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

Journal Article · · Nature (London)
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  1. University of California San Diego, La Jolla, CA (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  3. University of Houston, TX (United States)
  4. University of California, Santa Barbara, CA (United States)
  5. Johns Hopkins University, Baltimore, MD (United States)
  6. Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
  7. Honda Research Institute USA, Colombus, OH (United States)
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. However, the development of SSLSBs has been historically plagued by the insulating nature of sulfur and the poor interfacial contacts induced by its large volume change during cycling, impeding charge transfer among different solid components. 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.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Advanced Research Projects Agency - Energy (ARPA-E); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division (MSE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); National Science Foundation (NSF)
Grant/Contract Number:
SC0012704; AR0000781; EE0008864; AR0001191
OSTI ID:
2336571
Alternate ID(s):
OSTI ID: 2439230
Report Number(s):
BNL--225462-2024-JAAM
Journal Information:
Nature (London), Journal Name: Nature (London) Journal Issue: 8003 Vol. 627; ISSN 0028-0836
Publisher:
Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English

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