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Characterization of Polychlorinated Biphenyl Residues in the North End Lake and Port Elizabeth Harbour, South Africa

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Characterization of Polychlorinated Biphenyl Residues in the North End Lake and Port Elizabeth Harbour, South Africa CHARACTERIZATION OF POLYCHLORINATED BIPHENYL RESIDUES IN THE NORTH END LAKE AND PORT ELIZABETH HARBOUR, SOUTH AFRICA By Edwige Kampire Submitted in fulfilment of the requirements for the degree of Philosophiae Doctor in the Faculty of Science at the Nelson Mandela Metropolitan University Promoter: Dr G. Rubidge Co-Promoter: Prof J.B. Adams December 2015 DECLARATION I, Edwige Kampire (212438883), hereby declare that the thesis for Philosophiae Doctor is my own work and that it has not previously been submitted for assessment or completion of any postgraduate qualification to another University or for another qualification. …………………………………………………….. Edwige Kampire Official use: In accordance with Rule G4.6.3, 4.6.3 A treatise/dissertation/thesis must be accompanied by a written declaration on the part of the candidate to the effect that it is his/her own work and that it has not previously been submitted for assessment to another University or for another qualification. However, material from publications by the candidate may be embodied in a treatise/dissertation/thesis. i DEDICATION “To my husband Eugène Nzambitare and our children Nice Ukeye Nzambitare and Nick Nzambitare for their unfailing love, encouragement, advice and sacrifice during the completion of this study” 7 ii ACKNOWLEDGEMENTS I would like to express my sincere gratitude to many people and institutions throughout the course of this study. First and foremost, I would like to express my deepest gratitude to my promoters Dr. Gletwyn Rubidge and Prof. Janine Barbara Adams for giving me the opportunity to conduct my research under their supervision as well as for their advice, valuable scientific contributions, input and constant guidance throughout this research project. Profound appreciation goes to the Government of Rwanda through Rwanda Education Board (REB) for providing the scholarship and support. Thanks to the Nelson Mandela Metropolitan University (NMMU), University of Rwanda- College of Education for financial support and other facilities; . My gratitude goes to the manager of the North End Lake and Port Elizabeth Harbour Authority for their cooperation throughout the sampling activities of this project; . Many thanks to Mr. Anton Cloete for his assistance, guidance and patience during sampling in the harbour; . Thanks to all staff in the Chemistry Department for help with all facilities whenever it has been asked; . My gratitude goes to the technical staff at Nelson Mandela Metropolitan University (NMMU), in particular H. Schalekamp, F. Olivier and H. Marchant for all their help and guidance throughout the laboratory work and GC/MS instrumentation process; . Thanks to Dr. J. Pietersen and Dr. L. Human for statistical analysis of the data; . Thanks to Dr. A. Ogunlaja, P. Lee and D. Kimoro for GC/MS explanations; . I would like to thank all my lab colleagues in the chemistry section for their cooperation; . Thanks to Sithole Vhusomuzi and Adolph Nyamugama for providing maps of the sampling areas; . Thanks to Justine Webber who helped in the determination of sediment grain size and total organic matter; iii . Thanks to my mother, brothers and sisters for their advice, support and encouragement. There are no words to express my deepest thanks to you; . Finally and most importantly, the most enjoyable and heartfelt acknowledgement is for my husband and our children, for their love, patience, support and encouragement, without which I would never have completed this thesis. Above all to the Almighty God for the new revelation of wisdom, the courage, inspiration and divine strength to accomplish this study. Edwige Kampire iv ABSTRACT Persistent organic pollutants (POPs), including polychlorinated biphenyls (PCBs) are widespread in aquatic systems, they can bioaccumulate in the tissues of aquatic organisms, especially fish as they occupy a position near the top of the aquatic food web. PCBs are among the most toxic substances and have been shown to cause many adverse effects to humans and wildlife. High health risks are associated with populations that follow a diet high in fat content such as fish and shellfish in which PCBs bioaccumulate. Given the importance of industries and the potential health concerns of exposure to PCBs, the lack of information on environmental levels of PCBs in South Africa (SA) is significant and concerning. Less attention has been directed to analysis of PCBs in the South African environments due to high cost and lack of appropriate equipment. This study was the first conducted in order to assess the levels of PCBs in the environment of Nelson Mandela Bay Municipality (Port Elizabeth). The research was directed at determining the PCB levels in water, sediments, fish and mussels collected in the Nelson Mandela Bay Municipality. The sampling sites, North End Lake (NEL) and Port Elizabeth Harbour (PEH) were selected based on their location and the importance of activities taking place in these areas. In total 456 samples of water (dissolved and particulate phases), sediments, mussels and tissues of fish were analysed. Suitable analytical methods were based on the equipment and materials available at the Nelson Mandela Metropolitan University. Gas chromatography-mass spectrometry (GC/MS) was used to quantify PCBs in the samples using the internal standard method. Six indicator congeners (PCB nos. 28, 52, 101, 138, 153, 180) were chosen because they are mainly present in most PCB mixtures in environmental samples and they are recommended for regular monitoring. These congeners represent about 50% of the total non-dioxin like (NDL) PCBs in food. All these congeners were detected in the samples analysed. The total PCB concentrations in the sediments from the NEL and PEH ranged from 1.60 to 3.06 and from 0.56 to 2.35 ng g-1 dry weight, respectively. The concentrations of total PCBs in Mytilus galloprovincialis ranged from 14.48 to 21.37 ng g-1 wet weight and from 20.84 to 31.34 ng g-1 wet weight in Perna perna. Total PCBs in water ranged from 0.18 to 0.355 ng L-1. The concentrations of total PCBs in the liver, gonads, gills and muscle were 95.69, 57.49, 44.63, 34.14 ng g-1 lipid weight in Cyprinus carpio and 119.73, 59.21, 49.78, 34.63 ng g-1 in Oreochromis v mossambicus, respectively. Fish liver was the most contaminated organ due to its high lipid content compared to other parts of fish analysed. The NEL was found to be more contaminated than the PEH. The main potential sources of PCB pollutants in both areas of this study are industrial and municipal discharges. The NEL is surrounded by many industries and serves as a potential pollutant sink due to wastewater and inflow entering into this lake. Four 0.227 kg meals of the edible part of fish (muscle) per month were recommended based on the non-cancer health endpoint and one 0.227 kg meal per month was recommended based on the cancer health endpoint. This research contributed to notify the public and relevant governmental departments on the PCB pollution status of sediments, water and aquatic life in the PEH and NEL. Keywords: PCBs, tissues, mussels, sediments, dissolved phase, bioaccumulation, GC/MS, biodegradation, adverse human health effects. vi ACRONYMS AND ABBREVIATIONS AAP : American Academy of Pediatrics ADI : acceptable daily intake Ah : aryl hydrocarbon AhR : aryl hydrocarbon receptor ANOVA : Analysis of variance ASE : Accelerated solvent extraction ATSDR : Agency for Toxic Substances and Disease Registry BW : body weight CAS : Chemical Abstract Service CB : chlorobiphenyl CBA : Chlorobenzoic acid CCREM : Canadian Council of Resource and Environment CEPA : Canadian Environmental Protection Act CF : condition factor CI : chemical ionization CR : consumption rate CSF : cancer slope factor CSIR : Council of Scientific and Industrial Research dc : direct current vii DCM : dichloromethane DDT : dichlorodiphenyltrichloroethane DEAT : Department of Environmental Affairs and Tourism DL-PCBs : dioxin-like PCBs dw : dry weight EC : European Commission ECD : electron capture detector ECNI : electron negative capture ion EFSA : European Food Safety Authority EI : electron ionization EIP : Entrepreneurship and Innovation Programme ELISA : Enzyme-linked immunosorbent assay EPA : Environmental Protection Agency eV : electron volt FDA : Food and Drug Administration FID : flame ionisation detector FIFA : International Federation of Association Football GC : gas chromatography GC/MS : gas chromatography/mass spectrometry GPC : Gel permeation chromatography viii GPS : global positioning system HBCD : hexabromocyclododecane HCB : hexachlorobenzene HPLC : high-performance liquid chromatography HRGC/HRMS: high-resolution gas chromatography/high-resolution mass IUPAC : International Union of Pure and Applied Chemistry KOW : Octanol water partition coefficient LLE : liquid-liquid extraction LOD : Limit of detection LOI : loss on ignition LOQ : Limit of quantification LRMS : low resolution mass spectrometry lw : lipid weight m/z : mass-to-charge ratio MAE : microwave-assisted extraction MDLs : maximum detection limits MeSO2 : methylsulfonyl MS : mass spectrometry MSD : mass spectrometer detector MSPD : matrix solid-phase dispersion ix NCI : negative chemical ionisation NDL-PCBs : non-dioxin-like PCBs NEL : North End Lake NEMA : National Environmental Management Act NIOSH : National Institute of Occupational Safety and Health NIP : National Implementation Plan NMMU : Nelson Mandela Metropolitan University NOAA : National Oceanic and Atmospheric Administration OCPs : organochlorine pesticides OEHHA : Office
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