Hostname: page-component-78c5997874-m6dg7 Total loading time: 0 Render date: 2024-11-10T16:57:11.828Z Has data issue: false hasContentIssue false
  • English
  • Français

Chlorine Diffusion in Uranium Dioxide : Thermal Effects versus Radiation Enhanced Effects

Published online by Cambridge University Press:  19 October 2011

Yves Pipon ,
Nelly Toulhoat ,
Nathalie Moncoffre ,
Nicolas Bererd ,
Henri Jaffrezic ,
Marie France Barthe ,
Pierre Desgardin ,
Louis Raimbault ,
Andre M. Scheidegger  and
Gaelle Carlot
Yves Pipon
Affiliation:
pipon@ipnl.in2p3.fr, Institut de Physique Nucleaire de Lyon, CNRS/Universite Claude Bernard Lyon 1, 4 rue Enrico Fermi, Villeurbanne, 69622, France
Nelly Toulhoat
Affiliation:
nelly.toulhoat@univ-lyon1.fr, CNRS/IN2P3/IPNL, Université de Lyon / Université Claude Bernard Lyon 1 / IUT A Chimie, 4 rue Enrico Fermi, Villeurbanne, 69622, France
Nathalie Moncoffre
Affiliation:
moncof@ipnl.in2p3.fr, CNRS/IN2P3/IPNL, Université de Lyon / Université Claude Bernard Lyon 1 / IUT A Chimie, 4 rue Enrico Fermi, Villeurbanne, 69622, France
Nicolas Bererd
Affiliation:
bererd@ipnl.in2p3.fr, CNRS/IN2P3/IPNL, Université de Lyon / Université Claude Bernard Lyon 1 / IUT A Chimie, 4 rue Enrico Fermi, Villeurbanne, 69622, France
Henri Jaffrezic
Affiliation:
jaffrezic@ipnl.in2p3.fr, CNRS/IN2P3/IPNL, Université de Lyon / Université Claude Bernard Lyon 1 / IUT A Chimie, 4 rue Enrico Fermi, Villeurbanne, 69622, France
Marie France Barthe
Affiliation:
barthe@cnrs-orleans.fr, Centre d'Etudes et de Recherches par Irradiation, CNRS, 3A rue de la Ferollerie, Orleans cedex2, 45071, France
Pierre Desgardin
Affiliation:
desgardin@cnrs-orleans.fr, Centre d'Etudes et de Recherches par Irradiation, CNRS, 3A rue de la Ferollerie, Orleans cedex2, 45071, France
Louis Raimbault
Affiliation:
louis.raimbault@ensmp.fr, Centre d'Informatique Geologique (CIG), Ecole des Mines, 35 rue Saint Honore, Fontainebleau cedex, 77305, France
Andre M. Scheidegger
Affiliation:
andre.scheidegger@psi.ch, Nuclear Energy and Safety Department (NES), Laboratory for Waste Management, Paul Scherrer Institut, Villigen, 5235, Switzerland
Gaelle Carlot
Affiliation:
gaelle.carlot@cea.fr, DEN/DEC/SESC/LLCC, Commissariat a l'Energie Atomique, Centre de Cadarache, Saint Paul lez Durance, 13108, France
Get access

Abstract

Chlorine is present as an impurity in the UO2 nuclear fuel. 35Cl is activated into 36Cl by thermal neutron capture. In case of interim storage or deep geological disposal of the spent fuel, this isotope is known to be able to contribute significantly to the instant release fraction because of its mobile behavior and its long half life (around 300000 years). It is therefore important to understand its migration behavior within the fuel rod. During reactor operation, chlorine diffusion can be due to thermally activated processes or can be favoured by irradiation defects induced by fission fragments or alpha decay. In order to decouple both phenomena, we performed two distinct experiments to study the effects of thermal annealing on the behaviour of chlorine on one hand and the effects of the irradiation with fission products on the other hand. During in reactor processes, part of the 36Cl may be displaced from its original position, due to recoil or to collisions with fission products. In order to study the behavior of the displaced chlorine, 37Cl has been implanted into sintered depleted UO2 pellets (mean grain size around 18 μm). The spatial distribution of the implanted and pristine chlorine has been analyzed by SIMS before and after treatment. Thermal annealing of 37Cl implanted UO2 pellets (implantation fluence of 1013 ions.cm−2) show that it is mobile from temperatures as low as 1273 K (Ea=4.3 eV). The irradiation with fission products (Iodine, E=63.5 MeV) performed at 300 and 510 K, shows that the diffusion of chlorine is enhanced and that a thermally activated contribution is preserved (Ea=0.1 eV). The diffusion coefficients measured at 1473 K and under fission product irradiation at 510 K are similar (D = 3.10-14 cm2.s−1). Considering in first approximation that the diffusion length L can be expressed as a function of the diffusion coefficient D and time t by : L=(Dt)1/2, the diffusion distance after 3 years is L=17 μm. It results that there is a great probability for the chlorine contained in the UO2 grains to have reached the grain boundaries after 3 years, in the core of the fuel rod as well as at its periphery. Moreover, diffusion and concentration of chlorine at grain boundaries has been evidenced using SIMS mapping. Our results indicate therefore, that, during reactor operation and after, the majority of 36Cl is likely to have moved to grain boundaries, rim and gap. This fraction might then significantly contribute to the rapid or instant release of chlorine. This could have important consequences for safety assessment.

Keywords

ion-implantationCldiffusion
Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 985: Symposium NN – Scientific Basis for Nuclear Waste Management XXX , 2006 , 0985-NN05-03
Copyright
Copyright © Materials Research Society 2007

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. Johnson, L., Poinssot, C., Ferry, C. and Lovera, P., “Estimates of the instant release Fraction for UO2 and MOX Fuel at t = 0, A Report of the Spent Fuel Stability [SFS]”, Project of the 5th Euratom Framework Program (March 2005), Nagra Tech. Report NTB 04–08, Wettingen 2005.Google Scholar
2. Pipon, Y., Thermal and irradiation induced diffusion of chlorine in uranium dioxide”, PhD thesis (264–2006), Université Claude Bernard Lyon 1, France, December 2006.Google Scholar
3. Pipon, Y., Toulhoat, N., Moncoffre, N., Jaffrezic, H., Gavarini, S., Martin, P., Raimbault, L., Scheidegger, A. M., Radiochim. Acta 94, 705–711 (2006).Google Scholar
4. Pipon, Y., Toulhoat, N., Moncoffre, N., Raimbault, L., Scheidegger, A. M., Farges, F., Carlot, G., in press, J. Nucl. Mat., DOI : 10.1016/j.jnucmat.2007.01.212 (2007).Google Scholar
5. Pipon, Y., Bérerd, N., Moncoffre, N., Peaucelle, C., Toulhoat, N., Jaffrézic, H., Raimbault, L., Sainsot, P., Carlot, G., in press, Nucl. Instrum. Meth. B, DOI :10.1016/j.nimb.2007.01.105 (2007).Google Scholar
6. Ziegler, J. F., Biersaack, J. P., Littmark, U., “The Stopping and Range of Ions in Solids”, 1985, New York.Google Scholar
7. Desgardin, P., Liszkay, L., Barthe, M.-F. et al., Mater. Sci. Forum 363–365, 523 (2001).Google Scholar
8. Barthe, M.-F., Guilbert, S., Labrim, H., Desgardin, P., Sauvage, T., Blondiaux, G., Carlot, G., Garcia, P. and Piron, J.P., Mater. Sci. Forum 48, 445–446 (2004).Google Scholar
9. Labrim, H., Barthe, M.-F., Desgardin, P., Sauvage, T., Blondiaux, G., Corbel, C., Piron, J.P., Appl. Surf. Sci. 252, 3256 (2006).Google Scholar
10. Hocking, W. H., Verrall, R. A. and Muir, I. J., J. Nucl. Mater. 294, 45–52 (2001).Google Scholar
11. Akabori, M., and Fukuda, K., J. Nucl. Mater. 186, 47–53 (1991).Google Scholar
12. Matzke, H. J., Rad. Effects 75, 317–325 (1983).Google Scholar
13. Nakae, N., Harada, A., Kirihara, T., Nasu, S., J. Nucl. Mater. 71, 314 (1978).Google Scholar
14. Catlow, C. R., Proc.R. Soc. London Ser. A 353, 533–566 (1977).Google Scholar