Non-destructive measurements of uranium and thorium concentrations and quantities

The passive X-ray fluorescent-gamma spectrometry method and technique for uranium concentration measurements was developed and tested. It is based on the measurement of the intensity ratios of self-excited Ksub(α) X-rays of uranium to the intensity of the combined peak with 92.8 keV average energy. The last peak has 92.367 and 92.792 keV gamma rays of 234Th, representing the activities of 238U and its daughter isotopes, and 93.35 keV Th Ksub(α) X-rays representing the activities of 235U and its daughters. The results of the measurements do not depend on the size and the shape of the measurements. The procedure is developed to take automatically into account the presence of any absorber or cladding between the measured sample and the detector. The attainable precision of the measurements (at 95% confidence level) is 0.2 - 0.3%. If combined with enrichment measurements, and after suitable empirical calibration, the method can be used without standards. Gamma-spectrometric measurements of 238U and 232Th are based on the daughter isotopes' gamma activities. However, this is correct only when there is a corresponding equilibrium between 238U and 232Th and the daughter isotopes' activities. Where such equilibrium is not reached the status of the daughter products' activities regarding equilibrium, has to be taken into account. Two methods of quantitative corrections are proposed: (i) The use of an absolute determination of the 228Ac/224Ra activity ratio through self-calibrated measurements and individual activities and their correlation with the equilibrium activities. (ii) Use of two of the same sample measurements at two different moments during the unrestored equilibrium and the correlation of the measurement results with the 232Th activity. This method can be generally applied. (author)