Composite solid electrolytes(CSEs) containing polymer matrices and inorganic fillers hold promise for the next generation of solid-state batteries.However,the role of residual solvents in CSEs remains controversial.Th...Composite solid electrolytes(CSEs) containing polymer matrices and inorganic fillers hold promise for the next generation of solid-state batteries.However,the role of residual solvents in CSEs remains controversial.This study investigated the evolution and function of the residual solvent in a polymer-Li_2B_(12)H_(12) CSE.A partial reaction occurred between Li_2B_(12)H_(12) and solvent N,N-dimethylformamide(DMF),which produced dimethylaminomethanol(DMAM) in the CSE.Density functional theory calculations have revealed that DMA M forms stronger hydrogen bonds with polyvinylidene fluoride chains than DMF,which can have a plasticizing effect on the polymer matrix,leading to lower crystallinity and quicker segment motion.Therefore,this CSE exhibited improved Li-ion conducting properties,enabling the stable cycling of Li‖LiFePO_(4) solid-state batteries.This study provided insights into the role of residual solvents in CSEs.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.51971146,51971147,52171218 and 52271222)Shanghai Municipal Science and Technology Commission (No.21010503100)+3 种基金the Major Program for the Scientific Research Innovation Plan of Shanghai Education Commission (No.2019-01-07-00-07-E00015)Shanghai Outstanding Academic Leaders Plan,Guangxi Key Laboratory of Information Materials (Guilin University of Electronic Technology,201017-K)Shanghai Rising-Star Program (No.20QA1407100)General Program of Natural Science Foundation of Shanghai (No.20ZR1438400)。
文摘Composite solid electrolytes(CSEs) containing polymer matrices and inorganic fillers hold promise for the next generation of solid-state batteries.However,the role of residual solvents in CSEs remains controversial.This study investigated the evolution and function of the residual solvent in a polymer-Li_2B_(12)H_(12) CSE.A partial reaction occurred between Li_2B_(12)H_(12) and solvent N,N-dimethylformamide(DMF),which produced dimethylaminomethanol(DMAM) in the CSE.Density functional theory calculations have revealed that DMA M forms stronger hydrogen bonds with polyvinylidene fluoride chains than DMF,which can have a plasticizing effect on the polymer matrix,leading to lower crystallinity and quicker segment motion.Therefore,this CSE exhibited improved Li-ion conducting properties,enabling the stable cycling of Li‖LiFePO_(4) solid-state batteries.This study provided insights into the role of residual solvents in CSEs.