Structural and Interphasial Stabilities of Sulfurized Polyacrylonitrile (SPAN) Cathode

Tan, Sha; Rahman, Muhammad Mominur; Wu, Zhaohui; Liu, Haodong; Wang, Shen; Ghose, Sanjit; Zhong, Hui; Waluyo, Iradwikanari; Hunt, Adrian; Liu, Ping; Yang, Xiao-Qing; Hu, Enyuan

doi:10.1021/acsenergylett.3c00281

Title: Structural and Interphasial Stabilities of Sulfurized Polyacrylonitrile (SPAN) Cathode

Journal Article · 08 May 2023 · ACS Energy Letters

DOI: https://doi.org/10.1021/acsenergylett.3c00281 · OSTI ID:1984414

^[1]; Rahman, Muhammad Mominur ^[1]; Wu, Zhaohui ^[2]; Liu, Haodong ^[2]; Wang, Shen ^[2]; Ghose, Sanjit ^[3]; Zhong, Hui ^[4];

^[3];

^[2];

^[1];

^[1]

Brookhaven National Laboratory (BNL), Upton, NY (United States). Chemistry Division
Univ. of California San Diego, La Jolla, CA (United States)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Stony Brook Univ., NY (United States)

Sulfurized polyacrylonitrile (SPAN) has attracted a lot of attention because of its low cost, high capacity, and great reversibility. Due to its structural complexity and amorphous nature, reaction mechanism of SPAN is little understood. Here, for this paper, we study the structural and interphasial changes of SPAN using synchrotron-based pair distribution function (PDF) analysis and soft X-ray absorption spectroscopy (sXAS). PDF identifies key structural features, including C–S bond, sulfur dimer, and sulfur chain in SPAN. The sulfur dimer bridging the pyridine network partially converts to sulfur chain during the first charging. In the following cycles, sulfur chain goes through lithiation and delithiation with reversibility dependent on the electrolytes. SXAS reveals surface changes of SPAN. After the first cycle, a negatively charged carbon or fused benzene layer is formed, on top of which is another layer formed by the electrolyte decomposition. The layer formed by localized high concentration electrolyte is stable during cycling.

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

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Office of Sustainable Transportation. Vehicle Technologies Office (VTO)

Grant/Contract Number:: SC0012704

OSTI ID:: 1984414

Report Number(s):: BNL-224487-2023-JAAM

Journal Information:: ACS Energy Letters, Vol. 8, Issue 6; ISSN 2380-8195

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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