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Unveiling the autocatalytic growth of Li2S crystals at the solid-liquid interface in lithium-sulfur batteries

Author

Listed:
  • Zhen Wu

    (Nanjing University of Science and Technology
    Jiangsu University)

  • Mingliang Liu

    (Nanjing University of Science and Technology
    University of Fribourg)

  • Wenfeng He

    (Nanjing University of Science and Technology)

  • Tong Guo

    (Nanjing University of Science and Technology)

  • Wei Tong

    (Nanjing University of Science and Technology)

  • Erjun Kan

    (Nanjing University of Science and Technology)

  • Xiaoping Ouyang

    (Xiangtan University)

  • Fen Qiao

    (Jiangsu University)

  • Junfeng Wang

    (Jiangsu University)

  • Xueliang Sun

    (University of Western Ontario)

  • Xin Wang

    (Nanjing University of Science and Technology)

  • Junwu Zhu

    (Nanjing University of Science and Technology)

  • Ali Coskun

    (University of Fribourg)

  • Yongsheng Fu

    (Nanjing University of Science and Technology)

Abstract

Electrocatalysts are extensively employed to suppress the shuttling effect in lithium-sulfur (Li-S) batteries. However, it remains challenging to probe the sulfur redox reactions and mechanism at the electrocatalyst/LiPS interface after the active sites are covered by the solid discharge products Li2S/Li2S2. Here, we demonstrate the intrinsic autocatalytic activity of the Li2S (100) plane towards lithium polysulfides on single-atom nickel (SANi) electrocatalysts. Guided by theoretical models and experimental data, it is concluded that LiPS dissociates into Li2S2 and short-chain LiPS on the Li2S (100) plane. Subsequently, Li2S2 undergoes further lithiation to Li2S on the Li2S (100) surface, generating a new Li2S (100) layer, thus enabling the autocatalytic formation of a new Li2S (100) surface. Benefiting from the autocatalytic growth of Li2S, the concentration of LiPS in the electrolyte remains at a lower level, enabling Li-S batteries under high loading and low electrolyte conditions to exhibit superior electrochemical performance.

Suggested Citation

  • Zhen Wu & Mingliang Liu & Wenfeng He & Tong Guo & Wei Tong & Erjun Kan & Xiaoping Ouyang & Fen Qiao & Junfeng Wang & Xueliang Sun & Xin Wang & Junwu Zhu & Ali Coskun & Yongsheng Fu, 2024. "Unveiling the autocatalytic growth of Li2S crystals at the solid-liquid interface in lithium-sulfur batteries," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53797-y
    DOI: 10.1038/s41467-024-53797-y
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    References listed on IDEAS

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    1. Christian Prehal & Jean-Marc Mentlen & Sara Drvarič Talian & Alen Vizintin & Robert Dominko & Heinz Amenitsch & Lionel Porcar & Stefan A. Freunberger & Vanessa Wood, 2022. "On the nanoscale structural evolution of solid discharge products in lithium-sulfur batteries using operando scattering," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
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    4. Guangmin Zhou & Eunsu Paek & Gyeong S. Hwang & Arumugam Manthiram, 2015. "Long-life Li/polysulphide batteries with high sulphur loading enabled by lightweight three-dimensional nitrogen/sulphur-codoped graphene sponge," Nature Communications, Nature, vol. 6(1), pages 1-11, November.
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