Catalyzed Oxidation of Nuclear Graphite by Simulated Fission Products Sr, Eu, and I

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The influence of three fission products Sr, Eu, and I on the oxidation of IG-110 nuclear graphite was studied in the temperature range of 400 to 1000 °C. Sr and Eu were introduced as chlorides, and I was introduced as NaI. The temperature dependence of both CO2 and CO production during the graphite oxidation measured with mass spectroscopy and infrared spectrometry shows that the introduction of these three compounds to graphite significantly decreases the onset temperature for the oxidation of graphite. Among the three compounds, NaI is the most active towards the oxidation reaction, characterized by a significant decrease of the onset temperature from approximately 650 to 400 °C before and after its introduction to graphite. Separate measurements of CO2 and CO concentration at varying temperatures enable the calculation of the activation energy for the formation of CO2 and CO. The activation energies for the oxidation of pure and fission product-impregnated graphite samples decrease in the following order: standard IG-110 graphite, EuCl3-impregnated IG-110, SrCl2-impregnated IG-110, and NaI-impregnated IG-110. This trend indicates that the three compounds catalyze the oxidation of graphite at temperatures relevant to the operation of high-temperature gas-cooled reactors. Furthermore, it is found that the three compounds can also affect the molar ratio of reaction products CO2 and CO, and the rates of the graphite oxidation. At temperatures higher than about 850 °C, the impregnated samples exhibit lower CO2: CO ratios than the pure graphite. Different from EuCl3 and NaI, the introduction of SrCl2 decreases the graphite oxidation rates at temperatures higher than about 770 °C. Their catalytic mechanism can be understood based on a redox cycle of the intermediate active species, promoting the dissociation of molecular oxygen and transfer to the carbon.