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Characterization of a Plutonium-Bearing Zirconolite-Rich Synroc

Published online by Cambridge University Press:  03 September 2012

E. C. Buck
Affiliation:
Argonne National Laboratory, Argonne, IL 60439
B. Ebbinghaus
Affiliation:
Lawrence Livermore National Laboratory, Livermore, CA 94550
A. J. Bakel
Affiliation:
Argonne National Laboratory, Argonne, IL 60439
J. K. Bates
Affiliation:
Argonne National Laboratory, Argonne, IL 60439
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Abstract

A titanate-based ceramic waste form, rich in phases structurally related to zirconolite (CaZrTi2O7), is being developed as a possible method for immobilizing excess plutonium from dismantled nuclear weapons. As part of this program, Lawrence Livermore National Laboratory (LLNL) produced several ceramics that were then characterized at Argonne National Laboratory (ANL). The plutonium-loaded ceramic was found to contain a Pu-Gd zirconolite phase but also contained plutonium titanates, Gd-polymignyte, and a series of other phases. In addition, much of the Pu was remained as PuO2-x. The Pu oxidation state in the zirconolite was determined to be mainly Pu4+, although some Pu3+ was believed to be present.

Type
Research Article
Copyright
Copyright © Materials Research Society 1997

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References

REFERENCES

1. Oversby, V.M. and Ringwood, W. E., “Leaching Studies on Synroc at 95° and 200°C”, Rad. Waste Mgmt. 2, 223237 (1982).Google Scholar
2. Lumpkin, G. R. and Ewing, R. C., “Geochemical Alteration of Pyrochlore Group Minerals: Pyrochlore Subgroup”, Am. Miner. 80, 732743 (1995).10.2138/am-1995-7-810Google Scholar
3. McGlinn, P. J., Hart, K. P., Loi, E. H., and Vance, E. R., “pH Dependence of the Aqueous Dissolution Rates of Perovskite and Zirconolite at 90°C,” Mater. Res. Soc. Symp. Proc. 353, 847854 (1995).10.1557/PROC-353-847Google Scholar
4. Van Konynenburg, R. A. and Guiñan, M. W., Plutonium Doping ofSynroc-D, Lawrence Livermore National Laboratory Report UCRL-53425 (1983).Google Scholar
5. Vance, E. R., Ball, C. J., Day, R. A., Smith, K. L., Blackford, M. G., Begg, B. D., and Angel, P., “Actinide and Rare Earth Incorporation into Zirconolite”, J. Alloys Comp. 213/214, 406409 (1994).10.1016/0925-8388(94)90945-8Google Scholar
6. Standard Test Methods for Determining Chemical Durability of Nuclear Waste Glasses: The Product Consistency Test (PCT), ASTM Standard C1285–94, ASTM, Philadelphia PA (1994).Google Scholar
7. Wronkiewicz, D. J., Wang, L. M., Bates, J. K., and Tani, B. S., “Effects of Radiation on Glass Alteration in a Steam Environment”, 294, 183190 (1993).Google Scholar
8. White, T. J., “The Microstructure of Synthetic Zirconolite, Zirkelite, and Related Phases”, Am. Miner. 69, 11561172 (1984).Google Scholar
9. Fortner, J. A. and Buck, E. C., “The Chemistry of the Light Rare-Earth Elements as determined by Electron Energy Loss Spectroscopy”, Appl. Phys. Lett. 68, 38173819 (1996).10.1063/1.116627Google Scholar
10. Nunez, L. and Fortner, J. A., Argonne National Laboratory, private communication (1996).Google Scholar
11. Roof, R. B., X-ray Diffraction Data for Plutonium Compounds, Los Alamos National Laboratory Report LA-11619 (1989)Google Scholar
12. Ruh, R. and Wadsley, A. D., “The Crystal Structure of ThTi2O6 (Brannerite)”, Acta Cryst. 21, 974978 (1966).10.1107/S0365110X66004274Google Scholar
13. Vance, E. R., Angel, P. J., Begg, B. D., and Day, R. A., “Zirconolite-Rich Ceramics for High-Level Actinide Wastes,” Mater. Res. Soc. Symp. Proc. 333, 293298 (1994).10.1557/PROC-333-293Google Scholar
14. Wolf, S. F., Brown, N. R., Fortner, J. A., Buck, E. C., Dietz, N. L., and Bates, J. K., Environ. Sci. Technol. 31 (1997).10.1021/es960295+Google Scholar