Corrosion of Metal Inclusions In Bulk Vitrification Waste Packages

Abstract

The primary purpose of the work reported here is to analyze the potential effect of the release of technetium (Tc) from metal inclusions in bulk vitrification waste packages once they are placed in the Integrated Disposal Facility (IDF). As part of the strategy for immobilizing waste from the underground tanks at Hanford, selected wastes will be immobilized using bulk vitrification. During analyses of the glass produced in engineering-scale tests, metal inclusions were found in the glass product. This report contains the results from experiments designed to quantify the corrosion rates of metal inclusions found in the glass product from AMEC Test ES-32B and simulations designed to compare the rate of Tc release from the metal inclusions to the release of Tc from glass produced with the bulk vitrification process. In the simulations, the Tc in the metal inclusions was assumed to be released congruently during metal corrosion as soluble TcO4-. The experimental results and modeling calculations show that the metal corrosion rate will, under all conceivable conditions at the IDF, be dominated by the presence of the passivating layer and corrosion products on the metal particles. As a result, the release of Tc from the metal particles at the surfaces of fractures in the glass releases at a rate similar to the Tc present as a soluble salt. The release of the remaining Tc in the metal is controlled by the dissolution of the glass matrix. To summarize, the release of 99Tc from the BV glass within precipitated Fe is directly proportional to the diameter of the Fe particles and to the amount of precipitated Fe. However, the main contribution to the Tc release from the iron particles is over the same time period as the release of the soluble Tc salt. For the base case used in this study (0.48 mass% of 0.5 mm diameter metal particles homogeneously distributed in the BV glass), the release of 99Tc from the metal is approximately the same as the release from 0.3 mass% soluble Tc salt in the castable refractory block and it is released over the same time period as the salt. Therefore, to limit the impact of precipitated Fe on the release of 99Tc, both the amount of precipitated Fe in the BV glass and the diameter of these particles should be minimized.