TY  - JOUR
AU  - Pavan, Matilde
AU  - Münch, Konrad
AU  - Benz, Sebastian L.
AU  - Bernges, Tim
AU  - Henss, Anja
AU  - Zeier, Wolfgang G.
AU  - Janek, Jürgen
TI  - Role and Evolution of $FeS_2$ Cathode Microstructure in Argyrodite-Based All-Solid-State Lithium–Sulfur Batteries
JO  - Chemistry of materials
VL  - 37
IS  - 9
SN  - 0897-4756
CY  - Washington, DC
PB  - American Chemical Society
M1  - FZJ-2025-02655
SP  - 3185 - 3196
PY  - 2025
N1  - 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)
AB  - 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.
LB  - PUB:(DE-HGF)16
UR  - <Go to ISI:>//WOS:001477011300001
DO  - DOI:10.1021/acs.chemmater.4c03315
UR  - https://juser.fz-juelich.de/record/1042709
ER  -