Evaluation of DOE radionuclide solubility data and selected retardation parameters: description of calculational and confirmatory experimental activities

An experimentally oriented program has been initiated to support the NRC analysis and licensing activities related to high-level nuclear waste repositories. The program will allow the NRC to independently confirm key geochemical values used in the site performance assessments submitted by the DOE candidate repository site projects. Key radionuclide retardation factor values, particularly radionuclide solubility and sorption values under site specific geochemical conditions, are being confirmed. The initial efforts are being directed toward basalt rock/groundwater systems relevant to the BWIP candidate site in the Pasco Basin. Future work will consider tuff (NNWSI candidate site in Yucca Mountain) and salt (unspecified ONWI bedded or domal salt sites) rock/groundwater systems. Initial experimental results with technetium have confirmed the BWIP values for basalt/groundwater systems under oxic redox conditions: high solubility and no sorption. Under reducing redox conditions, however, the experimental work did not confirm the proposed technetium values recommended by BWIP. In the presence of hydrazine to establish reducing conditions, an apparent solubility limit for technetium of about 5E-7 mol/L was encountered; BWIP recommended calculated values of 1E-12 or greater than or equal to 1E-14 mol/L. Experimental evidence concerning sorption of reduced technetium species is incomplete at this time. Equilibrium speciation and saturation indices were calculated for well water data sets from BWIP using the computer code PHREEQUE. Oversaturation was indicated for hematite and quartz in all data sets. Near surface samples were undersaturated with respect to calcite, but most deep samples were oversaturated with respect to calcite and other carbonate minerals