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Anode Material of Vanadium Nitride for Supercapacitors: A Topic Review
Article in Journal of Materials Chemistry A · April 2020

DOI: 10.1039/D0TA01490G
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Journal of
Materials Chemistry A
REVIEW
Vanadium nitride for aqueous supercapacitors:

Cite this: J. Mater. Chem. A, 2020, 8,
a topic review
8218
Ying Liu,†a Qianghong Wu,†a Lingyang Liu,b Pantrangi Manasa,a Long Kanga
and Fen Ran *a
Supercapacitors have emerged as the most attractive complementary devices between batteries and
conventional capacitors, while a high performance electrode material is key to their energy storage
advancement. In recent years, research on electrode materials for supercapacitors has mainly focused
on the field of positive electrode materials. Compared with the positive electrode, the research on
negative electrode materials is mainly focused on carbon materials, and there are fewer types. As
a negative electrode material under aqueous alkaline test conditions, vanadium nitride has many
Received 8th February 2020
Accepted 7th April 2020
attractive advantages, such as a large potential window (in the range from 1.2 V to 0 V in alkaline
aqueous solution), high electrical conductivity, and high specific capacitance. In this review, we focus on
DOI: 10.1039/d0ta01490g
vanadium nitride based anode materials and carefully summary their energy storage mechanisms,
rsc.li/materials-a applications, advantages and disadvantages, and future development prospects.
storage and transfer of energy today mainly involve fuel cells

1. Introduction and electrochemical energy storage (EES) devices. EES devices
Due to the excessive exploitation of fossil fuels, the world faces mainly include various types of batteries and supercapacitors
severe environmental, ecological, and energy crises. The most (SCs).1–3 Compared with traditional batteries and fuel cells, the
direct and effective solution to all kinds of crises is to use bottleneck of the practical application of SCs is low energy
renewable green energy. However, there is a problem of uneven density (Fig. 1). To solve this problem, both designing suitable
distribution of renewable energy, which poses an important electroactive materials and selecting a suitable electrolyte are
challenge to the storage and transportation of energy. The crucial in boosting the energy harvesting. The electrolyte may be
aqueous or organic, where the former enables the device to
operate within a thermodynamic potential window of 1.23 V,
a
State Key Laboratory of Advanced Processing and Recycling of Non-ferrous Metals,
while the latter could output a maximum potential window of
School of Material Science and Engineering, Lanzhou University of Technology,
Lanzhou 730050, P. R. China. E-mail: ranfen@lut.edu.cn; ranfen@163.com 4 V. Traditional organic electrolyte materials have the advantage
b
Laboratory of Clean Energy Chemistry and Materials, State Key Laboratory of Solid of a large potential window and high energy density compared
Lubrication, Lanzhou Institute of Chemical Physics, Chinese of Academy of Sciences, to aqueous electrolytes. But with the advent of “water-in-salt”
Lanzhou 730000, P. R. China aqueous electrolytes, this advantage is gradually lost. And
† Dr Ying Liu and Dr Qianghong Wu contributed equally to this paper.
Ying Liu is a PhD student under Qianghong Wu received her B.S.

the supervision of Prof. Long and M.S. degrees from the
Kang and Prof. Fen Ran in the Lanzhou University of Tech-
State Key Laboratory of nology. Since 2018, she has been
Advanced Processing and Recy- pursuing her Ph. D. degree at the
cling of Non-ferrous Metal at the School of Materials Science and
Lanzhou University of Tech- Engineering at the Lanzhou
nology. Her research interest University of Technology under
focuses on vanadium nitride- the supervisor of Prof. Fen Ran
based anode materials for and Prof. Youzhi Wu. Her
supercapacitors. scientic research direction is
new energy materials.
8218 | J. Mater. Chem. A, 2020, 8, 8218–8233 This journal is © The Royal Society of Chemistry 2020
Review Journal of Materials Chemistry A
organic electrolytes are toxic, moisture-sensitive and costly performance electrode materials is a key challenge to achieve
compared to aqueous electrolytes. Furthermore, the viscosity is the desired goal of increasing energy density without sacricing
higher and ionic conductivity is lower for organic electrolytes their power density and cycle life.5
compared to those of aqueous electrolytes.4 Therefore, an SCs can be divided into two categories according to the
aqueous electrolyte is still the mainstream of the current energy storage mechanism: electric double layer capacitors
supercapacitor system also because of its low cost, good envi- and pseudocapacitors. Compared with double layer capaci-
ronmental friendliness, and potential high energy density tors, pseudocapacitors have higher energy density. However,
possibilities. However, since the traditional aqueous electrolyte conventional pseudocapacitors are mainly conductive poly-
is limited to thermodynamics and can't output wide potential mers and oxides, especially transition metal oxides. Tradi-
window, nding the electrode material with high capacitance tional transition metal oxides have been limited by poor
and large potential window within the potential range of stability and electronic conductivity. As potential alternative
aqueous electrolytes is the main research direction of state-of- materials, transition metal nitrides have received great atten-
the-art aqueous SCs. On the other hand, constructing high- tion due to their high electrical conductivity and have been
Lingyang Liu received his B.S. Long Kang is now a professor

degree in Material Chemistry and doctoral supervisor in the
from the Shandong University of School of Material Science and
Science and Technology in 2013 Engineering at the Lanzhou
and M.S. degree in Material University of Technology. He is
Physics and Chemistry from the mainly engaged in the research
Lanzhou University of Tech- and development of functional
nology in 2016. He is currently materials such as welding
pursuing his PhD degree at the metallurgy, electrochemical
Lanzhou Institute of Chemical energy storage and hydrogen
Physics (LICP), Chinese storage alloys.
Academy of Sciences (CAS). His
research interests are focused on
the design and fabrication of multifunctional energy storage
devices, especially supercapacitors, and the related functional
mechanism study.
Dr Pantrangi Manasa received Prof. Fen Ran received his PhD

her M.Sc. and PhD degrees from degree in biomedical engi-
Sri Venkateswara University, neering from Sichuan University
India. She is currently working (State Key Laboratory of Poly-
as a post-doctoral research mer Materials Engineering),
fellow at the State Key Labora- China in 2012. In 2013, he
tory of Advanced Processing and worked in the Department of
Recycling of Non-ferrous Metals, Chemical and Biochemical
School of Materials Science and Engineering at the National
Engineering at the Lanzhou University of Singapore, as
University of Technology under a research fellow. From 2015 to
the supervisor of Prof. Fen Ran. 2016, he worked in the Depart-
Her research interest has been ment of Chemistry and
focused mainly on the design and fabrication of new kinds of Biochemistry at the University of California, Santa Cruz, as
biomass derived energy storage devices. a visiting scholar. In 2018, he worked in the Department of
Materials at the University of California, Santa Barbara, as
a visiting professor. Starting from 2019, he became a full professor
at the State Key Laboratory of Advanced Processing and Recycling
of Non-ferrous Metals and School of Materials Science and Engi-
neering, Lanzhou University of Technology, China. His research
interests include advanced materials for energy and conversion
devices, e.g., supercapacitors and lithium-ion and sodium-ion
batteries, and biomedical polymeric materials, e.g., membrane
science, separation and purication, and blood contact materials.
This journal is © The Royal Society of Chemistry 2020 J. Mater. Chem. A, 2020, 8, 8218–8233 | 8219
Journal of Materials Chemistry A Review
This work opens a new path for the application of VN materials

in SCs. The material exhibits a high specic capacitance, but its
rate performance and cycle stability are unsatisfactory. The
authors indicate that the poor cycle stability of VN is caused by
the presence of oxides. All tests are performed under a very low
load package. The highest specic capacitance is recorded at
a low scan rate of 2 mV s1; when tested at 100 mV s1, it
decreases to 554 F g1. The obtained VN prepared at 1000 C
only exhibits a capacitance of 58.3 F g1 at 2 mV s1 (Fig. 2).
Subsequently, Hanumantha et al. also used this method to
prepare VN. The prepared VN was applied in conjunction with
commercial VN to study the effect of VN particle size on its
electrochemical performance using mechanical milling. And
they found that very ne nanoparticles of VN end up being rate
Fig. 1 Ragone plots of energy storage devices.
limited on account of poor electronic conductivity.12
In the 1980s and 1990s, Oyama et al. rst proposed
a temperature-controlled method for the synthesis of transition
utilized as active materials for SCs.6–9 Among transition metal metal nitrides and carbides. At that time, the gas atmosphere
nitrides, vanadium nitride (VN) has become the most well they used was a mixture of H2 and N2.83 Later, the authors tried
studied material for SCs, because of not only the high specic to use this method to reduce the oxide in NH3 to synthesize
capacitance but also the good electrical conductivity (about 1.6 transition metal nitrides such as VN,84 which was widely used in
106 S m1 for pure cubic VN). It is worth noting that VN the elds of hydrodenitrogenation, CO hydrogenation, and NH3
based materials are typically used as anode materials for SCs, synthesis.85 Zhou and others then introduced the VN synthe-
so their single-electrode electrochemical properties are usually sized by this method into the eld of electrochemical energy
tested in negative potential windows, which allows them to storage.13 And then Chen et al. used a solid-state temperature
form SC devices with most transition metal oxides. And program reaction to promote this method.14 A series of VN
compared to the anode material of traditional aqueous materials with different pore size (in the range of 15–110 nm)
supercapacitors (mainly carbon material), vanadium nitride structures were synthesized and systematic performance tests
has a maximum potential window of 1.2 V in an alkaline were performed on them. Chen et al. continued to rene the
aqueous solution system and an incomparable theoretical work of Choi et al. in O2 passivation and found that the domi-
specic capacitance30 (1350 F g1). nant state at the nitride surface are V5+ and V3+ states while not
the most likely V4+ oxidation state in the previous publica-
tions.10 Thompson et al. also synthesized VN using a pro-
grammed temperature reaction and further studied the theory
2. Vanadium nitride materials of the inuence of an oxygen passivation layer proposed by
Table 1 is compiled in order to let the reader know the elec- Chen et al. They rst passivated the synthetic VN to avoid bulk
trochemical characteristics of VN more intuitively. oxidation when exposed to air. At the same time, the passivated
VN has two main synthesis methods, one is a chemical material was activated in 0.3 M NaOH solution to remove the
synthesis method including different nitrogen source thermal oxygen-rich passivation layer. They found that aer activation,
reduction of precursors with vanadium sources and the other is the electrochemical stability and specic capacitance of VN
a physical synthesis method, which mainly refers to the materials changed signicantly.82
magnetron sputtering ball-milling method. Combustion Chen et al. also tried to test the electrochemical performance
synthesis is the most traditional method of synthesizing VN.10,11 of VN in different solution environments. The following reac-
The rst vanadium source for combustion synthesis is VCl4, tion may occur during these processes:
which is usually used to react with NH3 to prepare V(NH3)Cl to Vxþ2y=3 Nx Oy þ zMþ þ ze 4Vxþð2yzÞ=3 Nx Oy Mz zþ ðMþ
form a precursor; it is then reacted with NH4Cl at high
¼ Liþ ; Hþ .Þ (2)
temperature to prepare VN products. This method was rst
proposed by Choi et al.11 In their experiments, the introduction But the test window is 0.2–0.6 V under neutral and acidic
of O2 for passivation in the catalytic eld to treat the synthesized conditions, which is much smaller than that under alkaline
VN demonstrates that the oxides presented in the VN material conditions. VN has an acceptable capacitance retention rate in
play an important role in the performance of SCs. The prepared three kinds of electrolytes, which maintained approximately
nanometer-sized VN exhibits an impressive 1340 F g1 specic 80% of its maximal capacitance at 1 A g1. Wang et al.15 later
capacitance at 2 mV s1. And for the rst time, the possible tried to promote the study of electrolytes. They obtained the
reaction mechanism of VN under alkaline conditions is following reaction formula by using a common electrolyte for
proposed as in SCs (formula (1)). lithium batteries LiPF6 as the electrolyte:
VNxOy + OH 4 VNxOy//OH + VNxOy–OH (1)
Table 1 Electrochemical characteristics of VN-based materials
Potential Stability, cycle number, test

Materials Electrolyte window Specic capacitance Loading mass current Ref.
VN-400 C 1 M KOH (1.2–0) V 1350 F g1 0.25 mg cm2 ——, ——, 2 mV s1 10
KOH, pH z 12 (1.2–0.3) V About 430 F g1 0.21 mg cm2 Nearly 93%, 1000, 50 mV s1
KOH, pH z 12 (1.2–0.3) V About 380 F g1 0.41 mg cm2 Nearly 92%, 1000, 50 mV s1
KOH, pH z 14 (1.2–0.3) V About 400 F g1 0.29 mg cm2 Nearly 62.5%, 1000, 50 mV s1
KOH, pH z 14 (1.2–0) V About 430 F g1 0.40 mg cm2 Nearly 0%, 1000, 50 mV s1
VN-400 C 1 M KOH (1.2–0) V About 250 F g1 — Nearly 45%, 350, 50 mV s1 11
VN-500 C 1 M KOH (1.2–0) V About 200 F g1 — Nearly 65%, 350, 50 mV s1
VN-600 C 1 M KOH (1.2–0) V About 150 F g1 — Nearly 100%, 350, 50 mV s1
VN 1 M KOH (1.2–0) V About 1050 F g1 0.008 mg cm2 Nearly 20%, 200, 10 mV s1 12
1 M KOH (1.2–0) V About 300 F g1 0.03 mg cm2 Nearly 0%, 200, 10 mV s1
VN 1 M KOH (0.95–0.15) V 161 F g1 — ——, ——, 30 mV s1 13
1 M KOH (0.95–0.15) V 6.2 mF cm2 — ——, ——, 30 mV s1
1 M KOH (0.95–0.15) V 4.4 mF cm2 — ——, ——, 300 mV s1
1 M KOH — — — 70%, 400, ——
VN 1 M H2SO4 (0.2–0.6) V About 100 F g1 4–6 mg cm2 ——, ——, 100 mA g1 14
1 M KOH (1.2–0) V 225 F g1 4–6 mg cm2 ——, ——, 500 mA g1
3 M NaCl (0.2–0.6) V About 100 F g1 4–6 mg cm2 ——, ——, 100 mA g1
VN 1 M KOH (1.0–0) V 177 C g1 — ——, ——, 5 mA g1 15
1 M LiCl (1.0–0) V 90 C g1 — ——, ——, 5 mA g1
1 M LiPF6 (0–2.5) V 154 C g1 — ——, ——, 5 mA g1
V2O3-180 min (VN) 2 M KOH (1.0–0.1) V 152 F g1 7.60 mg cm2 56%, 1000, 1 A g1 16
VN nanowires LiCl/PVA gel (1.2–0) V 298.5 F g1 0.71 mg cm2 ——, ——, 1 A g1 17
LiCl/PVA gel (1.2–0) V About 225 F g1 0.71 mg cm2 95%, 10 000, 100 mV s1
Nanostructured VN 0.1 M KOH (1.0–0.3) V About 30 F g1 3 mg cm2 Nearly 100%, 3000, 50 mV s1 18
0.5 M KOH (1.0–0.3) V About 55 F g1 3 mg cm2 Nearly 100%, 3000, 50 mV s1
1 M KOH (1.0–0.3) V About 60 F g1 3 mg cm2 Nearly 95%, 3000, 50 mV s1
Sputtered VN thin 1 M KOH (1.2–0) V 422 F g1 25 nm thick ——, ——, 5 mV s1 19
lms
0.01 M KOH (1.2–0) V 24 F g1 480 nm thick Nearly 146%, 100, 200 mV s1
1 M KOH (1.2–0) V About 42 F g1 480 nm thick Nearly 202%, 100, 200 mV s1
5 M KOH (1.2–0) V About 47 F g1 480 nm thick Nearly 238%, 100, 200 mV s1
Sputtered VN thin 1 M KOH (1.2–0) V 238.2 mF cm2 1550 nm thick 78%, 2000, 25 mV s1 20
lms
Sputtered VN-100 C 1 M KOH (1–0.4) V 45 mF cm2 0.34 mm thick 70%, 10 000, 50 mV s1 21
Sputtered VN-350 C 1 M KOH (1–0.4) V 28 mF cm2 0.34 mm thick 70%, 10 000, 50 mV s1
Sputtered pure VN 1 M KOH, 1 M LiOH (1–0.4) V 2–3 mF cm2 1 nm–400 nm ——, ——, 3 mV s1 22
thick
Sputtered pure VN 1 M KOH (under (1–0.4) V 19 mF cm2 140 nm thick 96%, 10 000, 20 mV s1 23
N2 )
Milled VN 1 M KOH (1.2–0) V 25–60 F g1 0.25 mg cm2 Nearly 103%, 200, 100 mV s1 24
VN 0.5 M H2SO4 (0.5–0.5) V 114 F g1 4 mg cm2 ——, ——, 30 mV s1 25
2.0 M NaNO3 (0.7–0.3) V 45.7 F g1 4 mg cm2 ——, ——, 30 mV s1
1.0 M KOH (1.1–0) V 273 F g1 4 mg cm2 ——, ——, 30 mV s1
VN/PCNPs 2 M KOH (1.15–0) V 255 F g1 4 mg cm2 66%, 1000, 1 A g1 26
VN/NGr 6 M KOH (1.2–0) V 255 F g1 1 mg cm2 ——, ——, 10 mV s1 27
6 M KOH (1.2–0) V About 220 F g1 1 mg cm2 94%, 2000, 30 mV s1
Mesoporous VN 6 M KOH (1.1–0.1) V 598 F g1 — ——, ——, 4 A g1 28
6 M KOH (1.1–0.1) V About 450 F g1 — 83%, 5000, 10 A g1
Nanostructured VN 0.1 M KOH (0.9–0.1) V — 3 mg per piece 93%, 2700, 50 mV s1 30
0.1 M KOH (1.2–0) V About 650 mF cm2 3 mg per piece ——, ——, 2 mV s1
VN/CNTs 6 M KOH (1.2–0) V 270 F g1 7.2–8 mg cm2 ——, ——, 2 mV s1 39
0.5 M Na2SO4 (0.9–0) V — 30 mg cm2 115.9%, 1000, 50 mV s1
VN-MWCNT 0.5 M Na2SO4 (0.9–0) V 160 F g1 15 mg cm2 ——, ——, 2 mV s1 40
VN/CNT 0.5 M Na2SO4 (0.1–0.4) V 37.5 mF cm2 1300 nm thick ——, ——, 2 mV s1 41
0.5 M Na2SO4 (0.1–0.4) V About 12 mF cm2 1300 nm thick 85%, 2000, 200 mV s1
VN/CNTF KOH/PVA gel (1.2–0.2) V 188 F cm3 (564 mF — ——, ——, 1 mA cm2 42
cm2)
VN/NG 6 M KOH (1.2–0) V 445 F g1 2 mg cm2 ——, ——, 1 A g1 44
6 M KOH (1.2–0) V About 370 F g1 2 mg cm2 98.66%, 10 000, 10 A g1
Table 1 (Contd. )
Potential Stability, cycle number, test

Materials Electrolyte window Specic capacitance Loading mass current Ref.
3D VNPN/G 1 M KOH (1.0–0) V 164.4 F g1 2 mg cm2 ——, ——, 0.3 A g1 45
1 M KOH (1.0–0) V About 150 F g1 2 mg cm2 97.5%, 2500, 0.5 A g1
VNQD/CNF 6 M KOH (1.2–0.2) V 406.5 F g1 4 mg cm2 ——, ——, 0.5 A g1 46
1 M KOH (1.1–0.1) V About 380 F g1 3.51 mg cm2 90%, 10 000, 10 A g1
PCNS@VNNP 2 M KOH (1.2–0) V About 165 F g1 4 mg cm2 ——, ——, 1 A g1 47
2 M KOH (1.2–0) V About 120 F g1 4 mg cm2 62.5%, 5000, 5 A g1
VNQDs/PC 6 M KOH (1.15–0) V 281 F g1 4 mg cm2 ——, ——, 0.5 A g1 48
CF@VN 2 M KOH (1.1–0.1) V 104.05 F g1 4 mg cm2 ——, ——, 0.5 A g1 49
Nano-VN/IPC 2 M KOH (1.15–0) V 284 F g1 4 mg cm2 ——, ——, 0.5 A g1 50
CNS@VN 6 M KOH (1.2–0) V 300.4 F g1 4 mg cm2 ——, ——, 1 A g1 51
6 M KOH (1.2–0) V 178.8 F g1 4 mg cm2 70.8%, 5000, 5 A g1
VN/C 2 M KOH (1.2–0) V 195.7 F g1 4 mg cm2 ——, ——, 1 A g1 52
2 M KOH (1.2–0) V About 100 F g1 4 mg cm2 75%, 5000, 5 A g1
N-CNS/VNNPs 2 M KOH (1.2–0) V 280 F g1 4 mg cm2 ——, ——, 1 A g1 53
HPCF@VNNP 6 M KOH (1.1–0) V 240.5 F g1 4 mg cm2 ——, ——, 0.5 A g1 54
6 M KOH (1.1–0) V 210.8 F g1 4 mg cm2 98%, 10 000, 2 A g1
VN/C 6 M KOH (1.2–0) V 392 F g1 4 mg cm2 ——, ——, 0.5 A g1 55
6 M KOH (1.2–0) V 295 F g1 4 mg cm2 83.5%, 5000, 2 A g1
VNNP@GO 2 M KOH (1.2–0) V 109.7 F g1 4 mg cm2 ——, ——, 1 A g1 56
2 M KOH (1.2–0) V 90 F g1 4 mg cm2 93%, 5000, 2 A g1
VNNDs/CNSs 1 M KOH (1.1–0.1) V 573.1 F g1 3.51 mg cm2 ——, ——, 1.1 A cm3 62
TiN/VN 1 M KOH (1.0–0.1) V 170 F g1 2–5 mg cm2 ——, ——, 2 mV s1 63
1 M KOH (1.0–0.1) V About 130 F g1 2–5 mg cm2 89%, 500, 20 mV s1
TiN–VN 1 M KOH (1.2–0.2) V 247.5 F g1 — ——, ——, 2 mV s1 64
1 M KOH (1.2–0.2) V — — 88%, 500, 100 mV s1
3D carbon@TiN@VN 1 M KOH (0.6–0.2) V 198.3 F g1 — ——, ——, 5 A g1 65
1 M KOH (0.6–0.2) V 125 F g1 — About 83%, 4000, 5 mA cm2
MVN@NC NW lm 6 M KOH (1.1–0.2) V 282 mF cm2 — ——, ——, 1.44 mA cm 2 70
6 M KOH (1.1–0.2) V — — 91.8%, 12 000, 200 mV s1
Passivated VN 0.1 M H2SO4 (0.65–0.65) V 60 F g1 3 mg per piece Nearly 91.7%, 2700, 50 mV s1 82
Activated VN 0.1 M H2SO4 (0.65–0.65) V 100 F g1 3 mg per piece Nearly 90%, 2700, 50 mV s1
VN thick lms 1 M KOH (1.0–0.4) V 1.2 F cm2 16 mm thick ——, ——, 5 mV s1 86
1 M KOH (1.0–0.4) V About 0.85 F cm2 16 mm thick 80%, 20 000, 50 mV s1
VN4 1 M KOH (1.2–0) V About 162 mF cm2 — ——, ——, 5 mV s1 87
VN4 1 M KOH (1.2–0) V About 63 mF cm2 — 47.6%, 2000, 50 mV s1
VN@sVO2 1 M KOH (1.2–0) V 149.5 F g1 4 mg cm2 85%, 1000, 1 A g1 88
VN + xLi+ + xe 4 LixVN (3) Lucio-Porto et al., and the effect of the thickness of the prepared
VN lm on the capacitance performance was studied. A thin
This method which can effectively design the morphology of the lm with a thickness of 25 nm shows the highest specic
obtained materials by controlling the morphology of the capacitance (422 F g1) in a 1 M KOH electrolyte.19 Other
precursors has been most widely used to prepare VN (Fig. 3).16 researchers have studied the effects of different sputtering
At the same time, Lu et al. found that if VN is wrapped by LiCl times and different sputtering space compositions on the
gel, its structure does not collapse easily, which can effectively electrochemical properties of VN materials.20,21
improve its electrochemical cycle stability.17 They also tried to Due to the controllability of magnetron sputtering and in
prepare VN by reduction of Zn3(OH)2(V2O7)$(H2O)2 in order to further clarify the effect of oxides on the performance of
ammonia.18 The effect of KOH solution concentration on the VN materials in SCs, Bondarchuk et al.22 attempted to eliminate
performance of VN capacitors was also investigated. They found the presence of oxygen in an oxygen-free environment using
that the required transformation overpotential for V2+ to V3+ in magnetron sputtering to get insight into the details of the
concentrated KOH solutions is much lower than that in diluted electrochemical activity of pure VN materials. The authors
solutions, indicating that concentrated solutions are kinetically constructed a pure VN lm of 100–400 nm and found an
more favorable than diluted solutions. effective subsurface layer with an effective charge accumulation
The conventional magnetron sputtering method for thickness of 100 nm. It is also proved that there is no valence
preparing conventional VN materials was rst proposed by change in the electrochemical energy storage process of pure
Fig. 2 The (a) CVs of VN nanocrystals synthesized at 400 C at various scan rates (2–100 mV s1) in a 1 M KOH electrolyte (DV: 0 to 1.2 V) and (b)
specific capacitance versus scan rate with different active-material loading. (c) FTIR spectra of (I) VN nanocrystals obtained at 400 C, (II)
immersed in 1 M KOH solution for 24 h, and (III) after ten cycles. XPS spectra of VN nanocrystals (d) before and (e) after electrochemical cycling up
to 200 cycles. (f) CV of VN nanocrystals synthesized at 600 C scanned at 2 mV s1 in a 1 M KOH electrolyte and (g) cycling behavior of VN
nanocrystals synthesized at 400 C scanned at 50 mV s1 up to 1000 cycles (cell A: DV: 0.3 to 1.2 V/electrolyte pH z 12, cell B: DV: 0 to 1.2
V/electrolyte pH z 14, and cell C: DV: 0.3 to 1.2 V/electrolyte pH z 14). Copyright 2006 Willey.
VN. The early charge storage mechanism of VNxOy materials that the material was still partially oxidized (Fig. 4a). Second, in
involves the reduction of vanadium cations by hydroxyl groups, this work, the VN material did not reach the potential window of
which is not suitable for pure VN. Based on this situation, 1.2 V in the traditional water system (only 0.6 V). The reason for
Bondarchuk et al. proposed a space charge accumulation this is really worthy of further investigation (Fig. 4b).
mechanism as an alternative to the common surface faradaic The authors of the same group later determined the effect of
reactions (pseudocapacitance) and electrical double layer (EDL). the presence of oxygen in the electrolyte on the stability of VN
However, there are still some problems that cannot be ignored cycling. They demonstrated that VN is active for the oxygen
in this work. First, the authors also acknowledged in the article reduction reaction and the presence of oxygen in the electrolyte
that although they avoided VN oxidation as much as possible should be avoided.23 And the author believes that in order to
during the preparation process, the nal experiment showed maintain a good cycle life, the potential window should be kept
between 1.0 V and 0.4 V (Fig. 4c and d).
The discussion of VN surface oxides in recent reports is also
lively. Chen et al.87 studied the detailed surface chemistry
composition of VN by depositing VN by DC reactive sputtering
at different working pressures. They found that V2+ seems to
play a very important role in the oxide on the VN surface for
pseudocapacitance.
From another study of Hanumantha, the ball-milling
method offers another idea to improve the cycle life by adjust-
ing the composition of the surface oxide while maintaining
a high potential window.24 The authors prepared a VN material
with a single oxide of VO2 on the surface by a hybrid ball milling
process of LiN and V2O3 and found that the material has good
cycle stability while maintaining a potential window of 1.2 V
(Fig. 5). This theory was recently conrmed by the work of Liu
et al.88 This also veries the previous Chen et al.'s conjecture,
which has extraordinary signicance for the control of the
surface oxide composition of VN materials.
Fig. 3 Schematic illustration of the synthesis process of the
The synthesis processes of VN materials by the above-
V2O5$1.6H2O xerogel, V2O3, and VN. Copyright 2016 The Royal mentioned chemical methods need to be carried out under
Society of Chemistry. the dangerous conditions of high temperature and NH3 and has
Fig. 4 (a) V 2p and O 1s XPS spectra of another VN 160 nm film before and after electrochemical testing. Solid line depicts the V 2p and O 1s XPS
spectral range for the as-grown film which was exposed to the environment of an argon filled electrochemical cell (before coming into contact
with the electrolyte). The XPS spectra revealed 5 at% of oxygen. Dotted and dashed lines represent spectra recorded after charging to 0.4 V vs.
the Ag/AgCl electrode in 1 M KOH (positive cut-off potential) and after charging to 1 V vs. the Ag/AgCl electrode in 1 M KOH (negative cut-off
potential) respectively. The evolution of the oxygen 1 s line reflects the accumulation of contaminants: spectrum at 0.4 V was recorded before
the spectrum at 1 V; (b) CVs for a VN 240 nm thick film recorded in a KOH electrolyte with different concentrations: 0.1 M, 0.3 M, 1 M and 3 M
KOH. Copyright 2016 Elsevier. (c) Specific capacitance and (d) relative capacitance retention over 1000 cyclic voltammetry cycles at 20 mV s1 in
between 1.0 V and three different upper limits: 0.5 (-), 0.4 (C) and 0.3 V (:). The insets present the first (A) and 1000th (B) cyclic
voltammograms obtained for different potential windows (from left to right: (i) [1.0; 0.5]; (ii) [1.0; 0.4]; and (iii) [1.0; 0.3] V). Copyright
2016 Electrochemical Society.
high requirements for experimental operation and conditions, a main body of VN.25 This method effectively avoids the
so some researchers have proposed other methods for reducing potential safety hazards caused by the use of NH3. Subse-
vanadium-containing particles (such as oxides, chlorides, V- quently, Ran et al. modied this method to prepare a V-MOF
MOFs, etc.) with organic amines to get VN. precursor with a regular morphology and further obtained
Cheng et al. rst adopted a method of blending V2O5 with a VN composite with a higher specic capacitance.26 This
melamine to carry out high-temperature reduction in a rela- method was later promoted and studied many times. Repre-
tively safe N2 atmosphere and nally obtained a material having sentatively, Liu et al. obtained layered high cycle stability VN/
Fig. 5 (a) Galvanostatic charge–discharge profile of mechano-chemically synthesized VN at a current density of 100 mA g1 (active material
loading ¼ 1.1 mg cm2); (b) long term charge–discharge cyclability of mechano-chemically synthesized VN (current density ¼ 100 mA g1; active
material loading ¼ 1.1 mg cm2); (c) cycling behavior of VN made by mechano-chemical milling at a scan rate of 100 mV s1 (active material
loading ¼ 0.25 mg cm2). Copyright 2013 Electrochemical Society.
nitrogen-doped graphene composites by using dicyandiamide

instead of melamine.27 Other non-organic amines are used to
reduce the V source in N2 to prepare a VN-containing material,
which will be discussed in detail in Section 3.2.
In recent research work, Lee et al. proposed a method for the
preparation of VN by low-temperature urea reduction based on
the mechanism of coordination of organic amines and vana-
dium salts, which made it possible to synthesize VN under
further mild conditions.28 They used a mixture of urea and VCl4
to react at 70 C and directly obtained VN products without high
temperature conditions. However, the VN synthesized by this
method has a disadvantage that cannot be ignored, which is
a low coulombic efficiency is (Fig. 6) in an electrochemical
reaction process.
The research on the energy storage mechanism of VN has Fig. 7 Pseudocapacitive charge storage mechanisms of nano-
structured vanadium nitrides. Copyright 2019 Elsevier.
gone through several stages. As described earlier, the most clas-
sical and accepted theory is the reaction of VNxOy with OH,
including both EDL and pseudocapacitance. However, this
theory is relatively vague, and later generations have supple- effectively improve the cycling stability of VN. We will discuss the
mented them one aer another. Subsequently, it is proposed stability in detail later.
that, the charge storage of pure VN neither is the traditional
V3+N + 2OH + e 4 V2+N(OH)2 (4)
EDLC nor pseudocapacitance, but is the charge accumulation
effect. However, this theory is still controversial depending on
specic experimental circumstances. Aer that, Djire et al. ob-
tained the degree of pseudocapacitance of VN in aqueous solu-
tion by performing cyclic voltammetry and electrochemical 3. Vanadium nitride/carbon
impedance spectroscopy. The pseudocapacitance contribution to composites
the total capacitance in VN is much higher than EDL capacitance
and ranged from 85% in basic electrolytes to 87% in acidic In electric double layer capacitors, an electric double layer is
electrolytes.29 In recent work, they proposed a new reaction formed at the surface of the electrolyte electrode due to static
mechanism through in situ small angle neutron scattering (SANS) electricity to achieve energy storage. This requires that the mate-
and in situ X-ray absorption spectroscopy (XAS) (formula (4), rial needs to have a high specic surface area, good electronic
Fig. 7).30 Robert et al.86 adopted several advanced characterization conductivity, and stable properties in the electrolyte, and the
techniques to investigate the pseudocapacitive behavior of sput- carbon material meets these requirements.31–35 Pseudocapacitance
tered vanadium nitride lms in an aqueous electrolyte and put is achieved by a rapid reversible redox process on the surface of
forward the energy storage mechanism. The authors also agree the electrode material. Almost all transition metal nitrides, oxides,
with the important role of the V4+ oxide on the VN surface that we and hydroxides belong to this type of energy storage mechanism,
mentioned above. And the cycling stability results are also which makes these materials have a much better storage capaci-
consistent with those of the predecessors. That is, V4+ oxide can tance than carbon materials.36–38 As we have seen from the
previous article, when VN particles are excessively rened, it will
affect their conductivity. Therefore, designing a composite of
carbon materials and VN is a subject worthy of further study.
The purpose of the combination of VN and carbon materials
can be roughly divided into two categories, one is that the
rened VN is enhanced by combination with carbon materials,
and the other based on the results of Lu' research is that
wrapping the VN particles can increase the cycle stability.17
3.1 Shaped carbon composite VN

Shaped carbon materials have a relatively high degree of
graphitization and have unparalleled electronic conductivity
compared to other carbon materials. The combination of
a shaped carbon material (such as graphene, carbon nanotubes)
that has high electronic conductivity with VN particles can
Fig. 6 Galvanostatic charge–discharge curves of vanadium nitride maintain excellent specic capacitance of VN while providing
electrodes in a 6 M KOH electrolyte at current densities of (a) 4, (b) 6, better electronic conductivity, thereby exerting the synergistic
(c) 8, and (d) 10 A g1. Copyright 2016 Elsevier. advantages of the two.39–45
3.2 Amorphous carbon composite VN then carry out ammonia reduction to obtain a TiN/VN
composite. The cycle stability of the composite was signi-
Most of the carbon and VN composites that are obtained by the
cantly improved and remained at 89% aer 500 cycles; the
high temperature reduction method belong to this category.
authors attributed it to the fact that the material has good rate
More detailed research is done by Ran's group, who reported
performance (Fig. 8a). And the composite material has a higher
many materials prepared from different precursors using VN
specic capacitance due to good electron conductivity.63 Later,
quantum dots and carbon composites, all with excellent cycle
Zhou et al. used a coaxial spinning method to anneal in
stability.26–27,46–56,88 This composite method can form
a composite of various morphologies due to the malleable ammonia to obtain a tighter TiN–VN core–shell composite. And
carbon precursor being organic or macromolecular.43,57–62 the cycle stability is greatly improved compared with pure VN64
and about 88% of original capacitance was retained aer 500
cycles (Fig. 8b). Aer this, Pang et al. tried a three-dimensional
4. Other vanadium nitride-based composite material of TiN@VN grown on 3D carbon and ach-
composites ieved excellent cycle stability. Aer 2000 cycles, the specic
capacitance is only attenuated by 5%.65 For this excellent
In Sections 2 and 3, we have mentioned some non-negligible improvement, Guo et al. tried to apply a synthetic vanadium
problems in the synthesis method and mechanism. The most pentoxide core–shell heterostructure ber electrode to the
prominent ones are the poor cycle stability, and aer the wearable eld.66
particle is ned, as the continuity of the material structure is
destroyed, the electronic conductivity is attenuated, and the
capacitance is reduced. In response to these two outstanding 4.2 Ternary composites
problems, relevant researchers have carried out the operation of The ternary compound may come from an unexpected result
compounding other substances on VN materials and achieved during the experiment. Zhang et al. attempted to prepare VN from
good results. glucose and NH4VO3 in a non-reducing atmosphere (N2). The
product was determined to be a ternary complex of VN/V2O3/C.
4.1 Composites of VN/TiN This complex has amazing cycle stability. Aer cycling 4000 times,
It is well known that, as a transition metal element, the nitride the initial specic capacitance of 99.4% can still be maintained
of titanium (Ti) has excellent electronic conductivity and cycle (Fig. 8c).67 Jiang et al. also obtained a Ni/VN/NC ternary composite
stability. However, its specic capacitance is relatively too low. in a one-step process in an N2 atmosphere. It shows a remarkable
Dong et al. tried to combine the V2O5 gel with industrial TiN and cycle stability of 73.5% aer 5000 cycles (Fig. 8d).68
Fig. 8 (a) The capacitance retention of TiN/VN composite electrodes as a function of cycle number at a scan rate of 20 mV s1 in 1 mol L1 KOH
aqueous solution. Copyright 2011 Elsevier; (b) cycling performance of composite core–shell structured TiN–VN fibers at a scan rate of 100 mV
s1. Copyright 2011 American Chemical Society; (c) electrochemical properties of the VN/V2O3/C composite: cycling performance. Copyright
2011 Elsevier; (d) long-term cycling stabilities of the 3-Ni/NC, VN/NCs-7 and 3-Ni/VN/NCs-7 electrodes at 10 A g1. Copyright 2019 Elsevier.
5. Supercapacitor devices with VN- article about VN, the cyclic voltammetry curves are not consis-
tent with the curve summarized in Gogotsi's work.80,81 For
based materials as anodes formulas (2) and (3), it is a similar mechanism. It is believed
According to eqn (5), to obtain high energy density SCs,6,69 high that various ions form electric double layers with VN, but the
capacitance (C) and/or a large potential window (V) are needed, electrochemical curves prove that they do not conform to the
especially the latter. known theoretical curve.
Formula (4) proves that the energy storage of VN is directly
E ¼ 0.5 CV2 (5) related to OH embedding. According to the experimental
results (Fig. 10),27 the curve of the VN material is closer to that
VN has a 1.2 V large potential window (Table 1) in a conven- shown in Fig. 9 (type B). That is to say, there should be two
tional aqueous electrolyte. Especially in practical applications, control processes for the VN material, namely, intercalation and
energy density and power density are important indicators of partial redox. However, at the same time, it should be carefully
use. Based on this, VN is widely used as an excellent super- discussed whether the OH insertion and extraction process
capacitor anode material in various SC devices (Table 2). mentioned in formula (4) exists. Because of the high voltages
It is worth noting that due to the large energy density of required for the insertion and extraction of anions, this is not
capacitors composed of VN materials, they are used in many possible in aqueous environments. Therefore, we believe that
special supercapacitor devices. For example, wearable coaxial the VN material should be in the presence of hydroxyl groups
SCs, all-solid SCs, lithium ion hybrid capacitors, etc.42,58–60,70–72 adsorbed on the surface to complete the redox process, while the
cations are inserted into and escape from the lattice in this
process to achieve energy storage.
6. Energy storage mechanism
discussion 7. Cycling stability
As we mentioned earlier, the development of the energy storage Traditional VN materials have been plagued by a problem from
mechanism of VN can be expressed by formulas (1)–(4) above. the beginning, that is the problem of VN cycle stability. From
For the most widely accepted formula (1), it is shown that the Section 6, we can conclude that the energy storage mechanism
energy storage mechanism of the VN material involves the of VN materials includes two parts. First, the adsorption and
formation of an electric double layer and redox reaction with desorption of hydroxyl groups on the surface of VN and the
OH, which should be typical of Fig. 9 (type A). But in fact, in the occurrence of redox reactions should be directly related to the
Table 2 SC device performance of VN-based materials
Materials Electrolyte Potential window Energy density Power density Ref.
VN/CNT 6 M KOH (0–1) V 4.2 W h kg1 100 kW kg1 39

Co(OH)2//VN 2 M KOH (0–1.6) V 22 W h kg1 0.16 kW kg1 73
VN/CF//Ni(OH)2 6 M KOH (0–1.6) V 53–36 W h kg1 2.7–54 kW kg1 59
Ni/VN/NCs//CuCo2O4 2 M KOH (0–1.8) V 25 W h kg1 930 W kg1 68
VN//NiOx 1 M KOH (0.5–1.45) V 50 W h kg1 365 W kg1 74
PCNS@VNNP//NiO 2 M KOH (0–1.6) V 16 W h kg1 800 W kg1 45
Co3O4//CNS@VN 6 M KOH (0–1.6) V 18.8 W h kg1 800 W kg1 51
VNQD/PC//Ni(OH)2 6 M KOH (0–1.6) V 47.2 W h kg1 828.7 W kg1 48
CF@VN//AC 2 M NaNO3 (0–1.6) V 8.24 W h kg1 400 W kg1 49
VNQD/CNF//Ni(OH)2 6 M KOH (0–1.6) V 31.2 W h kg1 774.6 W kg1 26
HPCF@VNNP//Ni(OH)2 6 M KOH (0–1.6) V 39.3 W h kg1 400 W kg1 52
Ni(OH)2//VN/C 6 M KOH (0–1.6) V 43.0 W h kg1 800 W kg1 55
MnO2-CNT//VN-CNT 0.5 M Na2SO4 (0–1.8) V 38.7 W h kg1 7.3 W kg1 40
19.4 mW h cm3 3.7 mW cm3
VN/V2O3/C 1 M Na2SO4 (0–0.9) V 92 mW h m2 2.25 W m2 67
1.55 W h kg1 14 W kg1
VN thin lms 1 M KOH (0–0.6) V 2 mW h cm2 0.18 mW cm2 21
VN@C NWAs//CNT Na2SO4/PVA (0–1.8) V 96.07 mW h cm2 270 mW cm2 71
VN//NiO 1 M KOH (0.5–1.8) V 1 mW h cm2 40 mW cm2 75
NiCo2O4@Ni(OH)2/CNTF//VN NWs/CNTF KOH/PVA (0–1.6) V 103.8 mW h cm2 0.8 mW cm2 76
VN//Co(OH)2 KOH/PVA (0–1.5) V 12.4 mW h cm3 1750 mW cm3 77
VN nanobers LiCl/PVA (0–1) V 0.89 mW h cm3 0.016 W cm3 60
MVNN/CNT H3PO4/PVA (0–0.7) V 0.54 mW h cm3 0.4 W cm3 78
VN/CNTF//ZNCO/CNTF KOH/PVA (0–1.6) V 17.78 mW h cm3 80 mW cm3 42
VOx NW//VN NW LiCl/PVA (0–1.8) V 0.61 mW h cm3 0.85 W cm3 17
ZnCo2O4//VN KOH/PVA (0–1.6) V 64.76 mW h cm3 800 mW cm3 79
16 mm-thick VN MSC 1 M KOH (0–0.6) V 25 mW h cm2, 4 mW cm2 86
Fig. 9 (a, b, d, e, g, and h) Schematic cyclic voltammograms and (c, f, and i) corresponding galvanostatic discharge curves for various kinds of
energy-storage materials. A pseudocapacitive material will generally have the electrochemical characteristics of one, or a combination, of the
following categories: (b) surface redox materials (e.g., MnO2 in neutral, aqueous media), (d) intercalation-type materials (e.g., lithium insertion in
Nb2O5 in organic electrolytes), or (e) intercalation-type materials showing broad but electrochemically reversible redox peaks (e.g., Ti3C2 in
acidic aqueous electrolytes). Electrochemical responses in (g)–(i) correspond to battery-like materials. Copyright 2018 American Chemical
Society.
surface oxide layer of VN. Second, the energy storage of VN is et al.,22 pure VN is not a desirable electrode material. Although
also accompanied by intercalation capacitance, which should the inuence of the oxide on the surface of the VN material is
be directly related to the cations in the solution. Thus, the excluded, the potential window is also reduced. Then the best
factors that affect the cycling stability of VN also can be divided way is to nd a specic V surface oxide to achieve both. Fortu-
into two categories. nately, in subsequent work, the researchers found that V4+ oxide
(i) Choi et al.'s11 research found that narrowing the potential may be a very valuable VN surface oxide.23,8688 This oxide may
window can effectively improve the cycling stability of VN. This be the main source of surface pseudocapacitance on VN mate-
is caused by the fact that the V5+-containing oxides are contin- rials. At the same time, it can also improve the cycling stability
uously dissolved during the cycle, resulting in poor cycle of the material during cycling.
stability. However, according to previous work by Bondarchuk
Fig. 10 (a) CV curves of NGr, VN/NGr nanocomposites, and VN at 50 mV s1; (b) GCD curves of NGr, VN/NGr nanocomposites, and VN at 1 A g1.
Copyright 2013 The Royal Society of Chemistry.
(ii) The reduction in VN cycle stability caused by intercala- the most widely synthesis method for VN is still the high
tion capacitance is directly related to the collapse of the VN temperature reduction of NH3, which is dangerous, costly and
material structure. Work to solve this situation was actually not environmentally friendly. Although other researchers have
proposed long ago. Lu et al.17 mentioned that the VN material tried other effective cryo-security strategies, the VN yield is
can be wrapped with a gel electrolyte to prevent the degradation worrying. So, it is still important to nd a method for preparing
of the cycling stability caused by the collapse of its structure. VN with low energy consumption and high yield. (iv) Improving
Aer that, the composites of VN and carbon prepared from the electrochemical quality of devices. Although the energy
organic or polymer precursors have good cycle stability due to density of VN is high and the properties of the fabricated SC
this reason. Readers can read these articles carefully. Their devices are good, there is still a large room for improvement.
HRTEM pictures have one thing in common: aer high Besides, there is a possibility to expand the potential window of
temperature treatment, the precursor of carbon oen forms the device, for example, by using a “water-in-salt” electrolyte. (v)
a thin layer of carbon shell to wrap the VN material. In addition to VN and carbon, in fact, many transition metal
nitrides and carbides are good SC anode materials. However,
8. Conclusions compared with VN and carbon, their defects are obvious, such
as a small potential window and low specic capacitance. In
By summing up previous articles, the application scope and addition to focusing on VN materials, many of these materials
electrochemical performance of VN and its composites in can also be used as research directions.
supercapacitors are claried. These systematic studies show
that VN still has great potential as a negative electrode material Conflicts of interest
in supercapacitors. This review mentions a large number of VN
and its composite preparation methods, and these methods There are no conicts to declare.
have been developed in the direction of easy operation and cost
saving, which is more in line with the development concept of Acknowledgements
advanced society. In addition, in order to solve the poor cycle
performance of VN, researchers also provide a variety of effec- This work was partly supported by the National Natural Science
tive solutions. In addition, thanks to the advancement of Foundation of China (51203071, 51363014, 51463012, and
advanced characterization technologies and the development of 51763014), the Program for Hongliu Distinguished Young
scientic research methods, the energy storage mechanism of Scholars in the Lanzhou University of Technology, and Joint
VN materials has also become increasingly clear. fund between the Shenyang National Laboratory for Materials
Science and State Key Laboratory of Advanced Processing and
9. Challenges and prospects Recycling of Nonferrous Metals (18LHPY002).
VN is the most promising and well-studied material among References

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Anode Material of Vanadium Nitride for Supercapacitors: A Topic Review

Article in Journal of Materials Chemistry A · April 2020

Liu Lingyang Manasa Pantrangi

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Vanadium nitride for aqueous supercapacitors:

storage and transfer of energy today mainly involve fuel cells

Ying Liu is a PhD student under Qianghong Wu received her B.S.

Lingyang Liu received his B.S. Long Kang is now a professor

Dr Pantrangi Manasa received Prof. Fen Ran received his PhD

This work opens a new path for the application of VN materials

VNxOy + OH 4 VNxOy//OH + VNxOy–OH (1)

Table 1 Electrochemical characteristics of VN-based materials

Potential Stability, cycle number, test

Potential Stability, cycle number, test

nitrogen-doped graphene composites by using dicyandiamide

3.1 Shaped carbon composite VN

Table 2 SC device performance of VN-based materials

Materials Electrolyte Potential window Energy density Power density Ref.

VN/CNT 6 M KOH (0–1) V 4.2 W h kg1 100 kW kg1 39

VN is the most promising and well-studied material among References

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