The preparation of heterogeneous catalysts for the selective transformation of green chemicals and bio-renewables

The work presented in the thesis is comprised of two parts: the first component describes the preparation and optimisation of green catalysts for the oxidation of benzyl alcohol and other select oxidation reactions; the second section is an investigation into the development of catalysts active for...

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Bibliographic Details
Main Author: King, Gavin Morgan
Published: Cardiff University 2016
Subjects:
547
Online Access:http://ethos.bl.uk/OrderDetails.do?uin=uk.bl.ethos.704930
Description
Summary:The work presented in the thesis is comprised of two parts: the first component describes the preparation and optimisation of green catalysts for the oxidation of benzyl alcohol and other select oxidation reactions; the second section is an investigation into the development of catalysts active for the selective hydrogenation of the lignocellulose-derived platform chemicals furfural and furfuryl alcohol to value-added chemicals and biofuel additives. The first research chapter presents an investigation into the optimisation of the catalytic parameters for the preparation of titania-supported gold and palladium monometallic and bimetallic catalysts by the mixing, grinding, and thermal treatment of metal acetate precursors. The effect of metal loading, and metal ratio for the production of a catalyst optimised for the oxidation of various substrates including benzyl alcohol, glycerol, and for the direct synthesis of hydrogen peroxide, is presented. The catalysts have been physically characterised by X-ray photoelectron spectroscopy (XPS), and X-ray diffraction (XRD) with the information derived from which being used to help determine the origin of improved catalytic activity. The second research chapter describes an investigation into the selective hydrogenation of furfuryl alcohol over supported palladium, and modified-palladium catalysts. It has been shown that monometallic titania supported palladium catalysts can be very active for the selective production of 2-methylfuran for reactions performed at room temperature. It has been shown that through addition of a small amount of secondary metal (namely tin, 1 wt%) to the catalyst, the selectivity pattern can be shifted towards the ring-saturated products tetrahydrofurfuryl alcohol, and methyltetrahydrofuran. The final research chapter investigates the hydrogenation of furfural over monometallic palladium catalysts, bimetallic palladium catalysts modified with ruthenium, and a carbon supported monometallic ruthenium catalyst. The metal ratio for the bimetallic catalyst was varied in order to explore its efficacy for the selective production of value-added products. The reaction parameters were increased for the experiments conducted with Ru/C, the results showing that by tuning of temperature and pressure variables, the selectivity to desired products can be altered dramatically.