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Achieving physical blocking and chemical electrocatalysis of polysulfides by using a separator coating layer in lithium–sulfur batteries

锂硫电池中能同时实现多硫化锂的物理阻挡与化学 电催化作用的隔膜修饰层

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Abstract

The persistent challenges in slow redox reaction kinetics and the consequential issue of polysulfide shuttling still restrict the practical utilization of lithium-sulfur (Li–S) batteries. To address these problems, we present a meticulously designed separator coating layer composed of a hierarchical porous carbon framework decorated with FeS2 (FeS2/PCF). This innovative architecture enables simultaneous physical blockade of polysulfide diffusion and chemical electrocatalysis of polysulfide conversions. Polysulfide diffusion tests were conducted and the results demonstrate that PCF effectively hinders the polysulfide penetration and shuttling. Additionally, FeS2 with excellent electrocatalytic activity expedites the polysulfide transformation, as evidenced by secondary ion mass spectroscopy. Consequently, the modified Li–S batteries exhibit exceptional rate capability of 764 mA h g−1 at 5.0 C, and outstanding long-term cyclic stability with sustaining 698 mA h g−1 after 500 cycles at 1.0 C. Notably, the Li–S batteries achieve an impressive areal capacity of 7.52 mA h cm−2, while maintaining stable cyclic performances across a wide temperature range. This investigation offers valuable insights into the effective utilization of separator coating layers by employing both physical and chemical strategies.

摘要

锂硫电池的实际应用仍受制于一些挑战, 包括氧化还原动力学 缓慢和由此引发的穿梭效应等. 为解决这些问题, 我们巧妙合成了一种 由FeS2和分等级多孔碳结构(PCF)组成的隔膜修饰层. 这种新颖的结构 能同时实现对多硫化锂的物理阻挡与化学电催化效应. 多硫化锂扩散 实验证实PCF修饰的隔膜能够阻挡多硫化锂的渗透, 而飞行时间二次 离子质谱表明FeS2能催化多硫化锂快速转化. 因此, 修饰后的锂硫电池 表现出优异的倍率性能(5 C时比容量达764 mA h g−1)及显著的长循环 稳定性(1 C时循环500次后比容量为698 mA h g−1). 值得注意的是, 修饰 后的锂硫电池最高面积容量为7.52 mA h cm−2, 并且能够在较宽温域 (−20至60°C)保持高循环稳定性. 本研究为隔膜修饰层的高效应用提供 了有价值的见解

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (22005003), the Natural Science Research Project of Anhui Province Education Department (2022AH030046 and 2022AH050323), the Young Scholars of the Introduction and Education of Talents in Anhui Province, the Top Young Talents of Anhui University of Technology, and the Scientific Research Foundation of Anhui University of Technology for Talent Introduction.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Anhui University of Technology, Ma’anshan, 243002, China

    Qingzhu Wu  (吴庆柱), Liyuan Li  (李莉媛), Yushuang Zheng  (郑雨爽), Bo Peng  (彭波), Jie Xu  (徐杰), Ailin Xia  (夏爱林) & Lianbo Ma  (马连波)

  2. Carbon Cycle and Emission Control Research Center of Low-Carbon Research Institute, Institute of Clean Energy and Advanced Nanocatalysis, School of Chemistry and Chemical Engineering, Anhui University of Technology, Ma’anshan, 243002, China

    Konglin Wu  (吴孔林)

  3. Department of Mechanical and Aerospace Engineering, The Hong Kong University of Science and Technology, Hong Kong, 999077, China

    Lianbo Ma  (马连波)

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  1. Qingzhu Wu  (吴庆柱)
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  2. Liyuan Li  (李莉媛)
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  3. Yushuang Zheng  (郑雨爽)
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  4. Bo Peng  (彭波)
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  6. Konglin Wu  (吴孔林)
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  7. Ailin Xia  (夏爱林)
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  8. Lianbo Ma  (马连波)
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Contributions

Author contributions Wu Q, Wu K and Ma L designed and conceived the work. Wu Q and Ma L prepared and characterized the samples, and tested the battery performance. Li L, Zheng Y, Peng B and Xu J helped to analyze the data. Ma L wrote the original manuscript. Wu K and Xia A revised the manuscript. All the authors commented on the manuscript and have given approval to the final version of the manuscript.

Corresponding authors

Correspondence to Konglin Wu  (吴孔林) or Lianbo Ma  (马连波).

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Conflict of interest The authors declare that they have no conflict of interest.

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Supplementary information Supporting data are available in the online version of the paper.

Konglin Wu is an associate professor at the School of Chemistry and Chemical Engineering, Anhui University of Technology. He got his Bachelor’s degree and Master’s degree from Anhui Normal University in 2008 and 2011, respectively. He received his PhD degree from the Department of Chemistry, Tsinghua University in 2019 under the supervision of Prof. Yadong Li. His research interest focuses on the design and preparation of single atoms, clusters and micro/nanomaterials for energy storage and conversion, and organic catalysis.

Lianbo Ma is a professor at the School of Materials Science and Engineering, Anhui University of Technology. He received his PhD degree in physical chemistry from Nanjing University under the supervisions of Prof. Zhong Jin and Prof. Zheng Hu. Then, he got a postdoc position sponsored by the Hong Kong Innovation and Technology Fund (ITF), and worked at The Hong Kong University of Science and Technology (HKUST). His research mainly includes the development of novel micro/nanostructured materials for secondary batteries (lithium–sulfur batteries, zinc–iodine batteries, etc.), and the exploration of integrated energy conversion and storage systems.

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Achieving physical blocking and chemical electrocatalysis of polysulfides by using a separator coating layer in lithium–sulfur batteries

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Wu, Q., Li, L., Zheng, Y. et al. Achieving physical blocking and chemical electrocatalysis of polysulfides by using a separator coating layer in lithium–sulfur batteries. Sci. China Mater. 67, 107–115 (2024). https://doi.org/10.1007/s40843-023-2702-4

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