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Communication Dans Un Congrès Année : 2023

Determination of the 144Ce/238U ratio in spent nuclear fuel samples by double spike isotope dilution mass spectrometry

Résumé

Precise knowledge of the energy released by radioactive decay of nuclides (decay heat) after the shut down of a nuclear reactor is of major importance for spent fuel management and nuclear safety. Among those radionuclides, the 144Ce isotope is a fission product that significantly contributes to the decay heat for cooling time less than 10 years. The accurate quantification of this low abundance isotope in nuclear fuels is therefore required (1) to bring new constrains on neutronic calculation codes that predict the evolution of the spent nuclear fuel composition with time and (2) to improve the short-term management of irradiated fuels. An innovative method combining liquid chromatography with double spike isotope dilution and state of the art mass spectrometric techniques (MC-ICP-MS, TIMS) has been developed for this purpose. This new method was applied for the first time on two Mixed Oxide (MOx) spent nuclear fuel samples. It enabled the determination of 144Ce/238U atomic ratios of less than a hundred of ppm with expanded measurement uncertainty at around 1 % at the 95 % confidence level. This corresponds to a reduction of at least three times of the measurement uncertainty compared to classical gamma-ray approaches. In the case of UOX samples or irradiated fuels cooled for longer periods, the 144Ce content is even lower, i.e. 144Ce/238U in the range of a few ppm. Consequently, specific developments were carried out based on either extration techniques or HPLC and will also be discussed.
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Dates et versions

cea-04328749 , version 1 (07-12-2023)

Identifiants

  • HAL Id : cea-04328749 , version 1

Citer

Anthony Nonell, Aurélien Beaumais, Céline Caussignac, Sébastien Mialle, Guillaume Stadelmann, et al.. Determination of the 144Ce/238U ratio in spent nuclear fuel samples by double spike isotope dilution mass spectrometry. AnalytiX-2023, May 2023, OSAKA, Japan. ⟨cea-04328749⟩
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