TY  - JOUR
AU  - Li, Guo-Xing
AU  - Lennartz, Peter
AU  - Koverga, Volodymyr
AU  - Kou, Rong
AU  - Nguyen, Au
AU  - Jiang, Heng
AU  - Liao, Meng
AU  - Wang, Daiwei
AU  - Dandu, Naveen
AU  - Zepeda, Michael
AU  - Wang, Haiying
AU  - Wang, Ke
AU  - Ngo, Anh T.
AU  - Brunklaus, Gunther
AU  - Wang, Donghai
TI  - Interfacial solvation-structure regulation for stable Li metal anode by a desolvation coating technique
JO  - Proceedings of the National Academy of Sciences of the United States of America
VL  - 121
IS  - 4
SN  - 0027-8424
CY  - Washington, DC
PB  - National Acad. of Sciences
M1  - FZJ-2024-00722
SP  - e2311732121
PY  - 2024
AB  - 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.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:001164841400002
DO  - DOI:10.1073/pnas.2311732121
UR  - https://juser.fz-juelich.de/record/1021295
ER  -