The zinc-air battery (ZAB) exhibits promising potential for application in wearable devices due to its high energy density, low cost, and safety features. However, the semi-open structure of ZAB accelerates the evaporation of battery electrolytes and poses a potential risk of leakage. Herein, a novel polyacrylamide-co-sodium p-benzenesulfonate and carboxymethyl cellulose (PAS-CMC) double-network gel electrolyte was synthesized and utilized in a flexible ZAB. The prepared PAS-CMC exhibits exceptional electrical conductivity (315.53 mS cm−1), mechanical properties, as well as electrolyte retention capacity. The ZAB assembled by alkaline PAS-CMC exhibits remarkable stability during circulation for over 120 h. Compared with the traditional alkaline PAS-CMC electrolyte, the open-circuit voltage (2.03 V), operating voltage (1.90 V) and power density (164.3 mW cm−2) of the ZAB assembled by the acid-alkaline PAS-CMC prepared by the “sandwich” strategy have been significantly improved, showing excellent flexibility under various bending conditions without any degradation in performance. Furthermore, the interaction mechanisms between PAS-CMC/H2O and PAS-CMC/Zn were further elucidated by DFT calculation, thereby establishing a theoretical foundation for high-voltage flexible ZAB.
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