Versatile multi-faceted bimetallic catalysts for Benzylic C-H oxidation.

Abstract

In this thesis, the development of a new methodology for the C–H oxidation of a variety of organic substrates using a bimetallic vanadium-titanium molecular sieve, VTi AlPO-5, is presented. Preliminary studies using model substrate propylbenzene were conducted to elucidate trends in catalytic activity by varying a wide array of reaction and catalyst parameters. Following that is a series of studies documenting the uses of VTi AlPO-5 in the oxidation of other substrates, in which different types of reactivity were probed. The catalyst is highly active and capable of redox- as well as acid catalysis due to the inclusion of its vanadium and titanium centres, the combination of which has been found to be capable of effecting two-step syntheses in the same pot, or enhancing selectivity to very high levels in several reactions. The physicochemical nature of the material as well as spectroscopic investigation of the V and Ti centres in the catalyst has been investigated using a variety of techniques. This data, combined with the catalytic data obtained during reactions, led to the proposal of structures for the metal ions and a preliminary reaction mechanism.

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ORCID for David C. Harrowven: orcid.org/0000-0001-6730-3573

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