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

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Abstract：

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：

Cathodes Manganese compounds Lithium batteries Lithium Fluoride

Author Community：

[ 1 ] [Chen, Yawei]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, Menghao]Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo; 315200, China
[ 3 ] [Li, Menghao]Department of Materials Science and Engineering, Southern University of Science and Technology, Shenzhen; 518055, China
[ 4 ] [Jie, Yulin]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, Yue]Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou; 215123, China
[ 6 ] [Zhang, Zhengfeng]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing; 100124, China
[ 7 ] [Yu, Peiping]Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou; 215123, China
[ 8 ] [Li, Wanxia]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, Yang]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, Xinpeng]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, Zhanwu]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, Pengfei]Beijing Key Laboratory of Microstructure and Properties of Solids, Faculty of Materials and Manufacturing, Beijing University of Technology, Beijing; 100124, China
[ 13 ] [Cheng, Tao]Institute of Functional Nano and Soft Materials (FUNSOM), Soochow University, Suzhou; 215123, China
[ 14 ] [Gu, M. Danny]Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo; 315200, China
[ 15 ] [Jiao, Shuhong]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, Ruiguo]Hefei National Laboratory for Physical Science at Microscale, Department of Materials Science and Engineering, University of Science and Technology of China, Hefei; 230026, China

Reprint Author's Address：

[cheng, tao]institute of functional nano and soft materials (funsom), soochow university, suzhou; 215123, china

Email：

tcheng@suda.edu.cnm.danny.gu@gmail.comjiaosh@ustc.edu.cnrgcao@ustc.edu.cn

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Source ：

Joule

Year： 2025

Issue： 5

Volume： 9

3 9 . 8 0 0

JCR@2022

Cited Count：

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SCOPUS Cited Count：

ESI Highly Cited Papers on the List： 0 Unfold All

WanFang Cited Count：

Chinese Cited Count：

30 Days PV： 0

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