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Anomalous metal segregation in lithium-rich material provides design rules for stable cathode in lithium-ion battery

Author

Listed:
  • Ruoqian Lin

    (Brookhaven National Laboratory)

  • Enyuan Hu

    (Brookhaven National Laboratory)

  • Mingjie Liu

    (Brookhaven National Laboratory)

  • Yi Wang

    (Chinese Academy of Sciences)

  • Hao Cheng

    (Xiamen University)

  • Jinpeng Wu

    (Lawrence Berkeley National Laboratory)

  • Jin-Cheng Zheng

    (Xiamen University
    Xiamen University Malaysia)

  • Qin Wu

    (Brookhaven National Laboratory)

  • Seongmin Bak

    (Brookhaven National Laboratory)

  • Xiao Tong

    (Brookhaven National Laboratory)

  • Rui Zhang

    (University of California)

  • Wanli Yang

    (Lawrence Berkeley National Laboratory)

  • Kristin A. Persson

    (Lawrence Berkeley National Laboratory
    University of California Berkeley)

  • Xiqian Yu

    (Chinese Academy of Sciences)

  • Xiao-Qing Yang

    (Brookhaven National Laboratory)

  • Huolin L. Xin

    (Brookhaven National Laboratory
    University of California)

Abstract

Despite the importance of studying the instability of delithiated cathode materials, it remains difficult to underpin the degradation mechanism of lithium-rich cathode materials due to the complication of combined chemical and structural evolutions. Herein, we use state-of-the-art electron microscopy tools, in conjunction with synchrotron X-ray techniques and first-principle calculations to study a 4d-element-containing compound, Li2Ru0.5Mn0.5O3. We find surprisingly, after cycling, ruthenium segregates out as metallic nanoclusters on the reconstructed surface. Our calculations show that the unexpected ruthenium metal segregation is due to its thermodynamic insolubility in the oxygen deprived surface. This insolubility can disrupt the reconstructed surface, which explains the formation of a porous structure in this material. This work reveals the importance of studying the thermodynamic stability of the reconstructed film on the cathode materials and offers a theoretical guidance for choosing manganese substituting elements in lithium-rich as well as stoichiometric layer-layer compounds for stabilizing the cathode surface.

Suggested Citation

  • Ruoqian Lin & Enyuan Hu & Mingjie Liu & Yi Wang & Hao Cheng & Jinpeng Wu & Jin-Cheng Zheng & Qin Wu & Seongmin Bak & Xiao Tong & Rui Zhang & Wanli Yang & Kristin A. Persson & Xiqian Yu & Xiao-Qing Yan, 2019. "Anomalous metal segregation in lithium-rich material provides design rules for stable cathode in lithium-ion battery," Nature Communications, Nature, vol. 10(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:10:y:2019:i:1:d:10.1038_s41467-019-09248-0
    DOI: 10.1038/s41467-019-09248-0
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    Cited by:

    1. Elisa Musella & Angelo Mullaliu & Thomas Ruf & Paula Huth & Domenica Tonelli & Giuliana Aquilanti & Reinhard Denecke & Marco Giorgetti, 2020. "Detailing the Self-Discharge of a Cathode Based on a Prussian Blue Analogue," Energies, MDPI, vol. 13(15), pages 1-13, August.
    2. Jonathan Schwartz & Zichao Wendy Di & Yi Jiang & Jason Manassa & Jacob Pietryga & Yiwen Qian & Min Gee Cho & Jonathan L. Rowell & Huihuo Zheng & Richard D. Robinson & Junsi Gu & Alexey Kirilin & Steve, 2024. "Imaging 3D chemistry at 1 nm resolution with fused multi-modal electron tomography," Nature Communications, Nature, vol. 15(1), pages 1-10, December.

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