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Technetium and Molybdenum in Oxide Spent Nuclear Fuel: Impact on Release Estimates

Published online by Cambridge University Press:  17 March 2011

Jeffrey A. Fortner
Affiliation:
Argonne National Laboratory, Chemical Engineering Division, Argonne, IL 60439, email: [email protected]
A. Jeremy Kropf
Affiliation:
Argonne National Laboratory, Chemical Engineering Division, Argonne, IL 60439
Robert J. Finch
Affiliation:
Argonne National Laboratory, Chemical Engineering Division, Argonne, IL 60439
James C. Cunnane
Affiliation:
Argonne National Laboratory, Chemical Engineering Division, Argonne, IL 60439
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Abstract

Technetium-99 99Tc) is an important radionuclide in repository models owing to its relatively long half-life and the high aqueous solubility of compounds where it is inthe heptavalent state. The vast majority of the 99Tc inventory presently slatedfor disposal is contained in oxide commercial spent nuclear fuel (CSNF), where it is divided (along with its cohort, molybdenum) betweenexsolved, intermetallic “epsilon” particles and isolated, likely oxidized, atoms distributed in the uranium dioxide matrix. We present recent evidence from synchrotron x-ray fluorescence spectroscopy, electron microscopy, and fuel dissolution testing on the likely oxidation state, coordination environment, and physical disposition of technetium and molybdenum in CSNF. Effects of the relative proportioningof technetium and molybdenum among the metallic and oxidized states in CSNF, andtheir distribution in or near grain boundaries and gaps on release during CSNF corrosion testing are discussed.

Type
Research Article
Copyright
Copyright © Materials Research Society 2004

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References

1. , James L. , Jerden Jr., Margaret Goldberg, James Cunnane, Theodore Bauer, RoaldWigeland, and Russell Nietert, Mater. Res. Soc., These Proceedings.Google Scholar
2.U. S. Department of Energy (DOE), Office of Civilian Radioactive Waste Management, “CSNF Waste Form Degradation and Radionuclide Release Models,” ANL-EBS-MD-000015, (March, 2003).Google Scholar
3. Gray, W. J., Strachan, D. M., and Wilson, C. N., Mater. Res. Soc. Symp. Proc. 257, 353360 (1992).Google Scholar
4. Kleykamp, H., Paschoal, J. O., Pejsa, R., and Thommler, F., J. Nucl. Mater. 130, 426433 (1985).Google Scholar
5. Thomas, L. E. and Guenther, R. J., Mater. Res. Soc. Symp. Proc. 127, 293300 (1989).Google Scholar
6. Guenther, R. J., Blahnik, D. E., Campbell, T. K., Jenquin, U. P., Mendel, J. E., Thomas, L. E., and Thornhill, C. K., Pacific Northwest National Laboratory Report PNL-5109-103 (April, 1988).Google Scholar
7. Finn, P. A., Finch, R., Buck, E., and J. Bates, Mater. Res. Soc.Symp. Proc. 506, 123131 (1998).Google Scholar
8. Finch, R. J., Buck, E. C., Finn, P. A., and Bates, J. K., Mater. Res. Soc. Symp. Proc. 556, 431438 (1999).Google Scholar
9. Wronkiewicz, D.J., Watkins, C.S., Baughman, A.C., Miller, F.S., and Wolf, S.F., Mater. Res. Soc. Symp.Proc. Vol. 713 625632 (2002).Google Scholar
10. Cui, D., Eriksen, T., and , U-B Eklund, Mater. Res. Soc. Proc. Vol. 663, 427434 (2001).Google Scholar
11. Stern, E. A., in X-Ray Absorption: Principles, Applications, Techniques of EXAFS, SEXAFS, and XANES, edited by Koningsberger, D. C. and Prins, R., (Wiley-Interscience, New York, 1988).Google Scholar
12. Kropf, A. J., Fortner, J. A., Finch, R. J., Cunnane, J. C., and Karanfil, C., Proceedings of XAFS XII: The 12th International Conference on X-ray Absorption Fine-Structure Spectroscopy, Malmö, Sweden, June 22-27, 2003 (to be published in Physica Scripta).Google Scholar
13. Kropf, A. J., Karanfil, C., Segre, C. U., Finch, R. J., Fortner, J. A., Aase, S., Terry, J., Bunker, G., Chapman, L. D., Rev. Sci. Instrum. 74, 46964702 (2003).Google Scholar
14. Fortner, J. A., Finch, R. J., Kropf, A. J., and Cunnane, J. C., Proceedings of the International Conference on High-Level Waste Management, Las Vegas, NV March 30-April 4, 2003.Google Scholar
15. Fortner, J. A., Kropf, A. J., Finch, R. J., Mertz, C. J., Jerden, J. L., Goldberg, M. M., and Cunnane, J. C., Proceedings of GLOBAL 2003, New Orleans, LA, November 16-20, 2003.Google Scholar