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.

Iodine uptake in brown seaweed exposed to radioactive liquid discharges from the reprocessing plant of ORANO La Hague.

Iodine-129 is present in controlled liquid radioactive waste routinely released in seawater by the ORANO nuclear fuel reprocessing plant in La Hague (Normandy, France). Brown algae are known for their exceptional ability to concentrate iodine from seawater. They also potentially emit volatile iodine compounds in response to various stresses, such as during emersion at low tide. For these reasons, brown seaweed is routinely collected for radioactivity monitoring in the marine environment (Fucus serratus and Laminaria digitata). Despite the high concentration ratio, the exact mechanism of iodine uptake is still unclear. Chemical imaging by laser desorption/ionization mass spectrometry provided evidence that iodine is stored by kelps as I-. In this study we investigate in vivo iodine uptake in kelps (L. digitata) with an emphasis on seawater iodine chemical speciation. Our results showed that kelp plantlets were able to take up iodine in the forms of both IO3- and I-. We also observed transient net efflux of I- back to seawater but no IO3- efflux. Since the seaweed stores I- but takes up both IO3- and I-, IO3- was likely to be converted into I- at some point in the plantlet. One major outcome of our experiments was the direct observation of the kelp-based biogenic conversion of seawater IO3- into I-. On the basis of both IO3- and I- uptakes by the seaweed, we propose new steps in the possible iodine concentration mechanism used by brown algae.

Measurement and modelling of gaseous elemental iodine (I2) dry deposition velocity on grass in the environment.

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 (I2) 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 (R2 = 0.61) and for MIOSEC 3 (R2 = 0.71).

Comparison of RIMPUFF, HYSPLIT, ADMS atmospheric dispersion model outputs, using emergency response procedures, with (85)Kr measurements made in the vicinity of nuclear reprocessing plant.

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.

The TOCATTA-χ model for assessing 14C transfers to grass: an evaluation for atmospheric operational releases from nuclear facilities.

Radioactive (14)C is formed as a by-product of nuclear power generation and from the operation of nuclear fuel reprocessing plants like AREVA-NC La Hague (North France), which releases about 15 TBq per year of (14)C into the atmosphere. This article evaluates a recently improved radioecology model (TOCATTA-χ) to assess (14)C transfers to grassland ecosystems under normal operating conditions. The new version of the TOCATTA model (TOCATTA-χ) includes developments that were derived from PaSiM, a pasture model for simulating grassland carbon and radiocarbon cycling. The TOCATTA-χ model has been tested against observations of (14)C activity concentrations in grass samples collected monthly from six plots which are located around the periphery of the reprocessing plant. Simulated (14)C activities are consistent with observations on both intensively managed and poorly managed grasslands, but an adaptation of the mean turn-over time for (14)C within the plant is necessary in the model to account for different management practices. When atmospheric (14)C activity concentrations are directly inferred from observations, TOCATTA-χ performs better than TOCATTA (the root mean square error is decreased by 45%), but when atmospheric (14)C activity concentrations are not known and must be calculated, the uncertainty associated with the TOCATTA-χ model outcomes is estimated to be larger than the standard deviation of the observations.

Water to atmosphere fluxes of 131I in relation with alkyl-iodide compounds from the Seine Estuary (France).

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.