Fission Rates Measured Using High-Energy Gamma-Rays from Short Half-Life Fission Products in Fresh and Spent Nuclear Fuel

In recent years, higher discharge burn-ups and initial fuel enrichments have led to more and more heterogeneous core configurations in light water reactors (LWRs), especially at the beginning of cycle when fresh fuel assemblies are loaded next to highly burnt ones. As this trend is expected to continue in the future, the Paul Scherrer Institute has, in collaboration with the Swiss Association of Nuclear Utilities, swissnuclear, launched the experimental programme LIFE@PROTEUS. The LIFE@PROTEUS programme aims to better characterise interfaces between burnt and fresh UO2 fuel assemblies in modern LWRs. Thereby, a novel experimental database is to be made available for enabling the validation of neutronics calculations of strongly heterogeneous LWR core configurations. During the programme, mixed fresh and highly burnt UO2 fuel lattices will be investigated in the zero-power research reactor PROTEUS. One of the main types of investigations will be to irradiate the fuel in PROTEUS and measure the resulting fission rate distributions across the interface between fresh and burnt fuel zones. The measurement of fission rates in burnt fuel re-irradiated in a zero-power reactor requires, however, the development of new experimental techniques which are able to discriminate against the high intrinsic activity of the fuel. The principal goal of the present research work has been to develop such a new measurement technique. The selected approach is based on the detection of high-energy gamma-ray lines above the intrinsic background (i.e. above 2200 keV), which are emitted by short-lived fission products freshly created in the fuel. The fission products 88Kr, 142La, 138Cs, 84Br, 89Rb, 95Y, 90mRb and 90Rb, with half-lives between 2.6 min and 2.8 h, have been identified as potential candidates. During the present research work, the gamma-ray activity of short-lived fission products has, for the first time, been measured and quantitatively evaluated for re-irradiated burnt UO2 fuel samples with burn-ups of about 36 and 46GWd/t. Based on experiments carried out with these fuel samples in a reference test lattice of the PROTEUS reactor, fresh-to-burnt-fuel fission rate ratios could be determined. The 1σ uncertainties on the derived fission rate ratios are 1.7 to 3.4% and are mainly due to the statistical uncertainties. Calculated values of the fission rate ratios, as obtained using the Monte Carlo code MCNPX, have been shown to agree with the experimental results within these uncertainties. In deriving fresh-to-burnt-fuel fission rate ratios,142La and 138Cs have emerged as the preferred fission products. Their fission yields for the main fissile isotope (235U, 239Pu and 241Pu) are similar, which makes them relatively insensitive to the exact composition of the burnt fuel. Finally, a measurement station for the future LIFE@PROTEUS experiments has been proposed and evaluated, along with a detailed formulation of recommendations for optimised irradiation and measurement strategies. The estimated accuracy for the foreseen measurements of fission rate ratios between fresh and highly burnt fuel pins is 1 to 2%. The contribution of nuclear-data related uncertainties have been pointed out as possibly representing the main constraint on the achievable accuracy in future experiments. In brief, the present research work has established a novel experimental technique for measuring and comparing fission rates in fresh and highly burnt fuels in a zero-power research reactor such as PROTEUS. Moreover, possibilities have been presented for the further optimisation needed for a future, routine application of the technique.

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