Mercury occurs naturally and as a result of human activities. One such activity is the combustion of mineral-enriched, sub-bituminous coal to produce electricityan industry that has existed for over 100 years. Although coal is absolutely necessary to supply the power that South Africa and its neighbouring countries requires, the emitted gases, especially mercury, impact the environment and present a complex array of health-related problems. Controlling the impact of mercury present in the environment depends on the efforts of governments, scientists, business and industry, agriculture, environmental organizations and individuals. Mercury is emitted from the point sources in different forms. Accurate determination of the emitted forms or species of mercury has become a global interest. Determination of the various mercury species requires several well-understood analytical techniques for the confident assessment of potentially contaminated samples.
This study focuses on the development, validation and application of analytical methodologies that are capable of differentiating between the different forms of mercury in environmental samples (air, liquids and solids) from coal-fired power plants. Capillary electrophoresis with amperometric detection, high performance liquid chromatography with amperometric detection, and atomic fluorescence spectrometry methods were developed for mercury speciation. Very low detection limits observed using the methods. For capillary electrophoresis with amperometric detection, the detection limits were 0.005±0.002 μg/l for Hg2+ and 0.4±0.05 μg/l for MeHg+. Detection limits of 2±0.04 ppt and 0.01±0.02 μg/l for Hg2+ were observed for high performance liquid chromatography with amperometric detection and atomic fluorescence spectrometry respectively. These detection limits are attractive for the monitoring of mercury in the environment. Total mercury in solids (coal and ash) was measured by direct mercury measurement using a well-established method, involving the use of the mercury analyzer LECO AMA-254. Total gaseous mercury was measured using the Tekran 2537B system.
On application to environmental samples, very good correlations in results were observed between the different methods. Mercury speciation in South African coal after acid extraction showed that only Hg2+ species was detected from the extracts and that 96% of total Hg in acid extracts is in the Hg2+ species form.
Different trends in Hg speciation results at the Elandsfontein Air Quality Monitoring (AQM) station were observed over the sampling period. During winter sampling, Hg2+ was the predominant species, while Hg0 was predominant the species during summer sampling. Mercury speciation carried out at Duvha Power Station (units 1 and 2), equipped with fabric filter devices, revealed that the predominant form of Hg after the fabric filter devices was Hg2+, due to oxidation of Hg0 to Hg2+ as the flue gas temperature decreases. Mercury speciation at the Majuba Underground Coal Gasification flare revealed that although mercury is emitted from power plants in the form of different chemical species, with each species have a different fate in the atmosphere, the climate, wind direction and terrain also play roles in the transport of mercury emissions. Therefore, it is difficult to predict the transport patterns of emissions. Nonetheless, with correct measuring equipment and modelling, the patterns of emissions should be able to be predicted.
The patterns observed and data recorded at the Elandsfontein AQM station and Duvha Power Station, respectively, were however, insufficient to permit accurate modelling. This study raised a number of other questions which are too comprehensive for this study to address. Therefore, more comprehensive atmospheric and combustion studies should be done.
| Identifer | oai:union.ndltd.org:netd.ac.za/oai:union.ndltd.org:wits/oai:wiredspace.wits.ac.za:10539/14968 |
| Date | 22 July 2014 |
| Creators | Jongwana, Lulamile Theo |
| Source Sets | South African National ETD Portal |
| Language | English |
| Detected Language | English |
| Type | Thesis |
| Format | application/pdf |
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