Uncertainty and detection limits of 241Pu determination by liquid scintillation counting (LSC)

Highlights: • A method to determine ²⁴¹Pu by LSC, considering lixiviation yield, is presented. • Uncertainty and detection limit formulae are developed including lixiviation yield. • Sensitivity analysis of uncertainty, it being 5–30%, is done. • Detection limits are about 14–30 Bq kg^-1, depending on the total yield value. • Quench standard curves made with ³H and ²⁴¹Pu show differences around 3.5%. Determination of ²⁴¹Pu is an essential issue for radiation protection, as it is the precursor of some nuclides with high radiotoxicity. ²⁴¹Pu is a low energy beta emitter, which makes its measurement more challenging than that of Pu alpha emitters. The most widely used method for the measurement of ²⁴¹Pu is liquid scintillation counting (LSC). In this method, the assessment of Pu radiochemical yield is done by measuring the sample by alpha spectrometry before being lixiviated and measured by LSC. This double measurement affects uncertainty analysis, as well as decision threshold and detection limit, considering that both components of the total yield (radiochemical and lixiviation) should be contemplated. In this paper, and for quality assurance (QA) purposes, in-depth uncertainty and detection limit formulae for the proposed method, controlling correlations and considering all the parameters involved including chemical and lixiviation yields, have been developed. A sensitivity analysis of the uncertainty budget together with an assessment of ²⁴²Pu tracer quantity to be used, ensuring a total yield of at least 50% and a relative uncertainty of the leaching yield of at most 5%, have been carried out. In addition, an analysis of the impact of the real lixiviation yield value and its uncertainty on the results has been done. As a general conclusion, and considering the values of the parameters chosen for this work (samples of 1 g measured for 24 h by LSC), the ²⁴¹Pu uncertainties range from 5% to 30% depending on the activity concentration values and the detection limits range from 14 to 30 Bq kg^-1, depending on yield values. The main components of the uncertainty budget are the net ²⁴¹Pu and background counts obtained in the LSC measurement for low contaminated samples while this is the case for the alpha gross count rate in LSC measurement of the alpha calibration source for highly contaminated samples. In addition, an analysis of possible interference by Pu alpha emitters in the ²⁴¹Pu signal and a comparison of quench standard curves of ³H and ²⁴¹Pu are also performed.