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Title: Solubility Control of Technetium Release from Saltstone by Tc02•xH20

Saltstone leaching experiments were conducted using a modified single-pass flow-through method under anoxic conditions. The analytical results of leachates collected from these experiments were evaluated using thermodynamic modeling to determine if the data were consistent with potential solubility controlling phases. The results demonstrate that technetium concentrations in water in contact with Saltstone under anoxic conditions is controlled by the solubility of TcO2•xH2O (likely TcO2•1.6H2O). In our system equilibrium solubility appears to have been reached within two weeks at a concentration of approximately 1.5 x 10-6 M. This concentration is likely to vary as the composition of Saltstone pore fluid evolves over time. As the pH goes from the initial high values (~12.5-13) to lower values, the solubility of technetium will decrease significantly. The thermodynamic data used to determine the solubility of TcO2•1.6H2O were taken from the tabulation of critically selected thermodynamic data determined by the Nuclear Energy Agency. Solid phase characterization to demonstrate the presence of TcO2•xH2O was not possible due to the low concentrations of technetium in our samples. Previous solid phase characterization studies with cementitious waste forms that were very similar to our Saltstone samples as well as reaction products derived from reductive immobilization of TcO4- by amorphousmore » FeS clearly indicate the presence of TcO2 with varying degrees of hydration. Although, the presence of TcSx or other reduced technetium sulfide phases in our samples cannot be ruled out, release of technetium from Saltstone will be controlled by TcO2•1.6H2O because of its higher solubility. Our results clearly demonstrate that the release mechanism of technetium from Saltstone under reducing conditions is solubility controlled by TcO2•xH2O (likely TcO2•1.6H2O); however, distribution coefficients (Kds), that describe sorption and not solubility, were calculated for comparison with past literature values. After 84 days of reaction under anoxic conditions, the average Kd value for technetium was determined to be 610 mL/g. This value is similar to a value determined previously for a similar saltstone sample under reducing conditions at 56 days (712 ± 81 mL/g).« less
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Resource Type:
Journal Article
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Journal Name: Journal of Nuclear Materials, 437(1-3):424-431
Research Org:
Pacific Northwest National Laboratory (PNNL), Richland, WA (US)
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Country of Publication:
United States
Saltstone; technetium; solubility; TcO2•xH2O; TcO2•1.6H2O