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Long term plutonium solubility and speciation studies in a synthetic brine

Novak, Craig F.

The rate at which elements can be transported in groundwater systems is governed in part by the solubility of the element in the groundwater. This report documents plutonium solubility experiments in a brine simulant relevant to the Waste Isolation Pilot Plant. Approximately 1 to 2.5 mL of five stock solutions containing single oxidation states of plutonium (Pu(IV)-polymer, Pu{sup 3+}, Pu{sup 4+}, PuO{sub 2}{sup +}, and PuO{sub 2}{sup 2+}) were added to {approximately}75 mL of synthetic H-17 Brine in five reaction vessels. Initial plutonium concentrations ranged from 1.3 {times} l0{sup {minus}4} to 5.l {times} l0{sup {minus}4} M (moles per liter) total plutonium. Because these initial concentrations were far above the plutonium solubility limit in H-17 Brine, plutonium-containing solids precipitated. Aqueous plutonium concentrations were measured over time until steady-state was reached, requiring over 300 days in H-17 Brine.