In-situ high resolution photoelectron spectroscopy study on interaction of sodium with UO2+x film (0 ≤ x ≤ 1)

Autor: Loïc Favergeon, C. Andrello, Rachel Eloirdi, E.A. Tereshina-Chitrova, Ladislav Havela, Thomas Gouder, R.J.M. Konings, L. Desgranges
Přispěvatelé: CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Commissariat à l'énergie atomique et aux énergies alternatives (CEA), European Commission - Joint Research Centre [Karlsruhe] (JRC), Département Procédés de Transformations des Solides et Instrumentation (PTSI-ENSMSE), Centre Sciences des Processus Industriels et Naturels (SPIN-ENSMSE), École des Mines de Saint-Étienne (Mines Saint-Étienne MSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-École des Mines de Saint-Étienne (Mines Saint-Étienne MSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT), Laboratoire Georges Friedel (LGF-ENSMSE), Institut Mines-Télécom [Paris] (IMT)-Institut Mines-Télécom [Paris] (IMT)-Université de Lyon-Centre National de la Recherche Scientifique (CNRS), Département d'Etudes des Combustibles (DEC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), Service d'Analyses, d'Elaboration, d'Expérientations et d'Examens des combustibles (SA3E), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-CEA-Direction des Energies (ex-Direction de l'Energie Nucléaire) (CEA-DES (ex-DEN)), Laboratoire d'Analyse de la Migration des Radioéléments (LAMIR), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Département d'Etudes des Combustibles (DEC), Nuclear Physics Institute of the AS CR, Charles University [Prague] (CU), Faculty of Mathematics and Physics [Praha/Prague], Commission européenne - Centre commun de recherche (Joint Research Centre), Commissariat à l’énergie atomique et aux énergies alternatives - DEN/DEC/SA3E/LAMIR, Institute of Physics - ASCR, Faculty of Mathematics and Physics - Charles University
Rok vydání: 2021
Předmět:
Zdroj: Journal of Nuclear Materials
Journal of Nuclear Materials, Elsevier, 2021, 545, pp.152646. ⟨10.1016/j.jnucmat.2020.152646⟩
Journal of Nuclear Materials, 2021, 545, pp.152646. ⟨10.1016/j.jnucmat.2020.152646⟩
ISSN: 0022-3115
DOI: 10.1016/j.jnucmat.2020.152646
Popis: International audience; We studied in-situ the interaction of sodium metal with UO2+x (0 ≤ x ≤ 1) using thin films prepared by sputter deposition on Au substrate. X-ray Photoelectron Spectroscopy (XPS) and Grazing Incidence XRay Diffraction (GIXRD) characterized films before and after interaction. The results show that sodium does not reduce stoichiometric UO2 at room temperature. Plasmon loss peaks, observed at the Na1s photoemission (PE) line, are characteristic of metallic sodium particles, and point to a weak interaction between sodium and UO2. The oxidation of the sodium at room temperature takes place only on hyperstoichiometric uranium dioxide films. Indeed, sodium deposition on UO2+x (0 < x ≤ 1), eventually results in the complete reduction of U(VI) down to U(IV). Molecular and atomic oxygen affect differently the oxidation of uranium and sodium. The wetting of the gold by the sodium is much more important when sodium is oxidised by atomic oxygen. This leads to a shift of the Na1s core level peak, while molecular oxygen gives a peak broadening without shift. Atomic oxygen seems to play the same role as the interstitial oxygen present in the UO2+x film. The oxygen dissociation may be the limiting step of sodium oxidation on gold and on UO2. Heat treatment of sodium on UO3 at about 773 K leads to the formation of the NaUO3 film as demonstrated by a quantitative analysis by XPS and GIXRD. The results show also that once U(V) is formed, it stays stable up to at least 973 K, the temperature at which shrinkage of the film is observed.
Databáze: OpenAIRE