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Structural and Interphasial Stabilities of Sulfurized Polyacrylonitrile (SPAN) Cathode AITranslate

Sha Tan; Muhammad Mominur Rahman; Zhaohui Wu; Haodong Liu; Shen Wang; Sanjit Ghose; Hui Zhong; Iradwikanari Waluyo; Adrian Hunt; Ping Liu; XiaoQing Yang; Enyuan Hu;
Brookhaven National Laboratory; Brookhaven National Laboratory; University of California San Diego; University of California San Diego; University of California San Diego; Brookhaven National Laboratory; Stony Brook University; Brookhaven National Laboratory; Brookhaven National Laboratory; University of California San Diego; Brookhaven National Laboratory; Brookhaven National Laboratory
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Publisher: ACS
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Abstract AITranslate

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 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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DOI：https://doi.org/10.1021/acsenergylett.3c00281

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Citation Information:

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 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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GB/T 7714-2015 [1] Sha Tan, Muhammad Mominur Rahman, Zhaohui Wu, et al. ACS Energy Letters, 2023(8). DOI:10.1021/acsenergylett.3c00281.
MLA [1] Sha Tan, et al., ACS Energy Letters, no. 8, 2023, https://doi.org/10.1021/acsenergylett.3c00281.
APA [1] Sha Tan, Muhammad Mominur Rahman, Zhaohui Wu, Haodong Liu, Shen Wang, Sanjit Ghose, Hui Zhong, Iradwikanari Waluyo, Adrian Hunt, Ping Liu, XiaoQing Yang, & Enyuan Hu. (2023). ACS Energy Letters(8). https://doi.org/10.1021/acsenergylett.3c00281
IEEE [1] Sha Tan, Muhammad Mominur Rahman, Zhaohui Wu, Haodong Liu, Shen Wang, Sanjit Ghose, Hui Zhong, Iradwikanari Waluyo, Adrian Hunt, Ping Liu, XiaoQing Yang, and Enyuan Hu, ACS Energy Letters, no. 8, 2023, doi: 10.1021/acsenergylett.3c00281.