Nanocarbon-Edge-Anchored High-Density Pt Atoms for 3-nitrostyrene Hydrogenation: Strong Metal-Carbon Interaction.

Strong metal-support interaction (SMSI) has been widely used to improve catalytic performance and to identify reaction mechanisms. We report that single Pt atoms anchored onto hollow nanocarbon (h-NC) edges possess strong metal-carbon interaction, which significantly modifies the catalytic behavior of the anchored Pt atoms for selective hydrogenation reactions. The strong Pt-C bonding not only stabilizes single Pt atoms but also modifies their electronic structure, tunes their adsorption properties, and enhances activation of reactants. The fabricated Pt/h-NC single-atom catalysts (SACs) demonstrated excellent activity for hydrogenation of 3-nitrostyrene to 3-vinylaniline with a turnover number >31,000/h, 20 times higher than that of the best catalyst for such selective hydrogenation reactions reported in the literature. The strategy to strongly anchor Pt atoms by edge carbon atoms of h-NCs is general and can be extended to construct strongly anchored metal atoms, via SMSI, onto surfaces of various types of support materials to develop robust SACs.