%0 Journal Article
%A Li, Guo-Xing
%A Lennartz, Peter
%A Koverga, Volodymyr
%A Kou, Rong
%A Nguyen, Au
%A Jiang, Heng
%A Liao, Meng
%A Wang, Daiwei
%A Dandu, Naveen
%A Zepeda, Michael
%A Wang, Haiying
%A Wang, Ke
%A Ngo, Anh T.
%A Brunklaus, Gunther
%A Wang, Donghai
%T Interfacial solvation-structure regulation for stable Li metal anode by a desolvation coating technique
%J Proceedings of the National Academy of Sciences of the United States of America
%V 121
%N 4
%@ 0027-8424
%C Washington, DC
%I National Acad. of Sciences
%M FZJ-2024-00722
%P e2311732121
%D 2024
%X 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.
%F PUB:(DE-HGF)16
%9 Journal Article
%U <Go to ISI:>//WOS:001164841400002
%R 10.1073/pnas.2311732121
%U https://juser.fz-juelich.de/record/1021295