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@ARTICLE{Diddens:830218,
author = {Diddens, Diddo and Paillard, Elie-Elisée and Heuer,
Andreas},
title = {{I}mproving the {L}ithium {I}on {T}ransport in {P}olymer
{E}lectrolytes by {F}unctionalized {I}onic-{L}iquid
{A}dditives: {S}imulations and {M}odeling},
journal = {Journal of the Electrochemical Society},
volume = {164},
number = {11},
issn = {0013-4651},
address = {Pennington, NJ},
publisher = {Electrochemical Soc.},
reportid = {FZJ-2017-03792},
pages = {E3225 - E3231},
year = {2017},
abstract = {We present a theoretical study combining molecular dynamics
(MD) simulations with an analytical lithium ion transport
model [Maitra and Heuer, Phys. Rev. Lett. 2007, 98, 227802]
to highlight a novel strategy to increase the lithium
mobility in polymer electrolytes based on poly(ethylene
oxide) (PEO). This is achieved by using a
pyrrolidinium-based ionic liquid (IL) where the cation has
been chemically functionalized by a short oligoether side
chain [von Zamory et al., Phys. Chem. Chem. Phys. 2016,
18(31), 21539] as an additive. Since the oligoether moieties
at the pyrrolidinium cations form pronounced coordinations
to the lithium ions for sufficiently long side chains, the
ions can be detached from the PEO backbone. In this way, a
fundamentally new lithium ion transport mechanism is
established (shuttling mechanism), in which the lithium
dynamics is decoupled from the polymer dynamics, the latter
typically being slow under experimental conditions. Based on
our simulations, we incorporate this novel mechanism into
our existing model, which accurately reproduces the observed
lithium dynamics. We demonstrate that the use of
oligoether-functionalized IL additives significantly
increases the lithium diffusivity. Finally, we show that for
experimentally relevant electrolytes containing long polymer
chains, an even stronger increase of the lithium mobility
can be expected.},
cin = {IEK-12},
ddc = {540},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {131 - Electrochemical Storage (POF3-131)},
pid = {G:(DE-HGF)POF3-131},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000413263000010},
doi = {10.1149/2.0271711jes},
url = {https://juser.fz-juelich.de/record/830218},
}