Zinc-air batteries (ZnABs) with high theoretical capacity and environmental benignity are the most promising candidates for next-generation electronics.However,their large-scale applications are greatly hindered due to the lack of high-efficient and cost-effective electrocatalysts.Transition metal phosphides (TMPs) have been reported as promising electrocatalysts.Notably,(Ni1-xCrx)2P (0 ≤ x ≤ 0.15) is an unstable electrocatalyst,which undergoes in-situ electrochemical oxidation during the initial oxygen evolution reaction (OER) and even in the activation cycles,and is eventually converted to Cr-NiOOH serving as the actual OER active sites with high efficiency.Density functional theory (DFT) simulations and experimental results elucidate that the OER performance could be significantly promoted by the synergistic effect of surface engineering and electronic modulations by Cr doping and in-situ phase transformation.The constructed rechargeable ZnABs could stably cycle for more than 208 h at 5 mA cm-2,while the voltage degradation is negligible.Furthermore,the developed catalytic materials could be assembled into flexible and all-solid-state ZnABs to power wearable electronics with high performance.