Mussel-Inspired Self-Assembly of PtO4 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 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.