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Preparation of copper manganese oxide catalysts and their application for oxidation reactions

Clarke, Tomos J. 2015. Preparation of copper manganese oxide catalysts and their application for oxidation reactions. PhD Thesis, Cardiff University.
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Abstract

The total oxidation of naphthalene using copper manganese oxide catalysts was investigated. A study on the effects of calcination temperature on the materials determined that the presence of a disordered CuMn2O4 phase gave superior naphthalene oxidation activity and selectivity towards CO2 than a more crystalline material. The effects of doping catalysts with precious metals was also investigated for this reaction. Catalysts with various gold and silver loadings were prepared and tested. A lowering of the temperature of 50 % naphthalene conversion and CO2 production was observed when doping with silver but no promotion was observed when using gold. The preparation of copper manganese oxide catalysts by a mechanochemical route is reported. Investigation into the CO oxidation activity of samples prepared from oxide, acetate, and carbonate precursors was undertaken alongside investigations into the structure of the materials prepared. It was determined that use of carbonate precursors gave rise to the most active materials. The activity was attributed to migration of Cu2+ ions into the MnCO3 lattice, which allowed facile formation of disordered CuMn2O4 upon calcination. The effects of precipitating copper manganese oxide catalysts from various alcohol solvents was studied. The solvents investigated were linear alcohols with chain lengths from C2 to C5. It was found that the mixing of the aqueous base and alcoholic nitrate solutions had an effect on the oxidation state of both the precursor and calcined catalyst, which in turn affected the catalytic activity. A study on the effects of washing the catalyst precursors with water and chelating agent solutions is also reported. It was found that washing with water was efficient at removing sodium from the material but that after a point, manganese was also removed, with an adverse effect on activity. Washing with chelating agents was able to remove more Na+ than washing with water with positive effects on activity.

Item Type: Thesis (PhD)
Status: Unpublished
Schools: Chemistry
Subjects: Q Science > QD Chemistry
Date of First Compliant Deposit: 30 March 2016
Last Modified: 21 Oct 2016 05:33
URI: http://orca.cardiff.ac.uk/id/eprint/87067

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