Song Huimin, Münch 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 Jürgen, Pang Quanquan
Beijing Key Laboratory for Theory and Technology of Advanced Battery Materials, School of Materials Science and Engineering, Peking University, Beijing, China.
Institute of Physical Chemistry, Justus Liebig University Giessen, Giessen, Germany.
Nature. 2025 Jan;637(8047):846-853. doi: 10.1038/s41586-024-08298-9. Epub 2025 Jan 15.
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 storage. 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 I/I, 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 on charging at 2C (30 °C), while still maintaining 784 mAh g at 20C. Notably, a specific capacity of 432 mAh g 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.
全固态锂硫电池（ASSLSB）具有高比能量、高安全性和低成本的优势，是下一代储能的理想选择。然而，三相边界处缓慢的固-固硫氧化还原反应（SSSRR）导致的倍率性能差和循环寿命短的问题仍有待解决。在此，我们展示了一种由硫代硼磷酸锂碘化物（LBPSI）玻璃相固体电解质（GSEs）实现的快速SSSRR。基于I与I/I之间的可逆氧化还原，固体电解质（SE）不仅作为超离子导体，还作为表面氧化还原介质，促进固-固两相边界处的缓慢反应，从而大幅增加活性位点的密度。通过这种机制，ASSLSB表现出超快充电能力，在2C（30°C）充电时具有1497 mAh g的高比容量，而在20C时仍保持784 mAh g。值得注意的是，在60°C下以150C的极端速率充电时，比容量达到432 mAh g。此外，该电池在5C（25°C）下经过25000次循环表现出优异的循环稳定性，容量保持率为80.2%。我们期望我们在氧化还原介导的SSSRR方面的工作将为开发高能量、安全的先进ASSLSB铺平道路。
