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Thermodynamic study of the in-vessel corium - Application to the corium/concrete interaction

Andrea Quaini 1, 2
1 LM2T - Laboratoire de Modélisation, Thermodynamique et Thermochimie
SCCME - Service de la Corrosion et du Comportement des Matériaux dans leur Environnement : DEN/DPC/SCCME
Abstract : During a severe accident in a pressurised water reactor, the nuclear fuel can interact with the Zircaloy cladding, the neutronic absorber and the surrounding metallic structure forming a partially or completely molten mixture. The molten core can then interact with the reactor steel vessel forming a mixture called in-vessel corium. In the worst case, this mixture can pierce the vessel and pour onto the concrete underneath the reactor, leading the formation of the ex-vessel corium. Furthermore, depending on the considered scenario, the corium can be formed by a liquid phase or by two liquids, one metallic the other oxide. The objective of this thesis is the investigation of the thermodynamics of the prototypic in-vessel corium U-Pu-Zr-Fe-O. The approach used during the thesis is based on the CALPHAD method, which allows to obtain a thermodynamic model for this complex system starting from phase diagram and thermodynamic data. Heat treatments performed on the O-U-Zr system allowed to measure two tie-lines in the miscibility gap in the liquid phase at 2567 K. Furthermore, the liquidus temperatures of three Zr-enriched samples have been obtained by laser heating in collaboration with ITU. With the same laser heating technique, solidus temperatures have been obtained on the UO2-PuO2-ZrO2 system. The influence of the reducing or oxidising on the melting behaviour of this system has been studied for the first time. The results show that the oxygen stoichiometry of these oxides strongly depends on the oxygen potential and on the metal composition of the samples. The miscibility gap in the liquid phase of the U-Zr-Fe-O system has been also observed. The whole set of experimental results with the literature data allowed to develop the thermodynamic model of the U-Pu-Zr-Fe-O system. Solidification path calculations have been performed for all the investigated samples to interpret the microstructures of the solidified samples. A good accordance has been obtained between calculation and experimental results. Heat treatments on two ex-vessel corium samples showed the influence of the concrete composition on the nature of the liquid phases formed at high temperature. The observed microstructures have been interpreted by means of calculation performed with the TAF-ID database. In parallel, a novel experimental setup named ATTILHA based on aerodynamic levitation and laser heating has been conceived and developed to obtain high temperature phase diagram data. This setup has been validated on well-known oxide systems. Furthermore, this technique allowed to observe in-situ, by using an infrared camera, the formation of a miscibility gap in the liquid phase of the O-Fe-Zr system by oxidation of a Fe-Zr sample. The next step of the development will be the nuclearization of the apparatus to investigate U-containing samples. The implementation of a very fast visible camera (5000 Hz) to investigate the thermo-physical properties of in-vessel and ex-vessel corium mixtures is also underway. The synergy between the development of experimental and calculation tools will allow to improve the thermodynamic description of the corium and the severe accident code using thermodynamic input data.
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Andrea Quaini. Thermodynamic study of the in-vessel corium - Application to the corium/concrete interaction. Materials. Université Grenoble Alpes, 2015. English. ⟨NNT : 2015GREAI061⟩. ⟨tel-01311262⟩

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