Partitioning of fission products from irradiated nitride fuel using inductive vaporization
Irradiated nitride fuel (Pu{sub 0.3}Zr{sub 0.7})N fabricated at PSI in frame of the CONFIRM project and having a burn-up of 10.4 % FIMA (Fission per Initial Metal Atom) has been investigated by means of inductive vaporization. The study of thermal stability and release behavior of Pu, Am, Zr and fission products (FPs) was performed in a wide temperature range (up to 2300 C. degrees) and on different redox conditions. On-line monitoring by ICP-MS detected low nitride stability and significant loss of Pu and Am at T>1900 C. degrees during annealing under inert atmosphere (Ar). The oxidative pre-treatment of nitride fuel on air at 1000 C. degrees resulted in strong retention of Pu and Am in the solid, as well as of most FPs. Thermodynamic modelling of elemental speciation using GEM-Selektor v.3 code (Gibbs Energy Minimization Selektor), supported by a comprehensive literature review on thermodynamics of actinides and FPs, revealed a number of binary compounds of Cs, Mo, Te, Sr and Ba to occur in the solid. Speciation of some FPs in the fuel is discussed and compared to earlier results of electron probe microanalysis (EPMA). Predominant vapor species predicted by GEM-Selektor calculations were Pu(g), Am(g) and N{sub 2}. Nitrogen can be completely released from the fuel after complete oxidation at 1000 C. degrees. With regard to the irradiated nitride reprocessing technology, this result can have an important practical application as an alternative way for {sup 15}N recovery. (authors)