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@ARTICLE{Beltrop:829004,
author = {Beltrop, Kolja and Meister, Paul and Klein, Sven and
Heckmann, Andreas and Grünebaum, Mariano and Wiemhöfer,
Hans-Dieter and Winter, Martin and Placke, Tobias},
title = {{D}oes {S}ize really {M}atter? {N}ew {I}nsights into the
{I}ntercalation {B}ehavior of {A}nions into a
{G}raphite-{B}ased {P}ositive {E}lectrode for {D}ual-{I}on
{B}atteries},
journal = {Electrochimica acta},
volume = {209},
issn = {0013-4686},
address = {New York, NY [u.a.]},
publisher = {Elsevier},
reportid = {FZJ-2017-02821},
pages = {44 - 55},
year = {2016},
abstract = {There are many reports on electrochemical anion
intercalation into graphite using different types of
electrolyte mixtures for application in dual-graphite or
dual-ion cells, showing promising results in terms of
cycling stability, reversible capacity and Coulombic
efficiency. However, there is no clear understanding of the
influence of the anion/electrolyte characteristics on the
intercalation properties. In this work, we present a
comprehensive study of the intercalation behavior of a
series of imide-based ionic liquid (IL) electrolytes into a
graphite positive electrode with special emphasis on the
influence of anion size on the electrochemical parameters
such as the onset potential for anion uptake and the
reversible capacity. The onset potentials of anion
intercalation into graphite ranged between 4.42 V to 4.53 V
vs. Li/Li+ with the following descending order for the
studied anions: BETI > FSI > FTFSI > FSI/TFSI (molar ratio =
11:1) > TFSI > TFSI/FSI (molar ratio = 10:1). The
electrochemical results support the assumption that
electrolyte effects such as ion pair formation and
self-aggregation in the electrolyte overrule the influence
of the anion size (up to a certain point) in terms of the
onset potential for anion uptake. The charge/discharge
cycling performance was studied in view of reversible
capacity and Coulombic efficiency. In this context, the BETI
system shows only very poor intercalation ability whereas
the quaternary mixture TFSI/FSI displays a very promising
cycling behavior providing a specific capacity of ∼54 mAh
g−1 with a Coulombic efficiency exceeding $99\%.$
Furthermore, the characteristics of the different
imide-based electrolytes such as the oxidative stability
(TFSI > BETI > FTFSI > TFSI/FSI > FSI/TFSI > FSI) as well as
the influence on aluminum current collector dissolution were
studied to draw further conclusions about impact on the
Coulombic efficiency.},
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:000379504600006},
doi = {10.1016/j.electacta.2016.05.012},
url = {https://juser.fz-juelich.de/record/829004},
}