Healable and conductive sulfur iodide for solid-state Li-S batteries.
Jianbin ZhouManas Likhit Holekevi ChandrappaSha TanShen WangChaoshan WuHowie NguyenCanhui WangHaodong LiuSicen YuQuin R S MillerGayea HyunJohn HoloubekJunghwa HongYuxuan XiaoCharles SoulenZheng FanEric E FullertonChristopher J BrooksChao WangRaphaële J ClémentYan YaoEnyuan HuShyue Ping OngHaodong LiuPublished in: Nature (2024)
Solid-state Li-S batteries (SSLSBs) are made of low-cost and abundant materials free of supply chain concerns. Owing to their high theoretical energy densities, they are highly desirable for electric vehicles 1-3 . However, the development of SSLSBs has been historically plagued by the insulating nature of sulfur 4,5 and the poor interfacial contacts induced by its large volume change during cycling 6,7 , impeding charge transfer among different solid components. Here we report an S 9.3 I molecular crystal with I 2 inserted in the crystalline sulfur structure, which shows a semiconductor-level electrical conductivity (approximately 5.9 × 10 -7 S cm -1 ) at 25 °C; an 11-order-of-magnitude increase over sulfur itself. Iodine introduces new states into the band gap of sulfur and promotes the formation of reactive polysulfides during electrochemical cycling. Further, the material features a low melting point of around 65 °C, which enables repairing of damaged interfaces due to cycling by periodical remelting of the cathode material. As a result, an Li-S 9.3 I battery demonstrates 400 stable cycles with a specific capacity retention of 87%. The design of this conductive, low-melting-point sulfur iodide material represents a substantial advancement in the chemistry of sulfur materials, and opens the door to the practical realization of SSLSBs.