Promoting Oxygen Reduction Reaction on Atomically Dispersed Fe Sites via Establishing Hydrogen Bonding with the Neighboring P Atoms

Single atom catalysts (SACs) comprised of nitrogen‐coordinated transition metal (TM–N–C) moieties show encouraging performance towards the oxygen reduction reaction (ORR). Nevertheless, for the reactions involving multiple intermediates, single‐atom sites fail to satisfactorily optimize the adsorption of all intermediates. Here, a facile strategy is reported to construct Fe, P dual‐atom sites in multimodal porous carbon (Fe,P‐DAS@MPC), and its superiority in synergistically boosting ORR is demonstrated. Fe,P‐DAS@MPC exhibits excellent ORR performance with substantially positive onset potential (Eonset = 1.02 V) and half‐wave potential (E1/2 = 0.92 V). Theoretical analysis unveils the cooperative effect of dual‐atom sites composed of adjacent P and Fe atoms, and the aiding of hydrogen bonding interaction can promote the adsorption/desorption of intermediates. Additionally, a Zn–air battery based on the Fe,P‐DAS@MPC shows a high peak power density and exceptional cycling stability. These findings provide a novel avenue towards the design of electrocatalysts with dual‐atom sites for practical energy conversion applications. A novel two‐step strategy is introduced to sequentially immobilize P and Fe atoms towards dual‐atom sites in multimodal porous carbon (Fe,P‐DAS@MPC). The cooperative effect of adjacent P and Fe single atoms endows Fe,P‐DAS@MPC with enhanced electrochemical oxygen reduction reaction (ORR) performance. The theoretical studies reveal that the hydrogen bonding interaction can promote the adsorption/desorption of ORR intermediates from dual‐atom sites.