First quantitative constraints on chlorine 36 dry deposition velocities on grassland: Comparing measurements and modelling results

Abstract

Once released into the atmosphere, radionuclide dry deposition represents a major transfer process. It can be accurately characterized by its deposition velocity. However, this parameter is poorly constrained for most radionuclides, including chlorine 36. Chlorine 36 is a radionuclide of cosmogenic and anthropogenic origin. It may be discharged into the environment as gases and/or particles during the decommissioning of nuclear plants and the recycling of nuclear fuels. In this study, chlorine 36 deposition velocities are, for the first time, experimentally determined on grass downwind from the Orano La-Hague plant. The atmospheric chlorine 36 measurements were on average 50 nBq.m−3 for the gaseous fraction and 19 nBq.m3 for the particulate fraction. To measure the chlorine 36 transferred from the atmosphere to the grass, a method was devised for extracting the chlorides contained in solid matrices. With this method, chlorides were extracted with a mean efficiency of 83%. Chlorine 36 concentrations in the grass were on average 4 μBq.g−1, suggesting fast uptake of atmospheric chlorine 36. The yielded 36Cl dry deposition velocities varied with the season and were between 1 × 10−3 and 6 × 10−3 m s−1. The chlorine 36 depositions were modelled by adapting the existing deposition models and based on meteorological and micro-meteorological data. The dry deposition velocities calculated by the model showed less than one order of magnitude of difference with those determined experimentally. The deposition fluxes calculated by the model showed that the atmospheric depositions were predominantly gaseous chlorine 36 (>97%). However, on remote sites, the particulate fraction could be larger and have a greater influence on dry deposition. As chlorine 36 is a highly soluble and bioavailable element, these results will enable a better study of its behaviour in the environment and a more accurate evaluation of its dosimetric impact.