Burnup determination in irradiated fuel by means of isotopic analysis and comparison to CASMO calculations

One of the traditional methods for determining the burnup of irradiated Light Water Reactor (LWR) fuel is the 148Nd method according to ASTM E-321. Probably one of the largest sources for systematic errors in this method is the assumed fission yield, requiring knowledge of the fraction of fissions occurring in different fissile nuclides. Another traditional method for burnup determination is based on the uranium and plutonium isotopic composition; however, this method is rarely used for LWR fuel due to its rather simplified and rough assumptions regarding the neutron spectrum and fission fractions. However, modern physics codes like CASMO and HELIOS are instead able to calculate the amount of fission products and actinides formed or consumed during reactor operation in a much more sophisticated way. Isotopic Dilution Analysis with chemical separation of elements of interest, followed by isotopic analysis with a Thermal Ionization Mass Spectrometer (TIMS) is a well established method for determining the content of selected isotopes in samples of dissolved irradiated fuel. This method normally provides very accurate and precise results. High Performance Liquid Chromatography (HPLC) for elemental separations, combined with Inductively Coupled Plasma Mass Spectrometry (ICP-MS) has become a much faster alternative. In general, this method is somewhat less precise. This disadvantage is at least partly compensated by the possibility of analyzing a larger number of nuclides and samples. The local pellet burnup of a well characterised fuel sample irradiated in the Swedish Boiling Water Reactor Forsmark 3 to about 60 MWd/kgU was determined. Weight ratios of neodymium isotopes relative to 238U, analysed by Isotope Dilution Analysis applying HPLC-ICP-MS as well as 235U and 239Pu abundance values were compared to corresponding values calculated by a single-assembly CASMO-4 simulation. Input data were generated by CASMO-4/POLCA7 core tracking calculations. The overall result agreed very well with the burnup determined with methods corresponding to classical ASTM procedures by two independent laboratories. Thus, the present method is a well suited alternative. It is much faster and does not need any correction factors requiring knowledge of the fraction of fissions in different fissile isotopes. This eliminates the largest source for systematic errors. (author)