Partitioning of selected fission products from irradiated oxide fuel induced by thermal treatment

The release of fission products (FPs) from spent nuclear fuel (SNF) has been studied as a function of the temperature and redox conditions. The present paper concerns essentially the high temperature separation of Cs and Sr from irradiated pressurized (PWR) and boiling water reactor (BWR) fuel of different burn-up levels with use of an in-house designed system for inductive vaporization (InVap). Using thermodynamic calculations with the Module of Fission Product Release (MFPR) code along with annealing experiments on SNF in the InVap it was shown that the speciation of Cs and Sr, hence their release behavior at high temperature, is sensitive to the redox conditions during thermal treatment. It was demonstrated that annealing conditions in the InVap can be adjusted in the way to promote the release of selected FPs without significant loss of the fuel matrix or actinides: complete release of Cs and I was achieved during treatment of irradiated fuel at 1800 °C under reducing atmosphere (0.7% H2/Ar mixture). The developed partitioning procedure can be used for the SNF pretreatment as an advanced head-end step in the hydrometallurgical or pyrochemical reprocessing technology.