The electrochemical properties of alloy 690 in simulated pressurized water reactor primary water: Part I, effect of temperature

Journal of Nuclear Materials(2019)

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摘要
By anodic potentiostatic polarization and electrochemical impedance spectroscopy (EIS) measurements, the effect of temperature (200 °C, 250 °C, and 300 °C) on the electrochemical behavior of Alloy 690 was investigated in oxygenated borate buffer solution containing H3BO3 (2000 ppm B) + LiOH (2 ppm Li). The steady state passive current density was independent of the film formation potential at each temperature, indicating that the passive film is n-type in electronic character based on the predictions of the Point Defect Model (PDM). The passive current density increased and the absolute value of impedance decreased with increasing temperature, indicating a corresponding decrease in corrosion resistance. A mixed potential model (MPM), containing the PDM for describing the anodic passive dissolution of the alloy and the generalized Butler–Volmer equation for the cathodic oxygen reduction reaction was optimized on the experimental EIS data in order to extract model parameters, including kinetic parameters for the generation and annihilation of point defects in the barrier layer of the passive film. Metal (Cr,Ni,Fe) interstitials, which were found to have a higher concentration than oxygen vacancies, dominate the point defect structure of the barrier layer of the passive film at each temperature, thereby accounting for the n-type behavior of the passive film. With increasing temperature, the film thickness and defect density also increased, resulting in the decreased corrosion resistance of film. This indicates that the defect density of passive film plays a more important role on corrosion behavior of alloy than the film thickness.
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关键词
Alloy 690,Passive film,Anodic potentiostatic polarization,EIS,Optimization
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