Unveiling crystal orientation-dependent interface property in composite cathodes for solid-state batteries by in situ microscopic probe

Sunyoung Lee, Hayoung Park, Jae Young Kim, Jihoon Kim, Min-Ju Choi, Sangwook Han, Sewon Kim, Wonju Kim, Ho Won Jang, Jungwon Park () and Kisuk Kang ()
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Sunyoung Lee: Seoul National University
Hayoung Park: Seoul National University
Jae Young Kim: Seoul National University
Jihoon Kim: Seoul National University
Min-Ju Choi: Seoul National University
Sangwook Han: Seoul National University
Sewon Kim: Seoul National University
Wonju Kim: Seoul National University
Ho Won Jang: Seoul National University
Jungwon Park: Seoul National University
Kisuk Kang: Seoul National University

Nature Communications, 2024, vol. 15, issue 1, 1-11

Abstract: Abstract A critical bottleneck toward all-solid-state batteries lies in how the solid(electrode)-solid(electrolyte) interface is fabricated and maintained over repeated cycles. Conventional composite cathodes, with crystallographically distinct electrode/electrolyte interfaces of random particles, create complexities with varying (electro)chemical compatibilities. To address this, we employ an epitaxial model system where the crystal orientations of cathode and solid electrolyte are precisely controlled, and probe the interfaces in real-time during co-sintering by in situ electron microscopy. The interfacial reaction is highly dependent on crystal orientation/alignment, especially the availability of open ion channels. Interfaces bearing open ion paths of NCM are more susceptible to interdiffusion, but stabilize with the early formed passivation layer. Conversely, interfaces with closed ion pathway exhibit stability at intermediate temperatures, but deteriorate rapidly at high temperature due to oxygen evolution, increasing interfacial resistance. The elucidation of these distinct interfacial behaviors emphasizes the need for decoupling collective interfacial properties to enable rational design in solid-state batteries.

Date: 2024
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DOI: 10.1038/s41467-024-52226-4

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