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Volume 115
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Hydrogen-free cyclized polyacrylonitrile binder enables thermally robust lithium-ion batteries
Kai Chen a, Dian Zhang a, Feng Jiang a, Nai-Lu Shen a, Xiao-Hui Yan a, Ke-Feng Ren b, Xin Shen a *, Lungang Chen c, He Liu b *, Faxing Wang a, Shengjie Peng a, Yuping Wu a, Xin-Bing Cheng a *
a Z Energy Storage Center, School of Energy and Environment, Southeast University, Nanjing, 211189, China
b Jiangsu Key Laboratory of New Energy Devices & Interface Science, School of Chemistry and Materials Science, Nanjing University of Information Science and Technology, Nanjing, 210044, China
c Key Laboratory of Energy Thermal Conversion and Control of Ministry of Education, School of Energy and Environment, Southeast University, Nanjing, 211189, China
10.1016/j.partic.2026.05.005
Volume 115, August 2026, Pages 25-34
Received 15 April 2026, Revised 8 May 2026, Accepted 9 May 2026, Available online 16 May 2026, Version of Record 22 May 2026.
E-mail: shenx25@seu.edu.cn; liuhe@nuist.edu.cn; chengxb@seu.edu.cn
Highlights

• Cyclized polyacrylonitrile binder can inhibit the generation of hydrogen.

• Cyclized polyacrylonitrile binder serves as a lithium-ion storage material.

• Cyclized polyacrylonitrile binder suppresses side reactions of the electrolyte.


Abstract

Hydrogen generation during thermal runaway significantly elevates the risk of explosive combustion in lithium-ion batteries. Although hydrogen generated from binders constitutes a minor fraction, its absolute quantity remains substantial in large-scale stationary energy storage systems. Moreover, binder decomposition occurs during the later stages of thermal runaway with rapid reaction rates, further raising the danger level. Herein, graphite anode with polyacrylonitrile binder is in situ cyclized to eliminate the active hydrogen, while maintaining superior cohesiveness. On one hand, cyclized polyacrylonitrile with largely reduced hydrogen atoms can prevent binder-induced hydrogen generation and realize a reduction of hydrogen fraction by over 23%. As the three-dimensional cross-linking binders increase the thermal stability of anodes, the peak decomposition temperature of solid electrolyte interphase is increased from 150 to 200 °C to above 200 °C, while the peak reaction temperature between lithiated graphite and the electrolyte is delayed by at least 15 °C. On the other hand, the transformation from linear to cyclic molecular structures of cyclized polyacrylonitrile enables uniform and tight encapsulation of graphite and enhanced cohesiveness. Capacity retentions of 97% after 200 cycles in half cells and 72% after 800 cycles in full cells are achieved.

Graphical abstract
Keywords
Lithium-ion battery; Thermal runaway; Hydrogen; Binder; Cyclized polyacrylonitrile
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