Abstract
SummaryStrong 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 Pt1/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.
Highlights
Supported metal catalysts with metal particles finely dispersed on high-surface-area support materials are vital for many industrially important catalytic reactions
The 1.0 wt.% Pt1/hollow nanocarbon (h-NC) demonstrates excellent activity for hydrogenation of 3-nitrostyrene to 3-vinylaniline with a turnover number (TON) > 31,000/h, more than 20 times higher than that of the best catalyst for such selective hydrogenation reactions reported in the literature (Wei et al, 2014)
Synthesis of h-NCs, Pt1/h-NC single-atom catalysts (SACs), and Control Catalysts The h-NCs were synthesized via a catalytic decomposition and reductive evaporation process by using ZnO nanowires as catalyst/template and ethanol as feedstock
Summary
Supported metal catalysts with metal particles finely dispersed on high-surface-area support materials are vital for many industrially important catalytic reactions. The surface physicochemical properties of the supports play a crucial role in modifying the catalytic behaviors of supported metal species via the strong metal-support interaction (SMSI) (Lee et al, 2015; Tang et al, 2016a, 2016b; Vannice, 1979; Matsubu et al, 2017). The SMSI has been widely exploited to improve catalyst stability (Lee et al, 2015; Tang et al, 2016a, 2016b), identify reaction mechanisms (Matsubu et al, 2017; Bonanni et al, 2012), and enhance activity (Vannice, 1979; Sonstrom et al, 2011). It is highly desired to extend the applications of SMSI concept to broader catalyst systems, beyond metal particles, to tune catalytic properties for desirable performance
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