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Browsing Chemistry by Author "Hayes, John"
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Item Investigating the Geochemical Model for Molybdenum Mineralization in the JEB Tailings Management Facility at McClean Lake, Saskatchewan: An X‐ray Absorption Spectroscopy Study(American Chemical Society, 2015) Blanchard, Peter; Hayes, John; Grosvenor, Andrew; Rowson, John; Hughes, Kebbi; Brown, CaitlinThe geochemical model for Mo mineralization in the JEB Tailings Management Facility (JEB TMF), operated by AREVA Resources Canada at McClean Lake, Saskatchewan, was investigated using X-ray Absorption Near-Edge Spectroscopy (XANES), an elemental-specific technique that is sensitive to low elemental concentrations. Twenty five samples collected during the 2013 sampling campaign from various locations and depths in the TMF were analyzed by XANES. Mo K-edge XANES analysis indicated that the tailings consisted primarily of Mo6+ species: powellite (CaMoO4), ferrimolybdite (Fe2(MoO4)3·8H2O), and molybdate adsorbed on ferrihydrite (Fe(OH)3 − MoO4). A minor concentration of a Mo4+ species in the form of molybdenite (MoS2) was also present. Changes in the Mo mineralization over time were inferred by comparing the relative amounts of the Mo species in the tailings to the independently measured aqueous Mo pore water concentration. It was found that ferrimolybdite and molybdate adsorbed on ferrihydrite initially dissolves in the TMF and precipitates as powellite.Item Investigation of NdxY0.25–xZr0.75O1.88 inert matrix fuel materials made by a co-precipitation synthetic route(NRC Research Press, 2016) Hayes, John; Grosvenor, AndrewYttria-stabilized zirconia (YSZ) is a material that is being considered for use as an inert matrix fuel in nuclear reactors, but a complete characterization of these materials is required for them to be licensed for use. A series of NdxY0.25–xZr0.75O1.88 materials have been synthesized using a co-precipitation method, and the thermal stability of these materials has been studied by annealing them at 1400 and 1500 °C. (Nd was used as surrogate for Am.) The long-range and local structures of the materials were characterized via powder X-ray diffraction, scanning electron microscopy, wavelength dispersive spectroscopy, and X-ray absorption spectroscopy at the Zr K- and Y K-edges. These results were compared with the previous characterization of Nd-YSZ materials synthesized using a ceramic method. The results indicated that the ordering in the local metal–oxygen polyhedral remains relatively unaffected by the synthetic method, but there was increased long-range disorder in the materials prepared by the co-precipitation method. Further, it was found that the materials produced by the co-precipitation method were unexpect- edly unstable when annealed at high temperature. This study highlights the importance of determining the effect of synthetic method on material properties and demonstrates how the co-precipitation route could be used to produce inert matrix fuels.Item Investigation of the Thermal Stability of NdxScyZr1−x−yO2−δ Materials Proposed for Inert Matrix Fuel Applications(American Chemical Society, 2016) Hayes, John; Grosvenor, Andrew; Saoudi, MounaInert matrix fuels (IMF) consist of transuranic elements (i.e., Pu, Am, Np, Cm) embedded in a neutron transparent (inert) matrix and can be used to “burn up” (transmute) these elements in current or Generation IV nuclear reactors. Yttria-stabilized zirconia has been extensively studied for IMF applications, but the low thermal conductivity of this material limits its usefulness. Other elements can be used to stabilize the cubic zirconia structure, and the thermal conductivity of the fuel can be increased through the use of a lighter stabilizing element. To this end, a series of NdxScyZr1−x−yO2−δ materials has been synthesized via a co-precipitation reaction and characterized by multiple techniques (Nd was used as a surrogate for Am). The long-range and local structures of these materials were studied using powder X-ray diffraction, scanning electron microscopy, and X-ray absorption spectroscopy. Additionally, the stability of these materials over a range of temperatures has been studied by annealing the materials at 1100 and 1400 °C. It was shown that the NdxScyZr1−x−yO2−δ materials maintained a single cubic phase upon annealing at high temperatures only when both Nd and Sc were present with y ≥ 0.10 and x + y > 0.15.Item An investigation of the thermal stability of NdxYyZr1 x yO2 d inert matrix fuel materials(Elsevier, 2015) Hayes, John; Grosvenor, Andrew; Saoudi, MoundaAn important step in achieving a closed uranium fuel cycle is to develop new inert matrix fuel (IMF) materials for use in the burn-up of transuranic species (TRU; i.e., Pu, Np, Am, Cm). Cubic fluorite zirconia (ZrO2) has ideal properties for use in IMF applications, but it is not stable at room temperature and must be stabilized through the addition of small amounts of dopants such as Y. While Y-substituted zirconia (YSZ) has been extensively studied, relatively little work has been done to investigate how the addition of an actinide to the YSZ system affects the properties of these materials. To this end, the long-range and local structures of a series of NdxYyZr1 x yO2 d compounds (Nd was used as a surrogate for Am) were studied using powder X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray absorption spectroscopy (XAS) at the Zr K-, Zr L3-, Y K-, and Nd L3-edges. The thermal stability of Nd–YSZ materials was also investigated by annealing the materials at temperatures ranging between 600 and 1400 °C. These studies showed that the thermal stability of the NdxYyZr1-x-yO2-d system was improved by the addition of small amounts of Y (i.e. 5 at.%) to the system. Additionally, the XAS results showed that the local structure around Zr remained relatively constant; only changes in the second coordination shell were observed when the materials were annealed. These results strongly suggest that the addition of Y can significantly improve the thermal stability of zirconia-based IMFs. This study has also confirmed the importance and value of using advanced characterization techniques that are sensitive to the local struc- tures of a material (i.e., XAS).