Spectroscopic and Microscopic Characterization of Contaminant Uptake and Retention by Carbonates in the Soil and Vadose Zone

The research focus of this previous EMSP grant was assessment of the role that carbonate minerals play in the uptake and sequestration of metal and radionuclide contaminants in soils and the vadose zone for conditions relevant to the Hanford Site and other sites in the DOE Complex. The project was a collaboration among researchers at SUNY-Stony Brook and EMSL/PNNL. Carbonates, particularly calcite, are present in the Hanford subsurface as grain coatings, disseminated particles, and dense caliche layers. Calcite is also predicted to be forming beneath leaking tanks. A range of metal and radionuclide species that pose risks at Hanford and othe DOE istes were considered, including u(VI), Cr(CV), Cs, Pb(II), and selected lanthanides (as models for trivalent actinides). Batch sorption and co-precipitation experiments of these metals with pre-equilibrated calcite and selected uptake experiments on natural caliche formed the basis to determine the mechanisms of metal/radionuclide binding and to assess the effect on the stability of the sorbed species and the potential for remobilization. Our results provide ne information that can benefit DOE clean-up methodology and potentially provide new approaches for uptake of selected heavy metal