Catalytic oxidation of Carbon Monoxide and Methane with goldbased catalysts

Raphulu, Mpfunzeni Christer
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Gold has been regarded as being inert and catalytically inactive for many years compared with for example the platinum group metals. However, for the past decade gold has attracted a growing attention as both a heterogeneous and homogeneous catalyst and it has been shown that it can catalyze a wide range of reactions such as oxidation, hydrogenation, reduction, etc. This project entails the synthesis, characterization and testing of a suitable gold catalyst for the oxidation of carbon monoxide (CO), and some hydrocarbons (methane). In this project 2 wt% Au/TiO2; Au/TiO2-ZrO2; Au/TiO2-CeO2 catalysts were prepared by both deposition-precipitation and co-precipitation methods. Different synthesis conditions such as pH, catalyst ageing, and catalyst pretreatment were investigated in order to find suitable conditions for the preparation of catalyst that would be more active at lower temperature range (25 oC – 100 oC). The techniques used for catalyst characterization include, TGA, XRD, BET, XPS, TPR, XANES, HRTEM etc. in order to elucidate the catalyst surface structure and its suitability in affecting adsorption and subsequently catalytic activity. Carbon monoxide and methane oxidation reactions were undertaken in a tubular glass flow reactor. It was observed that when gold is well dispersed on a suitable support, it can catalyze total oxidation of CO at room temperature, provided that certain preparation and pretreatment conditions are followed. An uncalcined catalyst was found to be more active than the catalyst calcined at higher temperatures. This is due to the agglomeration of gold particles on the surface of the support according to our High Resolution Transmission Electron Microscopy results. With Mössbauer spectroscopy, it was observed that the addition of the second support metal oxide such as zirconia resulted in the decrease in agglomeration of gold particles. In such iv catalysts, a considerable amount of ionic species were preserved even after calcination at 400 oC resulting in the higher activity. With Au/TiO2, a batch of uncalcined catalyst dried at 120 oC overnight was leached with cyanide to remove the bulk metallic gold particles, supposedly leaving mostly ionic, small, and well dispersed gold particles and the activity of such leached catalyst was higher than that of the unleached sample. Methane oxidation was found to be very difficult compared with carbon monoxide, and only 8% conversion was achieved at 450 oC whereas a total CO oxidation was achieved at lower temperatures with the same catalyst. It is conclusive that small, ionic well dispersed gold species are necessary for CO oxidation and the adsorption and the active sites for this reaction may be different from those involved in methane oxidation.
PhD - Science
gold , methane , monoxide , oxidation , carbon