Cyclohexane oxidation using Au/MgO: an investigation of the reaction mechanism

Conte, Marco, Liu, Xi, Murphy, Damien Martin ORCID: https://orcid.org/0000-0002-5941-4879, Whiston, Keith and Hutchings, Graham John ORCID: https://orcid.org/0000-0001-8885-1560 2012. Cyclohexane oxidation using Au/MgO: an investigation of the reaction mechanism. Physical Chemistry Chemical Physics 14 (47) , pp. 16279-16285. 10.1039/c2cp43363j

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Abstract

The liquid phase oxidation of cyclohexane was undertaken using Au/MgO and the reaction mechanism was investigated by means of continuous wave (CW) EPR spectroscopy employing the spin trapping technique. Activity tests aimed to determine the conversion and selectivity of Au/MgO catalyst showed that Au was capable of selectivity control to cyclohexanol formation up to 70%, but this was accompanied by a limited enhancement in conversion when compared with the reaction in the absence of catalyst. In contrast, when radical initiators were used, in combination with Au/MgO, an activity comparable to that observed in industrial processes at ca. 5% conversion was found, with retained high selectivity. By studying the free radical autoxidation of cyclohexane and the cyclohexyl hydroperoxide decomposition in the presence of spin traps, we show that Au nanoparticles are capable of an enhanced generation of cyclohexyl alkoxy radicals, and the role of Au is identified as a promoter of the catalytic autoxidation processes, therefore demonstrating that the reaction proceeds via a radical chain mechanism.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Cardiff Catalysis Institute (CCI) Chemistry
Subjects:	Q Science > QD Chemistry
Publisher:	Royal Society of Chemistry
ISSN:	1463-9076
Funders:	INVISTA
Date of First Compliant Deposit:	30 March 2016
Last Modified:	02 Jul 2023 18:14
URI:	https://orca.cardiff.ac.uk/id/eprint/52632

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