Skip to main content
Log in

High-Temperature Oxidation of Zircaloy-4 in Air Studied with Labeled Oxygen and Raman Imaging

  • Original Paper
  • Published:
Oxidation of Metals Aims and scope Submit manuscript

Abstract

High-temperature oxidation of zirconium-based cladding materials is expected to be the primary cause of the fuel assemblies’ degradation in spent fuel storage pool loss-of-cooling accidents. Here, high-temperature Zircaloy-4 oxidation has been studied through two-stage oxidation experiments using 18O isotope. Particular attention is paid to the effect of a low-temperature pre-oxidation scale which aims to simulate the corrosion scale existing on spent fuel cladding. Raman imaging was used to investigate the 18O distribution in the scales exposed either to 18O2 or to 18O2 + N2 atmosphere at high temperature. Results were assessed against more conventional SIMS mapping. The use of the 18O isotope tracer technique associated with micro-Raman mapping of the scales is demonstrated to be a powerful method to investigate the transport properties in the scales and will help to gain understanding of the kinetic differences between different pre-oxides.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5

Similar content being viewed by others

References

  1. J. H. Baek and Y. H. Jeong, Journal of Nuclear Materials 361, 2007 (30).

    Article  Google Scholar 

  2. J. C. Brachet, V. Vandenberghe-Maillot, L. Portier, D. Gilbon, A. Lesbros, N. Waeckel, and J.-P. Mardon, Hydrogen content, preoxidation, and cooling scenario effects on post-quench microstructure and mechanical properties of Zircaloy-4 and M5 alloys in LOCA conditions, in Zirconium in Nuclear Industry: 15th International Symposium, ASTM STP 1505, eds. B. Kammenzind and M. Limbäck, (ASTM International, Sunriver, Oregon, 2008), pp. 91–118.

  3. T. Chuto, Oxidation of high burnup fuel cladding in LOCA conditions, in Fuel Safety Research Meeting, Tokai, Japan, May 19–20, 2010.

  4. T. Fuketa, JAERI experimental basis on RIA and LOCA, in OECD/CSNI/SEGFSM Meeting, OECD Headquarters, Paris, France, April 25–26, 2005.

  5. S. Guilbert, P. Lacote, G. Montigny, C. Duriez, J. Desquines and C. Grandjean, Effect of pre-oxide on Zircaloy-4 high temperature steam oxidation and post-quench mechanical properties, in Zirconium in Nuclear Industry: 17th International Symposium, ASTM STP 1543, eds. R. Comstock and P. Barbéris, (ASTM International, West Conshohocken, PA, 2014), pp. 1–27.

  6. M. Le Saux, J. C. Brachet, V. Vandenberghe, D. Gilbon, J. P. Mardon and B. Sebbari, Influence of pre-transient oxide on LOCA high temperature steam oxidation and post-quench mechanical properties of Zircaloy-4 and M5TM cladding, in Water Reactor Fuel Performance Meeting 2011, Chengdu, China, 2011, paper T3-040.

  7. S. Leistikow, G. Schanz and H. V. Berg, Kinetik und Morphologie der isothermen Dampf-Oxidation von Zircaloy 4 bei 700–1300°C, KFK 2587, 1978.

  8. B. Mazères, Etude expérimentale et modélisation de l’oxydation et des transformations de phases associées dans les gaines en alliage de zirconium, PhD Thesis, Institut National Polytechnique de Toulouse, 2013.

  9. V. Vrtilkova, Review of recent work at UJP PRAHA on the LOCA embrittlement criterion, in 6th Plenary Meeting of the OECD/CSNI/SEGFSM, Paris, April 25–26, 2005.

  10. K. Natesan, and W. K. Soppet, Air Oxidation Kinetics for Zr-Based Alloys, Argonne National Laboratory, US-NRC, NUREG/CR-5846, 2004.

  11. C. Duriez, D. Drouan and G. Pouzadoux, Journal of Nuclear Materials 441, 2013 (84).

    Article  Google Scholar 

  12. C. Duriez, M. Guerain., P. Lacote, and M. Mermoux, Effect of the pre-transient oxide on Zy-4 cladding degradation in air and air + steam atmospheres, in Fontevraud 8Contribution of Materials Investigations and Operating Experience to LWRs’ Safety, Performance and Reliability, Avignon, France, SFEN, September 15–18, 2014.

  13. S. N. Basu and J. W. Halloran, Oxidation of Metals 27, 1987 (143).

    Article  Google Scholar 

  14. N. S. McIntyre and M. J. Graham, Study of metal corrosion and oxidation phenomenon using secondary ion mass spectrometry, in Analytical Methods in Corrosion Science and Engineering, eds. P. Marcus and F. Mansfeld, 2006.

  15. I. Idarraga, M. Mermoux, C. Duriez, A. Crisci and J. P. Mardon, Oxidation of Metals 79, 2013 (289).

    Article  Google Scholar 

  16. I. Idarraga, M. Mermoux, C. Duriez, A. Crisci and J. P. Mardon, Journal of Nuclear Materials 421, 2012 (160).

    Article  Google Scholar 

  17. M. Guerain, M. Mermoux and C. Duriez, Corrosion Science 98, 2015 (140).

    Article  Google Scholar 

  18. A. Kasperski, C. Duriez and M. Mermoux, Combined Raman imaging and 18O tracer analysis for the study of Zircaloy-4 high temperature oxidation in spent fuel pool accident, in Zirconium in Nuclear Industry: 18th International Symposium, ASTM, submitted.

  19. B. K. Kim and H. O. Hamaguchi, Physica Status Solidi (B) 203, 1997 (557).

    Article  Google Scholar 

  20. M. Guerain, C. Duriez, J. L. Grosseau-Poussard and M. Mermoux, Corrosion Science 95, 2015 (11).

    Article  Google Scholar 

  21. B. Cox, Advances in Corrosion Science and Technology 5, 1976 (173).

    Article  Google Scholar 

  22. P. Bossis, D. Pêcheur, K. Hanifi, J. Thomazet, M. Blat and S. Yagnik, Journal of ASTM International 3, 2006 (1).

    Article  Google Scholar 

  23. M. Lasserre, V. Peres, M. Pijolat, O. Coindreau, C. Duriez and J. P. Mardon, Materials and Corrosion 65, 2014 (250).

    Article  Google Scholar 

Download references

Acknowledgements

This work has been performed within the frame of the DENOPI Project, funded by the French government as part of the “Investment for the Future” Program, Reference ANR-11-RSNR-0006. We warmly thank the whole DENOPI consortium for fruitful comments and discussions, and particularly the assistance of Dr. Christian Duriez (IRSN Cadarache, France). We also thank Etienne Bachelet from LCOGT for his advices on computer programming for data visualization.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Michel Mermoux.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Kasperski, A., Guérain, M., Mermoux, M. et al. High-Temperature Oxidation of Zircaloy-4 in Air Studied with Labeled Oxygen and Raman Imaging. Oxid Met 87, 501–513 (2017). https://doi.org/10.1007/s11085-017-9713-9

Download citation

  • Received:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11085-017-9713-9

Keywords

Navigation