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PreprintCC BY-NC-NDChemRxiv

Pore-network homogeneity for mechanically reliable powder-compacted solid-electrolyte separators

  • Hyeok-Rae Cho1,2
  • Hyeong-Jong Kim1,2,3
  • Jae-Seung Kim3,2
  • Beom Jin Park1,2
  • Youngkyung Kim1,2
  • Daeyeon Lee1,2
  • Jiwon Kim1,2
  • Hyojun Kim1,2
  • Sung-Kyun Jung1,2,3,4,5
  • SUNG-KYUN JUNG
5 affiliations
  1. 1Department of Materials Science and Engineering
  2. 2Seoul National University (SNU
  3. 3Institute for Rechargeable Battery Innovations Research
  4. 4School of Transdisciplinary Innovations
  5. 5Research Institute of Advanced Materials (RIAM
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Abstract

All-solid-state batteries (ASSBs) with alloy anodes require solid-electrolyte (SE) separators that sustain ion transport while accommodating repeated electrode-derived mechanical loads. However, the mechanical state of powder-compacted separators is commonly inferred from bulk porosity, averaged mechanical properties, or cell-level stack pressure changes, obscuring spatially heterogeneous local responses. Here, we show that pore-network homogeneity is a key determinant of the mechanical reliability of sulfide solid-electrolyte separators by governing local mechanical heterogeneity and stress localization. FIB-SEM tomography and spatially resolved nanoindentation reveal that a highly densified separator with a broad particle-size distribution (PSD) retains clustered pore-rich and mechanically compliant regions, whereas a narrower-PSD separator exhibits a more homogeneous pore network and local mechanical response. Despite comparable cell-level pressure evolution, the two separators show markedly different cycling stability. Post-cycling microscopy reveals cracking and interfacial delamination in the heterogeneous separator, while microstructure-resolved simulations reveal stronger local stress amplification consistent with these observations. Controlled digital structures with identical D50 and porosity further isolate PSD-dependent changes in pore architecture and stress distribution. These findings establish pore-network homogeneity as a key design criterion for mechanically reliable solid-electrolyte separators beyond ionic conductivity and bulk densification.

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Cite

BibTeXRIS
BibTeX
@misc{cho2026porenetwork,
  title = {{Pore-network homogeneity for mechanically reliable powder-compacted solid-electrolyte separators}},
  author = {Hyeok-Rae Cho and Hyeong-Jong Kim and Jae-Seung Kim and Beom Jin Park and Youngkyung Kim and Daeyeon Lee and Jiwon Kim and Hyojun Kim and Sung-Kyun Jung and SUNG-KYUN JUNG},
  howpublished = {ChemRxiv},
  year = {2026},
  month = oct,
  doi = {10.26434/chemrxiv.15009882/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009882/v1},
  note = {CC BY-NC-ND},
}
RIS
TY  - UNPB
TI  - Pore-network homogeneity for mechanically reliable powder-compacted solid-electrolyte separators
AU  - Hyeok-Rae Cho
AU  - Hyeong-Jong Kim
AU  - Jae-Seung Kim
AU  - Beom Jin Park
AU  - Youngkyung Kim
AU  - Daeyeon Lee
AU  - Jiwon Kim
AU  - Hyojun Kim
AU  - Sung-Kyun Jung
AU  - SUNG-KYUN JUNG
PY  - 2026
DA  - 2026/10/05
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009882/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009882/v1
AB  - All-solid-state batteries (ASSBs) with alloy anodes require solid-electrolyte (SE) separators that sustain ion transport while accommodating repeated electrode-derived mechanical loads. However, the mechanical state of powder-compacted separators is commonly inferred from bulk porosity, averaged mechanical properties, or cell-level stack pressure changes, obscuring spatially heterogeneous local responses. Here, we show that pore-network homogeneity is a key determinant of the mechanical reliability of sulfide solid-electrolyte separators by governing local mechanical heterogeneity and stress localization. FIB-SEM tomography and spatially resolved nanoindentation reveal that a highly densified separator with a broad particle-size distribution (PSD) retains clustered pore-rich and mechanically compliant regions, whereas a narrower-PSD separator exhibits a more homogeneous pore network and local mechanical response. Despite comparable cell-level pressure evolution, the two separators show markedly different cycling stability. Post-cycling microscopy reveals cracking and interfacial delamination in the heterogeneous separator, while microstructure-resolved simulations reveal stronger local stress amplification consistent with these observations. Controlled digital structures with identical D50 and porosity further isolate PSD-dependent changes in pore architecture and stress distribution. These findings establish pore-network homogeneity as a key design criterion for mechanically reliable solid-electrolyte separators beyond ionic conductivity and bulk densification.
ER  -