Flexible, Self-Healing, and Fire-Resistant Polymer Electrolytes Fabricated via Photopolymerization for All-Solid-State Lithium Metal Batteries

The cyclophosphazene-based self-healing polymer electrolytes (CPSHPE) is designed and fabricated via the copolymerization of hexa(4-ethyl acrylate phenoxy) cyclotriphosphazene (HCP), (2-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)ethyl methacrylate) (UPyMA), and poly(ethylene glycol) methyl ether methacrylate (PEGMA) under UV irradiation. The cross-linking structure formed by HCP could effectively enhance the mechanical strength of the polymer electrolyte, and the cyclotriphosphazene as the core is able to improve the flame-retardant properties. Benefiting from the phenyl groups in HCP and the cross-linking structure, the CPSHPE shows high thermal stability (up to 300 °C). On the other hand, the supramolecular network fabricated by the dynamic ureido-pyrimidinone (UPy) dimers endows the polymer electrolyte with good self-healing capability and is expected to improve the reliability of polymer lithium batteries. Moreover, the cells were fabricated with LiFePO4 (LFP), CPSHPE, and Li anodes show good reversible specific capacity. The CPSHPE could be a promising candidate as the multifunctional polymer electrolyte to improve the safety performance of lithium metal batteries.