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Prediction of Glass Durability as a Function of Environmental Conditions

Published online by Cambridge University Press:  21 February 2011

C. M. Jantzen
C. M. Jantzen*
Affiliation:
E. I. du Pont de Nemours & Co. Savannah River Laboratory Aiken, SC 29808
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Abstract

A thermodynamic model of glass durability has been applied to natural, ancient, and nuclear waste glasses. The durabilities of over 150 different natural and man-made glasses, including actual ancient Roman and Islamic glasses (Jalame ca. 350 A. D., Nishapur 10-11th century A. D., and Gorgon 9-11th century A.D.), have been compared. Glass durability has been shown to be a function of the thermodynamic hydration free energy, δGhvd, which can be calculated from glass composition and solution pH. Using this approach the durability of the most durable nuclear waste glasses examined was ˜106 years by comparison with the durability of the natural basalts of ˜106 years. The least durable waste glass formulations were comparable in durability to the most durable simulated medieval window glasses of ˜103 years. In this manner, the durability of nuclear waste glasses has been interpolated to be ˜106 years and no less than 103 years.

Hydration thermodynamics have been shown to be applicable to the dissolution of glass in various natural environments. Groundwater-glass interactions relative to geologic disposal of nuclear waste, hydration rind dating of obsidians, and/or other archeological studies can be modeled, e.g. the relative durabilities of six simulated medieval window glasses have been correctly predicted for both laboratory (one month) and burial (5 year) experiments.

The effects of solution pH on glass dissolution has been determined experimentally for the 150 different glasses and can be predicted theoretically by hydration thermodynamics. The effects of solution redox (oxidation potential expressed as Eh) on dissolution of glass matrix elements such as Si and B have been shown to be minimal. The combined effects of solution pH and Eh have been described and unified by construction of thermodynamically calculated Pourbaix (pH-Eh) diagrams for glass dissolution. The Pourbaix diagrams have been quantified to describe glass dissolution as a function of environmental conditions by use of the data derived from hydration thermodynamics.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 125: Symposium N – Materials Stability and Environmental Degradation , 1988 , 143
Copyright
Copyright © Materials Research Society 1988

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References

REFERENCES

1. Paul, A., Chemistry of Glasses, Chapman and Hall, NY (1982).Google Scholar
2. Paul, A., J. Mat. Sci., 12, 2246 (1977).Google Scholar
3. Charles, R. J., J. Appl. Phys., 29, 1549 (1958).CrossRefGoogle Scholar
4. Iler, R.K., Colloid Chemistry of Silica and Silicates, Cornell Univ. Press, Ithaca, NY (1955).CrossRefGoogle Scholar
5. Rimstidt, J. D. and Barnes, H. Z., Geochem. Cosmochem. Acta, 44, 1683 (1980).Google Scholar
6. Douglas, R. W. and El-Shamy, T. M. M., J. Am. Ceram. Soc., 50, 1 (1967).Google Scholar
7. Grambow, B., Glastechnische Berichte, 56, 566 (1983).Google Scholar
8. Wallace, R. M. and Wicks, G. G., Scientific Basis for Nuclear Waste Management, VI, D. Brookins, G. (Ed.) 23 (1983).Google Scholar
9. Lasaga, A. C., “Chemical Kinetics of Water-Rock Interactions”, J. Geophys. Res., 89, 4009(1984).Google Scholar
10. Kittrick, J. A., ACS Symposium Series 93, 401 (1979).Google Scholar
11. Pourbaix, M., “Atlas of Electrochemical Equilibria in Aqueous Solutions”, Eng.Trans. by Franklin, J.A., NACE, Houston, TX,644p (1974).Google Scholar
12. Garrels, R. M. and Christ, C. L., Solutions, Minerals, and Equilibria, Harper and Row, NY 435p. (1965).Google Scholar
13. Helgeson, H. C. and Mackenzie, F. T., Deep Sea Res., 17, 877 (1970).Google Scholar
14. Rimstidt, J. D., The Kinetics of Silica-Water Reactions, Unpublished PhD Thesis, The Pennsylvania State University, 135p (1979).Google Scholar
15. Newton, R. G. and Paul, A., Glass Technology, 21, 307 (1980).Google Scholar
16. US Dept. of Energy, Waste Form Selection for SRP High-Level Waste, Report No. DOE/EA-0179 (1982).Google Scholar
17. Ewing, R. C., Sci. Basis for Nuclear Waste Mgt.. I, McCarthy, G. J. (Ed.), Plenum Press, NY, 57 (1979).Google Scholar
18. Malow, G. and Ewing, R. C., Sci. Basis for Nuclear Waste Mgt.. III, Moore, J. G. (Ed.), Plenum Press, NY, 315 (1981).Google Scholar
19. Malow, G., Lutze, W. and Ewing, R. C., J. Non-Cryst. Solids, 67, 305 (1984).Google Scholar
20. Plodinec, M. J., Jantzen, C. M., and Wicks, G. G., Adv. in Ceramics, V.8, Wicks, G. G. and Ross, W. A., (Eds.), Am. Ceram.Soc., Columbus, OH, 491 (1984).Google Scholar
21. Plodinec, M. J., Jantzen, C. M. and Wicks, G. G., Sci. Basis for Nuclear Waste Mgt., VII. McVay, G. L. (Ed.), North-Holland, NY,755(1984).Google Scholar
22. Jantzen, C. M. and Plodinec, M. J., J. Non-Cryst. Solids, 67, 207 (1984).Google Scholar
23. Jantzen, C. M., Adv. in Ceramics V.20, Clarke, D. E., et. al. (Eds.) Am. Ceram. Soc., Columbus, OH, 703 (1986).Google Scholar
24. Jantzen, C. M., Nuclear Waste Glass Durability: I. Predicting Environmental Response from Thermodynamic (Pourbaix) Diagrams, DP-MS-87-2, J. Am. Ceram. Soc. (in press).Google Scholar
25. Jantzen, C. M., Pourbaix Diagram for the Prediction of Waste Glass Durability in Geologic Environments, Sci. Basis for Nuclear Waste Mgt.. XI Apted, M. J. and Westerman, R.E. (Eds.), Materials Research Society, Pittsburgh, PA, DP-MS-87-77 (in press).Google Scholar
26. Jantzen, C. M., Stability of Radioactive Waste Glasses in Groundwaters Assessed from Hydration Thermodynamics, Set. Basis for Nuclear Waste Mgt.. XII, Lutze, W. (Ed.) DP-MS-87-76X (in preparation).Google Scholar
27. Stevels, J. M., Progress in the Theory of the Physical Properties of Glass, Elsevier, NY (1948).Google Scholar
28. Stevels, J. M., Phillips Tech. Rev., 22, 300 (1960/1961).Google Scholar
29. Pettijohn, F. J., J. Geology. 49, 610 (1941).Google Scholar
30. Loughnan, F. C., Chemical Weathering of the Silicate Minerals, Elsevier, NY 141p. (1969).Google Scholar
31. Newton, R. G., J. Glass Studies. 17, 161 (1975).Google Scholar
32. Howitt, D. G., Phys. Chem. Glasses, 22, 29 (1981).Google Scholar
33. Goodman, C. H. L., Glass Technology, 28 [1].19 (1987).Google Scholar
34. Jantzen, C. M., Nuclear Waste Glass Durability: II. Structural Considerations, J. Am. Ceram. Soc. (in preparation).Google Scholar
35. Mendel, J.E., (compiler), U.S. DOE Report DOE/TIC-11400 (1981).Google Scholar
36. Bibler, N. E. and Jantzen, C. M., A Product Consistency Durability Test for SRP Nuclear Waste Glass, DP-MS-87-174 (1988).Google Scholar
37. Newton, R. G., Glass Technology 26[6], 293 (1985).Google Scholar
38. Newton, R. G., More Results from the Ballidon Glass Burial Experiment, Glass Technology (in press).Google Scholar
39. Jantzen, C. M. and Newton, R. G., Application of Hydration Thermodynamics to the Durability of Medieval Window Glasses (in preparation).Google Scholar
40. Wicks, G. G., Robnett, B. M., and Rankin, W. D., Sci. Basis for Nuclear Waste Mgt..V. Lutze, W., (Ed.), Elsevier Publ. Co., New York, 15 (1982).Google Scholar
41. Grambow, B., Adv. in Ceramics, V. 8, Wicks, G. G. and Ross, W. A., (Eds.), The American Ceramic Society, Columbus, OH, 474 (1984).Google Scholar
42. Grambow, B. and Strachan, D. M., Sci. Basis for Nuclear Waste Mgt., VII, McVay, G. L. (Ed.), North-Holland, New York, 623 (1984).Google Scholar
43. Cooke, D. and Paul, A., J. Br. Ceram. Soc., 77, 104 (1978).Google Scholar
44. Plodinec, M. J., MRS Bulletin. XII[5], 61 (1987).Google Scholar
45. Oversby, V. M., Leach Testing of Waste Forms: Interrelationship of ISO and MCC Type Tests, in Workshop on Leaching Mechanisms of Nuclear Waste Forms, PNL-4382, Richland, WA, 97–129 (1982).Google Scholar
46. Pederson, L. R., Buckwalter, C. Q., McVay, G. L. and Riddle, B. L., Sci. Basis for Nuclear Waste Mgt., VII, Brookins, D. G., (Ed.), North Holland, New York, 47 (1983).Google Scholar
47. Feng, X. and Barkatt, A., Waste Management ‘87. Vol. I, Post, R. G. and Wacks, M. E., (Eds.), 584 (1987).Google Scholar
48. Grambow, B., Sci. Basis for Nuclear Waste Mgt.. VIII, Jantzen, C.M., Stone, J. A., and Ewing, R. C., (Eds), Materials Research Society, Pittsburgh, PA, 15 (1985).Google Scholar
49. Jantzen, C. M., Nuclear Waste Glass Durability: III. The Role of Thermodynamics and Kinetics, J. Am. Ceram. Soc. (in preparation).Google Scholar
50. Blumer, M., Helv. Chim. Acta, 33,1568 (1950).Google Scholar
51. Krumbein, W.C. and Garrels, R.M., J. Geology, 60, 1 (1952).Google Scholar
52. Jantzen, C.M. and Bibler, N.E., Sci. Basis for Nucl. Waste Mgt..IX, O.Werme, L., (Ed.), Mat. Res. Soc., Pittsburgh, PA, 219 (1986).Google Scholar
53. Jantzen, C.M. and Wicks, G.G., Sci. Basis for Nucl. Waste Mgt, VIII, Jantzen, C.M., Stone, J. A., and Ewing, R. C., (Eds.), Mat. Res. Soc., Pittsburgh, PA, 29 (1985).Google Scholar
54. Adams, P.B., J. Non-Cryst. Solids. 67, 193 (1984).Google Scholar
55. Shamy, T. M. El, Phys. Chem. Glasses, 14[1] 1 (1973).Google Scholar
56. Hench, L.L. and Clark, D.E., J. Non-Cryst. Solids, 28, 83 (1978).Google Scholar