Hostname: page-component-78c5997874-8bhkd Total loading time: 0 Render date: 2024-11-14T17:31:35.847Z Has data issue: false hasContentIssue false
  • English
  • Français

Investigation of Valence State of U, Pu, and Am in Crystalline Host-Phases Using in situ Cathodoluminescence Spectroscopy

Published online by Cambridge University Press:  01 February 2011

Maria V. Zamoryanskaya ,
Boris E. Burakov  and
Vladimir M. Garbuzov
Maria V. Zamoryanskaya
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail: zam@mail.ioffe.ru and burakov@riand.spb.su
Boris E. Burakov
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail: zam@mail.ioffe.ru and burakov@riand.spb.su
Vladimir M. Garbuzov
Affiliation:
Laboratory of Applied Mineralogy and Radiogeochemistry, the V.G. Khlopin Radium Institute, 28, 2-nd Murinskiy ave., St. Petersburg, 194021, Russia, e-mail: zam@mail.ioffe.ru and burakov@riand.spb.su
Get access

Abstract

Ceramics compounds based on the pyrochlore, (Ca,Gd,Hf,An)2TiO7; zircon, (Zr,An)SiO4, and garnet, (Y,Gd,An‥)3(Al,Ga,An…)5O12, where An = U, Am, Pu, Np, Cm, structures have been investigated to determine their use as durable nuclear waste forms for the immobilization of weapons-grade plutonium and other actinides. U, Pu, and Am were incorporated into synthetic zircon, pyrochlore, and garnet and were investigated using in situ cathodoluminescence (CL) and compared with Ce3+, Ce4+, Eu2+ and Eu3+ in order to determine the valence state of the actinide dopants. The results obtained allow for the identification of Am3+ ions in synthetic zircon and garnet. The CL emission of Am3+ is characterized by narrow bands in the orange-red spectral region and is similar to CL emission of Eu3+ in zircon and garnet. No characteristic CL emission of Pu4+ was observed in zircon, pyrochlore or garnet. This is similar to CL emission of Ce4+, which does not have characteristic CL emission in the visible region of the spectrum. Although ions of Ce3+ were characterized by intense CL emission, no characteristic CL emission of Pu3+ was identified in zircon, pyrochlore, or garnet.

The CL study of U-doped garnet and pyrochlore allow for the identification of the presence of two forms of uranium: the uranyl ion, (UO2)2+, and tetrahedral complex, (UO4)2−. Ions of U4+ did not have characteristic CL emission in the visible region. The study of pyrochlore samples doped simultaneously with 238Pu and 238U revealed that CL intensity of the uranyl ion increases with increasing dose of self irradiation from the 238Pu. It was assumed that self-irradiation might cause the change of actinide valence state.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 807: Symposium Scientific Basis for Nuclear Waste Management XXVII , 2003 , 291
Copyright
Copyright © Materials Research Society 2004

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. Burakov, B. E., Proc. Intern. Conf. SAFE WASTE '93, 13–18/06/1993, Avignon, France, Vol. 2 (1993) pp. 19–28.Google Scholar
2. Anderson, E.B., Burakov, B. E. and Vasiliev, V.G., Proc. Intern. Conf. SAFE WASTE '93, 13–18/06/1993, Avignon, France, Vol. 2 (1993) pp. 29–33.Google Scholar
3. Ewing, R.C., Lutze, W. and Weber, W. J., J. Mater. Res. 10, 243 (1995).Google Scholar
4. Ebbinghaus, B., VanKonynenburg, R., Ryerson, F., et al., Proc. Int. Symp. WASTE MANAGEMENT '98, Tucson, AZ, USA, 1998, CD version, Rep. 65–04 (1998).Google Scholar
5. Burakov, B.E. and Strykanova, E.E., Proc. Intern. Conf. WASTE MANAGEMENT '98, Tucson, USA, 1–5/03/1998, CD-ROM, http://localhost:6017/html/sess34/34–05/34–05.htm (1998).Google Scholar
6. Burakov, B.E., Anderson, E.B., et al., in Scientific Basis for Nuclear Waste Management XXIII, edited by Smith, R.W. and Shoesmith, D.W. (Mat. Res. Soc. Proc. 608, Warrendale, PA, 2000) pp. 419–422.Google Scholar
7. Burakov, B.E. and Anderson, E.B., in Excess Weapons Plutonium Immobilization in Russia, edited by Jardine, J.L. and Borisov, G.B., UCRL-ID-138361, Proc. Meeting for Coordination and Review of Work, St. Petersburg Russia, 1–4/11/1999 (2000) pp. 167–179.Google Scholar
8. Burakov, B.E., Anderson, E.B., et al., in Scientific Basis for Nuclear Waste Management XXIV, edited by Hart, K.P. and Lumpkin, G.R. (Mat. Res. Soc. Proc. 663, Warrendale, PA, 2001) pp. 307–313.Google Scholar
9. Zamoryanskaya, M.V. and Burakov, B.E., in Scientific Basis for Nuclear Waste Management XXIII, edited by Smith, R.W. and Shoesmith, D.W. (Mat. Res. Soc. Proc. 608, Warrendale, PA, 2000) pp. 437–442.Google Scholar
10. Zamoryanskaya, M.V. and Burakov, B.E., in Scientific Basis for Nuclear Waste Management XXIV, edited by Hart, K.P. and Lumpkin, G.R. (Mat. Res. Soc. Proc. 663, Warrendale, PA, 2001) pp. 301–306.Google Scholar
11. Zamoryanskaya, M.V., Burakov, B.E., et al., in Scientific Basis for Nuclear Waste Management XXV, edited by McGrail, B.P. and Cragnolino, G.A. (Mat. Res. Soc. Proc. 713, Warrendale, PA, 2002) pp. 481–485.Google Scholar
12. Burakov, B.E., Hanchar, J.M., et al., Radiochimica Acta 89, 1 (2002).Google Scholar
13. Zamoryanskaya, M.V., Vainshenker, I.A. and Zamorianski, A.N., Equipment and Technique of Experiment, Vol.4, 104–106 (1987) (in Russian).Google Scholar
14. Arsenev, P.A., Hassan, H.V. and Chukichev, M.V., Phys. Status Solidi A, 28, K111 (1975).Google Scholar
15. Hessler, J.P. and Carnali, W.T., Am. Chem. Soc. Symp. Series, 131, 349 (1980).Google Scholar
16. Kaplianskiy, A.A. and Feofilov, P.P., Optics and Spectroscopy 16, 264 (1964).Google Scholar
17. Morozov, A.M., Morozova, L.G. and Feofilov, P.P., Optics and Spectroscopy 32, 50 (1972).Google Scholar