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Atomic-scale study clarifying the role of space-charge layers in a Li-ion-conducting solid electrolyte

Author

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  • Zhenqi Gu

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Jiale Ma

    (University of Science and Technology of China)

  • Feng Zhu

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Ting Liu

    (Tsinghua University
    Foshan (Southern China) Institute for New Materials)

  • Kai Wang

    (University of Science and Technology of China
    University of Science and Technology of China)

  • Ce-Wen Nan

    (Tsinghua University)

  • Zhenyu Li

    (University of Science and Technology of China)

  • Cheng Ma

    (University of Science and Technology of China
    University of Science and Technology of China
    National Synchrotron Radiation Laboratory)

Abstract

Space-charge layers are frequently believed responsible for the large resistance of different interfaces in all-solid-state Li batteries. However, such propositions are based on the presumed existence of a Li-deficient space-charge layer with insufficient charge carriers, instead of a comprehensive investigation on the atomic configuration and its ion transport behavior. Consequently, the real influence of space-charge layers remains elusive. Here, we clarify the role of space-charge layers in Li0.33La0.56TiO3, a prototype solid electrolyte with large grain-boundary resistance, through a combined experimental and computational study at the atomic scale. In contrast to previous speculations, we do not observe the Li-deficient space-charge layers commonly believed to result in large resistance. Instead, the actual space-charge layers are Li-excess; accommodating the additional Li+ at the 3c interstitials, such space-charge layers allow for rather efficient ion transport. With the space-charge layers excluded from the potential bottlenecks, we identify the Li-depleted grain-boundary cores as the major cause for the large grain-boundary resistance in Li0.33La0.56TiO3.

Suggested Citation

  • Zhenqi Gu & Jiale Ma & Feng Zhu & Ting Liu & Kai Wang & Ce-Wen Nan & Zhenyu Li & Cheng Ma, 2023. "Atomic-scale study clarifying the role of space-charge layers in a Li-ion-conducting solid electrolyte," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-37313-2
    DOI: 10.1038/s41467-023-37313-2
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    References listed on IDEAS

    as
    1. Feng Zhu & Md Shafiqul Islam & Lin Zhou & Zhenqi Gu & Ting Liu & Xinchao Wang & Jun Luo & Ce-Wen Nan & Yifei Mo & Cheng Ma, 2020. "Single-atom-layer traps in a solid electrolyte for lithium batteries," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
    2. Jürgen Janek & Wolfgang G. Zeier, 2016. "A solid future for battery development," Nature Energy, Nature, vol. 1(9), pages 1-4, September.
    3. Longlong Wang & Ruicong Xie & Bingbing Chen & Xinrun Yu & Jun Ma & Chao Li & Zhiwei Hu & Xingwei Sun & Chengjun Xu & Shanmu Dong & Ting-Shan Chan & Jun Luo & Guanglei Cui & Liquan Chen, 2020. "In-situ visualization of the space-charge-layer effect on interfacial lithium-ion transport in all-solid-state batteries," Nature Communications, Nature, vol. 11(1), pages 1-9, December.
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