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@ARTICLE{Stolz:906590,
author = {Stolz, Lukas and Hochstädt, Sebastian and Röser, Stephan
and Hansen, Michael Ryan and Winter, Martin and
Kasnatscheew, Johannes},
title = {{S}ingle-{I}on versus {D}ual-{I}on {C}onducting
{E}lectrolytes: {T}he {R}elevance of {C}oncentration
{P}olarization in {S}olid-{S}tate {B}atteries},
journal = {ACS applied materials $\&$ interfaces},
volume = {14},
number = {9},
issn = {1944-8244},
address = {Washington, DC},
publisher = {Soc.},
reportid = {FZJ-2022-01541},
pages = {11559–11566},
year = {2022},
abstract = {Lithium batteries with solid polymer electrolytes (SPEs)
and mobile ions are prone to mass transport limitations,
that is, concentration polarization, creating a
concentration gradient with Li+-ion (and counter-anion)
depletion toward the respective electrode, as can be
electrochemically observed in, for example, symmetric Li||Li
cells and confirmed by Sand and diffusion equations. The
effect of immobile anions is systematically investigated in
this work. Therefore, network-based SPEs are synthesized
with either mobile (dual-ion conduction) or immobile anions
(single-ion conduction) and proved via solvation tests and
nuclear magnetic resonance spectroscopy. It is shown that
the SPE with immobile anions does not suffer from
concentration polarization, thus disagreeing with Sand and
diffusion assumptions, consequently suggesting single-ion
(Li+) transport via migration instead. Nevertheless, the
practical relevance of single-ion conduction can be debated.
Under practical conditions, that is, below the limiting
current, the concentration polarization is generally not
pronounced with DIC-based electrolytes, rendering the
beneficial effect of SIC redundant and DIC a better choice
due to better kinetical aspects under these conditions.
Also, the observed dendritic Li in both electrolytes
questions a relevant impact of mass transport on its
formation, at least in SPEs.},
cin = {IEK-12},
ddc = {600},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:35192769},
UT = {WOS:000787543300048},
doi = {10.1021/acsami.2c00084},
url = {https://juser.fz-juelich.de/record/906590},
}