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@ARTICLE{Hoffknecht:1005101,
author = {Hoffknecht, Jan-Philipp and Wettstein, Alina and Atik,
Jaschar and Krause, Christian and Thienenkamp, Johannes and
Brunklaus, Gunther and Winter, Martin and Diddens, Diddo and
Heuer, Andreas and Paillard, Elie},
title = {{C}oordinating {A}nions “to the {R}escue” of the
{L}ithium {I}on {M}obility in {T}ernary {S}olid {P}olymer
{E}lectrolytes {P}lasticized {W}ith {I}onic {L}iquids},
journal = {Advanced energy materials},
volume = {13},
number = {1},
issn = {1614-6832},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2023-01300},
pages = {2202789 -},
year = {2023},
abstract = {Lithium salts with low coordinating anions such as
bis(trifluoromethanesulfonyl)imide (TFSI) have been the
state-of-the-art for polyethylene oxide (PEO)-based
“dry” polymer electrolytes for 3 decades. Plasticizing
PEO with TFSI-based ionic liquids (ILs) to form ternary
solid polymer electrolytes (TSPEs) increases conductivity
and Li+ diffusivity. However, the Li+ transport mechanism is
unaffected compared to their “dry” counterparts and is
essentially coupled to the dynamics of the polymer host
matrix, which limits Li+ transport improvement. Thus, a
paradigm shift is hereby suggested: the utilization of more
coordinating anions such as
trifluoromethanesulfonyl-N-cyanoamide (TFSAM), able to
compete with PEO for Li+ solvation, to accelerate the Li+
transport and reach a higher Li+ transference number. The
Li–TFSAM interaction in binary and ternary TFSAM-based
electrolytes is probed by experimental methods and discussed
in the context of recent computational results. In PEO-based
TSPEs, TFSAM drastically accelerates the Li+ transport
(increases Li+ transference number by a factor 6 and the Li+
conductivity by 2–3) and computer simulations reveal that
lithium dynamics are effectively re-coupled from polymer to
anion dynamics. Last, this concept of coordinating anions in
TSPEs is successfully applied in LFP||Li metal cells leading
to enhanced capacity retention $(86\%$ after 300 cycles) and
an improved rate performance at 2C.},
cin = {IEK-12},
ddc = {050},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1222 - Components and Cells (POF4-122) / 1223 - Batteries
in Application (POF4-122)},
pid = {G:(DE-HGF)POF4-1222 / G:(DE-HGF)POF4-1223},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000888918600001},
doi = {10.1002/aenm.202202789},
url = {https://juser.fz-juelich.de/record/1005101},
}