Poly(ethylene oxide)(PEO)based electrolytes have garnered considerable attention in all-solid-state lithium metal batteries with superior safety and energy density,but suffer fromlow-ion conductivity and poor cycling ...Poly(ethylene oxide)(PEO)based electrolytes have garnered considerable attention in all-solid-state lithium metal batteries with superior safety and energy density,but suffer fromlow-ion conductivity and poor cycling stability.Herein,a novel in-situ functional crosslinking strategy is proposed to overcome these limitations simultaneously,where a two-in-one bis-diazirine molecule(C1)is not only used as a rigid cross-linker,but also functions as an electron-withdrawing inducer.Benefitting from such an integration of two functionalities into one cross-linker,a rigid PEO electrolyte network can be facilely constructed,while exhibiting disrupted crystallization,robust mechanical strength,loosened Li-O binding to boost the Li+transport,and anion-rich Li+coordinated structure to favor the generation of a stable LiF-rich solid electrolyte interface.As a result,a remarkable ion conductivity of 1.4×10^(−3) S cm^(−1) is achieved at 60◦C together with a Li+transference number of 0.63.And the corresponding LiFePO4||Li and NCM811||Li filled batteries present significantly improved rate performance and capacity retention cycling life compared with the pristine PEO electrolyte,highlighting the great potential of in-situ functional crosslinking for high performance all-solid-state batteries.展开更多
基金supported by National Natural Science Foundation of China(No.52273198)Yunnan Fundamental Research Projects(No.202301BF070001-008)+2 种基金Graduate Research Program of Yunnan University(No.KC23235310)National Key Research and Development Program of China(Nos.2022YFB3803300 and 2023YFE0116800)Beijing Natural Science Foundation(IS23037).
文摘Poly(ethylene oxide)(PEO)based electrolytes have garnered considerable attention in all-solid-state lithium metal batteries with superior safety and energy density,but suffer fromlow-ion conductivity and poor cycling stability.Herein,a novel in-situ functional crosslinking strategy is proposed to overcome these limitations simultaneously,where a two-in-one bis-diazirine molecule(C1)is not only used as a rigid cross-linker,but also functions as an electron-withdrawing inducer.Benefitting from such an integration of two functionalities into one cross-linker,a rigid PEO electrolyte network can be facilely constructed,while exhibiting disrupted crystallization,robust mechanical strength,loosened Li-O binding to boost the Li+transport,and anion-rich Li+coordinated structure to favor the generation of a stable LiF-rich solid electrolyte interface.As a result,a remarkable ion conductivity of 1.4×10^(−3) S cm^(−1) is achieved at 60◦C together with a Li+transference number of 0.63.And the corresponding LiFePO4||Li and NCM811||Li filled batteries present significantly improved rate performance and capacity retention cycling life compared with the pristine PEO electrolyte,highlighting the great potential of in-situ functional crosslinking for high performance all-solid-state batteries.
