The rational design of metal oxide catalysts with enhanced oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) performance is crucial for the practical application of aqueous rechargeable zinc-air batteries (a-r-ZABs). Precisely regulating the electronic environment of metal-oxygen (M-O) active species is critical yet challenging for improving their activity and stability toward OER and ORR. Herein, we propose an atomic-level bilateral regulation strategy by introducing atomically dispersed Ga for continuously tuning the electronic environment of Ru-O and Mn-O in the Ga/MnRuO2 catalyst. The Ga/MnRuO2 catalyst breaks the stability-activity restriction, showing remarkable bifunctional performance with a low potential gap (ΔE) of 0.605 V and super durability with negligible performance degradation (300,000 ORR cycles or 30,000 OER cycles). The theoretical calculations revealed that the strong coupling electron interactions between Ga and Ru-O/Mn-O tuned the valence state distribution of the metal center, effectively modulating the adsorption behavior of *O/*OH, thus optimizing the reaction pathways and reducing the reaction barriers. The a-r-ZABs based on Ga/MnRuO2 catalysts exhibited excellent performance with a wide working temperature range of -20~60 °C and a long lifetime of 2308 hours (i.e., 13,848 cycles) under a current density of 5 mA cm-2 at -20 °C.
Keywords: Gallium; Oxygen electrocatalyst; Wide-temperature; zinc-air battery.
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