Etude de la dissolution du dioxyde d'uranium en milieu nitrique : une nouvelle approche visant à la compréhension des mécanismes interfaciaux

Abstract : The reprocessing of irradiated nuclear fuel passes through a stage of separation of uranium, plutonium and fission products by dissolution in nitric acid. To be able to optimize the process regardless of the fuel used, it is necessary to understand physical and chemical phenomena, kinetics and hydrodynamic parameters involved in the process, to allow its modelling and to be able to forecast behaviours during the operation. The state of the art can only provide limited guidance because it is based on macroscopic studies in reactors of hundreds of millilitres. The conclusions that can be drawn are therefore subject to the overlay of microscopic phenomena related to the complexity of the nitric mid, and to the composition and nature of the solid to dissolve that are generally poorly defined. It is therefore necessary to use another approach which is to separate and analyze the various processes involved. A model implementing a coupling between hydrodynamics and kinetics involved in the dissolution of a solid in the presence of autocatalytic species is then proposed. This model was used to highlight the need for observations of the concentrations of the species at the level of the reactive interface. A miniaturized reactor was designed, and experiments were conducted on copper beads, simulating the fuel, and provided initial observations of gas bubbles formed during dissolution. A novel method for monitoring pH in-situ at the level of the interface has been developed: a fluorescent marker enabled to visualize in-situ acidity and pH mapping during dissolution, and a direct visualization of the transfer process with diffusion layers. This method could be transposed in the nuclear area on uranium dioxide and has led to the understanding and modelling of the process of dissolution in nitric environment.
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Céline Delwaulle. Etude de la dissolution du dioxyde d'uranium en milieu nitrique : une nouvelle approche visant à la compréhension des mécanismes interfaciaux. Autre. Institut National Polytechnique de Lorraine, 2011. Français. ⟨NNT : 2011INPL078N⟩. ⟨tel-01749486⟩

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