Overcoming the conversion reaction limitation at three-phase interfaces using mixed conductors towards energy-dense solid-state Li–S batteries

Wang, Daiwei; Gwalani, Bharat; Wierzbicki, Dominik; Singh, Vijay; Jhang, Li-Ji; Rojas, Tomas; Kou, Rong; Liao, Meng; Ye, Lei; Jiang, Heng; Shan, Shuhua; Silver, Alexander; Ngo, Anh T.; Du, Yonghua; Li, Xiaolin; Wang, Donghai

doi:10.1038/s41563-024-02057-x

Title: Overcoming the conversion reaction limitation at three-phase interfaces using mixed conductors towards energy-dense solid-state Li–S batteries

Journal Article · 06 January 2025 · Nature Materials

DOI: https://doi.org/10.1038/s41563-024-02057-x · OSTI ID:2507152

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Pennsylvania State Univ., University Park, PA (United States)
Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Pennsylvania State Univ., University Park, PA (United States); Southern Methodist Univ., Dallas, TX (United States)

Lithium–sulfur (Li–S) all-solid-state batteries (ASSBs) hold great promise for next-generation safe, durable and energy-dense battery technology. However, solid-state sulfur conversion reactions are kinetically sluggish and primarily constrained to the restricted three-phase boundary area of sulfur, carbon and solid electrolytes, making it challenging to achieve high sulfur utilization. Here, in this study, we develop and implement mixed ionic–electronic conductors (MIECs) in sulfur cathodes to replace conventional solid electrolytes and invoke conversion reactions at sulfur–MIEC interfaces in addition to traditional three-phase boundaries. Microscopic and tomographic analyses reveal the emergence of mixed-conducting domains embedded in sulfur at sulfur–MIEC boundaries, helping promote the thorough conversion of active sulfur into Li₂S. Consequently, substantially improved active sulfur ratios (up to 87.3%) and conversion degrees (>94%) are achieved in Li–S ASSBs with high discharge capacity (>1,450 mAh g^–1) and long cycle life (>1,000 cycles). The strategy is also applied to enhance the active material utilization of other conversion cathodes.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Electricity (OE); USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); USDOE Office of Science (SC), Biological and Environmental Research (BER)

Grant/Contract Number:: AC05-76RL01830; EE0008862; SC0012704

OSTI ID:: 2507152

Report Number(s):: BNL--227526-2025-JAAM

Journal Information:: Nature Materials, Journal Name: Nature Materials Vol. 24; ISSN 1476-1122

Publisher:: Springer NatureCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Overcoming the conversion reaction limitation at three-phase interfaces using mixed conductors towards energy-dense solid-state Li–S batteries

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