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@ARTICLE{Szczuka:909829,
author = {Szczuka, Conrad and Karasulu, Bora and Groh, Matthias F.
and Sayed, Farheen N. and Sherman, Timothy J. and Bocarsly,
Joshua D. and Vema, Sundeep and Menkin, Svetlana and Emge,
Steffen P. and Morris, Andrew J. and Grey, Clare P.},
title = {{F}orced {D}isorder in the {S}olid {S}olution
{L}i3{P}–{L}i2{S}: {A} {N}ew {C}lass of {F}ully {R}educed
{S}olid {E}lectrolytes for {L}ithium {M}etal {A}nodes},
journal = {Journal of the American Chemical Society},
volume = {144},
number = {36},
issn = {0002-7863},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2022-03450},
pages = {16350 - 16365},
year = {2022},
abstract = {All-solid-state batteries based on non-combustible solid
electrolytes are promising candidates for safe energy
storage systems. In addition, they offer the opportunity to
utilize metallic lithium as an anode. However, it has proven
to be a challenge to design an electrolyte that combines
high ionic conductivity and processability with
thermodynamic stability toward lithium. Herein, we report a
new highly conducting solid solution that offers a route to
overcome these challenges. The Li–P–S ternary was first
explored via a combination of high-throughput crystal
structure predictions and solid-state synthesis (via ball
milling) of the most promising compositions, specifically,
phases within the Li3P–Li2S tie line. We systematically
characterized the structural properties and Li-ion mobility
of the resulting materials by X-ray and neutron diffraction,
solid-state nuclear magnetic resonance spectroscopy
(relaxometry), and electrochemical impedance spectroscopy. A
Li3P–Li2S metastable solid solution was identified, with
the phases adopting the fluorite (Li2S) structure with P
substituting for S and the extra Li+ ions occupying the
octahedral voids and contributing to the ionic transport.
The analysis of the experimental data is supported by
extensive quantum-chemical calculations of both structural
stability, diffusivity, and activation barriers for Li+
transport. The new solid electrolytes show Li-ion
conductivities in the range of established materials, while
their composition guarantees thermodynamic stability toward
lithium metal anodes.},
cin = {IEK-9},
ddc = {540},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {1223 - Batteries in Application (POF4-122)},
pid = {G:(DE-HGF)POF4-1223},
typ = {PUB:(DE-HGF)16},
pubmed = {36040461},
UT = {WOS:000850684900001},
doi = {10.1021/jacs.2c01913},
url = {https://juser.fz-juelich.de/record/909829},
}