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PreprintCC BYChemRxiv

Fracture mechanics favors lower-than-expected stack pressures in halide solidstate batteries

  • Liqun Guo1,2
  • Jie Zheng1,2
  • Lihong Zhao1,2
  • Santosh Thapa3,4
  • Yanliang Liang1,2
  • Phat Tieu1,2
  • Mai Le1,2
  • Yang-Tse Cheng3,4
  • Robert L. Sacci5,6
  • Jagjit Nanda7,8,9,10
  • Yan Yao1,2,11,12,13
13 affiliations
  1. 1Department of Electrical and Computer Engineering and Texas Center for Superconductivity
  2. 2University of Houston
  3. 3Department of Physics and Astronomy
  4. 4University of Kentucky
  5. 5Chemical Sciences Division
  6. 6Oak Ridge National Laboratory
  7. 7Applied Energy Division
  8. 8SLAC National Laboratory
  9. 9Department of Materials Science and Engineering
  10. 10Stanford University
  11. 11Department of Earth and Environmental Engineering
  12. 12Columbia University
  13. 13Columbia Climate School
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Abstract

All-solid-state batteries promise safer, more energy-dense storage than cells built on liquid electrolytes. Among solid-state electrolytes, halide electrolytes offer high ionic conductivity, anodic stability, and room-temperature processability, yet stable cycling is typically achieved under stack pressures of tens to hundreds of megapascals, for reasons that remain unclear. Here we identify the unusually high susceptibility of brittle halide electrolytes to fracture as the mechanism underlying and show that stack pressure—conventionally applied to suppress mechanical damage—can instead promote it by enhancing strain transfer from the active materials to the surrounding electrolyte. Operando scanning electron microscopy captures crack initiation and propagation within electrolyte domains in composite cathodes driven by active material volume changes, while nanoindentation reveals an exceptionally low fracture toughness of 0.23 MPa·m1/2 for the representative halide electrolyte Li3YCl6, substantially lower than the 0.7−1.0 MPa·m1/2 for typical sulfide and oxide electrolytes. Pressure-dependent electrochemical and morphological analyses show that, although modest pressure is sufficient to maintain interparticle contact, increasing pressure beyond this level promotes electrolyte fracture and accelerates capacity loss. Guided by this insight, we demonstrate an anode-free halide pouch cell that retains 85% of its capacity over 200 cycles at C/3 under only 2 MPa. Together, these findings show that the high stack pressures widely used in halide solid-state batteries primarily compensate for the consequences of electrolyte fracture rather than reflecting the pressure intrinsically required for stable operation, establishing a mechanical basis for low-pressure halide solid-state batteries.

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Cite

BibTeXRIS
BibTeX
@misc{guo2026fracture,
  title = {{Fracture mechanics favors lower-than-expected stack pressures in halide solidstate batteries}},
  author = {Liqun Guo and Jie Zheng and Lihong Zhao and Santosh Thapa and Yanliang Liang and Phat Tieu and Mai Le and Yang-Tse Cheng and Robert L. Sacci and Jagjit Nanda and Yan Yao},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15009212/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009212/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Fracture mechanics favors lower-than-expected stack pressures in halide solidstate batteries
AU  - Liqun Guo
AU  - Jie Zheng
AU  - Lihong Zhao
AU  - Santosh Thapa
AU  - Yanliang Liang
AU  - Phat Tieu
AU  - Mai Le
AU  - Yang-Tse Cheng
AU  - Robert L. Sacci
AU  - Jagjit Nanda
AU  - Yan Yao
PY  - 2026
DA  - 2026/09/21
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15009212/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15009212/v1
AB  - All-solid-state batteries promise safer, more energy-dense storage than cells built on liquid electrolytes. Among solid-state electrolytes, halide electrolytes offer high ionic conductivity, anodic stability, and room-temperature processability, yet stable cycling is typically achieved under stack pressures of tens to hundreds of megapascals, for reasons that remain unclear. Here we identify the unusually high susceptibility of brittle halide electrolytes to fracture as the mechanism underlying and show that stack pressure—conventionally applied to suppress mechanical damage—can instead promote it by enhancing strain transfer from the active materials to the surrounding electrolyte. Operando scanning electron microscopy captures crack initiation and propagation within electrolyte domains in composite cathodes driven by active material volume changes, while nanoindentation reveals an exceptionally low fracture toughness of 0.23 MPa·m1/2 for the representative halide electrolyte Li3YCl6, substantially lower than the 0.7−1.0 MPa·m1/2 for typical sulfide and oxide electrolytes. Pressure-dependent electrochemical and morphological analyses show that, although modest pressure is sufficient to maintain interparticle contact, increasing pressure beyond this level promotes electrolyte fracture and accelerates capacity loss. Guided by this insight, we demonstrate an anode-free halide pouch cell that retains 85% of its capacity over 200 cycles at C/3 under only 2 MPa. Together, these findings show that the high stack pressures widely used in halide solid-state batteries primarily compensate for the consequences of electrolyte fracture rather than reflecting the pressure intrinsically required for stable operation, establishing a mechanical basis for low-pressure halide solid-state batteries.
ER  -