Le formulaire de calcul DARWIN2.3, basé sur l’évaluation des données nucléaires JEFF-3.1.1, est dédié aux applications du cycle du combustible nucléaire. Il est validé expérimentalement pour le calcul du bilan matière par comparaison avec des mesures de rapports isotopiques réalisées sur des tronçons de combustibles irradiés en réacteur de puissance. Pour certains nucléides d’intérêt pour le cycle du combustible, la validation expérimentale montre que le calcul de la concentration en évolution pourrait être amélioré. C’est dans ce contexte que les travaux de thèse ont été menés : après s’être assuré que le biais Calcul / Expérience (C/E) est majoritairement dû aux données nucléaires, deux voies d’amélioration du calcul du bilan matière sont proposées et étudiées.La première voie d’amélioration s’attache à la ré-estimation des données nucléaires par assimilation des données intégrales. Elle consiste en l'assimilation des données provenant de la validation expérimentale du calcul du bilan matière avec DARWIN2.3 à l'aide du code d’évaluation des données nucléaires CONRAD. Des recommandations d’évolution d’évaluation, qui découlent de l’analyse de ces travaux, sont effectuées.La deuxième voie d’amélioration consiste à proposer de nouvelles expériences pour valider les données nucléaires impliquées dans la formation de nucléides pour lesquels on ne dispose pas d’expérience pour valider le calcul de la concentration avec DARWIN2.3. La faisabilité d’une expérience dédiée à la validation des sections efficaces des réactions de formation du 14C, à savoir 14N(n,p) et 17O(n,α), a été démontrée en ce sens. / The DARWIN2.3 calculation package, based on the use of the JEFF-3.1.1 nuclear data library, is devoted to nuclear fuel cycle studies. It is experimentally validated for fuel inventory calculation thanks to dedicated isotopic ratios measurements realized on in-pile irradiated fuel rod cuts. For some nuclides of interest for the fuel cycle, the experimental validation work points out that the concentration calculation could be improved. The PhD work was done in this framework: having verified that calculation-to-experiment (C/E) biases are mainly due to nuclear data, two ways of improving fuel inventory calculation are proposed and investigated. It consists on one hand in improving nuclear data using the integral data assimilation technique. Data from the experimental validation of DARWIN2.3 fuel inventory calculation are assimilated thanks to the CONRAD code devoted to nuclear data evaluation. Recommendations of nuclear data evaluations are provided on the basis of the analysis of the assimilation work. On the other hand, new experiments should be proposed to validate nuclear data involved in the buildup of nuclides for which there is no post-irradiation examination available to validate DARWIN2.3 fuel inventory calculation. To that extent, the feasibility of an experiment dedicated to the validation of the ways of formation of 14C, which are 14N(n,p) and 17O(n,α) reaction cross sections, was demonstrated.

Les études des scénarios électronucléaires modélisent le fonctionnement d’un parcnucléaire sur une période de temps donnée. Elles permettent la comparaison de différentesoptions d’évolution du parc nucléaire et de gestion des matières du cycle, depuis l’extraction duminerai jusqu’au stockage ultime des déchets, en se basant sur des critères tels que les puis-sances installées par filière, les inventaires et les flux, en cycle et aux déchets. Les incertitudessur les données nucléaires et les hypothèses de scénarios (caractéristiques des combustibles, desréacteurs et des usines) se propagent le long des chaînes isotopiques lors des calculs d’évolutionet au cours de l’historique du scénario, limitant la précision des résultats obtenus. L’objetdu présent travail est de développer, implémenter et utiliser une méthodologie stochastiquede propagation d’incertitudes dans les études de scénario. La méthode retenue repose sur ledéveloppement de métamodèles de calculs d’irradiation, permettant de diminuer le temps decalcul des études de scénarios et de prendre en compte des perturbations des paramètres ducalcul, et la fabrication de modèles d’équivalence permettant de tenir compte des perturbationsdes sections efficaces lors du calcul de teneur du combustible neuf. La méthodologie de calculde propagation d’incertitudes est ensuite appliquée à différents scénarios électronucléairesd’intérêt, considérant différentes options d’évolution du parc REP français avec le déploiementde RNR. / Nuclear scenario studies model nuclear fleet over a given period. They enablethe comparison of different options for the reactor fleet evolution, and the management ofthe future fuel cycle materials, from mining to disposal, based on criteria such as installedcapacity per reactor technology, mass inventories and flows, in the fuel cycle and in the waste.Uncertainties associated with nuclear data and scenario parameters (fuel, reactors and facilitiescharacteristics) propagate along the isotopic chains in depletion calculations, and throughoutthe scenario history, which reduces the precision of the results. The aim of this work isto develop, implement and use a stochastic uncertainty propagation methodology adaptedto scenario studies. The method chosen is based on development of depletion computationsurrogate models, which reduce the scenario studies computation time, and whose parametersinclude perturbations of the depletion model; and fabrication of equivalence model which takeinto account cross-sections perturbations for computation of fresh fuel enrichment. Then theuncertainty propagation methodology is applied to different scenarios of interest, consideringdifferent options of evolution for the French PWR fleet with SFR deployment.

Made available in DSpace on 2014-10-09T12:54:58Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:07:31Z (GMT). No. of bitstreams: 0 / Dissertacao (Mestrado) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Submitted by Claudinei Pracidelli (cpracide@ipen.br) on 2016-06-22T11:26:33Z No. of bitstreams: 0 / Made available in DSpace on 2016-06-22T11:26:33Z (GMT). No. of bitstreams: 0 / Tese (Doutorado em Tecnologia Nuclear) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

Made available in DSpace on 2014-10-09T12:54:58Z (GMT). No. of bitstreams: 0 / Made available in DSpace on 2014-10-09T14:07:31Z (GMT). No. of bitstreams: 0 / O processamento químico a partir do hexafluoreto de urânio (UF6), permite uma flexibilidade na produção de combustíveis à base de siliceto de urânio (U3Si2) e octóxido de urânio (U3O8). Atualmente no IPEN-CNEN/SP desenvolvem-se trabalhos visando o processamento de combustíveis com alta concentração de urânio, por meio da substituição do U3O8 por U3Si2. Para a obtenção de U3Si2, duas possibilidades podem ser consideradas na preparação da matéria-prima utilizada, que é o tetrafluoreto de urânio (UF4), são elas: a redução do urânio presente na solução hidrolisada do UF6 utilizando-se cloreto estanhoso (SnCl2) e a hidrofluoretação do dióxido de urânio (UO2) proveniente do tricarbonato de amônio e uranilo (TCAU). Descreve-se neste trabalho um procedimento para obtenção de tetrafluoreto de urânio (UF4), utilizando-se como matéria-prima os filtrados gerados na preparação de determinados compostos nos processos de reconversão do hexafluoreto de urânio (UF6), mais especificamente o amonioperóxidofluoranato (APOFU). Os filtrados consistem principalmente de uma solução contendo altas concentrações dos íons amônio (NH4 +), fluoreto (F-) e baixa concentração de urânio. O processo descrito visa principalmente a recuperação do NH4F e do urânio, como UF4, por meio da cristalização do bifluoreto de amônio (NH4HF2) e em uma etapa posterior, a adição deste ao UO2, ocorrendo a fluoração e decomposição. O UF4 obtido foi caracterizado química e fisicamente e será reciclado para ser usado na unidade de produção de urânio metálico para a obtenção de U3Si2, utilizado como combustível para o reator IEA-R1m. / Dissertacao (Mestrado) / IPEN/D / Instituto de Pesquisas Energeticas e Nucleares - IPEN/CNEN-SP

Submitted by Claudinei Pracidelli (cpracide@ipen.br) on 2016-06-22T11:26:33Z No. of bitstreams: 0 / Made available in DSpace on 2016-06-22T11:26:33Z (GMT). No. of bitstreams: 0 / 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. / Tese (Doutorado em Tecnologia Nuclear) / IPEN/T / Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

Les codes de simulation du cycle du combustible nucléaire sont des outils permettant d’évaluer les stratégies futures du cycle du combustible nucléaire et de comprendre la physique de ce cycle. Dans le contexte d’incertitude entourant l’évolution future du parc nucléaire français, notamment concernant le déploiement de Réacteurs à Neutrons Rapides au sodium (RNR-Na), la problématique de cette thèse est d’étudier des solutions alternatives de gestion du plutonium et des autres noyaux lourds, basées sur les Réacteurs à Eau Pressurisés (REP). Les stratégies étudiées s’appuient sur deux hypothèses. La première suppose un retard important dans le déploiement des RNR-Na, impliquant une stratégie d’attente visant à stabiliser l’inventaire en plutonium. La deuxième hypothèse suppose un abandon de la stratégie de déploiement des RNR. Dans ce cadre, une stratégie d’incinération du plutonium a été étudiée pour quantifier la capacité de réduction de l’inventaire par les REP. Le code de simulation CLASS, développé par le CNRS/IN2P3 et l’IRSN, est utilisé. Le multi-recyclage du plutonium en REP requiert un combustible dédié. Des développements ont été réalisés pour modéliser le combustible étudié, composé de MOX sur un support d'uranium enrichi. Une méthodologie innovante d’évaluation de scénarios nucléaires basée sur l’analyse globale de sensibilité a été appliquée. Cette méthode a permis d’identifier des scénarios de référence pour la stabilisation et la réduction de l’inventaire en plutonium et actinides mineurs. Des simulations du cycle détaillées ont été réalisées afin d'analyser la capacité des REP à gérer le plutonium à l’échelle du cycle. / Nuclear fuel cycle simulation codes are used to evaluate fuel cycle future strategies and understand the nuclear fuel cycle physics. In the context of uncertainty related to the future of French nuclear fleet, especially on theSodium Fast Reactor (SFR) deployment, the present work aims to study alternative solutions for plutonium and heavy isotopes management, based on Pressurized Water Reactor (PWR). Two hypothesis have been formulated to identify strategies. First, a delay has been expected in SFR deployment which induces a stabilization of plutonium inventory before SFR integration. The second hypothesis is based on the assumption that SFR won’t be deployed in France. For this specific case, a plutonium incineration strategy has been studied to quantify the PWR plutonium inventory reduction capacity. Fuel cycle simulations are performed using the fuel cycle simulator CLASS developed by the CNRS/IN2P3 in collaboration with IRSN. Plutonium multi-reprocessing in thermal reactor requires an innovative fuel. Developments have been made to simulate a fuel composed of MOX on enriched uranium support. An innovative methodology for fuel cycle simulation evaluation, based on Global Sensitivity Analysis, has been applied. This methodology leads to reference scenarios identification for plutonium and minor actinides inventories stabilization and reduction. Fuel cycle detailed simulations have been performed to produce fuel cycle data, to analyze PWR plutonium management at the cycle scale.

Ce travail de thèse s’inscrit dans le domaine de l’énergie nucléaire, de l’aval du cycle du combustible et du calcul des incertitudes. Le CEA doit concevoir le prototype ASTRID, réacteur à neutrons rapides refroidi au sodium (RNR), qui est l’un des concepts retenus au sein du forum Génération IV et dont la puissance résiduelle et l’estimation de son incertitude ont un impact important. Ce travail consiste à développer un code de propagation des incertitudes des données nucléaires sur la puissance résiduelle dans les RNR.La démarche s’est déroulée en trois temps.La première étape a permis de limiter le nombre de paramètres intervenant dans le calcul de la puissance résiduelle. Pour cela, un essai de puissance résiduelle sur le réacteur PHENIX (PUIREX 2008) a été interprété de façon à valider expérimentalement le formulaire d’évolution DARWIN pour les RNR et à quantifier les termes sources de la puissance résiduelle.La deuxième étape a eu pour but de développer un code de propagation des incertitudes : CyRUS (Cycle Reactor Uncertainty and Sensitivity). Une méthode de propagation déterministe a été retenue car elle permet des calculs rapides et fiables. Les hypothèses de linéarité et de normalité qu’elle entraîne ont été validées théoriquement. Le code a également été comparé avec succès à un code stochastique sur l’exemple de la fission élémentaire thermique de l’235U.La dernière partie a été une application du code sur des expériences de puissance résiduelle d’un réacteur, de bilan matière d’une aiguille combustible et d’une fission élémentaire de l’235U. Le code a démontré des possibilités de retour d’expériences sur les données nucléaires impactant l’incertitude de cette problématique.Deux résultats principaux ont été mis en évidence. Tout d’abord, les hypothèses simplificatrices des codes déterministes sont compatibles avec un calcul précis de l’incertitude de la puissance résiduelle. Ensuite, la méthode développée est intrusive et permet un retour d’expérience sur les données nucléaires des expériences du cycle. En particulier, ce travail a montré qu’il est déterminant de mesurer précisément les rendements de fission indépendants et de déterminer leurs matrices de covariances afin d’améliorer la précision du calcul de la puissance résiduelle. / This PhD study is in the field of nuclear energy, the back end of nuclear fuel cycle and uncertainty calculations. The CEA must design the prototype ASTRID, a sodium cooled fast reactor (SFR) and one of the selected concepts of the Generation IV forum, for which the calculation of the value and the uncertainty of the decay heat have a significant impact. In this study is developed a code of propagation of uncertainties of nuclear data on the decay heat in SFR.The process took place in three stages.The first step has limited the number of parameters involved in the calculation of the decay heat. For this, an experiment on decay heat on the reactor PHENIX (PUIREX 2008) was studied to validate experimentally the DARWIN package for SFR and quantify the source terms of the decay heat.The second step was aimed to develop a code of propagation of uncertainties : CyRUS (Cycle Reactor Uncertainty and Sensitivity). A deterministic propagation method was chosen because calculations are fast and reliable. Assumptions of linearity and normality have been validated theoretically. The code has also been successfully compared with a stochastic code on the example of the thermal burst fission curve of 235U.The last part was an application of the code on several experiments : decay heat of a reactor, isotopic composition of a fuel pin and the burst fission curve of 235U. The code has demonstrated the possibility of feedback on nuclear data impacting the uncertainty of this problem.Two main results were highlighted. Firstly, the simplifying assumptions of deterministic codes are compatible with a precise calculation of the uncertainty of the decay heat. Secondly, the developed method is intrusive and allows feedback on nuclear data from experiments on the back end of nuclear fuel cycle. In particular, this study showed how important it is to measure precisely independent fission yields along with their covariance matrices in order to improve the accuracy of the calculation of the decay heat.

In this thesis advanced fuel cycles for the incineration, i.e. deep–burn, of weapons–grade plutonium, reactor–grade plutonium from pressurised light water reactors and reactor–grade plutonium + the associated Minor Actinides in the 400 MWth Pebble Bed Modular Reactor Demonstration Power Plant was simulated with the VSOP 99/05 diffusion code. These results were also compared to the standard 9 g/fuel sphere U/Pu 9.6% enriched uranium fuel cycle. The addition of the Minor Actinides to the reactor–grade plutonium caused an unacceptable decrease in the burn–up and thus an unacceptable increase in the heavy metal (HM) content in the spent fuel, which is intended for direct disposal in a deep geological repository, without chemical reprocessing. All the Pu fuel cycles failed the adopted safety limits in that either the maximum fuel temperature of 1130°C, during normal operation, or the maximum power of 4.5 kW/sphere was exceeded. All the Pu cycles also produced positive Uniform Temperature Reactivity Coefficients, i.e. the coefficient where the temperature of the fuel and the graphite moderator in the fuel spheres are varied together. these positive temperature coefficients were experienced at low temperatures, typically below 700°C. This was due to the influence of the thermal fission resonance of 241Pu. The safety performance of the weapons–grade plutonium was the worst. The safety performance of the reactor–grade plutonium also deteriorated when the heavy metal loading was reduced from 3 g/sphere to 2 g or 1 g. In view of these safety problems, these Pu fuel cycles were judged to be not licensable in the PBMR DPP–400 reactor. Therefore a redesign of the fuel cycle for reactor–grade plutonium, the power conversion system and the reactor geometry was proposed in order to solve these problems. The main elements of these proposals are: v 1. The use of 3 g reactor–grade plutonium fuel spheres should be the point of departure. 232Th will then be added in order to restore negative Uniform Temperature Reactivity Coefficients. 2. The introduction of neutron poisons into the reflectors, in order to suppress the power density peaks and thus the temperature peaks. 3. In order to counter the reduction in burn–up by this introduction of neutron poisons, a thinning of the central reflector was proposed. / Thesis (PhD (Nuclear Engineering))--North-West University, Potchefstroom Campus, 2012.

In this thesis advanced fuel cycles for the incineration, i.e. deep–burn, of weapons–grade plutonium, reactor–grade plutonium from pressurised light water reactors and reactor–grade plutonium + the associated Minor Actinides in the 400 MWth Pebble Bed Modular Reactor Demonstration Power Plant was simulated with the VSOP 99/05 diffusion code. These results were also compared to the standard 9 g/fuel sphere U/Pu 9.6% enriched uranium fuel cycle. The addition of the Minor Actinides to the reactor–grade plutonium caused an unacceptable decrease in the burn–up and thus an unacceptable increase in the heavy metal (HM) content in the spent fuel, which is intended for direct disposal in a deep geological repository, without chemical reprocessing. All the Pu fuel cycles failed the adopted safety limits in that either the maximum fuel temperature of 1130°C, during normal operation, or the maximum power of 4.5 kW/sphere was exceeded. All the Pu cycles also produced positive Uniform Temperature Reactivity Coefficients, i.e. the coefficient where the temperature of the fuel and the graphite moderator in the fuel spheres are varied together. these positive temperature coefficients were experienced at low temperatures, typically below 700°C. This was due to the influence of the thermal fission resonance of 241Pu. The safety performance of the weapons–grade plutonium was the worst. The safety performance of the reactor–grade plutonium also deteriorated when the heavy metal loading was reduced from 3 g/sphere to 2 g or 1 g. In view of these safety problems, these Pu fuel cycles were judged to be not licensable in the PBMR DPP–400 reactor. Therefore a redesign of the fuel cycle for reactor–grade plutonium, the power conversion system and the reactor geometry was proposed in order to solve these problems. The main elements of these proposals are: v 1. The use of 3 g reactor–grade plutonium fuel spheres should be the point of departure. 232Th will then be added in order to restore negative Uniform Temperature Reactivity Coefficients. 2. The introduction of neutron poisons into the reflectors, in order to suppress the power density peaks and thus the temperature peaks. 3. In order to counter the reduction in burn–up by this introduction of neutron poisons, a thinning of the central reflector was proposed. / Thesis (PhD (Nuclear Engineering))--North-West University, Potchefstroom Campus, 2012.