Abstract

Summary Designing highly efficient interface catalysts with new interface-enhancing mechanisms for the oxygen reduction reaction (ORR) in acid solution still remains a significant challenge. Here, we report a class of stable PtFe-Fe 2 C Janus-like nanoparticle (NP) interface catalysts with an unrevealed barrier-free interface electron-transfer property that greatly boosts ORR catalytic activity and stability. The PtFe-Fe 2 C Janus-like NPs showed much higher catalytic activity for ORR than either PtFe or Fe 2 C NPs in both acidic and alkaline electrolytes. Density functional theory simulations revealed that a barrier-free interface electron transfer on the interface of PtFe-Fe 2 C Janus-like NPs is the main factor in enhancing ORR activity. This interface electron-transfer property makes them the most active for ORR among all reported PtFe-based nanocatalysts. We further demonstrate that this barrier-free interface electron-transfer property can be readily generalized to other systems, such as the hydrogen evolution reaction and H 2 O 2 reduction electrocatalysis, to achieve better electrocatalytic enhancement.

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