Structural and Interphasial Stabilities of Sulfurized Polyacrylonitrile (SPAN) Cathode

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

doi:10.1021/acsenergylett.3c00281

Structural and Interphasial Stabilities of Sulfurized Polyacrylonitrile (SPAN) Cathode

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

Research output: Contribution to journal › Article › peer-review

15 Scopus citations

Abstract

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.

Original language	English
Pages (from-to)	2496-2504
Number of pages	9
Journal	ACS Energy Letters
Volume	8
Issue number	6
DOIs	https://doi.org/10.1021/acsenergylett.3c00281
State	Published - Jun 9 2023
Externally published	Yes

Funding

The work at Brookhaven National Laboratory is supported by the Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office, of the US Department of Energy (DOE) through the Advanced Battery Materials Research (BMR) Program including the Battery500 Consortium under contract no. DE-SC0012704. The same program also supports the work at UC San Diego through the Pacific Northwest National Laboratory under contract no. PNNL-595241. This research used 28-ID-2 (XPD) and 23-ID-2 (IOS) beamlines of the National Synchrotron Light Source II, U.S. DOE Office of Science User Facilities, operated for the DOE Office of Science by Brookhaven National Laboratory under contract no. DE-SC0012704.

Funders	Funder number
Assistant Secretary for Energy Efficiency and Renewable Energy, Vehicle Technology Office
Battery500 Consortium	DE-SC0012704
U.S. Department of Energy
Office of Science
Brookhaven National Laboratory
University of California, San Diego
Pacific Northwest National Laboratory	23-ID-2, PNNL-595241

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abstract = "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.",

author = "Sha Tan and Rahman, {Muhammad Mominur} and Zhaohui Wu and Haodong Liu and Shen Wang and Sanjit Ghose and Hui Zhong and Iradwikanari Waluyo and Adrian Hunt and Ping Liu and Yang, {Xiao Qing} and Enyuan Hu",

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doi = "10.1021/acsenergylett.3c00281",

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AU - Tan, Sha

AU - Rahman, Muhammad Mominur

AU - Wu, Zhaohui

AU - Liu, Haodong

AU - Wang, Shen

AU - Ghose, Sanjit

AU - Zhong, Hui

AU - Waluyo, Iradwikanari

AU - Hunt, Adrian

AU - Liu, Ping

AU - Yang, Xiao Qing

AU - Hu, Enyuan

PY - 2023/6/9

Y1 - 2023/6/9

N2 - 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.

AB - 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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Structural and Interphasial Stabilities of Sulfurized Polyacrylonitrile (SPAN) Cathode

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