Measured Solubilities and Speculations from Oversaturation Experiments of Neptunium, Plutonium, and Americium in UE-25p No. 1 Well Water from the Yucca Mountain Region PDF Download
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Languages : en
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Languages : en
Pages : 103
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Solubility and speciation are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are a part of predictive transport models. Results are presented from solubility and speciation experiments of 237NpO2, 239Pu{sup 4+}, and 241Am{sup 3+}/Nd{sup 3+} in a modified UE-25p No. 1 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at two different temperatures (25° and 60°C) and three pH values (6.0, 7.0, 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations significantly decreased with increasing temperature at pH 6 and 7. The concentration at pH 8.5 hardly decreased at all with increasing temperature. At both temperatures the concentrations were highest at pH 8.5, lowest at pH 7, and in between at pH 6. For the americium/neodymium solutions, the solubility decreased significantly with increasing temperature and increased somewhat with increasing pH.
Author: Heino Nitsche
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Category : Americium
Languages : en
Pages : 95
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Author: Heino Nitsche
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Category : Americium
Languages : en
Pages : 144
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Languages : en
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Languages : en
Pages : 127
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Solubility and speciation data are important in understanding aqueous radionuclide transport through the geosphere. They define the source term for transport retardation processes such as sorption and colloid formation. Solubility and speciation data are useful in verifying the validity of geochemical codes that are part of predictive transport models. Results are presented from solubility and speciation experiments of 237NpO2, 239Pu{sup 4+}, 241Am{sup 3+}/Nd{sup 3+}, and 243Am{sup 3+} in J-13 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at three different temperatures (25°, 60°, and 90°C) and pH values (5.9, 7.0, and 8.5). The solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The neptunium solubility decreased with increasing temperature and pH. Plutonium concentrations decreased with increasing temperature and showed no trend with pH. The americium solutions showed no clear solubility trend with increasing temperature and increasing pH.
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Category : Power resources
Languages : en
Pages : 782
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Languages : en
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Category : Science
Languages : en
Pages : 660
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Languages : en
Pages : 2
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The total system performance assessment (TSPA) for the proposed repository at Yucca Mountain, NV, includes a wide variety of processes to evaluate the potential release of radionuclides from the Engineered Barrier System into the unsaturated zone of the geosphere. The principal processes controlling radionuclide release and mobilization from the waste forms are captured in the model to assess the dissolved concentrations of radionuclides in the source-term. The TSPA model of the source-term incorporates the far-from-equilibrium dissolution of, for example, spent nuclear fuel (SNF) to capture bounding rates of radionuclide availability as the SNF degrades. In addition, for individual radionuclides, the source-term model evaluates solubility constraints that are more indicative of longer-term, equilibrium processes that can limit the potential mass transport from the source term in those cases. These solubility limits represent phase saturation and precipitation processes that can occur either at the waste form as it alters, or at other locations in the near-field environment (e.g., within the invert) if chemical conditions are different. Identification and selection of applicable constraints for solubility-limited radionuclide concentrations is a primary focus in formulating the source-term model for the TSPA. Neptunium is a long-lived radionuclide that becomes a larger fraction of the potential dose as radioactive decay of other radionuclides proceeds. To delineate appropriate long-term source-term controls on dissolved neptunium concentrations, a number of alternative models have been defined. The models are based on data both collected within the Yucca Mountain Project and taken from published literature, and have been evaluated against independent data sets to assess their applicability. The alternative models encompass ones based on precipitation of neptunium within its own separate oxide phases (i.e., ''pure'' Np-phases), and those where neptunium is incorporated into the secondary (tertiary, quaternary, etc.) uranyl phases forming as alteration products of SNF (secondary phases). The constraints on dissolved neptunium concentrations from ''pure'' Np-phase models provide more elevated bounds compared to the values derived from models of trace incorporation of Np into secondary uranyl phases. Such secondary phase models depend on a larger set of processes and variables compared to more idealized solubility models for Np-oxides, and therefore, secondary phase models generally will have more complex bases to define adequately the expected behavior.
