Article Cosintering the Anode Active Material with Li7La3Zr2O12 Solid Electrolyte for the All-Solid-State Battery: How to Predict the Interfacial Reaction at Elevated Temperatures

Zongqi He (Interdisciplinary Graduate School of Engineering Sciences, Kyushu University) ; Ken Watanabe (Kyushu University) ; Koichi Suematsu (Kyushu University) ; Kazutaka Mitsuishi SAMURAI ORCID (Center for Basic Research on Materials, National Institute for Materials Science) ; Kengo Shimanoe (Kyushu University)

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Zongqi He, Ken Watanabe, Koichi Suematsu, Kazutaka Mitsuishi, Kengo Shimanoe. Cosintering the Anode Active Material with Li7La3Zr2O12 Solid Electrolyte for the All-Solid-State Battery: How to Predict the Interfacial Reaction at Elevated Temperatures. ACS Applied Energy Materials. 2025, 8 (22), . https://doi.org/10.1021/acsaem.5c02930

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(abstract)

Cosintered all-solid-state batteries using Li₇La₃Zr₂O₁₂ (LLZ) attract attention for their high energy density and long cycle life, but forming low-resistance interfaces through cosintering remains challenging due to reaction phases from interdiffusion at high temperatures. This study identifies the lithium concentration (CLi, mol/cm³) as a key index for predicting the reactivity between LLZ and various anode materials during cosintering at 850 °C. Mixing LLZ with anode materials of different CLi values reveals that interfacial reactions are significant with low CLi materials because of lithium loss in LLZ. In contrast, high CLi materials such as Li₂SnO₃, Li₂TiO₃, and Li₃SbO₄ suppress reactions with LLZ, though interdiffusion still occurs at the interface, as shown by TEM and lattice parameter analysis. Densified composite pellets using LLZTBO−Li₂SnO₃ and LLZTBO−Li₂TiO₃ were successfully sintered, and half-cell tests demonstrated high capacity and coulombic efficiency for cosintered LLZTBO−Li₂SnO₃ anodes. This approach offers a rapid method to screen cosintered electrodes for garnet-type solid electrolytes, advancing high energy density battery development.

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Keyword: Anode, Garnet-type LLZ, Cosintered, All-solid-state, Lithium battery

Date published: 2025-11-24

Publisher: American Chemical Society

Journal:

  • ACS Applied Energy Materials (ISSN: 25740962) vol. 8 issue. 22

Funding:

  • JST JPMJKP24P1

Manuscript type: Publisher's version (Version of record)

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First published URL: https://doi.org/10.1021/acsaem.5c02930

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Updated at: 2025-12-24 11:59:50 +0900

Published on MDR: 2025-12-24 16:20:29 +0900

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