Non-intrusive measurement of tritium activity in waste drums by modelling a 3He leak quantified by mass spectrometry

This study deals with a new method that makes it possible to measure very low tritium quantities inside radioactive waste drums. This indirect method is based on measuring the decaying product, 3He, and requires a study of its behaviour inside the drum. Our model considers 3He as totally free and its leak through the polymeric joint of the drum as two distinct phenomena: permeation and laminar flow. The numerical simulations show that a pseudo-stationary state takes place. Thus, the 3He leak corresponds to the tritium activity inside the drum but it appears, however, that the leak peaks when the atmospheric pressure variations induce an overpressure in the drum. Nevertheless, the confinement of a drum in a tight chamber makes it possible to quantify the 3He leak. This is a non-intrusive measurement of its activity, which was experimentally checked by using reduced models, representing the drum and its confinement chamber. The drum's confinement was optimised to obtain a reproducible 3He leak measurement. The gaseous samples taken from the chamber were purified using selective adsorption onto activated charcoals at 77 K to remove the tritium and pre-concentrate the 3He. The samples were measured using a leak detector mass spectrometer. The adaptation of the signal acquisition and the optimisation of the analysis parameters made it possible to reach the stability of the external calibrations using standard gases with a 3He detection limit of 0.05 ppb. Repeated confinement of the reference drums demonstrated the accuracy of this method. The uncertainty of this non-intrusive measurement of the tritium activity in 200-liter drums is 15% and the detection limit is about 1 GBq after a 24 h confinement. These results led to the definition of an automated tool able to systematically measure the tritium activity of all storage waste drums. (authors)