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Tritium is released to the environment by nuclear industries in various forms, mainly HTO. In impact studies leading to estimated doses for the population, atmospheric discharges are mainly taken into consideration because they generally lead to values higher than those related to liquid discharges. However, the tritium released in liquid environments can be transferred to the atmosphere by evaporation and then be transported to terrestrial ecosystems by wind. This study was carried out in France near a fuel reprocessing plant (RP) which discharges tritium into the western English Channel. We highlighted the influence of a mass of water enriched with tritium on the HTO levels in atmospheric water vapour downwind through 18 field campaigns. A hydrodynamic model able to simulate tritium activity in the water was coupled with an evaporation an atmospheric transport model. It allows to reconstitute variations in atmospheric tritium on the coast, depending on liquid discharges of tritium from the reprocessing plant. On this basis, when seawater containing 20-100 Bq.L -1 of tritium flows between 0 and 10 km off the coast, variations in atmospheric activity onshore can increase of 2-15 Bq.L -1 . Mean tritium quantities released by the sea into the atmosphere in the Western English Channel reached 130 TBq.y -1 over the 2017-2020 period. Emissions were estimated at 0.9-11.3 GBq km -2 .y -1 and depends principally on the distance from the liquid discharge point. If we compare the "marine" source term, in HTO form, with the direct source term for gaseous discharges, the marine source term is one order of magnitude greater for the marine region affected by liquid discharges. Finally, we estimate that approximately 1.1% of tritium stock discharged at sea (regulated and controlled) return to the atmosphere each year at the scale of the Western English Channel., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2022 Elsevier Ltd. All rights reserved.)

Tritium is a radionuclide released to the atmosphere by nuclear industries in various forms, mainly HTO and to a lesser extent HT. However, some nuclear sites may emit predominantly HT in the atmosphere. The HT is oxidized to HTO essentially in the top cm of soils, and that the formed HTO is then possibly released into the atmosphere. HTO is an assimilable form by plants. Therefore, it is important to understand the environmental behaviour of HT. In this work, we adapt the bacterial oxidation model of HT in soils of Ota et al. (2007) by laboratory experiments on soils typical of western France, and we have in particular adapted the frequency factor A and the Michaelis-Menten enzymatic reaction parameter (Km) on the basis of an Arrhenius equation in function of the porosity of the soil. We then applied this model to the environment near the reprocessing plant of Orano la Hague (France), which emits a significant amount of HT. Based on the adapted model, and knowing the atmospheric variations of HTO and HT over the period 2013-2016, we estimated that the mean HTO activity in soil due to atmospheric HT reached 0.6 Bq.L -1 (with a peak value of 5 Bq.L -1 ) while the mean value with all sources taken into account is 6.2 Bq.L -1 . Then, in an environment such as that surrounding the Orano La Hague plant, where near-field atmospheric HT activity is very high, the bacterial oxydation contribution to produce HTO in the soil can be considered as approximately 10%. The flux to the atmosphere from these source representing approximately. 1.5 Bq.m -2 .d -1 . If we consider an area of 2 km around the plant (i.e. 13 km 2 ), we estimate 218 Bq.s -1 of HTO was released by the soil, representing less than 0.1% of the direct atmospheric release of HTO around the site. From this work, it appears clear that this secondary source term from the soil is insignificant at this specific site., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

Assessing the impact of radioactive iodine on humans subsequent to a nuclear accident requires a better understanding of its behaviour in the environment. An original approach aimed at developing a model constrained by data collected during experimental campaigns has been developed. These experimental campaigns, named MIOSEC 2 and MIOSEC 3 respectively, were conducted in the middle of grassland. They are based on emissions of gaseous elemental iodine (I 2 ) into the atmosphere above the grassland to determine the dry deposition velocities of iodine on the grass and to model these velocities as a function of the environmental conditions, particularly wind friction velocity, sensible heat flux, and stomatal resistance. The measured dry deposition velocities were between 0.02 and 0.49 cm s -1 during MIOSEC 2, varying by more than one order of magnitude, and between 0.48 and 1.25 cm s -1 during MIOSEC 3. The dry deposition model for iodine developed as a result of these experiments relies on the micrometeorological characteristics of the atmospheric surface layer, the pertinent physical and chemical properties of the iodine and the surface properties of the grass; all these parameters were measured at the time of the experiments. Given the experimental conditions, the modelled dry deposition velocities varied between 0.11 and 0.51 cm s -1 during MIOSEC 2 and between 0.31 and 1.6 cm s -1 during MIOSEC 3. The dry deposition model for iodine indicates that the variations in deposition velocity are induced by the mechanical turbulence, since there is significant correlation between the dry deposition velocities of iodine and the wind friction velocities on grass. The model also shows that the higher deposition velocity values during MIOSEC 3 are due to the fact that the stomata were more open during the experiments. There is also significant correlation between the experimental results and modelled values both for MIOSEC 2 (R 2  = 0.61) and for MIOSEC 3 (R 2  = 0.71)., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2020 Elsevier Ltd. All rights reserved.)

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., (Copyright © 2019 Elsevier Ltd. All rights reserved.)

In-air tritium measurements were conducted around the AREVA NC La Hague reprocessing plant, as well as on other sites that are not impacted by the nuclear industry in northwest of France. The results indicate that the dominant tritium form around the AREVA site is HT (86%). HT and HTO levels are lower than 5 and 1 Bq. m -3 for hourly samples taken in the plume. No tritiated organic molecules (TOM) were detected. 26 measurement campaigns were performed and links were established between near-field 85 Kr, HT and HTO activities. Environmental measurements are in line with those taken at the discharge stack, and tend to demonstrate that there are no rapid changes in the tritium forms released. Out of the influence of any nuclear activities, the levels measured were below 13 mBq.m -3 for HT and 5 mBq.m -3 for HTO (<0.5 Bq. L -1 ). HTO level in air seems to be influenced by HTO activities in surrounding seawater., (Copyright © 2017 Elsevier Ltd. All rights reserved.)

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 3 H 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 3 H 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 14 C 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., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

Tritium ( 3 H) 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 3 H 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 3 H 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 3 H concentrations in the environment, adequate to develop and/or validate transfer models. It consisted first in characterizing the physico-chemical forms of 3 H present in the air around the plant. Then, 3 H 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 3 H 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., (Copyright © 2016 Elsevier Ltd. All rights reserved.)

The behaviour of tritium in the environment is linked to the water cycle. We compare three methods of calculating the tritium evapotranspiration flux from grassland cover. The gradient and eddy covariance methods, together with a method based on the theoretical Penmann-Monteith model were tested in a study carried out in 2013 in an environment characterised by high levels of tritium activity. The results show that each of the three methods gave similar results. The various constraints applying to each method are discussed. The results show a tritium evapotranspiration flux of around 15 mBq m(-2) s(-1) in this environment. These results will be used to improve the entry parameters for the general models of tritium transfers in the environment., (Copyright © 2015 Elsevier Ltd. All rights reserved.)

The aim of this work was to study the near-field dispersion of (85)Kr around the nuclear fuel reprocessing plant at La Hague (AREVA NC La Hague - France) under stable meteorological conditions. Twenty-two (85)Kr night-time experimental campaigns were carried out at distances of up to 4 km from the release source. Although the operational Gaussian models predict for these meteorological conditions a distance to plume touchdown of several kilometers, we almost systematically observed a marked ground signal at distances of 0.5-4 km. The calculated atmospheric transfer coefficients (ATC) show values (1) higher than those observed under neutral conditions, (2) much higher than those proposed by the operational models, and (3) higher than those used in the impact assessments., (Copyright © 2014 Elsevier Ltd. All rights reserved.)

The Institut de Radioprotection et de Sureté Nucléaire (IRSN) performed a series of (85)Kr air sampling campaigns at mesoscale distances (18-50 km) from the AREVA NC La Hague nuclear reprocessing plant (North West France) between 2007 and 2009. The samples were collected in order to test and optimise a technique to measure low krypton-85 ((85)Kr) air concentrations and to investigate the performance of three atmospheric dispersion models (RIMPUFF, HYSPLIT, and ADMS), This paper presents the (85)Kr air concentrations measured at three sampling locations which varied from 2 to 8000 Bq m(-3), along with the (85)Kr air concentrations output by the dispersion models. The dispersion models made reasonable estimates of the mean concentrations of (85)Kr field measurements during steady wind conditions. In contrast, the models failed to accurately predict peaks in (85)Kr air concentration during periods of rapid and large changes in wind speed and/or wind direction. At distances where we made the comparisons (18-50 km), in all cases, the models underestimated the air concentration activities., (Copyright © 2013 Elsevier Ltd. All rights reserved.)

Radioactive emissions into the atmosphere from the damaged reactors of the Fukushima Dai-ichi nuclear power plant (NPP) started on March 12th, 2011. Among the various radionuclides released, iodine-131 ((131)I) and cesium isotopes ((137)Cs and (134)Cs) were transported across the Pacific toward the North American continent and reached Europe despite dispersion and washout along the route of the contaminated air masses. In Europe, the first signs of the releases were detected 7 days later while the first peak of activity level was observed between March 28th and March 30th. Time variations over a 20-day period and spatial variations across more than 150 sampling locations in Europe made it possible to characterize the contaminated air masses. After the Chernobyl accident, only a few measurements of the gaseous (131)I fraction were conducted compared to the number of measurements for the particulate fraction. Several studies had already pointed out the importance of the gaseous (131)I and the large underestimation of the total (131)I airborne activity level, and subsequent calculations of inhalation dose, if neglected. The measurements made across Europe following the releases from the Fukushima NPP reactors have provided a significant amount of new data on the ratio of the gaseous (131)I fraction to total (131)I, both on a spatial scale and its temporal variation. It can be pointed out that during the Fukushima event, the (134)Cs to (137)Cs ratio proved to be different from that observed after the Chernobyl accident. The data set provided in this paper is the most comprehensive survey of the main relevant airborne radionuclides from the Fukushima reactors, measured across Europe. A rough estimate of the total (131)I inventory that has passed over Europe during this period was <1% of the released amount. According to the measurements, airborne activity levels remain of no concern for public health in Europe.

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.

The results of a 1-year long survey of trace metals concentrations (Al, Cd, Cr, Co, Cu, Fe, Mn, Hg, Ni, Pb, Zn) measured in beach sand, limpets and, occasionally, in fish and shellfish from the North Cotentin area (France), where nuclear industries are implanted, are presented. The objective of these study was to provide useful data for the validation of models predicting the impact of these industries on the marine environment. Even if differences were noted between sites for various metals, the levels are consistent with existing data published for similar site and do not appear to give evidence of contamination by industrial sites.

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.

This study presents an original work on measurements of stable and radioactive iodinated species in the Seine estuary (France), with estimates fluxes of volatile gaseous species from water to the atmosphere. Various iodinated compounds were identified in water and air in particular 131I in water, what is unusual. Concentrations and behaviour of iodinated elements in the Seine estuary seem similar to what has been observed in other European estuaries. MeI (Methyl Iodide) and Total Volatile Iodine (TVI) fluxes from water to air vary between 392 and 13949 pmol m(-2) d(-1) and between 1279 and 16484 pmol m(-2) d(-1), respectively. Water to air flux of TVI for the Seine river was estimated in the range 4-46 kg y(-1). Measurements of (131)I in water varying between 0.4 and 11.9 Bq m(-3). Fluxes of (131)I from water to atmosphere are in the range 2.4 x 10(5)-1.3 x 10(7)Bq y(-1), close to an annual discharge of (131)I by a nuclear reactor.

Measurements of (210)Po were carried out in various marine matrices (mussels, oysters, seaweed, fish, and abalones) and in seawater at several points along the French coast, over a period of 2 years (2003-2005). These measurements contribute to a better knowledge of this element, since few recent data exist for the French coast. Marked seasonal variations have been revealed in some species and there are differences according to the way of life of these species. Activities in mussels (Mytilus edulis) and oysters (Crassostrea gigas) are similar and varying between 90 and 600 Bq kg(-1) (d.w.). Activities in macroalgae (Fucus serratus) are lowest, between 4 and 16 Bq kg(-1) (d.w.). In oyster, abalone (Haliotis tuberculata) and fish (Solea solea, Sparus sp.), the strongest activities are measured in the digestive glands, the gills and the gonads. (210)Po/(210)Pb ratios in all cases have values of more than one for all species. From a significant number of measurements, CFs were calculated for seaweed (between 4.6 x 10(3) and 5.0 x 10(3)) and for molluscs, with highest CFs (>10(5)) found for the digestive gland and gills of the oysters, the digestive gland of the abalones and the liver of fish. Finally, the activities measured have made it possible to estimate the internal dose from chronic exposure due to (210)Po received by the marine organisms (0.05 microGh(-1) for macroalgae, between 0.70 and 1.5 microGh(-1) for mussels and oyster), and the contribution of seafood to the dose received by humans (46-129 microSvy(-1)).