Synthesis of High Purity Lithium Sulfide for Sulfide Solid Electrolyte Applications through Hydrogen Reduction of Lithium Sulfate

This paper is aimed to present a clean,inexpensive and sustainable method to synthesize high purity lithium sulfide(Li_(2)S)powder through hydrogen reduction of lithium sulfate(Li_(2)SO_(4)).A three-step reduction process has been successfully developed to synthesize well-crystallized and single-phase Li_(2)S powder by investigating the melting,sintering and reduction behavior of the mixtures of Li_(2)SO_(4)-Li_(2)S.High purity alumina was found to be the most suitable crucible material for producing high purity Li_(2)S,because it was not attacked by the Li_(2)SO_(4)-Li_(2)S melt during heating,as compared with other materials,such as carbon,mullite,quartz,boron nitride and stainless steel.The use of synthesized LizS resulted in higher purity and substantially higher room temperature ionic conductivity(2.77 mS·cm^(-1))for the argyrodite sulfide electrolyte Li_(6)PS_(5)Cl than commercial Li_(2)S(1.12 mS·cm^(-1)).This novel method offers a great opportunity to produce battery grade Li_(2)S for sulfide solid electrolyte applications.

Incorporation of Ionic Conductive Polymers into Sulfide Electrolyte-Based Solid-State Batteries to Enhance Electrochemical Stability and Cycle Life

Sulfide-based inorganic solid electrolytes are promising materials for high-performance safe solid-state batteries.The high ion conductivity,mechanical characteristics,and good processability of sulfide-based inorganic solid electrolytes are desirable properties for realizing high-performance safe solid-state batteries by replacing conventional liquid electrolytes.However,the low chemical and electrochemical stability of sulfide-based inorganic solid electrolytes hinder the commercialization of sulfide-based safe solid-state batteries.Particularly,the instability of sulfide-based inorganic solid electrolytes is intensified in the cathode,comprising various materials.In this study,carbonate-based ionic conductive polymers are introduced to the cathode to protect cathode materials and suppress the reactivity of sulfide electrolytes.Several instruments,including electrochemical spectroscopy,X-ray photoelectron spectroscopy,and scanning electron microscopy,confirm the chemical and electrochemical stability of the polymer electrolytes in contact with sulfide-based inorganic solid electrolytes.Sulfide-based solid-state cells show stable electrochemical performance over 100 cycles when the ionic conductive polymers were applied to the cathode.

Fluorine-Doped High-Performance Li_(6)PS_(5)Cl Electrolyte by Lithium Fluoride Nanoparticles for All-Solid-State Lithium-Metal Batteries

All-solid-state lithium-metal batteries(ASSLMBs)are widely considered as the ultimately advanced lithium batteries owing to their improved energy density and enhanced safety features.Among various solid electrolytes,sulfide solid electrolyte(SSE)Li_(6)PS_(5)Cl has garnered significant attention.However,its application is limited by its poor cyclability and low critical current density(CCD).In this study,we introduce a novel approach to enhance the performance of Li_(6)PS_(5)Cl by doping it with fluorine,using lithium fluoride nanoparticles(LiFs)as the doping precursor.The F-doped electrolyte Li_(6)PS_(5)Cl-0.2LiF(nano)shows a doubled CCD,from 0.5 to 1.0 mA/cm^(2) without compromising the ionic conductivity;in fact,conductivity is enhanced from 2.82 to 3.30 mS/cm,contrary to the typical performance decline seen in conventionally doped Li_(6)PS_(5)Cl electrolytes.In symmetric Li|SSE|Li cells,the lifetime of Li_(6)PS_(5)Cl-0.2LiF(nano)is 4 times longer than that of Li_(6)PS_(5)Cl,achieving 1500 h vs.371 h under a charging/discharging current density of 0.2 mA/cm^(2).In Li|SSE|LiNbO_(3)@NCM721 full cells,which are tested under a cycling rate of 0.1 C at 30℃,the lifetime of Li_(6)PS_(5)Cl-0.2LiF(nano)is four times that of Li_(6)PS_(5)Cl,reaching 100 cycles vs.26 cycles.Therefore,the doping of nano-LiF off ers a promising approach to developing high-performance Li_(6)PS_(5)Cl for ASSLMBs.

In situ formed LiF-Li_(3)N interface layer enables ultra-stable sulfide electrolyte-based all-solid-state lithium batteries

Sulfide solid electrolytes are promising for high energy density and safety in all-solid-state batteries due to their high ionic conductivity and good mechanical properties.However,the application of sulfide solid electrolytes in all-solid-state batteries with lithium anode is restricted by the side reactions at lithium/electrolytes interfaces and the growth of lithium dendrite caused by nonuniform lithium deposition.Herein,a homogeneous LiF-Li_(3)N composite protective layer is in situ formed via a manipulated reaction of pentafluorobenzamide with Li metal.The LiF-Li_(3)N layer with both high interfacial energy and interfacial adhesion energy can synergistically suppress side reactions and inhibit the growth of lithium dendrite,achieving uniform deposition of lithium.The critical current densities of Li_(10)GeP_(2)S_(12)and Li_(6)PS_(5)Cl are increased to 3.25 and 1.25 mA cm^(-2)with Li@LiF-Li_(3)N layer,which are almost triple and twice as those of Li-symmetric cells in the absence of protection layer,respectively.Moreover,the Li@LiF-Li_(3)N/Li10GeP2S12/Li@LiF-Li_(3)N cell can stably cycle for 9000 h at 0.1 mA cm^(-2)under 0.1 mA h cm^(-2),and Li@LiF-Li_(3)N/Li_(6)PS_(5)Cl/Li@LiF-Li_(3)N cell achieves stable Li plating/stripping for 8000 h at 0.1 mA cm^(-2)under10 m A h cm^(-2).The improved dynamic stability of lithium plating/stripping in Li@LiF-Li_(3)N/Li_(10)GeP_(2)S_(12)or Li_(6)PS_(5)Cl interfaces is proved by three-electrode cells.As a result,LiCoO_(2)/electrolytes/Li@LiF-Li_(3)N batteries with Li_(10)GeP_(2)S_(12)and Li_(6)PS_(5)Cl exhibit remarkable cycling stability of 500 cycles with capacity retentions of 93.5%and 89.2%at 1 C,respectively.

Realizing high-performance all-solid-state batteries with sulfide solid electrolyte and silicon anode:A review

Sulfide solid electrolyte(SE)is one of the most promising technologies for all-solid-state batteries(ASSBs)because of its high ionic conductivity and ductile mechanical properties.In order to further improve the energy density of sulfide-based ASSBs and promote practical applications,silicon anodes with ultrahigh theoretical capacity(4,200 mAh·g^(−1))and rich resource abundance have broad commercial prospects.However,significant challenges including bulk instability of sulfide SEs and poor utilization of silicon materials have severely impeded the ASSBs from becoming viable.In this review,we first introduce the critical bulk properties of sulfide SEs and the most recent improving strategies covering the ionic conductivity,air stability,electrochemical window,mechanical stability,thermostability and solvent stability.Next,we introduce the main factors affecting the compatibility of silicon and sulfide SE,including the carbon’s effect,particle size of silicon,external pressure,silicon composite matrix and the depth of silicon’s lithiation.Finally,we discuss possible research directions in the future.We hope that this review can provide a comprehensive picture of the role of nanoscale approaches in recent advances in ASSBs with sulfide and silicon,as well as a source of inspiration for future research.

The Contact Interface Engineering of All-Sulfide-Based Solid State Batteries via Infiltrating Dissoluble Sulfide Electrolyte

All-solid-state lithium batteries(ASSLBs)based on sulfide solid electrolytes(SEs)are one of the most promising strategies for next-generation energy storage systems and electronic devices.However,the poor chemical/electrochemical stability of sulfide SEs with oxide cathode materials and high interfacial impedance,particularly due to physical contact failure,are the major limiting factors to the development of sulfide SEs in ASSLBs.Herein,the composite cathode of MOF-derived Fe_(7)S_(8)@C and Li_(6)PS_(5)Br fabricated by an infiltration method(IN-Fe_(7)S_(8))with dissoluble sulfide electrolyte(dissoluble SE)is reported.Dissoluble SE can easily infiltrate the porous sheet-type Fe_(7)S_(8)@C cathode to homogeneously contact with Fe_(7)S_(8)nanoparticles that are embedded in the surrounding carbon matrixes and form a fast ionic transport network.Benefiting from applying dissoluble SE and Fe_(7)S_(8)@C,the IN-Fe_(7)S_(8)-based cells displayed a reversible capacity of 510 mAh g^(-1)after 180 cycles at 0.045 mA cm^(-2)at 30℃.This work demonstrates a novel and practical method for the development of high-performance all-sulfide-based solid state batteries.

Interfaces in Sulfide Solid Electrolyte‑Based All‑Solid‑State Lithium Batteries:Characterization,Mechanism and Strategy

Owing to the advantages of high energy density and environmental friendliness,lithium-ion batteries(LIBs)have been widely used as power sources in electric vehicles,energy storage systems and other devices.Conventional LIBs composed of liquid electrolytes(LEs)have potential safety hazards;thermal runaway easily leads to battery explosion and spontaneous combustion.To realize a large-scale energy storage system with higher safety and higher energy density,replacing LEs with solid-state electrolytes(SSEs)has been pursued.Among the many SSEs,sulfide SSEs are attractive because of their high ionic conductivities,easy processabilities and high thermostabilities.However,interfacial issues(interfacial reactions,chemo-mechanical failure,lithium dendrite formation,etc.)between sulfide SSEs and electrodes are factors limiting widespread application.In addition,the intrinsic interfacial issues of sulfide SSEs(electrochemical windows,diffusion mechanisms of Li^(+),etc.)should not be ignored.In this review,the behaviors,properties and mechanisms of interfaces in all-solid-state lithium batteries with a variety of sulfide SSEs are comprehensively summarized.Additionally,recent research progress on advanced characterization methods and designs used to stabilize interfaces is discussed.Finally,outlooks,challenges and possible interface engineering strategies are analyzed and proposed.

Interfacial challenges for all-solid-state batteries based on sulfide solid electrolytes

Sulfide solid electrolytes(e.g.,lithium thiophosphates)have the highest room-temperature ionic conductivity(-10^(-2) S cm^(-1))among solid Li-ion conductors so far,and thus have attracted ever-increasing attention for high energy-density and safety all-solid-state batteries(ASSBs).However,interfacial issues between sulfide electrolytes and electrodes have been the main challenges for their applications in ASSBs.The interfacial instabilities would occur due to side reactions of sulfides with electrodes,poor solid-solid contact,and lithium dendrites during charge/discharge cycling.In this review,we analyze the interfacial issues in ASSBs based on sulfide electrolytes,and in particular,discuss strategies for solving these interfacial issues and stabilize the electrode-electrolyte interfaces.Moreover,a perspective of the interfacial engineering for sulfide-based ASSBs is provided.

Improving thermal stability of sulfide solid electrolytes:An intrinsic theoretical paradigm

All-solid-state batteries(ASSBs)have been widely acknowledged as the key next-generation energy storage technology/device,due to their high safety and energy density.Among all solid electrolytes(SEs)that have been studied for ASSBs,sulfide SEs represent the most promising technical route due to their ultra-high ionic conductivity and desirable mechanical property.However,few results have been reported to study the thermal stability/safety issue of sulfide SEs and ASSBs.Herein,we develop the first-of-its-kind theoretical paradigm and a new conceptual parameter Th to quantitatively calculate/predict the essential thermal stability of sulfide SEs.This theoretical paradigm takes all types of parameters(e.g.crystal structure,localized polyhedra configuration,bond energy,bond type,bond number,normalization factor,and the energy correction factor)into consideration,and more importantly,can be simplified into one straightforward equation for its convenient application in any crystal-line systems.To prove its functionality,the typical experimental strategies(stoichiometric ratio control and elemental doping)are adopted for typical sul-fide SEs(Li7P3S11,Li3PS4)to improve their thermal stabilities,based on the predictions obtained from the derived theory and equation.Moreover,the potential doping elements to improve thermal stability of sulfide SEs are screened throughout the whole periodic table,and the theoretically predicted trends correspond well with experimental evidence.This work may represent the most critical breakthroughs in the research field of thermal stability for sul-fide SEs,not only because it fills the gap of this field,but also due to its precise and quantitative prediction based on a complete consideration of all parameters that determine their thermal stabilities.The handy model devel-oped herein can also be applied to any crystalline materials.

Perspective on powder technology for all-solid-state batteries:How to pair sulfide electrolyte with high-voltage cathode

Sulfide solid electrolytes(SEs)have attracted ever-increasing attention due to their superior roomtemperature ionic conductivity(~10^(-2) S cm^(-1)).Additionally,the integration of sulfide SEs and highvoltage cathodes is promising to achieve higher energy density.However,the incompatible interfaces between sulfide SEs and high-voltage cathodes have been one of the key factors limiting their applications.Therefore,this review presents a critical summarization of the interfacial issues in all-solid-state lithium batteries based on sulfide SEs and high-voltage cathodes and proposes strategies to stabilize the electrolyte/cathode interfaces.Moreover,the future research direction of electrolyte/cathode interfaces and application prospects of powder technology in sulfide-based ASSLBs were also discussed.

Interface engineering for composite cathodes in sulfide-based all-solid-state lithium batteries

All-solid-state lithium battery(ASLB)based on sulfide-based electrolyte is considered to be a candidate for the next-generation high-energy storage system.Despite the high ionic conductivity of sulfide solid electrolyte,the poor interfacial stability(mechanically and chemically)between active materials and sulfide solid electrolytes in composite cathodes leads to inferior electrochemical performances,which impedes the practical application of sulfide electrolytes.In the past years,various of strategies have been carried out to achieve an interface with low impedance in the composite cathodes.Herein,a review of recent progress of composite cathodes for all-solid-state sulfide-based lithium batteries is summarized,including the interfacial issues,design strategies,fabrication methods,and characterization techniques.Finally,the main challenges and perspectives of composite cathodes for high-performance all-solidstate batteries are highlighted for future development.

Integrated interface configuration by in-situ interface chemistry enabling uniform lithium deposition in all-solid-state lithium metal batteries

All-solid-state lithium metal batteries(ASSLMBs)are considered as one of the ultimate goals for the development of energy storage systems due to their high energy density and high safety.However,the mismatching of interface transport kinetics as well as interfacial instability induces the growth of lithium dendrite and thus,leads to severe degradation of battery electrochemical performances.Herein,an integrated interface configuration(IIC)consisting of in-situ generated Li I interphase and Li-Ag alloy anode is proposed through in-situ interface chemistry.The IIC is capable of not only regulating charge transport kinetics but also synchronously stabilizing the lithium/electrolyte interface,thereby achieving uniform lithium platting.Therefore,Li||Li symmetric cells with IIC achieve a critical current density of up to 1.6 mA cm^(-2)and achieve stable cycling over 1600 hours at a high current density of 0.5 mA cm^(-2).Moreover,a high discharge capacity of 140.1 mA h g-1at 0.1 C is also obtained for the Li(Ni_(0.6)Co_(0.2)Mn_(0.2))O_(2)(NCM622)full battery with a capacity retention of 65.6%after 300 cycles.This work provides an effective method to synergistically regulate the interface transport kinetics and inhibit lithium dendrite growth for high-performance ASSLMBs.

Synergy of I-Cl co-occupation on halogen-rich argyrodites and resultant dual-layer interface for advanced all-solid-state Li metal batteries

The(electro)chemical stability and Li dendrite suppression capability of sulfide solid electrolytes(SEs)need further improvement for developing all-solid-state Li batteries(ASSLBs).Here,we report advanced halogen-rich argyrodites via I and Cl co-occupation on the crystal lattice.Notably,a proper I content forms a single phase,whereas an excessive I causes precipitation of two argyrodite phases like a superlattice structure.The resultant synergistic effect of the optimized composition allows to gain high ionic conductivities at room temperature and-20℃,and enhances the(electro)chemical stability against Li and Li dendrite suppression capability.The Li|argyrodite interface is very sensitive to the ratio of I and Cl.A LiCl-and LiI-rich double-layer interface is observed from the cell using the SE with optimized composition,whereas too high I content forms only a single interface layer with a mixture of Lil and LiCl.This double-layer interface is found to effectively mitigate the Li/SE reaction.The proper designed argyrodite enables ASSLBs to achieve good electrochemical properties at a broad temperature range regardless of the electrode materials.This co-occupation strategy provides a novel exploration for advanced halogen-rich argyrodite system.

Synthesis and electrochemical performance of (100-x)Li7P3S11-xLi2OHBr composite solid electrolyte for all-solid-state lithium batteries

Li7P3S11solid electrolytes with high lithium-ion conductivity are promising candidates for use in all-solidstate lithium batteries.However,this electrolyte’s poor interfacial compatibility with lithium electrodes causes unstable cyclability.In this study,in order to address this problem,(100-x)Li7P3S11-xLi2OHBr(x=0,2,5,10,20,30,40,and 50)electrolytes are prepared by a high energy ball-milling technique and heat-treatment process.The resulting(100-x)Li7P3S11-xLi2OHBr(x=2,5,10,20,30,40,and 50)electrolytes provide improved electrochemical performance with good cycling stability and a wide electrochemical window of up to 10 V(vs.Li/Li+).Moreover,these electrolytes have high ionic conductivity of 10-4–10-5S/cm at room temperature.Particularly,the 90Li7P3S11-10Li2OHBr electrolyte displays the highest conductivity of 4.4×10-4S/cm at room temperature as well as improved cyclability.Moreover,90Li7P3S11-10Li2OHBr shows decreased interfacial resistance between the solid electrolyte and cathode electrode,which was revealed by Electrochemical Impedance Spectroscopy(EIS)analysis.The initial discharge capacity of 90Li7P3S11-10Li2OHBr was found to be 135 m Ah/g when used in a In|solid electrolyte|Li(Ni0.6Co0.2Mn0.2)O2 all-solid-state lithium battery(ASSLB).Thus,we can conclude the addition of Li2OHBr into the Li7P3S11results in enhanced electrochemical properties.

Ti_(3)C_(2)T_(x) MXene in-situ transformed Li_(2)TiO_(3) interface layer enabling 4.5 V-LiCoO_(2)/sulfide all-solid-state lithium batteries with superior rate capability and cyclability

All-solid-state lithium batteries(ASSLBs)based on sulfide electrolytes promise next-generation energy storage with high energy density and safety.However,the sulfide electrolytes suffer from phase instability and sluggish interfacial charge transport when pairing with layered oxide cathodes at high voltages.Herein,a simple and efficient strategy is proposed using two-dimensional Ti_(3)C_(2)T_(x)MXene as starting material to in-situ construct a 15 nm Li_(2)TiO_(3) layer on a typical oxide cathode,LiCoO_(2).The in-situ transformation of Ti_(3)C_(2)T_(x)into Li_(2)TiO_(3) layer occurs at a low temperature of 500℃,avoiding the phase deterioration of LiCoO_(2).The thin Li_(2)TiO_(3) layer is Li^(+)conducting and electrochemically stable,thereby preventing the interfacial decomposition of sulfide electrolytes induced by LiCoO_(2) at high voltages and facilitating Li+transport at the interface.Moreover,Li_(2)TiO_(3) can stabilize the layer structure of LiCoO_(2) at high voltages.Consequently,the sulfide-based ASSLB using LiCoO_(2)@Li_(2)TiO_(3) cathode can operate stably at a high voltage of up to 4.5 V(vs.Li+/Li),delivering an outstanding initial specific discharge capacity of 138.8 m Ah/g with a high capacity retention of 86.2% after 100 cycles at 0.2 C.The in-situ transformation strategy may also apply to other MXenes,offering a general approach for constructing other advanced lithiated coatings for oxide cathodes.

Dry electrode technology for scalable and flexible high-energy sulfur cathodes in all-solid-state lithium-sulfur batteries

All-solid-state lithium-sulfur batteries(ASSLSBs)employing sulfide solid electrolytes are one of the most promising next-generation energy storage systems due to their potential for higher energy density and safety.However,scalable fabrication of sheet-type sulfur cathodes with high sulfur loading and excellent performances remains challenging.In this work,sheet-type freestanding sulfur cathodes with high sulfur loading were fabricated by dry electrode technology.The unique fibrous morphologies of polytetrafluoroethylene(PTFE)binders in dry electrodes not only provides excellent mechanical properties but also uncompromised ionic/electronic conductance.Even employed with thickened dry cathodes with high sulfur loading of 2 mg cm^(-2),ASSLSBs still exhibit outstanding rate performance and cycle stability.Moreover,the all-solid-state lithium-sulfur monolayer pouch cells(9.2 m Ah)were also demonstrated and exhibited excellent safety under a harsh test situation.This work verifies the potential of dry electrode technology in the scalable fabrication of thickened sulfur cathodes and will promote the practical applications of ASSLSBs.

Tailoring lithium concentration in alloy anodes for long cycling and high areal capacity in sulfide-based all solid-state batteries

Lithium–indium(Li-In)alloys are important anode materials for sulfide-based all-solid-state batteries(ASSBs),but how different Li concentrations in the alloy anodes impact the electrochemical performance of ASSBs remains unexplored.This paper systematically investigates the impact that different Li concentrations in Li-In anodes have on the performance of ASSBs.We show that In with 1 wt%Li(LiIn-1)exhibits the best performance for ASSBs among all the tested Li-In anodes.In essence,LiIn-1 not only provides sufficient Li to compensate for first-cycle capacity loss in the anode but also facilitates the formation of a LiIn alloy phase that has the best charge transfer kinetics among all the Li_(x) In alloy phases.The ASSB with a LiIn-1 anode and a LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) cathode reached 3400 cycles at an initial capacity of 125 mAh/g.Remarkably,ASSBs with a high cathode active material(CAM)loading of 36 mg/cm 2 delivered a high areal capacity of 4.05 mAh/cm^(2) at high current density(4.8 mA/cm^(2)),with a capacity retention of 92% after 740 cycles.At an ultra-high CAM loading of 55.3 mg/cm^(2),the ASSB achieved a stable areal capacity of 8.4 mAh/cm^(2) at current density of 1.7 mA/cm 2.These results bring us one step closer to the practical application of ASSBs.

Air Stability of Solid‑State Sulfide Batteries and Electrolytes

Sulfides have been widely acknowledged as one of the most promising solid electrolytes(SEs)for all-solid-state batteries(ASSBs)due to their superior ionic conductivity and favourable mechanical properties.However,the extremely poor air stability of sulfide SEs leads to destroyed structure/performance and release of toxic H_(2)S gas,which greatly limits mass-production/practical application of sulfide SEs and ASSBs.This review is designed to serve as an all-inclusive handbook for studying this critical issue.First,the research history and milestone breakthroughs of this field are reviewed,and this is followed by an in-depth elaboration of the theoretical paradigms that have been developed thus far,including the random network theory of glasses,hard and soft acids and bases(HSAB)theory,thermodynamic analysis and kinetics of interfacial reactions.Moreover,the characterization of air stability is reviewed from the perspectives of H2S generation,morphology evolution,mass change,component/structure variations and electrochemical performance.Furthermore,effective strategies for improving the air stabilities of sulfide SEs are highlighted,including H_(2)S absorbents,elemental substitution,design of new materials,surface engineering and sulfide-polymer composite electrolytes.Finally,future research directions are proposed for benign development of air stability for sulfide SEs and ASSBs.

Boosting the energy density of sulfide-based all-solid-state batteries at low temperatures by charging to high voltages up to 6 V

Sulfide electrolyte-based all-solid-state batteries(ASSBs)are potential next generation energy storage technology due to the high ionic conductivity of sulfide electrolytes and potentially improved energy density and safety.However,the performance of ASSBs at/below subzero temperatures has not been explored systematically.Herein,low temperature(LT)performance of LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)|Li_(9.54)Si_(1.74)P_(1.44)S11.7Cl_(0.3)(LiSPSCl)|Li_(4)Ti_(5)O_(12)(LTO)ASSBs was investigated.By charging the ASSB to 6 V at−40℃,a capacity of 100.7 mAh∙g^(−1)at 20 mA∙g^(−1)was achieved,which is much higher than that charged to 4.3 V(4.6 mAh∙g^(−1))at−40℃.Moreover,atomic resolution microscopy revealed that the NCM811 remained almost intact even after being charged to 6 V.In contrast,NCM811 was entirely destructed when charged to 6 V at room temperature.The sharp difference arises from the large internal charge transfer resistance at LT which requires high voltage to overcome.Nevertheless,such high voltage is not harmful to the active material but beneficial to extracting most energy out of the ASSBs at LT.We also demonstrated that thinner electrolyte is favorable for LT operation of ASSBs due to the reduced ion transfer distance.This work provides new strategies to boost the capacity and energy density of sulfide-based ASSBs at LT for dedicated LT applications.

Challenges,interface engineering,and processing strategies toward practical sulfide-based all-solid-state lithium batteries

All-solid-state lithium batteries have emerged as a priority candidate for the next generation of safe and energy-dense energy storage devices surpassing state-of-art lithium-ion batteries.Among multitudinous solid-state batteries based on solid electrolytes(SEs),sulfide SEs have attracted burgeoning scrutiny due to their superior ionic conductivity and outstanding formability.However,from the perspective of their practical applications concerning cell integration and production,it is still extremely challenging to constructing compatible electrolyte/electrode interfaces and developing available scale processing technologies.This review presents a critical overview of the current underlying understanding of interfacial issues and analyzes the main processing challenges faced by sulfide-based all-solid-state batteries from the aspects of cost-effective and energy-dense design.Besides,the corresponding approaches involving interface engineering and processing protocols for addressing these issues and challenges are summarized.Fundamental and engineering perspectives on future development avenues toward practical application of high energy,safety,and long-life sulfide-based all-solid-state batteries are ultimately provided.