Flexible Zinc-Air batteries (FZABs) have been extensively investigated by researchers due to their exceptional safety and high energy density. The sandwich structure employed in FZABs imposes stringent demands on the electrolyte, necessitating good electrical conductivity and alkali resistance. In this paper, a carboxylation@Lignocellulose-based hydrogel polymer electrolyte with high ionic conductivity and excellent alkali resistance has designed and applied in FZABs. The carboxylation@lignocellulose is dissolved in a sodium hydroxide/urea/water system, followed by the incorporation of acrylamide monomers into the lignocellulose solution to prepare the hydrogel polymer electrolyte. The results combined suggest that the solid electrolyte exhibits improved ion conductivity, liquid absorption capability, and alkali resistance. Therefore, it has been confirmed that carboxyl functional groups have a positive effect on the performance of solid electrolytes. These characteristics enable the lignocellulose-based hydrogel polymer electrolyte FZAB to have an open-circuit voltage (1.34 V), a peak power density (141.55 mW cm−2), and a cycle lifetime to 65 h (555 cycles). Compared to FZABs based polyacrylamide-KOH hydrogel polymer electrolyte-based, FZABs utilizing lignocellulose-based hydrogel polymer electrolyte prepared in this paper demonstrate excellent performance.
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