Submitted by Fabio Sobreira Campos da Costa (fabio.sobreira@ufpe.br) on 2017-02-06T15:57:59Z No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) dissertação_Emerson_Farias_corrigida_sem_assinatura.pdf: 1653100 bytes, checksum: f58076ed14de44a96ed097b6dd697195 (MD5) / Made available in DSpace on 2017-02-06T15:57:59Z (GMT). No. of bitstreams: 2 license_rdf: 1232 bytes, checksum: 66e71c371cc565284e70f40736c94386 (MD5) dissertação_Emerson_Farias_corrigida_sem_assinatura.pdf: 1653100 bytes, checksum: f58076ed14de44a96ed097b6dd697195 (MD5) Previous issue date: 2011-05-10 / Nos últimos anos tem-se observado uma preocupação crescente da população em relação à presença de radionuclídeos no meio ambiente. As principais atividades que podem contribuir para o incremento da concentração desses contaminantes envolvem tanto processos industriais como aplicações médicas. Não menos importantes, no entanto, são os radionuclídeos naturais encontrados no ambiente, os quais podem ter suas concentrações aumentadas como resultado de beneficiamento de matéria prima para a extração de metais, como é o caso das areias minerais, ricas em cianita, ilmenita rutilo e zirconita, as quais podem apresentar elevadas concentrações de urânio e tório. A quantificação de radionuclídeos envolve, de maneira geral, técnicas de Instrumentação Nuclear. Dentre essas, as espectrometrias alfa e gama estão entre as mais utilizadas nas medições de radionuclídeos naturais em matrizes ambientais. Portanto, tornam-se cada vez mais importantes o estudo e o aperfeiçoamento das metodologias utilizadas em cada uma dessas técnicas, proporcionando maior precisão e exatidão nas determinações. Nesse contexto, o presente trabalho visou a comparação entre as diversas metodologias utilizadas nas técnicas de espectrometria alfa e espectrometria gama para a determinação de 238U e 232Th em amostras ambientais, especificamente em areias minerais. A validação das metodologias utilizadas foi feita utilizando-se materiais de referência fornecidos pela Agência Internacional de Energia Atômica. Para a técnica de Espectrometria Alfa as amostras foram previamente digeridas por fusão alcalina e receberam traçadores de 232U e 229Th. Após a purificação em resina de troca iônica e eletrodeposição em disco de aço inoxidável, as amostras foram contadas por um período de 80.000 segundos em um espectrômetro alfa.Para a espectrometria gama, alíquotas de 50 g de cada amostra foram acondicionadas em potes cilíndricos de plástico e contadas. As aquisições de dados foram feitas por um período de 80.000 segundos e as linhas gama utilizadas para a determinação do 238U foram as de 63 keV, 93 keV e 1001 keV. Para o 232Th, por outro lado, foram utilizadas as linhas de 338 keV, 911 keV e 969 keV. As quatro metodologias de determinação de 232Th (338 keV, 911 keV, 969 keV e espectrometria alfa) geraram valores de concentrações próximos daqueles constantes dos certificados em materiais de referência, indicando a viabilidade da utilização de qualquer das metodologias. Dentre as metodologias estudadas para a determinação de 238U, a espectrometria alfa e a espectrometria gama, pela linha de 1001 keV, foram as mais indicadas para amostras do tipo das analisadas no presente trabalho, pois apresentaram valores em concordância com os constantes dos certificados dos materiais de referência. Os resultados das análises das areias minerais mostraram concentrações de urânio-238 variando de 60 a 12.256 Bq.kg-1, com um valor médio de 3.634 Bq.kg-1. A concentração de atividade média observada nas amostras de zirconita foi de 6.723 Bq.kg-1, enquanto que a atividade média encontrada para as outras areias minerais associadas foi de 545 Bq.kg-1, ou seja, dentre as areias minerais presentes no depósito analisadas, as que merecem maior atenção, do ponto de vista da proteção radiológica, são as de zirconita. Por outro lado, as determinações de tório-232 mostraram concentrações de atividade variando de 40 a 7.205 Bq.kg-1 e um valor médio de 1.465 Bq.kg-1. Apenas duas amostras tiveram concentrações acima desse valor (ambas eram de areias minerais de zircão), o que reforça a necessidade de maior atenção, do ponto de vista da proteção radiológica, para as amostras de zirconita. / There has been a great concern in recent years related to the presence of radionuclides in the environment. The main activities which may contribute for the increase in the concentration of those contaminants in the environment involve industrial processes, as well as, medical applications. Not less important, however, are the natural radionuclides found in the environment, which can be concentrated as a result of raw material transformation. This is the case of mineral sands processing for the extraction of kyanite, ilmenite, rutile and zircon, which can have higher than normal concentrations of uranium and thorium. For the measurement of radionuclides as contaminants, the main forms of determination involve techniques of Nuclear Instrumentation. For this reason, it is very important to study and improve these techniques in order to obtain reliable results, as far as precision and accuracy are concerned. Thus, the present study aimed to compare the techniques of alpha spectrometry and gamma spectrometry for the determination of 238U and 232Th in environmental samples, specifically in mineral sands. The validation of the methodologies was carried out by using reference materials provided by the International Atomic Energy Agency. For the determination of 238U and 232Th by alpha spectrometry, samples were digested by alkaline fusion, spiked with 229Th and 232U tracers, purified by passing through an ion exchange resin, electrodeposited on stainless steel disks and counted for 80,000s. For the determination by gamma spectrometry, 50 g of each of the samples were placed in plastic cylindrical containers and counted for 80,000s. The main gamma lines used for determining 238U were 63 keV, 93 keV and 1001 keV. For 232Th, on the other hand, the 338 keV, 911 keV and 969 keV gamma lines were used. The four methodologies for the determination of 232Th, namely 338 keV, 911 keV, 969 keV and alpha spectrometry, led to concentration values in agreement with the certified values for the reference materials. Among the methods studied for the determination of 238U, alpha spectrometry and gamma spectrometry using the 1001 keV line, were the most suitable for the type of samples analyzed in this study. The results of the analyses performed for mineral sands showed concentrations of uranium-238 ranging from 60 to 12,256 Bq.kg-1, with an average of 3,634 Bq.kg-1. The average activity concentration observed in samples of zircon was 6, 723 Bq.kg-1, while the average activity found for other mineral sands was of 545 Bq.kg-1, showing that zircon sands deserve greater attention, from the standpoint of radiological protection, among the mineral sands analyzed. Moreover, the determinations of thorium-232 showed activity concentrations ranging from 40 to 7,205 Bq.kg-1 with an average of 1,465 Bq.kg-1. Only two samples showed 232Th concentrations above this value (both were of zircon sands), which reinforces the need for greater attention, from the point of view of radiological protection, for samples of zircon.

The predominant nuclear fuel used globally at present is uranium which is a finite resource. Thorium has been identified as an alternative nuclear fuel source that can be utilized in almost all existing uranium–based reactors and can significantly help in conserving limited uranium reserves. Furthermore, the elimination of proliferation risks associated with thorium–based fuel cycles is a key reason for re–evaluating the possible utilization of thorium in high temperature reactors. In addition to the many advantages that thorium–based fuel has over uranium–based fuel, there are vast thorium resources in the earth's crust that up until the present have not been exploited optimally. This study focuses on determining the amount of uranium ore that can be saved using thorium as a nuclear fuel in HTR's. Four identical 200 MWth high temperature reactors are considered which make use of different fuel cycles. These fuel cycles range from the conventional uranium fuel cycle to a thorium–based fuel cycle in which no U–238 is present and have been simulated using the VSOP–A system of computer codes. This study also considers the effect that protactinium, an isotope that occurs in thorium–based fuel cycles, will have on the decay heat production in the case of a depressurized loss of coolant (DLOFC) accident. / Thesis (M.Ing. (Nuclear Engineering))--North-West University, Potchefstroom Campus, 2011.

The predominant nuclear fuel used globally at present is uranium which is a finite resource. Thorium has been identified as an alternative nuclear fuel source that can be utilized in almost all existing uranium–based reactors and can significantly help in conserving limited uranium reserves. Furthermore, the elimination of proliferation risks associated with thorium–based fuel cycles is a key reason for re–evaluating the possible utilization of thorium in high temperature reactors. In addition to the many advantages that thorium–based fuel has over uranium–based fuel, there are vast thorium resources in the earth's crust that up until the present have not been exploited optimally. This study focuses on determining the amount of uranium ore that can be saved using thorium as a nuclear fuel in HTR's. Four identical 200 MWth high temperature reactors are considered which make use of different fuel cycles. These fuel cycles range from the conventional uranium fuel cycle to a thorium–based fuel cycle in which no U–238 is present and have been simulated using the VSOP–A system of computer codes. This study also considers the effect that protactinium, an isotope that occurs in thorium–based fuel cycles, will have on the decay heat production in the case of a depressurized loss of coolant (DLOFC) accident. / Thesis (M.Ing. (Nuclear Engineering))--North-West University, Potchefstroom Campus, 2011.

Denna studie behandlar upptaget av de hälsovådliga metallerna bly, kadmium, tallium, torium och uran i några viktiga grödor som vete, råg, potatis och sallat som används för humankonsumtion. Syftet var att studera faktorer och mekanismer som kan påverka grödornas upptag av dessa metaller. Målsättningen var även att utröna hur stor påverkan dessa faktorer har på grödornas upptag av Pb, Cd, Tl, Th och U. En litteraturstudie visade att de domesticerade grödorna vete, potatis, råg och sallat tar upp Pb, Cd, Tl, Th och U. Upptaget är störst hos sallat och potatis, förhöjda koncentrationer i åkermarken medför därför en ökad risk för att hälsovådliga koncentrationer återfinns i grödan. En ökad metallkoncentration av dessa grundämnen i marklösning och odlingssubstrat ger oftast högre metallkoncentrationer i aktuell gröda. De högsta koncentrationerna återfinns oftast i rötterna. Oorganiskt fosfatgödsel kan innehålla Pb, Cd, Tl, Th och U beroende på typ av råvara. Studier visar att fosfatgödsels kadmiuminnehåll åtminstone ger en ökad kadmiumhalt i grödor som råg, vete, potatis och sallat. En ökad användning av fosfatgödsel tycks även ge högre halter av torium och uran i vete. Stallgödsel från nötkreatur kan minska upptaget av bly och kadmium och arbuskulär mykorrhizasvamp kan binda metaller som bly och kadmium till rotvävnader och på så vis minska upptaget i växtdelar som används för humankonsumtion. Vetes upptag av kadmium och uran studerades i en experimentell hydroponisk dosstudie. Resultaten från den experimentella studien indikerade att förhöjd kadmiumhalt och urankoncentration i näringslösning kan ha gett upphov till förhöjda halter i vete, vilket i sin tur kan ha påverkat plantans tillväxt. I uranprovserien fastställdes att perlit tog upp uran. Utifrån data från försöken beräknades fördelningskonstanten Kd för löst uran/uranhalt i perlit. I denna provserie visade beräkningar att roten genom en aktiv process tog upp uran från näringslösningen. Resultaten indikerar att det finns risker med att äta grödor som odlats i jordar med höga halter av Pb, Cd, Tl, Th eller U. Hälsovådliga koncentrationer kan nås utan att något synligt symtom på kontaminering eller förgiftning hos grödan. / This study deals with the uptake of noxious metals lead, cadmium, thallium, thorium and uranium in some important crops such as wheat, rye, potatoes, and lettuce that are used for human consumption. The aim was to study factors and mechanisms that influence crop uptake of these metals. Another objective was also to define the impact of these factors on crop uptake of Pb, Cd, Tl, Th and U.  According to a literature review domesticated crops such as wheat, potatoes, rye, and lettuce take up Pb, Cd, Tl, Th and U. Lettuce and potatoes are the crop with the highest uptake. Elevated metal concentrations in arable land therefore entails a greater risk for harmful concentrations found in potato and lettuce. Increased concentrations of these elements in soil solution and growing medium usually give higher metal concentrations in the current crop. The highest concentrations are found mostly in the roots. Phosphate fertilizers may contain Pb, Cd, Tl, Th and U depending on the type of raw material used for manufacturing. Studies show that the cadmium content in phosphate fertilizer can give an increased cadmium content in crops such as rye, wheat, potatoes and lettuce. An increased use of phosphate fertilizers also appears to give higher levels of thorium and uranium in wheat. Animal manure from cattle may reduce the uptake of lead and cadmium and arbuscular mycorrhizal fungi can bind metals such as lead and cadmium to rot tissues and thus reduce the accumulation in plant parts used for human consumption. Wheat uptake of cadmium and uranium was studied in an experimental hydroponic dose study. The results of the experimental study indicated that elevated cadmium and uranium content in the nutrient solution increased the content of the element in the plant, which in turn may have affected the growth of the plant. The uranium sample series showed that perlite adsorbed uranium. Based on data from the trials the distribution constant Kd for dissolved uranium / uranium content in perlite was calculated. The results from the uranium sample series showed that the root through an active process took up uranium from the nutrient solution. The results indicate that there are risks associated with eating crops grown in soils with high levels of Pb, Cd, Tl, Th and U. Hazardous concentrations may be reached in the crops with no visible signs of contamination or poisoning.

Tenint en compte, les característiques i la presència d’urani i tori al medi ambient, així com la evolució de les directives que estipulen els nivells màxims de materials radioactius al medi ambient, en aquesta tesis es presenten dues revisions exhaustives i quatre mètodes analítics per a la determinació total e isotòpica de tori i urani, com alternatives a les separacions radioquímiques clàssiques, que es caracteritzen per ser laborioses i de llarga duració. Aquestes metodologies varen ser automatitzades mitjançant l’ús de tècniques d’anàlisis en flux multiconmutades, les quals proporcionen un important estalvi de reactius, amb la conseqüent reducció de cost per anàlisis i de generació de residus permetent una major freqüència d’anàlisis, i una mínima manipulació de les mostres. La espectrofotometria de llarg pas òptic i la espectrometria de masses de plasma acoblat inductivament (ICP-MS) varen ser les tècniques de detecció emprades en els mètodes desenvolupats com alternatives a detectors radiomètrics. / Taking into account the occurrence, the characteristics of uranium and thorium in the environment as well as the evolution of the directives which stipulate the limit values of radioactive materials in water samples, in this thesis two comprehensive reviews and four automated analytical systems for total and isotopic thorium and uranium determination are presented as alternatives to classical radiochemical separations which are laborious and time consuming. These methodologies have been automated exploiting multicommutated flow techniques, which provide minimal sample handling, low reagent consumption and waste generation and a high frequency of analysis. Long path length spectrophotometry and ICP-MS have been implemented in the developed methods as detection techniques instead of radiometric detectors in order to obtain fully automated, low cost and fast thorium and uranium analyzers. All the developed methods proposed in this thesis have been satisfactorily applied to environmental samples and have been validated with reference materials