Дисертації з теми "Fission products Analysis"

Dans les nouvelles centrales nucléaires dites 4ème génération, comme d’ailleurs les anciennes, le dioxyde d’uranium devra opérer dans des milieux hostiles de températures et d’irradiation avec la présence des produits de fission (PF) et des particules alpha (α). Le fonctionnement dans ces conditions extrêmes induira des déplacements d’atomes et dégradera les propriétés thermiques et mécaniques du combustible UO2. La compréhension du comportement des défauts lacunaires, des PF et de l’hélium est cruciale pour prévoir le comportement du dioxyde d’uranium au sein de ces futures installations nucléaires. La première partie de cette thèse est consacrée à l’étude des défauts lacunaires induits par l’implantation de krypton et d’iode (quelques MeV) dans l’UO2 polycristallin et leurs stades de recuits. L’analyse par spectroscopie d’annihilation de positons (PAS) a permis de mettre en évidence la création de défauts de Schottky VU-2VO dans le cas des implantations iode et la formation de clusters lacunaires contenant du gaz pour les implantations krypton. L’évolution en température de ces défauts générés dépend des paramètres d’implantation (nature des ions, énergie, fluence). Cette étude a montré les rôles importants que peuvent jouer les défauts lacunaires et la présence des gaz de fission dans l’évolution du matériau UO2. Ensuite, nous nous sommes intéressés à l’étude et à la caractérisation, par PAS et les techniques d’analyse par faisceau d’ions (NRA/C et RBS/C), du comportement de l’hélium dans l’UO2. Les mesures de NRA/C et RBS/C révèlent une localisation d’une grande fraction d’hélium dans les sites interstitiels octaédriques de la matrice UO2. La localisation de l’hélium reste stable dans ces sites pour T&lt; 600°C, évoluent légèrement entre 600 et 700°C et devient aléatoire à 800°C. Les mesures PAS mettent en évidence trois stades d’évolution des défauts lacunaires : la recombinaison par migration des interstitiels d’oxygène, l’agglomération des défauts entre 600 et 800°C et leur dissociation et élimination lorsque la température augmente. Ces résultats suggèrent que le transport d'hélium est assisté par les défauts lacunaires<br>In the new fourth generation nuclear plants, as in the old ones, uranium dioxide must operate in hostile environments of temperature and irradiation with the presence of fission products (FP) and alpha particles (α). Operation in these extreme conditions will induce atoms displacements and degrade the thermal and mechanical properties of UO2 fuel. Understanding the behavior of induced vacancy defects, FP and helium is crucial to predict the uranium dioxide behavior in the future nuclear reactors. The first part of this thesis is dedicated to the study of vacancy defects induced by krypton and iodine implantation (a few MeV) in the UO2 polycrystalline and of their evolution under annealing. Analysis by positron annihilation spectroscopy (PAS) has highlighted the creation of Schottky defects VU-2VO in the case of iodine implantations and formation of vacancy clusters containing the gas for krypton implantation. The temperature evolution of these defects depends on the implantation parameters (nature of the ion energy, fluence). This study showed the important roles that can play vacancy defects and the presence of fission gases in the evolution of UO2 material. Then we were interested in the study of the helium behavior in UO2 its location and migration, agglomeration and interaction with vacancy defects by using PAS and ion beam analysis (NRA/C and RBS/C). The NRA/C and RBS/C characterizations showed a localization of a large helium fraction in the octahedral interstitial sites of the UO2 matrix. The helium location in these sites remains stable for T &lt;600°C, changing slightly between 600 and 700°C and becomes random at 800°C. Positron annihilation spectroscopy reveals three stages of vacancy defects evolution : The recombination with oxygen interstitial migration, defects agglomeration between 600 and 800°C and their dissociation and elimination when the temperature increases. These results suggest that the He transport is assisted by the vacancy defects

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.<br>Neutron activation analysis is a method used in the determination of several elements in different kinds of matrices. However, when the sample contains high U levels the problem of 235U fission interference occurs. A way to solve this problem is to perform the correction using the interference factor due to U fission for the radionuclides used on elemental analysis. In this study, the interference factors due to U fission for the radioisotopes 141Ce, 143Ce, 140La, 99Mo, 147Nd, 153Sm and 95Zr in the research nuclear reactor IEA-R1 at IPEN-CNEN/SP were determined. These interference factors were determined experimentally, by irradiation of synthetic standards in a selected position in the reactor, and theoretically, determining the epithermal to neutron fluxes ratio in the same position where synthetic standards were irradiated and using reported nuclear parameters on the literature. The obtained interference factors were compared with values reported by other works. To evaluate the reliability of these factors they were applied in the analysis of studied elements in the certified reference materials NIST 8704 Buffalo River Sediment, IRMM BCR- 667 Estuarine Sediment e IAEA-SL-1 Lake Sediment.

Made available in DSpace on 2014-10-09T12:33:04Z (GMT). No. of bitstreams: 0<br>Made available in DSpace on 2014-10-09T14:06:06Z (GMT). No. of bitstreams: 0<br>Dissertação (Mestrado)<br>IPEN/D<br>Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP

Submitted by Claudinei Pracidelli (cpracide@ipen.br) on 2014-11-10T11:38:41Z No. of bitstreams: 0<br>Made available in DSpace on 2014-11-10T11:38:41Z (GMT). No. of bitstreams: 0<br>Dissertação (Mestrado em Tecnologia Nuclear)<br>IPEN/D<br>Instituto de Pesquisas Energeticas e Nucleares - IPEN-CNEN/SP