Mussel‐Inspired Self‐Assembly of PtO 4 Atomic Catalysts for Interfacial Synergistic Hydrogen Evolution

Abstract Molecular self‐assembly strategy for Pt‐O electrocatalysts is presented, achieved by facile solution processing of dopamine monomers. This mussel‐inspired strategy ensures a highly defined PtO 4 atomic structure with uniform monolayer deposition across various 2D nanomaterials. By leveraging the intimate interplay between PtO 4 sites and 2D substrates, while maintaining a consistent coordination environment, underlying mechanism for enhanced kinetics in interfacial synergistic hydrogen evolution reaction is systematically elucidated. Notably, the self‐assembled PtO 4 site exhibits up to a 30‐fold enhancement of mass activity compared to commercial Pt/C catalysts, contingent upon the choice of substrate material. Theoretical investigation illustrates facilitated electron transfer, optimized energy barriers, and additional reaction pathways resulting from the synergistic interplay between PtO 4 and Ti 3 C 2 O 2 MXene. This straightforward, energy‐efficient, and highly reliable scheme for atomic‐level catalysts prospects a valuable platform toward sub‐molecular level engineering of tailored electronic structures and properties.