Dynamic evolution of cathode-electrolyte interphase in lithium metal batteries with ether electrolytes - Details

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High-voltage　lithium　(Li)　metal　batteries　(HVLMBs)　have　attracted　tremendous　research　interest　in　the　past　decade　owing　to　their　high　energy　densities.　Electrode-electrolyte　interphases　in　HVLMBs　play　critical　roles　in　dictating　their　electrochemical　performance.　However,　despite　the　intensive　research　on　solid-electrolyte　interphase　(SEI)　of　Li　anode,　the　cathode-electrolyte　interphase　(CEI)　on　high-voltage　cathodes　remains　elusive.　Herein,　we　report　the　formation　and　dynamic　evolution　of　CEI　on　LiNi0.8Mn0.1Co0.1O2　(NMC811)　cathodes　in　ether-based　electrolytes.　We　reveal　that　the　solvent-derived　interphase　predominates　the　initial　CEI,　which　subsequently　evolves　into　a　Li　fluoride　(LiF)-rich　CEI　during　cycling.　Through　solvent　design,　the　weak-solvation　electrolyte　with　branched　ether　solvents　promotes　the　formation　of　a　conformal　CEI　layer　featuring　the　monodispersing　LiF　nanocrystals　(∼8　nm),　thereby　enabling　NMC811　cathodes　to　sustain　up　to　2,000　cycles.　This　work　addresses　the　long-standing　questions　regarding　CEI　evolution　and　provides　valuable　guidance　for　the　rational　electrolyte　design　for　HVLMBs.　©　2025　Elsevier　Inc.

Keyword：

high-voltage cathodes cathode-electrolyte interphase lithium fluoride lithium metal batteries ether electrolytes

Author Community：

[ 1 ] [Chen Y.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 2 ] [Li M.]Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo, 315200, China
[ 3 ] [Li M.]Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen, 518055, China
[ 4 ] [Jie Y.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 5 ] [Liu Y.]Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, China
[ 6 ] [Zhang Z.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 7 ] [Yu P.]Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, China
[ 8 ] [Li W.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 9 ] [Liu Y.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 10 ] [Li X.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 11 ] [Lei Z.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 12 ] [Yan P.]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing, 100124, China
[ 13 ] [Cheng T.]Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou, 215123, China
[ 14 ] [Gu M.D.]Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo, 315200, China
[ 15 ] [Jiao S.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China
[ 16 ] [Cao R.]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei, 230026, China

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Source ：

Joule

ISSN： 2542-4351

Year： 2025

3 9 . 8 0 0

JCR@2022

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ESI Highly Cited Papers on the List： 0 Unfold All

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30 Days PV： 8

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