Role of proton irradiation and relative air humidity on iron corrosion

This paper presents a study of the effects of proton irradiation on iron corrosion. Since it is known that in humid atmospheres, iron corrosion is enhanced by the double influence of air and humidity, we studied the iron corrosion under irradiation with a 45% relative humidity. Three proton beam intensities (5, 10 and 20 nA) were used. To characterise the corrosion layer, we used ion beam methods (Rutherford Backscattering Spectrometry (RBS), Elastic Recoil Detection Analysis (ERDA)) and X-ray Diffraction (XRD) analysis. The corrosion kinetics are plotted for each proton flux. A diffusion model of the oxidant species is proposed, taking into account the fact that the flux through the surface is dependent on the kinetic factor K. This model provides evidence for the dependence of the diffusion coefficient, D, and the kinetic factor, K, on the proton beam intensity. Comparison of the values for D with the diffusion coefficients for thermal oxygen diffusion in iron at 300 K suggests an enhancement due to irradiation of 6 orders of magnitude

Actinide diffusion in zirconium and the role of oxidation

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Fission Enhanced diffusion of uranium in zirconia

This paper deals with the comparison between thermal and Fission Enhanced Diffusion (FED) of uranium into zirconia, representative of the inner face of cladding tubes. The experiments under irradiation are performed at the Institut Laue Langevin (ILL) in Grenoble using the Lohengrin spectrometer. A thin $^{235}UO\_2$ layer in direct contact with an oxidized zirconium foil is irradiated in the ILL high flux reactor. The fission product flux is about 10$^{11}$ ions cm$^{-2}$ s$^{-1}$ and the target temperature is measured by an IR pyrometer. A model is proposed to deduce an apparent uranium diffusion coefficient in zirconia from the energy distribution broadening of two selected fission products. It is found to be equal to 10$^{-15}$ cm$^2$ s$^{-1}$ at 480$\circ$C and compared to uranium thermal diffusion data in ZrO$\_2$ in the same pressure and temperature conditions. The FED results are analysed in comparison with literature data

Modifications of oxidized Zircaloy-4 surface in contact with radiolysed wet air

International audienceIn the framework of radioactive waste geological disposal, the long term evolution of the nuclear wastes packages and the release of the radionuclides from the wastes have to be studied. Regarding compacted wastes (cladding tubes) coming from reprocessing of spent fuel, the Zircaloy-4 (zirconium alloy) cladding tubes have been activated and oxidized in reactors. In the disposal, the radioactive waste is exposed to humid air in a first phase and to water after the resaturation phase. In order to better assess the degradation process of these nuclear waste package, the influence of wet air proton radiolysis on the behavior of surface oxidized Zircaloy-4 has been investigated. Radiolysis experiments were performed using an irradiation cell which is associated to an extracted beam. Samples are exposed to wet air, under and without radiolysis, during 12 and 24 h. The water partial pressure has been fixed at 6 and 50 mbar in order to have, respectively, localized adsorbed water molecules and a thin film of adsorbed water. Before and after each treatment, sample surfaces were characterized by X-ray Photoelectron Spectroscopy (XPS) in order to identify the elements at the topmost surface of the solid. The wet air radiolysis causes changes at the surface of oxidized Zircaloy-4 and influences the corrosion phenomenon. Indeed, an enrichment of tin and the presence of nitrogen species were observed. It could be due to the formation of tritin(II) tetrahydroxide dinitrate and a Zr4+ tetramer on the topmost oxide surface

Zirconium oxidation under high energy heavy ion irradiation

This paper concerns the study of zirconium oxidation under irradiation with high energetic Xe ions. The irradiations were performed on the IRRSUD beam line at GANIL (Caen). The oxygen partial pressure was fixed at 10$^{-3}$ Pa and two temperature conditions were used, either 480$\circ$C reached by Joule effect heating or 280$\circ$C due to Xe energy deposition. Zirconia was fully characterized by Rutherford Backscattering Spectrometry, Transmission Electron Microscopy and Grazing Angle X-ray Diffraction. Apparent diffusion coefficients of oxygen in ZrO2 were determined from these experiments by using a model which takes into account a surface exchange between oxygen gas and the ZrO2 surface. These results are compared with thermal oxidation data

Use of the point defect model to interpret the iron oxidation kinetics under proton irradiation

This article concerns the study of iron corrosion in wet air under mega-electron-volt proton irradiation for different fluxes at room temperature and with a relative humidity fixed to 45%. Oxidized iron sample surfaces are characterized by ion beam analysis (Rutherford backscattering spectrometry and elastic recoil detection analysis), for the elemental analysis. The structural and physicochemical characterization is performed using the x-ray photoelectron spectroscopy and transmission electron microscopy techniques. We have also measured the iron oxidation kinetics. Radiation enhanced diffusion and transport processes have been evidenced. The modeling of the experimental data shows that the apparent oxygen diffusion coefficient increases whereas the oxygen transport velocity decreases as function of flux. Finally, the point defect model has been used to determine the electric field value in the samples. Results have shown that the transport process can be attributed to the presence of an electrical potential gradient

Diffusion thermique de l'uranium dans le zirconium - Application au stockage des gaines de combustibles

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Evolution de l'interface Zr/ZrO2_2 en condition reacteur - Mesure de la temperature

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Cladding of nuclear waste

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