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Maximizing interface stability in all-solid-state lithium batteries through entropy stabilization and fast kinetics

Author

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  • Xiangkun Kong

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

  • Run Gu

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

  • Zongzi Jin

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

  • Lei Zhang

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

  • Chi Zhang

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

  • Wenyi Xiang

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

  • Cui Li

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

  • Kang Zhu

    (University of Science and Technology of China)

  • Yifan Xu

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

  • Huang Huang

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

  • Xiaoye Liu

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

  • Ranran Peng

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

  • Chengwei Wang

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

Abstract

The positive electrode|electrolyte interface plays an important role in all-solid-state Li batteries (ASSLBs) based on garnet-type solid-state electrolytes (SSEs) like Li6.4La3Zr1.4Ta0.6O12 (LLZTO). However, the trade-off between solid-solid contact and chemical stability leads to a poor positive electrode|electrolyte interface and cycle performance. In this study, we achieve thermodynamic compatibility and adequate physical contact between high-entropy cationic disordered rock salt positive electrodes (HE-DRXs) and LLZTO through ultrafast high-temperature sintering (UHS). This approach constructs a highly stable positive electrode|electrolyte interface, reducing the interface resistance to 31.6 Ω·cm2 at 25 °C, making a 700 times reduction compared to the LiCoO2 | LLZTO interface. Moreover, the conformal and tight HE-DRX | LLZTO solid-state interface avoids the transition metal migration issue observed with HE-DRX in liquid electrolytes. At 150 °C, HE-DRXs in ASSLBs (Li|LLZTO | HE-DRXs) exhibit an average specific capacity of 239.7 ± 2 mAh/g at 25 mA/g, with a capacity retention of 95% after 100 cycles relative to the initial cycle—a stark contrast to the 76% retention after 20 cycles at 25 °C in conventional liquid batteries. Our strategy, which considers the principles of thermodynamics and kinetics, may open avenues for tackling the positive electrode|electrolyte interface issue in ASSLBs based on garnet-type SSEs.

Suggested Citation

  • Xiangkun Kong & Run Gu & Zongzi Jin & Lei Zhang & Chi Zhang & Wenyi Xiang & Cui Li & Kang Zhu & Yifan Xu & Huang Huang & Xiaoye Liu & Ranran Peng & Chengwei Wang, 2024. "Maximizing interface stability in all-solid-state lithium batteries through entropy stabilization and fast kinetics," Nature Communications, Nature, vol. 15(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51123-0
    DOI: 10.1038/s41467-024-51123-0
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    1. Jianping Huang & Peichen Zhong & Yang Ha & Deok-Hwang Kwon & Matthew J. Crafton & Yaosen Tian & Mahalingam Balasubramanian & Bryan D. McCloskey & Wanli Yang & Gerbrand Ceder, 2021. "Non-topotactic reactions enable high rate capability in Li-rich cathode materials," Nature Energy, Nature, vol. 6(7), pages 706-714, July.
    2. Yang Jin & Kai Liu & Jialiang Lang & Denys Zhuo & Zeya Huang & Chang-an Wang & Hui Wu & Yi Cui, 2018. "An intermediate temperature garnet-type solid electrolyte-based molten lithium battery for grid energy storage," Nature Energy, Nature, vol. 3(9), pages 732-738, September.
    3. Jürgen Janek & Wolfgang G. Zeier, 2016. "A solid future for battery development," Nature Energy, Nature, vol. 1(9), pages 1-4, September.
    4. Steven Chu & Arun Majumdar, 2012. "Opportunities and challenges for a sustainable energy future," Nature, Nature, vol. 488(7411), pages 294-303, August.
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