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

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 PtO₄ atomic structure with uniform monolayer deposition across various 2D nanomaterials. By leveraging the intimate interplay between PtO₄ 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 PtO₄ 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 PtO₄ and Ti₃C₂O₂ 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.