porous cm3/g (1.53 wt%) [143].
carbon with their morphological properties. Based on the referenced Olive pomace was used to produce highly porous carbon with KOH
literature in Table 8 , it is evident that hydrogen storage in porous activating agent. The produced carbon was tested for hydrogen storage
carbon at higher temperatures is significantly lower when compared to at different pressure and temperature. At 200 bar pressure, the prepared
hydrogen stored at cryogenic temperatures (77K). A similar type of carbon sample had a hydrogen storage capacity of 6 wt% and 1.22 wt%
statement is also given by author [47] in which hydrogen storage at 77 K at − 196 ◦ C and 25 ◦ C, respectively [102]. Similarly, fungi-based porous
is observed up to 5 wt% whereas at 296 K stores up to 1.3 wt%. carbon used for hydrogen storage had hydrogen uptake of up to 2.4 wt%
Panella et al. selected various carbon nanostructures (activated at 1 bar and − 196 ◦ C and at high pressure, upto 35 bar, hydrogen uptake
carbon, amorphous carbon nanotubes, SWCNTs and porous carbon) and reaches 4.2–4.7 wt% at − 196 ◦ C [17]. Single step process was used for
examined the hydrogen adsorption capabilities under high-pressure transforming Honeyvine milkweed to highly porous carbon with inter
conditions, both at room temperature and at 77 K. They observed that connected pore spaces. The developed carbon had a high surface area of
at room temperature, hydrogen storage capacity was a linear function of 756 m2/g and a hydrogen uptake capacity of ~1.75 wt% at 298 K and
pressure and at 77K. in study, A linear relation between hydrogen up 100 bars [144].
take and specific surface area (SSA) was observed for all samples. Among Typically, the porous carbon prepared from different biomass using
all samples, activated carbon having 2560 m2/g specific surface area template-free methods, i.e., with chemical and without chemicals, has
showed storage capacity of 4.5 wt% at 77 K [138]. Author [139] also good characteristics when compared with templated method of carbon
observed the hydrogen storage capacity as a function of total surface production. The number of problems associated with the template
area at 77K. A correlation between hydrogen storage and surface area method of carbon production were the reason where the template-free
was observed while treating SWCNT and activated carbon [140]. method of porous carbon came one step ahead. Two-dimensional
Table 5
Properties of porous carbon derived using different template.
Precursor Template used Size of template Surface area (m2/g) Pore volume (cm3/g) Ref.
Ethylene calcium-containing nanocrystalline Beta zeolite – 2280 1.95 [124]

Gelatine ZnO Nano particle – 2410 3.44 [128]
Polyvinyl Alcohol MgO nanoparticles – 1600 – [130]
Sucrose and dicyandiamide Potassium chloride (KCl) >5 μm 596 – [131]
Phenolic resin and sucrose CaCO3 <100 nm 850 3.3 [125]
Citrate salt ZnO/CaO <50 nm 1600 2.6 [132]
Fe oleate Fe3O4 ~12 nm ~1000 – [133]
Sucrose, gelatine KCl >5 μm <500 – [134]
9
Table 7
Comparison of different morphological properties of carbon precursor using different templates.
Precursors/ HPC Material Template used/Synthesis Properties Image Ref.
Carbon source
Resorcinol- Hierarchical macro- meso- Template free, Ca(NO3)2 impregnation SSA = 624 m2/g [182]
formaldehyde microporous carbon monolith followed by CO2 activation Mesopore volume
= 0.38 cm3/g
Micropore
volume = 0.22
cm3/g
SEM
Lignin Hierarchical macro-mesoporous Dual-templating, P123 as soft template, SSA = 803 m2/g [183]
carbon monolith mesoporous silica as hard template V (pore volume)
= 0.86 cm3/g
TEM
Phenolic resin Hierarchically macro/mesoporous Dual-templating, SiO2 opal as a hard SSA = 1667 m2/g [184]
carbon template, V (pore volume)
F127 or P123 as a soft template = 4.80 cm3/g
SEM
Sucrose Dual-templating, colloidal SSA = 818 m2/g [185]
Polymer and silica spheres V (pore volume)
= 1.29 cm3/g
SEM
(continued on next page)
10
Table 7 (continued )
Precursors/ HPC Material Template used/Synthesis Properties Image Ref.
Carbon source
Resol Hierarchically carbon spheres with Dual-templating, Monodisperse silica SSA = 972 m2/g [186]
hollow macro-porous core and spheres as hard template, F127 as soft V (pore volume)
mesoporous shell template = 1.27 cm3/g
SEM
Resols Hierarchically/bimodal macro- Dual-templating, Tri-block polymer SSA = 760 m2/g [187]
mesoporous carbon F127 as the soft V (pore volume)
template, monodispersed = 1.25 cm3/g
silica colloidal crystal as the hard
template
SEM
Corn cobs Hierarchically disordered Micro- Template free, Carbonization and KOH SSA = 2288 m2/g [142]
mesoporous carbon powder activation V (pore volume)
= 1.21 cm3/g
TEM
Glucose Hierarchical macroporous carbon Template free, Carbonization and KOH SSA = 3106.7 m2/ [188]
foam with bi-continuous micro- activation g
mesoporous V (pore volume)
= 1.82 cm3/g
SEM
Divinyl- benzene Uniform, macro-porous carbons with Dual-templating approach by mixing SSA = 465 m2/g [189]
mesoporous walls monodisperse polystyrene spheres and V (pore volume)
silica particles = 1.32 cm3/g
SEM
SSA= Specific surface area, V= Pore Volume, Ref. = Reference.
11
Table 8
Morphological parameters and hydrogen storage capacity of different activated carbon produced from biomass.
Precursor Type SSA m2/g Total Pore H2 Uptake (wt%) Temp. (K) H2 Uptake Ref.
Volume, (cm3/g) Pressure (MPa)
Jute fibers AC 1224 0.74 1.2 303 4.0 [1]

Coffee bean waste AC 2070 0.58 4.0 77 4.0 [15]
0.6 298 12
Corncob AC 3012 1.7 2.0 77 0.1 [54]
.44 298 5.0
Fungi AC 2500 1.56 2.4 77 0.1 [17]
4.7 3.5
Tangerine peel AC 1230 – 1.67 77 3.0 [83]
0.20 298
Olive pomace. AC 1043 0.46 6.0 77 20.0 [102]
1.22 298
Posidonia oceanica AC 2810 0.48 6.3 77 8.0 [10]
Wood Chips 2835 0.73 6.4
Meluca bark AC 1806 0.82 2.16 77 1.0 [103]
3170 1.51 4.08
2986 1.63 3.91
Rive husk AC 2537 1.31 1 303 27 [145]
PAN Fiber 3145 2.90 1.1 303 30
Beers lee AC 1927 0.797 2.92 77 0.1 [27]
2092 1.152 2.74
2408 1.505 2.43
Corn cob AC 3708 1.99 5.80 77 4.0 [190]
1.0 298 17.0
Hemp stem AC 922 0.49 1.57 77 0.1 [191]
1365 0.73 2.58
1917 1.02 2.81
2368 1.27 2.72
3018 1.73 2.94
3241 1.98 3.28
Tamarind seeds AC 1785 0.94 4.73 298 4.0 [105]
Peanut shell AC 1726 1.08 1.2 298 10.0 [192]
Coconut-shell AC 2800 2.17 0.85 298 10.0 [193]
Litchi trunk AC 3400 1.79 2.89 77 0.1 [194]
SSA= Specific surface area, Ref. = Reference, AC= Activated carbon.
hierarchical porous carbon having stacked layer was prepared from coal particularly suitable for hydrogen storage at ambient temperatures. The
tar pitch via template free method and prepared carbon possesses a KOH-activated PAN fiber precursor exhibited the highest hydrogen
specific surface area of 3114.2 m2/g. Similarly, a two-step process, i.e., adsorption capacity of 1.1 wt% at 30 ◦ C and 30 MPa, whereas the
first carbonization at 400 ◦ C for 2 h under nitrogen and second activa KOH-activated rice husk carbon achieves a hydrogen adsorption ca
tion using KOH at temperature up to 800 ◦ C for 2 h, was adopted for pacity of 1.0 wt% at 30 ◦ C and 27 MPa [145]. Similarly, to enhance the
producing porous carbon from Neolamarckia cadamba biomass. The storage capacity and surface characteristic, Corncob-based porous car
various ratio of KOH and carbon were tested for hydrogen uptake ca bon was derived by chemical activation selecting KOH as activating
pacity in which ratio KOH/Carbon ratio 3 provided the hydrogen uptake agent, and a high surface area of 3708 m2/g and a pore volume of 2.0
capacity of 2.81 wt% at 1 bar and 77 K demonstrating a relatively high cm3/g were obtained. Among the different sample combinations tested
capability for hydrogen storage at low pressure [18]. Apart from the for storage capacity the excess hydrogen uptake of 4th sample of corn
template-free method, ethylene was carbonized at 600 ◦ C to develop cob derived carbon was 3.21 wt% at 1 bar at cryogenic temperature, and
porous carbon with using the calcium-containing nanocrystalline Beta 5.80 wt% at about 40 bar at a cryogenic temperature [146].
zeolite as a template. The produced carbon contains both micro/ All the results shown above make biomass-based highly porous
mesopores and a high specific surface area of 2280 m2/g with 1.95 carbon a promising material for hydrogen storage and other application.
cm3/g total pore volume [124]. Biomass material reduces the load on other materials’ contribution to
However, among the different activating agents available for acti the field of carbon production and its applications also provide a novel
vation in template free method, potassium hydroxide is mostly adopted and next-generation material for commercial use. Scanning electron
for producing biomass-based porous carbon. Melaleuca bark was microscope is an analysis in which we characterize the porous carbon
biomass material used for producing porous carbon by adopting a two- based on porosity [147]. Various author uses SEM for characterization.
step process. Before starting carbonization, boiling with 1 M KOH so Table 7 give detail about the different SEM images with description. All
lution for 1 h, followed by washing with hot distilled water till neutral the SEM images presented in Table 7 are reproduced from respective
pH, and then drying for 24 h at 100 ◦ C as pre-treatment package was references.
carried out. The produced carbon is calcinated and activated at 750 ◦ C to
obtain high surface area of 3170 m2/g and a large hydrogen storage 6.3. Surface functional group and heteroatoms
capacity of around 4.08 wt% at 77 K and 10 bars [103]. Likewise, beer
lees were calcinated at 600 ◦ C for 1 h at different impregnation of KOH The surface functional groups are heteroatoms which are responsible
and activated at 800 ◦ C for 1 h. Beer lees-based porous activated carbon for the chemical reactivity of organic compounds. Apart from the re
shows a hydrogen storage capacity of 2.43–2.92 wt% at − 196 ◦ C having action these also provide information regarding chemical structure.
a high specific surface area ranging from 1927 to 2408 m2/g [27]. The Fourier transfer infra-red (FTIR) analysis was employed to examine the
combination of rice husk and PAN (Poly-acrylonitrile) as raw carbon existence of surface functional groups of active carbon in the organic
precursor, activated with KOH, resulted in the production of porous compound. Coconut shell was calcinated to produce carbon and FTIR
carbon. Micropore sizes of approximately 0.9–1.3 nm were found to be analysis of as prepared carbon showed there was no formation of
12
hydroxyl group formation in the carbon sample calcinated at 700 ◦ C. energy supply for the world’s growing energy needs. Out of the various
The presence of alkynes and aromatic compounds could be detected energy sources available, hydrogen energy stands out as the second-
through the stretching vibrations of the C – – C and C–
– – C bonds at highest in calorific value and boasts non-emissive properties [162].
− 1 − 1
wavelengths of 2336 cm and 1566 cm , respectively [148]. Likewise, The simple dehydrogenation model from porous carbon is shown in
the carbon prepared from jute fibers showed the presence of O–H, C–H, Fig. 7.
and C–C bond stretching. The wave band of 3400–3450 cm− 1, 2921 Hydrogen storage works on the principle of physisorption in which
cm− 1, and 1630–1640 cm− 1 were assigned to denote the presence of hydrogen molecule is attached to the porous carbon by weak van der
hydroxyl group, C–H symmetric and asymmetric vibration mode, and wall interaction [7,111,163]. Fast kinetic involvement in the phys
C═C stretching vibration mode respectively [1]. isorption process gives benefits to adsorption and desorption [163].
The inclusion of oxygenated functional groups, such as C– – O, OH, Dehydrogenation from the porous carbon was initiated by increasing the
and COOH, are crucial for enhancing the performance of biochar in temperature (thermal desorption) of the material [77,164] while
diverse applications [73]. Wheat straw-derived porous carbon was maintaining a low-pressure environment. The temperature required for
analyzed with FTIR. The presence of surface OH and COOH groups was hydrogen desorption depended on the specific material and the strength
found which is significantly enhanced the adsorption capacity of biochar of hydrogen binding to the carbon surface. Similarly, Sultana et al. also
when it was utilized as an adsorbent for the removal of heavy metals observed that the H2 uptake capacity decreases with increasing tem
[149]. On the other hand, using the first principle method, the effect of perature [111]. The removal of hydrogen atoms from the carbon
the surface functional group on hydrogen storage capacity was investi structure alters the surface chemistry and porosity of the material,
gated on Ti2X (X = C or N) monolayer. The findings indicate that the leading to changes in its properties.bon
monolayer Ti2X(OH)2 exhibited a reversible hydrogen storage capacity Zang et al. analyzed the composite made using grapefruit peel-
of approximately 2.7 wt%, surpassing that of the Ti2XO2 and Ti2XF2 derived biochar and MgH2 for hydrogen desorption analysis by gradu
monolayers. The OH group at the F site exhibits stronger binding energy ally applying heat The author reported that at temperature 250 ◦ C the
compared to the H atom. Consequently, H2 molecules will not undergo composite started releasing the hydrogen molecule which was 110 ◦ C
dissociation on the Ti2X(OH)2 monolayer. As a result, there is no loss of lower than the pure MgH2. Within 10 min at 350 ◦ C, the composite
1.8 wt% hydrogen storage capacity in the Ti2X(OH)2 monolayer [150]. material was completely dehydrogenated whereas the MgH2 material
The FTIR absorption peaks can be observed in lignin raw materials. was barely initiated to release hydrogen [20]. Similarly, according to
The O–H stretching vibrations of the hydroxyl group belongs to a strong Zhou et. al., hydrogen release and uptake could occur under highly
peak near 3428 cm− 1 [83,151–154]. The peak observed at approxi demanding conditions (at least 400 ◦ C for release and above 400 ◦ C and
mately 2938 cm− 1 was corresponding’s to the C–H stretching vibrations 10 MPa H2 for uptake) and also, they used lithium-based activated
of the methyl group, while the peak at around 2839 cm− 1 was related to carbon confine material for the study. They found that the material
the C–H stretching vibrations of the methylene group [83,151,155]. The started releasing hydrogen at 190 ◦ C and completed at 400 ◦ C showing
absorption peaks noticed at 1716 cm− 1 was attributed to the C– –O 13.6% dehydrogenation capacity [164]. Wang et al. tested the nano
stretching vibrations of the quinoid structure [153,154,156]. Addition confined lithium-based carbon material for dehydrogenation. They
ally, the peaks in the range of 1608 to 1419 cm− 1 arose from the C– –C found that at 175 ◦ C the material starts releasing hydrogen atom which
vibrations of the aromatic ring. The absorption peaks observed from was completely desorbed at 350 ◦ C within 30 min with 7.8% capacity
1327 to 1030 cm− 1 correspond to the vibrations of C–O stretching and [165].
O–H bending [157,157]. The peaks in the range of 910–532 cm− 1 could The further hydrogen received from dehydrogenation can be utilized
be attributed to the out-of-plane bending vibrations of C–C, C–H, and in various sectors. The utilization of stored hydrogen presents various
O–H [151,155]. Similarly, the porous carbon prepared from lignin based opportunities for cleaner and more sustainable energy applications
material displayed weaker and fewer adsorption peaks [136]. These across industries for ammonia [166] and methanol synthesis [167],
findings suggested that the degradation of organic structures in hard transportation sector for fuel cell/hydrogen cell [162,167,168] and
wood alkali lignin lead to increase in the specific surface area of porous hydrogen station [162], and power generation [169], hydro-processing
carbon and the enrichment of active sites, thereby enhancing its of crude oil and petroleum refineries [162,166].
preferred adsorption performance [158].
The behaviour of organic molecules can be determined by gaining 8. Hierarchical carbon uses for other emerging technology
knowledge about which type of functional groups and heteroatoms are
present. The presence of certain function groups such as hydrogen- 8.1. Uses for supercapacitor applications
containing bonds (O–H, C–H, COOH) improves the hydrogen
adsorption-desorption characteristic by creating the active site on the Hierarchical porous carbon is not only prominent material for
material surface. The present active site form weak interaction with hydrogen storage but it has wider applications in different fields. The
hydrogen molecule leading to improved storage capacity and revers use of carbon for supercapacitor material is one of the novel technolo
ibility. The hydrogen-containing surface function groups bind with gies that has been studied by various researchers. The mixture of alka
hydrogen molecule through hydrogen bonding and van der Waals forces line lignin water and KOH was used to produce hierarchical carbon
which significantly affect the hydrogen storage capability [159]. Simi keeping the temperature 700 ◦ C for 1 h under nitrogen flow. As prepared
larly, heteroatoms (Atom that do not contain carbon and hydrogen such carbon has a high specific surface area of 2109 m2/g, interconnected
as boron(B), Nitrogen(N), and Oxygen(O)) commonly found in organic pores, and a high capacitance of 254 F/g at 0.5 A/g [170]. Similarly, a
and inorganic material alter the electronic and chemical properties of double-step process is adopted for producing porous carbon from sword
the material. It also creates active sites for hydrogen adsorption due to bean shells following KOH activation. At cryogenic temperature, the
electronegativity difference and bonding characteristics in comparison hydrogen uptake capacity reaches up to 2.63 and 5.74 wt% at 1 bar and
to carbon and hydrogen atoms. To achieve efficient hydrogenation and 40 bars. In a three-electrode system, high specific capacities of 183 F/g
effective hydrogen storage, heteroatoms can be confined both geomet at 2 mV/s and 211 F/g at 0.5 A/g were obtained from cyclic voltam
rically and chemically into the carbon framework [160,161]. metry (CV) and galvanostatic charge-discharge (GCD) analyses [55].
Melamine foam has an excellent interconnected network and was used
7. Utilization of hydrogen stored as a supercapacitor material. The prepared carbon with KOH chemical
had a high specific capacitance of 217 F/g at 0.1 A/g and superior
Hydrogen presents a promising solution for efficient energy con cycling stability (specific capacitance retention of 89% after 10000 cy
version, storage, and utilization, ensuring a sustainable and reliable cles at 5 A/g) [171].
13
Fig. 7. Simple dehydrogenation model from porous carbon.
A novel technique for Moringa oleifera leaves was utilized to create PC) was prepared using salt templated followed by the molten sulfur
three-dimensional highly crumpled porous carbons (HCPCs) using a method and S-PC integrates the large hollow pores, substantial micro
post-activation-free method. At various scan rates, the HCPCs exhibited pores, and expanded interlayer spacing. The anode made of prepared S-
specific capacitances ranging from 183 to 217 F/g. Moreover, they PC demonstrated enhanced rate capability compared to pristine porous
demonstrated excellent retention, with over 90% maintained when the carbon (PC), with higher specific capacities of 351.5 mAh/g at 0.1 A/g
current density was increased from 1.0 to 50 A/g. Furthermore, these and 122.3 mAh/g at 20 A/g, respectively [175]. A new concept origi
HCPCs demonstrated exceptional cycling stability, and maintain their nated to overcome the challenges of poor cyclic stability and slow
performance over an impressive 20,000 charge/discharge cycle [172]. electroporation rate using MXene as cathode material and Nanoporous
Hybrid hollow polymeric microspheres carbon was prepared by one-step graphene as anode material. The selective anion kinetics were facilitated
process using polyphosphazene. Electrodes utilizing HCMSs demon by the nanoporous graphene anode, whereas the functionalized MXene
strated a specific capacitance of 314.6 F/g at a current density of 0.2 A/g cathode achieved cation selectivity through the variation in ion
in a 6 M KOH electrolyte. Additionally, a specific capacitance of 180.0 adsorption energy. A CDI cell is fabricated for a performance check and
F/g was achieved at a current density of 30 A/g, while maintaining a the constructed asymmetric CDI cell demonstrates an exceptional
high stability with 98.2% capacity retention after 2000 cycles [92]. A electro-sorption capacity of 49 mg/g and a high electro-sorption rate of
cage-like carbon nanomaterial has been prepared by hard templating 2.92 mg/g-min in a 5000 mg/L NaCl solution. Moreover, it exhibited
using potassium chloride. The result of performance characteristics excellent cycling stability with 100 cycles, making it one of the
showed the specific capacitance reached 251 F/g at 0.1 A/g and 201 F/g top-performing studies in the current state-of-the-art Capacitive Deion
at 10 A/g [131]. Likewise, excellent electrochemical performances, ization (CDI) research [176].
including a high capacitance of 254 F/g at 0.5 A/g and excellent rate
capability with 59% capacitance retention at 20 A/g was observed while 8.2. Others
testing the lignin-derived activated porous carbon [170].
Self-phosphorous doped porous carbon material without using the Use of porous activated carbon as a pollutant removal is now day
chemical agent for activation was developed using Honeyvine milkweed extensively popular. Hierarchical 3-dimensional porous carbon derived
material. The prepared porous carbon had a specific surface area of 756 from biomass is one of the best-suited materials for pollutant removal. In
m2/g and at a current density of 1 A/g, it demonstrated a remarkable industrial, agricultural, and municipal wastewater, the prevalent pol
specific capacitance of 253 F/g. Moreover, it displayed an impressive lutants are inorganic heavy metal ions (IHMIs) and organic macromo
capacitive retention of approximately 95% when subjected to a current lecular pollutants (OMPs). The bamboo biomass was calcinated
density of 5 A/g throughout 10,000 cycles [144]. Likewise, eggplant hydrothermally and zeolites was used as a template for activation. The
purchased from a local market was used to produce porous carbon at a as-prepared zeolite-activated porous carbon possessed a specific surface
low temperature of 400 ◦ C followed by chemical activation up to 900 ◦ C area of 879.1 m2/g, encompassing a significant quantity of micro-pores,
after pre-treatment, i.e., washing, and freeze-drying at − 40 ◦ C. The meso-pores, and macro-pores concurrently. It exhibits remarkable
resultant eggplant-derived hierarchical porous carbon had a high spe adsorption capacities for copper ions (Cu2+, 104.9 mg/g) and
cific surface area of 1947 m2/g with a good specific capacitance of 469 Rhodamine-B (Rh–B, 83.34 mg/g) [177]. Table 6 shows the different
F/g at 1 A/g, long life of 99.95% after 20,000 cycles, and excellent adsorption indicator value for bio-derived porous carbon [178,179].
capacitance retention of 90% at a high scan rate of 100 mV/s [173]. Methylene blue and Iodine number are two common parameters that
Hierarchical porous carbon is prepared using rice husk and coal. Out of are widely used by researchers for assessing the adsorption capacity and
the different treatment combinations, the rice husk-derived HPC surface area of porous activated carbon. Jujube was used to prepare
exhibited a specific capacitance of 352 F/g at 1 A/g, along with a hierarchical porous carbon and tested for adsorption. The maximum
retention rate of 100% after 10,000 cycles [174]. In addition to the adsorption capacity even reaches 925.93 mg/g and 1281.39 mg/g for
aforementioned findings, numerous studies are currently being con Methylene blue and Methylene orange, respectively [180]. Likewise, in
ducted to enhance the performance of bio-derived supercapacitor other experiment, authors found that maximum adsorption according to
material. the iodine number and methylene blue index as 784.58 mg/g and
Bo et al. suggested carbon material as a promising material for the 161.92 mg/g respectively [181].
anode of potassium ion batteries. A high sulfur-doped porous carbon (S-
14
9. Conclusion and outlook Data availability
This article aims to provide a deeper understanding of the hydrogen Data is already available in article.
storage mechanism utilizing carbon-based materials. The advancement
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Journal of Power Sources 587 (2023) 233648

Contents lists available at ScienceDirect

Journal of Power Sources

Next generation bio-derived 3D-hierarchical porous material for

• Carbon based material production with

Fig. 2. Classification of hydrogen material and methods for hydrogen storage.

Fig. 3. Simplified hydrogen storage model on metals.

pyrolysis temperature is recognized as the primary parameter that

carbonization and activation) [43]. The [82,83] reported two activation

5.1.1. Hard template method

K- Kelvin, AC - Activated Carbon, MOF- Metal organic framework, H2- Hydrogen.

Fig. 4. Proximate analysis of different biomass material.

Fig. 5. Ultimate analysis of various biomass.

Fig. 6. Schematic illustration of the endo-templating (soft templating) method.

Tea waste 402.25 Peanut hull 813.11

Ethylene calcium-containing nanocrystalline Beta zeolite – 2280 1.95 [124]

SSA= Specific surface area, V= Pore Volume, Ref. = Reference.

Jute fibers AC 1224 0.74 1.2 303 4.0 [1]

SSA= Specific surface area, Ref. = Reference, AC= Activated carbon.

Fig. 7. Simple dehydrogenation model from porous carbon.

9. Conclusion and outlook Data availability

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