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

• 成果类型: Article
• 署名作者: Song, Huimin; Muench, Konrad; Liu, Xu; Shen, Kaier; Zhang, Ruizhuo; Weintraut, Timo; Yusim, Yuriy; Jiang, Dequan; Hong, Xufeng; Meng, Jiashen; Liu, Yatao; He, Mengxue; Li, Yitao; Henkel, Philip; Brezesinski, Torsten; Janek, Juergen; Pang, Quanquan
• 署名单位: Peking University; Justus Liebig University Giessen; Justus Liebig University Giessen; Helmholtz Association; Karlsruhe Institute of Technology
• 刊物名称: Nature
• ISSN/ISSBN: 0028-3247
• DOI: 10.1038/s41586-024-08298-9
• 发表日期: 2025-01-23
• 关键词: superionic conductor; ionic-conductivity; redox; spectroscopy; glasses; metal; photoelectron; electrolytes; capacity; cathodes

摘要

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, 2, 3, 4-5. 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 degrees 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 degrees C. Furthermore, the cell demonstrates superior cycling stability over 25,000 cycles with 80.2% capacity retention at 5C (25 degrees C). We expect that our work on redox-mediated SSSRR will pave the way for developing advanced ASSLSBs that are high energy and safe.