Surface Complexation Modeling of U(VI) Sorption to Hanford Sediment with Varying Geochemical Conditions

Abstract

A series of U(VI) sorption experiments with varying pH, ionic strength, concentrations of dissolved U(VI), and alkalinity was conducted to provide a more realistic database for U(VI) sorption onto near-field vadose zone sediments at the proposed Integrated Disposal Facility (IDF) on the Hanford Site, Washington. The distribution coefficient (Kd) for U(VI) in a leachate that is predicted to result from the weathering of vitrified wastes disposed in the IDF is 0 mL/g due to the high sodium and carbonate concentrations and high pH of the glass leachate. However, when the pH and alkalinity of the IDF sediment native pore water increases during mixing with the glass leachate, U(VI) uptake is observed and the value of the U(VI) Kd increases 4.3 mL/g, because of U(VI) coprecipitation with newly formed calcite. A nonelectrostatic, generalized composite approach for surface complexation modeling was applied and a combination of two U(VI) surface species, monodentate (SOUO2+), and bidentate (SO2UO2(CO3)2-), simulated the measured U(VI) sorption data very well. The generalized composite surface complexation model, when compared to the constant or single-valued Kd model, more accurately predicted U(VI) sorption under the varying geochemical conditions expected at the IDF.