Microwave-assisted solvothermal synthesis of nanostructured Ga-Doped Li7La3Zr2O12 solid electrolyte with enhanced densification and Li-ion conductivity
Seong-Jun Jo,
Young Gyu Jeon,
Dong-Kyu Kim,
Sang Yeop Hwang,
Byeong-Heon Lee,
Chea Yun Kang,
Seung-Hwan Lee,
Sung-Hwan Lim,
R. Vasant Kumar,
Yu-Jin Han,
Kwang-Bum Kim,
Hyun-Kyung Kim
Affiliations
Seong-Jun Jo
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Young Gyu Jeon
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Dong-Kyu Kim
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Sang Yeop Hwang
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Byeong-Heon Lee
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Chea Yun Kang
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Seung-Hwan Lee
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
Sung-Hwan Lim
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea
R. Vasant Kumar
Department of Materials Science and Metallurgy, University of Cambridge, 27 Charles Babbage Road, Cambridge, CB3 0FS, UK
Yu-Jin Han
Ulsan Advanced Energy Technology R&D Center, Korea Institute of Energy Research, Ulsan, 44776, Republic of Korea; Corresponding author. Ulsan Advanced Energy Technology R&D Center, Korea Institute of Energy Research, Ulsan, 44776, Republic of Korea.
Kwang-Bum Kim
Department of Materials Science and Engineering, Yonsei University, 134 Shinchon-dong, Seodaemoon-gu, Seoul, 120-749, Republic of Korea; Corresponding author. Department of Materials Science and Engineering, Yonsei University, 134 Shinchon-dong, Seodaemoon-gu, Seoul, 120-749, Republic of Korea.
Hyun-Kyung Kim
Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea; Interdisciplinary Program in Advanced Functional Materials and Devices Development, Kangwon National University, Chuncheon, 24341, Republic of Korea; Corresponding author. Department of Battery Convergence Engineering, Kangwon National University, 1 Kangwondaehak-gil, Chuncheon, 24341, Republic of Korea.
Garnet-type Li7La3Zr2O12 (LLZO) Li-ion solid electrolytes are promising candidates for safe, next-generation solid-state batteries. In this study, we synthesize Ga-doped LLZO (Ga–LLZO) electrolytes using a microwave-assisted solvothermal method followed by low-temperature heat treatment. The nanostructured precursor (<50 nm) produced by the microwave-assisted solvothermal process has a high surface energy, facilitating the reaction for preparing garnet-type Ga–LLZO powders (<800 nm) within a short time (<5 h) at a low calcination temperature (<700 °C). Additionally, the calcined nanostructured Ga–LLZO powder can be sintered to produce a high-density pellet with minimized grain boundaries under moderate sintering conditions (temperature: 1150 °C, duration: 10 h). The optimal doping concentration was determined to be 0.4 mol% Ga, which resulted significantly increased the ionic conductivity (1.04 × 10−3 S cm−1 at 25 °C) and stabilized the cycling performance over 1700 h at 0.4 mA cm−2. This approach demonstrates the potential to synthesize oxide-type solid electrolyte materials with improved properties for solid-state batteries.
