Dual-Enhanced Charge Transfer through Prelithiation Strategy in Polymer Electrolyte Enables Robust LiF-Rich SEI for Ultralong-Life All-Solid-State Batteries - Details

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Abstract：

Lithium　fluoride　(LiF)-rich　solid　electrolyte　interface　(SEI)　is　critical　for　enabling　the　stable　operation　of　polymer-based　all-solid-state　lithium-metal　batteries　(ASSLMBs).　Precisely　controlling　the　C─F　dissociation　chemistry　in　fluorine-containing　lithium　salts　to　construct　a　LiF-rich　SEI　is　a　logically　viable　but　still　challenging　approach.　Current　strategies　for　constructing　LiF-rich　SEI　primarily　focus　on　designing　non-metal　polar　groups　and　related　structures.　In　contrast,　approaches　leveraging　metal-based　electron　donors　to　facilitate　charge　transfer　for　C─F　bond　cleavage　and　LiF　formation　remain　largely　unexplored.　Herein,　a　dual-enhanced　charge　transfer　mechanism　through　prelithiation　strategy　is　proposed　in　solid　polymer　electrolyte　(SPE)　for　C─F　bond　cleavage.　The　charge　transfer　occurs　between　LiTFSI　and　the　introduced　metal　sites　and　further　enhanced　by　lithiation　design,　thereby　achieving　a　robust　LiF-rich　SEI.　The　achieving　SPEs　enable　an　excellent　cyclability　of　Li|Li　cell　over　3800　h　at　0.3 mA　cm−2.　Li||LiFePO4　ASSLMBs　demonstrate　a　high　Coulombic　efficiency　of　≈100%　and　a　stability　of　1200　cycles　with　capacity　retention　of　80%　at　2C.　The　corresponding　pouch　cell　delivers　a　high　average　areal　capacity　of　2.41　mAh　cm−2　over　1600　h.　This　work　offers　a　novel　approach　for　constructing　LiF-rich　SEI　toward　durable　ASSLMBs.　©　2025　Wiley-VCH　GmbH.

Keyword：

dual-enhanced charge transfer mechanism LiF-rich SEI prelithiation strategy solid polymer electrolyte stable all-solid-state lithium metal batteries

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[ 1 ] [Zheng Y.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 2 ] [Zheng Y.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 3 ] [Yang N.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 4 ] [Yang N.]School of Materials and Energy, University of Electronic Science and Technology of China, Chengdu, 611731, China
[ 5 ] [Duan S.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 6 ] [Li Z.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 7 ] [Gao R.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 8 ] [Zhu Y.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 9 ] [Wang H.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 10 ] [Zhang T.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 11 ] [Li G.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 12 ] [Luo D.]State Key Laboratory of Catalysis, Power Battery & System Research Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 110623, China
[ 13 ] [Yang L.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 14 ] [Wang D.]Canadian Light Source, 44 Innovation Boulevard, Saskatoon, S7N 2V3, SK, Canada
[ 15 ] [Yan W.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 16 ] [Zhang J.]College of Materials Science and Engineering, Institute of New Energy Materials and Engineering, Fujian Engineering Research Center of High Energy Batteries and New Energy Equipment & Systems, Fuzhou University, Fuzhou, 350108, China
[ 17 ] [Chen Z.]Department of Chemical Engineering, University of Waterloo, 200 University Ave. W, Waterloo, N2L 3G1, ON, Canada
[ 18 ] [Chen Z.]State Key Laboratory of Catalysis, Power Battery & System Research Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 110623, China

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