A Fully Amorphous, Dynamic Cross‐Linked Polymer Electrolyte for Lithium‐Sulfur Batteries Operating at Subzero‐Temperatures

• Published in: Angewandte Chemie International Edition Vol. 63; no. 5; pp. e202316087 - n/a
• Main Authors: Zhang, Juan, Chou, Jia, Luo, Xiao‐Xi, Yang, Yi‐Ming, Yan, Ming‐Yan, Jia, Di, Zhang, Chao‐Hui, Wang, Ya‐Hui, Wang, Wen‐Peng, Tan, Shuang‐Jie, Guo, Jun‐Chen, Zhao, Yao, Wang, Fuyi, Xin, Sen, Wan, Li‐Jun, Guo, Yu‐Guo
• Format: Journal Article
• Language: English
• Published: Germany Wiley Subscription Services, Inc 25.01.2024
• Edition: International ed. in English
• Subjects: Batteries; Conduction heating; Electrochemistry; Electrolytes; Energy storage; Environmental conditions; Interface Stability; Ionic mobility; Liquid plasticizers; Lithium; Lithium sulfur batteries; Li−S Batteries; Low temperature; Low-Temperature Performance; Mathematical analysis; Mechanical properties; Plasticizers; Polymers; Solid Electrolyte Interfaces; Solid-State Batteries; Subzero temperature; Sulfur; Temperature; Interface Stability; Solid-State Batteries; Low-Temperature Performance; Li−S Batteries; Solid Electrolyte Interfaces
• ISSN: 1433-7851; 1521-3773; 1521-3773
• DOI: 10.1002/anie.202316087

Solid‐state lithium‐sulfur batteries have shown prospects as safe, high‐energy electrochemical storage technology for powering regional electrified transportation. Owing to limited ion mobility in crystalline polymer electrolytes, the battery is incapable of operating at subzero temperature. Addition of liquid plasticizer into the polymer electrolyte improves the Li‐ion conductivity yet sacrifices the mechanical strength and interfacial stability with both electrodes. In this work, we showed that by introducing a spherical hyperbranched solid polymer plasticizer into a Li+‐conductive linear polymer matrix, an integrated dynamic cross‐linked polymer network was built to maintain fully amorphous in a wide temperature range down to subzero. A quasi‐solid polymer electrolyte with a solid mass content >90 % was prepared from the cross‐linked polymer network, and demonstrated fast Li+ conduction at a low temperature, high mechanical strength, and stable interfacial chemistry. As a result, solid‐state lithium‐sulfur batteries employing the new electrolyte delivered high reversible capacity and long cycle life at 25 °C, 0 °C and −10 °C to serve energy storage at complex environmental conditions. We demonstrate a fully amorphous quasi‐solid polymer electrolyte with a dynamic cross‐linked network composed of a star‐shaped plasticising polymer and a linear poly‐1,3‐dioxolane. The electrolyte achieves high Li+ conductivity (2.96×10−4 S cm−1) and high tLi+ (0.81), and the as‐prepared solid‐state lithium‐sulfur batteries exhibit high reversible capacity and long cycle life when operating at subzero temperature conditions.