Experimental measurements of the bacterial oxidation of HT in soils: Impact over a zone influenced by an industrial release of tritium in HT form.

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 km2), 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.

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.

Atmospheric tritium concentrations under influence of AREVA NC La Hague reprocessing plant (France) and background levels.

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 85Kr, 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.

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.

In situ measurements of tritium evapotranspiration (³H-ET) flux over grass and soil using the gradient and eddy covariance experimental methods and the FAO-56 model.

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.

Near-field krypton-85 measurements in stable meteorological conditions around the AREVA NC La Hague reprocessing plant: estimation of atmospheric transfer coefficients.

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.

Estimation of marine source-term following Fukushima Dai-ichi accident.

Contamination of the marine environment following the accident in the Fukushima Dai-ichi nuclear power plant represented the most important artificial radioactive release flux into the sea ever known. The radioactive marine pollution came from atmospheric fallout onto the ocean, direct release of contaminated water from the plant and transport of radioactive pollution from leaching through contaminated soil. In the immediate vicinity of the plant (less than 500 m), the seawater concentrations reached 68,000 Bq.L(-1) for (134)Cs and (137)Cs, and exceeded 100,000 Bq.L(-1) for (131)I in early April. Due to the accidental context of the releases, it is difficult to estimate the total amount of radionuclides introduced into seawater from data obtained in the plant. An evaluation is proposed here, based on measurements performed in seawater for monitoring purposes. Quantities of (137)Cs in seawater in a 50-km area around the plant were calculated from interpolation of seawater measurements. The environmental halftime of seawater in this area is deduced from the time-evolution of these quantities. This halftime appeared constant at about 7 days for (137)Cs. These data allowed estimation of the amount of principal marine inputs and their evolution in time: a total of 27 PBq (12 PBq-41 PBq) of (137)Cs was estimated up to July 18. Even though this main release may be followed by residual inputs from the plant, river runoff and leakage from deposited sediments, it represents the principal source-term that must be accounted for future studies of the consequences of the accident on marine systems. The (137)Cs from Fukushima will remain detectable for several years throughout the North Pacific, and (137)Cs/(134)Cs ratio will be a tracer for future studies.