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

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, th...

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Main Authors: 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
Format: Article
Language:English
Published: Nature Portfolio 2025-07-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-025-61942-4
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author 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
author_facet 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
author_sort Zhijuan Zou
collection DOAJ
description 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.
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institution Kabale University
issn 2041-1723
language English
publishDate 2025-07-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj-art-467500c404864d2c92a5ef3a1dd63b222025-08-20T04:02:57ZengNature PortfolioNature Communications2041-17232025-07-0116111410.1038/s41467-025-61942-4γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cellsZhijuan Zou0Pengfei Liu1Ruiyang Dou2Kaijun Liu3Yunlong Wang4Lixian Song5Liping Tong6Guolu Yin7Wenbin Kang8Wenlong Cai9Yaping Zhang10Hongbing Chen11Yingze Song12State Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and TechnologyInstitute of Electronic Engineering, China Academy of Engineering PhysicsInstitute of Nuclear Physics and Chemistry, China Academy of Engineering PhysicsThe Key Laboratory of Optoelectronic Technology and Systems (Ministry of Education), Chongqing UniversityCollege of Materials Science and Technology, Nanjing University of Aeronautics and AstronauticsState Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and TechnologyState Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and TechnologyThe Key Laboratory of Optoelectronic Technology and Systems (Ministry of Education), Chongqing UniversityState Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and TechnologyDepartment of Adv. Energy Mater., College of Materials Science and Engineering, Sichuan UniversityState Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and TechnologyInstitute of Nuclear Physics and Chemistry, China Academy of Engineering PhysicsState Key Laboratory of Environment-Friendly Energy Materials, School of Materials and Chemistry, Southwest University of Science and TechnologyAbstract 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.https://doi.org/10.1038/s41467-025-61942-4
spellingShingle 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
γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells
Nature Communications
title γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells
title_full γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells
title_fullStr γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells
title_full_unstemmed γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells
title_short γ-Ray irradiated polyacrylamide networks enable high-performance Li||S pouch cells
title_sort γ ray irradiated polyacrylamide networks enable high performance li s pouch cells
url https://doi.org/10.1038/s41467-025-61942-4
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