journal article·2025-01-28

Deciphering the Sulfur-Involved Bonding Interactions in Sulfurized Polyacrylonitrile: The Formation Thermodynamics and the Roles in Electrochemical Characteristics

Jingyi Xie, Junxiong Chen, Lingling Guo, Yande Li, Yibo Wang, Shun Zheng, Nian Zhang, Jianwei Meng, Kaiyu Zhang, Qinghao Li, Tsu-Chien Weng, Pengfei Yu, Xiaosong Liu

ACS Nano· Volume 19· Issue 3
Publisher page

Abstract

Sulfurized polyacrylonitrile (SPAN) exhibits a very high cycle stability by overcoming the shuttle effect of conventional Li-S batteries. However, there are still controversies in SPAN about the bonding types of sulfur with the matrix, their critical synthesis temperature regions, and their roles in the electrochemical lithium storage reaction, seriously hindering the economical synthesis of SPAN, the optimization of performances, and the exploration of other SPAN-like alternatives. The key to solving the above problems lies in accurate measurements of the thermodynamic evolution of bonding interactions in the synthesis process as well as in the electrochemical process. In this study, soft and tender X-ray absorption spectroscopy (XAS) is utilized to achieve a fine resolution of specific bonding interactions through the selective excitation of C, N, and S. Sulfur-involved bonding interactions have been elucidated, including the bonding type, critical temperature region, linking site, and their interplays. Furthermore, their contributions to lithium storage and their regulations on electrochemical performances are discussed. This study demonstrates the resolving capability of XAS for organic electrode materials and provides insights for further analyzing the cyclability of SPAN and rationally designing alternatives from the perspective of bonding interactions.
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Research context

OpenAlex topics: Advanced Battery Materials and Technologies · Advancements in Battery Materials · Advanced Battery Technologies Research

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Affiliations

State Key Laboratory of Functional Materials for Informatics, Shanghai Institute of Microsystem and Information Technology, Chinese Academy of Sciences, Shanghai 200050, China

University of the Chinese Academy of Sciences, Beijing 100049, China

School of Physical Science and Technology, ShanghaiTech University, Shanghai 201210, China

Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China

National Synchrotron Radiation Laboratory, University of Science and Technology of China, Hefei, Anhui 230029, China

School of Chemistry and Chemical Engineering, In Situ Center for Physical Sciences and Global Institute of Future Technology, Shanghai Jiao Tong University, Shanghai 200240, China

Center for Transformative Science, ShanghaiTech University, Shanghai 201210, China

College of Physics, Center for Marine Observation and Communications, Qingdao University, Qingdao, Shandong 266071, China

Tianmu Lake Institute of Advanced Energy Storage Technologies, Liyang, Jiangsu 213300, China

Funding

National Key Research and Development Program of China · Science and Technology Commission of Shanghai Municipality · National Natural Science Foundation of China

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