材料科学
电解质
离子液体
离子电导率
电化学
化学工程
聚合物
法拉第效率
氯化物
离子键合
无机化学
有机化学
离子
复合材料
化学
电极
冶金
物理化学
工程类
催化作用
作者
Oi Man Leung,Leo W. Gordon,Robert J. Messinger,Themis Prodromakis,J.A. Wharton,Carlos Ponce de León,Theresa Schoetz
标识
DOI:10.1002/aenm.202303285
摘要
Abstract Chloroaluminate ionic liquids are commonly used electrolytes in rechargeable aluminum batteries due to their ability to reversibly electrodeposit aluminum at room temperature. Progress in aluminum batteries is currently hindered by the limited electrochemical stability, corrosivity, and moisture sensitivity of these ionic liquids. Here, a solid polymer electrolyte based on 1‐ethyl‐3‐methylimidazolium chloride‐aluminum chloride, polyethylene oxide, and fumed silica is developed, exhibiting increased electrochemical stability over the ionic liquid while maintaining a high ionic conductivity of ≈13 mS cm −1 . In aluminum–graphite cells, the solid polymer electrolytes enable charging to 2.8 V, achieving a maximum specific capacity of 194 mA h g −1 at 66 mA g −1 . Long‐term cycling at 2.7 V showed a reversible capacity of 123 mA h g −1 at 360 mA g −1 and 98.4% coulombic efficiency after 1000 cycles. Solid‐state nuclear magnetic resonance spectroscopy measurements reveal the formation of five‐coordinate aluminum species that crosslink the polymer network to enable a high ionic liquid loading in the solid electrolyte. This study provides new insights into the molecular‐level design and understanding of polymer electrolytes for high‐capacity aluminum batteries with extended potential limits.
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