Environmental context. Uranium-phosphate minerals have been identified as a long-term controlling phase that limit the mobility of uranium to groundwater in many contaminated subsurface environments. Complex, coupled processes confound the ability to isolate the rates attributed to individual processes. Results of this investigation provide the necessary information to refine current prediction on the release and long-term fate of uranium in subsurface environments. Abstract. The purpose of this investigation was to conduct a series of single-pass flow-through (SPFT) tests to (1) quantify the effect of temperature (23–90°C) and pH (6–10) on meta-torbernite dissolution; (2) compare the dissolution of meta-torbernite to other autunite-group minerals; and (3) evaluate the effect of aqueous phosphate on the dissolution kinetics of meta-torbernite. Results presented here illustrate meta-torbernite dissolution rates increase by ~100× over the pH interval of 6 to 10, irrespective of temperature. The power law coefficient for meta-torbernite, η = 0.59 ± 0.07, is greater than that quantified for Ca-meta-autunite, η = 0.42 ± 0.12. This suggests the stability of meta-torbernite is greater than that of meta-autunite, which is reflected in the predicted stability constants. The rate equation for the dissolution of meta-torbernite as a function of aqueous phosphate concentration is log rdissol (mol m–2 s–1) = –4.7 × 10–13 + 4.1 × 10–10[PO43–].
A laboratory testing program has been conducted to optimize polyphosphate remediation technology for implementation through a field-scale technology infiltration demonstration to stabilize soluble, uranium-bearing source phases in the vadose zone and capillary fringe. Source treatment in the deep vadose zone will accelerate the natural attenuation of uranium to more thermodynamically stable uranium-phosphate minerals, enhancing the performance of the proposed polyphosphate remediation within the 300 Area aquifer. The objective of this investigation was to develop polyphosphate remediation technology to treat uranium contamination contained within the deep vadose zone and capillary fringe. This chapter presents the results of an investigation that evaluated the rate and extent of reaction between polyphosphate and the uranium mineral phases present within the 300 Area, and autunite formation as a function of polyphosphate formulation and concentration. This information is critical for identifying the optimum implementation approach and controlling the flux of uranium to the underlying aquifer during remediation. Results from this investigation may be used to design a full-scale remediation of uranium at the 300 Area of the Hanford Site.
The objective of this investigation was to initiate numerous sets of concrete-soil half-cell tests to quantify 1) diffusion of I and Tc from concrete into uncontaminated soil after 1 and 2 years, 2) I and Re (set 1) and Tc (set 2) diffusion from fractured concrete into uncontaminated soil, and 3) evaluate the moisture distribution profile within the sediment half-cell. These half-cells will be section in FY2009 and FY2010. Additionally, 1) concrete-soil half-cells initiated during FY2007 using fractured prepared with and without metallic iron, half of which were carbonated using carbonated, were sectioned to evaluate the diffusion of I and Re in the concrete part of the half-cell under unsaturated conditions (4%, 7%, and 15% by wt moisture content), 2) concrete-soil half cells containing Tc were sectioned to measure the diffusion profile in the soil half-cell unsaturated conditions (4%, 7%, and 15% by wt moisture content), and 3) solubility measurements of uranium solid phases were completed under concrete porewater conditions. The results of these tests are presented.