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Thesis (Ph.D.) - University of Glasgow, 2008. / Ph.D. thesis submitted to the Department of Geographical and Earth Sciences, Faculty of Physical Sciences, University of Glasgow, 2008. Includes bibliographical references. Print version also available.

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Orientador: Wanilson Luiz Silva / Tese (doutorado) - Universidade Estadual de Campinas, Instituto de Geociências / Made available in DSpace on 2018-08-22T21:27:48Z (GMT). No. of bitstreams: 1 Campaner_VeridianaPolvani1981-_D.pdf: 3461719 bytes, checksum: 9a5bc42ac7776e7105fbf8108a902f11 (MD5) Previous issue date: 2013 / Resumo: A identificação de anomalias antrópicas de elementos no solo e na atmosfera necessita do discernimento de possíveis mistura e dispersão de fontes antrópica e natural. Em área com atividade minerária e termoelétrica a carvão, no município de Figueira (PR), foram investigadas a distribuição multielementar (e.g. As, Cd, Co, Cr, Cu, Hg, Mo, Ni, Pb, Sb, U, Zn e radionuclídeos) em carvão, cinzas, rochas, solo e no material particulado atmosférico (partículas fina e grossa). Nos perfis de solo e no solo de superfície, a influência do carvão e cinzas resultou em assinaturas geoquímicas As/Zr, Cd/Zr, Hg/Zr, Mo/Zr, Pb/Zr, Sb/Zr, U/Zr e Zn/Zr elevadas, devido à mistura destas razões de origem natural no solo com àquelas do carvão e das cinzas. Os diques de diabásio regionais apresentaram assinaturas geoquímicas Co/Zr, Cr/Zr, Cu/Zr, Ni/Zr e Sc/Zr na configuração da paisagem pedológica da área de estudo, onde a maior influência foi de rochas sedimentares. A intensidade das anomalias antrópicas no solo de superfície foi maior para As, Cd e Mo, seguidos por Hg, Zn, Pb, Sb e U (ordem decrescente de intensidade). Estas anomalias mostraram uma distribuição espacial no solo de superfície condizente com a direção predominante dos ventos na área, e sugerem que eventos de deposição atmosférica por longo período devem ter sido a principal fonte destes elementos no solo. No material particulado atmosférico, observou-se o enriquecimento dos mesmos elementos associados ao carvão e às cinzas. Entretanto, uma mistura de fontes natural (considerada por meio da avaliação das amostras de solo da base dos perfis) e antrópica (carvão e cinzas) foram reveladas por assinaturas geoquímicas As/Mo. O carvão e as cinzas de Figueira (PR) apresentaram assinaturas As/Mo iguais a 15,2 ± 4,25 e 15,9 ± 2,42, respectivamente. Estas assinaturas foram diferentes daquela encontrada no solo (As/Mo = 8,49 ± 3,13) e levemente contrastantes com a razão As/Mo dos materiais particulados atmosféricos finos e grossos (média igual a 11,4). Como resultado, o modelo As/Mo da área de estudo quantificou a contribuição do carvão e das cinzas em 41% e do solo em 59% na atmosfera. O carvão e as cinzas de Figueira (PR) apresentaram elevadas concentrações de 238U, 226Ra e 210Pb, especialmente. Dentre estes radionuclídeos, o 210Pb destacou-se por apresentar maior distribuição espacial no solo em função de suas atividades e condições de desequilíbrio com o 226Ra (210Pb/226Ra), avaliadas tanto nos perfis de solo quanto no solo de superfície. No material particulado atmosférico, as condições de desequilíbrio 210Pb/226Ra foram mais intensas nas proximidades da usina termoelétrica. Isso indica que o 210Pb deve ter tido uma fonte adicional na atmosfera por meio da emanação do gás 222Rn proveniente, particularmente, da queima do carvão na termoelétrica. Neste estudo a investigação holística de elementos químicos e radionuclídeos em área com atividade minerária contribuiu para uma avaliação mais consistente da influência antrópica no solo e na atmosfera / Abstract: The identification of elemental anomalies in soil and atmosphere caused by human activities is necessarily preceded by the identification of possible mixtures and dispersion of anthropic and natural sources. An area affected by mining and coal-fired thermoelectric power plant activities in the Figueira municipality (Paraná, Brazil) was investigated for multi-elemental distribution (e.g. As, Cd, Co, Cr, Cu, Hg, Mo, Ni, Pb, Sb, U, Zn, and radionuclides) in coal, ashes, rocks, soil, and in the atmospheric (fine- and coarse-grained) particulate material. In soil profiles and in the superficial soil, the influence of coal and ashes resulted in high As/Zr, Cd/Zr, Hg/Zr, Mo/Zr, Pb/Zr, Sb/Zr, U/Zr, and Zn/Zr geochemical signatures, due to the mixture of natural ratios of such elements found in soil with the ratios found in coal and ashes. As for natural ratios, the diabase dikes contributed with Co/Zr, Cr/Zr, Cu/Zr, Ni/Zr, and Sc/Zr geochemical signatures to the configuration of the pedological landscape of the study area, where the major influence comes from sedimentary rocks. The anthropic anomalies in superficial soil were, in descending order, higher for As, Cd, and Mo, followed by Hg, Zn, Pb, Sb, and U. The spatial distribution of these anomalies in the superficial soil were consistent with the predominant wind directions and suggests that long-term atmospheric deposition must have been the main source for these elements in the soil. The atmospheric particulate material is enriched in the elements associated with coal and ashes in soil. However, a mixture of natural sources (assessed by means of soil samples from the base of the soil sections) and anthropic sources (coal and ashes) was revealed by As/Mo ratios. The coal and ashes from Figueira yielded, respectively, As/Mo signatures of 15.2 ± 4.25 and 15.9 ± 2.42. These signatures differ from that obtained for soil (As/Mo = 8.49 ± 3.13), and slightly differ from the As/Mo value obtained for atmospheric particulate material (average As/Mo = 11.4). As a result, the As/Mo model for the study area helped quantify the contributions from coal and ashes (41%) and soil (59%) to the atmosphere. Coal and ashes from Figueira have high 238U, 226Ra, and 210Pb activities. The largest spatial distribution in soil corresponds to 210Pb, because of its chemical activities and disequilibrium with 226Ra (210Pb/226Ra), observed both in the soil profiles and in the superficial soil. In the atmospheric particulate material, the 210Pb/226Ra disequilibrium is more intense close to the coal-fired thermoelectric power plant. This indicates that an additional source for 210Pb in the atmosphere was the emanation of gas 222Rn resulting from the burning of coal in the plant. The holistic investigation carried out in this study involving chemical elements and radionuclides in an area affected by mining activities contributed for a more consistent evaluation of the anthropic influence in soil and atmosphere / Doutorado / Geologia e Recursos Naturais / Doutora em Ciências

This study describes the technique and procedures used for the simultaneous determination of elements involved in Instrumental Neutron Activation Analysis, applied to some geological samples as a sensitive and non-destructive tool. Using Isotopic Neutron Source, the delayed gamma-rays emitted due to neutron capture have been applied for the investigation of the elemental constituents and concentrations of major, minor and trace elements in such samples. The experimental investigations were carried out at the scale of researcher's practices at the chosen site by measuring soil/rock nutrient contents from hydrologically isolated farmland/site plots. Using detailed sampling procedures with special precautions, against contaminations, to yield meaningful results, soil/rock samples have been collected from selected areas of East Gojjam, pulverized, homogenized and prepared for irradiation. The samples were properly prepared together with known standards of potassium iodide or cupric sulphate or arsenic trioxide (one /or both at a time), and simultaneously irradiated in to isotopic neutron ux in the same irradiation position. After activation, the samples were subjected to gamma-ray spectrometry, using a high-purity germanium detection system and computerized multichannel analyzer. The gamma-ray spectra from the irradiated samples were measured by high resolution gamma-ray spectrometry with a calibrated germanium detector. Both qualitative and quantitative approach to data collection and analysis were used in order to gain insight into what should be acceptable to the community. The results obtained have a practical interest in view of possible applications to the technology of extraction and exploration of a variety of industrial, metallic, cement minerals, and geothermal energy and coal deposits. These results tend to agree with the lowest values reported in the literature, and the analytical precision is su cient for the determination of the standard deviation of the distribution of all elements in East Gojjam and these results were brie y discussed within the text of this research work. In carrying out the analysis, the best and most convenient method being the Instrumental and /non-destructive Neutron Activation Analysis was adopted, and NAA has matured and attained analytical competence providing not only rapid, quantitative, qualitative, simultaneous, multi􀀀element analysis but also crucial validation support to programmes using di erent analytical techniques. This method of analysis is generally multi-element and experimental conditions can be designed to be non􀀀destructive to the sample, and it plays a leading role among analytical techniques in the eld of environmental research related to human, animal and plant health. Studies of di erent radionuclide and trace elements in the environmental samples are very important for health physics, research and education. Many forms of elements are possible in environmental samples which may be hazardous for human being, animals and also plants. Most of them have the potential for both benefcial and harmful effects / Environmental Sciences / D. Phil. (Environmental Science)

This study describes the technique and procedures used for the simultaneous determination of elements involved in Instrumental Neutron Activation Analysis, applied to some geological samples as a sensitive and non-destructive tool. Using Isotopic Neutron Source, the delayed gamma-rays emitted due to neutron capture have been applied for the investigation of the elemental constituents and concentrations of major, minor and trace elements in such samples. The experimental investigations were carried out at the scale of researcher's practices at the chosen site by measuring soil/rock nutrient contents from hydrologically isolated farmland/site plots. Using detailed sampling procedures with special precautions, against contaminations, to yield meaningful results, soil/rock samples have been collected from selected areas of East Gojjam, pulverized, homogenized and prepared for irradiation. The samples were properly prepared together with known standards of potassium iodide or cupric sulphate or arsenic trioxide (one /or both at a time), and simultaneously irradiated in to isotopic neutron ux in the same irradiation position. After activation, the samples were subjected to gamma-ray spectrometry, using a high-purity germanium detection system and computerized multichannel analyzer. The gamma-ray spectra from the irradiated samples were measured by high resolution gamma-ray spectrometry with a calibrated germanium detector. Both qualitative and quantitative approach to data collection and analysis were used in order to gain insight into what should be acceptable to the community. The results obtained have a practical interest in view of possible applications to the technology of extraction and exploration of a variety of industrial, metallic, cement minerals, and geothermal energy and coal deposits. These results tend to agree with the lowest values reported in the literature, and the analytical precision is su cient for the determination of the standard deviation of the distribution of all elements in East Gojjam and these results were brie y discussed within the text of this research work. In carrying out the analysis, the best and most convenient method being the Instrumental and /non-destructive Neutron Activation Analysis was adopted, and NAA has matured and attained analytical competence providing not only rapid, quantitative, qualitative, simultaneous, multi􀀀element analysis but also crucial validation support to programmes using di erent analytical techniques. This method of analysis is generally multi-element and experimental conditions can be designed to be non􀀀destructive to the sample, and it plays a leading role among analytical techniques in the eld of environmental research related to human, animal and plant health. Studies of di erent radionuclide and trace elements in the environmental samples are very important for health physics, research and education. Many forms of elements are possible in environmental samples which may be hazardous for human being, animals and also plants. Most of them have the potential for both benefcial and harmful effects / Environmental Sciences / D. Phil. (Environmental Science)