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

Park, Se Hwan; Naik, Kaustubh G.; Vishnugopi, Bairav S.; Xiao, Xianghui; Drakopoulos, Michael; Vo, Nghia T.; Zhong, Zhong; Mukherjee, Partha P.; Hatzell, Kelsey B.

doi:10.1021/acsnano.5c04431

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

Journal Article · Wed Jun 11 00:00:00 EDT 2025 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5c04431· OSTI ID:2587798

^[1]; Naik, Kaustubh G. ^[2]; Vishnugopi, Bairav S. ^[2]; ^[3]; Drakopoulos, Michael ^[3]; ^[3]; Zhong, Zhong ^[3]; Mukherjee, Partha P. ^[2]; ^[1]

Princeton Univ., NJ (United States)
Purdue Univ., West Lafayette, IN (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)

Solid-state batteries can offer higher energy density and improved safety compared to lithium ion batteries, which use flammable liquid electrolytes. Increasing the ratio of cathode active materials in composite cathodes enhances the energy density and reduces manufacturing costs. Changes in the ratio of cathode active materials alter the microstructure and chemo-mechanical response of a cathode during operation. Understanding the relationship between composition, microstructure, and chemo-mechanical interactions is critical for optimizing solid-state cathodes. Here, in this study, we engineered composite cathodes with varying ratios of LiNi_0.8Co_0.1Mn_0.1O₂ and Li₆PS₅Cl to systematically investigate the role of microstructural evolution in long-term chemo-mechanical transformations. Chemo-mechanical stresses resulting from the volume changes of the cathode active materials led to degradation mechanisms, such as fracture and interfacial delamination. Active material fracture and delamination led to underutilization of active material and significant capacity decay during cycling. Coatings that suppress active material-active material interactions during cycling may aid in suppressing the generation of local stress hotspots.

View Accepted Manuscript (DOE)

Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0023438; SC0023462; SC0012704

OSTI ID:: 2587798

Report Number(s):: BNL--228862-2025-JAAM

Journal Information:: ACS Nano, Journal Name: ACS Nano Journal Issue: 24 Vol. 19; ISSN 1936-086X; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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