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@ARTICLE{Li:1021295,
author = {Li, Guo-Xing and Lennartz, Peter and Koverga, Volodymyr and
Kou, Rong and Nguyen, Au and Jiang, Heng and Liao, Meng and
Wang, Daiwei and Dandu, Naveen and Zepeda, Michael and Wang,
Haiying and Wang, Ke and Ngo, Anh T. and Brunklaus, Gunther
and Wang, Donghai},
title = {{I}nterfacial solvation-structure regulation for stable
{L}i metal anode by a desolvation coating technique},
journal = {Proceedings of the National Academy of Sciences of the
United States of America},
volume = {121},
number = {4},
issn = {0027-8424},
address = {Washington, DC},
publisher = {National Acad. of Sciences},
reportid = {FZJ-2024-00722},
pages = {e2311732121},
year = {2024},
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.},
cin = {IEK-12},
ddc = {500},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122) / 1222 -
Components and Cells (POF4-122) / 1223 - Batteries in
Application (POF4-122) / LiSi - Lithium-Solid-Electrolyte
Interfaces (13XP0224A)},
pid = {G:(DE-HGF)POF4-1221 / G:(DE-HGF)POF4-1222 /
G:(DE-HGF)POF4-1223 / G:(BMBF)13XP0224A},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001164841400002},
doi = {10.1073/pnas.2311732121},
url = {https://juser.fz-juelich.de/record/1021295},
}