3. Electronic Theses and Dissertations (ETDs) - All submissions
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Item Extending the understanding of metal loading sites on a novel titania nanocatalyst(2016) Malibo, Petrus MolaoaThe hydrothermal method of synthesis was successfully utilized to produce the rutile dandelion support onto which different noble metals were deposited using the deposition precipitation method to prepare the Au-TiO2, Pt-TiO2, Pd-TiO2 and Rh-TiO2 catalysts. The catalysts were prepared at different metals loadings. The deposition precipitation method was also employed to deposit the same metals (Au, Pt, Pd and Rh) onto the rutile (110) and (111) crystal surfaces to model the catalysts. Transmission electron microscopy, scanning electron microscopy and powder X-ray diffraction were used as the main characterization techniques to study the preferred deposition sites of the metals as well as the composition of the catalysts. TEM analysis showed the metals to deposit onto the sides and tips of the rutile nanorods making up the dandelion support structure. SEM analysis showed the metals to deposit onto the (110) and (111) crystal surfaces with the exception of Pd which deposited onto the (111) and (001) surfaces only. TEM analysis showed that the metals agglomerated following Temperature-Programmed Reduction (TPR) under H2 gas. TPR analysis showed strong-metal-support interaction for the Pt, Pd and Rh catalysts.Item Investigating the effect of gold-palladium bimetallic nanoparticles on TiO2 and the catalytic activity in CO oxidation(2013-04-29) Ntholeng, NthabisengIn 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.