Hostname: page-component-78c5997874-ndw9j Total loading time: 0 Render date: 2024-11-10T15:23:52.473Z Has data issue: false hasContentIssue false

Spent fuel matrix oxidation studies under dry storage conditions

Published online by Cambridge University Press:  10 January 2017

Jone M. Elorrieta*
Affiliation:
Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas, CIEMAT, Avenida Complutense 40, 28040, Madrid, Spain.
Laura J. Bonales
Affiliation:
Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas, CIEMAT, Avenida Complutense 40, 28040, Madrid, Spain.
Nieves Rodríguez-Villagra
Affiliation:
Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas, CIEMAT, Avenida Complutense 40, 28040, Madrid, Spain.
Valentín G. Baonza
Affiliation:
MALTA-Consolider Team. Departamento de Química Física I, Facultad de Ciencias Químicas, Universidad Complutense, 28040, Madrid, Spain.
Joaquín Cobos
Affiliation:
Centro de Investigaciones Energéticas, Medioambientales y Tecnológicas, CIEMAT, Avenida Complutense 40, 28040, Madrid, Spain.
Get access

Abstract

A good understanding of the spent fuel matrix (UO2) behavior under predisposal activities conditions is required for the proper performance assessment of a final repository. Hence, the oxidation evolution of UO2 under dry interim storage conditions, as a main predisposal action within the Spanish strategy, needs to be addressed. For this aim, in this work a detailed in situ Raman spectroscopy study of the surface oxidation of a UO2.00 disk heated in the presence of synthetic air at 573 K is presented. The spectra analysis required two previous studies. In the first one, UO2+x powder samples with controlled degree of non-stoichiometry were identified by thermogravimetric analysis and subsequently characterized by Raman spectroscopy. The equations obtained from this study enable estimating the oxidation degree of any UO2+x sample (for x < 0.20) at atmospheric conditions. The second one was performed in order to use these equations for the in situ experiments (at 573 K), since the shift of the bands due to temperature needs to be taken into account. Thus, the behavior of the Raman spectra as a function of temperature was analyzed and a correction term thereafter introduced in the initial equations.

Type
Articles
Copyright
Copyright © Materials Research Society 2017 

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

Ferry, C., Poinssot, C., Cappelaere, C., Desgranges, L., Jégou, C., Miserque, F., Piron, J.P., Roudil, D. and Gras, J.M., J. Nucl. Mater., 352, 246253 (2006).CrossRefGoogle Scholar
McEachern, R. J. and Taylor, P., J. Nucl. Mater., 254, 87121 (1998).CrossRefGoogle Scholar
Willis, B.T.M., Proc. Br. Ceram. Soc., 1, 919 (1964).Google Scholar
Willis, B.T.M., Nature, 197, 755756 (1963).CrossRefGoogle Scholar
Hering, H. and Pério, P., Bull Soc. Quim., M. 531 (1952).Google Scholar
Jolibois, P., Acad, C. R.. Sci., 224, 13951396 (1947).Google Scholar
He, H. and Shoesmith, D., Phys. Chem. Chem. Phys., 12, 81088117 (2010).CrossRefGoogle Scholar
Desgranges, L., Baldinozzi, G., Simon, P., Guimbretière, G. and Canizares, A., J. Raman Spectrosc., 43, 455458 (2012).CrossRefGoogle Scholar
Allen, G.C., Butler, I.S. and Tuan, N.A., J. Nucl. Mater., 144, 1719 (1987).CrossRefGoogle Scholar
Palacios, M.L. and Taylor, S.H., Appl. Spectrosc., 54, 13721378 (2000).CrossRefGoogle Scholar
Stefaniak, E.A., Alsecz, A., Sajó, I.E., Worobiec, A., Máthé, Z., Török, S. and Van Grieken, R., J. Nucl. Mater., 381, 278283 (2008).CrossRefGoogle Scholar
Pointurier, F. and Marie, O., Spectrochim. Acta, Part B, 65, 797804 (2010).CrossRefGoogle Scholar
Manara, D. and Renker, B., J. Nucl. Mater., 321, 233237 (2003).CrossRefGoogle Scholar
Jun-bo, L., Gan, L. and Shu-lan, G., Spectrosc. Spect. Anal., 34(2), 405409 (2014).Google Scholar
Bonales, L.J., Elorrieta, J.M., Lobato, A. and Cobos, J., Raman Spectroscopy, a Useful Tool to Study Nuclear Materials, Applications of Molecular Spectroscopy to Current Research in the Chemical and Biological Sciences, Mark Stauffer, Dr. (Ed.), InTech (2016).Google Scholar
Elorrieta, J.M., Bonales, L.J., Rodríguez-Villagra, N., Baonza, V.G. and Cobos, J., Phys. Chem. Chem. Phys., 18, 2820928216 (2016).CrossRefGoogle Scholar
Marlow, P.G., Russell, J.P. and Hardy, J.R., Philos. Mag., 14, 409410 (1966).CrossRefGoogle Scholar
Livneh, T. and Sterer, E., Phys. Rev. B, 73, 085118085119 (2006).CrossRefGoogle Scholar
Rousseau, G., Desgranges, L., Charlot, F., Millot, N., Nièpce, J.C., Pijolat, M., Valdivieso, F., Baldinozzi, G. and Berar, J. F., J. Nucl. Mater., 355, 1020 (2006).CrossRefGoogle Scholar
Talsky, G., Derivative Spectrophotometry: Low and High Order, Verlagsgesellschaft, Weinheim (Federal Republic of Germany) and Inc., New York, NY (USA) (1994).CrossRefGoogle Scholar