Hostname: page-component-8448b6f56d-wq2xx Total loading time: 0 Render date: 2024-04-15T09:05:31.268Z Has data issue: false hasContentIssue false

Modelling of Waste Form Performance and System Release

Published online by Cambridge University Press:  26 February 2011

Aaron Barkatt
Affiliation:
Vitreous State LaboratoryThe Catholic University of AmericaWashington, D.C. 20064
Pedro B. Macedo
Affiliation:
Vitreous State LaboratoryThe Catholic University of AmericaWashington, D.C. 20064
Barbara C. Gibson
Affiliation:
Vitreous State LaboratoryThe Catholic University of AmericaWashington, D.C. 20064
Charles J. Montrose
Affiliation:
Vitreous State LaboratoryThe Catholic University of AmericaWashington, D.C. 20064
Get access

Abstract

Kinetic and thermodynamic approaches to the derivation of long-term release rates of species from defense waste glass are reviewed. It is concluded that at high flow rates kinetic factors are pre-dominant, while at low flow rates saturation of the aqueous medium with respect to major matrix elements, particularly with respect to silica present in the glass and in its alteration products, becomes a controlling factor. Quantitative calculations indicate that under likely repository conditions the release rates can be expected, in general, to fall below the NRC criterion of 10−5 yr−1.

Type
Research Article
Copyright
Copyright © Materials Research Society 1985

Access options

Get access to the full version of this content by using one of the access options below. (Log in options will check for institutional or personal access. Content may require purchase if you do not have access.)

References

1. United States Nuclear Regulatory Commission Rules and Regulations, Title 10, Chapter 1, Code of Federal Regulations - Energy, Part 60 - Disposal of High-level Radioactive Wastes in Geologic Repositories, paragraph 60.111 - Performance Objectives, Federal Register, July 24 (1981).Google Scholar
2. Godbee, H. W. and Joy, D. S., Assessment of the Loss of Radioactive Isotopes from Waste Solids to the Environment. Part I: Background and Theory, ORNL-TM-4333, Oak Ridge National Laboratory, Oak Ridge, Tennessee (1974).Google Scholar
3. Machiels, A. J. and Pescatore, C., Modeling of Waste Form Leaching. Part II: Mechanistic Modeling of Nuclear Waste Form Leaching by Aqueous Solutions. Technical Report UILU-ENG-82–5360, University of Illinois, Urbana, Illinois (1974); or ONWI/E512–06000−2, Office of Nuclear Waste Isolation, Columbus, Ohio (1982).Google Scholar
4. Kuhn, W. L. and Peters, R. D., “Leach Models for a Commercial Nuclear Waste Glass”, in Scientific Basis for Nuclear Waste Management, Vol. VI, Brookins, D. G., ed., North-Holland, New York, pp. 167174 (1982).Google Scholar
5. Harvey, K., “A Semiunified Approach to Leach Testing of Nuclear Waste Forms”, Nucl. Chem. Waste Manage., 4, 201205 (1983).Google Scholar
6. Wallace, R. M. and Wicks, G. G., “Leaching Chemistry of Defense Borosilicate Glass”, in Scientific Basis for Nuclear Waste Management, Vol. VI, Brookins, D. G., ed., North-Holland, New York, pp. 23–28.Google Scholar
7. Plodinec, M. J., Jantzen, C. J. and Wicks, G. G., “A Thermodynamic Approach to Prediction of the Stability of Proposed Radwaste Glasses”, DP-MS-82−66, Savannah River Laboratory, Aiken, South Carolina (1982).Google Scholar
8. Grambow, B., “The Role of Metal Ion Solubility in the Leaching of Nuclear Waste Glasses”, in Scientific Basis for Nuclear Waste Management, Vol. V, Lutze, W., ed., North-Holland, New York, pp. 93102 (1982).Google Scholar
9. Chambre, P. L., Pigford, T. H., Fujita, A., Kanki, T., Kobayashi, R., Lung, H., Ting, D., Sato, Y. and Zavoshy, S. J., Analytical Performance Models for Geologic Repositories, LBL-14842, Lawrence Berkeley Laboratory, University of California, Berkeley, California (1982).Google Scholar
10. Macedo, P. B., Barkatt, Aa. and Simmons, J. H., “A Flow Model for the Kinetics of Dissolution of Nuclear Waste Glasses”, Nucl. Chem. Waste Manage., 3, 1321 (1982).Google Scholar
11. Barkatt, Aa., Macedo, P. B., Sousanpour, W., Barkatt, Al., Boroomand, M. A., Fisher, C. F., Shirron, J. J., Szoke, P. and Rogers, V. L., “The Use of a Flow Test and a Flow Model in Evaluating the Durability of Various Nuclear Waste-form Materials”, Nucl. Chem. Waste Manage., 4, 153169 (1983).Google Scholar
12. Hughes, A. E., Marples, J. A. C. and Stoneham, A. M., “The Significance of Leach Rates in Determining the Release of Radioactivity from Vitrified Nuclear Waste”, Nucl. Tech., 61, 496502 (1983).Google Scholar
13. Montrose, C. J., Macedo, P. B. and Barkatt, Aa., “Phenomenological Models of Nuclear Waste Glass Leaching”, Nucl. Tech., to be published.Google Scholar
14. Barkatt, Aa., Sousanpour, W., Barkatt, Al., Boroomand, M. A. and Macedo, P. B., “Leach Behavior of SRL TDS-131 Defense Waste Glass in Water at High/Low Flow Rates”, in Scientific Basis for Nuclear Waste Manaqement, Vol. VII, McVay, G. L., ed., North-Holland, New York, pp. 643653 (1984).Google Scholar
15. Apted, M. J. and Adiga, R., “The Role of Groundwater Flow in Release Rate Behavior of Borosilicate Glass”, this volume.Google Scholar
16. Aa. Barkatt, Macedo, P. B., Sousanpour, W., Barkatt, Al., Boroomand, M. A., Rogers, V. L., Nazari, A., Pimenov, G. and Shirron, J. J., “Leach Mechanisms of Borosilicate Glass Defense Waste Forms A Effects of Composition” in Waste Management '84, Vol.1, Arizona Board of Regents, Tucson, Arizona, pp. 627631 (1984).Google Scholar
17. Apted, M. J., “Overview of Hydrothermal Testing of Waste Package Barrier Materials at the Basalt Waste Isolation Project”, in Materials Characterization Center Workshop on Leaching Mechanisms of Nuclear Waste Forms, Mendel, J. E., ed., PNL-4382, Pacific Northwest Laboratory, Richland, Washington, pp. 161181 (1982).Google Scholar
18. Barkatt, Aa., Macedo, P. B., Sousanpour, W., Boroomand, M. A., Szoke, P. and Rogers, V. L., “Aluminosilicate Saturation as a Solubility Control in Leaching of Nuclear Waste-form Materials”, in Materials Characterization Center Workshop on Leaching Mechanisms of Nuclear Waste Forms, Mendel, J. E., ed., PNL-4382, Pacific Northwest Laboratory, Richland, Washington, pp. 2040 (1982).Google Scholar
19. Bates, J. K. and Steindler, M. J., “Alteration of Nuclear Waste Glass by Hydration”, in Scientific Basis for Nuclear Waste Management, Vol. VI,Brookins, D. G., ed., North-Holland, New York, pp. 8390 (1983).Google Scholar
20. Harker, A. B. and Flintoff, J. F., “Mechanisms of Enhanced Dissolution in Nuclear Waste Glasses”, this volume.Google Scholar
21. Barkatt, Aa., Gibson, B. C. and Brandys, M., “A Kinetic Model of Nuclear Waste Glass Dissolution in Flowing Water Environments”, this volume.Google Scholar
22. Gray, W. J., McVay, G. L., Barner, J. O., Shade, J. W. and Cote, R. W., “Evaluation of Spent Fuel as a Waste Form in a Salt Repository”, in Scientific Basis for Nuclear Waste Management, Vol. VII, McVay, G. L., ed., North-Holland, New York, pp. 437444 (1984).Google Scholar
23. Freeborn, W. P., Scheetz, B. E. and White, W. B., “The Role of Boron in Monitoring the Leaching of Borosilicate Glass Waste Forms”, this volume.Google Scholar
24. Plodinec, M. J., Wicks, G. G. and Bibler, N. E., An Assessment of Savannah River Borosilicate Glass in the Repository Environment, DP-1629, Savannah River Laboratory, Aiken, South Carolina (1982).Google Scholar
25. Ross, W. A., Westsik, J. H., Jr., Roberts, F. P. and Harvey, C. O., “Comparative Leach Testing of Alternative Transuranic Waste Forms”,Am. Ceram. Soc., 62, 10261029, 1035 (1983).Google Scholar
26. Smith, P. K. and Baxter, C. A., Fracture icate Glass Containing Nuclear Wastes, DP-1602, Savannah River Laboratory, Aiken, South Carolina (1981).Google Scholar
27. Interim Reference Repository Conditions for a Nuclear Waste Repository in Basalt, NWTS-16, The Reference Repository Conditions Interface Working Group, Office of Nuclear Waste Isolation, Columbus, Ohio (1981).Google Scholar
28. Barkatt, Aa. et al., “Mechanisms of Defense Waste Glass Dissolution”, submitted to Nucl. Tech.Google Scholar
29. Macedo, P. B. and Barkatt, Aa., Evaluation of Bulk Properties of Radwaste Glass and Ceramic Container Materials to Determine Long-Term Stability, NUREG/CR-2737, U.S. Nuclear Regulatory Commission, Washington, D.C. (1982).Google Scholar
30. Jones, T. E., Reference Material Chemistry - Synthetic Ground Water Formulation, RHO-BW-ST-37 P, Rockwell Hanford Operations, Richland, Washington (1982).Google Scholar