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@ARTICLE{Pavan:1042709,
author = {Pavan, Matilde and Münch, Konrad and Benz, Sebastian L.
and Bernges, Tim and Henss, Anja and Zeier, Wolfgang G. and
Janek, Jürgen},
title = {{R}ole and {E}volution of ${F}e{S}_2$ {C}athode
{M}icrostructure in {A}rgyrodite-{B}ased
{A}ll-{S}olid-{S}tate {L}ithium–{S}ulfur {B}atteries},
journal = {Chemistry of materials},
volume = {37},
number = {9},
issn = {0897-4756},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2025-02655},
pages = {3185 - 3196},
year = {2025},
note = {Support from the Federal Ministry of Education and Research
(BMBF) for the project KAROFEST (grant number
03XP0498A)Support within the BMBF projects SoLiS (grant
number 03XP0395D) and ProRec (grant number 03XP0537E)},
abstract = {All-solid-state lithium–sulfur batteries (ASSLSBs) are
emerging as a promising alternative for green energy
storage, offering high theoretical capacities and energy
densities by using inexpensive materials. To date, ASSLSBs
commonly suffer from poor cycle life and sluggish reaction
kinetics. A promising active material for ASSLSBs is iron
disulfide, $FeS_2$, due to its natural abundance, low cost,
and high theoretical capacity (894 $mAh·g^{–1}$) It
undergoes a displacement reaction with significant volume
changes whose effects can be locally constrained by using
small particles. Here, the influence of the positive
electrode microstructure on the electrochemical performance
of $FeS_2$-based ASSLSBs with Cl-rich argyrodite,
$Li_{5.5}PS_{4.5}Cl_{1.5}$, a mechanically soft sulfide
solid electrolyte with high ionic conductivity, is
investigated. Composites with different microstructures were
prepared using three different processing methods (i.e.,
hand grinding, ball mill, and mini mill). Their impact on
the electrochemical performance was evaluated, revealing
that homogeneously submicro-structured composites achieve
higher capacities (up to 4.28 $mAh·cm^{–2}$) and capacity
retention (87.2\% at the 50th cycle). Furthermore, finely
structured composites enhance the in situ formation of
active material from the solid electrolyte and increase its
accessible reversible capacity. Ex situ analyses (i.e.,
SEM-EDS and XPS) at different states of charge show that the
morphology of $FeS_2$ evolves forming core–shell like
submicro-structures.},
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:001477011300001},
doi = {10.1021/acs.chemmater.4c03315},
url = {https://juser.fz-juelich.de/record/1042709},
}