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A LaCl3-based lithium superionic conductor compatible with lithium metal

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  • Yi-Chen Yin

    (Hefei National Research Center for Physical Sciences at the Microscale, University of Science and Technology of China
    University of Science and Technology of China
    Key Laboratory of Precision and Intelligent Chemistry, 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
    Institute of Engineering Research, Hefei Gotion High-Tech Co. Ltd)

  • 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
    University of Science and Technology of China)

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.

Suggested Citation

  • 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-, 2023. "A LaCl3-based lithium superionic conductor compatible with lithium metal," Nature, Nature, vol. 616(7955), pages 77-83, April.
    • Handle: RePEc:nat:nature:v:616:y:2023:i:7955:d:10.1038_s41586-023-05899-8
    DOI: 10.1038/s41586-023-05899-8
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    Cited by:

    1. Xiang Xu & Yunxin Chen & Pengbin Liu & Hao Luo & Zexin Li & Dongyan Li & Haoyun Wang & Xingyu Song & Jinsong Wu & Xing Zhou & Tianyou Zhai, 2024. "General synthesis of ionic-electronic coupled two-dimensional materials," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    2. Chengyu Fu & Yifan Li & Wenjie Xu & Xuyong Feng & Weijian Gu & Jue Liu & Wenwen Deng & Wei Wang & A. M. Milinda Abeykoon & Laisuo Su & Lingyun Zhu & Xiaojun Wu & Hongfa Xiang, 2024. "LaCl3-based sodium halide solid electrolytes with high ionic conductivity for all-solid-state batteries," Nature Communications, Nature, vol. 15(1), pages 1-9, December.
    3. Daems, K. & Yadav, P. & Dermenci, K.B. & Van Mierlo, J. & Berecibar, M., 2024. "Advances in inorganic, polymer and composite electrolytes: Mechanisms of Lithium-ion transport and pathways to enhanced performance," Renewable and Sustainable Energy Reviews, Elsevier, vol. 191(C).
    4. Zhenyou Song & Tengrui Wang & Hua Yang & Wang Hay Kan & Yuwei Chen & Qian Yu & Likuo Wang & Yini Zhang & Yiming Dai & Huaican Chen & Wen Yin & Takashi Honda & Maxim Avdeev & Henghui Xu & Jiwei Ma & Yu, 2024. "Promoting high-voltage stability through local lattice distortion of halide solid electrolytes," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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