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

Zhijuan Zou, Pengfei Liu, Ruiyang Dou, Kaijun Liu, Yunlong Wang, Lixian Song (), Liping Tong, Guolu Yin (), Wenbin Kang, Wenlong Cai, Yaping Zhang, Hongbing Chen () and Yingze Song ()
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Zhijuan Zou: Southwest University of Science and Technology
Pengfei Liu: China Academy of Engineering Physics
Ruiyang Dou: China Academy of Engineering Physics
Kaijun Liu: Chongqing University
Yunlong Wang: Nanjing University of Aeronautics and Astronautics
Lixian Song: Southwest University of Science and Technology
Liping Tong: Southwest University of Science and Technology
Guolu Yin: Chongqing University
Wenbin Kang: Southwest University of Science and Technology
Wenlong Cai: Sichuan University
Yaping Zhang: Southwest University of Science and Technology
Hongbing Chen: China Academy of Engineering Physics
Yingze Song: Southwest University of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-61942-4

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