2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems...2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems,critical challenges such as interfacial resistance,limited ion transport,dendrite growth,and mechanical degradation hinder their widespread adoption.This review aims to provide a comprehensive analysis of the roles and fu nctions of Ti_(3)C_(2)T_(x) MXenes in SSBs,emphasizing their application as interlayers,anode/cathode additives,and current collectors,and highlighting their impact on interracial stability,ionic/electro nic transport,electrochemical performance,and cycling durability in SSB architectures.Unlike other 2D materials,Ti_(3)C_(2)T_(x) exhibits outsta nding metallic conductivity,tu nable surface terminations,hydrophilicity,and excellent mechanical flexibility,making it ideal for multifu nctional integration in SSBs,As a component in solid-state electrolytes(SSEs),Ti_(3)C_(2)T_(x) improves ionic conductivity and mecha nical strength.When used in electrodes,it serves as a conductive scaffold that enhances charge transport and structural durability.Additionally,its role as an interfacial interlayer effectively reduces interfacial impedance,accommodates volume changes,and suppresses dendrite formation.Its lightweight and high conductivity enable its use as a current collector.This review highlights recent advances in Ti_(3)C_(2)T_(x)-based components for SSBs like Li-,Na-,Zn,Li-S,etc.,emphasizing enha ncements in ion/electron transport,interfacial stability,and structural robustness.Finally,the review outlines challenges and opportunities along with a future outlook focused on improving the MXene oxidation,tailoring surface terminations,improving long-term stability,and exploring scalable fabrication strategies for MXene-based SSB components.展开更多
Micro silicon(mSi)is a promising anode candidate for all-solid-state batteries due to its high specific capacity,low side reactions,and high tap density.However,silicon suffers from its poor electronic and ionic condu...Micro silicon(mSi)is a promising anode candidate for all-solid-state batteries due to its high specific capacity,low side reactions,and high tap density.However,silicon suffers from its poor electronic and ionic conductivity,which is particularly severe on a micro scale and in solid-state systems,leading to increased polarization and inferior electrochemical performance.Doping can broaden the transmission pathways and reduce the diffusion energy barrier for electrons and lithium ions.However,achieving effective,uniform doping in mSi is challenging due to its longer diffusion paths and higher energy barriers.Therefore,current doping research is primarily limited to nanosilicon.In this study,we successfully used a Joule-heating activated staged thermal treatment to achieve full-depth doping of germanium(Ge)in the mSi substrate.The Joule-heating process activated the mSi substrate,resulting in abundant vacancy defects that reduced the diffusion barrier of Ge into the silicon lattice and facilitated full-depth Ge doping.Surprisingly,the resulting Si-Ge anode exhibited significantly enhanced electrical conductivity(70 times).Meanwhile,the improved Li-ion conductivity in mSi and the reduced Young’s modulus enhance the electrode reaction kinetics and integrity after cycling.Ge-doped silicon anodes demonstrate excellent electrochemical performance when applied in sulfide solid-state half-cells and full-cells.This work provides substantial insights into the rational structural design of mSi alloyed anode materials,paving the way for the development of high-performance solid-state Li-ion batteries.展开更多
The application of polymer electrolytes is expected to revitalize solidstate lithium metal batteries(SSLMBs)with high energy density and enhanced safety.However,practical deployment faces challenges from inadequate me...The application of polymer electrolytes is expected to revitalize solidstate lithium metal batteries(SSLMBs)with high energy density and enhanced safety.However,practical deployment faces challenges from inadequate mechanical properties of electrolyte and unstable interfaces in high-voltage SSLMB s.Herein,we design an asymmetric composite solid-state electrolyte(ACSE)composed of a cellulose framework in situ self-assembled with zeolitic imidazolate framework nanosheets(CP@MOF)embedded in a polymer matrix.The CP@MOF network provides the electrolyte with an elastic modulus of 1.19 GPa,effectively resisting Li dendrite penetration.Furthermore,theoretical calculations guided the compositional design of ACSE to address asynchronous interfacial requirements at cathode/electrolyte and anode/electrolyte interfaces,facilitating stable interphase formation and thus ensuring prolonged cycling of SSLMBs.Consequently,Li symmetric cells achieve extended cycling stability(>5000 h)with minimal polarization.The NCM811|Li full cell maintains 84.9%capacity retention after 350 cycles.Notably,assembled NCM811 pouch cells deliver practical energy densities of 337.9 Wh kg^(-1)and 711.7 Wh L^(-1),demonstrating exceptional application potential.This work provides novel insights into the application of ACSEs for high-energy-density SSLMBs.展开更多
All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lit...All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.展开更多
Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantia...Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.展开更多
[Background]Surfactin is a biosurfactant with remarkable surface/interfacial activity.Surfactin production suffers from high costs of carbon sources and severe foaming problem during fermentation.Unreasonable utilizat...[Background]Surfactin is a biosurfactant with remarkable surface/interfacial activity.Surfactin production suffers from high costs of carbon sources and severe foaming problem during fermentation.Unreasonable utilization of soybean residue(okara)can cause resource waste and environmental pollution.[Objective]To achieve sustainable production of surfactin and valueadded conversion of okara,we explored foam-free production of surfactin by Bacillus subtilis using okara as a low-cost substrate and evaluated its application prospects.[Methods]We evaluated and compared the feasibility of B.subtilis utilizing okara to synthesize surfactin through liquid and solid-state fermentation methods.Biosurfactants were extracted from solid-state culture via a weak alkaline water extraction method.The products were identified by HPLC-MS,and the physicochemical properties of the produced surfactin were analyzed.The solid-state medium for fermentation of okara was optimized by the response surface method.The viable count of B.subtilis in solid-state fermentation residue was determined by the plate colony counting method.[Results]The conversion rates of okara to surfactin were 0.6%−0.8%and 1.2%−1.5%in liquid and solid-state fermentation,respectively.Interestingly,solid-state fermentation of okara by B.subtilis achieved both high-yield and foam-free production of surfactin.Five surfactin homologues were produced from okara,mainly including surfactin-C13(34.16%),surfactin-C_(14)(23.95%),and surfactin-C_(15)(35.14%).The produced surfactin,with a critical micelle concentration of 35.0 mg/L,decreased water surface tension to(26.0±0.1)mN/m and emulsified crude oil with emulsifying activity index(EI24)(73.1±3.2)%.It was stable at 4−121℃,pH 5.0−11.0,and NaCl<150 g/L.Okara,NH_(4)Cl,and CaCl_(2)·2H_(2)O were significant components in the solid-state medium.The surfactin yield was increased by 52.1%through solid-state medium optimization.Adding wheat straw further enhanced surfactin production by improving aeration in the solid-state medium.B.subtilis AnPL-1 produced(263.2±7.8)mg surfactin in the optimized solid-state medium containing 14.8 g okara and 1.5 g wheat straw.The conversion rate of okara to surfactin was enhanced to 1.8%.In addition,the residue of solid-state fermentation was expected to be microbial fertilizer since it contained 4.27×10^(10)CFU/g of B.subtilis.[Conclusion]This study established a promising way for foam-free production of surfactin and value-added conversion of okara.展开更多
In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of...In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).展开更多
Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes.Here,we present a...Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes.Here,we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions,which self-assemble into flower-like spherulites with radially aligned lamellar crystals.This unique structure creates continuous Li^(+)transport highways through densely packed crystalline domains,achieving a record-high ionic conductivity of 1.70×10^(-4) S/cm at 25℃ for pristine PEO-based systems.Strategic incorporation of lithium montmorillonite(MMTli,10 wt%)further optimizes the composite electrolyte,balancing high ionic conductivity(1.47×10^(-4) S/cm)with enhanced electrochemical stability(4.99 V vs.Li^(+)/Li),elevated Li^(+)transference number(0.62),and mechanical robustness.The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO_(4)||Li solid-state batteries with 82%capacity retention after 200 cycles at 0.2 C under ambient conditions.This work pioneers a scalable processing paradigm for crystalline polymer electrolytes,offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.展开更多
Thermoplastic polyurethane(TPU)consists of a hardsegment and a soft segment,where the former affords mechanical strength and thermalstability,while the latter provides a possibility of good ionic conductivity by promo...Thermoplastic polyurethane(TPU)consists of a hardsegment and a soft segment,where the former affords mechanical strength and thermalstability,while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt.Thus,TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries.However,the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains,which greatly reduces the dissociation of lithium salts.Herein,a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate)(PEGDA)in fully dispersed TPU.Hence a stretchable solid-state electrolyte(denoted as TELL and the contrast sample was denoted as TLL)with high ionic conductivity of 7.18×10^(-4) S/cm was obtained at room temperature.The Li^(+)transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm^(2),while the contrast sample is short-circuited after 634 h of cycling.The LiFePO_(4)|TELL|Li cell achieves a capacity retention of 78.93%after 200 cycles at 2 C.The LiFePO_(4)|TLL| Li cellonly gains the capacity retention of 51.9%after 50 cyclesat the same current density.So,the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.展开更多
Li_(7)La_(3)Zr_(2)O_(12)-based electrolytes have got great promise for solid-state lithium(Li)metal batteries because of their high elastic modulus and wide electrochemical stability window.However,the insufficient co...Li_(7)La_(3)Zr_(2)O_(12)-based electrolytes have got great promise for solid-state lithium(Li)metal batteries because of their high elastic modulus and wide electrochemical stability window.However,the insufficient contact and heterogeneous Li deposition severely hinder their practical applications.Here,a flexible ternary polymethacrylate(PMA)matrix is designed to incorporate with Ta-doped Li_(7)La_(3)Zr_(2)O_(12)(LLZTO-PMA).The PMA matrix ensures excellent interfacial contact,while the synergistic effects of its polar carbonyl groups and its interaction with LLZTO creating fast interfacial Li^(+)pathways yield a high ionic conductivity of 0.266 mS cm^(-1)at 20℃.Moreover,the interaction between LLZTO and PMA matrix further guides the formation of a hybrid LiF/Li_(3)N-rich solid electrolyte interphase,which allows a fast Li^(+)interfacial kinetic due to its lowered Li^(+)diffusion barrier.Consequently,the LLZTO-PMA electrolyte contributes an ultra-stable Li anode interphase,attaining a lifespan exceeding 10,000 h in symmetric cells and retaining over 96%capacity after 600 cycles in full battery,demonstrating a breakthrough for high-performance solid-state batteries.展开更多
Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth ...Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.展开更多
Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies ...Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes.Among various solid-state electrolytes,solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes.In particular,Li1_(+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix.These systems also demonstrate robust mechanical properties and excellent electrode contact.While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications,this review provides a concise overview of the Li^(+)transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity.It highlights several modification approaches,including the use of fillers,additives,and LATP coatings,which markedly influence the performance of composite polymer electrolytes across different polymer matrices.Finally,the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.展开更多
With the widespread adoption of lithium-ion batteries(LIBs),safety concerns associated with flammable organic elec-trolytes have become increasingly critical.Solid-state lithium batteries(SSLBs),with enhanced safety a...With the widespread adoption of lithium-ion batteries(LIBs),safety concerns associated with flammable organic elec-trolytes have become increasingly critical.Solid-state lithium batteries(SSLBs),with enhanced safety and higher energy density potential,are regarded as a promising next-generation energy storage technology.However,the practical appli-cation of solid-state electrolytes(SSEs)remains hindered by several challenges,including low Li^(+)ion conductivity,poor interfacial compatibility with electrodes,unfavorable mechanical properties and difficulties in scalable manufacturing.This review systematically examines recent progress in SSEs,including inorganic types(oxides,sulfides,halides),organic types(polymers,plastic crystals,poly(ionic liquids)(PILs)),and the emerging class of soft solid-state electrolytes(S3Es),especially those based on“rigid-flexible synergy”composites and“Li+-desolvation”mechanism using porous frameworks.Critical assessment reveals that single-component SSEs face inherent limitations that are difficult to be fully overcome through compositional and structural modification alone.In contrast,S3Es integrate the strength of complementary components to achieve a balanced and synergic enhancement in electrochemical properties(e.g.,ionic conductivity and stability window),mechanical integrity,and processability,showing great promise as next-generation SSEs.Furthermore,the application-ori-ented challenges and emerging trends in S3E research are outlined,aiming to provide strategic insights into future develop-ment of high-performance SSEs.展开更多
This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature&l...This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.展开更多
Solid-state lithium batteries have become a research hotspot in the field of large-scale energy storage due to their excellent safety performance.The development of high-voltage positive electrode materials matched wi...Solid-state lithium batteries have become a research hotspot in the field of large-scale energy storage due to their excellent safety performance.The development of high-voltage positive electrode materials matched with lithium metal anode have advanced the energy density of solid-state lithium batteries close to or even exceeding that of lithium batteries based on a liquid electrolyte,which is expected to be commercialized in the future.However,in high voltage conditions(>4.3 V),the decomposition of electrolyte components,structural degradation,and interface side reactions significantly reduce battery performance and hinder its further development.This review summarizes the latest research progress of inorganic electrolytes,polymer electrolytes,and composite electrolytes in high-voltage solid-state lithium batteries.At the same time,the designs of high-voltage polymer gel electrolyte and high-voltage quasi solid-state electrolyte are introduced in detail.In addition,interface engineering is crucial for improving the overall performance of high-voltage solid-state batteries.Finally,we highlight the challenges faced by high-voltage solid-state lithium batteries and put forward our own views on future research directions.This review offers instructive insights into the advancement of high-voltage solid-state lithium batteries for large-scale energy storage applications.展开更多
Composite polymer electrolytes(CPEs)are considered as promising electrolytes for next-generation lithium batteries due to their superior advantages in safety,mechanical stability/flexibility,cathode compatibility,etc....Composite polymer electrolytes(CPEs)are considered as promising electrolytes for next-generation lithium batteries due to their superior advantages in safety,mechanical stability/flexibility,cathode compatibility,etc.However,achieving high Li+conductivity remains a major challenge,particularly at low temperatures.A key obstacle lies in the limited understanding of the complex interplay among amorphous components,including fillers,plasticizers,and residual solvents,which significantly hampers the rational design of high-performing CPEs.In this contribution,a polyvinylidene fluoride(PVDF)-based composite electrolyte has been developed,exhibiting high room-temperature ionic conductivity/mobility(>1 mS cm^(-1)/0.95×10^(-11)m^(2)s^(-1)),along with excellent electrochemical performances,including a wide stability window(4.8 V vs.Li/Li^(+)),superior charge/discharge capacity,and reversibility.By performing advanced solid-state nuclear magnetic resonance(ssNMR)techniques,in combination with systematic investigations into solid polymer electrolytes(SPEs),gel polymer electrolytes(GPEs),and CPEs,we establish an efficient NMR-based strategy for deconvoluting the structural and dynamic features of complex electrolyte systems.Notably,the simple1H magic-angle spinning(MAS)NMR spectroscopy enables the identification and monitoring of nearly all components in the composite matrix.Motion-sensitive1H-13C and1H-7Li correlation experiments further reveal that the rigidity of PVDF polymer chain segments and the presence of residual solvents are two critical factors governing Li+mobility.Moreover,we demonstrate that the order of the filler and plasticizer addition during the CPE fabrication significantly influences the performance of the electrolyte by regulating the retention of residual solvents.This work not only provides molecular-level insights into the structure-ion mobility relationships in the PVDF-based CPEs but also establishes a general NMR-based characterization approach for investigating other complex composite electrolyte materials.展开更多
The electro-chemo-mechanical mechanism is critical for understanding the initiation and propagation of lithium(Li)dendrites in solid-state lithium metal battery(SSLMB).Li dendrites often nucleate within surface defect...The electro-chemo-mechanical mechanism is critical for understanding the initiation and propagation of lithium(Li)dendrites in solid-state lithium metal battery(SSLMB).Li dendrites often nucleate within surface defects in the solid-state electrolyte,leading to internal short circuits that hinder practical application of SSLMB.While conventional experimental and finite element methods provide valuable insights,they are often costly,time-consuming,and inefficient for capturing the complicated stress evolution inside solid-state electrolyte.In this study,we propose a novel machine learning strategy that integrates prior knowledge and physics-informed constraints to predict the von Mises stress distribution induced by the internal defects of solid-state electrolyte.High-quality training datasets generated using a multiphysics simulation framework and key findings from previous studies were incorporated as physicsguided constraints to enhance prediction reliability and physical consistency of machine learning models.By employing a modified UNet architecture with squeeze-and-excitation module,it demonstrates remarkably high accuracy in stress prediction and exhibits excellent robustness and generalization across a wide range of defect scenarios.This model allows us to efficiently obtain the electro-chemo-mechanical failure of solid-state electrolyte,thereby guiding micro structural modifications and facilitating the design of SSLMB for practical applications.展开更多
Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials ...Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and sustainability.Despite the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing costs.This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in SSLBs.Furthermore,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application.Significantly,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes.Finally,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.展开更多
Halide solid-state electrolytes(HSSEs)with excellent ionic conductivity and high voltage stability are promising for all-solid-state Li-ion batteries(ASSLBs).However,they suffer from poor processability,mechanical dur...Halide solid-state electrolytes(HSSEs)with excellent ionic conductivity and high voltage stability are promising for all-solid-state Li-ion batteries(ASSLBs).However,they suffer from poor processability,mechanical durability and humidity stability,hindering their large-scale applications.Here,we introduce a dry-processing fibrillation strategy using hydrophobic polytetrafluoroethylene(PTFE)binder to encapsulate Li_(3)InCl_(6)(LIC)particles(the most representative HSSE).By manipulating the fibrillating process,only 0.5 wt%PTFE is sufficient to prepare free-standing LIC-PTFE(LIC-P)HSSEs.Additionally,LIC-P demonstrates excellent mechanical durability and humidity resistance.They can maintain their shapes after being exposed to humid atmosphere for 30 min,meanwhile still exhibit high ionic conductivity of>0.2m S/cm at 25℃.Consequently,the LIC-P-based ASSLBs deliver a high specific capacity of 126.6 m Ah/g at0.1 C and long cyclability of 200 cycles at 0.2 C.More importantly,the ASSLBs using moisture-exposed LIC-P can still operate properly by exhibiting a high capacity-retention of 87.7%after 100 cycles under0.2 C.Furthermore,for the first time,we unravel the LIC interfacial morphology evolution upon cycling because the good mechanical durability enables a facile separation of LIC-P from ASSLBs after testing.展开更多
Solid-state batteries have recently raised strong interest in the scientific community as possible advancement of battery technology beyond commercial lithium ion due to the promise of high energy densities and improv...Solid-state batteries have recently raised strong interest in the scientific community as possible advancement of battery technology beyond commercial lithium ion due to the promise of high energy densities and improved safety[1].In the core of development of high-performance solid-state batteries,is the development of solid-state electrolytes,which should be both sufficiently ionically conductive and offer stable interphases with high-energy electrodes,such as alkali metals and silicon[2,3].Recently,potassium-ion batteries have emerged as an alternative to lithium-ion batteries as a remedy to limited resources and uneven distribution of lithium,as well as due to the fact that low standard electrode potentials of K/K^(+) electrodes should lead to high operation voltages,competitive to those observed in commercial lithium batteries[4-6].展开更多
基金supported by a National Research Foundation of Korea(NRF)grant funded by the Korean government(MSIT)(NRF-2020R1A6A1A03043435 and 2020R1A2C1099862)supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(P0012451,The Competency Development Program for Industry Specialist)。
文摘2D MXenes,particularly Ti_(3)C_(2)T_(x),have emerged as promising multifu nctional materials for advancing solidstate batteries(SSBs).While SSBs offer superior safety and energy density over liquid-electrolyte systems,critical challenges such as interfacial resistance,limited ion transport,dendrite growth,and mechanical degradation hinder their widespread adoption.This review aims to provide a comprehensive analysis of the roles and fu nctions of Ti_(3)C_(2)T_(x) MXenes in SSBs,emphasizing their application as interlayers,anode/cathode additives,and current collectors,and highlighting their impact on interracial stability,ionic/electro nic transport,electrochemical performance,and cycling durability in SSB architectures.Unlike other 2D materials,Ti_(3)C_(2)T_(x) exhibits outsta nding metallic conductivity,tu nable surface terminations,hydrophilicity,and excellent mechanical flexibility,making it ideal for multifu nctional integration in SSBs,As a component in solid-state electrolytes(SSEs),Ti_(3)C_(2)T_(x) improves ionic conductivity and mecha nical strength.When used in electrodes,it serves as a conductive scaffold that enhances charge transport and structural durability.Additionally,its role as an interfacial interlayer effectively reduces interfacial impedance,accommodates volume changes,and suppresses dendrite formation.Its lightweight and high conductivity enable its use as a current collector.This review highlights recent advances in Ti_(3)C_(2)T_(x)-based components for SSBs like Li-,Na-,Zn,Li-S,etc.,emphasizing enha ncements in ion/electron transport,interfacial stability,and structural robustness.Finally,the review outlines challenges and opportunities along with a future outlook focused on improving the MXene oxidation,tailoring surface terminations,improving long-term stability,and exploring scalable fabrication strategies for MXene-based SSB components.
基金financially supported by the National Key Research and Development Program(2022YFE0127400)the National Natural Science Foundation of China(52172040,52202041,and U23B2077)+1 种基金Taishan Scholar Project of Shandong Province(tsqn202211086,ts202208832,tsqnz20221118)the Fundamental Research Funds for the Central Universities(23CX06055A).
文摘Micro silicon(mSi)is a promising anode candidate for all-solid-state batteries due to its high specific capacity,low side reactions,and high tap density.However,silicon suffers from its poor electronic and ionic conductivity,which is particularly severe on a micro scale and in solid-state systems,leading to increased polarization and inferior electrochemical performance.Doping can broaden the transmission pathways and reduce the diffusion energy barrier for electrons and lithium ions.However,achieving effective,uniform doping in mSi is challenging due to its longer diffusion paths and higher energy barriers.Therefore,current doping research is primarily limited to nanosilicon.In this study,we successfully used a Joule-heating activated staged thermal treatment to achieve full-depth doping of germanium(Ge)in the mSi substrate.The Joule-heating process activated the mSi substrate,resulting in abundant vacancy defects that reduced the diffusion barrier of Ge into the silicon lattice and facilitated full-depth Ge doping.Surprisingly,the resulting Si-Ge anode exhibited significantly enhanced electrical conductivity(70 times).Meanwhile,the improved Li-ion conductivity in mSi and the reduced Young’s modulus enhance the electrode reaction kinetics and integrity after cycling.Ge-doped silicon anodes demonstrate excellent electrochemical performance when applied in sulfide solid-state half-cells and full-cells.This work provides substantial insights into the rational structural design of mSi alloyed anode materials,paving the way for the development of high-performance solid-state Li-ion batteries.
基金the financial support from the National Natural Science Foundation of China(52072307,22408198)the Fundamental Research Funds for the Central Universities(XJJSKYQD202533)。
文摘The application of polymer electrolytes is expected to revitalize solidstate lithium metal batteries(SSLMBs)with high energy density and enhanced safety.However,practical deployment faces challenges from inadequate mechanical properties of electrolyte and unstable interfaces in high-voltage SSLMB s.Herein,we design an asymmetric composite solid-state electrolyte(ACSE)composed of a cellulose framework in situ self-assembled with zeolitic imidazolate framework nanosheets(CP@MOF)embedded in a polymer matrix.The CP@MOF network provides the electrolyte with an elastic modulus of 1.19 GPa,effectively resisting Li dendrite penetration.Furthermore,theoretical calculations guided the compositional design of ACSE to address asynchronous interfacial requirements at cathode/electrolyte and anode/electrolyte interfaces,facilitating stable interphase formation and thus ensuring prolonged cycling of SSLMBs.Consequently,Li symmetric cells achieve extended cycling stability(>5000 h)with minimal polarization.The NCM811|Li full cell maintains 84.9%capacity retention after 350 cycles.Notably,assembled NCM811 pouch cells deliver practical energy densities of 337.9 Wh kg^(-1)and 711.7 Wh L^(-1),demonstrating exceptional application potential.This work provides novel insights into the application of ACSEs for high-energy-density SSLMBs.
文摘All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.
基金National Natural Science Foundation of China,Grant/Award Number:52272225。
文摘Solid-state sodium batteries(SSSBs)have been highly prized as a promising alternative to conventional battery systems using organic liquid electrolytes due to their improved safety,higher energy density,and substantial resources and low cost of sodium.Na_(3)Zr_(2)Si_(2)PO_(12)(NZSP)solid electrolyte is attracting considerable interest owing to its excellent thermal and chemical stability and favorable compatibility with Na metal anode and high-voltage cathode.However,two main challenges of poor roomtemperature ionic conductivity and high interfacial resistance limit the application of NZSP electrolyte in SSSBs.So far,intensive efforts have been devoted to developing modification strategies to improve the room-temperature ionic conductivity of NZSP.This review aims to provide a comprehensive summary and discussion of some optimization strategies for enhancing the room-temperature ionic conductivity of the NZSP solid electrolyte.These optimization strategies are categorized into foreignion doping or substitution,sintering behavior modulation,and regulation of chemical composition based on precursors,and their optimization mechanisms are also elaborated.Finally,the prospects of NZSP-based solid electrolytes are presented.This review is expected to offer better guidance for designing and developing high-performance NZSP-based solid electrolytes for accelerating the practical application of SSSBs.
基金supported by the Research Start-up Foundation for Introduced Talent of Qufu Normal University(609601)。
文摘[Background]Surfactin is a biosurfactant with remarkable surface/interfacial activity.Surfactin production suffers from high costs of carbon sources and severe foaming problem during fermentation.Unreasonable utilization of soybean residue(okara)can cause resource waste and environmental pollution.[Objective]To achieve sustainable production of surfactin and valueadded conversion of okara,we explored foam-free production of surfactin by Bacillus subtilis using okara as a low-cost substrate and evaluated its application prospects.[Methods]We evaluated and compared the feasibility of B.subtilis utilizing okara to synthesize surfactin through liquid and solid-state fermentation methods.Biosurfactants were extracted from solid-state culture via a weak alkaline water extraction method.The products were identified by HPLC-MS,and the physicochemical properties of the produced surfactin were analyzed.The solid-state medium for fermentation of okara was optimized by the response surface method.The viable count of B.subtilis in solid-state fermentation residue was determined by the plate colony counting method.[Results]The conversion rates of okara to surfactin were 0.6%−0.8%and 1.2%−1.5%in liquid and solid-state fermentation,respectively.Interestingly,solid-state fermentation of okara by B.subtilis achieved both high-yield and foam-free production of surfactin.Five surfactin homologues were produced from okara,mainly including surfactin-C13(34.16%),surfactin-C_(14)(23.95%),and surfactin-C_(15)(35.14%).The produced surfactin,with a critical micelle concentration of 35.0 mg/L,decreased water surface tension to(26.0±0.1)mN/m and emulsified crude oil with emulsifying activity index(EI24)(73.1±3.2)%.It was stable at 4−121℃,pH 5.0−11.0,and NaCl<150 g/L.Okara,NH_(4)Cl,and CaCl_(2)·2H_(2)O were significant components in the solid-state medium.The surfactin yield was increased by 52.1%through solid-state medium optimization.Adding wheat straw further enhanced surfactin production by improving aeration in the solid-state medium.B.subtilis AnPL-1 produced(263.2±7.8)mg surfactin in the optimized solid-state medium containing 14.8 g okara and 1.5 g wheat straw.The conversion rate of okara to surfactin was enhanced to 1.8%.In addition,the residue of solid-state fermentation was expected to be microbial fertilizer since it contained 4.27×10^(10)CFU/g of B.subtilis.[Conclusion]This study established a promising way for foam-free production of surfactin and value-added conversion of okara.
基金the National Natural Science Foundation of China (52076076, 52006065)Fundamental Research Funds for Central Universities (2025JC003)Beijing Municipal Natural Science Foundation (3242022)
文摘In the realm of large-scale power system energy storage,sodium-based batteries represent a cost-effective post-lithium energy storage technology,making inorganic solid-state sodium batteries(ISSSB)a critical branch of this development.Inorganic solid-state electrolytes(ISSEs)are the core components of sodium batteries;however,they face significant challenges such as insufficient ionic conductivity,interfacial instability,and dendrite growth,all of which severely hinder practical application.This review critically assesses experimental protocols and theoretical frameworks related to mainstream ISSEs and systematizes optimization strategies aimed at overcoming these challenges.Leveraging integrated insights from both experimental and computational studies,the review first categorizes and summarizes the primary types of ISSEs,namely oxide-,sulfide-,and halide-based electrolytes.It then details interfacial optimization strategies focused on addressing three core interfacial issues:ion transport barriers resulting from mechanical incompatibility,side reactions stemming from electrochemical mismatch,and dendrite formation.Finally,the review advocates prioritizing in-depth research that integrates experimental and theoretical approaches to establish a closed-loop methodology encompassing predictive design,multiscale investigation,mechanistic exploration,and high-throughput automated experimentation,with feedback-driven refinement.This work serves as a comprehensive reference and systematic roadmap for future research on solid-state electrolytes(SSEs).
基金supported by the National Natural Science Foundation of China(No.42272044)the High-performance Computing Platform of China University of Geosciences Beijing。
文摘Polyethylene oxide(PEO)-based solid polymer electrolytes(SPEs)have long faced limitations due to low ionic conductivity at ambient temperature and poor interfacial stability with lithium metal anodes.Here,we present a structural engineering strategy to address these challenges through shear-induced crystallization of concentrated PEO-LiTFSI solutions,which self-assemble into flower-like spherulites with radially aligned lamellar crystals.This unique structure creates continuous Li^(+)transport highways through densely packed crystalline domains,achieving a record-high ionic conductivity of 1.70×10^(-4) S/cm at 25℃ for pristine PEO-based systems.Strategic incorporation of lithium montmorillonite(MMTli,10 wt%)further optimizes the composite electrolyte,balancing high ionic conductivity(1.47×10^(-4) S/cm)with enhanced electrochemical stability(4.99 V vs.Li^(+)/Li),elevated Li^(+)transference number(0.62),and mechanical robustness.The composite electrolyte enables stable Li plating/stripping over 800 h in symmetric Li||Li cells and powers LiFePO_(4)||Li solid-state batteries with 82%capacity retention after 200 cycles at 0.2 C under ambient conditions.This work pioneers a scalable processing paradigm for crystalline polymer electrolytes,offering new insights into ion transport mechanisms and validating clay minerals as multifunctional additives for next-generation energy storage systems.
基金financially supported by the National Natural Science Foundation of China(Nos.52263010 and 52372188)2023 Introduction of studying abroad talent program,Henan Provincial Key Scientific Research Project of Collegesand Universities(No.23A150038)+1 种基金Key Scientific Research Project of Education Department of Henan Province(No.22A150042)the National students'platform for innovation and entrepreneurship training program(No.201910476010).
文摘Thermoplastic polyurethane(TPU)consists of a hardsegment and a soft segment,where the former affords mechanical strength and thermalstability,while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt.Thus,TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries.However,the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains,which greatly reduces the dissociation of lithium salts.Herein,a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate)(PEGDA)in fully dispersed TPU.Hence a stretchable solid-state electrolyte(denoted as TELL and the contrast sample was denoted as TLL)with high ionic conductivity of 7.18×10^(-4) S/cm was obtained at room temperature.The Li^(+)transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm^(2),while the contrast sample is short-circuited after 634 h of cycling.The LiFePO_(4)|TELL|Li cell achieves a capacity retention of 78.93%after 200 cycles at 2 C.The LiFePO_(4)|TLL| Li cellonly gains the capacity retention of 51.9%after 50 cyclesat the same current density.So,the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.
基金supported by the National Natural Science Foundation of China(No.22305106)the Postdoctoral Fellowship Program of CPSF(GZC20230682)Beijing Key Laboratory of High-Entropy Energy materials and Devices,Beijing Institute of Nanoenergy and Nanosystems(No.GS 2025ZD005)。
文摘Li_(7)La_(3)Zr_(2)O_(12)-based electrolytes have got great promise for solid-state lithium(Li)metal batteries because of their high elastic modulus and wide electrochemical stability window.However,the insufficient contact and heterogeneous Li deposition severely hinder their practical applications.Here,a flexible ternary polymethacrylate(PMA)matrix is designed to incorporate with Ta-doped Li_(7)La_(3)Zr_(2)O_(12)(LLZTO-PMA).The PMA matrix ensures excellent interfacial contact,while the synergistic effects of its polar carbonyl groups and its interaction with LLZTO creating fast interfacial Li^(+)pathways yield a high ionic conductivity of 0.266 mS cm^(-1)at 20℃.Moreover,the interaction between LLZTO and PMA matrix further guides the formation of a hybrid LiF/Li_(3)N-rich solid electrolyte interphase,which allows a fast Li^(+)interfacial kinetic due to its lowered Li^(+)diffusion barrier.Consequently,the LLZTO-PMA electrolyte contributes an ultra-stable Li anode interphase,attaining a lifespan exceeding 10,000 h in symmetric cells and retaining over 96%capacity after 600 cycles in full battery,demonstrating a breakthrough for high-performance solid-state batteries.
基金supported by the National Natural Science Foundation of China(Grant Nos.52002094)the Guangdong Basic and Applied Basic Research Foundation(Grant Nos.2025A1515011995)+3 种基金the Shenzhen Science and Technology Innovation Program(GXWD20221030205923001)the Shandong Provincial Natural Science Foundation of China(Grant Nos.ZR2024QE525)the Shenzhen Key Laboratory of New Materials Technology(Grant Nos.SYSPG20241211173609003)the State Key Laboratory of Precision Welding&Joining of Materials and Structures(Grant Nos.2024-Z-17,2024-T-08)。
文摘Sulfide solid electrolytes are considered promising candidates for all-solid-state lithium batteries(ASSLBs)because of their high ionic conductivity and favorable mechanical properties.However,the uncontrolled growth of lithium dendrites at the lithium metal-electrolytes interface remains a major obstacle to their practical application.In this work,we introduced a scalable three-dimensional(3D)Li-B skeleton structure designed to suppress dendrite formation.The alloy anode demonstrates a lower Young's modulus,which helps alleviate the accumulation of localized stresses at the interface.Additionally,the 3D alloy anode provided a uniform potential distribution,which promoted homogeneous lithium deposition.Benefiting from these structural advantages,symmetric cells with the Li-B alloy achieved a high critical current density of 2.8 mA cm^(-2).Notably,Li-B‖LPSCI‖LVO-NCM ASSLBs exhibited long-term cycling stability,retaining 97.8%of their capacity after 1500 cycles at 2 C.Furthermore,ASSLBs incorporating the Li-B alloy showed cycling stability comparable with Li-In-based cells,while delivering a higher energy density.Overall,this work presents a practical strategy that may accelerate the commercialization of sulfide-based ASSLBs.
基金supported by grants from the National Natural Science Foundation of China(Grant Nos.52302303,52472247,52172229,52272201,52072136,51972257)the Natural Science Foundation of Hubei Province(JCZRYB202500537).
文摘Solid-state lithium batteries are considered one of the most promising next-generation energy storage technologies owing to their safety and high energy density.The key to solid-state lithium battery advancement lies in the design and optimization of suitable solid-state electrolytes.Among various solid-state electrolytes,solid-state composite polymer electrolytes offer the combined benefits of solid inorganic electrolytes and solid polymer electrolytes.In particular,Li1_(+x)Al_(x)Ti_(2-x)(PO_(4))_(3)(LATP)/polymer composite polymer electrolytes exhibit high ionic conductivity due to LATP and improved flexibility from the polymer matrix.These systems also demonstrate robust mechanical properties and excellent electrode contact.While recent reviews have primarily focused on the performance of LATP/polymer composite polymer electrolytes and the general effects of composite polymer electrolyte modifications for solid-state lithium battery applications,this review provides a concise overview of the Li^(+)transport mechanisms in LATP/polymer composite polymer electrolytes and strategies to enhance ionic conductivity.It highlights several modification approaches,including the use of fillers,additives,and LATP coatings,which markedly influence the performance of composite polymer electrolytes across different polymer matrices.Finally,the review addresses the challenges of LATP/polymer composite polymer electrolytes and outlines key research directions for developing advanced composite polymer electrolytes for high-performance solid-state lithium batteries.
基金the financial support from the National Key R&D Program of China (Grant No. 2021YFB3800300)the supports from National Key R&D Program of China (Grant No. 2022YFB3807700)+6 种基金the National Natural Science Foundation of China (Grant No. U20A20248)the supports from the National Natural Science Foundation of China (Grant Nos. W2441017, 22409103)the “Innovation Yongjiang 2035” Key R&D Program (Grant Nos. 2024Z040, 2025Z063)the National Key R&D Program of China (Grant No. 2023YFC2812700)the Natural Science Foundation of Shandong Province (Grant No. ZR2024YQ008)funding supports from the National Key R&D Program of China (Grant No. 2021YFB3800300)science and technology innovation fund for emission peak and carbon neutrality of Jiangsu province (Grant Nos. BK20220034, BK20231512)。
文摘With the widespread adoption of lithium-ion batteries(LIBs),safety concerns associated with flammable organic elec-trolytes have become increasingly critical.Solid-state lithium batteries(SSLBs),with enhanced safety and higher energy density potential,are regarded as a promising next-generation energy storage technology.However,the practical appli-cation of solid-state electrolytes(SSEs)remains hindered by several challenges,including low Li^(+)ion conductivity,poor interfacial compatibility with electrodes,unfavorable mechanical properties and difficulties in scalable manufacturing.This review systematically examines recent progress in SSEs,including inorganic types(oxides,sulfides,halides),organic types(polymers,plastic crystals,poly(ionic liquids)(PILs)),and the emerging class of soft solid-state electrolytes(S3Es),especially those based on“rigid-flexible synergy”composites and“Li+-desolvation”mechanism using porous frameworks.Critical assessment reveals that single-component SSEs face inherent limitations that are difficult to be fully overcome through compositional and structural modification alone.In contrast,S3Es integrate the strength of complementary components to achieve a balanced and synergic enhancement in electrochemical properties(e.g.,ionic conductivity and stability window),mechanical integrity,and processability,showing great promise as next-generation SSEs.Furthermore,the application-ori-ented challenges and emerging trends in S3E research are outlined,aiming to provide strategic insights into future develop-ment of high-performance SSEs.
文摘This study shows that sulfide solid-state electrolytes,β-Li_(3)PS_(4)and Li_(6)PS_(5)Cl,are flammable solids.Both solid-state electrolytes release sulfur vapor in a dry,oxidizing environment at elevated temperature<300℃.Sulfur vapor is a highly flammable gas,which then auto-ignites to produce a flame.This behavior suggests that an O_(2)-S gas-gas reaction mechanism may contribute to all-solid-state battery thermal runaway.To improve all-solid-state battery safety,current work focuses on eliminating the O_(2)source by changing the cathode active material.The conclusion of this study suggests that all-solidstate battery safety can also be realized by the development of solid-state electrolytes with less susceptibility to sulfur volatilization.
基金supported by the National Key R&D Program of China(2024YFA1211100)the National Natural Science Foundation of China(52301278,22479080,52202254,92372001,22393900,and 92372203)+2 种基金the Natural Science Foundation of Jiangsu Province(BK20230937,BK20220966)the Science and Technology Plans of Tianjin(23JCYBJC00170,24JCJQJC00220,and 24ZXZSSS00390)the Fundamental Research Funds for the Central Universities(02063253167,30922010708)。
文摘Solid-state lithium batteries have become a research hotspot in the field of large-scale energy storage due to their excellent safety performance.The development of high-voltage positive electrode materials matched with lithium metal anode have advanced the energy density of solid-state lithium batteries close to or even exceeding that of lithium batteries based on a liquid electrolyte,which is expected to be commercialized in the future.However,in high voltage conditions(>4.3 V),the decomposition of electrolyte components,structural degradation,and interface side reactions significantly reduce battery performance and hinder its further development.This review summarizes the latest research progress of inorganic electrolytes,polymer electrolytes,and composite electrolytes in high-voltage solid-state lithium batteries.At the same time,the designs of high-voltage polymer gel electrolyte and high-voltage quasi solid-state electrolyte are introduced in detail.In addition,interface engineering is crucial for improving the overall performance of high-voltage solid-state batteries.Finally,we highlight the challenges faced by high-voltage solid-state lithium batteries and put forward our own views on future research directions.This review offers instructive insights into the advancement of high-voltage solid-state lithium batteries for large-scale energy storage applications.
基金financially supported by the National Natural Science Foundation of China(Grant No.22325405,22432005,22321002,and 22404159)the Dalian Science and Technology Talent Innovation Program(Grant No.2024RG009)+2 种基金the China Postdoctoral Science Foundation(Grant Number 2024M753120)the LiaoNing Revitalization Talents Program(XLYC2203134)the ANSO Scholarship for Young Talents for financial support。
文摘Composite polymer electrolytes(CPEs)are considered as promising electrolytes for next-generation lithium batteries due to their superior advantages in safety,mechanical stability/flexibility,cathode compatibility,etc.However,achieving high Li+conductivity remains a major challenge,particularly at low temperatures.A key obstacle lies in the limited understanding of the complex interplay among amorphous components,including fillers,plasticizers,and residual solvents,which significantly hampers the rational design of high-performing CPEs.In this contribution,a polyvinylidene fluoride(PVDF)-based composite electrolyte has been developed,exhibiting high room-temperature ionic conductivity/mobility(>1 mS cm^(-1)/0.95×10^(-11)m^(2)s^(-1)),along with excellent electrochemical performances,including a wide stability window(4.8 V vs.Li/Li^(+)),superior charge/discharge capacity,and reversibility.By performing advanced solid-state nuclear magnetic resonance(ssNMR)techniques,in combination with systematic investigations into solid polymer electrolytes(SPEs),gel polymer electrolytes(GPEs),and CPEs,we establish an efficient NMR-based strategy for deconvoluting the structural and dynamic features of complex electrolyte systems.Notably,the simple1H magic-angle spinning(MAS)NMR spectroscopy enables the identification and monitoring of nearly all components in the composite matrix.Motion-sensitive1H-13C and1H-7Li correlation experiments further reveal that the rigidity of PVDF polymer chain segments and the presence of residual solvents are two critical factors governing Li+mobility.Moreover,we demonstrate that the order of the filler and plasticizer addition during the CPE fabrication significantly influences the performance of the electrolyte by regulating the retention of residual solvents.This work not only provides molecular-level insights into the structure-ion mobility relationships in the PVDF-based CPEs but also establishes a general NMR-based characterization approach for investigating other complex composite electrolyte materials.
基金financially supported by the National Natural Science Foundation of China(22479067)Yunnan Young Talents Program for“Xingdian Talent Support Plan”(KKXX202551007)。
文摘The electro-chemo-mechanical mechanism is critical for understanding the initiation and propagation of lithium(Li)dendrites in solid-state lithium metal battery(SSLMB).Li dendrites often nucleate within surface defects in the solid-state electrolyte,leading to internal short circuits that hinder practical application of SSLMB.While conventional experimental and finite element methods provide valuable insights,they are often costly,time-consuming,and inefficient for capturing the complicated stress evolution inside solid-state electrolyte.In this study,we propose a novel machine learning strategy that integrates prior knowledge and physics-informed constraints to predict the von Mises stress distribution induced by the internal defects of solid-state electrolyte.High-quality training datasets generated using a multiphysics simulation framework and key findings from previous studies were incorporated as physicsguided constraints to enhance prediction reliability and physical consistency of machine learning models.By employing a modified UNet architecture with squeeze-and-excitation module,it demonstrates remarkably high accuracy in stress prediction and exhibits excellent robustness and generalization across a wide range of defect scenarios.This model allows us to efficiently obtain the electro-chemo-mechanical failure of solid-state electrolyte,thereby guiding micro structural modifications and facilitating the design of SSLMB for practical applications.
基金National Natural Science Foundation of China(22322903,52072061)Natural Science Foundation of Sichuan,China(2023NSFSC1914)Beijing National Laboratory for Condensed Matter Physics(2023BNLCMPKF015)。
文摘Solid-state lithium batteries(SSLBs)are regarded as an essential growth path in energy storage systems due to their excellent safety and high energy density.In particular,SSLBs using conversion-type cathode materials have received widespread attention because of their high theoretical energy densities,low cost,and sustainability.Despite the great progress in research and development of SSLBs based on conversiontype cathodes,their practical applications still face challenges such as blocked ionic-electronic migration pathways,huge volume change,interfacial incompatibility,and expensive processing costs.This review focuses on the advantages and critical issues of coupling conversion-type cathodes with solid-state electrolytes(SSEs),as well as state-of-the-art progress in various promising cathodes(e.g.,FeS_(2),CuS,FeF_(3),FeF_(2),and S)in SSLBs.Furthermore,representative research on conversion-type solid-state full cells is discussed to offer enlightenment for their practical application.Significantly,the energy density exhibited by the S cathode stands out impressively,while sulfide SSEs and halide SSEs have demonstrated immense potential for coupling with conversion-type cathodes.Finally,perspectives on conversion-type cathodes are provided at the material,interface,composite electrode,and battery levels,with a view to accelerating the development of conversion-type cathodes for high-energy–density SSLBs.
基金supported by the 261 Project of MIITthe National Natural Science Foundation of China(Nos.52250010,52201242,U23A20574)the Young Elite Scientists Sponsorship Program by CAST(No.2021QNRC001)。
文摘Halide solid-state electrolytes(HSSEs)with excellent ionic conductivity and high voltage stability are promising for all-solid-state Li-ion batteries(ASSLBs).However,they suffer from poor processability,mechanical durability and humidity stability,hindering their large-scale applications.Here,we introduce a dry-processing fibrillation strategy using hydrophobic polytetrafluoroethylene(PTFE)binder to encapsulate Li_(3)InCl_(6)(LIC)particles(the most representative HSSE).By manipulating the fibrillating process,only 0.5 wt%PTFE is sufficient to prepare free-standing LIC-PTFE(LIC-P)HSSEs.Additionally,LIC-P demonstrates excellent mechanical durability and humidity resistance.They can maintain their shapes after being exposed to humid atmosphere for 30 min,meanwhile still exhibit high ionic conductivity of>0.2m S/cm at 25℃.Consequently,the LIC-P-based ASSLBs deliver a high specific capacity of 126.6 m Ah/g at0.1 C and long cyclability of 200 cycles at 0.2 C.More importantly,the ASSLBs using moisture-exposed LIC-P can still operate properly by exhibiting a high capacity-retention of 87.7%after 100 cycles under0.2 C.Furthermore,for the first time,we unravel the LIC interfacial morphology evolution upon cycling because the good mechanical durability enables a facile separation of LIC-P from ASSLBs after testing.
文摘Solid-state batteries have recently raised strong interest in the scientific community as possible advancement of battery technology beyond commercial lithium ion due to the promise of high energy densities and improved safety[1].In the core of development of high-performance solid-state batteries,is the development of solid-state electrolytes,which should be both sufficiently ionically conductive and offer stable interphases with high-energy electrodes,such as alkali metals and silicon[2,3].Recently,potassium-ion batteries have emerged as an alternative to lithium-ion batteries as a remedy to limited resources and uneven distribution of lithium,as well as due to the fact that low standard electrode potentials of K/K^(+) electrodes should lead to high operation voltages,competitive to those observed in commercial lithium batteries[4-6].
