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PreprintCC BYChemRxiv

Pressing Mode Determines Densification Uniformity and Dimensional Stability in Sulfide Solid-State Batteries

7 affiliations
  1. 1Department of Materials Science and Engineering
  2. 2NTNU Norwegian University of Science and Technology
  3. 3Christian Doppler Laboratory for Solid-State Batteries
  4. 4AVL List GmbH
  5. 5AIT Austrian Institute of Technology GmbH
  6. 6Institute of Chemical Technologies and Analytics
  7. 7Vienna University of Technology

Abstract

Pressure-assisted densification is essential for manufacturing sulfide solid-state batteries because electrochemical performance critically depends on intimate solid–solid contact within the electrode stack. However, how the applied stress state governs the co-densification of mechanically dissimilar layers and their electrochemical functionality remains poorly understood. Here, we investigate the pressure-assisted consolidation of Li6PS5Cl separator/composite cathode bilayers under uniaxial and isostatic loading. Despite the contrasting mechanical response of the compliant separator and rigid composite cathode, all processing routes follow the same three-stage ceramic compaction mechanism. Isostatic loading and elevated temperature do not alter this mechanism but substantially improve densification efficiency and, more importantly, suppress the radial strain and center-to-edge density gradients inherent to uniaxial processing. The resulting lateral deformation compromises dimensional stability, which becomes increasingly critical for large-area electrodes and multilayer stacking. At the same time, locally under-densified edge regions provide mechanically weak, porous pathways for metal filament propagation and subsequent short circuiting. Warm isostatic pressing suppresses both lateral deformation and spatial densification heterogeneity, demonstrating that these limitations can be overcome by controlling the stress state during consolidation. These findings establish that a scalable densification process must provide not only sufficient average density, but homogeneous consolidation across the complete electrode while preserving its geometry, providing processing criteria for the development of large-area solid-state batteries.

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BibTeX
@misc{agrawal2026pressing,
  title = {{Pressing Mode Determines Densification Uniformity and Dimensional Stability in Sulfide Solid-State Batteries}},
  author = {Meenal Agrawal and Mika Serna Malmer and Mohsen Sadeqi-Moqadam and Quoc-Anh Tran and Roman Zettl and Volker Hennige and Daniel Rettenwander},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008313/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008313/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Pressing Mode Determines Densification Uniformity and Dimensional Stability in Sulfide Solid-State Batteries
AU  - Meenal Agrawal
AU  - Mika Serna Malmer
AU  - Mohsen Sadeqi-Moqadam
AU  - Quoc-Anh Tran
AU  - Roman Zettl
AU  - Volker Hennige
AU  - Daniel Rettenwander
PY  - 2026
DA  - 2026/09/04
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008313/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008313/v1
AB  - Pressure-assisted densification is essential for manufacturing sulfide solid-state batteries because electrochemical performance critically depends on intimate solid–solid contact within the electrode stack. However, how the applied stress state governs the co-densification of mechanically dissimilar layers and their electrochemical functionality remains poorly understood. Here, we investigate the pressure-assisted consolidation of Li6PS5Cl separator/composite cathode bilayers under uniaxial and isostatic loading. Despite the contrasting mechanical response of the compliant separator and rigid composite cathode, all processing routes follow the same three-stage ceramic compaction mechanism. Isostatic loading and elevated temperature do not alter this mechanism but substantially improve densification efficiency and, more importantly, suppress the radial strain and center-to-edge density gradients inherent to uniaxial processing. The resulting lateral deformation compromises dimensional stability, which becomes increasingly critical for large-area electrodes and multilayer stacking. At the same time, locally under-densified edge regions provide mechanically weak, porous pathways for metal filament propagation and subsequent short circuiting. Warm isostatic pressing suppresses both lateral deformation and spatial densification heterogeneity, demonstrating that these limitations can be overcome by controlling the stress state during consolidation. These findings establish that a scalable densification process must provide not only sufficient average density, but homogeneous consolidation across the complete electrode while preserving its geometry, providing processing criteria for the development of large-area solid-state batteries.
ER  -