Column-Test Data Analyses and Geochemical Modeling to Determine Uranium Reactive Transport Parameters at a Former Uranium Mill Site (Grand Junction, Colorado)

Abstract

The long-term release of uranium from residual sources at former uranium mill sites was often not considered in prior conceptual and numerical models, as contaminant removal focused on meeting radiological standards. To determine the reactive transport parameters, column tests were completed with various influent waters (deionized water, site groundwater, and local river water) on sediment from identified areas with elevated uranium on the solid phase in (1) vadose-zone (VZ) sediments, (2) saturated-zone sediments with higher organic carbon content, and (3) both vadose- and saturated-zone sediments with additional gypsum content. The gypsum was precipitated when low-pH, high-sulfate, tailings fluids or acidic waste disposal water were buffered by natural aquifer calcite dissolution. In general, the resulting uranium release was higher in the sediments with greater uranium concentrations. However, the addition of deionized water (DI) to the VZ sediments delayed the uranium release until higher-alkalinity groundwater was added. Higher-alkalinity river water continued to remove uranium from the VZ sediments for an extended number of pore volumes, with the uranium being above typical standards. Thus, river flooding is more efficient at removing uranium from VZ sediments than precipitation events (DI water in column tests). Organic carbon provides a stronger uranium sorption surface, which can be explained with geochemical modeling or a larger constant sorption coefficient (Kd). Without organic carbon, the typical sorption in sands and gravels is easily measurable, but sorption is stronger at lower, water-phase uranium concentrations. This effect can be simulated with geochemical modeling, but not with a constant Kd. Areas with gypsum create situations in which geochemical sorption is more difficult to simulate, which is likely due to the presence of uranium within mineral coatings. All the above mechanisms for uranium release must be considered when evaluating remedial strategies. Column testing provides initial input parameters that can be used in future reactive transport modeling to evaluate long-term uranium release rates and concentrations.