Tritium in precipitation on 5 sites in North-West France during the 2017-2019 period.

Between October 2017 and May 2019, measurements of tritium in rainwater were carried out at several sites in north-west France. Tritium is an important tracer for hydroclimatic studies and this work provided up-to-date data that we compared with Global Network for Isotopes in Precipitation (GNIP) measurements. Of the various sites studied, some could potentially be affected by atmospheric gaseous emissions from the nuclear industries in the region (reprocessing plant, nuclear power plant). On our reference site, the activities measured in rainwater are often below the decision threshold (<0.15 Bq.L-1). Two other sites with little impact from nuclear industries have mean activities of less than 0.7 Bq.L-1. At the two Cherbourg sites closer to the nuclear industries, the activities in rainwater are slightly higher on average, though still close to 1 Bq.L-1, but the activities are more variable when the rainfall accompanies an air mass from the Orano La Hague nuclear site. Using existing GNIP data and a simple model to simulate predicted data up to 2019, it is shown that all our measured data are comparable with the predicted activities for GNIP stations with a marine influence, in the case of the reference site and the sites with little impact from nuclear industries, and for GNIP stations with a continental influence, in the case of the other sites. Seasonal variation in activities was detected, with greater activities in the spring-summer period corresponding to the well known 'spring leak' phenomenon. This study also reveals significant differences between the activities measured on the western side of France (influenced by the Atlantic Ocean) and those measured in a continental zone. The mean levels of tritium in rainwater in France, excluding any nuclear influence, can be estimated on average at less than 0.3 Bq.L-1 in the western marine zone, and at around 1 Bq.L-1 in the continental zones.

Tritium forms discrimination in ryegrass under constant tritium exposure: From seed germination to seedling autotrophy.

Uncertainties remain regarding the fate of atmospheric tritium after it has been assimilated in grasslands (ryegrass) in the form of TFWT (Tissue Free Water Tritium) or OBT (Organically Bound Tritium). One such uncertainty relates to the tritium forms discrimination during transfer from TFWT to OBT resulting from photosynthesis (OBTphoto), corresponding to the OBTphoto/TFWT ratio. In this study, the OBT/TFWT ratio is determined by experiments in the laboratory using a ryegrass model and hydroponic cultures, with constant activity of tritium in the form of tritiated water (denoted as HTO) in the "water" compartment (liquid HTO) and "air" compartment (HTO vapour in the air). The OBTphoto/TFWT ratio and the exchangeable OBT fraction are measured for three parts of the plant: the leaf, seed and root. Plant growth is modelled using dehydrated biomass measurements taken over time in the laboratory and integrating physiological functions of the plant during the first ten days after germination. The results suggest that there is no measurable discrimination of tritium in the plant organic matter produced by photosynthesis.

The VATO project: Development and validation of a dynamic transfer model of tritium in grassland ecosystem.

In this paper, a dynamic compartment model with a high temporal resolution has been investigated to describe tritium transfer in grassland ecosystems exposed to atmospheric 3H releases from nuclear facilities under normal operating or accidental conditions. TOCATTA-χ model belongs to the larger framework of the SYMBIOSE modelling and simulation platform that aims to assess the fate and transport of a wide range of radionuclides in various environmental systems. In this context, the conceptual and mathematical models of TOCATTA-χ have been designed to be relatively simple, minimizing the number of compartments and input parameters required. In the same time, the model achieves a good compromise between easy-to-use (as it is to be used in an operational mode), explicative power and predictive accuracy in various experimental conditions. In the framework of the VATO project, the model has been tested against two-year-long in situ measurements of 3H activity concentration monitored by IRSN in air, groundwater and grass, together with meteorological parameters, on a grass field plot located 2 km downwind of the AREVA NC La Hague nuclear reprocessing plant, as was done in the past for the evaluation of transfer of 14C in grass. By considering fast exchanges at the vegetation-air canopy interface, the model correctly reproduces the observed variability in TFWT activity concentration in grass, which evolves in accordance with spikes in atmospheric HTO activity concentration over the previous 24 h. The average OBT activity concentration in grass is also correctly reproduced. However, the model has to be improved in order to reproduce punctual high concentration of OBT activity, as observed in December 2013. The introduction of another compartment with a fast kinetic (like TFWT) - although outside the model scope - improves the predictions by increasing the correlation coefficient from 0.29 up to 0.56 when it includes this particular point. Further experimental investigation will be undertaken by IRSN and EDF next year to better evaluate (and properly model) other aspects of tritium transfer where knowledge gaps have been identified in both experimental and modelling areas.

The VATO project: An original methodology to study the transfer of tritium as HT and HTO in grassland ecosystem.

Tritium (3H) is mainly released into the environment by nuclear power plants, military nuclear facilities and nuclear reprocessing plants. The construction of new nuclear facilities in the world as well as the evolution of nuclear fuel management might lead to an increase of 3H discharges from the nuclear industry. The VATO project was set up by IRSN (Institut de Radioprotection et de Sûreté Nucléaire) and EDF (Electricité de France) to reduce the uncertainties in the knowledge about transfers of 3H from an atmospheric source (currently releasing HT and HTO) to a grassland ecosystem. A fully instrumented technical platform with specifically designed materials was set up downwind of the AREVA NC La Hague reprocessing plant (Northwest of the France). This study, started in 2013, was conducted in four main steps to provide an hourly data set of 3H concentrations in the environment, adequate to develop and/or validate transfer models. It consisted first in characterizing the physico-chemical forms of 3H present in the air around the plant. Then, 3H transfer kinetics to grass were quantified regarding contributions from various compartments of the environment. For this purpose, an original experimental procedure was provided to take account for biases due to rehydration of freeze-dried samples for the determination of OBT activity concentrations in biological samples. In a third step, the 3H concentrations measured in the air and in rainwater were reconstructed at hourly intervals. Finally, a data processing technique was used to determine the biological half-lives of OBT in grass.

A study of the atmospheric dispersion of a high release of krypton-85 above a complex coastal terrain, comparison with the predictions of Gaussian models (Briggs, Doury, ADMS4).

Atmospheric releases of krypton-85, from the nuclear fuel reprocessing plant at the AREVA NC facility at La Hague (France), were used to test Gaussian models of dispersion. In 2001-2002, the French Institute for Radiological Protection and Nuclear Safety (IRSN) studied the atmospheric dispersion of 15 releases, using krypton-85 as a tracer for plumes emitted from two 100-m-high stacks. Krypton-85 is a chemically inert radionuclide. Krypton-85 air concentration measurements were performed on the ground in the downwind direction, at distances between 0.36 and 3.3 km from the release, by neutral or slightly unstable atmospheric conditions. The standard deviation for the horizontal dispersion of the plume and the Atmospheric Transfer Coefficient (ATC) were determined from these measurements. The experimental results were compared with calculations using first generation (Doury, Briggs) and second generation (ADMS 4.0) Gaussian models. The ADMS 4.0 model was used in two configurations; one takes account of the effect of the built-up area, and the other the effect of the roughness of the surface on the plume dispersion. Only the Briggs model correctly reproduced the measured values for the width of the plume, whereas the ADMS 4.0 model overestimated it and the Doury model underestimated it. The agreement of the models with measured values of the ATC varied according to distance from the release point. For distances less than 2 km from the release point, the ADMS 4.0 model achieved the best agreement between model and measurement; beyond this distance, the best agreement was achieved by the Briggs and Doury models.

Solid partitioning and solid-liquid distribution of 210Po and 210Pb in marine anoxic sediments: roads of Cherbourg at the northwestern France.

A sequential extraction protocol has been used to determine the solid-phase partition of (210)Po and (210)Pb in anoxic marine sediment from the roads of Cherbourg (France) in the central English Channel. Measurements were also obtained in pore waters, in which (210)Po activities range between 1 and 20 mBq L(-1) and (210)Pb activities between 2.4 and 3.8 mBq L(-1), with highest activities in the topmost layer. These activities are higher than in seawater, suggesting that sediment act as a source of both (210)Po and (210)Pb for overlying water. The (210)Po profile in the pore waters is apparently correlated with those obtained for Fe, Mn and SO(4)(2)(-), suggesting an influence of early diagenetic processes on the (210)Po solid-liquid distribution. In the sediment, (210)Po is predominantly bound to organic matter or chromium reducible sulphides, and residuals (clay minerals and refractory oxides). Our results indicate that (210)Po is not significantly bound to AVS, i.e. acid volatile sulphides: bioturbation could play a role by the early redistribution of (210)Po bound to acid volatile sulphides in the sediment. (210)Po, (210)Pb and Pb exhibit differences in terms of distribution, probably due to a different mode of penetration in the sediment. This work provides information on solid and liquid distribution of (210)Po and (210)Pb in marine sediment. These data are very scarce in the literature.

In situ metrology of 85Kr plumes released by the COGEMA La Hague nuclear reprocessing plant.

The IRSN (Institut de Radioprotection et de Sûreté Nucléaire, France) has started an in situ study of the behaviour of atmospheric releases close-by the COGEMA La Hague nuclear reprocessing plant. The study is designed to improve information on the dispersion of radioactive pollutants very close to the emission point--a 100 m height chimney. In this situation, close to the emission and height of the emission, Gaussian models generally used to predict the behaviour of atmospheric releases are not well adapted. The study is based on the characterisation of the 85Kr emitted during normal operations of the reprocessing process. Temporal and spatial variations of the plume shape were investigated with intensive in situ measurements. Live in situ techniques to measure the electrons and the photons emitted by the 85Kr have been implemented and will be described. Preliminary results showing the interest of the techniques were presented. Variations of the dose rates created by the photon flux of a plume were directly measured and correlated to other quantities.