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  • About
  • The Global ETD Search service is a free service for researchers to find electronic theses and dissertations. This service is provided by the Networked Digital Library of Theses and Dissertations.
    Our metadata is collected from universities around the world. If you manage a university/consortium/country archive and want to be added, details can be found on the NDLTD website.
1

Análise neutrônica e especificação técnica para o combustível a dispersão UMo-Al com adição de veneno queimável / Neutronic analysis and technical specification for a UMo-Al dispersion fuel with burnable poison addition

Muniz, Rafael Oliveira Rondon 03 December 2015 (has links)
Este trabalho apresenta a análise neutrônica do combustível a dispersão de UMo-Al em relação ao aumento da densidade de urânio e faz uma comparação com o combustível de U3Si2-Al. Neste estudo, a densidade de urânio do U3Si2-Al é variada de 3,0 à 5,5 gU/cm3 e a do UMo-Al entre 4,0 à 7,5 gU/cm3 e com a porcentagem em massa de molibdênio com 7 e 10 %. Neste trabalho também é proposta a aplicação de veneno queimável metálico no cerne do combustível de UMo-Al, uma vez que este combustível é metálico e é analisada a utilização de gadolínio (Gd) e európio (Eu) como veneno queimável. A utilização do Gd como veneno queimável foi analisada com o fator de multiplicação infinito (k∞) através do programa celular HRC desenvolvido pelo IPEN e composto pelos códigos HAMMERTECHNION para a analise de célula, ROLAIDS para o cálculo de auto blindagem dos actinídeos e CINDER-2 empregado para a fissão e transmutação dos actinídeos. O núcleo do reator simulado foi similar ao do RMB (Reator Multipropósito Brasileiro) composto por um arranjo de 5x5 posições com 23 elementos combustíveis e dois blocos de alumínio. Para o európio, foram utilizados os programas SERPENT e CITATION. Os cálculos de queima foram realizados considerando uma potência de 30 MW durante três ciclos do RMB de 97 dias. Os resultados obtidos mostram que a porcentagem em massa do molibdênio têm uma grande influência no comportamento neutrônico devido a seção de choque de absorção do molibdênio ser considerável. Portanto, foi escolhida a porcentagem de 7 % de Mo para os estudos com veneno queimável. Para o núcleo proposto, o európio mostrou-se melhor, pois apresenta uma queima mais gradual que o gadolínio. Foi realizada uma simulação com o programa SERPENT com adição de 6 % de silício, o que mostrou que a adição de Si não causa mudança significativa no ciclo de operação do reator. Para validação da metodologia de cálculo, foi elaborada uma especificação técnica e fabricadas 12 miniplacas combustíveis de UMo-Al sem veneno queimável. As miniplacas foram irradiadas no núcleo do reator IPEN/MB-01, em quatro configurações de núcleo, para obtenção da reatividade inserida. Os resultados simulados obtidos para a inserção de reatividade pelas miniplacas nos diversos núcleos analisados apresentaram alta concordância com os resultados experimentais. / This work presents the neutronic analysis of the UMo-Al dispersion fuel concerning uranium density increase and shows comparisons relatively to the U3Si2-Al fuel. The U3Si2-Al uranium density varied from 3.0 to 5.5 gU/cm3 while that of UMo-Al fuel varied from 4.0 to 7.5 gU/cm3. The molybdenum mass content in the former case varies from 7 to 10 % in mass. Here, it is also proposed the utilization of burnable poison nuclides in the UMo-Al fuel meat. Since the fuel is metallic, gadolinium and europium were chosen as candidates to cope with this task. A recently developed cell code at IPEN (HRC) composed of the coupling of the codes HAMMER-TECHNION for the cell analysis, ROLAIDS for the actinide self-shielding calculations and CINDER-2 for the actinide and fission transmutation was employed for the neutronic analyses of UMo-Al. The simulated reactor core was similar to the one of RMB (Brazilian Multipurpose Reactor) composed of an array of 5x5 positions with 23 fuel elements and 2 aluminum blocks. A second analysis of the europium case employed the SERPENTE and CITATION codes. The burnup calculations were performed considering a power of 30 MW during three cycles of RMB 97 days. The analyses revealed that the molybdenum content has a great impact in the core reactivity due to its high absorption cross section. A value of 7 % was found adequate for the molybdenum mass content. The analyses also reveal that europium is a better burnable poison than gadolinium for the core cycle length and power level under consideration. It was realized a simulation with the computer code SERPENT with addition of 6 % silicon in UMo-Al fuel. The silicon does not change significantly the reactor operation cycle. To validate the calculation methodology it was developed a technical specification and fabricated 12 UMo-Al fuel miniplates without burnable poison. The miniplates were irradiated in the IPEN-MB/01 reactor core for four core configurations, in order to obtain the inserted reactivity. The simulated results for the reactivity insertion by the fuel miniplates in the analyzed cores showed high agreement with the experimental results.
2

Análise neutrônica e especificação técnica para o combustível a dispersão UMo-Al com adição de veneno queimável / Neutronic analysis and technical specification for a UMo-Al dispersion fuel with burnable poison addition

Rafael Oliveira Rondon Muniz 03 December 2015 (has links)
Este trabalho apresenta a análise neutrônica do combustível a dispersão de UMo-Al em relação ao aumento da densidade de urânio e faz uma comparação com o combustível de U3Si2-Al. Neste estudo, a densidade de urânio do U3Si2-Al é variada de 3,0 à 5,5 gU/cm3 e a do UMo-Al entre 4,0 à 7,5 gU/cm3 e com a porcentagem em massa de molibdênio com 7 e 10 %. Neste trabalho também é proposta a aplicação de veneno queimável metálico no cerne do combustível de UMo-Al, uma vez que este combustível é metálico e é analisada a utilização de gadolínio (Gd) e európio (Eu) como veneno queimável. A utilização do Gd como veneno queimável foi analisada com o fator de multiplicação infinito (k∞) através do programa celular HRC desenvolvido pelo IPEN e composto pelos códigos HAMMERTECHNION para a analise de célula, ROLAIDS para o cálculo de auto blindagem dos actinídeos e CINDER-2 empregado para a fissão e transmutação dos actinídeos. O núcleo do reator simulado foi similar ao do RMB (Reator Multipropósito Brasileiro) composto por um arranjo de 5x5 posições com 23 elementos combustíveis e dois blocos de alumínio. Para o európio, foram utilizados os programas SERPENT e CITATION. Os cálculos de queima foram realizados considerando uma potência de 30 MW durante três ciclos do RMB de 97 dias. Os resultados obtidos mostram que a porcentagem em massa do molibdênio têm uma grande influência no comportamento neutrônico devido a seção de choque de absorção do molibdênio ser considerável. Portanto, foi escolhida a porcentagem de 7 % de Mo para os estudos com veneno queimável. Para o núcleo proposto, o európio mostrou-se melhor, pois apresenta uma queima mais gradual que o gadolínio. Foi realizada uma simulação com o programa SERPENT com adição de 6 % de silício, o que mostrou que a adição de Si não causa mudança significativa no ciclo de operação do reator. Para validação da metodologia de cálculo, foi elaborada uma especificação técnica e fabricadas 12 miniplacas combustíveis de UMo-Al sem veneno queimável. As miniplacas foram irradiadas no núcleo do reator IPEN/MB-01, em quatro configurações de núcleo, para obtenção da reatividade inserida. Os resultados simulados obtidos para a inserção de reatividade pelas miniplacas nos diversos núcleos analisados apresentaram alta concordância com os resultados experimentais. / This work presents the neutronic analysis of the UMo-Al dispersion fuel concerning uranium density increase and shows comparisons relatively to the U3Si2-Al fuel. The U3Si2-Al uranium density varied from 3.0 to 5.5 gU/cm3 while that of UMo-Al fuel varied from 4.0 to 7.5 gU/cm3. The molybdenum mass content in the former case varies from 7 to 10 % in mass. Here, it is also proposed the utilization of burnable poison nuclides in the UMo-Al fuel meat. Since the fuel is metallic, gadolinium and europium were chosen as candidates to cope with this task. A recently developed cell code at IPEN (HRC) composed of the coupling of the codes HAMMER-TECHNION for the cell analysis, ROLAIDS for the actinide self-shielding calculations and CINDER-2 for the actinide and fission transmutation was employed for the neutronic analyses of UMo-Al. The simulated reactor core was similar to the one of RMB (Brazilian Multipurpose Reactor) composed of an array of 5x5 positions with 23 fuel elements and 2 aluminum blocks. A second analysis of the europium case employed the SERPENTE and CITATION codes. The burnup calculations were performed considering a power of 30 MW during three cycles of RMB 97 days. The analyses revealed that the molybdenum content has a great impact in the core reactivity due to its high absorption cross section. A value of 7 % was found adequate for the molybdenum mass content. The analyses also reveal that europium is a better burnable poison than gadolinium for the core cycle length and power level under consideration. It was realized a simulation with the computer code SERPENT with addition of 6 % silicon in UMo-Al fuel. The silicon does not change significantly the reactor operation cycle. To validate the calculation methodology it was developed a technical specification and fabricated 12 UMo-Al fuel miniplates without burnable poison. The miniplates were irradiated in the IPEN-MB/01 reactor core for four core configurations, in order to obtain the inserted reactivity. The simulated results for the reactivity insertion by the fuel miniplates in the analyzed cores showed high agreement with the experimental results.
3

Thermal Properties of Uranium-Molybdenum Alloys: Phase Decomposition Effects of Heat Treatments

Creasy, John Thomas 2011 December 1900 (has links)
Uranium-Molybdenum (U-Mo) alloys are of interest to the nuclear engineering community for their potential use as reactor fuel. The addition of molybdenum serves to stabilize the gamma phase of uranium, as well as increasing the melting point of the fuel. Thermal properties of U-Mo alloys have not been fully characterized, especially within the area of partial phase decomposition of the gamma phase of the alloy. Additional data was acquired through this research to expand the characterization data set for U-Mo alloys. The U-Mo alloys used for this research were acquired from the Idaho National Laboratory and consisted of three alloys of nominal 7, 10, and 13 percent molybdenum by weight. The sample pins were formed by vacuum induction melt casting. Once the three sample pins were fabricated and sent to the Fuel Cycle and Materials Laboratory at Texas A&M University, the pins were homogenized and sectioned for heat treatment. Several heat treatments were performed on the samples to induce varying degrees of phase decomposition, and the samples were subsequently sectioned for phase verification and thermal analysis. An Electron Probe Microanalyzer with wavelength dispersive spectroscopy was used to observe the phases in the samples as well as to characterize each phase. The density of each sample was determined using Archimedes method. Finally, a light flash analyzer was used to determine thermal diffusivity of the samples up to 300 degrees C as well as to estimate the thermal conductivity. For U-10Mo, thermal diffusivity increased with increasing phase decomposition from gamma to alpha +U2Mo while U-7Mo saw a flattening of the thermal diffusivity curve with increased phase decomposition.
4

Estudos microestruturais  sobre interações químicas na liga U-Mo com Al / Microstructural studies on chemical interactions in U-10Mo alloy with Al

Ilson Carlos Martins 01 December 2010 (has links)
Objetiva-se, com a pesquisa da liga U-Mo, a obtenção de material nuclear para confecção de elementos combustíveis de alta densidade de urânio para reatores de pesquisa de alto desempenho. A política internacional de não proliferação de armas nucleares limita o nível de enriquecimento para reatores de pesquisa em 20% U235. Ligas de U-Mo com 6-10 % peso de Mo podem levar a uma densidade de até 9 gU/cm3, no núcleo da placa combustível. As placas do elemento combustível MTR (Materials Testing Reactor), são fabricadas a partir de briquetes (U-Mo + pó Al) encapsulados em placas de Al, soldadas e laminadas. No entanto, a liga U-Mo é muito reativa na presença de Al. Os produtos dessa reação são indesejáveis, do ponto de vista nuclear, pois geram uma camada de interação química (IL) formada durante ciclagens térmicas e exposição a fissões nucleares. Como a IL tem baixa condutividade térmica, falhas estruturais no elemento combustível, em operação, podem ser causadas. O presente estudo oferece uma nova técnica de formação de pares de interdifusão que promove os contatos da liga U-Mo, na forma de tabletes, envolvidos em matriz de A1 (placas), selada por laminação. Criam-se, assim, condições ideais para a investigação da difusão, com reduzida possibilidade de oxidação nas interfaces de contato, simulando-se, ainda, as condições de laminação a quente no primeiro passe de redução, durante a fabricação da placa combustível MTR. Optou-se por trabalhar com um teor de Mo de 10% em peso na liga U-Mo, para se garantir uma maior formação da fase , uma vez que esse teor favorece uma maior estabilidade química dessa fase. A liga de Al utilizada como matriz dos pares de interdifusão foi a AA1050, por apresentar menores teores de impureza. Os pares de interdifusão U-10Mo/AA1050 foram tratados, termicamente, em duas faixas de temperaturas (1500C e 5500C) e em três tempos de aquecimento (5h, 40h e 80h), visando-se simular o processo de interdifusão e formação da camada de interação química. As análises da camada de interação U-10Mo/AA1050, feitas por MEV/EDS e por difração de Raios X, revelaram uma interdifusão de baixa evolução em Al (cerca de 8% atômico), na região U-Mo. Não houve a formação dos produtos típicos esperados, como (U,Mo)Alx=2,3,4. Associou-se esse fato, provavelmente, à presença do silício na liga AA1050 que, potencialmente, criou uma barreira de poucos micrômetros, impedindo o Al de se difundir de forma mais efetiva para o interior da liga U-10Mo. Sugeriu-se a possível formação de um produto intermetálico de Al com Si, U e Mo. Em especial, foi citada a possibilidade da ocorrência do intermetálico Al3.21 Si0.47, causando esse efeito de bloqueio. / This research refers to the study of U-Mo alloy as an alternative material for producing nuclear fuel elements with high density of uranium, for research reactors of high perfor-mance. The international non-proliferation of nuclear weapons has enrichment level li-mited to 20% U235. U-Mo alloys with 6-10 wt% Mo can lead to a density up to 9 gU/cm3, inside the fuel core. The MTR fuel element plates are made from briquettes (U-Mo powder + Al) encapsulated in Al plates, then welded and rolled However, the U-Mo alloy is very reactive in the presence of Al. The reaction products of this interaction are undesirable from the standpoint of nuclear usage, since they cause a chemical interaction layer (IL) formed during thermal cycling and exposure to nuclear fission neutrons. As the IL has low thermal conductivity, they may cause structural failure in the fuel element during opera-tion. The present study provides a new preparation technique for interdiffusion pairs made by hot rolling. The U-Mo alloy, in tablet format, is involved by matrix Al-plates, which is sealed and then hot rolled. This way to prepare the diffusion couples is an ideal condition to avoid the oxidation at the contact interface at U-Mo/Al. The hot rolling preparation also simulates the first reduction pass during MTR fuel plate manufacture. We chose to work with a Mo content of 10 wt% in U-Mo alloy to ensure greater phase formation, since this level favors a greater chemical stability in this phase. The Al alloy matrix was used as the AA1050 since it contains small impurity amounts. The interdiffusion couples U-10Mo/AA1050 were thermally treated in two temperature ranges (1500C and 5500C) and three soaking times (5h, 40h and 80h) to simulate the interdiffusion process and formation of chemical interaction layer. The analysis of the interaction layer U-10Mo/AA1050 was made by SEM/EDS and X-ray diffraction. It revealed a general trend of low interdiffusion of Al (about 8 atomic %) inside U-Mo. There was no formation of typical products as ex-pected (U, Mo)Alx= 2,3,4. This fact is probably linked to the silicon presence, co-diffusing in the system. Connected with this fact, there was the presence of silicon in the alloy AA1050, which potentially created a barrier that prevented Al to diffuse more effectively, beyond few micrometers into the U-10Mo bulk. A possible formation of intermetallic Al with Si, U and Mo was suggested. In particular, the occurrence of the intermetallic Al3.21Si0.47, causing this blocking effect, was mentioned.
5

Estudos microestruturais  sobre interações químicas na liga U-Mo com Al / Microstructural studies on chemical interactions in U-10Mo alloy with Al

Martins, Ilson Carlos 01 December 2010 (has links)
Objetiva-se, com a pesquisa da liga U-Mo, a obtenção de material nuclear para confecção de elementos combustíveis de alta densidade de urânio para reatores de pesquisa de alto desempenho. A política internacional de não proliferação de armas nucleares limita o nível de enriquecimento para reatores de pesquisa em 20% U235. Ligas de U-Mo com 6-10 % peso de Mo podem levar a uma densidade de até 9 gU/cm3, no núcleo da placa combustível. As placas do elemento combustível MTR (Materials Testing Reactor), são fabricadas a partir de briquetes (U-Mo + pó Al) encapsulados em placas de Al, soldadas e laminadas. No entanto, a liga U-Mo é muito reativa na presença de Al. Os produtos dessa reação são indesejáveis, do ponto de vista nuclear, pois geram uma camada de interação química (IL) formada durante ciclagens térmicas e exposição a fissões nucleares. Como a IL tem baixa condutividade térmica, falhas estruturais no elemento combustível, em operação, podem ser causadas. O presente estudo oferece uma nova técnica de formação de pares de interdifusão que promove os contatos da liga U-Mo, na forma de tabletes, envolvidos em matriz de A1 (placas), selada por laminação. Criam-se, assim, condições ideais para a investigação da difusão, com reduzida possibilidade de oxidação nas interfaces de contato, simulando-se, ainda, as condições de laminação a quente no primeiro passe de redução, durante a fabricação da placa combustível MTR. Optou-se por trabalhar com um teor de Mo de 10% em peso na liga U-Mo, para se garantir uma maior formação da fase , uma vez que esse teor favorece uma maior estabilidade química dessa fase. A liga de Al utilizada como matriz dos pares de interdifusão foi a AA1050, por apresentar menores teores de impureza. Os pares de interdifusão U-10Mo/AA1050 foram tratados, termicamente, em duas faixas de temperaturas (1500C e 5500C) e em três tempos de aquecimento (5h, 40h e 80h), visando-se simular o processo de interdifusão e formação da camada de interação química. As análises da camada de interação U-10Mo/AA1050, feitas por MEV/EDS e por difração de Raios X, revelaram uma interdifusão de baixa evolução em Al (cerca de 8% atômico), na região U-Mo. Não houve a formação dos produtos típicos esperados, como (U,Mo)Alx=2,3,4. Associou-se esse fato, provavelmente, à presença do silício na liga AA1050 que, potencialmente, criou uma barreira de poucos micrômetros, impedindo o Al de se difundir de forma mais efetiva para o interior da liga U-10Mo. Sugeriu-se a possível formação de um produto intermetálico de Al com Si, U e Mo. Em especial, foi citada a possibilidade da ocorrência do intermetálico Al3.21 Si0.47, causando esse efeito de bloqueio. / This research refers to the study of U-Mo alloy as an alternative material for producing nuclear fuel elements with high density of uranium, for research reactors of high perfor-mance. The international non-proliferation of nuclear weapons has enrichment level li-mited to 20% U235. U-Mo alloys with 6-10 wt% Mo can lead to a density up to 9 gU/cm3, inside the fuel core. The MTR fuel element plates are made from briquettes (U-Mo powder + Al) encapsulated in Al plates, then welded and rolled However, the U-Mo alloy is very reactive in the presence of Al. The reaction products of this interaction are undesirable from the standpoint of nuclear usage, since they cause a chemical interaction layer (IL) formed during thermal cycling and exposure to nuclear fission neutrons. As the IL has low thermal conductivity, they may cause structural failure in the fuel element during opera-tion. The present study provides a new preparation technique for interdiffusion pairs made by hot rolling. The U-Mo alloy, in tablet format, is involved by matrix Al-plates, which is sealed and then hot rolled. This way to prepare the diffusion couples is an ideal condition to avoid the oxidation at the contact interface at U-Mo/Al. The hot rolling preparation also simulates the first reduction pass during MTR fuel plate manufacture. We chose to work with a Mo content of 10 wt% in U-Mo alloy to ensure greater phase formation, since this level favors a greater chemical stability in this phase. The Al alloy matrix was used as the AA1050 since it contains small impurity amounts. The interdiffusion couples U-10Mo/AA1050 were thermally treated in two temperature ranges (1500C and 5500C) and three soaking times (5h, 40h and 80h) to simulate the interdiffusion process and formation of chemical interaction layer. The analysis of the interaction layer U-10Mo/AA1050 was made by SEM/EDS and X-ray diffraction. It revealed a general trend of low interdiffusion of Al (about 8 atomic %) inside U-Mo. There was no formation of typical products as ex-pected (U, Mo)Alx= 2,3,4. This fact is probably linked to the silicon presence, co-diffusing in the system. Connected with this fact, there was the presence of silicon in the alloy AA1050, which potentially created a barrier that prevented Al to diffuse more effectively, beyond few micrometers into the U-10Mo bulk. A possible formation of intermetallic Al with Si, U and Mo was suggested. In particular, the occurrence of the intermetallic Al3.21Si0.47, causing this blocking effect, was mentioned.
6

Étude des relations microstructures : propriétés d'usage, de poudres fissiles d'alliages U(Mo) / Study of relationships between microstructures and usual properties, of U(Mo) alloys fissile particles

Champion, Guillaume 14 October 2013 (has links)
Cette thèse participe au développement d’un combustible particulaire uranium-molybdène dans le cadre de la conversion des réacteurs de recherche de haute-performance en France et à travers le monde, à l’utilisation de combustibles faiblement enrichis (LEU : Low Enriched Uranium à opposer à HEU : High Enriched Uranium). Ce dernier se présente sous la forme d’une dispersion de particules uranifères U(Mo) dans une matrice à base d’aluminium et une question majeure persiste quant à l’interaction se produisant entre le composé U(Mo) et la matrice d’aluminium. En effet, il a été constaté que sous certaines conditions d’irradiation, cette interaction donne lieu à un gonflement instable de la plaque combustible qui résulte d’une percolation accentuée et imprévisible de bulles de gaz de fission à l’interface entre une couche d’interaction formée autour des particules U(Mo) et la matrice aluminium. Cette thèse s’est attachée à développer plusieurs solutions « remèdes » visant à modifier et/ou diminuer, voire inhiber l’interaction combustible/matrice et à améliorer la rétention des bulles de gaz de fission. Pour atteindre ces objectifs, deux voies ont été testées au cours de la thèse, (i) l’amélioration des propriétés microstructurales intrinsèques de l’alliage U(Mo) et (ii) la modification de l’interface âme combustible / matrice, par le dépôt de couches à effet barrière. En ce qui concerne le premier axe de recherche, une campagne de caractérisation des poudres de référence a, au préalable, été réalisée, permettant d’identifier des paramètres clés pour le développement de produits à microstructure « optimisée ». Deux produits innovants ont ainsi été développés puis soumis à caractérisation : une poudre atomisée-broyée et une poudre obtenue par magnésiothermie. Nous avons démontré que ces produits peuvent être un atout vis-à-vis de la problématique de rétention des bulles de gaz de fission. En ce qui concerne la problématique de la formation d’une couche d’interaction, un troisième produit, reposant sur le génie des procédés, a été développé : une poudre U(Mo) atomisée, revêtue d’une couche type alumine. Nous avons démontré qu’une couche comprise entre 100 et 200 nm permettait d’inhiber la croissance d’une couche d’interaction activée thermiquement. Nos recommandations finales ont ainsi pu être données en vue de la réalisation de tests d’irradiation « en-pile » pour la qualification d’un combustible U(Mo) optimisé. / This thesis enters in the Material and Testing Reactors (MTRs) framework where the necessity to use a Low-Enriched Uranium (LEU) fuel has led to the development of a dense fissile material based on U(Mo) alloys. The designed fuel is a composite material, made of dispersed U(Mo) particles embedded in an Al based matrix. Post-Irradiation Examinations of these LEU fuel plates showed that the irradiation behaviour of the fuel is not fit for purpose yet. This is mainly due to the growth of an interaction layer between the fuel and the matrix and to the bad gas retention efficiency of the fuel particles. This thesis had for purpose the development of several solutions in order to modify and/or decrease or even inhibit the fuel/matrix interaction and to increase the gas retention capacities of the fuel. In order to achieve so, two solutions have been tested during this thesis, (i) optimization of the U(Mo) alloy intrinsic microstructural properties and (ii) modificationof the fuel meat/matrix interface, through the deposition of a layer acting as a ''diffusion barrier''. Concerning the first axe of study, a characterization campaign of the reference powders has been realized, as a first step, in order to identify the key parameters for the development of products showing an “optimized” microstructure. Two novel products have then been developed: one based on a combined process associating “atomization + grinding” and another, which consists in a magnesiothermy process. These products were subject to characterization: X-Ray and neutron diffraction, electron backscattered diffraction and transmission electron microscopy have been performed in particular. We managed to show that these powders can be an advantage concerning the issue with the gas retention capacities of the fuel. Concerning the growth of the interaction layer, a third product, using process engineering, has been developed: an U(Mo) atomized powder, coated with an alumina like layer. We managed to show that a thickness between 100 and 200 nm of the layer allowed inhibiting the growth of a thermally activated interaction layer. Finally, our recommendations have been given in order to realize irradiation tests “in-pile” for the qualification of an optimized U(Mo) fuel.
7

Etude du procédé de CVD en lit fluidisé en vue de revêtir des particules denses pour applications nucléaires / Study of the fluidized bed chemical vapor deposition process on very dense powder for nuclear applications

Vanni, Florence 21 September 2015 (has links)
Cette thèse s’inscrit dans le cadre du développement d’un combustible nucléaire faiblement enrichi pour les réacteurs de recherche, constitué de particules d’uranium-molybdène mélangées à une matrice d’aluminium. Dans certaines conditions sous irradiations, les particules d’U(Mo) interagissent avec la matrice d’aluminium, provoquant un gonflement rédhibitoire de la plaque combustible. Pour inhiber ce phénomène, une solution consiste à déposer, à la surface des particules d’U(Mo), une fine couche de silicium, pour créer un effet barrière. Cette thèse a concerné l’étude du procédé de dépôt chimique à partir d’une phase vapeur (CVD) en lit fluidisé à partir de silane pour déposer le silicium sur la poudre d’U(Mo), qui a une densité exceptionnelle de 17,5. Pour atteindre cet objectif, deux axes d’études ont été traités au cours de la thèse : l’étude et l’optimisation de la mise en fluidisation d’une poudre aussi dense, puis celles du procédé de dépôt de silicium. Pour le premier axe, une campagne d’essais a été réalisée sur poudre simulante de tungstène dans différentes colonnes de fluidisation en verre et en acier avec des diamètres internes compris entre 2 et 5 cm, à température ambiante et à haute température (650°C), proche de celle des dépôts. Cette campagne a permis d’identifier des phénomènes d’effets de bord au sein du lit fluidisé, pouvant conduire à des dépôts hétérogènes ou à des prises en masse. Des dimensions de colonnes de fluidisation et des conditions opératoires permettant une fluidisation satisfaisante de la poudre ont pu être identifiées, ouvrant la voie à l’étude du dépôt de silicium. Plusieurs campagnes d’essais de dépôt sur poudre simulante, puis sur poudre U(Mo), ont ensuite été menées dans le cadre du second axe d’étude. L’influence de la température du lit, de la fraction molaire d’entrée en silane dilué dans l’argon, et du débit total de fluidisation, a été étudiée pour différents diamètres de réacteur et pour diverses masses de poudre. Des analyses de caractérisation morphologique et structurale (MEB, DRX...) ont révélé un dépôt de silicium uniforme sur toute la poudre et autour de chaque grain, majoritairement cristallisé et dont l’épaisseur atteint les objectifs visés. Des recommandations précises ont ainsi pu être émises pour optimiser les caractéristiques du dépôt de silicium sur la poudre combustible U(Mo) par le procédé de CVD en lit fluidisé. / This thesis is part of the development of low-enriched nuclear fuel, for the Materials Test Reactors (MTRs), constituted of uranium-molybdenum particles mixed with an aluminum matrix. Under certain conditions under irradiations, the U(Mo) particles interact with the aluminum matrix, causing unacceptable swelling of the fuel plate. To inhibit this phenomenon, one solution consists in depositing on the surface of the U(Mo) particles, a thin silicon layer to create a barrier effect. This thesis has concerned the study of the fluidized bed chemical vapor deposition (CVD) process to deposit silicon from silane, on the U(Mo) powder, which has an exceptional density of 17,500 kg/m3. To achieve this goal, two axes were treated during the thesis: the study and the optimization of the fluidization of a so dense powder, and then those of the silicon deposition process. For the first axis, a series of tests was performed on a surrogate tungsten powder in different columns made of glass and made of steel with internal diameters ranging from 2 to 5 cm, at room temperature and at high temperature (650°C) close to that of the deposits. These experiments helped to identify wall effects phenomena within the fluidized bed, which can lead to heterogeneous deposits or particles agglomeration. Some dimensions of the fluidization columns and operating conditions allowing a satisfactory fluidization of the powder were identified, paving the way for the study of silicon deposition. Several campaigns of deposition experiments on the surrogate powder and then on the U(Mo) powder were carried out in the second axis of the study. The influence of the bed temperature, the inlet molar fraction of silane diluted in argon, and the total gas flow of fluidization, was examined for different diameters of reactor and for various masses of powder. Morphological and structural characterization analyses (SEM, XRD…) revealed a uniform silicon deposition on all the powder and around each particle, mostly crystallized and whose thickness reached the objectives. Specific recommendations were proposed to optimize the characteristics of the silicon deposit on the U(Mo) powder by the fluidized bed CVD process.

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