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Since the first human release of radionuclides on Earth at the end of the Second World War, impact assessments have been implemented. Radionuclides are now ubiquitous, and the impact of local accidental release on human activities, although of low probability, is of tremendous social and economic consequences. Although radionuclide inventories (at various scales) are essential as input data for impact assessment, crucial information on physicochemical speciation is lacking. Among the metallic radionuclides of interest, cobalt-60 is one of the most important activation products generated in the nuclear industry. In this work, a marine model ecosystem has been defined because seawater and more generally marine ecosystems are final receptacles of metal pollution. A multistep approach from quantitative uptake to understanding of the accumulation mechanism has been implemented with the sea urchin

Cet article décrit la plate-forme CERES® développée au CEA et utilisée pour l’évaluation des conséquences sur la population de rejets de radionucléides dans l’environnement. Les modèles disponibles sont présentés et les grands principes sont décrits.

International audience; Atmospheric transport modeling has been used to interpret the unprecedented number of multi-isotope detections of radioxenons observed during the six months of the qualification process by the Comprehensive Nuclear-Test-Ban Treaty Organization of the new SPALAX-NG system (Système de Prélèvement Automatique en Ligne avec l’Analyse du Xénon - Nouvelle Génération). Highest $^{133}$Xe activity concentrations were found to be systematically associated with the concomitant measurement of several other radioxenons at the prevailing wind direction of north/northeast pointing to the Institute for Radio Elements (IRE), a medical isotope production facility located in Fleurus (Belgium). The lowest $^{133}$Xe activity concentrations were not associated with a prevailing wind direction or other radioxenons, indicating the contribution of distant sources (global background). The IRE's average source terms for $^{133}$mXe and to a lesser extent for $^{133}$Xe (slightly overestimated by a factor of 1.7) showed good agreement with the literature values, while corrections by a factor of ~23 and ~53 were proposed for $^{131}$mXe and $^{135}$Xe since the initial values were underestimated. However, detections of $^{131}$mXe alone and some low-activity concentrations of $^{133}$Xe associated with only one of the other radioxenons could not be linked to the IRE releases. Analysis of these cases suggests the contribution of local source releases that have been difficult to identify to date. In addition to the global background, releases from such local sources, if not identified, could affect the analysis of the isotopic ratios measured following a nuclear test. The characterization of these local contributions is now possible owing to the capacity of the SPALAX-NG and other new generation measurements systems.

The solubility, migration behavior and bioavailability of radionuclides in the marine environment strongly depend on their speciation. This focus article reviews the state-of-the-art and recent advances in the determination of radionuclide speciation in seawater, which is still challenging because of the very high ionic strength of the medium associated with ultra-trace concentrations of these elements in the oceans. In particular, we have highlighted the contribution and usefulness of synchrotron-based techniques such as X-ray absorption spectroscopy. Within this scope, we overview some major radionuclides in seawater, their natural or anthropogenic origin, and their reactivity and natural concentrations. We outline the theoretical speciation models currently used, based on thermodynamic stability constants, and compare them to published experimental data recently obtained from spectroscopic investigation of radionuclides in natural seawater samples. Finally, we discuss some leading perspectives on radionuclide speciation using X-ray absorption spectroscopy in environmental samples at concentrations that must deal with spectroscopy detection limits.

Uranium speciation and bioaccumulation were investigated in the sea urchin

International audience; Uranium speciation and bioaccumulation were investigated in the sea urchin Paracentrotus lividus. Through accumulation experiments in a well-controlled aquarium followed by ICP-OES analysis, the quantification of uranium in the different compartments of the sea urchin was performed. Uranium is mainly distributed in the test (skeletal components), as it is the major constituent of the sea urchin, but in terms of quantity of uranium per gram of compartment, the following rating: intestinal tract > gonads >> test, was obtained. Combining both extended X-ray Absorption Spectroscopy and time-resolved laser-induced fluorescence spectroscopic analysis, it was possible to identify two different forms of uranium in the sea urchin, one in the test, as a carbonato-calcium complex, and the second one in the gonads and intestinal tract, as a protein complex. Toposome is a major calcium-binding transferrin-like protein contained within the sea urchin. EXAFS data fitting of both contaminated organs in vivo and the uranium-toposome complex from protein purified out of the gonads revealed that it is suspected to complex uranium in gonads and intestinal tract. This hypothesis is also supported by the results from two imaging techniques, i.e., Transmission Electron Microscopy and Scanning Transmission X-ray Microscopy. This thorough investigation of uranium uptake in sea urchin is one of the few attempts to assess the speciation in a living marine organism in vivo.

International audience; Uranium is naturally present in seawater at trace levels and may in some cases be present at higher concentrations, due to anthropogenic nuclear activities. Understanding uranium speciation in seawater is thus essential for predicting and controlling its behavior in this specific environmental compartment and consequently, its possible impact on living organisms. The carbonato calcic complex Ca2UO2(CO3)(3) was previously identified as the main uranium species in natural seawater, together with CaUO2(CO3)(3)(2-). In this work, we further investigate the role of the alkaline earth cation in the structure of the ternary uranyl-carbonate complexes. For this purpose, artificial seawater, free of Me2+ and Ca2+, using Sr2+ as a spectroscopic probe was prepared. Combining TRLIF and EXAFS spectroscopy, together with DFT and theoretical thermodynamic calculations, evidence for the presence of Sr alkaline earth counter ion in the complex structure can be asserted. Furthermore, data suggest that when Ca2+ is replaced by SO2+, SrUO2(CO3)(3)(2-) is the main complex in solution and it occurs with the presence of at least one mono dentate carbonate in the uranyl coordination sphere.

In the ocean, complex interactions between natural and anthropogenic radionuclides, seawater, and diverse marine biota provide a unique window through which to examine ecosystem and trophic transfer mechanisms in cases of accidental dissemination. The nature of interaction between radionuclides, the marine environment, and marine species is therefore essential for better understanding transfer mechanisms from the hydrosphere to the biosphere. Although data pertaining to the rate of global transfer are often available, little is known regarding the mechanism of environmental transport and uptake of heavy radionuclides by marine species. Among marine species, sponges are immobile active filter feeders and have been identified as hyperaccumulators of several heavy metals. We have selected the Mediterranean sponge Aplysina cavernicola as a model species for this study. Actinide elements are not the only source of radioactive release in cases of civilian nuclear events; however, their physicochemical transfer mechanisms to marine species remain largely unknown. We have targeted europium(III) as a representative of the trivalent actinides such as americium or curium. To unravel biological uptake mechanisms of europium in A. cavernicola, we have combined radiometric (γ) measurements with spectroscopic (time-resolved laser-induced fluorescence spectroscopy, TRLIFS, and X-ray absorption near-edge structure, XANES) and imaging (transmission electron microscopy, TEM, and scanning transmission X-ray microscopy, STXM) techniques. We have observed that the colloids of NaEu(CO

The present part of the publication (Part II) deals with long range dispersion of radionuclides emitted into the atmosphere during the Fukushima Dai-ichi accident that occurred after the March 11, 2011 tsunami. The first part (Part I) is dedicated to the accident features relying on radionuclide detections performed by monitoring stations of the Comprehensive Nuclear Test Ban Treaty Organization network. In this study, the emissions of the three fission products Cs-137, I-131 and Xe-133 are investigated. Regarding Xe-133, the total release is estimated to be of the order of 6 × 1018 Bq emitted during the explosions of units 1, 2 and 3. The total source term estimated gives a fraction of core inventory of about 8 × 1018 Bq at the time of reactors shutdown. This result suggests that at least 80 % of the core inventory has been released into the atmosphere and indicates a broad meltdown of reactor cores. Total atmospheric releases of Cs-137 and I-131 aerosols are estimated to be 1016 and 1017 Bq, respectively. By neglecting gas/particulate conversion phenomena, the total release of I-131 (gas + aerosol) could be estimated to be 4 × 1017 Bq. Atmospheric transport simulations suggest that the main air emissions have occurred during the events of March 14, 2011 (UTC) and that no major release occurred after March 23. The radioactivity emitted into the atmosphere could represent 10 % of the Chernobyl accident releases for I-131 and Cs-137.

The CERES application ( Code d’Evaluations Rapides Environnementales et Sanitaires ) has been developed by CEA. It is used to evaluate the consequences on human health of releases of isotopes in the environment, either for emergency planning or for safety evaluation. Various types of emissions can be simulated: atmospheric accidental emission, atmospheric emission during normal operation or emission in liquid media under normal operation. Two versions exist, one devoted to radiological impact, the other one devoted to toxic impact.

The fate of radionuclides in the environment is a cause of great concern for modern society, seen especially in 2011 after the Fukushima accident. Among the environmental compartments, seawater covers most of the earth's surface and may be directly or indirectly impacted. The interaction between radionuclides and the marine compartment is therefore essential for better understanding the transfer mechanisms from the hydrosphere to the biosphere. This information allows for the evaluation of the impact on humans via our interaction with the biotope that has been largely undocumented up to now. In this report, we attempt to make a link between the speciation of heavy elements in natural seawater and their uptake by a model marine organism. More specifically, because the interaction of actinides with marine invertebrates has been poorly studied, the accumulation in a representative member of the Mediterranean coralligenous habitat, the sponge Aplysina cavernicola, was investigated and its uptake curve exposed to a radiotracer (241)Am was estimated using a high-purity Ge gamma spectrometer. But in order to go beyond the phenomenological accumulation rate, the speciation of americium(III) in seawater must be assessed. The speciation of (241)Am (and natural europium as its chemically stable surrogate) in seawater was determined using a combination of different techniques: Time-Resolved Laser-Induced Fluorescence (TRLIF), Extended X-ray Absorption Fine Structure (EXAFS) at the LIII edge, Attenuated Total Reflectance Fourier Transform Infrared (ATR-FTIR) spectroscopy and Scanning Electron Microscopy (SEM) and the resulting data were compared with the speciation modeling. In seawater, the americium(III) complex (as well as the corresponding europium complex, although with conformational differences) was identified as a ternary sodium biscarbonato complex, whose formula can be tentatively written as NaAm(CO3)2·nH2O. It is therefore this chemical form of americium that is accumulated by the sponge A. cavernicola.

Seawater contains radionuclides at environmental levels; some are naturally present and others come from anthropogenic nuclear activity. In this report, the molecular speciation in seawater of uranium(VI) and neptunium(V) at a concentration of 5 × 10(-5) M has been investigated for the first time using a combination of two spectroscopic techniques: Time-resolved laser-induced fluorescence (TRLIF) for U and extended X-ray absorption fine structure (EXAFS) for U and Np at the LIII edge. In parallel, the theoretical speciation of uranium and neptunium in seawater at the same concentration is also discussed and compared to spectroscopic data. The uranium complex was identified as the neutral carbonato calcic complex UO2(CO3)3Ca2, which has been previously described in other natural systems. In the case of neptunium, the complex identified is mainly a carbonato complex whose exact stoichiometry is more difficult to assess. The knowledge of the actinide molecular speciation and reactivity in seawater is of fundamental interest in the particular case of uranium recovery and more generally regarding the actinide life cycle within the biosphere in the case of accidental release. This is the first report of actinide direct speciation in seawater medium that can complement inventory data.