Geometric and Electronic Engineering in Co/VN Nanoparticles to Boost Bifunctional Oxygen Electrocatalysis for Aqueous/Flexible Zn‐Air Batteries

Abstract Modulating metal‐metal and metal‐support interactions is one of the potent tools for augmenting catalytic performance. Herein, highly active Co/VN nanoparticles are well dispersed on three‐dimensional porous carbon nanofoam (Co/VN@NC) with the assistance of dicyandiamide. Studies certify that the consequential disordered carbon substrate reinforces the confinement of electrons, while the coupling of diverse components optimizes charge redistribution among species. Besides, theoretical analyses confirm that the regulated electron configuration can significantly tune the binding strength between the active sites and intermediates, thus optimizing reaction energy barriers. Therefore, Co/VN@NC exhibits a competitive potential difference (ΔE, 0.65 V) between the half‐wave potential of ORR and OER potential at 10 mA cm −2 , outperforming Pt/C+RuO 2 (0.67 V). Further, catalyst‐based aqueous/flexible ZABs present superior performances with peak power densities of 156 and 85 mW cm −2 , superior to Pt/C‐based counterparts (128 and 73 mW cm −2 ). This research provides a pivotal foundation for the evolution of bifunctional catalysts in the energy sector.