All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the unde...All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the undesirable side reactions of sulfide-based solid electrolytes(SEs),resulting in poor electrochemical properties with increased interfacial resistance.Here,we propose a wet chemical method rationally designed to achieve a conformal coating of lithium-indium chloride(Li_(3)InCl_(6))onto vapor-grown carbon fibers(VGCFs)as conductive agents.First,with the advantage of the Li_(3)InCl_(6) protective layer,use of VGCF@Li_(3)InCl_(6) leads to enhanced interfacial stability and improved electrochemical properties,including stable cycle performance.These results indicate that the Li_(3)InCl_(6) protective layer suppresses the unwanted reaction between Li_(6)PS_(5)Cl(LPSCl)and VGCF.Second,VGCF@Li_(3)InCl_(6) effectively promotes polytetrafluoroethylene(PTFE)fibrillization,leading to a homogeneous electrode microstructure.The uniform distribution of the cathode active material(CAM)in the electrode results in reduced charge-transfer resistance(R_(ct))and enhanced Li-ion kinetics.As a result,a full cell with the LiNi_(x)Mn_(y)Co_(z)O_(2)(NCM)/VGCF@Li_(3)InCl_(6) electrode shows an areal capacity of 7.7mAhcm^(−2) at 0.05 C and long-term cycle stability of 77.9%over 400 cycles at 0.2 C.This study offers a strategy for utilizing stable carbon-based conductive agents in sulfide-based ASSBs to enhance their electrochemical performance.展开更多
Anode-free all-solid-state batteries(AF-ASSBs)have received significant attention as a next-generation battery system due to their high energy density and safety.However,this system still faces challenges,such as poor...Anode-free all-solid-state batteries(AF-ASSBs)have received significant attention as a next-generation battery system due to their high energy density and safety.However,this system still faces challenges,such as poor Coulombic efficiency and short-circuiting caused by Li dendrite growth.In this study,the AF-ASSBs are demonstrated with reliable and robust electrochemical properties by employing Cu-Sn nanotube(NT)thin layer(~1μm)on the Cu current collector for regulating Li electrodeposition.Li_(x)Sn phases with high Li-ion diffusivity in the lithiated Cu-Sn NT layer enable facile Li diffusion along with its one-dimensional hollow geometry.The unique structure,in which Li electrodeposition takes place between the Cu-Sn NT layer and the current collector by the Coble creep mechanism,improves cell durability by preventing solid electrolyte(SE)decomposition and Li dendrite growth.Furthermore,the large surface area of the Cu-Sn NT layer ensures close contact with the SE layer,leading to a reduced lithiation overpotential compared to that of a flat Cu-Sn layer.The Cu-Sn NT layer also maintains its structural integrity owing to its high mechanical properties and porous nature,which could further alleviate the mechanical stress.The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM)|SE|Cu-Sn NT@Cu cell with a practical capacity of 2.9 mAh cm^(−2) exhibits 83.8%cycle retention after 150 cycles and an average Coulombic efficiency of 99.85%at room temperature.It also demonstrates a critical current density 4.5 times higher compared to the NCM|SE|Cu cell.展开更多
基金supported by the Korea Institute for Advancement of Technology(KIAT)grant funded by the Korean Government(MOTIE)(RS-2024-00417730,HRD Program for Industrial Innovation)supported by the Technology Innovation Program(or Industrial Strategic Technology Development Program-Materials&Components Technology Development Program)(20024261),Development of thick film electrodes and cell manufacturing technology for a high-performance lithium iron phosphate battery with energy density of over 200 Wh/kg was funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea).
文摘All-solid-state batteries(ASSBs)have garnered significant interest as the next-generation in battery technology,praised for their superior safety and high energy density.However,a conductive agent accelerates the undesirable side reactions of sulfide-based solid electrolytes(SEs),resulting in poor electrochemical properties with increased interfacial resistance.Here,we propose a wet chemical method rationally designed to achieve a conformal coating of lithium-indium chloride(Li_(3)InCl_(6))onto vapor-grown carbon fibers(VGCFs)as conductive agents.First,with the advantage of the Li_(3)InCl_(6) protective layer,use of VGCF@Li_(3)InCl_(6) leads to enhanced interfacial stability and improved electrochemical properties,including stable cycle performance.These results indicate that the Li_(3)InCl_(6) protective layer suppresses the unwanted reaction between Li_(6)PS_(5)Cl(LPSCl)and VGCF.Second,VGCF@Li_(3)InCl_(6) effectively promotes polytetrafluoroethylene(PTFE)fibrillization,leading to a homogeneous electrode microstructure.The uniform distribution of the cathode active material(CAM)in the electrode results in reduced charge-transfer resistance(R_(ct))and enhanced Li-ion kinetics.As a result,a full cell with the LiNi_(x)Mn_(y)Co_(z)O_(2)(NCM)/VGCF@Li_(3)InCl_(6) electrode shows an areal capacity of 7.7mAhcm^(−2) at 0.05 C and long-term cycle stability of 77.9%over 400 cycles at 0.2 C.This study offers a strategy for utilizing stable carbon-based conductive agents in sulfide-based ASSBs to enhance their electrochemical performance.
基金Korea Institute of Energy Technology Evaluation and Planning,Grant/Award Number:20214000000520Ministry of Trade,Industry and Energy,Grant/Award Number:20009985。
文摘Anode-free all-solid-state batteries(AF-ASSBs)have received significant attention as a next-generation battery system due to their high energy density and safety.However,this system still faces challenges,such as poor Coulombic efficiency and short-circuiting caused by Li dendrite growth.In this study,the AF-ASSBs are demonstrated with reliable and robust electrochemical properties by employing Cu-Sn nanotube(NT)thin layer(~1μm)on the Cu current collector for regulating Li electrodeposition.Li_(x)Sn phases with high Li-ion diffusivity in the lithiated Cu-Sn NT layer enable facile Li diffusion along with its one-dimensional hollow geometry.The unique structure,in which Li electrodeposition takes place between the Cu-Sn NT layer and the current collector by the Coble creep mechanism,improves cell durability by preventing solid electrolyte(SE)decomposition and Li dendrite growth.Furthermore,the large surface area of the Cu-Sn NT layer ensures close contact with the SE layer,leading to a reduced lithiation overpotential compared to that of a flat Cu-Sn layer.The Cu-Sn NT layer also maintains its structural integrity owing to its high mechanical properties and porous nature,which could further alleviate the mechanical stress.The LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM)|SE|Cu-Sn NT@Cu cell with a practical capacity of 2.9 mAh cm^(−2) exhibits 83.8%cycle retention after 150 cycles and an average Coulombic efficiency of 99.85%at room temperature.It also demonstrates a critical current density 4.5 times higher compared to the NCM|SE|Cu cell.
