Hostname: page-component-78c5997874-lj6df Total loading time: 0 Render date: 2024-11-08T04:56:04.901Z Has data issue: false hasContentIssue false

Corrosion of Glass-Bonded Sodalite as a Function of pH and Temperature

Published online by Cambridge University Press:  10 February 2011

L. R. Morss
Affiliation:
Chemical Technology Division, Argonne National Laboratory, Argonne, IL 60439
M. L. Stanley
Affiliation:
Chemical Technology Division, Argonne National Laboratory, Argonne, IL 60439
C. D. Tatko
Affiliation:
Chemical Technology Division, Argonne National Laboratory, Argonne, IL 60439
W. L. Ebert
Affiliation:
Chemical Technology Division, Argonne National Laboratory, Argonne, IL 60439
Get access

Abstract

This paper reports the results of corrosion tests with glass-bonded sodalite, a ceramic waste form (CWF) that is being developed to immobilize radioactive electrorefiner salt used to condition spent sodium-bonded nuclear fuel, and with sodalite and binder glass, the two major components of the CWF. These tests were performed with dilute pH-buffered solutions in the pH range of 5-10 at temperatures of 70 and 90°C to determine the pH dependences of the forward dissolution rates of the CWF and its components. The tests show that the pH dependences of the dissolution rates of sodalite, binder glass, and glass-bonded sodalite are similar to the pH dependence of dissolution rate of borosilicate nuclear waste glasses, with a negative pH dependence in the acidic region and a positive pH dependence in the basic region. The dissolution rates are higher at 90°C than at 70°C. Our results on the forward dissolution rates and their temperature and pH dependences will be used as components of a waste form degradation model to predict the long-term behavior of the CWF in a nuclear waste repository.

Type
Research Article
Copyright
Copyright © Materials Research Society 2000

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

REFERENCES

1 ANL-NT-119, Ceramic Waste Form Handbook, Morss, L. R., compiler, 1999.Google Scholar
2 Knauss, K. G. and Wolery, T. J., “Dependence of Albite Dissolution Kinetics of pH and Time at 25° and 70°C,” Geochim. Cosmochim. Acta 50, 248 12497 (1986).Google Scholar
3 Knauss, K. G. and Wolery, T. J., “Muscovite Dissolution as a Function of pH and Time at 70°C,” Geochim. Cosmochim. Acta 53, 14931501 (1989).Google Scholar
4 Knauss, K. G., Bourcier, W. L., McKeegan, K. D., Merzbacher, C. I., Nguyen, S. N., Ryerson, F. J., Smith, D. K., Weed, H. C., “Dissolution Kinetics of a Simple Analogue Nuclear Waste Glass as a Function of pH, Time, and Temperature,” Mat. Res. Soc. Syrup. Proc., 176, 371381 (1990).Google Scholar
5 Oelkers, E. H., Schott, J., Devidal, J., “The Effect of Aluminum, pH, and Chemical Affinity on the Rates of Aluminosilicate Dissolution Reactions. Geochim. Cosmochim. Acta 58, 20112024 (1994).Google Scholar
6 Abraitis, P. K., Vaughan, D. J., Livens, F. R., Monteith, J., Trivedi, D. P., Small, J. S., “Dissolution of a Complex Borosilicate Glass at 60°C: The Influence of pH and Proton Absorption on the Congruence of Short-Term Leaching,” Mat. Res. Soc. Symp. Proc. 506, 4754 (1998).Google Scholar
7 Bourcier, W., “Affinity Functions for Modeling Glass Dissolution Rates,” UCRL-JC- 131186 (1998).Google Scholar
8 Aagaard, P. and Helgeson, H. C., “Thermodynamic and Kinetic Constraints on Reaction Rates among Mineral and Aqueous Solutions, I. Theoretical Considerations,” Am. J. Science, 282, 237285 (1982).Google Scholar
9 American Society for Testing and Materials, “Annual Book of ASTM Standards,” 12.01, Standard Test Method for Static Leaching of Monolithic Waste Forms for Disposal of Radioactive Waste, C1220-98, pp. 116 (1998).Google Scholar
10 McGrail, B. P., Ebert, W. L., Bakel, A. J., Peeler, D. K., “Measurement of Kinetic Rate Law Parameters on a Na-Ca-Al Borosilicate Glass for Low-Activity Waste,” J. Nucl. Materials 249, 1765–189 (1997).Google Scholar
11 Harned, H. S. and Owen, B. B., The Physical Chemistry of Electrolytic Solutions, 3rd ed. (Reinhold, New York, 1958), pp. 643649.Google Scholar
12 Montgomery, K., “The Synthesis and Dissolution of Sodialite: Implications for Nuclear Waste Disposal,” M. Sc. Thesis, Dept. of Geology, University of Alberta, Canada (1986).Google Scholar