Journal
CHEMISTRY-A EUROPEAN JOURNAL
Volume 9, Issue 18, Pages 4353-4361Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/chem.200304916
Keywords
alcohols; amines; heterogeneous catalysis; molecular; oxygen; supported catalysts
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The Ru/Al2O3 catalyst was prepared by modification of the preparation of Ru(OH)(3).nH(2)O. The present Ru/Al2O3 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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