In-situ polymerized solid-state lithium metal batteries have garnered significant attention due to their conformal interface contact and continuous pathways for lithium ion(Li^(+))conduction.However,their electrochemi...In-situ polymerized solid-state lithium metal batteries have garnered significant attention due to their conformal interface contact and continuous pathways for lithium ion(Li^(+))conduction.However,their electrochemical performance is often hindered by slow Li^(+)transport within high-area-loading cathodes.This study presents an in-situ poly(ε-caprolactone)electrolyte with gradient molar mass(iGPCE)through lithium metal anode(LMA)-induced anionic ring-opening polymerization.Our electrochemical and kinetic analyses reveal that the iGPCE,characterized by low molar mass(M),significantly enhances Li~+diffusion within high-area-loading cathodes and bulk electrolytes,thereby reducing concentration polarization and promoting uniform electrochemical reactions.Moreover,the high M region on LMA side acts as artificial solid electrolyte interphases,stabilizing the stripping and plating of lithium.Consequently,Li//LFP(20 mg cm^(-2))and Li//NCM622(7.4 mg cm^(-2))utilizing iGPCE exhibit stable charge/discharge behaviors.This study offers a fresh approach to accelerate Li~+diffusion kinetics of high-area-loading batteries and suggests broad applicability in other systems.展开更多
基金supported by the Key Scientific Research Project of Colleges and Universities in Henan(24A480006 and 24A530005)the Natural Science Foundation of Henan Province(242300420337)。
文摘In-situ polymerized solid-state lithium metal batteries have garnered significant attention due to their conformal interface contact and continuous pathways for lithium ion(Li^(+))conduction.However,their electrochemical performance is often hindered by slow Li^(+)transport within high-area-loading cathodes.This study presents an in-situ poly(ε-caprolactone)electrolyte with gradient molar mass(iGPCE)through lithium metal anode(LMA)-induced anionic ring-opening polymerization.Our electrochemical and kinetic analyses reveal that the iGPCE,characterized by low molar mass(M),significantly enhances Li~+diffusion within high-area-loading cathodes and bulk electrolytes,thereby reducing concentration polarization and promoting uniform electrochemical reactions.Moreover,the high M region on LMA side acts as artificial solid electrolyte interphases,stabilizing the stripping and plating of lithium.Consequently,Li//LFP(20 mg cm^(-2))and Li//NCM622(7.4 mg cm^(-2))utilizing iGPCE exhibit stable charge/discharge behaviors.This study offers a fresh approach to accelerate Li~+diffusion kinetics of high-area-loading batteries and suggests broad applicability in other systems.
