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Aerobic Oxidation of Cyclohexane on Catalysts Based on Twinned and Single-Crystal Au75Pd25 Bimetallic Nanocrystals

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    Aerobic Oxidation of Cyclohexane on Catalysts Based on Twinned and Single-Crystal Au75Pd25 Bimetallic Nanocrystals
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    Hefei National Laboratory for Physical Sciences at the Microscale, Key Laboratory of Strongly-Coupled Quantum Matter Physics of Chinese Academy of Sciences, Center of Advanced Nanocatalysis (CAN-USTC), CAS Centre for Excellence and Synergetic Innovation Centre in Quantum Information and Quantum Physics, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui 230026, P. R. China
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    *E-mail: [email protected]
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    Cite this: Nano Lett. 2015, 15, 5, 2875–2880
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    https://doi.org/10.1021/nl5045132
    Published April 3, 2015
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    Abstract

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    Bimetallic Au75Pd25 nanocrystals with shapes of icosahedron and octahedron were synthesized by adding different amounts of iodide ions, and were employed as catalysts for solvent-free aerobic oxidation of cyclohexane. Although both icosahedrons and octahedrons were bounded by {111} facets, the turnover frequency number of Au75Pd25 icosahedrons reached 15 106 h–1, almost three times as high as that of Au75Pd25 octahedrons. The conversion of cyclohexane reached 28.1% after 48 h using Au75Pd25 icosahedrons, with the selectivity of 84.3% to cyclohexanone. Density functional theory calculations along with X-ray photoelectron spectroscopy examinations reveal that the excellent catalytic performance of AuPd icosahedrons could be ascribed to twin-induced strain and highly negative charge density of Au atoms on the surface.

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    Experimental details, catalytic performance in the aerobic oxidation of cyclohexane that was reported previously, histograms of particle size distribution, percentages of Au and Pd species remaining in the reaction solution, TEM image of the products, the aerobic oxidation of cyclohexane catalyzed by Au75Pd25 icosahedrons and octahedrons, carbon balance and residual metal of AuPd icosahedrons and octahedrons after different rounds of the reaction, TEM images of Au75Pd25 icosahedrons, atomic structures of (a) a Au icosahedron with 309 atoms and (b) a Au octahedron with 146 atoms, atomic structures of (a) a Au75Pd25 icosahedron with 309 atoms and (b) a Au75Pd25 octahedron with 146 atoms, surface strain on (a) a Au icosahedron and (b) a Au octahedron, surface strain fields on Au and Au75Pd25 nanocrystals, projected d-DOS of surface atoms on Au75Pd25 nanocrystals, projected d-DOS of surface atoms on Au nanocrystals, the d-band center of surface atoms on Au and Au75Pd25 nanocrystals, Bader charges on (a) a Au icosahedron and (b) a Au octahedron, Bader charges of surface Au atoms on Au and Au75Pd25 nanocrystals, additional references. This material is available free of charge via the Internet at http://pubs.acs.org.

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    Cite this: Nano Lett. 2015, 15, 5, 2875–2880
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    https://doi.org/10.1021/nl5045132
    Published April 3, 2015
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