Scope, kinetics, and mechanistic aspects of aerobic oxidations catalyzed by ruthenium supported on alumina |
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Authors: | Yamaguchi Kazuya Mizuno Noritaka |
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Institution: | Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan. |
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Abstract: | The Ru/Al(2)O(3) catalyst was prepared by modification of the preparation of Ru(OH)(3).n H(2)O. The present Ru/Al(2)O(3) catalyst has high catalytic activities for the oxidations of activated, nonactivated, and heterocyclic alcohols, diols, and amines at 1 atm of molecular oxygen. Furthermore, the catalyst could be reused seven times without a loss of catalytic activity and selectivity for the oxidation of benzyl alcohol. A catalytic reaction mechanism involving a ruthenium alcoholate species and beta-hydride elimination from the alcoholate has been proposed. The reaction rate has a first-order dependence on the amount of catalyst, a fractional order on the concentration of benzyl alcohol, and a zero order on the pressure of molecular oxygen. These results and kinetic isotope effects indicate that beta-elimination from the ruthenium alcoholate species is a rate-determining step. |
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Keywords: | alcohols amines heterogeneous catalysis molecular oxygen supported catalysts |
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