Understanding of Corrosion Mechanisms of Zirconium Alloys after Irradiation: Effect of Ion Irradiation of the Oxide Layers on the Corrosion Rate

The irradiation damage in the fuel cladding material is mainly caused by the neutron flux resulting from the fission reactions occurring in the fuel. From an experimental point of view, the neutrons have the disadvantage to activate materials by neutron capture rendering them difficult to handle. To avoid these constraints inherent in the handling of radioactive material, the radiation effects on the corrosion resistance of zirconium alloys can be studied by irradiating the materials with ions. A new experimental approach using ion irradiation was performed in the Microscopy and Irradiation Damage Studies Laboratory of the CEA in Saclay, with the aim to study more specifically the influence of the irradiation damages in the oxide on the corrosion rate of the zirconium alloys. This study was, moreover, focused on a particular distribution of defects in the oxide layer, basically, localised close to the metal/oxide interface. From the results of the irradiation of the metal/oxide interface, it was clearly shown that, whatever the incident ion, the irradiation of the internal interface results in a significant increase of the oxygen diffusion flux ratios between the most irradiated Zircaloy-4 and the unirradiated one, whereas that of the oxide formed on M5(TM) induces a big decrease of the oxygen diffusion flux in the film. These effects are less marked with helium ions compared to protons (M5(TM) is a trademark of AREVA NP registered in the United States and in other countries). Finally, the oxide irradiation impact on the oxygen diffusion through the layer could explain the corrosion acceleration factor observed on Zy4 during the first cycles of irradiation, but cannot alone explain observed corrosion accelerations under high burn-up conditions. The discussion on the oxide irradiation effects puts forward the probable role of the residual charge left by ion implantation.