Accelerated O─O Bond Cleavage and Stabilized Fe Sites by Synergistic d─p Fe─Sn Dual‐Atom Pair for Enhanced Oxygen Reduction

Abstract

Abstract Atomically dispersed FeNC materials have emerged as the promising catalysts for replacing precious Pt‐based catalysts in the oxygen reduction reaction (ORR). However, their widespread application remains limited by sluggish kinetics and the long‐term stability of the isolated Fe single‐atom sites. Herein, we report a highly active and durable catalyst (FeSnNC) featuring d‐block iron and p‐block‐metal tin dual‐atom pair sites. In situ infrared spectroscopy and X‐ray absorption spectroscopy, together with ab initio molecular dynamics and density functional theory calculations reveal that the Fe─Sn dual‐atom pair sites enable the bridge absorption of O 2 and facilitate direct O─O bond cleavage. The redirection of *OH desorption to the Sn site alleviates Fe‐site degradation, while Sn incorporation can also reinforce the Fe─N bond, jointly enhancing ORR activity and durability. Under alkaline conditions, the catalyst delivers a half‐wave potential of 0.91 V and a kinetic current density of 69 mA cm −2 at 0.85 V, with negligible performance loss after 10,000 cycles. When applied in a zinc–air battery, FeSnNC exhibits a peak power density of 262 mW cm −2 and a cycling lifetime exceeding 1,100 hours at 10 mA cm −2 . This work demonstrates the great potential of d–p metal atomic pair sites in ORR catalysis and provides new insights into the rational design of atomically precise metal catalysts.