Tailoring Metal‐Support Interactions With Single‐Atom Polymer Coatings: A Universal Strategy for High‐Performance Catalysts

ABSTRACT Conventional approaches to tuning metal‐support interactions (MSI) through metal doping often lack the flexibility needed to meet diverse catalytic requirements. Here, we report a versatile atomically dispersed metal‐doped polymer coating (MPC) strategy that enables precise engineering of supported catalysts for enhanced performance. As a representative example, an atomically dispersed Cu‐doped polydopamine (PDA‐Cu) coating induces a lower surface electron density on Pt nanoparticles, yielding a Pt/SiO 2 @PDA‐Cu catalyst that shows exceptional activity and selectivity (≥ 98.0%) toward 4‐aminostyrene in 4‐nitrostyrene hydrogenation. This action mechanism is unequivocally demonstrated through combined density functional theory calculations and experimental characterization. Furthermore, we demonstrate the broad applicability of this MPC strategy by successfully modifying various supported catalysts, including Pd/CeO 2 , Pt/COF‐300 and Pd/SBA‐15. This approach not only preserves the inherent advantages of both the original supports (magnetism, porosity, photoelectric properties) and the MPCs (design flexibility, hydrophilicity), but also creates synergistic effects that significantly enhance catalytic performance. Our work provides a general platform for the rational design of advanced catalytic systems with tailored properties.