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Deciphering the critical role of interstitial volume in glassy sulfide superionic conductors

Author

Listed:
  • Han Su

    (Zhejiang University
    University of Western Ontario1151 Richmond St.)

  • Yu Zhong

    (Zhejiang University)

  • Changhong Wang

    (University of Western Ontario1151 Richmond St.
    Eastern Institute of Technology)

  • Yu Liu

    (Zhejiang University
    University of Western Ontario1151 Richmond St.)

  • Yang Hu

    (University of Western Ontario1151 Richmond St.)

  • Jingru Li

    (Zhejiang University)

  • Minkang Wang

    (Zhejiang University)

  • Longan Jiao

    (Ltd.)

  • Ningning Zhou

    (Ltd.)

  • Bing Xiao

    (Ltd.)

  • Xiuli Wang

    (Zhejiang University)

  • Xueliang Sun

    (University of Western Ontario1151 Richmond St.
    Eastern Institute of Technology)

  • Jiangping Tu

    (Zhejiang University)

Abstract

Sulfide electrolytes represent a crucial category of superionic conductors for all-solid-state lithium metal batteries. Among sulfide electrolytes, glassy sulfide is highly promising due to its long-range disorder and grain-boundary-free nature. However, the lack of comprehension regarding glass formation chemistry has hindered their progress. Herein, we propose interstitial volume as the decisive factor influencing halogen dopant solubility within a glass matrix. We engineer a Li3PS4-Li4SiS4 complex structure within the sulfide glassy network to facilitate the release of interstitial volume. Consequently, we increase the dissolution capacity of LiI to 40 mol% in 75Li2S-25P2S5 glass. The synthesized glass exhibits one of the highest ionic conductivities among reported glass sulfides. Furthermore, we develop a glassy/crystalline composite electrolyte to mitigate the shortcomings of argyrodite-type sulfides by utilizing our synthesized glass as the filler. The composite electrolytes effectively mitigate Li intrusion. This work unveils a protocol for the dissolution of halogen dopants in glass electrolytes.

Suggested Citation

  • Han Su & Yu Zhong & Changhong Wang & Yu Liu & Yang Hu & Jingru Li & Minkang Wang & Longan Jiao & Ningning Zhou & Bing Xiao & Xiuli Wang & Xueliang Sun & Jiangping Tu, 2024. "Deciphering the critical role of interstitial volume in glassy sulfide superionic conductors," Nature Communications, Nature, vol. 15(1), pages 1-14, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-46798-4
    DOI: 10.1038/s41467-024-46798-4
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    References listed on IDEAS

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    1. Fudong Han & Andrew S. Westover & Jie Yue & Xiulin Fan & Fei Wang & Miaofang Chi & Donovan N. Leonard & Nancy J. Dudney & Howard Wang & Chunsheng Wang, 2019. "High electronic conductivity as the origin of lithium dendrite formation within solid electrolytes," Nature Energy, Nature, vol. 4(3), pages 187-196, March.
    2. 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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