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Chemo-Mechanical Behavior and Stability of High-Loading Cathodes in Solid-State Batteries.

Se Hwan Park1, Kaustubh G Naik2, Bairav S Vishnugopi2

  • 1Andlinger Center for Energy and the Environment, Princeton University, Princeton, New Jersey 08540, United States.

ACS Nano
|June 11, 2025
PubMed
Summary

Engineered solid-state battery cathodes with varying ratios of active materials revealed that microstructural changes cause chemo-mechanical stresses. These stresses lead to material fracture and capacity decay, highlighting the need for protective coatings.

Keywords:
cathodechemo-mechanicsfracturesolid-state batteriesstress

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Area of Science:

  • Materials Science
  • Electrochemistry
  • Battery Technology

Background:

  • Solid-state batteries offer enhanced safety and energy density over traditional lithium-ion batteries.
  • Composite cathodes in solid-state batteries are key for improving energy density and reducing costs.
  • Understanding cathode microstructure and chemo-mechanical behavior is vital for performance.

Purpose of the Study:

  • To investigate the impact of varying cathode active material ratios on microstructural evolution.
  • To analyze the chemo-mechanical transformations and degradation mechanisms in composite cathodes.
  • To establish a link between composition, microstructure, and long-term performance.

Main Methods:

  • Engineered composite cathodes with different ratios of LiNi0.8Co0.1Mn0.1O2 and Li6PS5Cl.
  • Systematically studied microstructural evolution during operation.
  • Analyzed chemo-mechanical stresses and their effect on degradation.

Main Results:

  • Varying active material ratios altered cathode microstructure and chemo-mechanical response.
  • Volume changes induced chemo-mechanical stresses, leading to fracture and delamination.
  • Material degradation resulted in underutilization and significant capacity fade during cycling.

Conclusions:

  • Microstructural evolution and associated chemo-mechanical stresses are critical failure modes in solid-state battery cathodes.
  • Active material fracture and delamination directly cause capacity decay.
  • Protective coatings could mitigate stress hotspots and improve battery longevity.