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@ARTICLE{Chiou:1006634,
author = {Chiou, Min-Huei and Verweyen, Elisabeth and Diddens, Diddo
and Wichmann, Lennart and Schmidt, Christina and Neuhaus,
Kerstin and Choudhary, Aditya and Bedrov, Dmitry and Winter,
Martin and Brunklaus, Gunther},
title = {{S}election of {P}olymer {S}egment {S}pecies {M}atters for
{E}lectrolyte {P}roperties and {P}erformance in {L}ithium
{M}etal {B}atteries},
journal = {ACS applied energy materials},
volume = {6},
number = {8},
issn = {2574-0962},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2023-01767},
pages = {4422–4436},
year = {2023},
abstract = {Control of homogeneous lithium deposition governs prospects
of advanced cell development and practical applications of
high-energy-density lithium metal batteries. Polymer
electrolytes are thus explored and employed to mitigate the
growth of high-surface-area lithium species while enhancing
the reversibility of the lithium reservoir upon cell
cycling. Herein, an in-depth understanding of the
distribution of membrane properties and lithium deposition
behavior affected by the selection of polymer segment
species is derived. It is demonstrated that severely
localized lithium deposits featuring needle-like
morphologies may be readily observed when electrostatic
fields (or partial charges) and the amount of Li+
coordinators of the primary and secondary polymer segment
species appear rather dissimilar, leading to a sudden cell
failure at early stages of cell operation. In comparison,
employment of optimized copolymer electrolytes enables
superior cell performance at 1C even with thicker cathodes
(6.3 mg cm–2). Additionally, the improvement of
cell-cycling stability due to enhancement of similarity of
dipole moments and partial charge distributions among
copolymer segments are also demonstrated for different
polymer systems, contributing to avoidance of undesired
lithium protrusions, also reflecting a viable concept for
the design of future copolymer electrolytes.},
cin = {IEK-12},
ddc = {540},
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)},
pid = {G:(DE-HGF)POF4-1221 / G:(DE-HGF)POF4-1222 /
G:(DE-HGF)POF4-1223},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000973157300001},
doi = {10.1021/acsaem.3c00571},
url = {https://juser.fz-juelich.de/record/1006634},
}