Abstract

Understanding the effects of catalyst surface structure on a catalytic reaction is of fundamental importance in catalysis chemistry. Herein, a series of Pt-on-Au (Ptm^Au, m refers to the atomic Pt/Au ratio; Au size: 3.2 ± 0.4 nm) nanostructures with Pt dispersion in the range of 38% to 100% are used to study the structure sensitivity of the hydrogenation reactions of 1,3-butadiene and ethylene, respectively. The specific catalytic rates for both reactions are observed to increase with a decrease in the Pt dispersion or increasing m in Ptm^Au, demonstrating the structure-sensitive nature of both reactions over the Ptm^Au nanostructures. These observations strongly contrast with the structure insensitivity of the same reactions over our deliberately prepared counterpart Pt/SiO2 catalysts with Pt dispersion varying in 6%∼100% and also those documented in literature and thus identify a distinct feature of Pt in the Ptm^Au nanostructures. Characterization results from XANES spectroscopy and DRIFTS of adsorbed ...

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