Journal Article

FZJ-2024-00722

http://join2-wiki.gsi.de/foswiki/pub/Main/Artwork/join2_logo100x88.png Interfacial solvation-structure regulation for stable Li metal anode by a desolvation coating technique

Li, G.-X. (First author) ; Lennartz, P.FZJ* ; Koverga, V. ; Kou, R. ; Nguyen, A. ; Jiang, H. ; Liao, M. ; Wang, D. ; Dandu, N. ; Zepeda, M. ; Wang, H. ; Wang, K. ; Ngo, A. T. ; Brunklaus, G. (Corresponding author)FZJ* ; Wang, D. (Corresponding author)

2024
National Acad. of Sciences Washington, DC

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Please use a persistent id in citations: doi:10.1073/pnas.2311732121  doi:10.34734/FZJ-2024-00722

Abstract: Rechargeable lithium (Li) metal batteries face challenges in achieving stable cycling due to the instability of the solid electrolyte interphase (SEI). The Li-ion solvation structure and its desolvation process are crucial for the formation of a stable SEI on Li metal anodes and improving Li plating/stripping kinetics. This research introduces an interfacial desolvation coating technique to actively modulate the Li-ion solvation structure at the Li metal interface and regulate the participation of the electrolyte solvent in SEI formation. Through experimental investigations conducted using a carbonate electrolyte with limited compatibility to Li metal, the optimized desolvation coating layer, composed of 12-crown-4 ether-modified silica materials, selectively displaces strongly coordinating solvents while simultaneously enriching weakly coordinating fluorinated solvents at the Li metal/electrolyte interface. This selective desolvation and enrichment effect reduce solvent participation to SEI and thus facilitate the formation of a LiF-dominant SEI with greatly reduced organic species on the Li metal surface, as conclusively verified through various characterization techniques including XPS, quantitative NMR, operando NMR, cryo-TEM, EELS, and EDS. The interfacial desolvation coating technique enables excellent rate cycling stability (i.e., 1C) of the Li metal anode and prolonged cycling life of the Li||LiCoO2 pouch cell in the conventional carbonate electrolyte (E/C 2.6 g/Ah), with 80% capacity retention after 333 cycles.

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Contributing Institute(s):

1. Helmholtz-Institut Münster Ionenleiter für Energiespeicher (IEK-12)

Research Program(s):

1. 1221 - Fundamentals and Materials (POF4-122) (POF4-122)
2. 1222 - Components and Cells (POF4-122) (POF4-122)
3. 1223 - Batteries in Application (POF4-122) (POF4-122)
4. LiSi - Lithium-Solid-Electrolyte Interfaces (13XP0224A) (13XP0224A)

Appears in the scientific report 2024

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Database coverage:
; ; ; BIOSIS Previews ; Biological Abstracts ; Clarivate Analytics Master Journal List ; Current Contents - Agriculture, Biology and Environmental Sciences ; Current Contents - Life Sciences ; Ebsco Academic Search ; Essential Science Indicators ; IF >= 10 ; JCR ; National-Konsortium ; SCOPUS ; Science Citation Index Expanded ; Web of Science Core Collection ; Zoological Record

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