Characterization of uranium in bituminized radioactive waste drums by self-induced X-ray fluorescence

This paper reports the experimental qualification of an original uranium characterization method based on fluorescence X rays induced by the spontaneous gamma emission of bituminized radioactive waste drums. The main 661.7 keV gamma ray following the ¹³⁷Cs decay produces by Compton scattering in the bituminized matrix an intense photon continuum around 100 keV, i.e. in the uranium X-ray fluorescence region. 'Self-induced' X-rays produced without using an external source allow a quantitative assessment of uranium as ¹³⁷Cs and uranium are homogeneously mixed and distributed in the bituminized matrix. The paper presents the experimental qualification of the method with real waste drums, showing a detection limit well below 1 kg of uranium in 20 min acquisitions while the usual gamma rays of ²³⁵U (185 keV) or ²³⁸U (1001 keV of ^234mPa in the radioactive decay chain) are not detected. The relative uncertainty on the uranium mass assessed by self-induced X-ray fluorescence (SXRF) is about 50%, with a 95% confidence level, taking into account the correction of photon attenuation in the waste matrix. This last indeed contains high atomic numbers elements like uranium, but also barium, in quantities which are not known for each drum. Attenuation is estimated thanks to the peak-to-Compton ratio to limit the corresponding uncertainty. The SXRF uranium masses measured in the real drums are in good agreement with long gamma-ray spectroscopy measurements (1001 keV peak) or with radiochemical analyses. (authors)