Iodine behaviour under LWR accident conditions: Lessons learnt from analyses of the first two Phebus FP tests

摘要

The International Phebus Fission Product programme, initiated in 1988 and performed by the French "Institut de Radioprotection et de Surete Nucleaire" (IRSN), investigates through a series of in-pile integral experiments, key phenomena involved in light water reactor (LWR) severe accidents. The tests cover fuel rod degradation and the behaviour of fission products released via the primary coolant circuit into the containment building. The results of the first two tests, called FPT0 and FPT1, carried out under low pressure, in a steam rich atmosphere and using fresh fuel for FPT0 and fuel burned in a reactor at 23 GWdt~(-1) for FPT1, were immensely challenging, especially with regard to the iodine radiochemistry. Some of the most important observed phenomena with regard to the chemistry of iodine were indeed neither predicted nor pre-calculated, which clearlyshows the interest and the need for carrying out integral experiments to study the complex phenomena governing fission product behaviour in a PWR in accident conditions. The three most unexpected results in the iodine behaviour related to early detection during fuel degradation of a weak but significant fraction of volatile iodine in the containment, the key role played by silver rapidly binding iodine to form insoluble Agl in the containment sump and the importance of painted surfaces in the containment atmosphere for the formation of a large quantity of volatile organic iodides. To support the Phebus test interpretation small-scale analytical experiments and computer code analyses were carried out. The former, helping towards a better understanding of overall iodine behaviour, were used to develop or improve models while the latter mainly aimed at identifying relevant key phenomena and at modelling weaknesses. Specific efforts were devoted to exploring the potential origins of the early-detected volatile iodine in the containment building. If a clear explanation has not yet been found, the non-equilibrium chemical processes favoured in the primary coolant circuit and the early radiolytic oxidation of iodides in the condensed water films are at present the most likely explanations. Models that were modified or developed and embodied in the computer codes for organic iodide formation/destruction in the gas phase and Ag-I reactions in the sump lead, in agreement with the Phebus findings respectively to greatly enhanced organic iodide formation kinetics and long term concentration in the containment atmosphere on one hand and, in the conditions of Phebus experiments, to significantly limited molecular iodine volatilisation from the sump in so far as silver was in excess compared to iodine, on the other hand. Organic iodides then quickly gain in importance and become the predominant volatile iodine species at long term.