A LaCl3-based lithium superionic conductor compatible with lithium metal

Yi-Chen Yin, Jing-Tian Yang, Jin-Da Luo, Gong-Xun Lu, Zhongyuan Huang, Jian-Ping Wang, Pai Li, Feng Li, Ye-Chao Wu, Te Tian, Yu-Feng Meng, Hong-Sheng Mo, Yong-Hui Song, Jun-Nan Yang, Li-Zhe Feng, Tao Ma, Wen Wen, Ke Gong, Lin-Jun Wang, Huan-Xin Ju, Yinguo Xiao, Zhenyu Li (), Xinyong Tao () and Hong-Bin Yao ()
Additional contact information
Yi-Chen Yin: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Jing-Tian Yang: University of Science and Technology of China
Jin-Da Luo: University of Science and Technology of China
Gong-Xun Lu: College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou
Zhongyuan Huang: School of Advanced Materials, Peking University, Shenzhen Graduate School
Jian-Ping Wang: University of Science and Technology of China
Pai Li: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Feng Li: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Ye-Chao Wu: University of Science and Technology of China
Te Tian: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Yu-Feng Meng: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Hong-Sheng Mo: University of Science and Technology of China
Yong-Hui Song: University of Science and Technology of China
Jun-Nan Yang: University of Science and Technology of China
Li-Zhe Feng: University of Science and Technology of China
Tao Ma: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Wen Wen: Shanghai Synchroton Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences
Ke Gong: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Lin-Jun Wang: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
Huan-Xin Ju: PHI China Analytical Laboratory, CoreTech Integrated Ltd
Yinguo Xiao: School of Advanced Materials, Peking University, Shenzhen Graduate School
Zhenyu Li: Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China
Xinyong Tao: College of Materials Science and Engineering, Zhejiang University of Technology, Hangzhou
Hong-Bin Yao: Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China

Nature, 2023, vol. 616, issue 7955, 77-83

Abstract: Abstract Inorganic superionic conductors possess high ionic conductivity and excellent thermal stability but their poor interfacial compatibility with lithium metal electrodes precludes application in all-solid-state lithium metal batteries1,2. Here we report a LaCl3-based lithium superionic conductor possessing excellent interfacial compatibility with lithium metal electrodes. In contrast to a Li3MCl6 (M = Y, In, Sc and Ho) electrolyte lattice3–6, the UCl3-type LaCl3 lattice has large, one-dimensional channels for rapid Li+ conduction, interconnected by La vacancies via Ta doping and resulting in a three-dimensional Li+ migration network. The optimized Li0.388Ta0.238La0.475Cl3 electrolyte exhibits Li+ conductivity of 3.02 mS cm−1 at 30 °C and a low activation energy of 0.197 eV. It also generates a gradient interfacial passivation layer to stabilize the Li metal electrode for long-term cycling of a Li–Li symmetric cell (1 mAh cm−2) for more than 5,000 h. When directly coupled with an uncoated LiNi0.5Co0.2Mn0.3O2 cathode and bare Li metal anode, the Li0.388Ta0.238La0.475Cl3 electrolyte enables a solid battery to run for more than 100 cycles with a cutoff voltage of 4.35 V and areal capacity of more than 1 mAh cm−2. We also demonstrate rapid Li+ conduction in lanthanide metal chlorides (LnCl3; Ln = La, Ce, Nd, Sm and Gd), suggesting that the LnCl3 solid electrolyte system could provide further developments in conductivity and utility.

Date: 2023
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DOI: 10.1038/s41586-023-05899-8

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