PNNL

Abstract

The inhibitory effect of phosphate mineral precipitation on uranium release was evaluated using a U(VI)-contaminated sediment collected from the US Department of Energy (DOE) Hanford site. The sediment contained U(VI) that was associated with diffusion-limited intragrain regions within its mm-size granitic lithic fragments. The sediment was first treated to promote phosphate mineral precipitation in batch suspensions spiked with 1 and 50 mM aqueous phosphate, and calcium in a stoichiometric ratio of mineral hydroxyapatite. The phosphate-treated sediment was then leached to solubilize contaminant U(VI) in a column system using a synthetic groundwater that contained chemical components representative of Hanford groundwater. Phosphate treatment significantly decreased the extent of U(VI) release from the sediment. Within the experimental duration of about 200 pore volumes, the effluent U(VI) concentrations were consistently lower by over one and two orders of magnitude after the sediment was treated with 1 and 50 mM of phosphate, respectively. Measurements of solid phase U(VI) using various spectroscopes and chemical extraction of the sediment collectively indicated that the inhibition of U(VI) release from the sediment was caused by: 1) U(VI) adsorption to the secondary phosphate precipitates and 2) the transformation of initially present U(VI) mineral phases to less soluble forms.