Dissertations / Theses on the topic 'Uranium cycle'

Uranium mining and nuclear power is a controversial topic as of late, especially in light of the recent Fukushima event. Although the actual use of nuclear fuel has minimal environmental impact, its issues come at the very beginning and end of the fuel’s life cycle in both the mining and fuel disposal process. This paper focuses on a life cycle analysis (LCA) of uranium mine in the desert nation of Namibia in Southern Africa. The goal of this LCA is to evaluate the environmental effects of uranium mining. The LCA focuses on water and energy embodiment such that they can then be compared to other mines. The functional unit of the analysis is 1kg of yellowcake (uranium oxide). The processes considered include mining and milling at Langer Heinrich Uranium (LHU). The impact categories evaluated include the categories in ReCiPe assessment method with a focus of water depletion, and cumulative energy demand. It was found that the major environmental impacts are marine ecotoxicity, human toxicity, freshwater eutrophication, and freshwater ecotoxicity. These mainly came from electricity consumption in the mining and milling process, especially electricity generated from hard coal. Milling tailings was also a contributor, especially for marine ecotoxicity and human toxicity. The other electricity generation types, including nuclear, hydro, natural gas, and diesel contribute to marine exotoxicity and human toxicity as well. Hydro-electricity, tailings form milling, sodium carbonate, and nuclear electricity also cause freshwater eutrophication at the LHU mine. The major contributor of the water depletion was hard coal generated electricity consumption as well. Tailings also led to a level of water depletion that was significant but much smaller than that of the coal-based electricity. In terms of energy, weighting portrayed the main energy used to be nuclear power, in terms of MJ equivalents. Nuclear power was then followed by fossil fuels and finally hydropower. Most of the energy used was for the uranium mining process rather than the milling process. As expected, the direct water, and energy values, 0.5459 m3 and 97.34 kWh per kg of yellowcake, were much lower than the LCA embodiment values of 282.67 m3 and 76,479 kWh per kg of yellowcake. When compared to other mines, the water use at LHU was found to be much lower while the energy use was found to be much higher.

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Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

COORDENAÇÃO DE APERFEIÇOAMENTO DO PESSOAL DE ENSINO SUPERIOR
CONSELHO NACIONAL DE DESENVOLVIMENTO CIENTÍFICO E TECNOLÓGICO
O ciclo do combustível nuclear é o conjunto de etapas do processo industrial que transforma o mineral urânio até sua utilização como combustível nuclear. Em todas as etapas do ciclo os trabalhadores estão expostos a partículas contendo urânio. Para avaliar os riscos é necessário conhecer a taxa de deposição, a concentração e a cinética da partícula no trato respiratório. Os testes de solubilidade in vitro, permitem um estudo sistemático da solubilidade de qualquer composto. Nesse estudo foram utilizadas amostras de DUA, TCAU e UO2 em contato com o liquido pulmonar simulado e estas foram analisadas pela técnica de PIXE (Particle Induced X rays Emission) para determinação da fração de urânio solubilizada e pela técnica de 252 Cf-PDMS (Plasma Desorption Mass Spectrometry) para a determinação da especiação química. Os objetivos específicos foram: (i) Identificar os compostos de urânio na fração respirável do aerossol nas etapas selecionadas do ciclo de combustível nuclear; (ii) identificar e determinar a solubilidade dos compostos de urânio em líquido pulmonar simulado; (iii) Determinar os parâmetros de solubilidade dos compostos de urânio. Os valores dos parâmetros de solubilidade determinados neste estudo para o DUA, TCAU e UO2 são: fr, = 0,83; sr = 0,51 d -1 e ss = 0,0075 d -1 ; fr = 0,60; sr = 0,70 d -1 e ss = 0,00089 d -1 e fr = 0,19; sr = 0,47 d -1 e ss = 0,0019 d -1 , respectivamente.
The nuclear fuel cycle is the industrial process that converts the uranium ore, to its use as fuel, inside of a nuclear power station. In all steps from the nuclear cycle workers are exposure to uranium dust particles. To evaluate the risk due particles incorporation data like deposition, concentration and kinetics of the particles in the respiratory tract must be know The in vitro solubility test allows a systemic understanding about the compound solubility. Samples of DUA, TCAU e UO2 and SLF was collected in different time interval and the uranium concentration was determined by PIXE (Particle Induced X rays Emissions) technique and the uranium compounds were identified by 252 Cf-PDMS (Plasma Desorption Mass Spectrometry). The specific objectives were: (i) identifying uranium compounds in the respirable fractions of aerosol (ii) identified and determinated the uranium coumpounds solubility in simulated lung fluid (iii) determinated the solubility parameters to this uranium compounds. The solubility parameters to DUA, TCAU and UO2 are: fr, = 0,83; sr = 0,51 d -1 and ss = 0,0075 d -1; fr = 0,60; sr = 0,70 d -1 and ss = 0,00089 d -1 e fr = 0,19; sr = 0,47 d -1 e ss = 0,0019 d -1, respectively.

Thesis (Ph. D.)--Massachusetts Institute of Technology, Dept. of Nuclear Engineering, 2003.
Includes bibliographical references (p. 189-194).
A heterogeneous LWR core design, which employs a thorium/uranium once through fuel cycle, is optimized for good economics, wide safety margins, minimal waste burden and high proliferation resistance. The focus is on the Whole Assembly Seed and Blanket (WASB) concept, in which the individual seed and blanket regions each occupy one full-size PWR assembly in a checkerboard core configuration. A Westinghouse 4-loop 1150 MWe PWR was selected as the reference plant design. The optimized heterogeneous core, after several iterations, employs 84 seed assemblies and 109 blanket assemblies. Each assembly has the characteristic 17x17 rod array. The seed fuel is composed of 20 w/o enriched annular UO2 pellets. Erbium is used in the fresh seed to help regulate local power peaking and reduce soluble boron concentrations. Erbium was evenly distributed into all pin central holes except for the peripheral pins and four corner pins of each assembly where more erbium was used due to their higher power level. The blanket fuel is a mixture of 87% ThO2 - 13% UO2 by volume, where the uranium is enriched to 10 w/o. The blanket fuel pin diameter is larger than the seed fuel pin diameter. There are two separate fuel management flows: a standard three-batch scheme is adopted for the seed (18 month cycle length) and a single-batch for the blanket, which is to stay in the core for up to 9 seed cycles. The WASB core design was analyzed by well known tools in the nuclear industry. The neutronic analysis was performed using the Studsvik Core Management System (CMS), which consists of three codes: CASMO-4, TABLES-3 and SIMULATE-3. Thermal-hydraulic analysis was performed using EPRI's VIPRE-01.
(cont.) Fuel performance was analyzed using FRAPCON. The radioactivity and decay heat from the spent seed and blanket fuel were studied using MIT's MCODE (which couples MCNP and ORIGEN) to do depletion calculations, and ORIGEN to analyze the spent fuel characteristics after discharge. The analyses show that the WASB core can satisfy the requirements of fuel cycle length and safety margins of conventional PWRs. The coefficients of reactivity are comparable to currently operating PWRs. However, the reduction in effective delayed neutron fraction (eff) requires careful review of the control systems because of its importance to short term power transients. Whole core analyses show that the total control rod worth of the WASB core is about 1/3 less than those of a typical PWR for a standard arrangement of Ag-In-Cd control rods in the core. The use of enriched boron in the control rods can effectively improve the control rod worth. The control rods have higher worth in the seed than in the blanket. Therefore, a new loading pattern has been designed so that almost all the control rods will be located in seed assemblies. However, the new pattern requires a redesign of the vessel head of the reactor, which is an added cost in case of retrofitting in existing PWRs. Though the WASB core has high power peaking factors, acceptable MDNBR in the core can be achieved under conservative assumptions by using grids with large local pressure loss coefficient in the blanket. However, the core pressure drop will increase by 70% ...
by Dean Wang.
Ph.D.

Thesis (S.M.)--Massachusetts Institute of Technology, Dept. of Nuclear Science and Engineering, 2012.
Cataloged from PDF version of thesis.
Includes bibliographical references (p. 110-111).
Reactors utilizing a highly energetic neutron spectrum, often termed fast reactors, offer large fuel utilization improvements over the thermal reactors currently used for nuclear energy generation. Conventional fast reactor deployment has been hindered by the perceived need to use plutonium as fuel, coupling the commercial introduction of fast reactors to the deployment of large-scale thermal reactor used fuel reprocessing. However, the future of used fuel treatment in the United States is highly uncertain, creating a bottleneck for the introduction of fast reactor technology. A strategy centered around using uranium-fueled fast reactor cores in a once-through mode-a uranium startup fast reactor (USFR)-decouples fast reactor commercialization from fuel reprocessing and enables transition to a recycle mode once the technology becomes available and economic. The present work investigates the optimal strategy for recycling spent fuel from once-through sodium cooled fast reactors (SFRs), by analyzing the performance of various designs. A range of acceptable transitions are described and their economic, breeding, nonproliferation, and safety performance are characterized. A key finding is that the burnups of all cores were limited by the allowable fluence to the cladding rather than by the core reactivity. The carbide cores achieve fluence-limited burnups 15-25% greater than the comparable metal cores, though the metal cores can be optimized via decrementing the fuel volume fraction to reach fluence-limited burnups within 10% of the carbide cores. The removal of minor actinides from the recycled fuel has a minimal impact on the achievable burnups of both types of fuels, decreasing the fluence-limited burnup by less than half a percent in all cases. Similarly, long-term storage of the USFR fuel had minimal impact on the achievable burnups of all cores, decreasing the fluencelimited burnup by no more than 2% in all cases. Levelized fuel costs were in the range of 5.98 mills/kWh to 7.27 mills/kWh for the carbide cores, and 6.81 mills/kWh to 7.57 mills/kWh for the optimized metal cores, which is competitive with fuel costs of current LWRs and once-through SFRs. The metal and carbide multicore cores, made using slightly more than one once-through SFR core, functioned as slight fissile burners with fissile inventory ratios (FIRs) near 0.9. The uranium+ cores, made using one oncethrough SFR core plus natural uranium makeup, functioned in a fissile self-sustaining mode with FIRs near unity. All cores discharged fuel that was less attractive for weapon use than that of an LWR. The carbide cores had maximum sodium void worths in the range of $2.81-$2.86, approximately half the worth of the metal cores, which were in the range of $4.97-$5.14. Carbide and metal multicore cores possessed initial reactivities in the range of 15,000 pcm, requiring either multi-batch staggered reloading or control system modifications to achieve acceptable shutdown margins. The uranium+ carbide and metal cores achieved acceptable shutdown margin with the nominal control configuration and the single-batch reloading scheme. The overall conclusion is that USFR spent fuel is readily usable for recycle.
by Joshua Richard.
S.M.

La connaissance du comportement géochimique de l’uranium (U) dans l’environnement est essentielle pour en limiter la propagation dans les milieux contaminés. Ce travail de thèse visait avant tout à déterminer l’évolution sur plusieurs milliers d’années des phases non-cristallines de U dans les sédiments naturellement riches en U (jusqu’à plus de 1000 µg/g) du lac Nègre, dans le massif du Mercantour (Alpes-Maritimes, France). Grâce aux rapports isotopiques de U (δ238U et (234U/238U)) et à la spectroscopie d’absorption X (XAS) au seuil L3 de U, il est montré que U est déposé initialement sous forme d’espèces mononucléaires liées à la matière organique, et est rapidement réduit en U(IV). En moins de 700 ans, ces phases sont transformées en polymères de U(IV)-silice avec une structure locale proche de la coffinite (USiO4·nH2O). Cette transformation souligne l’impact de l’abondance de ligands qui limitent la précipitation de phases cristallines de U, mais ne réduit que faiblement la labilité de U, dont la mobilité potentielle reste importante après plus de 3000 ans. A l’échelle du bassin versant, U provient initialement de fractures dans la roche-mère granitique, puis est piégé en grandes quantités dans les sols, en particulier dans la zone humide en amont du lac (jusqu’à > 5000 µg/g U), avant d’être transporté vers le lac par érosion. Cette fixation dans les sols a lieu par complexation sur la matière organique dont certaines structures biologiques, avant réduction partielle en U(IV). On trouve ainsi surtout des formes mononucléaires de U, mais aussi des phases polymériques de U(VI) potentiellement issues d’un vieillissement de U après des milliers d’années d’accumulation
Understanding the geochemical behavior of uranium (U) in the environment is crucial for the limitation of U dissemination in contaminated systems. The primary objective of this thesis was to determine the potential evolution of noncrystalline U phases over thousand years in naturally U-rich lacustrine sediments (up to more than 1000 µg/g) from Lake Nègre, in the Mercantour-Argentera Massif (South-East France). Using U isotopic ratios (δ238U and (234U/238U)) and U L3-edge X-ray absorption spectroscopy (XAS), we show that U is first deposited as organic-bound mononuclear species and is readily reduced to U(IV). In less than 700 years, these species transform into U(IV)-silica polymers with a local structure close to that of coffinite (USiO4·nH2O). This transformation highlights the role of ligand abundance in limiting the precipitation of crystalline U phases, but only slightly reduces the lability of uranium which potential mobility remains significant even after several thousand years. At the watershed scale, U originates from fractures in the granitic bedrock and is subsequently scavenged in the soils, especially in the wetland upstream of the lake (up to > 5000 µg/g), before being transported through erosion. Uranium scavenging in the soils occurs through complexation by organic matter including particular biological structures, followed by partial reduction to U(IV). U is thus mainly present in mononuclear species but also in polymeric U(VI) phases which may potentially result from U aging after thousand years of accumulation

L'uranium, élément lithophile et incompatible, peut être utilisé en traceur géochimique pour discuter des différents modèles de formation et d'évolution de la croûte continentale. Ce travail de thèse, ciblé sur la ceinture Pan-Africaine du Lufilien en Zambie, caractérise le cycle de l'U et les minéralisations d'U pour ce segment de croûte continentale. Les séries silicoclastiques/évaporitiques de la ceinture du Lufilien, encaissant les minéralisations d'U, se sont déposées en contexte de rift (bassin du Roan) lors de la dislocation du supercontinent Rodinia au Néoprotérozoïque inférieur. Les âges U-Pb des grains de zircon détritique de ces séries métasédimentaires soulignent une source principalement Paléoprotérozoïque. Ces mêmes grains de zircon présentent des signatures isotopiques epsilonHf inférieures au CHUR (entre 0 et -15) et des âges modèles TDM Hf, compris entre ~2.9 et 2.5 Ga. Ces données suggèrent donc la formation d'une croûte continentale précoce, et donc une extraction mantellique de l'U dès la fin de l'Archéen puis une remobilisation par déformation et métamorphisme au cours du Protérozoïque. L'U aurait donc été remobilisé et re-concentré au cours d'orogenèses successives jusqu'au cycle Pan-Africain. Durant ce cycle Pan-Africain, la datation U-Pb et la signature REY (REE et Yttrium) des cristaux d'uraninite caractérisent un premier évènement minéralisateur, daté vers 650 Ma, associé à la circulation de fluides de bassin expulsés des évaporites du Roan, circulant à l'interface socle/couverture, dans ce contexte de rift continental. Un second événement minéralisateur, daté vers 530 Ma et contemporain du pic métamorphique, est assuré par des fluides métamorphiques issus de la dissolution des évaporites, en contexte de subduction/accrétion continentale. Quelques remobilisations tardives de l'U sont observées lors de l'exhumation des roches métamorphiques
Uranium is an incompatible and lithophile element and can be used as a geochemical tracer to discuss the generation and the evolution of continental crust. This thesis, focused on the Pan-African Lufilian belt in Zambia, characterizes the U cycle for this crustal segment. Silici-clastic and evaporitic sediments have been deposited within an intracontinental rift during the dislocation of the Rodinia supercontinent during the early Neoproterozoic. U-Pb ages on detrital zircon grains in these units indicate a dominant Paleoproterozoic provenance. The same zircon grains show subchondritic epsilonHf (between 0 and -15) and yield Hf model ages between ~2.9 and 2.5 Ga. These data suggest that the continental crust was generated before the end of the Archean associated with U extraction from the mantle. This old crust has been reworked by deformation and metamorphism during the Proterozoic. U has been remobilized and re-concentrated during several orogenic cycles until the Pan-African orogeny. During this Pan-African cycle, U-Pb and REY (REE and Yttrium) signatures of uranium oxides indicate a first mineralizing event at ca. 650 Ma during the continental rifting. This event is related to late diagenesis hydrothermal processes at the basement/cover interface with the circulation of basinal brines linked to evaporites of the Roan. The second stage, dated at 530 Ma, is connected to metamorphic highly saline fluid circulations, synchronous to the metamorphic peak of the Lufilian orogeny. These fluids are derived from the Roan evaporite dissolution. Some late uranium remobilizations are described during exhumation of metamorphic rocks and their tectonic accretion in the internal zone of the Lufilian orogenic belt

Uranium exploration and mining activities in Namibia have increased rapidly since 2003, which increase not only poses a significant impact on the country’s economy, but also on its unique and pristine natural environment. The nature and extent of the environmental impacts associated with uranium mining requires a sound environmental law and policy framework that regulates uranium activities, impacts and aspects during each phase of the project life cycle of a uranium mine. It also requires of authorities to establish and enhance environmental protection and sustainability during uranium mining operations and to ensure that all environmental impacts that inevitably occur as a result of uranium mining activities are addressed in a holistic and integrated manner during each phase of the project life cycle of a uranium mine. In order to do this the country must develop and maintain an efficient and effective environmental governance regime. Namibia’s environmental law and policy framework that regulates uranium mining does not cover the entire PLC of uranium mining. It is vital that the current loops in the country’s existing environmental regulatory framework be closed and that an efficient and effective environmental governance regime, as envisaged in this study, be established. This will enable the administering agents to actively promote and maintain the welfare of the people, ecosystems, essential ecological processes and the biodiversity of Namibia, as well as the utilisation of living natural resources on a sustainable basis to the benefit of all Namibians, both present and future, as pledged in the Namibian Constitution.
Thesis (LL.M. (Environmental law))--North-West University, Potchefstroom Campus, 2012.

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Tese (Doutoramento)
IPEN/T
Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

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Tese (Doutoramento)
IPEN/T
Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

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Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

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IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

De manière à répondre à l'accroissement des besoins en uranium, l'exploitation de nouvelles ressources de composition minéralogique variée devient une nécessité. De plus, dans une perspective de développement durable, les procédés d'exploitation et de traitement des minerais d'uranium requièrent une optimisation afin de réduire leur empreinte environnementale. Dans ce but, il est nécessaire d'acquérir des données thermodynamiques fiables relatives aux systèmes d'intérêt, dont en particulier les phosphates et les vanadates d'uranium (VI). Dans ce contexte, une étude multiparamétrique de la dissolution de la méta-torbernite Cu0,8(H3O)0,2(UO2)2(PO4)2,8H2O, de la méta-autunite Ca(UO2)2(PO4)2,6H2O, de la méta-ankoleïte K2(UO2)2(PO4)2,6H2O et de la carnotite K2(UO2)2(VO4)2,3H2O a été entreprise. Dans un premier temps, des analogues à ces quatre phases minérales ont été préparés par différentes méthode, basées sur une voie sèche pour la carnotite et sur des voies humides pour les trois phases phosphatées. Elles ont ensuite été caractérisées d'un point de vue structural, microstructural et chimique. Des structures cristallographiques similaires ont ainsi été mises en évidence au sein desquelles les polyoxoanions (PO43- ou V2O86-) et les groupements uranyle forment des feuillets parallèles entre lesquels s'insèrent les contres cations (Cu2+, Ca2+ ou K+) et les molécules d'eau. Hormis pour la méta-ankoleïte, les analogues synthétiques ont également été comparées à des minerais naturels. Il a ainsi été possible de mettre en évidence des différences d'ordre chimique (présence d'impuretés dans les échantillons naturels) et morphologique (tailles de grains, notamment). La dissolution de ces phases a ensuite été étudiée, tant d'un point de vue cinétique que thermodynamique, à travers des études menées en conditions statiques et dynamiques, dans différents milieux acides (H2SO4, HNO3 et HCl) et à plusieurs températures. Les vitesses de dissolution mesurées sont proches de 1 g.m-2.j-1 pour les quatre phases. Dans les conditions utilisées, la dissolution de la méta-autunite s'est avérée incongruente (précipitation de phosphates d'uranyle), empêchant la détermination des constantes de solubilité. En outre, la dissolution de la méta-ankoleïte a conduit à un échange cationique aboutissant à la formation de solutions solides (H3O)2xK2x-2(UO2)2(PO4)2, 6H2O (0 < x < 2) dont les constantes de solubilité ont pu être calculées. Enfin, les expériences menées sur la méta-torbernite et la carnotite ont conduit à des réactions de dissolution congruentes qui ont permis d'accéder aux données thermodynamiquement d'intérêt telles que leur produit de solubilité et leurs grandeurs standards associées à la dissolution (DrH°, DrG° et DrS°) ou à la formation (DfG° = -6100 ± 5 kJ.mol-1 pour la méta-torbernite et DfG° = -4632 ± 7 kJ.mol-1 pour la carnotite) de chacune de ces phases. Les résultats obtenus montrent que les constantes de solubilité des trois phases phosphatées sont très faibles (10-53 < Ks,0° < 10-45) et ont des valeurs qui diffèrent peu selon la nature du contre cation, en bon accord avec leurs similitudes structurales. D'autre part, la comparaison des grandeurs thermodynamiques déterminées dans ce travail, montre que la carnotite (Ks,0° = 10-63) est plus stable que les phases phosphatées étudiées. La différence observée peut s'expliquer par la structure des feuillets à base de vanadates. Cette étude a ainsi permis d'obtenir des premières valeurs de solubilité pour les phosphates et les vanadates d'uranium(VI) présents dans les gisements d'intérêt économique et d'établir un premier modèle d'estimation de la solubilité pour des phases similaires. Ces données ont également été utilisées lors d'une modélisation en conditions environnementales afin de déterminer la nature des phases susceptibles de se former dans un cas réel (eaux d'un lac proche d'un gisement d'uranium)
In the current context of restart of the nuclear energy, the needs in uranium are expected to increase significantly. Moreover, in a perspective of sustainable development, the exploitation, the treatment and the purification of uranium ores need to be optimized. It is thus necessary to determine reliable thermodynamic data (and especially solubility constants) for the systems of interest, especially uranium(VI) phosphates and vanadates. In this aim, a multiparametric study of the dissolution of meta-torbernite Cu0.8(H3O)0.2(UO2)2(PO4)2.8H2O, meta-autunite Ca(UO2)2(PO4)2.6H2O, meta-ankoleïte K2(UO2)2(PO4)2.6H2O and carnotite K2(UO2)2(VO4)2.3H2O was undertaken.First, analogues of these four minerals were synthesized, based only on dry chemistry process for carnotite or on wet chemistry methods for the phosphate phases. They were then extensively characterized (in terms of structure, microstructure and chemical composition). It particularly highlighted the similar structures of such compounds. The anionic groups (PO43- or V2O86-) and uranyl form parallel layers between which counter cations (Cu2+, Ca2+ or K+) and water molecules are inserted. However, the counter cations present in the interlayer space of the three phosphate phases present different lability. The synthetic phases were also compared to their natural analogues, except for meta-ankoleïte, which allowed us to point out significant differences in the composition (presence of impurities in natural samples) and the morphology (grain size).The dissolution of these phases was then studied from a kinetic and thermodynamic point of view, through leaching tests in static and dynamic conditions, in various acid media (sulfuric, nitric and hydrochloric) and at different temperatures. In these conditions, the dissolution of meta-autunite was found to be uncongruent due to the precipitation of uranyl phosphate then avoidinf the determination of solubility constants. Similarly, the dissolution of meta-ankoleite was preceded by a cation exchange step between K+ and H3O+ leading to the formation of (H3O)2xK2x-2(UO2)2(PO4)2.6H2O (0 < x < 2) solid solutions, whose solubility constant have been evaluated. Finally, meta-torbernite and carnotite presented congruent dissolutions which allowed the determination of thermodynamic data of interest such as solubility products and standard enthalpy, Gibbs free energy and entropy associated with the dissolution reaction (DrH°, DrG° and DrS°) and formation of each phase (DfH°, DfG° and DfS°).The results obtained evidenced very low and similar solubility constants for the three phosphate phases studied (10-53 < Ks,0° < 10-45). Such small variation directly came from the closely related crystal structures previously described. In addition, the difference in composition of the sheets between phosphate and vanadate phases led to greater stability of carnotite (Ks,0° = 10-63) compared to phosphates phases. The solubility values derived from this study for phosphates and vanadates uranium(VI) allowed estimating values for similar phases. These data were also used in a geochemical model for the prediction of neoformed phases in a real case (water of a lake near an uranium deposit)

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Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Le sujet porte sur l'étude géochimique et métallogénique des minéralisations uranifères (gisement de bertholène) et de barytine-sulfures (gisement de Lacan et du nord du massif cristallin des Palanges).

Au cours de ces dernières décennies, des études ont étés menées pour identifier plusieurs traceurs des matériaux du cycle du combustible nucléaire, dans le cadre de la lutte contre la prolifération nucléaire. Ces matériaux sont généralement collectés lors d’inspections dans des installations nucléaires, ou saisis lors de contrôles de trafics illicites. Les informations fournies par ces traceurs sont parcellaires et ne permettent pas de déterminer avec exactitude la provenance et l’historique industriel de ces matériaux.Le but de ce travail de thèse est de démontrer le potentiel de l’utilisation des isotopes du molybdène pour le traçage des matériaux du cycle du combustible nucléaire. Le choix s’est porté sur le molybdène car en raison de la similarité de leurs propriétés chimiques, le molybdène et l’uranium sont étroitement associés dans les minerais d’uranium et tout au long de la chaîne de purification de l’uranium. L’étude s’est focalisée sur une partie de l’amont du cycle du combustible, depuis l’extraction des minerais d’uranium jusqu’à la production des concentrés miniers d’uranium : divers procédés physiques et chimiques sont appliqués, à la fois pour purifier l’uranium et abaisser la concentration en molybdène.Au cours de cette étude, une nouvelle méthode de séparation du molybdène a été développée pour caractériser sa composition isotopique dans des minerais, minéraux et concentrés miniers d’uranium. La variabilité des compositions isotopiques du molybdène dans un gisement d’uranium est principalement due aux mécanismes d’adsorption et/ou de précipitation du molybdène. Les gisements magmatiques et sédimentaires ont des compositions isotopiques différentes, ce qui permet ainsi leurs distinctions. Les concentrés miniers d’uranium produits à partir de ces deux types de gisements ont des compositions isotopiques similaires aux minerais. Ces résultats soulignent ainsi le potentiel des isotopes du molybdène comme traceur des origines des concentrés miniers d’uranium. Cependant, un fractionnement des isotopes du molybdène a été établi lors de la production des concentrés miniers d’uranium pour deux usines au Niger. Les procédés de purification de l’uranium tels que la lixiviation, l’extraction par solvant et la précipitation ont été reproduits en laboratoire sur des échantillons réels pour expliquer le fractionnement isotopique du molybdène lors de la production des concentrés miniers. Au cours de ces procédés, le fractionnement peut être positif (lixiviation), négatif (extraction par solvant, précipitation à l’eau oxygénée) ou nul (précipitation à l’ammoniaque). Dans le cas des échantillons du Niger, la somme de ces procédés est négative, dans le sens des données expérimentales que nous avons obtenues, démontrant ainsi également le potentiel de l’utilisation des isotopes du molybdène comme traceur des procédés de transformations des matériaux du cycle du combustible nucléaire
Nuclear forensics aims at determining the age, provenance as well as industrial or storage history of uranium ores and uranium ore concentrates that are part of the nuclear fuel cycle. Several potential tracers have already been identified for this purpose. However, these tracers are not providing always unambiguous information. This study is focused on establishing Mo isotopes as a new tracer of uranium ore provenance and of ore processing for its application in nuclear forensics. Molybdenum and uranium share a number of common geochemical properties. In the nuclear fuel cycle, molybdenum is an impurity that is difficult to separate during uranium extraction and purification processes, while its concentration is required to be lower than some specification limits. We focused this study on the first part of the nuclear fuel cycle, from the uranium ores extraction to the production of uranium ore concentrates.We developed an enhanced separation method for Mo from a uranium-rich matrix (uranium ores, uranium minerals, uranium ore concentrates) in order to analyze the mass fractionation induced by processes typical of the nuclear fuel cycle. Molybdenum isotopic compositions in uranium ores depend of adsorption and precipitation processes. The δ98Mo values of sedimentary uranium ores is shifted to negative values relative to magmatic ores. This provides a means of distinguishing these types of uranium ores. Uranium ores concentrates produced from both uranium ore natures (magmatic and sedimentary) have Mo isotope compositions similar to the uranium ores. These results suggest that molybdenum isotopes have a strong potential of as a tracer for identifying the origin of the uranium ore concentrates. However, Mo isotopes fractionations were established during the production of uranium ore concentrates in the both Niger mills. We reproduced in laboratory the lixiviation, solvent extraction and precipitation processes to explain these observations. The Mo isotopes fractionation is positive for the lixiviation process, negative for the solvent extraction and precipitation with hydrogen peroxide, and null for ammonia precipitation. In the case of the Niger samples, the sum of these processes is negative and agrees with our experimental data. Mo isotopes have a strong potential as a tracer for identifying the origin and transformation of uranium in the nuclear fuel cycle, in the framework of nuclear forensics

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Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

La prévisibilité des changements dans la qualité et la quantité des ressources hydriques renouvelables repose sur une étude quantitative des mécanismes qui contrôlent ces paramètres. En lien avec cette problématique, la présente étude privilégie une approche fondée sur le monitoring géochimique des exports fluviaux dissous (2H-18O, cations majeurs, carbone organique dissous (COD), Nd, Sr, 87Sr/86Sr, U, (234U/238U)). L’étude a pour objectif (i) de tracer le cycle de l’eau et (ii) de documenter les taux d’altération chimique des roches au sein bassins hydrographiques des baies d’Hudson, de James et d’Ungava (HJUB) ainsi que du fleuve Saint-Laurent. La région d’étude couvre plus de 2,8x106 km2 sur 15 degrés de latitude. Les rivières Koksoak, Great Whale, La Grande et des Outaouais et les fleuves Nelson et Saint-Laurent ont fait l’objet d’un suivi temporel alors que dix autres rivières de la région ont été échantillonnées ponctuellement (durant la fonte des neiges et l’étiage estival) afin de fournir des informations complémentaires. Les teneurs en 2H-18O des rivières étudiées présentent des variations saisonnières systématiques dont l’amplitude atteint 1 à 5‰ (18O). L’appauvrissement en isotopes lourds marquant la fonte des neiges constitue le trait caractéristique des profils isotopiques saisonniers. Lors de la période libre de glace, des enrichissements graduels en isotopes lourds sont observés en réponse à l’évaporation. La rivière La Grande est une exception à cette règle en raison de l’effet tampon causé par les réservoirs hydroélectriques qui la ponctuent. Lorsque rapportées dans un graphique 2H vs 18O, les rivières définissent des droites évaporatoires situées sous la droite des eaux météoriques et ayant une pente plus faible que cette dernière. À partir de bilans de masses isotopiques, il a été estimé que 10% de l’eau atteignant le bassin de la rivière des Outaouais est évaporée avant de rejoindre l’exutoire de cette dernière dans le fleuve Saint-Laurent. De façon similaire, on estime à 5-15% les taux d’évaporation dans les bassins hydrographiques du nord-est du Canada. Les rivières drainant les bassins hydrographiques contigus du nord-est du Canada définissent un gradient isotopique latitudinal (18O(‰ vs VSMOW) = -0. 36*Latitude+4. 4‰) parallèle à celui rapporté pour les précipitations au niveau de la même région. Cette observation tend à indiquer que le gradient isotopique hérité des précipitations est conservé dans les rivières, malgré les processus subséquents à la recharge des bassins. Au sein des bassins de l’HJUB, les taux d’altération des roches ont été étudiés à partir des exports fluviaux dissous. Les rivières du bouclier présentent des concentrations en cations majeurs variant entre 62 et 360 M, des teneurs en néodyme ([Nd]) allant de 0. 57 à 4. 72 nM et des teneurs en COD variant entre 241 et 1777 M. En comparaison, le fleuve Nelson présente des concentrations en cations majeurs plus élevées (1200-2276 M), des [Nd] plus faibles (0. 14-0. 45 nM) et des [COD] intermédiaires (753-928 M). Au sein des rivières Koksoak, Great Whale et Nelson, les concentrations en cations dissous (Na-KMg- Ca-Sr) présentent des variations saisonnières qui transcrivent l’effet des conditions hydro-climatiques. Comme pour les teneurs en 2H-18O, la dilution causée par la fonte des neiges constitue le trait caractéristique des chroniques saisonnières. Les rivières étudiées exportent vers l’HJUB un flux cationique dissout (Na-K-Mg-Ca-Sr) de 8x106 tonnes*an-1. Au sein des bassins hydrographiques, les taux d’altération chimique (cationique) des roches varient entre 1. 0 et 5. 6 tonnes*km-2*an-1. Le contrôle lithologique est proéminent, tel que suggéré par la relation établie entre l’abondance de roches volcaniques et sédimentaires (V+S%) dans les bassins et les taux d’altération cationiques des roches (ACR): ACR=0. 8*(V+S%)+0. 9. Les flux de Nd sont découplés des taux d’altération des roches mais corrélés aux flux de COD (r2=0. 95). Ces derniers diminuent vers le nord et semblent tributaires des conditions hydro-climatiques. Les exports fluviaux d’uranium ont été étudiés afin de fournir des précisions sur les processus d’altération des roches. Les rivières drainant le Bouclier canadien et la Plate-Forme Intérieure présentent des signatures [U] vs (234U/238U) distinctes. Dans le fleuve Nelson (Plate-Forme Intérieure) les [U] varient entre 1. 05 et 2. 45 nM et les déséquilibres (234U/238U) atteignent 1. 21 à 1. 25. Les [U] sont plus faibles au sein des du Bouclier canadien (0. 04 – 1. 24 nM) alors que les déséquilibres (234U/238U) sont plus variables (1. 11 – 1. 99). Dans l’ensemble, les rivières étudiées exportent 3. 4x105 moles*an-1 d’uranium vers l’HJUB, avec un ratio (234U/238U) moyen de 1. 27. Les flux d’U sont découplés des taux d’altération des roches et l’accumulation d’uranium au sein de dépôts organiques semble intervenir sur les budgets à l’échelle des bassins. Les signatures (234U/238U) distinctes des rivières étudiées pourraient offrir la possibilité de tracer les exports fluviaux dissous au sein du domaine océanique de l’HJUB
The predictability of changes in the quality and quantity of renewable water resources relies on a quantitative study of the mechanisms that control these parameters. In connection with this problem, this study favors an approach based on the geochemical monitoring of dissolved riverine exports (δ2H-18O, major cations, dissolved organic carbon (DOC), [Nd], [Sr], 87Sr/86Sr, [U], (234U/238U)). The study aims at (i) tracing the water cycle and at (ii) quantifying rock chemical weathering rates in major river basins in central and eastern Canada. The study area covers more than 2. 8 x106 km2 over 15 degrees of latitude and encompasses the major basins of Hudson Bay, James and Ungava (HJUB) as well as the St. Lawrence River. The Koksoak, Great Whale, La Grande, Nelson, Ottawa and St. Lawrence rivers were monitored in time whereas ten other rivers flowing within the same region were sampled during spring snowmelt and summer baseflow, providing complementary data. The studied rivers present systematic seasonal 18O-2H patterns with amplitudes reaching 1 to 5 ‰ (18O). Heavy-isotope depletions mark the snowmelt event and gradual heavy-isotope enrichments occur in response to evaporation during the ice-off season. The La Grande River constitutes an exception due to the buffering effect of hydroelectric reservoirs that smooth out the temporal isotopic fluctuations. When reported in a 2H vs 18O chart, the studied rivers define Local Evaporation Lines (LEL) extending below the Meteoric Water Line (MWL). Isotopic mass balance calculations suggest that approximately 10% of the total inflow to the Ottawa River Basin is lost through evaporation before reaching its outlet in the St. Lawrence River. The rivers draining contiguous basins of Northeastern Canada define a River Water Line (RWL) arising from imbricate Local Evaporation Lines (LEL). A method using the distance between the RWL and the MWL is proposed for estimating the average evaporation over inflow ratio (5 to 15%) at the scale of the study area. These rivers also define a latitudinal isotopic gradient (18O (‰ vs. VSMOW) = -0. 36 * Latitude +4. 4 ‰) that is parallel to that reported for precipitation over the same region. This observation suggests that the isotopic gradient inherited rainfall is preserved in rivers, despite the subsequent hydrological processes occurring within the basins. Landscape chemical denudation rates were addressed based on the dissolved chemistry of rivers flowing into the HJUB. The rivers of the Canadian Shield depict major cation concentrations ranging between 62 and 360 μM, neodymium concentrations ([Nd]) of 0. 57 to 4. 72 nM and variable dissolved organic carbon concentrations ([DOC]) (241 – 1777 μM). In comparison, the Nelson River (Interior Platform) shows higher major cation concentrations (1200 – 2276 μM), lower [Nd] (0. 14 to 0. 45 nM) and intermediate [DOC] (753 – 928 M). Within the HJUB basins, the dissolved cation concentrations (Na-K-Mg-Ca-Sr) show seasonal variations that transcribe the effect of hydro-climatic conditions. As for 2H-18O patterns, the dilution caused by snowmelt constitutes the main feature of the seasonal patterns. Altogether, the studied rivers export 8x106 tons*yr-1 of dissolved major cations and 50 tons*yr-1 of dissolved Nd towards the HJUB. Basin scale total rock cationic denudation rates (TRCDR) range from 1. 0 to 5. 3 tons*yr-1*km2 and are essentially controlled by lithology, as illustrated by the relationship established between rock denudation rates and the proportion of sedimentary and volcanic rocks (%S+V) within the basins: TRCDR=0. 08(%S+V)+0. 9. Contrastingly, dissolved Nd exports are decoupled from rock weathering rates and seem to be strongly dependent upon organic matter cycling, as illustrated by the tight coupling between Nd and DOC fluxes. These fluxes decrease northwards, likely in response to the hydro-climatic gradient. Riverine dissolved U contents were studied in order to provide further information regarding weathering sources and processesin the HJUB region. The rivers draining the Canadian Shield vs. That draining the Interior Platform depict distinct [U] vs. (234U/238U) clusters. In the Nelson River (draining the Interior Sedimentary Platform), U-concentrations are highest (1. 05 - 2. 45 nM) whereas (234U/238U) show little variability (1. 21 – 1. 25). U concentrations are comparatively lower in the rivers of the Canadian Shield (0. 04 – 1. 24 nM) whereas (234U/238U) span from 1. 11 to 1. 99. Altogether, the studied rivers export 3. 4x105 moles. Yr-1 of U towards the HJUB, with an amount-weighted average (234U/238U) of 1. 27. At the scale of the study area, U and major cations exports are decoupled, suggesting that rock weathering processes do not solely control U budgets. First-order calculations reveal that U accumulation in peatlands could significantly impact basin-scale U budgets. The distinct [U] vs (234U/238U) clusters defined by the monitored rivers of the HJUB region (Koksoak, Great Whale, La Grande and Nelson) should allow tracing the source of dissolved U in the nearby oceanic domain

O Brasil com o propósito de se tornar autossuficiente na produção de radioisótopos e fontes radioativas usados na medicina nuclear, na agricultura e no meio ambiente desenvolveu o projeto de um reator multipropósito de 30 megawatts de potência para atender a demanda nacional. No Instituto de Pesquisas Energéticas e Nucleares (IPEN), o Centro de Combustível Nuclear (CCN) é responsável pela fabricação dos combustíveis para o reator IEA-R1 e, possivelmente, pelos combustíveis do reator multipropósito. Com o intuito de atender a demanda para os reatores foi projetada uma nova planta de fabricação com a capacidade máxima de 60 combustíveis por ano, o qual atualmente é de dez. O aumento da produção consequentemente aumentará o volume de efluentes gerados. A atual preocupação com o meio ambiente faz-se necessário elaborar um plano de gestão para tornar o processo sustentável, o qual ocasionará em benefícios ambientais, econômicos e sociais. O processo produtivo do combustível gera vários tipos de efluentes, contendo urânio ou não, sendo sólidos, líquidos e gasosos com características físicas e químicas variadas. Esse estudo tem como objetivo identificar, caracterizar e segregar os efluentes gerados em todo o processo produtivo de obtenção do combustível nuclear do tipo MTR (Materials Testing Reactors). No desenvolvimento do presente trabalho foram utilizadas como base a Resolução n° 357, de 17 de março 2005, e a Resolução n° 430, de 13 de maio de 2011 do Conselho Nacional do Meio Ambiente CONAMA. Com os resultados obtidos foi possível determinar que os efluentes líquidos são os principais aspectos que podem causar contaminação ao meio ambiente, e a atual situação do CCN mostra que 30% do efluente líquido possui tratamento de recuperação de urânio; 20% dos efluentes líquidos são reutilizados na composição química em que foi gerado; 35% descartado diretamente ao meio ambiente de acordo com a legislação. O restante dos efluentes líquidos, cerca de 15%, estão em fase de desenvolvimento do processo de tratamento.
Brazil with the purpose of becoming self-sufficient in the production of radioisotopes and radioactive sources used in nuclear medicine, agriculture and the environment has developed the project of a multipurpose reactor of 30 megawatts of power to meet the national demand. At the Instituto de Pesquisas Energéticas e Nucleares (IPEN), the Centro de Combustível Nuclear (CCN) is responsible for manufacturing fuels for the IEA-R1 reactor and, possibly, the multipurpose reactor fuels. In order to meet the demand for the reactors, a new manufacturing plant with a maximum capacity of 60 fuels per year has been designed, which is currently ten. The increase in production will consequently increase the volume of effluents generated. The current concern with the environment makes it necessary to elaborate a management plan to make the process sustainable, which will lead to environmental, economic and social benefits. The production process of the fuel generates several types of effluents - containing uranium or not - being solid, liquid and gaseous with varied physical and chemical characteristics. This study aims to identify, characterize and segregate the effluents generated in the entire production process of obtaining the nuclear fuel type MTR (Materials Testing Reactors). In the development of this paper, Resolution 357 of March 17, 2005, and Resolution No. 430 of May 13, 2011 of the National Environmental Council - CONAMA, were used. With the results obtained it was possible to determine that the liquid effluents are the main aspects that can cause contamination to the environment, and the current situation of the CCN shows that 30% of the liquid effluent has uranium recovery treatment; 20% of the liquid effluents are reused in the chemical composition in which it was generated; 35% discarded directly to the environment according to the legislation. The rest of the liquid effluents, about 15%, are in the development phase of the treatment process.

Dans de nombreux gisements métalliques, notamment en contexte sédimentaire et en particulier dans le cas des shales noirs, des relations spatiales voire génétiques sont décrites entre la matière organique et les métaux. Une série de shales/schistes noirs affectés par des conditions thermo barométriques croissantes a été sélectionnée afin d'étudier le comportement et le devenir de l'uranium de la sédimentation au métamorphisme. Dans les Alum Shales cambro ordoviciens (Suède) faiblement enfouis, l'uranium reste dispersé et n'apparaît sous aucune forme minéralogique identifiable. Le passage des Alum Shales dans la fenêtre pétrolière et la génération d'hydrocarbures n'a pas provoqué de remobilisation identifiable de la concentration primaire, les hydrocarbures migrés ne transportant pas l'uranium. En revanche, le métamorphisme de faciès schiste vert associé à l'orogénèse calédonienne a entraîné une réexpression de la minéralisation uranifère sous la forme d'uraninite, d'urano titanates et/ou de phospho silicates à U, Ti, Zr, Y. Dans le cas des schistes noirs paléoprotérozoïques de Talvivaara (Finlande), le métamorphisme de faciès amphibolite a provoqué la remobilisation de l'uranium synsédimentaire et la cristallisation synmétamorphique, pendant l'orogénèse svécofennienne à 1880 1870 Ma, de cristaux d'uraninite fréquemment inclus dans des nodules carbonés. Cette étude montre que l'uranium, préconcentré au moment de la sédimentation, reste immobile pendant les premiers stades d'enfouissement mais est remobilisé dans les conditions P T croissantes et cristallise sous forme d'oxydes d'uranium pouvant évoluer vers des (phospho-)silicates d'uranium
In many metallic deposits, especially in sedimentary context and particularly in black shales, spatial or genetic relationships are described between organic matter and metals. Several black shales/schists affected by increasing thermo barometric conditions were selected to study the behavior and fate of uranium from sedimentation to high grade metamorphism. In shallow buried cambro ordovician Alum Shales (Sweden), uranium is dispersed and is not detectable as a particular mineralogical expression. Thermal maturation of the Alum Shales and hydrocarbon generation did not cause any identifiable remobilization of primary concentration, since migrated hydrocarbons did not carry uranium. In contrast, greenschist facies metamorphism associated with the Caledonian orogeny resulted in a re expression of uranium mineralization as uraninite or urano titanate crystals, which may evolve into U Ti Zr Y phospho silicates. In the case of Talvivaara, amphibolite facies metamorphism caused remobilization of synsedimentary uranium and synmetamorphic crystallization, during Svecofennian orogeny at 1880 1870 Ma, of uraninite crystals that are frequently included in carbonaceous nodules. This study shows that uranium, which is preconcentrated during sedimentation, remains immobile in the early stages of burial but is remobilized with increasing PT conditions and crystallizes as uranium oxides and/or uranium (phospho-)silicates

Ce travail de thèse s'est intéressé aux effets de l'uranium appauvri (U) sur le poisson zèbre, Danio rerio. L'hypothèse de travail majeure est que les effets de l'U peuvent se traduire par des modifications du métabolisme. Par conséquent nous avons caractérisé la performance physiologique par le biais de la théorie des bilans d'énergie dynamique (DEB) car c'est la seule théorie qui quantifie simultanément l'ingestion, l'assimilation, la croissance, la reproduction, la maturation, la maintenance et le vieillisse¬ment au cours du cycle de vie entier à des niveaux de nourriture variable. Un modèle DEB a ainsi été construit et a permis de quantifier et de prédire la manière dont la performance physiologique du poisson zèbre dépend de son niveau de nutrition (et de la température). Nous avons montré que le développement s'accélère après la naissance jusqu'à la métamorphose où l'accélération cesse. De plus les coûts de maintenance somatique sont très élevés.Un module spécifiant la toxico-cinétique de l'U, chez un individu qui se nourrit, croit et se reproduit, a été incorporé dans le modèle DEB. Le modèle a été appliqué aux données de toxicité (publiés et acquis pendant la thèse) afin de découvrir quel processus est affecté par l'U. Les résultats montrent qu'à partir de 0 nM, l'U augmenterait les coûts de croissance et diminuerait l'assimilation et/ou augmenterait le coût de la maintenance somatique. Nous n'avons pas pu détecter d'effets notables sur la maturation. Une étude histologique révèle que l'U altère l'intégrité de la paroi intestinale et pourrait perturber l'homéostasie des interactions hôte-bactéries
The aim of this dissertation is to characterize the toxicity of depleted uranium (U) on the metabolism of zebrafish, Danio rerio. The underlying hypothesis of this work is that effects of U show up as effects on the metabolism of the individual. Consequently, we characterized physiological performance using Dynamic Energy Budget (DEB) theory since it is the only theory which simultaneously specifies ingestion, assimilation, growth, reproduction, maturation, maintenance and ageing over the whole life-cycle at varying food availability. Thus a DEB model was built which quantifies and predicts how the physiological performance of zebrafish relates to food level (and temperature). We showed that development accelerates after birth until metamorphosis after which acceleration ceases. Furthermore, somatic maintenance costs are very high.A module specifying toxico-kinetics of U in a feeding, growing and reproducing individual was incorporated into the DEB model. The model was then applied to toxicity data (from the literature or acquired during this thesis) in order to determine which processes are affected by U. Our results show that, from 0 nM onwards, U increases costs for growth and either increases somatic maintenance or decreases assimilation. We were unable to detect effects on maturation. A histological study showed that U alters histology of the gut wall and may perturb host-microbe homeostasis. By accounting for differences in initial conditions between individuals we were able to explain a number of seemingly contradictory results. The take home message is: observations on individuals should not be averaged for groups of individuals

L'objectif de ces travaux de thèse était de caractériser la toxicité de l'uranium sur le métabolisme du poisson zèbre, Danio rerio. Puisque les effets de l'uranium se traduisent par des modifications de la performance du métabolisme, la question suivante se pose: que savons-nous du métabolisme du poisson zèbre témoin? Très peu de chose. En effet, nos connaissances à ce sujet sont assez limitées en dépit d'un grand nombre de travaux sur le développement de ce poisson. C'est pourquoi les trois premiers chapitres de ce manuscrit sont dédiés à la caractérisation du métabolisme témoin du Danio. J'ai utilisé la théorie des bilans d'énergie dynamique (DEB) pour procéder à cette caractérisation; à l'heure actuelle c'est la seule théorie qui quantifie l'ingestion, l'assimilation, la croissance, la reproduction, la maturation, la maintenance et le vieillissement pendant le cycle de vie entier d'un organisme. L'effet de l'uranium sur l'organisme implique un effet sur au moins une des processus cités ci-avant. Étant donné que la longévité du poisson zèbre est d'environ quatre ans et demi, et que l'intensité des effets liés à un stress chimique est inversement proportionnel à la taille, nous avons centré nos efforts sur les stades de vie précoces (embryon, juvénile et reproduction adulte). De surcroît, les stades de vies précoces semblent plus sensibles aux effets de l'uranium surtout au niveau des effets sur la croissance.

D'importants progrès ont été réalisés dans le domaine de la quantification du développent, de la croissance et de la reproduction du poisson zèbre. Il s'est avéré que le poisson zèbre accélère son développent après la naissance (c'est-à-dire l'instant où l'individu commence à se nourrir), jusqu'à la métamorphose, où l'accélération cesse. Ce processus a été constaté chez d'autre espèces de poissons, mais pas toutes. Une autre conclusion surprenante était que la maintenance somatique est beaucoup plus élevée que la valeur typique d'un poisson. Nous n'arrivons pas encore à expliquer pourquoi. De plus nous avons découvert que les détails sur la physiologie reproductive sont importants pour caractériser les effets de l'uranium: chez l'adulte les ressources allouées à la reproduction sont stockées dans un compartiment où siègent les processus de préparation de "batch " d'œufs (=buffer de reproduction). Il est donc important de comprendre ce processus pour comprendre comment le poisson zèbre élimine l'uranium via les œufs.

La théorie DEB spécifie que l'individu atteint un stade de développement à un niveau de maturité donné. Selon la température et/ou la nourriture, ce niveau de maturité peut être atteint à des tailles ou des âges différents. Nous avons élargi le concept pour inclure tous les stades de développement (définis sur la base de critères morphologiques) publiés dans les atlas de développement. Ce travail nous a permis d'expliquer par la théorie DEB à présent la variabilité en termes de taille et d'âge.

Dans le but de tester si la théorie DEB peut expliquer des perturbations au niveau de la maturation, nous avons étudié le développement de deux espèces de grenouilles taxonomiquement proches et de taille similaires. Une des espèces possède un développement typique comprenant un stade embryonnaire, un stade têtard qui se nourrit et puis un stade juvénile avec la morphologie typique d'une grenouille. Par contre la deuxième espèce témoigne d'une accélération du développement après l'éclosion mais avant la naissance- qui correspond au stade de développement où l'individu commence à se nourrir. Cette accélération est trahie par une augmentation de la respiration et un retard de la croissance avec au final une diminution de la taille à chaque stade de développement par rapport à la première espèce. Cette accélération s'estompe après la métamorphose (le moment où les jeunes grenouilles quittent l'eau). Toutes les différences entre les deux types de développement ont été expliquées par la théorie DEB en considérant qu'un seul paramètre changeait temporairement de valeur: la fraction de la réserve mobilisée vers la croissance et la maintenance somatique. La conclusion est que les perturbations observées au niveau de la maturation et de la variabilité de l'âge et la taille entre les différents stades de développement soutiennent empiriquement la façon que la théorie DEB incorpore la maturation.

Non seulement notre étude requérait une quantification détaillée de la maturation, mais elle requérait aussi la prise en compte de périodes (prolongées) de jeune, et ce plus particulièrement pour les stades précoces. Selon la théorie DEB la maintenance est alimentée avec l'énergie mobilisée de la réserve. Dès lors que la nourriture devient rare ou disparait cette dernière ne suffit plus pour alimenter la maintenance somatique. Nous avons détaillé ce cas de figure en modélisant le lien entre les processus de rajeunissement et d'amaigrissement extrême et la probabilité de survie. Les prédictions du modèle sont en accord avec les trajectoires de survie de larves obtenues en conditions de laboratoire. Certaines poissons libèrent plus d'un million d'œufs par événement de ponte et pourtant, si la dynamique de la population est stable, à chaque génération chaque poisson n'est remplacé que par un seul individu. Le processus de survie des larves représente une grande énigme irrésolue dans le domaine de la dynamique de populations de poisson.

Par le biais de ces travaux de doctorat, nous disposons à présent d'un outil permettant de comprendre, et de prédire, la manière dont la performance physiologique du poisson zèbre dépend de son niveau de nutrition. Le modèle a été utilisé pour détecter les modifications induites par l'uranium sur la performance physiologique d'un individu exposé par rapport à celle du témoin. A cette fin, nous avons développé un modèle dynamique qui spécifie la manière dont l'uranium s'accumule et s'élimine chez un individu qui se nourrit, grandit et se reproduit. Nous avions imaginé que l'uranium pourrait affecter le système immunitaire ainsi que d'autres mécanismes de défense cellulaire (e.g. système antioxydant). Selon la théorie DEB, l'allocation des ressources à la maturation comprend une fraction fixe de la réserve mobilisée auquel est soustrait le coût de maintenance de la maturité. Notre idée est que les coûts du système immunitaire et de défense cellulaire contribuent à la maintenance de la maturité. Si l'uranium augmentait les coûts de ce dernier alors la maturation ralentira, ainsi j'ai porté une attention soutenu aux taux de maturation.

Nous avons montré que l'uranium altère l'histologie de la paroi intestinale (acteur majeure dans l'assimilation des nutriments) et pourrait potentiellement modifier l'homéostasie des interactions hôte-bactérienne (acteur majeur dans l'assimilation et l'immunité inné). De plus nos travaux suggèrent que l'uranium augmenterait les coûts de synthèse de la structure et diminuerait l'assimilation et/ou augmenterait le coût de la maintenance somatique. Chose étonnante, malgré ce que nous pensions, nous n'avons pas pu détecter d'effets notables sur la maturation à ces faibles concentrations. Puisque la maturation interagit avec la croissance, la reproduction et la maintenance, je considère néanmoins que les travaux que j'ai pu mener sur la maturation sont pertinents. La toxicité de l'uranium est telle que les effets sur le coût de la synthèse de la structure et de la maintenance somatique sont estimés proches de 0 nM d'uranium dans l'eau.

Un résultat très important se dégageant de ces travaux est que la condition des poissons (structure, maturité, réserve, buffer de reproduction, stade de préparation des "batch") au début de l'expérience dépend de l'individu et conditionne la réponse de celui-ci au stress pendant (toute) l'expérience. Ce problème s'aggrave lorsque nous travaillons avec des poissons zèbres adultes car la contribution de la masse du buffer de reproduction par rapport à la masse totale diffère de manière important entre chaque individu. Ceci affecte alors non seulement les trajectoires de masse dans le temps, mais aussi la concentration interne, car la reproduction représente une voie importante d'élimination de l'uranium. La quantité totale de réserve (à savoir : réserve + buffer de reproduction) conditionne la sévérité de l'effet toxique contribuant ainsi à la variabilité dans les données. En prenant en compte les différences entre les conditions initiales de chaque individu, j'ai pu expliquer les résultats contradictoires publiés dans la littérature ainsi qu'expliquer mes propres résultats sur les effets de l'uranium. La leçon à retenir est que des données acquises sur des individus ne devraient pas être moyennées sur des groupes d'individus.

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Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq)
A demanda por combustível nuclear para reatores de pesquisa está aumentando em nível mundial, enquanto várias de suas fábricas têm pequeno volume de produção. Este trabalho estabeleceu um modelo conceitual com duas estratégias para o aumento da capacidade produtiva dessas fábricas. Foram abordadas as fábricas que produzem elementos combustíveis tipo placa carregados com LEU U3Si2-Al, tipicamente usados em reatores nucleares de pesquisa. A primeira estratégia baseia-se na literatura da área de administração da produção e é uma prática frequente nas fábricas em geral. A segunda estratégia aproveita a possibilidade de desmembrar setores produtivos, comum em instalações de produção de combustível nuclear. Ambas as estratégias geraram diferentes cenários de produção, os quais devem ser seguros em relação à criticalidade. Foram coletados dados de uma fábrica real de combustível nuclear para reatores de pesquisa. As duas estratégias foram aplicadas a esses dados com a finalidade de testar o modelo proposto, o que configurou um estudo de caso. A aplicação das estratégias aos dados coletados deu-se por meio de simulação de eventos discretos em computador. Foram criados diversos modelos de simulação para abranger todos os cenários gerados, de forma que o teste indicou um aumento da capacidade produtiva de até 207% sem necessidade de aquisição de novos equipamentos. Os resultados comprovam que o modelo atingiu plenamente o objetivo proposto. Como principal conclusão pode-se apontar a eficácia do modelo proposto, fato que foi validado pelos dados da fábrica.
Tese (Doutorado em Tecnologia Nuclear)
IPEN/T
Instituto de Pesquisas Energéticas e Nucleares - IPEN-CNEN/SP
CNPq:310274/2012-5

Cette thèse consiste en une étude préparatoire de la mesure du rapport alpha de l'233U entre 1eV et 10keV, facteur nécessaire pour calculer le pouvoir de régénération de réacteurs basés sur le cycle 232Th/233U. Cette mesure peut être effectuée au LPSC, sur la plateforme PEREN qui est composée d'un spectromètre à temps de ralentissement au plomb couplé à un GEnérateur de NEutrons Pulsé Intense (GENEPI). Les taux de capture et de fission sont mesurés grâce à 8 scintillateurs YAP utilisés en coïncidence et entourant une chambre à fission. Des mesures préliminaires sur l'235U ont présenté un rapport signal sur bruit très faible malgré les améliorations successives apportées. Les contributions du bruit de fond ont été comprises et quantifiées expérimentalement et via des simulations (MCNP et GEANT4). Il est cependant indispensable d'améliorer le rapport signal sur bruit d'au moins un ordre de grandeur pour obtenir la capture d'un élément fissile sur un tel dispositif expérimental.

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Dissertacao (Mestrado)
IPEN/D
Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Cette thèse consiste en une étude préparatoire de la mesure du rapport alpha de l'233U entre 1eV et 10keV, facteur nécessaire pour calculer le pouvoir de régénération de réacteurs basés sur le cycle 232Th/233U. Cette mesure peut être effectuée au LPSC, sur la plateforme PEREN qui est composée d'un spectromètre à temps de ralentissement au plomb couplé à un GEnérateur de NEutrons Pulsé Intense (GENEPI). Les taux de capture et de fission sont mesurés grâce à 8 scintillateurs YAP utilisés en coïncidence et entourant une chambre à fission. Des mesures préliminaires sur l’235U ont présenté un rapport signal sur bruit très faible malgré les améliorations successives apportées. Les contributions du bruit de fond ont été comprises et quantifiées expérimentalement et via des simulations (MCNP et GEANT4). Il est cependant indispensable d’améliorer le rapport signal sur bruit d’au moins un ordre de grandeur pour obtenir la capture d’un élément fissile sur un tel dispositif expérimental
This Ph-D thesis was intended to prepare a precise measurement of the alpha ratio of 233U between 1eV and 10keV. This ratio is a key-parameter to calculate the breeding ratio of reactors based on the 232Th/233U cycle. This measurement would be performed, at the LPSC, on the experimental platform PEREN which is composed of a lead slowing-down time spectrometer associated with an intense pulsed neutron generator. Capture and fission rates are measured thanks to 8 scintillators YAP used in coincidence and surrounding a fission chamber. Preliminary tests using 235U resulted in a very low signal to background ratio despite the successive improvements. The different components of the background were identified and quantified experimentally and thanks to simulation tools (MCNP and GEANT4). Nevertheless, the signal to background ratio has still to be increased by about a factor 10 at least, to allow the measurement of the capture of a fissile element with such an experimental setup

Este trabalho apresenta uma nova metodologia, simples e de baixo custo, para quantificação direta de urânio em compostos do ciclo do combustível nuclear, baseada na espectroscopia no infravermelho com transformada de Fourier (FTIR), utilizando a técnica de pastilhamento em KBr. Diferentes matrizes foram utilizadas para o desenvolvimento e validação analítica: nitrato de uranilo complexado com TBP (UO2(NO3)2.2TBP) em fase orgânica e nitrato de uranilo (UO2(NO3)2) em fase aquosa. O método para matriz de urânio em fase orgânica (UO2(NO3)2.2TBP em hexano/incorporado em KBr) apresentou linearidade (r = 0,9980) dentro da faixa analítica de 0,20% 2,85% de urânio na pastilha de KBr, LD de 0,02% e LQ de 0,03%, exatidão com recuperações acima de 101,0%, robustez e precisão (DPR < 1,6%). O método para matriz de urânio em fase aquosa (UO2(NO3)2/incorporado em KBr) apresentou linearidade (r = 0,9900) dentro da faixa analítica de 0,14% 0,29% de urânio na pastilha de KBr, LD de 0,01% e LQ de 0,02%, exatidão com recuperações acima de 99,4%, robustez e precisão (DPR < 1,6 %). Amostras de processo do ciclo do combustível nuclear foram submetidas a avaliação intralaboratorial e os resultados foram comparados estatisticamente por outras técnicas: Espectrometria de Fluorescência de Raios-X (FRX) e gravimetria. Os testes estatísticos (t-Student e Fischer) indicaram que a técnica por FTIR e as de referência são equivalentes, demonstrando que a nova metodologia pode ser empregada com sucesso nas análises de rotina para o controle de qualidade dos compostos nucleares.
This work presents a low cost, simple and new methodology for direct quantification of uranium in compounds of the nuclear fuel cycle, based on Fourier Transform Infrared (FTIR) spectroscopy using KBr pressed discs technique. Uranium in different matrices were used to development and validation: UO2(NO3)2.2TBP complex (TBP uranyl nitrate complex) in organic phase and uranyl nitrate (UO2(NO3)2) in aqueous phase. The parameters used in the validation process were: linearity, selectivity, accuracy, limits of detection (LD) and quantitation (LQ), precision (repeatability and intermediate precision) and robustness. The method for uranium in organic phase (UO2(NO3)2.2TBP complex in hexane/embedded in KBr) was linear (r = 0.9980) over the range of 0.20% 2.85% U/ KBr disc, LD 0.02% and LQ 0.03%, accurate (recoveries were over 101.0%), robust and precise (RSD < 1.6%). The method for uranium aqueous phase (UO2(NO3)2/embedded in KBr) was linear (r = 0.9900) over the range of 0.14% 1.29% U/KBr disc, LD 0.01% and LQ 0.02%, accurate (recoveries were over 99.4%), robust and precise (RSD < 1.6%). Some process samples were analyzed in FTIR and compared with gravimetric and X-ray fluorescence (XRF) analyses showing similar results in all three methods. The statistical tests (t-Student and Fischer) showed that the techniques are equivalent. The validated method can be successfully employed for routine quality control analysis for nuclear compounds.

A detailed reactor core modeling of the LOVIISA-2 PWR and FORSMARK-3BWR was performed in the Serpent 2 Continuous Energy Monte-Carlocode.Both models of the reactors were completed but the approximations ofthe atomic densities of nuclides present in the core differedsignificantly.In the LOVIISA-2 PWR, the predicted atomic density for the nuclidesapproximated by Chebyshev Rational Approximation method (CRAM)coincided with the corrected atomic density simulated by the Serpent2 program. In the case of FORSMARK-3 BWR, the atomic density fromCRAM poorly approximated the data returned by the simulation inSerpent 2. Due to boiling of the moderator in the core of FORSMARK-3,the model seemed to encounter problems of fission density, whichyielded unusable results.The results based on the models of the reactor cores are significantto the FANCSEE Nuclear fuel cycle simulator, which will be used as adataset for the nuclear fuel cycle burnup in the reactors.
FANCSEE

Important geochemical and tectonic events in the Paleoproterozoic Era lay the foundation for the status and operation of the modern Earth, including the initial rise of atmospheric oxygen paving the path for animal evolution, and the emergence of modern plate tectonic processes leading to the amalgamation of the Canadian Shield (Laurentia). Rudimentary geological and geochronological documentation of Paleoproterozoic sedimentary basins is the foundation from which we can ask larger questions about geochemical changes or plate tectonic events on the evolving Earth, since those questions are largely answered by analyzing the sedimentary record. This thesis outlines the stratigraphy, detrital zircon U-Pb geochronology, elemental and isotopic geochemistry, and basin evolution of the Paleoproterozoic Penrhyn and Piling basins on the Rae craton in Arctic Canada, which record important tectonic and geochemical events on both a regional and global scale. The concentration of the redox-sensitive trace element, U, in seawater has not been constant throughout geologic time and is linked to changes in oceanic and atmospheric oxygen content. Secular variations in the record of U contents of shales and iron formations indicate that the redox state of the atmosphere-ocean system after the Great Oxidation Event (GOE) was more dynamic than previously thought. Trends towards lower oxygen content recorded after ~2.05 Ga in the middle Proterozoic suggest that oxygen level decreased. This is contrary to traditional models assuming unidirectional atmospheric oxygen rise throughout the Proterozoic. The data demonstrate the earliest signal of oxidative U cycling, manifested in 2.47 - 2.43 Ga iron formations, and show that oxygenation was a protracted process initiated shortly after the end of the Archean. It has been proposed that a global and long-lived magmatic and tectonic shutdown event from ~2.45 to 2.22 Ga played a causal role in the GOE, since it overlaps the time interval in which atmospheric oxygen initially rose on Earth. Coupled U-Pb, Hf, and O isotope data on magmatic and detrital zircon determine that plate tectonic processes continued to operate during this interval. It is argued instead that plate tectonic processes are necessary to promote conditions favorable for atmospheric oxygen to rise.

Dans le but d'étudier les possibilités de gestion avancée du plutonium dans les réacteurs actuels, 8 stratégies de multi-recyclage du plutonium dans des REP sont étudiées. Suite à des études à l'équilibre, il a été montré que, en utilisant des assemblages homogènes, l'utilisation du thorium ne permet pas de réduire les inventaires de plutonium en cycle à l'équilibre ni la production d'américium. En répartissant les différents types de combustibles au sein d'un même assemblage, certaines stratégies thoriées permettent cependant d'obtenir des inventaires et des productions d'américium inférieur aux meilleures stratégies utilisant uniquement le cycle uranium. Cependant dans tous les cas, le faible taux de conversion des combustibles thoriés en REP conduit à l'impossibilité de faire baisser la consommation de ressources de plus de quelques pour-cent par rapport aux stratégies sans thorium. Afin d'étudier la transition, une participation active au développement du code de scénario CLASS a eu lieu. Elle a aboutie à la simulation de deux scénarios parmi ceux étudiés à l'équilibre avec CLASS. Ces simulations ont montrées des écarts avec les scénarios simulés précédemment. Les causes majeures de ces écarts ont été identifiées et quantifiées
In order to study the possibility of advanced management of plutonium in existing reactors, 8 strategies for plutonium multi-recycling in PWRs are studied. Following equilibrium studies, it was shown that, by using homogeneous assemblies, the use of thorium cannot reduce the plutonium inventory of equilibrium cycle or production of americium. By distributing the different fuel types within the same assembly, some thoriated strategies allow however lower inventories and lower production americium best strategies using only the uranium cycle. However, in all cases, low fuel conversion theories in PWRs makes it impossible to lower resource consumption more than a few percent compared to strategies without thorium. To study the transition, active participation in development of the scenario code CLASS has been taken. It led to the two simulation scenarios among those studied in equilibrium with CLASS. These simulations have shown discrepancies with previously simulated scenarios. The major causes of these differences were identified and quantified

A breed-and-burn molten salt reactor (BBMSR) concept is proposed to address the Generation IV fuel cycle sustainability objective in a once-through cycle with low enrichment and no reprocessing. The BBMSR uses separate fuel and coolant molten salts, with the fuel contained in assemblies of individual tubes that can be shuffled and reclad periodically to enable high burnup. In this dual-salt configuration, the BBMSR may overcome several limitations of previous breed-and-burn (B$\&$B) designs to achieve high uranium utilisation with a simple, passively safe design. A central challenge in design of the BBMSR fuel is balancing the neutronic requirement of large fuel volume fraction for B$\&$B mode with the thermal-hydraulic requirements for safe and economically competitive reactor operation. Natural convection of liquid fuel within the tubes aids heat transfer to the coolant, and a systematic approach is developed to efficiently model this complex effect. Computational fluid dynamics modelling is performed to characterise the unique physics of the system and produce a new heat transfer correlation, which is used alongside established correlations in a numerical model. A design framework is built around this numerical model to iteratively search for the limiting power density of a given fuel and channel geometry, applying several defined temperature and operational constraints. It is found that the trade-offs between power density, core pressure drop, and pumping power are lessened by directing the flow of coolant downwards through the channel. Fuel configurations that satisfy both neutronic and thermal-hydraulic objectives are identified for natural, 5$\%$ enriched, and 20$\%$ enriched uranium feed fuel. B$\&$B operation is achievable in the natural and 5$\%$ enriched versions, with power densities of 73 W/cm$^3$ and 86 W/cm$^3$, and theoretical uranium utilisations of 300 $\mathrm{MWd/kgU_{NAT}}$ and 25.5 $\mathrm{MWd/kgU_{NAT}}$, respectively. Using 20$\%$ enriched feed fuel relaxes neutronic constraints so a wider range of fuel configurations can be considered, but there is a strong inverse correlation between power density and uranium utilisation. The fuel design study demonstrates the flexibility of the BBMSR concept to operate along a spectrum of modes ranging from high fuel utilisation at moderate power density using natural uranium feed fuel, to high power density and moderate utilisation using 20$\%$ uranium enrichment.

Microbial metal reduction contributes to biogeochemical cycling, and reductive precipitation provides the basis for bioremediation strategies designed to immobilize radionuclide contaminants present in the subsurface. Facultatively anaerobic ×-proteobacteria of the genus Shewanella are present in many aquatic and terrestrial environments and are capable of respiration on a wide range of compounds as terminal electron acceptor including transition metals, uranium and transuranics. S. putrefaciens is readily cultivated in the laboratory and a genetic system was recently developed to study U(VI) reduction in this organism. U(VI) reduction-deficient S. putrefaciens point mutant Urr14 (hereafter referred to as CCMB1) was found to retain the ability to respire several alternate electron acceptors. In the present study, CCMB1 was tested on a suite of electron acceptors and found to retain growth on electron acceptors with high reduction potential (E¡¬0) [O2, Fe(III)-citrate, Mn(IV), Mn(III)-pyrophosphate, NO3-] but was impaired for anaerobic growth on electron acceptors with low E¡¬0 [NO2-, U(VI), dimethyl sulfoxide, trimethylamine N-oxide, fumarate, ×-FeOOH, SO32-, S2O32-]. Genetic complementation and sequencing analysis revealed that CCMB1 contained a point mutation (H108Y) in a CcmB homolog, an ABC transporter permease subunit required for c-type cytochrome maturation in E. coli. The periplasmic space of CCMB1 contained low levels of cytochrome c and elevated levels of free thiol equivalents (-SH), an indication that redox homeostasis was disrupted. Anaerobic growth ability, but not cytochrome c maturation activity, was restored to CCMB1 by adding exogenous disulfide bond-containing compounds (e.g., cystine) to the growth medium. To test the possibility that CcmB transports heme from the cytoplasm to the periplasm in S. putrefaciens, H108 was replaced with alanine, leucine, methionine and lysine residues via site-directed mutagenesis. Anaerobic growth, cytochrome c biosynthesis or redox homeostasis was disrupted in each of the site-directed mutants except H108M. The results of this study demonstrate, for the first time, that S. putrefaciens requires CcmB to produce c-type cytochromes under U(VI)-reducing conditions and maintain redox homeostasis during growth on electron acceptors with low E¡¬0. The present study is the first to examine CcmB activity during growth on electron acceptors with widely-ranging E¡¬0, and the results suggest that cytochrome c or free heme maintains periplasmic redox poise during growth on electron acceptors with E¡¬0 < 0.36V such as in the subsurface engineered for rapid U(VI) reduction or anoxic environments dominated by sulfate-reducing bacteria. A mechanism for CcmB heme translocation across the S. putrefaciens cytoplasmic membrane via heme coordination by H108 is proposed.

Les réacteurs `a neutrons rapides refroidis au sodium `a cycle uranium 238/plutonium 239, dont la faisabilité technique a déj`a ´et´e ´eprouv´ee, permettent de s'affranchir du prob- lème des ressources d'uranium naturel en r´ealisant la r´eg´en´eration de l'´elément fissile du combustible. En outre, une gestion des déchets visant `a réduire la production et la ra- diotoxicité des actinides mineurs produits par le réacteur peut ˆetre mise en oeuvre en transmutant les AM en coeur (transmutation homog`ene). Une autre alternative pour min- imiser les d´echets est l'utilisation d'un autre couple fertile-fissile : le thorium 232 et l'ura- nium 233 (Th/U). La comparaison des deux cycles est men´ee sur les aspects neutroniques et la sˆuret´e et sur la production de d´echets, en utilisant un Monte Carlo ´evoluant. Con- cernant la radiotoxicit´e des d´echets, mˆeme si on ne d´egage pas v´eritablement d'avantages clairs pour un cycle ou l'autre, le cycle Th/U r´eduit la radiotoxicit´e durant les p´eriodes o`u elle est la plus ´elev´ee. La transmutation homog`ene r´eduit significativement, pour les deux cycles, la radiotoxicit´e des d´echets, de facteurs variables selon la p´eriode de temps consid- ´er´e. Toutefois, elle se fait au d´etriment d'une augmentation importante de l'inventaire des AM dans le coeur. Si l'on consid`ere la fin de jeu, l'inventaire du coeur du r´eacteur devient alors un d´echet. Le gain apport´e par la transmutation, en prenant en compte `a la fois la radiotoxicit´e du coeur et des d´echets cumul´es, sera quantifi´e, et montre que la transmuta- tion n'offre pas de gain consid´erable si l'incin´eration des ´el´ements fissiles principaux (Pu ou U selon le cycle) n'est pas mise en oeuvre lors de l'arrˆet de la fili`ere.

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.

Des etudes geochronologiques u-pb et geochimiques ont ete effectuees sur differentes formations ortho- et para derivees du sud-est du massif central. Les granites du mendic et des palanges, temoins directs du magmatisme cadomien, sont respectivement dates a 6039 ma et 54018 ma. Leur encaissant micaschisteux montre une evolution multiepisodique en accord avec les donnees u-pb obtenues sur les formations metasedimentaires et les leucogranites de la chaine varisque. Dans le gneiss de decazeville une composante crustale d'age indetermine est identifie, et l'evenement majeur correspond a la migmatisation hercynienne. Une discussion conjointe des donnees de bertholene geochronologiques et geochimiques de l'encaissant granitique et du gisement conduisent a admettre un lien genetique entre le magmatisme cadomien et les concentrations uraniferes spatialement liees a la discordance entre le socle des palanges et la couverture permo-carbonifere. Le mecanisme propose pour liberer l'uranium des phases minerales porteuses est la metamictisation combinee avec le facteur tectonique. Les premiers resultats de datation par dosage du xenon de mineraux uraniferes des gisements de bertholene, de lodeve et des pierres plantees confirment l'ensemble des evolutions proposees pour chacun de ces massifs

The West Pacific Warm Pool (WPWP) plays an important role in the global heat budget and global hydrologic cycle, so knowledge about its past variability would improve our understanding of global climate. Variations in WPWP precipitation are most notable during El Niño-Southern Oscillation events, when climate changes in the tropical Pacific impact rainfall not only in the WPWP, but around the globe. The stalagmite records presented in this dissertation provide centennial-to-millennial-scale constraints of WPWP precipitation during three distinct climatic periods: the Last Glacial Maximum (LGM), the last deglaciation, and the Holocene. In Chapter 2, the methodologies associated with the generation of U/Th-based absolute ages for the stalagmites are presented. In the final age models for the stalagmites, dates younger than 11,000 years have absolute errors of ±400 years or less, and dates older than 11,000 years have a relative error of ±2%. Stalagmite-specific 230Th/232Th ratios, calculated using isochrons, are used to correct for the presence of unsupported 230Th in a stalagmite at the time of formation. Hiatuses in the record are identified using a combination of optical properties, high 232Th concentrations, and extrapolation from adjacent U/Th dates. In Chapter 3, stalagmite oxygen isotopic composition (d18O) records from N. Borneo are presented which reveal millennial-scale rainfall changes that occurred in response to changes in global climate boundary conditions, radiative forcing, and abrupt climate changes. The stalagmite d18O records detect little change in inferred precipitation between the LGM and the present, although significant uncertainties are associated with the impact of the Sunda Shelf on rainfall d18O during the LGM. A millennial-scale drying in N. Borneo, inferred from an increase in stalagmite d18O, peaks at ~16.5ka coeval with timing of Heinrich event 1, possibly related to a southward movement of the Intertropical Convergence Zone (ITCZ). An inferred precipitation maximum (stalagmite d18O minimum) during the mid-Holocene in N. Borneo supports La Niña-like conditions and/or a southward migration of the ITCZ over the course of the Holocene as likely mechanisms for the observed millennial-scale trends. In Chapter 4, stalagmite Mg/Ca, Sr/Ca, and d13C records reflect hydrologic changes in the overlying karst system that are linked to a combination of rainfall variability and cave micro-environmental effects. Dripwater and stalagmite geochemistry suggest that prior calcite precipitation is a mechanism which alters dripwater geochemistry in slow, stalagmite-forming drips in N. Borneo. Stalagmite Mg/Ca ratios and d13C records suggest that the LGM climate in N. Borneo was drier and that ecosystem carbon cycling may have responded to the drier conditions. Large amplitude decadal- to centennial-scale variability in stalagmite Mg/Ca, Sr/Ca and d13C during the deglaciation may be linked to deglacial abrupt climate change events.

Différents corps métamorphiques et magmatiques dans leLlimousin et dans les Pyrénées orientales ont été datés par la méthode u/pb à la microsonde ionique et 4 0ar/ 3 9ar sur monograin. Les résultats permettent d'avancer de nouvelles idées sur l'évolution orogénique de ces segments de la chaîne varisque. 1. Pyrénées orientales. L'orthogneiss de canigou-caranca a été daté par la méthode u/pb à la microsonde ionique sur zircons selectionnes. Les âges 2 0 6pb/ 2 3 8u des trois echantillons analyses varient entre 460 et 500 ma. Cet âge invalide le modèle classique de disposition en socle et couverture des séries métamorphiques. 2. Limousin. Le protolithe de la leptynite de vergonzac qui fait partie de l'unité supérieure des gneiss, a été daté à 525 6 ma (u/pb sur zircons a la microsonde ionique). Cet âge est compatible avec les âges des autres unités métamorphiques du Limousin. La mise en place du leucogranite péralumineux de blond a été datée à 319 7 ma (u/pb sur zircons a la microsonde ionique). Les âges 4 0ar/ 3 9ar sur muscovites de cette intrusion varient entre 311 et 306 ma. Ils sont interprétés non pas comme des âges de refroidissement, mais comme caractérisant une activite magmatique et hydrothermale importante. Les granitoides sous couverture du seuil du Poitou ont donné des âges 4 0ar/ 3 9ar sur biotites et amphiboles entre 350 et 345 ma. Une modélisation numérique a permis de les interpréter en termes de refroidissement et d'exhumation. Les minéralisations a w et sn de moulin-barret et de puy-les-vignes ont fourni des âges de 324 ma, ce qui implique l'existance d'un épisode de minéralisations au namurien. Une synthèse de tous les résultats permet de proposer une exhumation et une extension tardi-orogenique précoce, respectivement vers 340 ma et 320 ma. 3. Méthodologie. Quelques réflexions sur la calibration des analyses u/pb à la microsonde ionique sont proposées. La forme des spectres d'âge 4 0ar/ 3 9ar, leur signification en termes d'âge et l'interprétation des âges 4 0ar/ 3 9ar sont abordées.

Robust and reliable quantitative proliferation resistance assessment tools are critical to a strengthened nonproliferation regime and to the future deployment of nuclear fuel cycle technologies. Efforts to quantify proliferation resistance have thus far met with limited success due to the inherent subjectivity of the problem and interdependencies between attributes that contribute to proliferation resistance. This work focuses on the diversion of nuclear material by a state and defers other threats such as theft or terrorism to future work. A new approach is presented that assesses the problem through four stages of proliferation: the diversion of nuclear material, the transportation of nuclear material from an internationally safeguarded nuclear facility to an undeclared facility, the transformation of material into a weapons-usable metal, and weapon fabrication. A complete and concise set of intrinsic and extrinsic attributes of the nation, facility and material that could impede proliferation are identified. Quantifiable inputs for each of these attributes are defined. For example, the difficulty of handling the diverted material is captured with inputs like mass and bulk, radiation dose, heating rate and others. Aggregating these measurements into an overall value for proliferation resistance can be done in multiple ways based on well-developed decision theory. A preliminary aggregation scheme is provided along with results obtained from analyzing a small spent fuel reprocessing plant to demonstrate quantification of the attributes and inputs. This quantification effort shows that the majority of the inputs presented are relatively straightforward to work with while a few are not. These few difficult inputs will only be useful in special cases where the analyst has access to privileged, detailed or classified information. The stages, attributes and inputs of proliferation presented in this work provide a foundation for proliferation resistance assessments which may use multiple types of aggregation schemes. The overall results of these assessments are useful in comparing nuclear technologies and aiding decisions about development and deployment of that technology.

The sintering behavior of uranium and uranium-zirconium alloys in the alpha phase were characterized in this research. Metal uranium powder was produced from pieces of depleted uranium metal acquired from the Y-12 plant via hydriding/dehydriding process. The size distribution and morphology of the uranium powder produced by this method were determined by digital optical microscopy. Once the characteristics of the source uranium powder were known, uranium and uranium-zirconium pellets were pressed using a dual-action punch and die. The majority of these pellets were sintered isothermally, first in the alpha phase near 650°C, then in the gamma phase near 800°C. In addition, a few pellets were sintered using more exotic temperature profiles. Pellet shrinkage was continuously measured in situ during sintering. The isothermal shrinkage rates and sintering temperatures for each pellet were fit to a simple model for the initial phase of sintering of spherical powders. The material specific constants required by this model, including the activation energy of the process, were determined for both uranium and uranium-zirconium. Following sintering, pellets were sectioned, mounted, and polished for imaging by electron microscopy. Based on these results, the porosity and microstructure of the sintered pellets were analyzed. The porosity of the uranium-zirconium pellets was consistently lower than that of the pure uranium pellets. In addition, some formation of an alloyed phase of uranium and zirconium was observed. The research presented within this thesis is a continuation of a previous project; however, this research has produced many new results not previously seen. In addition, a number of issues left unresolved by the previous project have been addressed and solved. Most notably, the low original output of the hydride/dehydride powder production system has been increased by an order of magnitude, the actual characteristics of the powder have been measured and determined, shrinkage data was successfully converted into a sintering model, an alloyed phase of uranium and zirconium was produced, and pellet cracking due to delamination has been eliminated.

A family of top-down statistical models describing energy consumption in the mining, milling, and refining of uranium are formulated. The purpose of the models is to estimate the energy-to-grade dependence for uranium extraction, while defining a minimum grade that can be feasibly mined and produced. The results serve as a basis for understanding the factors governing energy consumption in the production of U3O8. The models are applied to a considerably larger data set of operating mines than in any previous effort. In addition, the validity of the modeling approach is established by modeling energy for two other commodities, gold and copper, thereby showing it can be applied to other metals. Statistical measures of explanatory power show that the models the energy-to-grade relationship is well-described for both uranium and gold. For copper, there was insufficient data over a broad range of ore grades to obtain a model that passed statistical confidence measures. The results show that mining of lower-grade deposits of uranium is likely to be less energy-intensive than previous investigators concluded. It is shown that the uncertainty in the results is dominated by the contribution of the grade-independent component of energy consumption.
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This thesis presents a detailed study of life cycle greenhouse gas (GHG) emissions intensity during the uranium mining-milling phase of the nuclear fuel cycle for three paired uranium mine-mill operations in northern Saskatchewan (SK). The study period runs from 2006 – 2013 for two of the three pairs, and from 1995-2010 for the third. The life cycle analysis has been conducted based on the ISO 14040:2006 standard using a Process Chain Analysis methodology. This study differs from previous studies of GHG emissions intensity during the uranium mining-milling phase of the nuclear fuel cycle in two key respects. First, it has a very large system boundary which includes the uranium exploration and mine-mill decommissioning phases. Second, it utilizes a life cycle inventory database to include many processes which would normally fall outside of the system boundary due to their small individual contributions. These differences contribute to a more accurate result. The production-weighted average life cycle GHG emissions intensity is estimated as 45 kg CO2e/kg U3O8 at an average ore grade of 9.12% U3O8 based on relative U3O8 production volumes at Mine-Mill A, B, and C from 2006 to 2010. The 95% confidence interval for the production-weighted average result ranges from 42 to 49 kg CO2e/kg U3O8, indicating that overall uncertainty in the result is low. Life cycle GHG emission intensity for the three uranium mine-mill pairs are 84, 66, and 35 kg CO2e/kg U3O8 at average ore grades of 0.71%, 1.54%, and 11.5% U3O8 respectively. Nearly 90% of life cycle GHG emissions are associated with operation of the uranium mine-mills, primarily from energy consumption during operation (69% of total) transport of materials and personnel (7.0%), and use of reagents (5.6%). Remaining processes each individually account for less than 5% of the total. In calculating emissions from electricity consumption, the base-case emission intensities reported above use a province-wide electricity emission factor because the utility does not differentiate its emissions by region. However, the facilities included in this study are all located in Northern Saskatchewan, which is powered exclusively by hydropower. Application of a regional emission factor reduces the production-weighted average life cycle GHG emission intensity to 26 kg CO2e/kg U3O8 with a 95% confidence interval of 25 to 29 kg CO2e/kg U3O8. This represents a 42% reduction in life cycle GHG emission intensity from the base case. Due to the high uranium ore grades found in SK uranium deposits, life cycle GHG emissions intensity for uranium from SK is among the lowest in the world. Further, the life cycle GHG emission intensity estimate from uranium mining-milling in SK is a small (approximately 10%) contributor to the life cycle GHG emissions intensity from the nuclear fuel cycle for light water reactors overall, amounting to approximately 1.2 g CO2e/kWh electricity (0.6 g CO2e/kWh electricity calculated using the regional hydroelectric power source).

The comparison of nuclear facilities based on their barriers to nuclear material proliferation has remained a difficult endeavor, often requiring expert elicitation for each system under consideration. However, objectively comparing systems using a set of computable metrics to derive a single number representing a system is not, in essence, a nuclear nonproliferation specific problem and significant research has been performed for business models. For instance, Multi-Attribute Utility Analysis (MAUA) methods have been used previously to provide an objective insight of the barriers to proliferation. In this paper, the Proliferation Resistance Analysis and Evaluation Tool for Observed Risk (PRAETOR), a multi-tiered analysis tool based on the multiplicative MAUA method, is presented. It folds sixty three mostly independent metrics over three levels of detail to give an ultimate metric for nonproliferation performance comparison. In order to reduce analysts' bias, the weighting between the various metrics was obtained by surveying a total of thirty three nonproliferation specialists and nonspecialists from fields such as particle physics, international policy, and industrial engineering. The PRAETOR was used to evaluate the Fast Breeder Reactor Fuel Cycle (FBRFC). The results obtained using these weights are compared against a uniform weight approach. Results are presented for five nuclear material diversion scenarios: four examples include a diversion attempt on various components of a PUREX fast reactor cycle and one scenario involves theft from a PUREX facility in a LWR cycle. The FBRFC was evaluated with uranium-plutonium fuel and a second time using thorium-uranium fuel. These diversion scenarios were tested with both uniform and expert weights, with and without safeguards in place. The numerical results corroborate nonproliferation truths and provide insight regarding fast reactor facilities' proliferation resistance in relation to known standards.