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<p>Binders are essential for maintaining positive electrode integrity in Li||S batteries and significantly affect their performance. However, commercial linear binders often have disordered networks, poor binding efficiency, and insufficient mechanical strength. To address these challenges, three-dimensional covalent binders offer a promising solution. Traditional methods for producing cross-linked binders require additives and result in poorly controlled polymer networks due to the stochastic nature of liquid-phase polymerization. Moreover, the mechanisms by which reticulated binders stabilize the positive electrode remain unclear, requiring investigation under operando conditions. Herein, we present an approach to tailor cross-linked polyacrylamide networks using solid-state operando γ-ray irradiation chemistry, which eliminates additives and produces a pure, ordered network with remarkable binding capabilities. By integrating in situ high-resolution optical frequency domain reflectometry, multiscale synchrotron radiation characterization, and virtual simulations, this study reveals the role of binders in dynamically encaging and confining sulfur. Specifically, γ-ray-enabled polyacrylamide networks enhance battery performance through mechanical strengthening, optimized sulfur regeneration, and improved re-occupancy. Consequently, the well-designed composite positive electrode structure with only 5.0 wt% binder improves soft-packaged Li||S battery performance across various scenarios. Notably, a 1.2-Ah pouch cell achieves 410.1 Wh kg<sup>−1</sup> specific energy with a low electrolyte/sulfur ratio of 3.0 µL mg<sup>–1</sup>.</p>

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γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年7月22日

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  • Zhijuan Zou,
  • Pengfei Liu,
  • Ruiyang Dou,
  • Kaijun Liu,
  • Yunlong Wang,
  • Lixian Song,
  • Liping Tong,
  • Guolu Yin,
  • Wenbin Kang,
  • Wenlong Cai,
  • Yaping Zhang,
  • Hongbing Chen,
  • Yingze Song

摘要

Binders are essential for maintaining positive electrode integrity in Li||S batteries and significantly affect their performance. However, commercial linear binders often have disordered networks, poor binding efficiency, and insufficient mechanical strength. To address these challenges, three-dimensional covalent binders offer a promising solution. Traditional methods for producing cross-linked binders require additives and result in poorly controlled polymer networks due to the stochastic nature of liquid-phase polymerization. Moreover, the mechanisms by which reticulated binders stabilize the positive electrode remain unclear, requiring investigation under operando conditions. Herein, we present an approach to tailor cross-linked polyacrylamide networks using solid-state operando γ-ray irradiation chemistry, which eliminates additives and produces a pure, ordered network with remarkable binding capabilities. By integrating in situ high-resolution optical frequency domain reflectometry, multiscale synchrotron radiation characterization, and virtual simulations, this study reveals the role of binders in dynamically encaging and confining sulfur. Specifically, γ-ray-enabled polyacrylamide networks enhance battery performance through mechanical strengthening, optimized sulfur regeneration, and improved re-occupancy. Consequently, the well-designed composite positive electrode structure with only 5.0 wt% binder improves soft-packaged Li||S battery performance across various scenarios. Notably, a 1.2-Ah pouch cell achieves 410.1 Wh kg−1 specific energy with a low electrolyte/sulfur ratio of 3.0 µL mg–1.