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Title: High-temperature leaching of an actinide-bearing, simulated high-level waste glass

Technical Report ·
DOI:https://doi.org/10.2172/6494366· OSTI ID:6494366

The chemical durability of a simulated high-level waste glass when exposed to high-temperature geologic solutions was investigated. In this study, simulated high-level waste glass-beads (76 to 68 glass)l doped with technetium, uranium, neptunium, plutonium, curium and americium were leached in deionized water, Waste Isolation Pilot Plant salt brine B, and 0.03M sodium bicarbonate solution at 150 and 250/sup 0/C for 2, 4, 8, 16, and 32 days. The resulting solutions were analyzed for several nonradioactive glass components and for the radioactive dopants. The glass exhibited incongruent leaching behavior, i.e., the normalized releases (g-glass/m/sup 2/) based on the different elements spanned four orders of magnitude. Normalized releases based on boron, molybdenum, sodium, cesium, silicon, and technetium were the same within a factor of three. Most of the nonradioactive components of the glass were released more to the salt brine than to the other two solutions. However, silicon, boron, molybdenum, technetium, and the actinides had their lowest releases in the salt brine. Reaction-layer thickness on the glass surface and weight losses of the glass beads were also smallest in the brine solution. Actinide releases were highest in the sodium bicarbonate solution. Calcium, strontium and barium releases decreased with time and temperature; the releases of most other elements increased with time and temperature. Solubility appears to be limiting the release of most elements. The leachate pH is controlled by chemical species within the original leachant and by species released as the glass leached. Carbonate ion complexes with some elements including uranium, effectively increasing their release. The more soluble elements including sodium, boron, molybdenum and technetium provide an indication of the actual rate of reaction between the glass and water.

Research Organization:
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
DOE Contract Number:
AC06-76RL01830
OSTI ID:
6494366
Report Number(s):
PNL-3172; ON: DE83008755
Resource Relation:
Other Information: Portions are illegible in microfiche products. Original copy available until stock is exhausted
Country of Publication:
United States
Language:
English