Summary: | A thesis submitted in fulfilment of the requirements for
the degree of Master of Science in the Faculty of science, Department of Chemistry
University of the Witwatersrand
Private Bag X03
Wits
2050 === In recent years, studies have shown that supported Au catalysts have high activity for CO
oxidation at low or ambient temperatures. However, the activity of these catalysts is
dependent on a lot of synthesis conditions as reproducibility of small sized gold particles is hard. In this study supported Au catalysts were prepared via deposition precipitation-method (DP). The small sized Au particles were supported on TiO2 (P25). The suitable synthesis conditions such as pH, aging, metal loading and catalyst pre-treatment were investigated in order to obtain optimum synthesis conditions. The catalysts were characterized with TEM, XRD, and HRTEM. It was found that 3.7 nm Au particles were best synthesized when Au metal loading is 3% at pH 8 and aged for 72 h. The suitable calcination temperature was 200 °C. It was found that the Au particle size was 4.5 nm when Au was supported on SiO2 thus making TiO2 a suitable support. Bimetallic catalyst was synthesized via DP where Pd metal was incorporated as the second metal. It was found that the type of bimetallic formed was heterostructed where both metals where separately attached on the support. The interatomic distance measured from HRTEM results confirmed that both metal were individually attached on the support. XRD results showed that there was no Au-Pd alloy phase or PdO confirming that the Pd metal on the support was indeed in metallic form.
Carbon monoxide (CO) oxidation reactions were undertaken in a tubular glass flow reactor. The monometallic Au catalyst showed superior activity at 200 °C with almost 100% CO conversion. It was also observed that the activity of these catalyst decreased as temperature increased. The CO-TPD studies showed that as temperature increased there was a low CO adsorption due to a decrease in adsorption sites. Varying Pd composition in the bimetallic catalyst did not enhance catalytic activity. However, 25Au75Pd catalyst showed a better conversion as compared to other Au-Pd catalysts. Temperatures studies on bimetallic catalysts showed that as temperature increased there was a decrease in activity. The observed decrease could be attributed to catalyst formation of large particle aggregates. It was also assumed that the low activity was due to how these catalysts were prepared as there was no surfactant utilized during preparation.
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