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@ARTICLE{Helm:908088,
author = {Helm, Bianca and Minafra, Nicolò and Wankmiller, Björn
and Agne, Matthias T. and Li, Cheng and Senyshyn, Anatoliy
and Hansen, Michael Ryan and Zeier, Wolfgang G.},
title = {{C}orrelating {S}tructural {D}isorder to ${L}i^+$ {I}on
{T}ransport in ${L}i_{4–x}{G}e_{1–x}{S}b_x{S}_4$ (0 ≤
x ≤ 0.2)},
journal = {Chemistry of materials},
volume = {34},
number = {12},
issn = {0897-4756},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2022-02367},
pages = {5558–5570},
year = {2022},
abstract = {Strong compositional influences are known to affect the
ionic transport within the thio-LISICON family, however, a
deeper understanding of the resulting structure - transport
correlations have up until now been lacking. Employing a
combination of high-resolution neutron diffraction,
impedance spectroscopy and nuclear magnetic resonance
spectroscopy, together with bond valence site energy
calculations and the maximum entropy method for determining
the underlying Li+ scattering density distribution of a
crystal structure, this work assesses the impact of the Li+
substructure and charge carrier density on the ionic
transport within the Li4-xGe1-xSbxS4 substitution series. By
incorporating Sb5+ into Li4GeS4, an anisometric expansion of
the unit cell is observed. An additional Li+ position is
found as soon as (SbS4)3− polyhedra are present, leading
to a better local polyhedral connectivity and a higher
disorder in the Li+ substructure. Here, we are able to
relate structural disorder to an increase in configurational
entropy, together with a two order-of-magnitude increase in
ionic conductivity. This result reinforces the typically
believed paradigm that structural disorder leads to
improvements in ionic transport.},
cin = {IEK-12},
ddc = {540},
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},
UT = {WOS:000819657500001},
doi = {10.1021/acs.chemmater.2c00608},
url = {https://juser.fz-juelich.de/record/908088},
}