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DOE OSTI · 3375241

Pressure Heterogeneity and Material Utilization in Thin-Film Solid-State Cathodes

Park, Se Hwan [Kookmin University, Seoul (Korea, Republic of); Princeton University, NJ (United States)]·Naik, Kaustubh G. [Purdue University, West Lafayette, IN (United States)]·Li, Zhuo [Princeton University, NJ (United States); Purdue University, West Lafayette, IN (United States)] (ORCID:0000000163883398)·Vishnugopi, Bairav S. [Purdue University, West Lafayette, IN (United States)]·Xiao, Xianghui [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000271423452)·Drakopoulos, Michael [Brookhaven National Laboratory (BNL), Upton, NY (United States)]·Vo, Nghia T. [Brookhaven National Laboratory (BNL), Upton, NY (United States)]·Zhong, Zhong [Brookhaven National Laboratory (BNL), Upton, NY (United States)]·Shyam, Badri [Xerion Advanced Battery Corporation, Kettering, OH (United States)]·Joshi, Prerna [Xerion Advanced Battery Corporation, Kettering, OH (United States)] (ORCID:0000000231571821)·Yang, Heng [Xerion Advanced Battery Corporation, Kettering, OH (United States)] (ORCID:000000017431932X)·Mukherjee, Partha P. [Purdue University, West Lafayette, IN (United States)]·Zahiri, Beniamin [University of Illinois Urbana-Champaign, IL (United States)] (ORCID:0000000305086416)·Braun, Paul V. [University of Illinois Urbana-Champaign, IL (United States)]·Hatzell, Kelsey B. [Princeton University, NJ (United States)]
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Abstract

Intimate interfacial contact between the solid electrolyte and the cathode active material is critical for maximizing cathode utilization in solid-state batteries. However, volume changes during electrochemical cycling induce internal stresses that drive interfacial degradation, particularly under nonuniform stack pressure. In this study, we employ in situ energy-dispersive X-ray diffraction tomography to visualize and quantify reaction heterogeneities across a 3 mm-diameter solid-state cathode with a well-defined interface. Our results reveal that regions under a lower stack pressure exhibit reduced material utilization and reversibility, which negatively affect the high-pressure regions. Interfacial degradation further impedes lithium-ion transport and amplifies microscale reaction heterogeneity. These findings highlight the critical role of stack pressure distribution in governing interfacial stability and electrochemical performance, offering important design insights into practical solid-state battery systems.

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36 MATERIALS SCIENCE

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Park, Se Hwan [Kookmin University, Seoul (Korea, Republic of); Princeton University, NJ (United States)], Naik, Kaustubh G. [Purdue University, West Lafayette, IN (United States)], Li, Zhuo [Princeton University, NJ (United States); Purdue University, West Lafayette, IN (United States)] (ORCID:0000000163883398), Vishnugopi, Bairav S. [Purdue University, West Lafayette, IN (United States)], Xiao, Xianghui [Brookhaven National Laboratory (BNL), Upton, NY (United States)] (ORCID:0000000271423452), Drakopoulos, Michael [Brookhaven National Laboratory (BNL), Upton, NY (United States)], Vo, Nghia T. [Brookhaven National Laboratory (BNL), Upton, NY (United States)], Zhong, Zhong [Brookhaven National Laboratory (BNL), Upton, NY (United States)], Shyam, Badri [Xerion Advanced Battery Corporation, Kettering, OH (United States)], Joshi, Prerna [Xerion Advanced Battery Corporation, Kettering, OH (United States)] (ORCID:0000000231571821), Yang, Heng [Xerion Advanced Battery Corporation, Kettering, OH (United States)] (ORCID:000000017431932X), Mukherjee, Partha P. [Purdue University, West Lafayette, IN (United States)], Zahiri, Beniamin [University of Illinois Urbana-Champaign, IL (United States)] (ORCID:0000000305086416), Braun, Paul V. [University of Illinois Urbana-Champaign, IL (United States)], Hatzell, Kelsey B. [Princeton University, NJ (United States)]. 2026-06-08. Pressure Heterogeneity and Material Utilization in Thin-Film Solid-State Cathodes. https://doi.org/10.1021/acsenergylett.6c01154

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DOE OSTI2026

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