DOE OSTI · 2507152
Overcoming the conversion reaction limitation at three-phase interfaces using mixed conductors towards energy-dense solid-state Li–S batteries
Abstract
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 Li 2 S. 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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Wang, Daiwei [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000328111071), Gwalani, Bharat [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000230216676), Wierzbicki, Dominik [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:0000000305587405), Singh, Vijay [Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000249852445), Jhang, Li-Ji [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:000000033376849X), Rojas, Tomas [Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0000000157454255), Kou, Rong [Pennsylvania State Univ., University Park, PA (United States)], Liao, Meng [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000285698860), Ye, Lei [Pennsylvania State Univ., University Park, PA (United States)], Jiang, Heng [Pennsylvania State Univ., University Park, PA (United States)], Shan, Shuhua [Pennsylvania State Univ., University Park, PA (United States)] (ORCID:0000000288400177), Silver, Alexander [Pennsylvania State Univ., University Park, PA (United States)], Ngo, Anh T. [Univ. of Illinois, Chicago, IL (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)] (ORCID:0009000345124795), Du, Yonghua [Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)] (ORCID:000000032655045X), Li, Xiaolin [Pacific Northwest National Laboratory (PNNL), Richland, WA (United States)] (ORCID:0000000277280157), Wang, Donghai [Pennsylvania State Univ., University Park, PA (United States); Southern Methodist Univ., Dallas, TX (United States)] (ORCID:0000000172618510). 2025-01-06. Overcoming the conversion reaction limitation at three-phase interfaces using mixed conductors towards energy-dense solid-state Li–S batteries. https://doi.org/10.1038/s41563-024-02057-x
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