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A Glass Durability Model Based on Understanding Glass Chemistry and Structural Configurations of the Glass Constituents

Published online by Cambridge University Press:  10 February 2011

Xiangdong Feng  and
Todd B. Metzger
Xiangdong Feng
Affiliation:
Pacific Northwest National Laboratory, Recleaned, Washington, 99352, X_Feng@PNL.gov
Todd B. Metzger
Affiliation:
Alfred University, Alfred, New York.
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Abstract

An improved structural bond strength (SBS) model has been developed to quantify the correlation between glass compositions and their chemical durabilities. The SBS model assumes that the strengths of the bonds between cations and oxygens and the structural roles of the individual elements in the glass are the predominant factors controlling the composition dependence of the chemical durability of glasses. The structural roles of oxides in glass are classified as network formers, network breakers, and intermediates. The structural roles of the oxides depend on glass composition and the redox state of oxides. A12O3, ZrO2, Fe2O3, and B2O2 are assigned as network formers only when there are sufficient alkalis to bind with these oxides. CaO can also improve durability by sharing non-bridging oxygen with alkalis, relieving Si0 2 from alkalis. The binding order to alkalis is AI2O3>ZrO2>Fe2O 2>B2O2>CaO>SiO2. The percolation phenomenon in glass is also taken into account. The concentration of network formers has to reach a critical value for a glass to become durable; durable glasses are sufficient in network formers and have a complete network structure; poor durability glasses are deficient in network formers and the network is incomplete and discontinuous. The SBS model is capable of correlating the 7-day product consistency test durability of 42 low-level waste glasses with their composition with an R2 of 0.87, which is better than 0.81 obtained with an eight-coefficient empirical first-order mixture model on the same data set.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 432: Symposium S – Aqueous Chemistry and Geochemistry of Oxides , 1996 , 27
Copyright
Copyright © Materials Research Society 1997

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References

1. Feng, X., “Composition Effects on Chemical Durability and Viscosity of Nuclear Waste Glasses: Systematic Studies and Structural Thermodynamic Models,” Ph.D. Thesis, The Catholic University of America, Washington, DC, pg. 151 (1988).Google Scholar
2. Feng, X. and Barkatt, A., “Structural Thermodynamic Model for the Durability and Viscosity of Nuclear Waste Glasses,” Mat. Res. Soc. Symp. Proc. 112, 543–554 (1988).Google Scholar
3. Feng, X., Saad, E. E., and Pegg, I. L., “A Model for the Viscosity of Multicomponent Glass Melts,” Ceram. Trans. 9, 457–468 (1990).Google Scholar
4. Abrajano, T. A., Bates, J. K. and Bohlke, J. K., “Linear Free Energy Relationships in Glass Corrosion,” Mat. Res. Soc. Symp. Proc. 125, 383–392 (1988).Google Scholar
5. Tovena, I., Advocat, T., Ghaleb, D., Vernaz, E., and Larche, F., “Thermodynamic and Structural Models Compared with the Initial Dissolution Rates of'‘SON’ Glass Sample,” Mat. Res. Soc. Symp. Proc. 333 595 (1994).Google Scholar
6. Jantzen, C. M., Bibler, N. E., Beam, D. C., Ramsey, W. R., and Waters, B. J.. 1992. Nuclear Waste Glass Product Consistency Test (PCT), Ver. 5.0. WSRC-TR-90-539, Rev. 2, Westinghouse Savannah River Company, Aiken, South Carolina. Google Scholar
7. Zachariasen, W. H., “The Atomic Arrangement in Glass,” J. Am. Chem. Soc. 54, 3841 (1932).Google Scholar
8. Bobkova, N. M., Gorodetstkaya, O. G., Yankovskaya, S. A., and Tizhovka, Th.S., “Study of the Structural Role of Zirconium in Aluminoborosilicate and Borosilicate Glasses,” Fizikai Khi 9.R. Rossin, J. Bersan, and G. Urbain, Rev. Hautes Temperatures et Refractaires 1, 159 (1964).Google Scholar
9. Boyd, D. C. and Thompson, D. A., in Kirk-Othmer: Encyclopedia of Chemical Technology, 3rd Ed,. John Wiley and Sons, New York, pp. 807–880 (1980).Google Scholar
10. Riebling, E. F., Jour. Chemistry, 42, 2811 (1964).Google Scholar
11. Bunker, B. C., Arnold, G.W., Day, D.E., Bray, P.J., “The effect of molecular structure on borosilicate glass leaching,” J. Non-Cryst. Solids, 87, 226(1986)Google Scholar
12. Feng, X., Pegg, I. L., Barkatt, A., Macedo, P. B., Cucinell, S. J., and Lai, S., “Correlation Between Composition Effects on Glass Durability and the Structural Role of the Constituent Oxides,” Nucl. Technol. 85, 334–345 (1989).Google Scholar
13. X., Feng, Hrma, P.R., Westsik, J.H. Jr., Brown, N. R., Schweiger, M.J., Li, H., Vienna, J.D., Chen, G., Piepel, G.F., Peeler, D.K., Smith, D.E., Chang, C., Palmer, S.E., Kim, D., Peng, Y., Hahn, W.K., Bakel, A.J., and Ebert, W.L., “Glass Optimization for Vitrification of Hanford Site Low-Level Tank Waste,” Pacific Northwest National Laboratory Report PNNL-10918, March 1996, Richland, Washington Google Scholar
14. Ellison, A. J. G., Mazer, J. J., and Ebert., W. L. 1994 “Effects of Glass Composition on Waste Form Durability: A Critical Review.” Argonne National Laboratory Report, ANL-94/28, Argonne, Illinois.Google Scholar
15. Alexander, M.N., Onorato, P.I.K., Struck, C.W. and Rozen, J. Rt, “Structure of Alkali (Alumino Silicate Glasses, 1. TI+ Luminescence and the Nonbridging Oxygen Issue,” J. Non-Cryst. Solids, 79, 137(1986)Google Scholar
16. Greenblatt, S. and Bray, P.J., “A Discussion of the Fraction of Four-Co-Ordinated Boron Atoms Present in Borate Glasses,” Phy. Chem. Glasses, 8, 213(1967)Google Scholar
17. Dell, W.J. and Bray, P.J., “”B NMR Studies and Structural Modeling of Na2O-B2O3-SiO2 Glasses of High Soda Content,” J. Non-Crys. Solids, 58, 1(1983).Google Scholar
18. Sun, K. H., “Fundamental Conditions of Glass Formation,” J. Am. Ceram. Soc. 30, 277 (1947).Google Scholar
19. Fajans, K and Barber, D. S. W., “Properties and Structures of Vitreous and Crystalline Boron Oxide,” J. Amer. Chem. Soc. 74, 276 (1952).Google Scholar
20. Krogh-Moe, J., “Structure of Boron Oxide and Alkali Borate Glasses,” Phys. Chem. Glasses 1, 26 (1960).Google Scholar
21. Kinoshita, M., Harado, M., Sato, Y., and Hariguchi, Y., “Percolation Phenomenon for Dissolution of Sodium Borosilicate Glasses in Aqueous Solutions,” J. Am. Ceram. Soc. 74(4), 783(1991)Google Scholar
22. Dean, J. A., Lange's Handbook of Chemistry, 13th Ed., McGraw-Hill Book Company, New York, pp. 5–14 (1985).Google Scholar
23. Turkdogan, E. T. and Bills, P. M., Am. Ceram. Soc. Bull. 39, 682 (1960).Google Scholar