No Brasil e no mundo a tecnologia nuclear vem ocupando posição de destaque com diversas aplicações na indústria, geração de energia, meio ambiente e na medicina, melhorando a qualidade de exames e tratamentos, consequentemente, a vida das pessoas. O urânio é o principal elemento utilizado em instalações nucleares, servindo como material base desde a geração de eletricidade à fabricação de radiofármacos. Nos anos 50, em meio à guerra fria, a então recém-criada Agência Internacional de Energia Atômica se propôs a supervisionar instalações nucleares e incentivar a fabricação de combustíveis nucleares com baixo teor de urânio, conhecidos como combustíveis do tipo Material Test Reactor (MTR), fabricados inicialmente na forma de U3O8 e mais tarde o U3Si2, ambos dispersos em alumínio. A utilização desta tecnologia requer uma constante melhoria de todos os processos que envolvem a fabricação do MTR sujeita a diversos protocolos internacionais, os quais procuram garantir a confiabilidade desse combustível do ponto de vista prático e ambiental. Dentro desse contexto, o controle de impurezas, do ponto de vista da economia de nêutrons, afeta diretamente a qualidade de qualquer combustível nuclear, fazendo-se necessário um controle rigoroso. A literatura reporta procedimentos que, além de gerar resíduos, são demorados e dispendiosos, pois necessitam de curva de calibração univariada e materiais de referência. Assim, o objetivo deste trabalho é estabelecer e validar uma metodologia de análise química quantitativa não destrutiva, de baixo custo e tempo de análise, tal como, minimizar a geração de resíduo para a determinação multielementar dos maiores constituintes (Utotal e Si) e as impurezas (B, Mg, Al, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Cd e outros) presentes em U3O8 e U3Si2, atendendo as necessidades de reatores nucleares na qualificação de combustíveis nucleares do tipo MTR. Para tanto, foi aplicada a técnica de fluorescência de raios X que permite análises químicas rápidas e não destrutivas, além de não necessitar de tratamentos químicos prévios (dissolução, digestão e outros) na fase de preparação de amostras. Para as correções de efeitos espectrais e de matriz foram aplicados e avaliados os métodos de parâmetros fundamentais, de curva de calibração univariada e de calibração multivariada. Os resultados foram comparados por meios de testes estatísticos em conformidade com a norma ISO 17025 com os MRCs (123(1-7) e 124(1-7)) de U3O8 da New Brunswick Laboratory (NBL) e 16 amostras de U3Si2 cedidas pelo CCN do IPEN-CNEN-SP. A quimiometria demonstrou-se um método promissor para a determinação de maiores e menores constituintes em combustíveis nuclear a base de U3O8 e U3Si2, uma vez que a precisão e exatidão são estatisticamente iguais aos métodos de análises volumétrica, gravimétrica e ICP-OES. / In Brazil and worldwide the nuclear power has occupied a prominent position with many applications in industry, power generation, environment and medicine, improving the quality of tests and treatments, therefore people\'s lives. Uranium is the main element used in nuclear facilities and its employed as base material to generation of electricity in the manufacture of radiopharmaceuticals. In the \'50s, during the Cold War, the then newly created International Atomic Energy Agency proposed to oversee nuclear facilities and encourage the manufacture of nuclear fuels with low-enriched uranium (LEU) fuel came then type Material Test Reactor (MTR), manufactured initially in U3O8 and U3Si2 later, both dispersed in aluminum. The use of this technology requires a constant improvement of all processes involving the manufacture of MTR subject to several international protocols, which seek to ensure the reliability of the fuel from the standpoint of practical and environmental. In this context, the control of impurities, from the point of view of neutron economy, directly affects the quality of any nuclear fuel, so strict control is necessary. The literature has reported procedures which, beyond generating residues, are lengthy and costly, they need calibration curve and consequently reference materials. The aim of this work is to establish and validate a methodology for nondestructive quantitative chemical analysis, low cost and analysis time, as well as minimize the generation of waste, for multielement determination of major constituents (Utotal and Si) and impurities (B, Mg, Al, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Cd and others) present in U3O8 and U3Si2, meeting the needs of nuclear reactors in the nuclear fuel qualification type MTR. For that purposes, will be applied the X-ray fluorescence technique which allows fast chemical and nondestructive analysis, aside from sample preparation procedures that do not require previous chemical treatments (dissolving, digesting, and others). To corrections like effects of spectral and matrix were applied and evaluated the fundamental parameter method, univariate calibration curve and multivariate calibration. The results were compared by means of statistical tests in accordance with ISO 17025 in MRCs (123 (1-7) and 124 (1-7)) MCRs of U3O8 from New Brunswick Laboratory (NBL) and 16 U3Si2 samples provided by CC of IPEN/CNEN-SP. The chemometrics is a promising method to determination of minor and major constituents on the U3Si2 and U3O8 basis nuclear fuel, because the precision and accuracy are statistically equal volumetric analysis, gravimetric and ICP-OES methods.

No Brasil e no mundo a tecnologia nuclear vem ocupando posição de destaque com diversas aplicações na indústria, geração de energia, meio ambiente e na medicina, melhorando a qualidade de exames e tratamentos, consequentemente, a vida das pessoas. O urânio é o principal elemento utilizado em instalações nucleares, servindo como material base desde a geração de eletricidade à fabricação de radiofármacos. Nos anos 50, em meio à guerra fria, a então recém-criada Agência Internacional de Energia Atômica se propôs a supervisionar instalações nucleares e incentivar a fabricação de combustíveis nucleares com baixo teor de urânio, conhecidos como combustíveis do tipo Material Test Reactor (MTR), fabricados inicialmente na forma de U3O8 e mais tarde o U3Si2, ambos dispersos em alumínio. A utilização desta tecnologia requer uma constante melhoria de todos os processos que envolvem a fabricação do MTR sujeita a diversos protocolos internacionais, os quais procuram garantir a confiabilidade desse combustível do ponto de vista prático e ambiental. Dentro desse contexto, o controle de impurezas, do ponto de vista da economia de nêutrons, afeta diretamente a qualidade de qualquer combustível nuclear, fazendo-se necessário um controle rigoroso. A literatura reporta procedimentos que, além de gerar resíduos, são demorados e dispendiosos, pois necessitam de curva de calibração univariada e materiais de referência. Assim, o objetivo deste trabalho é estabelecer e validar uma metodologia de análise química quantitativa não destrutiva, de baixo custo e tempo de análise, tal como, minimizar a geração de resíduo para a determinação multielementar dos maiores constituintes (Utotal e Si) e as impurezas (B, Mg, Al, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Cd e outros) presentes em U3O8 e U3Si2, atendendo as necessidades de reatores nucleares na qualificação de combustíveis nucleares do tipo MTR. Para tanto, foi aplicada a técnica de fluorescência de raios X que permite análises químicas rápidas e não destrutivas, além de não necessitar de tratamentos químicos prévios (dissolução, digestão e outros) na fase de preparação de amostras. Para as correções de efeitos espectrais e de matriz foram aplicados e avaliados os métodos de parâmetros fundamentais, de curva de calibração univariada e de calibração multivariada. Os resultados foram comparados por meios de testes estatísticos em conformidade com a norma ISO 17025 com os MRCs (123(1-7) e 124(1-7)) de U3O8 da New Brunswick Laboratory (NBL) e 16 amostras de U3Si2 cedidas pelo CCN do IPEN-CNEN-SP. A quimiometria demonstrou-se um método promissor para a determinação de maiores e menores constituintes em combustíveis nuclear a base de U3O8 e U3Si2, uma vez que a precisão e exatidão são estatisticamente iguais aos métodos de análises volumétrica, gravimétrica e ICP-OES. / In Brazil and worldwide the nuclear power has occupied a prominent position with many applications in industry, power generation, environment and medicine, improving the quality of tests and treatments, therefore people\'s lives. Uranium is the main element used in nuclear facilities and its employed as base material to generation of electricity in the manufacture of radiopharmaceuticals. In the \'50s, during the Cold War, the then newly created International Atomic Energy Agency proposed to oversee nuclear facilities and encourage the manufacture of nuclear fuels with low-enriched uranium (LEU) fuel came then type Material Test Reactor (MTR), manufactured initially in U3O8 and U3Si2 later, both dispersed in aluminum. The use of this technology requires a constant improvement of all processes involving the manufacture of MTR subject to several international protocols, which seek to ensure the reliability of the fuel from the standpoint of practical and environmental. In this context, the control of impurities, from the point of view of neutron economy, directly affects the quality of any nuclear fuel, so strict control is necessary. The literature has reported procedures which, beyond generating residues, are lengthy and costly, they need calibration curve and consequently reference materials. The aim of this work is to establish and validate a methodology for nondestructive quantitative chemical analysis, low cost and analysis time, as well as minimize the generation of waste, for multielement determination of major constituents (Utotal and Si) and impurities (B, Mg, Al, Cr, Mn, Fe, Co, Ni, Cu, Zn, Mo, Cd and others) present in U3O8 and U3Si2, meeting the needs of nuclear reactors in the nuclear fuel qualification type MTR. For that purposes, will be applied the X-ray fluorescence technique which allows fast chemical and nondestructive analysis, aside from sample preparation procedures that do not require previous chemical treatments (dissolving, digesting, and others). To corrections like effects of spectral and matrix were applied and evaluated the fundamental parameter method, univariate calibration curve and multivariate calibration. The results were compared by means of statistical tests in accordance with ISO 17025 in MRCs (123 (1-7) and 124 (1-7)) MCRs of U3O8 from New Brunswick Laboratory (NBL) and 16 U3Si2 samples provided by CC of IPEN/CNEN-SP. The chemometrics is a promising method to determination of minor and major constituents on the U3Si2 and U3O8 basis nuclear fuel, because the precision and accuracy are statistically equal volumetric analysis, gravimetric and ICP-OES methods.

The newest European high performance material testing reactor, the Jules Horowitz Reactor, is under construction at CEA Cadarache research center in France. The reactor will support existing and future nuclear reactor technologies, with the first criticality expected at the end of this decade. The current/reference CEA methodology for simulating the thermalhydraulic behavior of the reactor gives reliable results. The CATHARE2 code simulates the full reactor circuit with a simplified approach for the core. The results of this model are used as boundary conditions in a three-dimensional FLICA4 core simulation. However this procedure needs further improvement and simplification to shorten the computational requirements and give more accurate core level data. The reactor’s high performance (e.g. high neutron fluxes, high power densities) and its design (e.g. narrow flow channels in the core) render the reactor modeling challenging compared to more conventional designs. It is possible via thermal-hydraulic or solely hydraulic Computational Fluid Dynamics (CFD) simulations to achieve a better insight of the flow and thermal aspects of the reactor’s performance. This approach is utilized to assess the initial modeling assumptions and to detect if more accurate modeling is necessary. There were no CFD thermal-hydraulic publications available on the JHR prior to the current PhD thesis project. The improvement process is split into five steps. In the first step, the state-of-the-art CEA methodology for thermal-hydraulic modeling of the reactor using the system code CATHARE2 and the core analysis code FLICA4 is described. In the second and third steps, a CFD thermal-hydraulic simulations of the reactor’s hot fuel element are undertaken with the code STAR-CCM+. Moreover, a conjugate heat transfer analysis is performed for the hot channel. The knowledge of the flow and temperature fields between different channels is important for performing safety analyses and for accurate modeling. In the fourth step, the flow field of the full reactor vessel is investigated by conducting CFD hydraulic simulations in order to identify the mass flow split between the 36 fuel elements and to describe the flow field in the upper and lower plenums. As a side study a thermal-hydraulic calculation, similar to those performed in previous steps is undertaken utilizing the outcome of the hydraulic calculation as an input. The final step culminates by producing an improved, more realistic, purely CATHARE2 based, JHR model, incorporating all the new knowledge acquired from the previous steps. The primary outcome of this four year PhD research project is the improved, more realistic, CATHARE2 model of the JHR with two approaches for the hot fuel element. Furthermore, the project has led to improved thermal-hydraulic knowledge of the complex reactor (including the hot fuel element), with the most prominent findings presented. / <p>QC 20161208</p> / DEMO-JHR