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Fundamental Science of f-Elements in Selected Immobilization Glasses: Significance for TRU Disposal Schemes

Published online by Cambridge University Press:  10 February 2011

R. G. Haire
Affiliation:
Oak Ridge National Laboratory, Chemical and Analytical Sciences Division, P. 0. Box 2008, MS-6375, Oak Ridge, TN 37831, USA
Z. Assefa
Affiliation:
Oak Ridge National Laboratory, Chemical and Analytical Sciences Division, P. 0. Box 2008, MS-6375, Oak Ridge, TN 37831, USA
N. Stump
Affiliation:
Dept. Of Physical Science, Winston-Salem State University, 601 Martin Luther King, Jr. Drive, Winston-Salem, NC 27110, USA
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Abstract

We have investigated certain aspects of the fundamental chemistry and materials science of the 4fand several 5f-elements in three glass matrices. Two of these matrices were high-temperature (850° and 1450°C melting points) silicate-based glasses and the third was a sol-gel glass. Optical spectroscopy was the principal investigating tool. One aspect of the work here was to ascertain the oxidation state exhibited by these elements in the different glasses, as well as the factors that control and/or may alter this state. An important finding was noting a general correlation between the oxidation states obtained in the two high-temperature glasses and those observed in the oxides of these elements. Of the twenty three f-elements considered here, only three exceptions (Ce, Am and Bk) or examples of variable behavior (Pr, Tb, U and Cf) to this correlation were noted. One explanation offered for the exceptions is based on the stability afforded by the oxides' fluorite lattice. The correlation also applied to the sol-gel glasses after they had been heated. Other oxidation states for some elements could be obtained in the sol-gel glasses prepared at 25°C. Presented here is a summary of the oxidation states observed for these elements in three glass matrices and how these states correlate with those observed in the oxides of these elements and with the relative oxidation potentials for the elements.

Type
Research Article
Copyright
Copyright © Materials Research Society 1998

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References

REFERENCES

1 Haire, R. G. and Eyring, L., in Handbook on the Pliysics and Chemistry of Rare Earths, Vol. 18. Lanthanides/Actinides: Chemistry, edited by Gschneidner, K. A. Jr., Eyring, L., Choppin, G. R. and Lander, G. H. (North-Holland, New York, 1994) pp.413505.Google Scholar
2 Johnson, W. D., J. Am. Ceram. Soc., 48, 184(1965).Google Scholar
3 Leskela, M. and Su-Kkanen, J., J. Less-Common Metals, 112, 71 (1985).Google Scholar
4 Larson, E. M., Lytle, F. W., Eller, P. G., Greegar, R. B. and Eastman, M. P., J. Non-Cryst. Solids, 116, 57 (1990).Google Scholar
5 Paul, A., Mulhollard, M. and Zamar, M. S., J. Mat. Sci., 11, 2082 (1976).Google Scholar
6 Farger, F., Cosmochemica 55, 3303 (1991).Google Scholar
7 Schreiber, H. D., Balazr, G. Bryan and Williams, Barbara J., J. Am. Ceramic Soc., 65, 449 (1982).Google Scholar
8 Schreiber, H. D., J. Less-Common Metals, 91,129(1983).Google Scholar
9 Muller, I.S., J. Non-Crystall. Solids, 134, 147(1991).Google Scholar
10 Karraker, D. G., I. Am. Ceram. Soc., 65, 53(1982).Google Scholar
11 Eller, P. G., Jarvinen, G. D., Purson, J. D., Pennenian, R. A., Ryan, R. R., Lytle, F. W. and Greegor, R. B., Radiochimica Acta, 39, 17 (1985).Google Scholar
12 Dai, S., unpublished results.Google Scholar
13 Stump, S., Haire, R. G. and Dai, S., Mat. Res. Soc. Proc., Vol 465, editors Gray, Win. J. and Triay, I.R., (MRS, Penn, 1997) pp.4754.Google Scholar
14 Haire, R. G. and Stump, N. A., Mat. Res. Soc. Proc., Vol 465, editors Gray, Wm. J. and Triay, I.R., (MRS, Penn, 1997) pp.3946.Google Scholar
15 Nugent, L.J., Baybarz, R. D., Burnett, J. L and Ryan, J. R., Inorg, J.. Nucl. Chem., 33, 2503 (1971).Google Scholar