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@ARTICLE{Overhoff:1029093,
author = {Overhoff, Gerrit Michael and Verweyen, Elisabeth and
Roering, Philipp and Winter, Martin and Brunklaus, Gunther},
title = {{E}nhancing the {E}lectrochemical {P}erformance of
{B}lended {S}ingle-{I}on {C}onducting {P}olymers by {S}mart
{M}odification of the {P}olymer {S}tructure},
journal = {ACS applied energy materials},
volume = {7},
number = {14},
issn = {2574-0962},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2024-04953},
pages = {5893-5904},
year = {2024},
abstract = {Single lithium-ion conducting polymers represent a
promisingclass of electrolytes that potentially enable the
utilization of lithium metal anodes in next-generation
batteries. The immobilization of anions within the
polymer’s structure in principle mitigates issues related
to localized ion depletion, resulting in decreased cell
polarization when compared to common dual-ion conductors
comprising poly(ethylene oxide) and lithium salt. However,
the intrinsic rigidity of these materials often necessitates
incorporation of flowable components and blending with other
polymers, such as poly(vinylidene
fluoride-co-hexafluoropropylene) (PVdF-HFP), to enhance the
mechanical flexibility of the resulting polymer membranes.
Within polymer blends, distinct phases may be present, and
the distribution of plasticizers among these phases is
highly crucial as they act as carrier molecules for Li+
transport. In this study, we thus explored the impact of
polymer chain modification from a rigid aromatic single-ion
conducting polymer to a more flexible polymer by introducing
ethylene glycol units into the backbone. Notably, this
alteration yielded a substantial decrease of 100 °C of the
glass transition temperature and a 6-fold increase in ionic
conductivity (0.5 mS cm−1 @ 40 °C) after blending with
PVdF-HFP and addition of ethylene carbonate/dimethyl
carbonate. Atomistic molecular dynamics simulations suggest
that this enhancement can be attributed to a high
concentration of plasticizer within the Li+ containing
phase. In symmetric Li||Li cells, exceptional performance
was achieved, demonstrating operation at high limiting
current density and successful plating/stripping for 1000 h
at 0.2 mA cm−2. When paired with high-voltage NMC
cathodes, the introduced polymer structures exhibited
noteworthy capacity retention after 800 cycles, emphasizing
advantages brought forth by flexible and adapted polymer
architecture.},
cin = {IMD-4},
ddc = {540},
cid = {I:(DE-Juel1)IMD-4-20141217},
pnm = {1222 - Components and Cells (POF4-122) / 1221 -
Fundamentals and Materials (POF4-122) / FB2-POLY -
Zellplattform Polymere (BMBF-13XP0429A)},
pid = {G:(DE-HGF)POF4-1222 / G:(DE-HGF)POF4-1221 /
G:(DE-Juel1)BMBF-13XP0429A},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001263167400001},
doi = {10.1021/acsaem.4c01117},
url = {https://juser.fz-juelich.de/record/1029093},
}