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Radiation Effects on Hollandite Ceramics developed for Radioactive Cesium Immobilization

Published online by Cambridge University Press:  01 February 2011

V. Aubin
Affiliation:
LCAES (UMR CNRS 7574), ENSCP, 11 rue P.M. Curie, 75231 Paris, France
D. Caurant
Affiliation:
LCAES (UMR CNRS 7574), ENSCP, 11 rue P.M. Curie, 75231 Paris, France
D. Gourier
Affiliation:
LCAES (UMR CNRS 7574), ENSCP, 11 rue P.M. Curie, 75231 Paris, France
N. Baffier
Affiliation:
LCAES (UMR CNRS 7574), ENSCP, 11 rue P.M. Curie, 75231 Paris, France
S. Esnouf
Affiliation:
Commissariat à l'Energie Atomique, DSM/DRECAM/LSI, 91128 Palaiseau, France
T. Advocat
Affiliation:
Commissariat à l'Energie Atomique, DEN/DIEC/SCDV, 30207 Bagnolssur-Cèze, France
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Abstract

Progress on separating the long-lived fission products from the high level radioactive liquid waste (HLW) has led to the development of specific host matrices, notably for the immobilization of cesium. Hollandite (nominally BaAl2Ti6O16), one of the main phases constituting Synroc, receives renewed interest as specific Cs-host wasteform. The radioactive cesium isotopes consist of short-lived Cs and Cs of high activities and Cs with long lifetime, all decaying according to Cs+→Ba2++e- (β) + γ. Therefore, Cs-host forms must be both heat and (β,γ)-radiation resistant. The purpose of this study is to estimate the stability of single phase hollandite under external β and γ radiation, simulating the decay of Cs. A hollandite ceramic of simple composition (Ba1.16Al2.32Ti5.68O16) was essentially irradiated by 1 and 2.5 MeV electrons with different fluences to simulate the β particles emitted by cesium. The generation of point defects was then followed by Electron Paramagnetic Resonance (EPR). All these electron irradiations generated defects of the same nature (oxygen centers and Ti3+ ions) but in different proportions varying with electron energy and fluence. The annealing of irradiated samples lead to the disappearance of the latter defects but gave rise to two other types of defects (aggregates of light elements and titanyl ions). It is necessary to heat at relatively high temperature (T=800°C) to recover an EPR spectrum similar to that of the pristine material. The stability of hollandite phase under radioactive cesium irradiation during the waste storage is discussed.

Type
Research Article
Copyright
Copyright © Materials Research Society 2004

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References

REFERENCES

1. Madic, C., Lecomte, M., Baron, P. and Boullis, B., C. R. Physique 3, 797 (2002)Google Scholar
2. Mesko, M.G., Day, D.E. and Bunker, B.C., Waste Management 20, 271 (2000)Google Scholar
3. Bart, F., Sounilhac, S., Dussossoy, J.L., Bonnetier, A. and Fillet, C., in American Ceramic Society Conference Proceedings 1999, Ceram. Tr. 119, 353 (2001)Google Scholar
4. Stinton, D.P., Lackey, W.J. and Angelini, P., J. Am. Ceram. Soc. 66 (6), 389 (1983)Google Scholar
5. Strachan, D. M. and Schulz, W. W., Am. Ceram. Soc. Bull. 58(9), 865 (1979)Google Scholar
6. Carter, M.L., Vance, E.R., Mitchell, D.R.G., Hanna, J.V., Zhang, Z. and Loi, E., J. Mater. Res. 17, 2578 (2002)Google Scholar
7. Platt, R.G., Mineral. Mag. 58, 49 (1994)Google Scholar
8. Weber, W.J., Mat. Res. Soc. Sym. Proc 44, 671 (1985)Google Scholar
9. Bursill, L.A., Smith, D.J., J. Solid State Chem. 69 (1987) 343 Google Scholar
10. Aubin, V., Caurant, D., Gourier, D., Baffier, N., Advocat, T., Bart, F., Leturcq, G and Costantini, J M., Scientific Basis for Nuclear Waste Management XXVII, Kalmar, Sweden (2003) Mater. Res. Soc. Symp. Proc. (in press)Google Scholar
11. Hess, N.J., Espinosa, F.J., Conradson, S.D., Weber, W.J., J. Nucl. Mater. 281, 22 (2000)Google Scholar
12. Yamaga, M., Yosida, T, Henderson, B., O'Donnell, K.P. and Date, M., J. Phys. Condens. Matter 4, 7285 (1992)Google Scholar
13. Marfunin, A.S., in Spectroscopy, luminescence and radiation centers in Minerals (Springer, Verlag 1979) pp. 257262 Google Scholar
14. Kubo, R., Kawabata, A. and Kobayashi, S., Ann. Rev. Mater. Sci. 14, 49 (1984)Google Scholar