Journal of Energy Storage 54 (2022) 105290

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Journal of Energy Storage

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Review Article

Recent progress on biomass waste derived activated carbon electrode

materials for supercapacitors applications—A review
Pantrangi Manasa a, Sangaraju Sambasivam b, Fen Ran a, *
a
State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals, School of Materials Science and Engineering, Lanzhou University of Technology,
Lanzhou 730050, PR China
b
National Water and Energy Center, United Arab Emirates University, Al Ain 15551, United Arab Emirates

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

Keywords: The investigation of renewable, cost-effective, and environmentally gracious electrode materials with high
Biomass adsorption, fast ion/electron transport, and tunable surface chemistry is immediately desirable for the devel­
Porous carbon opment of next-generation biocompatible energy-storage devices. In recent years, biomass-derived carbon
Energy storage devices
electrode materials for energy storage have attracted significant attention because of their widespread avail­
Electrode materials
ability, renewable nature, and low cost. More importantly, their inherent uniform and precise biological struc­
Supercapacitor
tures can be utilized as templates for fabricating electrode materials with controlled and well-defined geometries.
The current review mainly spotlights on recent research progress towards biomass derived carbon electrode
materials include plant, fruit, vegitable, animal waste, and microorganism based carbon electrode materials for
supercapacitor applications. And over view of different synthesis methods for conversion and activation of
biomass waste are discussed. Furthermore, summary and future research trends in this filed are projected.

1. Introduction carbonization and activation [3]. During the thermal carbonization

process, the biomasses are heated under high temperature and inert gas
Energy is essential in everyday life. In the future, sufficient and protection, while the heteroatoms in the backbones of the bio­
sustainable production of energy will be a prime issue. Currently, more macromolecules are escaped, leaving the carbon skeletons with a porous
than 80 % of the energy used by society is supplied by fossil fuels, such as structure. Upon subsequent activation, the remaining carbon skeletons
oil, coal, and natural gas, none of which is renewable. Therefore, energy can form interconnected 3D structures with relatively high conductivity,
must be supplied by sustainable sources before fossil fuels are depleted. surface area and porosity, making them excellent candidates for energy
Although currently energy is produced from renewable natural sources, storage applications, especially supercapacitors.Since batteries, fuel
such as solar, wind, hydro, and geothermal heat, their energy sources are cells, and conventional capacitors are generally considered as clean
too limited in time and space to make a significant impact [1]. To resolve energy devices. Supercapacitors (SCs) are clean energy storage devices
the issues related to energy production and environmental pollution, with power delivery/energy storage performance between batteries and
petroleum-based fuels must be replaced with sustainable and renewable capacitors. Depending on the charge storage mechanism, their energy/
energy sources. Unutilized biomass and waste materials produced dur­ power performance can be tuned and made application specific.
ing energy production can be effectively utilized to synthesize carbon Generally, SCs are used with main power source to provide initial ac­
materials for energy storage/conversion devices, such as batteries, celeration for boosting up the hybrid electric vehicles. SCs are also used
supercapacitors, solar cells, and fuel cells. This approach will further in military, space, and industrial applications where high power density
resolve the difficulties related to safe recycling of waste ingredients and is required while maintaining optimum value of energy density.
also the consumption of fossil fuels. Combustion of waste materials or Considering their power delivery rates, SCs are also recognized as pulsed
fossil fuels however creates anxieties related to environment protection. power sources. SCs also provide backup power in electric appliances
Biomass-derived carbons are formed by converting the natural where quick charge delivery is required. In 2006, first electric double
products, including plants, food microorganisms, and animal waste [2] layer supercapacitor-based buses were launched in Shanghai (China).
into porous carbon materials through artificial processes such as thermal The main obstacle was the shortcoming of energy storage (5 %)

* Corresponding author.
E-mail address: [email protected] (F. Ran).

https://doi.org/10.1016/j.est.2022.105290
Received 19 May 2022; Received in revised form 28 June 2022; Accepted 7 July 2022
Available online 13 July 2022
2352-152X/© 2022 Elsevier Ltd. All rights reserved.
P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

compared to batteries. One can say that the energy density per unit on the porosity and surface area. To modify the morphology, various
weight is too small that supercapacitors alone are not capable to drive a strategies such as the addition of surfactants and physical treatment
bus effectively for a few miles. techniques are employed [41–45]. At present, the use of various biomass
Batteries also limit its applications in advanced technologies due to materials as carbon sources for the preparation of self-doped porous
low power delivery and weight issues in light weight motor vehicles. carbon (PC) electrodes have become a hot topic in the field of energy
Electric car based upon batteries consumes a large amount of energy to storage and conversion (Fig. 1). Obviously, the research on biomass
start and achieve required acceleration. These issues can be solved by derived carbon materials provides not only a new way for high value-
fabricating a hybrid device composed of electrodes having super­ added utilization of biomass resources, but also a better understanding
capacitor and batteries-type characteristics [4]. The use of electro­ of the relationship between the structure and electrochemical proper­
chemical energy storage and conversion devices to allow the storage of ties, ultimately aiding the rational design of more efficient biomass-
surplus energy has attracted considerable attention. based carbon materials for practical applications. The researcher to­
Currently electrochemical energy storage (EDLC) and conversion wards potential utilization of biomass in a more efficient way. The most
devices have been actively pursued for electric vehicle applications, but economical and green synthesis approach is the carbonization (enrich­
the devices still require durable and inexpensive sources to keep the ment of carbon content) of biomass/waste, which solves the purpose,
maintenance cost low. On the other hand, it is almost impossible to find recycling of biomass as well as providing valuable carbon materials.
a device that fulfills all the requirements for practical application [5–8]. Carbon materials are efficiently used in sensing, energy storage, and
The development of electrochemical energy storage and conversion conversion devices (photovoltaic, batteries, fuel, cells, conventional
devices of various types is a way to solve these problems and combine capacitors, and supercapacitors).
them in creative methods. Sustainable and clean energies are the most While research in the area of biomass derived activated carbon (ACs)
important current issues, renewable energy sources like solar and wind electrode materials for supercapacitors has been very intense in the last
will not have impact unless an efficient technology is developed to store few decades, only limited number of reviews with limited focal points
the energy that the renewable energy systems produce. Electrochemical are available. But still there are several aspects that require more
capacitors also called as supercapacitors offer clean energy mitigation exhaustive coverage and in-depth discussion, especially of the under­
effects when combined with renewable energy systems. Carbon is the lying mechanisms of biomass precursor selection and conversion tech­
most versatile material used in both energy conversion and storage ap­ niques to make suitable and perfect electrode materials with optimized
plications [9–11]. structural properties for advanced supercapacitor applications. Here we
However, there is indeed a need to develop more sustainable variants focus on novel kind of different biomass derived activated carbon ma­
of classical carbon materials. In this regard, the biomass derived mate­ terials for supercapacitors electrode and provides details of various
rials could be a good alternate to explore new carbon-based materials for biomass synthesis methods and discuss the insights and updates related
sustainable energy conversion and energy storage systems [12–15]. to the future research trends of biomass derived carbon materials for
Biomass is a well-known raw material for the production of carbon next-generation clean energy applications and will be of interest to the
materials used in SCs electrodes. Since these materials are available in broad advanced energy materials research community.
huge quantities and rich in carbon content, such materials can be used to
synthesize enriched carbon materials in an environmentally friendly 2. Biomass resources
way. Electrode materials play a significant role in the performance of
supercapacitors. Carbon-based materials, conducting polymers and Biomass refers to materials or by-products derived from animals and
transition metals are commonly utilized electrode materials [16–20]. In plants that can act as a potential source of energy. Biomass constitutes
the past few decades, research mainly focused on the development of carbohydrates, lignin, starch, proteins and lipids these components vary
electrodes from waste and agro-industrial resources. Activated carbon is depending upon the geographical condition and source. The biomass
predominantly amorphous and porous in nature [21,22]. Commonly resources are abundant, including energy crops, agricultural crops and
incorporated activated carbons are prepared from fossil sources, which their residues, wood and wood wastes, municipal wastes and animal
are expensive, so an alternative solution is necessary [23–25]. wastes, aquatic plants and algae [46]. However, these biomaterials can
The use of agricultural waste-based biomass material as a precursor all be categorized into four major types, i.e., the plant-based, fruit and
material to prepare carbon-based energy storage devices has gained vegetable-based, microorganism-based, and animal-based biomass
attraction due to the material's availability and low cost [26]. Various (Figure 2). By understanding the chemical and elemental compositions
biomass-derived carbons have been utilized as supercapacitor electrodes of different types of biomasses, one can precisely predict the composi­
including activated carbon, porous materials, aerogel or hydrogel, gra­ tion and structure of the corresponding biomass-derived carbons.
phene, carbon nanotube (CNT), and fullerene [27–30]. Typically, biomass can store chemical energy transformed from solar
The limiting factors such as high surface area and favorable pore size energy in the plant tissues by the photosynthesis process. Therefore,
of electrode materials for a specific electrolyte control the efficiency in biomass energy is also considered as an important renewable energy
terms of energy density and power density of SCs. Porous materials source, such as solar, wind, hydroelectricity and geothermal, and more
facilitate charge storage and transport of ions while high surface area is significantly, utilizing this energy will not add CO2 into the environ­
useful to store energy on the surface. Large specific surface area (SSA) ment. To date, energy from biomasses has been widely used to meet the
and availability of carbonaceous materials in different forms and di­ increasing energy needs, for instance, heating and cooking, electricity
mensions make them an attractive option in SCs application. The surface generating and vehicle fueling proximate and ultimate analysis reports
chemistry of carbon can easily be tuned and they have excellent con­ proved that biomass is rich in carbon, hydrogen, oxygen and nitrogen,
ductivity, good stability, high surface area, low cost, favorable pore size and it also shows traces of chlorine and sulfur.
distribution, and efficient compatibility with various materials in Burning biomass is not the only way to release its energy. Biomass
forming composites [31–35]. Biomass-derived carbon electrodes are a can be converted to other usable forms of energy like methane gas or
promising alternative as the biomass-derived carbon consists of high transportation fuels like ethanol and biodiesel. Methane gas is the main
specific surface area inherited with excellent electrical conductivity, ingredient of natural gas. Smelly stuff, like rotting garbage, and agri­
making them a potential candidate in energy storage applications [36]. cultural and human waste, release methane gas - also called “landfill
The presence of boron, nitrogen and other elements in biomass materials gas” or “biogas.” Crops like corn and sugar cane can be fermented to
can be doped as heteroatom, resulting in additional active sites [37–40]. produce the transportation fuel, ethanol. Biodiesel, another trans­
These features make activated carbon an appropriate option for various portation fuel, can be produced from left-over food products like vege­
electrochemical storage. The capacitance of a supercapacitor depends table oils and animal fats. Biofuels derived from biomass include

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

Fig. 1. Schematic of biomass derived supercapacitor.

Fig. 2. Schematic of different types of bio mass resources.

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

firewood, wood shavings, and pellets, some fruit stones such as olives causes obstructions in aromatic carbon formation. The presence of
and avocados, as well as nutshells. Of these, cut and chopped firewood is highly crosslinked, high molecular weight and the presence of thermally
the least processed, and is usually burned directly in domestic appli­ stable biomacromolecules such as chitin, keratin and lignin enhance the
ances such as stoves and boilers. The chips come from the crushing of aromatic carbon formation and yields superior biochar during the
biomass both agricultural and forest, with their size being variable carbonization process. The presence of low contents of non-crosslinked
depending on the manufacturing process from which they are derived, and molecular weight, aliphatic compounds need to be avoided other­
or the transformation process that they have undergone. Finally, pellets wise causes impede in aromatic carbon formations. Hence, the selection
are the most elaborate biofuel, and consist of small cylinders 6 to 12 mm of the biomass precursor is crucial as the source influence the final
in diameter and 10 to 30 mm in length that are obtained by pressing carbon yield and its structural characteristics, which is obligatory for the
biofuels with binders. Pellets are used especially in fuels with a low energy storage and environmental applications.
energy/volume ratio [47,48]. Fruit stones and seeds, as well as fruit
husks, though used to a lesser extent than other standardized fuels such 3. Significance of biomass derived carbon materials
as fuelwood, wood chips and pellets, also represent an increasingly used
solid biofuel. Indeed, it has been shown that mango stone, peanut shell Incredible efforts have been made to tailor the structure, composi­
and sunflower seed husk have a high energy potential, with a Higher tion, porosity, and geometry of porous carbon materials to attain high
Heating Value (HHV) similar to other commercialized biofuels [49–51]. electrochemical performance. The predominant characteristics of
This fact, together with the increasing worldwide production of these biomass derived carbon materials such as highly effective specific sur­
by-products, makes them especially attractive for thermal energy gen­ face area, extraordinary electrical conductivity, lightweight, chemical
eration, as well as to reduce CO2 emissions. Biomass is present in a va­ and thermal stability and cost-effective are indicates it's a perfect suit­
riety of different materials: wood, sawdust, straw, seed waste, manure, able electrode material for supercapacitors. Electrode materials in
paper waste, household waste, wastewater, etc. [52]. As compared to supercapacitors have very high surface area and porous network which
other electrode materials for the energy and environmental applications, provides for easy diffusion of electrolyte ions and charge storage
the biomass-derived carbon consists of several critical advantages: i) through electrostatic attraction. Surface properties always play a
cheap and its abundant availability, ii) environmentally friendly, iii) In- dominant role in the energy storage devices [58].
situ nano-porous structure formation, and iv) versatility in processing. Compared to the other advanced electrode materials for super­
The biochar content of the biomass, the development of microstructure, capacitors, such as CNT and graphene, the biomass-derived carbons may
and heteroatom doping of the porous carbons (PCs) depend on the obtain several critical advantages, including: (a) Cost-effectiveness: the
chemical structure of the biomass and its elemental composition. Hence, precursors of biomass-derived carbons are cheap and abundant, which
it is very important to investigate the characteristics of the precursors at are mostly from plant organs, food and animal wastes, and microor­
elemental and molecular level to get optimized specific capacitance for ganisms. (b) In-situ nanoporous structure formation: the skeleton of the
practical applications [53]. Biomass materials can not only be directly biomacromolecules is preserved as they are converted to carbon under
used by burning or indirectly be used by converting into liquid or gas inert gas protection, forming interconnected conductive. (C) Versatility
fuel, such as bioethanol or biodiesel [54], but also be used to derive in products and processing: various kinds of bioprecursors can be con­
many important chemicals, which is also a challenging topic in chem­ verted into biomass-derived carbons through similar processing steps,
istry and biology for green and sustainable utilization of biomass waste including carbonization, activation, and purification. On the other hand,
[55]. Biochar and ACs are the most common products from biomass different chemicals, i.e., metallic compounds, can be introduced to the
materials. Briefly, biochar usually can be obtained by burning or py­ conversion process which further endows the biomass-derived carbons
rolysis (low oxygen) of biomass materials, which often produced highly with exceptional electrochemical capacitive and catalytic properties. (d)
porous structure with a high specific surface area. Such special porous Environmentally friendly: compared with the synthesis processes of CNT
structure is beneficial to absorbing nutritive cations and anions for the and graphene, the fabrication of biomass-derived carbons does not
growth of soil-beneficial microorganisms, improving the fertility of soil require high-pressure conditions and harsh chemicals, therefore it is
and bringing great agricultural benefits [56]. Even though the major more energy-saving and environmentally friendly. On the other hand,
research attention in biomass-derived carbons has been drawn to the the utilization of biowastes as precursors to fabricate high-performance
search of unique biomass precursors which simultaneously possess high biomass-derived carbons also represents the state-of-the-art green
carbon contents, hierarchical nanoporous structures and heteroatom pathway to obtain functional carbon materials.
compositions that are extremely beneficial for the formation of inter­ Understanding the surface phenomena is the key to tune the energy
connected meso/microporous structure and N/O-containing surface storage device using biowaste based porous nano carbons [59]. Acti­
functional groups during the carbonization/activation processes, by vated carbon is a non-hazardous carbon-bearing product with a porous
which would greatly enhance the corresponding EDLC-supercapacitor structure and a very large internal surface area. The chemical structure
application. Biomass exists in a variety of different materials: wood, of activated carbon can be defined as a crude form of graphite, with a
sawdust, straw, seed waste, manure, paper waste, household waste, random amorphous structure that is highly porous over a range of pore
wastewater, etc. [57]. The characteristics of some materials allow them sizes, from visible cavities and gaps to those of molecular dimensions.
to be used as fuels directly; however, others require a series of pre­ Treatment with activated carbon is based primarily on the phenomenon
treatments, which require different technologies before they can be known as adsorption, in which molecules of a liquid or gas adhere to an
used. Biomass has its flaws, but also its strengths. Among its great external or internal surface of a solid substance. Activated carbon has a
benefits is the forest use of the territory, which would also serve to clean very large internal surface area (up to 1, 500 m2 g− 1) which makes it
the forest and thus prevent forest fires, and the ability to generate jobs. highly suitable for adsorption. Activated carbon can be impregnated
Biomass generates continuous employment such as the extraction of raw with certain chemicals in order thus to enhance its properties for certain
materials from the countryside and the bush. Nowadays, the use of applications. According to the mechanism of EDLCs, high specific sur­
biomass as biofuel represents a field of great interest to the scientific face areas of carbon materials provide large electrode/electrolyte in­
community. terfaces for ion adsorption, effectively optimizing the capacitance
Paul Thomas et. al [23] described criteria's for the precursor selection [60,61]. In addition, the pore size distribution, the configuration of
of biomass-derived carbon. According to their report, the presence of pores and their connectivity influence the ion and electron movement in
nitrogen content boosts in situ-generation of nitrogen-doped carbon carbons, and thus affect their electrochemical properties [62]. Gener­
with superior conductivity and better cycling stability. However, it is ally, a narrow pore size distribution and ordered pore structure are
necessary to choose precursors with low oxygen content otherwise it pursued to improve rate performance and power density, because they

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

are beneficial to rapid ion transport. SSA is dependent on the size of the demonstrate outstanding capacitive performances through the integra­
particles, as well as on the structure and porosity of the material [63]. tion of various advantages. The specific surface area of some biomass
SSAs and pore properties of biomass-derived carbons can be tuned by derived carbon materials as indicated in Table 1.
different synthetic methods. Zhimin Zou et al. reported highly mesoporous carbon flakes derived
Biomass materials generally show very multiple dimensions for from a kapok fiber for high power electrochemical energy storage in
macrostructures. Biomass-derived active carbon can be perfectively organic electrolyte. According to their report, Carbon flakes with a high
maintained or formed unique frameworks, such as spherical, tubular, specific surface area of 3010 m2 g− 1, a pore volume of 2.756 cm3 g− 1 and
honeycomb or graphene-like carbon. More interestingly, biomass ma­ an ultrahigh mesoporous volumetric ratio of 97.6 % were prepared from
terials usually show intriguing structures, such as hierarchical organi­ tubular kapok fibres through a simple low-temperature pre‑carboniza­
zation, periodic pattern or some special nanoachitectures, which endow tion and KOH activation process. The low-temperature pre‑carboniza­
them with certain unique functionalities, such as anti-refection, super- tion in air was effectively dewaxed the biomass and the thus obtained
hydrophobicity, structural coloration and biological self-assembly [64]. thin precursor was adequately wetted and etched by KOH, both of which
Although the applications of biomass materials are different, the might have resulted in the much-improved textural properties. When
fundamental challenge is always the same that is how to improve per­ used as electrode materials of symmetric supercapacitors in organic
formance by optimizing their structures. A fundamental understanding electrolyte, the carbon flakes displayed high energy density at high
of the conversation mechanisms is needed to obtain high-performance power density, e.g., 24 Wh kg− 1 at 24, 029 W kg− 1, which was among
chemical feedstocks which will help us to solve those energy and envi­ the best values reported so far on biomass derived porous carbon elec­
ronmental challenges. trodes. The results reported in this work indicated that both the selection
The electrochemical performance of supercapacitors probably in­ of bioresources and pre‑carbonization treatment were important for
creases with specific surface area, but the function is diversified. Pore preparation of carbonaceous electrode materials with tailored texture
framework (porosity and size distribution) is another important factor properties and enhanced electrochemical energy storage performance.
on energy storage power of active energy materials in supercapacitors. Therefore biomass-derived carbon materials are considered as a group of
Macropores (>50 nm) can act as ion buffering reservoirs, decreasing very promising electrode materials for electrochemical energy storage
convey distances from electrolyte to electrode. Mesopores (2–50 nm) (EES) by virtue of their naturally diverse and intricate micro­
can offer channels for the charge transfer. Micropores (<2 nm) ensure architectures, extensive and low-cost source, environmental friendli­
high specific surface area and contribute electrical double layer capac­ ness, and feasibility to be produced in a large scale [73–77]. However,
itance [65,66]. The schematic representation of micropore, mesopore the practical application of raw biomass-derived carbon materials in EES
and macropore in a carbon particle show in Fig. 3. Large amounts of is limited by their relatively rare storage sites and low diffusion kinetics.
micropores provide abundant cumulative space for electrons; mesopores In recent years, various strategies from structural design to material
shorten the diffusion distance of ions and reduce the diffusion resistance composite manipulation have been explored to overcome these prob­
so that ions can easily penetrate into the inner micropores; and macro­ lems [78–82].
pores act as the storage layer for the buffer ions, which are helpful for
ion transport. In addition, the high electrical conductivity reduces the 4. Optimization of fabrication process of biomass derived
electronic resistance of the device, and the oxygen functional groups carbon
ensure good wettability and increase the surface area for ion contact.
Currently, efforts have paid to fabricate hierarchical porous carbon Synthesis procedure for preparing electrodes for energy storage de­
with different dimension through adjusting experimental parameters vices should be cost-effective, environment-friendly, and easy, so that a
such as activation reagent amount [67], activation temperature [68], sustainable product can be developed. In this regard, the porous carbons
and activation reagent type [69]. Here, micropores can provide large with variable heteroatom doping, a high surface area, and a suitable
surface areas and rich active sites to promote electrochemical perfor­ morphology can have good charge storage characteristics, a high spe­
mance; however, pore sizes must match ion sizes in order for micro pores cific capacitance, eco-friendly nature, a good cycle life, and compati­
to be able to positively affect capacitive performance in which both bility with different electrolytes, i.e., aqueous, organic, and ionic liquids.
larger and smaller pores can lead to significant drops in capacitance due In combination to the above advantages, if the synthetic procedure can
to ion sieving effects [70]. In addition, macro pores can act as ion buffer be made ecofriendly and be cost-effective, then a low-cost high-capacity
reservoirs to boost ion transport, whereas mesopores can provide low- SC device can be obtained. Here, the biomass-derived PC come into
resistance pathways for electrolyte ions to accelerate ion diffusion ki­ view. Biomass-derived carbons are synthesized from various natural
netics, leading to high rate capability and high power density [71,72]. products, with high carbon content, like egg shell membrane, coconut
Because of all of this, carbon materials with multi scale pores can shell, lignin, cellulose, orange peel, egg white, mushrooms, chitin,
human hair, bacterial cellulose, different kinds of plants, agricultural
waste products, etc., and can be broadly categorized into four cate­
gories: plant-based biomass, fruit-based biomass, animal-based biomass,
and microorganism-based biomass [83–91]. Apart from the choice of
above precursors, the process adopted for synthesis of the PC also plays
an important role in determining their morphology. However, it is very
important to stop over oxidation of the carbons as it leads to collapse of
its pores, thus leading to increased interface resistance [92]. In this
section, synthesis of natural biomass-derived carbons will be discussed.
Normally, the manufacture of activated carbons can be divided into two
categories: physical activation with employing CO2 or steam and
chemical activation (where KOH, KHCO3, ZnCl2, H3PO4, and FeCl3 are
usually used as activating agents) [93]. Physical activation is done by
carbonization at low temperature under an inert atmosphere to remove
non‑carbon elements, followed by activation at high temperature with
employing CO2 or steam. In chemical activation, biomass is treated with
Fig. 3. Schematic representation of micropore, mesopore and macropore in a chemical reagents, followed by the carbonization at 400–900 ◦ C.
carbon particle. (Reprinted with permission of Ref. [66]. Compared with physical activation, chemical activation is widely used

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

Table 1
Summary of bio mass derived carbon electrodes for super capacitor applications.
Biomass Activation agent Activation temperature (◦ C) BET surface area Specific capacitance Electrolyte Current density Ref.
and Time (m2 g− 1) (F g− 1) (A g− 1)

Banana CO2 900 (1.5 h) 1414 179 6 M KOH 1 [118]

Jute fiber HTC + KOH 800 (1 h) 1902 346 6 M KOH 1 [127]
Juncus effuses. L K2CO3 800 (2 h) 2338 357 6 M KOH 1 [128]
Rhus typhina fruits KOH 700 (2 h) 2675 568 1 M H2SO4 1 [129]
Tea waste KOH 700 (1.5 h) 1610 332 6 M KOH 1 [130]
Cauliflower KOH 700(1 h) 2604 311 6 M KOH 1 [131]
1
Glucose KOH 700 (2 h) 2021 206 1 M H2SO4 10 mV s− [132]
American poplar fruit KOH 600 (2 h) 942 423 6 M KOH 1 [133]
Algae KOH 700 (1 h) 1338 353 2 M KOH 1 [134]
Aloe leaf KOH 700 (1 h) 1890 410 1 M H2SO4 0.5 [135]
1
Biogas slurry KOH 800 (1 h) 514 289 6 M KOH 10 mV s− [136]
Biomass straw KOH 900 (2 h) 177 250 3 M KOH 1 [137]
Cotton KOH-KNO3 800 (2 h) 1508 278 6 M KOH 1 [138]
Wheat straw KOH 800 (2 h) 2115 294 3 M KOH 1 [139]
eulaliopsis binata KOH 850 (2 h) 2273 373 6 M KOH 0.5 [140]
Leaves of Euonymus KOH 800 (2 h) 1268 303 6 M KOH 0.2 [141]
japonicas
Fish gill KOH 800 (1 h) 2082 334 6 M KOH 2 [142]
Cotton stalk KOH 800 (2 h) 1964 254 1 M H2SO4 0.2 [143]
Hemp stem KOH 800 (1 h) 2801 167 1 M LiPF6 1 [144]
Endothelium corneum KOH 900 (2 h) 2149 198 6 M KOH 1 [145]
gigeriae galli
Soybean lecithin KOH 800 (1 h) 1803 285 1 M KOH 0.5 [146]
Kapok fibres KOH 850 (4 h) 3010 144 1 M TEABF4/ 0.2 [147]
PC
Human hair KOH 800 (2 h) 1306 340 6 M KOH 1 [148]
Corn silk KOH 900 (2 h) 1246 160 6 M KOH 1 [149]
Orange peel KOH – 2521 407 3 M KOH 0.5 [150]
Paulownia flower KOH 800 (1 h) 1471 297 1 M H2SO4 1 [151]
Pinecone KOH 800 (1 h) 1515 137 1 M Na2SO4 1 [152]
Shaddock endotheliums KOH 750 (1 h) 1265 550 1 M H2SO4 0.2 [153]
Jujube fruit NaOH 650 (2 h) 1135 460 6 M KOH 1 [61]
Mangosteen peel NaOH 700 (2 h) 2623 375 6 M KOH 1 [162]
Lignocellulosic Bio mass ZnCl2 800 (2 h) 1197 233 2 M KOH 1.6 [170]
Silk ZnCl2 900 (1 h) 2494 242 EMIMBF4 0.1 [171]
Elaeocarpus tectorius shell H3PO4 900 (3 h) 860 385 1 M H2SO4 2 [178]
Tamarindus indica Fruit H3PO4 900 (2 h) 847 285 1 M KOH 1 [179]
Shell
Jackfruit peel waste H3PO4 900 (4 h) 1585 324 1 M Na2SO4 1 [180]
Cow dung H3PO4 900 (4 h) 2450 347 1 M Na2SO4 1 [180]
Amaranthus Direct 700 (3 h) 1172 326 6 M KOH 0.5 [162]
carbonization
Perilla frutescens direct pyrolysis 700 (2 h) 655 270 6 M KOH 0.5 [163]
Toboco rods HTC + KOH 800 (1 h) 2115 287 6 M KOH 0.5 [170]
Microalgae HTC + KOH 700 (2 h) 2876 280 1 M H2SO4 1 [171]
Fungi HTC NA 80 196 800 (2 h) 1 [172]
Taro stem KOH 800 (2 h) 1012 236 6 M KOH 0.1 [228]
Jute sticks direct pyrolysis 850 (5 h) 2000 150 KOH/ 1 [224]
Glycerolgel
Dragon fruit peel KOH 800 (2 h) 2667 427 6 M KOH 0.5 [231]
Betel nut HNO3 800 (2 h) NA 423 6 M KOH 0.5 [250]
Hibiscus sabdariffa fruits KOH 800 (2 h) 1720 195 2 M KOH 0.5 [251]
Garlic skin KOH 850 (2 h) 2818 427 6 M KOH 0.5 [265]

owing to its higher yields, lower reaction temperature; lager BET surface (element) by pyrolysis in an inert environment [95]. Pyrolysis and hy­
area and is cost-effective mostly. However, the synthesis of these car­ drothermal carbonization (HTC) are two predominant methods to
bons requires a mass of chemical reagents and the chemical reagents can convert biomass into carbon. Pyrolysis is carried out in an inert or
be remained to form residues easily after washing process. Synthesis limited oxygen atmosphere at elevated temperatures, while HTC refers
routes to biochars and activated carbons from biomass has depicted in to a thermo-chemical process used to convert biomass to carbonaceous
Fig. 4. materials [96].

4.1.1. Pyrolysis
4.1. Carbonization
In general, biochar can be produced on various pyrolysis platforms,
such as slow pyrolysis, fast pyrolysis, pyrolytic gasification, and so on.
High temperature treatment of carbonaceous substrate in the
Typical operating conditions and biochar yields of these pyrolysis plat­
absence of air and in the presence of inert medium (N2, argon) that
forms can be found in the literature [97–100]. The slow pyrolysis of
removes the volatile organics either in the form of gases such as CO2, CO,
biomass (also termed “biomass carbonization”) is an ancient technology
H2O, or condensed liquids is known as carbonization [94]. The resulting
for biochar production. It is normally performed over a temperature
product is char which contain pure carbon structure with small amount
range of 300–800 ◦ C with a heating rate of 5–7 ◦ C min− 1 and a residence
of nitrogen and hydrogen. In simpler words, carbonization of organic
time of >1 h [98]. The biochar derived through pyrolysis of biomass is
material results in a solid residue with increasing content of carbon

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

Fig. 4. Synthesis routes to biochars and activated carbons from biomass (Reprinted with permission of Ref. [86]).

porous, and subsequent activation increases pore volume and specific low specific surface area and poor porosity in nature. To modify its
surface area [101]. Carbon electrodes obtained as a result of direct py­ chemical and physical properties, subsequent activation or carboniza­
rolysis without activation demonstrates high performance [102]. Ao tion is mandatory [109]. Yusuf Osman Donar et al. [110] prepared and
Wang et al. [103] carried out an experimental study on preparation of characterized of agricultural waste biomass based hydrochars. Yong-
electrode material from amaranthus through direct carbonization, Qing Zhao et al. [111] reported porous carbon has been derived from
which is renewable and abundant, without any activation. Carbon py­ tobacco rods via HTC and followed by KOH activation. The prepared
rolyzed at 700 ◦ C (XC-700) shows the best electrochemical energy electrode exhibits high capacitance with 286.6 F g− 1 at 0.5 A g− 1,
storage performance. Bei Liu et al. [104] fabricated O/N-co-doped excellent rate performance with 212.1 F g− 1 even at 30 A g− 1, and
porous carbon nanosheets by the direct pyrolysis of perilla frutescens outstanding cyclic stability with 96 % capacitance retention after 10,
(PF) leaves. Under optimum pyrolysis temperature (700 ◦ C), exhibit a 000 cycles at 5 A g− 1. Furthermore, supercapacitor devices can deliver
hierarchical pore structure with a moderate BET surface area (655 m2 an energy density of 31.3 Wh kg− 1 at 0.5 A g− 1 and power density of
g− 1) and a relatively low pore volume (0.44 cm3 g− 1). In addition, the 11.8 kW kg− 1 at 15 A g− 1. Likewise, M. Sevilla et al. [112] reported
PFC-700-based symmetric supercapacitor offers a high volumetric en­ microalgae derived carbon through HTC and H. Zhu et al. [113] pre­
ergy density (14.8 Wh L− 1 at 490 W L− 1) as well as a high stability pared promising electrode from fungi via hydrothermal synthesis. The
(about 96.1 % of capacitance retention after 10, 000 cycles at 2 A g− 1). hydrochar based porous carbon materials exhibits a high number of
Similarly, Biswal et al. [105] developed a high-specific surface area heteroatoms and demonstrated a high specific surface area and porous
microporous carbon without any activation techniques. Biomass in­ structure [108–113].
cludes impurities such as Mg, Ca, K, and Na, which further act as acti­
vation agents [106].
4.2. Physical activation
4.1.2. Hydrothermal carbonization
Physical activation occurs in assorted oxidizing atmospheres. The
Hydrothermal carbonization (HTC) is an active area of research in
carbonized biomass is placed in air, oxygen (O2), carbon dioxide (CO2),
synthesizing carbon-rich materials because of its ability to transform wet
water vapor, or the mixed atmosphere, and then treated at high tem­
biomass into valuable products [107]. The hydrochars can be directly
perature for a period of time to acquire the final product. In the initial
utilized as electrodes for energy storage applications [108]. The
stage of physical activation, the products formed on the surface of the
hydrochar produced through hydrothermal carbonization possesses a
carbon particles in the previous carbonization process first reacts with

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

oxidizing atmosphere to generate some micropores and mesopores. temperature. The carbon between the crystallites was burned out by a
Meanwhile, the oxidizing atmosphere further reacts with carbon to form series of chemical reactions, resulting in the formation of micropores.
carbon oxides, and pores are created inside the carbon material by The activation time and temperature should be well controlled. Gener­
releasing gas. It is worth noting that physical activation is more effective ally, the pore size increases with the increase of activation time and
than chemical activation in avoiding the combination of impurities and processing temperature, while the carbon yield decreases due to the loss
activators [114]. Physical activation is a widely used two-step process to in the reactions. If the activation time is too long and the temperature is
activate carbon precursors, which involves pyrolysis carbonization too high, the micropores will be destroyed. In the activation process, the
process of raw materials (below 1, 000 K) followed by a controlled main reaction is [128].
gasification process at relatively higher temperatures (>1, 150 K) in the
4KOH + C→K2 CO3 + K2 O + 2H2 (1)
presence of oxidizing gases such as carbon dioxide, steam, air or their
mixtures [115]. In the first stage of carbonization process, raw materials Carbon was etched by KOH, and the reaction released hydrogen.
are carbonized into chars with rudimentary pore structure in an inert Consequently, micropores or voids formed. At temperatures lower than
atmosphere at a moderate temperature. Physical activation approaches 500 ◦ C, dehydration of KOH happened following the reaction shown by
include CO2 activation, which can slowly modify the carbon surface to Eq. (2).
create micropores. According to literature survey, the CO2 activation
2KOH→K2 O + 2H2 O (2)
time is prolonged the size and number of micropores increased. Some
micropores gradually expanded to become mesopores and macropores The generated water vapor sustained the reforming reactions of Eqs.
[116]. The CO2 activation step can be performed during the carbon­ (3) and (4).
ization, which simplifies the process and greatly reduces the cost of the
H2 O + C→CO + 2H2 (3)
activation process. More importantly, it is facile to control the specific
surface area and pore structure of carbon materials by adjusting the
CO + H2 O→CO2 + 2H2 (4)
activation time. Recently, Jenny Pena et.al [117] reported pyrolysis
chars and physically activated carbons prepared from buckwheat husks The carbon dioxide and potassium oxide further reacted with to
for catalytic purification of syngas. From their analysis, physical acti­ produce potassium carbonate according to Eq. (5):
vation, which is more environmentally friendly, is conducted at elevated
K2 O + CO2 →K2 CO3 (5)
temperatures in the presence of an oxidizing agent (steam or CO2) for a
controlled time, which can be seen as partial gasification. Thus, the Therefore, the activation of carbon by KOH generated hydrogen and
mechanisms of forming AC through physical activation exhibit many potassium carbonate as the main products. Carbon monoxide and car­
analogies with pyro-gasification. Lei E. et al. [118] worked on a porous bon dioxide formed as the by-products. Dehydration of KOH and reac­
self-templated N-doped carbon aerogel derived from banana flesh ob­ tion of carbon precursor with water occur around 400 ◦ C, while there is
tained through one-step carbonization followed by CO2 activation. As formation of K2CO3 and reaction of CO around 450–650 ◦ C identified by
per their analysis, a porous N-doped banana carbon aerogel was fabri­ the evolution of CO and CO2. Finally, the generation of pores occurs at
cated by a simple carbonization and CO2 activation procedure. The pore around 700 ◦ C by reaction with K2CO3 and CO2 and also because of the
characteristics depended strongly on the CO2 activation times. The reduction of K2O to K by carbon. After heat treatment, the residual KOH
specific surface area and pore distribution of the carbon aerogels could and the salts formed during the activation process are removed through
be controlled by changing the CO2 activation time. A specific surface repeated washing with dilute HCl (0.1 M) until pH = 7 is obtained. The
area and total pore volume of 1, 414.97 m2 g− 1 and 0.746 cm3 g− 1 were various forms of activation (physical and chemical) lead to the devel­
achieved. The physical activation method has a simple production opment of dangling bonds on the surface of the carbon, which ultimately
process, low cost, and no pollution, and it has broad development lead to the creation of oxygen functionality through the creation of free
prospects and commercial value [119]. Accelerating the reaction speed, radicals.
shortening the reaction cycle, and reducing the reaction energy con­
sumption are the key factors affecting the further development of the 4.3.1. Alkali activation
physical method activation process [120]. KOH is a most often used chemical for activating biomass-derived
carbons. A rough carbon surface could be induced by the activation of
4.3. Chemical activation KOH, which brings about a high SSA and a porous structure that are
advantageous in charge storage. The detailed mechanism of KOH acti­
Chemical activation is known as a single step method of preparation vation has not been fully understood because of the complex variables
activated carbon in the presence of chemical agent such as zinc chloride, including the experimental parameters as well as the reactivity of
potassium hydroxide, sodium hydroxide and phosphoric acid, potassium different carbon precursors [83–90]. In a general view, the development
chloride, Nitric acid. In comparison to physical activation method, of a large SSA and high porosity in KOH-activated carbons is the result of
chemical activation has the following advantages: i) the pores are well the synergistic, comprehensive actions, including chemical activation
developed and pore size is controllable, ii) materials with high surface and carbon lattice expansion by metallic K intercalation. For a given
area are produced, iii) yield carbon is high, iv) it involves only one step, carbon precursor, experimental variables of KOH activation include the
and v) it has lower pyrolysis temperature. For energy storage applica­ mass ratio of KOH/biomass, heating rate, activation temperature and
tions such as supercapacitors, the first two advantages strengthen the time. The normally adopted variables are the following: i) the KOH/
use of chemical activation. In this activation, the biomass is often pre­ biomass mass ratio ranges from 2 to 5; ii) a heating rate of 3–10 ◦ C
treated with different chemicals such as strong acids (H2SO4, HNO3), min− 1; and iii) the activation temperature and time are 550–900 ◦ C and
weak acids (H3PO4, H3BO3), salts (ZnCl2), and strong bases (NaOH, 1–4 h, respectively. Xianjun Wei et al. [129] designed and fabricated
KOH) [121–127]. The mixture is then heated in inert atmosphere at hierarchically interconnected porous carbons through the pyrolysis of
temperatures between 400 ◦ C and 900 ◦ C. Among all the above chem­ Rhus typhina fruits and followed by KOH activation. They were followed
icals, the most commonly used activating agent for SC electrode material by an efficient and economic approach to create micropores or meso­
preparation is KOH as it yields carbons with high specific surface area pores on the nano-sheet wall of macropores. Firstly, the Rhus typhina
(SSA) along with development of higher pore volume. KOH activation fruits powder the RTF powder was subjected to pyrolysis in a tube
occurs in different stages at different temperatures. The reaction furnace at 600 ◦ C for 2 h at a 5 ◦ C min− 1 heating rate under a continuous
mechanisms were proposed as described below. After the contact with flow of high purity nitrogen, cooled down to room temperature, and an
the KOH, the grains of the raw materials were activated at a high initial carbon was obtained. Then the pyrolysed sample activated with

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

KOH at different ratios at maximum temperature of 800 ◦ C. The related and clean treatments of pre‑carbonization, acid washing and KOH
N-doped carbon consists of a plenty of micropores and owns high spe­ activation procedures. The contained inert inorganic impurities were
cific surface area of 2, 675 m2 g− 1, resulting in high performances for completely removed by acid and KOH treatments, resulting in much
supercapacitors, such as ultrahigh specific capacitance of 568 F g− 1 at 1 increased carbon porosity. The prepared biomass porous carbon has a
A g− 1. This novel and sustainable biomass-derived carbon material holds high pore volume with a large surface area of 1, 610 m2 g− 1. The porous
a bright future for fabricating high energy supercapacitors. This is a two- carbon exhibited the high specific capacitances of 332 F g− 1 at 1 A g− 1,
step activation process. and 222 F g− 1 at 100 A g− 1 when current density increased 100 times,
Abrar Khan et al. [130] successfully prepared the highly porous representing an outstanding rate performance. Besides, the porous car­
carbon with tube-like structures from tea-waste raw material using facile bon has achieved an excellent long-cycling life with only 2.2 % loss of its

Fig. 5. Synthesis flow and SEM, TEM images of cauliflower derived carbon (Reprinted with permission from Ref. [131]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

initial capacitance over 100, 000 cycles even at 100 A g− 1. The observed cycles at 30 A g− 1, indicating its practical application prospect.
desirable electrochemical behavior of the new biomass porous carbon Highly ordered hierarchical porous carbon derived from biomass
derived from tea waste would be a competitive candidate as cathode waste mangosteen peel as superior cathode material for high perfor­
material in the development of high-performance and green super­ mance supercapacitor by NaOH chemical activation work done by
capacitors for advanced energy storage devices. Bao Men et. al [131] Viengkham Yang and his group [162]. According to their analysis, a
reported high-performance nitrogen-doped hierarchical porous carbon facile combined method of carbonization and NaOH treatment processes
derived from cauliflower for advanced supercapacitors. Combined with has been used to obtain porous carbon from waste mangosteen peel. he
the high content of active heteroatoms, the sample exhibits high specific obtained porous carbon has a large surface area of 2, 623 m2 g− 1 and
capacitance of 311 F g− 1. Furthermore, the energy density of the displays a stone-like morphology with highly ordered hierarchical meso-
assembled symmetric supercapacitor as high as 20.5 Wh kg− 1 at a power pores structure as shown in Fig. 6. Also, the porous carbon offers a su­
density of 448.8 W kg− 1. Meanwhile shows excellent rate capability and perior specific capacitance (357 F g− 1 at 1 A g− 1) and an outstanding
long-term cyclic stability. rate performance (190 F g− 1 at 100 A g− 1) which is much higher than the
The resultant characteristics as shown in Fig. 5. Recently, the KOH earlier published biomass porous carbon materials.
activation has earned the attention of scientific community as it has
recognized and demonstrated as promising technique to develop carbon 4.3.2. Metal chloride activation
materials with an excellent surface area of >3000 m2 g− 1 from a variety In zinc chloride (ZnCl2) activation, the liquid chemical is intercalated
of bio mass sources [132–153]. The tremendous porosity nature makes it into the carbon matrix to produce pores at temperature above the
more suitable towards broad energy and environmental applications melting point of chemical agent. The reaction between the carbon atoms
[154–160]. Similar to KOH, NaOH is also used in chemical activation to and dehydrating agent is promoted in the extended inter layers of car­
optimize the structure properties [134,149–152]. Viengkham Yang et al. bon. The application of ZnCl2 in chemical activation generally improves
[161] reported a new highly porous natural carbon material from the carbon content through the formation of aromatic graphitic struc­
renewable and inexpensive jujube fruits as a carbon source applied in ture [163–167]. Angela A. Spagnoli et al. [168] discussed cashew nut
supercapacitors through two step chemical activation. i.e., precarbo­ shell based carbons activated with ZnCl2 and described its structural and
nation fallowed by NaOH activation at 650 ◦ C for 2 h. The porous carbon surface parameters. The dried shell of cashew nuts impregnation with
of jujube fruit exhibited high surface area of 1135 m2 g− 1. The acquired ZnCl2 solution at various ratios. The samples were heated at 400 ◦ C
results demonstrate that porous carbon displays the specific capacitance under N2 flow. The samples activated at the ratio of 1.5: 1.0 has been
of 587 F g− 1 at 100 A g− 1. Moreover, the assembled symmetrical coin- exhibited higher surface area of 1, 100 m2 g− 1. Mohammed Nabil
like supercapacitors with wide potential window of 2.5 V in 1 M Mahamad and his coworkers [169] prepared activated carbon from the
Et4NBF4/AN organic electrolyte offer a high energy density of 23.7 Wh pineapple waste biomass (leaves, stem, crown) impregnated with ZnCl2.
kg− 1 at 0.629 kW kg− 1 with remaining 94 % capacitance over 10, 000 Resulting activated carbon with the highest surface area was chosen for

Fig. 6. Schematic illustration of the MP-PC derived from the biomass mangosteen peel through combined method of pre‑carbonization and activation processes
(Reprinted with permission of Ref. [162]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

subsequent studies and was characterized for its surface area, surface 4.3.3. Phosphoric acid activation
chemistry properties, functional groups, porosity and surface Besides to potassium hydroxide and ZnCl2, phosphoric acid (H3PO4)
morphology. is also one of the activating agents in chemical activation for biomass
The activated carbon exhibits high porous structure attributed to the derived carbon [173–177]. Recently, Bose Nirosha et al. [178] demon­
dehydration effect of ZnCl2 and the oxidation of organic compounds. strated phosphorus-doped porous carbon is prepared from a new
Due to its high surface area (914.67 m2 g− 1) and adsorption capacity at biomass (elaeocarpus tectorius) at three different temperatures using a
288.34 mg g− 1 pineapple waste biomass as cheap and efficient raw facile H3PO4 activation approach carbon obtained at 900 ◦ C possesses a
materials to produce activated carbon for dye removal from wastewa­ high phosphorus content, 2.5 % (by mass), and a large interlayer dis­
ters. Apart from the inherent properties of activated carbon, the per­ tance of the porous carbon with more expanded channels facilitating the
formance of activated carbon in dye adsorption could also be prompted penetration of ions into the interlayers and a rapid adsorption of ions
by external factors such as solution pH, ionic strength, temperature, suitable for ultra-high volumetric capacitance. The optimized carbon
foreign matters, etc. Recently, Lignocellulosic biomass-derived, gra­ (900 ◦ C) delivers high gravimetric capacitance (385 F g− 1 at 0.2 A g− 1)
phene sheet like porous activated carbon for electrochemical super­ and volumetric capacitance (543 F cm3 at 0.2 A g− 1) in 1 M H2SO4. In 1
capacitor and catechin sensing has been done by Vediyappan Veeramani M Na2SO4 electrolyte, it still exhibits a gravimetric capacitance of 203
and his coworkers [170]. Activated carbon has been derived from Fg− 1 at 0.3 Ag− 1 and a volumetric capacitance of 286 F cm3 at 0.3 A g− 1
Bougainvillea spectabilis by using ZnCl2 activation at 800 ◦ C for 2 h. The Additionally, a coin cell asymmetric device fabricated using this carbon
obtained grapheme sheet like porous carbon exhibited high surface area works in a wide potential window from 0 to 1.5 V with 96 % capacitance
of 1, 197 m2 g− 1 along with good specific capacitance of 233 F g− 1 at 1.6 retention in 1 M H2SO4 aqueous electrolyte for 1, 000 cycles and yields a
A g− 1 current density. high energy density of 27 Wh kg− 1, showing the utility for the devel­
The preparation scheme and morphology of the bougainvillea spec­ opment of wearable electronic devices. M. Sivachidambaram [179] and
tabilis by using ZnCl2 activation as shown in Fig. 7. Jianhua Hou et al. his team worked on phosphoric acid activated nanoporous carbon
[171] reported ZnCl2 activated nitrogen doped porous carbon derived derived from tamarindus indica fruit shell at different temperatures.
from silk. The material exhibits hierarchical porous carbon nanosheets. TS9NPAC sample exhibited highly nanoporous structure along with
The as-obtained HPNC-NS show favorable features for electrochemical good specific surface area of 847 m2 g− 1 and high capacitance of 285 F
energy storage such as high specific surface area (SBET: 2, 494 m2 g− 1), g− 1. Also, they stated that H3PO4 chemical activation will help to in­
high volume of hierarchical pores (2.28 cm3 g− 1), nanosheet structures, crease specific surface area as well as additive capacitive nature of the
rich N-doping (4.7 %). The HPNC-NS supercapacitor's electrode in ionic activated carbon. Rajabathar Jothi Ramalingam et al. [180], synthesized
liquid electrolytes exhibit a capacitance of 242 F g− 1 and energy density porous activated carbon from fruit peel and cow dung waste for modi­
of 102 Wh kg− 1 (48 Wh L− 1), with high cycling life stability (9 % loss fied electrode fabrication and application. The activation process is
after 10, 000 cycles). Despite the fact that ZnCl2 activation is a mature carried out by phosphoric acid treatment followed by calcination at
domain of research in activated carbon production, there are still rooms different temperature conditions. As per their analysis, the phosphoric
for improvement in overcoming the zinc chloride toxicity and recycla­ acid activation and clay molded calcination method was effective to
bility upon activation [163,165,168,172]. produce high surface area carbon materials with multi porous

Fig. 7. Synthesis of graphene sheet-like activated carbon (GPAC) and its applications as an electrode material for supercapacitors and catechin sensor and SEM (a and
b) and TEM (c and d) images of the as-synthesized GPAC sample. (Reprinted with permission of Ref. [170].

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

architecture. The improved surface area values are useful for catalysis supercapacitors. Recently, the interest for using biomass derived carbon
application and higher specific capacitance values are obtained for both materials in supercapacitors is increasing, and as a result a variety of
AP-9 and CD-9 samples. Moreover, KOH, NaOH, ZnCl2, and H3PO4 biomass precursors such as fruits, vegetables, animal products, plants,
chemical activation, some researchers also used microwave-induced and microorganisms and disposable wastes have been employed to
activation [181–185] and physicochemical activation [186–194] con­ obtain electrode material for supercapacitor. As a result of the envi­
sisting of a chemical activation step followed by physical activation to ronmental friendliness, inexpensive and abundance in nature, renew­
further control the porosity of the activated carbon. Though there are able resource-based materials have been widely used in fabrication of
great efforts have been focused on converting bio-waste into high- supercapacitor electrodes corresponding with the sustainable develop­
valued carbon material. However, it is still a great challenge to ach­ ment. Carbon materials possess various structures, low density, ideal
ieve high carbon yield and controllable porous size distribution for re­ stability, nontoxic, and high conductivity and are most widely used for
searchers [1,90,173,177,195–197]. KOH, ZnCl2, and H3PO4 are the supercapacitor electrodes, including activated carbons, template car­
three mainly used chemical activation agents. In comparison, H3PO4 bons, carbon nanotubes, graphene, and carbon aero gels [198–207].
activated carbons exhibits relatively low specific surface area, while Recently novel kind of biomass derived carbon materials have been
both ZnCl2 and KOH can easily generate the higher surface area. In order studied with great interest due to its excellent electrochemical storage of
to enhance the SSA, KOH activation is most preferable to generate energy [127–177]. Here we summarize different new kind of biomass
biomass derived activated carbon. While ZnCl2 is dehydrating and derived carbon electrode materials for supercapacitor applications.
deoxygenating agent. Table 1 summarizes the biomass derived carbon
electrodes for supercapacitors. 6. Plant derived carbon electrodes for supercapacitors
According to Table 1, it can be clearly observed that the biomass-
derived carbons that are activated with KOH show higher specific It is a rather simple term for all organic materials that seems from
capacitance, higher SSA. This phenomenon can be attributed to the well- plants, trees, crops and algae. The components of biomass include cel­
developed microporosity within the porous carbon framework created lulose, hemicelluloses, lignin, extractives, lipids, proteins, simple sugars,
from the KOH etching. Compared with KOH, ZnCl2 is not as efficient in starches, water, hydrocarbons, ash, and other compounds. Plant
permeating the carbon lattice formation of amorphous carbon struc­ biomass is a kind of renewable, eco-friendly, abundant, and clean energy
tures, which lower the material conductivity and deteriorate the mate­ [208–217]. The utilization of plant biomass can reduce reliance on fossil
rial performance in supercapacitors. When a biomass precursor is fuels and improve the problem of environmental pollution. Most agri­
activated with increasing concentrations of zinc chloride, phosphoric culture, forestry, and food wastes contain ligno-cellulosic resources. The
acid and potassium hydroxide there is a strong development of porosity, composition of ligno-cellulose can be used to produce biofuels, like
initially centred in the microporosity. Consequently, there is a degree of bioethanol, biogas, organic acids, and chemicals. Plant biomass is
activation, specific for each chemical that develops the maximum vol­ mostly composed of three elements: 42–47 % of carbon (C), 40–44 % of
ume of micropores without an appreciable contribution from meso­ oxygen (O), and 6 % of hydrogen (H), all percentages in dry matter. This
porosity. KOH only produces widening of the microporosity to more elemental composition of biomass is followed by the so-called macro­
heterogeneous micropores, whereas ZnCl2 develops both wide micro­ nutrients, which are essential for biomass production: nitrogen (N),
pores and low mesopores, and H3PO4 also develops large mesopores and phosphorus (P), potassium (K), calcium (Ca), magnesium (Mg), and
even macropores. These results are explained by the differences in the sulfur (S). Moreover, plants also need some additional elements in lower
activation mode of each chemical. On the other hand, the KOH activa­ quantities, micronutrients, and trace elements, such as sodium (Na),
tion can also combine with physical activation (e.g., CO2 activation) and chlorine (Cl), iron (Fe), manganese (Mn), copper (Cu), zinc (Zn), mo­
the co-addition of heteroatom source such as melamine and thiourea, lybdenum (Mo), nickel (Ni), selenium (Se), and silicon (Si), summing all
which can simultaneously generate the biochar with controlled surface together up to 4 % [1–10,102,182,218–227].
functional groups and heteroatom doping that remarkably enhance the The quantitative chemical compositions of plant-based biomass vary
material supercapacitive performance. with geographical parameters, species-classifications and depend on
organs. However, the qualitative chemical compositions of plant-based
5. Biomass derived carbon materials in supercapacitor biomass consist of hemicellulose, cellulose, lignin, and extractives
electrodes [23]. There is much effort focusing on utilizing biomass to fabricate
energy storage devices, but less consideration has been paid on taro
As discussed earlier, electrode material is a key component of stem, which has been investigated to use for ORR and SCs for the first
supercapacitor consequently is the focus of numerous current re­ time. Donglin He et al. [228] reported a simple, inexpensive and readily
searches. Interestingly most of the SCs are based on carbons materials, scalable method to manufacture three-dimensional N-doped porous
because of their properties which include: good chemical stability, good carbon (3DNPC) by pretreatment of activation with KOH and post pro­
electrical conductivity, large specific surface areas and highly porous cessing of doping with melamine. The method has three advantages as
surface, availability, and low-moderate cost [26,27]. There are an follow: i) a sustainable biomass, taro stem, is used as carbon source; ii)
enormous number of carbon materials produced from a variety of facile preparation method with no templates is needed; and iii) the
carbonization and activation procedures and precursors ranging from resultant 3DNPCs possess large specific surface area (SSA), high level of
conventional activated carbons (ACs) to more sophisticated materials pyridinic and graphitic N. Moreover, the 3DNPCs present high specific
like carbon nanotubes and graphene that have been evaluated as elec­ capacitance (236.4 F g− 1 at 0.1 A g− 1) and outstanding cycling stability
trode materials for supercapacitors. Specifically, ACs has been used as (92.3 % retention after 5, 000 cycles at 3 A g− 1) for SCs in 6 M KOH
electrode materials in supercapacitors due to their unique characteris­ solution. The reproducible biomass materials, simple synthetic method,
tics such as high surface area, high conductivity, and versatility and and outstanding property make 3DNPC a potential candidate for ORR
relatively low cost. Nowadays, they are widely utilized as electrode catalyst in FCs and electrode material in SCs. The pyrolyzing the mixture
materials in commercial EDLCs. ACs can be obtained from a variety of of taro stems and KOH contains abundant macropores, micropores and
natural or synthetic carbonaceous precursors. The use of biomasses as mesopores with large surface area of 1, 012 m2 g− 1 with plentiful
raw materials to obtain ACs is an environmentally viable, and porosity. The prepared 3DNPC-800 is basically a carbon structure with
economically feasible alternative that have been attracting much in­ no metal-based oxides or carbides present, as demonstrated by the SAED
terest lately. Because biomass is rich in natural polymers, low in inor­ pattern. HAADF-STEM and elemental mapping images show a uniform
ganic impurities, and has significant amounts of heteroatoms such as O, distribution of nitrogen and oxygen hetero depicted in Fig. 8. The
N, S, P, B, etc., the biomass-derived electrodes show high capacitance in assembled all solid-state symmetric supercapacitor exhibits a high-

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

Fig. 8. Schematic illustration for the synthesis route of 3DNPC and Depicting images of SEM for TSC (a), 3DPC-800 (b), 3DNPC-800 (c); TEM (d) and HRTEM (e)
images (inset: FR-TEM image) and the corresponding selected area electron diffraction (SAED) pattern (f) of 3DNPC-800; (g) HAADF-STEM image and the corre­
sponding elemental mapping images of 3DNPC-800. (Reprinted with permission of Ref. [228]).

power density of 5, 000 W kg− 1 with an energy density of 5.56 Wh kg− 1. to the micro- and mesoporous nature that was confirmed using FE-SEM
Materials which possess high specific capacitance in device configura­ and HR-TEM analysis.
tion with low cost are essential for viable application in supercapacitors. The symmetric supercapacitor device fabricated using this activated
M. Karnan et al. [90] fabricated a flexible high-energy supercapacitor carbon electrodes in ionic liquid could power a red LED for >20 min
device using porous activated high-surface-area carbon derived from upon charging for <20 s. The energy density obtained for ionic liquid
aloe leaf (A. vera) as a precursor. A. vera derived activated carbon electrolyte and four FSSC devices connected in series is about 40 and 22
electrodes have shown for their application in supercapacitors using Wh kg− 1, respectively which is significantly higher than that of bio­
aqueous, nonaqueous, and all-solid-state device configurations exhibi­ derived carbon. The high performance by the A. vera derived activated
ted in Fig. 9. The chemical activation of A. vera derived carbon materials carbon promises its viable application in supercapacitor. The use of
with KOH showed a maximum specific capacitance of 410 F g− 1 at 0.5 A biocarbon derived from A. vera plants with high performance in super­
g− 1, 126 F g− 1 at 0.1 A g− 1, and 244 F g− 1 at 0.5 A g− 1 current density in capacitors will significantly reduce the cost of the energy storage device
aqueous, nonaqueous, and all-solid-state configuration, respectively. for practical applications. The other plant-based biomass derived
The high performance of A. vera derived activated carbon was attributed supercapacitors such as chrysopogon zizanioides roots [229] exhibits

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

Fig. 9. Schematic representation for the preparation of activated porous carbon from aloe Plant Leaf and FE-SEM images of AV-700, (a-d) Photographic images of
FSSC device showing flexibility, bendability of the device, and four cells connected in series to light the blue LED. (e) CV profiles of FSSC device fabricated with AV-
700 electrode at different bending angles; (f) Ragone plot for AV-700 fabricated FSSC devices. (Reprinted with permission of Ref. [90]). (For interpretation of the
references to colour in this figure legend, the reader is referred to the web version of this article.)

device specific capacitance of 253 Fg− 1 and high energy density of 16.6 characteristics [235]. Hemicellulose and cellulose are less stable to
Wh Kg− 1 along with power density of 2, 000 W kg− 1 at 0.5 A g− 1 thermal decomposition as compared to lignin, and contribute low car­
measured current density with capacity retention of 98 % at 5, 000 bon yield. However, the hemicellulose, lignin and cellulose components
cycles. Bamboo char [230] derived supercapacitor exhibits 222 F g− 1 contribute porosity of biochar yield [236]. It was noted that there were
capacitance with 84 % capacity retention at 5, 000 cycles with energy no substantial interactions between hemicellulose and cellulose during
density of 6.65 Wh kg− 1 in PVA/KOH gel electrolyte. While the recent thermal pyrolysis at 500 ◦ C; however, observed apparent interactions
report of Jute sticks [231] derived supercapacitor in KOH/Glycerol gel between lignin and cellulose components [237]. Therefore, it is critical
showed 140 F g− 1 specific capacitance and high energy density of 20 to select the plant biomass precursor's rich in nitrogen content and lignin
Wh/Kg with 95 % capacity retention at 10, 000 cycles. Investigations fraction, low in oxygen content and cellulose fraction to obtain the
over the elemental composition of precursors, as the presence of the biochar yield with good conductivity, controllable defects and a high
nitrogen and oxygen content in precursors influencing the microstruc­ degree of graphitization to make it appropriate for environmental and
ture, capacitance and conductivity. energy storage applications.
It has been determined that high oxygen content in precursors result
in less crystalline and more defects also more volatile compounds gets 7. Fruit and vegetable derived carbon electrodes for
released during the pyrolysis and thermal decomposition process supercapacitors
[232–234] whereas the presences of higher levels of nitrogen content
could result in nitrogen-doped carbon with enhanced electrochemical The carbohydrates, lipids, ash, crude proteins and fibres are the

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

major constituents of fruit-based biomass [238–242]. As per literature derived carbon electrode materials for supercapacitors have been stud­
survey [124,131,151,161,179,180], fruit peel and vegetable waste ied and reported. Even though there are numerous studies on fruit and
consist lipid content ranges from 0.7 to 9.96 % and 1.4–28.6 %, and vegetable waste derived carbon materials, but still there is no systematic
crude protein yields from 3.5 to 28.6 % and 5.8–43.4 % respectively. studies for the stable energy density.
Also, the presence of phosphorous and nitrogen content in crude lipids Therefore, scientists paid much attention to find new kind of biomass
and proteins may succor in-situ development of heteroatom-doped precursors for perfect and sustainable energy storage applications. For
carbons [243–247]. The crude fibres consisting of hemicellulose, example, Dayakar Gandla et al. [248] Designed the mesopore-
lignin and cellulose are the significant contributors for the carbon yield. dominated activated carbon electrodes from the dragon fruit peel was
However, the mass fractions of crude fibres are significantly lower and witnessed a significant breakthrough in enhancing the electrolyte
generally rich in cellulose which has an influence over graphitic struc­ breakdown voltage and energy density of supercapacitors. The mecha­
ture and yield in biochar. In recent years fruit and vegetable biomass nism is exhibited in Fig. 10. The electrode with the optimum N-doping

Fig. 10. Schematic illustration of the synthesis of N-doped porous AC from a dragon fruit peel and (a) Effect of optimal pore width on the working voltage of EDLC
made of various carbon electrodes published. (b) Ragone plot showing the specific energy vs specific power of N-dfAC-0.5 in comparison with the reported carbon-
based symmetric supercapacitors. (c, d) Schematic illustration of 2D projected views of small and large ions accessing to micro- and mesopores of commercial YP-50F
AC and hierarchical AC, respectively (Reprinted with permission of Ref. [248]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

content (3.4 at. %) exhibits the highest specific capacitance of 427 F g− 1 based electrolyte exhibited high capacitance, high rate capability and
at 5 mA cm− 2 and cyclic stability of 123 % capacitance retention until robust long-term cyclic stability. No capacitance decay occurred after 8,
50, 000 charge-discharge cycles at 500 mA cm− 2 in aqueous 6 M KOH 000 cycles. The cyclic stability also yielded the maximum energy density
electrolytes. They designed a 4 V symmetric coin cell supercapacitor of 32.08 Wh kg− 1 at a power density of 700.43 W kg− 1. The performance
cell, which exhibits a remarkable specific energy and specific power of of the assembled asymmetric supercapacitor is attributed to nitrogen
112 W h kg− 1 and 3214 W kg− 1, respectively, in organic electrolytes. doping and higher porosity of the NPC and direct growth on the con­
The cell also exhibited a significantly higher cycle life (109 % capaci­ ducting substrate to avoid adhesion resulting in an intercrossed and
tance retention) after 5, 000 GCD cycles at the working voltage of ≥3.5 V interlinked urchin-like porous morphology of the NiCo2O4@NF. As
than commercial YP-50 AC (~60 % capacitance retention). The larger prepared NiCo2O4||NPC asymmetric capacitor is inexpensive, environ­
debye length of the diffuse ion layer permitted by the mesopores can mentally safe, with high energy density and robust cyclic stability.
explained the higher voltage window, and the polar N-doped species in Therefore, this report will lead to the design of cost-effective asymmetric
the dfAC enhanced the capacitance and ion transport. The results endow super capacitors using fruit waste biomass. Ju Fang et al. [250]
a new path to design high-capacity and high-working voltage EDLCs demonstrated excellent electrochemical performances with high
from eco-friendly and sustainable biomass materials by properly tuning capacitance of 423 F g− 1 at 0.5 A g− 1, Remarkable energy density of
their pore structure. 61.7 Wh kg− 1 and power density of 7, 500 W kg− 1 were achieved by
Nazish Parveen et al. [249] constructed an aqueous potassium ion- hetero atoms doped betel nut derived biomass-based coin-type sym­
based asymmetric supercapacitor using nitrogen-doped porous carbon metric supercapacitors. Hibiscus sabdariffa fruits derived high perfor­
(NPC) derived from waste orange peel and sea urchin-like intercrossed mance symmetric supercapacitor has been constructed by H. A.
and interconnected NiCo2O4 array on Ni foam for negative and positive Hamouda et al. [251]. The symmetrical supercapacitor has a high en­
electrodes, respectively. A scalable and smart approach was used to ergy density of 13.1 W h kg− 1 at a power density of 225.00 W kg− 1. After
transform waste orange peel into NPC, which was interconnected with 5, 000 cycles, the initial capacitance still retains 96 %. Vegetable crop
urchin-like NiCo2O4@NF synthesized via hydrothermal method. These widely cultivated around the world. The enormous consumption of
NPC and urchin-like NiCo2O4@NF were utilized as anode and cathode vegetables leads to production of tons of vegetable waste, which are left
materials in half-cell using aqueous electrolyte resulting in remarkable to rot without proper utilization because bio-waste production leads to
capacitance of 268.5 F g− 1 and 1300 F g− 1 indicating electro active environmental issue. For long term use, it is stored. However, due to
features for application as aqueous K+ based asymmetric super­ reasons (such as attack by bacteria of fungi) some vegetables gets rotten
capacitors. The schematic device configuration represented in Fig. 11. and is considered a biomass waste. Every year, this biomass waste occurs
Further, as fabricated asymmetric capacitor using NPC as anode and in large quantities; of the order of thousand tonnes. This waste is buried
urchin-like NiCo2O4@NF as working cathode in an aqueous potassium- in soil, dumped into land, burned or thrown away, which results in

Fig. 11. Steps involved in the synthesis of NPC from waste orange peel and Schematic diagram of morphological evaluation NiCo2O4@NF. Schematic representation
of asymmetric capacitor fabrication using waste orange peel-derived NPC as anode and urchin-like NiCo2O4 as cathode. Ragone plot and specific capacitance
performance comparison of NiCo2O4//NPC asymmetric supercapacitor (Reprinted with permission of Ref. [249]). (For interpretation of the references to colour in
this figure legend, the reader is referred to the web version of this article.)

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

environmental degradation. However, this bio-waste can be used as a Qing Zhang et al. [265] derived 3D hierarchical porous carbon
carbon precursor for preparation of AC and can serve as active electrode electrode from garlic skin. The as-obtained carbon presents a high spe­
material for supercapacitor. The vegetable peel contains carbonaceous cific surface area of 2, 818 m2 g− 1. As the electrode material for a
materials composed of large amount of cellulose as well as vitamin and supercapacitor, due to its unique interconnected porous structure, this
protein which reveals the application in the field of absorption of heavy garlic skin-derived carbon exhibits excellent electrochemical perfor­
metal ions from water and anode for batteries [252–256]. So far re­ mance and cycling stability. At a current density of 0.5 A g− 1, the
searchers develop soybean derived carbon for high performance super­ capacitance is up to 427 F g− 1 (162 F cm− 3). Even at a high current
capacitors [257–263]. Recently, Jianhua Yu et al. [264] develops a low density of 50 A g− 1, the capacitance can be maintained to a high value of
temperature pre‑carbonization, hydrothermal stabilization and KOH 315 F g− 1 (120 F cm− 3). After charging-discharging at a current density
activation method to derive N, O, P, and S co-doped porous carbon of 4.5 A g− 1 for 5, 000 cycles, the capacitance retention is as high as 94
materials from protein-rich soybeans as a negative electrode for asym­ %. The energy density under the power density of 310.67 W kg− 1 is
metric supercapacitor and effectively enhances specific capacitances in 14.65 W h kg− 1. The results suggested that this garlic skin-derived 3D
both acidic and alkaline aqueous electrolytes. Specially, the derived hierarchical porous carbon is a promising electrode material for high-
porous carbon demonstrates an ultra-high specific capacitance of 685.1 performance supercapacitors. And they proposed the special structure
F g− 1 at 0.5 A g− 1 in 2 M KOH and 439.5 F g− 1 at 1 A g in 1 M H2SO4, and composition of these natural materials may also contribute to the
respectively. Moreover, a superior cycling stability is achieved with a formation of the skeleton, because their plant epidermis is made up of
capacitance retention of 80 % after 13, 000 cycles at a current density of rich protein, carbohydrate and cellulose [268,269]. It has been
20 A g in 2 M KOH. An asymmetric supercapacitor consisting of soybean- demonstrated that plants with half-transparent thin flakes such as onion
derived carbon and NiCo-sulfide delivers a high energy density of 41.8 and elm samara, which have similar structure to garlic skin, lead to the
Wh kg− 1 at a power density of 750 W kg− 1. The findings above indicate formation of three-dimensional PCNS frameworks [270,271].
hydrothermal process can effectively stabilize heteroatoms (N and P), This structure has great benefits in improving electrochemical per­
improve graphitization and thereby enhance capacitive properties of formance. The schematic of garlic skin derived carbon structures shown
biomass-derived carbon materials. in Fig. 12. Therefore, agro-waste-derived porous carbon has received
As a kind of cultivated plant, garlic is used both as food and for more attention as electrode material for high-performance super­
medicinal applications, which has rapid growth rate, short maturation capacitor application due to its diversity and reproducibility. Also,
cycle, and high yield. Garlic contains rich mineral elements, involving received more attention due to their intrinsic and extrinsic character­
phosphorus (P), magnesium (Mg), calcium (Ca), iron (Fe), zinc (Zn), istics such as high surface area, low cost, comparatively high electronic
copper (Cu), manganese (Mn), selenium (Se), etc., which are very conductivity, affordable to large-scale applications and easy synthesis
important for forming the biomass porous carbon and making the ma­ method have been provided the scope to look for new natural renewable
terial more widely used. In addition, natural garlic can effectively absorb resources particularly from bio-diversified one exhibiting moderate
and transport ions and water molecules for its metabolism due to its supercapacitor performance.
well-connected microtexture and multichannel structures [265–267].
Thus, garlic can be carbonized to synthesize biomass carbon with special 8. Animal waste derived carbon electrodes for supercapacitors
interconnected, multichannel, and porous structures, which facilitate
ion transport as well as electrolyte penetration and enhance energy Besides plants and their fruits, biomass-derived carbons can also be
storage capability. produced from animal waste. Chitin is a type of nontoxic, abundant,

Fig. 12. Characterization of the garlic skin-derived nanoporous carbon. (a) Photograph of garlic, (b) photograph of as-received garlic skin, (c) SEM image of the
garlic skin; (d-i) SEM images of the garlic skin derived 3D hierarchical porous carbon: (e) is the enlarged image of the marked region (I) in (d), and (f) is the cross-
section of (e). (g) is the enlarged image of the marked region (II) in (d) and the front view of the lamellar structure, (h) is the side view of the lamellar structure, and
(i) is the enlarged image of the marked region in (h), from which a lot of pores can be observed. And typical cyclic voltammetry curves of the GHC-17 electrode at
different scan rates, from 5 to 200 mV s− 1. (b) Galvanostatic charge-discharge curves of GHC-17 electrode at different current densities, from 0.5 to 50.0 A g− 1. (c)
Specific capacitance as a function of current density. (d) Comparison of the gravimetric capacitance of some previously reported carbon-based supercapacitor
electrodes. (Reprinted with permission of Ref. [265]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

naturally occurring polysaccharide. Porous carbon from chitin has a carbon source, N/S source, but also as a microporous porogen during
attracted special attention due to its high nitrogen content, allowing carbonization. The features of unique honeycomblike hierarchical pore
direct fabrication of N-enriched carbon without additional nitrogen structure, large specific surface area of 927 m2 g− 1 and high heteroatom
sources. The faradaic reactions between nitrogen and electrolyte doping (N: 5.13 at. %, S: 2.51 at. %) Simultaneously exist, significantly
contribute pseudocapacitance, which could substantially improve the improving the electrochemical performance of as-obtained carbon ma­
performance of the supercapacitor its annual biosynthesis amount is terials shown in Fig. 13.
about multibillion tons, which is almost same with the annual produc­ A high capacitance of 302 F g− 1 and an excellent cycling stability
tion of cellulose. Chitin consists of β-(1, 4)-linked-2- cetamido-2-deoxy- with 99 % capacity retention over 5, 000 cycles have been obtained in
D-glucopyranose units (GlcNAc), and contains about 6.9 wt% nitrogen KOH electrolyte. Notably, the assembled symmetric flexible solid-state
from N-acetamido group [272–277]. This property endows NAG a po­ supercapacitors still maintain excellent capacitance property and sta­
tential application for preparing N-containing carbon materials for bility under the extreme temperatures (− 20 ◦ C ~ 100 ◦ C) and bending
supercapacitor. It will be a novel application of chitin-based biomass if (0◦ ~ 180◦ ). Furthermore, in Na2SO4 electrolyte, the supercapacitors
the performance is desirable. Certainly, to achieve N-doped carbon with display an outstanding energy density of 17.6 Wh kg− 1 at a power
large surface area and porous structure, template is also essential during density of 250 W kg− 1.
the whole carbonizing process [278]. For example, Li Sun et al. [279] The fascinating performance significantly endows 3D honeycomb-
prepared 3D honeycomb-like N/S-codoped hierarchically porous carbon like N/S-codoped hierarchically porous carbon materials with great
from chitosan-protic salt ([Chit][HSO4]) by a combined method of potential for high-efficient energy storage. According to above discus­
double soft-template and solvent-free self-assembly. The key to this sion, a nanostructured carbon with hierarchical porosity and heter­
preparation strategy: no any solvents or catalysts are used; F127 and oatomic modification is desirable electrode material for high
sodium dodecyl sulfate are respectively used as mesoporous and mac­ performance supercapacitors. Template methods are commonly used to
roporous soft templates, as well as [Chit][HSO4] not only can be used as prepare hierarchical porous carbons. However, the relatively high cost

Fig. 13. The synthesis process of N/S-HPCM and (a) Photograph of arthropods, the inset is chitosan. (b) SEM image of N/S-HPCM, the inset is the photograph of a
honeycomb. (c) High resolution SEM images of N/S-HPCM. (d) TEM image of N/S-HPCM and Electrochemical measurement for N/S-HPCM in 1 M Na2SO4: (a) CV
curves at different scan rates. (b) GVD curves at different current densities. (Reprinted with permission of Ref. [279]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

and complicated process including template carbonization, template with high SSA and hierarchically porous structure was obtained, and the
removal and post activation limit their application to some extent interpenetrating hierarchical pore structure could promote the fast
[280–282]. Recently, Si Zheng et al. [283] reported template-free and movements of electrolyte ions.
one-step carbonization-activation method has been used to prepared When HCM served as the substrate of PANI to construct the HCM-
chitin nanoparticles. According to their study, the sample activated at PANI composites for symmetric supercapacitor (SSC), the SSC exhibi­
800 ◦ C (ACNC-800) possessed an ultra-high specific surface area (2631 ted remarkable rate capability and cycling durability of 90.6 % capaci­
m2 g− 1) and nitrogen content (7.1 %), showing good electrochemical tance retention after 10, 000 cycles, confirming the high efficiency of
performance. At a current density of 0.5 A g− 1, the specific capacitance HCM in constructing hybrid electrode materials for supercapacitors. The
was 245 F g− 1 in the three-electrode system and 227 F g− 1 in the two- graphic illustration of the entire process shown in Fig. 14. Si Zheng et al.
electrode system. Moreover, the material maintained excellent cycling [294] reported the preparation of carbon nanospheres directly from
stability over 10, 000 cycles with the retention capability of 98 %. This chitin nanogels for the first time. Chitin nanogels were prepared by a
work provides a template-free and one-step carbonization-activation mechanical agitation induced sol-gel transition method with high effi­
method to utilize chitin from the seafood waste (crab shell) as promising ciency. Interconnected porous framework of N-doped carbon nano­
electrode material for high-performance supercapacitor. However, spheres (nitrogen content of 3.2 %) was obtained by directly pyrolyzing
direct carbonization of bulk chitin does not offer sufficient control over the chitin nanogels. The prepared typical carbon had a high BET surface
porosity and microstructure. Recently, chitin microspheres [284] area (up to 1, 363 m2 g− 1). Besides, the chitin nanospheres could be used
nanofibers [285] and aerogels [286] were selected as precursors for N- in organic electrolyte, demonstrating a specific capacitance of 107 F g− 1
doped carbon, which demonstrated large surface area, hierarchical at 1.0 A g− 1 in TEABF4-AN electrolyte and an excellent cycling stability,
porosity and high electrochemical performance. Importantly, chitin with a capacitance retention of 95 % after 10, 000 cycles at 10 A g− 1.
derived carbon showed favorable retention of morphology due to the Therefore, the presence of higher concentration of nitrogen, chemi­
stiffness of chitin chains [287–292]. Therefore, a preformed chitin pre­ cal stability, and bulk availability in nature, chitin is another favorable
cursor with well define nanostructure provides great opportunities for bio-precursor for the wide range of application. Chitin is capable of
new nanocarbon materials. developing crosslinking networks of chitin- catecholamine and chitin­
Lingfeng Gao et al. [293] fabricated hierarchically porous carbon glucan complexes and are also capable of constituting intermolecular
chitin nanofibrous microspheres via a facile and innovative method, hydrogen bonds [295]. The chitin has higher thermal stability and
which could be employed for the manufacture of different porous ma­ carbon yield compared to cellulose. The extraction of chitin content
terials. By the combining of the compatibility between chitin and chi­ from the biomass is carried out using chemical deproteinization,
tosan and the dissolubility of chitosan in acid solution, the micro- chemical demineralisation and mechanical grinding [296]. The final
mesopores generated in the chitin nanofibers of the microspheres, in yield of extraction depends on biomass precursors, and the processing
which chitosan as a pore-forming agent. After carbonization, the HCM method employed its ranges from 4 to 40 % [297,298]. The nitrogen

Fig. 14. Graphical illustrations of the formation process (a), two-electrode system(b), and porous structure of the nanofibers (c) for the HCM-PANI (Reprinted with
permission of Ref. [293]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

content of extracted chitin from animal-based biomass matches with 988 m2 g− 1 and pore volume of 1.76 cm3 g− 1. With the unique porous
nitrogen concentration levels with microorganism-based biomass, nature, the carbon exhibited a specific capacitance of 306 and 149 Fg− 1
promising its suitability towards energy and environmental in aqueous and organic electrolyte, respectively. Moreover, this carbon
applications. also shows high capacitance retention of 77 % at large current density of
30 A g− 1 and exhibited an outstanding cycling stability with 95.7 %
9. Microorganism derived carbon electrodes for supercapacitors capacitance preservation after 15, 000 cycles in 6 M KOH electrolyte.
Recently, Yang Zhao et al. [302] reported bamboo fungi derived carbon
The microorganisms are classified as bacteria, algae, and fungus, nanofoam for high performance supercapacitors. The schematic illus­
consist of proteins, lipids, carbohydrates, nucleic and amino acids. These tration is shown in Fig. 15.
microorganisms grow in extreme environmental conditions and their The prepared carbon electrode exhibits remarkable supercapacitor
simple cultivation yields large quantities. The heteroatoms doping of performance, showing a high specific capacitance (367 F g- 1 at 0.5 A g-
1
nitrogen functionalities were from high protein content found in these ) and outstanding rate capacity (capacitance retention up to 74.7 %
micro-organisms [299]. The major components present in the even at 20 A g- 1). More promisingly, the assembled symmetric super­
microorganism-based biochar is matching with fruit and plant derived capacitor based the carbon foam delivers a high energy density of 24.6
biomass however, the elements and actual molecules that constitute Wh kg-1 at a power density of 400 W kg- 1 and excellent long-term sta­
these components are substantially different [300]. In microorganism- bility (only 4.3 % capacitance loss after 10, 000 cycles). Bacterial cel­
based precursors mushrooms are the major precursors. As going into lulose (BC), a bio-product produced from fermentation, has attracted
detail, the fruiting part of the mushroom is more often utilized for the much attention due to its wide availability, low cost, renewability, and
fabrication as compared to other parts such as mycelium. Mushrooms porous nature [303–305]. Bacteria are a large group of prokaryotic
are an attractive option due to the presence of rich nitrogen content. For microorganisms. They can replicate rapidly and persist in high numbers
example, Ping Cheng et al. [301] prepared a hierarchically porous car­ in almost any moist environment. Despite their wide application in food
bon with natural shiitake mushroom. The first step involves the acti­ and pharmaceutical industries, little attention has been paid to their role
vation of shiitake mushroom with H3PO4, while the second step is to in material science. Detailed investigations have revealed that the bac­
further activate the product with KOH. terial cells consist of peptidoglycan, a polymer consisting of sugars and
The resulting carbon is comprised of abundant micro-, mesopores amino acids that forms a mesh-like layer outside the bacterial plasma
and interconnected macropores that has a specific surface area up to 2, membrane. Co2P2O7 microplate/bacterial cellulose-derived carbon

Fig. 15. a) Schematic illustration of synthesis process for ZCH-PC. (b) Schematic illustration of the formation mechanism of ZCH-PC (Reprinted with permission
of Ref. [302]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

nanofiber composites with enhanced electrochemical performance have wastes to produce value-added products [307]. Bingjun Zhu et al. [308]
been reported by L. Wannasen et al. [306], the Co2P2O7 composite with published tailoring biomass-derived carbon for high performance super
CNFs can reduce the charge transfer resistance of electrodes through capacitors from controllably cultivated algae microspheres. As per their
electron transfer optimization, which indicates an improvement in report, a high-performance “green” carbon-based supercapacitor elec­
electron transport capacity. Furthermore, high electrical conductivity trode material is synthesized from selected algae microspheres, which
can decrease the charge transfer resistance of the electrodes, thus are grown under controlled cultivation conditions. The best-performing
leading to an increased power density. Algae biomass is known to grow ample possesses a high specific surface area of 1, 337.9 m2 g− 1 with a
fast in eutrophicated water bodies. Its excessive accumulation does hierarchically porous structure and naturally intrinsic nitrogen dopant.
serious damage to the marine ecosystem. It not only promotes bacteria This leads to an excellent specific capacitance of 353 F g− 1 at 1 A g− 1 and
growth but also hinders the tourism development. Therefore, a practical 92 % capacitance retention even after 10, 000 charge-discharge cycles at
and feasible method to solve this problem is to take advantage of these 20 A g− 1, which makes it superior to many recently reported biomasses-

Fig. 16. Diagram of sharia bambusicola derived heteroatoms doped spongy-like carbon via KOH activation for supercapacitors and SEM images of (A) pre‑car­
bonized carbon and (B, C) BFDC-2. (D) TEM images of BFDC-2. (E) XRD, (F) Raman, (G) N2 sorption isotherms, (H) pore-size distribution and (I) XPS patterns of
BFDC (Reprinted with permission of Ref. [306]).

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P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

and synthetically derived carbon electrode materials. It is found that heteroatom doping, can lead to the development of high-performance
residual nitrogen and metal contents in algae-derived carbon are highly carbons with tuned order and enhanced conductivity for superior elec­
influenced by biomass components, such as proteins. The content of trochemical applications. In summary, activated carbon electrode ma­
these components can be controlled by adjusting the concentrations of terials have been derived from cost-effectiveness, eco-friendly biomass
nutrients in cultivation media. However, nitrogen in algae proteins is resources, which can act as an excellent candidate for the development
not pyrolytically stable, and studies indicate that excessive residual of various supercapacitors with enhanced electrochemical performance,
metal content plays the role of “dead mass” and results in a less- high-rate capability, and cycling stability, were discussed in this review.
developed porous structure. Also different synthesis methods have been described in detail for con­
Therefore, this suggests that both biomass selection and cultivation version of biomass into activated carbon along with significance of
should aim for proteins with a more stable nitrogen content and mini­ biomass derived carbon materials for supercapacitors. Although the
mized content of electrochemically inactive metals such as Mg and Ca. reported biomass derived carbon electrodes have exhibited rather high
Hence, this study does not just demonstrate a green candidate electrode performance in the laboratory scale more researchers are still required
material for high-performance supercapacitors, but also provides an to meet the demand for commercial applications.
innovative selection and cultivation strategy to improve the capacitive
performance of biomass-derived carbon. Fungi are a large group of 10.1. Future prospectives
eukaryotic organisms, dissimilar to plants, animals, and bacteria. They
have been widely applied in the food and pharmaceutical industries due Activated carbon is a new innovative solution towards extensive
to their worldwide abundance and their essential role in the decompo­ environmental and energy applications. Despite various studies being
sition of organic matter and the nutrient cycling. Nevertheless, carried out regarding the production and application of biomass-derived
compared with their use in nutrition, their potential applications in carbon, a number of research gaps remain.
material science have been ignored. Detailed investigations indicate that
the composition of fungal cells is rich in chitin, unlike the cellulosic cell 1. The utilization of naturally abundant biomass to prepare biomass-
wall of plants [309–312]. derived carbons with high functional performance in super­
Recently, Xinran Hu et al. [313] studied heteroatoms (N-, Si-) self- capacitor application is green, cost-saving and sustainable. While the
doped spongy carbon derived from wild fungus sharia bambusicola as advantages of biomass energy are plenty, there are also some
electrode materials for supercapacitors. The morphology of wild fungus shortcomings, including: (i) Biomass energy is not as efficient as
is depicted in Fig. 16. This study provides a simple and efficient con­ fossil fuels (ii) It is not entirely clean (iii) Can lead to deforestation
version of wild fungus sharia bambusicola to heteroatoms (N-, Si-) (iv) Biomass plants require a lot of space.
doped spongy carbon materials via simple chemical activation. The 2. The biomass composition, production techniques and the role of
activated carbon exhibits a maximum specific capacitance of 339 F g− 1 activation agent have a significant effect on activated biochar.
at 0.5 A g− 1, excellent rate and cycling stability. This remarkable Further studies are needed to determine optimum biomass compo­
supercapacitor performance can be attributed to the hierarchical porous sition and production procedures for various distinctive applications
structure, abundant pore volume (0.84 cm3 g− 1) and a small number of for both electrochemical and adsorbent. Good knowledge regarding
heteroatoms doping. the interrelation between surface area, pore size and surface chem­
Hence, microorganism is naturally formed by different high-surface istry have a vital influence over both adsorption and energy appli­
area cellular structures that can lead to a large surface area with cations to design nanostructures materials to bring out promising
potentially controllable porosity in the resultant carbons. As all other and impressive improvements.
living organisms, microbes are comprised mainly of carbon, hydrogen, 3. Considering the diversity of biomass resources, fundamental studies
oxygen, nitrogen, phosphor and sulfur with trace amounts of other el­ are necessary to understand and control the properties of biomass
ements. On top of their high carbon content which serve as the main derived carbon materials that are prepared using different biomass
structure in microbes, their rich nitrogen, phosphor, and sulfur contents precursors and methods. However, the processability, final structure
fruitfully provide abundant heteroatoms as dopant. It is important to and functional performance of the as-prepared biomass-derived
highlight that such heteroatom functionalities can enhance surface carbon are strongly correlated with the chemical composition,
structural properties which leads the electrode materials for suitability macroscopic structural hierarchy, and the sublevel microstructural
of practical applications. characteristics of the biomass precursors. Thus, it requires rational
design in the processes of precursor selection, carbonization, and
10. Summary activation to obtain high-performance biomass-derived carbon with
optimized SSA, specific capacitance and conductivity for super­
The search for a clean, renewable source is of high significance due to capacitor applications.
the depletion of conventional resources and to reduce the amount of CO2 4. The current review mainly spotlights on novel kind of biomass
generated. Biowastes are considered as one of the most versatile, green, derived activated carbon electrodes for supercapacitors. Although
and renewable resources for the production of comprehensive variety of activated biochar possesses superior characteristics, studies based on
carbon structures. These carbon materials are reported to possess its intrinsic properties are lacking due to its hydrophobic nature.
interesting characteristics suitable for several applications related to Capacitive performance of supercapacitor not only limited on the
environmental and energy conversion/storage. More specifically, the surface area but also depends on various other factors such as pore
consumption of various naturally available biomass resources to derive distribution and structure, surface functionalities and electrical
functional porous carbons with significant impact in multiple fields is conductivity. Furthermore, the presence of ultra-small micropores in
considered green, economical, and sustainable. Though, the processing the low surface area contributes positively towards energy storage
ability, molecular arrangement, and overall functioning of synthesized and adsorption applications. Therefore, the selection of appropriate
biomass-derivative carbons are intensely interconnected with chemical methods for calculating physical and structural parameters that are
configuration, microscopic structure, including sublevel microstructural appropriate for applications remains a puzzling topic for future
features of the precursors used for synthesis. Thus, it necessitates the studies.
sensible design, including careful selection of precursor, carbonization, 5. So far, the chemical activation method via KOH, NaOH etc. is a
and activation technique to acquire high-performance carbon or carbon familiar tool for made porous carbon with a rich porous structure,
composites from biomass with enhanced surface area and pore hierar­ particularly for micropores. It ought to be significant that a huge
chy. However, an improved process, including efficient activation and amount of volatile-gases will be produced since the reaction among

22
P. Manasa et al. Journal of Energy Storage 54 (2022) 105290

KOH and carbon matrix at high temperature, these volatile gases, [8] Qi-Qi Yang, Lin-Feng Gao, Zhi-Yuan Zhu, Hu. Chen-Xia, Zhi-Peng Huang, Rui-
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other activation strategies should be urbanized to meet up the de­ Yufeng Wu, Recent progress on porous carbon derived from Zn and Al based
metal-organic frameworks as advanced materials for supercapacitor applications,
mand of industrialization. J. Energy Storage 44 (2021), 103263.
6. Even though the state-of-the-art research on the biomass-derived [10] Ying Liu, Lingyang Liu, Long Kang, Fen Ran, Energy storage mechanism of
carbon for supercapacitors has shown relatively higher specific ca­ vanadium nitride via intercalating different atomic radius for expanding
interplanar spacing, Energy Environ. Mater. 5 (2022) 565–571.
pacitances compared to conventional carbon nanomaterials (e.g., [11] Fen Ran, Kuiwen Shen, Yongtao Tan, Bowu Peng, Shaohua Chen, Weijie Zhang,
CNT, CNF), and excellent high-rate performance and cyclability, Xiaoqin Niu, Lingbin Kong, Long Kang, Activated hierarchical porous carbon as
several critical challenges are still associated with the development electrode membrane accommodated with triblock copolymer for supercapacitors,
J. Membr. Sci. 514 (2016) 366–375.
of biomass-derived carbon for supercapacitors. Biomass offers op­ [12] Ravi Kali, T.N. Balaji Padya, P.K.Jain Rao, Solid waste-derived carbon as anode
portunities for making flexible electrodes. This will open up a new for high performance lithium-ion batteries, Diam. Relat. Mater. 98 (2019) 1–6.
research area. With continual research on this research topic, there [13] Pallabi Samaddar, Yong Sik Ok, Ki-Hyun Kim, Eilhann E. Kwon, Daniel C.
W. Tsang, Synthesis of nanomaterials from various wastes and their new age
could be great opportunities to achieve practical applications of applications, J. Clean. Prod. 197 (2018) 1190–1209.
biochar materials in the fields of renewable energy conversion and [14] Fujuan Wang, Xiaohong Shi, Junlei Zhang, Tianqi He, Liang Yang,
storage. Prospective feasible approaches of activated carbon on Tianyun Zhang, Fen Ran, Bacterial cellulose-derived Miro/mesoporous carbon
anode materials controlled by poly(methyl methacrylate) for fast sodium ion
combined energy storage and environment applications need further
transport, Nanoscale 14 (14) (2022) 3609–3617.
investigations. A lot of interdisciplinary studies over various science [15] Sedahmed Osman, Raja Arumugam Senthil, Junqing Pan, Lulu Chai, Yanzhi Sun,
streams need to understand and explore the detailed chemical Yufeng Wu, Hierarchically activated porous carbon derived from zinc-based
mechanisms to develop new novel sustainable materials to deliver fluorinecontaining metal-organic framework as extremely high
specificcapacitance and rate performance electrode material for
better applications in the field of sustainable energy and environ­ advancedsupercapacitors, J. Colloid Interface Sci. 591 (2021) 9–19.
mental applications. Further studies are vital to minimize the pre­ [16] J. Tian, Z. Liu, Z. Li, W. Wang, H. Zhang, Hierarchical S-doped porous carbon
vailing knowledge gaps. derived from by-product lignin for high-performance supercapacitors, RSC Adv. 7
(2017) 12089–12097.
[17] Wenlin Zhang, Yunlong Yang, Muchakayala Ravi, Lingbin Kong, Long Kang,
Declaration of competing interest Fen Ran, Interconnected porous composites electrode materials of Carbon@
Vanadium nitride by directly absorbing VO3-, Electrochim. Acta 306 (2019)
113–121.
The authors declare that they have no known competing financial [18] Yongtao Tan, Lei Meng, Yanqin Wang, Wenju Dong, Lingbin Kong, Long Kang,
interests or personal relationships that could have appeared to influence Fen Ran, Negative electrode materials of molybdenum nitride/N-doped carbon
the work reported in this paper. nano-fiber via electrospinning method for high-performance supercapacitors,
Electrochim. Acta 277 (2018) 41–49.
[19] M. Klose, R. Reinhold, F. Logsch, F. Wolke, J. Linnemann, U. Stoeck, S. Oswald,
Data availability M. Uhlemann, J. Balach, J. Markowski, P. Ay, L. Giebeler, Softwood lignin as a
sustainable feedstock for porous carbons as active material for supercapacitors
using an ionic liquid electrolyte, ACS Sustain. Chem. Eng. 5 (2017) 4094–4102.
No data was used for the research described in the article.
[20] Raja Arumugam Senthil, Viengkham Yang, Junqing Pan, Yanzhi Sun, A green and
economical approach to derive biomass porous carbon from freely available
Acknowledgments feather finger grass flower for advanced symmetric supercapacitors, J. Energy
Storage 35 (2021) 1–10.
[21] Bing Li, Hongyou Zhang, Dabin Wang, Hong Lv, Cunman Zhang, Agricultural
This work was partly supported by China Postdoctoral Science waste-derived activated carbon for high performance lithium-ion capacitors, RSC
Fundation (2020M673637XB), the National Natural Science Foundation Adv. 7 (2017) 37923–37928.
of China (51203071, 51363014, 51463012, 51763014, and 52073133), [22] Bing Li, Hongyou Zhang, Cunman Zhang, Agricultural waste-derived activated
carbon/graphene composites for high performance lithium-ion capacitors, RSC
Joint fund between Shenyang National Laboratory for Materials Science Adv. 9 (2019) 29190–29194.
and State Key Labo- ratory of Advanced Processing and Recycling of [23] Paul Thomas, Chin Wei Lai, Mohd Rafie Bin Johan, Recent developments in
Nonferrous Metals (18LHPY002), and the Program for Hongliu Distin- biomass-derived carbon as a potential sustainable material for super-capacitor-
based energy storage and environmental applications, J. Anal. Appl. Pyrolysis
guished Young Scholars in Lanzhou University of Technology. 140 (2019) 54–85.
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