Pyrochlore-type oxides (A2B2O7) and glass-ceramic composites have been investigated for nuclear waste sequestration applications due to the remarkable compositional diversity and structural flexibility of these materials. These properties can enhance the incorporation of radioactive waste elements and resistance to radiation induced structural damage. Radiation induced structural damage can be simulated by bombarding materials using high-energy heavy ions. The study has shown how the metal-oxygen bond covalency, cationic radii ratio (rA/rB), and oxygen vacancies of pyrochlore type oxides affect the resistance of these materials to radiation induced damage. RE2Ti2O7 (RE=La–Lu), Yb1.85Ca0.15Ti2O7-δ, Yb2Ti1.85Fe0.15O7-δ, and Gd2Ti2-xSnxO7 were synthesized by the ceramic method and investigated by X-ray absorption near edge spectroscopy (XANES), which allows for the study of the effect of elemental substitution on the electronic structure of materials. Surface sensitive glancing angle and total electron yield XANES (GA/TEY XANES) spectra have been used to study the damaged surface of the materials, as the high energy ions can only implant in the near-surface region (~ 450 nm) of the pellets. These measurements have allowed for an investigation of how the local structure of the materials changed after ion implantation and discussed in terms of coordination number and bonding environment. After investigating the ceramic materials, the glass-ceramic composite materials containing Gd2Ti2O7 pyrochlore type crystallites in a (borosilicate- and Fe-Al-borosilicate) glass were investigated. These glass-ceramic materials were synthesized and analyzed by backscattered electron (BSE) images and XANES spectra. The study has shown how the Gd2Ti2O7 crystallites interact within a glass matrix depending on glass composition, pyrochlore loading, and annealing temperature. Further, the GA-XANES spectra from these materials have shown that the glass ceramic composite materials show a similar response to ion implantation as pure ceramics (i.e., Gd2Ti2O7). All of these studies and techniques could provide a better understanding of how to develop and design materials for nuclear waste sequestration applications.

Zirconium and its alloys have been used extensively in both light and heavy water reactors where neutron irradiation is known to cause microstructural evolution, leading to degradation of mechanical properties and dimensional instabilities. Dimensional instabilities due to irradiation growth are particularly crucial for Zr alloy Excel which is the proposed candidate material for the conceptual CANDU-Super Critical Water Cooled Reactors (SCWR) pressure tube. This study employs the in-situ ion irradiation technique and transmission electron microscopy to investigate the irradiation induced microstructural evolution in Zr and Zr alloy Excel. The current study is presented as a manuscript format dissertation comprised of five manuscript chapters. Chapter 3 reports the formation of irradiation induced prismatic defects directly from cascade collapse in pure Zr at low dose (0.008 dpa) in a temperature range of 300oC-500oC. The morphology and yield of these defects are found to be temperature and dose dependent. In Chapter 4, irradiating Zircaloy-2 under similar conditions to pure Zr, reveals that nucleation rate of small prismatic loops increases, whereas their growth is suppressed which indicates that these defect clusters are not only temperature dependent but also impurity dependent. Chapters 5, 6 and 7 report the irradiation induced microstructural changes at various temperatures up to a dose of 10 dpa, in several microstructures of Zr alloy Excel, achieved by different solution treatments. The major focus of these experimental studies was the formation of <c>-component loops in α-phase; decomposition of β-phase; and irradiation induced microchemical changes. It was found that nucleation and growth of <c>-component loops is strongly dependent on irradiation temperature, parent microstructure, and presence of alloying elements. <c>-component loops nucleate above a threshold incubation dose which decreases with an increase of irradiation temperature. Energy dispersive X-ray spectroscopy (EDS) mapping on irradiated microstructures revealed the formation of small Sn clusters in α-phase which have a significant effect on the morphology of <c>-component loops. Fe plays an important role in the nucleation of <c>-component loops, as it distributes itself during irradiation either from β-phase or from pre-existing secondary phase precipitates in α-phase. Furthermore irradiation induced decomposition of β-phase was observed in the form of ω-phase precipitation and irradiation induced clustering of alloying elements. / Thesis (Ph.D, Mechanical and Materials Engineering) -- Queen's University, 2013-12-31 23:50:30.352

Diss. (sammanfattning) Stockholm : Karol. inst., 2004. / Härtill 4 uppsatser.

Diss. (sammanfattning) Stockholm : Karol. inst., 2006. / Härtill 4 uppsatser.

Diss. (sammanfattning) Linköping : Linköpings universitet, 2007. / Härtill 5 uppsatser.

Neste trabalho obtivemos curvas de corrente induzida por raios-x no teflon FEP que apresentou as seguintes características: a) Inicialmente a corrente subiu, atingindo um máximo em torno dos 10s; b) Decaiu lentamente durante aproximadamente meia-hora, e; c) Atingiu um estado estacionário daí por diante. Ao se desligar a radiação, registrou-se a componente atrasada desta corrente. Usamos amostras de 25&#956m de espessura e área irradiada foi de 12,5cm2 ; o campo aplicado da ordem de 104V/cm e taxa de exposição da ordem de 102 R/S. Verificamos que depois de completada de uma medida da corrente induzida num amostra, esta não voltava a se repetir se realizada depois algumas horas; a corrente então não apresentava um máximo, indo diretamente ao valor estacionário; porém se recuperava com o tempo, repetindo a primeira medida depois de algumas semanas. Para mostrar que esta subida e descida da corrente induzida, não era devido a um efeito de campo, realizamos uma medida onde aplicamos o campo intermitente por curtos períodos de tempo, enquanto a amostra era irradiada. O resultado se mostrou igual aos realizados com tensão aplicada permanentemente. Estudamos ainda a dependência da condutividade induzida com a taxa de exposição e com o campo. Finalmente construímos um modelo teórico para o material que permitiu a obtenção de parâmetros do mesmo concordantes com o esperado. Acrescentamos a este trabalho uma curva que mostra o efeito da variação da temperatura sobre uma medida longa da absorção dielétrica. / In this work we measured X-ray indeuced currents in teflon FEP wich show the following features: a) At the beginning the current increases and reaches a maximum at about 10s; b) It decays slowly during 30 minutes, when a steady state is reached slowly during 30 minutes, when a steady state is reached the delayed conductvity was also measured. The sample were 25&#956m thick and the irradiated área was 12,5cm2; the applied field was of the order of 104 V/cm and the dose rate of the order of 102 R/S. It was observed that a new measurement of the induced conductivity does not duplicate the first one, but after a few hours it come backs to the original one. In order to show that the increase and the deacrease of the current is not caused by na electric field effect we realized a measurement where we polled the sample intermitently while it was irradiated. The current thus obtained had about the same values of the first measuments, when the voltage was applied all the time during the measurement. We also measured the absorption current f a teflon sample wich shows after some days the effect of its variation due the variation of the ambiental temperature.

La radiothérapie thoracique peut induire le développement de pneumopathies aiguës et de fibroses. La dysfonction du système vasculaire participe au développement de lésions radiques. Dans l'intestin, un KO endothélial de PAI-1 protège les souris de la fibrose radique. Le premier objectif de ce projet est d'explorer le rôle de PAI-1 dans l'apparition de la fibrose radique pulmonaire. L'irradiation thoracique de souris à 17 Gy altère sévèrement le parenchyme pulmonaire et l'analyse histologique révèle que l'invalidation de PAI-1 aggrave les lésions à 2 et 13 semaines. Cette invalidation ne protège donc pas les animaux des dommages radiques pulmonaires. L'organisation en parallèle du poumon permet d'envisager une tolérance à de fortes doses par fraction sur des petits volumes. Des irradiations en conditions stéréotaxiques ont donc été réalisées chez la souris. Les analyses histologiques montrent une déstructuration alvéolaire et un fort infiltrat inflammatoire au niveau de la zone cible. Un œdème est observable dans l'ensemble du poumon ipsilatéral deux semaines après irradiation. Le poumon ipsilatéral est également affecté par des altérations de structure, tel un épaississement des septa alvéolaires. Ces bouleversements se traduisent également au niveau transcriptomique. A la vue de l'ensemble de ces altérations, un test à l'effort a été réalisé pour évaluer l'impact potentiel sur la fonction pulmonaire. Les résultats mettent en évidence une diminution des performances des animaux. Les analyses sont à approfondir mais elles démontrent l'importance de s'intéresser aux tissus sains situés hors du volume cible mais recevant des fractions variables de la dose délivrée. / Radiation-induced endothelial dysfunction is known to participate to the development of normal tissue damage. PAI- is implicated in the phenotypic changes of irradiated endothelial cells and KOendo mice are protected from radiation damage to the gut. Whole thorax of PAI-1 KOendo and floxed mice were exposed to 17 Gy. Histological analyzes showed that PAI-1 KOendo induces a worsening of injuries at 2 and 13 weeks. Consequently, contrary to the gut no protection from radiation-induced lung damage is observed in PAI-1 KOendo mice. Our second aim was to study the effects of a single high dose stereotactic irradiation on pulmonary tissues. Histological analyzes and scanner imaging show important injuries on the targeted volume. An ipsilateral edema can also be observed 2 weeks after irradiation. Ipsilateral lung is moreover importantly damaged. A thickening of alveolar septa is notably observable. A transcriptomic analysis show important similarities between tissues from the ipsilateral lung and the focal lesion. As really highly damages have been observed in both scanner and histological analyzes, we decided to perform forced physical activity test on treadmill. A drastic decrease of maximal distance traveled has been observed from two weeks. These experiments highlighted a deficiency in respiratory function and all of these results show the importance of non-targeted irradiated pulmonary volume in the development of radiation-induced fibrosis. Effect of an endothelium-specific deletion of HIF-1α has been investigated in this model of stereotactic irradiation. Only few differences have been observed between KOendo and control mice. Experiments are still ongoing.

Kyoto University (京都大学) / 0048 / 新制・論文博士 / 博士(工学) / 乙第12335号 / 論工博第4013号 / 新制||工||1466(附属図書館) / 27190 / UT51-2009-D550 / (主査)教授 森山 裕丈, 教授 伊藤 秋男, 教授 高木 郁二 / 学位規則第4条第2項該当

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This review contains the results of EPR/ENDOR experiments on DNA constituents in the solid-state. Most of the results presented involve single crystals of the DNA bases, nucleosides and nucleotides. The emphasis is on low-temperature ENDOR results. Typical experiments involve irradiations at or near helium temperatures in attempts to determine the primary radiation induced oxidation and reduction products. The use of the ENDOR technique allows one to determine the protonation state of the initial products. Subsequent warming of the sample facilitates a study of the reactions that the primary products undergo. A summary of the results is provided to show the relevance the study of model compounds has in understanding the radiation chemistry of DNA.