Uranium Release from Acidic Weathered Hanford Sediments: Single-Pass Flow-Through and Column Experiments

Abstract

The reaction of acidic radioactive waste with sediments can induce mineral transformation reactions that, in turn, control contaminant fate. Here, sediment weathering by synthetic uranium containing acid solutions was investigated using bench-scale experiments to simulate waste disposal conditions at Hanford's cribs (Hanford, WA). During acid weathering, the presence of phosphate exerted a strong influence over uranium mineralogy and a rapidly precipitated, crystalline uranium phosphate phase (meta-ankoleite [K(UO2)(PO4).3H(2)O] was identified using spectroscopic and diffraction-based techniques. In phosphate-free system, uranium oxyhydroxide minerals such as K-compreignacite [K-2(UO2)(6)O-4(OH)(6).7H(2)O] were formed. Single-pass flow-through (SPFT) and column leaching experiments using synthetic Hanford pore water showed that uranium precipitated as meta-ankoleite during acid weathering was strongly retained in the sediments, with an average release rate of 2.67 X 10(-12) mol g(-1) s(-1). In the absence of phosphate, uranium release was controlled by dissolution of uranium oxyhydroxide (compreignacitetype) mineral with a release rate of 1.05-2.42 X 10(-1) mol g(-1) s(-1). The uranium mineralogy and release rates determined for both systems in this study support the development of accurate U-release models for the prediction of contaminant transport. These results suggest that phosphate minerals may be a good candidate for uranium remediation approaches at contaminated sites.