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Heterogeneous gold and palladium based catalysts for solvent-free oxidation of toluene

Saiman, Mohd Izham Bin 2012. Heterogeneous gold and palladium based catalysts for solvent-free oxidation of toluene. PhD Thesis, Cardiff University.
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Catalyzed oxidation of aromatic hydrocarbons with molecular oxygen has been studied for several decades. For example, toluene can be converted into oxidation products such as benzyl alcohol, benzaldehyde, benzoic acid and benzyl benzoate. At present, the principal industrial production of benzoic acid via the oxidation of toluene involves the use of homogeneous cobalt catalysts in an air pressurized aqueous acetic acid mixture in the presence of Mn ions. However, the use of solvent causes difficulties in the separation of catalysts and products, equipment corrosion, and due to the environmental hazards associated with the use of liquid acids as solvent. Developing solvent free toluene oxidation having great activity has attracted special attention as a promising environmentally friendly reaction. Recently, gold based supported catalyst have been found to be highly effective oxidation catalyst where a number of important discoveries have been made such as in hydrogen peroxide synthesis and selective oxidation of alcohols to aldehydes. As a proof of concept for the following studies, oxidation of toluene and other aromatic hydrocarbons were carried out in round bottom flask with TBHP as oxidant. At mild condition (80 ºC), it was evident that Au-Pd supported catalyst is capable of oxidising aromatics C-H bonds on toluene and derivatives and TBHP as oxidant also have been discovered well in this thesis. The catalyst preparation method was shown to be very important in the formation of active site catalysts. The sol-immobilisation catalyst with a narrow distribution of small particles, was more active than Au-Pd alloy having Au-core palladium shell with PdO dominance on the surface via impregnation catalyst. In addition to that, the choice of support is crucial and this study discovered carbon as a preferred support give enhance on performance activity of toluene. At the same time, the distribution of products can be altered with the choice of preparation methods and support. The synergistic effect of Au and Pd was confirmed by superior catalytic activity compared to monometallic catalyst. Investigations of reaction conditions such as reaction time, reusability, pre-treatment conditions, metal ratio, and mass of catalyst were fully investigated. It was found that the activity and selectivity of the catalyst was highly dependent on these variables. Reaction mechanism was proposed and it was based on catalytic evaluation data. Even though, the proposed mechanism was contradicted by the EPR data study, it was believed that the reactive oxygen species (ROS) was involved in the surface of catalyst and give effect of the catalytic activity. Overall, the oxidation of toluene was successfully studied by using Au-Pd supported catalyst and can not be denied that the importance of TBHP as oxidant involve in this process has been proven.

Item Type: Thesis (PhD)
Status: Unpublished
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Date of First Compliant Deposit: 30 March 2016
Last Modified: 19 Mar 2016 23:01

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