Hostname: page-component-848d4c4894-r5zm4 Total loading time: 0 Render date: 2024-07-01T18:11:08.670Z Has data issue: false hasContentIssue false

Syntheses of Titanate-Based Hosts for the Immobilization of Pu(III) and Am(III)

Published online by Cambridge University Press:  03 September 2012

Shara S. Shoup
Affiliation:
Chemical and Analytical Sciences Division, Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, TN 37831–6110.
Carlos E. Bamberger
Affiliation:
Chemical and Analytical Sciences Division, Oak Ridge National Laboratory, P.O. Box 2008, Oak Ridge, TN 37831–6110.
Get access

Abstract

Syntheses of novel titanate-based waste forms, potentially suitable for immobilizing Pu(III) and Am(III), have been performed. The dititanate compounds An2Ti2O7 (An=Pu or Am) were found to have a monoclinic structure. A series of pyrochlore-type solid solutions between An2Ti2O7 and the cubic pyrochlore Ln2Ti2O7 (Ln=Gd, Er, or Lu) has been established, and limits of solid solubility for An2Ti2O7 were determined. These limits were found to increase as the ionic radius of the lanthanide in the host decreased. Strontium-containing titanate compounds SrAn2Ti4O12 were also prepared and were characterized as exhibiting a perovskite-type structure. Such compounds could serve as waste hosts for the immobilization of not only the actinide but also 90 Sr. A 2 month leaching study of Er1.78Pu0.22Ti2O7 and SrPu2Ti4O12 by WIPP “A” brine was performed. Very low amounts (< 1 ppm) of Pu(III) were leached. Although the ionic radius of Np(III) is similar to that of Pu(III) and Am(III), analogous Np compounds could not be prepared in any of the titanate systems investigated.

Type
Research Article
Copyright
Copyright © Materials Research Society 1997

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

REFERENCES

1. Ringwood, A.E., Kesson, S.E., Ware, N.G., Hibberson, W., and Major, A., Nature 278, p. 219 (1979).Google Scholar
2. Burakov, B.E., Anderson, E.B., Rovsha, V.S., Ushakov, S.V., Ewing, R.C., Lutze, W., and Weber, W. J. in Scientific Basis for Nuclear Waste Management XIX, edited by Murphy, W.M. and Knecht, D.A. (Mater. Res. Soc. Proc. 412, Pittsburgh, PA 1996), p. 3339.Google Scholar
3. Bamberger, C.E., Dunn, H.W., Begun, G.M., and Landry, S.A., J. Less-Common Met. 109, p. 209(1986).Google Scholar
4. Bamberger, C.E., Haverlock, T.J., Shoup, S.S., Kopp, O.C., and Stump, N.A., J. Alloys and Compounds 204, p. 101 (1994).Google Scholar
5. Shoup, S.S., Haverlock, T.J., and Bamberger, C.E., J. Amer. Ceram. Soc. 78, p. 1261 (1995).Google Scholar
6. Shoup, S.S., Bamberger, C.E., Haverlock, T.J., and Peterson, J.R., J. Nucl. Mater, in press.Google Scholar
7. Dosch, R.G. and Lynch, A.W., Interaction of Radionuclides with Geomedia Associated with the Waste Isolation Pilot Plant Site in New Mexico, Sandia National Laboratory Report SAND78–0297(1978).Google Scholar
8. Williams, D., A FORTRAN Lattice Constant Refinement Program,. Ames Laboratory Report IS-1052 (1964).Google Scholar
9. Materials Characterization Center, Nuclear Waste Materials Handbook Test Methods ÍRev 6), Pacific Northwest Laboratories Report DOE/TIC 11400 (1985).Google Scholar
10. Gross Alpha and Gross Beta Radioactivity in Drinking Water, EPA-600/900.0 (1980).Google Scholar
11. Powder Diffraction File, International Centre for Diffraction Data, Newtown Square, PA.Google Scholar
12. Shannon, R.D., Acta Crystallogr. A 32, p. 751 (1976).Google Scholar
13. Vance, E.R., Angel, P.J., Begg, B.D., and Day, R.A. in Scientific Basis for Nuclear Waste Management XVII, edited by Ewing, R.C. (Mater. Res. Soc. Proc. 333, Pittsburgh, PA 1994), p. 293298.Google Scholar
14. Clinard, F.W. Jr., Hobbs, L.W., Land, C.C., Peterson, D.E., Rohr, D.L., and Roof, R.B., J. Nucl. Mater. 105, p. 248(1982).Google Scholar
15. Tabuteau, A. and Pages, M. in The Handbook on the Physics and Chemistry of the Actinides, edited by Freeman, A.J. and Keller, C. (Elsevier, Amsterdam, Netherlands, 1985), p. 185241.Google Scholar
16. Vance, E.R., Hart, K.P., Day, R.A., Begg, B.D., Angel, P.J., Loi, E., Weir, J., and Oversby, V.M., in Scientific Basis for Nuclear Waste Management XIX, edited by Murphy, W.M. and Knecht, D.A. (Mater. Res. Soc. Proc. 412, Pittsburgh, PA 1996), p. 4955.Google Scholar