Aqueous Thermodynamics and Complexation Reactions of Anionic Silica and Uranium Species to High Concentration. Annual Report, June 1, 2002-May 31, 2003.
Highly basic tank wastes contain several important radionuclides, including 90Sr, 99Tc, and 60Co, as well as actinide elements (i.e., isotopes of U, Pu, and Am). These highly basic tank wastes are known to have leaked into the vadose zone at the Hanford Site. Upon entering the sediments in the vadose zone, the highly basic solutions dissolve large concentrations of silica from the silica and aluminosilicate minerals present in the subsurface. These dissolution reactions alter the chemical composition of the leaking solutions, transforming them from a highly basic (as high 2M NaOH) solution into a pore solution with a very high concentration of dissolved silica and a significantly reduced pH. This moderately basic (pH 9 to 11), high-silica solution has the potential to complex radionuclides and move through the subsurface. Such strong radionuclide complexation is a currently unconsidered transport vector that has the potential to expedite radionuclide transport through the vadose zone. These strong complexation effects have the ability to significantly alter current conceptual models of contaminant migration beneath leaking tanks. In this project, we are determining the aqueous thermodynamics and speciation of dissolved silica and silica-radionuclide complexes to high silica concentration. We are also initiating studies of U(VI) speciation under strongly basic conditions.
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