The microstructure design for thermal conduction pathways in polymeric electrical encapsulation materials is essential to meet the stringent requirements for efficient thermal management and thermal runaway safety in ...The microstructure design for thermal conduction pathways in polymeric electrical encapsulation materials is essential to meet the stringent requirements for efficient thermal management and thermal runaway safety in modern electronic devices.Hence,a composite with three-dimensional network(Ho/U-BNNS/WPU)is developed by simultaneously incorporating magnetically modified boron nitride nanosheets(M@BNNS)and non-magnetic organo-grafted BNNS(U-BNNS)into waterborne polyurethane(WPU)to synchronous molding under a horizontal magnetic field.The results indicate that the continuous in-plane pathways formed by M@BNNS aligned along the magnetic field direction,combined with the bridging structure established by U-BNNS,enable Ho/U-BNNS/WPU to exhibit exceptional in-plane(λ//)and through-plane thermal conductivities(λ_(⊥)).In particular,with the addition of 30 wt%M@BNNS and 5 wt%U-BNNS,theλ//andλ_(⊥)of composites reach 11.47 and 2.88 W m^(-1) K^(-1),respectively,which representing a 194.2%improvement inλ_(⊥)compared to the composites with a single orientation of M@BNNS.Meanwhile,Ho/U-BNNS/WPU exhibits distinguished thermal management capabilities as thermal interface materials for LED and chips.The composites also demonstrate excellent flame retardancy,with a peak heat release and total heat release reduced by 58.9%and 36.9%,respectively,compared to WPU.Thus,this work offers new insights into the thermally conductive structural design and efficient flame-retardant systems of polymer composites,presenting broad application potential in electronic packaging fields.展开更多
The implementation of ultrahigh-Ni cathodes in high-energy lithium-ion batteries(LIBs)is constrained by significant structural and interfacial degradation during cycling.In this study,doping-induced surface restructur...The implementation of ultrahigh-Ni cathodes in high-energy lithium-ion batteries(LIBs)is constrained by significant structural and interfacial degradation during cycling.In this study,doping-induced surface restructuring in ultrahigh-nickel cathode materials is rapidly facilitated through an ultrafast Joule heating method.Density functional theory(DFT)calculations,synchrotron X-ray absorption spectroscopy(XAS),and single-particle force test confirmed the establishment of a stable crystal framework and lattice oxygen,which mitigated H2-H3 phase transitions and improved structural reversibility.Additionally,the Sc doping process exhibits a pinning effect on the grain boundaries,as shown by scanning transmission electron microscopy(STEM),enhancing Li~+diffusion kinetics and decreasing mechanical strain during cycling.The in situ development of a cation-mixing layer at grain boundaries also creates a robust cathode/electrolyte interphase,effectively reducing interfacial parasitic reactions and transition metal dissolution,as validated by STEM and time-of-flight secondary ion mass spectrometry(TOF-SIMS).These synergistic modifications reduce particle cracking and surface/interface degradation,leading to enhanced rate capability,structural integrity,and thermal stability.Consequently,the optimized Sc-modified ultrahigh-Ni cathode(Sc-1)exhibits 93.99%capacity retention after 100 cycles at 1 C(25℃)and87.06%capacity retention after 100 cycles at 1 C(50℃),indicating excellent cycling and thermal stability.By presenting a one-step multifunctional modification approach,this research delivers an extensive analysis of the mechanisms governing the structure,microstructure,and interface properties of nickel-rich layered cathode materials(NCMs).These results underscore the potential of ultrahigh-Ni cathodes as viable candidates for advanced lithium-ion batteries(LIBs)in next-generation electric vehicles(EVs).展开更多
MnCO_(3)represents a potentially high-capacity and low-cost anode candidate to replace graphite for enhancing energy density of commercial lithium-ion batteries,but it suffers from poor electrical conductivity and ser...MnCO_(3)represents a potentially high-capacity and low-cost anode candidate to replace graphite for enhancing energy density of commercial lithium-ion batteries,but it suffers from poor electrical conductivity and serious volumetric change,largely hindering its practical applications.展开更多
Lithium metal anode is one of the ideal anode materials for the next generation of high-energy-density battery systems.Unfortunately,the uneven nucleation of Li leads to dendrite growth and volume changes during cycli...Lithium metal anode is one of the ideal anode materials for the next generation of high-energy-density battery systems.Unfortunately,the uneven nucleation of Li leads to dendrite growth and volume changes during cycling,resulting in poor electrochemical performance and potential safety hazards,which hinder its practical application.In this work,a low-cost chicken-bonederived carbon material(CBC)with a biomimetic structure was designed and synthesized using a simple one-step carbonization method.Combining theoretical calculations and experimental results,the self-doped N and S heteroatoms in CBC are demonstrated to effectively reduce the binding energy with Li atoms and lower the nucleation overpotential.After uniform nucleation,the Li metal grows in a spherical shape without dendrites,which is related to the reduction of the local current density inside the biomimetic crosslinking structure of CBC.Benefiting from this favorable Li growth behavior,the Li@CBC electrode achieves ultra-low nucleation overpotential(15.5 mV at 0.1 mA cm^(−2))and superdense lithium deposition(zero volume expansion rate at a capacity of 2 mAh cm^(−2))without introducing additional lithiophilic sites.The CBC retains a high Coulombic efficiency of over 98%in 479 cycles(1 mA cm^(−2)and 1 mAh cm^(−2))when applied in a half-cell with Li,and shows an excellent rate and cycling performance when applied in a full cell with LiFePO4 as the cathode.展开更多
Aqueous zinc-ion batteries(AZIBs)are pivotal for achieving net-zero goals,yet their commercialization is impeded by zinc dendrites,parasitic reactions,and interfacial instability.Current debates persist on the interpl...Aqueous zinc-ion batteries(AZIBs)are pivotal for achieving net-zero goals,yet their commercialization is impeded by zinc dendrites,parasitic reactions,and interfacial instability.Current debates persist on the interplay between zincophilic-hydrophilic and zincophobic-hydrophobic interactions at the anode-electrolyte interface.Herein,a conceptual framework that decouples these competing effects was proposed,enabling the rational design of a dual-layer architecture with an inner zincophilic layer for Zn^(2+)flux homogenization and an outer hydrophobic layer for water shielding.Through in situ and ex situ analyses,the synergistic mechanism was elucidated.During the cycling process,the zincophilic interface guides uniform Zn deposition,while the hydrophobic coating suppresses H_(2)O-induced side reactions.This dual modification achieves a Zn||Cu cell with an unprecedented 99.89%Coulombic efficiency and 975-cycle stability.This work resolves the long-standing controversy over interfacial affinity design,offering a scalable and industrially viable strategy to enhance AZIBs’durability without sacrificing energy density.展开更多
The burgeoning growth in electric vehicles and portable energy storage systems necessitates advances in the energy density and cost-effectiveness of lithium-ion batteries(LIBs),areas where lithium-rich manganese-based...The burgeoning growth in electric vehicles and portable energy storage systems necessitates advances in the energy density and cost-effectiveness of lithium-ion batteries(LIBs),areas where lithium-rich manganese-based oxide(LLO)materials naturally stand out.Despite their inherent advantages,these materials encounter significant practical hurdles,including low initial Coulombic efficiency(ICE),diminished cycle/rate performance,and voltage fading during cycling,hindering their widespread adoption.In response,we introduce an ionic-electronic dual-conductive(IEDC)surface control strategy that integrates an electronically conductive graphene framework with an ionically conductive heteroepitaxial spinel Li_(4)Mn_(5)O_(12)layer.Prolonged electrochemical and structural analyses demonstrate that this IEDC heterostructure effectively minimizes polarization,mitigates structural distortion,and enhances electronic/ionic diffusion.Density functional theory calculations highlight an extensive Li^(+)percolation network and lower Li^(+)migration energies at the layered-spinel interface.The designed LLO cathode with IEDC interface engineering(LMOSG)exhibits improved ICE(82.9%at 0.1 C),elevated initial discharge capacity(296.7 mAh g^(-1)at 0.1 C),exceptional rate capability(176.5 mAh g^(-1)at 5 C),and outstanding cycle stability(73.7%retention at 5 C after 500 cycles).These findings and the novel dual-conductive surface architecture design offer promising directions for advancing highperformance electrode materials.展开更多
The rapid expansion of the automotive sector has significantly increased the demand for highperformance lithium-ion batteries,positioning Ni-rich layered cathodes as a promising solution due to their high energy densi...The rapid expansion of the automotive sector has significantly increased the demand for highperformance lithium-ion batteries,positioning Ni-rich layered cathodes as a promising solution due to their high energy density and cost-efficiency.However,these cathodes face critical challenges,including thermal instability and structural degradation at an elevated temperature,which hinder their practical application.This study introduces an advanced surface reconstruction strategy combining a LiScF_(4)coating,Sc/F surface co-doping,and a cation-mixing layer to address these issues.The LiScF_(4)coating serves as a durable protective barrier,reducing electrolyte decomposition,minimizing transition metal dissolution,and enhancing lithium-ion transport.Sc/F surface co-doping stabilizes lattice oxygen by increasing the energy barrier for oxygen vacancy formation and minimizing oxygen release,thereby suppressing phase transitions and interfacial side reactions.Additionally,the cation-mixing layer improves interfacial stability by alleviating lattice strain and supporting reversible cation migration,ensuring prolonged durability during cycling and under high-temperature conditions.These integrated modifications work synergistically to mitigate various degradation mechanisms,significantly improving the thermal stability,structural integrity,and electrochemical performance of Ni-rich cathodes.This approach offers a viable pathway for incorporating Ni-rich cathodes into advanced lithium-ion batteries,making them well-suited for applications requiring high thermal stability.Moreover,this research provides valuable guidance for the development of a multi-component modification strategy,paving the way for future innovations in energy storage materials and advancing high-performance battery technology.展开更多
Lithium metal is a compelling choice as an anode material for high-energy-density batteries,attributed to its elevated theoretical specific energy and low redox potential.Nevertheless,challenges arise due to its susce...Lithium metal is a compelling choice as an anode material for high-energy-density batteries,attributed to its elevated theoretical specific energy and low redox potential.Nevertheless,challenges arise due to its susceptibility to high-volume changes and the tendency for dendritic development during cycling,leading to restricted cycle life and diminished Coulombic efficiency(CE).Here,we innovatively engineered a kind of porous biocarbon to serve as the framework for a lithium metal anode,which boasts a heightened specific surface area and uniformly dispersed ZnO active sites,directly derived from metasequoia cambium.The porous structure efficiently mitigates local current density and alleviates the volume expansion of lithium.Also,incorporating the ZnO lithiophilic site notably reduces the nucleation overpotential to a mere 16 mV,facilitating the deposition of lithium in a compact form.As a result,this innovative material ensures an impressive CE of 98.5%for lithium plating/stripping over 500 cycles,a remarkable cycle life exceeding 1200 h in a Li symmetrical cell,and more than 82%capacity retention ratio after an astonishing 690 cycles in full cells.In all,such a rationally designed Li composite anode effectively mitigates volume change,enhances lithophilicity,and reduces local current density,thereby inhibiting dendrite formation.The preparation of a highperformance lithium anode frame proves the feasibility of using biocarbon in a lithium anode frame.展开更多
Alzheimer's disease is characterized by two major neuropathological hallmarks—the extracellularβ-amyloid plaques and intracellular neurofibrillary tangles consisting of aggregated and hyperphosphorylated Tau pro...Alzheimer's disease is characterized by two major neuropathological hallmarks—the extracellularβ-amyloid plaques and intracellular neurofibrillary tangles consisting of aggregated and hyperphosphorylated Tau protein.Recent studies suggest that dysregulation of the microtubuleassociated protein Tau,especially specific proteolysis,could be a driving force for Alzheimer's disease neurodegeneration.Tau physiologically promotes the assembly and stabilization of microtubules,whereas specific truncated fragments are sufficient to induce abnormal hyperphosphorylation and aggregate into toxic oligomers,resulting in them gaining prion-like characteristics.In addition,Tau truncations cause extensive impairments to neural and glial cell functions and animal cognition and behavior in a fragment-dependent manner.This review summarizes over 60 proteolytic cleavage sites and their corresponding truncated fragments,investigates the role of specific truncations in physiological and pathological states of Alzheimer's disease,and summarizes the latest applications of strategies targeting Tau fragments in the diagnosis and treatment of Alzheimer's disease.展开更多
Sodium-ion batteries(SIBs)with advantages of abundant resource and low cost have emerged as promising candidates for the next-generation energy storage systems.However,safety issues existing in electrolytes,anodes,and...Sodium-ion batteries(SIBs)with advantages of abundant resource and low cost have emerged as promising candidates for the next-generation energy storage systems.However,safety issues existing in electrolytes,anodes,and cathodes bring about frequent accidents regarding battery fires and explosions and impede the development of high-performance SIBs.Therefore,safety analysis and high-safety battery design have become prerequisites for the development of advanced energy storage systems.The reported reviews that only focus on a specific issue are difficult to provide overall guidance for building high-safety SIBs.To overcome the limitation,this review summarizes the recent research progress from the perspective of key components of SIBs for the first time and evaluates the characteristics of various improvement strategies.By orderly analyzing the root causes of safety problems associated with different components in SIBs(including electrolytes,anodes,and cathodes),corresponding improvement strategies for each component were discussed systematically.In addition,some noteworthy points and perspectives including the chain reaction between security issues and the selection of improvement strategies tailored to different needs have also been proposed.In brief,this review is designed to deepen our understanding of the SIBs safety issues and provide guidance and assistance for designing high-safety SIBs.展开更多
Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes of...Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes often declines because of capacity fading during cycling. This decline is primarily attributed to anisotropic lattice strain and oxygen release from cathode surfaces. Given notable structural transformations, complex redox reactions, and detrimental interface side reactions in LRMOs, the development of a single modification approach that addresses bulk and surface issues is challenging. Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions. The internal spinel-like phase coating layer, featuring threedimensional(3D) lithium-ion diffusion channels, effectively blocks oxygen release from the cathode surface and mitigates lattice strain. In addition, the external Li_(3)PO_(4) coating layer, noted for its superior corrosion resistance, enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals. Notably, the spinel phase, as excellent interlayer, securely anchors Li_(3)PO_(4) to the bulk lattice and suppresses oxygen release from lattices. Consequently, these modifications considerably boost structural stability and durability, achieving an impressive capacity retention of 83.4% and a minimal voltage decay of 1.49 m V per cycle after 150 cycles at 1 C. These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability.展开更多
The rapid development of electric vehicles and portable energy storage systems demands improvements in the energy density and cost-effectiveness of lithium-ion batteries,a domain in which Lithium-rich layered cathode(...The rapid development of electric vehicles and portable energy storage systems demands improvements in the energy density and cost-effectiveness of lithium-ion batteries,a domain in which Lithium-rich layered cathode(LLO)materials inherently excel.However,these materials face practical challenges,such as low initial Coulombic efficiency,inferior cycle/rate performance,and voltage decline during cycling,which limit practical application.Our study introduces a surface multi-component integration strategy that incorporates oxygen vacancies into the pristine LLO material Li1.2Mn_(0.6)Ni_(0.2)O_(2).This process involves a brief citric acid treatment followed by calcination,aiming to explore rate-dependent degradation behavior.The induced surface oxygen vacancies can reduce surface oxygen partial pressure and diminish the generation of O_(2)and other highly reactive oxygen species on the surface,thereby facilitating the activation of Li ions trapped in tetrahedral sites while overcoming transport barriers.Additionally,the formation of a spinel-like phase with 3D Li+diffusion channels significantly improves Li^(+)diffusion kinetics and stabilizes the surface structure.The optimally modified sample boasts a discharge capacity of 299.5 mA h g^(-1)at a 0.1 C and 251.6 mA h g^(-1)at a 1 C during the initial activation cycle,with an impressive capacity of 222.1 mA h g^(-1)at a 5 C.Most notably,it retained nearly 70%of its capacity after 300 cycles at this elevated rate.This straightforward,effective,and highly viable modification strategy provides a crucial resolution for overcoming challenges associated with LLO materials,making them more suitable for practical application.展开更多
Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For ins...Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.展开更多
Single-crystal Ni-rich cathodes are a promising candidate for high-energy lithium-ion batteries due to their higher structural and cycling stability than polycrystalline materials.However,the phase evolution and capac...Single-crystal Ni-rich cathodes are a promising candidate for high-energy lithium-ion batteries due to their higher structural and cycling stability than polycrystalline materials.However,the phase evolution and capacity degradation of these single-crystal cathodes during continuous lithation/delithation cycling remains unclear.Understanding the mapping relationship between the macroscopic electrochemical properties and the material physicochemical properties is crucial.Here,we investigate the correlation between the physical-chemical characteristics,phase transition,and capacity decay using capacity differential curve feature identification and in-situ X-ray spectroscopic imaging.We systematically clarify the dominant mechanism of phase evolution in aging cycling.Appropriately high cut-off voltages can mitigate the slow kinetic and electrochemical properties of single-crystal cathodes.We also find that second-order differential capacity discharge characteristic curves can be used to identify the crystal structure disorder of Ni-rich cathodes.These findings constitute a step forward in elucidating the correlation between the electrochemical extrinsic properties and the physicochemical intrinsic properties and provide new perspectives for failure analysis of layered electrode materials.展开更多
Aqueous Zn^(2+)-ion batteries(AZIBs),recognized for their high security,reliability,and cost efficiency,have garnered considerable attention.However,the prevalent issues of dendrite growth and parasitic reactions at t...Aqueous Zn^(2+)-ion batteries(AZIBs),recognized for their high security,reliability,and cost efficiency,have garnered considerable attention.However,the prevalent issues of dendrite growth and parasitic reactions at the Zn electrode interface significantly impede their practical application.In this study,we introduced a ubiquitous biomolecule of phenylalanine(Phe)into the electrolyte as a multifunctional additive to improve the reversibility of the Zn anode.Leveraging its exceptional nucleophilic characteristics,Phe molecules tend to coordinate with Zn^(2+)ions for optimizing the solvation environment.Simultaneously,the distinctive lipophilicity of aromatic amino acids empowers Phe with a higher adsorption energy,enabling the construction of a multifunctional protective interphase.The hydrophobic benzene ring ligands act as cleaners for repelling H_(2)O molecules,while the hydrophilic hydroxyl and carboxyl groups attract Zn^(2+)ions for homogenizing Zn^(2+)flux.Moreover,the preferential reduction of Phe molecules prior to H_(2)O facilitates the in situ formation of an organic-inorganic hybrid solid electrolyte interphase,enhancing the interfacial stability of the Zn anode.Consequently,Zn||Zn cells display improved reversibility,achieving an extended cycle life of 5250 h.Additionally,Zn||LMO full cells exhibit enhanced cyclability of retaining 77.3%capacity after 300 cycles,demonstrating substantial potential in advancing the commercialization of AZIBs.展开更多
The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Her...The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Herein,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the ICE.The thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical performance.The SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic products.Thus,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G anodes.LHCE also leads to uniform decomposition and high stability of the SEI with abundant organic components.As a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 C.NCM 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.展开更多
基金support from the National Natural Science Foundation of China(22268025,52473083,and 22475176)Key Research and Development Program of Yunnan Province(202403AP140036)+2 种基金Natural Science Basic Research Program of Shaanxi(2024JC-TBZC-04)Applied Basic Research Program of Yunnan Province(202201AT070115 and 202201BE070001-031)supported by the Innovation Capability Support Program of Shaanxi(2024RS-CXTD-57).
文摘The microstructure design for thermal conduction pathways in polymeric electrical encapsulation materials is essential to meet the stringent requirements for efficient thermal management and thermal runaway safety in modern electronic devices.Hence,a composite with three-dimensional network(Ho/U-BNNS/WPU)is developed by simultaneously incorporating magnetically modified boron nitride nanosheets(M@BNNS)and non-magnetic organo-grafted BNNS(U-BNNS)into waterborne polyurethane(WPU)to synchronous molding under a horizontal magnetic field.The results indicate that the continuous in-plane pathways formed by M@BNNS aligned along the magnetic field direction,combined with the bridging structure established by U-BNNS,enable Ho/U-BNNS/WPU to exhibit exceptional in-plane(λ//)and through-plane thermal conductivities(λ_(⊥)).In particular,with the addition of 30 wt%M@BNNS and 5 wt%U-BNNS,theλ//andλ_(⊥)of composites reach 11.47 and 2.88 W m^(-1) K^(-1),respectively,which representing a 194.2%improvement inλ_(⊥)compared to the composites with a single orientation of M@BNNS.Meanwhile,Ho/U-BNNS/WPU exhibits distinguished thermal management capabilities as thermal interface materials for LED and chips.The composites also demonstrate excellent flame retardancy,with a peak heat release and total heat release reduced by 58.9%and 36.9%,respectively,compared to WPU.Thus,this work offers new insights into the thermally conductive structural design and efficient flame-retardant systems of polymer composites,presenting broad application potential in electronic packaging fields.
基金supported by the National Key R&D Program of China(2022YFB3803501)the National Natural Science Foundation of China(22179008,22209156)+5 种基金support from the Beijing Nova Program(20230484241)support from the China Postdoctoral Science Foundation(2024M754084)the Postdoctoral Fellowship Program of CPSF(GZB20230931)support from beamline BL08U1A of Shanghai Synchrotron Radiation Facility(2024-SSRF-PT-506950)beamline 1W1B of the Beijing Synchrotron Radiation Facility(2021-BEPC-PT-006276)support from Initial Energy Science&Technology Co.,Ltd(IEST)。
文摘The implementation of ultrahigh-Ni cathodes in high-energy lithium-ion batteries(LIBs)is constrained by significant structural and interfacial degradation during cycling.In this study,doping-induced surface restructuring in ultrahigh-nickel cathode materials is rapidly facilitated through an ultrafast Joule heating method.Density functional theory(DFT)calculations,synchrotron X-ray absorption spectroscopy(XAS),and single-particle force test confirmed the establishment of a stable crystal framework and lattice oxygen,which mitigated H2-H3 phase transitions and improved structural reversibility.Additionally,the Sc doping process exhibits a pinning effect on the grain boundaries,as shown by scanning transmission electron microscopy(STEM),enhancing Li~+diffusion kinetics and decreasing mechanical strain during cycling.The in situ development of a cation-mixing layer at grain boundaries also creates a robust cathode/electrolyte interphase,effectively reducing interfacial parasitic reactions and transition metal dissolution,as validated by STEM and time-of-flight secondary ion mass spectrometry(TOF-SIMS).These synergistic modifications reduce particle cracking and surface/interface degradation,leading to enhanced rate capability,structural integrity,and thermal stability.Consequently,the optimized Sc-modified ultrahigh-Ni cathode(Sc-1)exhibits 93.99%capacity retention after 100 cycles at 1 C(25℃)and87.06%capacity retention after 100 cycles at 1 C(50℃),indicating excellent cycling and thermal stability.By presenting a one-step multifunctional modification approach,this research delivers an extensive analysis of the mechanisms governing the structure,microstructure,and interface properties of nickel-rich layered cathode materials(NCMs).These results underscore the potential of ultrahigh-Ni cathodes as viable candidates for advanced lithium-ion batteries(LIBs)in next-generation electric vehicles(EVs).
基金supported by the National Natural Science Foundation of China(Nos.52102088 and 22075026)support from Teli Fellowship,Beijing Institute of Technology,and facility support from Analysis&Testing Center,and Experimental Center of Materials Sciences&Engineering at Beijing Institute of Technology.
文摘MnCO_(3)represents a potentially high-capacity and low-cost anode candidate to replace graphite for enhancing energy density of commercial lithium-ion batteries,but it suffers from poor electrical conductivity and serious volumetric change,largely hindering its practical applications.
基金National Natural Science Foundation of China,Grant/Award Numbers:22179005,92372207。
文摘Lithium metal anode is one of the ideal anode materials for the next generation of high-energy-density battery systems.Unfortunately,the uneven nucleation of Li leads to dendrite growth and volume changes during cycling,resulting in poor electrochemical performance and potential safety hazards,which hinder its practical application.In this work,a low-cost chicken-bonederived carbon material(CBC)with a biomimetic structure was designed and synthesized using a simple one-step carbonization method.Combining theoretical calculations and experimental results,the self-doped N and S heteroatoms in CBC are demonstrated to effectively reduce the binding energy with Li atoms and lower the nucleation overpotential.After uniform nucleation,the Li metal grows in a spherical shape without dendrites,which is related to the reduction of the local current density inside the biomimetic crosslinking structure of CBC.Benefiting from this favorable Li growth behavior,the Li@CBC electrode achieves ultra-low nucleation overpotential(15.5 mV at 0.1 mA cm^(−2))and superdense lithium deposition(zero volume expansion rate at a capacity of 2 mAh cm^(−2))without introducing additional lithiophilic sites.The CBC retains a high Coulombic efficiency of over 98%in 479 cycles(1 mA cm^(−2)and 1 mAh cm^(−2))when applied in a half-cell with Li,and shows an excellent rate and cycling performance when applied in a full cell with LiFePO4 as the cathode.
基金supported by the National Natural Science Foundation of China(U2130204)the Joint Funds of the National Key R&D Program of China(2022YFB2502102)+1 种基金the Young Elite Scientists Sponsorship Program by CAST(YESS20200364)the Beijing Outstanding Young Scientists Program(BJJWZYJH01201910007023)。
文摘Aqueous zinc-ion batteries(AZIBs)are pivotal for achieving net-zero goals,yet their commercialization is impeded by zinc dendrites,parasitic reactions,and interfacial instability.Current debates persist on the interplay between zincophilic-hydrophilic and zincophobic-hydrophobic interactions at the anode-electrolyte interface.Herein,a conceptual framework that decouples these competing effects was proposed,enabling the rational design of a dual-layer architecture with an inner zincophilic layer for Zn^(2+)flux homogenization and an outer hydrophobic layer for water shielding.Through in situ and ex situ analyses,the synergistic mechanism was elucidated.During the cycling process,the zincophilic interface guides uniform Zn deposition,while the hydrophobic coating suppresses H_(2)O-induced side reactions.This dual modification achieves a Zn||Cu cell with an unprecedented 99.89%Coulombic efficiency and 975-cycle stability.This work resolves the long-standing controversy over interfacial affinity design,offering a scalable and industrially viable strategy to enhance AZIBs’durability without sacrificing energy density.
基金National Natural Science Foundation of China,Grant/Award Numbers:22179008,21875022Yibin“Jie Bang Gua Shuai”,Grant/Award Number:2022JB004+2 种基金Beijing Nova Program,Grant/Award Number:20230484241Postdoctoral Fellowship Program of CPSF,Grant/Award Number:GZB20230931Special Support of Chongqing Postdoctoral Research Project,Grant/Award Number:2023CQBSHTB2041。
文摘The burgeoning growth in electric vehicles and portable energy storage systems necessitates advances in the energy density and cost-effectiveness of lithium-ion batteries(LIBs),areas where lithium-rich manganese-based oxide(LLO)materials naturally stand out.Despite their inherent advantages,these materials encounter significant practical hurdles,including low initial Coulombic efficiency(ICE),diminished cycle/rate performance,and voltage fading during cycling,hindering their widespread adoption.In response,we introduce an ionic-electronic dual-conductive(IEDC)surface control strategy that integrates an electronically conductive graphene framework with an ionically conductive heteroepitaxial spinel Li_(4)Mn_(5)O_(12)layer.Prolonged electrochemical and structural analyses demonstrate that this IEDC heterostructure effectively minimizes polarization,mitigates structural distortion,and enhances electronic/ionic diffusion.Density functional theory calculations highlight an extensive Li^(+)percolation network and lower Li^(+)migration energies at the layered-spinel interface.The designed LLO cathode with IEDC interface engineering(LMOSG)exhibits improved ICE(82.9%at 0.1 C),elevated initial discharge capacity(296.7 mAh g^(-1)at 0.1 C),exceptional rate capability(176.5 mAh g^(-1)at 5 C),and outstanding cycle stability(73.7%retention at 5 C after 500 cycles).These findings and the novel dual-conductive surface architecture design offer promising directions for advancing highperformance electrode materials.
基金supported by the National Natural Science Foundation of China(22179008)support from the Beijing Nova Program(20230484241)+1 种基金support from the China Postdoctoral Science Foundation(2024M754084)the Postdoctoral Fellowship Program of CPSF(GZB20230931)。
文摘The rapid expansion of the automotive sector has significantly increased the demand for highperformance lithium-ion batteries,positioning Ni-rich layered cathodes as a promising solution due to their high energy density and cost-efficiency.However,these cathodes face critical challenges,including thermal instability and structural degradation at an elevated temperature,which hinder their practical application.This study introduces an advanced surface reconstruction strategy combining a LiScF_(4)coating,Sc/F surface co-doping,and a cation-mixing layer to address these issues.The LiScF_(4)coating serves as a durable protective barrier,reducing electrolyte decomposition,minimizing transition metal dissolution,and enhancing lithium-ion transport.Sc/F surface co-doping stabilizes lattice oxygen by increasing the energy barrier for oxygen vacancy formation and minimizing oxygen release,thereby suppressing phase transitions and interfacial side reactions.Additionally,the cation-mixing layer improves interfacial stability by alleviating lattice strain and supporting reversible cation migration,ensuring prolonged durability during cycling and under high-temperature conditions.These integrated modifications work synergistically to mitigate various degradation mechanisms,significantly improving the thermal stability,structural integrity,and electrochemical performance of Ni-rich cathodes.This approach offers a viable pathway for incorporating Ni-rich cathodes into advanced lithium-ion batteries,making them well-suited for applications requiring high thermal stability.Moreover,this research provides valuable guidance for the development of a multi-component modification strategy,paving the way for future innovations in energy storage materials and advancing high-performance battery technology.
基金supported by the National Natural Science Foundation of China(22179005,92372207)Fundamental Research Funds for the Central Universities(2022CX01017).
文摘Lithium metal is a compelling choice as an anode material for high-energy-density batteries,attributed to its elevated theoretical specific energy and low redox potential.Nevertheless,challenges arise due to its susceptibility to high-volume changes and the tendency for dendritic development during cycling,leading to restricted cycle life and diminished Coulombic efficiency(CE).Here,we innovatively engineered a kind of porous biocarbon to serve as the framework for a lithium metal anode,which boasts a heightened specific surface area and uniformly dispersed ZnO active sites,directly derived from metasequoia cambium.The porous structure efficiently mitigates local current density and alleviates the volume expansion of lithium.Also,incorporating the ZnO lithiophilic site notably reduces the nucleation overpotential to a mere 16 mV,facilitating the deposition of lithium in a compact form.As a result,this innovative material ensures an impressive CE of 98.5%for lithium plating/stripping over 500 cycles,a remarkable cycle life exceeding 1200 h in a Li symmetrical cell,and more than 82%capacity retention ratio after an astonishing 690 cycles in full cells.In all,such a rationally designed Li composite anode effectively mitigates volume change,enhances lithophilicity,and reduces local current density,thereby inhibiting dendrite formation.The preparation of a highperformance lithium anode frame proves the feasibility of using biocarbon in a lithium anode frame.
基金supported by the Neural Regeneration Co-innovation Center of Jiangsu Province,Nantong University(to DC)the National Natural Science Foundation of China,Nos.81872853(to DC),81870941(to JHG)the Science and Technology Project of Nantong City,Nos.JC22022022(to FW)and JC2021059(to JM)。
文摘Alzheimer's disease is characterized by two major neuropathological hallmarks—the extracellularβ-amyloid plaques and intracellular neurofibrillary tangles consisting of aggregated and hyperphosphorylated Tau protein.Recent studies suggest that dysregulation of the microtubuleassociated protein Tau,especially specific proteolysis,could be a driving force for Alzheimer's disease neurodegeneration.Tau physiologically promotes the assembly and stabilization of microtubules,whereas specific truncated fragments are sufficient to induce abnormal hyperphosphorylation and aggregate into toxic oligomers,resulting in them gaining prion-like characteristics.In addition,Tau truncations cause extensive impairments to neural and glial cell functions and animal cognition and behavior in a fragment-dependent manner.This review summarizes over 60 proteolytic cleavage sites and their corresponding truncated fragments,investigates the role of specific truncations in physiological and pathological states of Alzheimer's disease,and summarizes the latest applications of strategies targeting Tau fragments in the diagnosis and treatment of Alzheimer's disease.
基金supported by the Natural Science Foundation of China(52272188,U22A20227)the Natural Science Foundation of Beijing(2232025)+2 种基金the Natural Science Foundation of Chongqing(2022NSCQ-MSX2179)the Department of Science and Technology of Henan Province(Z20221343029)the Experimental Center of Advanced Materials in Beijing Institute of Technology。
文摘Sodium-ion batteries(SIBs)with advantages of abundant resource and low cost have emerged as promising candidates for the next-generation energy storage systems.However,safety issues existing in electrolytes,anodes,and cathodes bring about frequent accidents regarding battery fires and explosions and impede the development of high-performance SIBs.Therefore,safety analysis and high-safety battery design have become prerequisites for the development of advanced energy storage systems.The reported reviews that only focus on a specific issue are difficult to provide overall guidance for building high-safety SIBs.To overcome the limitation,this review summarizes the recent research progress from the perspective of key components of SIBs for the first time and evaluates the characteristics of various improvement strategies.By orderly analyzing the root causes of safety problems associated with different components in SIBs(including electrolytes,anodes,and cathodes),corresponding improvement strategies for each component were discussed systematically.In addition,some noteworthy points and perspectives including the chain reaction between security issues and the selection of improvement strategies tailored to different needs have also been proposed.In brief,this review is designed to deepen our understanding of the SIBs safety issues and provide guidance and assistance for designing high-safety SIBs.
基金National Natural Science Foundation of China (22179008, 21875022)Yibin ‘Jie Bang Gua Shuai’ (2022JB004)+3 种基金support from the Beijing Nova Program (20230484241)support from the Postdoctoral Fellowship Program of CPSF (GZB20230931)Special Support of the Chongqing Postdoctoral Research Project (2023CQBSHTB2041)Initial Energy Science & Technology Co., Ltd (IEST)。
文摘Lithium-rich manganese-based oxides(LRMOs) exhibit high theoretical energy densities, making them a prominent class of cathode materials for lithium-ion batteries. However, the performance of these layered cathodes often declines because of capacity fading during cycling. This decline is primarily attributed to anisotropic lattice strain and oxygen release from cathode surfaces. Given notable structural transformations, complex redox reactions, and detrimental interface side reactions in LRMOs, the development of a single modification approach that addresses bulk and surface issues is challenging. Therefore,this study introduces a surface double-coupling engineering strategy that mitigates bulk strain and reduces surface side reactions. The internal spinel-like phase coating layer, featuring threedimensional(3D) lithium-ion diffusion channels, effectively blocks oxygen release from the cathode surface and mitigates lattice strain. In addition, the external Li_(3)PO_(4) coating layer, noted for its superior corrosion resistance, enhances the interfacial lithium transport and inhibits the dissolution of surface transition metals. Notably, the spinel phase, as excellent interlayer, securely anchors Li_(3)PO_(4) to the bulk lattice and suppresses oxygen release from lattices. Consequently, these modifications considerably boost structural stability and durability, achieving an impressive capacity retention of 83.4% and a minimal voltage decay of 1.49 m V per cycle after 150 cycles at 1 C. These findings provide crucial mechanistic insights into the role of surface modifications and guide the development of high-capacity cathodes with enhanced cyclability.
基金supported by the National Key R&D Program of China(2021YFB2401800)the National Natural Science Foundation of China(21875022,22179008)+4 种基金the Yibin‘Jie Bang Gua Shuai’(2022JB004)the support from the Beijing Nova Program(20230484241)the support from the Postdoctoral Fellowship Program of CPSF(GZB20230931)the support from the 4B7B beam line of Beijing Synchrotron Radiation Facility(2021-BEPC-PT-005924,2021-BEPC-PT-005967)BL08U1A beam line of Shanghai Synchrotron Radiation Facility(2021-SSRF-PT-017710)。
文摘The rapid development of electric vehicles and portable energy storage systems demands improvements in the energy density and cost-effectiveness of lithium-ion batteries,a domain in which Lithium-rich layered cathode(LLO)materials inherently excel.However,these materials face practical challenges,such as low initial Coulombic efficiency,inferior cycle/rate performance,and voltage decline during cycling,which limit practical application.Our study introduces a surface multi-component integration strategy that incorporates oxygen vacancies into the pristine LLO material Li1.2Mn_(0.6)Ni_(0.2)O_(2).This process involves a brief citric acid treatment followed by calcination,aiming to explore rate-dependent degradation behavior.The induced surface oxygen vacancies can reduce surface oxygen partial pressure and diminish the generation of O_(2)and other highly reactive oxygen species on the surface,thereby facilitating the activation of Li ions trapped in tetrahedral sites while overcoming transport barriers.Additionally,the formation of a spinel-like phase with 3D Li+diffusion channels significantly improves Li^(+)diffusion kinetics and stabilizes the surface structure.The optimally modified sample boasts a discharge capacity of 299.5 mA h g^(-1)at a 0.1 C and 251.6 mA h g^(-1)at a 1 C during the initial activation cycle,with an impressive capacity of 222.1 mA h g^(-1)at a 5 C.Most notably,it retained nearly 70%of its capacity after 300 cycles at this elevated rate.This straightforward,effective,and highly viable modification strategy provides a crucial resolution for overcoming challenges associated with LLO materials,making them more suitable for practical application.
基金supported by the National Natural Science Foundation of China(22179006)。
文摘Metal-organic frameworks(MOFs)are among the most promising materials for lithium-ion batteries(LIBs)owing to their high surface area,periodic porosity,adjustable pore size,and controllable chemical composition.For instance,their unique porous structures promote electrolyte penetration,ions transport,and make them ideal for battery separators.Regulating the chemical composition of MOF can introduce more active sites for electrochemical reactions.Therefore,MOFs and their related composites have been extensively and thoroughly explored for LIBs.However,the reported reviews solely include the applications of MOFs in the electrode materials of LIBs and rarely involve other aspects.A systematic review of the application of MOFs in LIBs is essential for understanding the mechanism of MOFs and better designing related MOFs battery materials.This review systematically evaluates the latest developments in pristine MOFs and MOF composites for LIB applications,including MOFs as the main materials(anode,cathode,separators,and electrolytes)to auxiliary materials(coating layers and additives for electrodes).Furthermore,the synthesis,modification methods,challenges,and prospects for the application of MOFs in LIBs are discussed.
文摘Single-crystal Ni-rich cathodes are a promising candidate for high-energy lithium-ion batteries due to their higher structural and cycling stability than polycrystalline materials.However,the phase evolution and capacity degradation of these single-crystal cathodes during continuous lithation/delithation cycling remains unclear.Understanding the mapping relationship between the macroscopic electrochemical properties and the material physicochemical properties is crucial.Here,we investigate the correlation between the physical-chemical characteristics,phase transition,and capacity decay using capacity differential curve feature identification and in-situ X-ray spectroscopic imaging.We systematically clarify the dominant mechanism of phase evolution in aging cycling.Appropriately high cut-off voltages can mitigate the slow kinetic and electrochemical properties of single-crystal cathodes.We also find that second-order differential capacity discharge characteristic curves can be used to identify the crystal structure disorder of Ni-rich cathodes.These findings constitute a step forward in elucidating the correlation between the electrochemical extrinsic properties and the physicochemical intrinsic properties and provide new perspectives for failure analysis of layered electrode materials.
基金supported by the Joint Funds of the National Natural Science Foundation of China(U2130204)the National Natural Science Foundation of China(52002022)+1 种基金the Young Elite Scientists Sponsorship Program by CAST(YESS20200364)the Beijing Outstanding Young Scientists Program(BJJWZYJH01201910007023).
文摘Aqueous Zn^(2+)-ion batteries(AZIBs),recognized for their high security,reliability,and cost efficiency,have garnered considerable attention.However,the prevalent issues of dendrite growth and parasitic reactions at the Zn electrode interface significantly impede their practical application.In this study,we introduced a ubiquitous biomolecule of phenylalanine(Phe)into the electrolyte as a multifunctional additive to improve the reversibility of the Zn anode.Leveraging its exceptional nucleophilic characteristics,Phe molecules tend to coordinate with Zn^(2+)ions for optimizing the solvation environment.Simultaneously,the distinctive lipophilicity of aromatic amino acids empowers Phe with a higher adsorption energy,enabling the construction of a multifunctional protective interphase.The hydrophobic benzene ring ligands act as cleaners for repelling H_(2)O molecules,while the hydrophilic hydroxyl and carboxyl groups attract Zn^(2+)ions for homogenizing Zn^(2+)flux.Moreover,the preferential reduction of Phe molecules prior to H_(2)O facilitates the in situ formation of an organic-inorganic hybrid solid electrolyte interphase,enhancing the interfacial stability of the Zn anode.Consequently,Zn||Zn cells display improved reversibility,achieving an extended cycle life of 5250 h.Additionally,Zn||LMO full cells exhibit enhanced cyclability of retaining 77.3%capacity after 300 cycles,demonstrating substantial potential in advancing the commercialization of AZIBs.
基金National Natural Science Foundation of China,Grant/Award Number:22179006Natural Science Foundation of Zhejiang Province,Grant/Award Number:LQ23E020002+4 种基金National Natural Science Foundation of China,Grant/Award Numbers:52202284,52072036Cooperation between Industry and Education Project of Ministry of Education,Grant/Award Number:220601318235513WenZhou Natural Science Foundation,Grant/Award Numbers:G20220019,G20220021State Key Laboratory of Electrical Insulation and Power Equipment,Xi'an Jiaotong University,Grant/Award Number:EIPE22208Key Research and Development Program of Henan province,China,Grant/Award Number:231111242500。
文摘The commercialization of silicon-based anodes is affected by their low initial Coulombic efficiency(ICE)and capacity decay,which are attributed to the formation of an unstable solid electrolyte interface(SEI)layer.Herein,a feasible and cost-effective prelithiation method under a localized highconcentration electrolyte system(LHCE)for the silicon-silica/graphite(Si-SiO_(2)/C@G)anode is designed for stabilizing the SEI layer and enhancing the ICE.The thin SiO_(2)/C layers with-NH_(2) groups covered on nano-Si surfaces are demonstrated to be beneficial to the prelithiation process by density functional theory calculations and electrochemical performance.The SEI formed under LHCE is proven to be rich in ionic conductivity,inorganic substances,and flexible organic products.Thus,faster Li+transportation across the SEI further enhances the prelithiation effect and the rate performance of Si-SiO_(2)/C@G anodes.LHCE also leads to uniform decomposition and high stability of the SEI with abundant organic components.As a result,the prepared anode shows a high reversible specific capacity of 937.5 mAh g^(-1)after 400 cycles at a current density of 1 C.NCM 811‖Li-SSGLHCE full cell achieves a high-capacity retention of 126.15 mAh g^(-1)at 1 C over 750 cycles with 84.82%ICE,indicating the great value of this strategy for Si-based anodes in large-scale applications.
