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
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
In recent years,due to the increasing demand for portable electronic devices,rechargeable solid-state battery technology has developed rapidly.Lithium-ion batteries are the systems of choice,offering high energy densi...In recent years,due to the increasing demand for portable electronic devices,rechargeable solid-state battery technology has developed rapidly.Lithium-ion batteries are the systems of choice,offering high energy density,flexible and lightweight design,and longer lifespan than comparable battery technologies.Therefore,a better understanding of the relationship between electrochemical mechanism and structural properties from theory and experiment will enable us to accelerate the development of high-performance and security batteries.This review discusses the interplay between theoretical calculation and experiment in the study of lithium ion battery materials.We introduce the application of theoretical calculation method in solid-state batteries through the combination of theory and experiment.We present the concept and assembly technology of solid-state batteries are reviewed.The basic parameters of solid-state electrolytes,especially sulfide-based solid-state electrolytes and their interface mechanisms with high-voltage cathode materials,are analyzed by theoretical methods.We present an overview on the scientific challenges,fundamental mechanisms,and design strategies for solid-state batteries,especially focusing on the issues of stability on solid-state electrolytes and the associated interfaces with both cathode and electrolyte.Owing to the theoretical models,we can not only reveal the unprecedented mechanism from the atomic scale,but also analyze the interface problems in the battery thoroughly,thus effectively designing more promising electrolyte and interface coating materials.It blazed a new trial for engineering an interphase with improved interfacial compatibility for a long-term cyclability.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
Severe structural fractures and persistent side reactions at the interface with liquid electrolytes have hindered the commercialization of silicon(Si)anodes.Solid-state electrolytes present a promising solution to add...Severe structural fractures and persistent side reactions at the interface with liquid electrolytes have hindered the commercialization of silicon(Si)anodes.Solid-state electrolytes present a promising solution to address these issues.However,the high interfacial resistance of rigid ceramic electrolytes and the limited ionic conductivity of polymer electrolytes remain significant challenges,further complicated by the substantial volume expansion of Si.In this work,we chemically grafted a flame-retardant,self-healing polyurethane-thiourea polymer onto Li_(7)P_(3)S_(11)(SHPUSB-40%LPS)via nucleophilic addition,creating an electrolyte with exceptional ionic conductivity,high elasticity,and strong compatibility with Si anodes.We observed that FSI^(-)was strongly adsorbed onto the LPS surface through electrostatic interactions with sulfur vacancies,enhancing Li^(+)transport.Furthermore,SHPUSB-40%LPS exhibits dynamic covalent disulfide bonds and hydrogen bonds,enabling self-assembly of the electrolyte at the interface.This dynamic bonding provides a self-healing mechanism that mitigates structural changes during Si expansion and contraction cycles.As a result,the Si anode with SHPUSB-40%LPS presents excellent cycling stability,retaining nearly 53.5%of its capacity after 300 cycles.The practical applicability of this design was validated in a 2 Ah all-solid-state Si‖LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)pouch cell,which maintained a stable Li-ion storage capacity retention of 76.3%after 350cycles at 0.5C.This novel solid-state electrolyte with selfhealing properties offers a promising strategy to address fundamental interfacial and performance challenges associated with Si anodes.展开更多
The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength,ionic conductivity,and thickness.Here,we propose Al_(2)O_(3)-coated polyimide(AO/PI)porous film as ...The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength,ionic conductivity,and thickness.Here,we propose Al_(2)O_(3)-coated polyimide(AO/PI)porous film as a high-strength substrate to support fast-ion-conducting polymer-in-salt(PIS)solid-state electrolytes,aiming to suppress lithium dendrite growth and improve full-cell performance.The Al_(2)O_(3)coating layer not only refines the wettability of polyimide porous film to PIS,but also performs as a high modulus protective layer to suppress the growth of lithium dendrites.The resulting PI/AO@PIS exhibits a small thickness of only 35μm with an outstanding tensile strength of 11.3 MPa and Young's modulus of 537.6 MPa.In addition,the PI/AO@PIS delivers a high ionic conductivity of 0.1 m S/cm at 25°C.As a result,the PI/AO@PIS enables symmetric Li cells to achieve exceptional cyclability for over 1000 h at 0.1 m A/cm2without noticeable lithium dendrite formation.Moreover,the PI/AO@PIS-based LiFePO4||Li full cells demonstrate outstanding rate performance(125.7 m Ah/g at 5 C)and impressive cycling stability(96.1%capacity retention at 1 C after 200 cycles).This work highlights the efficacy of enhancing the mechanical properties of polymer matrices and extending cell performance through the incorporation of a dense inorganic interface layer.展开更多
Security risks of flammability and explosion represent major problems with the use of conventional lithium rechargeable batteries using a liquid electrolyte.The application of solid-state electrolytes could effectivel...Security risks of flammability and explosion represent major problems with the use of conventional lithium rechargeable batteries using a liquid electrolyte.The application of solid-state electrolytes could effectively help to avoid these safety concerns.However,integrating the solid-state electrolytes into the all-solid-state lithium batteries is still a huge challenge mainly due to the high interfacial resistance present in the entire battery,especially at the interface between the cathode and the solid-state electrolyte pellet and the interfaces inside the cathode.Herein,recent progress made from investigations of cathode/solid-state electrolyte interfacial behaviors including the contact problem,the interlayer diffusion issue,the space-charge layer effect,and electrochemical compatibility is presented according to the classification of oxide-,sulfide-,and polymer-based solid-state electrolytes.We also propose strategies for the construction of ideal next-generation cathode/solid-state electrolyte interfaces with high room-temperature ionic conductivity,stable interfacial contact during long cycling,free formation of the space-charge region,and good compatibility with high-voltage cathodes.展开更多
In the past few years,the all-solid lithium battery has attracted worldwide attentions,the ionic conductivity of some all-solid lithium-ion batteries has reached 10^(-3)-10^(-2) S/cm,indicating that the transport of l...In the past few years,the all-solid lithium battery has attracted worldwide attentions,the ionic conductivity of some all-solid lithium-ion batteries has reached 10^(-3)-10^(-2) S/cm,indicating that the transport of lithium ions in solid electrolytes is no longer a major problem.However,some interface issues become research hotspots.Examples of these interfacial issues include the electrochemical decomposition reaction at the electrode-electrolyte interface;the low effective contact area between the solid electrolyte and the electrode etc.In order to solve the issues,researchers have pursued many different approaches.The addition of a buffer layer between the electrode and the solid electrolyte has been at the center of this endeavor.In this review paper,we provide a systematic summarization of the problems on the electrode-solid electrolyte interface and detailed reflection on the latest works of buffer-based therapies,and the review will end with a personal perspective on the improvement of buffer-based therapies.展开更多
The solid-solid electrode-electrolyte interface represents an important component in solid-state batteries(SSBs),as ionic diffusion,reaction,transformation,and restructuring could all take place.As these processes str...The solid-solid electrode-electrolyte interface represents an important component in solid-state batteries(SSBs),as ionic diffusion,reaction,transformation,and restructuring could all take place.As these processes strongly influence the battery performance,studying the evolution of the solid-solid interfaces,particularly in situ during battery operation,can provide insights to establish the structure-property relationship for SSBs.Synchrotron X-ray techniques,owing to their unique penetration power and diverse approaches,are suitable to investigate the buried interfaces and examine structural,compositional,and morphological changes.In this review,we will discuss various surface-sensitive synchrotron-based scattering,spectroscopy,and imaging methods for the in situ characterization of solid-solid interfaces and how this information can be correlated to the electrochemical properties of SSBs.The goal is to overview the advantages and disadvantages of each technique by highlighting representative examples,so that similar strategies can be applied by battery researchers and beyond to study similar solid-solid interface systems.展开更多
The formation mechanism of calcium vanadate and manganese vanadate and the difference between calcium and manganese in the reaction with vanadium are basic issues in the calcification roasting and manganese roasting p...The formation mechanism of calcium vanadate and manganese vanadate and the difference between calcium and manganese in the reaction with vanadium are basic issues in the calcification roasting and manganese roasting process with vanadium slag.In this work,CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples were prepared and roasted for different time periods to illustrate and compare the diffusion reaction mechanisms.Then,the changes in the diffusion product and diffusion coefficient were investigated and calculated based on scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS) analysis.Results show that with the extension of the roasting time,the diffusion reaction gradually proceeds among the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples.The regional boundaries of calcium and vanadium are easily identifiable for the CaO–V_(2)O_(5) diffusion couple.Meanwhile,for the MnO_(2)–V_(2)O_(5) diffusion couple,MnO_(2) gradually decomposes to form Mn_(2)O_(3),and vanadium diffuses into the interior of Mn_(2)O_(3).Only a part of vanadium combines with manganese to form the diffusion production layer.CaV_(2)O_(6) and MnV_(2)O_(6) are the interfacial reaction products of the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples,respectively,whose thicknesses are 39.85 and 32.13μm when roasted for 16 h.After 16 h,both diffusion couples reach the reaction equilibrium due to the limitation of diffusion.The diffusion coefficient of the CaO–V_(2)O_(5) diffusion couple is higher than that of the MnO_(2)–V_(2)O_(5) diffusion couple for the same roasting time,and the diffusion reaction between vanadium and calcium is easier than that between vanadium and manganese.展开更多
Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electr...Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electrolyte during cycles. In this work, we construct a robust functional interface layer on the modified LiB electrode which considerably improves the electrochemical stability of lithium metal electrode in solid state batteries. It is found that the functional interface layer consisting of polydioxolane, polyiodide ion and Li TFSI effectively restrains the growth of lithium dendrites through the redox shuttle reaction of I-/I3-and maintains a good contact between lithium anode and solid electrolyte during cycles. Benefit from these two advantages, the modified Li-B anode exhibits a remarkable cyclic performance in comparison with those of the bare Li-B anode.展开更多
Thin and flexible composite solid-state electrolyte(SSE) is considered to be a prospective candidate for lithium-oxygen(Li-O_(2)) batteries with the aim to address the problems of unsatisfied safety, terrible durabili...Thin and flexible composite solid-state electrolyte(SSE) is considered to be a prospective candidate for lithium-oxygen(Li-O_(2)) batteries with the aim to address the problems of unsatisfied safety, terrible durability as well as inferior electrochemical performance. Herein, in order to improve the safety and durability, a succinonitrile(SN) modified composite SSE is proposed. In this SSE, SN is introduced for eliminating the boundary between ceramic particles, increasing the amorphous region of polymer and ensuring fast ionic transport. Subsequently, the symmetric battery based on the proposed SSE achieves a long cycle life of 3000 h. Moreover, the elaborate cathode interface through the SN participation effectively reduces the barriers to the combination between lithium ions and electrons, facilitating the corresponding electrochemical reactions.As a result, the solid-state Li-O_(2)battery based on this SSE and tuned cathode interface achieves improved electrochemical performance including large specific capacity over 12,000 m Ah g^(-1), enhanced rate capacity as well as stable cycle life of 54 cycles at room temperature. This ingenious design provides a new orientation for the evolution of solid-state Li-O_(2)batteries.展开更多
Li/garnet/LiFePO_(4) solid-state battery was fabricated.The cathode contains LiFePO_(4),Ketjen black,poly(vinylidene fluoride):LiTFSI polymer as active material,electric conductor and Li-ion conducting binder,respecti...Li/garnet/LiFePO_(4) solid-state battery was fabricated.The cathode contains LiFePO_(4),Ketjen black,poly(vinylidene fluoride):LiTFSI polymer as active material,electric conductor and Li-ion conducting binder,respectively.Polyvinylpyrrolidone was added into the cathode to improve cathode/electrolyte interfacial performance.When combined with polyvinylpyrrolidone additive,poly(vinylidene fluoride):polyvinylpyrrol idone:LiTFSI blend forms,and the cathode/electrolyte interfacial resistance reduces from 10.7 kΩto 3.2 kΩ.The Li/garnet/LiFePO_(4) solid-state battery shows 80%capacity retention after 100 cycles at 30℃and 0.05 C.This study offers a general strategy to improve cathode/electrolyte interfacial performance and may enable the practical application of solid-state Li-metal batteries.展开更多
Solid-state sodium batteries(SSSBs)are poised to replace lithium-ion batteries as viable alternatives for energy storage systems owing to their high safety and reliability,abundance of raw material,and low costs.Howev...Solid-state sodium batteries(SSSBs)are poised to replace lithium-ion batteries as viable alternatives for energy storage systems owing to their high safety and reliability,abundance of raw material,and low costs.However,as the core constituent of SSSBs,solid-state electrolytes(SSEs)with low ionic conductivities at room temperature(RT)and unstable interfaces with electrodes hinder the development of SSSBs.Recently,composite SSEs(CSSEs),which inherit the desirable properties of two phases,high RT ionic conductivity,and high interfacial stability,have emerged as viable alternatives;however,their governing mechanism remains unclear.In this review,we summarize the recent research progress of CSSEs,classified into inorganic-inorganic,polymer-polymer,and inorganic-polymer types,and discuss their structure-property relationship in detail.Moreover,the CSSE-electrode interface issues and effective strategies to promote intimate and stable interfaces are summarized.Finally,the trends in the design of CSSEs and CSSE-electrode interfaces are presented,along with the future development prospects of high-performance SSSBs.展开更多
Interfacial bonding is one of the most challenging issues in the fabrication,and hence comprehensively influences the properties of diamond-based metal matrix composites(MMCs)materials.In this work,solid-state(S/S)int...Interfacial bonding is one of the most challenging issues in the fabrication,and hence comprehensively influences the properties of diamond-based metal matrix composites(MMCs)materials.In this work,solid-state(S/S)interface reaction between single-crystal synthetic diamond and chromium(Cr)metal was critically examined with special attention given to unveil the role of crystal orientation in the for-mation and growth of interfacial products.It has been revealed that catalytically converted carbon(CCC)was formed prior to chromium carbides,which is counterintuitive to previous studies.Cr 7 C 3 was the first carbide formed in the S/S interface reaction,aided by the relaxation of diamond lattices that re-duces the interfacial mismatch.Interfacial Cr 7 C 3 and Cr 3 C 2 carbides were formed at 600 and 800℃,respectively,with the growth preferred on diamond(100)plane,because of its higher density of surface defects than(111)plane.Interfacial strain distribution was quasi-quantitively measured using windowed Fourier Transform-Geometric Phase Analysis(WFT-GPA)analysis and an ameliorated strain concentration was found after the ripening of interfacial carbides.Textured morphologies of Cr_(3)C_(2) grown on diamond(100)and(111)planes were perceived after S/S interface reaction at 1000℃,which is reported for the first time.The underlying mechanisms of Cr-induced phase transformation on diamond surface,as well as the crystal orientation dependent growth of interfacial carbides were unveiled using the first-principles calculation.The formation and growth mechanisms of Cr_(3)C_(2) were elucidated using SEM,TEM and XRD analyses.Finally,an approach for tailoring the interfacial microstructure between synthetic diamond and bonding metals was proposed.展开更多
Solid-state lithium batteries(SSLBs)with high safety have emerged to meet the increasing energy density demands of electric vehicles,hybrid electric vehicles,and portable electronic devices.However,the dendrite format...Solid-state lithium batteries(SSLBs)with high safety have emerged to meet the increasing energy density demands of electric vehicles,hybrid electric vehicles,and portable electronic devices.However,the dendrite formation,high interfacial resistance,and deleterious interfacial reactions caused by solid-solid contact between electrode and electrolyte have hindered the commercialization of SSLBs.Thus,in this review,the state-of-the-art developments in the rational design of solid-state electrolyte and their progression toward practical applications are reviewed.First,the origin of interface instability and the sluggish charge carrier transportation in solid-solid interface are presented.Second,various strategies toward stabilizing interfacial stability(reducing interfacial resistance,suppressing lithium dendrites,and side reactions)are summarized from the physical and chemical perspective,including building protective layer,constructing 3D and gradient structures,etc.Finally,the remaining challenges and future development trends of solidstate electrolyte are prospected.This review provides a deep insight into solving the interfacial instability issues and promising solutions to enable practical high-energy-density lithium metal batteries.展开更多
High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions wit...High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.展开更多
Poly(ethylene oxide)(PEO)-based solid polymer electrolyte(SPE)is considered as a promising solid-state electrolyte for all-solid-state lithium batteries(ASSLBs).Nevertheless,the poor interfacial stability with high-vo...Poly(ethylene oxide)(PEO)-based solid polymer electrolyte(SPE)is considered as a promising solid-state electrolyte for all-solid-state lithium batteries(ASSLBs).Nevertheless,the poor interfacial stability with high-voltage cathode materials(e.g.,LiCoO_(2))restricts its application in high energy density solid-state batteries.Herein,high-voltage stable Li_(3)AlF_(6) protective layer is coated on the surface of LiCoO_(2) particle to improve the performance and investigate the failure mechanism of PEO-based ASSLBs.The phase transition unveils that chemical redox reaction occurs between the highly reactive LiCoO_(2) surface and PEO-based SPE,resulting in structure collapse of LiCoO_(2),hence the poor cycle performance of PEO-based ASSLBs with LiCoO_(2) at charging voltage of 4.2 V vs Li/Li+.By sharp contrast,no obvious structure change can be found at the surface of Li_(3)AlF_(6)-coated LiCoO_(2),and the original layered phase was well retained.When the charging voltage reaches up to 4.5 V vs Li/Li+,the intensive electrochemical decomposition of PEO-based SPE occurs,leading to the constant increase of cell impedance and directly causing the poor performance.This work not only provides important supplement to the failure mechanism of PEO-based batter-ies with LiCoO_(2),but also presents a universal strategy to retain structure stability of cathode-electrolyte interface in high-voltage ASSLBs.展开更多
Solid-state supercapacitors(SSCs)are emerging as one of the promising energy storage devices due to their high safety,superior power density,and excellent cycling life.However,performance degradation and safety issues...Solid-state supercapacitors(SSCs)are emerging as one of the promising energy storage devices due to their high safety,superior power density,and excellent cycling life.However,performance degradation and safety issues under extreme conditions are the main challenges for the practical application.With the expansion of human activities,such as space missions,polar exploration,and so on,the investigation of SSC with wide temperature tolerance,high energy density,power density,and sustainability is highly desired.In this review,the effects of temperature on SSC are systematically illustrated and clarified,including the properties of the electrolyte,ion diffusion,and reaction dynamics of the supercapacitor.Subsequently,we summarize the recent advances in wide-temperature-range SSCs from the aspect of electrolyte modification,electrode design,and interface adjustment between electrode and electrolyte,especially with critical concerns on ionic conductivity and cycling stability.In the end,a perspective is presented,expecting to promote the practical application of the SSC in harsh conditions.展开更多
All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrode...All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrodes with high-nickel layered cathodes and inorganic solid electrolytes is one of the important problems to be solved.In addition,the interface and mechanical problems of high-nickel layered cathodes and inorganic solid electrolyte composite electrodes have not been thoroughly addressed.In this paper,the possible interface and mechanical problems in the preparation of high-nickel layered cathodes and inorganic solid electrolytes and their interface reaction during charge–discharge and cycling are reviewed.The mechanical contact problems from phenomena to internal causes are also analyzed.Uniform contact between the high-nickel cathode and solid electrolyte in space and the ionic conductivity of the solid electrolyte are the prerequisites for the good performance of a high-nickel layered cathode.The interface reaction and contact loss between the high-nickel layered cathode and solid electrolyte in the composite electrode directly affect the passage of ions and electrons into the active material.The buffer layer constructed on the high-nickel cathode surface can prevent direct contact between the active material and electrolyte and slow down their interface reaction.An appropriate protective layer can also slow down the interface contact loss by reducing the volume change of the high-nickel layered cathode during charge and discharge.Finally,the following recommendations are put forward to realize the development vision of high-nickel layered cathodes:(1)develop electrochemical systems for high-nickel layered cathodes and inorganic solid electrolytes;(2)elucidate the basic science of interface and electrode processes between high-nickel layered cathodes and inorganic solid electrolytes,clarify the mechanisms of the interfacial chemical and electrochemical reactions between the two materials,and address the intrinsic safety issues;(3)strengthen the development of research and engineering technologies and their preparation methods for composite electrodes with high-nickel layered cathodes and solid electrolytes and promote the industrialization of all-solid-state batteries.展开更多
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 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financial support from the National Natural Science Foundation of China(Nos.52171082 and 51001091)the Program for Innovative Research Team(in Science and Technology)in University of Henan Province(No.21IRTSTHN003)+2 种基金partially supported by the Provincial Scientific Research Program of Henan(No.182102310815)Nuclear Material Technology Innovation Fund for National Defense Technology Industry(No.ICNM-2021-YZ-02)the Science and Technology Project of Henan Province(No.232102241036).
文摘In recent years,due to the increasing demand for portable electronic devices,rechargeable solid-state battery technology has developed rapidly.Lithium-ion batteries are the systems of choice,offering high energy density,flexible and lightweight design,and longer lifespan than comparable battery technologies.Therefore,a better understanding of the relationship between electrochemical mechanism and structural properties from theory and experiment will enable us to accelerate the development of high-performance and security batteries.This review discusses the interplay between theoretical calculation and experiment in the study of lithium ion battery materials.We introduce the application of theoretical calculation method in solid-state batteries through the combination of theory and experiment.We present the concept and assembly technology of solid-state batteries are reviewed.The basic parameters of solid-state electrolytes,especially sulfide-based solid-state electrolytes and their interface mechanisms with high-voltage cathode materials,are analyzed by theoretical methods.We present an overview on the scientific challenges,fundamental mechanisms,and design strategies for solid-state batteries,especially focusing on the issues of stability on solid-state electrolytes and the associated interfaces with both cathode and electrolyte.Owing to the theoretical models,we can not only reveal the unprecedented mechanism from the atomic scale,but also analyze the interface problems in the battery thoroughly,thus effectively designing more promising electrolyte and interface coating materials.It blazed a new trial for engineering an interphase with improved interfacial compatibility for a long-term cyclability.
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supported financially by the National Natural Science Foundation of China(No.52172202)Science and Technology Program of Guangzhou,China(No.SL2024A03J00326)+1 种基金Key Research and Development project of High-Level Scientific and Technological Talent Introduction for Luliang City(No.2023RC27)the Basic Research Program(Free Exploration Category)Project for Shanxi Province(No.202303021222251)
文摘Severe structural fractures and persistent side reactions at the interface with liquid electrolytes have hindered the commercialization of silicon(Si)anodes.Solid-state electrolytes present a promising solution to address these issues.However,the high interfacial resistance of rigid ceramic electrolytes and the limited ionic conductivity of polymer electrolytes remain significant challenges,further complicated by the substantial volume expansion of Si.In this work,we chemically grafted a flame-retardant,self-healing polyurethane-thiourea polymer onto Li_(7)P_(3)S_(11)(SHPUSB-40%LPS)via nucleophilic addition,creating an electrolyte with exceptional ionic conductivity,high elasticity,and strong compatibility with Si anodes.We observed that FSI^(-)was strongly adsorbed onto the LPS surface through electrostatic interactions with sulfur vacancies,enhancing Li^(+)transport.Furthermore,SHPUSB-40%LPS exhibits dynamic covalent disulfide bonds and hydrogen bonds,enabling self-assembly of the electrolyte at the interface.This dynamic bonding provides a self-healing mechanism that mitigates structural changes during Si expansion and contraction cycles.As a result,the Si anode with SHPUSB-40%LPS presents excellent cycling stability,retaining nearly 53.5%of its capacity after 300 cycles.The practical applicability of this design was validated in a 2 Ah all-solid-state Si‖LiNi_(0.6)Mn_(0.2)Co_(0.2)O_(2)pouch cell,which maintained a stable Li-ion storage capacity retention of 76.3%after 350cycles at 0.5C.This novel solid-state electrolyte with selfhealing properties offers a promising strategy to address fundamental interfacial and performance challenges associated with Si anodes.
基金the financial support from the 261Project of MIIT and Natural Science Foundation of Jiangsu Province(No.BK20240179)。
文摘The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength,ionic conductivity,and thickness.Here,we propose Al_(2)O_(3)-coated polyimide(AO/PI)porous film as a high-strength substrate to support fast-ion-conducting polymer-in-salt(PIS)solid-state electrolytes,aiming to suppress lithium dendrite growth and improve full-cell performance.The Al_(2)O_(3)coating layer not only refines the wettability of polyimide porous film to PIS,but also performs as a high modulus protective layer to suppress the growth of lithium dendrites.The resulting PI/AO@PIS exhibits a small thickness of only 35μm with an outstanding tensile strength of 11.3 MPa and Young's modulus of 537.6 MPa.In addition,the PI/AO@PIS delivers a high ionic conductivity of 0.1 m S/cm at 25°C.As a result,the PI/AO@PIS enables symmetric Li cells to achieve exceptional cyclability for over 1000 h at 0.1 m A/cm2without noticeable lithium dendrite formation.Moreover,the PI/AO@PIS-based LiFePO4||Li full cells demonstrate outstanding rate performance(125.7 m Ah/g at 5 C)and impressive cycling stability(96.1%capacity retention at 1 C after 200 cycles).This work highlights the efficacy of enhancing the mechanical properties of polymer matrices and extending cell performance through the incorporation of a dense inorganic interface layer.
基金National Natural Science Foundation of China(U2001220)the Local Innovative Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01N111)+1 种基金the Shenzhen Technical Plan Project(Nos.JCYJ20180508152210821,JCYJ20170817161221958,and JCYJ20180508152135822)the Shenzhen All-Solid-State Lithium Battery Electrolyte Engineering Research Center(XMHT20200203006).
文摘Security risks of flammability and explosion represent major problems with the use of conventional lithium rechargeable batteries using a liquid electrolyte.The application of solid-state electrolytes could effectively help to avoid these safety concerns.However,integrating the solid-state electrolytes into the all-solid-state lithium batteries is still a huge challenge mainly due to the high interfacial resistance present in the entire battery,especially at the interface between the cathode and the solid-state electrolyte pellet and the interfaces inside the cathode.Herein,recent progress made from investigations of cathode/solid-state electrolyte interfacial behaviors including the contact problem,the interlayer diffusion issue,the space-charge layer effect,and electrochemical compatibility is presented according to the classification of oxide-,sulfide-,and polymer-based solid-state electrolytes.We also propose strategies for the construction of ideal next-generation cathode/solid-state electrolyte interfaces with high room-temperature ionic conductivity,stable interfacial contact during long cycling,free formation of the space-charge region,and good compatibility with high-voltage cathodes.
基金financially supported by the Fundamental Research Funds for the Central Universities of China(No.FRF-BD-19-008A)the Brain Pool program funded by the Ministry of Science and ICT through the National Research Foundation of Korea(No.2019H1D3A2A02100593)the National Research Foundation of Korea(NRF)grant funded by the Korean government(Nos.2019R1C1C 1006310,2020R1I1A1A01072996,2021K2A9A2A06044652,and 2019R1A2C1002844).
文摘In the past few years,the all-solid lithium battery has attracted worldwide attentions,the ionic conductivity of some all-solid lithium-ion batteries has reached 10^(-3)-10^(-2) S/cm,indicating that the transport of lithium ions in solid electrolytes is no longer a major problem.However,some interface issues become research hotspots.Examples of these interfacial issues include the electrochemical decomposition reaction at the electrode-electrolyte interface;the low effective contact area between the solid electrolyte and the electrode etc.In order to solve the issues,researchers have pursued many different approaches.The addition of a buffer layer between the electrode and the solid electrolyte has been at the center of this endeavor.In this review paper,we provide a systematic summarization of the problems on the electrode-solid electrolyte interface and detailed reflection on the latest works of buffer-based therapies,and the review will end with a personal perspective on the improvement of buffer-based therapies.
文摘The solid-solid electrode-electrolyte interface represents an important component in solid-state batteries(SSBs),as ionic diffusion,reaction,transformation,and restructuring could all take place.As these processes strongly influence the battery performance,studying the evolution of the solid-solid interfaces,particularly in situ during battery operation,can provide insights to establish the structure-property relationship for SSBs.Synchrotron X-ray techniques,owing to their unique penetration power and diverse approaches,are suitable to investigate the buried interfaces and examine structural,compositional,and morphological changes.In this review,we will discuss various surface-sensitive synchrotron-based scattering,spectroscopy,and imaging methods for the in situ characterization of solid-solid interfaces and how this information can be correlated to the electrochemical properties of SSBs.The goal is to overview the advantages and disadvantages of each technique by highlighting representative examples,so that similar strategies can be applied by battery researchers and beyond to study similar solid-solid interface systems.
基金supported by the National Natural Science Foundation of China(Nos.52174277 and 51874077)the Fundamental Funds for the Central Universities,China(No.N2225032)+1 种基金the China Postdoctoral Science Foundation(No.2022M720683)the Postdoctoral Fund of Northeastern University,China。
文摘The formation mechanism of calcium vanadate and manganese vanadate and the difference between calcium and manganese in the reaction with vanadium are basic issues in the calcification roasting and manganese roasting process with vanadium slag.In this work,CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples were prepared and roasted for different time periods to illustrate and compare the diffusion reaction mechanisms.Then,the changes in the diffusion product and diffusion coefficient were investigated and calculated based on scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS) analysis.Results show that with the extension of the roasting time,the diffusion reaction gradually proceeds among the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples.The regional boundaries of calcium and vanadium are easily identifiable for the CaO–V_(2)O_(5) diffusion couple.Meanwhile,for the MnO_(2)–V_(2)O_(5) diffusion couple,MnO_(2) gradually decomposes to form Mn_(2)O_(3),and vanadium diffuses into the interior of Mn_(2)O_(3).Only a part of vanadium combines with manganese to form the diffusion production layer.CaV_(2)O_(6) and MnV_(2)O_(6) are the interfacial reaction products of the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples,respectively,whose thicknesses are 39.85 and 32.13μm when roasted for 16 h.After 16 h,both diffusion couples reach the reaction equilibrium due to the limitation of diffusion.The diffusion coefficient of the CaO–V_(2)O_(5) diffusion couple is higher than that of the MnO_(2)–V_(2)O_(5) diffusion couple for the same roasting time,and the diffusion reaction between vanadium and calcium is easier than that between vanadium and manganese.
基金supported by the National Natural Science Foundation of China (NO. 21805113)the Fundamental Research Funds for the Central Universities (NO. 11618410 and NO. 11619103)the China Postdoctoral Science Foundation (NO. 2019M653271)。
文摘Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electrolyte during cycles. In this work, we construct a robust functional interface layer on the modified LiB electrode which considerably improves the electrochemical stability of lithium metal electrode in solid state batteries. It is found that the functional interface layer consisting of polydioxolane, polyiodide ion and Li TFSI effectively restrains the growth of lithium dendrites through the redox shuttle reaction of I-/I3-and maintains a good contact between lithium anode and solid electrolyte during cycles. Benefit from these two advantages, the modified Li-B anode exhibits a remarkable cyclic performance in comparison with those of the bare Li-B anode.
基金the partial financial support from the National Natural Science Foundation of China (22075171,21805182 and 22179080)。
文摘Thin and flexible composite solid-state electrolyte(SSE) is considered to be a prospective candidate for lithium-oxygen(Li-O_(2)) batteries with the aim to address the problems of unsatisfied safety, terrible durability as well as inferior electrochemical performance. Herein, in order to improve the safety and durability, a succinonitrile(SN) modified composite SSE is proposed. In this SSE, SN is introduced for eliminating the boundary between ceramic particles, increasing the amorphous region of polymer and ensuring fast ionic transport. Subsequently, the symmetric battery based on the proposed SSE achieves a long cycle life of 3000 h. Moreover, the elaborate cathode interface through the SN participation effectively reduces the barriers to the combination between lithium ions and electrons, facilitating the corresponding electrochemical reactions.As a result, the solid-state Li-O_(2)battery based on this SSE and tuned cathode interface achieves improved electrochemical performance including large specific capacity over 12,000 m Ah g^(-1), enhanced rate capacity as well as stable cycle life of 54 cycles at room temperature. This ingenious design provides a new orientation for the evolution of solid-state Li-O_(2)batteries.
基金Funded by the National Natural Science Foundation of China(Nos.51772314,51532002,51771222 and 51702346)the Natural Science Foundation of Shanghai City(17ZR1434600)。
文摘Li/garnet/LiFePO_(4) solid-state battery was fabricated.The cathode contains LiFePO_(4),Ketjen black,poly(vinylidene fluoride):LiTFSI polymer as active material,electric conductor and Li-ion conducting binder,respectively.Polyvinylpyrrolidone was added into the cathode to improve cathode/electrolyte interfacial performance.When combined with polyvinylpyrrolidone additive,poly(vinylidene fluoride):polyvinylpyrrol idone:LiTFSI blend forms,and the cathode/electrolyte interfacial resistance reduces from 10.7 kΩto 3.2 kΩ.The Li/garnet/LiFePO_(4) solid-state battery shows 80%capacity retention after 100 cycles at 30℃and 0.05 C.This study offers a general strategy to improve cathode/electrolyte interfacial performance and may enable the practical application of solid-state Li-metal batteries.
基金China Postdoctoral Science Foundation,Grant/Award Numbers:2022TQ0065,2023M730614Science and Technology Commission of Shanghai Municipality,Grant/Award Numbers:21ZR1409300,23160714000+3 种基金Shanghai Post-doctoral Excellence Program,Grant/Award Number:2022029Thail and Science research and Innovation Fund Chulalongkorn University,The Program Management Unit for Human Resources&Institutional Development,Research and Innovation,Grant/Award Number:B41G670026National Key Research and Development Program of China,Grant/Award Number:2022YFB2502004Key Basic Research Program of Science and Technology Commission of Shanghai Municipality,Grant/Award Number:23520750400。
文摘Solid-state sodium batteries(SSSBs)are poised to replace lithium-ion batteries as viable alternatives for energy storage systems owing to their high safety and reliability,abundance of raw material,and low costs.However,as the core constituent of SSSBs,solid-state electrolytes(SSEs)with low ionic conductivities at room temperature(RT)and unstable interfaces with electrodes hinder the development of SSSBs.Recently,composite SSEs(CSSEs),which inherit the desirable properties of two phases,high RT ionic conductivity,and high interfacial stability,have emerged as viable alternatives;however,their governing mechanism remains unclear.In this review,we summarize the recent research progress of CSSEs,classified into inorganic-inorganic,polymer-polymer,and inorganic-polymer types,and discuss their structure-property relationship in detail.Moreover,the CSSE-electrode interface issues and effective strategies to promote intimate and stable interfaces are summarized.Finally,the trends in the design of CSSEs and CSSE-electrode interfaces are presented,along with the future development prospects of high-performance SSSBs.
基金supported by the National Natural Science Foundation of China (No.51835004)the National Technology Development Project in Fujian province (No.2021L3012)funding support from Australia Research Council (ARC)through the Discovery Project Program (No.DP210102061).
文摘Interfacial bonding is one of the most challenging issues in the fabrication,and hence comprehensively influences the properties of diamond-based metal matrix composites(MMCs)materials.In this work,solid-state(S/S)interface reaction between single-crystal synthetic diamond and chromium(Cr)metal was critically examined with special attention given to unveil the role of crystal orientation in the for-mation and growth of interfacial products.It has been revealed that catalytically converted carbon(CCC)was formed prior to chromium carbides,which is counterintuitive to previous studies.Cr 7 C 3 was the first carbide formed in the S/S interface reaction,aided by the relaxation of diamond lattices that re-duces the interfacial mismatch.Interfacial Cr 7 C 3 and Cr 3 C 2 carbides were formed at 600 and 800℃,respectively,with the growth preferred on diamond(100)plane,because of its higher density of surface defects than(111)plane.Interfacial strain distribution was quasi-quantitively measured using windowed Fourier Transform-Geometric Phase Analysis(WFT-GPA)analysis and an ameliorated strain concentration was found after the ripening of interfacial carbides.Textured morphologies of Cr_(3)C_(2) grown on diamond(100)and(111)planes were perceived after S/S interface reaction at 1000℃,which is reported for the first time.The underlying mechanisms of Cr-induced phase transformation on diamond surface,as well as the crystal orientation dependent growth of interfacial carbides were unveiled using the first-principles calculation.The formation and growth mechanisms of Cr_(3)C_(2) were elucidated using SEM,TEM and XRD analyses.Finally,an approach for tailoring the interfacial microstructure between synthetic diamond and bonding metals was proposed.
基金supported by the National Key R&D Program(2022YFE0206400)the National Natural Science Foundation of China(52202256)+4 种基金the Natural Science Foundation of Jiangsu Province of China(BK20220612)the Science and Technology Development Fund,Macao SAR(0096/2020/A2,0013/2021/AMJ,and 0082/2022/A2)the Opening Project of the Key Laboratory of Jiangsu Province for Silk Engineering,Soochow University(KJS2277)the funds from Jiangsu University“Qinglan Project”the Young Elite Scientists Sponsorship Program of the Jiangsu Association for Science and Technology
文摘Solid-state lithium batteries(SSLBs)with high safety have emerged to meet the increasing energy density demands of electric vehicles,hybrid electric vehicles,and portable electronic devices.However,the dendrite formation,high interfacial resistance,and deleterious interfacial reactions caused by solid-solid contact between electrode and electrolyte have hindered the commercialization of SSLBs.Thus,in this review,the state-of-the-art developments in the rational design of solid-state electrolyte and their progression toward practical applications are reviewed.First,the origin of interface instability and the sluggish charge carrier transportation in solid-solid interface are presented.Second,various strategies toward stabilizing interfacial stability(reducing interfacial resistance,suppressing lithium dendrites,and side reactions)are summarized from the physical and chemical perspective,including building protective layer,constructing 3D and gradient structures,etc.Finally,the remaining challenges and future development trends of solidstate electrolyte are prospected.This review provides a deep insight into solving the interfacial instability issues and promising solutions to enable practical high-energy-density lithium metal batteries.
基金financially supported by the National Natural Science Foundation of China(Nos.22102212 and 22479067).
文摘High-nickel ternary cathodes hold a great application prospect in solid-state lithium metal batteries to achieve high-energy density,but they still suffer from structural instability and detrimental side reactions with the solid-state electrolytes.To circumvent these issues,a continuous uniform layer polyacrylonitrile(PAN)was introduced on the surface of LiNi_(0.8)Mn_(0.1)Co_(0.1)O_(2) via in situ polymerization of acrylonitrile(AN).Furthermore,the partial-cyclized treatment of PAN(cPAN)coating layer presents high ionic and electron conductivity,which can accelerate interfacial Li+and electron diffusion simultaneously.And the thermodynamically stabilized cPAN coating layer cannot only effectively inhibit detrimental side reactions between cathode and solid-state electrolytes but also provide a homogeneous stress to simultaneously address the problems of bulk structural degradation,which contributes to the exceptional mechanical and electrochemical stabilities of the modified electrode.Besides,the coordination bond interaction between the cPAN and NCM811 can suppress the migration of Ni to elevate the stability of the crystal structure.Benefited from these,the In-cPAN-260@NCM811 shows excellent cycling performance with a retention of 86.8%after 300 cycles and superior rate capability.And endow the solid-state battery with thermal safety stability even at hightemperature extreme environment.This facile and scalable surface engineering represents significant progress in developing high-performance solid-state lithium metal batteries.
基金We acknowledge financial support from The Shenzhen Science and Technology Research Grant(No.JCYJ20200109140416788)Soft Science Research Project of Guangdong Province(No.2017B030301013)The National Natural Science Foundation of China(No.52102200).
文摘Poly(ethylene oxide)(PEO)-based solid polymer electrolyte(SPE)is considered as a promising solid-state electrolyte for all-solid-state lithium batteries(ASSLBs).Nevertheless,the poor interfacial stability with high-voltage cathode materials(e.g.,LiCoO_(2))restricts its application in high energy density solid-state batteries.Herein,high-voltage stable Li_(3)AlF_(6) protective layer is coated on the surface of LiCoO_(2) particle to improve the performance and investigate the failure mechanism of PEO-based ASSLBs.The phase transition unveils that chemical redox reaction occurs between the highly reactive LiCoO_(2) surface and PEO-based SPE,resulting in structure collapse of LiCoO_(2),hence the poor cycle performance of PEO-based ASSLBs with LiCoO_(2) at charging voltage of 4.2 V vs Li/Li+.By sharp contrast,no obvious structure change can be found at the surface of Li_(3)AlF_(6)-coated LiCoO_(2),and the original layered phase was well retained.When the charging voltage reaches up to 4.5 V vs Li/Li+,the intensive electrochemical decomposition of PEO-based SPE occurs,leading to the constant increase of cell impedance and directly causing the poor performance.This work not only provides important supplement to the failure mechanism of PEO-based batter-ies with LiCoO_(2),but also presents a universal strategy to retain structure stability of cathode-electrolyte interface in high-voltage ASSLBs.
基金Special Fund for Carbon Peak and Carbon Neutralization Scientific and Technological Innovation Project of Jiangsu Province,Grant/Award Number:BE2022042National Natural Science Foundation of China,Grant/Award Numbers:22201275,51873086,51673096,51873086,51673096+2 种基金the Project on the Enterprises-Universities-Research Cooperation of Kucap Smart Technology(Nanjing)Co.,Ltd.,Grant/Award Number:202240607Postgraduate Research&Practice Innovation Program of Jiangsu Province,Grant/Award Number:KYCX23-1407Anhui Provincial Natural Science Foundation,Grant/Award Number:2208085QB32。
文摘Solid-state supercapacitors(SSCs)are emerging as one of the promising energy storage devices due to their high safety,superior power density,and excellent cycling life.However,performance degradation and safety issues under extreme conditions are the main challenges for the practical application.With the expansion of human activities,such as space missions,polar exploration,and so on,the investigation of SSC with wide temperature tolerance,high energy density,power density,and sustainability is highly desired.In this review,the effects of temperature on SSC are systematically illustrated and clarified,including the properties of the electrolyte,ion diffusion,and reaction dynamics of the supercapacitor.Subsequently,we summarize the recent advances in wide-temperature-range SSCs from the aspect of electrolyte modification,electrode design,and interface adjustment between electrode and electrolyte,especially with critical concerns on ionic conductivity and cycling stability.In the end,a perspective is presented,expecting to promote the practical application of the SSC in harsh conditions.
文摘All-solid-state batteries potentially exhibit high specific energy and high safety,which is one of the development directions for nextgeneration lithium-ion batteries.The compatibility of all-solid composite electrodes with high-nickel layered cathodes and inorganic solid electrolytes is one of the important problems to be solved.In addition,the interface and mechanical problems of high-nickel layered cathodes and inorganic solid electrolyte composite electrodes have not been thoroughly addressed.In this paper,the possible interface and mechanical problems in the preparation of high-nickel layered cathodes and inorganic solid electrolytes and their interface reaction during charge–discharge and cycling are reviewed.The mechanical contact problems from phenomena to internal causes are also analyzed.Uniform contact between the high-nickel cathode and solid electrolyte in space and the ionic conductivity of the solid electrolyte are the prerequisites for the good performance of a high-nickel layered cathode.The interface reaction and contact loss between the high-nickel layered cathode and solid electrolyte in the composite electrode directly affect the passage of ions and electrons into the active material.The buffer layer constructed on the high-nickel cathode surface can prevent direct contact between the active material and electrolyte and slow down their interface reaction.An appropriate protective layer can also slow down the interface contact loss by reducing the volume change of the high-nickel layered cathode during charge and discharge.Finally,the following recommendations are put forward to realize the development vision of high-nickel layered cathodes:(1)develop electrochemical systems for high-nickel layered cathodes and inorganic solid electrolytes;(2)elucidate the basic science of interface and electrode processes between high-nickel layered cathodes and inorganic solid electrolytes,clarify the mechanisms of the interfacial chemical and electrochemical reactions between the two materials,and address the intrinsic safety issues;(3)strengthen the development of research and engineering technologies and their preparation methods for composite electrodes with high-nickel layered cathodes and solid electrolytes and promote the industrialization of all-solid-state batteries.
