Ampere-Hour-Scale Quasi-Solid-State Zinc–Air Batteries with a Wide Operating Temperature Range (−50 to 60 °C)

Quasi-solid-state Zn–air batteries typically exhibit limited rate capability (<10 mA cm–2), primarily due to sluggish oxygen electrocatalysis and unstable electrochemical interfaces. Herein, we report a realistic quasi-solid-state Zn–air battery featuring multiactive sites' MnFeCoNiRu high-entropy alloys uniformly anchored in carbon nanofibers (MnFeCoNiRu/CNF) as the air cathode and a poly(acrylamide-co-acrylic acid) organohydrogel as an antifreezing conductor electrolyte. The proposed (MnFeCoNiRu/CNF) exhibits superb bifunctional activity (ΔE = 0.64 V) and stability (>10,000 cycles) toward a reversible oxygen reaction, outperforming commercial Pt/C and RuO2, which is mainly due to MnFeCoNiRu/CNF possessing different active sites in oxygen reactions, as evidenced by in situ Raman spectroscopy and density functional theory. Furthermore, a poly(acrylamide-co-acrylic acid) organohydrogel with its multiple intermolecular hydrogen bond network modified by the addition of dimethyl sulfoxide reveals strength at a freezing temperature (−50 °C) with high chemical/mechanical robustness. A high capacity of 7.15 Ah and an energy density of 110 Wh kgcell–1 are normally measured in a quasi-solid-state Zn–air battery with a cycle test under 500 mA and 250/500 mAh conditions. Quasi-solid-state Zn–air batteries operate effectively at rates of 5–2000 mA over a wide temperature range from −50 to 60 °C.