Abstract
The chemical behaviour of the main elements present in a PWR irradiated fuel sample (UO2 fuel, Zr from the Zircaloy-cladding, Pu, Np, and fission products such as Ba, Ce, Cs, Gd, I, La, Mo, Nd, Pd, Rh, Ru, Sr, Tc, Te, etc.) submitted to a nuclear severe accident type sequence (VERDON-1 experiment) has been investigated by thermodynamic calculations using the TAF-ID database. Particular emphasis has been placed on the chemical behaviour of the fission products Ba, Cs, Mo, and Zr, and the interactions between the Zircaloy-cladding and the UO2 matrix. Calculation results have been compared to experimental observations completed during the VERDON-1 experiment (instantaneous release of fission products and final chemical state of elements in the sample). Results presented in this manuscript do not account for non-equilibrium phenomena that have a major impact on fission product behaviour (e.g., chemical diffusion, mass transport induced by temperature gradients in the fuel pellet, etc.). None the less, these TAF-ID calculations have described accurately the melting of the sample following the formation of a mixed (U,Zr)O2-x phase because of the interaction between the fuel and the Zircaloy-cladding. Furthermore, calculations have assisted in the explanation of the instantaneous released fractions observed for Ba and Mo during the experiment (as a function of the experiment atmosphere and temperature).
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