Journal of Science: Advanced Materials and Devices 8 (2023) 100586
Contents lists available at ScienceDirect
Journal of Science: Advanced Materials and Devices
journal homepage: www.elsevier.com/locate/jsamd
Original Article
Chitosan-derived carbon aerogel nanocomposite as an active electrode
material for high-performance supercapacitors
Le Hong Quan a, b, Ung Thi Dieu Thuy c, Pham Viet Nam d, Nguyen Van Chi a,
Tang Xuan Duong a, Nguyen Van Hoa e, *
a
Coastal Branch of the Joint Vietnam - Russia Tropical Science and Technology Research Center, 30 Nguyen Thien Thuat, Nha Trang, Vietnam
Graduate University of Science and Technology, Vietnam Academy of Science and Technology, 18 Hoang Quoc Viet, Cau Giay, Ha Noi, Vietnam
Institute of Materials Science, Vietnam Academy of Science and Technology, 18 Hoang Quoc Viet, Cau Giay, Ha Noi, Vietnam
d
Faculty of Food Science and Technology, Ho Chi Minh City University of Food Industry, 140 Le Trong Tan, Tan Phu, Ho Chi Minh City, Vietnam
e
Department of Chemical Engineering, Nha Trang University, 2 Nguyen Dinh Chieu, Nha Trang, Vietnam
b
c
a r t i c l e i n f o
a b s t r a c t
Article history:
Received 15 December 2022
Received in revised form
24 April 2023
Accepted 23 May 2023
Available online 25 May 2023
The valorization of shrimp wastes to develop advanced materials brings economic and environmental
advantages. This paper presents a facile and eco-friendly synthesis of shrimp chitosan-derived carbon
(CCS) and CCS/NiO@Ni(OH)2 (CSSN) aerogel nanocomposite for supercapacitor application, in which NiO
and Ni(OH)2 nanoparticles were tightly attached to the porous surface of CCS aerogel. As a result, CCSN300 aerogel carbonized at 300 C has high porosity and electrical conductivity and demonstrates its
potential as an active electrode material for supercapacitors. The CCSN-300 aerogel material electrode
exhibits a high capacitance of 316 mAh g1 at 1.0 A g1. Furthermore, the CCS//CCSN-300 device had a
capacitance of 209 F g1 at 1.0 A g1 and over 84% remaining after the 10,000 cycles. Moreover, it has a
high energy density of 65 Wh kg1 at a power density of 1500 W kg1. The results demonstrate that
chitosan-derived carbon composites hold great promise in high application efficiency for energy storage.
© 2023 Vietnam National University, Hanoi. Published by Elsevier B.V. This is an open access article
under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
Keywords:
Chitosan
Chitosan-derived carbon
Aerogel nanocomposites
Supercapacitor
1. Introduction
Currently, the demand for energy around the world is
increasing. With constant efforts, researchers are finding ways to
replace fossil fuels with renewable energy sources such as solar and
wind power to fulfill sustainability. However, one of the significant
issues with this renewable energy is the continuous storing of
energy while passively dependent on factors like the sun and wind.
Therefore, the demand for energy storage systems is exploding, and
energy storage devices are creating a strong attraction in the
research world today. Among them, the role of supercapacitors is
considered the golden key to sustainable energy [1e4].
The ideal material for supercapacitor electrodes should have the
following properties: large capacitance, high conductivity, large
surface area, low density, and large porosity with suitable pore size.
Generally, three primary materials commonly used for electrode
coating for supercapacitors are metal oxides/hydroxides/sulfides
* Corresponding author.
E-mail address: hoanv@ntu.edu.vn (N. Van Hoa).
Peer review under responsibility of Vietnam National University, Hanoi.
(MOHS), conductive polymers, and carbon materials [5e9]. However, each of those materials has its advantages and drawbacks. For
example, MOHS materials have high electrical potential due to
redox reactions but have low conductivity and are less stable when
charged/discharged repeatedly [9]. Meanwhile, carbonaceous materials with high electrical conductivity and large porosity but low
capacitance [10]. Finally, conductive polymers have high strength
but low porosity [9].
So far, composite materials of two or three components above
are mentioned to overcome the above problem because they have
the following advantages: (i) enhance the surface area and porosity
of the material; (ii) improve the conductivity of the electrode; (iii)
decrease the size of nanoparticles or polymers due to the uniform
distribution of components in the assembly. Therefore, the properties of composite materials have outstanding features and greatly
enhance supercapacitors' performance by increasing capacity and
energy density. In addition, it is worth noting that the electrochemical performance of the electrodes is improved when carbon
is combined with pseudo-capacitive materials due to carbon's
electrical conductivity and the metal compounds' redox activity
[11e13].
https://doi.org/10.1016/j.jsamd.2023.100586
2468-2179/© 2023 Vietnam National University, Hanoi. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/
licenses/by-nc-nd/4.0/).
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
2.3. Characterization
Metal oxides, hydroxides, and sulfides such as RuO2, NiO, MnO2,
Ni(OH)2, MoS2, and conductive polymers such as polypyrrole and
polyaniline are common materials for supercapacitors [14e17]. For
example, among various transition metal oxides, NiO and Ni(OH)2
are widely studied as active electrode materials for supercapacitors
due to their high capacitance, easy preparation, high chemical
stability, and low cost. However, they have poor electrical conductivity and a low electron transport rate.
Carbon aerogel is a potential material for supercapacitor
fabrication due to its high conductivity, large surface area, and
good flexibility [18e20]. Carbon aerogel is often studied and
prepared from graphene by chemical reduction and freeze-drying.
However, due to the relatively high cost of graphene raw materials, its practical application and commercial production trade
still face many difficulties [21e24]. Chitosan (CS) is a biopolymer,
commercially produced mainly from shrimp shells, which is discharged from seafood factories in massive amounts [25]. The
molecular structure of chitosan contains many amino groups
(-NH2). In addition, in the chitosan molecule, there are functional
groups in which the oxygen and nitrogen atoms of the functional
group have unused electron pairs, so they can create complexes
and coordinate with most transition metals. After forming the
aerogel and being carbonized, the resulting product is an N-doped
carbon aerogel with good electrical conductivity and electrochemical properties.
Based on those considerations, this work aimed to prepare
carbon/NiO@Ni(OH)2 (CCSN) aerogel nanocomposite for energy
storage application, in which carbon was derived from chitosan.
The as-prepared materials were characterized by scanning electron
microscopy (SEM), X-ray diffraction (XRD), X-ray spectroscopy
(EDX), and BET surface measurement. In addition, the electrochemical performance of the CCSN nanocomposites was investigated in both three- and two-electrode systems.
The morphology and elemental mapping of samples were
characterized using scanning electron microscopy (SEM, Hitachi, S4800). The phase composition of CCSN aerogels was analyzed using
X-ray diffraction analysis (XRD, PANalytical, X'Pert-PRO MPD) under Cu Ka radiation. The chemical structure of samples was determined by a Fourier transform infrared spectrometer (FTIR, Nicolet
iS10, Thermo Scientific) from 500 to 4000 cm1 at a resolution of
16 cm1 for 32 scans. BrunauereEmmetteTeller (BET) and BarretteJoynereHalenda (BJH) methods were applied to determine
the specific surface area and pore size, respectively.
2.4. Electrochemical measurements
Chitosan (CS, deacetylation of 95%, viscosity of ca. 200 mPa s)
was prepared from shrimp shells in our laboratory. Acetic acid
(CH3COOH, 99%), sodium hydroxide (NaOH, 99%), Glutaraldehyde
(GA, 50%), nickel (II) nitrate hexahydrate (Ni(NO3)2$6H2O, 99%)
were purchased from SigmaeAldrich and used as received.
An electrochemical workstation Autolab PGSTAT204N (Metrohm, Netherlands) was employed to investigate the electrochemical performances. In a three-electrode configuration, the
Platinum foil and an Ag/AgCl electrode were used as counter and
reference electrodes, respectively. The working electrode was
fabricated by pressing a paste of 80 wt.% aerogel, 10 wt.% carbon
black, and 10 wt.% chitosan solution binder on a nickel foam collector (1.0 cm 1.0 cm). All electrochemical tests were conducted
at room temperature using a 6 M KOH electrolyte solution.
On the other hand, the electrochemical performance of the
CCSN aerogels was investigated in an asymmetrical two-electrode
configuration in a 6 M KOH electrolyte solution. The setup is built
into a stainless cell with filter paper as the separator. The electrode
is cut into circular films approximately 15 mm in diameter. Cyclic
voltammetry (CV) was measured at different scan rates from 2 to
200 mV s1 and within a potential range of 0.0 0.4 V (for the
three-electrode system) and 0.0 1.5 V (for the two-electrode
system). The capacitance and rate capability were evaluated
based on galvanostatic charge/discharge (GCD), measured at
various current densities from 1.0 to 7.5 A g1 at a potential window
of 0.0 0.4 V (for the three-electrode system) and 0.0 1.5 V (for
the two-electrode system). A chargeedischarge test of 10,000 cycles was implemented at a constant current density of 5.0 A g1.
Electrochemical impedance spectroscopy (EIS) was performed in a
frequency range of 102 105 Hz with an AC amplitude of 5.0 mV.
The specific capacitance (Q, mAh g1) was calculated from the
GCD through a three-electrode system using the following equation
(1) [1,2]:
2.2. Preparation of CCSN aerogels
Q¼
Fig. 1 shows a schematic process regarding preparing chitosanderived carbon aerogel nanocomposite for supercapacitors. Firstly,
CS was dissolved in a 2.0 wt.% acetic acid aqueous solution to form
a 2.0 wt.% CS solution. Then, 1.75 g (6 mmol) of Ni(NO3)2$6H2O
was added to the 100 ml CS solution and stirred for 30 min to
homogenize the mixture. Next, 1.0 wt.% GA was injected into the
CS solution containing Ni2þ and stirred for 30 min. Next, soak the
resulting solution in a container containing 10 wt.% NaOH solution
till the gelation was completed. The CS-Ni(OH)2 hydrogels were
washed with deionized water repeatedly to be neutral. Next, the
hydrogel samples were frozen at 40 C for 24 h and dried by
lyophilization to get CS-Ni(OH)2 aerogels. Finally, the CS-Ni(OH)2
aerogels were converted into CCS-NiO@Ni(OH)2 (CCSN) nanocomposites in a tube furnace at different temperatures under a
nitrogen atmosphere. The heating rate is 5 C min1. The activation temperatures were 300, 400, and 500 C, and the obtained
samples were denoted as CCSN-300, CCSN-400, and CCSN-500,
respectively.
where I is the discharge current (A), t is the discharge time (s), and
m is the mass of the active material (g).
For the asymmetrical device, the capacitance was calculated
from GCD curves according to the following equation (2) [26]:
2. Experimental
2.1. Materials
C¼
It
m
2It
mDV
(1)
(2)
where C is the capacitance (F g1), t is the discharge time (s), m is
the total mass of the active material at the two electrodes (g), and
DV is the working voltage window (V).
The energy density (E, Wh kg1) and power density (P, kW kg1)
were calculated from GCD tests in the following equations (3) and
(4), respectively [4,26]:
E¼
2
1
C DV 2
2 3:6
(3)
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
Fig. 1. Schematic diagram of the preparation of CCSN aerogel nanocomposite for supercapacitor application.
E
P ¼ 3600
t
52.2 correspond to the (100) and (110) crystal planes of Ni(OH)2.
Therefore, it can be concluded that the formation of CCSN composites is doped with a small amount of Ni(OH)2. The obtained XRD
is also consistent with other studies [27e31].
The FTIR spectra of CS and various CCSN aerogels are shown in
Fig. 3. The characteristic absorption peaks of CS are at 3500 cm1
(OeH and NeH), 1645 cm1 (C¼O stretching vibration), 1545 cm1
(NeH bending vibration), 1135 and 1224 cm1 (-CH2 and CeO
distinct groups) [32]. The CCSN samples have peaks at 3500,
1645, and 1545 cm1 attenuated in descending order at 300, 400,
and 500 C, which may be caused by the reduction of OeH, C¼O,
and NeH groups after heating at high temperatures. For the CCSN300 sample, the absorption band is around 500e600 cm1, corresponding to the NieO vibration band [26], and is significantly
weakened for the CCSN-400 and CCSN-500 samples.
Fig. 4 presents SEM images of bare CCS, pristine NiO@Ni(OH)2,
and CCSN samples. It can be seen that the surface of CCSN-400 and
CCSN-500 aerogels is relatively smooth with few visible/neutral
pores (Fig. 4aed). Meanwhile, the surface of the CCSN-300 sample
(4)
where C is the capacitance from the two-electrode tests (F g1), t is
the discharge time (s), and DV is the working voltage window (V).
3. Results and discussion
The phase structures of CS and CCSN composites were analyzed
by XRD. Fig. 2 shows the XRD patterns of bare CS and various CCSN
nanocomposites. The XRD pattern of the CS sample shows a broad
weak band at 2q of 11 and 25 corresponding to the (020) and
(110) planes in typical carbons. For the CCSN-300, CCSN-400, and
CCSN-500 samples, the XRD pattern spectra exhibit diffraction
peaks at 2q of 43.2 and 76 , corresponding to the (200) and (222)
crystal planes of NiO nanoparticles, respectively. However, no
diffraction peaks relating to CS were observed, indicating the formation of an amorphous carbonaceous structure in the prepared
CCSN nanocomposites. The diffraction peaks at 2q of 39.2 and
Fig. 2. XRD patterns of (a) bare CCS, (b) CCSN-300, (c) CCSN-400, and (d) CCSN-500
samples.
Fig. 3. FTIR spectra of (a) bare CCS, (b) CCSN-300, (c) CCSN-400, and (d) CCSN-500
samples.
3
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
Fig. 4. SEM images of (a) bare CCS, (b) pristine NiO@Ni(OH)2, (c) CCSN-500, (d) CCSN-400, (e) CCSN-300, and (f) TEM image of CCSN-300.
CCSN-400 and CCSN-500 is of type IV, characteristic of adsorbents
mesoporous. The hysteresis loop of CCSN-300 is of type H3 [33],
showing that the sample contains many slit holes. The CCSN-300
delay loop is not closed. This phenomenon is common in materials with well-developed pore structures and may be related to the
expansion effect of the microporous adsorbent gas [34,35] and
pressure-dependent elastic deformation behavior [36]. The
desorption curves of CCSN-300 changed relatively modestly, corresponding to the pore shape of the primarily cylindrical CCSN-300
sample. The pore size distribution graph according to Barrett e
Joyner e Halenda (BJH) of the CCSN samples is shown in Fig. 6b. The
pore distribution was mainly mesoporous and ranged from 3 to
8 nm without any macroporous features. The calculated maximum
surface area for the CCSN-300, CCSN-400, CCSN-500 samples is
approximately 38, 25, 22 m2 g1, respectively. The average pore
diameter for the CCSN-300, CCSN-400, and CCSN-500 samples was
around 3.5, 3.4, and 3.6 nm, respectively (Table 1). As an active
material for supercapacitors, this porous nanolayer is helpful with
high porosity and more active sites, resulting in a fast discharge rate
for the redox reaction. The specific surface area and the pore volume of CCS are 817 m2 g1 and 0.083 cm3 g1, respectively, which is
a good negative material when assembled with the CCSN in an ACS
is high porosity, and pores can be observed clearly (Fig. 4e). At
higher magnification, the porous surfaces and walls of the 3D
porous lattice were filled with interconnected and open pores
(Fig. 4f). Therefore, the high specific surface area and hierarchical
porous structure in CCSN-300 aerogel are better than CCSN-400
and CCSN-500 samples. It indicated the high potential of CCSN300 aerogel for electrode materials. Fig. 4f shows the TEM image
of the CCSN-300 sample with a hierarchical porous structure,
which presents a well-distribution of the NiO and Ni(OH)2 nanoparticles on the porous CCS matrix. Fig. 5 shows the K-edge signals
of C, Ni, and O and the EDX spectrum of the CCSN-300 sample. Once
again, a uniform distribution of C, Ni, and O was observed, confirming the even deposition of NiO and Ni(OH)2 nanoparticles on
the CCS sheets.
A survey of the surface properties of CCS and different CCSN
samples was carried out by BET measurement. Fig. 6a shows the
nitrogen adsorptionedesorption isotherms. The isotherms of CCSN
show a hysteresis ring with relatively high pressure (P/P0) between
0.0 and 1.0. The slope increases from 0.3 to 0.9, corresponding to a
relatively high pressure indicating pore size mesopores [7]. The
shape of the adsorption hysteresis loop is related to the pore shape.
According to the IUPAC classification [33], the hysteresis loop of
4
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
Fig. 5. (a) SEM images of CCSN-300, EDX mappings of (b) carbon, (c) nickel, (d) oxygen, and (e) EDX spectrum of the CCSN-300 sample.
Fig. 6. (a) The BET nitrogen adsorption isotherm plot, and (b) the pore size distribution of the CCSN-300, CCSN-400, and CCSN-500 samples.
curves of NiO@Ni(OH)2 and CCSN active materials at a scan rate of
50 mV s1 in the potential range from 0.0 to 0.4 V in a 6 M KOH
electrolyte. The CV curve of the NiO@Ni(OH)2 and all CCSN samples
show a pair of separate redox peaks on the CV curves, indicating
that they both have characteristics of typical pseudo-capacitance
device. The reduced specific surface area of CCSN compared to CCS
may be the doping blocks of metal oxide and hydroxide particles
into the pores of the carbon material.
The working electrode's electrochemical performance was
studied using a three-electrode system. Fig. 7a shows the typical CV
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L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
There are two reasons for this phenomenon: (i) CS acts to prevent
agglomeration of NiO and Ni(OH)2 nanoparticles and provides a
high surface area, resulting in a more extensive electrical activity
range for the redox reactions; (ii) CCSN-300 with a superior specific
surface area is superior to other samples, making ion diffusion
easier throughout the surface of the material.
Fig. 7b presents the Nyquist plots of the CCSN-300, CCSN-400,
and CCSN-500 electrodes. The inset shows the Nyquist plot at the
high-frequency region. All three electrodes exhibited small charge
transfer resistance (Rct), and no obvious semicircle appeared in the
high-frequency region. In addition, the total resistance of the CCSN300 electrode is lower than the other two types. Fig. 7c shows the
Table 1
Parameters on the pore structure of various chitosan-derived carbon aerogels.
Sample
SBET (m2 g1)
Vpore (cm3 g1)
dBJH (nm)
CCS
CCSN-300
CCSN-400
CCSN-500
817
38
25
22
0.083
0.046
0.084
0.094
3.5
3.5
3.4
3.6
caused by the reversible Farada transition between Ni2þ and Ni3þ.
Among them, the CV curve of CCSN-300 has the largest area,
indicating excellent electrochemical efficiency among electrodes.
Fig. 7. (a) CV curves of the different electrodes at a scan rate of 50 mV s1 in 6M KOH, (b) Nyquist plots of the various electrodes, (c) Capacities of the various electrodes at different
current densities, (d) CV curves of the CCSN-300 electrodes at different scan rates, (e) Galvanostatic discharge plots of the CCSN-300 electrode at different current densities, (f) The
capacitance stability and coulombic efficiency of the CCSN-300 at 5 A g1.
6
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
active mass. From the above data, the CCSN-300 electrode was
chosen as the positive electrode to investigate the further electrochemical performance in supercapacitor devices.
The electrochemical properties of CCS//CCSN-300 asymmetric
supercapacitors were studied, and the results are shown in Fig. 8.
For a supercapacitor to achieve good performance, it is necessary to
ensure a charge balance qþ ¼ q. Therefore, the mass of electrode
materials was optimized, and the mass ratio mþ/m was found to
be about 0.24. The CV curve of the CCS electrode at a scan rate of
50 mV s1 with of the potential window 1.1 0.0 V as shown inset
in Fig. 8a. The CV curves of the CCS electrode presented a nearly
regular rectangular shape without obvious redox peaks, representing an electrical double-layer capacitive behavior [38]. In
addition, the overall enhanced electrochemical performance of the
CCS electrode due to the pseudo-capacitive contribution made by
functional groups (N) alongside electric double capacitance originating from the physical interactions of electrode/electrolyte ions
on the high surface area interface. The CV curves of asymmetric
supercapacitors at different scan rates in the potential range of
0.0e1.5 V are presented in Fig. 8a. As can be seen, the shape of the
CV curves does not change much as the scan rate increases from 2
to 200 mV s1, which indicates a good capacitance state of the
asymmetric supercapacitor.
Fig. 8b presents the discharge curves of asymmetric supercapacitors at current densities from 1.0 to 7.5 A g1 over a potential
window of 1.5 V. The CCS//CCSN-300 device exhibits good capacitance retention even at high current densities, 209 F g1 at 1.0 A g1
and about 55% retention at a high current density of 7.5 A g1 as
illustrated in Fig. 8c. Fig. 8d demonstrates the cyclic stability of the
CCS//CCSN-300 supercapacitor after 10,000 cycles at a current
density of 5.0 A g1. It shows good capacitance retention (84.3%)
and coulombic efficiency (89.0%) over 10,000 cycles, opening up the
potential application of CCS//CCSN-300 in supercapacitor technology. Fig. 8e shows the energy (E, Wh kg1) and power densities (P,
W kg1) of the asymmetric device. It revealed a change in energy
density values from 65 to 35 Wh kg1 and an increased power
density value from 1500 to 11,250 W kg1 at different current
densities. Besides, the energy density and power density of the
CCS//CCSN-300 device are higher than those of some chitosanderived carbon and graphene-based supercapacitors in the literature (Table 3).
LEDs have confirmed the practical application of the fabricated
asymmetric supercapacitor. A 1.5 V LED is individually lit using two
CCS//CCSN-300 devices connected in series (Fig. 8f). After charging
the supercapacitor for 30 s, the LED bulb can be effectively illuminated for 2 min. This result opens a new direction for sustainable
energy related to seafood waste as a valuable energy source for
developing supercapacitors.
capacities of the electrodes at different current densities. The capacities of the CCSN-300, CCSN-400, and CCSN-500 electrodes
were calculated as 316, 102, and 28 mAh g1, respectively, at 1 A g1
current density. They indicated that the CCSN-300 electrode has
the highest capacities, consistent with the CV curve survey results
above.
The redox peak current of the CCSN-300 electrode has increased
significantly with an increasing scan rate (Fig. 7d). Furthermore, the
anodic peak current densities and the cathode peak current densities increase linearly with the scan rate, indicating that the prepared carbon aerogel has abundant redox reaction during charge
storage. Furthermore, clear redox peaks were observed at a high
scanning rate (200 mV s1), which suggests the rapid transport of
electrons and ions and the possibility of rate good of the prepared
electrode.
Galvanostatic discharge time was executed to inspect the stability of the CCSN electrode. The galvanostatic discharge plots of the
CCSN-300 electrode at different current densities are presented in
Fig. 7e. It can be observed that at low current densities, the
discharge plots display a broader plateau. The related reactions can
occur during the charging/discharging process as follows.
NiO þ OH 4 NiOOH þ e
(5)
NiðOHÞ2 þ OH 4NiOOH þ H2 O þ e
(6)
Based on the galvanostatic discharge plots, the capacities of the
CCSN-300 electrode were calculated as 316, 299, 265, 240, 238, 205,
and 168 mAh g1, respectively, at a current density of 1.0, 1.5, 2.5,
3.0, 4.0, 5.0, 7.5 A g1. The degradation of capacitance at high current densities can be attributed to the large mesopores of the
composite with diameters of 5e40 nm [37] and the destruction of
the NiO and Ni(OH)2 nanoparticles. Table 2 compares the electrochemical performance of the CCSN-300 electrode with other
related works. It indicates that the CCSN nanocomposite is comparable with reported chitosan-based electrode materials in the
literature.
To evaluate the capacitance stability of the CCSN-300 electrode,
we evaluated the electrode capacitance after 10,000 charge/
discharge cycles at a current density of 5.0 A g1; the result is
shown in Fig. 7f. The specific capacitance was reduced by about 24%
from the original value after 10,000 cycles. In addition, the
coulombic efficiency of the CCSN-300 electrode retention to
85e100% over the entire 10,000 cycles. The main reason may be the
NiO or Ni(OH)2 in the composites decaying during the charge/
discharge processes. Besides, the contraction and volume expansion of NiO or Ni(OH)2 due to redox reactions during the charge/
discharge may lead to electron permeability errors and loss of
Table 2
Comparison of the electrochemical performance between the CCSN-300 electrode and other previously reported related materials.
Electrode materials
Specific capacitance (F g1)
Current density (A g1)
Electrolyte
Ref.
Chitosan-based carbon
Chitosan-based carbon
Chitosan-based carbon
Chitosan-based carbon
Chitosan-based carbon
Bagasse-based carbon
Chitosan-Mxene
Graphene-NiO
Graphene-NiO
Graphene-NiO
CCSN-300
210
958.33
110
197
41
142.1
257
240
632
243
790 F g1
1
5
5 mV s1
0.2
1
0.5
5
3 mV s1
2
3 mV s1
1
6M
6M
6M
6M
1M
6M
3M
6M
6M
6M
6M
[37]
[39]
[40]
[23]
[41]
[42]
[43]
[44]
[45]
[46]
This work
7
KOH
KOH
KOH
KOH
Na2SO4
KOH
KOH
KOH
KOH
KOH
KOH
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
Fig. 8. (a) CV curves of the CCS//CCSN-300 device at different scan rates in 6M KOH, (b) Galvanostatic discharge plots at different current densities, (c) The capacitance retentions at
different current densities, (d) The capacitance retention and coulombic efficiency at 5 A g1; e) Ragone plots at different current densities, and (f) two ASC devices connected in
series.
Table 3
Comparison of the energy density and power density between this study and previously reported devices.
Positive materials
Negative materials
Energy density (Wh kg1)
Power density (W kg1)
Ref.
Chitosan-based carbon
Chitosan-based carbon
Chitosan-based carbon
Chitosan-based carbon
Chitosan-based carbon
Bagasse-based carbon
Chitosan-Mxene
Graphene-NiO
Graphene-NiO
Graphene-NiO
CCSN-300
Chitosan-based
Chitosan-based
Chitosan-based
Chitosan-based
Chitosan-based
AC
AC
AC
AC
AC
Chitosan-based
5.62
43.75
5.8
27.4
28.74
19.74
19.31
47.3
30.56
47.5
65
120
516.25
1900
400
400
500
3906
140
2800
145
1500
[37]
[39]
[40]
[23]
[41]
[42]
[43]
[44]
[45]
[46]
This work
carbon
carbon
carbon
carbon
carbon
carbon
8
L.H. Quan, U.T. Dieu Thuy, P.V. Nam et al.
Journal of Science: Advanced Materials and Devices 8 (2023) 100586
4. Conclusion
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We have successfully synthesized a chitosan-derived carbon
aerogel nanocomposite for supercapacitor application. The resulting composite material has a high capacity of 316 mAh g1 at a
current density of 1.0 A g1. Besides, the assembled asymmetric
device (CCS//CCSN) has a capacitance of 209 F g1 at 1.0 A g1.
Furthermore, this ASC device has a high energy density of 65 Wh
kg1 at a power density of 1500 W kg1 with cyclic stability of
84.3% after 10,000 cycles. The exemplary capacitive behavior is
attributed to the unique features of chitosan-based carbon aerogels
embedded with NiO@Ni(OH)2 nanoparticles with high specific
surface area, pore volume, proper pore size, reasonable pore size
distribution, and even distribution of nanoparticles. In practical
testing, a series connection of two CCS//CCSN supercapacitors can
illuminate LED bulbs (3 V) for 2 min with the 30s of charging time.
The research suggests an excellent potential fabrication of low-cost
and high-electrochemical performance nanomaterials for energy
storage.
Declaration of competing interests
The authors declare that they have no known competing
financial interests or personal relationships that could have
appeared to influence the work reported in this paper.
Acknowledgments
Le Hong Quan was funded by the Master, Ph.D. Scholarship
Programme of Vingroup Innovation Foundation (VINIF), Code
VINIF.2022. TS098. Coastal Branch of the Joint Vietnam - Russia
Tropical Science and Technology Research Center, Vietnam support
to carry out experiments.
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