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Investigation of the Hydrothermal Interaction of 99Tc-Doped Glass with Basalt Repository Nuclear Waste Package Components

Published online by Cambridge University Press:  26 February 2011

David G. Coles
Affiliation:
Pacific Northwest Laboratory, Richland, WA 99352
S. A. Simonson
Affiliation:
Pacific Northwest Laboratory, Richland, WA 99352
L. E. Thomas
Affiliation:
Westinghouse-Hanford Co., Richland, WA 99352
J. A. Schranke
Affiliation:
Pacific Northwest Laboratory, Richland, WA 99352
S. G. McKinley
Affiliation:
Pacific Northwest Laboratory, Richland, WA 99352
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Abstract

Hydrothermal experiments using basalt-repository nuclear waste package components have been carried out at 200°C and 30 MPa using 99Tc-doped PNL 76–68 waste glass. This work was conducted in support of the Basalt Waste Isolation Project. The experiments were carried out in rocking autoclaves that allowed for periodic solution sampling. Preliminary results that illustrated the effect of basalt on 99Tc solution behavior were discussed previously[l]. In this paper, we continue those observations by discussing the additional experiments that investigated the effects of steel. We also include the post-experiment solid phase analyses from all test configurations.

The effect of steel on glass dissolution was observed to be minimal when basalt was not present, i.e., there were no discernible differences in the amount of glass dissolved (based on boron release), with or without steel present.

The 99Tc solution concentration results showed that basalt, steel, and a combination of basalt and steel have an ability to dramatically lower the concentration of 99Tc in the solution, probably through a redox mechanism[2]. Solid run product analyses showed that without basalt present, a gel-like secondary phase consisting of an iron, zinc clay with an apparent smectite structure formed. When basalt was present clinoptilolite formed as the major secondary phase, due primarily to the presence of aluminum in the basalt mesostasis. Separation of the various solid run products and residual initial solid phases has not yet been achieved. Such a separation would facilitate the identification of the phase or phases with which 99Tc was associated. The solution results indicated that 99Tc, a potentially mobile radionuclide, may be incorporated in a relatively insoluble phase in the environment of a basalt repository. In addition, no synergistic effects between waste package components were observed that would increase the concentration of 99Tc in solution.

Type
Research Article
Copyright
Copyright © Materials Research Society 1985

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References

1. Coles, D.G. and Apted, M. J.. 1983. “The Behavior of 99Tc in Doped-Glass/Basalt Hydrothermal Interaction Tests”, in the Proceedings of the November 1983 Materials Research Society Symposium D, Scientific Basis for Nuclear Waste Management VII, edited by McVay, G. L., p. 129136.Google Scholar
2. Jantzen, C.M., 1983. “Methods of Simulating Lower Redox Potential (Eh) for a Basalt Repository”, in the Proceedings of the November 1983 Materials Research Society Symposium D, Scientific Basis for Nuclear Waste Management VII, edited by McVay, G. L., p. 613–621.CrossRefGoogle Scholar
3. M.J., Smith et al. 1980. “Engineered Barrier Development for a Nuclear Waste Repository Located in Basalt: An Integration of Current Knowledge”, RHO-BWI-ST-7, Rockwell Hanford Operations, Richland, Washington.Google Scholar
4. Apted, M.J. 1982. “Overview of Hydrothermal Testing of Waste Package Barrier Materials at the Basalt Waste Isolation Project”, RHOBW-SA-228, Rockwell Hanford Operations, Richland, WA and PNL-4382, Pacific Northwest Laboratory, Richland, Washington.Google Scholar
5. Chambre, P. L., Pigford, T. H., and Zavosky, S.. 1982. Solubility-Limited Dissolution Rate in Groundwater, UCB-NE-4016, University of California, Berkeley, California.Google Scholar
6. Myers, J. et al. 1983. “Hydrothermal Reaction of Simulated WasteForms with Barrier Materials under Conditions Expected in a Nuclear Waste Repository in Basalt”. SD-BWI-TI-141, Rockwell Hanford Operations, Richland, Washington.Google Scholar
7. Coles, D.G. 1983. “The Effect of Basalt on the Release of 99Tc, 237Np, and 239Pu from Borosilicate Glass under Hydrothermal Conditions”. SD-BWI-TI-190. Rockwell Hanford Operations, Richland, Washington.Google Scholar
8. Jones, T.E. 1982. Reference Material Chemistry, Synthetic Groundwater Formulation. RHO-BW-ST-37P, Rockwell Hanford Operations, Richland, Washington.Google Scholar
9. Meyer, R. E., Arnold, W. D., and Case, F. I.. 1984. “Valence Effects on the Sorption of Nuclides on Rocks and Minerals”, Oak Ridge National Laboratory Report ORNL-5978, and NRC Report NUREG/CR-3389.Google Scholar
10. Jensen, B. S. 1982. Migration Phenomena of Radionuclides into the Geosphere, Harwood Academic Publishers, London.Google Scholar
11. Benson, L. V. and Teague., L. S. 1979. A Study of Rock-Water-Nuclear Waste Interactions in the Pasco Basin, Washington. LBL-9677, Lawrence Berkeley Laboratory, Berkeley, California.Google Scholar