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@ARTICLE{Hartel:1032476,
author = {Hartel, Johannes and Banik, Ananya and Ali, Md Yusuf and
Helm, Bianca and Strotmann, Kyra and Faka, Vasiliki and
Maus, Oliver and Li, Cheng and Wiggers, Hartmut and Zeier,
Wolfgang},
title = {{I}nvestigating the {I}nfluence of {T}ransition {M}etal
{S}ubstitution in {L}ithium {A}rgyrodites on {S}tructure,
{T}ransport, and {S}olid-{S}tate {B}attery {P}erformance},
journal = {Chemistry of materials},
volume = {36},
number = {21},
issn = {0897-4756},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2024-06269},
pages = {10731 - 10745},
year = {2024},
note = {FESTBATT funded by the Bundesministerium für Bildung und
Forschung (BMBF; project 03XP0430F), Deutsche
Forschungsgemeinschaft under project number 459785385},
abstract = {Lithium argyrodites have gained significant attention as
candidates for solid electrolytes in solid-state batteries
due to their superior ionic conductivities and favorable
mechanical properties. However, during charging, oxidative
decomposition reactions occur at the interface between the
solid electrolyte and cathode active material, which impede
cell performance. In this study, transition metal
substitution of the solid electrolyte is investigated with
the intention of tuning the composition of the cathode
electrolyte interphase (CEI) and thereby improving the
cycling performance. Hence, the
$Li_{5.5–2x}Zn_xPS_{4.5}Cl_{1.5}$ (0 ≤ x ≤ 0.15) and
$Li_{6–2x}Zn_xPS_5Br$ (0 ≤ x ≤ 0.15) substitution
series are investigated to elucidate how substitution
affects structure, $Li^+$ transport, and the performance of
the materials as catholytes in solid-state batteries.
Corefinement of the neutron and powder X-ray diffraction
data unveils the occupation of $Li^+$ positions by
$Zn^{2+}$. This leads to blocking of $Li^+$ transport
pathways within the $Li^+$ cages causing a decrease of ionic
conductivities along with increasing activation energies for
$Li^+$ transport. By using a combination of cycling
experiments, impedance spectroscopy and X-ray photoelectron
spectroscopy, the composition of the CEI and the
state-of-charge dependence of the CEI growth when using
$Li_{5.5–2x}Zn_xPS_{4.5}Cl_{1.5}$|NCM-83 composites was
investigated in half-cells, revealing that $Zn^{2+}$
substitution leads to faster decomposition kinetics and
affects the CEI composition. Overall, this work explores the
influence of Li+ substitution by $Zn^{2+}$ on structure and
transport in lithium argyrodites and the potential of
transition metal substitutions as means to tune the kinetics
of CEI growth, the CEI composition, and thereby cell
performance.},
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},
UT = {WOS:001348337400001},
doi = {10.1021/acs.chemmater.4c02281},
url = {https://juser.fz-juelich.de/record/1032476},
}