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A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries

Author

Listed:
  • Tong-Tong Zuo

    (Justus Liebig University Giessen
    Justus-Liebig-University Giessen)

  • Raffael Rueß

    (Justus Liebig University Giessen
    Justus-Liebig-University Giessen)

  • Ruijun Pan

    (Justus Liebig University Giessen
    Justus-Liebig-University Giessen
    The University of Texas at Austin)

  • Felix Walther

    (Justus Liebig University Giessen
    Justus-Liebig-University Giessen)

  • Marcus Rohnke

    (Justus Liebig University Giessen
    Justus-Liebig-University Giessen)

  • Satoshi Hori

    (Tokyo Institute of Technology)

  • Ryoji Kanno

    (Tokyo Institute of Technology)

  • Daniel Schröder

    (Technische Universität Braunschweig)

  • Jürgen Janek

    (Justus Liebig University Giessen
    Justus-Liebig-University Giessen)

Abstract

All-solid-state batteries are intensively investigated, although their performance is not yet satisfactory for large-scale applications. In this context, the combination of Li10GeP2S12 solid electrolyte and LiNi1-x-yCoxMnyO2 positive electrode active materials is considered promising despite the yet unsatisfactory battery performance induced by the thermodynamically unstable electrode|electrolyte interface. Here, we report electrochemical and spectrometric studies to monitor the interface evolution during cycling and understand the reactivity and degradation kinetics. We found that the Wagner-type model for diffusion-controlled reactions describes the degradation kinetics very well, suggesting that electronic transport limits the growth of the degradation layer formed at the electrode|electrolyte interface. Furthermore, we demonstrate that the rate of interfacial degradation increases with the state of charge and the presence of two oxidation mechanisms at medium (3.7 V vs. Li+/Li 80%) triggers the structural instability and oxygen release at the positive electrode and leads to more severe degradation.

Suggested Citation

  • Tong-Tong Zuo & Raffael Rueß & Ruijun Pan & Felix Walther & Marcus Rohnke & Satoshi Hori & Ryoji Kanno & Daniel Schröder & Jürgen Janek, 2021. "A mechanistic investigation of the Li10GeP2S12|LiNi1-x-yCoxMnyO2 interface stability in all-solid-state lithium batteries," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-26895-4
    DOI: 10.1038/s41467-021-26895-4
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    References listed on IDEAS

    as
    1. M. Armand & J.-M. Tarascon, 2008. "Building better batteries," Nature, Nature, vol. 451(7179), pages 652-657, February.
    2. Simon Randau & Dominik A. Weber & Olaf Kötz & Raimund Koerver & Philipp Braun & André Weber & Ellen Ivers-Tiffée & Torben Adermann & Jörn Kulisch & Wolfgang G. Zeier & Felix H. Richter & Jürgen Janek, 2020. "Benchmarking the performance of all-solid-state lithium batteries," Nature Energy, Nature, vol. 5(3), pages 259-270, March.
    3. Jürgen Janek & Wolfgang G. Zeier, 2016. "A solid future for battery development," Nature Energy, Nature, vol. 1(9), pages 1-4, September.
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    1. Xing Zhou & Chia-Yu Chang & Dongfang Yu & Kai Zhang & Zhi Li & Shi-Kai Jiang & Yizhou Zhu & Yongyao Xia & Bing Joe Hwang & Yonggang Wang, 2025. "Li2ZrF6 protective layer enabled high-voltage LiCoO2 positive electrode in sulfide all-solid-state batteries," Nature Communications, Nature, vol. 16(1), pages 1-12, December.

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