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Hydrothermal reaction of simulated waste forms with barrier materials under conditions expected in a nuclear waste repository in basalt

Technical Report ·
OSTI ID:5201562
Simulated spent fuel, simulated defense high-level waste, and simulated and {sup 99}Tc-doped commercial high-level waste (PNL 76-68) were reacted with groundwater, both in the presence and absence of basalt, simulating expected conditions for a nuclear waste repository located in basalt at the Hanford Site, Washington. Experiments were performed in gold bag sampling autoclaves at temperatures between 90{degree}C and 300{degree}C, at 30 megapascals pressure. During the course of the experiments, samples of the fluid phase were periodically withdrawn from the autoclaves and were analyzed for pH as well as major, minor, and trace cations and anions. At 200{degree}C and 300{degree}C, all dissolved species displayed either steady-state concentrations or decreasing concentrations after the first 1,000 hrs. At 100{degree}C, some dissolved components had not reached steady-state concentrations after 6000 hr. Solids characterization suggests that the formation of secondary alteration phases such as alkali feldspar, smectite clays, scapolite, and a variety of uranium-bearing silicate phases, imposes solubility limits on the release of many analog elements of potential radionuclides. These steady-state (or solubility) concentration limits can be coupled with measured hydrologic flow rates to calculate radionuclide release rates from the waste form for a nuclear waste repository located in basalt.
Research Organization:
Rockwell International Corp., Richland, WA (USA). Rockwell Hanford Operations
Sponsoring Organization:
DOE/RW
DOE Contract Number:
AC06-77RL01030
OSTI ID:
5201562
Report Number(s):
RHO-BWI-TI-141; ON: TI90005859
Country of Publication:
United States
Language:
English

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