Orientador: Wagner dos Santos Oliveira / Tese (doutorado) - Universidade Estadual de Campinas, Faculdade de Engenharia Química / Made available in DSpace on 2018-08-23T04:04:19Z (GMT). No. of bitstreams: 1 Jeronimo_AdroaldoClovis_D.pdf: 4228405 bytes, checksum: c8569d86097f26c1f29121c0181597cd (MD5) Previous issue date: 2013 / Resumo: As atividades de investigação, avaliação e prevenção das emissões químicas com potencial para causar doenças ocupacionais nos inúmeros processos químicos representam atividades importantes sob o ponto de vista da preservação à saúde humana, segurança e meio ambiente. Este estudo apresenta metodologia para o monitoramento dos riscos ocupacionais e ambientais nos processos de conversão de compostos de urânio no ciclo de combustível nuclear. Nos tópicos estudados a atenção está voltada para o risco e perigo à saúde ocupacional relacionado à exposição às substancias químicas perigosas integradas nos demais estágios dos processos. As questões de saúde, segurança e meio ambiente exercem papeis cruciais neste e em inúmeros processos de engenharia, envolvendo uma rede de atividades que, se não gerenciados de forma adequada, podem causar danos à saúde das pessoas e seu meio. Desta forma, aumenta-se a necessidade de métodos alternativos de prevenção aos riscos com participação multidisciplinar para refinar continuamente a busca de melhoria nos sistemas químicos em estudo. A compreensão de perigo nos demais estágios do processo são questões aqui abordadas. Por ser impossível estudar a imensidade de processos químicos, são selecionadas algumas substâncias que servirão de base para avaliação das situações de exposição. As anomalias dessas situações de riscos aconteceram simultaneamente com o gerenciamento das atividades de P&D, que culminaram com o domínio da tecnologia de produção do hexafluoreto de urânio pelo Brasil / Abstract: The activities of research, evaluation and prevention of chemical emissions with potential to cause occupational diseases in the endless number chemical processes represents important activities under the viewpoint of the preservation the human health, hazards and environment. This I study presents methodology for monitoring of environmental and occupational risks in the uranium compounds conversion processes of compounds of uranium in nuclear fuel cycle. In the topics studied attention is focused on the risk and hazards the occupational health, related to the occupational exposure to hazards chemicals integrated in other stages of the processes. The issues of health, safety and environment exert crucial roles in this an in many engineering processes, involving a network of activities that, if not managed properly, can cause damage to the health of the people and its environment. In this way, increase-it needs alternative methods of preventing to the risks with multidisciplinary participation to continually refine the search for improvements in the chemical systems under study. The understandings of danger in other stages of the process are issues addressed here. By it be impossible researched the immensity of chemical processes, are selected some substances that serve as the basis for assessment of exposure situations. The anomalies of these situations of risks happen simultaneously to the management of the activities of P&D, which culminate with the mastery of the technology of production of uranium hexafluoride by Brazil / Doutorado / Desenvolvimento de Processos Biotecnologicos / Doutor em Engenharia Química

URhGe is the first ferromagnet discovered that shows superconductivity at ambient pressure. It shows a rich temperature-magnetic field phase diagram with a re-emergence of superconductivity at high magnetic field where the moments rotate. This suggests that the quantum fluctuations associated with the moment rotation may provide the pairing interaction for superconductivity. The objective of this thesis was to study these critical fluctuations with inelastic neutron scattering and heat capacity measurements, using the latter to test the bulk nature of the superconductivity and determine the types of gap nodes to help test this hypothesis. To perform the heat capacity measurements, it was necessary to develop an apparatus that measures milligram samples in the temperature range 50-1000 mK, and magnetic field range 0-12 T. The field exerts a mechanical force upon the sample, which causes it to rotate, perturbing the system destructively. The apparatus developed in this thesis overcomes this diffculty by holding the sample with tensioned kevlar wires. Testing was done by making measurements on UPt3, a well characterised superconductor. It was then used to measure URhGe in zero magnetic field. The extension to measurements in high magnetic field were not performed however, due to the structural integrity of the apparatus being weak - this was in an attempt to reduce the thermodynamic signature of the background. After many iterations of apparatus design and build, the device was proved not appropriate for high fields. A discussion of the zero-field data, as well as the design and build process, is given. The Curie temperature of URhGe is suppressed with magnetic field (applied along the b-axis), reaching zero temperature at the moment rotation transition referred to above. Small angle neutron scattering (SANS) was measured at both zero and finite fields to detect the evolution and relaxation of the critical fluctuations. The scattering is inelastic and the SANS measurement integrates over energy. Nevertheless it was possible to compare models with different dynamical dependences for the magnetic relaxation. In field, however, the magnitude of the fluctuations was strongly reduced, falling below the detection limit at half the critical field. Comparing Landau damping to various forms of non-Landau damping, a result was found that agrees with that for the ferromagnetic superconductors UGe2 and UCoGe, but the lack of critical scattering at field is found to be in contradiction with NMR measurements, which is discussed. UAu2 is a new material on the heavy fermion landscape. The crystal structure found suggests some frustrated magnetism, culminating in a Neél temperature of 43 K and a further transition at 400 mK; this suggests some new quantum criticality not seen before, and so heat capacity measurements were performed with the already-tested apparatus to see if, as the resistivity measurements suggest, a Fermi-liquid state is found. Results revealed differences between annealed and non-annealed samples in their thermodynamic signature, and the behaviour expected for antiferromagnetic spin-fluctuations is found to continue to temperatures below 150 mK, suggesting the existence of a quantum critical point. The validity of these results along with implications are discussed.

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Title: Variations of actinide magnetism in uranium-base hydrides and other selected systems. Author: Anna Maria Adamska Department / Institute: Department of Condensed Matter Physics Supervisor of the doctoral thesis: Doc. RNDr. Ladislav Havela, CSc., the Department of Condensed Matter Physics Faculty of Mathematics and Physics Charles University, Prague, Czech Republic and Assoc. Prof. Dr. hab. Nhu-Tarnawska Hoa Kim Ngan, Institute of Physics, Pedagogical University, Kraków, Poland. Abstract: Actinide magnetism was studied in three different types of systems. Variations of magnetic properties of UTGe hydrides as a function of hydrogen concentration prove that doping of U intermetallics by interstitial hydrogen leads to stronger magnetic properties, primarily caused by an increase of the inter-uranium separation. Sputter-deposited UFe2+x films, which are derived from the UFe2 Laves phase but have an amorphous structure, exhibit an increase of the Curie temperarture (to more than 400 K) with the Fe excess, which could not be achieved in the bulk. This is understood as a result of the prominent role of the 3d magnetism of Fe. Notoriously weakly magnetic plutonium was studied in the form of the alloy in the ζ-phase, which exists between 35 and 70 % U in Pu. Its susceptibility increases in a comparison to pure...

Dans cette thèse, on étudie la criticalité quantique ferromagnétique dans trois composés ternaires à base d'uranium, par des mesures thermodynamiques et de transport sur des échantillons monocristallins, à basse température et sous haute pression. URhSi et URhAl sont des systèmes ferromagnétiques itinérants, tandis que UCoAl est un système paramagnétique étant proche d'une instabilité ferromagnétique. Tous ont une phase ordonnée de type Ising. Dans le composé orthorhombique URhSi, on montre que la température de Curie diminue lorsqu'un champ magnétique est appliqué perpendiculairement à l'axe facile d'aimantation, et une transition de phase quantique est attendue autour de 40~T. Dans le système hexagonal URhAl, on établit le diagramme de phase pression--température pour la première fois, lequel indique une transition de phase quantique vers 5~GPa. Dans le composé isostructural UCoAl, on étudie la transition métamagnétique par des mesures d'aimantation, d'effet Hall, de résistivité et de dichroïsme circulaire magnétique des rayons X. On observe des phénomènes de relaxation magnétique intrigants, avec des sortes de marches. L'effet Hall et la résistivité ont été mesurés à des températures de réfrigérateur à dilution, sous pression hydrostatique jusqu'à 2,2~GPa, et sous champ magnétique jusqu'à 16~T. La transition métamagnétique se termine sous pression et champ magnétique au niveau d'un point critique quantique terminal. Dans cette région, il se produit une forte augmentation de la masse effective, et une différence intrigante entre champ montant et descendant apparaît dans la résistivité transverse. Ce pourrait être la signature d'une nouvelle phase, éventuellement reliée aux phénomènes de relaxation observés dans les mesures d'aimantation, et résultant de frustrations au sein du réseau quasi-Kagomé que forment les atomes d'uranium dans cette structure cristalline. / In this thesis we explore the ferromagnetic quantum criticality in three uranium-based ternary compounds, by means of thermodynamical and transport measurements on single crystal samples, at low temperature and high pressure. URhSi and URhAl are itinerant ferromagnets, while UCoAl is a paramagnet being close to a ferromagnetic instability. All of them have Ising-type magnetic ordering. In the orthorhombic compound URhSi, we show that the Curie temperature decreases upon applying a magnetic field perpendicular to the easy magnetization axis, and a quantum phase transition is expected around 40~T. In the hexagonal system URhAl, we establish the pressure--temperature phase diagram for the first time, indicating a quantum phase transition around 5~GPa. In the isostructural compound UCoAl, we investigate the metamagnetic transition with measurements of magnetization, Hall effect, resistivity and X-ray magnetic circular dichroism. Some intriguing magnetic relaxation phenomena are observed, with step-like features. Hall effect and resistivity have been measured at dilution temperatures, under hydrostatic pressure up to 2.2 GPa and magnetic field up to 16~T. The metamagnetic transition terminates under pressure and magnetic field at a quantum critical endpoint. In this region, a strong effective mass enhancement occurs, and an intriguing difference between up and down field sweeps appears in transverse resistivity. This may be the signature of a new phase, supposedly linked to the relaxation phenomena observed in magnetic measurements, arising from frustration on the quasi-Kagome lattice of uranium atoms in this crystal structure.

Submitted by Pedro Silva Filho (pfsilva@ipen.br) on 2017-11-22T17:00:26Z No. of bitstreams: 0 / Made available in DSpace on 2017-11-22T17:00:26Z (GMT). No. of bitstreams: 0 / Conselho Nacional de Desenvolvimento Científico e Tecnológico (CNPq) / A demanda por combustível nuclear para reatores de pesquisa está aumentando em nível mundial, enquanto várias de suas fábricas têm pequeno volume de produção. Este trabalho estabeleceu um modelo conceitual com duas estratégias para o aumento da capacidade produtiva dessas fábricas. Foram abordadas as fábricas que produzem elementos combustíveis tipo placa carregados com LEU U3Si2-Al, tipicamente usados em reatores nucleares de pesquisa. A primeira estratégia baseia-se na literatura da área de administração da produção e é uma prática frequente nas fábricas em geral. A segunda estratégia aproveita a possibilidade de desmembrar setores produtivos, comum em instalações de produção de combustível nuclear. Ambas as estratégias geraram diferentes cenários de produção, os quais devem ser seguros em relação à criticalidade. Foram coletados dados de uma fábrica real de combustível nuclear para reatores de pesquisa. As duas estratégias foram aplicadas a esses dados com a finalidade de testar o modelo proposto, o que configurou um estudo de caso. A aplicação das estratégias aos dados coletados deu-se por meio de simulação de eventos discretos em computador. Foram criados diversos modelos de simulação para abranger todos os cenários gerados, de forma que o teste indicou um aumento da capacidade produtiva de até 207% sem necessidade de aquisição de novos equipamentos. Os resultados comprovam que o modelo atingiu plenamente o objetivo proposto. Como principal conclusão pode-se apontar a eficácia do modelo proposto, fato que foi validado pelos dados da fábrica. / Tese (Doutorado em Tecnologia Nuclear) / IPEN/T / Instituto de Pesquisas Energéticas e Nucleares - IPEN-CNEN/SP / CNPq:310274/2012-5

Microstructure changes in uranium and uranium/metal alloys due to radiation damage are of great interest in nuclear science and engineering. Titanium has attracted attention because of its similarity to Zr. It has been proposed for use in the second generation of fusion reactors due to its resistance to radiation-induced swelling. Aluminum can be regarded as a standard absorbing material or backing material for irradiation targets. Initial study of thin aluminum films irradiation by �������Cf fission fragments and alpha particles from source has been conducted in the Radiation Center, Oregon State University. Initial study of thin aluminum films irradiation by �������Cf fission fragments and alpha particles from source has been conducted in the Radiation Center, Oregon State University. Aluminum can be regarded as a standard absorbing material or backing material for irradiation targets. The AFM investigation of microstructure damages of thin aluminum surfaces revealed that the voids, dislocation loops and dislocation lines, formed in the thin aluminum films after bombardment by �������Cf fission fragments and alpha particles, depends on the irradiation dose. The void swelling and diameter and depth of voids increase linearly with the fluence of particles and dose; however, the areal density of voids decreased when formation of dislocation loops began. Study of deposition of uranium on titanium backing material by molecular plating and characterization of produced U/Ti film has been performed. The U/Ti film has smooth and uniform surfaces but the composition of the deposits is complex and does not include water molecules which probably involve the presence of U (VI). A possible structure for the deposits has been suggested. X-ray diffraction pattern of U/Ti films showed that The U/Ti film has an amorphous structure. Uranium films (0.500 mg/cm��) and stack of titanium foils (thickness 0.904 mg/cm��) were used to study the microstructural damage of the uranium film and its backing material. Irradiation of U/Ti film and Ti foils with 1 MeV/u (136 MeV) �������Xe�������� ions in was performed in the Positive Ion Injector (PII) unit at the Argonne Tandem Linear Accelerator System (ATLAS) Facility at Argonne National Laboratory, IL. Pre- and post- irradiation of samples was analyzed by X-ray diffraction, Scanning Electron Microscopy/Energy Dispersive Spectroscopy (SEM/EDS) and Atomic Force Microscopy (AFM). The irradiation of U/Ti films results in the formation of a crystalline U���O��� phase and polycrystalline Ti phase. Annealing of the thin uranium deposit on a titanium backing at 800��C in the air atmosphere condition for an hour produced a mixture of UO���, U���O���, Ti, TiO and TiO��� (rutile) phases; meanwhile, annealing at 800oC for an hour in the argon environment produced a mixture of ��-U���O���, Ti and TiO��� (rutile) phases. These phenomena indicate that the damage during irradiation was not due to foil heating. Microstructural damage of irradiated uranium film was dominated by void and bubble formation. The microstructure of irradiated titanium foils is characterized by hillocks, voids, polygonal ridge networks, dislocation lines and dislocation networks. Theory predicts that titanium undergoes an allotropic phase transformation at 882.5 ��C, changing from a closed-packed hexagonal crystal structure (��-phase) into a body-centered cubic crystal structure (��- phase). When the titanium foils were irradiated with 136MeV �������Xe�������� at beam intensity of 3 pnA corresponding to 966��C, it was expected that its structure can change from hexagonal-close packed (hcp) to body-centered cubic (bcc). However, in contrast to the theory, transformation from ��-Ti (hcp) phase to fcc-Ti phase was observed. This phenomenon indicates that during irradiation with high energy and elevated temperature, the fcc-Ti phase more stable than the hcp-Ti Phase. / Graduation date: 2012