电解质
材料科学
快离子导体
离子电导率
电化学窗口
热稳定性
电化学
脂质微区
锂(药物)
化学工程
化学稳定性
化学
物理化学
电极
膜
内分泌学
工程类
医学
生物化学
作者
Ye Guo,Xufeng Hong,Mengxue He,Junjie Song,Lujun Zhu,Chao Zheng,Yue Ma,Yun An,Kaier Shen,Weize Shi,Yongfeng Jia,Muhammad Burhan Shafqat,Peng Gao,Dingguo Xia,Fangfang Chen,Quanquan Pang
标识
DOI:10.1002/adma.202417829
摘要
Solid polymer electrolytes (SPEs) are promising for high-energy and high-safety solid-state lithium metal batteries (LMBs). Here, a polycationic solid electrolyte (PCSE) is described that leverages the inherent high thermal/chemical stability of the polycationic domain and the anion trapping (FMAT) effect of another fluorinated microdomain for stable and fast-charging high-voltage LMBs. Specifically, while the polycationic imidazolium backbone ensures high segmental flexibility facilitating the Li+ mobility, the fluorinated microdomain effectively traps the bis(trifluoromethanesulfonyl)imide anions by strong dipole interactions, imparting localized solvation and restricted mobility of the anions, as well as improved oxidation stability. As a result, the PCSE exhibits a high ionic conductivity of 1.4 mS cm-1, a high Li+ transference number of 0.50, and a wide electrochemical window of ∼5.5 V at 25 °C. By way of in situ thermal polymerization of the electrolyte within assembled cells, the PCSE enables ultra-stable cycling of Li|LiNi0.8Co0.1Mn0.1O2 cells with a capacity retention of 98.1% after 500 cycles at 0.2 C at ambient temperatures. The work on the molecular design of PCSEs represents a fundamentally unique perspective for the rational design of SPEs with balanced properties that are historically challenging for high-energy, long-life, ambient-temperature solid-state LMBs.
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