Carbon-based interface engineering and architecture design for high-performance lithium metal anodes

Metallic lithium(Li)is considered the“Holy Grail”anode material for the nextgeneration of Li batteries with high energy density owing to the extraordinary theoretical specific capacity and the lowest negative electrochemical potential.However,owing to inhomogeneous Li-ion flux,Li anodes undergo uncontrollable Li deposition,leading to limited power output and practical applications.Carbon materials and their composites with controllable structures and properties have received extensive attention to guide the homogeneous growth of Li to achieve high-performance Li anodes.In this review,the correlation between the behavior of Li anode and the properties of carbon materials is proposed.Subsequently,we review emerging strategies for rationally designing high-performance Li anodes with carbon materials,including interface engineering(stabilizing solid electrolyte interphase layer and other functionalized interfacial layer)and architecture design of host carbon(constructing three-dimension structure,preparing hollow structure,introducing lithiophilic sites,optimizing geometric effects,and compositing with Li).Based on the insights,some prospects on critical challenges and possible future research directions in this field are concluded.It is anticipated that further innovative works on the fundamental chemistry and theoretical research of Li anodes are needed.

A layered multifunctional framework based on polyacrylonitrile and MOF derivatives for stable lithium metal anode

Composite Li metal anodes based on three-dimensional(3D) porous frameworks have been considered as an effective material for achieving stable Li metal batteries with high energy density.However,uneven Li deposition behavior still occurs at the top of 3D frameworks owing to the local accumulation of Li ions.To promote uniform Li deposition without top dendrite growth,herein,a layered multifunctional framework based on oxidation-treated polyacrylonitrile(OPAN) and metal-organic framework(MOF) derivatives was proposed for rationally regulating the distribution of Li ions flux,nucleation sites,and electrical conductivity.Profiting from these merits,the OPAN/carbon nano fiber-MOF(CMOF) composite framework demonstrated a reversible Li plating/stripping behavior for 500 cycles with a stable Coulombic efficiency of around 99.0% at the current density of 2 mA/cm~2.Besides,such a Li composite anode exhibited a superior cycle lifespan of over 1300 h under a low polarized voltage of 18 mV in symmetrical cells.When the Li composite anode was paired with LiFePO_(4)(LFP) cathode,the obtained full cell exhibited a stable cycling over 500 cycles.Moreover,the COMSOL Multiphysics simulation was conducted to reveal the effects on homogeneous Li ions distribution derived from the above-mentioned OPAN/CMOF framework and electrical insulation/conduction design.These electrochemical and simulated results shed light on the difficulties of designing stable and safe Li metal anode via optimizing the 3D frameworks.

Surface Patterning of Metal Zinc Electrode with an In‑Region Zincophilic Interface for High‑Rate and Long‑Cycle‑Life Zinc Metal Anode

The undesirable dendrite growth induced by non-planar zinc(Zn)deposition and low Coulombic efficiency resulting from severe side reactions have been long-standing challenges for metallic Zn anodes and substantially impede the practical application of rechargeable aqueous Zn metal batteries(ZMBs).Herein,we present a strategy for achieving a high-rate and long-cycle-life Zn metal anode by patterning Zn foil surfaces and endowing a Zn-Indium(Zn-In)interface in the microchannels.The accumulation of electrons in the microchannel and the zincophilicity of the Zn-In interface promote preferential heteroepitaxial Zn deposition in the microchannel region and enhance the tolerance of the electrode at high current densities.Meanwhile,electron aggregation accelerates the dissolution of non-(002)plane Zn atoms on the array surface,thereby directing the subsequent homoepitaxial Zn deposition on the array surface.Consequently,the planar dendrite-free Zn deposition and long-term cycling stability are achieved(5,050 h at 10.0 mA cm^(−2) and 27,000 cycles at 20.0 mA cm^(−2)).Furthermore,a Zn/I_(2) full cell assembled by pairing with such an anode can maintain good stability for 3,500 cycles at 5.0 C,demonstrating the application potential of the as-prepared ZnIn anode for high-performance aqueous ZMBs.

Hard-carbon hybrid Li-ion/metal anode enabled by preferred mesoporous uniform lithium growth mechanism

To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.

3D Artificial Array Interface Engineering Enabling Dendrite-Free Stable Zn Metal Anode

The ripple effect induced by uncontrollable Zn deposition is considered as the Achilles heel for developing high-performance aqueous Zn-ion batteries.For this problem,this work reports a design concept of 3D artificial array interface engineering to achieve volume stress elimination,preferred orientation growth and dendrite-free stable Zn metal anode.The mechanism of MXene array interface on modulating the growth kinetics and deposition behavior of Zn atoms were firstly disclosed on the multi-scale level,including the in-situ optical microscopy and transient simulation at the mesoscopic scale,in-situ Raman spectroscopy and in-situ X-ray diffraction at the microscopic scale,as well as density functional theory calculation at the atomic scale.As indicated by the electrochemical performance tests,such engineered electrode exhibits the comprehensive enhancements not only in the resistance of corrosion and hydrogen evolution,but also the rate capability and cyclic stability.High-rate performance(20 mA cm^(-2))and durable cycle lifespan(1350 h at 0.5 mA cm^(-2),1500 h at 1 mA cm^(-2)and 800 h at 5 mA cm^(-2))can be realized.Moreover,the improvement of rate capability(214.1 mAh g^(-1)obtained at 10 A g^(-1))and cyclic stability also can be demonstrated in the case of 3D MXene array@Zn/VO2battery.Beyond the previous 2D closed interface engineering,this research offers a unique 3D open array interface engineering to stabilize Zn metal anode,the controllable Zn deposition mechanism revealed is also expected to deepen the fundamental of rechargeable batteries including but not limited to aqueous Zn metal batteries.

Recent advanced development of stabilizing sodium metal anodes

As the application of next-generation energy storage systems continues to expand,rechargeable secondary batteries with enhanced energy density and safety are imperative for energy iteration.Sodium-ion batteries(SIBs)have attracted extensive attention and are recognized as ideal candidates for large-scale energy storage due to the abundant sodium resources and low cost.Sodium metal anodes(SMAs)have been considered as one of the most attractive anode materials for SIBs owing to their high specific capacity(1166 mAh g^(-1)),low redox potential,and abundant natural resources.However,the uncontrollable dendrite growth and inevitable side reactions on SMA lead to the continuous deterioration of the electrochemical performance,causing serious safety concerns and limiting their practical application in the future.Therefore,the construction of stable dendrite-free SMAs is a pressing problem for advanced sodium metal batteries(SMBs).In this review,we comprehensively summarize the research progress in suppressing the formation of sodium dendrite,including artificial solid electrolyte interphase(SEI),liquid electrolyte modification,three-dimensional(3D)host materials,and solid-state electrolyte.Additionally,key aspects and prospects of future research directions for SMAs are highlighted.We hope that this timely review can provide an overall picture of sodium protection strategies and stimulate more research in the future.

Lithiophilicity: The key to efficient lithium metal anodes for lithium batteries

Lithium metal anode of lithium batteries,including lithium-ion batteries,has been considered the anode for next-generation batteries with desired high energy densities due to its high theoretical specific capacity(3860 mA h g^(-1))and low standards electrode potential(-3.04 V vs.SHE).However,the highly reactive nature of metallic lithium and its direct contact with the electrolyte could lead to severe chemical reactions,leading to the continuous consumption of the electrolyte and a reduction in the cycle life and Coulombic efficiency.In addition,the solid electrolyte interface formed during battery cycling is mainly inorganic,which is too fragile to withstand the extreme volume change during the plating and stripping of lithium.The uneven flux of lithium ions could lead to excessive lithium deposition at local points,resulting in needle-like lithium dendrites,which could pierce the separator and cause short circuits,battery failure,and safety issues.In the last five years,tremendous efforts have been dedicated to addressing these issues,and the most successful improvements have been related to lithiophilicity optimizations.Thus,this paper comprehensively reviewed the lithiophilicity regulation in lithium metal anode modifications and highlighted the vital effect of lithiophilicity.The remaining challenges faced by the lithiophilicity optimization for lithium metal anodes are discussed with the proposed research directions for overcoming the technical challenges in this subject.

Review on lithium metal anodes towards high energy density batteries

Lithium metal anode(LMA) is a promising candidate for achieving next-generation high-energy-density batteries due to its ultrahigh theoretical capacity and most negative electrochemical potential. However, the practical application of lithium metal battery(LMB) is largely retarded by the instable interfaces, uncontrolled dendrites, and rapid capacity deterioration. Herein, we present a comprehensive overview towards the working principles and inherent challenges of LMAs. Firstly, we diligently summarize the intrinsic mechanism of Li stripping and plating process. The recent advances in atomic and mesoscale simulations which are crucial in guiding mechanism study and material design are also summarized. Furthermore, the advanced engineering strategies which have been proved effective in protecting LMAs are systematically reviewed, including electrolyte optimization, artificial interface, composite/alloy anodes and so on. Finally, we highlight the current limitations and promising research directions of LMAs. This review sheds new lights on deeply understanding the intrinsic mechanism of LMAs, and calls for more endeavors to realize practical Li metal batteries.

Elucidating the suppression of lithium dendrite growth with a void-reduced anti-perovskite solid-state electrolyte pellet for stable lithium metal anodes

Solid-state lithium-metal batteries,with their high theoretical energy density and safety,are highly promising as a next-generation battery contender.Among the alternatives proposed as solid-state electrolyte,lithium-rich anti-perovskite(Li RAP)materials have drawn the most interest because of high theoretical Li^(+)conductivity,low cost and easy processing.Although solid-state electrolytes are believed to have the potential to physically inhibit the lithium dendrite growth,lithium-metal batteries still suffer from the lithium dendrite growth and thereafter the short circuiting.The voids in practical Li RAP pellets are considered as the root cause.Herein,we show that reducing the voids can effectively suppress the lithium dendrite growth.The voids in the pellet resulted in an irregular Li^(+)flux distribution and a poor interfacial contact with lithium metal anode;and hence the ununiform lithium dendrites.Consequently,the lithium-metal symmetric cell with void-reduced Li_(2)OHCl-HT pellet was able to display excellent cycling performance(750 h at 0.4 m A cm^(-2))and stability at high current density(0.8 m A cm^(-2)for 120 h).This study provides not only experimental evidence for the impact of the voids in Li RAP pellets on the lithium dendrite growth,but also a rational pellet fabrication approach to suppress the lithium dendrite growth.

Full-chain enhanced ion transport toward stable lithium metal anodes

The dendrite growth that results from the slow electrode process kinetics prevents the lithium(Li) metal anode from being used in practical applications. Here, full-chain enhanced ion transport for stabilizing Li metal anodes is proposed. Experimental and theoretical studies confirm that full-chain enhanced ion transport(electrocrystallization, mass transport in the electrolyte and diffusion in solid electrolyte interphase) under magnetoelectrochemistry contributes to a homogeneous, dense, and dendrite-free morphology. Specifically, the enhanced electrocrystallization behavior promotes the Li nucleation;the enhanced mass transport in the electrolyte alleviates the ion concentration gradient at the electrode surface, which helps to inhibit dendrite growth;and the enhanced diffusion in the solid electrolyte interphase further homogenizes the Li deposition behavior, obtaining regular and uniform Li particles.Consequently, the Li metal anode has exceptional cycling stability in both symmetric and full cells,and the pouch cell performs long cycles(170 cycles) in practice evaluation. This work advances fundamental knowledge of the magneto-dendrite effect and offers a new perspective on stabilizing metal anodes.

Uniform nanoplating of metallic magnesium film on titanium dioxide nanotubes as a skeleton for reversible Na metal anode

To meet the low-cost concept advocated by the sodium metal anode,this paper reports the use of a pulsed electrodeposition technology with ionic liquids as electrolytes to achieve uniform nanoplating of metallic magnesium films at around 20 nm on spaced titanium dioxide(TiO_(2))nanotubes(STNA-Mg).First,the sodiophilic magnesium metal coating can effectively reduce the nucleation overpotential of sodium metal.Moreover,three-dimensional STNA can limit the volume expansion during sodium metal plating and stripping to achieve the ultrastable deposition and stripping of sodium metals with a high Coulombic efficiency of up to 99.5%and a small voltage polarization of 5 mV in symmetric Na||Na batteries.In addition,the comparative study of sodium metal deposition behavior of STNA-Mg and STNA-Cu prepared by the same route further confirmed the advantage of magnesium metal to guide sodium metal growth.Finally,the prepared STNA-Mg-Na metal anode and commercial sodium vanadium phosphate cathode were assembled into a full cell,delivering a discharge capacity of 110.2 mAh·g^(-1)with a retention rate of 95.6%after 110 cycles at 1C rate.

Unraveling the heterogeneity of solid electrolyte interphase kinetically affecting lithium electrodeposition on lithium metal anode

The stability and uniformity of solid electrolyte interphase(SEI)are critical for clarifying the origin of capacity fade and safety issues for lithium metal anodes(LMA).However,understanding the interplay of SEI heterogeneity and Li electrodeposition is limited by the coupling of complex electrochemistry and mechanics processes.Herein,the correlation between the SEI failure behavior and Li deposition morphology is investigated through a quantitative electrochemical-mechanical model.The local deformation and stress of SEI during Li electrodeposition identify that the heterogeneous interface between different components first fails.Compared with the well-known mechanical strength,component uniformity plays the most important role in the initial SEI failure and uneven Li deposition,and a relative component uniformity(p>0.01)represents a proper balance to ensure the stability of the naturally heterogeneous SEI.Furthermore,the component regulation of SEI via the designed electrolyte experimentally demonstrates that improving component uniformity benefits SEI stability and the uniform Li electrodeposition for LMA,thereby increasing the capacity by~20%after 300 cycles.These fundamental understandings and proposed strategy can be not only used to guide the SEI optimization via the electrolyte regulation,but also extended to the rational designs of artificial SEI for high-performance LMA.

Stable lithium metal anode enabled by a robust artificial fluorinated hybrid interphase

One of the key challenges for achieving stable lithium(Li) metal anode is the construction of the rational solid electrolyte interphase(SEI),but its realization still faces enormous challenges.In this work,a robust artificial fluorinated hybrid interphase consisting of lithium-bismuth(Li3Bi) alloy and lithium-fluoride(LiF) was designed to regulate Li deposition without Li dendrite growth.The obtained hybrid interphase showed the high Li+diffusion rate(3.5 × 10^(-4)S cm^(-1)),high electron resistivity(9.04 × 10^(4)Ω cm),and high mechanical strength(1348 MPa),thus enabling the uniform Li deposition at the Li/SEI interface.Specifically,Li3Bi alloy,as a superionic conductor,accelerated the Li+transport and stabilized the hybrid interphase.Meanwhile,LiF was identified as a superior electron-blocker to inhibit the electron tunneling from the Li anode into the SEI.As a result,the modified Li anode showed the stable Li plating/stripping behaviors over 1000 cycles even at 20 mA cm^(-2).Moreover,it also enabled the Li(50 μm)‖LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(4.4 mA h cm^(-2)) full cell to achieve an average Coulombic efficiency(CE) of 99.6%and a high-capacity retention of 79.2% after 100 cycles,whereas the bare Li anode only exhibited a low-capacity retention of 8.0%.This work sheds light on the internal mechanism of Li+transport within the hybrid interface and provides an effective approach to stabilize the interface of Li metal anode.

Fast capture and stabilization of Li‐ions via physicochemical dual effects for an ultra‐stable self‐supporting Li metal anode

Lithium(Li)metal is regarded as one of the most promising anode candidates for next-generation batteries due to its extremely high specific capacity and low redox potential.However,its application is still hindered by the uncontrolled growth of dendritic Li and huge volume fluctuation during cycles.To address these issues,flexible and self-supporting three-dimensional(3D)interlaced Ndoped carbon nanofibers(NCNFs)coated with uniformly distributed 2D ultrathin NiCo_(2)S_(4)nanosheets(denoted CNCS)were designed to eliminate the intrinsic hotspots for Li deposition.Physicochemical dual effects of CNCS arise from limited surface Li diffusivity with a higher Li affinity,leading to uniform Li nucleation and less random accumulation of Li,as confirmed by ab initio molecular dynamics simulations.Due to the unique structure,exchange current density is reduced significantly and metallic Li is further contained within the interspace between the NCNF and NiCo_(2)S_(4)nanosheets,preventing the formation of dendritic Li.The symmetric cell with a Li/CNCS composite anode shows a long-running lifespan for almost 1200 h,with an exceptionally low and stable overpotential under 1mA cm^(-2)/1 mAh cm^(-2).A full cell coupled with a LiFePO4 cathode at a low N/P ratio of 2.45 shows typical voltage profiles but more significantly enhanced performance than that of a LiFePO4 cathode coupled with a bare Li anode.

Manipulating the ion-transference and deposition kinetics by regulating the surface chemistry of zinc metal anodes for rechargeable zinc-air batteries

Aqueous zinc-air battery(ZAB)has attractive features as the potential energy storage system such as high safety,low cost and good environmental compatibility.However,the issue of dendrite growth on zinc metal anodes has seriously hindered the development of ZAB.Herein,the N-doped carbon cloth(NC)prepared via magnetron sputtering is explored as the substrate to induce the uniform nucleation of zinc metal and suppress dendrite growth.Results show that the introduction of heteroatoms accelerates the migration and deposition kinetics of Zn^(2+)by boosting the desolvation process of Zn^(2+),eventually reducing the nucleation overpotential.Besides,theoretical calculation results confirm the zincophilicity of N-containing functional group(such as pyridine N and pyrrole N),which can guide the nucleation and growth of zinc uniformly on the electrode surface by both promoting the redistribution of Zn^(2+) in the vicinity of the surface and enhancing its interaction with zinc atoms.As a result,the half-cell assembled with magnetron sputtered carbon cloth achieves a high zinc stripping/plating coulombic efficiency of 98.8%and long-term stability of over 500 cycles at 0.2 mA cm^(-2).And the Coulombic efficiency reached about 99.5%at the 10th cycle and maintained for more than 210 cycles at a high current density of 5.0 mA cm^(-2).The assembled symmetrical battery can deliver 220 plating/stripping cycles with ultra-low voltage hysteresis of only 11 mV.In addition,the assembled zinc-air full battery with NC-Zn anode delivers a high special capacity of about 429 mAh g_(Zn)^(-1) and a long life of over 430 cycles.The effectiveness of surface functionalization in promoting the transfer and deposition kinetics of Zn^(2+) presented in this work shows enlightening significance in the development of metal anodes in aqueous electrolytes.

In Situ Formed Tribofilms as Efficient Organic/Inorganic Hybrid Interlayers for Stabilizing Lithium Metal Anodes

The practical application of Li metal anodes(LMAs)is limited by uncontrolled dendrite growth and side reactions.Herein,we propose a new friction-induced strategy to produce high-performance thin Li anode(Li@CFO).By virtue of the in situ friction reaction between fluoropolymer grease and Li strips during rolling,a robust organic/inorganic hybrid interlayer(lithiophilic LiF/LiC_(6)framework hybridized-CF_(2)-O-CF_(2)-chains)was formed atop Li metal.The derived interface contributes to reversible Li plating/stripping behaviors by mitigating side reactions and decreasing the solvation degree at the interface.The Li@CFO||Li@CFO symmetrical cell exhibits a remarkable lifespan for 5,600 h(1.0 mA cm^(-2)and 1.0 mAh cm^(-2))and 1,350 cycles even at a harsh condition(18.0 mA cm^(-2)and 3.0 mAh cm^(-2)).When paired with high-loading LiFePO4 cathodes,the full cell lasts over 450 cycles at 1C with a high-capacity retention of 99.9%.This work provides a new friction-induced strategy for producing high-performance thin LMAs.

Simultaneous regulation on coordination environment and interfacial chemistry via taurine for stabilized Zn metal anode

Aqueous Zn-ion batteries(AZIBs)are the potential options for the next-generation energy storage scenarios due to the cost effectiveness and intrinsic safety.Nevertheless,the industrial application of AZIBs is still impeded by a series of parasitic reactions and dendrites at zinc anodes.In this study,taurine(TAU)is used in electrolyte to simultaneously optimize the coordination condition of the ZnSO4electrolyte and interfacial chemistry at the anode.TAU can preferentially adsorb with the zinc metal and induce an in situ stable and protective interface on the anode,which would avoid the connection between H_(2)O and the zinc metal and promote the even deposition of Zn^(2+).The resulting Zn//Zn batteries achieve more than 3000 hours long cyclic lifespan under 1 mA cm^(-2)and an impressive cumulative capacity at 5 mA cm^(-2).Moreover,Zn//Cu batteries can realize a reversible plating/stripping process over 2,400cycles,with a desirable coulombic efficiency of 99.75%(1 mA cm^(-2)).Additionally,the additive endows Zn//NH_(4)V_(4)O_(10)batteries with more stable cyclic performance and ultrafast rate capability.These capabilities can promote the industrial application of AZIBs.

Gas‐phase fluorination of conjugated microporous polymer microspheres for effective interfacial stabilization in lithium metal anodes

Lithium(Li)metal anodes have attracted extensive attention due to their ultrahigh theoretical capacity and low potential.However,the uneven deposition of Li near the unstable electrode/electrolyte interfaces leads to the growth of Li dendrites and the degradation of active electrodes.Herein,we directly fluorinate alkyne-containing conjugated microporous polymers(ACMPs)microspheres with fluorine gas(F_(2))to introduce a novel fluorinated interlayer as an interfacial stabilizer in lithium metal batteries.Using density functional theory methods,it is found that as-prepared fluorinated ACMP(FACMP)has abundant partially ionic C–F bonds.The C–F bonds with electrochemical lability yield remarkable lithiophilicity during cycling.The in situ reactions between the active C–F bonds and Li ions enable transfer of lithium fluoride microcrystals to the solid electrolyte interphase(SEI)layers,guaranteeing effective ionic distribution and smooth Li deposition.Consequently,Li metal electrodes with the fluorinated interlayers demonstrate excellent cycling performances in both half-batteries and full cells with a lithium bis(trifluoromethanesulfonyl)imide electrolyte as well as a nonfluorinated lithium bis(oxalate)borate electrolyte system.This strategy is highly significant in customizable SEI layers to stabilize electrode interfaces and ensure high utilization of Li metal anodes,especially in a nonfluorinated electrolyte.

Ultrathin and Air-Stable Lithium Metal Anodes with Superlong Cycling Life in Ether/Ester-Based Electrolytes

Ultrathin and air-stable Li metal anodes hold great promise toward high-energy and high-safety Li metal batteries(LMBs).However,the application of LMBs is technically impeded by existing Li metal anodes with large thickness,high reactivity,and poor performance.Here,we developed a novel and scalable approach for the construction of a 10-μm-thick flexible and air-stable Li metal anode by conformally encapsulating Li within a multifunctional VN film.Specifically,the highly lithiophilic VN layer guides a uniform deposition of Li,while abundant and multilevel pores arising from assembly of ultrathin nanosheets enable a spatially confined immersion of metallic Li,thus ensuring an ultrathin and sandwiched Li anode.More impressively,the strong hydrophobicity of VN surface can effectively improve the stability of anode to humid air,whereas the highly conductive framework greatly boosts charge transfer dynamics and enhances Li utilization and high-rate capability.Benefiting from such fascinating features,the constructed Li-VN anode exhibits ultrastable cycling stability in both ether(2500 h)and carbonate(900 h)electrolytes,respectively.Moreover,even exposed to ambient air for 12 h,the anode still can retain~78%capacity,demonstrating excellent air-defendable capability.This work affords a promising strategy for fabricating high-performance,high-safety,and low-cost LMBs.

Recent Progress and Prospects on Dendrite-free Engineerings for Aqueous Zinc Metal Anodes

Rechargeable zinc-ion batteries with mild aqueous electrolytes are one of the most promising systems for large-scale energy storage as a result of their inherent safety,low cost,environmental-friendliness,and acceptable energy density.However,zinc metal anodes always suffer from unwanted dendrite growth,leading to low Coulombic efficiency and poor cycle stability and during the repeated plating/stripping processes,which substantially restrict their further development and application.To solve these critical issues,a lot of research works have been dedicated to overcoming the drawbacks associated with zinc metal anodes.In this overview,the working mechanisms and existing issues of the zinc metal anodes are first briefly outlined.Moreover,we look into the ongoing processes of the different strategies for achieving highly stable and dendrite-free zinc metal anodes,including crystal engineering,structural engineering,coating engineering,electrolyte engineering,and separator engineering.Finally,some challenges being faced and prospects in this field are provided,together with guiding significant research directions in the future.