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DeBurgomaster, Paul Christopher

Publications and source records attributed to DeBurgomaster, Paul Christopher.

Surface area and particle size distribution of plutonium oxides derived from the direct oxidation of Pu metal (LA-UR-18-22581)

The intent of this paper is to interrogate the physical characteristics of PuO 2 powders and aggregates produced by direct metal oxidation to examine possible relationships between process parameters and the physical characteristics of the product. The majority of the PuO 2 samples considered were generated during the pre-production and production phases of the Advanced Recovery and Integrated Extraction System (ARIES) program at Los Alamos National Laboratory (LANL). Oxide formed passively on Pu metal surfaces at ambient atmospheric conditions is also characterized. Plutonium oxide powders from the ARIES Direct Metal Oxidation (DMO) furnace and muffle furnace process lines are very consistent in terms of their bulk and tapped density, specific surface area (SSA) and particle size distribution (PSD). The SSAs of calcined PuO 2 generated in the ARIES DMO-2 and muffle furnaces are between 0.1 and 0.5 m2/g. Oxides from both the DMO-2 and muffle furnaces also had similar tri-modal PSDs with maxima at 0.73–3.16 μm, 10.9–18.5 μm, and 41.3–63.0 μm. The PSDs of the oxide formed passively on Pu metal surfaces at ambient conditions were unimodal, with near-Gaussian distributions and D50 close to 1 μm. In conclusion, the oxide formed passively at ambient conditions also had significantly higher SSAs (6–8 m 2 /g).

36 MATERIALS SCIENCE↗

Water Solubility of Plutonium and Uranium Compounds and Residues at TA-55

Understanding the water solubility of plutonium and uranium compounds and residues at TA-55 is necessary to provide a technical basis for appropriate criticality safety, safety basis and accountability controls. Individual compound solubility was determined using published solubility data and solution thermodynamic modeling. Residue solubility was estimated using a combination of published technical reports and process knowledge of constituent compounds. The scope of materials considered includes all compounds and residues at TA-55 as of March 2016 that contain Pu-239 or U-235 where any single item in the facility has more than 500 g of nuclear material. This analysis indicates that the following materials are not appreciably soluble in water: plutonium dioxide (IDC=C21), plutonium phosphate (IDC=C66), plutonium tetrafluoride (IDC=C80), plutonium filter residue (IDC=R26), plutonium hydroxide precipitate (IDC=R41), plutonium DOR salt (IDC=R42), plutonium incinerator ash (IDC=R47), uranium carbide (IDC=C13), uranium dioxide (IDC=C21), U 3 O 8 (IDC=C88), and uranium filter residue (IDC=R26). This analysis also indicates that the following materials are soluble in water: plutonium chloride (IDC=C19) and uranium nitrate (IDC=C52). Equilibrium calculations suggest that PuOCl is water soluble under certain conditions, but some plutonium processing reports indicate that it is insoluble when present in electrorefining residues (R65). Plutonium molten salt extraction residues (IDC=R83) contain significant quantities of PuCl 3 , and are expected to be soluble in water. The solubility of the following plutonium residues is indeterminate due to conflicting reports, insufficient process knowledge or process-dependent composition: calcium salt (IDC=R09), electrorefining salt (IDC=R65), salt (IDC=R71), silica (IDC=R73) and sweepings/screenings (IDC=R78). Solution thermodynamic modeling also indicates that fire suppression water buffered with a commercially-available phosphate buffer would significantly reduce the solubility of PuCl 3 by the precipitation of PuPO 4 .

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗