Atomic-Level Tailoring of the Electronic Metal-Support Interaction Between Pt-Co 3 O 4 Interfaces for High Hydrogen Evolution Performance.

Atomic-level modulation of the metal-oxide interface is considered an effective approach to optimize the electronic structure and catalytic activity of metal catalysts but remains highly challenging. Here, we employ the atomic layer deposition (ALD) technique together with a heteroatom doping strategy to effectively tailor the electronic metal-support interaction (EMSI) at the metal-oxide interface on the atomic level, thereby achieving high hydrogen evolution performance and Pt utilization. Theoretical calculations reveal that the doping of N atoms in Co 3 O 4 significantly adjusts the EMSI between Pt-Co 3 O 4 interfaces and, consequently, alters the d-band center of Pt and optimizes the adsorption/desorption of reaction intermediates. This work sheds light on the atomic-level regulation and mechanistic understanding of the EMSI in metal-oxide, while providing guidance for the development of advanced EMSI electrocatalysts for various future energy applications.