Solubility and speciation results from over- and undersaturation experiments on neptunium, plutonium, and americium in water from Yucca Mountain region well UE-25p number-sign 1

Solubility and speciation are important in understanding aqueous radionuclide transport through the geosphere. Results are compared from solubility and speciation experiments from oversaturation and undersaturation of 237NpO2+, 239Pu4+, and 241Am3+/Nd3+ in a modified UE-25p-1 groundwater (from the Yucca Mountain region, Nevada, which is being investigated as a potential high-level nuclear waste disposal site) at 60 C and three pH values (6.0, 7.0, 8.5). In the oversaturation experiments, the solubility-controlling steady-state solids were identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The characterized solids were then reintroduced into fresh solutions of the modified UE-25p-1 groundwater to approach the steady state from undersaturation. For the undersaturation experiments, the solubility-controlling steady-state solids were also identified and the speciation and/or oxidation states present in the supernatant solutions were determined. The Np solubility decreased with increasing pH in both the over- and undersaturation experiments. The steady-state concentrations from the two experiments agreed to within an order of magnitude. Pu concentrations from over- and undersaturation agree very well in the pH 6 and 7 experiments. The pH 8.5 oversaturation experiment resulted in a steady-state concentration one order of magnitude above its undersaturation counterpart. For the Am/Nd solutions, the pH 6 and pH 7 experiments resulted in equivalent steady-state concentrations from both over and undersaturation. The pH 8.5 oversaturation experiment was 100 times more soluble than its undersaturation counterpart. 48 refs