Healable and conductive sulfur iodide for solid-state Li–S batteries

Jianbin Zhou, Manas Likhit Holekevi Chandrappa, Sha Tan, Shen Wang, Chaoshan Wu, Howie Nguyen, Canhui Wang, Haodong Liu, Sicen Yu, Quin R. S. Miller, Gayea Hyun, John Holoubek, Junghwa Hong, Yuxuan Xiao, Charles Soulen, Zheng Fan, Eric E. Fullerton, Christopher J. Brooks, Chao Wang, Raphaële J. Clément, Yan Yao, Enyuan Hu, Shyue Ping Ong () and Ping Liu ()
Additional contact information
Jianbin Zhou: University of California, San Diego
Manas Likhit Holekevi Chandrappa: University of California, San Diego
Sha Tan: Brookhaven National Laboratory
Shen Wang: University of California, San Diego
Chaoshan Wu: Materials Science and Engineering Program and Texas Center for Superconductivity at the University of Houston, University of Houston
Howie Nguyen: University of California
Canhui Wang: Johns Hopkins University
Haodong Liu: University of California, San Diego
Sicen Yu: University of California, San Diego
Quin R. S. Miller: Pacific Northwest National Laboratory
Gayea Hyun: University of California, San Diego
John Holoubek: University of California, San Diego
Junghwa Hong: University of California, San Diego
Yuxuan Xiao: Center for Memory and Recording Research, University of California, La Jolla
Charles Soulen: University of California, San Diego
Zheng Fan: University of Houston
Eric E. Fullerton: Center for Memory and Recording Research, University of California, La Jolla
Christopher J. Brooks: Honda Research Institute USA, 99P Labs
Chao Wang: Johns Hopkins University
Raphaële J. Clément: University of California
Yan Yao: Materials Science and Engineering Program and Texas Center for Superconductivity at the University of Houston, University of Houston
Enyuan Hu: Brookhaven National Laboratory
Shyue Ping Ong: University of California, San Diego
Ping Liu: University of California, San Diego

Nature, 2024, vol. 627, issue 8003, 301-305

Abstract: Abstract 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 vehicles1–3. However, the development of SSLSBs has been historically plagued by the insulating nature of sulfur4,5 and the poor interfacial contacts induced by its large volume change during cycling6,7, impeding charge transfer among different solid components. Here we report an S9.3I molecular crystal with I2 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–S9.3I 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.

Date: 2024
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DOI: 10.1038/s41586-024-07101-z

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