Ruthenium release modelling in air and steam atmospheres under severe accident conditions using the MAAP4 code

Abstract

In a nuclear power plant (NPP), a severe accident is a low probability sequence that can lead to core fusion and fission product (FP) release to the environment (source term). For instance during a loss-of-coolant accident, water vaporization and core uncovery can occur due to decay heat. These phenomena enhance core degradation and, subsequently, molten materials can relocate to the lower head of the vessel. Heat exchange between the debris and the vessel may cause its rupture and air ingress. After lower head failure, steam and air entering in the vessel can lead to degradation and oxidation of materials that are still intact in the core. Indeed, Zircaloy-4 cladding oxidation is very exothermic and fuel interaction with the cladding material can decrease its melting temperature by several hundred of Kelvin. FP release can thus be increased, noticeably that of ruthenium under oxidizing conditions. Ruthenium is of particular interest because of its high radio-toxicity due to 103Ru and 106Ru isotopes and its ability to form highly volatile compounds, even at room temperature, such as gaseous ruthenium tetra-oxide (RuO4). It is consequently of great need to understand phenomena governing steam and air oxidation of the fuel and ruthenium release as prerequisites for the source term issues. A review of existing data on these phenomena shows relatively good understanding. In terms of oxygen affinity, the fuel is oxidized before ruthenium, from UO2 to UO2+x. Its oxidation is a rate-controlling surface exchange reaction with the atmosphere, so that the stoichiometric deviation and oxygen partial pressure increase. High temperatures combined with the presence of oxygen in the atmosphere lead to fuel expansion and formation of cracks. In these conditions, intra- and inter-granular diffusions of ruthenium in the fuel matrix are so enhanced that it is possible to consider an instantaneous volatilisation of ruthenium oxides at the fuel surface. Based on these considerations, a completely new model has been implemented in the EDF local version of the MAAP4.07 severe accident code (Modular Accident Analysis Program), owned by EPRI (Electric Power Research Institute). The fuel oxidation modelling takes into account many kinds of atmospheres (steam and/or air and/or hydrogen), the stoichiometric evolution and the oxygen partial pressure of the fuel matrix. The release of ruthenium oxides is calculated considering their particular reaction constants. The model was assessed by the simulation of different CEA-VERCORS experiments in air, steam and mixed atmospheres. These experiments are specifically designed to study FP release from fuel under different atmospheres and temperatures. This paper deals with the main results obtained with MAAP4.07 when simulating these tests.