Hostname: page-component-76fb5796d-9pm4c Total loading time: 0 Render date: 2024-04-26T23:34:33.523Z Has data issue: false hasContentIssue false

Performance Assessment of Zircon as a Waste Form for Excess Weapons Plutonium Under Deep Borehole Burial Conditions

Published online by Cambridge University Press:  15 February 2011

W. J. Weber
Affiliation:
Pacific Northwest National Laboratory, P.O. Box 999, Richland, WA 99352
R. C. Ewing
Affiliation:
Dept. of Earth and Planetary Sciences, University of New Mexico, Albuquerque, NM 87131
W. Lutze
Affiliation:
Dept. of Chemical and Nuclear Engr., University of New Mexico, Albuquerque, NM 87131
Get access

Abstract

Zircon (ZrSiO4) is proposed as a waste form for excess weapons-grade plutonium. Zircon is an extremely durable ceramic that is often found as an accessory mineral in Precambrian terranes with ages up to 4 billion years. The chemical durability of zircon in groundwater far exceeds that of other waste forms, as modeled leach rates may be as low as 10-11 g/m2d. At least 10 wt% Pu can substitute for Zr in zircon. Self-radiation damage from alpha decay leads to a crystalline-to-amorphous transformation that is modeled as a function of time and temperature for deep borehole conditions. Based on the results of this assessment, zircon could meet all necessary durability and criticality criteria required for a Pu waste form. The types of data used in this analysis are generally not available for other crystalline ceramics or glasses.

Type
Research Article
Copyright
Copyright © Materials Research Society 1996

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

1. Management and Disposition of Excess Weapons Plutonium (National Academy of Sciences, Washington, D.C., 1994).Google Scholar
2. Management and Disposition of Excess Weapons Plutonium - Reactor-Related Options(National Academy of Sciences, Washington, D.C., 1995).Google Scholar
3. Halsey, W.G., Jardine, L.J., Walter, C.E., in Disposal of Weapons Plutonium, edited by Merz, E. (Kluwer Academic Publishers, Holland, in press).Google Scholar
4 Burakov, B.E., in Proceedings of SAFE WASTE '93, Vol. 2, (1993) pp. 1928.Google Scholar
5. Ewing, R.C., Lutze, W., and Weber, W.J., J. Mater. Res. 10, 243 (1995).Google Scholar
6. Ewing, R.C., Weber, W.J. and Lutze, W., in Disposal of Weapons Plutonium, edited by Merz, E. (Kluwer Academic Publishers, Holland, in press).Google Scholar
7. Komarneni, S. and Roy, R., in Zircon, Science and Technology, edited by Sōmiya, S. (Uchidarokakuho, Japan, 1988), pp. 289298.Google Scholar
8. Weber, W.J., J. Mater. Res. 5, 2687 (1990); J. Am. Ceram. Soc. 76, 1729 (1993).Google Scholar
9. Murakami, T., Chakoumakos, B.C., Ewing, R.C., Lumpkin, G.R. and Weber, W.J., Am. Mineral. 76, 1510 (1991).Google Scholar
10. Weber, W.J., Ewing, R.C. and Wang, L.–M., J. Mater. Res. 9, 688 (1994).Google Scholar
11 Krogh, T.E., Geotimes 40 (11) 20 (1995).Google Scholar
12. Maas, R., Kinny, P.D., Williams, I.S., Froude, D.O. and Compston, W., Geochim. Cosmochim. Acta 56, 1281 (1992).Google Scholar
13. Moorbath, S., Nature 321, 725 (1986).Google Scholar
14. Froude, D.O., Ireland, T.R., Kinny, P.D., Williams, I.S., Compston, W., Williams, I.R. and Myers, J.S., Nature 304, 616 (1983).Google Scholar
15. Liu, D.Y., Nutman, A.P., Compston, W., Wu, J.S., and Shen, Q.H., Geology 20, 339 (1992).Google Scholar
16. Nutman, A.P., Friend, C.R.L., Kinny, P.D., McGregor, V.R., Geology 21, 415 (1993).Google Scholar
17. Ireland, T.R. and Wlotzka, F., Earth and Planetary Science Letters 109, 1 (1992).Google Scholar
18. Black, L.P., Chemical Geology 65, 25 (1987).Google Scholar
19. Hansen, B.T. and Friderichsen, J.D., Lithos 23, 209 (1989).Google Scholar
20. Sinha, A.K., Wayne, D.M. and Hewitt, D.A., Geochim. Cosmochim Acta 56, 3551 (1992).Google Scholar
21. Kamo, S.L. and Krogh, T.E., Geology 23, 281 (1995).Google Scholar
22. Deutsch, A. and Schärer, U., Geochim. Cosmochim. Acta 54, 3427 and 3435 (1990).Google Scholar
23. Claoué-Long, J.C., Sobolev, N.V., Shatsky, V.S. and Sobolev, A.V., Geology 19, 710 (1991).Google Scholar
24. Holland, H.D. and Gottfried, D., Acta Crystallogr. 8, 291 (1955).Google Scholar
25. Lumpkin, G.R. and Ewing, R.C., Phys. Chem. Minerals 16, 2 (1988).Google Scholar
26. Ellsworth, S., Navrotsky, A., and Ewing, R.C., Phys. Chem. Minerals 21, 140 (1994).Google Scholar
27. Pidgeon, R.T., O'Neil, J.R. and Silver, L.T., Science 154, 1538 (1966).Google Scholar
28. Craig, H., Science 159, 447 (1968).Google Scholar
29. Tole, M.P., Geochim. Cosmochim. Acta 49, 453 (1985).Google Scholar
30. Ewing, R.C., Haaker, R.F. and Lutze, W., in Scientific Basis for Nuclear Waste Management V, edited by Lutze, W. (Mater. Res. Soc. Proc. 11, Elsevier Science Publishers, New York, 1982), pp. 389397.Google Scholar
31. Petit, J.–C., Dran, J.–C. and Mea, G. Della, Bull. Minéral. 110, 25 (1987).Google Scholar
32. Lutze, W. and Ewing, R.C., in Radioactive Waste Forms for the Future, edited by Lutze, W. and Ewing, R.C. (North-Holland Physics, Amsterdam, 1988) pp. 699740.Google Scholar
33. Özkan, H., J. Applied Phys. 47, 4772 (1976).Google Scholar
34. Chakoumakos, B.C., Oliver, W.C., Lumpkin, G.R. and Ewing, R.C., Radiat. Eff. Defects Solids 118, 393 (1991).Google Scholar
35. Chakoumakos, B.C., Murakami, T., Lumpkin, G.R. and Ewing, R.C., Science 236, 1556 (1987).Google Scholar
36. Wayne, D.M. and Sinha, A.K., Contrib. Mineral. and Petrol. 98, 109 (1988).Google Scholar
37. Lee, J.K.W. and Tromp, J., Jour. Geophysical Research 100, 17, 753 (1995).Google Scholar
38. Weber, W.J., presented at the Am. Ceram. Soc. Meeting, Seattle, WA, 1995 (unpublished).Google Scholar
39. Virk, H.S., Radiat. Eff. Defects Solids 133, 87 (1995).Google Scholar
40. Cherniak, D.J., Hanchar, J.M., and Watson, E.B., Trans. Am. Geophys. Union 74, 651 (1993).Google Scholar
41. Watson, E.B. and Cherniak, D.J., Trans. Am. Geophys. Union 76, S299 (1995).Google Scholar