Date: March 21, 2009
Creator: O'Day, Peggy A.; Chorover, Jon; Mueller, Karl; Steefel, Carl & Serne, R. Jeff
Description: The goal of our project is a predictive-mechanistic understanding of the coupling between mineral weathering and contaminant (Cs, Sr, I) fate in caustic waste-impacted sediments at the Hanford Site. Through bench-scale experiments, we have identified geochemical transformations that alter the mobility of priority pollutants (Cs, Sr, I) in subsurface environments characteristic of high-level radioactive waste (HLRW)-impacted DoE sites. Our studies are designed to model the unique chemistry of this subsurface contamination, to quantify rates of contaminant uptake and release, and to identify molecular mechanisms of time-dependent, irreversible sequestration of contaminants into the solid phase. Our approach is to link quantitative macroscopic measures of contaminant mobility and partitioning to the molecular-scale mechanisms that mediate them. We have found that the molecular mechanisms themselves change with time and system composition in response to the evolving chemistry of contaminant-solution-mineral interactions. Specifically, our results show that contaminant fate is closely coupled to the major silicate incongruent weathering reactions that occur when soil solids are contacted with aqueous solutions under conditions that are far from equilibrium. Neoformed precipitates - including carbonate, feldspathoid and zeolite phases, have been observed to sequester Cs and Sr under caustic waste conditions. In contrast, iodide is less effectively sequestered into ...
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