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Selective Amplification of C[DOUBLE BOND]O Bond Hydrogenation on Pt/TiO2: Catalytic Reaction and Sum-Frequency Generation Vibrational Spectroscopy Studies of Crotonaldehyde Hydrogenation

Authors

  • Griffin Kennedy,

    1. Department of Chemistry, University of California, Berkeley, CA 94720 (USA)
    2. Materials Sciences and Chemical Sciences Divisions, Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (USA)
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  • Dr. L. Robert Baker,

    1. Department of Chemistry, University of California, Berkeley, CA 94720 (USA)
    2. Materials Sciences and Chemical Sciences Divisions, Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (USA)
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  • Prof. Gabor A. Somorjai

    Corresponding author
    1. Department of Chemistry, University of California, Berkeley, CA 94720 (USA)
    2. Materials Sciences and Chemical Sciences Divisions, Lawrence Berkeley National Laboratory, Berkeley, CA 94720 (USA)
    • Department of Chemistry, University of California, Berkeley, CA 94720 (USA)===

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  • This work was funded by the Director, Office of Science, Office of Basic Energy Sciences, Division of Chemical Sciences, Geological, and Biosciences of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231.

Abstract

The hydrogenation of crotonaldehyde in the presence of supported platinum nanoparticles was used to determine how the interaction between the metal particles and their support can control catalytic performance. Using gas-phase catalytic reaction studies and in situ sum-frequency generation vibrational spectroscopy (SFG) to study Pt/TiO2 and Pt/SiO2 catalysts, a unique reaction pathway was identified for Pt/TiO2, which selectively produces alcohol products. The catalytic and spectroscopic data obtained for the Pt/SiO2 catalyst shows that SiO2 has no active role in this reaction. SFG spectra obtained for the Pt/TiO2 catalyst indicate the presence of a crotyl-oxy surface intermediate. By adsorption through the aldehyde oxygen atom to an O-vacancy site on the TiO2 surface, the C[DOUBLE BOND]O bond of crotonaldehyde is activated, by charge transfer, for hydrogenation. This intermediate reacts with spillover H provided by the Pt to produce crotyl alcohol.

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