Poly(benzoxazine)-Based Gel Polymer Electrolytes for Lithium Metal Batteries With Ultralong Lifespans.

Gel polymer electrolyte (GPE) is a desirable candidate for high-safety lithium batteries but is still plagued by the dynamic fluctuations of liquid electrolyte components, which induce localized fluid aggregation or leakage, ultimately leading to performance instability or even degradation. Here, we develop a novel poly(benzoxazine-propylene-oxide)-based GPE, achieving superior electrochemical performance and high safety simultaneously. Through molecular architecture design, the strategic incorporation of long-chain propylene-oxide segments and amide functionalities into the benzoxazine backbone endows the polymer matrix with enhanced lithium-ion transport capability.