Quasi-Solid Electrolytes with Flexible Branches and Rigid Skeletons for High-Temperature Li Metal Batteries

IF 8.3 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY ACS Applied Materials & Interfaces Pub Date : 2025-03-14 DOI:10.1021/acsami.4c18835
Lanhua Ma, Jiwei Zhao, Mengjie Li, Hai Su, Yong Li, Yuansheng Liu, Hang Liu, Ewa Zygadło-Monikowska, Yunhua Xu
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Abstract

Quasi-solid electrolytes are poised to revolutionize the next generation of high-energy-density lithium metal batteries. However, they face considerable challenges in operating at high temperatures due to severe side reactions, particularly with high-voltage cathodes. Here, we fabricated a nonflammable quasi-solid electrolyte (QSE) using an in situ copolymerization method. This electrolyte features a copolymer host with both flexible branches and a rigid skeleton, along with fire-retardant fluorine- and phosphorus-based plasticizers. The flexible branches reduce crystallinity and facilitate lithium-ion migration, while the rigid skeleton provides excellent high-temperature stability. The optimized fluorine–phosphorus mixed plasticizer provides effective sequestration of highly reactive oxygen/hydroxide radicals, along with a wide electrochemical window (up to 4.7 V vs Li+/Li), thereby ensuring excellent interface stability and safety characteristics. Consequently, the resulting quasi-solid electrolyte demonstrates remarkable physicochemical and electrochemical properties, enabling highly reversible lithium plating-stripping processes and good compatibility with cathodes. Using the nonflammable QSE, a high capacity retention of 82.3% is achieved for LiFePO4 after 1000 cycles at a high current density of 5 C and 80 °C. The good compatibility with high-voltage cathodes was demonstrated by the stable cycling of LiCoO2 over 400 cycles at a high cutoff voltage of 4.5 V and an elevated temperature of 60 °C.

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ACS Applied Materials & Interfaces
ACS Applied Materials & Interfaces 工程技术-材料科学:综合
CiteScore
16.00
自引率
6.30%
发文量
4978
审稿时长
1.8 months
期刊介绍: ACS Applied Materials & Interfaces is a leading interdisciplinary journal that brings together chemists, engineers, physicists, and biologists to explore the development and utilization of newly-discovered materials and interfacial processes for specific applications. Our journal has experienced remarkable growth since its establishment in 2009, both in terms of the number of articles published and the impact of the research showcased. We are proud to foster a truly global community, with the majority of published articles originating from outside the United States, reflecting the rapid growth of applied research worldwide.
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