First measurements of chlorine 36 (36Cl) wet deposition fluxes in the vicinity of Orano La Hague nuclear reprocessing plant in France.

Chlorine 36 (36Cl) is a radionuclide of natural and anthropogenic origin, mainly used as a tracer in geochemical studies. Owing to analytical constraints and its low environmental levels, knowledge of 36Cl behavior in the environment is still very limited. In this study, we use environmental measurements to report for the first time the wet deposition fluxes of 36Cl downwind an anthropogenic source, the Orano nuclear reprocessing plant, which chronically emits 36Cl into the environment. Measurements of 36Cl in rainwater samples at our study site were 1-2 orders of magnitude above the environmental background. The isotope ratios 36Cl/Cl of the samples and the 36Cl content in the rainwater averaged 2.3x10-12 at at-1 and 1.7x108 at l-1 respectively. A decrease in these levels was observed 20 km away from the study site, outside the plant's gas plume, indicating that the marking of 36Cl on the study site is related to the plant discharges. Over the sampling period, wet deposition fluxes at the study site averaged 3.4x103 at m-2s-1, with significant values measured when precipitations scavenge the plant's gas plume down onto our study site. Analysis of these fluxes also revealed the presence of a significant rainout phenomenon in the study area. These results provide new data on the wet deposition flux of 36Cl and will thus enable better assessment of impact studies in a context of decommissioning or accidents involving nuclear power plants.

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

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.