All-solid-state Li–S batteries with fast solid–solid sulfur reaction

Huimin Song, Konrad Münch, Xu Liu, Kaier Shen, Ruizhuo Zhang, Timo Weintraut, Yuriy Yusim, Dequan Jiang, Xufeng Hong, Jiashen Meng, Yatao Liu, Mengxue He, Yitao Li, Philip Henkel, Torsten Brezesinski, Jürgen Janek and Quanquan Pang ()
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Huimin Song: Peking University
Konrad Münch: Justus Liebig University Giessen
Xu Liu: Peking University
Kaier Shen: Peking University
Ruizhuo Zhang: Karlsruhe Institute of Technology (KIT)
Timo Weintraut: Justus Liebig University Giessen
Yuriy Yusim: Justus Liebig University Giessen
Dequan Jiang: Peking University
Xufeng Hong: Peking University
Jiashen Meng: Peking University
Yatao Liu: Peking University
Mengxue He: Peking University
Yitao Li: Peking University
Philip Henkel: Karlsruhe Institute of Technology (KIT)
Torsten Brezesinski: Karlsruhe Institute of Technology (KIT)
Jürgen Janek: Justus Liebig University Giessen
Quanquan Pang: Peking University

Nature, 2025, vol. 637, issue 8047, 846-853

Abstract: Abstract With promises for high specific energy, high safety and low cost, the all-solid-state lithium–sulfur battery (ASSLSB) is ideal for next-generation energy storage1–5. However, the poor rate performance and short cycle life caused by the sluggish solid–solid sulfur redox reaction (SSSRR) at the three-phase boundaries remain to be solved. Here we demonstrate a fast SSSRR enabled by lithium thioborophosphate iodide (LBPSI) glass-phase solid electrolytes (GSEs). On the basis of the reversible redox between I− and I2/I3−, the solid electrolyte (SE)—as well as serving as a superionic conductor—functions as a surficial redox mediator that facilitates the sluggish reactions at the solid–solid two-phase boundaries, thereby substantially increasing the density of active sites. Through this mechanism, the ASSLSB exhibits ultrafast charging capability, showing a high specific capacity of 1,497 mAh g−1sulfur on charging at 2C (30 °C), while still maintaining 784 mAh g−1sulfur at 20C. Notably, a specific capacity of 432 mAh g−1sulfur is achieved on charging at an extreme rate of 150C at 60 °C. Furthermore, the cell demonstrates superior cycling stability over 25,000 cycles with 80.2% capacity retention at 5C (25 °C). We expect that our work on redox-mediated SSSRR will pave the way for developing advanced ASSLSBs that are high energy and safe.

Date: 2025
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DOI: 10.1038/s41586-024-08298-9

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