The Critical Role of Fillers in Composite Polymer Electrolytes for Lithium Battery

With excellent energy densities and highly safe performance,solidstate lithium batteries(SSLBs)have been hailed as promising energy storage devices.Solid-state electrolyte is the core component of SSLBs and plays an essential role in the safety and electrochemical performance of the cells.Composite polymer electrolytes(CPEs)are considered as one of the most promising candidates among all solid-state electrolytes due to their excellent comprehensive performance.In this review,we briefly introduce the components of CPEs,such as the polymer matrix and the species of fillers,as well as the integration of fillers in the polymers.In particular,we focus on the two major obstacles that affect the development of CPEs:the low ionic conductivity of the electrolyte and high interfacial impedance.We provide insight into the factors influencing ionic conductivity,in terms of macroscopic and microscopic aspects,including the aggregated structure of the polymer,ion migration rate and carrier concentration.In addition,we also discuss the electrode-electrolyte interface and summarize methods for improving this interface.It is expected that this review will provide feasible solutions for modifying CPEs through further understanding of the ion conduction mechanism in CPEs and for improving the compatibility of the electrode-electrolyte interface.

Optimized CeO_(2) Nanowires with Rich Surface Oxygen Vacancies Enable Fast Li-Ion Conduction in Composite Polymer Electrolytes

Low-cost and flexible solid polymer electrolytes are promising in all-solid-state Li-metal batteries with high energy density and safety.However,both the low room-temperature ionic conductivities and the small Li^(+)transference number of these electrolytes significantly increase the internal resistance and overpotential of the battery.Here,we introduce Gd-doped CeO_(2) nanowires with large surface area and rich surface oxygen vacancies to the polymer electrolyte to increase the interaction between Gd-doped CeO_(2) nanowires and polymer electrolytes,which promotes the Li-salt dissociation and increases the concentration of mobile Li ions in the composite polymer electrolytes.The optimized composite polymer electrolyte has a high Li-ion conductivity of 5×10^(-4)4 S cm^(-1) at 30℃ and a large Li+transference number of 0.47.Moreover,the composite polymer electrolytes have excellent compatibility with the metallic lithium anode and high-voltage LiNi_(0.8)Mn _(0.1)Co_(0.1)O_(2)(NMC)cathode,providing the stable cycling of all-solid-state batteries at high current densities.

Enhanced Electrochemical Performance of Poly(ethylene oxide)Composite Polymer Electrolyte via Incorporating Lithiated Covalent Organic Framework

The lithiated covalent organic framework(named TpPa-SO_(3) Li),which was prepared by a mild chemical lithiation strategy,was introduced in poly(ethylene oxide)(PEO)to produce the composite polymer electrolytes(CPEs).Li-ion can transfer along the PEO chain or across the layer of TpPa-SO_(3) Li within the nanochannels,resulting in a high Li-ion conductivity of3.01×10^(-4)S/cm at 60℃.When the CPE with 0.75 wt.%TpPa-SO_(3) Li was used in the LiFePO_(4)‖Li solid-state battery,the cell delivered a stable capacity of 125 mA·h/g after 250 cycles at 0.5 C,60℃.In comparison,the cell using the CPE without TpPa-SO_(3) Li exhibited a capacity of only 118 mA·h/g.

Electrochemical behaviors of novel composite polymer electrolytes for lithium batteries

A novel composite polymer electrolyte was prepared by blending an appropriateamount of LiClO_4 and 10 percent (mass fraction) fumed SiO_2 with the block copolymer of poly(ethylene oxide) (PEO) synthesized by poly (ethylene glycol) (PEG) 400 and CH_2C1_2 The ionicconductivity, electrochemical stability, interfacial characteristic and thermal behavior of thecomposite polymer electrolyte were studied by the measurements of AC impedance spectroscopy, linearsweep voltammetry and differential scanning calorimetry (DSC), respectively. The glass transitiontemperature acts as a function of salt concentration, which increases with the LiClO_4 content.Lewis acid-base model interaction mechanism was introduced to interpret the interactive relationbetween the filled fumed SiO_2 and the lithium salt in the composite polymer electrolyte. Over thesalt concentration range and the measured temperature, the maximum ionic conductivity of thecomposite polymer electrolyte (10^(-4.41) S/cm) appeared at EO/Li=25 (mole ratio) and 30 deg C, andthe beginning oxidative degradation potential versus Li beyond 5 V.

Ultrathin poly(cyclocarbonate-ether)-based composite electrolyte reinforced with high-strength functional skeleton

Composite polymer electrolytes(CPEs)are considered to be the most promising to break through the performance and safety limitations of traditional lithium-ion batteries because of their excellent electrochemical and mechanical properties.Aiming at the performance limitations of the most common polyether matrix such as poly(ethylene oxide)(PEO),a novel poly(cyclocarbonate-ether)polymer matrix was prepared by in-situ thermal curing,the weaker interaction between its C=O bond and Li^(+)can promote the rapid transport of Li^(+).Adding ionic liquid and active filler LLZTO to the matrix can synergistically reduce the crystallinity of matrix and promote the dissociation of lithium salts.In addition,a 3D functional skeleton made of polyacrylonitrile(PAN)and lithium fluoride(LiF)can greatly improve the mechanical strength of polymer matrix after cold pressing,and Li F is also conducive to interface stability.The thickness of the optimal sample(VP6L/CPL)was only 25μm,and its ionic conductivity,lithium ion transference number,and electrochemical stability window were as high as 7.17×10^(-4)S cm^(-1)(25℃),0.54 and 5.4 V,respectively,while the mechanical strength reaches 6.1 MPa,which can fully inhibit the growth of lithium dendrites.The excellent electrochemical performance and mechanical strength enable the assembled Li|VP6L/CPL|Li battery to be continuously charged for over 200 h and cycled stably for more than 2300 h,and Li|VP6L/CPL|LFP battery can be stably cycled for more than 400 and 550 cycles at 1 C(40℃)and 0.5 C(25℃),respectively.

Particles in composite polymer electrolyte for solid-state lithium batteries:A review

Solid-state lithium batteries(SSLBs)have been identified as one kind of the most promising energy conversion and storage devices because of their safety,high energy density,and long cycling life.The development of solid-state electrolyte is vital to commercialize SSLBs.Composite polymer electrolyte(CPE),derived by compositing inorganic particles into solid polymer electrolyte has become the most practical species for SSLBs because it inherits the advantages of polymer electrolyte and simultaneously achieves enhanced ionic conductivity and mechanical properties.The characteristics of inorganic particles and their interaction with polymers strongly impact the performance of CPE,improving its ionic conductivity,mechanical properties,thermal and electrochemical stability,as well as interface compatibility with both electrodes.In this review,the effects of particle characteristics including its species,size,proportion,morphology on the ionic conductivity and mechanical properties of CPE are reviewed.Meanwhile,some novel composite strategies are also introduced including surface modification,hybridization,and alignment of particles in polymer matrices,as well as some new preparation methods of CPE.The interactions between particles and other components in CPE including polymer matrices or lithium salt are particularly focused herein to reveal the lithium conductive mechanism.Finally,a perspective on the direction of future CPE development for SSLBs is presented.

Composite polymer electrolytes reinforced by a three-dimensional polyacrylonitrile/Li_(0.33)La_(0.557)TiO_(3)nanofiber framework for room-temperature dendrite-free all-solid-state lithium metal battery

Substituting liquid electrolytes with solid elec-trolytes is considered as an important strategy to solve the problem of flammability and explosion for traditional lithium-ion batteries(LIB).However,neither inorganic solid electrolytes(ISE)nor solid polymer electrolytes(SPE)alone can meet the operating requirements for room-temperature(RT)all-solid-state lithium metal batteries(ASSLMB).Here,we report a three-dimensional(3D)nanofiber framework reinforced polyethylene oxide(PEO)-based composite polymer electrolytes(CPE)through con-structing a nanofiber framework combining polyacryloni-trile(PAN)and fast Li-ion conductor Li_(0.33)La_(0.557)TiO_(3)(LLTO)framework by electrospinning method.Mean-while,the PEO electrolyte filled in the pores of the PAN/LLTO nanofiber framework can effectively isolate the direct contact between the chemically active Ti^(4+)in LLTO with lithium metal,thereby avoiding the occurrence of interfacial reactions.Enhanced electrochemical stability makes a wide electrochemical window up to 4.8 V with an ionic conductivity of about 9.87×10^(-5)S·cm^(-1)at RT.Benefiting from the excellent lithium dendrite growth inhibition ability of 3D PAN/LLTO nanofiber framework,especially when the mass of LLTO reaches twice that of the PAN,Li/Li symmetric cell could cycle stably for 1000 h without a short circuit.In addition,under 30℃,the LiFePO_(4)/Li ASSLMB using such CPE delivers large capacities of 156.2 and 140 mAh·g^(-1)at 0.2C and 0.5C,respectively.These results provide a new insight for the development of the next generation of safe,high-perfor-mance ASSLMBs.

Physicochemical properties of a novel composite polymer electrolyte doped with vinyltrimethoxylsilane-modified nano-La_2O_3

Nano-La2O3 was modified with the vinyltrimethoxylsilane by hydrolysis and a novel poly （vinylidene fluoride-co-hexafluoropropylene） （PVDF-HFP） based composite polymer electrolyte doped with the modified nano-La2O3 was prepared by phase inversion method. The physicochemical properties were studied by SEM, FT-IR, XRD, TG and electrochemical methods. The results of FT-IR indicated that the nano-La2O3 was successfully modified with vinyltrimethoxylsilane. The XRD analysis showed that the incorporation of modified nano-La2O3 into the polymer electrolyte membranes could effectively reduce the crystallinity of PVDF-HFP, and the characterizations also suggested that thermal stability and electrochemical stability window could reach to 382°C and 5.1V, respectively; the reciprocal temperature dependence of ionic conductivity followed Vogel-Tamman-Fulcher （VTF） relation, ionic conductivity at room temperature was up to 3.5×10-3S/cm and lithium ions transference number was up to 0.42; the interfacial resistance increased at initial value about353Ω/cm2 and reached a steady value about 559Ω/cm2 after 5d storage at 30°C. The fabricated Li/As-prepared electrolytes/LiCoO2 coin cell showed excellent rate and cycle performances.

Electrochemical Performance of PEO_(10)LiX-Li_2TiO_3 Composite Polymer Electrolytes

The conductivities of polyethylene oxide (PEO)-based polymer electrolytes (PE) can be improved by the addition of inorganic inert powder. The composite polymer electrolytes (CPE) PEO10LiX (X=4ClO- or 322N(CFSO)-)-Li2TiO3 were prepared by solution casting with inorganic solid electrolyte Li2TiO3 powder as a filler. Results showed that the conductivities of PEO10LiClO4-3wt% Li2TiO3 and PEO10LiN(CF3SO2)2-10wt% Li2TiO3 at 30 ℃ were 8.6×10-6 and 5.6×10-5 S·cm-1, respectively. The conductivities of CPE increased with the decrease of filler抯 particle size. The ionic conduction mechanism analysis showed that there may be three conduction routes in the CPE, i.e., PEO bulk, polymer-filler interface and Li2TiO3 crystal.

Bacterial Cellulose Composite Solid Polymer Electrolyte With High Tensile Strength and Lithium Dendrite Inhibition for Long Life Battery

The development of metallic lithium anode is restrained by lithium dendrite growth during cycling.The solid polymer electrolyte with high mechanical strength and lithium ion conductivity could be applied to inhibit lithium dendrite growth.To prepare the high-performance solid polymer electrolyte,the environment-friendly and cheap bacterial cellulose(BC)is used as filler incorporating with PEO-based electrolyte owing to good mechanical properties and Li salts compatibility.PEO/Li TFSI/BC composite solid polymer electrolytes(CSPE)are prepared easily by aqueous mixing in water.The lithium ion transference number of PEO/Li TFSI/BC CSPE is 0.57,which is higher than PEO/Li TFSI solid polymer electrolyte(SPE)(0.409).The PEO/Li TFSI/BC CSPE exhibits larger tensile strength(4.43 MPa)than PEO/Li TFSI SPE(1.34 MPa).The electrochemical window of composite electrolyte is widened 1.43 V by adding BC.Density functional theory calculations indicate that flex of PEO chains around Li atoms is suppressed,suggesting the enhanced lithium ion conductivity.Frontier molecular orbitals results suggest that an unfavorable intermolecular charge transfer lead to achieve higher potential for BC composite electrolyte.All solid-state Li metal battery with PEO/Li TFSI/BC CSPE delivers longer cycle life for 600 cycles than PEO/Li TFSI SPE battery(50 cycles).Li symmetrical battery using PEO/Li TFSI/BC CSPE could be stable for 1160 h.

The critical role of inorganic nanofillers in solid polymer composite electrolyte for Li+transportation

Compared with commercial lithium batteries with liquid electrolytes,all-solidstate lithium batteries(ASSLBs)possess the advantages of higher safety,better electrochemical stability,higher energy density,and longer cycle life;therefore,ASSLBs have been identified as promising candidates for next-generation safe and stable high-energy-storage devices.The design and fabrication of solid-state electrolytes(SSEs)are vital for the future commercialization of ASSLBs.Among various SSEs,solid polymer composite electrolytes(SPCEs)consisting of inorganic nanofillers and polymer matrix have shown great application prospects in the practice of ASSLBs.The incorporation of inorganic nanofillers into the polymer matrix has been considered as a crucial method to achieve high ionic conductivity for SPCE.In this review,the mechanisms of Li+transport variation caused by incorporating inorganic nanofillers into the polymer matrix are discussed in detail.On the basis of the recent progress,the respective contributions of polymer chains,passive ceramic nanofillers,and active ceramic nanofillers in affecting the Li+transport process of SPCE are reviewed systematically.The inherent relationship between the morphological characteristics of inorganic nanofillers and the ionic conductivity of the resultant SPCE is discussed.Finally,the challenges and future perspectives for developing high-performance SPCE are put forward.This review aims to provide possible strategies for the further improvement of ionic conductivity in inorganic nanoscale filler-reinforced SPCE and highlight their inspiration for future research directions.

Ameliorating the interfacial issues of all-solid-state lithium metal batteries by constructing polymer/inorganic composite electrolyte

Lithium metal is one of the most promising anodes for next-generation batteries due to its high capacity and low reduction potential.However,the notorious Li dendrites can cause the short life span and safety issues,hindering the extensive application of lithium batteries.Herein,Li_(7)La_(3)Zr_(2)O_(12)(LLZO)ceramics are integrated into polyethylene oxide(PEO)to construct a facile polymer/inorganic composite solid-state electrolyte(CSSE)to inhibit the growth of Li dendrites and widen the electrochemical stability window.Given the feasibility of our strategy,the designed PEO-LLZO-LiTFSI composite solid-state electrolyte(PLLCSSE)exhibits an outstanding cycling property of 134.2 mAh g^(-1) after 500 cycles and the Coulombic efficiency of 99.1%after 1000 cycles at 1 C in LiFePO_(4)-Li cell.When cooperated with LiNi_(0.6)Co_(0.2)Mn_(0.2)O_(2)(NCM622)cathode,the PLL-CSSE renders a capacity retention of 82.4%after 200 cycles at 0.2 C.More importantly,the uniform dispersion of LLZO in PEO matrix is tentative tested via Raman and FT-IR spectra and should be responsible for the improved electrochemical performance.The same conclusion can be drawn from the interface investigation after cycling.This work presents an intriguing solid-state electrolyte with high electrochemical performance,which will boost the development of all-solid-state lithium batteries with high energy density.

Synthesis and characterization of mixing soft-segmented waterborne polyurethane polymer electrolyte with room temperature ionic liquid

Composite polymer electrolytes based on mixing soft-segment waterborne polyurethane （WPU） and 1-butyl-3-methylimidazolium bis[（trifluoromethyl）sulfonyl]imide （BMImTFSI） have been prepared and characterized. The addition of BMImTFSI results in an increase of the ionic conductivity. At high BMImTFSI concentration （BMImTFSI/WPU = 3 in weight ratio）, the ionic conductivity reaches 4.27 × 10^-3 S/cm at 30 ℃. These composite polymer electrolytes exhibit good thermal and electrochemical stability, which are high enough to be applied in lithium batteries.

Comprehensively-modified polymer electrolyte membranes with multifunctional PMIA for highly-stable all-solid-state lithium-ion batteries

Polyethylene oxide(PEO)-based electrolytes have obvious merits such as strong ability to dissolve salts(e.g.,LiTFSI)and high flexibility,but their applications in solid-state batteries is hindered by the low ion conductance and poor mechanical and thermal properties.Herein,poly(m-phenylene isophthalamide)(PMIA)is employed as a multifunctional additive to improve the overall properties of the PEO-based electrolytes.The hydrogen-bond interactions between PMIA and PEO/TFSI-can effectively prevent the PEO crystallization and meanwhile facilitate the LiTFSI dissociation,and thus greatly improve the ionic conductivity(two times that of the pristine electrolyte at room temperature).With the incorporation of the high-strength PMIA with tough amide-benzene backbones,the PMIA/PEO-LiTFSI composite polymer electrolyte(CPE)membranes also show much higher mechanical strength(2.96 MPa),thermostability(4190℃)and interfacial stability against Li dendrites(468 h at 0.10 mA cm-2)than the pristine electrolyte(0.32 MPa,364℃and short circuit after 246 h).Furthermore,the CPE-based LiFePO4/Li cells exhibit superior cycling stability(137 mAh g^-1 with 93%retention after 100 cycles at 0.5 C)and rate performance(123 mAh g^-1 at 1.0 C).This work provides a novel and effective CPE structure design strategy to achieve comprehensively-upgraded electrolytes for promising solid-state battery applications.

A cerium-doped NASICON chemically coupled poly(vinylidene fluoride-hexafluoropropylene)-based polymer electrolyte for high-rate and high-voltage quasi-solid-state lithium metal batteries

The isolated inorganic particles within composite polymer electrolytes(CPEs) are not correlated to the Li^(+)transfer network,resulting in the polymer dominating the low ionic conductivity of CPEs.Therefore,we developed novel quasi-solid-state CPEs of a Ce-doped Na super ion conductors(NASICON)Na_(1.3+x)Al_(0.3)Ce_(x)Ti_(1.7-x)(PO_(4))_(3)(NCATP) chemically coupled poly(vinylidene fluoride-hexafluoropropylene)(PVDF-HFP)/Li-bis(trifluoromethanes-ulfonyl)imide(LiTFSI) matrix.A strong interaction between Ce^(3+)from NCATP and TFSI-anion from the polymer matrix contributes to the fast Li+transportation at the interface.The PVDF-HFP/NCATP CPEs exhibit an ionic conductivity of 2.16 × 0^(-3) S cm^(-1) and a Li^(+) transference number of 0.88.A symmetric Li/Li cell with NCATP-integrated CPEs at 0.1 mA cm^(-2) presents outstanding cycling stability over 2000 h at 25℃.The quasi-solid-state Li metal batteries of Li/CPEs/LiFePO_(4) at 2 C after 400 cycles and Li/CPEs/LiCoO_(2) at 0.2 C after 120 cycles deliver capacities of 100 and 152 mAh g^(-1) at 25℃,respectively.

SiO_(2) nanofiber composite gel polymer electrolyte by in-situ polymerization for stable Li metal batteries

Gel polymer electrolytes(GPEs) are promising alternatives to liquid electrolytes applied in high-energydensity batteries.Here superior SiO_(2) nanofiber composite gel polymer electrolytes(SNCGPEs) are developed via in-situ ionic ring-opening polymerization of 1,3-dioxolane(DOL) monomers in SiO_(2) nanofiber membrane(PDOL-SiO_(2)) for lithium metal batteries.The oxygen atoms of PDOL together with Si-O of SiO_(2) construct a more efficient channel for Li^(+) migration.Consequently,the lithium ion transference number(t_(Li^(+)) and ionic conductivity(σ) at 30℃ of PDOL-SiO_(2) are 0.80 and 1.68×10^(-4)S/cm separately.PDOL-SiO_(2) manifests the electrochemical decomposition potentials of 4.90 V.At 0.5 mA/cm^(2),Li|PDOL-SiO_(2) |Li cell shows a steady cycling performance for nearly 1400 h.LFP|PDOL-SiO_(2) |Li battery can steadily cycle at 0.5 C with a capacity retention rate of 89% after 200 cycles.While cycling at 2 C,the capacity retention rate can maintain at 78% after 300 cycles.This contribution provides a innovative strategy for accelerating Li^(+)transportation via designing PDOL molecular chains throughout the SiO_(2) nanofiber framework,which is crucial for high-energy-density LMBs.

Recent research progress on quasi-solid-state electrolytes for dye-sensitized solar cells

Dye-sensitized solar cells （DSSCs） are the most promising, low cost and most extensively investigated solar cells. They are famous for their clean and efficient solar energy conversion. Nevertheless this, long-time sta- bility is still to be acquired. In recent years research on solid and quasi-solid state electrolytes is extensively in- creased. Various quasi-solid electrolytes, including composites polymer electrolytes, ionic liquid electrolytes, thermoplastic polymer electrolytes and thermosetting polymer electrolytes have been used. Performance and stability of a quasi-solid state electrolyte are between liquid and solid electrolytes. High photovoltaic performances of QS-DSSCs along better long-term stability can be obtained by designing and optimizing quasi-solid electrolytes. It is a prospective candidate for highly efficient and stable DSSCs.

A flexible solid polymer electrolyte enabled with lithiated zeolite for high performance lithium battery

Solid-state lithium batteries using composite polymer electrolytes(CPEs)have attracted much attention owing to their higher safety compared to liquid electrolytes and flexibility compared to ceramic electrolytes.However,their unsatisfactory lithium-ion conductivity still limits their development.Herein,a high ion conductive CPE with multiple continuous lithium pathways is designed.This new electrolyte consists of poly(vinylidene fluorideco-hexafluoropropylene)(PVDF-HFP)and lithiated X type zeolite(Li-X),which possesses a high ionic conductivity(1.98×10^(-4)S/cm),high lithium transference number(t_(Li^(+))=0.55),wide electrochemical window(4.7 V),and excellent stability against the lithium anode.Density functional theory(DFT)calculation confirms that the Lewis acid sites in zeolite can graft with N,N-dimethylformamide(DMF)and PVDF-HFP chains,resulting in decreased crystallinity of polymer and providing rapid Li+transmission channels.When used in a full cell,the solid Li|Li-X-3%|LiFePO_(4) cell displays excellent cycling stability and rate performance at room temperature and 60℃.Furthermore,pouch cells with the Li-X-3%electrolyte exhibit brilliant safety under extreme conditions,such as folding and cutting.Thus,this proposed zeolite-PVDF-HFP CPE represents a promising potential in the application of making a safer,higher performing,and flexible solid-state lithium battery.

A nano fiber–gel composite electrolyte with high Li^(+) transference number for application in quasi-solid batteries

As their Liþtransference number(tLiþ),ionic conductivity,and safety are all high,polymer electrolytes play a vital role in overcoming uncontrollable lithium dendrites and low energy density in Li metal batteries(LMBs).We therefore synthesized a three-dimensional(3D)semi-interpenetrating network-based single-ion-conducting fiber–gel composite polymer electrolyte(FGCPE)via an electrospinning,initiation,and in situ polymerization method.The FGCPE provides high ionic conductivity(1.36 mS cm^(-1)),high t_(Li+)(0.92),and a high electrochemical stability window(up to 4.84 V).More importantly,the aromatic heterocyclic structure of the biphenyl in the nanofiber membrane promotes the carbonization of the system(the limiting oxygen index value of the nanofiber membrane reaches 41%),giving it certain flame-retardant properties and solving the source-material safety issue.Due to the in situ method,the observable physical interface between electrodes and electrolytes is virtually eliminated,yielding a compact whole that facilitates rapid kinetic reactions in the cell.More excitingly,the LFP/FGCPE/Li cell displays outstanding cycling stability,with a capacity retention of 91.6%for 500 cycles even at 10C.We also test the FGCPE in high-voltage NMC532/FGCPE/Li cells and pouch cells.This newly designed FGCPE exhibits superior potential and feasibility for promoting the development of LMBs with high energy density and safety.

Recent progress of composite solid polymer electrolytes for all-solid-state lithium metal batteries

In comparison with lithium-ion batteries(LIBs)with liquid electrolytes,all-solid-state lithium batteries(ASSLBs)have been considered as promising systems for future energy storage due to their safety and high energy density.As the pivotal component used in ASSLBs,composite solid polymer electrolytes(CSPEs),derived from the incorporation of inorganic fillers into solid polymer electrolytes(SPEs),exhibit higher ionic conductivity,better mechanical strength,and superior thermal/electrochemical stability compared to the single-component SPEs,which can significantly promote the electrochemical performance of ASSLBs.Herein,the recent advances of CSPEs applied in ASSLBs are presented.The effects of the category,morphology and concentration of inorganic fillers on the ionic conductivity,mechanical strength,electrochemical window,interfacial stability and possible Li+transfer mechanism of CSPEs will be systematically discussed.Finally,the challenges and perspectives are proposed for the future development of high-performance CSPEs and ASSLBs.