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@ARTICLE{Fallon:1041124,
author = {Fallon, M. Jewels and Faka, Vasiliki and Lange, Martin
Alexander and Kraft, Marvin and Suard, Emmanuelle and
Connolly, Eamonn T. and Francisco, Brian E. and Squires,
Alexander G. and Zeier, Wolfgang G.},
title = {{E}xploring the {A}nion {S}ite {D}isorder {K}inetics in
{L}ithium {A}rgyrodites},
journal = {Journal of the American Chemical Society},
volume = {147},
number = {12},
issn = {0002-7863},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2025-02158},
pages = {10151 - 10159},
year = {2025},
note = {funding from the Deutsche Forschungsgemeinschaft under
project number 459785385},
abstract = {Lithium argyrodites $Li_6PS_5X (X = Cl, Br, I)$ are a
promising class of solid-state electrolytes with the
potential to achieve high conductivities (>10
$mS·cm^{–1})$ necessary for use in solid-state batteries.
Previous research has shown that structural factors, in
particular, site disorder between the sulfide and halide
anions, can impact the ionic conductivity of lithium
argyrodites. One current hypothesis for this correlation
between anion site disorder and ionic transport is a
connection to the lithium-ion substructure. However, as
there is limited research surrounding the anion disordering
process itself, this relationship has yet to be fully
understood. This research explores the impact of the
composition and synthesis on the anion disordering process
through the $Li_{6+x}P_{1–x}Si_xS_5Br$ ($x$ = 0 to 0.4 in
0.1 steps) series of substitutions quenched from different
annealing temperatures. Ex situ and in situ diffraction
studies show that the anion site disorder within the
compounds increases upon Si introduction only for samples
quenched from higher annealing temperatures but remains
relatively constant at lower annealing temperatures. Based
on in situ diffraction measurements, we further monitor the
effects of anion mobility at elevated temperatures allowing
inference of slower anion disordering kinetics with changing
compositional content. We complement the experimental work
using nudged-elastic band calculations showing the overall
preference of anions for their specific sites and the
possibility of anion mobility. This work provides insight
into the argyrodites and shows that the anion disordering
can be monitored and that the composition has strong
influences on the disordering process.},
cin = {IMD-4},
ddc = {540},
cid = {I:(DE-Juel1)IMD-4-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
pubmed = {40073401},
UT = {WOS:001445829000001},
doi = {10.1021/jacs.4c14466},
url = {https://juser.fz-juelich.de/record/1041124},
}