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.

Spatial and temporal variations of plutonium isotopes (238Pu and 239,240Pu) in sediments off the Rhone River mouth (NW Mediterranean).

The dispersion and fate of the Rhone River inputs to the Gulf of Lions (Northwestern Mediterranean Sea) have been studied through the spatial and temporal distributions of plutonium isotopes in continental shelf sediments. Plutonium isotopes ((238)Pu and (239,240)Pu) are appropriate tracers to follow the dispersion of particulate matter due both to their high affinity for particles and their long half-lives. In the Rhone River valley, plutonium isotopes originate from both the weathering of the catchment basin contaminated by global atmospheric fallout, and the liquid effluents released from the Marcoule reprocessing plant since 1961. This work presents a first detailed study on (238)Pu and (239,240)Pu distributions in sediments from the Rhone prodelta to the adjacent continental shelf, since the decommissioning of Marcoule in 1997. The vertical distribution of Pu isotopes has been analysed in a 4.75 m long core sampled in 2001 at the Rhone mouth. Despite this length, plutonium is found at the last 10 cm, manifesting the high sedimentation rate of the prodeltaic area and its ability for trapping fine-grained sediments and associated contaminants. The highest (238)Pu and (239,240)Pu concentrations reached 1.26 and 5.97 Bq kg(-1) respectively and were found within the layer 280-290 cm. The (238)Pu/(239,240)Pu activity ratios (AR) demonstrated an efficient and huge trapping of the Pu isotopes derived from Marcoule. The fresh sediments, located on the top of the core, show lower plutonium activity concentrations and lower (238)Pu/(239,240)Pu ratios. This decrease is in close relation with the shut down of the Marcoule reprocessing plant in 1997. In 2001, plutonium isotopes were also analysed in 21 surface sediments located offshore and concentrations ranged from 0.03 to 0.17 Bq kg(-1) for (238)Pu and from 0.33 to 1.72 Bq kg(-1) for (239,240)Pu. The (238)Pu/(239,240)Pu AR ranged from 0.24 close to the river mouth to 0.06 southwards, indicating the decreasing influence of the Marcoule releases (global fallout AR 0.03-0.05 and Marcoule AR 0.30). This is in good agreement with the main direction spread of the Rhone River plume and the bottom current. This dataset has been compared to those obtained in the same area in 1984 and 1990 in order to follow the time trend in Pu concentrations. This comparison highlights the decrease with time in plutonium concentrations close to the Rhone River mouth, but further away this reduction is not so evident.

Distribution of organic carbon, selected stable elements and artificial radionuclides among dissolved, colloidal and particulate phases in the Rhône River (France): preliminary results.

The behaviour of radionuclides discharged from nuclear facilities in the Rhône River depends on their distribution among the dissolved, colloidal and particulate phases. A large water sample was fractionated using sequential ultrafiltration. Size distributions of organic carbon, Fe, Al, Si, Ca, Mg, Cu, Zn, 137Cs, 60Co and 106Ru were obtained. Our results show that organic colloids account for 11% of the total organic carbon content. Approximately 20% of the dissolved (< 450 nm) Fe and Al are in colloidal classes. 137Cs is not significantly transferred by the colloidal phase while 25% of 60Co or 106Ru is associated with organic and inorganic colloids.

Ultrafiltration of large volumes for the determination of colloidally bound artificial radionuclides in natural waters.

A methodology based on large volume ultrafiltration (> 1000 l) is developed in order to characterize the artificial radionuclides associated with the colloidal populations in natural waters. "Inorganic elements" and organic carbon sinks or sources due to sorption or post desorption within the ultrafiltration assembly/membranes of the Sartorius system are underlined and discussed from methodological step experiments as well as recoveries obtained for artificial radionuclides such as 106Ru, 125Sb, 137Cs and 239+240Pu fractionating natural waters from the Rhône River (France), its estuary and the Mediterranean Sea (Gulf of Lions).

Long-term variations of man-made radionuclide concentrations in a bio-indicator Mytilus galloprovincialis from the French Mediterranean coast.

Results from a 14-year monitoring (1984-1997) of man-made radionuclide (137Cs and 106Ru) levels in Mytilus galloprovincialis collected monthly on the French Mediterranean coast are presented. In this area sources of man-made radionuclides are on the one hand atmospheric fallout from both the past nuclear testings and the Chernobyl accident and on the other hand discharges from nuclear installations located on the Rhône River banks, especially those from the spent nuclear fuel reprocessing plant in Marcoule. Long-term variations of radionuclide concentrations in Mytilus demonstrated seasonal variations which are linked to the reproductive cycle of these organisms as well as to variations in land-based inputs of man-made radionuclides. A comparative study of these seasonal variations has been carried out with the aid of spectral analysis. Due to differences in released activities and discharge patterns, flow rates appear to govern mainly the 137Cs variations in the Rhône waters, whereas 106Ru variations are driven by the discharges. In the area under the influence of the Rhône outflow, 137Cs variations in mussels are characterized by seasonal variations which are themselves inversely correlated with variations of 137Cs concentrations in Rhône waters. This cyclic component seems to be closely linked to the mussel reproductive cycle. The possible influence of other parameters is discussed.