PNNL

Abstract

High level nuclear wastes (HLW) from Hanford’s plutonium reprocessing are stored in massive, buried, single-shell tanks in eighteen tank farms. The wastes were initially hot because of radioactive decay, and many exhibited extreme chemical character in terms of pH, salinity, and radionuclide concentration. At present, 67 of the 149 single shell tanks are suspected to have released over 1.9 million L of tank waste to the vadose zone, with most leak events occurring between 1950 and 1975. Boreholes have been placed through the largest vadose zone plumes to define the extent of contaminant migration, and to develop conceptual models of processes governing the transformation, retardation, and overall transport of tank waste residuals. Laboratory studies with sediments so collected have shown that ion exchange, precipitation and dissolution, and surface complexation reactions have occurred between the HLW and subsurface sediments moderating their chemical character, and retarding the migration of select contaminants. Processes suspected to facilitate the far-field migration of immobile radionuclides including stable aqueous complex formation and mobile colloids were found to be potentially operative, but unlikely to occur in the field, with the exception of cyanide-facilitated migration of 60Co. Fission product oxyanions are the most mobile of tank waste constituents because their adsorption is suppressed by large concentrations of waste anions; the vadose zone clay fraction is negative in surface charge; and, unlike Cr, their reduced forms are unstable in oxidizing environments. Reaction/process-based transport modeling is beginning to be used for predictions of future contaminant mobility and plume evolution.