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Espectrometria gama em elementos combustiveis tipo placa irradiadosZEITUNI, CARLOS A. 09 October 2014 (has links)
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06173.pdf: 6069998 bytes, checksum: 60ab3760f99f6d97fd52766b4d449ab5 (MD5) / Dissertacao (Mestrado) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP
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Medidas de seccoes de choque para reacoes de captura de neutrons no sup(57)Co, sup(137)Cs e sup(241)Am considerando a formacao de estados isomericosMAIDANA, NORA L. 09 October 2014 (has links)
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06881.pdf: 7889902 bytes, checksum: 7e22a20905b1e2b2ff4ed4439b25e2bb (MD5) / Tese (Doutoramento) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP
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Contribution à l'étude du relâchement des produits de fission hors de combustibles nucléaires en situation d'accident grave : effet de la pO2 sur la spéciation du Cs, Mo et Ba / Contribution to the study of fission products release from nuclear fuels in severe accident conditions : effect of the pO2 on Cs, Mo and Ba speciationLe Gall, Claire 16 November 2018 (has links)
Comprendre les mécanismes de spéciation des Produits de Fission (PF) dans le combustible nucléaire est un enjeu majeur pour pouvoir estimer précisément le terme source d’un accident grave. Parmi les nombreux PF créés, certains sont très réactifs et peuvent avoir un impact radiologique important en cas de relâchement dans l’atmosphère. C’est notamment le cas du césium (Cs), du molybdène (Mo) et du baryum (Ba). C’est dans ce contexte que s’inscrit le travail de thèse qui propose d’apporter des données expérimentales sur l’effet du potentiel oxygène sur la spéciation du Cs, du Mo et du Ba dans des combustibles nucléaires, à différents stades d’un accident grave.Une approche thermodynamique a été utilisée en support à l’interprétation des données expérimentales obtenues dans le cadre de ce travail. Deux types d’échantillons ont été étudiés: des combustibles MOX irradiés et des matériaux simulant un combustible UO2 à fort taux de combustion, obtenus par frittage à haute température (SIMFuel). Les échantillons ont été traités thermiquement dans des conditions représentatives d’un accident grave survenant dans un Réacteur à Eau Pressurisée (REP). Les conditions expérimentales ont couvert une gamme de température allant de 400°C à 2530°C et des potentiels oxygène situés entre -470 kJ.mol(O2)-1 et -100 kJ.mol(O2)-1. Les échantillons ont été caractérisés finement avant et après chaque traitement à l’aide de techniques complémentaires comme la microscopie optique et électronique, la microsonde et le SIMS dans le cas de l’irradié. Des mesures de XANES sur synchrotron ont été réalisées sur SIMFuel et ont conduit à des résultats importants en termes de spéciation des PF. Enfin, la technique de Spark Plasma Sintering (SPS) a été explorée avec succès pour la fabrication de SIMFuel contenant du Cs, du Mo et du Ba sous des formes chimiques représentatives d’un combustible REP en fonctionnement nominal.Ce travail a permis de mettre en évidence l’effet de la température en conditions oxydantes sur le comportement du combustible et des PF. Une oxydation du Mo, initialement présent sous forme métallique dans les inclusions blanches du combustible, en MoO2 a été observée dès 1000°C en conditions oxydantes. Une interaction entre le MoO2 formé et le Ba contenu dans la phase oxyde a eu lieu dans les mêmes conditions, menant à la formation de BaMoO4. Le potentiel oxygène joue aussi un rôle important dans le phénomène d’interaction pastille-gaine, en favorisant la diffusion des espèces en conditions oxydantes, diminuant ainsi la température de fusion du combustible. / In the nuclear community, it is a top priority to gain in-depth understanding of fission product (FP) speciation mechanisms occurring in nuclear fuel in order to precisely estimate the source term of a severe accident. Among the FP produced, some are highly reactive and may have a strong radiological impact if released into the environment. This is particularly the case of cesium (Cs), molybdenum (Mo) and barium (Ba). In this context, the objective of this study is to provide experimental data on the effect of the oxygen potential on Cs, Mo and Ba speciation in nuclear fuels at different stages of a severe accident.A thermodynamic approach was coupled with the experimental work to support the interpretation of experimental data. Two types of samples were studied in detail: irradiated MOX fuels and simulated high burn-up UO2 fuels produced through sintering at high temperature (SIMFuel). The samples were submitted to thermal treatments in conditions representative of a pressurised water reactor (PWR) severe accident. This approach made it possible to cover a temperature range from 400°C up to 2530°C and oxygen potentials from -470 kJ.mol(O2)-1 to -100 kJ.mol(O2)-1. The samples were characterized before and after each test using complementary techniques like OM, SEM, EPMA and SIMS in the case of irradiated fuels. XANES measurements using synchrotron radiation facilities were performed on SIMFuels and provided valuable results on FP speciation. Moreover, spark plasma sintering (SPS) was successfully investigated for the production of SIMFuel samples containing Cs, Mo and Ba in a chemical state representative of PWR fuel in normal operating conditions.This work highlighted the effect of oxidizing severe accident conditions on the fuel and FP behavior. Oxidation of Mo initially contained in the fuel’s metallic inclusions into MoO2 was observed to take place around 1000°C in oxidizing conditions. An interaction between MoO2 and the oxide phase containing Ba took place in the same conditions, leading to the formation of BaMoO4. The oxygen potential also plays an important role in fuel-cladding interactions, enhancing the diffusion of species in oxidizing conditions and lowering the temperature at which fuel melting occurs.
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Determinação de fatores de interferência de produtos de fissão do urânio na análise por ativação neutrônica / Determination of uranium fission products interference factors in neutron activation analysisRIBEIRO JUNIOR, IBERE S. 10 November 2014 (has links)
Submitted by Claudinei Pracidelli (cpracide@ipen.br) on 2014-11-10T11:38:41Z
No. of bitstreams: 0 / Made available in DSpace on 2014-11-10T11:38:41Z (GMT). No. of bitstreams: 0 / Dissertação (Mestrado em Tecnologia Nuclear) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP
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Couplage RMN et rayonnement synchrotron à haute température pour l’étude de fluorures fondus : application aux fluorures de zirconium / Coupling NMR with Synchrotron radiation at high temperature for the study of molten fluorides : applied to zirconium fluoridesMaksoud, Louis 14 October 2013 (has links)
Les fluorures fondus sont utilisés dans les Réacteurs à Sels Fondus tels que le réacteur non modéré, à neutrons rapides, MSFR où le sel fondu LiF-ThF4 joue le rôle du combustible et du liquide caloporteur. La formation des produits de fissions (PF) tels que les lanthanides, au cours du fonctionnement de ce réacteur, peut modifier les propriétés physicochimiques du bain fondu. Il est ainsi important de caractériser le bain fondu de point de vue structural et dynamique afin de remonter à ses propriétés. En raison des problèmes de radioactivité liés au thorium, et des conditions requises liées aux méthodes spectroscopiques utilisées, le système étudié dans ce manuscrit est le LiF-ZrF4-LaF3 (le zirconium et le lanthane étant des PF potentiels). L'approche développée dans cette thèse combine des mesures par spectroscopies RMN et EXAFS à 850 °C avec des simulations de dynamique moléculaire. Dans le bain fondu, nous avons montré la coexistence de complexes à base de zirconium et de lanthane de différentes coordinences, dont les proportions et les interactions dépendent de la composition. En fonction de la teneur en ZrF4, les espèces [ZrF7]3- majoritaires évoluent peu mais se connectent davantage via des fluors pontants. L’ajout de LaF3 au mélange stabilise la coordinence 7 autour du zirconium et tend à enrichir l’environnement du lanthane en fluors. Un ordre à moyenne portée s’établit entre les différents complexes à base de zirconium et de lanthane par l’intermédiaire des fluors pontants. La dynamique des espèces est ralentie en fonction de l’ajout de ZrF4 et LaF3. Nous avons noté un effet important sur la structure et la dynamique des espèces à partir de 10% mol. LaF3 ajouté au mélange. Les données obtenues par cette approche originale de la chimie du bain fondu dans le RSF en présence des PF, sont fondamentales pour améliorer la séparation de ces derniers et optimiser le procédé. / Molten fluorides are used in Molten Salt Reactors MSR such as the non moderated fast reactor MSFR, where the molten salt LiF-ThF4 is the fuel and the coolant. The formation of fission products (FP) such as lanthanides, during the reactor operation, possibly modifies the physicochemical properties of the melt. It is therefore important to characterize the melt from the structural and the dynamics point of view in order to determine its properties. Because of problems related to the radioactivity of thorium, as well as requirements related to spectroscopic methods, the system studied in this thesis is the LiF-ZrF4-LaF3 (zirconium and lanthanum are possible FP). The approach followed in this thesis combines measurements by NMR spectroscopy and EXAFS at 850 °C with molecular dynamics simulations. In the molten salt, we have shown the existence of zirconium and lanthanum complexes with different coordination numbers, whose proportions depend on the composition. Depending on the content of ZrF4, [ZrF7]3- species are dominant but change slightly and are further connected between each other’s via bridging fluorine. The addition of LaF3 to the mixture stabilizes the 7 coordination number around the zirconium and tends to enrich the environment of lanthanum with fluorides. A medium-range order is established between the various complexes containing zirconium and lanthanum due to bridging fluorine. Species dynamics is slower when the amount of either ZrF4 or LaF3 is higher. We noted a significant effect on the structure and dynamics of species starting 10 mol%. LaF3 added to the medium. The data obtained by this novel approach concerning the chemistry of the molten salt in MSR containing FP, are fundamental to improve the separation of these products and optimize the process.
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Determinação de fatores de interferência de produtos de fissão do urânio na análise por ativação neutrônica / Determination of uranium fission products interference factors in neutron activation analysisRIBEIRO JUNIOR, IBERE S. 10 November 2014 (has links)
Submitted by Claudinei Pracidelli (cpracide@ipen.br) on 2014-11-10T11:38:41Z
No. of bitstreams: 0 / Made available in DSpace on 2014-11-10T11:38:41Z (GMT). No. of bitstreams: 0 / A análise por ativação com nêutrons é um método utilizado na determinação de diversos elementos em diferentes tipos de matrizes. Entretanto, quando a amostra contém altos teores de U ocorre o problema de interferência devido aos produtos de fissão do isótopo 235U. Um dos métodos de tratar este problema é fazer a correção usando fatores de interferência devido à fissão do U para os radionuclídeos utilizados nas análises dos elementos. No presente estudo foram determinados os valores dos fatores de interferência devido à fissão do U para os radioisótopos 141Ce, 143Ce,140La, 99Mo, 147Nd, 153Sm e 95Zr no reator nuclear de pesquisas IEA-R1 do IPEN-CNEN/SP. Esses fatores de interferência foram determinados experimentalmente, por meio da irradiação dos padrões sintéticos em uma determinada posição do reator, e teoricamente, determinando a razão dos fluxos de nêutrons epitérmicos e térmicos na mesma posição onde os padrões sintéticos foram irradiados e utilizando parâmetros nucleares da literatura. Os fatores de interferência obtidos foram comparados com os valores reportados em outros estudos. Para avaliar esses fatores de interferência, eles foram aplicados em análises dos elementos alvo deste estudo, nos materiais de referência certificados NIST 8704 Buffalo River Sediment, IRMM BCR-667 Estuarine Sediment e IAEA-SL-1 Lake Sediment. / Dissertação (Mestrado em Tecnologia Nuclear) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP
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Study of Fission Products (Cs, Ba, Mo, Ru) behaviour in irradiated and simulated Nuclear Fuels during Severe Accidents using X-ray Absorption Spectroscopy, SIMS and EPMA / Etude du comportement des produits de fission (Ba, Cs, Mo et Ru) dans des combustibles nucléaires irradiés et leurs simulants en situations d’accidents graves par spectroscopie d’absorption des rayons X, SIMS et μsondeGeiger, Ernesto 14 January 2016 (has links)
L’identification des mécanismes de relâchement des Produits de Fission (PF) hors de combustible nucléaire irradié lors d’un accident grave est primordiale pour le développement de codes capables d’estimer précisément le terme source (nature et quantité des radionucléides émis dans l’environnement). Parmi les différents PF, les Ba, Cs, Mo et le Ru sont particulièrement intéressants, car ils peuvent interagir entre eux ou avec d’autres éléments et donc affecter leur relâchement. Dans le cadre de cette thèse, deux axes de travail ont été mis en place avec l’objectif d’identifier les phases chimiques présentes avant l’accident et leur évolution au cours de l’accident lui-même. L’approche expérimentale a consisté à reproduire les conditions d’un accident nucléaire à l’échelle du laboratoire, en utilisant des échantillons de combustibles irradiés et des matériaux modèles (UO₂ vierge dopés en 12 PF). Le principal avantage de ces derniers est l’utilisation de méthodes de spéciation chimique comme la Spectroscopie d’Absorption des rayons X, qui n’est pas aujourd’hui encore disponible pour les combustibles irradiés. Trois échantillons de combustible irradié ont été étudies, représentatifs de l’état initial (i.e. avant l’accident), d’une étape intermédiaire en température (1773K) et d’un état avancé d’accident nucléaire (2873K). Pour les matériaux modèles, plusieurs séquences accidentelles (de 573K à 1973K) ont été réalisés. Les résultats expérimentaux ont permis d’établir un nouveau mécanisme de relâchement des PF en en fonction des conditions oxydantes et réductrices du scénario accidentel. Ces résultats ont démontré aussi l’importance des matériaux modèles pour l’étude des accidents nucléaires graves, en complémentarité aux combustibles irradiés. / The identification of Fission Products (FP) release mechanism from irradiated nuclear fuels during a severe accident is of main importance for the development of codes for the estimation of the source-term (nature and quantity of radionuclides released into the environment). Among the many FP Ba, Cs, Mo and Ru present a particular interest, since they may interact with each other or other elements and thus affect their release. In the framework of this thesis, two work axes have been set up in order to identify, firstly, the chemical phases initially present before the accident and, secondly, their evolution during the accident itself. The experimental approach consisted in reproducing nuclear severe accidents conditions at laboratory scale using both irradiated fuels and model materials (natural UO₂ doped with 12 FP). The advantage of these latter is the possibility of using characterization methods such as X-ray Absorption Spectroscopy which are not available for irradiated fuels. Three irradiated fuel samples have been studied, representative to an initial state (before the accident), to an intermediate stage (1773K) and to an advanced stage (2873K) of a nuclear severe accident. Regarding to model materials, many accident sequences have been carried out, from 573 to 1973K. Experimental results have allowed to establish a new release mechanism, considering both reducing and oxidizing conditions during an accident. These results have also demonstrated the importance of model materials as a complement to irradiated nuclear fuels in the study of nuclear severe accidents.
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Fuel failure analysis in Boiling Water Reactors (BWR) using Machine Learning. : A comparison of different machine learning algorithms and their performance at predicting fuel failures.Borg, Sofia January 2024 (has links)
In collaboration with Westinghouse Electric AB this project aims to study the possibilities with using machine learning methods to predict fuel failure in a Boiling Water Reactors (BWRs). The main objective has been to create a dataset consisting of both empirical measurements and simulated samples from a physics model and evaluate different machine learning algorithms, that use these datasets to predict fuel defects. The simulated data is created using a physics model derived from the ANS-5.4 standard which allows for good control over specific parameter values. Three machine learning algorithms were deemed fit for this type of problem and used throughout the project: Random Forest (RF), K-Nearest Neighbor (KNN) and Neural Network (NN). Both classification and regression type problems have been assessed. All three methods showed good results for the classification problems, where the goal was to predict if there was a fuel failure or not. All models reached an accuracy above 97% and performed well, the RF model had the highest overall, with an accuracy of 98.2 %. However, the NN method made the fewest false negative predictions and can therefore be seen as the best model for this purpose. For the regression, problems with the aim of predicting escape rates, both the RF and KNN had similar promising results with very small errors overall. Yet, there is a slight increase in errors when predicting higher escape rates for both models. This is most likely due to the available data being of mostly low escape rates. The NN did not perform well with this problem, the predictions having large error for both low and high escape rates, a possible explanation is the lack of data. To improve the results, and create even better models, the empirical measurements need to contain more information such as defect location and fuel failure size, also an increase in the number of samples taken at fuel failure operation would be valuable.
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Studies of Accelerator-Driven Systems for Transmutation of Nuclear Waste / Studier av acceleratordrivna system för transmutation av kärnavfallDahlfors, Marcus January 2006 (has links)
<p>Accelerator-driven systems for transmutation of nuclear waste have been suggested as a means for dealing with spent fuel components that pose potential radiological hazard for long periods of time. While not entirely removing the need for underground waste repositories, this nuclear waste incineration technology provides a viable method for reducing both waste volumes and storage times. Potentially, the time spans could be diminished from hundreds of thousand years to merely 1.000 years or even less. A central aspect for accelerator-driven systems design is the prediction of safety parameters and fuel economy. The simulations performed rely heavily on nuclear data and especially on the precision of the neutron cross section representations of essential nuclides over a wide energy range, from the thermal to the fast energy regime. In combination with a more demanding neutron flux distribution as compared with ordinary light-water reactors, the expanded nuclear data energy regime makes exploration of the cross section sensitivity for simulations of accelerator-driven systems a necessity. This fact was observed throughout the work and a significant portion of the study is devoted to investigations of nuclear data related effects. The computer code package EA-MC, based on 3-D Monte Carlo techniques, is the main computational tool employed for the analyses presented. Directly related to the development of the code is the extensive IAEA ADS Benchmark 3.2, and an account of the results of the benchmark exercises as implemented with EA-MC is given. CERN's Energy Amplifier prototype is studied from the perspectives of neutron source types, nuclear data sensitivity and transmutation. The commissioning of the n_TOF experiment, which is a neutron cross section measurement project at CERN, is also described.</p>
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Studies of Accelerator-Driven Systems for Transmutation of Nuclear Waste / Studier av acceleratordrivna system för transmutation av kärnavfallDahlfors, Marcus January 2006 (has links)
Accelerator-driven systems for transmutation of nuclear waste have been suggested as a means for dealing with spent fuel components that pose potential radiological hazard for long periods of time. While not entirely removing the need for underground waste repositories, this nuclear waste incineration technology provides a viable method for reducing both waste volumes and storage times. Potentially, the time spans could be diminished from hundreds of thousand years to merely 1.000 years or even less. A central aspect for accelerator-driven systems design is the prediction of safety parameters and fuel economy. The simulations performed rely heavily on nuclear data and especially on the precision of the neutron cross section representations of essential nuclides over a wide energy range, from the thermal to the fast energy regime. In combination with a more demanding neutron flux distribution as compared with ordinary light-water reactors, the expanded nuclear data energy regime makes exploration of the cross section sensitivity for simulations of accelerator-driven systems a necessity. This fact was observed throughout the work and a significant portion of the study is devoted to investigations of nuclear data related effects. The computer code package EA-MC, based on 3-D Monte Carlo techniques, is the main computational tool employed for the analyses presented. Directly related to the development of the code is the extensive IAEA ADS Benchmark 3.2, and an account of the results of the benchmark exercises as implemented with EA-MC is given. CERN's Energy Amplifier prototype is studied from the perspectives of neutron source types, nuclear data sensitivity and transmutation. The commissioning of the n_TOF experiment, which is a neutron cross section measurement project at CERN, is also described.
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