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Traboulsi, A., Vandenborre, J., Blain, G., Humbert, B., Barbet, J. & Fattahi, M. (2014) Radiolytic Corrosion of Uranium Dioxide: Role of Molecular Species. J. Phys. Chem. C, 118 1071–1080.
Added by: Florent Boucher (2016-04-29 09:26:45) |
| Type de référence: Article DOI: 10.1021/jp409994y Numéro d'identification (ISBN etc.): 1932-7447 Clé BibTeX: Traboulsi2014 Voir tous les détails bibliographiques  |
Catégories: PMN Mots-clés: alpha-radiolysis, dissolution rates, hydrogen-peroxide, nuclear-fuel uo2, oxidation, raman-spectra, reducing conditions, spent fuel, waste-disposal conditions, water radiolysis Créateurs: Barbet, Blain, Fattahi, Humbert, Traboulsi, Vandenborre Collection: J. Phys. Chem. C |
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In this work, the oxidative corrosion of UO2 particles by molecular species produced by He-4(2+) radiolysis of water (simulated by irradiation with a He-4(2+) beam) has been investigated as a function of the absorbed dose under open and closed atmospheres. This work was carried out by coupling for the first time (1) characterization of the UO2 surface after oxidation, (2) analysis of H-2 and H2O2 produced by water radiolysis, and (3) quantification of the uranium species leached into the solution during irradiation. Oxidation of the surface of the UO2 particles was characterized by Raman spectroscopy. H-2 and H2O2 were analyzed by micro gas chromatography and UV-vis spectrophotometry, respectively. Inductively coupled plasma mass spectrometry was used to quantify the soluble uranium species released into the solution. The results showed that, when the ultrapure water above the UO2 particles was irradiated in an open atmosphere, metastudtite was formed on the UO2 surface, indicating its oxidation by the H2O2 produced by water radiolysis. This oxidation was accompanied by migration of soluble uranium species [U(VI)] into the irradiated solution. After irradiation in a closed atmosphere, oxidation of the UO2 surface and migration of soluble uranium species were limited due to the presence of H-2. The inhibition does not occur by direct effect of H-2 on H2O2 but more probably by adsorption of H-2 molecules on the UO2 surface.
Added by: Florent Boucher |