X. Cagnat

Behaviour of radiocaesium in coastal rivers of the Fukushima Prefecture (Japan) during conditions of low flow and low turbidity--Insight on the possible role of small particles and detrital organic compounds.

To investigate riverine transfers from contaminated soils of the Fukushima Prefecture in Japan to the marine environment, suspended sediments, filtered water, sediments and detrital organic macro debris deposited onto river beds were collected in November 2013 within small coastal rivers during conditions of low flow rates and low turbidity. River waters were directly filtered on the field and high efficiency well-type Ge detectors were used to analyse radiocaesium concentrations in very small quantities of suspended particles and filtered water (a few mg to a few g). For such base-flow conditions, our results show that the watersheds studied present similar hydro-sedimentary behaviours at their outlets and that the exports of dissolved and particulate radiocaesium are comparable. Moreover, the contribution of these rivers to the instantaneous export of radiocaesium to the ocean is similar to that of the Abukuma River. Our preliminary results indicate that, in the estuaries, radiocaesium concentrations in suspended sediments would be reduced by more than 80%, while radiocaesium concentration in filtered waters would be maintained. Significant correlations between radiocaesium concentrations and radiocaesium inventories in the soils of the catchments indicate that there was at that time little intra and inter-watershed variability in the transfer processes of radiocaesium from lands to rivers at this regional scale. The apparent liquid-solid partition coefficient (KD) values acquired for the lowest loads/finest particles complement the values acquired by using sediment traps and highlight the strong capacity of the smallest particles to transfer radiocaesium. Finally, but not least, our observations suggest that there could be a significant transfer of highly contaminated detrital biomass from forest litter to the downstream rivers in a rather conservative way.

Tracing the origin of suspended sediment in a large Mediterranean river by combining continuous river monitoring and measurement of artificial and natural radionuclides.

Delivery of suspended sediment from large rivers to marine environments has important environmental impacts on coastal zones. In France, the Rhone River (catchment area of 98,000 km(2)) is by far the main supplier of sediment to the Mediterranean Sea and its annual solid discharge is largely controlled by flood events. This study investigates the relevance of alternative and original fingerprinting techniques based on the relative abundances of a series of radionuclides measured routinely at the Rhone River outlet to quantify the relative contribution of sediment supplied by the main tributaries during floods. Floods were classified according to the relative contribution of the main subcatchments (i.e., Oceanic, Cevenol, extensive Mediterranean and generalised). Between 2000 and 2012, 221 samples of suspended sediment were collected at the outlet and were shown to be representative of all flood types that occurred during the last decade. Three geogenic radionuclides (i.e., (238)U, (232)Th and (40)K) were used as fingerprints in a multivariate mixing model in order to estimate the relative contribution of the main subcatchment sources-characterised by different lithologies-in sediment samples collected at the outlet. Results showed that total sediment supply originating from Pre-Alpine, Upstream, and Cevenol sources amounted to 10, 7 and 2.10(6)tons, respectively. These results highlight the role of Pre-Alpine tributaries as the main sediment supplier (53%) to the Rhone River during floods. Other fingerprinting approaches based on artificial radionuclide activity ratios (i.e., (137)Cs/(239+240)Pu and (238)Pu/(239+240)Pu) were tested and provided a way to quantify sediment remobilisation or the relative contributions of the southern tributaries. In the future, fingerprinting methods based on natural radionuclides should be further applied to catchments with heterogeneous lithologies. Methods based on artificial radionuclides should be further applied to catchments characterised by heterogeneous post-Chernobyl (137)Cs deposition or by specific releases of radioactive effluents.

Fission product activity ratios measured at trace level over France during the Fukushima accident

The nuclear accident of Fukushima Dai-ichi (Japan) which occurred after the tsunami that impacted the northeast coasts of Japan on March 11th, 2011 led to significant releases of radionuclides into the atmosphere and resulted in the detection of those radionuclides at a global scale. In order to track airborne radionuclides from the damaged reactors and to survey their potential impact on the French territory, the French Institute of Radiation Protection and Nuclear Safety (Institut de Radioprotection et de Sureté Nucléaire IRSN) set up an enhanced surveillance system to give quick results as needed and later give quality trace level measurements. Radionuclides usually measured at trace levels such as (137)Cs and in a very sporadic way (131)I were reported. Radionuclides that we had never measured in air since the Chernobyl accident: (134)Cs, (136)Cs, the mother/daughter pairs (129m)Te-(129)Te and (132)Te-(132)I, and (140)La (from the mother-daughter pair (140)Ba- (140)La) were also reported. Except the (131)I/(137)Cs ratio, activity concentration ratios were constant. These ratios could be used to help source term assessment, or as data for transfer studies realized after the passage of contaminated air masses, typically using the (134)Cs/(137)Cs ratio.

Uranium decay daughters from isolated mines: Accumulation and sources.

This study combines in situ gamma spectrometry performed at different scales, in order to accurately locate the contamination pools, to identify the concerned radionuclides and to determine the distribution of the contaminants from soil to bearing phase scale. The potential mobility of several radionuclides is also evaluated using sequential extraction. Using this procedure, an accumulation area located downstream of a former French uranium mine and concentrating a significant fraction of radioactivity is highlighted. We report disequilibria in the U-decay chains, which are likely related to the processes implemented on the mining area. Coupling of mineralogical analyzes with sequential extraction allow us to highlight the presence of barium sulfate, which may be the carrier of the Ra-226 activities found in the residual phase (Ba(Ra)SO4). In contrast, uranium is essentially in the reducible fraction and potentially trapped in clay-iron coatings located on the surface of minerals.

Environmental consequences of uranium atmospheric releases from fuel cycle facility: II. The atmospheric deposition of uranium and thorium on plants.

Uranium and thorium isotopes were measured in cypress leaves, wheat grains and lettuce taken in the surroundings of the uranium conversion facility of Malvési (South of France). The comparison of activity levels and activity ratios (namely (238)U/(232)Th and (230)Th/(232)Th) in plants with those in aerosols taken at this site and plants taken far from it shows that aerosols emitted by the nuclear site (uranium releases in the atmosphere by stacks and (230)Th-rich particles emitted from artificial ponds collecting radioactive waste mud) accounts for the high activities recorded in the plant samples close to the site. The atmospheric deposition process onto the plants appears to be the dominant process in plant contamination. Dry deposition velocities of airborne uranium and thorium were measured as 4.6 × 10(-3) and 5.0 × 10(-3) m s(-1), respectively.

Environmental releases from fuel cycle facility: part 1: radionuclide resuspension vs. stack releases on ambient airborne uranium and thorium levels.

Airborne activity levels of uranium and thorium series were measured in the vicinity (1.1 km) of a uranium (UF4) processing plant, located in Malvési, south of France. Regarding its impact on the environment, this facility is characterized by its routine atmospheric releases of uranium and by the emission of radionuclide-labelled particles from a storage pond filled with waste water or that contain dried sludge characterized by traces of plutonium and thorium ((230)Th). This study was performed during a whole year (November 2009-November 2010) and based on weekly aerosol sampling. Thanks to ICP-MS results, it was possible to perform investigations of uranium and thorium decay product concentration in the air. The number of aerosol filters sampled (50) was sufficient to establish a relationship between airborne radionuclide variations and the wind conditions. As expected, the more the time spent in the plume, the higher the ambient levels. The respective contributions of atmospheric releases and resuspension from local soil and waste ponds on ambient dust load and uranium-bearing aerosols were estimated. Two shutdown periods dedicated to facility servicing made it possible to estimate the resuspension contribution and to specify its origin (local or regional) according to the wind direction and remote background concentration. Airborne uranium mainly comes from the emission stack and, to a minor extent (∼20%), from wind resuspension of soil particles from the surrounding fields and areas devoted to waste storage. Moreover, weighed activity levels were clearly higher during operational periods than for shutdown periods.

Leda: A gamma-gamma coincidence spectrometer for the measurement of environment samples

This paper presents a new gamma-gamma coincidence spectrometer to measure the radioactivity in environmental samples. This system, called Leda, is made of 2 HPGe and 1 NaI(Tl). The different analysis channels (single, in coincidence or in anti-coincidence) possible thanks to the digital electronics are described. Results obtained with environmental samples are shown. Despite its low efficiency, this method improves the detection limits for all emitters due to its very low background, and thus decreases the counting time.

Low level measurement of (60)Co by gamma ray spectrometry using γ-γ coincidence.

This paper presents the latest development of the laboratory to measure the natural and artificial massic activities in environmental samples. The measurement method of coincident emitters by gamma-gamma coincidence using an anti-Compton device and its digital electronics is described. Results obtained with environmental samples are shown. Despite its low efficiency, this method decreases detection limits of (60)Co for certain samples compared to conventional gamma-ray spectrometry due to its very low background.

Characterisation of naturally occurring radionuclides in the Lower Rhone River (France): preliminary results from suspended solid monitoring

Long term time series acquired in the frame of radioecological monitoring programmes are useful tools for exploring the variability of naturally occurring radionuclide contents. The data set was established in order to investigate the role of discharge, flood type and flood chronicles on such variability within the suspended sediments. Preliminary results show that radionuclide geochemical properties as well as suspended sediment nature and particle residence time may in some particular cases significantly affect the U-Th series nuclide equilibrium.