Tritium and radiocarbon levels in the Rhône river delta and along the French Mediterranean coastline.

The Rhône is characterised by a heavy concentration of nuclear-based industries including nuclear power stations and nuclear sites housing civilian and military facilities. Here, we report the results of a four-year survey (2010-2013) of tritium and radiocarbon levels in a variety of matrices within the Rhône delta and along the French Mediterranean coastline. The aim of the study is to create a spatial reference framework of environmental levels of these two radionuclides, which are the most prevalent in radioactive effluents from nuclear power stations. Although both tritium and radiocarbon levels in the samples analysed are very low and can only be detected using ultra-sensitive analytical techniques, they clearly show the influence of the tritium and radiocarbon discharges carried by the Rhône plume along the Mediterranean coast. The tritium content of suspended matter and sediments of the Rhône is a special case, which shows elevated tritium values not seen in other French rivers with similar nuclear facilities. The north-south spatial distribution of this tritium anomaly shows that these trace values are at their highest in the upper Rhône, close to the Swiss border and upstream of Creys Malville, the northernmost nuclear power station on the Rhône. This points to a legacy of past tritium releases by the watchmaking industry. A dedicated study would be needed to clearly identify the source and the exact nature of this contamination.

Towards speciation of organically bound tritium and deuterium: Quantification of non-exchangeable forms in carbohydrate molecules.

An original methodology to quantitatively explore exchangeability of hydrogen isotopes in carbohydrate molecules is proposed. To access the speciation of organically bound hydrogen isotopes, isotopic exchanges were carried out under a soft path regime in the vapor phase at 20 °C with set (D,T/H) vapor pressure ratios. When steady states were reached, the fraction of exchangeable hydrogen of microcrystalline cellulose, alpha-cellulose and wheat grains were obtained and ranged from 13 to 31% (versus a theoretical value of 30%). In cellulose, and more specifically in microcrystalline cellulose, the molecular hydrogen bonds as well as the different conformations of the network seemed to decrease the hydroxyl groups of glucose units available for isotopic exchange. On the contrary, the assumed enzymatic hydrolysis of the constitutive molecules of wheat starch into low-molecular weight carbohydrate molecules enhanced the exchangeable pool. An average value of the activity between non-exchangeable organically bound tritium (NE-OBT) and non-exchangeable organically bound hydrogen was calculated for wheat grains, (TH)NE  = 0.55 ±â€¯0.03 Bq.g-1 of hydrogen atoms.

Carbon-14 transfer into potato plants following a short exposure to an atmospheric 14CO2 emission: observations and model predictions.

To improve the understanding of the environmental (14)C behaviour, the International Atomic Energy Agency (IAEA) coordinated a Tritium and C-14 Working Group (T&C WG) in its EMRAS (Environmental Modelling for Radiation Safety) programme. One of the scenarios developed in the frame of T&C WG involved the prediction of time dependent (14)C concentrations in potato plants. The experimental data used in the scenario were obtained from a study in which potatoes (Solanum tuberosum cv. Romano) were exposed to atmospheric (14)CO(2) in a wind tunnel. The observations were used to test models that predict temporal changes in (14)C concentrations in leaves at each sampling time for each experiment and (14)C concentrations in tubers at the final harvest of each experiment. The experimental data on (14)C dynamics in leaves are poorly reproduced by most of the models, but the predicted concentrations in tubers are in good agreement with the observations.

Modelling tritium flux from water to atmosphere: application to the Loire River.

Tritium (³H or T) is one of the major radionuclides released by nuclear power plants (NPP) into rivers. However, tritiated water (HTO) flux from water to air is seldom considered when assessing health effects of such releases. The aim of this paper is to present the result of a research program, called LORA, conducted on the Loire River (France). To improve our understanding of HTO flux from surface water to air, three field campaigns were organised during the NPP's radioactive releases to measure simultaneously the activity concentrations in air on the riverbank, using an innovative system, and in river water. The measurements showed that during radioactive releases, water vapour was enriched in ³H. These results were used to calibrate exchange velocities. The average of these estimated exchange velocities was more than one order of magnitude higher than those calculated in the literature from indoor experiments. The variability of these values was also larger, showing that outdoor studies cover a wide range of conditions influencing HTO flux. No correlation was observed between exchanges velocities and meteorological conditions. However, there was a significant difference between day and night with a higher value observed during the day. Two approaches used to calculate HTO evaporation from water (i.e. the approach based on water evaporation and the approach considering that HTO follows its own concentration gradient) were included in a hydrodynamic model, which was used to evaluate HTO air activity along the Loire River. In conclusion, only the approach considering that HTO follows its own gradient led to a good agreement between measurements and predictions. A one-year simulation was done to estimate the contribution of this process to the dose. Its contribution can be considered as negligible in this case compared to the other pathways such as ingestion of water or foodstuffs.

Measured and modelled tritium concentrations in freshwater Barnes mussels (Elliptio complanata) exposed to an abrupt increase in ambient tritium levels.

To improve understanding of environmental tritium behaviour, the International Atomic Energy Agency (IAEA) included a Tritium and C-14 Working Group (WG) in its EMRAS (Environmental Modelling for Radiation Safety) program. One scenario considered by the WG involved the prediction of time-dependent tritium concentrations in freshwater mussels that were subjected to an abrupt increase in ambient tritium levels. The experimental data used in the scenario were obtained from a study in which freshwater Barnes mussels (Elliptio complanata) were transplanted from an area with background tritium concentrations to a small Canadian Shield lake that contains elevated tritium. The mussels were then sampled over 88 days, and concentrations of free-water tritium (HTO) and organically-bound tritium (OBT) were measured in the soft tissues to follow the build-up of tritium in the mussels over time. The HTO concentration in the mussels reached steady state with the concentration in lake water within one or two hours. Most models predicted a longer time (up to a few days) to equilibrium. All models under-predicted the OBT concentration in the mussels one hour after transplantation, but over-predicted the rate of OBT formation over the next 24h. Subsequent dynamics were not well modelled, although all participants predicted OBT concentrations that were within a factor of three of the observation at the end of the study period. The concentration at the final time point was over-predicted by all but one of the models. The relatively low observed concentration at this time was likely due to the loss of OBT by mussels during reproduction.

Carbon-14 transfer into rice plants from a continuous atmospheric source: observations and model predictions.

Carbon-14 (14C) is one of the most important radionuclides from the perspective of dose estimation due to the nuclear fuel cycle. Ten years of monitoring data on 14C in airborne emissions, in atmospheric CO2 and in rice grain collected around the Tokai reprocessing plant (TRP) showed an insignificant radiological effect of the TRP-derived 14C on the public, but suggested a minor contribution of the TRP-derived 14C to atmospheric 14C concentrations, and an influence on 14C concentrations in rice grain at harvest. This paper also summarizes a modelling exercise (the so-called rice scenario of the IAEA's EMRAS program) in which 14C concentrations in air and rice predicted with various models using information on 14C discharge rates, meteorological conditions and so on were compared with observed concentrations. The modelling results showed that simple Gaussian plume models with different assumptions predict monthly averaged 14C concentrations in air well, even for near-field receptors, and also that specific activity and dynamic models were equally good for the prediction of inter-annual changes in 14C concentrations in rice grain. The scenario, however, offered little opportunity for comparing the predictive capabilities of these two types of models because the scenario involved a near-chronic release to the atmosphere. A scenario based on an episodic release and short-term, time-dependent observations is needed to establish the overall confidence in the predictions of environmental 14C models.

A dynamic model for assessing radiological consequences of tritium routinely released in rivers. Application to the Loire River.

A dynamic model for assessing the transfer of tritium in a food chain was applied to the Loire River, where 14 nuclear power plants situated on five different sites operate. The model considers several potential exposure pathways in the aquatic and terrestrial ecosystems: transfer of tritium through the aquatic food chain (especially fish); use of river water for agricultural purposes (irrigation) and transfer of radionuclides through the terrestrial food chain (vegetables, meat, milk); subsequent internal exposure of humans due to ingestion of contaminated foodstuffs. For biological environmental compartments, the transfer of tritium to organic matter (i.e. OBT) was simulated. For each of the parameters introduced in this model, a probability density function, allowing further uncertainty and sensitivity analyses, was proposed. Uncertainty/sensitivity analyses were performed to determine a confidence interval for the mean annual dose to critical groups and to identify the parameters responsible for the uncertainty and subsequent research priorities.

Conceptual approaches for the development of dynamic specific activity models of 14C transfer from surface water to humans.

Carbon-14 is a particularly interesting radionuclide from the perspective of dose estimation. Many nuclear facilities, including power reactors, release 14C into the environment, and much of this is as 14CO2. This mixes readily with stable CO2, and hence enters the food chain as fundamental biomolecules. This isotopic mixing is often used as the basis for dose assessment models. The present model was developed for the situation of 14C releases to surface waters, where there are distinct changes in the water 14C activity concentrations throughout the year. Complete isotopic mixing (equilibrium) cannot be assumed. The model computes the specific activity (activity of 14C per mass of total C) in water, phytoplankton, fish, crops, meat, milk and air, following a typical irrigation-based food-chain scenario. For most of the biotic compartments, the specific activity is a function of the specific activity in the previous time step, the specific activity of the substrate media, and the C turnover rate in the tissue. The turnover rate is taken to include biochemical turnover, growth dilution and mortality, recognizing that it is turnover of C in the population, not a tissue or an individual, that is relevant. Attention is paid to the incorporation of 14C into the surface water biota and the loss of any remaining 14CO2 from the surface water-air interface under its own activity concentration gradient. For certain pathways, variants in the conceptual model are presented, in order to fully discuss the possibilities. As an example, a new model of the soil-to-plant specific activity relationship is proposed, where the degassing of both 14C and stable C from the soil is considered. Selection of parameter values to represent the turnover rates as modeled is important, and is dealt with in a companion paper.

Parameterization of a dynamic specific activity model of 14C transfer from surface water-to-humans.

Carbon-14 is a particularly interesting radionuclide from the perspective of dose estimation because it mixes readily with stable CO2, and hence enters the food-chain as fundamental biomolecules. A model was developed for the situation of 14C releases to surface waters, where there are distinct changes in the water 14C activity concentrations throughout the year. The model computes the specific activity in water, phytoplankton, fish, crops, meat, milk and air, following a typical irrigation-based food-chain scenario. This paper describes the derivation of the required 14C-specific parameter values. Many of the key parameters are not commonly measured, at least not in the context of dose assessment. Thus, inference from other sources of data was required, and this is the scientific contribution described in this paper. The best estimates and appropriate measures of statistical dispersion are provided. This required consideration of both the temporal and spatial averaging domains to ensure they were correct for parameters as defined in the model. The model coupled with these parameter values represents several new developments for modelling 14C transfers.

A dynamic model for assessing radiological consequences of routine releases in the Loire river: parameterisation and uncertainty/sensitivity analysis.

A dynamic model for assessing the transfer of several radionuclides ((58)Co, (60)Co, (110 m)Ag, (134)Cs, (137)Cs, (54)Mn and (131)I) in a food-chain was applied on the Loire river, where 14 nuclear power plants situated on five different sites operate. The model considers the following potential exposure pathways: (i) transfer of radionuclides through the aquatic food chain and the subsequent internal exposure of humans due to ingestion of contaminated water and/or fish; (ii) use of river water for agricultural purposes (irrigation), transfer of radionuclides through the terrestrial food chain and the subsequent internal exposure of humans due to ingestion of contaminated foodstuffs; (iii) internal exposure due to inhalation of dust originating from resuspension of contaminated soil particles; (iv) external exposure from radionuclides present in the river or deposited on the river sediments or the soil. For each of the parameters introduced in this model, a probability density function, allowing further uncertainty and sensitivity analysis, was proposed. Uncertainty/sensitivity analysis were performed to: (i) compare calculations to empirical data; (ii) determine a confidence interval for the mean annual dose to critical groups; and (iii) identify the parameters responsible for the uncertainty and subsequent research priorities.

Comparative recoveries of Naegleria fowleri amoebae from seeded river water by filtration and centrifugation.

Detection of pathogenic Naegleria fowleri in environmental water samples, which is necessary for the prevention of primary amoebic meningoencephalitis, generally requires concentrating the samples. Two concentration techniques, filtration and centrifugation, were used to study the recovery of N. fowleri, in vegetative or cystic form, that had been mixed with the two other thermotolerant Naegleria species, N. lovaniensis and N. australiensis. Counting of amoebae was performed by the most probable number method on 10 water replicates of 100 ml and 10 ml each. With both concentration methods, recovery was better for cysts than for trophozoites (53% +/- 21% versus 5% +/- 5% by filtration and 57% +/- 25% versus 22% +/- 5% by centrifugation). The recovery of Naegleria trophozoites by filtration was very low, and centrifugation was significantly better than filtration in recovery of Naegleria trophozoites (22% +/- 5% versus 5% +/- 5%; P < 0.001). For cysts, however, filtration appeared as efficient as centrifugation, with equivalent values for recovery (53% +/- 21% versus 57% +/- 25%; P > 0.7). Although the recovery of cysts of N. fowleri obtained by filtration (51% +/- 24%) appeared higher than that by centrifugation (36% +/- 23%), the difference was not significant (P > 0.1). Both concentration methods have highly variable recovery rates, making accurate quantification of low concentrations (< 100/liter) of N. fowleri in the environment difficult.