PNNL

Abstract

A series of U(VI) adsorption experiments with varying pH, ionic strength, concentrations of dissolved U(VI) and carbonate was conducted to provide a more realistic database for U(VI) adsorption onto near-field vadose zone sediments at the proposed Integrated Disposal Facility (IDF) on the Hanford Site. The distribution coefficient, Kd, for U(VI) in predicted “pure” glass leachate is 0 mL/g because the glass leachate has high sodium and carbonate concentrations and high pH. The zero adsorption result suggests that uranium will exhibit no retardation when the subsurface geochemistry is controlled by glass leachate. However, U(VI) can be sequestrated even when the pH, carbonate and sodium concentrations reached levels similar to “pure” glass leachate, because U(VI) coprecipitates with calcite. When glass leachate interacts with existing porewater or surrounding sediments, sorption is observed and the numerical value of the U(VI) Kd varies significantly. A non-electrostatic, general 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 very well the measured U(VI) adsorption data. The general composite surface complexation model, compared to the constant or single-valued Kd model, more accurately predicted U(VI) adsorption under the varying geochemical conditions expected at the IDF.