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@ARTICLE{Helm:1024272,
author = {Helm, Bianca and Strotmann, Kyra and Böger, Thorben and
Samanta, Bibek and Banik, Ananya and Lange, Martin A. and
Li, Yuheng and Li, Cheng and Hansen, Michael Ryan and
Canepa, Pieremanuele and Zeier, Wolfgang G.},
title = {{R}educing the {D}efect {F}ormation {E}nergy by
{A}liovalent {S}n(+{IV}) and {I}sovalent {P}(+{V})
{S}ubstitution in ${L}i_3{S}b{S}_4$ {P}romotes {L}i${^+}$
{T}ransport},
journal = {ACS applied energy materials},
volume = {7},
number = {5},
issn = {2574-0962},
address = {Washington, DC},
publisher = {ACS Publications},
reportid = {FZJ-2024-02079},
pages = {1735 - 1747},
year = {2024},
abstract = {The search for highly conducting Li+ solid electrolytes
focuses on sulfide- and halide-based materials, where
typically the strongly atomic disordered materials are the
most promising. The atomic disorder corresponds to a
flattened energy landscape having similar relative site
energies for different Li+ positions facilitating motion. In
addition, the highly disordered Li+ conductors have
negligible defect formation energy as moving charges are
readily available. This work investigates the isovalent
Li3Sb1–xPxS4 (0 ≤ x ≤ 0.5) and the aliovalent
Li3+xSb1–xSnxS4 (0 ≤ x ≤ 0.2) substitution series of
thio-LISICON materials by using X-ray diffraction,
high-resolution neutron diffraction, impedance spectroscopy,
and defect calculations. The starting composition Li3SbS4
has a low ionic conductivity of ∼10–11 S·cm–1 and
both substituents improve the ionic conductivity strongly by
up to 4 orders of magnitude. On the one hand, in substituted
Li3SbS4 structures, only minor structural changes are
observed which cannot sufficiently explain the significant
impact on the Li+ conductivity. On the other hand, the Li+
carrier density reveals a correlation to the activation
energy and first-principles defect calculations, displaying
significantly reduced defect formation energy upon
substitution. Here, we show within two different
substitution series that the defect formation energy plays a
major role for ionic motion in this class of thio-LISICON
materials.},
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:001176923300001},
doi = {10.1021/acsaem.3c02652},
url = {https://juser.fz-juelich.de/record/1024272},
}