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Oxidation and Release of Ruthenium from White Inclusions

Abstract

In this paper the laboratory test results on oxidation and release of ruthenium as a fission product element are summarised. The ruthenium appears in the nuclear fuel pellets of pressurized water reactors as one of the fission product elements during burnup. In case of severe accident when the air can contact the degraded hot fuel, the ruthenium oxidises and its gaseous oxides, especially the RuO4, release rapidly from the pellets to the environment. Because of high radio- and chemotoxicity of ruthenium tetra-oxide further experimental study of oxidation and release is essential. It is well known that ruthenium in the irradiated fuel UO2 fuel appears in small metallic alloy precipitations together with fission product elements as Mo, Rh, Pd and Tc. The precipitations are seen in the metallographic pictures as white inclusions. This separate effect study focused on the differences in the release rate of gaseous ruthenium oxides when pure ruthenium or Mo-Ru-Rh-Pd metallic alloy is present in the simulated nuclear fuel. The oxidation and release were studied at constant reaction temperatures of 1000 or 1100 Celsius. The tests showed that during high-temperature oxidation of the Mo-Ru-Rh-Pd alloy in air flow the release rate of gaseous ruthenium oxides is reduced to 60-80% compared to the value measured in case of oxidation of pure metallic ruthenium powder in the same thermal-hydraulic conditions. Furthermore, if additional elements and chemical compounds representing other fission products were added in the alloy, a time delay of 30 to 60 min appeared in the release of gaseous ruthenium to the room-temperature environment. One of the main results was that in the outlet air flow reaching the environment the partial pressure of RuO4 was far above what could be expected for room-temperature equilibrium conditions. It was pointed out that the highly volatile RuO4 can decompose in solid, non-volatile RuO2 and O2. The X-ray fluorescence analysis results showed that some ruthenium compounds deposited on the colder circuit walls of the test facility. This suggests RuO4 is not fully airstable, i.e., its stability in air can be limited in time.JRC.F.4-Nuclear design safet

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