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Selective oxidation of hydrocarbons using supported gold, silver, copper and bimetallic catalysts.

Xu, Yi-Jun. 2006. Selective oxidation of hydrocarbons using supported gold, silver, copper and bimetallic catalysts. PhD Thesis, Cardiff University.

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Abstract

Supported gold catalysts can provide tuneable activity for liquid phase selective oxidation of alkenes, in particular cyclohexene and cis-cyclooctene, using molecular oxygen from air under mild conditions. Selective oxidation can be readily kick-started using a nano-crystalline gold catalyst supported on carbon along with a small amount of TBHP as initiator. Extremely high selectivity, ca. 98%, for partial oxidation products with significant conversion has been obtained using a bismuth-modified gold catalyst for selective oxidation of cyclohexene. In the case of cis-cyclooctene oxidation, high selectivity to partial oxidation products has also been achieved at a high rate of reaction, without the use of solvent, which is a major tenet of green chemistry. Gold catalysts are also active for the selective oxidation of cyclohexane to cyclohexanol and cyclohexanone. The gas-phase epoxidation of propene to propene epoxide (PO) has been studied using only molecular oxygen as oxidant over a series of supported Ag, Cu, Au and bimetallic (Au-Cu, Cu-Ag and Au-Ag) catalysts. It has been found that the support has an important effect on the catalyst performance. A Au-Cu catalyst exhibited very high selectivity to PO, ca. 96%, at a propene conversion, ca. 0.14%, at relatively low temperature, 200 C. The intrinsic instability of PO leads to the observation of high selectivity to PO only at low temperature.

Item Type: Thesis (PhD)
Status: Unpublished
Schools: Chemistry
Subjects: Q Science > QD Chemistry
ISBN: 9781303175121
Funders: EPSRC
Date of First Compliant Deposit: 30 March 2016
Last Modified: 12 Feb 2016 23:12
URI: http://orca.cardiff.ac.uk/id/eprint/54322

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