biostudies-literatureYoon YHNational Research Foundation of Korea, Ministry of Science and ICTe07807https://www.ebi.ac.uk/biostudies/studies/S-EPMC12499478biostudies-literatureUnknown12(37)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<sub>4</sub> atomic structure with uniform monolayer deposition across various 2D nanomaterials. By leveraging the intimate interplay between PtO<sub>4</sub> 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<sub>4</sub> 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 facilitateAdvanced science (Weinheim, Baden-Wurttemberg, Germany)Mussel-Inspired Self-Assembly of PtO<sub>4</sub> Atomic Catalysts for Interfacial Synergistic Hydrogen Evolution.PMC12499478RS-2025-00521316Jeyakumar KLee CWBalamurugan JCheng CWKim SOYoon YHLee HSasikala SPKim JBLee GSfalseMussel-Inspired Self-Assembly of PtO<sub>4</sub> 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 PtO<sub>4</sub> atomic structure with uniform monolayer deposition across various 2D nanomaterials. By leveraging the intimate interplay between PtO<sub>4</sub> 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<sub>4</sub> 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 facilitate2025-01-01T00:00:00Z2025 Oct2026-06-04T04:49:27.118Z2026-05-05T03:12:38.733ZS-EPMC124994784058327710.1002/advs.202507807