Browsing by Subject "zirconium"
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Item Atomic Diffusion in the Uranium-50wt% Zirconium Nuclear Fuel System(2013-06-17) Eichel, DanielAtomic diffusion phenomena were examined in a metal-alloy nuclear fuel system composed of ?-phase U-50wt%Zr fuel in contact with either Zr-10wt%Gd or Zr-10wt%Er. Each alloy was fabricated from elemental feed material via melt-casting, and diffusion samples of nominal 1.5 mm thickness were prepared from the resulting alloy slugs. The samples were assembled into diffusion couples and annealed for periods of 14, 28, and 56 days at temperatures of 550?C, 600?C, and 650?C. Thus, the U-50Zr/Zr-10Er system and the U-50Zr/Zr-10Gd system were each annealed for three different time periods at each of three different temperatures, for an initial total of 18 diffusion interfaces that were to be studied. In practice, data was collected from only 12 of the 18 interfaces. At 650?C, the U-50wt%Zr alloy exists in the ?-phase region, which enabled the comparison of diffusion behavior between the ? phase and ? phase. Diffusion samples were examined by collecting composition profiles across the diffusion interface for each element via electron probe microanalysis. From the resulting experimental data diffusion coefficients were evaluated. Diffusion coefficients were found to be on the order of 10^-19 m2/s in the ?-phase systems, and 10^-17 m^2/s in the ?-phase systems. It was observed that atomic mobility of all diffusing species was generally greater in the U-50Zr/Zr-10Gd system than in the U-50Zr/Zr-10Er system; furthermore, it was found that diffusion rates were considerably higher above the phase transformation temperature into the ? phase, as indeed would be expected in the more open structure of the body-centered cubic ? phase, as compared to the hexagonal ?-phase U-Zr. However, values for diffusion coefficients measured in this study were considerably smaller than those found in past studies of ?-phase U-Zr, which are on the order of 10^-17 m^2/s. It is likely that diffusion was inhibited by the formation of stable metal oxides resulting from oxygen contamination; it is also possible that diffusion was suppressed by the presence of the erbium and gadolinium.Item Characterization of Alpha-Phase Sintering of Uranium and Uranium-Zirconium Alloys for Advanced Nuclear Fuel Applications(2012-02-14) Helmreich, GrantThe sintering behavior of uranium and uranium-zirconium alloys in the alpha phase were characterized in this research. Metal uranium powder was produced from pieces of depleted uranium metal acquired from the Y-12 plant via hydriding/dehydriding process. The size distribution and morphology of the uranium powder produced by this method were determined by digital optical microscopy. Once the characteristics of the source uranium powder were known, uranium and uranium-zirconium pellets were pressed using a dual-action punch and die. The majority of these pellets were sintered isothermally, first in the alpha phase near 650?C, then in the gamma phase near 800?C. In addition, a few pellets were sintered using more exotic temperature profiles. Pellet shrinkage was continuously measured in situ during sintering. The isothermal shrinkage rates and sintering temperatures for each pellet were fit to a simple model for the initial phase of sintering of spherical powders. The material specific constants required by this model, including the activation energy of the process, were determined for both uranium and uranium-zirconium. Following sintering, pellets were sectioned, mounted, and polished for imaging by electron microscopy. Based on these results, the porosity and microstructure of the sintered pellets were analyzed. The porosity of the uranium-zirconium pellets was consistently lower than that of the pure uranium pellets. In addition, some formation of an alloyed phase of uranium and zirconium was observed. The research presented within this thesis is a continuation of a previous project; however, this research has produced many new results not previously seen. In addition, a number of issues left unresolved by the previous project have been addressed and solved. Most notably, the low original output of the hydride/dehydride powder production system has been increased by an order of magnitude, the actual characteristics of the powder have been measured and determined, shrinkage data was successfully converted into a sintering model, an alloyed phase of uranium and zirconium was produced, and pellet cracking due to delamination has been eliminated.Item Comprehensive Investigation of the Uranium-Zirconium Alloy System: Thermophysical Properties, Phase Characterization and Ion Implantation Effects(2013-07-31) Ahn, SangjoonUranium-zirconium (U-Zr) alloys comprise a class of metallic nuclear fuel that is regularly considered for application in fast nuclear energy systems. The U-10wt%Zr alloy has been demonstrated to very high burnup without cladding breach in the Experimental Breeder Reactor-II (EBR-II). This was accomplished by successfully accommodating gaseous fission products with low smear density fuel and an enlarged cladding plenum. Fission gas swelling behavior of the fuel has been experimentally revealed to be significantly affected by the temperature gradient within a fuel pin and the multiple phase morphologies that exist across the fuel pin. However, the phase effects on swelling behavior have not been yet fully accounted for in existing fuel performance models which tend to assume the fuel exists as a homogeneous single phase medium across the entire fuel pin. Phase effects on gas bubble nucleation and growth in the alloy were investigated using transmission electron microscopy (TEM). To achieve this end, a comprehensive examination of the alloy system was carried out. This included the fabrication of uranium alloys containing 0.1, 2, 5, 10, 20, 30, 40, and 50 wt% zirconium by melt-casting. These alloys were characterized using electron probe micro-analysis (EPMA), differential scanning calorimetry (DSC), and thermogravimetric analysis (TGA). Once the alloys were satisfactorily characterized, selected U-Zr alloys were irradiated with 140 keV He^(+) ions at fluences ranging from 1 ? 10^(14) to 5 ? 10^(16) ions/cm^(2). Metallographic and micro-chemical analysis of the alloys indicated that annealing at 600 ?C equilibrates the alloys within 168 h to have stable ?-U and ?-UZr_(2) phase morphologies. This was in contrast to some reported data that showed kinetically sluggish ?-UZr_(2) phase formation. Phase transformation temperatures and enthalpies were measured using DSC-TGA for each of the alloys. Measured temperatures from different time annealed alloys have shown consistent matches with most of the features in the current U-Zr phase diagram which further augmented the EPMA observed microstructural equilibrium. Nevertheless, quantitative transformation enthalpy analysis also suggests potential errors in the existing U-Zr binary phase diagram. More specifically, the (?-U, ?2) phase region does not appear to be present in Zr-rich (> 15 wt%) U-Zr alloys and so further investigation may be required. To prepare TEM specimens, characterized U-Zr alloys were mechanically thinned to a thickness of ~150 ?m, and then electropolished using a 5% perchloric acid/95% methanol electrolyte. Uranium-rich phase was preferentially thinned in two phase alloys, giving saw-tooth shaped perforated boundaries; the alloy images were very clear and alloy characterization was accomplished. During in-situ heating U-10Zr and U-20Zr alloys up to 810 ?C, selected area diffraction (SAD) patterns were observed as the structure evolved up to ~690 ?C and the expected ?-U ? ?-U phase transformation at 662 ?C was never observed. For the temperature range of the (?-U, ?2) phase region, phase transformation driven diffusion was observed as uranium moved into Zr-rich phase matrix in U-20Zr alloy; this was noted as nonuniform bridging of adjacent phase lamellae in the alloy. From the irradiation tests, nano-scale voids were discovered to be evenly distributed over several micrometers in U-40Zr alloys. For the alloys irradiated at the fluences of 1 ? 10^(16) and 5 ? 10^(16) ions/cm^(2), estimated void densities were proportional to the irradiation doses, (250 ? 40) and (1460 ? 30) /?m^(2), while void sizes were fairly constant, (6.0 ? 1.5) and (5.2 ? 1.2) nm, respectively. Measured data could be foundational inputs to the further development of a semi-empirical metal fuel performance model.Item Hydride production in zircaloy-4 as a function of time and temperature(2009-05-15) Parkison, Adam JosephThe experiments performed for this thesis were designed to define the primary process variables of time, temperature, and atmosphere for an engineering system that will produce metal powder from recycled nuclear fuel cladding. The proposed system will hydride and mill Zircaloy cladding tubes to produce fine hydride powder and then dehydride the powder to produce metal; this thesis is focused on the hydride formation reaction. These experiments were performed by hydriding nuclear grade Zircaloy-4 tubes under flowing argon-5% hydrogen for various times and temperatures. The result of these experiments is a correlation which relates the rate of zirconium hydride formation to the process temperature. This correlation may now be used to design a method to efficiently produce zirconium hydride powder. It was observed that it is much more effective to hydride the Zircaloy-4 tubes at temperatures below the a-B-d eutectoid temperature of 540?C. These samples tended to readily disassemble during the hydride formation reaction and were easily ground to powder. Hydrogen pickup was faster above this temperature but the samples were generally tougher and it was difficult to pulverize them into powder.Item Methods for Investigating Gas Bubble Formation in Uranium-Zirconium Alloys(2013-05-06) Mews, Kathryn Ann WrightUranium-zirconium alloy nuclear fuels have many advantages as compared with ceramic fuels, especially for fast reactor systems. However, metallic fuels aren?t currently used in commercial power production due in part to issues with fuel swelling during irradiation. A major contributor to this expansion issue, the formation of fission gasses into bubbles, is examined here. Methods to evaluate evolution of fission gas bubbles within a U-Zr alloy are discussed and refined. Specifically, transmission electron microscopy (TEM) for viewing bubbles within the interior of the alloy is investigated. One constraint on the use of the TEM is the lack of literature pertaining to what thinning techniques are successful for U-10Zr alloy. Both initial and final thinning techniques were investigated. After thinning was complete, the specimens were viewed via TEM to determine their suitability. In addition, samples of U-Zr alloy were irradiated with gas atoms in an accelerator to simulate bubble initiation and formation and viewed via TEM. Only preliminary investigations were completed. Evaluated electrolyte solutions included one part phosphoric acid to two parts sulfuric acid and two parts water (A), one part phosphoric acid to one part ethanol and one part glycerol (B), one part hydrochloric acid to one part water (C), two parts methanol to 13 parts phosphoric acid (D), and one part perchloric acid to nine parts acetic acid (G). Positive responses were received from the solutions A, C, and G which generated electron transparent areas with few to no process induced artifacts. TEM trials with each electrolyte were performed on un-irradiated U-10Zr alloy. These trials indicated that the polishing methods would work but are not yet optimal. In addition, U-10Zr alloy was irradiated and viewed in the TEM where those polished with electrolyte A consistently included the presence of large circular features that could indicate bubbles or voids. The foundation was laid for further study to be done on this topic through the use of electropolishing solutions as final thinning techniques. Additional work that is recommended includes: electropolishing parameter refinement; implantation of heavier gas atoms or at elevated temperatures; annealing of the implanted alloy; and computer modeling of resulting first principles phenomena.