Corrosion Science and Technology

The Corrosion Science Society of Korea (한국부식방식학회)
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In-situ Raman Spectroscopic Study of Nickel-base Alloys in Nuclear Power Plants and Its Implications to SCC

  • Kim, Ji Hyun (Department of Nuclear Engineering, Massachusetts Institute of Technology) ;
  • Bahn, Chi Bum (Department of Nuclear Engineering, Seoul National University) ;
  • Hwang, Il Soon (Department of Nuclear Engineering, Seoul National University)
  • Published : 2004.10.01
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Abstract

Although there has been no general agreement on the mechanism of primary water stress corrosion cracking (PWSCC) as one of major degradation modes of Ni-base alloys in pressurized water reactors (PWR's), common postulation derived from previous studies is that the damage to the alloy substrate can be related to mass transport characteristics and/or repair properties of overlaid oxide film. Recently, it was shown that the oxide film structure and PWSCC initiation time as well as crack growth rate were systematically varied as a function of dissolved hydrogen concentration in high temperature water, supporting the postulation. In order to understand how the oxide film composition can vary with water chemistry, this study was conducted to characterize oxide films on Alloy 600 by an in-situ Raman spectroscopy. Based on both experimental and thermodynamic prediction results, Ni/NiO thermodynamic equilibrium condition was defined as a function of electrochemical potential and temperature. The results agree well with Attanasio et al.'s data by contact electrical resistance measurements. The anomalously high PWSCC growth rate consistently observed in the vicinity of Ni/NiO equilibrium is then attributed to weak thermodynamic stability of NiO. Redox-induced phase transition between Ni metal and NiO may undermine the integrity of NiO and enhance presumably the percolation of oxidizing environment through the oxide film, especially along grain boundaries. The redox-induced grain boundary oxide degradation mechanism has been postulated and will be tested by using the in-situ Raman facility.

Keywords

References

  1. J.M. Gras, 'Stress corrosion cracking of steam generator tubing materials - review and assessment', Parkins Symposium on Fundamentals Aspects of Stress Corrosion Cracking, TMS, 1992, p411
  2. T.M. Angeliu, P.L. Andresen, and F.P. Ford, 'Applying slip-oxidation to the SCC of austenitic materials in BWR/PWR environments',Corrosion 98, NACE(1998), Paper No.262
  3. T. Magnin, J-M. Boursier, D. Noel, R. Rios, and F. Vaillant, 'Corrosion-deformation interaction during stress corrosion crackin~ of alloy 600 in primary water', Proceedings of the 6$^th$ International Symposium on Environmental Degradation of Materials in Nuclear Power System - Water Reactors, TMS, 1993, p.669
  4. P.M. Scott and M. Le Calvar, 'Some possible mechanisms of intergranular stress corrosion cracking of alloy 600 in primary water', Proceedings of the 6$^th$ InternationalSymposiumon Environmental Degradation of Materials in Nuclear Power System - Water Reactors, TMS, 1993, p.657
  5. P.M. Scott, 'An Overview of internal oxidation as a possible explanation of intergranular stress corrosion cracking of alloy 600 in PWRs', Proceedings of the 9$^th$ International Symposium on Environmental Degradation of Materials in Nuclear Power System - Water Reactors, TMS, 1999, p.3
  6. G. Was, T.M. Angeliu, and J.K. Sung, 'Deformation and intergranular cracking behavior of Ni-Cr-Fe alloys at high temperature', Proceedings of the 'Specialist Meeting on Environmental Degradation of Alloy600', Airlie House, VA, April 1993,EPRI Report TR-I 04898, 1996, p.24-1
  7. M.M. Hall, 'Thermally activated low temperature creep and primary water stress corrosion cracking of NiCrFe alloys', Proceedings of the 'Specialist Meeting on Environmental Degradation of Alloy600', Airlie House, VA, April 1993, EPRI Report TR-I04898, 1996, p.6-1
  8. R.S. Pathania, and A.R. McIlree, 'A review of the effect of hydrogen on stress corrosion crackin~ of alloy 600 in 360$^{\circ}C$ water', Proceedings of the 3$^rd$ International Symposium on Environmental Degradation of Materials in Nuclear Power System- Water Reactors, AIME, 1987, p.551
  9. T. Cassagne and A. Gelpi, 'Crack growth rate measurements an alloy 600 steam generator tubing in prima교 and hydrogenated AVT water', Proceedings of the 8$^th$ International Symposium on Environmental Degradation of Materials in Nuclear Power System Water Reactors, TMS, 1993, p.679
  10. C. Soustelle, M. Foucault, and P. Combrade, 'PWSCC of alloy 600: a parametric study of surface film effects', Proceedings of the 9$^th$ International Symposium on Environmental Degradation of Materials in Nuclear Power System - Water Reactors, TMS, 1999, p.105
  11. T. Cassagne, B. Fleury, F. Vaillant, O. De Bouvier, and P. Combrade, 'An Update of the Influence of Hydrogen on the PWSCC of nickel base alloy in high temperature water', Proceedings of the 8th International Symposium on Environmental Degradation of Materials in Nuclear Power System - Water Reactors, TMS, 1, 307 (1997)
  12. D. Caron, PhD. Thesis, INSA-Lyon Scientific and Technical University, France, 2000
  13. D.M. Himmelblau, 'Solubilities of inert gases in water O'C to near the critical point of water', J Chem. Eng. Data, 5, 10 (1960)
  14. W.S. Hurst, M.S. Hodes, W.J. Bowers Jr., V.E. Bean, J.E. Maslar, and K.A. Smith, 'Optical flow cell and apparatus for solubility, salt deposition and Raman spectroscopic studies in aqueous solutions near the water critical point', Journal of Supercritical Fluids 22 (2002): p.151
  15. J.H. Kim and I.S. Hwang, 'Development of in-situ Raman spectroscopic system of surface oxide films of metals and alloys in high temperature water conditions', submitted to Nuclear Engineering and Design (Feb., 2004)
  16. J.E. Maslar, W.S. Hurst, W.J. Bowers Jr., J.H. Hendricks, and M.1. Aquino, 'In situ Raman spectroscopic investigation of nickel hydrothermal corrosion', Corrosion 58, 225 (2002)
  17. J.E. Maslar, W.S. Hurst, W.J. Bowers Jr., and lH. Hendricks, 'In situ Raman spectroscopic investigation of stainless steel hydrothermal corrosion', Corrosion 58, 739 (2002)
  18. M.D. Cunha Belo, 'Composition, structure and properties of the oxide films formed on the stainless steels 316L in a primary type PWR environment', Corrosion Science, 40, 447 (1998)
  19. J.E. Maslar, W.S. Hurst, W.J. Bowers Jr., J.H. Hendricks, M.1. Aquino, and I. Levin, 'In situ Raman spectroscopic investigation of chromium surface under hydrothermal conditions', Applied Surface Science, 180, 102 (2001)
  20. R.L. McCreery, Raman spectroscopy for chemical analysis, (Wiley-Interscience, 2000)
  21. A.F. Well, Structural inorganic chemistry, 5$^th$ ed., (Oxford: Clarendon Press, 1984)
  22. F.A. Cotton, and G. Wilkinson, Advanced inorganic chemistry, A comprehensive test, 5$^th$ ed. (New York, NY:Wiley, 1980)
  23. R.G. Snyder and J.A. Ibers, 'O-H-O and O-D-O potential energy curves for chromous acid', J Chem. Phys. 36, 1356 (1962)
  24. J.E. Maslar, W.S Hurst, T.A. Vanderah, and I. Levin, 208 'The Raman spectra of Cr$_3$O$_8$ and Cr$_2$O$_5$,', J Raman Spectrosc. 32, 201 (2001)
  25. B.M. Weckhuysen, I.E. Wachs, and R.A. Schoonheydt, 'Surface chemistry and spectroscopy of chromium in inorganic oxides', Chem. Rev. 96, 3327 (1996)
  26. J.B.B. Heyns, J.J. Cruywagen, and K.T. Carron, 'Raman spectroscopic investigation of chromium (VI) equilibrium-another look', J Raman Spectrosc. 30, 335 (1999)
  27. G. Michel and R. Machiroux, 'Raman spectroscopic investigation of the Cr$_2$O$_4$$^2$-/Cr$_2$O$_47$$^2$- equilibrium in aqueous solution', J Raman Spectrosc. 14, 22 (1983)
  28. J.H. Kim, Ph. D. Dissertation, Seoul National University, Republic of Korea (2003)
  29. J. Gui and T. M. Devine, 'The influence of sulfate ions on the surface enhanced raman spectra of passive films formed on iron', Corros. Sci. 36, 441 (1994)
  30. C. A. Melendres, J. Acho and R. L. Knight, J Electrochem. Soc. 138, 877 (1991)
  31. T. Nakagawa, N. Totsuka, T. Terachi, and N. Nakajima, 'Influence of dissolved hydrogen on oxide film and PWSCC of alloy 600 in PWR primary water,' Journal of Nuclear Science and Technology, 40, 39 (2003)
  32. 'MULTEQ, Equilibrium of an electrolytic solution with vapor-liquid partitioning, Volume 3: Theory manual', EPRI NP-5561-CCML, Vol. 3, EPRI, Palo Alto, CA, 1992
  33. SA Attanasio, D.S. Morton, M.A. Ando, N.F. Panayotou, and C.D. Thompson, 'Measurement of the nickel/nickel oxide phase transition in high temperature hydrogenated water using the contact electric resistance (CER) techniques', Proceedings of the 10$^th$ International Symposium on Environmental Degradation of Materials in Nuclear Power System - Water Reactors, NACE, 2001
  34. E. Hillner, Zirconium in the Nuclear Industry, ASTM STP 633, p.211, Philadelphia, 1977
  35. B.G. Park, I.S. Hwang, 'Corrosion induced clogging and plugging in water-cooled generator cooling circuit', International conference on water chemistry in nuclear reactors systems, Chimie 2002, Avignon, France, April 22-26, 2002
  36. D.S. Morton, S.A. Attanasio, and G.A. Young, 'Primary water SCC understanding and characterization through fundamental testing in the vicinity of the nickel/nickel oxide phase transition', Proceedings of the 10$^th$ International Symposium on Environmental Degradation of Materials in Nuclear Power System - Water Reactors, NACE, 2001