Uranium(VI) Adsorption and Surface Complexation Modeling onto Background Sediments from the F-Area Savannah River Site

The mobility of an acidic uranium waste plume in the F-Area of Savannah River Site is of great concern. In order to understand and predict uranium mobility, U(VI) adsorption experiments were performed as a function of pH using background F-Area aquifer sediments and reference goethite and kaolinite (major reactive phases of F-Area sediments), and a component-additivity (CA) based surface complexation model (SCM) was developed. Our experimental results indicate that the fine fractions (≤45 μm) in sediments control U(VI) adsorption due to their large surface area, although the quartz sands show a stronger adsorption ability per unit surface area than the fine fractions at pH < 5.0. Kaolinite is a more important sorbent for U(VI) at pH < 4.0, while goethite plays a major role at pH > 4.0. Our CA model combines an existing U(VI) SCM for goethite and a modified U(VI) SCM for kaolinite along with estimated relative surface area abundances of these component minerals. The modeling approach successfully predicts U(VI) adsorption behavior by the background F-Area sediments. The model suggests that exchange sites on kaolinite dominate U(VI) adsorption at pH < 4.0, goethite and kaolinite edge sites cocontribute to U(VI) adsorption at pH 4.0-6.0, and goethite dominates U(VI) adsorption at pH > 6.0.