The intergranular microcracking in polycrystalline Ni-rich cathode particle is led by anisotropic volume change and stress corrosion along grain boundary,accelerating battery performance decay.Herein,we have suggested...The intergranular microcracking in polycrystalline Ni-rich cathode particle is led by anisotropic volume change and stress corrosion along grain boundary,accelerating battery performance decay.Herein,we have suggested a simple but advanced solid-state method that ensures both uniform transition metal distribution and single-crystalline morphology for Ni-rich cathode synthesis without sophisticated coprecipitation.Pelletization-assisted mechanical densification(PAMD)process on solid-state precursor mixture enables the dynamic mass transfer through the increased solid-solid contact area which facilitates the grain growth during sintering process,readily forming micro-sized single-crystalline particle.Furthermore,the improved chemical reactivity by a combination of capillary effect and vacancyassisted diffusion provides homogeneous element distribution within each primary particle.As a result,single-crystalline Ni-rich cathode with PAMD process has eliminated a potential evolution of intergranular cracking,thus achieving superior energy retention capability of 85%over 150 cycles compared to polycrystalline Ni-rich particle even after high-pressure calendering process(corresponding to electrode density of~3.6 g cm^(-3))and high cut-off voltage cycling.This work provides a concrete perspective on developing facile synthetic route of micron-sized single-crystalline Ni-rich cathode materials for high energy density lithium-ion batteries(LIBs).展开更多
The rapid electrification of transportation and grid systems has placed lithium-ion batteries(LIBs)at the forefront of energy storage innovation.Lithium iron phosphate(LiFePO4,LFP),with its superior safety,long cycle ...The rapid electrification of transportation and grid systems has placed lithium-ion batteries(LIBs)at the forefront of energy storage innovation.Lithium iron phosphate(LiFePO4,LFP),with its superior safety,long cycle life,and cost advantages,has become a cornerstone cathode material.However,the limited energy density(ED),attributed to its relatively low nominal voltage(~3.2 V)and moderate specific capacity(~170 mAh g−1),hinders its competitiveness in high-energy applications.Furthermore,electrochemical characteristics related to poor charge transfer kinetics and material circularity also limit its overall value.This review highlights recent advances in material design,electrode engineering,and system-level optimization aimed at overcoming these challenges.Key strategies include precision doping,multifunctional coating,and nanostructuring to enhance conductivity and rate performance,development of high-tap-density powders and ultra-thick electrodes for improved ED,and hierarchical electrode architectures and advanced conductive networks for efficient ion/electron transport.Additional focus is given to low-temperature performance,scalable and sustainable synthesis routes,and recycling pathways that ensure long-term environmental viability.Emerging directions such as dry electrode processing,solid-state integration,and artificial intelligence/machine learning-driven optimization are also discussed as transformative tools for accelerating LFP innovation.By integrating these multidisciplinary strategies,LFP can evolve from a safe and stable cathode into a high-performance,sustainable solution for electric vehicles,grid storage,and next-generation energy systems.展开更多
基金supported by the National Research Foundation of Korea(NRF)grant funded by the Korea government(MEST)(2021R1A2C1095408)supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(2022R1A6A1A03051158)。
文摘The intergranular microcracking in polycrystalline Ni-rich cathode particle is led by anisotropic volume change and stress corrosion along grain boundary,accelerating battery performance decay.Herein,we have suggested a simple but advanced solid-state method that ensures both uniform transition metal distribution and single-crystalline morphology for Ni-rich cathode synthesis without sophisticated coprecipitation.Pelletization-assisted mechanical densification(PAMD)process on solid-state precursor mixture enables the dynamic mass transfer through the increased solid-solid contact area which facilitates the grain growth during sintering process,readily forming micro-sized single-crystalline particle.Furthermore,the improved chemical reactivity by a combination of capillary effect and vacancyassisted diffusion provides homogeneous element distribution within each primary particle.As a result,single-crystalline Ni-rich cathode with PAMD process has eliminated a potential evolution of intergranular cracking,thus achieving superior energy retention capability of 85%over 150 cycles compared to polycrystalline Ni-rich particle even after high-pressure calendering process(corresponding to electrode density of~3.6 g cm^(-3))and high cut-off voltage cycling.This work provides a concrete perspective on developing facile synthetic route of micron-sized single-crystalline Ni-rich cathode materials for high energy density lithium-ion batteries(LIBs).
基金supported by the National R&D Program through the National Research Foundation of Korea(NRF)funded by Ministry of Science and ICT(RS-2024-00408156 and RS-2025-16069043)the National Research Foundation of Korea(NRF)grant funded by the Korea government(Ministry of Science and ICT,MSIT)(RS-2024-00343847).
文摘The rapid electrification of transportation and grid systems has placed lithium-ion batteries(LIBs)at the forefront of energy storage innovation.Lithium iron phosphate(LiFePO4,LFP),with its superior safety,long cycle life,and cost advantages,has become a cornerstone cathode material.However,the limited energy density(ED),attributed to its relatively low nominal voltage(~3.2 V)and moderate specific capacity(~170 mAh g−1),hinders its competitiveness in high-energy applications.Furthermore,electrochemical characteristics related to poor charge transfer kinetics and material circularity also limit its overall value.This review highlights recent advances in material design,electrode engineering,and system-level optimization aimed at overcoming these challenges.Key strategies include precision doping,multifunctional coating,and nanostructuring to enhance conductivity and rate performance,development of high-tap-density powders and ultra-thick electrodes for improved ED,and hierarchical electrode architectures and advanced conductive networks for efficient ion/electron transport.Additional focus is given to low-temperature performance,scalable and sustainable synthesis routes,and recycling pathways that ensure long-term environmental viability.Emerging directions such as dry electrode processing,solid-state integration,and artificial intelligence/machine learning-driven optimization are also discussed as transformative tools for accelerating LFP innovation.By integrating these multidisciplinary strategies,LFP can evolve from a safe and stable cathode into a high-performance,sustainable solution for electric vehicles,grid storage,and next-generation energy systems.
