Leaching of fully radioactive high-level waste glass

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Abstract
As part of continuing Department of Energy (DOE)-sponsored studies in waste management, the Pacific Northwest Laboratory (PNL) has been conducting the High-Level Waste Immobilization Program. The purpose of this program is to develop and demonstrate technology for incorporating nuclear wastes into final waste forms. The preparation and leach testing of fully radioactive, zinc borosilicate glass, which was prepared from power reactor waste, are described. Leach testing using the International Atomic Energy Association (IAEA) procedure was performed in deionized water for a period of 1.75 years. Leach rates were determined for activation products, fission products, and actinides. These rates ranged from 4 x 10/sup -5/ g of glass/cm/sup 2/-day, based on cesium, to 4 x 10/sup -9/ g of glass/cm/sup 2/-day, based on cerium. Following is the ranking of the release rates of the elements, from highest to lowest: Cs > Sr > Co > Sb > Mn > Pu > Eu > Rh > Cm > Ce. A similar leach test, using the same glass composition but with nonradioactive elements, has recently been completed. The leach rates of Cs and Sr for the nonradioactive glass were found to be in close agreement with those in this study. Slopes calculated frommore » curves of cumulative fractions leached show that radioisotope release begins with a diffusion-type mechanism and changes gradually to a silicate lattice alteration mechanism. Changes in sampling frequency altered the apparent release mechanism when leachant changes were longer than one month. The leach rates were quite constant for samples taken from the top to the bottom of the glass melt, indicating a homogeneous product. Safety assessment studies and modeling programs use leach rates to predict the amount of radioactive material released should the waste be contacted by aqueous solutions. Further tests, focusing on geologic storage conditions and using fully radioactive wastes, are planned. « less

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