Radiolytic oxidation of iodine in the containment at high temperature and dose rate

Iodine Chemistry is one of the areas of top interest in the field of nuclear power plants (NPP) severe accidents studies. The strong radiological impact of iodine on man health and environment, mostly through its isotope I-131, has made it a key point to get an accurate prediction of the potential iodine release from the NPP containment to the environment in the low probable event of an accident leading to core melt. Released from the fuel as a gaseous form, iodine enters the containment in gaseous or particulate form and undergoes deposition processes that eventually take it to the containment surfaces and sump. Once in the sump, iodine, when present as soluble compounds, gets dissolved as non volatile iodide (I-). Nonetheless, in the presence of radiation and particularly in acidic sumps, iodine can be oxidized to volatile forms such as molecular iodine (I2) and can escape from the sump to the containment atmosphere (sump radiolysis process), thus increasing its potential contribution to the iodine source term. Iodine sump radiolysis has been extensively studied experimentally in the past decades. Experiments have revealed that parameters such as pH, temperature and total iodine concentration have a large impact on iodine volatility. However, experimental data at elevated temperatures (> 80OC) and elevated dose rates (> 1 kGy.h-1) anticipated in containment during a postulated severe accident are too scarce to provide for these relevant conditions an accurate determination of the volatile iodine fractions. Furthermore, some data were obtained from post-irradiation analysis and iodine concentration may be underestimated at the time of measurements compared with that during irradiation, due to post-irradiation reactions. To complete the existing database, the EPICUR program was launched by IRSN (Institut de Radioprotection et de Surete Nucleaire) and experiments have been performed in the frame of the International Source Term Program (ISTP) to provide on-line measurements of iodine volatilisation during irradiation at elevated temperatures and dose rates. This paper presents a description of the EPICUR facility and an overview of the experiments carried out so far to investigate radiolytic oxidation under those conditions in which data are to date insufficient. Experiments were performed using iodide solutions labelled with radioactive iodine (131I). Gamma spectrometers were used to measure the rate of iodine volatilization on-line at 80 and 120OC at a dose rate of 1.5 kGy.h-1. The impact of dissolved oxygen and pH on the production of molecular iodine was also investigated. Tests indicate that iodine volatilization rates increased with decreasing temperature and in the absence of oxygen. On the other hand, the iodine volatility decreases strongly with increasing pH. A comparison with existing experimental data in the field is provided together with perspectives for the modelling work. (author)