MATEC Web of Conferences 382, 01015 (2023) https://doi.org/10.

1051/matecconf/202338201015
AMME 2023

Research Status and Optimization Methods of Zinc Ion Battery

Shurui Wang
College of Materials Science and Engineering, Shandong University, Jinan 250100, China

Abstract: Up against the energy shortage and aggravating environmental pollution, it is extremely urgent to
develop renewable clean energy. With efficient energy storage and energy conversion, electrochemical energy
storage is the key direction for the development of energy storage technology in the future. Besides, aqueous
zinc ion battery has attracted researchers because of its low cost and high theoretical specific capacity.
Cathode materials for aqueous zinc ion batteries are roughly divided into manganese-based compounds,
vanadium-based compounds, Prussian blue analogues, etc, which usually use zinc metal as an anode.
Electrolytes include solid hydrogel electrolytes and liquid ion electrolytes. However, some problems exist in
cathode materials, such as elements dissolution and low discharge voltage, while anode materials have
problems in zinc dendrite growth and side reactions, and water decomposition occurs in electrolytes. In recent
years, researchers have devoted themselves to optimizing aqueous zinc ion batteries in different ways, so as
to obtain their high performance. In this paper, the general situation of zinc ion battery is introduced at first,
and then the research status is emphatically expounded from the perspectives of problems existing in cathode
materials, anode materials, electrolyte, and their optimization methods, which provides references for
developing high-performance aqueous zinc ion battery.

Keywords: Zinc Ion Battery; Optimization Method; Diffusion Kinetics; Side Reaction Inhibition.

1. Introduction aqueous rechargeable batteries based on different valence

carriers have been developed, such as sodium ion batteries,
Recently, due to the continuous consumption of fossil potassium ion batteries, calcium ion batteries, zinc ion
fuels, energy shortage and the greenhouse effect have batteries, and so on [1]. Among many rechargeable
been aggravated, with the sustainable development of aqueous batteries, zinc ion battery has attracted
human society facing a severe test. On this basis, using researchers. This is because there are abundant zinc
renewable clean energy such as wind energy, solar energy, resources in nature, and zinc cathode is low in cost and
and tidal energy to gradually replace fossil energy has good in safety. More importantly, it has the advantages of
become the main energy revolution [1-4]. Therefore, low redox potential and high theoretical capacity (820
efficient energy storage and energy conversion are mAh·g-1) [10], which endows with the advantages of
imperative [5]. With high energy density, fast response, aqueous electrolyte and zinc cathode.
low cost, and convenient installation, electrochemical Cathode materials for aqueous zinc ion batteries can be
energy storage is the key direction for the development of roughly divided into manganese-based compounds,
energy storage technology in the future [4, 6]. In the vanadium-based compounds, Prussian blue analogues,
rechargeable battery system, lithium-ion batteries have and other composite materials [11]. Zinc metal is usually
achieved great success because of their high energy used as the anode, and electrolytes include solid hydrogel
density, good cycle stability, enduring cycle, and mature electrolytes and liquid ion electrolytes. Because of the
preparation technology. However, lithium resources are diverse potential electrolytes, zinc is advantageous in high
limited in nature, and high-cost flammable, and toxic redox potential, high safety, low toxicity, reversibility of
organic electrolytes are unsafe, which easily leads to zinc deposition/stripping, long cycle life, high volumetric
environmental problems, hindering the further energy density, etc., so aqueous zinc ion batteries are in
development of lithium-ion batteries [7]. Compared with the rapid development [12]. However, there are some
organic electrolytes with certain potential safety issues, problems in cathode materials, such as electrode
aqueous electrolytes are safer and more reliable [8, 9]. degradation caused by manganese dissolution, low
More importantly, the ionic conductivity of aqueous discharge voltage of vanadium-based compounds [13],
electrolytes is two magnitude orders higher than that of zinc dendrite growth, water/oxygen-related side reactions
organic electrolytes, which improves the power density [9, 14], and water decomposition in the electrolyte, etc.
and fast charging and discharging ability [5]. At present,

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AMME 2023

The further application of aqueous zinc ion batteries still [7, 18]. As a cathode material for aqueous zinc ion
needs a lot of related research and improvement. batteries, manganese-based oxides have been widely
Based on this, this paper first introduces the general studied in recent years. The common manganese-based
situation of aqueous zinc ion batteries, and then combines oxides have various crystal types (α-, β-, γ-, δ-, λ-, R-type)
the latest research, with a focus on the current progress of of MnO2, Mn2O3, and Mn3O4 [19]. The theoretical
cathode materials, anode materials, and electrolytes of capacity of MnO2 is 308 mAh/g and its voltage window is
aqueous zinc ion batteries. Finally, their future 0.8-1.8 V. The crystal structure can be divided into three
development is prospected, which provides references for types, including tunnel structure, spinel structure, and
preparing high-performance aqueous zinc ion batteries. layered structure, which have the advantages of high
natural abundance, low cost, low toxicity, high theoretical
capacity, and environmental affinity [7, 13, 19]. Mn2O3 is
2. Cathode Material superior in energy density and simple in the synthesis
Cathode materials can be roughly divided into process, while Mn3O4 has good cycling performance [20,
manganese-based compounds, vanadium-based 21]. However, when manganese-based oxides are used as
compounds, Prussian blue analogues, and other composite cathode materials for aqueous zinc ion batteries, there are
materials [11]. Manganese resources are abundant in the still some problems, such as structural deformation,
crust, and manganese-based oxides have tunnel and inevitable manganese dissolution, and low inherent
layered structures, which are beneficial to the diffusion electronic conductivity [7, 22]. Therefore, researchers in
kinetics of Zn2+ with high specific capacity. For example, recent years often use the doping of other elements,
surface coating, composite materials building, defect
MnO2 has a theoretical capacity of 616 mAh·g-1 [15].
engineering, and other different modification methods to
Vanadium-based compounds often have layered or
optimize manganese-based cathode materials, so as to
channel structures, which is beneficial to the diffusion
obtain high-performance aqueous zinc ion batteries [7].
kinetics of Zn2+ as well as the intercalation and removal
Zhang et al. [21] prepared a Ni-doped Mn2O3 (NM)
during charge and discharge. They, a kind of promising
derived from NiMn layered double hydroxide (NiMn-
zinc ion storage materials, also have the advantages of
LDH), which has a high specific capacity of 252 mAh/g,
high specific capacity (> 300 mAh·g-1), rapid reaction three times that of pure Mn2O3. When it was applied to the
kinetics, and multivalent state of vanadium [3]. As a cathode of the Zn/NM20 battery, a high energy density of
transition metal, ferricyanate, with an open structure, the 327.5 Wh/kg was achieved under the condition of 0.14
Prussian blue analogue is beneficial to the intercalation kW/kg, and the capacity retention rate was 85.6% after
and removal of Zn2+, realizing the cation storage with 2500 cycles (Figure 1a). The results show that doping Ni2+
different valences [16]. In addition, organic electrode can promote electron rearrangement, improve the
materials with low prices, less environmental pollution, conductivity and reaction kinetics of nanomaterials,
and large theoretical capacity have great advantages in the reduce the formation energy, stabilize the Mn-O bond,
storage of monovalent and divalent cations such as and improve the electrochemical performance of
quinone compounds. Some synthetic nano-materials have nanomaterials. Introducing cationic vacancies is effective
also been proven to be used as cathode materials such as to improve the low inherent conductivity of manganese-
CNF/GNP composite aerogels, etc [17]. However, there based oxide materials. These defect structures enrich the
are electrode degradation problems related to manganese active sites of ion storage, reduce the electrostatic
dissolution in manganese-based compounds, which are interaction between zinc ions and cathode materials, and
caused by Jahn-Teller structural distortion, repeated effectively promote the diffusion kinetics of ions [19]. Bo
structural phase transition, and irreversible phase formed et al. [19] optimized the traditional MnO cathode material
by repeated intercalation and deprivation of Zn2+ in by using the Al doping modified MnO. The aqueous zinc
ZnSO4 electrolyte. There are some problems in vanadium- ion battery assembled by this material has a capacity
based compounds, such as low discharge voltage, poor retention rate of 89% after 500 cycles at 0.1 A/g and 1.0
electronic conductivity, and electrode degradation [13]. A/g (Figure 1b). The results show that Al-doped
The bound water and adsorbed water in Prussian blue modification introduces a large number of Mn vacancies,
analogues are unstable during the charging and which effectively promotes the diffusion of zinc ions,
discharging, with their low theoretical specific capacity increases the specific surface area and pore size of MnO,
[2]. The above defects seriously affect the performance of and makes the cathode wetter to the electrolyte. In
aqueous zinc ion batteries. In recent years, researchers addition, Al-MnO was transformed into R-MnO2 during
have devoted themselves to preparing new cathode charge and discharge, which effectively inhibited the
materials by doping other elements or defects, surface dissolution of manganese. Constructing nanostructures
coating, or modification to improve the performance of and hybridizing with conductive materials is another
aqueous zinc ion batteries [2]. effective strategy to improve conductivity and adapt to
structural changes during cycling, among which graphene
2.1 Manganese-Based Materials has been widely used to hybridize with various electrode
Manganese is the tenth most abundant element on the materials [23]. Wang et al. [23] prepared an independent
earth, and is a common transition metal element. With mixed nanostructure composed of ultra-long manganese
many different oxidation states, it can form multivalent dioxide nanowires and graphene nanosheets, with a
manganese oxide phases with different atomic structures specific capacity of 317 mAh/g at 0.1 A/g (Figure 1c),
which can provide a high energy density of 436 Wh/kg,

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with 0.011% as the capacity attenuation rate of each cycle In addition, phosphorylation may also be a means to solve
in 2000 cycles. The research shows that the unique 1D/2D the problem of manganese-based cathode materials.
nanostructure not only promotes strong electrochemical However, manganese phosphate has electrochemical
synergy, but also withstands severe mechanical hysteresis, which makes it difficult to find intercalation
deformation such as bending and folding. Cao et al. [24] carriers for zinc ions with strong electrostatic interaction.
prepared MnO2/graphite nano-sheet hybrid by ball milling In order to solve the above problems, Li et al. [28]
method. When it was used as a cathode of the aqueous prepared carbon-coated Na3Mn2(P2O7)(PO4) (NMPP@C)
zinc ion battery, the capacity retention rate was 80.8% by liquid phase method and freeze drying technology,
after 1000 cycles at 0.1 A/g and 80 mAh/g at 1 A/g (Figure which showed a peak capacity of 150 mAh/g through
1d), which was significantly better than pure MnO2 constant current activation, with the final capacity stable
cathode material. The reasons are as follows. ① The size at 90 mAh/g and 1.45 V as the discharge platform (Figure
of MnO2 particles decreased significantly through the ball 1g). The aqueous zinc ion battery assembled by it shows
milling process, increasing specific surface area and excellent rate performance and good cycle performance.
exposing more active sites. ② The chemical bonding The results show that the structure of NMPP@C material
between MnO2 and graphite nanosheets enhances the is decomposed during constant current stimulation.
internal stability and interfacial adhesion of the material. Besides, the generated α-MnO2 and Zn2P2O•5H2O are
③ Graphite nanosheets have good mechanical properties used as electrochemical reagents, α-MnO2 as
and effectively restrain the volume change during cycling. electron/proton host, and Zn2P2O•5H2O as zinc ion host.
Wang et al. [25] prepared a new type of γ-MnO2-graphene
composite material. When it was used in a ZnMnO2
battery, the specific capacity was 301 mAh/g at 0.5 A/g
and 95.8 mAh/g at 10 A/g, which was significantly better
than the traditional MnO2 cathode (Figure 1e). The results
show that γ-MnO2 with tunnel structure is beneficial to the
intercalation/detachment process of zinc ions. Graphene
has a large surface area, good electrical conductivity, and
mechanical stability, which improves the poor electrical
conductivity and poor cycle stability of manganese-based
materials.
The construction of an electrode-electrolyte interface
(EEI) is often used to improve the stability of the electrode,
Figure. 1 (a) Cycle performance of Mn2O3, NM10,
which also plays a good role in solving the manganese
NM15, NM20, and NM30 [21]; (b) Long-term cycling
dissolution. Zuo et al. [26] synthesized a manganese
performance of pure MnO and 5% Al-MnO at current
sulfate nano-layer on MnO2 cathode in situ by
density of 1 A/g [19]; (c) Rate performance of
electrochemical treatment. After cyclic activation, the
MnO2/rGO (reduced graphene oxide) at various current
manganese sulfate nano-layer was transformed into δ-
densities [23]; (d) Rate performance of MnO2, MG5,
MnO2 nano-layer (MON) interface phase with rich
MG10, MG20 [24]; (e) Capacity and capacity retention
interlayer water, while MnO2 coated with MON was used
of MnO2 and MnO2-graphene electrodes [25]; (f)
as cathode material for an aqueous zinc ion battery. After
Cycling performance of pure MnO2 and MON-coated
1000 cycles at 10 A/g, the capacity retention rate was 85.9%
MnO2 at current density of 10 A/g [26]; (g) Charge-
(Figure 1f), which was significantly better than pure
discharge curves of NMPP@C at 0.1 C [28];
MnO2 cathode. The results show that the interlayer phase
of MOM is rich in interlayer water, which realizes the
transition from zinc ion-dominated insertion to proton-
dominated insertion, inhibits the dissolution of
manganese, and improves the electrochemical
performance. As for layered manganese-based materials,
the introduction of metal ions (Ca2+, Zn2+, Na+) and crystal
water as interlayer columns can alleviate the poor cycle
stability caused by structural deformation and manganese
dissolution [27]. Sun et al. [27] prepared
Ca0.28MnO2•0.5H2O (CaMnO) electrode material by pre-
inserting Ca2+ and water molecules into δ-MnO2 as
interlayer columns. In 1M electrolyte of ZnSO4/0.1 M
MnSO4, CaMnO had no obvious capacity attenuation
after 5000 cycles and the discharge capacity was 124
mAh/g at 3.5 A/g, showing excellent electrochemical
performance. It is proved that the doping of water and
calcium ions can essentially stabilize the structure of
layered manganese-based materials.

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Table 1 Performance of Different New Manganese- batteries [5]. However, the problems such as low average
Based Electrode Materials in Batteries working voltage and easy structure collapse of vanadium-
based compounds still need further study and solution
Manganese-Based
Electrode Material
Performance References [13]. Researchers often dope other metal ions, construct
345 mAh/g at 0.1 conductive coatings, use oxygen defect engineering, and
Al-doped MnO A/g, 89% at 1.0 A/g [19] different preparation methods to improve the performance
after 500 cycles of vanadium-based cathode materials [29]. Xu et al. [30]
The high specific prepared a cathode material with excellent performance
capacity is 252
mAh/g. When used (V2O5@PEDOT/CC) by uniformly depositing
in Zn/NM20 battery, V2O5@poly (3, 4-ethylene dioxythiophene) (PEDOT)
the energy output of hybrid nanosheet array on flexible carbon cloth (CC),
Ni-doped Mn2O3 327.5 Wh/kg is [21] which has a maximum capacity of 360 mAh/g at 0.1 A/g
achieved at 0.14
kW/kg, and the and a capacity retention rate of 97% after 600 cycles at 1
capacity retention A/g (Figure 2a). The results show that the V2O5 nanosheet
rate is 85.6% after array enriches the active sites of zinc storage. PEDOT
2500 cycles coating has good electrical conductivity and structural
The specific
capacity is 317 stability, which improves the diffusion kinetics of zinc
mAh/g at 0.1 A/g, ions and acts as a protective layer to inhibit structural
which can withstand collapse during the cycle. Su-Ho et al. [31] optimized the
severe mechanical diffusion kinetics of zinc ions in V2O5 thin films by
Independent mixed deformation of
nanostructure composed bending and folding.
controlling the number of oxygen vacancies in the
of manganese dioxide When used in zinc [23] oxidation lattice. The prepared V2O5-x thin films were
nanowires and graphene ion battery, the 57.2 mAh/g at 20C and 105.2 mAh/g at 5C (Figure 2b).
nanosheets energy density is The introduction of oxygen vacancies effectively reduced
436 Wh/kg, and the
capacity decay rate
the strong electrostatic interaction between zinc ions and
of each cycle is matrix oxide materials, improving the diffusion kinetics
0.011% in 2000 of zinc ions. Chen et al. [32] prepared hollow V2O5
cycles nanosphere cathode by template-free solvothermal
230 mAh/g at 0.1
A/g; 80 mAh/g at 1
method, which was 327 mAh/g at 0.1 A/g, 146 mAh/g at
MnO2/graphite nanosheet A/g, the capacity 20 A/g (Figure 2c), and 147 mAh/g after 6000 cycles at
[24]
hybrid retention rate is 10 A/g, with a capacity retention rate of 69.7%. The
80.8% after 1000 results show that the hollow nanostructure can effectively
cycles
301 mAh/g at 0.5
reduce the structural stress during cycling, shorten the ion
γ-MnO2-graphene transfer path, and optimize the diffusion kinetics of zinc
A/g, 95.8 mAh/g at [25]
composites
10 A/g ions. Deng et al. [33] improved the reversibility of high-
MnO2 of δ-MnO2
The capacity temperature argon-treated VO2 (AVO) materials during
retention rate was deep circulation through an in-situ self-conversion
Nanolayer Coating with [26]
85.9% after 1000
Rich Interlayer Water
cycles at 10 A/g electrochemical strategy. When the prepared AVO
In 1M electrolyte of microsphere materials were used as cathodes of aqueous
ZnSO4/0.1 M zinc ion batteries, they were 446 mAh/g at 0.1 A/g and
MnSO4, there was 323 mAh/g at 10 A/g (Figure 2d), which could be stably
no obvious capacity
Ca0.28MnO2•0.5H2O
attenuation after [27] circulated for more than 4000 times at 20 A/g, with an
（CaMnO） energy density of 308 Wh/kg. According to the research,
5000 cycles, and the
discharge capacity hydrated V2O5 (V2O5•nH2O) is formed due to the
was 124 mAh/g at insertion of water molecules and electrochemical
3.5 A/g
The peak capacity is
oxidation phase transition during the first charging
150 mAh/g, the process. As the main active substance in the subsequent
Carbon coated
Na3Mn2(P2O7)(PO4)
final capacity is 90
[28]
cycle, this substance provides abundant active sites and
mAh/g, and the can carry out highly reversible redox reactions.
（NMPP@C）
discharge platform
is 1.45 V vs
By pre-intercalation of guest metal ions (Li+, Na+, Zn2+,
K+), the interlayer spacing can be increased and the
diffusion kinetics of zinc ions can be improved to reduce
2.2 Vanadium-Based Materials charge polarization effect and optimize the structural
Vanadium-based compounds have a variety of crystal stability of vanadium-based electrode materials [34].
structures, such as layered structure, tunnel structure, Zhang et al. [34] synthesized potassium vanadium oxide
NASICON structure, etc., which are beneficial to realize (K0.23V2O5) with tunnel structure by hydrothermal method.
the rapid transfer of multiple electrons, local electrical When this material is used as cathode material, the
neutrality, and polarization alleviation caused by zinc ion capacity retention rate is 92.8% and the specific capacity
intercalation. In addition, vanadium-based compounds is 103 mAh/g after 500 cycles under the condition of 2.0
have abundant oxidized states that can be converted to A/g (Figure 2e). In addition, the ion diffusion rate is
each other, which shows a more stable structure and a 1.88*10-9 -2.6*10-8 cm2/s. The research shows that the
wider range of changes when used in aqueous zinc ion introduction of K+ increases the interlayer spacing of

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vanadium-based electrode materials, which not only

optimizes the diffusion kinetics of zinc ions, and improves
the ion diffusion rate and conductivity, but also reduces
the possibility of structural collapse.
More importantly, the researchers also found that high-
performance cathode materials for zinc ion batteries can
be obtained by combining pre-intercalation, constructing
conductive coatings, and oxygen vacancy defect
engineering [29]. Tan et al. [29] prepared a material that
is poly (3, 4-ethylene dioxythiophene) (PEDOT) coated,
manganese ion intercalated, and oxygen-enriched Figure. 2 (a) Rate performance of V2O5@PEDOT/CC,
hydrated V2O5 (MnVOH@PEDOT) by one-step V2O5/CC, and V2O5 powders at different current
hydrothermal method. When the material was used as the densities [30]; (b) Rate performance of H-V2O5-x and L-
cathode of aqueous zinc ion battery, it was 455.8 mAh/g V2O5-x at different current densities [31]; (c) Rate
at 0.2 A/g and 336.0 mAh/g at 8A/g (Figure 2f). After performance of hollow V2O5 nanospheres and
2000 cycles, the capacity retention rate was 84.8% with commercial V2O5 [32]; (d) Rate performance of AVO
good rate performance and cycle stability. The results (argon-treated VO2), VO (untreated VO2), and OVO
show that PEDOT coating has high conductivity, which (air-treated VO2) materials [33]; (e) Electrochemical
improves the conductivity of external electrons and properties of K0.23V2O5 at 2.0 A/g [34]; (f) Rate
effectively prevents vanadium oxide from dissolving. performance of MnVOH@PEDOT, MnVOH, and
Manganese ion intercalation not only enlarges the VOH@PEDOT cathodes [29]; (g) Rate performance of
interlayer spacing, improves the diffusion kinetics of zinc Fe2V4O13 cathode material at different current densities
ion, but also plays the role of “pillar” and maintains the of 0.2-10.0 A/g [35]; (h) Cycling performance of Fe2V4O13
structural stability of the cathode. In addition, the oxygen cathode material at 10 A/g [35]; (i) Cycling performance
vacancy introduced in V2O5 improves the conductivity of of hexagonal Cs0.3V2O5 cathode material at 2 A/g [36];
internal electrons. Table 2 Performance of Different New Vanadium-Based
Besides, in the research on the application of various Electrode Materials in Batteries
metal vanadates (such as potassium vanadate, sodium
vanadate, etc.) to aqueous zinc ion batteries, researchers Vanadium-Based Electrode
Performance References
found that compared with monovalent alkali metal cations Material
Material that is poly (3, 4- 455.8 mAh/g at 0.2
(such as Na+, K+, etc.), polyvalent metal ions combined ethylene dioxythiophene) A/g, 336.0 mAh/g at
with oxygen atoms can produce different ionic bonds and (PEDOT) coated, manganese 8A/g, and 84.8% [29]
layer sizes with better crystal structure [35]. Yang et al. ion intercalated, oxygen- capacity retention
enriched hydrated V2O5 after 2000 cycles
[35] synthesized Fe2V4O13 by simple solution chemical 360 mAh/g at 0.1
reaction. Through in-situ and non-in-situ characterization A/g, 232 mAh/g at
under different states of charge and discharge, it shows 20 A/g, retention of
V2O5@PEDOT/CC 97% after 600 [30]
that the structure of the material is highly reversible, cycles at 1 A/g, and
which is 380 mAh/g at 0.2 A/g (Figure 2g) and 83% 89% after 1000
capacity retention after 1000 cycles at 10 A/g (Figure 2h). cycles at 5 A/g
57.2 mAh/g at 20 C
The reversible phase transition from ferric vanadate to V2O5-x thin film material and 105.2 mAh/g at [31]
zinc vanadate and the intercalation/de-intercalation 5C
mechanism of zinc ion storage in tunnel structure were 327 mAh/g at 0.1
A/g, 146 mAh/g at
observed simultaneously, which provided a new direction 20 A/g, 147 mAh/g
for the design and research of zinc ion batteries. Under Hollow V2O5 nanospheres [32]
after 6000 cycles at
certain synthesis conditions, nanomaterials with 10 A/g, and 69.7%
retention
unconventional phases can be prepared by adjusting the 446 mAh/g at 0.1
reaction kinetics, realizing the process from structural A/g, 323 mAh/g at
modulation of cathode materials to property improvement 10 A/g, and more
AVO microsphere material than 4000 cycles at [33]
[36]. Qu et al. [36] prepared a hexagonal Cs0.3V2O5 20 A/g, with an
cathode material with a specific capacity of 543.8 mAh/g energy density of
at 0.1 A/g and a capacity retention rate of 87.8% after 308 Wh/kg
1000 cycles at 2 A/g (Figure 2i). The results show that The capacity
retention rate was
compared with orthogonal V2O5, the hexagonal K0.23V2O5 92.8% of 2.0 A/g, [34]
framework structure with Cs has strong stability and good 103 mAh/g after
electrical conductivity, and the open framework structure 500 cycles
380 mAh/g at 0.2
optimizes the diffusion kinetics of zinc ions. A/g and 83%
Fe2V4O13 capacity retention [35]
rate after 1000
cycles at 10 A/g
543.8 mAh/g at 0.1
A/g, retention rate
Hexagonal Cs0.3V2O5 [36]
was 87.8% after
1000 cycles at 2 A/g

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2.3 Prussian Blue Analogues 3. Anode Material

Hexaminometalate, commonly known as Prussian blue
analogues (PBAs), is a material with an open frame and Zinc is the most commonly used anode material in
face-centered cubic lattice structure, which is high in solid aqueous zinc ion batteries due to its abundant zinc
diffusion coefficient (10-9—10-8 cm2/s) and ionic resources, good chemical stability, low redox potential,
conductivity [16]. PBAs are considered a promising and easy processing [22]. However, dendrite growth and
cathode material for aqueous zinc ion batteries because of water/oxygen side reactions are two key problems
their good rate performance, reversible insertion of affecting the cycle performance of the zinc anode. The
various metal ions, good ionic conductivity, high safety, electrode position process of zinc tends to form irregular
non-toxicity, and low cost [1, 16, 37]. Liu et al. [37] zinc dendrites. When zinc dendrites grow on a large scale,
constructed a zinc ion secondary battery with a metal zinc it is easy to penetrate the separator and cause a serious
anode, biological ionic liquid-water electrolyte, and nano- battery short circuit [9]. Secondly, the side reaction
structured Prussian blue analogue cathode. At 10 mA/g, seriously harms the cycle performance of the aqueous zinc
the discharge voltage platform of the battery was ~ 1.1 V, ion battery [14]. In order to solve the above problems,
and the specific capacity was 120 mAh/g. The results researchers have adopted surface modification, structural
show that the open framed PBAs cathode has large design of a new zinc anode, and electrolyte optimization
channels, which optimizes the reversible to improve the performance of the zinc anode [41].
insertion/removal of zinc ions, and the zinc anode has
good compatibility with biological ionic liquid-water 3.1 Surface Modification
electrolyte. However, PBAs have the problems of Constructing an artificial protective layer on the zinc
structural destruction and insufficient active sites during anode is a promising method to effectively inhibit
ion insertion/removal, which leads to low theoretical dendrite growth of the zinc anode, which mainly includes
specific capacity and poor cycle stability [38]. On this two strategies including physical shielding and inducing
basis, Zeng et al. [38] prepared a cathode material of PBA uniform diffusion of ions. For example, nano-CaCO3
hollow sphere zinc ion battery that is cobalt-replaced and coating and ZnF2 coating can promote the redistribution
manganese-rich (CoMn-PBA HSs) by template ion of zinc ions and inhibit dendrite growth, and carbon
exchange method. The specific capacity is 128.6 mAh/g nanotube-modified coating can construct a uniform
at 0.05 A/g and 50.4 mAh/g at 2 A/g. After 1000 cycles, electric field and induce uniform deposition of zinc [42,
the capacity retention rate is 76.4% with high reversible 43]. A direct method of physical shielding is to construct
capacity, good rate performance, and cycle stability. The an artificial interface layer to inhibit the growth of zinc
results show that the manganese-rich hollow structure dendrites, which requires the artificial interface layer to
enriches the active sites, provides a large surface area, have good mechanical properties. Another method is to
optimizes the diffusion kinetics of zinc ions, and adapts to induce uniform migration of zinc ions by ion tunneling
the large volume change during repeated charge and confinement, chemisorption, and electrostatic interaction
discharge, inhibiting the structure collapse. Cobalt [43]. Lu et al. [42] constructed a layered double oxide
substitution further stabilizes the crystal structure and (LDO) artificial interface protection coating to solve the
improves the cycle stability and cycle life. above problems. The coulomb efficiency of the coating is
99.7% after 2800 cycles. Zn@LDO symmetric battery can
2.4 Other Cathode Materials stably cycle more than 6600 times under the condition of
Organic compounds and other new materials are also 5 mA/cm2 (Figure 3a) and more than 5000 times under
often used as cathodes for aqueous zinc ion batteries. Liu the condition of 10 mA/cm2 (Figure 3b). After 1600
et al. [39] prepared a new type of metal-organic cycles at 1A/g, the capacity retention rate of Zn@LDO/α-
framework (MOF) cathode by solvothermal method. MnO2 was 86%. The results show that LDO immobilizes
When the current density is 50 mA/g, the initial specific anions in ZnSO4 electrolytes by electrostatic attraction,
capacity is 90.7 mAh/g, which can be stably cycled more which reduces the concentration gradient of zinc ions and
than 200 times at the current density of 1 A/g with high inhibits the growth of dendrites. In addition, zinc ions are
specific capacity and good cycle stability. In addition, the adsorbed by interlayer anions, which inhibits the two-
material can maintain high stability in the range of pH 0- dimensional diffusion and aggregation on the anode
12 for 30 days, which is beneficial to good recyclable zinc surface, resulting in dendrite growth.
ion batteries. Cerium oxide has attracted researchers However, the side reaction caused by the direct contact
because of its unique crystal structure, bonds, properties, between the electrolyte and anode is another problem that
and changeable oxidation state. Zhang et al. [40] prepared limits the electrochemical performance of zinc ion
a spindle-shaped cerium oxide (CeO2) particle by batteries, and unilateral inhibition of zinc dendrite growth
hydrothermal method and used it as cathode material of and side reaction cannot completely solve the above
aqueous zinc ion batteries. The average specific discharge problems [44]. This is because dendrite growth and side
capacity of 500 cycles at the current density of 120 mA/g reactions promote each other, and dendrite formation
was 95.7 mAh/g, and the average discharge capacity of increases the specific surface area of the anode, which
100 cycles at the current density of 60 mA/g was 158.8 intensifies the contact area between the anode and
mAh/g. electrolyte, significantly accelerating the rate of hydrogen
evolution reaction (HER). Besides, HER aggravates
electrochemical corrosion. By-products of

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electrochemical corrosion will be unevenly deposited on inhibits the side reaction. Meanwhile, the gradient
the anode surface to promote dendrite growth [45]. conductivity changes the electric field distribution at the
Therefore, synergistic inhibition of dendrite growth and bottom of the microchannel, the ion flux of zinc ions, and
side reactions is very important. Liu et al. [44] constructed the local current density, thus realizing the controllable
a hybrid surface modification coating on a zinc anode that uniform deposition of zinc ions and preventing the short
is hydrophobic organic polyvinylidene fluoride (PVDF)- circuit caused by the uneven growth of dendrites at the top.
inorganic mesoporous silicon material (SBA15). When The 3D printing technology is applied to the manufacture
the coating is used in a zinc anode symmetric battery, it of a new three-dimensional structure of zinc anode, which
can stabilize the cycle for more than 1650h at 3 mA/cm2; improves the reversibility of zinc anode and zinc
When the coating is applied to Zn||V2O5 battery (PVDF- utilization rate [48]. Wu et al. [48] printed graphene array
SBA15@Zn||V2O5), the capacity retention rate is 82.14% brackets (3DGs) with tubular structure (3DGT) and
after 1000 cycles, which is significantly better than 23.55% columnar structure (3DGP) current collectors in 3D
of traditional Zn||V2O5 battery (Figure 3c) and effectively through digital light processing technology. Under the
inhibits zinc dendrite growth and side reactions. The condition of 2 mA/cm2 (1 mAh/cm2), the cycle time of
results show that the uniformly distributed porous 3DGT@Zn exceeds 1100h, the cycle time of 3DGP@Zn
structure of SBA15 provides a uniform diffusion path for exceeds 900h, and the zinc utilization rate is 5%, which is
the diffusion of zinc ions and induces the uniform significantly better than that of traditional zinc symmetric
deposition and distribution of zinc ions on the zinc anode. battery (Figure 4d and Figure 4e). More importantly,
Meanwhile, hydrophobic PVDF effectively inhibits the when 3DGs@Zn anode is used in a soft-pack battery with
side reaction between free water molecules and zinc V2O5 cathode material, the capacity is 2.26 mAh/cm2
anode (Figure 3d). under the conditions of N/P (1.74:1) and high zinc
utilization rate (47.12%), which is significantly better
than that of zinc foil//V2O5 soft-pack battery. The research
shows that the tubular columnar structure of 3D printing
is highly ordered, which can alleviate the significant
volume change during reversible deposition/dissolution
of zinc, induce uniform deposition of Zn, and effectively
improve the utilization rate of zinc.
Figure. 3 (a) Long-term constant current cycle
performance of Zn//Zn and Zn@LDO//Zn@LDO
symmetric batteries at 5 mA/cm2 [42]; (b) Long-term
constant current cycle performance of Zn//Zn and
Zn@LDO//Zn@LDO symmetric cells at 10 mA/cm2
[42]; (c) Long-term cycle stability of Zn||V2O5 and
PVDF-SBA15@Zn||V2O5 batteries at 1 A/g [44]; (d)
Hydrogen evolution volumes of a bare zinc anode and
PVDF-SBA15@Zn anode in different cycles [44];

3.2 Structure Design of New Zinc Anode

The structure design of a new zinc anode is another
effective method to restrain the dendrite growth and side Figure. 4 (a) Working voltage image of zinc symmetric
reaction of zinc. Constructing a three-dimensional zinc battery with a current density of 1 mA/cm2 and capacity
anode is promising to stabilize zinc anode. The three- of 1 mAh/cm2 [47]; (b) Working voltage image of zinc
dimensional structure increases reaction sites and the symmetric cells at 10 mA/cm2 and 10 mAh/cm2 [47]; (c)
specific surface area of reaction sites while reducing the Corrosion curves of different electrodes [47]; (d) Cycle
local electric field intensity during Zn deposition [46]. On performance of 3DGT@Zn///V2O5, 3DGP @ Zn///V2O5,
this premise, it is a promising method to design a three- and Zn///V2O5 batteries at 4 A/g [48]; (e) Cycle
dimensional zinc anode with a gradient structure. The performance of 3DGT @ Zn///V2O5, 3DGP @
three-dimensional zinc anode with a gradient structure Zn///V2O5, and Zn///V2O5 soft-pack batteries at 4
also improves the local charge transport dynamics and mA/cm2 [48];
optimizes the Zn deposition process, effectively inducing
the uniform deposition of Zn [47]. Cao et al. [47] reported
an imprinted gradient zinc anode (polyvinylidene-Sn@Zn, 3.3 Electrolyte Optimization
PVDF-Sn@Zn), which is a double gradient structure that Using electrolytic additives, such as Mxene, surfactants,
circulates stably for 1200h at 1 mA/cm2 and 1 mAh/cm2 small organic molecules, etc., is a simple method to
(Figure 4a) and for 200h at 10 mA/cm2 and 10 mAh/cm2 effectively stabilize the solid electrolyte interface (SEI)
(Figure 4b), effectively inhibiting zinc dendrite growth film and inhibit the formation of zinc dendrites, which can
and side reactions (Figure 4c). The results show that the achieve a longer cycle life of zinc anode [49]. Wu et al.
hydrophobic PVDF layer can effectively prevent the [49] used 2-methylimidazole (Hmim) as an electrolyte
corrosion of Zn by electrolyte, and the hydrophilic additive to construct a strong inorganic/organic zinc-rich
conductive layer of Sn has a high redox potential, which (Zn4SO4 (OH)6/Zn(Hmim)) solid electrolyte interface film

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in situ, thus realizing a highly stable dendrite-free zinc Table 3 Effect of Different New Zinc Anode on Zinc Ion
cathode. The coulomb efficiency of this dendrite-free zinc Battery
cathode reaches 97.32% (Figure 5a), which can be stably
Anode material Performance References
circulated for more than 2000h. When the electrolyte
Zn@LDO symmetric
additive is used in Zn||V2O5 battery, it shows good cycle battery can stably cycle
performance (Figure 5b). The results show that the zinc more than 6600 times at
affinity of Hmim and its chelation with zinc ions together 5mA/cm2 and more than
Zinc anode coated
lead to the increase of initial nucleation sites and induce 5000 times at 10
with layered double [42]
mA/cm2. After 1600
the homogeneous deposition of zinc. In addition, the oxide (LDO)
cycles at 1A/g of
change in the coordination environment reduces the ion Zn@LDO/α-MnO2, the
diffusion coefficient and increases the nucleation capacity retention rate
overpotential, which makes the grain size smaller at the was 86%
PVDF-
initial stage of zinc deposition. The organic/inorganic Zinc anode with
SBA@Zn||PVDF-
solid electrolyte interfacial film formed by in-situ hydrophobic organic
SBA@Zn battery can
polyvinylidene
construction has good chemical stability and thermal fluoride (PVDF)-
cycle stably for more
stability, which inhibits side reactions and dendrite than 1650h at 3
inorganic mesoporous [44]
mA/cm2. The capacity
growth. A variety of organic electrolyte additives, such as silicon material
retention rate of PVDF-
acetonitrile, dimethyl carbonate, silk peptide, saccharin, (SBA15) hybrid
SBA15@ Zn||V2O5
surface modification
etc., have been developed as a method to inhibit the coating
battery after 1000 cycles
growth of zinc dendrites [50, 51] since organic was 82.14%
It was stable for 1200h
molecule/polymer electrolyte additives can regulate the at 1 mA/cm2, 1
electrochemical behavior of the interface. Wang et al. [50] Polyvinylidene-
mAh/cm2, and for 200h [47]
Sn@Zn
prepared a new colloidal electrolyte by dispersing oleic at 10 mA/cm2, 10
acid (OA) into a 2M ZnSO4 solution. This colloidal mAh/cm2
At 2 mA/cm2 (1
electrolyte realizes highly reversible zinc deposition with mAh/cm2), the cycle
a coulomb efficiency of 99.63% (Figure 5c). When the time of 3DGT@Zn is
electrolyte is used in the ZnMnO2 battery, it can be stably 3DGs@Zn
over 1100h, and the
[48]
cycled more than 1000 times at 1 A/g (Figure 5d). The cycle time of
3DGP@Zn is over
results show that oleic acid additive combines with zinc 900h, and the utilization
metal to form an oleic acid adsorption layer on the anode rate of zinc is 5%
surface. This adsorption layer can homogenize zinc Zn (2-
The coulomb efficiency
deposition, form a flat zinc metal anode, and separate the reached 97.32%, and the
methylimidazole [49]
cycle was stable for
zinc metal negative electrode from the electrolyte, thus electrolyte additive)
more than 2000h
effectively inhibiting side reactions. Xu et al. [51] adopted The coulomb efficiency
a bifunctional zinc gluconate electrolyte as a new zinc salt Zn (new ZnSO4-OA reaches 99.63%, and the
[50]
for zinc ion batteries. Experiments show that only 0.3 M colloidal electrolyte) cycle life exceeds 3340
zinc gluconate (Figure 5e) is needed to integrate the cation times
After 125 cycles, the
source and anion interface, which obtains an efficient Zn (zinc gluconate
coulomb efficiency is [51]
dendrite-free zinc anode interface without other electrolyte)
85%
electrolytes. According to the results, zinc gluconate can
carry out a stable electrochemical process of zinc
plating/stripping and provide zinc gluconate anions to 4. Electrolyte
build an artificially stable dendritic-free anion interface to
The electrolyte is another important factor that determines
realize dendritic-free zinc deposition.
the performance of aqueous zinc ion batteries. Suitable
electrolytes can keep good reversibility of zinc
deposition/stripping and release a wide electrochemical
window. ZnSO4 and Zn （ CF3SO3 ） 2 are the most
common base electrolytes in aqueous zinc ion batteries [52].
ZnSO4 electrolyte has a wide electrochemical window
(0.2 ~ 2V wide voltage window) and good anode stability.
Compared with ZnSO4 electrolyte, Zn（CF3SO3）2 has a
wider electrochemical window (wide operating voltage ~
Figure. 5 (a) Coulomb efficiency of zinc 2.0 V), better reversibility, and faster zinc
plating/stripping at 1 mA/cm2 (capacity 1 mAh/cm2) deposition/dissolution kinetics [52, 53]. Common
[49]; (b) Cycle performance of Zn||V2O5 battery with and aqueous zinc ion electrolytes include solid hydrogel
without Hmim [49]; (c) Coulomb efficiency of Zn||Cu electrolytes and liquid ionic liquid. Among them,
battery in different electrolytes at 1 mA/cm2 and 0.5 hydrogel electrolyte shows good flexibility, mechanical
mAh/cm2 [50]; (d) Cycle performance of Zn||MnO2 durability, temperature adaptability, and electrochemical
battery at 1 A/g [50]; (e) MD-simulated three- stability [54]. However, electrolyte also faces severe
dimensional images of zinc gluconate system at 0.3 M challenges such as water decomposition reaction [55]. At
[51]; present, researchers often add additives to electrolytes to

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improve their performance of electrolytes, which can also

inhibit the dendrite growth of zinc anode and improve the
reversibility and stability of the anode, preventing the
dissolution of cathode materials [53, 56, 57]. Zhang et al.
[58] used the MgSO4 electrolyte as an additive in the
ZnSO4 electrolyte, and prepared MgxV2O5•nH2O
（ MgVO）nanoribbon material as the cathode of the
battery. The results show that when the ratio of electrolyte
to additive concentration is 1: 1 (1.0 M ZnSO4–1.0 M
MgSO4), the MgVO cathode has a specific capacity of Figure. 6 (a) Rate performance of MgVO cathode in five
374 mAh/g at 100 mA/g (Figure 6a), a capacity retention electrolytes with different concentration ratios [58]; (b)
rate of 90.3% after 200 cycles at 1 A/g (Figure 6b), and a Cycling performance of MgVO cathode in electrolytes
reversible capacity of 175 mAh/g at 5 A/g. Zhao et al. [59] with different concentration ratios at 1 A/g [58]; (c)
used a small amount of perfluorooctanoic acid (PFOA) as Coulomb efficiency of Zn||Cu battery in different
an additive, and the coulomb efficiency of the Zn||Cu electrolytes [59]; (d) Rate performance of
battery using this additive was improved (Figure 6c). The Zn||Na0.65Mn2O4 battery in different electrolytes [59]; (e)
zinc symmetric battery using this additive achieved Ionic conductivity of PDMAAm/Zn(CF3SO3)2 ionic gel
reversible deposition for up to 2200h, and the in multiple rupture/healing cycles [60]; (f) Long-term
Zn||Na0.65Mn2O4 battery using this additive reached 153 cycle performance and coulomb efficiency of
mAh/g at 5 A/g (Figure 6d). The results show that the PDMAAm/Zn(CF3SO3)2 ion gel based zinc ion battery at
PFOA additive forms an adsorption layer at the interface 3.0 A/g [60];
between electrolyte and electrode, which redistributes the
flux of zinc ions at the interface, inhibits the tendency of 5. Results and Prospects
anions migrating to the negative electrode, and makes the
zinc plating/stripping process of aqueous zinc ion battery In this paper, the research progress of aqueous zinc ion
more stable. The long perfluorocarbon chain in the PFOA batteries is reviewed, which is embodied in cathode
additive has hydrophobic properties, which effectively materials, anode materials, and electrolytes. As for
inhibits the side reactions related to water and expands the cathode materials, we found that there are some problems
working window of the electrolyte to 2.1 V. in manganese-based cathode materials, such as structural
In addition, in recent years, the research on flexible deformation, manganese dissolution, and low inherent
wearable devices puts forward new requirements for the electronic conductivity. Adopting doping elements,
development of non-traditional flexible batteries with surface coating, constructing high-conductive composites,
light, thin, and integrated configuration [8]. Hydrogel defect engineering, and other methods can effectively
electrolyte not only has mechanical properties such as inhibit manganese dissolution, alleviate volume change,
flexibility and foldability of solid electrolyte, but also has and improve conductivity. The problems of vanadium-
diffusion characteristics and high conductivity of water- based cathode materials such as low average working
electrolyte [55], which is imperative for the development voltage and easy collapse of structure can be solved by
of flexible wearable aqueous zinc ion battery [60]. In doping, surface coating, and defect engineering. In
addition, Li et al. [60] designed and synthesized poly (N, addition, it is found that Prussian blue analogues and other
N’-dimethylacrylamide)/zinc trifluoromethane sulfonate cathode materials still need further research and
(PDMAAm/Zn (CF3SO3)2) ionic gel with high operating development. As for anode materials, in order to solve the
voltage window in ionic liquid solvent 1-butyl-3- dendrite growth and water/oxygen-related side reactions,
methylimidazole trifluoromethane sulfonic acid. The we found that surface modification, structure optimization,
ionic gel exhibited good mechanical strength and ionic and electrolyte optimization are more effective. As for the
conductivity with a drawing strain rate of 893.7%, a electrolyte, we found that the electrochemical
drawing strength of 151.0 kPa, and an ionic conductivity performance of the electrolyte was effectively improved
of 0.96 mS/cm (Figure 6e). After 5 rupture/healing cycles, by adding additives. To sum up, this paper provides
the healing rate reached 87.2%, which showed excellent references for improving the research and development of
flexibility and cycle stability after healing under 808 nm cathode materials, anode materials, and electrolytes of
near-infrared light irradiation. In addition, the battery has aqueous zinc ion batteries, and in the meantime, looks
a high discharge voltage of 2.5 V and can stably cycle forward to the future development of aqueous zinc ion
more than 1500 times at 3.0 A/g, which shows good batteries.
electrochemical performance (Figure 6f).

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