3. Electronic Theses and Dissertations (ETDs) - All submissions
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Item Reduction of SO2 by CO over gold supported catalysts(2018) Ngwenya, Mphumzile ThelmaSulphur dioxide is a toxic air pollutant that affects the environment and human life. The catalytic reduction of SO2 to produce the less harmful elemental sulphur has been investigated since the 1940s. This offers a single step flue gas desulphurization process compared to using wet or dry flue gas desulphurization methods. In this research, the catalytic reduction of SO2 by CO was investigated over gold nanoparticles supported on an easily reducible amphoteric metal oxide (TiO2), an alkaline metal oxide (ZnO) and an acidic metal oxide (γ-Al2O3). In comparison, Au/TiO2 catalyst had the highest SO2 conversion of 86.4 % at 300 oC and a gas hourly space velocity of 3 600 mL.gcat -1.h-1 and 2 000 ppm of SO2, with Au/ZnO and Au/Al2O3 having very low average SO2 conversions of 1.8 and 1.4 %, respectively. The optimum reaction temperature was found to be 300 oC as irreversible deactivation of the catalyst by sintering of the Au nanoparticles occurs above 300 oC as observed from the high resolution transmission electron microscopy images of catalysts after the reaction. The products of the reaction, CO2 and sulphur, identified as crystalline sulphur in the form of S8, were observed in the reactor product stream, however, the reaction intermediate carbonyl sulphide was not observed. The optimum feed ratio, CO:SO2, for high SO2 conversions was the stoichiometric ratio of 2:1 over Au/TiO2. The flue gas concentrations of SO2 and CO of 420 ppm and 50 ppm Abstract M. T. Ngwenya University of the Witwatersrand Page iii were also used to investigate the activity of the catalysts. Very high SO2 conversions were observed at these low concentrations despite the limiting CO. The surface analysis of Au/TiO2 after the reaction showed that there was 1 % atomic concentration of S species which was later identified as SOx, where x is 2, 3 or 4; however, there was no accumulation on the catalyst observed after 144 hours. This observation confirmed that the redox reaction mechanism was probably followed with SO2 dissociating into S via adsorbed SOx on the catalysts surface and CO oxidation occurring on the Au-support interface with the excess O adatoms on the support surface. Pre-treatment of Au/TiO2 with 0.5 vol% SO2 enhanced the activity of the catalyst at reaction temperatures less than 150 oC, yet the untreated catalyst showed higher activities at 300 oC. The addition of O2, which is present in flue gas, to the reaction feed stream reduced the conversion of SO2 by 51.9 % as this offered a competing reaction, the direct oxidation of CO. When the O2 feed was removed, the conversion of SO2 increased showing that its effect was reversible.Item An assessment of spatial and temporal variations of nitrogen dioxide over Mpumalanga highveld(2017) Malaza, Lucky SamuelHigh concentrations of nitrogen containing compounds are a growing concern in the Mpumalanga Highveld with satellite measurements confirming high NO2 in different hotspots around the globe including Mpumalanga Highveld. Nitrogen oxides are produced from the eight coal fired power stations in Mpumalanga Highveld, a petrochemical industry in Secunda, steel processing plants in Middelburg and Emalahleni and tail emissions from traffic in the Mpumalanga Highveld. Monitoring of these trace gases is important to estimate an impact that they cause to human health and the environment and also to implement air quality emission standards by government Authorities. A 2008 data from Elandsfontein monitoring station and seven other monitoring stations in the Mpumalanga Highveld have been compared with the 2008 satellite data taken from Ozone Monitoring Instrument (OMI) overpass over the Mpumalanga Highveld. Elandsfontein monitoring station is situated on the highly industrialized Mpumalanga Highveld and its purpose is to monitor impacts of stack emissions on air quality. The study focuses on a 2008 nitrogen dioxide dataset which was taken from Elandsfontein monitoring station. An analysis of data from other monitoring stations located in Ermelo, Bulfour, Hendrina, two stations in Middelburg, Emalahleni, Standerton and Secunda have been undertaken to indicate temporal variation and spatial distribution of nitrogen dioxide in the Mpumalanga Highveld. Temporal variability and spatial distribution of nitrogen dioxide in the Mpumalanga Highveld were estimated by analyzing the ground based measurements and satellite data sets. Smoke stacks emit NO into the atmosphere where it reacts with atmospheric oxygen to form NO2. Subsequent reactions of NO2 result in the formation of ozone. The satellite derived data has been modelled and compared with the ground measured data. Meteorological factors including diurnal and temporal variations of the NO2 concentrations have been analyzed to establish differences and similarities between the two data sets. Vertical column densities of nitrogen oxides from satellite measurements with high resolution are presented in mole x (1015)/cm2 and together with ground measured data from other eight air quality monitoring stations have been converted into μg/m3. Analysis of both data sets have been done on the same units, μg/m3 . Seasonal and diurnal variations between the two data sets seem to form the same graphical trends by showing high concentrations during winter than in summer. Ground measured and satellite born datasets do not agree because clouds, air mass factor, aerosols and surface albedo create retrieval errors on the satellite data.