Thermodynamics applied to severe accidents - Present activities and perspectives
Résumé
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 our work is the investigation of the thermodynamics of the prototypic in-vessel corium U-Pu-Zr-Fe-O. The current approach is based on the CALPHAD method, which allows to obtain a thermodynamic model for this complex system starting from phase diagram and thermodynamic data. In this frame, 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 JRC-Karlsruhe. With the same laser heating technique, solidus temperatures have been obtained on the UO$_2$-PuO$_2$-ZrO$_2$ 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. 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. 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.
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