Non‐Covalent Interaction of Atomically Dispersed Cu and Zn Pair Sites for Efficient Oxygen Reduction Reaction

Abstract Dual–single‐atom catalysts with synergistic effect of adjacent atomic metal sites show a great potential for oxygen reduction reaction (ORR). Herein, a dynamical synthetic strategy is demonstrated for the rational design of dual‐atom catalyst ((Zn, Cu) − NC) with non‐covalent Cu and Zn sites as nitrogen‐doped carbon as support. Owing to the non‐covalent interaction of Zn and Cu atomic pair sites, (Zn, Cu) − NC exhibits significant performances for ORR, surpassing the catalysts with individual Zn or Cu site. The theoretical calculations reveal that (Zn, Cu) − NC can highly activate the linear O 2 molecule via the non‐covalent interaction between Zn and Cu pairs, providing the more effective overlap between the metal 3d orbitals and O 2p orbital. Therefore, the ORR activity is optimized with the improvement of the adsorption configuration and adsorption energy of O 2 . Further, both liquid and quasi‐solid zinc − air batteries with (Zn, Cu) − NC as air cathodes achieve remarkable energy density and stability. This research proposes a facile synthetic strategy to construct single‐atom catalysts and presents an insightful understanding of the non‐covalent interplay between heteronuclear metal atoms in dual‐atom catalysts.