As a high-energy-density primary battery,the Li-SOCl_(2) battery offers significant advantages over other primary systems,including a high operating voltage,wide temperature tolerance,and low self-discharge rate.Howev...As a high-energy-density primary battery,the Li-SOCl_(2) battery offers significant advantages over other primary systems,including a high operating voltage,wide temperature tolerance,and low self-discharge rate.However,owing to the irreversible electrochemical reaction mechanism,despite its energy density of up to 700 Wh kg^(-1) at the cell level,this battery system has remained confined to the category of primary batteries,thereby limiting its use in cyclic applications.Recent advances in electrochemical technologies have enabled the reversible redox chemistry of Li-SOCl_(2) batteries,transforming them into rechargeable systems.This article provides a systematic overview of the technical evolution,reaction mechanisms,safety constraints,engineering countermeasures,and electrochemical performance enhancement of Li-SOCl_(2) primary batteries since their introduction.First,the modification methods for the lithium anode,carbon cathode,electrolyte,and electrocatalyst in Li-SOCl_(2) primary batteries are discussed,along with their mechanisms for improving electrochemical performance.We then review the SOCl_(2)-based rechargeable Li metal batteries(LMBs)that evolved from the Li-SOCl_(2) primary batteries.With their higher energy density,these systems have become promising candidates to replace traditional Li-ion batteries(LIBs).This review focuses on the construction of key components,such as the positive electrode carrier,novel alloy anode,and electrolyte,as well as their impact on electrochemical performance in rechargeable batteries.Finally,we summarize current research progress and propose future directions for SOCl_(2)-based LMBs aimed at enhancing overall electrochemical performance.These insights provide a theoretical foundation for the development of next-generation high-energy-density energy-storage technologies.展开更多
1.Introduction Driven by the growing demand for energy storage systems in portable electronic devices,electric vehicles,and unmanned aerial vehicles,lithium-ion batteries(LIBs)have received considerable and sustained ...1.Introduction Driven by the growing demand for energy storage systems in portable electronic devices,electric vehicles,and unmanned aerial vehicles,lithium-ion batteries(LIBs)have received considerable and sustained attention.The performance of routine LIBs is approaching the ceiling,particularly in terms of energy density,making it difficult to meet the ever-increasing demand for energy density[1].展开更多
Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by t...Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by the poor conductivity andthe irreversible dissolution of conventionalε-MnO_(2)deposits.Herein,we report a scalable semisolid slurryelectrode architecture that enables stable MnO_(2)deposition/dissolution using a three-dimensional percolatingnetwork of carbon nanotubes(CNTs)as both conductivematrix and deposition host.The slurry systempromotes the formation of highly conductiveγ-MnO_(2)owing to enhanced charge transfer kinetics,enablingoverall dissolution rather than the localized separationtypically seen in traditional electrodes.The Zn-MnO_(2)slurry cell exhibits a reversible areal capacity approaching 60 mAh cm^(-2).Moreover,theflowable nature of the slurry allows electrochemically inactive MnO_(2)formed during dissolution to be reconnected and reactivated by CNTs inthe rheological network,ensuring deep utilization and cycling stability.This work establishes a slurry electrode strategy to improve electrolyticMnO_(2)reactions and offers a viable pathway toward renewable aqueous batteries for grid-scale applications.展开更多
Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because ...Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.展开更多
Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms lig...Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.展开更多
Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a no...Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.展开更多
Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_...Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.展开更多
Understanding how aging influences the thermal hazards of lithium-ion batteries(LIBs)is critical for enhancing their safety across a wide range of applications.This study systematically investigates the thermal runawa...Understanding how aging influences the thermal hazards of lithium-ion batteries(LIBs)is critical for enhancing their safety across a wide range of applications.This study systematically investigates the thermal runaway(TR)behavior of LIBs,with particular emphasis on combined-pathway aging,evaluated in terms of normalized usable capacity(U_(E)).Key thermal safety parameters,i.e.,TR triggering temperature,mass loss,and heat generation under diverse aging conditions,are quantified.To enable a fair comparison,thermal hazards are evaluated based on equivalent usable capacity,revealing that aged cells exhibit lower TR triggering temperatures and higher heat generation than fresh cells under thermal abuse with elevated thermal risks.Mechanistic analysis identifies lithium plating,solid electrolyte interphase(SEI)formation,and lithium depletion,particularly under high-temperature charging,as the dominant contributors to increased hazard.Using an aging-stressor matrix,a trade-off between high-C-rateinduced thermal instability and high-temperature-induced thermal stability is discovered and quantified,underscoring the strong dependence of thermal hazards on specific aging pathways.This work advances the fundamental understanding of aging-induced safety risks in LIBs and offers practical guidance for the development of safer battery systems,optimized charging protocols,and improved battery management strategies across applications in electric vehicles,consumer electronics,and grid-scale energy storage.展开更多
Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread applica...Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread application.In this study,hemin was employed as a multi-functional artificial interface for the first time to inhibit the disordered growth of zinc dendrites and mitigate side reactions.Theoretical calculations indicate that hemin is preferentially adsorbed onto the zinc anode,thus blocking the interaction between the active zinc anode and electrolyte.Compared with zinc foil,the Hemin@Zn anode demonstrates enhanced corrosion resistance,a decrease in hydrogen evolution,and more orderly deposition of zinc.As expected,the symmetric cell with Hemin@Zn anode can sustain up to 4000 h at 0.2 mA/cm^(2),0.2 mAh/cm^(2).Asymmetric Zn//Cu cells exhibit an average coulombic efficiency exceeding 99.72 % during 500 cycles.Moreover,the full cell Hemin@Zn//NH_(4)V_(4)O_(10) delivers a superior capacity up to 367 m Ah/g and the discharge capacity retention reaches 124 mAh/g after 1200 cycles even at a current density of 5 A/g.This work provides a simple and effective method for constructing a robust artificial interface to promote the application of long-life AZIBs.展开更多
Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully syn...Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.展开更多
Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity c...Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity carbon nanotubes(CNT)conductive materials,and electrode thickening.However,these methods are still limited due to the limitation in the capacity of high-nickel NCM,aggregation of CNT conductive materials,and nonuniform material distribution of thick-film electrodes,which ultimately damage the mechanical and electrical integrity of the electrode,leading to a decrease in electrochemical performance.Here,we present an integrated binder-CNT composite dispersion solution to realize a high-solids-content(>77 wt%)slurry for high-mass-loading electrodes and to mitigate the migration of binder and conductive additives.Indeed,the approach reduces solvent usage by approximately 30%and ensures uniform conductive additive-binder domain distribution during electrode manufacturing,resulting in improved coating quality and adhesive strength for high-mass-loading electrodes(>12 mAh cm^(−2)).In terms of various electrode properties,the presented electrode showed low resistance and excellent electrochemical properties despite the low CNT contents of 0.6 wt%compared to the pristine-applied electrode with 0.85 wt%CNT contents.Moreover,our strategy enables faster drying,which increases the coating speed,thereby offering potential energy savings and supporting carbon neutrality in wet-based electrode manufacturing processes.展开更多
The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.Howeve...The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.展开更多
Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures,bringing challenges to the application of lithium-ion batteries(LIBs)at low temperatures.H...Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures,bringing challenges to the application of lithium-ion batteries(LIBs)at low temperatures.Herein,the ester solvent of methyl propionate(MP)with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes.Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions.The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied.As a result,methyl pentafluoropropionate(M5F)with five fluorine atoms was selected for its optimal interactions with both Li+and MP solvent in the primary solvation structure,contributing to desired solvation structure for fast interfacial transport.The LiFePO_(4)(LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8%after 120 cycles and retained 81.2%of room-temperature capacity when charged and discharged at−30℃.1 Ah LFP||graphite pouch cell with high cathode loading(20 mg/cm^(2))in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at−20℃.This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application.展开更多
The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightfor...The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.展开更多
Magnesium batteries are attracting growing interest as next-generation energy storage technology due to their high safety,cost-effectiveness,and resource abundance.However,their development remains limited by sluggish...Magnesium batteries are attracting growing interest as next-generation energy storage technology due to their high safety,cost-effectiveness,and resource abundance.However,their development remains limited by sluggish Mg^(2+)transport kinetics at the electrode/electrolyte interface.Herein,we propose an electrolyte design strategy that modulates the Mg^(2+)solvation structure by introducing tetrahydrofuran(THF)as a co-solvent into a borate-based electrolyte,Mg[B(hfip)_(4)](MBF)in dimethoxyethane(DME).THF,selected from a series of linear and cyclic ethers,has a comparable dielectric constant and donor number to DME,but its cyclic structure introduces steric hindrance that induces competitive coordination with Mg^(2+).This competition weakens Mg^(2+)-solvent interactions,yielding a more labile solvation structure and enhanced desolvation kinetics.As a result,Mg||Mg cells employing the optimized MBF/1D1T electrolyte(DME:THF=1:1,v:v)exhibit a significantly reduced Mg plating/stripping overpotential of 120 mV at 10 mA cm^(-2),compared with 316 mV at 8 mA cm^(-2)with MBF/DME,along with exceptional cycling stability exceeding 1200 h.Furthermore,representative sulfide cathodes such as CuS and VS_(4)demonstrate faster activation and improved high-rate performance in the presence of MBF/1D1T.展开更多
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.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
The principal challenge in optimizing biomass-derived hard carbon(HC)is the concurrent enhancement of specific capacity,cycling durability,and rate performance,as these properties are closely related to the disordered...The principal challenge in optimizing biomass-derived hard carbon(HC)is the concurrent enhancement of specific capacity,cycling durability,and rate performance,as these properties are closely related to the disordered carbon network and abundant pore structure.However,inadequate controllability of morphology,insufficiently regulated pore structures,and the complexity of post-processing modifications hinders the practical application of HC.In this work,a high-temperature and high-pressure expansion pretreatment technique is proposed to regulate the structure of starch precursors,enabling the precise design of ordered graphitic-like microcrystals and closed pores within HC.The optimized starch-based HC displayed remarkable electrochemical efficiency,with a reversible capacity of 332.0 mAh g^(-1),an initial Coulombic efficiency of 90.4%,and stable cycling over 3000 cycles.Meanwhile,advanced full-cell utilizing Na4Fe3(PO_(4))_(2)P_(2)O_(7) cathode achieve stable cycling performance exceeding 1000 cycles,demonstrating outstanding performance.This research innovatively employs a green expansion process to achieve structural regulation of HC,thereby providing an environmentally friendly and economically viable technical pathway for its large-scale production.展开更多
Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation...Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.展开更多
Solar energy represents a transformative,inexhaustible,and eco-friendly solution for sustainable power generation.However,its intermittent nature requires efficient energy storage technologies to maximize utilization....Solar energy represents a transformative,inexhaustible,and eco-friendly solution for sustainable power generation.However,its intermittent nature requires efficient energy storage technologies to maximize utilization.A promising approach involves integrating photoactive materials into the cathodes of zinc-ion batteries(ZIBs),enabling direct solar energy capture and storage while improving electrochemical performance.This review systematically explores the emerging field of light-driven ZIBs(LDZIBs),focusing on two main operational modes:photo-assisted ZIBs(PAZIBs),where light enhances battery performance,and photo-rechargeable ZIBs(PRZIBs),which can be directly charged by light without external power sources.We comprehensively examine the classification,working mechanisms,and material integration strategies for these systems.Key advances in electrode design,innovative materials,and potential application scenarios for both PAZIBs and PRZIBs are highlighted.Finally,we discuss the major challenges and future research directions aimed at improving the efficiency,stability,and scalability of LDZIBs to facilitate their commercialization as a cornerstone technology for future solar energy storage.展开更多
基金financially supported by the National Natural Science Foundation of China(No.22309138)the Hubei Province Natural Science Foundation(No.2024AFB815)+1 种基金the Postdoctoral Project of Hubei Province(No.2024HBBHXF056)the Department of Science and Technology of Hubei Province(No.2025CSA001)。
文摘As a high-energy-density primary battery,the Li-SOCl_(2) battery offers significant advantages over other primary systems,including a high operating voltage,wide temperature tolerance,and low self-discharge rate.However,owing to the irreversible electrochemical reaction mechanism,despite its energy density of up to 700 Wh kg^(-1) at the cell level,this battery system has remained confined to the category of primary batteries,thereby limiting its use in cyclic applications.Recent advances in electrochemical technologies have enabled the reversible redox chemistry of Li-SOCl_(2) batteries,transforming them into rechargeable systems.This article provides a systematic overview of the technical evolution,reaction mechanisms,safety constraints,engineering countermeasures,and electrochemical performance enhancement of Li-SOCl_(2) primary batteries since their introduction.First,the modification methods for the lithium anode,carbon cathode,electrolyte,and electrocatalyst in Li-SOCl_(2) primary batteries are discussed,along with their mechanisms for improving electrochemical performance.We then review the SOCl_(2)-based rechargeable Li metal batteries(LMBs)that evolved from the Li-SOCl_(2) primary batteries.With their higher energy density,these systems have become promising candidates to replace traditional Li-ion batteries(LIBs).This review focuses on the construction of key components,such as the positive electrode carrier,novel alloy anode,and electrolyte,as well as their impact on electrochemical performance in rechargeable batteries.Finally,we summarize current research progress and propose future directions for SOCl_(2)-based LMBs aimed at enhancing overall electrochemical performance.These insights provide a theoretical foundation for the development of next-generation high-energy-density energy-storage technologies.
基金supported by the Beijing Natural Science Foundation(L243019)the National Natural Science Foundation of China(22393900,22393904)+3 种基金the National Key Research and Development Program(2021YFB2500300)the JBGS project from Ordos(JBGS2024001)the Tsinghua University Initiative Scientific Research Programthe“Shuimu Tsinghua Scholar Program of Tsinghua University”。
文摘1.Introduction Driven by the growing demand for energy storage systems in portable electronic devices,electric vehicles,and unmanned aerial vehicles,lithium-ion batteries(LIBs)have received considerable and sustained attention.The performance of routine LIBs is approaching the ceiling,particularly in terms of energy density,making it difficult to meet the ever-increasing demand for energy density[1].
基金supported by the National Natural Science Foundation of China(No.22109181,U24A2060,22279023,and 22309031)the National Key R&D Program of China(2024YFE0101100)+6 种基金the Hunan Provincial Science and Technology Plan Projects of China(No.2017TP1001)the Hunan Provincial Natural Science Foundation of China(No.2025JJ40011)the Fundamental Research Funds for the Central Universities(20720250005)the Science and Technology Commission of Shanghai Municipality(25DZ3002901,2024ZDSYS02,25PY2600100)the Shanghai Pilot Program for Basic Research-Fudan University 21TQ1400100(25TQ012)the AI for Science Foundation of Fudan University(FudanX24A1035)the National Research Foundation,Singapore,under its Singapore-China Joint Flagship Project(Clean Energy).
文摘Electrolytic Zn-MnO_(2)batteries arepromising candidates for safe and sustainable energystorage owing to their high voltage,environmentalbenignity,and cost-effectiveness.However,practicalapplications are hindered by the poor conductivity andthe irreversible dissolution of conventionalε-MnO_(2)deposits.Herein,we report a scalable semisolid slurryelectrode architecture that enables stable MnO_(2)deposition/dissolution using a three-dimensional percolatingnetwork of carbon nanotubes(CNTs)as both conductivematrix and deposition host.The slurry systempromotes the formation of highly conductiveγ-MnO_(2)owing to enhanced charge transfer kinetics,enablingoverall dissolution rather than the localized separationtypically seen in traditional electrodes.The Zn-MnO_(2)slurry cell exhibits a reversible areal capacity approaching 60 mAh cm^(-2).Moreover,theflowable nature of the slurry allows electrochemically inactive MnO_(2)formed during dissolution to be reconnected and reactivated by CNTs inthe rheological network,ensuring deep utilization and cycling stability.This work establishes a slurry electrode strategy to improve electrolyticMnO_(2)reactions and offers a viable pathway toward renewable aqueous batteries for grid-scale applications.
文摘Lithium–sulfur(Li–S)batteries are promisingcandidates for next-generation energy storagegiven their high energy density and potential low cost.Chemically activated carbon(CAC)is often used fortheir cathodes,because it has a high specific surfacearea for sulfur loading.We have developed a pressurizedphysical activation(PPA)method that producedan activated carbon(PPAC)with a high specific surfacearea comparable to that of CAC.The pore structure of PPAC could be changed and its use as a cathode material for Li–Sbatteries was investigated.Battery tests at different capacity rates(C-rates)showed that it had a much improved high-rate performancewith a discharge capacity of 900 mAh/(g of sulfur)at 1 C,in contrast to only 600 mAh/(g of sulfur)for CAC.Porestructure analyses showed that PPAC prepared at a high activation temperature(1000℃)had unusual channel-like mesoporesbetween the microdomains that are the basic structural units of artificial carbon materials.These are connected to microporesdeveloped in each microdomain,and deliver ions from the surroundings to the internal pores and vice versa.The well-developedmicropores and mesopores of PPAC respectively ensured the high adsorption of lithium polysulfides and a high rate ofion diffusion.Compared to CAC,PPAC is a high-performance,low-cost cathode material that is promising for use in futureLi–S batteries.
文摘Herein,3‑aminopropyltriethoxysilane(APTES)was used to modify F‑containing silica slag(SS)by simple grafting and served as a multifunctional barrier layer.The amino group(—NH2)in the amino‑modified SS(NH2‑SS)forms ligand bonds or hydrogen bonds with sulfur ions in lithium polysulfides(LiPSs),thus inhibiting the shuttle effect.Electrochemical analyses demonstrated that lithium‑sulfur(Li‑S)batteries employing the NH2‑SS interlayer exhibited discharge specific capacities of 1048 and 789 mAh·g^(-1) at 0.2C and 2C,respectively,and even at 4C,the initial discharge specific capacity remained at 590 mAh·g^(-1),outperforming the Li‑S battery with unmodified SS as the interlayer.
文摘Despite their high theoretical capacity and energy density,lithiumsulfur(Li–S)batteries still face challenges such as soluble lithium polysulfides(LiPSs)shuttling and sluggish redox kinetics.In this work,we used a novel MoS_(2)-Mo_(2)C heterostructure anchored on a carbon sponge(CS)as a Li_(2)S host to solve these problems.A simple hydrothermal process following carbothermal reduction was used to construct the MoS_(2)-Mo_(2)C heterostructure,enabling control of the phases and integration of MoS_(2) and Mo_(2)C.Structural characterization confirmed the coherent interface of the heterostructure with a precise orientation relationship between the two phases and their uniform distribution.An evaluation of the adsorption and catalytic performance of the material showed that it has an exceptional LiPSs adsorption capacity with faster conversion from Li_(2)S_(4) to Li_(2)S_(2).Density functional theory calculations further confirmed these results.As a result,the cathode had a high initial discharge capacity of 693 mAh g^(−1) at 0.2 C and achieved stable cycling at 2 C for 500 cycles with a low decay rate of 0.107%per cycle.The heterostructure design,coupled with the macroporous CS framework,effectively prevented the shuttling and increased sulfur utilization,offering a promising way to produce practical high-energydensity Li–S batteries.
文摘Li_(3)V_(2)(PO_(4))_(3) is a promising high-voltage cathode for zincion batteries,but it suffers from a poor electronic conductivity and vanadium dissolution in aqueous electrolytes.The growth of carboncoated Li_(3)V_(2)(PO_(4))_(3)(LVP@C)nanoparticles on carbon nanofibers(CNFs)has been achieved by an electrospinning technique followed by calcination.The protective carbon coating prevents the aggregation of the LVP nanoparticles and suppresses V dissolution by preventing direct contact with aqueous electrolytes.The CNFs derived from the electrospun nanofibers provide a 3D network to increase the electronic conductivity of the LVP electrode,and the LVP@C-CNF hybrid film can be directly used as a freestanding cathode for zinc-ion batteries without adding conductive additives and binders.A mechanism for the formation of a uniform and continuous carbon coating has been proposed.This nanostructure,combined with the uniform and intact carbon coverage,significantly increases the electronic conductivity.This LVP@C-CNF freestanding electrode has an excellent rate capability(47.3%retention at 2 C)and cycling stability(61.2%retention after 100 cycles)within the voltage range 0.6 V to 1.95 V and is highly suitable for zinc-ion battery applications.
文摘Understanding how aging influences the thermal hazards of lithium-ion batteries(LIBs)is critical for enhancing their safety across a wide range of applications.This study systematically investigates the thermal runaway(TR)behavior of LIBs,with particular emphasis on combined-pathway aging,evaluated in terms of normalized usable capacity(U_(E)).Key thermal safety parameters,i.e.,TR triggering temperature,mass loss,and heat generation under diverse aging conditions,are quantified.To enable a fair comparison,thermal hazards are evaluated based on equivalent usable capacity,revealing that aged cells exhibit lower TR triggering temperatures and higher heat generation than fresh cells under thermal abuse with elevated thermal risks.Mechanistic analysis identifies lithium plating,solid electrolyte interphase(SEI)formation,and lithium depletion,particularly under high-temperature charging,as the dominant contributors to increased hazard.Using an aging-stressor matrix,a trade-off between high-C-rateinduced thermal instability and high-temperature-induced thermal stability is discovered and quantified,underscoring the strong dependence of thermal hazards on specific aging pathways.This work advances the fundamental understanding of aging-induced safety risks in LIBs and offers practical guidance for the development of safer battery systems,optimized charging protocols,and improved battery management strategies across applications in electric vehicles,consumer electronics,and grid-scale energy storage.
基金financially supported by the National Natural Science Foundation of China (No.52372188)Natural Science Foundation of Henan (Nos.242300421625,252300421333)+4 种基金CAS Henan Industrial Technology Innovation & Incubation Center (No.2024121)Key Scientific Research Project of Education Department of Henan Province (Nos.22A150042,23A150038,and 24A150019)2023 Introduction of studying abroad talent programthe China Postdoctoral Science Foundation (No.2019 M652546)Key Project of Science and Technology of Henan Province (No.252102240007)。
文摘Aqueous zinc-ion batteries(AZIBs) are regarded as one of the most promising energy conversion and storage devices.Nevertheless,side reactions and dendrite growth on the zinc metal anode hinder their widespread application.In this study,hemin was employed as a multi-functional artificial interface for the first time to inhibit the disordered growth of zinc dendrites and mitigate side reactions.Theoretical calculations indicate that hemin is preferentially adsorbed onto the zinc anode,thus blocking the interaction between the active zinc anode and electrolyte.Compared with zinc foil,the Hemin@Zn anode demonstrates enhanced corrosion resistance,a decrease in hydrogen evolution,and more orderly deposition of zinc.As expected,the symmetric cell with Hemin@Zn anode can sustain up to 4000 h at 0.2 mA/cm^(2),0.2 mAh/cm^(2).Asymmetric Zn//Cu cells exhibit an average coulombic efficiency exceeding 99.72 % during 500 cycles.Moreover,the full cell Hemin@Zn//NH_(4)V_(4)O_(10) delivers a superior capacity up to 367 m Ah/g and the discharge capacity retention reaches 124 mAh/g after 1200 cycles even at a current density of 5 A/g.This work provides a simple and effective method for constructing a robust artificial interface to promote the application of long-life AZIBs.
基金financially supported by the National Natural Science Foundation of China (52272209)
文摘Niobium-based oxides show great potential in anode materials for fast-charging lithium-ion batteries,but their practical application remains hindered by intrinsically low conductivity.In this study,we successfully synthesize nano-sized Wadsley-Roth FeNb_(11)O_(29)through Fe-driven phase transformation of Nb_(2)O_(5),which delivers a high specific capacity(280.5 mA h g^(−1)at 0.25 C)along with abundant redox-active sites.Moreover,the Wadsley-Roth shear structure of FeNb_(11)O_(29)facilitates rapid Li^(+)diffusion and guarantees exceptional structural stability.Theoretical calculations further confirm that FeNb_(11)O_(29)has a narrow band gap,which significantly enhances the conductivity.Owing to these merits,FeNb_(11)O_(29)achieves a full charge/discharge cycle within merely 25 s at 75 C rate and retains remarkable cycling stability over 2500 cycles.As a consequence,our assembled FeNb_(11)O_(29)||LiFePO_(4)full cell demonstrates ultra-long cyclability(>10000 cycles)and outstanding fast-charging capability(complete cycling within 2 min at 30 C).These findings highlight nano-sized FeNb_(11)O_(29)as a highly promising anode candidate for next-generation fast-charging LIBs.
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MSIT)(No.2022M3H4A6A0103720142)the National Research Council of Science&Technology(NST)grant by the Korea government(MSIT)(No.GTL24011-000)+1 种基金the Technology Innovation Program(RS-2024-00404165)through the Korea Planning&Evaluation Institute of Industrial Technology(KEIT)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)supported by the Samsung SDI Co.Ltd.and the Korea Institute of Science and Technology(KIST)institutional program(2E33942,2E3394B)。
文摘Strategies for achieving high-energy-density lithium-ion batteries include using high-capacity materials such as high-nickel NCM,increasing the active material content in the electrode by utilizing high-conductivity carbon nanotubes(CNT)conductive materials,and electrode thickening.However,these methods are still limited due to the limitation in the capacity of high-nickel NCM,aggregation of CNT conductive materials,and nonuniform material distribution of thick-film electrodes,which ultimately damage the mechanical and electrical integrity of the electrode,leading to a decrease in electrochemical performance.Here,we present an integrated binder-CNT composite dispersion solution to realize a high-solids-content(>77 wt%)slurry for high-mass-loading electrodes and to mitigate the migration of binder and conductive additives.Indeed,the approach reduces solvent usage by approximately 30%and ensures uniform conductive additive-binder domain distribution during electrode manufacturing,resulting in improved coating quality and adhesive strength for high-mass-loading electrodes(>12 mAh cm^(−2)).In terms of various electrode properties,the presented electrode showed low resistance and excellent electrochemical properties despite the low CNT contents of 0.6 wt%compared to the pristine-applied electrode with 0.85 wt%CNT contents.Moreover,our strategy enables faster drying,which increases the coating speed,thereby offering potential energy savings and supporting carbon neutrality in wet-based electrode manufacturing processes.
基金financial support from the National Natural Science Foundation of China(52473248,52203123,52125301,22279070 and U21A20170)the State Key Laboratory of Polymer Materials Engineering(Grant No:sklpme 2023-1-05 and sklpme 2024-2-04)+3 种基金the Ministry of Science and Technology of China(No.2019YFA0705703)the Sichuan Science and Technology Program(2023NSFSC0991 and 2025ZNSFSC1411)the Fundamental Research Funds for the Central Universitiespartially sponsored by the Double First-Class Construction Funds of Sichuan University.
文摘The development of shape-customizable and bulk flexible electrochemical devices through processing technologies as versatile as those used for plastics promises to revolutionize the future of battery technology.However,this pursuit has been fundamentally hindered by the absence of transformative battery materials capable of delivering the necessary electrochemical functions,robust interface adhesion,and,crucially,the suitable rheological properties required for on-demand shaping.In this work,we introduce a concept of a multifunctional plasticine electrode matrix(PEM)featuring nano-interpenetrating networks(nano-IPN)to address this challenge.Utilizing the nonflammable liquid-electrolyte hydration combined with conductive nanomaterials,we have realized a PEM in the form of a multifunctional nanocomposite that integrates ion and electron conduction,component binding,non-flammability,and plasticine-like moldability.With this PEM,we have successfully fabricated a variety of bulk-flexible electrodes with high mass loading of active material(AM)(>70 wt%)using industry-friendly extrusion and compression molding techniques.Moreover,these high AM-loading composite electrodes achieve an unparalleled bulk conformability and flexibility,remaining structurally intact even under severe mechanical stress.Ultimately,we have successfully produced shape-patternable and flexible batteries via extrusion molding.This study underscores the potential of the PEM to revolutionize battery microstructures,interfaces,manufacturing processes,and performance characteristics.
基金supported by the National Key R&D Program of China(No.2022YFB3803400)National Natural Science Foundation of China(Nos.52102054,52020105010,51927803,52188101 and 52072378)+1 种基金Liaoning Province Science and Technology Planning Project(No.2022-BS-007)Fujian Science and Technology Program(No.2023T3025).
文摘Commercial carbonate electrolytes suffer from ion transport difficulty in bulk electrolytes and interphase at low temperatures,bringing challenges to the application of lithium-ion batteries(LIBs)at low temperatures.Herein,the ester solvent of methyl propionate(MP)with low melting point and low viscosity was used to tackle ion transport difficulty in electrolytes.Fluorinated ester was further added to accelerate interfacial transport through intermolecular interactions.The influence of fluorinated esters with different fluorination degrees on the solvation structure of electrolytes and the performance of batteries was further studied.As a result,methyl pentafluoropropionate(M5F)with five fluorine atoms was selected for its optimal interactions with both Li+and MP solvent in the primary solvation structure,contributing to desired solvation structure for fast interfacial transport.The LiFePO_(4)(LFP)||graphite cell with LiFSI-MP-M5F electrolyte exhibited a high cyclability of 85.8%after 120 cycles and retained 81.2%of room-temperature capacity when charged and discharged at−30℃.1 Ah LFP||graphite pouch cell with high cathode loading(20 mg/cm^(2))in LiFSI-MP-M5F electrolyte exhibited 0.85 Ah capacity when charged and discharged at−20℃.This work provides a guidance for electrolyte design by synergistic fluorinated and non-fluorinated solvents for LIBs at low-temperature application.
基金supported by Shaanxi Fundamental Science Research Project for Chemistry and Biology(23JHQ011)Natural Science Foundation of Shaanxi(2024JC-YBMS-115)Natural Science Basic Research Plan in Shaanxi Province of China(2025JC-YBMS-141)。
文摘The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.
基金supported by the National Natural Science Foundation of China(NSFC,Grant Nos.52222211 and 52472209)the State Key Laboratory of Materials-Oriented Chemical Engineering(Grant No.SKL-MCE-23A05)+1 种基金“333”Project of Jiangsu Provincethe Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Magnesium batteries are attracting growing interest as next-generation energy storage technology due to their high safety,cost-effectiveness,and resource abundance.However,their development remains limited by sluggish Mg^(2+)transport kinetics at the electrode/electrolyte interface.Herein,we propose an electrolyte design strategy that modulates the Mg^(2+)solvation structure by introducing tetrahydrofuran(THF)as a co-solvent into a borate-based electrolyte,Mg[B(hfip)_(4)](MBF)in dimethoxyethane(DME).THF,selected from a series of linear and cyclic ethers,has a comparable dielectric constant and donor number to DME,but its cyclic structure introduces steric hindrance that induces competitive coordination with Mg^(2+).This competition weakens Mg^(2+)-solvent interactions,yielding a more labile solvation structure and enhanced desolvation kinetics.As a result,Mg||Mg cells employing the optimized MBF/1D1T electrolyte(DME:THF=1:1,v:v)exhibit a significantly reduced Mg plating/stripping overpotential of 120 mV at 10 mA cm^(-2),compared with 316 mV at 8 mA cm^(-2)with MBF/DME,along with exceptional cycling stability exceeding 1200 h.Furthermore,representative sulfide cathodes such as CuS and VS_(4)demonstrate faster activation and improved high-rate performance in the presence of MBF/1D1T.
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.
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 by the National Natural Science Foundation of China(5257043994)the Natural Science Foundation of Yunnan Province(202501AS070125,202501CF070129)+1 种基金the Innovation Capacity Construction and Enhancement Projects of Engineering Research Center of Yunnan Province(2023-XMDJ-00617107)the Scientific and Technological Project of Yunnan Precious Metals Laboratory(YPML-20240502015).
文摘The principal challenge in optimizing biomass-derived hard carbon(HC)is the concurrent enhancement of specific capacity,cycling durability,and rate performance,as these properties are closely related to the disordered carbon network and abundant pore structure.However,inadequate controllability of morphology,insufficiently regulated pore structures,and the complexity of post-processing modifications hinders the practical application of HC.In this work,a high-temperature and high-pressure expansion pretreatment technique is proposed to regulate the structure of starch precursors,enabling the precise design of ordered graphitic-like microcrystals and closed pores within HC.The optimized starch-based HC displayed remarkable electrochemical efficiency,with a reversible capacity of 332.0 mAh g^(-1),an initial Coulombic efficiency of 90.4%,and stable cycling over 3000 cycles.Meanwhile,advanced full-cell utilizing Na4Fe3(PO_(4))_(2)P_(2)O_(7) cathode achieve stable cycling performance exceeding 1000 cycles,demonstrating outstanding performance.This research innovatively employs a green expansion process to achieve structural regulation of HC,thereby providing an environmentally friendly and economically viable technical pathway for its large-scale production.
基金supported by the introduction of Talent Research Fund in Nanjing Institute of Technology(YKJ202204)the National Natural Science Foundation of China(52401282 and 52300206)the Natural Science Foundation of Jiangsu Province(BK20230701 and BK20230705).
文摘Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.
基金supported by the Shanghai Pujiang Program(24PJA090).
文摘Solar energy represents a transformative,inexhaustible,and eco-friendly solution for sustainable power generation.However,its intermittent nature requires efficient energy storage technologies to maximize utilization.A promising approach involves integrating photoactive materials into the cathodes of zinc-ion batteries(ZIBs),enabling direct solar energy capture and storage while improving electrochemical performance.This review systematically explores the emerging field of light-driven ZIBs(LDZIBs),focusing on two main operational modes:photo-assisted ZIBs(PAZIBs),where light enhances battery performance,and photo-rechargeable ZIBs(PRZIBs),which can be directly charged by light without external power sources.We comprehensively examine the classification,working mechanisms,and material integration strategies for these systems.Key advances in electrode design,innovative materials,and potential application scenarios for both PAZIBs and PRZIBs are highlighted.Finally,we discuss the major challenges and future research directions aimed at improving the efficiency,stability,and scalability of LDZIBs to facilitate their commercialization as a cornerstone technology for future solar energy storage.
