Oxidation and Release of Ruthenium from White Inclusions

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

Oxidation and Release of Ruthenium from Short Fuel Rods above 1500oC

The fission product ruthenium is radiotoxic and in oxidized form as ruthenium-tetroxide (RuO4) also chemical toxic. During fuel element change or in case of a leakage in fuel storages, air flows in the containment or fuel storage. If the circulation pump fails, the fuel elements are heated-up, and at high temperatures gaseous ruthenium oxides are formed and rapidly released from the fuel. Due to the significant higher volatility of RuO4 in the Chernobyl Catastrophe the measured concentration of the Ru-isotopes in the fall-outs was comparable to those of iodine and caesium. In order to get more insight in the chemical and physical behaviour of this fission product under severe accident conditions, the Ruthenium release was studied in a series of Separate Effect Tests (RUSET). In the test short fuel rod segments were used and exposed to air and steam atmosphere at high temperatures. The experiments in air atmosphere showed, that the partial pressures of the released Ru-oxides was two orders of magnitudes lower compared to those measured in previous tests with Ru-powder diluted in a ZrO2 matrix. It was found that ruthenium was not released in steam atmosphere in the examined temperature range. Furthermore, the temperature dependence of the deposition was detected by XRF analysis.JRC.F.4-Nuclear design safet

Experimental investigation of the late phase of spent fuel pool accidents

Experimental programmes have been carried out in order to investigate the behaviour of nuclear fuel components in high-temperature air atmosphere, which characterises the main conditions of the late phase of spent fuel pool accidents. The tests provided new data on the oxidation of zirconium cladding in different atmospheres, on the oxidation and release of ruthenium from fuel pellets and on the integral behaviour of fuel bundles. The integral test confirmed that water injection into the spent fuel storage pool is the right measure to terminate a severe accident