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Contrôle microstructural des réactions rédox à l'interface solide/solution lors de la dissolution d'oxydes mixtes à base d'uranium (IV)

Abstract : In the field of the use of actinides mixed oxides as potential fuels for the Gen(III) and Gen(IV) nuclear reactors, solid solutions with general formula U1-xThxO2, U1-xCexO2-y, U0.75Nd0.25O1.875, U0.75Gd0.25O1.875 and Th0.75Nd0.25O1.875 were prepared by thermal conversion of oxalate precursors. Dense pellets exhibiting various physico-chemical and microstructural properties (in terms of composition, homogeneity, densification rate, …) were prepared through sintering then submitted to dissolution tests.The multiparametric study of the dissolution, performed in nitric, sulfuric and hydrochloric media clearly underlined the important effect of the chemical composition on the chemical durability of the samples. Indeed, several parameters (including partial order related to proton activity, apparent activation energy) confirmed the significant modification of the preponderant dissolution mechanism for uranium-enriched samples. Moreover, the role of various nitrogen-based species was evidenced at the solid/solution interface.The evolving of solid/solution interfaces (reactive surface area, composition) during dissolution was monitored by the means of operando ESEM experiments. Preferential dissolution zones (triple junctions, grain boundaries, inter- and intra-granular porosities) were clearly observed for uranium-depleted samples. They induce a significant increase of the reactive surface area even for short progress of the reaction. On the contrary, the dissolution appeared more homogenous for uranium-enriched samples due to the existence of a preponderant mechanism associated to the oxidation of the uranium(IV) at the interface.
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Florent Tocino. Contrôle microstructural des réactions rédox à l'interface solide/solution lors de la dissolution d'oxydes mixtes à base d'uranium (IV). Matériaux. Université Montpellier, 2015. Français. ⟨NNT : 2015MONTS247⟩. ⟨tel-02107707⟩

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