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Etude structurale de la synthèse de microsphères d’U1-xAmxO2±δ dédiées à la fabrication de couvertures chargées en américium

Abstract : One of the studied routes to reduce nuclear waste amount, is, after plutonium recycling, americium (Am) heterogeneous transmutation in fast neutron reactors, through the generation of short-lives and inert elements. Am irradiation requires the fabrication of U1-xAmxO2±δ pellets and the CRMP (Calcined Resin Microsphere Pelletization) process is currently considered as one the most promising candidate among other fabrication routes. It is based, before pellet sintering, on the compaction of U1-XAmXO2±δ oxide microspheres, synthetized through the thermal conversion of ion exchange resin microspheres, loaded with UO22+ and Am3+ cations. Compared to standard methods using powder metallurgy, CRMP process favours pressing step (easy microsphere flow) while limiting generation of highly radioactive Am-based fine particles. In this context, this PhD work was focused on the exhaustive characterization of CRMP process different steps, from a mechanistic and structural point of view. The cation molecular complex used in the resin was thus determined, highlighting carboxylic bidendate ligand binding around U and Am elements. Thermal conversion was also in-situ followed, and the structures of the different synthetized compounds evidenced and accurately characterized, i.e. (U1-XAmX)3O8 et U1-XAmXO2±δ. Am substitution in each of them was explained, revealing related distortions around U and Am cations. Finally, sintering of U1-XAmXO2-δ microspheres shaped into pellets was studied, showing a two-step densification. This unusual behavior corresponds to multi-scale reorganization into the material during sintering thermal treatment, associated to the presence of nanoparticles in the green pellet that sinter at low temperature.
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Marie Caisso. Etude structurale de la synthèse de microsphères d’U1-xAmxO2±δ dédiées à la fabrication de couvertures chargées en américium. Chimie inorganique. Université Montpellier, 2016. Français. ⟨NNT : 2016MONTT204⟩. ⟨tel-01758936⟩

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