2022 - Recent Trends in Supercapacitor-Battery Hybrid Energy Storage Devices Based On Carbon Materials

Journal of Energy Storage 52 (2022) 104938
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Journal of Energy Storage

journal homepage: www.elsevier.com/locate/est
Review Article
Recent trends in supercapacitor-battery hybrid energy storage devices

based on carbon materials
Santhi Maria Benoy a, b, Mayank Pandey c, Dhrubajyoti Bhattacharjya a, b, Binoy K. Saikia a, b, *
a
Coal & Energy Division, CSIR-North East Institute of Science & Technology, Jorhat 785006, Assam, India
b
Academy of Scientific & Innovative Research (AcSIR), Ghaziabad 201002, India
c
Department of Physics, Kristu Jayanti College (Autonomous), Bangalore 560077, India
A R T I C L E I N F O A B S T R A C T
Keywords: Currently, tremendous efforts have been made to obtain a single efficient energy storage device with both high
Hybrid capacitors energy and power density, bridging the gap between supercapacitors and batteries where the challenges are on
Electrochemical energy storage devices combination of various types of materials in the devices. Supercapacitor-battery hybrid (SBH) energy storage
Li-ion capacitor
devices, having excellent electrochemical properties, safety, economically viability, and environmental sound
Na-ion capacitor
ness, have been a research hotspot in the current world of science and technology. Carbon derivatives from 0D to
K-ion capacitor
E-vehicles 3D, e.g., activated carbon, graphene, porous carbon etc., are employed as one of the promising electrode ma
terials due to abundance in reserve, economical viability, adjustable pore size, and wide range of operation
potential. Hybrid supercapacitor applications are on the rise in the energy storage, transportation, industrial, and
power sectors, particularly in the field of hybrid energy vehicles. In view of this, the detailed progress and status
of electrochemical supercapacitors and batteries with reference to hybrid energy systems is critically reviewed in
this paper. The focus is also given to the recent trends in porous and graphene-based carbon electrode materials
in asymmetric capacitor and metal ion capacitors (e.g. Li-ion, Na-ion, and K-ion capacitors) and its electro
chemical properties for its potential applications. The output of this unique review will serve as a database for
extending the R&D in the field of supercapacitor-battery hybrid system for possible applications including e-
vehicles.
1. Introduction consuming devices, which are mainly divided into three types: con
ventional gasoline combustion engines, hydrogen combustion engines
The rise in prominence of renewable energy resources and storage (CE), and hydrogen fuel cells. There are different types of energy storage
devices are owing to the expeditious consumption of fossil fuels and for various applications, as shown in Fig. 2 [4].
their deleterious impacts on the environment [1]. A change from com Supercapacitors, fuel cells, second-generation Li-ion batteries and
munity of “energy gatherers” those who collect fossil fuels for energy to superconducting magnetic storage devices are some of the promising,
one of “energy farmers”, who utilize the energy vectors like biofuels, sustainable EESDs, among which secondary batteries, and super
electricity, hydrogen, or other synthetic fuels, is inevitable [2]. The urge capacitors are considered to be the major contributors. Supercapacitors/
for electrical energy is increasing since electrical appliances usage has ultracapacitors can bridge the gap between batteries and normal ca
increased. But the conversion of electrical energy from renewable en pacitors, reducing greenhouse gas pollution with prolonged cycle effi
ergy resources is intermittent and an intermediate energy storage device ciency, fast charging-discharging stability, and great power density
is required for the regular supply [3]. Researchers and industrialists are (such as 10 kW kg− 1). Conversely, batteries own the property of high
in quest of Electrochemical Energy storage devices (EESD) with high energy density but poor cycle stability and low power density (like 265
energy density and power density with optimized cycle life, economi Wh kg− 1). Thus, each technology alone cannot fulfil the commercial
cally viable, and eco-friendliness. Fig. 1, known as a Ragone plot, ex requirements. To overcome this, various electrochemical energy storage
presses the energy-power performance of conventional capacitors, devices have been designed and developed by combining the advantages
batteries, supercapacitors, and their hybrids. It also describes fuel- of supercapacitors and rechargeable batteries, known as hybrid energy
* Corresponding author at: Coal & Energy Division, CSIR-North East Institute of Science & Technology, Jorhat 785006, Assam, India.
E-mail address: bksaikia@neist.res.in (B.K. Saikia).
https://doi.org/10.1016/j.est.2022.104938
Received 7 March 2022; Received in revised form 7 May 2022; Accepted 18 May 2022
Available online 30 May 2022
2352-152X/© 2022 Elsevier Ltd. All rights reserved.
S.M. Benoy et al. Journal of Energy Storage 52 (2022) 104938
Fig. 1. The energy-power performance of conventional capacitors, batteries,

and supercapacitors along with their hybrids demonstrated by Ragone plot [5].
Fig. 3. Classification and compositions of hybrid energy storage devices [12]
density of supercapacitors without compromising the power density

[8–10]. This idea opens up doors for developing hybrid energy storage
devices (HESD) that can combine the properties of supercapacitor and
rechargeable batteries, including the advancement of fundamental
principles and technological prospects. The SBH intends to obtain
comparable performance to batteries in terms of energy capacity and
supercapacitor resulting from power capability and cycle stability. This
can be attained by hybridization of either materials and/or electrodes in
the same devices. However, the material approach prioritizes the syn
thesis and design of composite or hybrid supercapacitor or battery
electrode material used in electrochemical energy storage devices [8]. In
SBH, the negative electrode is of carbonaceous materials of high power
density assembled with positive electrode of battery-grade and redox
active material which enables the faradic reaction process [11]. The SBH
is further divided into Lithium-ion SBHs (LISBHs), acid SBHs (ADSBHs),
Sodium ion SBH (NaISBHs), alkaline SBH (AlSBHs), and others
depending on the electrolytes [12] as graphically represented in Fig. 3.
Fig. 2. Different types of energy storage devices for sustainable applica

tions [4]. 1.1. Carbon-based electrode materials in SBH
storage devices. The hybrid energy storage device is classified into The most common electrode materials used in SBH are activated
asymmetric supercapacitor (ASC), with different capacitive electrodes carbon (AC) and graphene-based materials. Graphene, a two dimen
and supercapacitor-battery hybrid (SBH) with one battery type electrode sional graphite sheet recognized as an advanced carbon nanomaterial
and the other based on the capacitive method. Therefore, the SBH is for using in SBH systems [13]. Recently, graphene, because of its unique
considered to be an auspicious next generation energy storage device. properties from both physical and chemical aspects, has been attractive
The charge storage mechanism of supercapacitors and secondary for numerous applications in electrochemical energy storage systems.
batteries proceeds through two electrodes, an electrolyte, current col Graphene is also known for its exceptional electrical conductivity and
lector, and a separator which permit the ion transfer and prevent the outstanding mechanical properties and large theoretical specific surface
electrodes from coming into contact. Based on the charge storage area. Therefore, reports from many research groups have verified its
mechanism, supercapacitor is classified as Electric Double Layer Ca potential to innovate the current EES landscape [14,15]. Activated
pacitors (EDLC) and Pseudocapacitors. EDLC make use of induced carbon (AC) is one of the excellent forms of carbon due to the good
electro-ionic charge-storage mechanism wherein the pseudocapacitor electrical conductivity, cost-efficiency, pore structure, and accessibility
depends on faradaic redox processes limited to the electrode–electrolyte of material since it is used as a conductive agent in energy storage de
interface which is electroactive phase [2]. In a battery, the energy is vices. Similarly, AC was used as positive/negative electrode for super
directly stored or released by the conversion of chemical energy to capacitor devices and carbon backbone for growing a hierarchical
electric energy [6,7]. However, secondary batteries, such as lith nanostructure [3].
ium–sulfur (Li–S) batteries, lithium-ion batteries (LIBs), and flow bat In this review, the basic working principle of hybrid capacitors and
teries (FBs), undergo repeated and reversible charging and discharging, their components, such as EDLCs and Pseudocapacitors, are compared
which has an adverse effect on the life span of batteries [8]. and discussed. The main focus is given to the current development,
Multifarious research has been conducted to enhance the energy principles, construction, working, applications, and future perspective
of supercapacitor-battery hybrid devices. The basics of Lithium-ion
2
ergy is stored by the accumulation of charges on two parallel metal

electrodes which separated by dielectric medium with a potential dif
ference between them. The capacitance C of parallel plate capacitor is
given by.
C = εεrA/d (1)
where, A is the area of the metal plate, ε is the permittivity of the me
dium, and d is the distance between the metal plates, respectively. The
ions present in the electrolytes are adsorbed by the electrode material
and, thus, a charge separation occurs, resulting in polarization at elec
trode electrolyte interface. The double-layer thickness is on the order of
5–10 Ao. The surface charge generation mechanism takes place by
means of surface dissociation, adsorption of ions from the solution, and
defects in the crystal lattice of a material; which depends on the con
centration of electrolyte and ion size [16]. The small charge storing area
and large separation area are limiting factors to the capacitor. Where in
EDLC, more energy can be stored due do the high-porous electrode
material [17]. The schematic representation of a conventional and
electrochemical capacitor is given in Fig. 5.
Fig. 4. Schematic representation and compositions of electrochemical devices The EDLC concept was first reported in the nineteenth century by
von Helmholtz and later modified by Gouy et al. [18]. Their studies
capacitor (LIC), Sodium-ion capacitor (SIC), and Potassium-ion Capac noted that the charge is stored on to the electrochemically stable elec
itor (KIC), along with the recent progress, is also included in this article. trode material by the reversible adsorption of electrolyte ion and double
layer is formed at electrode-electrolyte interface upon application of an
electric field [19]. The electron transport across the electrode-
1.2. General principle of electrochemical capacitors
electrolyte interface, is absent in non-faradic process. During charging
the electrons move from the anode to the cathode via an external circuit.
Electrochemical energy storage devices are classified into super
While in the electrolyte, anions flow toward the anode and cations flow
capacitors, batteries including primary and secondary batteries, and
towards the cathode [20]. During discharging, the reverse process oc
hybrid systems. Each has positive and negative electrodes, a separator,
curs. Since no chemical change is happening in the entire process, it
and current collector. The schematic representation of an electro
assures cycle stability and more power density.
chemical energy storage device is given in Fig. 4. Electrodes are loaded
The EDLC has two electrodes with metallic current collectors placed
with active material, which helps in the conduction mechanism of ions
in electrolyte solution and separated by a separator to avoid neutrali
with the help of electrolytes. A permeable membrane placed between
zation of oppositely charged electrodes. Then, the capacitance is
two oppositely charged electrodes is the separator that prevents the
calculated from the Eq. (2):
electrodes from short circuiting and self-discharge. Current collectors
are used to efficiently transfer electrons from electrodes to the cell ter ε˳A
C= (2)
minals. The casing protects the cell from evaporation of electrolyte and d
from the negative impact from outside. Here, C is the capacitance in Farads, ε˳ is the permittivity of free
space, A is the surface area, and d is the width of electric double layer,
1.3. Electric Double Layer Capacitors (EDLC) also known as Debye length. From the equation, it is already known that
the capacitance depends on the accessible surface area that is different
The capacitance mechanism of Electric Double Layer Capacitors is from specific surface area obtained from Bruauer-Emmet-Teller (BET)
similar to that of dielectric capacitors. In conventional capacitors, en surface area analysis, because all pores are not available for the charge
Fig. 5. Schematic representation of conventional and electrochemical capacitor.
3
Table 1
Summary of various EDLC electrode materials based on carbon.
Electrode material Electrolyte Cell voltage Power Density (W Energy Density (Wh Specific capacitance (F/ Refs.
(V) kg-1) kg− 1) g)
TiO2@AC 1 M Na2SO4 1.2 4200 28 282 [25]

Flexible PANI/rGO 1 M H2SO4 0.8 368 24.45 299 [26]
AC on surface of rGO 1 M Na2SO4 1.6 469.24 11.9 541 [27]
rGO 2 M KOH 1 – – 114 [24]
Porous carbon derived from eucalyptusbark 0.5 M NaTFSI in 2.5 57 K 32.8 155 [28]
EMITFSI
AC TEABF4/AN 2.5 681 20 80 [10]
rGO (AEI-TFSI) 2 940 61 250 [29]
Miller straw AC 2 M KOH 1 101 18.67 144 [30]
Shochu waste 1 M TEABF4/PC, 2.5 – 44 152 [31]
derived AC
Crumpled nitrogen doped graphene-like EMIMBF4 4.1 1000 82 239 [32]
material
Porous carbon from 2 M KOH 1.2 234 6.26 265 [9]
Sugarcane bagasse
AC from automated shredder residue 2 M KOH 3 – – 280 [33]
single− /few-layer graphene flakes γ-Butyrolactone/ 3 7500 23.5 101 [34]
[EMIM][TFSI]
Hierarchical porous carbons 6 M KOH 0.9 – 10.48 384 [35]
AC from baobab 6 M KOH 0.8 400 20.86 59 [36]
fruit shell
Nitrogen- doped resorcinol/ 6 M KOH 1 – – 208 [37]
formaldehyde carbon aerogels
storage process. in the potential window of 2.5 V and a specific capacitance of 26 F/g
The selection of electrode material plays a vital role in the properties Woodward et al. [22] reported that r-GO containing carboHIPES, with a
of EDLC. Surface properties greatly impact capacitance because the coulombic efficiency ≥95%, is a promising EDLC electrode material.
charge storage is herein a surface process [21]. Among the various [22]
electrode materials, carbon derivatives are most commonly explored Reece et al. [23] fabricated a structural supercapacitor with a novel
due to their cost effectiveness, accessibility, and their ability to exist in solid composite electrolyte of 1 M TEABF4 in propylene carbonate (PC)
different forms like fibres, forms and nanotubes. The most common and epoxy with a high surface area (1500 m2/g) activated‑carbon-fiber
electrode materials utilized for EDLC are based on carbons, such as electrode. The electrochemical properties were presented by varying the
activated carbon, carbon nanotubes, and graphene. Some recent works electrolyte composition and reported that the increased proportion of
on supercapacitors with EDLC behaviour is summarised in the Table 1. epoxy enhanced the structural properties of material flexural modulus of
Woodward et al. [22] synthesized carbon foams from poly(divinyl 24.1 GPa and flexural strength of 1.357 GPa for the 2:1 w/w epoxy:
benzene) polymerization of the minority phase of either SiO2 nano liquid electrolyte mixture [23]. Tamilselvi et al. [24] demonstrated a
particle or reduced graphene oxide -stabilised water-in-DVB HIPEs with way to convert coconut waste to r-GO using simple catalytic oxidation
a surface area of 1820 m2/g and electrical conductivity of 285 Sm− 1. The using ferrocene catalyst and a specific capacitance of 111 F/g in 2-M
electrochemical analysis of sample was done by using an ionic liquid, 1- KOH was reported. On the other hand, the influence of annealing tem
ethyl-3-methylimidazolium bis(trifluoro methyl sulfonyl)imide (EMI- perature on N-doped porous carbon balls was studied, demonstrating
TFSI), an electrolyte, in two electrode system. The system showed an that N annealing at 700 ◦ C raised a specific capacitance of 413 F/g and
energy and power density of 5.2 Wh kg− 1 and 280 W kg− 1, respectively, capacitive retention of 96.5% after 5000 cycles [22]. The enhancement
Fig. 6. A schematic representation of mechanism of energy storage in pseudocapacitors.
4
Table 2
Summary of various pseudocapacitor electrode materials based on carbon materials/composites.
Electrode material Electrolyte Cell voltage Power density (W Energy density (Wh Specific capacitance (F/ Refs.
(V) kg− 1) kg− 1) g)
Cr2O3 nanoparticles 6 M KOH 1V 312.5 12.5 340 [46]

Ni3BHT 1 M LiPF6 1.7 V – – 227 [47]
PHATN 6 M KOH 1V – – 686 [45]
Co3V2O8 – – – – 790 [48]
Fe-Alco-doped α-Ni(OH)2 and Ni(HCO3)2 6 M KOH 0.5 370 30.27 495.6 [49]
composites
FeCo2O4 NSs@NiO NWs composite 3 M KOH 0.5 – – 4746.2 [50]
MoS2/rGO 1 M H2SO4 1.5 370 23.0 361 [51]
TGCN/PANI – – 400 33.57 298.31 [52]
MnCo2O4 HSs/NF – – 250.1 37.1 648.4 [53]
THPP-PA-Mn 1.0 M Na2SO4 1 1000 12.6 90.9 [54]
VO(OH)2/CNT 1 M LiClO4/PC 2.2 63.65 32 265 [55]
NiCoHC/CDs 6 M KOH 1.5 – – 1964.6 [56]
CuFeS2 1 M LiOH 1.4 166 4.74 95 [57]
of specific capacitance was strongly dependent on the nitrogen efficient and broadband information exchangeability with living sys
anchoring associated with excellent micropore volume and surface area tems. Han et al. [43] made a wireless optoelectronic pseudocapacitor
of the carbon materials. which utilized dissociation of photogenerated exciton to convert optical
energy to safe capacitive current. Peruifoy et al. [44] synthesized porous
carbon consist of perylene diimide and triptycene sub-units and ana
1.4. Pseudocapacitor lysed the pseudocapacitance properties and got a specific capacitance of
350 F/g. Russel et al. [45] synthesized an organic pseudocapacitor
The concept of pseudocapacitor was first used to explain the material composed of perylene diimide and hexaazatrinaphthylene with
reversible capacitance associated with electrochemical adsorption of single electrode capacitance of 700 F/g in 6-M KOH electrolyte. Thus,
species on the electrode surface, and their electrochemical characteris the combination of complementary organic compounds gives an in
tics resemble the capacitive signature [38,39]. The storage mechanism crease in available energy and molecular contortion to permit both facile
of pseudocapacitors is different from the EDLC due to its non- diffusion and long-range charge delocalization (Table 2).
electrostatic nature. Pseudocapacitors store energy by means of revers
ible faradic redox reaction, and also via adsorption or desorption, at the
electrode surface as in Fig. 6. When a potential is applied across 1.5. Asymmetric capacitors
electrode-electrolyte interface in pseudocapacitor, charge transfer takes
place similar to the electrochemical process in batteries. Thus, the Asymmetric supercapacitors theoretically cover a wide range of en
pseudocapacitance is given by the equation: ergy storage devices consisting of two different electrode materials,
different redox active materials, or the same EDLC carbon with different
dQ surface functional groups. A hybrid capacitor is a special category of
C= (3)
dV asymmetric capacitor [58]. Usually carbon-derived materials are used as
Here, dQ is the charge acceptance and dV is the difference between the cathode, and a metal or metal oxide electrode serves as an anode.
electrode potential. The pseudocapacitors have high capacitance and Metal electrodes have a high intrinsic volumetric capacity and, thus,
power density compared to EDLC due to surface active redox reaction high energy densities and cycling stability than symmetric super
and possesses fast discharge than batteries. capacitors. This is the case seen for carbon and MnO2 on nickel foam-
For pseudocapacitor, the total capacitance is the sum of pseudoca based electrode because of the desirable porous structure, high spe
pacitive contribution through electronic charge transfer and the electric cific capacitance and rate capability of electrode materials, and the
double layer component at the electrode and electrolyte interface. capability to be cycled in wide potential range [57,58]. The self-
Pseudocapacitance is a faradic charge storage mechanism based on fast discharge of a capacitor can be handled by incorporating an asym
and highly reversible surface or near surface redox reaction. However, metric capacitor with the simple rocking-chair mechanism. [61]. By
the electrical response of EDLC and pseudocapacitor is ideally the same using this functionality, the maximum potential is ensured at zero cur
[39]. A material can have intrinsic or extrinsic pseudocapacitance rent. Over time, it is observed that with nearly all electrolytes, a
depending upon the ranges of particle size and morphologies of the depletion of ions and electrodes causes a decrease in conductivity and an
material [41]. Pseudocapacitors and battery materials can also be increase in internal resistance. The newly designed electrolytes could
distinguished by electroanalytical methods, with their kinetics being feasibly evade this pressing concern. Attaining high operating potential
limited by surface related process as opposed to diffusion-controlled is also a challenge to overcome. [60]. There are two main parameters as
reaction governing the electrochemical response of battery electrode. in the case of asymmetric supercapacitor,
In a pseudocapacitive electrode, different charge storage mechanism can
1
be distinguished such as underpotential deposition, redox reaction of Energy density E = Ccell V2 (4)
2
transition metal oxides, intercalation pseudocapacitance, and reversible
electrochemical doping and de-doping in conducting polymers [40]. The The energy stored by capacitor (E) is proportional to the cell
capacitance of pseudocapacitor is usually higher than that of EDLC, but capacitance (Ccell) and the voltage difference between electrodes (V).
the power performance is lower due to slower faradic process involved The maximum power output Pmax is given by,
[41]. Pseudocapacitive electrodes have more chances for swelling and /
Power density Pmax = V2 (4*ESR) (5)
shrinking on charging and discharging cycles, leading to poor mechan
ical stability and low cycle life [42]. These electrodes are mainly oxide The voltage depends on the type of electrolyte used. Based on elec
metals, carbon doped with metal, and polymers owing to conductive trolyte the asymmetric supercapacitor is further divided into aqueous
property. and non-aqueous.
The integration of pseudocapacitor and organic photovoltaics has Boota et al. [62] synthesized three conducting polymer containing
5
Table 3
Summary of various Asymmetric capacitor electrode materials based on carbon materials.
Electrode material Electrolyte Cell voltage Power density (W kg-1) Energy density (Wh kg− 1) Specific capacitance (F/g) Refs.
Ni–Co–Mn hydroxide//AC 3 M KOH 1.6 1650 44.4 117.45 [63]

Ni-Mn hydroxide//AC 3 M KOH 0.5 1703 42.8 1680 [64]
GdMnO2/Ni(OH)2// PVA/KOH 1.6 2332 60.25 – [65]
Fe3O4/GO
Fe-SnO2@CeO2/// 2 M KOH 1.5 32.2 7390 348 [66]
AC
NiMoO4/NiO// AC 3 M KOH 1.7 96.2 38 1982 [67]
CoP@NF// 6 M KOH 0.8 325 24 1349 [68]
CMK-3@NF a
Mn(PO3)2/NPG//Mn(PO3)2/NPG 6 M KOH 0.6 726.73 96.2 213.8 [69]
NPCN/MnO2-f// 1 M Na2SO4 1.8 182 41.5 96 [70]
NPCN-f
NiCo2O4@NiMoO4/NF// 6 M KOH 1.5 750 64.2 2806 [71]
AC
MoS2-MoO2/3DSG// 6 M KOH 1.7 683.94 87.38 1150.37 [72]
FeS2/3DSG
CeO2/NiV–LDH (2:2)//Bi2O3 3 M KOH 1.6 1595.2 62.5 – [73]
K-MnO2//AC 1MNa2SO4 2.2 550 56 366 [74]
NiCo2Al-LDH/N-GO//AC 2 M KOH 1.6 11.39 42.25 80 [75]
NiCo2S4/NF// 6 M KOH 1.8 9568.3 45.4 203.4 [76]
T-Nb2O5/3DNG
NCS/C// PC 2 M KOH 184.4 53.7 154 [77]
Fig. 7. Schematic representation of different hybridization possible between battery and supercapacitor materials.
hybrids and used oxidative polymerization to deposit on rGO. They An example of basic asymmetric supercapacitor is an activated car
compared the electrochemical properties of asymmetric capacitor using bon (EDLC) anode and Li4Ti5O12 (Faradaic electrode) cathode in an
a rGO polymer cathode and MXene anode in 3-M H2SO4 in the potential organic electrolyte [80]. The combination of materials, electrodes, and
window of 1.45 V. The PANI-containing device showed an energy the combination of the whole supercapacitor and battery either in ma
density of 17 K Wh kg− 1 and 88% capacitive retention, after 20,000 terial level or device level comes under the category of hybrid devices
cycles (Table 3). and are known as internal and external hybrid devices, respectively
[81], as depicted in Fig. 7. At the device level, the EDLC and the battery
can be integrated into modules in tandems. A device-level energy stor
1.6. Hybrid capacitors age system requires power-conversion electronics to manage both de
vices independently. Because of these requirements, device-level hybrid
The concept of hybrid supercapacitor came into existence to enhance systems are multicomponent and generally suffer from manufacturing
the energy density to a range of 20–30 Wh kg− 1. The mechanism and complexity, higher cost, and increased weight or volume. Hence,
storage principle of hybrid capacitor is the combination of EDLC and material-level hybridization is better than external hybridization. In
pseudocapacitor depending on the configuration, whether symmetric or material-level hybridization, one electrode is capacitive in nature
asymmetric. When composed of two different electrodes from different (pseudocapacitive or EDLC) and the other has a battery-level charge-
materials, hybrid supercapacitors show better electrochemical proper storage process.
ties than individual ones and have better cycle stability and affordability The total performance of hybrid capacitors is determined by the
[78]. Thus, the commercially available hybrid supercapacitors are electrodes and electrolyte. As discussed in the previous section, the
asymmetric with conducting polymer electrodes are of prime interest classification of hybrid electrodes is based on dominant electrode
[79].
6
Fig. 8. Schematic diagram of metal ion capacitor [84].
behaviour. The first classification consisting of composite electrodes

comprises incorporated carbon with either conducting polymers or
metal oxides. The second class of hybrid supercapacitors comprises two
different materials with redox properties, while the third type of
supercapacitor contains a battery-type material electrode and super
capacitor electrode [16]. The hybrid capacitor, which consists of a
battery and supercapacitor electrode, exhibits better performance. This
review will be primarily focussed on supercapacitor-battery hybrid
(SBH) devices with electrodes based on advanced carbon materials.
Along with this, the detailed mechanisms of metal ion capacitors like
lithium-ion capacitor (LIC), sodium-ion capacitor (SIC), potassium-ion
capacitor (KIC), along with the recent electrochemical properties, will
also be discussed in the subsequent sections.
During the charge and discharge process of SBH, anions or cations
move to the electrodes, and bulk redox reactions happen at battery-type
electrodes while ion accumulation or separation or rapid-charge transfer
occur in capacitive electrodes, so the electrons flow through the external
circuit [82]. The energy density can be improved by: (i) capacitive
improvement, e.g., the capacitance of SBH can be increased by 2×
compared with EDLC since the capacity of battery electrode is higher
than that of the capacitive electrode, (ii) Voltage expansion, e.g., by
choosing the appropriate battery-type electrode that works in separate Fig. 9. Schematic diagram of mechanism of LIC [90].
potential range, output voltage of full SBH and full capacitance can be
used [83]. A typical metal ion capacitor is given in Fig. 8. The SBH can additives which enhances the composition features. As discussed earlier,
show capacitive performance similar to a convectional capacitor with an aqueous electrolyte has the advantages of higher ion mobility and
linear galvanostatic charge discharge diagram (GCD) and rectangular low viscosity, but has only low potential window up to 1.2 V. Alkaline
cyclic voltammogram (CV). The fundamentals of capacitors are appli sulphates (Li2SO4), nitrates (LiNO3), as well as hydrates (LiOH) are some
cable here where the capacitance (C) is directly proportional to the aqueous electrolytes that are commonly used [88]. LIC can be divided
charge stored (Q) and the potential difference between the electrodes into two types as described below and expressed in Fig. 9 [89].
(V).
Q (i) Capacitor-type electrode acting as cathode and battery-type
C= (6) electrode as an anode, e.g., LTO//AC system: During charging,
V
the anions get absorbed in the pores or in the defects of cathode
1.6.1. Li-ion capacitor (LIC) and Li + ions get intercalated on to active material of the anode.
Among the different nonaqueous metal-ion supercapacitors, LIC has On the other hand, while discharging the absorbed anions are
attained the most attention. The first supercapacitor-battery hybrid was released from cathode and Li ions are deintercalated from anode.
a lithium-ion supercapacitor fabricated by using a nanostructured (ii) Battery-type electrode acting as cathode and capacitor type
Li4Ti5O12 (LTO) anode and an activated‑carbon (AC) cathode [85]. LIC anode, e.g., AC//LiFePO4 system. Here, during charging, the Li+
has a high-energy lithium insertion/desertion-type electrode and high- ions de-intercalate from cathode and enter into the electrolyte. At
power EDLC-type electrode by physical adsorption or desorption the same time, Li+ ions in the electrolyte migrate and are
behaviour using an appropriate LIB-EDLC hybrid electrolyte [84]. adsorbed in the anode. The discharge process will be reversed.
Because it is hybrid in nature, it has a property of LIB and supercapacitor
viz. high specific energy, high cycle life, high specific power, etc. [86]. The energy density of LIC is given by,
The anions are adsorbed to/desorbed from the anode with high surface ∫
area as well as intercalation/de-intercalation of Li-ion occurring at the E = V dq (7)
cathode during a charge/discharge process [87]. Also, the electrolyte is
responsible for the storage of charges inside the cell and can be aqueous V is operating potential and q is the capacity. At the surface of
or non-aqueous. The electrolyte has three main components: i) Li salt as capacitor, electrode has a reversible ion adsorption or fast redox reac
the charge carrier, ii) the solvent to dissolve components, and iii) tion that helps to have a power density comparable to that of
7
Fig. 10. Effect of electrolyte parameters on energy storage (ES) devices.
supercapacitors. For practical applications of LIC, its lifespan as well as has capacitive behaviour as well and capacitive material contain
cycle life is important. The mass ratio between the battery electrode and partially faradic reactions. This helps to improve the cathode capacity
supercapacitor electrode play an important role in the cycle life of LIC and hence the power and energy density of SIC. Hence, the way of
[91]. For an asymmetric cell, charges of both electrodes should be determining capacitive and faradic contribution are important in the
balanced (Q anode = Qcathode). The charge stored can be expressed as Q = case of SIC [99]. The faradaic and capacitive contribution can be
C*m, where, C is specific capacity and m is mass of electrode. Then the determined from the cv graph by using power law equation:
optimized mass ratio between capacitor type and battery type can be
I = avb (8)
calculated according to the following Eq. [92]:
Here, I and v are current and sweep rate; and ab are adjustable pa
m(cathode) C(anode)*ΔE anode
= (8) rameters. The carbon derived materials used in SIC are discussed in the
m(anode) C(Cathode)*ΔEcathode
upcoming sections.
where, C, m, and ΔE are the specific capacitance, mass of electrode, and
potential window for the cathode and anode, respectively. It is note 1.6.3. Potassium-ion capacitor (KIC)
worthy that the fabrication of carbon materials with high capacity is the Potassium-ion capacitors can be considered as an alternative for LIC
primary aim of LIC since the capacitance of capacitor is comparatively and SIC since the availability of potassium in the earth's crust is larger
less to that of battery-type electrode [90,91]. Hence, to improve the than that of Li as well as its low-cost. Here, aluminium foil can be used as
capacitor electrode, the specific surface area and porosity have to be current collector instead of Cu, further reducing the manufacturing cost
enhanced along with introducing pseudocapacitive material or hetero [100]. Since the chemical and physical properties K and Li are similar,
atom doping [92–95]. The developments in carbon derivatives used is LIC and KIC have similar working principles. The larger size of K+ ion
discussed below. can cause destruction of electrode structure and, thus, can restrict
development of battery type electrode. In KIC, the K+ ions are stored in
1.6.2. Sodium-ion capacitor (SIC) battery-type material and an intercalation reaction is the dominant
The sodium-ion capacitor (SIC) consists of two electrodes with one charge storage mechanism. The battery-type materials requires large
capacitive property and the other battery-like properties along with an channels for storing the K+ ion [101]. In capacitor type materials, charge
electrolyte and separator [96]. As with the LIC, the capacitive electrode storage is done by adsorption and desorption on the surface. In 2012,
can be anode or cathode and the battery-type as the counter electrode Chen and co-workers [102] proposed the first nonaqueous sodium-ion
[97,98]. capacitor device using 1-M NaClO4 in propylene carbonate (PC) elec
Since it is a hybrid device, it has storage mechanism similar to trolyte. An interpenetrating network composite composed of layered
sodium-ion battery and SC [98]. As in the first case, capacitive cathode V2O5 nanowires and carbon nanotubes (CNTs) was synthesized by using
stores charge through EDLC mechanism and anode faradaic reaction a simple hydrothermal process. Such architecture facilitates fast sodium
occurs in the bulk of electrode materials. The energy density of SIC can ion insertion/extraction and electron transfer [102]. The carbon-based
be determined from the same equation as that of LIC. Various materials electrode materials used in KIC will be discussed in the subsequent
like hydroxides, sulphides, transition metal oxides, etc., are designed sections.
into various forms of nanostructures in which the electrochemical
property could be neither purely capacitive nor faradic. The advanced
electrode materials for SIC anticipate that battery-type material partially
8
Fig. 11. Classification of electrolyte.
1.7. Electrolytes in SBH devices potential window, the aqueous electrolyte decomposes into hydrogen
and hydroxyl ion [106–108]. The aqueous electrolytes have both high
An electrolyte is a key component in electrochemical energy storage capacitance and conductance but are lacking in cycle stability, energy
devices (EESD) to conduct electricity by means of ion transport, with a density, and leakage problems. Neutral electrolytes are more promising
great impact on cycle stability, rate performance, energy capacity, and among the aqueous electrolytes because they are less corrosive, less
safety of devices. To increase the power and energy density, increasing expensive, and more environmentally friendly, and hence are used more
the potential window is a best option, which demands new electrode and frequently. Inorganic salt solutions, such as lithium, zinc, magnesium,
electrolyte material that are chemically, physically, and electrochemi potassium, and sodium salts are the most used aqueous neutral elec
cally stable in the potential window. In general, an electrolyte is either a trolytes [98,102]. On the other hand, for organic electrolyte and ionic
liquid or solid, and basically is an ionic conductor but an electronic liquid, the potential window is higher but, possesses low ionic conduc
insulator [103]. According to the principles and purpose of EESD, an tivity. Ionic liquids, another type of electrolytes, are pure liquid salts in
electrolyte should have following properties: nature and are defined as room-temperature liquids composed of cations
and anions with a melting point at or below room temperature. Also
i. Wide potential window known as room temperature molten salt or liquid organic salt [109],
ii. High chemical and thermal stability they have wide liquid temperature range, practically zero or negligible
iii. High ionic conductivity volatility, highly ionized environment, and a large potential window
iv. Nontoxic and safe [110]. On the other hand, the solid state electrolytes avoid potential
v. Economically viable leakage issues but have low conductivity [111]. Halder et al. [113]
vi. Chemical inertness to the other components constructed an alkaline supercapacitor-battery hybrid device using NS-
doped reduced CTH@NG and graphene in 1-M KOH with an excellent
As discussed in the previous section, the development of electrolytes energy density of 53.8 Wh kg− 1 and power density of 800 W kg− 1 [112].
or solutions with large potential window is equally important as that of A dual‑carbon cation electrolyte consisting of Li+ and spiro-1,1′ -bipyr
efficient electrode material. On the other hand, the size of the electrolyte rolidinium (SBP+) was also proposed for an LTO//AC asymmetric
ion should match with the pore size of the electrode material. The factors capacitor with high energy and power density [113].
affecting the performance of ES are shown in Fig. 10. The ionic con
ductivity, ion mobility, and viscosity of electrolyte affect the internal 2. Carbon nanomaterials: types, properties, synthesis strategies,
resistance of the energy storage devices. The aging and cycle life sta and applications
bility depends on the decomposition of electrolyte [104].
Different types of electrolytes have been developed. They are clas The development of novel carbon nanomaterials gives rise to new
sified into liquid, solid, and redox active electrolyte, as in Fig. 11. The fields and directions in research. From fullerenes and carbon nanotubes
potential operating windows of aqueous, organic, and ionic liquid discovered from last century to graphene and carbon quantum dots in
electrolytes are in the range of 1 to 1.2 V, 2.5 to 2.7 V, and 4 V, this century, researchers and industry departments have been paying
respectively [105]. If the applied voltage exceeds the corresponding close attention to carbon nanomaterials. [114]. Carbon nanomaterial
9
Fig. 12. Different allotropes of carbon [116].
with high surface area and porosity are suitable materials for electro biomass, etc. [8,101,102]. The outstanding mechanical, thermal, and
chemical energy storage devices [115]. Fig. 12 shows different types of electrical properties of graphene have led it to a promising electrode
allotropes of carbon and carbon derivatives that can be used for such material for the fabrication of energy storage devices. Large surface
purpose. area, good electrical conductivity, strong van der Waals force of
Activated carbons were the first material used for making EDLC, and attraction, and micoporosity enhance the importance of this material. It
the first choice for metal-ion capacitors and also the only electrode was also reported that graphene was used as an electrode material since
material that achieved successful commercialization. It is an excellent it's electrochemical properties do not depend on the distribution of pores
carbon material that has been put through physical and chemical pro at solid state, as compared to other carbon materials such as AC, CNT,
cesses to enhance porosity, conductivity, and surface area [117]. By etc., [121–123]. Graphene has a surface area of up to 2630 m2g− 1 [124].
incorporating materials like metal oxides, conducting polymers, or other The higher surface area increases the electrochemical performance of
carbon material, the properties of activated carbon are improved easily material. If the entire specific surface area is utilized, graphene has the
[118]. In comparison with the porous‑carbon materials, activated car potential of achieving specific capacitance of 550 F/g, also if it is single
bon got great attention due to its lower cost of manufacturing; large layer graphite, both of the surfaces easily accessible to electrolyte [125].
range of operating temperature; cycle stability; good chemical corrosion Various methods are available for the synthesis of graphene including
resistance; and having various available resources like wood, bio-waste, chemical vapor deposition (CVD), arc-discharge method, micro
coal, etc. The chemical activation involves a low-temperature heating mechanical exfoliation, epitaxial growth, unzipping of CNT, electro
(400-800 ◦ C) with activating agents like KOH, NaOH, Phosphoric acid, chemical and chemical methods, and intercalation methods [126–130].
Zinc chloride, etc.. Physical activation usually involves high tempera In order to use the maximum intrinsic surface capacitance and specific
ture treatment of carbon materials from 800 to 1000 ◦ C in presence of surface area of single layer graphene, it is required to prevent restacking
oxidizing gases like CO2, air, and steam. Depending on the raw material of graphene sheets in the synthesis step.
and activation method used, AC shows various physicochemical prop The discovery of carbon nanotubes (CNT) was a significance
erties with well-developed surface area up to 3000 m2g− 1 [119]. advancement in science and engineering of carbon nanomaterials. A
Depending on the porosity of synthesized AC, it can be divided into great attention was given to CNT due to its unique pore structure, good
microporous (<2 nm), mesoporous (2–50 nm), and macroporous (>50 electrochemical properties, and excellent mechanical and thermal sta
nm) [120]. bility [91]. It has mesopores that are interconnected, allowing contin
Graphene is considered as one of the advanced carbon nanomaterials uous charge distribution that utilizes almost all of the accessible surface
which is a two dimensional solitary sheet of carbon atoms [13]. Gra area. Since the electrolyte ion can diffuse into this mesoporous network,
phene has been synthesized from various precursors like coal, graphite, graphene has a lower ESR value than the AC [126]. CNT is classified into
10
Fig. 13. Schematic Illustration of (a) As-Synthesized 1 D Carbon-Based Materials; (b) Assembled Asymmetric Supercapacitor; and (c) Asymmetric CDI Device [138].
single-walled and multiwalled based on the number of layers and are 2.1. Carbon materials for symmetric supercapacitor
used as an electrode material [103,104]. The readily accessible surface
area and good electrical conductivity made them a high-power electrode Based on the composition of electrode materials, electrochemical
material capable of giving good support to active materials due to their capacitors can be symmetric, asymmetric, and hybrid. The symmetrical
high mechanical resilience and open tubular network. Even though the supercapacitor consist of two identical electrodes in terms of chemical
specific surface area is less compared to activated carbon, it can be composition and mass regardless of whether both electrodes exhibit a
activated chemically by using KOH, NaOH, etc., or can be decorated pure capacitive or pseudocapacitive behaviour [131]. Porous carbon,
without affecting its nanotubular morphology [105,106]. commonly activated carbon, is used as the electrode material in both
aqueous and organic electrolytes. The size and shape of pores can be
tuned, enabling access of the high surface area of the ACs by the solvated
11
Fig. 14. Stepwise fabrication of asymmetric supercapacitor device [139].
ion clusters during operation in a wide temperature range of − 100 to supercapacitors (ASCs). Ding et al. [136] put forward a strategy inspired
60 ◦ C [132]. As discussed above, an electric double layer requires high from biomimetic mineralization to synthesize a hierarchical flower-like
surface area carbon-electrode material in aqueous or organic electro Mn3O4@N, P-doped carbon composite in which, Mn3O4 nanosheets
lytes. They can be fabricated as spirally wound or button cells. Various offer large active regions, and their covalent C-O-Mn bonds with NPC
carbon materials such as activated carbon, carbide-derived carbons, ensure the fast electron transfer kinetics. A 2.6-V flexible aqueous
graphene, carbon aerogel, porous carbon, carbon nanotubes, and carbon asymmetric supercapacitor (FAAS) was fabricated by integrating an
onions have been used as supercapacitor electrode material [59]. For Mn3O4@NPC cathode with an electrochemically reduced porous‑carbon
aqueous electrolytes, safety and low cost are of crucial importance from anode and a PVA-Na2SO4- hydrogel electrolyte that can deliver a high
the industrial point of view. Due to potential limitation, aqueous-based energy density of 76.96 Wh kg− 1 at a power density of 1.30 kW kg− 1
symmetric capacitors are still one order-of- magnitude smaller [136]. Sun and co-workers [137] prepared a composite electrode with
compared to aqueous-free electrolytes. To improve cell voltage, organic vanadium pentoxide (V2O5) and carbon nanotube arrays by supercritical
and ionic liquids are used which got a high decomposing potential but CO2 impregnation and subsequent annealing and used it as a binder-free
are expensive and toxic. Due to high conductivity and environmental negative electrode for aqueous ASCs. The asymmetric capacitor showed
friendliness, aqueous electrolytes are still promising. In comparison with energy density of 32.3 Wh kg− 1 at a power density of 118 W kg− 1 and
acidic and alkaline electrolytes, neutral electrolytes can endure high capacitance retention of 76% after 5000 cycles in the potential window
potential window due to low hydrogen or hydroxide concentration in a 1.7 V [137]. Even though carbon-based materials are desirable in areas
neutral medium. A facile carbon-surface passivation strategy by rational such as supercapacitors and capacitive deionization, the traditional
functionalization with fluorine-containing functional groups can in commercial materials are heterogeneous and prone to agglomeration at
crease the energy density of activated carbons [133]. The carbon nanoscale with structural limitation of electrochemical and desalination
nanofiber recovered from carbon fiber reinforced polymers through an performance due to poor transport channels and low capacitance of
aerobic process of air can work in a potential window of 2.4 V in 1-M prepared electrodes. Zhang et al. [138] introduced the facile strategy for
Na2SO4 with a capacitive retention of 93% after 10,000 cycles [134]. controllable preparation of two types of hollow carbon-based nanotubes
A hybrid electrolyte based on superconcentrated LiFSi with hybrid (HCTs) with amorphous mesoporous structures, which are synthesized
ethylene carbonate/dimethyl carbonate and water electrolyte can be by employing a MnO2 linear-template method and calcination of poly
used in a symmetric supercapacitor fabricated using activated carbon. mer precursors as shown in Fig. 13. The fabricated asymmetric MnO2//
This electrolyte shows properties of both aqueous and non-aqueous NHCT supercapacitor displays the energy density of 55.8 Wh kg− 1 at a
electrolyte and a potential window of 2.5 V [135]. power density of 803.9 W kg− 1.
Kaipannan and Marappan [139] reported the fabrication of an
asymmetric capacitor using Ni(OH)2 nanosheets and activated carbon as
2.2. Carbon materials for aqueous asymmetric capacitor positive and negative electrodes in 3.5-M KOH. The asymmetric super
capacitors stack connected in series exhibited a stable device voltage of
Carbonaceous material can be either used as a cathode or anode 9.6 V and delivered a stored high energy and power of 30 mWh and
following different action mechanisms [124]. A capacitive asymmetric 1632 mW, respectively. The fabricated device shows an excellent elec
supercapacitor means the device involves pseudocapacitive or capaci trochemical stability and high retention of 81% initial capacitance after
tive electrodes, while a hybrid capacitor refers to a device pairing 100,000 charge-discharges cycling at high charging current of 500 mA.
electrodes with different charge-storage mechanisms. Aqueous Li-ion The positive electrode material Ni(OH)2 nanosheets was prepared
SBH is another attractive hybrid device due to its nonvolatility, non through chemical decomposition of nickel hexacyanoferrate complex
toxicity, and nonflammability along with high ionic conductivity of which is given in Fig. 14. In that study, the negative electrode, activated
aqueous electrolyte. Optimizing the performance of electrode materials porous carbon (OPAA-700) was obtained from orange peel waste
is crucial for improving the energy density of aqueous asymmetric
12
Table 4
Summary of various carbon materials for aqueous asymmetric capacitors.
Positive electrode Negative electrode Electrolyte Potential window Energy density (Whkg− 1) Power density (W g− 1) Refs.
MnMoO4@MWCNT Activated carbon 1 M KOH 0.45 18.1 362.4 [140]

HNCXs/Mn3O4 HCXs 1 M Li2SO4 2.2 44.5 5600 [141]
W18O49 NWs-rGO rGO AlCl3 28.5 751 [142]
NiS/ACNT AC 36 806 [143]
MnO2@ Carbon cloth TiO2@ Carbon cloth 6 M KOH 2.6 – – [144]
Ni-Co hydroxide/ AC 1 M KOH 1.6 34.7 1550 [145]
rGO/CNT
Mn3O4-Graphite paper AC 1M Na2SO4 1.6 47 2024 [146]
CoS/graphene AC 2M KOH 1.5 29 800 [147]
Co0.85Se N-doped porous carbon network 2M KOH 1.6 21.1 400 [148]
N doped porous carbon 1M H2SO4 1.6 26.3 404.2 [149]
K0.3WO3
VS2 nanosheets AC 6 M KOH 1.4 42 700 [150]
N-C/MnO2 N-C/Fe2O3 5 M LiCl 1.6 – – [151]
Fig. 15. A simple schematic classification of cathode anode material for LIC.
exhibiting a high specific capacity of 1126C/g and high specific capac type electrodes in LIC [154–159]. The capacitance depends mainly on
itance of 311 F/g at current density of 2 A/g, respectively (Table 4). the ion adsorption and desorption on the surface of carbon-based elec
Thus, the Ni(OH)2 nanosheets delivered a good rate performance and trodes [147,148]. In LIC, the electrochemical performance of carbon
remarkable capacitance retention of 96% at high current density of 32 materials are also significantly affected by the porosity and pore size
A/g [139]. distribution, and, to provide pseudocapacitance, some functional groups
are also introduced. [52,53] [161]. It is observed that the carbon ma
terial development is progressing, leading to the advancement of prop
2.3. Carbon materials for non-aqueous metal-ion capacitor
erties of LIC [162].
In LIC, activated carbon is the first electrode material of choice and
2.3.1. Li-ion capacitor
the only material which successfully achieved commercialization. On
The energy and power density of depend mainly on the design of
the other hand, to increase the operation voltage between the electrodes,
electrode materials in the devices [142,143]. Therefore, different ma
hybrid LIC's with asymmetric graphene electrodes are used. There is a
terials like polyanions, metal compounds, and metalloid/metal com
lack of a lithium ion source in graphite/activated carbon hybrid systems
pounds have been used in LIC for battery-type electrodes due to their
[163]. Therefore, pre-lithiation is suggested to enhance energy storage
good electrochemical performance and high gravimetric specific ca
capacity and electrical conductivity of electrodes. It is reported that after
pacity. A simple schematic classification of cathode anode material for
pre-lithiation, the lithiated-SG (Li-SG) electrode showed excellent ca
LIC is give in Fig. 15. The factors like large volume variation, less con
pacity in lithium intercalation and de-intercalation and was used as the
ductivity, and high polarization, etc., limit further development of
anode of the LIC device which exhibited energy density of 222 Wh kg− 1
electrodes in LIC. As a solution, carbon materials were often incorpo
at a power density of 410 W kg− 1 [164]. An important limitation to LIC
rated into due to properties like high surface area, excellent electrolyte
technology is the kinetic imbalance between the capacitive electrode
accessibility, and high conductivity. It can also act as an active material
and Faradaic insertion electrode. Shen et al. [165], demonstrated Li3VO4
of battery-type electrode in LIC directly because of the presence of active
with low Li-ion insertion voltage and fast kinetics and used in lithium-
sites for Li+ intercalation/deintercalation [144,145]. Rather than
ion capacitors. A new kind of LIC has been fabricated by using the
battery-type electrodes, different large specific surface area
Li3VO4/NC nano wires as an anode and activated carbon (AC) as a
porous‑carbon materials like graphene, activated carbon, biomass-
cathode. From the voltage profiles of Li3VO4 and AC, the maximum
derived carbon are some of the promising candidates for capacitor-
13
(a) SEM ,TEM images of Li3VO4 NC Nano wires [165]
(b) Electrochemical evaluation of the Li3VO4//AC LICs [165]

Fig. 16. (a) SEM,TEM images of Li3VO4/NC Nano wires [165]
(b) Electrochemical evaluation of the Li3VO4//AC LICs [165].
work voltage is estimated to be 4.2 V and delivers a high energy density reports are available for an easy, eco-friendly, and cheap synthesis
of 136.4 Wh kg− 1 at a power density of 532 W kg− 1. The SEM, TEM, and method to synthesize carbon composite from pyrolysis/activation of
electrochemical analysis of Li3VO4/NC Nano wires is summarised in coffee waste and graphene oxide [149]. The optimized electrodes are
Fig. 16 (a) and (b) [165]. used as dual‑carbon LIC in terms of power, energy, and cyclability with
Biomass-derived products also can be used in this purpose and an energy 100 Wh kg-1 at power density 9000 W kg-1. The kenaf plant
14
Fig. 17. Schematic illustration and electrochemical analysis of M-Co9S8@NCF//PNCF LIC [171].
can also be used as biomass carbon precursor for the synthesis of porous additives like carbon black creates a synergetic effect on improving the
activated carbons which was used as a cathode [166]. The LIC showed a cycle stability and rate capability. Using AC as anode and SiOx modified
specific capacity 195 mA h g− 1 at a current rate of 0.1 A g− 1good rate with CB can reach 1549 mAh g− 1 in the voltage range of 0.01–2.0 V
capability at current rates ranging from 0.1 to 4 A g− 1, and excellent [170]. A convenient method to construct metal sulfide-based free-
cycling stability in organic electrolyte [166]. Carbons materials derived standing electrode for the advanced lithium-ion storage devices was
from bio-waste are more useful because they can easily store energy due offered by Zhang et al. [171], in which Co9S8 nanoparticles embedded
to their high conductivity and surface area. However, their large-scale on melamine foam derived three-dimensional (3D) carbon foam (M-
processing is challenging as derived materials can be rather heteroge Co9S8@NCF) was successfully constructed by an in-situ anchoring and
neous and homogenization requires ball milling, a process that can annealing method; and porous nitrogen-doped carbon foam (PNCF) was
damage carbons via oxidation. However, caffeine-derived noble synthesized as the cathode. M-Co9S8@NCF//PNCF LIC device was then
nitrogen-doped carbon was prepared that withstands the ball milling fabricated, which achieves a high energy density (166 Wh kg− 1 at 182
process without significant oxidation which is found to be a good per W kg− 1), high power density (83 Wh kg− 1 at 7674 W kg− 1), as well as
formance cathode material for LIC in 1-M LiPF6 in ethylene carbonate satisfactory capacitance retention (83.5% at 5 A g− 1 after 5000 cycles)
and diethyl carbonate electrolyte [151]. Lin et al. [167] synthesized which is given in Fig. 17. A general and effective protocol for ultrafast
porous carbon from biomass through the pyrolysis of rubber wood and manufacturing of graphene-based carbon materials toward high-
used as a cathode along with lithium titanate (LTO) as anode. The performance LIC was also provided by An et al. [172]. The fast self-
synthesized carbon showed great surface area, 1365 m2/g, and good propagating high-temperature synthesis (SHS) method used for the
electrochemical properties. However, the kinetic mismatch usually synthesis of graphene/soft carbon (G/SC) composites and graphene/
arising in LIC was overcome by using spray-dried LTO modified through activated carbon (G/AC) composites. G/SC exhibits superior rate capa
ionic doping and surface coating [167]. On the other hand, using bility of 200 mA h g− 1 at 4 A g− 1 along with a high specific capacity of
quantum dots can reduce the volumetric stress, shorten migration dis 360 mA h g− 1 at 0.1 A g− 1. G/AC exhibits a greatly enhanced conduc
tance of Li ions, and improve anodic dynamics. Lian et al. [168] used tivity of 2941 S m− 1 and good capacity retention of 84% at 10 A g− 1. The
quantum dots-coated nitrogen-rich biomass carbon prepared by simple LIC fabricated using G/SC and G/AC exhibited high energy density of
and green hydrothermal-annealing method. The carbon derived from 151 Wh kg− 1 and a high-power density of 18.9 kW kg− 1 [172]. More
egg can improve composite conductivity and Li+ redox kinetics and, over, G/SC is synthesized on a large-scale and assembled into a large-
hence, the electrochemical performance [152]. The assembled T- capacity LIC pouch cell (1170 F or 650 mA h), which shows an excel
Nb2O5@NC//NCC delivers remarkable power density (8750 W kg− 1), lent energy density of 31.5 W h kg− 1 and 93.8% capacity retention after
energy density (67.2 Wh kg-1), and good long cycling durability (82.1%) 10,000 cycles at 50 ◦ C.
and capacity retention after 3000 cycles [153]. Je•zowski et al. [173] uncovered a unique approach based on the use
For LIC, electrode potential tuning has been widely regarded as an of a lithiated organic material, namely 3,4-dihydroxybenzonitrile
efficient technology to improve the performance, in which a mostly pre- dilithium in combination with AC. This compound can irreversibly
lithiated anode is used for desired potential. Qin et al. [169] reported provide lithium cations to the graphite electrode during an initial
precious regulation of cathode potential from N-doped carbon nano charging step without any negative effects with respect to further
sheets and paired with pre-lithiated anode. This can optimize potential operation of the LIC. Thus, it promotes a much safer and economical
window (1.6–4.5 V) and specific capacitance and also enhance a 17-fold electrochemical system by the suppression of auxiliary lithium electrode
increase in energy density, power density, and cycle stability. Silicon- when compared with conventional LIC. A low lithium-extraction po
based anode material has limited electrical conductivity and using tential minimizes the risk of electrolyte electrochemical oxidation and a
15
Table 5
Summary of various Carbon materials used for Li-ion capacitor.
Anode Cathode Potential Energy density Power density Cycling stability Ref.
window (V) (Wh kg–1) (W kg− 1)
Graphene with oxidized- N,P co-doped porous AC 0.02–4.3 170.6 216 [174]
polydopamine coating
Co-NCF/G AC 77.17 6801 [175]
Sorghum core-derived carbon sheets Sorghum core-derived carbon sheets 4.5 124.8 107 66% capacity retention after [176]
5000 cycles
Nitrogen doped Nitrogen doped 4.5 206.7 225 0.0013% capacitance decay per [160]
carbon nanospheres carbon nanospheres cycle within 10,000 cycles
Silicon/flake graphite/carbon biomass-derived porous carbon 2–4.5 159 945 80% capacity retention rate [177]
nanocomposite after 8000 cycles
Nitrogen-doped porous carbon nitrogen-doped porous carbon 2–4 95.08 300 80.1% capacity retention after [178]
microsphere microsphere activated 5000 cycles
Porous MnO@C PC-75 0–4.5 117.6 410 76% capacity retention after [179]
nanocubes 3000 cycles
Sn-C Biomass derived activated carbon 2–4.5 195.7 731.25 70% retention after 5000 cycles [180]
Co3ZnC@N-doped Carbon microporous carbon cathode 1–4.5 141.4 10.3 k 80% capacity retention after [181]
nanopolyhedra 1000 cycles
Si/Cu bilayer fabric AC 1.5–4.2 210 193 90% capacity retention after [182]
30,000 cycle
Hard carbon LiFePO4/AC 2.0–3.8 20 4200 92% capacity retention after [183]
100,000 cycles
Quinone/ester-based oxygen Quinone/ester-based oxygen 0–4 144 200 70.8% is achieved after 10,000 [184]
functional group incorporated functional group incorporated cycles
Carbon Carbon
rGO decorated with nanosized SnO2 thermally expanded and physically 1.5–4.2 186 142 70% capacity retention after [185]
activated rGO 5000 cycles
SiOx/graphite AC 1–4 29.3 10,000 87.1% capacity retention after [186]
1000
Natural graphite AC 2.8–4.2 196 456 – [187]
Commercial soft carbon activated carbon/Li3N 2–4.1 74.7 12,900 91% after 10,000 cycles [188]
Ti3C2Tx/CNT AC 1–4 67 258 81.3% after 5000 cycles [189]
cNiCo2O4 nanocomposites from MOF VACNF 1–4.2 136.9 40,000 90% retention after 9000 cycles [190]
derivatives
Activated nitrogen-doped graphene Porous nitrogen-doped graphene 4.5 187.9 2250 93.5% retention after 3000 [191]
sheet sheet cycles
ZTO/rGO SCCB 0–4.5 204 112.5 76% of the capacity after 1000 [192]
cycles
Pre-lithiated graphite Zn90Co10-APC 2–4 108 150,000 – [193]
Porous carbon from silkworm Porous carbon from silkworm 2.1–4.5 138.4 495.9 77.8% of the capacity after [194]
excrement excrement 8000 cycles
Defect-rich and N-doped hard carbon NPCM-A 1–4 101.7 250 82.2% capacity retention after [195]
3000 cycles
SnS2/Reduced Graphene Oxide 2D B/N codoped carbon 0–4.5 149.5 35,000 90% after 10,000 cycles [196]
Mn3O4/3D-graphene activated polyaniline-derived 3–4.5 97.2 6250 76.8% after 3000 cycles [197]
carbon nanorods
B,O,N doped AC 2–4.5 203.6 225 84.5% retention after 5000 [198]
Carbon nanosheets cycles
high irreversible capacity promotes a mass reduction when used in Wh kg− 1, a high power output of 14,200 W kg− 1, and an ultra-stable
combination with AC in positive electrode. By replacing customary cycling life that is 90.7% capacitance retention after 10,000 cycles
lithiated transition metal oxides used as a lithium source for graphite [199]. Activated carbon derived from polyimide can retain the original
pre-lithiation in LICs, Li2DHBN offers the possibility to build full carbon/ microflower-like nanosheet morphology of the polyimide precursor with
organic LIC (Table 5). This method not only restores the low-CO2 foot energy and power density as 66 Wh kg− 1 and 196 W kg− 1, respectively
print of LICs, but also possesses far-reaching potential with respect to and 82.4% capacitance retention is obtained in the potential window
designing a wide range of greener hybrid devices based on other 1–4.2 V [200]. In 2018, Chen et al. [172] developed a hybrid sodium-
chemistries, comprising entirely recyclable components which is given based dual-ion capacitors (NDICs) with nitrogen-doped microporous
in Fig. 17 [173]. hard carbons (NPHCs), soft carbon as an anode using 1-M NaPF6 in the
ethylene carbonate (EC), and dimethyl carbonate (DMC) as electrolyte.
2.3.2. Na-ion capacitor (NIC) The hybrid NDICs presented an ultrahigh energy density of 245.7 Wh
To date, numerous battery type materials such as metal oxides, kg− 1 at a power density of 1626 W kg and is expected to be a potential
polyanions, and hard carbon have been explored for NIC applications. candidate for the next generation of energy storage devices [201].
On the other hand, various high-surface-area carbonaceous materials Pseudocapacitive storage mechanism of both ClO−4 and Na+ ions in
such as activated carbon, biomass-derived carbon, carbon nanotubes carbon cathode/anode with a novel NH3 plasma strategy at room tem
(CNTs), and graphene have also been reported for the capacitor-type perature was done by Cai et al. [202]. With their ingenious NH3-plasma
electrode. Hu et al. [199] fabricated carbon–carbon architectural by strategy, which breaks the barriers of conventional methods of synthe
synthesizing carbon nanosheet with large interlayer spacing of 0.41 nm sizing N-functional carbon materials, various types and substances of N/
from biowaste pine cone shell and triazine framework-derived carbon O pseudocapacitive sites can be controlled directionally and accurately.
was obtained through isothermal synthesis. NIC was fabricated using The NICs deliver an energy density of 107 Wh kg− 1 at a power density of
carbon nanosheet and triazine framework-derived carbon as anode and 200 W kg-1. Subburam et al. [203] demonstrated a facile approach for
cathode, respectively. The device delivered a high energy density of 111 the synthesis of porous carbon nanosheet for application as an anode in
16
(a) SEM, TEM and HRTEM of porous carbon nanosheet (PCNs-600 samples)
showing their interlayer spacings [203].
(b) XRD, Raman, and FTIR spectra of porous carbon nanosheet (PCNs-600 samples)
[203].
Fig. 18. (a) SEM, TEM and HRTEM of porous carbon nanosheet (PCNs-600 samples) showing their interlayer spacings [203]. (b) XRD, Raman, and FTIR spectra of
porous carbon nanosheet (PCNs-600 samples) [203].
17
Fig. 19. Electrochemical analysis of NIC from PCNs- C600//superconductive carbon black [203].
NICs. They used PVA and ascorbic acid as carbon precursor in NaCl oxygen functional group generated provide sufficient active sites to store
template and carbonized at temperatures 600, 700, and 800 ◦ C, followed Na ions through reversible redox reaction. The resultant NIC had
by simple freeze drying. The morphological studies of porous carbon excellent cycling stability of 83% capacity retention after 8000 cycles at
were done by FESEM and TEM showing an interlayer spacing of 0.4 nm 1.0 Ag− 1 with the corresponding Coulombic efficiency of 99.9% [203].
with larger interlayer spacing of carbon materials favourable for the Na+ Yuan et al. [204] proposed the design and preparation of nanohybrid
storage, efficiently promoting the storage capacity. The XRD peak V2O5 nanoparticles embedded in a multichannel CNF with high con
analysis also shows two peaks at 21.3 and 23.6 degree, corresponding to ductivity and high mass transport. An asymmetric NIC was fabricated as
interlayer spacings of 0.41 nm and 0.36 nm, respectively. On the other the AC//V2O3@MCNF with a significant energy/power density of 96
hand, the Raman spectra of the as-synthesized PCNs samples observed to Wh kg− 1 at 250 W kg− 1, as well as a good stability of 80.9% capacitance
be exhibited two main characteristic peaks at around 1352 and 1586 retention over 10,000 cycles. The majority of the study focuses on
cm− 1 corresponding to the D-and G-band positions as in Figs.18 (a) and development of new material rather than addressing the associated ki
(b). netic issues. Fabrication of NICs with identical electrodes that can
The NIC was assembled using pre-sodiated PCNs-C600 as the anode simultaneously function as battery-type and capacitor-type electrodes is
and superconductive carbon black (SCCB) as the cathode in the potential one of the effective solutions for the kinetic issue. Thangavel et al. [205]
window of 0.01–4.5 V, as given in Fig. 19. The CV and GCD analysis of designed self-assembled N,S-doped 2D graphene into a highly connected
SIC device shows specific capacitance of 45.67 F/g at current density 3D architecture using sacrificial silica template as a bifunctional elec
0.05 A/g, energy density of 128 Wh k g − 1 at 112.5 W k g− 1, and power trode. The N and S atoms have higher electronegativity and larger
density of 17,034 W kg− 1at 24 Wh k g− 1. The highly interconnected atomic size, respectively, which can change the structure, charge, and
porous structure is favourable for the electrolyte penetration and surface spin densities of carbon. The graphene framework incorporated by
18
Fig. 20. Electrochemical performance of NS-GHNS//NS-GHNS; (a) schematic working mechanism; (b) CV Curves; (c) Charge/discharge profile; (d) Ragone plot; (e)
cyclic stability; (f) 3D plot comparison of energy power cycle behaviour [205].
functional heteroatom increases the electrolyte wettability of electrode is substantiated by the excellent performance of the 3D-CoO-NrGO
surface and creates more active effect sites. For NIC set up, active ma electrode. The fabricated NIC showed an energy and power density
terial, carbon black, and CMC mixed in the ratio 7.5:1:1.5 coated on Cu- 153 Wh kg− 1 and 41 W kg− 1, respectively, in 1-M NaPF6 in PC [206]. A
foil used as the anode and active material, carbon black, PVDF in the novel dual‑carbon NIC was assembled with hierarchical porous hollow
weight ratio 7.5:1:1.5 and coated on stainless steel coil used as the multicavity carbon spheres (HMCSs) as an intercalated anode and acti
cathode. The Fig. 20 provides the electrochemical analysis of NS- vated HMCSs (AHMCSs) as a capacitive cathode by Liu et al. [207]. The
GHNS//NS-GHNS. The 1-M NaClO4 in a mixture of ethylene carbonate combination endows the SIHC with superior energy densities of 140.1
and diethyl carbonate (1:1 vol.) was used as an electrolyte and gave a Wh kg− 1 at power density 380 W kg− 1 and 80.8% capacitance retention
potential range of 1.5–4.2 V with a high energy density of 121 Wh kg− 1 after 4400 cycles in 1-M NaPF6 in diethyl carbonate and ethylene car
at 100 W kg− 1. A high-performance NIC based on a highly pseudoca bonate electrolyte (Table 6).
pacitive interface-engineered 3DCoO-NrGO anode and activated carbon
cathode was reported [206]. The synergetic effect of Na-ion intercala 2.3.3. K-ion capacitor (KIC)
tion into NrGO layers, CoO conversion reaction, and pseudocapacitive Potassium-ion capacitors (KIC) are an emerging technology that
Na-ion storage resulting from numerous Na2O/Co/NrGO nanointerfaces potentially offers integrated superiorities of the high-power density of
19
Table 6
Summary of various carbon materials for Na-ion capacitors.
N-doped 3D carbon nitrogen-doped hierarchical porous 0–4 115 200 – [208]

AC
Free-standing fibrous nitrogen-doped highly porous salt-templated carbon 0.5–4 95 190 89.9% capacitance [209]
carbon materials retention after 1000 cycles
GarlicderivedHardCabon Porous carbon 1.5–4.2 156 355 73% capacity after [210]
10,000 cycles
MoO2@rGO Goat Hair 0.01–3 79 95 78% capacity after 1000 [211]
derived AC cycles
Fe1− xS N-doped carbon nanosheet 88 11,500 93% capacity after 9000 [212]
cycles
Tin foil N and S 0–4.4 250.35 676 100% capacity retention [213]
co-doped hollow carbon nanobelts after 10,000 cycles
Al2O3-coated NMNC Al2O3-coated NMNC 0–3 63 6600 98% of its initial value after [214]
10,000 cycles
MoSe2@ hollow bowl-like carbon hollow bowl-like carbon 1–4 118 50 83% after 5000 cycles [215]
PI/rGO rGO 0–4 55.5 395 60% after 1000th cycle [216]
Activated carbon Na–Sn4P3 2.2–3.8 37 1000 94% after 6500 cycles [217]
N,S co-doped hollow carbon nanofiber AC 0–4 116.4 20,000 81% after 3000 cycles [218]
Metallasilsesquioxane- Metallasilsesquioxane-derived porous 0–3.2 137 3454 91% after 2000 cycles [219]
derived porous carbon nanosheet carbon nanosheet
Bacterial cellulose-derived carbon Bacterial cellulose-derived carbon 1.5–4 59.2 276 48.6% [220]
nanofibers nanofibers after 5000 cycles
SnSe/rGO. AC 1–4 83 58 70% after 5000 cycles [221]
Porous carbon matric decorated with AC 1–3.8 93 280 – [222]
NiSx
N-C@CNT AC 0.3–3.8 108.1 100 80% after 3000 cycles [223]
Porous carbon nanosheets HPC 0–4 119 200 82% capacity retention [224]
after 8000 cycles
Carbon/Nitrogen-doped carbon Salt templeted carbon 1–4 61 100 90% capacity retention [225]
nanocomposites after 1300 cycles
NiCo2O4 modified hollow carbon AC 0.5–4 99 600 85% after 5000 [226]
tubular bundles cycles
Hierarchically porous carbon HPC800 0–4 103 70 81.1% after 2500 cycles [227]
(HPC550)
utilized as capacitive electrode material in KIC, however, it shows un

satisfactory results due to limited ion accessibility in nanopores. For K-
ion storage anode, a suitable material that can reversibly host large-
sized K+ (ionic radius of 1.38 Å) and offer long-cycling stability by
sustaining volume changes upon charging/discharging processes is
highly desirable. Ideally, anode materials with large interlayer spacing,
high electronic, and ionic conductivity are sought to achieve satisfactory
electrochemical performance. However, the concept of hybrid devices
has rarely been reported in potassium-ion energy storage device. Pham
et al. [228] reported nonaqueous KIC with K4Nb6O17 (KNO) nanosheet
array as anode and orange peel-derived graphene-like carbon (OPAC) as
a cathode. It is noted that the utilization of biomass as precursor reduces
the cost of production. Considering the good electrochemical perfor
mance of the individual half-cell, KNO//OPAC KIC was then fabricated
in the potential window 0–3.5 V with the cell-delivered specific capac
itance of 68 F/g at current density 0.12 A/g and a capacity retention of
87% after 5000 cycles, as given in Fig. 22. The cell delivered an energy
density of 116 Wh kg− 1 at a power density of 216 W kg− 1, indicating that
KIC based on layered niobates and waste-derived carbons have the po
tential to bridge the gap between rechargeable batteries and the
supercapacitors [228].
Cao et al. [230] explored starch-derived hierarchically porous
nitrogen-doped carbon (SHPNC) along with an activated‑carbon cath
ode for dual‑carbon-based KIC. In their study, the hierarchical structure
and nitrogen-rich-doped in the SHPNC anode result in a distensible
interlayer space to buffer volume expansion during K+ insertion/
Fig. 21. General classification of electrodes for K-ion capacitor [229].
extraction, offering more electrochemical active sites to achieve high
specific capacity, and has highly efficient channels for fast ion/electron
capacitors and high energy density of Potassium-ion batteries (KIB) due
transports. KIC device displayed ultra-long cycling life with an energy
to their unique combination of a capacitor-type cathode and a battery-
density of 31 Wh kg− 1 after 10,000 cycles at a high current density of
type anode in organic electrolytes. The electrode materials in KIC is
1000 mA g− 1, which can maintain 75.4% capacity compared with its
depicted in Fig. 21. Usually commercial-grade activated carbon is
initial value, as well as a nearly perfect coulombic efficiency [230]. Li
20
Fig. 22. Electrochemical properties of KNO//OPAC; (a) Galvanostatic charge discharge; (b) variation of specific capacitance with current density; (c) Long life span
measured; (d) Ragone plot with other LIC and NIC devices shown for comparison [228].
Fig. 23. Schematic illustration for MoP@NC-1//AC device and electrochemical analysis [232].
21
Table 7
Summary of various carbon materials used for K-ion capacitors.
P-CVO–N@GO AC 0.5–4 78.2 112.5 96.8% beyond 3000 cycles [235]

Spent black tea derived biomorphic KBT activated 0–3 121 1178 – [236]
carbon electrode (KBT)
Biomass derived Oriented Carbon 3D Porous carbon 0.5–3.7 140 643 84.6% after 5000 cycles [237]
Microsphere
B,N co-doped porous carbon B,N co-doped porous carbon 0–4 174 497 78% capacity retention [238]
after 6000 cycles
N rich biomass carbon AC 0.5–4 127 2371 – [239]
Heteroatom doped CNT AC 0–4 59 21,428 80.9% after 14,000 cycles [240]
P,N-co-doped Carbon mesoporous AC 0–4 175 160 85.8% after 3000 cycles [241]
nanotube
Black phosphorus nanosheet AC 0–4.3 93 97 99.5% after 6500 cycles [242]
TiO2/NC-HN AC 0–4 108 97 100% capacity retention [243]
after 3000 cycles
Mn-MOF-derived porous carbon Polyaniline derived porous carbon 1–4.2 120 26,000 79% after 120,000 cycles [244]
N-doped carbon nanosheets AC 1.5–4.2 90 3000 – [245]
submicrospheres
Cocoon silk-derived, hierarchically AC 0.01–4.2 135 112 75.4% after 3750 cycles [246]
porous N doped carbon
3DN-doped microporous carbon AC 0–4.2 63 19,091 84.7% after 12,000 cycles [247]
polyhedron
N-doped CNT AC 0.01–4 117 1713 81.6% after 2000 cycles [248]
NbSe2/NSeCNF AC 0.01–4 113 180 83% after 10,000 cycles [249]
N-MoSe2/ AC 0.5–4 119 39.6 95% after 1500 cycles [250]
Graphene
N-doped CNT Laser scribed GO 1–4 65 80 91% capacity retention [251]
over 5000 cycles
3D-N doped framework carbon 3D N doped framework AC 0–4.2 163 210 91.7% capacity retention [252]
after 10,000 cycles
Oxygen-rich carbon nanosheets AC 0–4.2 149 21,000 80% capacity retention [253]
after 5000 cycles
N doped Hierarchical Porous Hollow Activated N-Doped Hierarchical 0.01–4 114.2 8203 80.4% capacity retention [254]
Carbon Spheres Porous Hollow Carbon Spheres 5000 cycles
and co-workers [231] put forward self-sacrificial template method to

fabricate Se and N co-doped 3D macroporous carbon. Benefiting from
the advantages of 3D-hierarchical-porous architecture, enlarged inter
layer space and abundant heteroatoms doping, the KIC made of Se/N-
3DMpC anode and the A-Se/N3DMpC cathode delivered energy den
sity of 91 Wh kg− 1 at a high power density of 8100 W kg− 1 and exhibit
outstanding cycling stability [231]. The unique confined Nitrogen-
doped‑carbon nanosheet (NC) with abundantly decorated ultrafine MoP
nanoparticles can also endow structural compatibility, relieve volume
expansion, and provide conductive pathways for K+ diffusion and
electron transfer. The ultrafine MoP nanoparticles could activate the
neighbouring areas in NC skeletons to efficiently improve the binding
energy toward potassium ions and demonstrate enhanced conductivity
with the partial generation of MoP ionic bonds. Thus, the fabricated KIC
showed an energy and power density of 69.7 Wh kg− 1 and 2041 W kg− 1
in the potential window 0.01 to 4 V and a long cycle stability with 89.9%
capacitance retention after 800 cycles which is shown in Fig. 23 [232].
Chen and co-workers [233] proposed a plain-hill model of carbon
structure to solve this problem using CaCl2 as both complexing agent
and oxygen scavenger. A symmetrical cell is made using 1-M KFSI
Fig. 24. The HESS test bed used for the experimental validation of different
electrode in the potential window 0–4.5 V and a high energy density of
HESS topologies and control algorithms [260].
178.4 Wh kg− 1 at 1115 W kg− 1. A 75.2% capacity retention is obtained
at 5 A g − 1 after 10,000 cycles with nearly 100% Coulombic efficiency
and a 51.4% capacity retention was achieved even after 30,000 cycles, done in the potential range 0.01–4 V which delivered an energy and
[233]. Soft carbon is a promising anode material for KIC but the skin-like power density of 171 Wh kg− 1 and 20,000 W kg− 1, respectively [234]
carbon film K+ storage sites [234]. Zhang and co-workers [234] devel (Table 7).
oped a simple oxidation method to remove the skin-type carbon film
and, thus, obtained accordion-like, ordered carbon-sheet architectures 3. Applications
with a hierarchical porous architecture composed of micropores, mes
opores, and macropores. A full KIC is fabricated by N-GQD@ASC-500 as Many variations of SBH and its associated energy management sys
the anode, porous carbon (PC) derived from waste cabbage leaves as the tem have been proposed by researchers over the past decades
cathode in KPF6 in PC electrolyte. The electrochemical analysis was [235–237]. These SBH designs are normally intended to serve large-
scale utilities, smart-grid, electric vehicles, and other high-power
22
Fig. 25. (a)The photograph of red LED powered by two charged supercapacitor under different bending angles connected in series; (b-d) optical picture of self
powered system equipped on lab coat in which strap connected with electronic watch [262]. (For interpretation of the references to colour in this figure legend, the
reader is referred to the web version of this article.)
applications, and they require extensive sensing, computation, and In recent years, with the rapid development of flexible electronic
communication, which significantly increase the system complexity and devices, flexible energy storage devices have attracted more and more
implementation [255–257]. The majority of studies regarding SBH have attention. Apart from high electrochemical performance for battery-
been carried out by utilizing this technology in electric and hybrid ve supercapacitor hybrid devices, their flexibility is getting increased
hicles [258]. The exhaustion of traditional energy sources and the attention. Wang et al. [261] designed and fabricated a novel cathode
deterioration of the environment are becoming more and more serious, based on nickel-plated cotton cloth (NPCC), which is coated with Ni–Co
which make the application of new energy technology particularly ur selenide nanowires for flexible energy storage devices. Moreover, a
gent. Meanwhile, in order to meet the market-oriented standards, flexible high-performance SBH device was designed based on the
extensive attention has been directed to the rapid growth of new energy Ni4.5Co4.5-Selenide nanowires/NPCC cathode, a silk fabric separator,
products, such as hybrid electric vehicles and smart wearing equipment, and Fe3C/carbon fiber anode. This BSH device shows a large energy
which are inseparable from low-cost and efficient energy storage devices density of 47.4 Wh kg− 1 at the power density of 1.5 kW kg− 1 [261]. Zhou
[259]. A fully active battery-supercapacitor hybrid device was et al. [262] activated an interconnected lignin-derived carbon fibrous
addressed by Song et al. [260] based on a 5th-order averaged model, a network (AILCFN) by electrospinning followed by heat treatment. The
sliding-mode current controller, and a Lyapunov function-based voltage unique interconnected structure between fibres in AILCFN is designed
controller (Fig. 24). They have also proved that robust tracking of by controlling the ratio of soft Kraft lignin fractions with different
different variables can be achieved within a large range of SBH pa thermal mobility. The assembled AILCFN/Ni-Co-S//AILCFN-3 BSH ex
rameters and the simulation result demonstrates the feasibility of the hibits a high energy density of 30.8 Wh kg− 1 with a power density of 0.8
proposed sliding-mode controller in semi-active HESS applications. The kW kg− 1 and demonstrates both excellent cyclability and flexibility. The
proposed controller can be implemented with any kind of EMS and used photograph of red LED powered by two charged supercapacitors is given
in EV/PHEV applications. in Fig. 25 [262]. The self-powered system assembled onto a lab coat can
Fig. 26. Battery supercapacitor and solar panel used for the solar PV water pumping system experiment using batteries and supercapacitors [263].
23
continuously provide power for the electronic watch under sunlight Uncited references
illumination and dark environment. Das et al. [263] put forward a novel
approach to analyse the performance of a solar PV-water-pumping sys [94,95,107,108,121,122,127–130,154,155,157–159,255,256]
tem (SPVWPS) using batteries and supercapacitors. In that work, four
different configurations of SPVWPS using energy storage devices, bat Declaration of competing interest
teries, and supercapacitors were tested and compared on sunny days
during January and February 2017 at Haldia (India). The study reveals Not arise.
that the supercapacitor-based configuration gives highest instantaneous
efficiency. The centrifugal pump powered by SPVWPS using batteries Acknowledgements
delivers a maximum of 2964 L per day for 2-m dynamic head whereas
for 3-m dynamic head SPVWPS using supercapacitor delivers a Authors are thankful to Director, CSIR-NEIST for his interest and
maximum of 1826 L per day. In terms of their potential applications, it is permission to publish the review paper. The funds received from MeitY
critical to promote novel energy storage technologies in order to meet (GPP348) are gratefully acknowledged. Dr. Jim Hower edited a version
the growing demands of microelectronic products and electric vehicles. of the manuscript.
The battery supercapacitor and solar panel used for the solar PV water
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2022 - Recent Trends in Supercapacitor-Battery Hybrid Energy Storage Devices Based On Carbon Materials

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Journal of Energy Storage 52 (2022) 104938

Contents lists available at ScienceDirect

Journal of Energy Storage

Recent trends in supercapacitor-battery hybrid energy storage devices

Fig. 1. The energy-power performance of conventional capacitors, batteries,

Fig. 3. Classification and compositions of hybrid energy storage devices [12]

density of supercapacitors without compromising the power density

Fig. 2. Different types of energy storage devices for sustainable applica­

ergy is stored by the accumulation of charges on two parallel metal

Fig. 5. Schematic representation of conventional and electrochemical capacitor.

TiO2@AC 1 M Na2SO4 1.2 4200 28 282 [25]

Fig. 6. A schematic representation of mechanism of energy storage in pseudocapacitors.

Cr2O3 nanoparticles 6 M KOH 1V 312.5 12.5 340 [46]

Ni–Co–Mn hydroxide//AC 3 M KOH 1.6 1650 44.4 117.45 [63]

Fig. 8. Schematic diagram of metal ion capacitor [84].

behaviour. The first classification consisting of composite electrodes

Fig. 10. Effect of electrolyte parameters on energy storage (ES) devices.

Fig. 11. Classification of electrolyte.

Fig. 12. Different allotropes of carbon [116].

Fig. 14. Stepwise fabrication of asymmetric supercapacitor device [139].

MnMoO4@MWCNT Activated carbon 1 M KOH 0.45 18.1 362.4 [140]

(a) SEM ,TEM images of Li3VO4 NC Nano wires [165]

(b) Electrochemical evaluation of the Li3VO4//AC LICs [165]

N-doped 3D carbon nitrogen-doped hierarchical porous 0–4 115 200 – [208]

utilized as capacitive electrode material in KIC, however, it shows un­

P-CVO–N@GO AC 0.5–4 78.2 112.5 96.8% beyond 3000 cycles [235]

and co-workers [231] put forward self-sacrificial template method to

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Fig. 2. Different types of energy storage devices for sustainable applica

utilized as capacitive electrode material in KIC, however, it shows un