Chemical Engineering Journal 397 (2020) 125418

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Chemical Engineering Journal

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

Recent advances and challenges in biomass-derived porous carbon T

nanomaterials for supercapacitors
⁎
Zijiong Li , Dongfang Guo, Yanyue Liu, Haiyan Wang, Lingli Wang
School of Physics & Electronic Engineering, Zhengzhou University of Light Industry, Zhengzhou 450002, PR China

H I GH L IG H T S

• Biomass-derived porous carbon is widely used for electrochemical energy storage.

• Various activation methods and mechanisms of biomaterials are summarized.
• Potential future development and challenges of biomass-derived are discussed.

A R T I C LE I N FO A B S T R A C T

Keywords: In recent years, the recycling of low-cost and wide-source biomass has caused great concern. The obtained
Porous carbon biomass-derived porous carbon (BDPC) is widely used as the electrode material of new energy storage device in
Biomass the field of electrochemistry due to its unique properties such as large specific surface area, developed pore
Activation structure, acid and alkali resistance, excellent conductivity, and adjustable pore size. At the same time, efficient
Electrochemical
energy storage devices have been gradually developed and upgraded. Various hybrid supercapacitors (sodium
Supercapacitor
ion, potassium ion, lithium ion, zinc ion, etc.) are widely used as new green energy equipment in hybrid power
vehicles and portable electronic products. In this review, various activation methods and mechanisms are in-
troduced in detail, and the application and research progress of biomaterials in electrochemical energy storage in
the past three years are reviewed. The effects of different activation processing methods on the surface mod-
ification and micromachining of the obtained carbon materials on the electrochemical performance are briefly
discussed. Finally, this paper summarizes the current research status of biomass-derived porous carbon in energy
storage, potential future development directions and current challenges to promote the application of biomass-
derived porous carbon materials in various fields, which provide useful insights for further development and
utilization of biomass.

1. Introduction
In recent years, the energy crisis and ecological pollution caused by
the consumption of fossil fuels have become increasingly serious and
have brought high governance costs at the same time. Therefore, the
development of clean energy and the study of energy efficiency have
aroused widespread concern [1]. Undoubtedly, it is very important to
promote society towards renewable and sustainable energy and trans-
form the utilization of resources. However, the imperfection of new
energy storage systems, incomplete commercial development, and
many difficult issues need to be resolved, which will cause the current
status of energy use to continue for a long time. Meanwhile, researchers
continue to try to find suitable strategies and develop new methods or
materials to solve these problems in order to minimize environmental
pollution and waste of resources [2]. The most intuitive result is that
there has been an increase in the production of green clean energy from
sources in the past decades and substantial clean energy is used in
various electric vehicles and equipment. Because the use of energy is
limited by uneven spatial and temporal distribution, there is an urgent
need for the emergence of alternative energy storage strategies and
efficient energy conversion technologies [3]. A key requirement for
making full use of the intermittent power generated by these renewable
resources is an efficient energy storage system [1]. The rapid popula-
tion and economic growth has led to an increase in the use of energy
equipment, leading to high energy consumption and huge social pres-
sure, and ultimately the problem of energy shortage is inevitable. In
addition, the booming industry, improvement of living conditions, and
increased awareness of environmental protection will accelerate the

⁎
Correspondence author.
E-mail address: zijiongli@zzuli.edu.cn (Z. Li).

https://doi.org/10.1016/j.cej.2020.125418
Received 15 October 2019; Received in revised form 20 March 2020; Accepted 20 April 2020
Available online 11 May 2020
1385-8947/ © 2020 Elsevier B.V. All rights reserved.
Z. Li, et al.
Fig. 1. Comparison of power and energy density of different energy storage devices. (Reprinted with permission from Reference [12]).
development of renewable and clean energy [4].
As an important part of energy utilization, how to improve the ef-
ficiency of energy storage systems has always been the focus of research
and improvement by scientists around the world. In order to meet the
needs of modern society and respond to emerging ecological problems,
it is vital to find and develop new, low-cost and environment-friendly
energy conversion and storage systems [5]. A series of energy storage
and conversion devices have been developed for commercial applica-
tions, such as fuel cells, batteries, supercapacitors [6–11]. In order to
realize the opportunities brought by the development of different en-
ergy storage equipment and give full play to their advantages, it is
necessary to fully understand the relationship between power and en-
ergy of different energy storage equipment as shown in Fig. 1 [12].
Battery systems are currently used as the main energy storage devices in
the core components of mobile electronic products. It has undergone
several major improvements in the past 30 years of practice and have
evolved from the earliest lead-acid batteries to the widely used alkaline
metal ion batteries [13–19]. Lithium ion battery (LIB) has been widely
applied in various fields as the most successful power source to date
[20–22]. However, due to the many limitation of electrode materials in
terms of safety, environmental protection, cycle stability, high cost, and
power density, LIB is difficult to develop to a new height in the short
term [23]. In addition, the low specific power is also an important
factor limiting its further development. Despite many shortcomings,
batteries will remain the most important energy storage device until the
emergence of new and efficient energy storage devices [24]. Fuel cells
are power generation devices that directly convert chemical energy
existing in fuel and oxidant into electrical energy [25,26], so Fuel cells
have outstanding energy conversion efficiency. Based on many ad-
vantages such as fuel diversity, high efficiency, flexible assembly, fast
load response, and strong environmental affinity, fuel cells can be used
as a promising energy storage device to replace rechargeable batteries
[27]. However, fuel cells has high installation costs, unsatisfactory
starting speeds (less than internal combustion engine), imperfect hy-
drogen storage technology, incomplete infrastructure and the same low
specific power as battery, and the bottlenecks in terms of price and
technology have been limiting the development of fuel cells.
2
Chemical Engineering Journal 397 (2020) 125418
Electrochemical capacitor (EC), also known as supercapacitor, is
actually new energy storage device lying between the range of usual
capacitor and battery, and it has received extensive attention in recent
decades due to multiple strengths [28]. The advantages of super-
capacitor over batteries and fuel cells are mainly reflected in the fol-
lowing aspects: (1) High specific power. The specific power of super-
capacitor can reach 102~104 W kg−1, which is much higher than the
level of batteries and fuel cells [29]; (2) long charging/discharging
cycles Long cycle life. After 500,000 to 1 million high-speed deep
charge-discharge, supercapacitor still maintains high performance, and
the capacity and internal resistance have only been reduced by 10% to
20% [30]; (3) Wide operating temperature range. Acetonitrile (AN) or
propylene carbonate-based supercapacitors typically have a tempera-
ture range of −40 °C to 70 °C [31]. Due to the stability of adsorption
and desorption of ions in supercapacitor at low temperature, its capa-
city change is much smaller than that of battery; (4) Maintenance-free.
Thanks to the load capacity during charge and discharge, super-
capacitor can be repeated stably, so theoretically no maintenance is
required; (5) Green and environmental protection. In the production
process, heavy metals and other harmful chemicals that are polluting
the environment may not be used as raw materials for supercapacitor,
so supercapacitor belongs to a green power source.
As a representative of electrical energy storage devices, super-
capacitor has been thoroughly studied for its simple principle and high
dynamic of charge propagation. Moreover, supercapacitor has larger
specific capacity, higher specific energy or capacity density, wider op-
erating temperature range and extremely long service life than tradi-
tional capacitors. And compared with batteries, it is environmentally
friendly and has higher specific power [32]. Supercapacitor has re-
ceived widespread attention due to the filling of energy and energy gaps
between batteries and traditional capacitors, which makes up for the
shortcomings of the other two energy storage devices to some extent
[33]. In short, the application of supercapacitor has become an im-
portant energy storage technology, which will play a key role in the
large-scale deployment of many applications such as intermittent re-
newable energy and smart grids [1]. On the other hand, supercapacitor
has been applied to many energy storage applications including
Z. Li, et al.
household and industrial fields [32,34,35]. It is worth noting that the
unique advantages of low temperature operation, long service life,
safety, excellent stability, low cost and fast charge-discharge time will
drive supercapacitor into a promising power supply device to replace
battery equipment. To sum up, the development of has good prospects.
To sum up, supercapacitor has a good development prospect in the
future.
2. The role of biomass materials in supercapacitor
The energy storage of supercapacitors results from the accumulation
of charge or reversible redox reaction. Therefore, supercapacitors can
be divided into three main categories according to the energy storage
mechanism: electric double layer capacitor (EDLC) and pseudocapa-
citor and the hybrid supercapacitor composed of their combinations
[36]. Electric double layer capacitors generally use carbon materials as
electrode materials (such as activated carbon, carbon black, carbon
nanotubes, carbon aerogels, graphene, etc.), and form an electric
double layer on the surface of the electrode active material by ion
migration, using electrons or ions The charge formed by the aligned
arrangement creates a capacitance. This process is a physical reaction.
Faraday capacitors generally use metal oxides (hydroxides, sulfides,
etc.) or conductive polymers as electrode materials (such as RuO2, Ni
(OH)2, MnO2, polyaniline, polypyrrole, polythiophene, etc.). Surface/
near-surface fast reversible redox reactions generate and store electrical
energy, so higher capacitance can be obtained. Hybrid supercapacitors,
combining the advantages of the first two types of capacitors, the
electric double layer capacitor electrode and the plutonium capacitor
electrode are used as the capacitor poles to assemble the hybrid su-
percapacitor, so the energy storage process of the hybrid supercapacitor
has both physical and chemical processes.
The electrode material determines the innate characteristics of su-
percapacitor. As a key component directly affecting the performance of
supercapacitor, electrode material mainly including the following
types: carbon-based materials (activated carbon, carbon nanotubes,
carbon fibers, graphene), metal oxides (Manganese Dioxide, Ruthenium
Dioxide, Nickel Oxide, Cobaltosic Oxide), conducting polymers (poly-
aniline and polypyrrole) and the related composite [12]. Among var-
ious types of electrode materials, metal oxides stand out in pseudoca-
pacitor because of their high natural abundance, simple synthesis and
good electrochemical stability [37]. Unfortunately, the low con-
ductivity of metal oxides results in sluggish reaction kinetics, which
limits their further development and practical applications [38]. Con-
ductive polymers have been studied for a long time [39]. Conductive
polymers can be considered as important research directions for su-
percapacitor electrode materials due to low cost, high environmental
stability, high charge storage capacity, high conductivity and excellent
reversibility. However, the conductive polymer often swells and shrinks
during the charge and discharge process, which will cause the con-
ductive polymer-based electrode to deteriorate its mechanical proper-
ties and capacity during the cycle [40]. Most conductive polymers
currently face the same problem. At present, the main disadvantage of
conductive compounds is poor cycle stability relative to carbon mate-
rials; and compared to metal oxides, their specific capacitance, energy
density, and power density are lower. In short, the cyclic stability of
conductive polymer electrode materials is far from perfect and has
become the biggest obstacle to the development of conductive poly-
mers.
Carbon materials are generally cheap and available and have good
chemical stability and environmental adaptability [42], they are the
best choice for materials of EDLC. As a typical representative of carbon
materials, carbon nanotubes [43] and grapheme [44] are different from
traditional graphite. They are quasi-one-dimensional and two-dimen-
sional nanomaterials composed of carbon atoms with only one atomic
layer thickness, respectively. Among them, graphene has high specific
surface area, excellent electrical conductivity, good mechanical
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Chemical Engineering Journal 397 (2020) 125418
properties and chemical stability [45], which is expected to solve the
problems of low effective specific capacity, poor multiplier perfor-
mance, short cycle life and poor safety performance in the field of en-
ergy storage. Meanwhile, graphene has a wide range of applications in
the new energy field and is promising. In principle, graphene as an
excellent two-dimensional conductive material can be directly applied
to electrode materials or composite materials with structural regulation
functions in new energy batteries [46–49]. Although the current gra-
phene production process and its good yield have been greatly im-
proved [50–53], it is still difficult to meet the requirements of in-
dustrialization or large-scale production and the macro demand in the
field of energy storage. In addition, there is a problem of effective re-
combination between graphene and electrode material active materials.
Due to the chemical inertness and agglomeration of grapheme [54], the
recombination is mostly a weak physical interaction. Therefore, its
structural stability is poor, which seriously affects its practical appli-
cation. These unfavorable factors, including high cost, will prevent the
large-scale application of new energy graphene batteries in the short
term.
Activated carbon is also widely used in the field of electrochemical
energy storage. In most cases, the specific capacitance is mainly de-
termined by the specific surface area and pore size distribution [42].
The specific surface area of traditional activated carbon is relatively
small, and the contact resistance between the particles and the elec-
trolyte ions is large [55], which not only leads to its poor conductivity
and specific capacitance but also limits the energy storage and con-
version efficiency inside the material [56]. With the advent of porous
carbon nanomaterials, the research of porous carbon for super-
capacitors has been pushed to a new climax. Porous carbon belongs to
porous separation material with a developed pore structure, ultra-high
specific surface area, strong adsorption capacity, good chemical stabi-
lity, easy regeneration, and many other advantages. It can be used for
environmental restoration, catalysis, energy storage and conversion
[2,57]. As shown in Fig. 2, carbon materials can be used not only in
electric double layer capacitors, but also in hybrid capacitor devices,
and have a wide range of applications. Porous carbon materials can be
used as an important part of electrode materials for supercapacitors
because of the supply of a large number of electric double layer capa-
citors [12]. Benefit from large specific surface area, low cost, con-
venient handling and modification, ordered nanoporous carbon-based
materials are ideal electrode materials for supercapacitors, which have
been reflected in different applications [32,58–69]. Therefore, the
reasonable acquisition and utilization of porous carbon is of great sig-
nificance for the future development of electrode materials [70]. With
Fig. 2. Different types of supercapacitors and electrode materials. (Reprinted
with permission from Reference [41]).
Z. Li, et al.
the advancement and development of science and technology, the
connection between energy storage applications and waste utilization
has become closer [1]. Porous carbon materials can be directly ex-
tracted from biomass, which is a huge advantage that other types of
electrode materials cannot match.
Biomass refers to all organic matter formed directly or indirectly
through the photosynthesis of green plants, including all animals,
plants, microorganisms and excretion and metabolites produced by
these organisms, which are clean, renewable and diverse and can be
used as an excellent precursor for the preparation of carbon-based
materials [67]. Many porous carbon-based materials can be extracted
from biomass by relatively facile synthesis and easy-to-synthetic
methods, so that is considered an attractive way of natural acquisition
[2]. In addition, biomass materials are widely distributed in nature and
have abundant resources. One of the most effective and promising ways
to provide sustainable energy for energy storage equipment is to con-
vert biomass into ordered “nanostructured porous carbon” with various
electrochemical properties. Agricultural and forestry biomass is cheap,
diverse and renewable, so using waste agricultural and forestry biomass
as a raw material for porous carbon is an important part of future
carbon material research. Porous carbon nanomaterials have many
characteristics, such as large specific surface area, rich pore structure,
adjustable pore size, and stable chemical properties, so they have good
electrical conductivity and excellent cycle stability when used as elec-
trode materials in solution electrolyte systems [35]. In recent years,
more and more people are committed to the research of green and clean
energy storage devices, especially in the field of biomass-based elec-
trode materials.
Biomass-derived porous carbon (BDPC) has received widespread
attention as an electrode material for supercapacitors profit from eco-
nomic value, practicality, adjustable physical/chemical characteristics,
and environmental protection [71,72]. As shown in Fig. 3, a series of
biomass-derived carbon materials with various unique structures have
been widely used in various types of supercapacitors (sodium ion su-
percapacitors, lithium ion supercapacitors, zinc ion supercapacitors,
etc.) [6,10,15,16,18,19,22,24,32,38,59,65,68,73–104]. In addition to
many inherent advantages such as cheap, availability, and renewable,
the rational application of BDPC is also an effective method for waste
treatment and reuse [90]. By processing biomass, various forms of
porous carbon containing a large number of beneficial natural func-
tional groups and heteroatoms (such as O, N, S, P) are synthesized.
Surface heteroatoms play an important role in enhancing the capacitive
performance of carbon electrodes [32]. According to X-ray photoelec-
tron spectroscopy (XPS) analysis, in addition to carbon atoms with
many sp3 bonds and heteroatoms, BDPC also contain heteroatoms such
Fig. 3. Biomass-derived carbon materials with diverse structures used in var-
ious electrochemical energy storage devices.
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Chemical Engineering Journal 397 (2020) 125418
as N, O, P, and S. It has been reported that C=O near 531.7 eV can
effectively improve hydrophilicity [105]. N atoms in the form of pyr-
idine-N and pyrrole-N are also beneficial to enhance the wettability
between the electrode and the electrolyte [106]. Studies have shown
that negatively-charged pyridine-N and pyrrole-N can trigger the gen-
eration of rubidium capacitors [86]. Positively-charged graphitized-N
and oxidized-N are helpful for electron transfer, which are all conducive
to improving the conductivity of carbon materials [107]. In addition,
some oxidation states of S (C-SOx-C) exist on the surface of carbon
materials, which is also expected to enhance its wettability to electro-
lytes [32,108]. The rich structure of nanopore is conducive to the ex-
cellent rate performance of the material in terms of internal electron
transfer. And these beneficial natural functional groups and heteroa-
toms provide a high level of pseudocapacitance contribution to some
extent [2]. Therefore, heteroatom doping of porous carbon is an ef-
fective strategy to improve electrode capacitance performance. Com-
pared with other carbon products, BDPC can be prepared from biomass
in one step. In addition, biomass products have a natural bionic struc-
ture. Thanks to the superiority, integrity and coordination of the bionic
structure, many tedious material structure adjustment procedures have
been reduced, which will greatly improve the problem of chemical
consumption.
BDPC is derived from abundant renewable resources and contains
more heteroatom elements. It has characteristics of pseudocapacitance
contribution, high electron density, and simultaneous activation [12].
In recent years, the demand for high-performance electrodes has led to
the further development of research and synthesis technologies for
BDPC. A large amount of woody biomass has been studied as electrode
materials for supercapacitors, such as walnut shells [109], bamboo
bagasse [110], raw cotton [80], corn silk [93], pistachio nutshell [111],
rice husks [58], oil palm shell [70], coconut shells [103], broad bean
shells [112], Acacia tree bark [113], onions [68], cornstalk [114], co-
conut shell [115], shiitake mushroom [72], bamboo [116], etc. Woody
biomass is mainly composed of cellulose, hemicellulose and lignin. A
large amount of carbon exists in woody biomass, which is the best
choice for making low-cost porous carbon. Biomass becomes a porous
carbon with high specific surface area and developed pores after car-
bonization or activation treatment. The existence of a large number of
micropores and mesopores provides more effective transmission chan-
nels for charged ions, and the electrical conductivity of the material is
significantly improved. Many high-quality electrode materials have
been obtained from woody biomass. Today, the study of BDPC is no
longer limited to woody biomass, and a comprehensive study of a series
of biomass precursors has been conducted. A large number of animal-
based biomass including cuttlebone [91], fish skin [32], cicada slough
[86], goat hair [92], cow drug [117] are also used as electrodes for
various energy storage devices material. According to the unique
composition and structure of biomass, the electrodes derived from it
show excellent capacitance performance in electrochemical systems. It
is well known that commercial activated carbon is usually extracted
from natural precursors rich in resources [118]. In recent years, carbon
aerogels [61,80,119,120] have also been favored by many researchers.
These materials all belong to the scope of BDPC. Although the value of
many BDPC has been proven in research, there are still many challenges
we need to face. Large-scale synthesis, development, and further com-
mercial applications still require continuous efforts to expand, which is
the only way to develop materials.
3. Synthesis methods of porous activated carbon
Most untreated biomasses are hard and contain a large amount of
impurities, so they are not suitable for direct use as electrode materials
for electrochemical energy storage devices. And the appropriate specific
surface area, balanced pore distribution, favorable heteroatom func-
tional groups, and the type of electrolyte will affect the conductivity
and ion diffusion rate of the carbon electrode in the electrolyte and
Z. Li, et al.
Table 1
Effect of pyrolysis conditions on the production of biochar and its related products.
Type of pyrolysis Temperature range (°C) Heating rate (°C min−1)
Slow 300–800 < 10 °C min−1
Fast 400–600 > 10 °C min−1
Flash < 650 ~1000 °C min−1
Gasification 700–1500 ~1000 °C min−1
Reproduced with permission from reference [2].
cause differences in electrochemical performance between different
carbon materials. Therefore, we need to find the most suitable material
processing strategy. A reasonable processing method is a prerequisite
for the synthesis of low-cost, highly efficient biomass-derived carbon
electrode materials. It is especially important to fully understand the
synthesis method and mechanism before processing raw materials
[121]. At present, there are two main methods for synthesizing acti-
vated carbon: pyrolysis carbonization and hydrothermal carbonization
[122].
3.1. High-temperature pyrolysis carbonization
biomass is converted into biochar by heat treatment at moderate
temperatures in the absence of oxygen with the process known as
pyrolysis [123]. Pyrolysis is derived from the original method of
burning charcoal, which is an irreversible chemical and physical pro-
cess. It is considered to be the most direct method for synthesizing
biomass-derived carbon materials (most carbon can be preserved).
Pyrolysis is mainly divided into slow/fast pyrolysis, low/high tem-
perature pyrolysis and dry/wet pyrolysis as shown in Table 1. Among
them, high temperature pyrolysis is most commonly used to prepare
activated carbon. High-temperature pyrolysis carbonization refers to
placing the precursor in a high-temperature environment under the
protection of an inert gas, and the impurity elements inside the material
are decomposed and discharged as a gas to form a pore structure. Be-
sides, the desired product can be obtained by appropriately changing
the pyrolysis conditions [124]. In different pyrolysis conditions, tem-
perature is considered to be the dominant parameter controlling the
structure and function of the final product. The thermal decomposition
curves [2] of these components in different temperature ranges are
shown in Fig. 4. The specific surface area and pore structure of the
material have been initially improved. Although some biomass-derived
carbon has good capacitance performance without further activation
Fig. 4. Thermal decomposition curves of major biopolymers in typical lignocellulosic biomass. (Reference from [124]).
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Chemical Engineering Journal 397 (2020) 125418
Holding time (sec) Biochar/Bio-oil/Syngas (%)
min-hrs ~35/30/35
0.5–5 ~10–12/70–75/13–20
<1 ~10/65–70/20–25
Secs ~10/5/85
after pyrolysis carbonization treatment and even better than the pro-
duct after activation, most carbon materials prepared by direct calci-
nation usually have lower specific surface area and poor pore structure,
which is not beneficial for electrochemical applications.
Direct activation or reactivation of the material during pyrolysis is
an effective way to optimize the internal structure of the material.
Activation mainly includes the following possible processes:
1. Open the original occlusion hole. Disordered carbon atoms and
heteroatoms react to open the blocked gaps and expose the micro-
crystalline surface;
2. Expand the original pores. Carbon atoms exposed on the surface of
the microcrystals are further burned to enlarge the original pores
and pores;
3. Form new pores. Non-uniform combustion on the surface of the
crystallites results in the formation of new pores; the pore walls
between adjacent micropores are completely burned out to form
mesopores or macropores.
The activation process can be used to make pores in the original
activated carbon by etching to further adjust the pore structure [125],
which can promote the synthesis of bioactive compounds with large
specific surface area, rich functional groups and heteroatom doping.
Substance-derived porous carbon. The activation strategy mainly in-
cludes physical activation and chemical activation.
Table 2 summarizes summarizes examples of BDPC synthesized
using different activation methods in the past three years, including
various precursors and activators [1].
3.2. Physical activation
Physical activation occurs in various oxidizing environments. The
carbonized biomass is placed in air, oxygen (O2), carbon dioxide (CO2),
Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Table 2
Activated carbon materials prepared by different preparation methods.
Carbonization method Activation method Activating agent Biomass-based raw materials Reference
Pyrolysis Chemical KOH Pistachio nutshell, corn silk, absorbent cotton, goat [32,61,63,69,71,77,86,89,92,93,111,112,126–133]
carbonization activation hair, sorghum vinasse, fish skin, cicada slough, stiff
silkworm, soybean dreg, broad beans shells, Jujun
grass, amygdalus pedunculata shell, elm samara,
cornstalk, peanut shells, tremella, squid gladius
chitin, Silkworm excrement, wax gourd, Banana peel
NaOH Polysaccharide, lotus seed shell, tea residue [134–136]
NaOH/KOH Cuttlebones, rice husk [91,137]
KOH/K3Fe(CN)6 Bamboo bagasse [110]
KHCO3 Shiitake mushroom, [72]
NH4H2PO4/KHCO3 Pomelo peel [79]
ZnCl2 Teak wood sawdust, S. bengalense, potato waste [59,66,83]
residue
H3PO4 Waste particleboard, Kanlow Switchgras, Persian [60,138–141]
ironwood, waste circuit boards, shrimp shell
Zn(NO)3 Raw cotton [80]
CH3COOK Bean curd [122]
Physical Air Rice husk, cotton fabric, beams [58,65,142]
activation Steam Barley straw, waste tea, pine nut shell, needle coke [84,143–145]
CO2 Vine shoots, sugarcane bagasse [146,147]
Steam/CO2 Coffee endocarp [148]
Physico-chemical KOH Peanut shell [90]
activation CO2/NaOH Borassus aethiopum shells [149]
ZnCl2 Coffee grounds [150]
Microwave KOH/NaOH Banana peel, sugarcane bagasse, coal tar pitch, [151–154]
induced/assisted camellia oleifera shell
activation CO2 Banana stem, oil palm shell, [70,155]
H3PO4 Bamboo, sawdust, cocoa pod husk [156–158]
ZnCl2 Macadamia nut endocarp, cotton, Eragrostis [159–161]
planaNees leaves
Steam Rice straw, palm shell, palm kernel shell [162–164]
Template assisted/ NaOH lotus seed shell [165]
induced activation ZnCl2 Alginate, cotton carbon, alginate, [166,167,166]
FeCl3 Chitosan, [168]
ZnO Ethylenediaminete tretraacetic acid [169]
CaCO3 Dopamine, soft pitch [170,171],
K2CO3 Soybean meal [172]
CH3COOK Potassium acetate [173]
KOH Petroleum pitch [174]
Hydrothermal Chemical ZnCl2 Citrus peel, lentinus edodes, Teak wood [175,176,66]
carbonization activation KOH Biomass resources (peanut shell, wheat straw, rice [90]
straw, corn stalk, cotton stalk, soybean stalk)
H3PO4 Rose branch [177]
NaOH Coconut shell [178]
Template assisted/ MnCO3 Agaric, [179]
induced activation Glucose Yeast powder, [180]
ethylene oxide/ Chitosan [181]
propylene oxide
block copolymer
CH3COOH Hazelnut shell [182]
Microwave NaOH Resorcinol and formaldehyde [183]
induced/assisted
activation

water vapor, or the mixed atmosphere, and then treated at high tem-
perature for a period of time to obtain the final product. In the initial
stage of physical activation, the products formed on the surface of the
carbon particles in the previous carbonization process first reacts with
oxidizing atmosphere to generate some micropores and mesopores.
Meanwhile, the oxidizing atmosphere further reacts with carbon to
form carbon oxides, and pores are created inside the carbon material by
releasing gas. It is worth noting that physical activation is more effec-
tive than chemical activation in avoiding the combination of impurities
and activators [184]. Here are some common physical activation
methods:
3.2.1. Steam activation
As a representative of physical activation, steam activation has at-
tracted more and more attention due to simple process, low operation
difficulty, and environment-friendly [185]. First, water vapor is ad-
sorbed on the carbon surface to release hydrogen and oxygen. The
presence of hydrogen prevents the continuous reaction at the active
site, and the released oxygen further reacts with carbon monoxide se-
parated from the carbon surface to form carbon dioxide [186]. At the
same time, a large number of micropores are generated. However, the
detailed mechanism of steam activation is still being explored due to its
complexity. The reaction between water vapor and carbon requires a
large amount of heat, so the reaction generally occurs above 750 °C
[187]. When the activation temperature is higher than 900 °C, it is
difficult to enter the pores due to excessive diffusion of water vapor in
the carbide particles, and the reaction cannot proceed uniformly. In
contrast, a slightly lower activation temperature is beneficial to the
complete diffusion of water vapor into the pores, which promotes a
more complete carbide reaction and facilitates the uniformity of the
reaction [188]. Based on the analysis of the relationship between the
activation temperature, activation time, and steam flow on the struc-
ture and properties of the resulting product, Qin et al. [144] used
pyrolyzed pine nut shell as the precursor and obtained porous carbon

6
Z. Li, et al.
with specific surface of 956 m2 g−1 area and mesoporous ratio of 37.1%
by steam activation under high temperature of 850 °C. Ima et al. [145]
prepared a mesoporous activated carbon with maximum specific sur-
face area of 1134 m2 g−1 and mesoporous volume ratio of 78% using
needle coke via two-stage steam activation process under high tem-
perature. Zhou J. et al. [84] used waste tea to prepare porous carbon by
steam activation. When the activation temperature was 800 °C, the
maximum specific surface area of porous carbon was 995 m2 g−1.
3.2.2. Carbon dioxide activation
CO2, as the culprit of the greenhouse effect, is widely distributed on
the earth and has abundant resources. Research on the chemical con-
version and recycling of CO2 is necessary for resource utilization and
environmental protection. Among these oxidizing gases, CO2 can be
used as an environmental-friendly activator for the materials [189],
which is promising due to green and ease of handling [125]. Since the
activation rate is relatively slower than steam activation, the use of CO2
is beneficial to control the activation process, but requires a higher
reaction temperature of 850–1100 °C [190]. Nabais et al. [146] pro-
duced activated carbon from a novel biomass precursor (vine) by CO2
activation, the product had significant BET surface area of 1173 m2 g−1
and micropore volume of up to 0.53 cm3 g−1. Guo Xin et al. [191] used
ganodorma lucidum as carbon precursors to fabricate three-dimen-
sional porous hollow activated carbon microspheres with the distinctive
spore-nanostructures by a simple, green, and low-cost method, and the
samples exhibited superhigh specific surface area of 3053 m2 g−1 and
hierarchically porous structure. Although there have been fewer studies
on carbon dioxide activation compared to steam activation, CO2 also
has a good activation effect [192,193].
3.2.3. Air activation
In theory, air is also a cheap and available gaseous oxidant, which
can be used as a gas activator for the production of porous carbon.
However, the redox reaction of oxygen and carbon is a severe exo-
thermic reaction, and the direct use of air to activate carbon may cause
excessive combustion of the raw materials and fail to effectively form
pores. Robert et al. [142] Successfully synthesized activated carbon and
composite activated carbon for the first time using carbon formed from
air-treated wood. In the case of products with a packing density of
0.7–1.14 g cm−3, they still retain a lot of micropores and an ultra-high
specific surface area of 1121–2487 m2 g−1. Wang et al. [194] dealed
oxidized polyacrylonitrile fibers to synthesize N-enriched (20.8 wt%)
porous carbon fibers in one step by low-temperature carbonization and
air activation. A large number of narrow micropores are formed inside
the product, which also provides a convenient strategy for the pre-
paration of porous carbon with high nitrogen content.
3.2.4. Microwave assisted/induced physical activation
For conventional heating devices, a temperature gradient from the
center to the surrounding area is inevitably generated because of the
fixed nature of the heat source, which will cause uneven heating from
the sample surface to the inside [196]. In addition, the conventional
heating process requires longer processing time and more stringent
experimental conditions. These unfavorable factors will affect the ac-
tivation efficiency and incur additional processing costs. meanwhile,
the loss of gaseous products have an adverse effect on the quality of the
porous carbon [197]. Microwave pyrolysis activation is a new tech-
nology for preparing activated carbon. In microwave systems, heat is
generated by volume. Microwaves transmitted to biological tissues
cause the polar side chains of the dipole molecules and proteins to
oscillate at a high frequency, and eventually a large amount of heat is
generated due to the electromagnetic oscillations of the molecules and
high-speed molecular motion. Heating at the molecular level raises the
temperature quickly and uniformly, which is not possible with con-
ventional heating devices. The difference between traditional heating
and microwave heating is shown in Fig. 5 [195]. The microwave-
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Chemical Engineering Journal 397 (2020) 125418
induced activation reaction is performed in a closed internal space, so
most problems related to conventional pyrolysis activation can be
solved, which is conducive to improving work efficiency, saving re-
sources and costs, and shortening the experimental cycle [196,198].
Therefore, microwave heating is considered to be a more controllable,
economical, and energy-efficient method. Extensive studies on micro-
wave pyrolysis have been performed on the effects of different para-
meters on the yield distribution and characteristics of the main products
[199–202]. Lam et al. [162] combined microwave heating and steam
activation to extract high-quality activated carbon from waste palm
shell. The obtained activated carbon has high and uniform porosity, a
fixed carbon content of 73 wt% and a specific surface area of 763.1 m2
g−1. In short, due to the many advantages of microwave-induced
physical activation technology, it has been used to prepare BDPC with
some good results [161–164].
The physical activation of materials using an oxidizing atmosphere
is a common top-down activation method. It is known that this method
can effectively form nanopores on the carbon surface [203]. However,
because it relies on oxidizing carbon atoms to form a pore structure and
requires a higher activation temperature, simple physical activation is
difficult to achieve the same effect as chemical activation. In many
cases, physical activation cannot produce a large specific surface area
and a large number of pore channels have poor yields. Specifically, the
shape of the product obtained by the physical activation method is
mainly granular, and its pore size distribution is mainly micropores,
which is more suitable for liquid phase adsorption and substances with
smaller molecular weight and molecular diameter in the gas phase. The
physical activation method has a simple production process, low cost,
and no pollution, and it has broad development prospects and com-
mercial value [204]. Accelerating the reaction speed, shortening the
reaction cycle, and reducing the reaction energy consumption are the
key factors affecting the further development of the physical method
activation process [205].
3.3. Chemical activation
The chemical activation method refers to mixing the chemical ac-
tivator with the raw material, and heating at a high temperature under
the protection of inert gas for carbonization and activation. The acti-
vator usually reacts with the precursor at an elevated temperature to
form pores. Compared with the physical activation method, it has the
advantages of short activation time, easy control of the activation re-
action, and large specific surface area of the product. It has become the
main production method of high-performance activated carbon today.
The shape of the product obtained by the chemical activation method is
mainly powder, and its pore size distribution can be controlled by ad-
justing the ratio of the activator, which is more flexible than physical
activation. There is no doubt that chemical activation is widely used in
materials processing. There are many chemical activators for material
processing, such as Potassium hydroxide(KOH), Zinc chloride(ZnCl2),
Phosphoric acid(H3PO4) and so on. It saves time and increases pro-
ductivity. In addition, chemical activation has several distinct ad-
vantages: (1) Chemical activation need not the participation of oxi-
dizing atmosphere. It is only necessary to mix the activator with a
carbon source and then sinter in inert atmosphere; (2) Chemical acti-
vation has better pore structure system and controllable pore size
[206], and the specific surface area of the product is even close to
4000 m2 g−1; (3) Chemical activation has a higher yield [207], because
the dehydrogenation of chemicals can inhibit the formation of tar and
reduce the production of other volatile substances; (4) Porous carbon
with various structures and performance requirements can be prepared
by a one-step method. Here are some common chemical activation
methods:
3.3.1. Alkali activation
Alkali activation is one of the oldest, most common and most
Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 5. The difference of heating principle between traditional heating and microwave heating. (Reprinted with permission from Reference [195]).

Fig. 6. (a) SEM image of the original product and corresponding element distribution, (b, c) SEM, (d) atomic force microscope (AFM), and (e) TEM image of the
obtained microporous carbon nanosheets (MPCNS). (F) TEM image and corresponding element mapping image (EDX) of MPCNS. (Reprinted with permission from
Reference [32]).

effective chemical activation methods, and has been used in many
simple activation processes [147,208,209]. KOH is a typical re-
presentative in alkali activation. When KOH is used as activator, the
formation of tar can be effectively suppressed, and the reaction rate can
be increased. In short, the product obtained after KOH activation has
higher specific surface area and optimized electrochemical perfor-
mance. In addition, KOH activation has the advantages of low reaction
temperature, high conversion rate, high specific surface area, and
developed micropores, which are widely used in the activation of
carbon materials. Although KOH activation is a well-known method in
the preparation of porous carbon, due to the complexity of experi-
mental parameters based on the reactivity and variables of different
precursors, the activation mechanism has not been well understood
[210]. In general, KOH activation can be considered to have gone
through the following steps: a. KOH and carbon react to form po-
tassium-containing compounds (K2CO3, K2O) to obtain pore structure;

8
Z. Li, et al.
b. Intermediate products including H2O and CO2 can further react with
carbon to produce pores; c. The generated potassium can be inter-
calated into a partially crystallized carbon material and expanded to
obtain pore channels [172]. According to the results of previous studies
[111], it was detected that KOH activated the carbon source through
the entire reaction. Here is the overall reaction equation [210]:
6KOH + 2C → 2K + 3H2 + 2K2CO3
KOH starts to be converted into K2CO3 at 400 °C, and KOH is
completely consumed when the temperature reaches 600 °C. Due to the
interaction of metallic potassium in the carbon matrix, the space be-
tween the carbon atom layers has expanded, which has led to an in-
crease in the total pore volume [211]. Finally, these salts and alkalis
can be removed by acid washing to obtain a porous carbon material
with developed pore structure and high specific surface area [212].
Under the synergistic and comprehensive effects of various reactions,
the porosity and specific surface area of carbon materials are greatly
improved, which is beneficial to the material's ion transmission rate,
electrical conductivity, and electrochemical performance. Therefore,
alkali activation is widely used in the field of electrochemistry. Jia et al.
[86] Synthesized a heteroatom-doped porous carbon from cicada
slough by simple KOH activation. The obtained porous carbon has de-
veloped microporosity, high specific surface area of 1676 m2 g−1 and
ultra-high proportion of natural heteroatom functional groups, among
which the heteroatom ratio of nitrogen, oxygen, sulfur, and phosphorus
is as high as 12.06%. The porous carbon with these excellent properties
is well suited for electrochemical applications.
JinNiu et al. [32] demonstrated a sustainable and effective strategy
for synthesizing O, N, S ternary-doped microporous carbon nanosheets
by treating fish skin with KOH. As shown in the Fig. 6, the obtained
carbon nanosheets is only 8 nm and retain a large number of O, N, and S
heteroatoms derived from fish skin. The unique nanostructure also
brings a large number of micro-mesopores and a specific surface area of
1017 m2 g−1 to the material. Kim et al. [130] reported the synthesis of
microporous oxygen and nitrogen doped activated carbon from squid
chitin by KOH activation. The synthesized porous carbon has large
surface area of 1129 m2 g−1 and developed microporous network, and
a nitrogen content closed 4.04% in the form of pyridine/pyrrole-N,
graphite-N and N-oxide groups. In a word, the heteroatom doping and
the porous structure with uniform pore size distribution and good
porosity are beneficial to the performance of the electrodes. With the
help of KOH activation, Yu et al. [132] prepared wax gourd base-
d porous carbons (WGPCs) porous carbon (WGPC) with micro/meso-
porous structure with a specific surface area up to 2919 m2 g−1. Yang
et al. [71] used Tremella to prepare hierarchical porous carbon. and the
obtained product has an ultra-high BET specific surface area of 3760 m2
g−1 and a very high mesopore volume ratio of 72% after KOH activa-
tion. Similarly, NaOH and NaHCO3 are also used in chemical activation
to optimize the structure of the material [72,91,134,136,137]. Endo
et al. [134] prepared a polysaccharide (food residue)-derived activated
carbon with a specific surface area of 2498.6 m2 g−1 and a pore volume
of 1.08 cm3 g−1 using NaOH activation. Cao et al. [127] Used silkworm
feces as precursors to prepare honeycomb porous carbon with high
specific surface area and uniform pore distribution by KOH activation
for high stability lithium ion hybrid electrochemical capacitor (Li-HEC)
electrode materials. The obtained carbon material (PC-SE-700) has a
higher surface area (2826 m2 g−1) and nitrogen doping characteristic as
shown in Fig. 7, which is very beneficial for improving the capacitance
performance and wettability of the electrode.
3.3.2. Metal chloride activation
Zinc chloride(ZnCl2) has a long history in the production of acti-
vated carbon and is still one of the most important activators in che-
mical activation. Researchers at home and abroad have used ZnCl2 as
an activator to prepare many porous carbon materials with excellent
properties [59,60,66,83,150,159–161], but the activation mechanism is
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Chemical Engineering Journal 397 (2020) 125418
still in the exploration stage. Research by Hayashi et al. [213] found
that ZnCl2 has an effect on lignin in the range of 200~600 °C: The
dehydrogenation of ZnCl2 limits the formation of tar, leading to the
aromatization of lignocellulose; And the molecules impregnated inside
the carbon serve as a skeleton. The final carbon polymer is carbonized
and deposited on the skeleton, and the product becomes a porous ac-
tivated carbon with a huge surface area when ZnCl2 is removed by acid
washing. Jain et al. [66] used ZnCl2 as an activator to synthesize me-
sopore-dominant material activated carbon (AC-HBP) with specific
surface area up to 2108 m2 g−1. Under the assisted oxidation of H2O2
and H3PO4, the porous carbon material has a mesoporous specific
surface area of 1423 m2 g−1, which provides an effective strategy for
developing activated carbon with high mesoporous ratio from hydrate
precursor. Rawal's [83] research team applied ZnCl2 to activate porous
carbon SbAS in Bengal flag leaves. The unique porous structure brings
the material a high specific surface area of 2090 m2 g−1 and a suitable
pore volume. Zhou et al. [214] introduced a promising ZnCl2 activation
process. During the activation process, part of the ZnCl2 on the surface
of the biomass (corn straw, bamboo flour, wood chips) is converted into
ZnO and loaded on activated carbon for mercury removal. Finally,
porous carbon with high specific surface area (1475 m2 g−1) and large
pore volume (1.884 m3 g−1) is was prepared via one-step activation. In
recent years, FeCl2 and FeCl3 have also been used for chemical acti-
vation to prepare activated carbon [215–217].
3.3.3. Phosphoric acid activation
The preparation of porous carbon from wood by phosphoric acid
activation has been developed for decades [147,218]. The phosphoric
acid activation method is mainly applicable to wood agricultural and
forestry biomass with cell wall structure of plant fiber raw materials
and its processing residues. Because phosphoric acid activation has
great advantages than ZnCl2 activation in terms of cost, environmental
protection and activated carbon yield, it is widely used in industrial
production. Phosphoric acid activation is similar to the principle of
ZnCl2 activation, but the detailed studies on the mechanism of phos-
phoric acid activation are still scarce. Phosphoric acid activation is
roughly divided into five processes: 1. Promote hydrolysis. Phosphoric
acid can significantly promote the hydrolysis of oligosaccharides such
as cellulose and hemicellulose to form oligosaccharides or mono-
saccharide products [219,220]; 2. Catalytic dehydration. Phosphoric
acid can catalyze the dehydration of oligosaccharides and their de-
gradation products [221,222]; 3. Crosslinking. During the heat treat-
ment, phosphoric acid can undergo significant cross-linking reactions
with biopolymers. This is the main mechanism difference between the
two chemical activation methods of phosphoric acid and zinc chloride,
and it is also an important process for the formation of a developed pore
structure by the phosphoric acid activation method [223]; 4. Promote
aromatization. Graphite-like crystallites are the main structure of plant
fiber biomass, which originates from the aromatization of carbon atoms
in the precursor and the condensation of aromatic rings. Therefore, the
aromatization of carbon atoms is the chemical basis of carbonization. 5.
Making holes. Phosphoric acid molecular aggregates provide a place for
the deposition of nascent carbon atoms produced by the precursor, and
the void left after removing phosphoric acid becomes the pores of ac-
tivated carbon [224]. Molina et al. [225] studied the relationship be-
tween phosphoric acid concentration and phosphorus content in lig-
nocellulose on pore volume change and pore size distribution of peach
core activated carbon. This result provides an important basis for se-
lecting the optimal phosphoric acid activation conditions. Oginni et al.
[138] used Kanlow Switchgrass dealed with pyrolysis as a precursor
material and used one-step H3PO4 activation to prepare biomass-de-
rived activated carbon with high adsorption capacity. According to the
structure, surface chemical properties and microstructure character-
ization results of activated carbon, it has specific surface area of
1373 m2 g−1 and pore volume of 1.45 cm3 g−1. Bahramifar et al. [139]
prepared Persian ironwood-derived activated carbon/metal oxide
Z. Li, et al.
Fig. 7. (a) A schematic illustration of the fabrication process for porous carbon. (b, c) SEM images of PC-SE precursor. (d) SEM image of PC-SE-700. (e–h) EDS
elemental mapping of PC-SE-700. (Reprinted with permission from Reference [131]).
composites with excellent properties by optimizing the ratio of acti-
vator and activation temperature. Phosphoric acid activation sig-
nificantly improved the hollow structure of the material, and the final
product exhibited high specific surface area of 1945 m2 g−1 and pore
volume of 1.59 cm3 g−1. Some researchers have prepared a series of
biomass-derived activated carbon with excellent properties through
phosphoric acid activation [140,141,177].
3.3.4. Microwave-induced/assisted chemical activation
Microwave-induced/assisted activation can not only be applied to
physical activation, but also has obvious optimization effects in terms of
chemical activation. Strong polar activators (KOH, H3PO4, ZnCl2, etc.)
are adsorbed by the capillary channels of the biomass material, and
rapidly heated under the action of microwaves to promote the reaction
between the raw materials and the activator, which ultimately leads to
the production of porous activated carbon. The high heat generated by
the microwave in a short time has a uniform activation effect and
avoids the destruction of the heating device by chemical reagents. Liu
et al. [156] prepared bamboo-based porous carbon with specific surface
area up to 1432 m2 g−1 through a microwave-induced activation pro-
cess, and phosphoric acid was used as an activator in this experiment.
The results show that the microwave-induced activation process is more
efficient and economical than the traditional thermal process, and the
carbon product has a higher yield. Ahmad et al. [226] developed a
method for preparing peanut shell-derived activated carbon (GSAC)
with excellent adsorption properties using microwave-assisted KOH
activation. The synthesized sample GSAC has standard mesoporous
carbon characteristics, and it showed surface area of 733.30 m2 g−1,
pore volume of 0.375 cm3 g−1 and pore size of 2.69 nm, respectively.
Guo et al. [154] prepared an oxygen-rich camellia shell-derived porous
carbon (KMAC) via microwave-assisted KOH activation. The obtained
KMAC has three-dimensional porous structure, large specific surface
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Chemical Engineering Journal 397 (2020) 125418
area (1229 m2 g−1), and abundant oxygen functional groups (C/O ratio
of 1.66). Lam et al. [151] combined microwave pyrolysis and chemical
activation through analysis of pore characteristics and operating para-
meters to provide feasibility for the preparation of activated carbon
with excellent micro-mesoporous structure of high BET surface area and
pore volume. Li et al. [157] used a sawdust as a precursor to synthesize
activated carbon with microwave-assisted phosphoric acid activation.
The product has a high specific surface area of 1509 m2 g−1 and high
mesoporous volume (omesopore fraction is 83.3%). At the same time, it
has been confirmed that drying before microwave activation is an ef-
fective strategy for the preparation of activated carbon with high and
medium porosity. Lei et al. [158] converted cocoa pod shells to valu-
able activated carbon by microwave-assisted activation. The results
showed that the microwave-assisted phosphoric acid activation product
obtained higher yield and better performance than KOH activation, and
its specific surface area and total pore volume were as high as
1237.47 m2 g−1 and 1.11 cm3 g−1, respectively. Villota et al. [227]
studied the effects of activation chemicals and pyrolysis time on the
kinetics of microwave heating and their efficiency relationship with the
technical and economic aspects of the process, which provided us with
an idea for finding the optimal activation scheme. Sun et al. [160] used
response surface methodology to explore and optimize cotton-derived
activated carbon fibers prepared with microwave-assisted ZnCl2 acti-
vation, and studied the effects of microwave power, activation time,
and activator concentration on the performance of the final product.
Microwave-assisted activation technology is a highly efficient activa-
tion method that greatly optimizes the material processing time and
internal structure [70,228].
Template assisted activation. The template method refers to mixing
a specific template agent before carbon source precursor material high
temperature carbonization or carbon source precursor material forma-
tion process to form a mixture of carbon source precursor and template
Z. Li, et al.
agent, so that carbonization occurs in the space network formed by the
template agent and the final carbon material obtains porous structure
after removing the template agent. When choosing the appropriate
template, its topography and surface functionalization are two im-
portant considerations. In general, the topography of the template will
determine the topography of the final product. In addition, by selec-
tively combining certain surface functional groups (such as carboxyl,
phenols, quinones, and lactones) to functionalize the surface of the
template, the structure and morphology of the final product can also be
effectively controlled. Adding template to chemical activation is a
common activation method to purposefully adjust the microstructure of
the obtained activated carbon. The template method has been widely
used in the preparation of activated carbon. Xu et al. [165] proposed an
in-situ hard template strategy combined with sodium hydroxide acti-
vation to prepare hierarchical porous carbon with high surface area
from biomass for supercapacitors. In the experiment, nano-Na2CO3 and
nano-Na3PO4 particles were encapsulated in the lotus seed shell-derived
carbon matrix as an in-situ hard template. The final carbon produced
has developed hierarchical pores, ultra-high specific surface area of
3188 m2 g−1, large pore volume 3.2 cm3 g−1, and abundant O, N, and P
heteroatoms. A product with hierarchical porous structure and ex-
cellent performance is considered to be a promising and efficient
electrode material. Xu et al. [169] proposed a simple and effective
method for preparing nitrogen-doped hierarchical porous carbon by
direct pyrolysis of ethylenediamine tetraacetic acid disodium zinc salt
(C10H12N2O8Na2Zn·xH2O). Pyrolysis of carbon precursors is used di-
rectly for nitrogen sources, hard templates, and activators. Finally, it is
easy to obtain hierarchical porous carbon with large surface area
(1368 m2 g−1) and high nitrogen content (6.71%). Zhang et al. [170]
proposed a new strategy for the synthesis of two-dimensional soft pitch-
derived hierarchical porous carbon (HPC) using oyster shells as tem-
plates and activator precursors as shown in Fig. 8. CaCO3 in the oyster
shell allows the soft pitch to diffuse into the template sufficiently, and
CaO converted from CaCO3 acts as the self-activator. The synthesized
HPC is filled with interconnected pore networks, and the inter-
connected hierarchical porous structure also improves the capacitive
properties of the material. In recent years, research on the synthesis of
carbon materials by the template method has been relatively active, and
it has been able to effectively control the synthesized carbon materials
in terms of pore structure, morphology, and element doping. In addi-
tion, the method of pore formation of precursors by introducing tem-
plates such as inorganic salts and oxides has also been developed
[165–168,171,173,229].
In addition to the above activation methods, there are many effec-
tive and impressive activation methods that are worth exploring. The
single activation method is usually unable to achieve the desired acti-
vation effect. The combination of physical and chemical activation or
the use of unique activators provides broad prospects for material
performance modification. Wei Liu et al. [91] used a sustainable pre-
cursor (cuttlebone) as a raw material and processed the precursor
through direct pyrolysis and optimized air oxidation activation (AOA)
technology to fabricate a unique N, O dual-doped biomass-derived
nanosheet. As shown in Fig. 9, after dual treatments of physical acti-
vation and chemical activation, the resulting product has an extremely
high N-doping amount (13.9%) hierarchically optimized porous struc-
ture. The sample showed high specific surface area of 1489 m2 g−1 and
total pore volume of 1.09 cm3 g−1. This is also the first report to in-
crease the nitrogen doping content of the material by air treatment.
More importantly, the product exhibits excellent power density and
cycle stability when used as sodium-ion battery electrode. Garba et al.
[149] used the borassus aethiopum shell as precursor to prepare the
mesoporous carbon with optimized electrochemical properties by
combining physical and chemical activation. The results show that a
high proportion and coordinated porous structure are particularly cri-
tical for the electrochemical performance of the electrode, this con-
clusion has been confirmed by many experiments results
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Chemical Engineering Journal 397 (2020) 125418
[84,126,147,230]. From a materials perspective, many studies have
shown that BDPC has excellent potential for electrochemical applica-
tions.
Undoubtedly, chemical activation is widely used in materials pro-
cessing and produces a lot of porous carbon products with excellent
properties. Compared to physical activation, chemical activation saves
time and resources and is more productive. In particular, the micro-
wave induced/assisted chemical activation method solves many diffi-
culties in the synthesis of porous carbon and improves the work effi-
ciency [205]. Among the new processes for preparing activated carbon,
it is a simple, environmentally friendly, energy-saving and efficient
activation method. The template-induced auxiliary chemical activation
method opens a new channel for the preparation of biomass-based
hierarchical porous carbon and makes the preparation of materials
more targeted [231]. However, there are still more serious problems
with chemical activation. For example, incomplete removal of residual
activators can cause severe corrosion and environmental pollution to
heating equipment. The volatilization of the activator (such as ZnCl2)
during the activation process will cause serious environmental pollu-
tion and personal injury, as well as a series of problems such as diffi-
culty in recycling, which will indirectly lead to high energy consump-
tion and increased activation costs. Although the template induced/
assisted method does not have hidden safety problems, the template
method has a huge challenge that it is difficult to control the uniformity
of the pores, and the uniform pore making is difficult to achieve in
large-scale preparation. In addition, the industrialization and large-
scale development of microwave-assisted activated carbon also have
limitations [232], so further research is needed to solve this difficulty.
In short, how to realize the large-scale production of porous carbon
using a simple process, safe and environmentally friendly porous
carbon preparation technology, and at the same time ensure the uni-
formity and controllability of the pore structure of the carbon material,
which is a problem urgently needed by those skilled in the art Im-
portant technical issues.
3.4. Hydrothermal carbonization
At present, in addition to high-temperature calcination and pyr-
olysis, the hydrothermal technology can also be applied to the pre-
paration of activated carbon. Among the thermochemical conversion
technologies of biomass, hydrothermal technology also belongs to one
of the main thermochemical methods. The hydrothermal method uses
water as reaction medium, and generates pressure from external
heating to act on the precursor to obtain the hydrothermal carbon
material. As its name implies, the solvothermal method is derived from
the hydrothermal method, which refers to the use of other solutions
instead of water as the reaction medium to achieve better treatment
results. The carbon content of hydrothermal charcoal obtained is not
very high when water is used as the medium, and carbon materials
prepared by solvothermal methods (such as ion heating and molten salt
method have relatively high content of carbon elements. The process of
hydrothermal carbonization technology involves five chemical reaction
steps: hydrolysis, dehydration, decarboxylation, polymerization, and
aromatization [233]. The biomass hydrothermal/solvothermal carbo-
nization process takes place in a closed reaction vessel, and uses an
aqueous solution as the reaction medium. Finally, the biomass is pyr-
olyzed and carbonized by the pressure generated by the heating reac-
tion. Hydrothermal/solvothermal technology does not require harsh
experimental conditions and dry biomass, and has the advantages of
simple operation and high efficiency. Therefore, hydrothermal carbo-
nization of biomass is a promising synthetic method. The hydrothermal
carbonization technology was first proposed in 1913 for converting
cellulose into coal-like materials [234], and then it has been paid new
attention in the field of material synthesis [235]. Hydrothermal car-
bonization technology is more suitable for readily soluble and decom-
posable biomass. Generally, precursors are processed through direct
Z. Li, et al.
Fig. 8. SEM images of (a) CaCO3 spheres and (b) N-doped graded porous carbon NPCS-1 (the inset shows a high-resolution SEM image of CaCO3 spheres), (c, e) TEM
image and (d) HRTEM image of NPCS-1, (g, f) Mapping image (C, N) of NPCS-1. (Reprinted with permission from Reference [170]).
hydrothermal carbonization or continued activation to synthesize de-
rivatives with certain characteristics. Hydrothermal technology can
convert biomass into valuable solid, liquid and gaseous fuels [236].
Biomass-derived products treated by hydrothermal carbonization
technology mainly include two types: one product is an insoluble solid
phase product, such as carbon microspheres with a large number of
hydroxyl functional groups such as carbonyl groups on the surface;
Another product is a soluble organic product, such as furfural com-
pounds, organic acids, aldehydes, and the like. For example, carbohy-
drates can form carbon microsphere particles after hydrothermal car-
bonization, which has very good thermochemical stability and good
thermal and electrical conductivity. In recent years, through the study
of hydrothermal carbonization mechanism [237–241], it has shown
great potential application value in many fields.
Hameed et al. [178] extracted the derived solid product (hydrochar)
from coconut shell by hydrothermal carbonization and further chemi-
cally treated it to produce biomass-derived porous carbon (specific
surface area of 1227 m2 g−1) with high adsorption performance.
Manyala et al. [242] used a simple solvothermal method and two-step
12
Chemical Engineering Journal 397 (2020) 125418
eco-friendly hydrothermal strategy to synthesize Co-Mn layered double
hydroxide nanosheets and Quercus Suber-derived porous carbons with
coordinated morphology and structural properties, respectively. The
assembled hybrid capacitor device exhibits excellent specific energy
and specific power. Zhao et al. [243] prepared a novel tobacco rods-
derived carbon by combining hydrothermal carbonization and po-
tassium hydroxide activation. The sample has high specific surface area
(2115 m2 g−1), hierarchical porous structure, rich heteroatom func-
tional groups, and good electrical conductivity, and can be used as an
ideal electrode material in electrochemistry. Vilches et al. [244] syn-
thesized method olive oil agricultural waste-derived activated carbon
electrode material from the olive oil lungs rich in sulfur and oxygen
functionalities on the surface by solvothermal. Through this method of
carbonization and chemical activation of solid residues, the final ma-
terial obtains excellent texture characteristics (the surface has a large
proportion of sulfur and oxygen heteroatoms, high surface area, and
large micropore and mesopore volumes). Because the traditional sol-gel
method is limited in the preparation of porous carbon by cumbersome
processes, high cost and regulation of pore structure. Liang et al. [245]
Z. Li, et al.
Fig. 9. SEM images of (a) cuttlebone and (b, c) CBCS, (d, e) TEM images of CBCS, (f) HRTEM image of CBCS, (g) EDS elemental mapping of CBCS, (h-j) SEM, TEM and
HRTEM images of CBCS-A3. (Reprinted with permission from Reference [91]).
used corn starch as precursor and borax as structure directing agent to
prepare uniformly dispersed microcarbon spheres through optimized
hydrothermal carbonization process. This method provides a simple
and novel method for the preparation of boron-doped carbon materials.
Appropriately adding templates or additives in the preparation of
porous carbon by the hydrothermal method is also an effective method
for regulating the microstructure of the obtained products. Yang et al.
[179] prepared a composite sample with a specific surface area of
1052 m2 g−1, a reasonable pore size distribution, and self-doped MnO@
fungus-derived carbon by built-in template method and hydrothermal
treatment. The synthesized hierarchical porous carbon microcube
composite is very suitable for electrochemical energy storage as shown
in Fig. 10. Du et al. [180] used yeast cell templates to prepare nitrogen-
doped porous hollow carbon spheres through hydrothermal pre-
carbonization and pyrolytic carbonization. This research innovatively
combines biomass and energy and synthesizes products with excellent
electrochemical properties. Zhang et al. [246] first proposed a simple
and novel self-sacrificial salt template method to optimize the micro-
porous structure of porous carbon monomers synthesized by sol-
vothermal methods, and the specific surface area of the synthesized
porous carbon monomer significantly reached 1131 m2 g−1. It is worth
noting that this method is also suitable for controlling the nanopore
13
Chemical Engineering Journal 397 (2020) 125418
structure of other porous materials. As shown in Fig. 11, Shahrokhian
et al. [247] synthesized hierarchical microspheres of ternary Zn-Co-S
nanosheet decorated biomass derived hydrothermal carbon spheres for
the positive electrode materials of hybrid supercapacitor. The obtained
carbon-based conduct has optimized porous structure and nitrogen
atom modification, and the assembled energy storage device exhibits
high-performance capacitance characteristics and cycle durability. Ad-
vanced asymmetric design and optimized synthesis methods have re-
sulted in very promising high-performance energy storage equipment.
Wu et al. [181] used F127 (ethylene oxide/propylene oxide block co-
polymer) and ionic liquid as soft template to synthesize chitosan-de-
rived nitrogen-doped carbon material with controlled morphology, and
analyzed the optimization effect of different templates on the product.
In addition, benefiting from the advantages of simplicity, economy, and
pollution-free, bagasse [248], pine cones [249], fungus [250], peanut
shell [251], and hemp stem [252] are all used to prepare biomass-de-
rived activated carbon by hydrothermal carbonization technology.
Brahim et al. [236] compiled the chemical composition, calorific value,
and approximate analysis data of different types of biomass and ana-
lyzed the factors that affect the production of biomass-derived hydro-
thermal carbon, such as temperature, residence time, pressure and
catalyst, which provides important parameters and references for the
Z. Li, et al.
Fig. 10. Morphology characterization. (a, b) SEM images of the MnO@C composite, and (c) elemental mapping of Mn, O and C. (d-f) SEM images and (g-f) TEM
images of PCM sample. (Reprinted with permission from Reference [179]).
development of the best material synthesis scheme in the future. In
addition to conventionally increasing the porosity and specific surface
area, the chemical properties of hydrothermal carbon materials can be
adjusted and optimized by adding amino acids, glycoproteins, etc.
[125,253].
In short, hydrothermal treatment technology has been widely used
for decades across the world. It can be seen that the internal structure
and surface chemistry of biomass can be changed by hydrothermal
carbonization reaction to convert low-value waste biomass into en-
vironmental-friendly multifunctional carbon materials, which can be
applied to separation, energy conversion and catalysis field [254]. The
focus of hydrothermal carbon materials is mainly on the controlled
synthesis and uniformity of the materials (microstructure or mor-
phology). It can be seen from the previous work that the direct hy-
drothermal treatment of carbon materials has a large and uneven par-
ticle size, and some products require continued chemical activation for
processing. At present, the preparation of small and dispersed carbon
materials (hydrothermal carbon balls or carbon particles) is still very
difficult. In addition, hydrothermal carbonization technology has a
limited scope of application and can play a better role in the treatment
of fiber and other carbohydrates, which also limits the development and
application of the technology.
In summary, the introduction of pore structure during the pre-
paration of porous carbon depends on the nature of the biomass, the
pyrolysis conditions and the type of activation. Generally, hard nut-like
biomass and insoluble biomass are more suitable for high-temperature
14
Chemical Engineering Journal 397 (2020) 125418
pyrolysis treatment, and water-soluble fibers (carbohydrates) are sui-
table for hydrothermal synthesis. And the structure of the precursor
material, the activation temperature and the ratio of the activator are
the most critical factors affecting the pore distribution and micro-
structure of the resulting product. Reasonable adjustment of the acti-
vation environment (temperature, pressure, etc.) and the concentration
of the activator are important prerequisite for preparing high-perfor-
mance carbon electrode materials. And there are still many unresolved
problems in the activation phase of the material and no synthetic
techniques with comprehensive advantages. First, there are many ac-
tivation mechanisms that have yet to be resolved and need to be ex-
plored. In addition, the pore size of the material cannot be precisely
adjusted during the activation process. Because there are many factors
in the experiment, it is difficult to obtain the ideal product. With the
rapid development of industry and the high requirements for devices
today, there is still a long way to go to further overcome process
technology and processing efficiency to synthesize optimized carbon
materials with ideal properties.
4. Synthesis and application of biomass-derived carbon in
electrochemistry
Graphene [44] is a two-dimensional carbon nanomaterial with hive
lattice characteristics, and belongs typical representative in the field of
carbon materials [255]. Graphene has demonstrated strong application
potential due to ultrahigh specific surface area of 2630 m2 g−1 [256],
Z. Li, et al.
Fig. 11. (a–c) SEM images of Zn-Co-S decorated HTCSs at different magnifications, (d, e) the corresponding EDS maps of the elements C, O, S, Co, Zn, and Ni.
(Reprinted with permission from Reference [247]).
excellent electron mobility, good electrical conductivity, stable struc-
ture, and controllable chemical properties. Based on various out-
standing performances, in recent years, it has become the focus of re-
search in the fields of chemistry, materials science, condensed matter
physics and electronics [45,257]. There are many different types of
carbon sources in nature. After processing them, derived carbons with
excellent properties and various shapes (sheet, spheres, block, etc.) and
structures (0-dimensional, one-dimensional, two-dimensional, three-
dimensional) can be synthesized. On the one hand, the high degree of
graphitization can improve the conductivity of the material; on the
other hand, the pore structure is also conducive to the insertion and
extraction of energy storage ions on the surface of the material. Based
on the above requirements, biomass is one of the best carbon source
choices. Using biomass as a precursor material can not only achieve
waste recycling, but also an optimal way to prepare high-performance
and low-cost carbon electrode materials. However, the performance of
untreated raw materials is very poor, and the electrochemical perfor-
mance of the products after carbonization and activation treatment can
be significantly improved and enhanced. In general, the appropriate
specific surface area, balanced pore distribution, favorable heteroatom
functional groups, and the type of electrolyte will affect the con-
ductivity and ion diffusion rate of the carbon electrode in the electro-
lyte and cause differences in electrochemical performance of carbon
materials between different energy storage devices [77]. The following
summarizes the latest research progress of biomass-derived porous
carbon materials prepared by activation in recent years, more detailed
parameters (such as activator, specific surface area, pore size distribu-
tion, element content, yield, etc.) can be seen in Table 3.
From the table we can intuitively find that there are great differ-
ences in the porous carbon prepared by different activation methods.
Moreover, the effect of KOH activation is particularly significant. The
specific surface area of the obtained porous carbon is as high as
3800 m2 g−1 [71], which is much higher than the graphene's 2630 m2
15
Chemical Engineering Journal 397 (2020) 125418
g−1. Many heteroatoms in the precursor were retained after the acti-
vation treatment. It is worth noting that heteroatom doping is also an
effective method to improve the electrochemical performance of elec-
trode materials. And heteroatom doping of N, P and S is widely used to
change the capacitance characteristics [88]. Atomic doping provides
pseudo-capacitance for the material by increasing the charge mobility,
the wettability of the carbon surface and the surface redox reaction in
the electrolyte solution [261]. Jia et al. [86] used a simple KOH acti-
vation method to prepare porous carbon materials with graded pores.
Excellent electrical double layer capacitance performance is shown in
electrochemical systems attributed to good porosity, a high ratio de-
rived heteroatom functional groups of 12.06% and a high specific
surface area of 1676 m2 g−1. In summary, reasonable specific surface
area, well-balanced pore size distribution, appropriate heteroatom
functional groups are critical to improving the performance of material
capacitive storage [77]. Electrochemical performance testing is the
most effective means of verifying material quality, which is directly
related to practical applications. Testing and analysis are performed
primarily in three-electrode systems and two-electrode systems. There
are many methods for testing electrochemical performance of capaci-
tors, such as cycling voltammetry (CV), galvanostatic charge-discharge
(GCD) and electrochemical impedance spectroscopy (EIS) [1].
CV is used to characterize the rate properties of materials multi-
cycle capacitance retention and long-life cycle stability of carbon ma-
terials can be detected by GCD. EIS, also known as AC impedance
spectroscopy, it is used to infer the equivalent circuit diagram for
porous carbon electrode testing. The Nyqusit curve is obtained by EIS,
which represents the impedance and capacitance values of the electrode
material at different test frequencies. CV is the most commonly used
test method for studying the electrochemical properties of electrode
materials. The reversibility, peak current and peak potential of the
electrode during charge and discharge can be obtained intuitively from
CV, which is crucial to judge whether the electrode has ideal
Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Table 3
Structural characteristics, element distribution and other related parameters of BDPC prepared using different activators.
Raw materials Agent SBET Smicro Smeso Vtotal Vmicro Vmeso dAve. (nm) Composition (%) Field (%) Ref.
(m2/g) (m2/g) (m2/g) (cm3/g) (cm3/g) (cm3/g)
C O N S P

Cuttlebones KOH 1489 1.09 0.27 0.82 80.6 10.5 8.9 1 [91]
Shiitake mushroom KOH 1788 1.12 0.74 0.38 2.5 70.8 27.9 1.3 15 [72]
Pomelo peel KHCO3 2726 1411 1315 1.73 0.83 0.9 0.89 83.84 15.34 0.7 0.12 [79]
Corn silk KOH 2550 0.95 1.95 89.37 9.14 1.49 [93]
Cotton KOH 2307 1.18 0.77 0.41 92.6 7.4 [61]
Cotton Zn(NO)3·6H2O 2183 586 1597 1.83 0.09 1.74 1.2 90.08 7.95 1.97 4.9 [80]
Goat hair KOH 2042 0.31 86.47 7.51 6.02 [92]
Sorghum vinasse KOH 3047 1.35 0.62 0.73 1.9 [126]
Cotton-shirt Air 617 0.14 3.8 82.8 9 8.2 [65]
Fish skin KOH 1017 939 78 0.422 75.55 14.02 8.18 2.25 [32]
Cicada slough KOH 1767 0.94 0.663 0.277 2.9 87.94 8.94 2.72 0.13 0.27 [86]
Corn stalk core KOH 2139 1370 769 1.16 0.73 0.43 [230]
Stiff silkworm KOH 2523 1.37 1.09 0.28 2.5 91.4 5.1 3.5 [77]
Soybean dreg KOH 1837 1.05 0.71 0.34 87.01 11.41 1.58 4.33 [69]
Teak wood ZnCl2 2108 1423 685 2.2 0.17 2.03 39 [66]
Corncobs KOH 3054 1.5 0.738 0.763 89.45 9.49 0.3 [258]
Tree bark KOH 1018 0.67 0.43 0.23 2.59 93.97 2.82 [113]
Beancurd CH3COOK 1735 1605 130 1.1 0.82 0.28 2.53 85.7 5.2 1.33 [122]
Saccharumbengalense ZnCl2 2090 1800 290 0.33 0.281 0.049 2.05 95.07 4.8 [83]
Cornstalk KOH 1736 0.92 0.59 0.33 90.9 9.1 [129]
Jujun grass KOH 2532 1203 1.601 1.077 0.524 90.17 9.3 0.53 [127]
Soybean KOH 2251 1.209 2.15 89.93 8.38 1.69 [64]
Elm samara KOH 1947 1.33 0.8 0.53 2.19 94.45 4.9 0.65 [128]
Coconut shell Self-activation 1194 0.528 0.446 0.071 2.02 13.8 [115]
Peanut shell KOH 2396 1548 848 1.31 0.845 0.464 1.71 85.91 13.5 0.58 [89]
Corn stover Microwave pyrolysis 1432 0.762 0.615 0.147 2.13 83.16 16.46 0.38 [73]
Eragrostic ZnCl2 1250 323.8 0.7296 0.1423 66.1 25.45 1.95 [161]
Palm shell CO2 574 514 60 0.244 0.198 0.046 1.7 [70]
Tremella KOH 3760 1212 1004 2.15 0.6 1.55 84 10 1.4 [71]
Lotus seed shell NaOH 3188 3.2 2.37 0.83 3 79.45 14.54 3.1 2.92 [165]
The squid gladius KOH 1129 1081 48.4 0.14 1.28 80.9 14.8 4.3 33 [130]
Silkworm KOH 2826 1.54 0.799 0.732 82.86 14.85 2.29 13.9 [131]
Wax gourd KOH 2919 2449 470 1.84 1.48 0.36 2.5 80.8 17.9 1.0 0.3 2.91 [132]
Alginate ZnCl2 2589 1353 1236 1.875 4.329 [166]
Camellia oleifera shell KOH 1553 1.33 2.7 57.37 34.55 [154]
Dopamine CaCO3 1984 1.29 0.94 0.34 88.3 6.36 5.34 [170]
Oyster shell CaCO3 1258 876 382 0.79 92.51 2.16 1.06 57.7 [171]
Soybean meal K2CO3 2580 1.19 0.21 0.98 13 [172]
Petroleum pitch KOH 1922 1782 140 1.21 0.83 0.38 2.51 86.49 13.51 [174]
Hazelnut shells Mg(CH3COO)2·4H2O 552 0.3 79.8 13.5 0.5 55 [182]
Peanut shell KOH 1994 1.1 0.76 0.34 2 92.76 6.8 0.44 [90]
Yeast cells Glucose 912 671 229 0.57 78.14 22.39 3.4 [180]
Pomelo peel (NH4)2HPO4 808 442 366 0.438 0.237 0.201 2.16 25 [259]
Wheat straw KOH 2115 1.42 0.88 0.54 [260]
Bagasse wastes KOH 2296 1658 638 1.34 2.63 [248]
Chitosan KHCO3 879 0.447 0.271 0.176 86.5 8.2 5.3 [104]

capacitance characteristics. In addition to this, the specific capacitance I Δt

C=
of the electrodes at different scan rates is obtained from CV by further mΔV
data analysis and calculation, thereby obtaining some basic capacitive For the two-electrode system, the specific capacitances (C, F g−1),
properties of the electrode material. The calculation formula of the the power density (P, W kg−1) and energy density (E, Wh kg−1) were
capacitor is as follows [262]: calculated on the basis of charge/discharge profiles through the fol-
lowing formula [91]:
∫ IdV
C= 4I Δt
vmΔV C=
mΔV
where C (F g−1) is the specific capacitance of the electrode, I (A) is the
2 Vb
response current, ΔV (V) is the magnitude of the potential window, ν (V C=
mv (Vb − Va)
∫V a
IdV
s−1) is the scan rate, m (g) is the mass of the working electrode active
material. 1
E= C (ΔV )2
The GCD curve obtained by the cross-flow charge-discharge test can 8
be used to calculate the specific capacity change of the electrode, as
E
well as other related electrochemical properties such as the rate char- P=
acteristics of the electrode, the energy density, the power density and so Δt
forth, the cycle stability can also be studied simultaneously. where C (F g−1) is the specific capacitance of the electrode; I (A) is the
For the three-electrode system, the specific capacitance (C) derived discharge current; Vb and Va (V) are the high and low potential limit of
from GCD tests can be calculated using the following equation [1]: the CV tests; Δt (s) is the discharge time; ΔV (V) is the potential window;
v (V s−1) is the scan rate; m (mg) is the mass of the active materials in

16
 Table 4
BDPCs for electrochemical energy storage based on different precursors in recent years.
Z. Li, et al.

Raw materials Agent SBET Vtotal Specific Electrolyte Current Cell configuration Maximum Maximum Electrolyte Capacitor Type Ref
(m2/g) (cm3/g) capacity (/g) density (A/ specific energy specific power (Symmetric/
g) (Wh/kg) (W/kg) Asymmetric)

Onion KOH 1915 1.04 180 6 M KOH 0.5 A/g 2E [68]

Beancurd CH3COOK 1735 1.1 315 1 M H2SO4 0.1 A/g 2E [122]
403 1 M H2SO4 0.1 A/g 3E
245 6 M KOH 0.1 A/g 2E
336 6 M KOH 0.1 A/g 3E
Biocompatible graphene Template (Egg 1020 534 6 M KOH 1 A/g 3E [263]
foams albumen)
Camellia oleifera shell KOH 1533 1.33 315 2 M H2SO4 0.5 A/g 3E [154]
251 6 M KOH 0.5 A/g 3E
Cotton KOH 2307 1.18 283 6 M KOH 1 A/g 3E [61]
Soybean KOH 2251 1.21 248 1 M H2SO4 0.1 A/g 2E [64]
White sugar KOH 713 0.445 242 1 M Na2SO4 1 A/g 2E 19 (750 W/kg) 43,900 (4.69Wh/ 1 M Na2SO4 S [34]
kg)
Shiitake mushroom KHCO3 1788 1.12 354 1 M H2SO4 1 A/g 3E 55.2 (1250 W/kg) 62,500 (43.3Wh/ 1 M TEABF4/PC S [72]
kg)
Corn silk KOH 2550 0.95 127 1 M NaClO4 0.3 A/g 2E 109 (1600 W/kg) 12,160 (43.5Wh/ 1 M NaClO4 A [93]
kg)
Cotton Zn(NO)3·6H2O 2183 1.83 365 6 M KOH 0.5 A/g 3E 16.1 (200 W/kg) 3700 (5.5Wh/kg) 6 M KOH S [80]
Goat hair KOH 2042 0.31 298 1 M NaClO4 0.04 A/g 2E 79 (95 W/kg) 0.75 M NaPF6 A [92]
sorghum vinasse KOH 3047 1.35 329 2 M KOH 1 A/g 3E 49.5 (737 W/kg) 10,800 (22.7Wh/ 1 M TEABF4/AN S [126]
kg)
Fish skin KOH 1017 0.422 438 6 M KOH 0.1 A/g 3E 12.5 Wh/L 9670 W/L (3.1 6 M KOH S [32]
(24 W/L) Wh/L)

17
Cicada slough KOH 1767 0.94 355 6 M KOH 1 A/g 3E 9 (227 W/kg) 4000 (4Wh/kg) 6 M KOH S [86]
274 6 M KOH 1 A/g 2E
Bamboo KOH 2221 1.238 293 3 M KOH 0.5 A/g 3E 10.9 (63 W/kg) 3200 (9Wh/kg) 3 M KOH S [116]
Corn stalk core KOH 2139 1.16 317 6 M KOH 1 m V/s 2E 6.8 (250 W/kg) 28,340 (4.5Wh/ 6 M KOH S [230]
kg)
Stiff silkworm KOH 2523 1.37 304 6 M KOH 1 A/g 3E 7.9 (234 W/kg) 3500 (3.1Wh/kg) 6 M KOH S [77]
235 6 M KOH 1 A/g 2E
Soybean dreg KOH 1837 1.05 321 6 M KOH 1 A/g 3E 22.1 (875 W/kg) 4377 (11.78Wh/ 1 M EMIMBF4 S [69]
kg)
Teak wood ZnCl2 2108 2.2 131 1 M LiPF6 0.1 A/g 2E 111 (150 W/kg) 7800 (8Wh/kg) 1 M LiPF6 A [66]
Jujun grass KOH 2532 1.601 335 6 M KOH 1 A/g 3E 72.7 (1204 W/kg) 12,500 (38.8Wh/ 6 M KOH S [127]
336 6 M KOH 1 A/g 2E kg)
Amygdaluspedunculata shell KOH 2059 358 1 M Na2SO4 0.5 A/g 2E 49.7 (248 W/kg) 16,400 (27.8Wh/ 1 M Na2SO4 S [63]
kg)
Elm samara KOH 1947 1.33 470 6 M KOH 1 A/g 3E 43 (500 W/kg) 20,000 (22.2Wh/ EMIMBF4 S [128]
370 6 M KOH 1 A/g 2E kg)
Cornstalk KOH 1736 0.92 301 6 M KOH 2 A/g 3E 20.2 (398 W/kg) 17,600 (7Wh/kg) 1 M Na2SO4 S [129]
231 1 M Na2SO4 0.5 A/g
Peanut shell KOH/Air 2396 1.31 213 1 M NaClO4 0.1 A/g 2E 201 (286 W/kg) 16,500 (50Wh/ 1 M NaClO4 A [89]
kg)
Palm shell CO2 574 0.244 362 1 M H2SO4 2 mV/s 2E 14.29 (259 W/kg) 1 M H2SO4 S [70]
Quercus Suber K2CO3 1056 0.63 65 1 M KOH 0.5 A/g 2E 20.3 (435 W/kg) 3000 (11.2Wh/ 1 M KOH A [242]
kg)
Tobacco rods KOH 2115 1.22 286 1 M KOH 0.5 A/g 3E 31.3 (650 W/kg) 11,800 (10Wh/ 1 M CH3(C2H5)3NBF4/ S [243]
kg) AN
Hemp stem KOH 2801 1.7 160 1 M KOH 1 A/g 2E 19.8 (380 W/kg) 21,000 (9.2Wh/ 1 M LiPF6 A [252]
kg)
bagasse wastes KOH 2296 1.4 320 1 M Na2SO4 0.5 A/g 3E 20 (182 W/kg) 54,000 1 M Na2SO4 S [248]
45 6 M KOH 0.2 A/g 2E (10.65Wh/kg)
(continued on next page)
Chemical Engineering Journal 397 (2020) 125418
 Table 4 (continued)

Raw materials Agent SBET Vtotal Specific Electrolyte Current Cell configuration Maximum Maximum Electrolyte Capacitor Type Ref
Z. Li, et al.

(m2/g) (cm3/g) capacity (/g) density (A/ specific energy specific power (Symmetric/
g) (Wh/kg) (W/kg) Asymmetric)

Lycopodium clavatum CO2 3053 1.43 305 1 M TEABF4/ 0.1 A/g 2E 56 (60 W/kg) 17,000 (47.7Wh/ 1 M TEABF4/AN S [191]
AN kg)
lotus seed shell NaOH 3188 3.2 286 6 M KOH 0.5 A/g 3E 11.8 (30 W/kg) 102,000 3 M H2SO4 S [165]
(1.02Wh/kg)
Squid gladius KOH 1129 0.14 204 1 M H2SO4 0.5 A/g 3E 4.53 (199 W/kg) 9939 (1.9Wh/kg) 1 M H2SO4 S [130]
Silkworm KOH 2826 1.54 378 6 M KOH 0.5 A/g 3E 242.2 (325.3 W/ 6473 (186.5Wh/ 1 M LIPF6 A [131]
330 1 M H2SO4 3E kg) kg)
Wax gourd KOH 2919 1.84 341 6 M KOH 0.5 A/g 3E 19.2 (448.5 W/ 8625 (16.3Wh/ 0.5 M Na2SO4 S [132]
172 0.5 M Na2SO4 0.5 A/g 2E kg) kg)
Alginate ZnCl2 2589 1.875 316 6 M KOH 0.5 A/g 3E 16.1 (250 W/kg) 2500 (5.8Wh/kg) 6 M KOH S [166]
Dopamine CaCO3 1984 1.29 270 6 M KOH 0.5 A/g 3E 14.4 (427 W/kg) 8500 (7.8Wh/kg) 5 M LiTFSI S [170]
173 2E
Soybean meal K2CO3 2000 0.81 160 1 M H2SO4 0.2 A/g 2E 50 (150 W/kg) 23,000 (20Wh/ EMImTFSI/AN S [172]
Glucose 155 1 M Li2SO4 kg)
Petroleum pitch KOH 1922 1.21 267 BMIMPF6 0.05 A/g 2E 148.3 (204.2 W/ 10,000 (6.3Wh/ BMIMPF6 6 M KOH S [174]
293 6 M KOH 0.05 A/g kg) kg)
10 (25.6 W/kg)
Hazelnut shells Mg(CH3COO)2·4H2O 552 0.3 323 1 M H2SO4 1 A/g 3E 11.1 (156 W/kg) 3686 (6.2Wh/kg) 1 M Na2SO4 S [182]
Peanut shell KOH 1994 1.1 160 1 M Na2SO4 0.2 A/g 3E 169.4 (120.5 W/ 1865 (30Wh/kg) 1 M Na2SO4 A [90]
kg)
Yeast cells Glucose 912 0.57 255 1 M Na2SO4 1 A/g 3E 41 (500 W/kg) 7901 (23Wh/kg) 1 M Na2SO4 A [180]
Bagasse ZnCl2 1506 0.88 118 1 M LIPF6 0.25 A/g 2E 116.9 (500 W/kg) 10,000 (87.7Wh/ 1 M LIPF6 S [264]
kg)
Pomelo peel (NH4)2HPO4 808 0.438 240 2 M KOH 0.5 A/g 3E 11.7 (160 W/kg) 2500 (7Wh/kg) M Na2SO4 S [259]

18
Wheat straw KOH 2115 1.42 294 3 M KOH 1 A/g 3E 11 (260 W/kg) 4200 (9.6Wh/kg) 3 M KOH S [260]
Bagasse wastes KOH 2296 1.34 320 6 M KOH 0.5 A/g 3E 20 (182 W/kg) 54,000 (10.6Wh/ 1 M Na2SO4 S [248]
kg)
Chitosan KHCO3 879 0.447 307.8 1 M ZnSO4 0.1 A/g 2E 191 (58 W/kg) 3633 (92.5Wh/ 1 M ZnSO4 A [104]
kg)
Chemical Engineering Journal 397 (2020) 125418
Z. Li, et al.
the electrode; E (Wh kg−1) is the average energy density; P (W kg−1) is
the average power density. Table 4 summarizes biomass-derived carbon
for electrochemical energy storage prepared by different activation
methods and precursors in recent years. It can be seen from the table
that the carbon electrodes obtained by different raw materials and ac-
tivation methods also have great differences in performance.
Lin et al. [68] synthesized the porous carbon with angstrom-sized
pores by KOH activation using onions as precursors. The obtained
porous carbon has high specific surface area of 1915 m2 g−1 and pore
volume of 1.04 cm3 g−1. And the assembled symmetrical super-
capacitor showed specific capacitance of 180F g−1 at 0.5 A g−1 in 6 M
KOH. Using non-toxic and mild CH3COOK as the activator, Zhou et al.
[122] prepared cost-effective, high-performance Beancurd-derived ni-
trogen-doped hierarchical porous carbon (HPC) by an efficient two-step
chemical activation method. The optimized carbon product has high
BET specific surface area (1735 m2 g−1) and nitrogen content (1.33 at.
%). The two-electrode electrochemical test was performed in H2SO4
and KOH aqueous electrolytes. At a current density of 0.1 A g−1, the
material still has ultra-high specific capacitances of 315 and 245F g−1,
respectively. And supercapacitors exhibit excellent capacitance char-
acteristics and cycle stability (a retention rate of 93.5% after 10,000
cycles at a current density of 1 A g−1). Liu et al. [263] used egg al-
bumen as template material to mix with graphite oxide and synthesize
biocompatible graphene foams (GFs) rich in heteroatoms. Although the
specific surface area of the material was only 1020 m2 g−1, GFs had a
relatively thin graphene skeleton, a honeycomb interconnected porous
structure and concentrated mesopore distribution thanks to the egg
albumen template, which provided a strong basis for the excellent
structure and performance. The sample GF-800 exhibited ultrahigh
specific capacitance up to 534F g−1 at 1 A g−1 and 308F g−1 at 100 A
g−1. In addition, the sample showed outstanding long-term stability
that the capacitance retention is up to 96.1% at high current density of
10 A g−1 after 10,000 cycles. In short, this simple and scalable strategy
reveals the huge application potential of carbon materials. Guo et al.
[154] converted low-value biomass (camellia oleifera shell) into porous
carbon materials with economic and practical value for energy storage
electrodes through fast and convenient microwave-assisted chemical
activation. The obtained oxygen-enriched porous carbon (KMAC) has
three-dimensional porous structure, high surface area (1229 m2 g−1),
and abundant oxygen functional groups (oxygen content up to 33.55%)
which are favorable for electrochemical characteristics. Thanks to
oxygen functional groups, the prepared electrode materials have ideal
capacitance characteristics in 2 M H2SO4 (315F g−1 at 0.5 A g−1) and
6 M KOH (251F g−1 at 0.5 A g−1) electrolytes. Based on air oxidation
activation (AOA) technique, Liu et al. [91] fabricated a unique N, O
dual-doped biocarbon nanosheet with hierarchical porosity by direct
pyrolysis of low-cost cuttlebones. The results show that the N-doped
amount of the sample processed by AOA increased from 7.5% to 13.9%
as shown in Fig. 9. The sample also has high specific surface area
(1489 m2 g−1) and large pore volume (1.09 cm3 g−1). This is also the
first example of increasing the nitrogen doping content of carbon by air
treatment. The assembled Na + capacitors exhibit high energy-power
density and good cycle stability. As shown in Fig. 12, the electrode
system achieves excellent Na + storage capacity of 640 mA h g−1
compared to Li+-storage in carbon materials. After 10,000 GCDs at a
high current density of 10 A g−1, the capacitance retention rate exceeds
90%. Lei et al. [61] reported the synthesis of low-cost cotton-derived
flexible carbon fiber aerogels for supercapacitors. Through carboniza-
tion and KOH chemical activation, the obtained aerogel has a twisted
tubular structure, an ultra-high specific surface area of 2436 m2 g−1
and a high proportion of micro-mesopore distribution, which provides
sufficient channels for ion transmission inside the electrode material. At
current density of 1 A g−1, the aCF-6 electrode shows high specific
capacitance of 283F g−1 in a 6 M KOH aqueous electrolyte. Even at 100
A g−l large current density, the electrode still has an excellent capaci-
tance retention of 79.1%. In addition, the capacitance of the aCF-6
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Chemical Engineering Journal 397 (2020) 125418
electrode shows only 3% attenuation after continuous 20,000 GCD
cycles at 4 A g−1 due to the unique structure advantage. In summary,
the aCF-6 electrode derived from biomass has excellent cyclic stability
and long-period constant ion and electron transport characteristics.
Yang et al. [64] successfully prepared porous carbon rich in O, N het-
eroatoms for electrode materials of electrochemical capacitors using
soybean as a precursor. By conveniently adjusting the mass ratio of
activator (KOH) to the carbonized product, the synthesized porous
carbon AC-4 has a maximum specific surface area of 2251 m2 g−1, and
a pore volume of 1.21 cm3 g−1. The unique structure, developed graded
porosity and rich heteroatoms (O and N) lead to its high specific ca-
pacitance, good rate capacity and excellent cycle stability. The elec-
trode showed the maximum capacitance value of 248F g−1 at 0.1 A
g−1. Even at a current density of 20 A g−1, the capacity retention rate
remains at 56.7%, and after 10,000 cycles, the capacity retention rate is
as high as 98.75%. This porous carbon material prepared by a low-cost
method shows excellent potential in energy conversion and storage
devices. Manyala et al. [34] proposed a simple two-step synthesis route
to produce cost-effective and high-porosity carbon material by acidic
dehydration and activation of white sugar. Although the prepared
sample ASC 400 does not have an excellent specific surface area
(713 m2 g−1), it has better electrochemical performance than other
samples. As shown in Fig. 13, the assembled symmetrical super-
capacitor showed maximum specific capacitance of 242.67F g−1 at 1 A
g−1 in 1 M Na2SO4 electrolyte. Meanwhile, the corresponding energy
density and power density are 19 Wh kg−1 and 750 W kg−1, respec-
tively. Even at power density of 43900 W kg−1, the energy density
remains at 4.69 Wh kg−1. After 10,000 GCD cycles at specific current of
3 A g−1, the electrode has no significant capacitance loss (only 11.8%).
Thanks to its good power efficiency, the device can be used as an es-
tablished material for high-power supercapacitor applications.
Yuan et al. [72] used a low-cost KHCO3 activation strategy to pro-
duce a highly economical, scalable, eco-friendly porous biomass (shii-
take)-derived carbon. In this experiment, sample CKHCO3 synthesized
with KHCO3 as an activator has better electrochemical behavior than
KOH. The optimized mushroom-derived carbon has a pore volume with
surface area of 1788.1 m2 g−1, pore volume of 1.12 cm3 g−1, and high
content of N (1.3 at.%). In the three-electrode test, the C electrode
exhibited a satisfactory specific capacitance of 354.8F g−1 at a current
density of 1.0 A g−1 in 1 M H2SO4. Thanks to the large surface area,
optimized pore size and capacitive contribution of heteroatoms (N and
O), CKHCO3 // CKHCO3 symmetrical capacitor has the largest energy
density of 55.2 Wh kg−1 and power density of 62.5 kW kg−1 in 1
MTEABF4/PC electrolyte. In addition, the device also has excellent
cycle stability and Na+ storage characteristics, showing great potential
in energy-related practical applications and commercial-level biomass-
derived porous carbon. Nallathamby et al. [93] used KOH to activate
corn silk derived carbon (CSC) as suitable electrode material for sodium
ion storage applications. Corn silks are composed of carbohydrates,
proteins and vitamins. Nitrogen-doped (1.5%) graded porous carbon
can be obtained through the activation of corn shreds. The obtained
product has a large specific surface area (2550 m2 g−1) and a con-
siderable pore volume (0.95 cm3 g−1), which can be used to make
symmetrical batteries and capacitors. The practical feasibility of its
application in energy storage systems has been proven in manufactured
Na+ batteries. Under different current density conditions, the max-
imum specific energy density and maximum specific power density of
the symmetric coin cell system were 109 Wh kg−1 (0.324 A g−1) and
12.16 kW kg−1 (2.5 A g−1). This achievement provides a new way for
the preparation of reusable biological waste-derived activated carbon
for the development of sodium ion capacitors. Chen et al. [80] suc-
cessfully produced N-doped porous carbon fiber aerogel (N-CFA) by a
one-pot method using raw cotton as the fiber template. Thanks to the
introduction of ZIF-8, the synthesized N-CFA porous material has high
surface area (2183 m2 g−1), large pore volume (1.83 cm3 g−1), rich
pore structure and high N content (1.97%). Carbon fiber aerogels with
Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 12. Electrochemical characterization of various NIC devices. (A) Schematic diagram of charge storage mechanism for the assembled CBCS//CBC-C NIC; (b)
cyclic voltammetry (CV) curves of CBCS-A3//CBCS-C NICs with various mass ratios and CBCS//CBC-C NIC devices; (c) CV curves of CBCS-A3//CBCS-C NICs at
different scan ratios; (d) galvanostatic profiles of CBCS-A3//CBC-C NIC device; (e) Ragone plots of CBCS-A3//CBC-C NIC and CBCS//CBC-C NIC, energy-power
density performance comparison with state-of-the-art reported energy-storage systems in literature, (f) cycling performance of CBCS-A3//CBC-C NIC. (Reprinted with
permission from Reference [91]).

these unique structures are promising and ideal electrode materials for
electrochemical capacitors. In addition, the obtained N-CFA also has
elasticity and good flexibility, which are conducive to providing fast
charge discharge rate and excellent rate performance. It can be clearly
seen from picture 13 that the N-CFA electrode has high specific capacity
of 365F g−1 at 0.5 A g−1 in 6 M KOH. N-CFA shows an excellent rate
capability of 65.8% in the range of 0.5 A g−1 to 100 A g−1. After
10,000 cycles of charge-discharge at a current density of 5 A g−1, the
electrode has good stability and a high capacitance retention rate of
93.6%. The assembled symmetrical electrode system also has an op-
timal energy density of 16.1 Wh kg−1 and a power density of
3700 W kg−1, which can be widely used in super capacitors, lithium ion
batteries, sensors and other fields. Nithya et al. [92] synthesized a goat
wool-derived porous carbon with specific surface area of up to 2042 m2
g−1 by KOH activation for the cathode material of Na+ hybrid su-
percapacitors. The hybrid supercapacitor assembled from the obtained
material (cathode) and MoO2@rGO composite material (anode) showed
good capacitance characteristics and cycle stability. The electrodes
show excellent electrochemical performance even in a half-cell con-
figuration. The composed sodium ion hybrid capacitor device has an
energy density of 79 W h kg−1 and a power density of 95 W kg−1 at a
current density of 0.04 A g−1 in 0.75 M NaPF6 electrolyte. And the
electrode still maintained 78% of its initial capacitance after 1000 cy-
cles at 0.07 A g−1. The high surface area of porous carbon provides a
feasible channel for ion adsorption and desorption, thereby sig-
nificantly improving the electrochemical performance of the cathode.
This combination of hybrid supercapacitors provides a strong founda-
tion for sodium ion storage applications and is of great significance for
achieving large-scale applications of high energy and power density
energy storage devices. Li et al. [126] synthesized highly porous carbon
material with graphene nanosheet microstructures from biomass waste
(sorghum vinasse) by a simple chemical activation method. The syn-
thesized porous carbon HPC has high specific surface area of about
3000 m2 g−1 and pore volume of 1.35 cm3 g−1. The unique graphene
nanosheet structure inside the sample leads to the existence of a large
number of micropores and mesopores, thereby providing a large
number of capacitive reaction sites. The obtained sample HPC exhibited
significant electrochemical characteristics in 2 M KOH and 1 M H2SO4
electrolytes, and the specific capacities were 329F g−1 and 311F g−1 at
1.0 A g−1, respectively. The assembled symmetrical supercapacitor has

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Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 13. (a) CV curves at different scan rates, (b) CD curves at various specific currents, (c) Specific capacitance changes at different current densities, (d) Ragone
plots, and (e) Cyclic stability test of symmetry ASC 400 device, (f) Ragone chart of the device, with some other sugar-based material electrodes recently reported from
the literature. (Reprinted with permission from Reference [34]).

an optimal energy density of 49.5 Wh kg−1 and a power density of
10.8 kW kg−1 in 1 M TEABF4/AN electrolyte, which is superior to many
wood porous carbon electrodes. And this simple and efficient carbon
material extraction strategy is very promising in the field of energy
storage (Fig. 14).
Wang et al. [32] synthesized ternary doped hierarchical porous
carbon nanosheets (MPCNS) by KOH activation using fish skin as a
precursor as shown in Fig. 6. It is worth noting that the high specific
surface area (1017 m2 g−1) of the pore structure often leads to a
decrease in the density of porous carbon electrode materials, which can
cause the problem of poor volume performance. It can be clearly seen
that the nanosheet structure and the existence of a large number of
heteroatoms inside the material. The large number of heteroatoms on
the electrode surface not only effectively improves the hydrophilicity,
but also provides additional pseudo-capacitance [265]. The contact
between the electrode material and the electrolyte ions has been sig-
nificantly improved because the highly conductive porous carbon
structure provides a large specific surface area and rich capacitive

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Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 14. Specific capacitances at different current densities (a) and GCD curves of N-CFA, PC, and CFA at 1 A g−1, respectively (inset). Nyquist plots (b) and their
corresponding high-frequency ranges (inset). Cycle stability of the electrode at 5.0 A g−1 (c) of N-CFA and Ragone plots compared with the reported biomass-derived
carbons (d). Schematic illustration of the carbon fiber modified by ZIF-8 for supercapacitors (e). (Reprinted with permission from Reference [80]).

reaction sites, which ultimately significantly improves the electro-
chemical performance of the material [266]. The MPCNS exhibited
integrated high gravimetric capacitance of 438F g−1 and volumetric
performance of 447F cm−3 at the current density of 0.1 A g−1 as
electrode for SCs in aqueous electrolyte. In addition, the assembled
symmetrical supercapacitor has a gravimetric energy density of 12.5
Wh L−1 (24 W L−1) and a gravimetric power density of 9670 W L−1
(3.1 Wh L−1) in 6 M KOH. This provides an advantageous strategy for
preparing electrodes for use as supercapacitors with high gravimetric
and volume comprehensive performance in aqueous electrolytes. Sun
et al. [86] Synthesized heteroatom-rich cicada-derived porous carbon
(PCCS) through a simple chemical activation process. Porous carbon

22
Z. Li, et al.
PCCS is rich in natural heteroatom functional groups (atomic ratio of
nitrogen, oxygen, sulfur and phosphorus is 12.06%), developed mi-
cropores (micropore pore volume accounts for 67%) and high specific
surface area (1676 m2 g−1). With high specific surface area and regular
pore structure, the presence of heteroatoms helps to provide sufficient
ion attachment sites inside the electrode, efficient ion transmission
channels, and significant pseudo-capacitance contributions. In the
three-electrode test, the PCCS electrode has an ultra-high specific ca-
pacity of 355F g−1 at 1 A g−1 in 6 M KOH, and a specific capacity of
284F g−1 at a large current density of 30 A g−1. The almost linear and
symmetrical charge-discharge curves show that all electrodes have
good capacitance performance [266]. In addition, the electrode exhibits
excellent rate performance, and after 3000 cycles at a current density of
10 A g−1, the capacitance retention is still greater than 90%. In the
assembled symmetrical two-electrode test, the electrode exhibited a
maximum energy density of 9.0 Wh kg−1 and an optimal energy den-
sity of 9000 W kg−1. Chen et al. [116] Successfully prepared bamboo-
derived porous carbon (ABC) with high specific surface area and me-
soporous structure through two steps of carbonization and activation.
The specific surface area, total pore volume, and average pore diameter
of biomass-derived carbon can be controlled by adjusting the activation
temperature. The carbon material ABC-900, which is synthesized at
900 °C, has the best mesoporous structure (pore volume of 1.24 cm3
g−1) and has a high specific surface area (2221.1 m2 g−1). In 3 M KOH
aqueous electrolyte, ABC-900 exhibits a maximum specific capacitance
of 293F g−1 at 0.5 A g−1 and excellent rate capability (specific capa-
citance maintains 193.8 F g−1 at 20 A g−1). The symmetrical super-
capacitor assembled by ABC-900 delivers an optimal energy density of
10.9 Wh kg−1 (63 W kg−1) and power density of 3200 W kg−1 (9 Wh
kg−1) in 3 M KOH. These excellent research results confirm the po-
tential of activated biomass carbon materials for supercapacitors. Han
et al. [230] used cornstalk core as carbon precursor to prepare high-
performance biomass-derived carbon for electrode materials for elec-
trochemical capacitors. By studying the effects of temperature and the
ratio of activator (KOH) to carbon (mKOH/mC) on the structure of the
resulting material, they synthesized porous carbon material (PCM) with
a large specific surface area of 2139 m2 g−1 and a total pore volume of
1.16 cm3 g−1. In 6 M KOH electrolyte solution, the assembled dual-
electrode electrochemical system obtained an optimal specific capaci-
tance of 317F g−1 at a scan rate of 1 mV s−1. The capacitor can retain
more than 93% of its initial capacitance after 10,000 cycles at a scan
rate of 200 mV s−1. In addition, the device can achieve high power
density of 28.3 kW kg−1 (4.5 Wh kg−1) and high energy density of 6.8
Wh kg−1 (250 W kg−1). From the above, corn stalks can already be
used as raw materials for preparing carbon electrodes for electro-
chemical capacitors with high capacitance performance.
Yu et al. [128] prepared an elm fruit-derived porous carbon na-
nosheet with a three-dimensional scaffolding frameworks by KOH ac-
tivation. 3D porous carbon PCNS-6 has a high specific surface area of
1947 m2 g−1, an optimized pore structure and a high pore volume of
1.33 cm3 g−1, which is very beneficial for ion transport inside the
electrode. In 6 M KOH electrolyte, the electrode PCNS-6 has capacity of
470F g−1 and 310F g−1 in three-electrode and two-electrode system at
the current density of 1.0 A g−1. In addition, as shown in Fig. 15, the
electrode still has excellent capacitance retention and high cycle sta-
bility (loss is only 2%) after 50,000 cycles at 10 A g−1. It is worth
noting that the assembled symmetrical electrode has an excellent en-
ergy density of 43 Wh kg−1 in EMIMBF4 and power density of
500 W kg−1, even the energy density remains 22.2 Wh kg−1 at the high
power density of 20000 W kg−1. In short, electrode materials with such
excellent electrochemical properties can be widely used in the field of
energy storage. Liao et al. [77] synthesized a microporous carbon ma-
terial (SSMC) with developed pores from low-cost silkworm by simple
carbonization and further activation steps. SSMC has an ultra-high
specific surface area of 2523 m2 g−1, a large pore volume of 1.37 m3
g−1, and rich heteroatom functional group (3.5 at% N content and 5.1
23
Chemical Engineering Journal 397 (2020) 125418
at% O element). Carbon materials with high specific surface area, good
pore size distribution, and proper heteroatom content are very bene-
ficial for enhancing the performance of electric double layer capacitors
for energy storage. When the current density is 1 A g−1, the device
using SSMC as the electrode material achieved high specific capaci-
tances of 304F g−1 and 223.5F g−1 in the three-electrode and two-
electrode systems, respectively. The symmetrical two-electrode device
in a 6 M KOH aqueous electrolyte provides a high energy density of 7.9
Wh kg−1 (234 W kg−1) and the power density of 3500 W kg−1 (3.1 Wh
kg−1). This is of great significance for the deployment of high-perfor-
mance energy storage devices using eco-friendly biomass materials.
Aravindan et al. [66] synthesized teak sawdust-derived mesoporous
activated carbon (AC-HBP) as an electrode material for high-perfor-
mance lithium-ion capacitors (LIC) by ZnCl2 activation. The optimized
porous carbon AC-HBP obtained by the hydrothermal carbonization
process has a specific surface area of up to 2108 m2 g−1 (mesopore ratio
of 66%) and pore volume of 2.2 cm3 g−1. The assembled hybrid LIC has
excellent capacitance characteristics and excellent energy density.
Through different ways of regulation, the final mixing device achieved
a maximum energy density of 111 Wh kg−1 (150 W kg−1) and an
optimal power density of 7800 W kg−1 in 1 M LiPF6 electrolyte. This
work opens up new avenues for developing high-energy and power-
density lithium-ion capacitors. Hierarchical porous carbon rich in N/O
co-doping was extracted from soybeans by Lin et al. [69] via KOH ac-
tivation method. The obtained porous carbon has a 3D network struc-
ture with developed interconnections, specific surface area (1837 m2
g−1), high level of micropores (0.71 cm3 g−1), and high content of
nitrogen (1.58 at. %) and oxygen (11.41 at. %), which is advantageous
for the electrochemical performance of the capacitor as well as high-
speed ion transmission and storage. In a three-electrode system, the
porous carbon electrode exhibits an excellent specific capacity of
321.1F g−1 at the current density of 1 A g−1, and has excellent cycle
stability of 99.5% even after 10,000 cycles. The corresponding sym-
metrical capacitor system has the most optimal energy density of 22.1
Wh kg−1 and power density of 4377 W kg−1 in EMIMBF4 electrolyte.
This result is better than many other biomass-derived carbon elec-
trodes. By studying the optimization of pore size and volume distribu-
tion, Xie et al. [127] invented a simple and effective method for ionic
thermal carbonization to optimize the porous structure of carbon ma-
terials. They prepared a series of nitrogen-doped graded porous carbons
with unique sub-micron size, high surface area and rich mesopores
using Junjun grass as precursor. The obtained optimized porous carbon
ITC-JG-900 has a large specific surface area of 2532 m2 g−1 and me-
sopore pore volume of 1.077 cm3 g−1. In the electrolyte of 6 M KOH,
the electrode ITC-JG-900 shows a satisfactory specific capacitance of
336F g−1 at 1 A g−1 and maintains capacitance of 222F g−1 even at 10
A g−1 (66% of capacitance retention). The assembled symmetrical ca-
pacitor device has an amazing specific capacitance of 336F g−1 at 1 A
g−1, and the energy density and power density are as high as 72.7 Wh
kg−1 (1204 W kg−1) and 12500 W kg−1 (38.8 Wh kg−1) in 6 M KOH, it
maintains a high level under different current densities. This is superior
to most biomass-derived carbons tested in aqueous electrolytes. Li et al.
[89] used a peanut shell as precursor to synthesize hierarchical porous
material with high specific surface area (2396 m2 g−1) and oxygen
doping (oxygen content up to 13.51 wt%) through a novel and efficient
strategy combining KOH activation and air activation. Carbon is used in
sodium ion hybrid capacitors (NIC). Compared to lithium-ion capacitors
(LIC), assembled asymmetric sodium-ion hybrid capacitors provide an
amazing combination of energy and power cycling stability. At current
density of 0.1 A g−1, the specific capacity of the electrode is 213F g−1
in 1 M NaClO4, and the maximum energy density and power density are
as high as 201 Wh kg−1 (286 W kg−1) and 16500 W kg−1 (50 Wh
kg−1). In addition, the hybrid equipment has excellent cycle stability,
and the equipment maintains capacity retention rate of 88% after
100,000 tests at 51.2 A g−1 (Fig. 16).
Manyala et al. [242] used a convenient two-step eco-friendly
Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 15. Electrochemical performance characteristics of the two-electrode system of PCNS-6 in EMIMBF4 electrolyte (a) CV curves from 5 to 200 mV s−1 at different
scan rates in a voltage window of 0 to 3 V; (b) Charge-discharge curves at different current densities from 0.25 to 5 A g−1. (C) Gravimetric capacitances at different
current densities. (D) Cyclic stability measured at 5 A g−1. (E) Nyquist plots before and after 5000 cycles. (F) Ragone plot of PCNS-6 compared to reported results. (g)
15 LEDs and (h) a small fan powered by the supercapacitor device. (Reprinted with permission from Reference [128]).

hydrothermal synthesis route to synthesize soft wood (Quercus Suber)
derived activated carbon with high pore structure and good texture
characteristics. The raw materials are optimized through K2CO3, and
the final activated carbon has a specific surface area of 1056 m2 g−1
and a pore volume of 0.65 cm3 g−1. In this resertch, Co-Mn layered
double hydroxide (LDH) nanosheets were used as the positive electrode,
and activated carbon was used as the negative electrode to successfully
assemble the hybrid capacitor device. It can be clearly seen from picture
15 the hybrid device showed a specific capacitance of 65F g−1 and a
high energy density (435 W kg−1) of 20.3 Wh kg−1 at a current density
of 0.5 A g−1. In addition, the device has a capacitance retention rate of
99.7% after 10,000 consecutive charge and discharge cycles, and there
is almost no capacitance loss. This is a hybrid device with high energy
density. Zhao et al. [243] used a novel hydrothermal carbonization and
KOH activation strategy to prepare tobacco rods-derived carbon for
supercapacitors. Although various activated carbons come from dif-
ferent types of precursors, the products ensure similar properties, such
as high specific surface area (up to 2115 m2 g−1), layered porous
structure and rich heteroatom functional groups. In the three-electrode
test, the carbon electrode TC has a specific capacitance of 286.6F g−1 at
a current density of 0.5 A g−1, and the capacitance remains at 212.1F
g−1 even at 30 A g−1. In addition, the assembled symmetrical super-
capacitor device has an energy density of 31.3 Wh kg−1 at 0.5 A g−1
and a maximum power density of 11.8 kW kg−1 at 15 A g−1. Yang et al.
[63] Made full use of lignocellulosic biomass resources (Amygdalus-
pedunculata shell) to synthesize porous carbon electrode materials with
high capacitance performance. In 1 M Na2SO4, the obtained symme-
trical electrode system has a high specific capacitance of 358.4 F g−1 at
current density of 0.5 A g−1. In addition, the symmetrical device also
exhibits a remarkable high energy density (49.7 Wh kg−1) and power
density (16400 W kg−1). This showed the great potential of lig-
nocellulosic biomass-derived carbon as an electrode material in high-
performance supercapacitors. Lei et al. [129] Used corn straw as a
biomass precursor to synthesize hierarchical porous carbon nanosheets

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Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 16. (a) CV curves of AC and Co-Mn LDH at a scan rate of 25 mV s−1, (b) CV curve of Co-Mn-LDH // AC hybrid battery for different operating voltages at
25 mV s−1 in 1 M KOH, (c) CV plots from 5 mV s−1 to 100 mV s−1, (d) GCD plots from 0.5 A g−1–5.0 A g−1 in the same voltage window, (e) Specific capacitance at
different current densities and (f) Ragone diagram. (Reprinted with permission from Reference [242]).

(aCS) for capacitive energy storage by carbonization and chemical ac-
tivation. The obtained porous carbon aCS has a two-dimensional sheet-
like structure, high specific surface area (1736 m2 g−1) and rich mi-
cropores. In a three-electrode system, the electrodes have excellent
capacitance performance of 301F g−1 and 231F g−1 in KOH and
Na2SO4 electrolytes, respectively. The symmetrical two-electrode de-
vice can provide a specific energy of 20.2 Wh kg−1 at a power density
of 398 W kg−1 at 1 M Na2SO4, and can also provide a high power
density of up to 17600 W kg−1. Sun et al. [252] combined hydro-
thermal treatment and chemical activation to prepare ultra-high spe-
cific surface area (2801 m2 g−1) and large pore volume (1.7 cm3 g−1) of
graded porous carbon materials from hemp stems. The synthesized
Hurd-x-5 carbon material can be used to prepare electrodes for super-
capacitors. When the current density is 1 A g−1, the asymmetric su-
percapacitor device exhibits a high specific capacitance of 160F g−1.
The device also has a high power density of 21 kW kg−1 and a high
energy density of 19.8 Wh kg−1, showing excellent electrochemical
performance. This experiment also revealed the simple relationship
between the specific surface area capacitance and pore distribution of
carbon materials and the specific capacitance of electrochemical
double-layer capacitors, further promoting the research progress of the
preparation of high-performance electrochemically active materials

25
Z. Li, et al.
using biomass and biological waste. Bagasse-derived hierarchical
structure carbon (BDHSC) with adjustable porosity and optimized
electrochemical performance was successfully prepared by Zheng et al.
[248] By combining efficient hydrothermal carbonization with KOH
activation. The synthesized porous carbon BDHSC has an inter-
connected framework with high specific surface area (2296 m2 g 1) and
high pore volume (1.34 cm3 g−1), which is advantageous for electro-
chemistry. The BDHSC carbon electrode has a high specific capacitance
(320F g−1 at 0.5 A g−1) and excellent rate performance (capacity re-
tention rate exceeds 70.8% at a high current density of 50 A g−1) in a
three-electrode system. The assembled symmetrical supercapacitor
showed high energy density of 20 Wh kg−1 (182 W kg−1) and power
density of 54 kW kg−1 (10.65 Wh kg−1) in 1 M Na2SO4 electrolyte.
Hierarchical porous activated carbon has broad application prospects in
high-performance energy storage devices. Guo et al. [191] Successfully
synthesized highly porous biomass-derived hollow carbon microspheres
(ACM) through a green and sustainable CO2 activation strategy. With
the high specific surface area of 3053 m2 g−1, the ideal microstructure
and nanostructure promote the obtained ACM to exhibit good electrical
conductivity and electrochemical stability. The ACM electrode has ex-
cellent double-layer capacitance performance. In TEABF4 organic
electrolyte, the specific capacitance can reach 308F g−1 at 0.1 A g−1,
and the specific capacitance can maintain 263F g−1 at 20 A g−1. And
the assembled symmetrical capacitor has a capacitance retention rate of
93.8% after 10,000 charge and discharge cycles, as well as high energy
density (57 Wh kg−1) and excellent power density (17 kW kg−1).
Cao et al. [131] used silkworm manure as precursor to prepare
honeycomb porous carbon with high specific surface area and hier-
archical pore distribution for the electrode material of lithium ion hy-
brid electrochemical capacitor (Li-HEC) with high capacitance and
stability. The obtained carbon material (PC-SE-700) has a higher sur-
face area (2826 m2 g−1) and nitrogen doping characteristics as shown
in Fig. 7, which is beneficial to improving the capacitance performance
and wettability of the electrode. As shown in Fig. 17, the symmetrical
super capacitor made by PC-SE-700 has an energy density of 138.4 Wh
kg−1 at a power density of 495.9 W kg−1. The Li-HEC composed of PC-
Fig. 17. (a) Schematic illustration of PC-SE-700//Si/C Li-HEC. (b) CV curves of PC-SE-700//Si/C at different scan rates. (c) GCD curves of PC-SE-700//Si/C at
different current densities. (d) Ragone diagram of PC-SE//Si/C compared with other Li-HEC devices reported in the literature in terms of energy density vs. power
density. (e) Cyclic performance test at 2.0 A g−1. The illustration is a demonstration of powering the LED by a PC-SE-700//Si/C device. (Reprinted with permission
from Reference [131]).
26
Chemical Engineering Journal 397 (2020) 125418
SE-700 shows a higher energy density of 242.2 Wh kg−1 at 1 M LIPF6,
excellent rate performance and stability. The hybrid device still has an
energy density of 186.5 Wh kg−1 at the highest power density of
6473 W kg−1. Xu et al. [132] used KOH to activate the precursor (wax
gourd) rich in natural porous structures and heteroatoms to successfully
synthesize a heteroatom-doped porous carbon (WGPC-4) with a high
specific surface area (2920 m2 g−1) and rich micro-mesopore structure
as an ideal electrode material for sodium ion capacitors. The optimized
porous carbon WGPC-4 contains higher oxygen of 17.9 at.% and ni-
trogen contents of 1.0 at.%, respectively. In the three-electrode system,
WGPC-4 electrode exhibited a high specific capacitance of 333F g−1 at
1 A g−1 in 6 M KOH. At the same time, the symmetrical battery as-
sembled in 0.5 M Na2SO4 aqueous electrolyte also has excellent cycle
stability (92.5% capacity retention rate after 5000 cycles), excellent
energy density 19.2 Wh kg−1 and power density 8625 W kg−1. In
summary, the calabash-derived graded porous carbon can be used as an
ideal electrode material in electrochemical applications. Based on the
use of low-toxic or non-toxic potassium salts as templates (KCl and
K2CO3) and activators (K2CO3), Sevilla et al. [172] synthesized a bio-
mass(soybean meal)-derived hierarchically porous carbon with 3D
skeleton through an efficient salt template-assisted chemical activation
method. The obtained 3D hierarchical porous carbon has a high specific
surface area of 2000 m2 g−1 and total pore volume of 1.19 cm3 g−1. In
ionic liquid electrolyte (EMImTFSI/AN), the symmetrical electrode
system shows the best energy density of 50 Wh kg−1 and power density
of 23 kW kg−1. Chen et al. [90] selected a sustainable biomass shell
(peanut shell) as precursor to synthesize hierarchical porous carbon
with excellent specific surface area (1994 m2 g−1) and pore volume
(cm3 g−1) for the positive material for sodium ion hybrid capacitors.
The hybrid capacitor 1 M Na2SO4 electrolyte assembled from hier-
archical porous carbon BPC-5 can provide a high specific energy of
169.4 Wh kg−1 at power density of 120.5 W kg−1 over many similar
biomass carbons. Du et al. [180] Successfully synthesized nitrogen-
doped porous hollow carbon spheres from live yeast cells by two-step
hydrothermal precarbonization and pyrolytic carbonization. The ob-
tained porous carbon exhibited an ultra-high specific capacitance of
Z. Li, et al. Chemical Engineering Journal 397 (2020) 125418

Fig. 18. (a) Schematic of the electrochemical reaction mechanism of a LIC; (b) CV curves within the voltage range of 0–4.5 V at various scan rates, and (c)
galvanostatic charge-discharge curves at various current densities of the NDPC-0.5//NDPC-0.5 LIC, (d) Ragone plots of the NDPC-0.5//NDPC-0.5 LIC compared with
previously reported LICs and (e) cycling stability of NDPC-0.5//NDPC-0.5 LIC at a current density of 2 A g−1. (Reprinted with permission from Reference [261]).

255F g−1 in an aqueous electrolyte at a current density of 1 A g−1.
Afterwards, the MnO2/HCS-30 electrode material with the best per-
formance was obtained by in-situ hydrothermal deposition. Asymmetric
supercapacitors were assembled with HCS as the negative electrode. In
1 M Na2SO4, the asymmetric device can obtain an optimal energy
density of 41.4 Wh kg−1 under a voltage window of 2.0 V at the power
density of 500 W kg−1 and an optimal power density of 7901 W kg−1
(23.0 Wh kg−1). In addition, the asymmetric device also has excellent
cycle stability. This provides a good strategy for the use of biomass-
derived carbon.
Zou et al. [264] successfully produced high-performance N-doped
porous carbon (NDPC) as a sustainable electrode material for lithium
ion capacitors (LIC) by using bagasse as precursor through an efficient,
environmentally friendly, and low-cost eutectic salt activation method.
The synthesized hierarchical porous carbon NDPC-0.5 has a large spe-
cific surface area of 1506 m2 g−1 and rich heteroatom distribution
(nitrogen of 9.56% and oxygen of 5.38%). As shown in Fig. 18, Ni-
trogen-rich doping can induce more active sites and increase the spe-
cific capacity of the material. The full-carbon lithium-ion two-electrode
capacitor (NDPC-0.5//NDPC-0.5) assembled by NDPC-0.5 shows ex-
cellent electrochemical performance. In the electrolyte of 1 M LIPF6, the
device has an amazing energy density of 116.9 Wh kg−1 at power
density of 500 W kg−1, the energy density remains 87.7 Wh kg−1 at
maximum power density of 10,000 W kg−1. In addition, the device also
has good cycle stability, with a capacity retention rate of 81% after
8000 cycles at 2 A g−1. Therefore, Biomass-derived carbon with

27
Z. Li, et al.
Fig. 19. (a) Schematic diagram of the structure and working mechanism of Zn-HSC hybrid device; (b) Typical charge-discharge curve of Zn-HSC. The insert shows
two Zn-HSC lights up green LED; (c) Comparison of Zn-HSC and other equipment on the relationship diagram of energy density and power density. (Reprinted with
permission from Reference [103]). (For interpretation of the references to colour in this figure legend, the reader is referred to the web version of this article.)
excellent electrochemical properties has promising commercial value.
Porous biomass-derived carbons (BDCs) was prepared by Chen et al.
[72] who used mushroom as biomass raw material via a series of ac-
tivating agents, the best electrochemical performance was exhibited
during they used KHCO3 as an eco-friendly activator. As Fig. 10 dis-
plays, thanks to high surface area (1788.1 m2 g−1), high-density micro-
mesopores generated during activation, the contribution of high-con-
tent N atoms (1.3 at. %), a superior volumetric of 354.8F g−1 and
gravimetric capacity of 220.0F cm−3at 1.0 A g−1 in three-electrode
system was exhibited at a current density of 1.0 A g−1 when using 1 M
H2SO4 as the electrolyte solution in the three-electrode system, it is
worth noting that the specific capacity of the electrode can still be
maintained up to 266.0F g−1 (50 mA cm−2) at a high current density of
10 A g−1. In addition, the assembled CKHCO3//CKHCO3 symmetrical
capacitor also was given excellent long-term cycling capability, a high
weight/volume energy density of 55.2 Wh kg−1/34.2 Wh L−1 was
showed at power of 1250 W kg−1. At the same time, the obtained
CKHCO3 electrode material showed remarkable Na+- storage perfor-
mance when evaluated as an anode material, which provided a good
strategy for the future development of porous BDC and its practical
application. Wang et al. [258] used corncob as raw material to prepare
porous carbon by KOH activation and the specific surface area and
porosity of the material were effectively improved after activation. The
obtained C850 had an ultrahigh specific surface area of 3054 m2 g−1
and high pore volume of 1.5 cm3 g−1 and the surface of the material
28
Chemical Engineering Journal 397 (2020) 125418
was rich in a large number of functional groups. The products exhibited
good electrical conductivity and preeminent electrochemical perfor-
mance thanks to well-developed micro-mesopores. At current density of
0.5 A g−1, the C850 showed a high specific capacity of 401.6F g−1 in
0.5 M H2SO4 and 328.4F g−1 in 6 M KOH aqueous electrolyte, re-
spectively. Carbon fiber aerogel is superior to conventional electrode
materials for EDLCs, it has attracted wide attention due to the large
specific surface area, abundant porous structure, stable chemical
properties and large specific surface area, which can promote it as one
of the most promising electrode materials in SCs. Du et al. [80] used Zn
(NO3)2·6H2O to treat raw cotton for preparation of N-doped porous
carbon fiber aerogel (N-CFA) with good flexibility, favorable mechan-
ical durability and high specific surface area. Therefore, the N-CFA
showed outstanding electrochemical performance with a high capacity
of 365F g−1 at 0.5 A g−1 and an extraordinary rate capability of 65.8%
from 0.5 to 100 A g−1 as a binder-free electrode in SCs. Moreover, N-
CFA also exhibited a high capacitance retention of 93.6% at current of 5
A g−1 after 10,000 continuous cycles. This approach may provide a
low-cost and practical method to synthesize high-performance N-doped
carbon aerogels for electrodes from biomass.
In summary, although the potassium ion/sodium ion symmetrical
capacitor energy storage device assembled from a biomass-derived
carbon electrode has achieved a good power density, its energy density
is not particularly prominent. The energy density of potassium ion/
sodium ion symmetrical capacitor devices is mainly concentrated in the
Z. Li, et al.
range of 5–60 Wh kg−1. The energy density deficiency can be effec-
tively improved by improving energy storage ions (such as lithium ions)
or assembling asymmetric energy storage devices. However, the ex-
isting energy storage systems often have some shortcomings, such as
low specific energy of supercapacitors, hidden safety hazards of li-
thium-ion batteries, and poor cycle stability of alkaline zinc-manganese
batteries[99]. In addition, the development of rechargeable devices
based on polyvalent cations has attracted widespread attention as
multivalent ions (M2+ or M3+) have more electronic contributions than
monovalent ions (M+) [103]. Metal zinc has high specific capacity
(5855 mA cm−3 or 823 mA g−1), low redox potential 0.76 V (based on
hydrogen electrode), outstanding stability in the atmosphere and water
electrolyte, low cost and rich resources can be used as a promising
hybrid supercapacitor anode material [96,267,268]. In recent years, a
novel zinc ion hybrid capacitor has been extensively researched with
excellent electrochemical performance, low cost, high safety, rich ma-
terial and stable cycle life, and has become an effective strategy to
achieve both high energy density and high power density energy sto-
rage devices.
Tang et al. [103] successfully combined zinc ion hybrid super-
capacitors (Zn-HSC) by combining low-cost bio-carbon-derived porous
materials (cathode) and zinc foil (anode and current collector). Opti-
mized Zn-HSC achieves high energy density and excellent rate perfor-
mance. In 1 M Zn(CF3SO3)2 electrolyte, Zn-HSC has a high discharge
capacitance of 170F g−1 at a current density of 0.1 A g−1, and achieves
85% capacitance even at 2 A g−1 Retention rate. In addition, Zn-HSC
also has high energy density and cyclic stability. The mixing device has
an energy density of 52.7 Wh kg−1 at 1725 W kg−1 and can maintain
an initial specific capacitance of 91% after 20,000 cycles at 2 A g−1. In
this work, Zn foil is used as the anode and current collector as shown in
Fig. 19. This method effectively improves the convenience of energy
storage devices and is an effective strategy for developing low-cost and
recyclable energy storage systems. Yan et al. [104] prepared a nitrogen-
doped graded porous carbon using chitosan as a precursor for the
cathode of an aqueous rechargeable zinc ion hybrid supercapacitor. The
obtained hierarchical porous carbon N-HPC is rich in heteroatoms
(nitrogen content of 5.2% and oxygen content of 8.2%).The water-
based rechargeable zinc ion hybrid supercapacitor assembled from N-
HPC and zinc foil has excellent energy storage performance and energy
density in ZnSO4 electrolyte. The hybrid device has a high capacity of
136.8 mAh g−1 (307.8F g−1) at a current density of 0.1 A g−1. The unit
also has a high energy density of 191 Wh kg−1 (58 W kg−1) and a high
power density of 3633 W kg−1 (92.5 Wh kg−1). The device has ex-
cellent cycle stability (capacity retention rate of 90.9%) after 5000
cycle tests. N-HPC can be used as a promising electrode material for
high-safety, long-life, and low-cost zinc ion mixing devices.
Cha et al. [269] reported a novel hierarchically nanostructured 2D-
Zn metal electrode-ion supercapacitor (ZIC). Thanks to the layered
structure of 2D-Zn metal, the ion diffusion capacity and energy storage
performance in the electrode are significantly improved. The hybrid
device assembled by zinc foil and activated carbon also shows ex-
tremely excellent ultra-high capacitance performance and energy den-
sity. The device has an ultra-high specific capacitance of 468F g−1 at a
current density of 0.5 A g−1 in 1 M ZnSO4. As shown in the Fig. 20, the
maximum energy density shown by 2 D-Zn/1.8/1.0ZIC is 208 Wh kg−1
at power density of 500 W kg−1, even at maximum power density of
20000 W kg−1 The high level of 66 Wh kg−1 is still maintained. In
addition, the capacitance retention rate of the hybrid device reaches an
amazing 99%. After test of 10,000 cycles at current density of 10.0 A
g−1, it shows extremely excellent cycle stability. It is worth noting that
the flexible ZIC energy storage device assembled from 2D-Zn/1.8/1.0
also has excellent point electrochemical stability in different forms
(straight, folded, and knotted states). Ma et al. [270] Designed a novel
hybrid metal ion capacitor (ZHS) that can achieve both high energy
density and high power density. The hybrid device consists of an acti-
vated carbon (AC) anode and a V2O5 cathode. Through testing, it was
29
Chemical Engineering Journal 397 (2020) 125418
found that optimizing the mass ratio of cathode and anode can sig-
nificantly improve the metal ion energy storage capacity of the hybrid
device, and the capacity and power density of the hybrid device are
significantly improved. The comparison results of different electrolytes
(ZnSO4 and Zn(CF3SO3)2) show that the hybrid device has better elec-
trochemical characteristics in aqueous electrolyte. The hybrid super-
capacitor has an initial capacity retention rate of 97.3% after 6000
charge-discharge cycles at a current density of 0.5 A g−1. In addition,
the assembled AC //2M ZnSO4 //V2O5 ZHS can achieve a maximum
specific capacity of 57.4 mAh g−1 and an energy density of 34.6 Wh
kg−1 in the operating voltage range of 0–2 V, respectively.
In addition, there are many biomass-derived products with excellent
properties used in the field of electrochemical energy storage
[100,104,130,165,182,248,259,260,271]. It is obvious to us that acti-
vation is only one of the important means to improve the performance
of materials at this stage, and the recycling of large-scale biomass re-
quires more effective strategies to implement. The combination of dif-
ferent materials, the improvement of energy storage ions, the in-
troduction of templates [263] and the use of directing agents [88] are
all mature solutions to improve the properties of materials.
5. Conclusion and outlook
In this review, the preparation methods, activation mechanisms,
and application progress of various types of electrochemical energy
storage devices for various BDPC are summarized in detail in the past
three years. Biomass-derived carbon has attracted widespread attention
and has made significant progress in the development of super-
capacitors [24]. As an important member of the electrode material fa-
mily in the field of energy storage, BDPC materials have a unique
structure, high power density, fast charge-discharge cycles, long-cycle
cycle stability, and safety. BDPC synthesized by different activation
methods can have a large specific surface area of 3,800 m2 g−1 [71],
and the prepared electrode exhibits ultra-high power density and an
optimal specific capacitance of 470F g−1 [128]. Therefore, BDPC ma-
terials can be used as a series of most promising and suitable alter-
natives to energy materials in industry and are expected to be widely
used as electrode materials for next-generation high-performance en-
ergy storage equipment [272]. In the past ten years, the explosive
growth of research on high energy density energy storage devices and
the miniaturization of electronic equipment have been witnessed
[273,274].
In general, although carbon-based electrodes have a long history of
development, there is still much work to do before more can be
achieved on the road to commercialization, especially with regard to
rechargeable systems. Researchers have conducted many excellent
studies to alleviate the problems they face, but most of the current
carbon materials have significant shortcomings in energy density,
which is still not enough for commercial applications, and there are still
several aspects to be further studied improve. This can be comprehen-
sively evaluated from different dimensions based on the overall per-
formance of the electrodes in the energy storage system [275]. Despite
obvious achievements in the study of biomass-derived carbon over the
past decade, there are still some urgent challenges that need to be ad-
dressed:
1. Increase yield. Although many high-performance electrode mate-
rials with electrochemical properties can be obtained through pro-
cessing, too low productivity is an important factor limiting their
large-scale application. Therefore, there is an urgent need to opti-
mize the synthesis process to increase the yield, which can be im-
proved by previously reported material synthesis processes to in-
crease the yield.
2. Regulate material structure. At present, there are limited means for
regulating materials. If some biomass materials with ideal structure
and chemical composition can be planted according to needs, the
Z. Li, et al.
Fig. 20. Electrochemical characterization of 2D-Zn/1.8/1.0 ZIC. (a) Nyquist plot before charge-discharge test, (b) CV curve at scan rate of 10 mV s−1 in potential
range of 0.2–1.8 V, (c) Specific capacitance obtained at current density of 0.5 to 20.0 A g−1 in potential range of 0.2–1.8 V, (d) Ragone diagram (curve of energy and
power density), (e) Cyclic stability test after 10,000 cycles at current density of 10.0 A g−1. (Reprinted with permission from Reference [269]).
advantages of bio-based bionic structural materials will be further
exerted. We should pay more attention to using various inorganic/
organic drugs with nanostructures to fine-tune the properties and
functionalization of activated porous carbon, which is also a good
way to increase commercial value.
3. Develop novel biomass-based composite materials. It is also an in-
teresting exploration to develop the next generation of functional
hybrid products by coupling porous carbon with inorganic and or-
ganic nanostructured materials.
4. Optimize the energy density of biomass-based carbon electrodes. At
present, the preparation of lithium-ion batteries and other types of
hybrid supercapacitors can alleviate this problem to a certain extent.
Based on various advantages, zinc ion hybrid capacitors are a pro-
mising development direction.
5. Selection of electrolyte. It is worth noting that, in addition to the
effects of material processing methods on material properties,
electrolytes also have a significant effect on electrode performance.
This can be further studied through deep simulation calculations.
6. Explore an efficient and environmentally friendly activation
method. At present, irritating chemicals and large amounts of
carbon emissions are still generated during the activation of carbon
materials. There is an urgent need to optimize the activation process
and explore a novel, efficient, and environmentally friendly method
for activating porous carbon.
Biomass recycling provides an advantageous strategy for future
businesses, and they can be used in a variety of applications, such as
supercritical carbon, catalysis, and fuel cells [276]. In addition, we can
also cultivate some of the most ideal precursors of biomass that meet
the structure and chemical composition according to demand. All in all,
how to prepare raw materials according to our needs, optimize material
processing methods, and increase productivity are the challenges we
face today. The current state of bio-derived porous carbon is very ex-
citing and can be classified as an emerging advanced nanomaterial in
the future. In short, all of these accurate, comprehensive, repeatable
30
Chemical Engineering Journal 397 (2020) 125418
and reliable data can help improve the efficacy of materials in the in-
tended application. With the further development of various types of
energy storage devices, BDPC will play an important role in future
development [23].
Declaration of Competing Interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influ-
ence the work reported in this paper.
Acknowledgments
The authors are grateful for support from the Henan Science and
Technology Project (No. 202102210057 and No. 2018-557) and the
Technology Innovation Team of Zhengzhou University of Light
Industry.
Authors’ contributions
Zijiong Li supervised the whole work. Dongfang Guo drafted the
manuscript. All authors read and approved the final manuscript.
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