In Situ Forming Asymmetric Gel Polymer Electrolyte Enhances the Performance of High-Voltage Lithium Metal Batteries

With the rapid evolution of electric vehicle technology, concerns regarding range anxiety and safety have become increasingly pronounced. Battery systems with high specific energy and enhanced security, featuring ternary cathodes paired with lithium (Li) metal anodes, are poised to emerge as next-generation electrochemical devices. However, the asymmetric configuration of the battery structure, characterized by the robust oxidative behavior of the ternary cathodes juxtaposed with the vigorous reductive activity of the Li metal anodes, imposes elevated requisites for the electrolytes. Herein, a well-designed gel polymer electrolyte with asymmetric structure was successfully prepared based on the Ritter reaction of cyanoethyl poly(vinyl alcohol) (PVA-CN) and cationic ring-opening polymerization of s-Trioxane. With the aid of the sieving effect of separator, the