Achieving Highly Durable Intermetallic PtMn₃N Electrocatalyst via the Strong Metal‐N Bonds toward Oxygen Reduction Reaction

Abstract Pt‐based intermetallic compounds have been considered promising electrocatalysts in the practical applications of fuel cells; however, the development of Pt‐based catalysts that meet performance targets of high activity, maximized stability, and low cost remains a huge challenge. Herein, an atomically ordered and low‐Pt intermetallic nitride (PtMn 3 N) catalyst are synthesized consisting of a strained Pt shell and PtMn 3 N core on carbon support via the KCl‐matrix protection strategy. The PtMn 3 N catalyst represents a high mass activity of 0.70 A mg Pt −1 at 0.9 V and a specific activity degradation of 4.2% after 5000 potential cycles for the oxygen reduction reaction (ORR) in rotating disk electrode (RDE) testing, which substantially outperformed commercial Pt/C (0.25 A mg Pt −1 and 17.4%). Density functional theory calculations reveal that the introduction of Mn elements to the Pt lattice is beneficial to produce appropriate compressive strain to weaken the binding energy of oxygen species and the introduction of N elements to promote the strong metal‐N interactions is conducive to alleviating the dissolution of metal atoms, allowing for displaying the prominent durability. This work provides an effective strategy of N‐doped Pt‐based intermetallic compounds to enhance the corrosion resistance of 3d transition metals and to enhance the ORR performance.