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Adding gold as the third element forming ternary Pt-based core–shell nanoparticles (NPs) is an efficient strategy for enhancing the durability of the cathode during the oxygen reduction reaction (ORR). Herein, using high-index (221) facets as a model catalyst, we discovered from density functional theory calculations that the inert Au atoms localized at the surface edge sites of Pt-based NPs can effectively promote the elementary steps of the ORR. Our results show that at the working potential (U = 0.8 V), the ORR at step/edges sites on Ni@AuPt core–shell NPs is kinetically much more facile than on pure Pt NPs, and the rate-determining step is likely to be O2 protonation forming *OOH against *O protonation forming *OH on Pt NPs. We identified that the surface activity of Pt atoms of core–shell NPs can be well explained by either the d-band model or the coordination-number model, which have the same chemical nature origin. Our study provides a fundamental understanding of functionality of step/edge sites of Pt-based core–shell NPs for the ORR, which can be used for engineering practical cathode catalysts with atomic efficiency and precision by maximizing the occupancy of gold atoms at edge sites.

Graphical abstract: Promoting the oxygen reduction reaction with gold at step/edge sites of Ni@AuPt core–shell nanoparticles

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