3. Electronic Theses and Dissertations (ETDs) - All submissions
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Item Characterization, bioavailability and health risk assessment of mercury in dust impacted by gold mining(2015-05-25) Yalala, Bongani NdhlovuGold mining in South Africa has been the backbone of the economy for many years. With it came economic well-being, the growth and development of satellite towns, cities and metropolitan cities, e.g. Johannesburg-a place of gold. Unfortunately, it also came with adverse effects, most of which are now evident, after a century of mining, with little or no regard for pollution prevention or any form of remediation. Of interest, in this study, is the presence of tailings storage facilities (TSFs) found within the residential areas, in close proximity to commercial district and industry, having been built around them. Currently, some 270 TSFs lie dormant, pregnant with vast number of toxic heavy metals from the initially low efficient but selective gold processing techniques. This led to the deposition of the sand dumps, with high sulphur, iron, chromium, cadmium, arsenic, and mercury amongst other toxic metals. Exposure to oxygen, and water, the pyrites were oxidized and formed acid mine drainage (AMD), which resulted in the leaching out all toxic heavy metals into ground water and surface water causing serious water pollution and environmental degradation. Due to the low efficient gold processing technique, some gold amount was discarded together with the tailings materials. The reprocessing of these dumps led to the generation of dust, which is easily distributed over large areas of land. The unrehabilitated, semi-rehabilitated, and the abandoned TSFs contributed to all forms of pollution, majorly, windblown dust from unprotected tops and sides, AMD leaching toxic heavy metals. In this study, mercury, one of the most toxic elements found within the vast TSFs was determined. This was carried out as part of a larger environmental impact assessment on the effects and scale of pollution from the gold mining in the Witwatersrand. The study area consisted of the greater Johannesburg area, covering commercial business district (CBD), the industrial areas (Aeroton, City Deep, Germiston, Selby, Springs), and the residential areas (Alberton, Boksburg, Centurion, Germiston, Greenside, Sandton, Springs). Dust samples were collected from paved surfaces in the streets, and accessible buildings, were sieved into three sieved into three fractions (PM100, PM50, PM25), and most of the work focused on the smallest size fraction (PM25) in order to study impact of inhalable and respirable dust. Three sequential extraction procedures (modified BCR-the European Community Bureau of Reference, selective sequential procedure (SSE), and novel sequential extraction procedure (n-SEP)) were applied for partitioning and evaluating the mobility, availability and persistence of mercury in urban dusts. Bioavailability of mercury was assessed by leaching dust with artificial gastric and lung fluids which mimicked body conditions. Contamination levels were assessed based on the enrichment factor (EF), contamination factor (Cf) and geoaccumulation index (Igeo) were calculated to further assess the environmental risk and provide a preliminary estimate of the main sources of mercury in street dust. Non-carcinogenic effects and carcinogenic effects due to exposure to urban street dusts were assessed for both children and adults. The total mercury (HgTOT) ranged from 269 to 1350 μg kg-1. In the PM25 size fraction, mercury exhibited the following decreasing order of HgTOT: industrial area > CBD > residential area. This order shows that the HgTOT concentration in the street dust decreased with increased distance from the TSFs. The highlight was that the highest HgTOT was reported in industrial areas next to the TSFs, tailings reprocessing areas, and tailings footprints. Furthermore, in residential areas grossly affected by TSFs and tailings reprocessing, reported high HgTOT values similar to those reported for industrial samples. These results indicated that the presence of TSFs were largely responsible for the mercury found in the dust. The results from the characterization of the dust showed a large concentration of fine particulate matter, with the characteristically high quartz (74 – 98 wt. %), and minor minerals phases such as chloritoid, chlorite, K-feldspar, jarosite, mica, muscovite, pyrite, and pyrophyllite, all below 10 wt. %. These have been known to enrich trace metals, hence a high concentration of mercury. The close proximity of the tailings to the communities led to the determination of bioavailability of mercury from dust. The bioaccessible Hg extracted by lung fluid (up to 3% of HgTOT) was higher than that of gastric fluid (up to 1% of HgTOT) and was related to the mobile pool of Hg in dust. This suggests that human exposure to Hg in dust via inhalation is greater than that via the gastric tract. These values were very similar to the values obtained from water soluble phase in the sequential extraction procedure (average 1.4% of HgTOT). This indicated that these fluids were able to extract the most bioavailable fraction of Hg, which is responsible for most of the transformation reactions involving mercury. Contamination assessment factor was carried out to classify the pollution levels and indicate whether they are from natural or anthropogenic sources. Based on the EF, Cf, and Igeo, 70, 82, and 84% of the street dust samples were classified as heavily enriched, very highly contaminated, and strongly polluted by mercury, respectively, indicating that they are of anthropogenic origin. The human health risk model was useful in identifying the areas of health risks from exposure to mercury pollution. It showed that children were more vulnerable than adults when exposed to mercury in dust via ingestion. The cancer risk for exposure to As, Cd, and Cr by both children and adults was significantly high for oral ingestion of dust. Cr (VI) was the highest contributor followed by As and lastly Cd. For inhalation pathway, the possibility of developing cancer after a lifetime exposure was low and below the acceptable limits (10-6).Item Small mammal community dynamics and associated trophic niche widths in a mining-impacted catchment(2014-09-03) Davies, Christopher HughUnable to load abstract.Item Mercury speciation in air from coal fired power stations(2014-07-22) Jongwana, Lulamile TheoMercury 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.Item Assessment of algae as mercury bioindicators in acid mine drainage waters and their potential for phytoremediation(2014-07-22) Tshumah-Mutingwende, Rosamond Rosalie Marigold SetswaThe use of algae as heavy metal bioindicators in aquatic environments has received much attention. In this study, the performance of a common freshwater living green alga, Cladophora sp. as a mercury bioindicator and its potential for phytoremediation applications was assessed by various parameters which included the influence of contact time, pH, initial mercury concentration and the presence of competing metal cations. A rapid uptake of mercury by Cladophora sp. was displayed. More than 99% of mercury in solution was removed within the first 5 min of contact and equilibrium was attained after 10 min. High adsorption capacities of 800 mg kg-1, 530 mg kg-1 and 590 mg kg-1 at pH 3, 6.5 and 8.5 respectively were obtained at the optimum mercury concentration of 1.0 mg l-1. Competitive adsorption studies showed that the selectivity of heavy metal cations by Cladophora sp. was in the following order: Hg2+ ˃Fe2+˃Cu2+˃ Zn2+ ˃ Co2+. These results indicate that living Cladophora sp. algae are suitable for use as mercury bioindicators in AMD waters and are also suitable for the removal of mercury in AMD conditions.Item Characterization and modeling of mercury speciation in industrially polluted areas due to energy production and mineral processing in south africa(2012-08-27) Makiese, Julien Gilles LusilaoCoal combustion is recognized as the primary source of anthropogenic mercury emission in South Africa followed by gold mining. Coal is also known to contain trace concentrations of mercury which is released to the environment during coal mining, beneficiation or combustion. Therefore, determining the mercury speciation in coal is of importance in order to understand its behavior and fate in the environment. Mercury was also used, at a large extent, in the Witwatersrand Basin (South Africa) for gold recoveries until 1915 and is still used in illegal artisanal mining. Consequences of these activities are the release of mercury to the environment. Nowadays, gold (and uranium) is also recovered through the reprocessing of old waste dumps increasing the concern related to mercury pollution. While much effort has been put in the northern hemisphere to understand and control problems related to anthropogenic mercury release and its fate to the ecosystem, risk assessment of mercury pollution in South Africa was based, until very recently, on total element concentrations only or on non systematic fragmental studies. It is necessary to evaluate mercury speciation under the country’s semi arid conditions, which are different to environmental conditions that exist in the northern hemisphere, and characterize potential sources, pathways, receptors and sinks in order to implement mitigation strategies and minimize risk. In this study, analytical methods and procedures have been developed and/or optimized for the determination of total mercury and the speciation of inorganic and organic forms of mercury in different sample matrices such as air, coal, sediment, water and biota. The development of an efficient and cost effective method for total gaseous mercury (TGM) determination was achieved using nano-gold supported metal oxide (1% wt Au) sorbents and cold vapor atomic fluorescence spectrometry (CV-AFS). Analytical figures of merit and TGM concentrations obtained when using Au/TiO2, as a mercury trap, were similar to those obtained with traditional sorbents. The combination of isotope dilution with the hyphenated gas chromatography-inductively coupled plasma mass spectrometry (ID GC-ICP-MS) was also achieved and used successfully for the speciation analysis of mercury in solid, liquid and biological samples. The developed, or optimized, methodologies were used to estimate the average mercury content and characterize the speciation of mercury in South African coals, and also to study the speciation of mercury in selected South African environmental compartments impacted by gold mining activities. The obtained average mercury content in coals collected from the Highveld and Waterberg coalfields (0.20 ± 0.03 mg kg-1) was close to the reported United States Geological Survey (USGS) average for South African coals. Speciated isotope dilution analyses and sequential extraction procedures revealed the occurrence of elemental mercury, inorganic and organo-mercury species, and also the association of mercury mainly to organic compounds and pyrite. The environmental pollution assessment was conducted within the Witwatersrand Basin, at four gold mining sites selected mainly for their mining history and from geophysical information obtained through satellite images. This study showed a relatively important pollution in three of the four sites, namely the Vaal River west site near Klerksdorp, the West Wits site near Carletonville (both in the North-West Province) and the Randfontein site in the West Rand (Gauteng Province). Only one site, the closed Rietfontein landfill site in the East Rand (Gauteng Province) was found to be not impacted by mercury pollution. The methylation of mercury was characterized in all sites and factors governing the mercury methylation process at the different study sites were also investigated. Geochemical models were also used to explain the distribution, transport and fate of mercury in the study systems.