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A High-Performing Asymmetric Supercapacitor of

Molybdenum Nitride and Vanadium Nitride Thin Films as
Binder-Free Electrode Grown through Reactive Sputtering
Ravikant Adalati, Ashwani Kumar, Yogesh Kumar, and Ramesh Chandra*

have high specific energy; however, main

Transition-metal nitride (TMN) thin-film-based electrodes are recognized for issue with battery is that it has the low spe-
high-performance, stable, flexible, and smart supercapacitors (SCs), as they cific power compared with the SC. On the
exhibit extensive voltage range, good sustainability, and high electrical con- contrary, SCs have high specific power and
discharge maximum amount of energy in a
ductivity. Herein, using reactive DC magnetron sputtering, molybdenum nitride
very short duration, which we need for new
(Mo2N) and vanadium nitride (VN) thin films are deposited on 304 stainless steel generation fast devices and applications
substrate at 200  C for asymmetric SC (ASC) applications. ASC is constructed wherein high and fast power output is
using VN@SS as negative electrode and γ-Mo2N@SS as positive electrode and required.[2] A full SC device is just like
examines the electrochemical behavior in aqueous solutions of 1 M Na2SO4 at the battery, made up of four parts: positive
electrode, negative electrode, electrolyte,
several scan rates and current densities. To scrutinize the crystallographic details
and separator. Out of these four compo-
and electronic configuration of as-deposited thin-film electrodes, X-ray diffraction nents, electrode materials mainly decide
and X-ray photoelectron spectroscopy are used. To visualize the surface mor- cost and performance of the SC. In this sce-
phology, film thickness, and elemental composition, field-emission scanning nario, nanostructured materials proved to
electron microscopy and energy dispersive X-ray analysis is used. The results be a worthy choice for better performance
imply that TMN thin-film-based electrodes bestow super-hydrophilic nature and SC.[3] Hence, intensive research has been
devoted toward designing and fabrication
give enhanced capacitance value along with excellent rate performance. This
of high-quality nanostructured electrode
work demonstrates VN@SS and γ-Mo2N@SS thin-film-based electrode for ASC, materials. For instance, recently, different
which show a high capacitance of 85.50 Fg
1 and a high specific power of types of transition metal compound-based
23.3 Wh kg
1 with a broadened voltage window of 1.4 V, and this is a electrode have attracted enormous atten-
potential candidate for energy storage devices. tion due to their unique physio-chemical
properties, such as high electrical conductiv-
ity, high hardness, electrochemical stability,
and wear and corrosion resistances.[4]
These properties of transition metal compound make them a
1. Introduction promising and active electrode material to be used for SCs.
In current scenario, for fast working appliances, scientists mostly To make SC more effective and promising energy device,
work to develop and design the advanced energy storage devices. researchers are working on the various kinds of transition metal
Batteries, rechargeable batteries, conventional capacitor, and compounds, such as oxides, carbides, phosphides, and nitrides.
supercapacitor (SC) are some of the devices, which are used now- Out of these metal compounds, all have some advantages as well
as disadvantages. In case of metal oxide-based electrodes, even
adays in several applications to store electrical energy.[1] Batteries
though these electrodes show high capacitance value, the main
problem is to have their relatively poor electrical conductivity,
R. Adalati, Dr. A. Kumar, Dr. R. Chandra which, in turn, hinders their capacitive performance rate.[5]
Nano Science Laboratory Non-oxide materials, such as metal sulfide and metal carbide-
Institute Instrumentation Centre based active electrodes, have high electrical conductivity and
Indian Institute of Technology
Roorkee 247667, India hydrophilic nature. For instance, 1 T MoS2 and Ti3C2, both
E-mail: ramesh.chandra@ic.iitr.ac.in the electrodes have the ultrahigh volumetric capacitance of
Dr. Y. Kumar 650 and 900 F cm
3, respectively. However, these types of elec-
Department of Physics and Astrophysics trodes are restricted to have 1 V s
1 highest sweep rate.[6] On the
ARSD College other hand, transition-metal nitrides (TMNs), such as TiN, show
University of Delhi high electrical conductivity compared with their respective metal
Delhi 110007, India
carbides, which, in turn, offers high energy storage.[7] It has been
The ORCID identification number(s) for the author(s) of this article confirmed that the electronic structure of metal host is strongly
can be found under https://doi.org/10.1002/ente.202000466. affected by introducing N (nitrogen) atoms. These metal nitrides
DOI: 10.1002/ente.202000466 attained great consideration as an electrode material for SC,

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as they possessed unique physio-chemical properties, high elec- capacitance of 85.50 Fg
1 with a comparably good specific
trical conductivity, structural stability, and good electrocatalytic energy of 23.3 Wh kg
1 and a better capacitance retention of
property. Here, in this work, we have developed molybdenum 95.23% over the 5000 charge–discharge cycles, and this ASC
nitride (Mo2N) and vanadium nitride (VN) thin-film electrodes, can be useful for fast and advance energy storage electronic
and these electrodes fully use their surface catalyst and high con- devices.
ductivity to produce high-performing SC. Their respective metal
oxide (MoOx and VOx) shows relatively low capacity and rate
capability compared with their metal nitride (MoN and VN).[8] 2. Experimental Section
Chen et al.[9] synthesized Mo2N thin films on titanium substrate 2.1. Preparation of Electrodes
using a sputtering method. In this report, gamma-Mo2N,
thin-film electrode was also successfully prepared by reactive Metal nitride films were prepared by the sputtering technique
magnetron direct current (DC) sputtering and acquired and deposited on the 304 SS substrate, to prepare binder-free
highly oriented gamma-Mo2N thin film even at 200  C (low tem- electrode. Targets with 99.9% purity of vanadium and molybde-
perature compared with Chen et al.’s work), by varying some num were used as cathode to deposit VN and molybdenum
sputtering parameters (Ar/N2 gas flow, applied DC power, nitride (Mo2N) thin films, respectively. To reduce the contami-
and deposition pressure). This hydrophilic natured Mo2N nation and to deposit high-quality electrodes, chamber
shows good adhesion to the 304 stainless steel (304 SS) substrate before deposition pumped up to a pressure of 3  10
6 Torr
(2 cm2 large area). (0.4  10
3 Pa). The working pressure in chamber during all dep-
According to used energy storage mechanism and electrode ositions is set constant at 10 mTorr (1.33 Pa), whereas the N2 and
material, SCs can be classified into two types, pseudo-capacitors Ar gas flow ratio is optimized for each target material to get
and electrochemical double-layer capacitors (EDLCs). A pseudo- desired material. The 304 SS substrate cleaned in acetone by son-
capacitor stores energy by Faradic redox reactions that occur icating it for 15 min and mounted 5 cm away from surface of the
on the surfaces of electrode, whereas the EDLC stores energy target. Deposition was carried out at a substrate temperature of
by adsorbing electrons onto the interface of electrode–electrolyte 200  C with 100 W target power, whereas the deposition time is
double layer.[10] optimized to obtain the required thickness of the films, for each
Furthermore, high specific power, long cycling stability, and target material. The schematic view for the fabrication of ASC
the ability of fast charging with capability of releasing energy 10 cell and direct deposition of electrode on current collector with-
times faster than the present day batteries give SCs advantages out any binder by reactive sputtering is shown in Figure 1. The
over the other present energy storage devices.[11] However, SCs optimized deposition parameters of VN@SS and Mo2N@SS
have low specific energy than batteries, due to which auxiliary thin films are shown in Table S1, Supporting Information.
applications of SCs are limited.[12]
Researchers are working on SC with respect to increasing their
specific energy. SCs with high and comparable power and energy 2.2. Characterization of the Thin-Film Electrode
densities with long cyclic stability are promising candidate to
satisfy the necessary energy demand for new age fast and advance The crystallography study of thin-film electrodes was done by
electronic devices.[13] Specific energy (E) is depended on the X-ray diffraction (XRD) (Bruker AXS). The surface morphology,
square of applied Voltage (V) and capacitance (C) of the SC, as elemental composition, stoichiometry, surface topography, and
per this equation: E ¼ 1/2CV2. This, in fact, provides information hydrophilicity were characterized by field-emission scanning
that E can be enhanced by either increasing capacitance or broad- electron microscopy (FE-SEM) (Carl Zeiss, Ultra plus), energy
ening the potential window of the cell. Capacitance of the cell dispersive X-ray analysis (EDAX) (Oxford instrumental), atomic
can be increased using various types of novel electrode materials, force microscopy (AFM) (NT-MDT NTEGRA), and contact angle
such as transition metal compounds and working potential win- measurement (Kruss DSA 100 easy drop). Elemental configura-
dow can be broadened using organic or ionic liquid electrolyte.[14] tion and oxidation states were obtained using X-ray photoelectron
One effective and simple way is to combine two different spectroscopy (XPS) (PHI Versa Probe). Electrochemical study
nanostructure material-based active electrodes with complemen- of electrodes was done using electrochemical workstation
tary operating potentials windows in an identical electrolyte to (CHI-660D) in 1 M Na2SO4 aqueous electrolyte. Further devel-
develop aqueous asymmetric SC (ASC), and this technique oped VN//Mo2N ASC also electrochemically tested in full-cell
will extend their operating voltage to get enhance energy density setup.
of SC.[15]
Herein, we have developed high-quality thin films of metal 3. Results and Discussion
nitrides in controlled vacuum using reactive sputtering to
broaden the working voltage toward the achievement of high 3.1. Structural Study and Morphology of Electrodes
energy density. These films were grown on the 304 SS substrate
at 200  C in a mixed Ar–N2 atmosphere. To exhibit the practical Morphologies of the deposited TMN-based electrodes were
feasibility, we have manufactured asymmetric cell using VN acquired by FE-SEM and shown in Figure 2, with the elemental
as negative and molybdenum nitride (γ-Mo2N) as positive color mapping by EDAX. Typical SEM image of top view of the
electrodes, respectively. The electrochemical study of assembled VN active electrode is shown in Figure 2a, and cross-sectional
ASC shows an optimum potential window of 1.4 V in 1 M view image of VN thin-film active electrode displays 519 nm thick
Na2SO4 electrolyte. Fabricated ASC shows the enhanced film growth (see the inset of Figure 2a). It appears that triangular

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Figure 1. Schematic representation of metal nitride thin films fabrication by sputtering technique and development of ASC device.

Figure 2. Surface morphology, FE-SEM images, and color elemental mapping of a,b) VN electrode and c,d) Mo2N electrode. The insets shows the
cross-sectional view, respectively.

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nanoflake-like prismatic structures are growing on the SS 304 sub- no. 00-025-1252). In addition, in this XRD pattern, neither
strate with voids between the triangular nanoflakes.[16] Figure 2c vanadium oxide nor metallic vanadium was spotted, indicating
shows the top view image of Mo2N active electrode with the cross- the growth of high purity of the VN nanoflake. Main peeks
sectional view image in the inset of Figure 2c, which confirm of Mo2N observed at 37.30 and 63.24 are attributed to the
the 580 nm thickness of the thin-film electrode. EDAX elemental (111) and (220) planes of cubic phase of Mo2N (JCPDS ICDD
color mapping confirms the uniform deposition and distribution no. 00-003-0907). Peeks other than main peek presented in both
of vanadium and nitrogen in the VN thin-film active electrode; the XRD curve are from the SS substrate. Grain size of deposited
see Figure 2b. Molybdenum (Mo) and nitrogen (N) are uniformly thin film was estimated by the Scherrer formula, and it is found
distributed in the Mo2N thin-film active electrode; see Figure 2d. around 53.8 nm for the VN active electrode and 36.60 nm for the
XRD curves of VN nanoflakes and Mo2N active electrodes Mo2N active electrode.
are shown in Figure 3 with bare SS diffraction pattern. VN The 3-D AFM images revealed the topography of both the active
nanoflakes main peek observed at 38.60 , which is attributed electrodes, as shown in Figure 4a,b. An analysis was done using
to the (111) planes of the cubic phase of VN (JCPDS ICDD the instrument’s data analysis software (NTMDT) and calculates
the root mean square surface roughness (δrms) for Mo2N and VN
active electrode, 3.6 and 5.11 nm, respectively; these low values of
roughness increase the hydrophilicity of the electrodes according
to the Wenzel equation and corroborate with the contact angle
result.[17] The 3D AFM surface topography suggests that the nano-
structure growth also confirms by the FE-SEM surface morphology.
Furthermore, the contact angle for distilled water (DW) and
used electrolyte Na2SO4 of active thin-film electrodes were exam-
ined by the sessile drop method and shown in Figure 4c,d. The
contact angle value of DW and Na2SO4 for Mo2N was found to be
56 and 24 , respectively, whereas the VN value of DW and
Na2SO4 was found to be 68 and 26 , respectively. These mea-
sured contact angle values confirm that both of the electrodes
have hydrophilic nature for the DW and super-hydrophilic nature
for used electrolyte Na2SO4. Active electrodes show the interca-
lation pseudo-capacitance charge storage mechanism, due to
super-hydrophilic behavior of active electrodes, and this conclu-
sion can be supported by reported data as Jilei Liu et al. talk about
insertion/de-insertion of cations without phase change, which
they confirm with the X-ray absorption spectroscopy. Jilei Liu
Figure 3. Crystalline study, XRD patterns of SS substrate, VN, and Mo2N et. al. and co-workers demonstrated that cyclic voltammetry
electrode. (CV) curves does not show any redox peak, same as EDLC typical

Figure 4. AFM topography of a) Mo2N and b) VN and contact angle measurement of c) Mo2N and d) VN.

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behaviour. In particular, a continuous, highly reversible change result.[23]The survey spectra of VN and Mo2N exhibited the
in the oxidation state results in the pseudocapacitors (PC) reveal- presence of V 3p, V 3s, V 2p, V 2s, N 1s and Mo 4s, Mo 3d,
ing slightly deviated rectangular shape of CV curve. In PC only Mo 3p, N 1s, Mo 3s, respectively; see Figure 5a,d. These mention
intercalation pseudo-capacitance shows behaviour near to species occurred without any impurities. In survey spectra of
EDLC.[18] Used aqueous electrolyte makes intimate contact with both the electrodes, C1s also occurred due to carbon tape or other
the active electrodes of the SC because of the super-hydrophilic contamination, presented in the chamber.
nature of active electrodes. It is well known that the hydrophilic To classify and assign components related to different chemi-
nature of the electrode surface is an substantial factor for cal environment, high-resolution (HR) XPS spectra of respective
better performance of the electrochemical SC.[19] Mane et al.[20] core elements were deconvoluted with the help of Gaussian func-
reported 21 contact angle for SnO2 thin-film electrode for high- tion. The HR XPS study of V 2p and N 1s in the full range spectra
performance SC application.[21] The surface energy of Mo2N and of the VN active electrode is shown in Figure 5b,c. The study of
VN thin-film active electrodes is obtained using two different fluids, surface chemistry of electrodes was done by decomposing the
i.e., water and diiodomethane calculated by Owens and Wendt V 2p and N 1s peaks. The investigation of the V 2p3/2 region
methods and found to be 45.23 and 35.16 mN m
1, respectively.[22] points out it to be a superposition of four peaks (which are at
517.10, 515.50, 514.20, and 513.40 eV binding energies), corre-
3.2. XPS Analysis of As-Deposited Thin-Film Electrodes sponding to the oxidation states of Vþ5 2p3/2, Vþ4 2p3/2,
Vþ3 2p3/2, and Vþ2 2p3/2, respectively. First, three oxidation states
XPS study was done to find out the presence of the elements and may come because of the slightest presence of vanadium oxide
their oxidation states in Mo2N and VN active electrodes, as in various stoichiometries VxOy, and Vþ2 2p3/2 state indicates the
shown in Figure 5a–f, and data were analyzed by PHI formation of VN.[24] The analysis of N 1s and deconvoluted peeks
Multipak software. The information depth for XPS is very shal- demonstrate the existence of VN, VOxNy, and N–X on the surface
low (5–10 nm), because it is a surface-sensitive technique. of VN electrode.[25]
However, when we acquired the survey scan, the traces of all ele- HR XPS of Mo 3d and N 1s in the survey spectrum of Mo2N
mental species are observed with distinctive intensities and core electrode is shown in Figure 5e,f. Peaks for Mo 3d and N 1s in the
level binding energies. For quantitative analysis, the peak area full spectrum of XPS were clearly observed. Mo3d energy region
and peak height sensitivity factor are used to determine the per- fitted by three pairs of 3d3/2–3d5/2 doublet attribute to different
centage atomic concentrations. The method, which utilizes peak valences includes Mo2N, Moþ6, and Moþ5. In HR XPS of N 1s,
area sensitivity factors typically, is the more accurate and satis- Mo 3p3/2 and N 1s peaks are so closed to each other, so that tail of
factory for quantitative work. To make this outcome more reli- both the peaks overlapped.[9–26] HR N 1s peaks are different for
able, we pick 2–4 spots on the sample surface and record the both the electrodes, because exact binding energy of an electron
XPS survey scan. Here, we determine the chemical composition depends not only upon the level from which photoemission is
at every spot and make a conclusion to find out a more accurate occurring but also upon the formal oxidation state and the local

Figure 5. XPS spectra a) survey scan of VN and b,c) HR spectrum of V 2p and N 1S, and d) survey scan of Mo2N and b,c) Mo 3 d and N 1S, HR spectrum.

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chemical and physical environment of the atom. Change in any indicates that these electrodes have good rate capability and excel-
one gives rise to small shifts in the peak position of the HR-XPS lent degree of reversibility. The specific and interfacial areal
spectrum. As, Mo and V, both exist in different oxidation states, capacitance values of the active electrodes are calculated
then their interaction with the nitride will be different due to the from CV curve using equations (S1 and S2, Supporting
coulombic interaction between the photo-emitted electron and Information) at several scan rates, presented in Figure S1a,b,
the ion core. This interaction is responsible in the diversity of Supporting Information. This also exhibits that the capacitance
nitride peak in the HR-XPS spectra.[27] values of active electrodes fall to lower values with the increasing
scan rate (10–100 mV s
1), which can be attributed to low diffu-
3.3. Electrochemical Performance of Individual Electrodes sion of electrolyte ions. At high scan rate (100 mV s
1), mostly
the outer surface layer of the active electrode material, take place
The prepared Mo2N and VN active electrodes were electrochem- in charge-discharge process and which results the less involve-
ically tested in aqueous 1 M Na2SO4 electrolyte, to scrutinize their ment of electroactive material.[29] The calculated capacitance
capacitive behavior, mechanistic ion transport properties and values of both the active electrodes and area of CV curve at
electrochemical stability before ASC device fabrication, pre- several scan rates are tabulated in Table S2, Supporting
sented in Figure 6. CV curves of Mo2N and VN active electrode Information.
at several scan rate from 10 to 100 mV s
1, whereas potential The electrochemical behavior of electrodes was further analyzed
window was 0 to þ0.7 V for Mo2N and
0.7 to 0 V for VN elec- using the galvanostatic charge–discharge (GCD) technique.
trode, show in Figure 6a,b. For both the electrodes, the shapes of GCD curves of electrodes at various current densities from
CV curves, at various scan rates, are quasi-rectangular, demon- 0.5 to 10 mA cm
2 with their respective positive and negative
strating the intercalation pseudo-capacitance charge potential working window, 0 to þ0.7 V for Mo2N and
0.7 to
storage mechanism as corroborated by the hydrophilic nature 0 V for VN active electrode, are shown in Figure S2a,b, Supporting
of electrodes. Although, these CV curves shows no particular Information. Specific and interfacial areal capacitance of electro-
peak, indicates that both the electrode shows near to EDLC des was calculated from GCD curves using equations (S3 and S4,
behavior. As a trademark behavior of reversible electrode, these Supporting Information) at different current densities shown in
electrode store charge through fast redox reactions.[28] With Figure 6c. VN active electrode has a high specific capacitance
increasing scan rate, the area of CV curves increases, which of 229 Fg
1 at 0.5 mA cm
2 in negative potential window, whereas

Figure 6. Electrochemical study of electrodes CV curves of a) Mo2N and b) VN active electrodes collected at a various scan rate in a three-electrode cell
c) areal and specific capacitance as a function of current density for both the electrodes and d) Nyquist plot of electrodes.

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the Mo2N shows 165 Fg
1 at 0.5 mA cm
2 in positive potential q
¼ qþ (1)
window. From Figure 6c, it is clear that the capacitance value
decreases, as the current density increases for both the active elec- Stored charge in both the electrode can be calculated using
trodes. This may happen because of increased electronic field in Equation (2).
the three electrode cell, which is proportional to the current
q ¼ C s  ΔV  m (2)
density and alter both the faradic and EDLC charge–discharge pro-
cesses. This decrement in capacitance with the increased current where Cs, m, and ΔV are the specific capacitance, active mass,
density can be attribute to the ion exchange mechanism, where at and potential window of that electrode.
low current density (0.5 mA cm
2), a high capacitance value Mass balance can be done by obtaining mass ratio between the
observed because ions of used electrolyte have enough time to active electrodes with the help of Equation (3)
intercalate into the electrode during charging and discharging pro-
cess.[30] Calculated specific and interfacial areal capacitance mþ C
 ΔV

¼ (3)
values at various current densities for both the electrodes are dis- m
C þ  ΔV þ
played in Table S3, Supporting Information. Nyquist plot for both
the electrodes is also shown in Figure 6d; both the plots have ver- where C represents the capacitance, ΔV represents the working
tical line in low-frequency region, and this represent that both the potential window, and m is the active electrode mass. Here, neg-
electrodes have ideal capacitive behavior. ative and positive signs associate with negative and positive elec-
trodes. We found that mass ratio between positive electrode and
negative electrode would be mþ/m
¼ 1.5, considering the
3.4. Electrochemical Study of ASC capacitance value at 0.5 mA cm
2 current density. Hence, the
mass loading of active positive electrode and negative electrodes
ASC is developed using VN as negative electrode (anode) because was well balanced to 0.3 and 0.19 mg cm
2, respectively.
of its negative potential working window (
0.7 to 0 V), whereas Furthermore, exploring the performance of VN//Mo2N ASC
Mo2N was used as positive electrode (cathode) due to its positive was tested in 1 M Na2SO4 using full-cell setup. Typical CV curve
potential working window (0–0.7 V). Schematic view of the metal of the cell from 0 to 1.4 V at a scan rate from 10 to 100 mV s
1 is
nitride-based ASC device is shown in Figure 7. We found that presented in Figure 8b. CV curve at a scan rate from 10 to
working potential window for VN and Mo2N active electrodes 100 mV s
1 retains the shape of curve and even at high potential
was in between
0.7 and 0 V and between 0 and 0.7 V, respec- scan rate does not show any sign of distortion in shape, indicat-
tively, as shown in Figure 8a. In case of ASC, sum of potential ing that the VN//Mo2N ASC had excellent reversibility and ideal
window of both the electrodes will work as cell voltage, resulting capacitive behavior.[32] The variation of capacitance value with a
in the operational potential window for VN//Mo2N ASC would scan rate of the VN//Mo2N ASC was calculated using equations
be 0–1.4 V. (S5 and S6, Supporting Information) from CV curve in terms of
It is essential to find out the balancing of mass between the mass and total area of electrodes and presented in Figure S3a,
negative and positive electrodes, prior to fabricating ASC device. Supporting Information. As scan rate increases, the capacitance
Here, we measure mass of current collector (SS) before and value gradually decreases, because only outer active surface of
after deposition, and by subtracting them, we get mass of active electrode takes place in charge storage, and due to the time
electrode. Mass balance between the electrodes is calculated constraints, diffusion mostly limited by the motion of Naþ ions
by balancing the store charge on electrodes with the help of and proton, resulting in the less electrochemical use of the
Equation (1).[31] electro-active material.[33] All calculated capacitance values at
various scan rate and area of CV curves tabulated in Table S4,
Supporting Information.
VN//Mo2N ASC was further analyzed using GCD at a current
density 0.5, 1, 5, and 10 mA cm
2, as shown in Figure S3b,
Supporting Information. For every current density, all curves
are symmetrical and highly linear, and they indicate that the
VN//Mo2N ASC has high electrochemical reversibility and
charge discharge properties, also confirmed by CV curve.
Capacitance at various current densities of the ASC is calculated
from GCD curve using equations (S7 and S8, Supporting
Information) in terms of mass and total area of electrodes, pre-
sented in Figure 8c and tabulated in Table S5, Supporting
Information. Calculated maximum specific capacitance value
was found to be 85.50 Fg
1 at 0.5 mA cm
2 current density
and gradually decreases with the increasing current density, even
at 10 mA cm
2, and the capacitance value was found to be
49.8 Fg
1 (presented in Table S4, Supporting Information).
CV and GCD curve of the VN//Mo2N ASC does not show
Figure 7. Schematic illustration of the assembled metal nitride thin-film- ideal shapes, typically found for EDLCs. This is because
based VN//Mo2N ASC device. both the electrodes show intercalation pseudo-capacitance

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Figure 8. Study of the as-constructed VN//Mo2N ASC device: a) CV of VN@SS anode and Mo2N@SS cathode at a scan rate of 10 mV s
1, b) CV curves
for several scan rates, c) areal and specific capacitance as a function of current density, d) Nyquist plot (and inset displays the magnified plot at high-
frequency region), e) Ragone plot of ASC, and f ) life span tested at 5 mA cm
2 current density for 5000 cycles (inset displays the first five and last
few cycles).

charging–discharging mechanism, as both the electrodes have equations (S9 and S10, Supporting Information). Plot between
super-hydrophilic nature. Figure 8d displays Nyquist plot from specific power and energy, known as Ragone plot shown in
100 mHz to 100 kHz frequency range where straight line in Figure 8e, and all calculated values for VN//Mo2N ASC are pre-
low-frequency region implies excellent capacitive behavior with- sented in Table S6, Supporting Information. Fabricated
out diffusion limitation in the fabricated VN//Mo2N ASC.[34] VN//Mo2N ASC has a high specific energy of 23.3 Wh kg
1
Furthermore, to investigate the efficiency of fabricated with a good specific power of 2700 W kg
1 at a low current den-
VN//Mo2N ASC, we calculate specific power and energy at var- sity of 0.5 mA cm
2. This ASC also shows good specific energy
ious current densities (0.5, 1, 5, and 10 mA cm
1) using for a high power density at 10 mA cm
2. These values of ASC

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are more promising than previously reported ASC device, such Keywords
as VOx//VN-ASC (2.1 Wh kg
1),[14b] MnO2//polyaniline
asymmetric supercapacitors, binder-free electrodes, metal nitride thin
(13.5 Wh kg
1),[35] MnO2//Fe2O3 (17.3 Wh kg
1),[36] Bi2O3//
films, sputtering techniques
activated carbon (AC) (10.2 Wh kg
1),[37] WO3//AC

1 [38]
(11.9 Wh kg ), Ni-CoO//AC (12 Wh kg
1),[39] CuS//AC Received: May 22, 2020
(15.06 Wh kg
1),[40] graphene//Ni6MnO8 (16.5 Wh kg
1),[41] Revised: July 21, 2020
AC//boron nitride/carbon (17 Wh kg
1),[42] AC//CaMoO4 Published online: August 18, 2020
(18.68 Wh kg
1),[43] AC//Ni3S2/multi-walled carbon nanotube-
carbon nanoparticle (19.8 Wh kg
1),[44] and Ni-doped Co–
Co2N//porous carbon (20.40 Wh kg
1).[45] To justify the perfor- [1] a) G. Gao, H. B. Wu, S. Ding, L.-M. Liu, X. W. Lou, Small 2015, 11,
mance of device, cycling test over 5000 cycles for the VN//Mo2N 804; b) M. Armand, J. M. Tarascon, Nature 2008, 451, 652; c) S. Najib,
E. Erdem, Nanoscale Adv. 2019, 1, 2817.
ASC was carried out at 5 mA cm
2 current density. Figure 8f
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The authors declare no conflict of interest. D.-H. Kim, Adv. Mater. Interfaces 2018, 5, 1800283.

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