Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,...Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,conventional carbon coatings are limited by their volume expansion and structural degradation,which lead to capacity fading and reduced durability.This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide(SiO_(x))-based materials using aqueous quasi-defect-free reduced graphene oxide(QrGO)without post-treatment,unlike conventional graphene oxide(GO)-based coating methods.This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating.The QrGO-based composite anode material has several advantages,including reduced cracking due to volume expansion and enhanced charge carrier transport,as well as an increased Si content of 20 wt.%compared to the 5 wt.%in typical commercial Si-based active materials.In particular,the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate.The full cell exhibited long-term stability and capacity that were twice that of commercial SiO_(x)-based cells.Therefore,the QrGO-based one-step coating process represents a scalable,transformative,and commercially viable strategy for developing high-performance LIBs.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
Achieving high-level integration of composite micro-nano structures with different structural characteristics through a minimalist and universal process has long been the goal pursued by advanced manufacturing researc...Achieving high-level integration of composite micro-nano structures with different structural characteristics through a minimalist and universal process has long been the goal pursued by advanced manufacturing research but is rarely explored due to the absence of instructive mechanisms.Here,we revealed a controllable ultrafast laser-induced focal volume light field and experimentally succeeded in highly efficient one-step composite structuring in multiple transparent solids.A pair of spatially coupled twin periodic structures reflecting light distribution in the focal volume are simultaneously created and independently tuned by engineering ultrafast laser-matter interaction.We demonstrated that the generated composite micro-nano structures are applicable to multi-dimensional information integration,nonlinear diffractive elements,and multi-functional optical modulation.This work presents the experimental verification of highly universal all-optical fabrication of composite micro-nano structures with independent controllability in multiple degrees of freedom,expands the current cognition of ultrafast laser-based material modification in transparent solids,and establishes a new scientific aspect of strong-field optics,namely,focal volume optics for composite structuring transparent solids.展开更多
Metal additive manufacturing(MAM)enables near-net shape production of components with minimized waste and excellent mechanical performance based on multi-scale microstructural heterogeneity.Espe-cially,the dislocation...Metal additive manufacturing(MAM)enables near-net shape production of components with minimized waste and excellent mechanical performance based on multi-scale microstructural heterogeneity.Espe-cially,the dislocation cell network that often bears elemental segregation or precipitation of a secondary phase contributes to enhancing the strength of additively manufactured materials.The cell boundaries can also act as active nucleation sites for the formation of precipitates under post-MAM heat treatment,as the chemical heterogeneity and profuse dislocations generate a driving force for precipitation.In this work,we subjected a Co_(18)Cr_(15)Fe_(50)Ni_(10)Mo_(6.5)C_(0.5)(at%)medium-entropy alloy fabricated by laser powder bed fusion(LPBF)to post-LPBF annealing at 900℃for 10 min.Microstructural investigation revealed that the cell boundaries of the as-built sample,which were decorated by Mo segregation,are replaced byμphase andM_(6)C typecarbide precipitatesduringannealingwhile thegrainstructureand sizeremain unaffected,indicating that the post-LPBF annealing delivered the proper amount of heat input to alter only the cell structure.The yield strength slightly decreased with annealing due to a reduction in the strengthening effect by the cell boundaries despite an increased precipitation strengthening effect.How-ever,the post-LPBF annealing improved the strain hardenability and the ultimate tensile strength was enhanced from∼1.02 to∼1.15 GPa owing to reinforced back stress hardening by the increased disloca-tion pile-up at the precipitates.Our results suggest that the cell structure with chemical heterogeneity can be successfully controlled by careful post-MAM heat treatment to tailor the mechanical performance,while also providing insight into alloy design for additive manufacturing.展开更多
Advancing aqueous zinc-ion batteries(AZIBs)are significantly challenged by the need to find cathode materials that can provide both high capacity and fast reaction kinetics.Tellurium telluride,a topological insulator,...Advancing aqueous zinc-ion batteries(AZIBs)are significantly challenged by the need to find cathode materials that can provide both high capacity and fast reaction kinetics.Tellurium telluride,a topological insulator,has emerged as a promising cathode candidate for AZIBs,garnering increasing attention.However,the complete understanding of its electrochemical reaction mechanism and its unsatisfactory energy storage performance are major obstacles to the practical use.In this work,we synthesize a bimetallic bismuth-nickel telluride with Te vacancies,defined as Bi_(2)Te_(3-x)/NiTe_(2),which forms a topological insulator/topological Dirac semimetal heterostructure through a hydrothermal approach.The electrochemical reaction mechanism of Bi_(2)Te_(3-x)/NiTe_(2),along with its phase and structural changes are elucidated by using in-situ X-ray diffraction,various electrochemical techniques,and ex-situ characterizations.The influences of Bi_(2)Te_(3-x)/NiTe_(2)on the electronic structure,interracial electron transfer,migration barrier,and ion adsorption energy are investigated by using density functional theory calculations.Our findings reveal that Bi_(2)Te_(3-x)/NiTe_(2)exhibits excellent specific capacity,stable cycling,and superior rate capability as a cathode material for AZIBs.Moreover,further studies demonstrate that Bi_(2)Te_(3-x)/NiTe_(2)maintains exceptional performance at low temperatures of-15 and-5℃,and also retains stability and flexibility when integrated into flexible battery packs.展开更多
基金supported by Korea Electrotechnology Research Institute(KERI)Primary research program through the National Research Council of Science&Technology(NST)funded by the Ministry of Science and ICT(MSIT)(No.25A01015)by the Technology Innovation Program(20019091)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)by the National Research Council of Science&Technology(NST)grant from the Korea government(MSIT)(No.GTL24012-000).
文摘Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,conventional carbon coatings are limited by their volume expansion and structural degradation,which lead to capacity fading and reduced durability.This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide(SiO_(x))-based materials using aqueous quasi-defect-free reduced graphene oxide(QrGO)without post-treatment,unlike conventional graphene oxide(GO)-based coating methods.This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating.The QrGO-based composite anode material has several advantages,including reduced cracking due to volume expansion and enhanced charge carrier transport,as well as an increased Si content of 20 wt.%compared to the 5 wt.%in typical commercial Si-based active materials.In particular,the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate.The full cell exhibited long-term stability and capacity that were twice that of commercial SiO_(x)-based cells.Therefore,the QrGO-based one-step coating process represents a scalable,transformative,and commercially viable strategy for developing high-performance LIBs.
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financially supported by the National Key Research and Development Program of China(No.2021YFB2802001)the National Natural Science Foundation of China(Grant Nos.12304349,U20A20211,62275233)the Postdoctoral Fellowship Program of CPSF(GZB20230628,GZC20241465)。
文摘Achieving high-level integration of composite micro-nano structures with different structural characteristics through a minimalist and universal process has long been the goal pursued by advanced manufacturing research but is rarely explored due to the absence of instructive mechanisms.Here,we revealed a controllable ultrafast laser-induced focal volume light field and experimentally succeeded in highly efficient one-step composite structuring in multiple transparent solids.A pair of spatially coupled twin periodic structures reflecting light distribution in the focal volume are simultaneously created and independently tuned by engineering ultrafast laser-matter interaction.We demonstrated that the generated composite micro-nano structures are applicable to multi-dimensional information integration,nonlinear diffractive elements,and multi-functional optical modulation.This work presents the experimental verification of highly universal all-optical fabrication of composite micro-nano structures with independent controllability in multiple degrees of freedom,expands the current cognition of ultrafast laser-based material modification in transparent solids,and establishes a new scientific aspect of strong-field optics,namely,focal volume optics for composite structuring transparent solids.
基金supported by the National Research Founda-tion of Korea(NRF)grant funded by the Korean government(MSIT)(Nos.2021R1A2C3006662 and RS-2023-00281246)supported by the Principal R&D project(contract no.PNK9950)of the Korean Institute of Materials Science(KIMS).
文摘Metal additive manufacturing(MAM)enables near-net shape production of components with minimized waste and excellent mechanical performance based on multi-scale microstructural heterogeneity.Espe-cially,the dislocation cell network that often bears elemental segregation or precipitation of a secondary phase contributes to enhancing the strength of additively manufactured materials.The cell boundaries can also act as active nucleation sites for the formation of precipitates under post-MAM heat treatment,as the chemical heterogeneity and profuse dislocations generate a driving force for precipitation.In this work,we subjected a Co_(18)Cr_(15)Fe_(50)Ni_(10)Mo_(6.5)C_(0.5)(at%)medium-entropy alloy fabricated by laser powder bed fusion(LPBF)to post-LPBF annealing at 900℃for 10 min.Microstructural investigation revealed that the cell boundaries of the as-built sample,which were decorated by Mo segregation,are replaced byμphase andM_(6)C typecarbide precipitatesduringannealingwhile thegrainstructureand sizeremain unaffected,indicating that the post-LPBF annealing delivered the proper amount of heat input to alter only the cell structure.The yield strength slightly decreased with annealing due to a reduction in the strengthening effect by the cell boundaries despite an increased precipitation strengthening effect.How-ever,the post-LPBF annealing improved the strain hardenability and the ultimate tensile strength was enhanced from∼1.02 to∼1.15 GPa owing to reinforced back stress hardening by the increased disloca-tion pile-up at the precipitates.Our results suggest that the cell structure with chemical heterogeneity can be successfully controlled by careful post-MAM heat treatment to tailor the mechanical performance,while also providing insight into alloy design for additive manufacturing.
基金supported by the National Natural Science Foundation of China(No.52372223)the Science Foundation of Shaanxi Province(No.2023-JC-ZD-03 and 2022GD-TSLD-15)Shaanxi Fundamental Science Research Project for Mathematics and Physics(No.23JSQ005)。
文摘Advancing aqueous zinc-ion batteries(AZIBs)are significantly challenged by the need to find cathode materials that can provide both high capacity and fast reaction kinetics.Tellurium telluride,a topological insulator,has emerged as a promising cathode candidate for AZIBs,garnering increasing attention.However,the complete understanding of its electrochemical reaction mechanism and its unsatisfactory energy storage performance are major obstacles to the practical use.In this work,we synthesize a bimetallic bismuth-nickel telluride with Te vacancies,defined as Bi_(2)Te_(3-x)/NiTe_(2),which forms a topological insulator/topological Dirac semimetal heterostructure through a hydrothermal approach.The electrochemical reaction mechanism of Bi_(2)Te_(3-x)/NiTe_(2),along with its phase and structural changes are elucidated by using in-situ X-ray diffraction,various electrochemical techniques,and ex-situ characterizations.The influences of Bi_(2)Te_(3-x)/NiTe_(2)on the electronic structure,interracial electron transfer,migration barrier,and ion adsorption energy are investigated by using density functional theory calculations.Our findings reveal that Bi_(2)Te_(3-x)/NiTe_(2)exhibits excellent specific capacity,stable cycling,and superior rate capability as a cathode material for AZIBs.Moreover,further studies demonstrate that Bi_(2)Te_(3-x)/NiTe_(2)maintains exceptional performance at low temperatures of-15 and-5℃,and also retains stability and flexibility when integrated into flexible battery packs.
