Studtite Formation Assessed by Raman Spectroscopy and 18O Isotopic Labeling during the Oxidative Dissolution of a MOX Fuel
| Autor: | Sylvain Peuget, Caroline Marques, Sandrine Miro, Magaly Tribet, Lola Sarrasin, Véronique Broudic, C. Jégou |
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| 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), Institut des Sciences et technologies pour une Economie Circulaire des énergies bas carbone (ISEC), Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA), This study was funded by the CEA and EDF as part of the PRECCI research program |
| Rok vydání: | 2021 |
| Předmět: |
Chemistry
Radiochemistry Oxidative phosphorylation Surfaces Coatings and Films Electronic Optical and Magnetic Materials Isotopic labeling symbols.namesake General Energy Studtite [PHYS.COND.CM-MS]Physics [physics]/Condensed Matter [cond-mat]/Materials Science [cond-mat.mtrl-sci] symbols Physical and Theoretical Chemistry Raman spectroscopy Dissolution MOX fuel |
| Zdroj: | Journal of Physical Chemistry C Journal of Physical Chemistry C, 2021, 125 (35), pp.19209-19218. ⟨10.1021/acs.jpcc.1c04392⟩ |
| ISSN: | 1932-7455 1932-7447 |
| DOI: | 10.1021/acs.jpcc.1c04392 |
| Popis: | The authors thank the technicians from DHA-Atalante facility who strongly participated to this experiment: Loïck Chauvin,Nathalie Vaissières, Manuel Delaville and Maxime Fagard.; International audience; The formation of studtite has been studied during the oxidative dissolution of a MIMAS MOX fuel disc in aerated water enriched in $^{18}$O under a gamma radiation source, coupling Raman spectroscopy and solution analyzes. The use of isotopic labeling allowed following the reactions responsible for the precipitation of studtite. At the beginning of the experiment, different $^{18}$O enrichments in the uranyl and peroxide bonds of the studtite were observed. While the uranyl bond was primarily enriched in $^{18}$O, the peroxide bond contained large amounts of $^{16}$O. This result suggests an oxygen contribution coming from different radiolytic species for each bond: H$_2$O$_2$ and radicals. The comparison with a UO$_2$ sample leached in similar conditions ruled out a role of the Pu alpha self-irradiation in this different behavior. Yet, the influence of the MOX MIMAS heterogeneous microstructure and chemistry is observed with the preferential dissolution of the UO$_2$ grains, the Pu-rich areas being much more stable with regard to the dissolution. In addition, the studtite first precipitates preferentially on the Pu-poor areas of the sample before covering the entire surface, including the plutonium-enriched aggregates, at the end of the experiment. |
| Databáze: | OpenAIRE |
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