Temporal trajectories of artificial radiocaesium 137Cs in French rivers over the nuclear era reconstructed from sediment cores.

137Cs is a long-lived man-made radionuclide introduced in the environment worldwide at the early beginning of the nuclear Era during atmospheric nuclear testing's followed by the civil use of nuclear energy. Atmospheric fallout deposition of this major artificial radionuclide was reconstructed at the scale of French large river basins since 1945, and trajectories in French nuclearized rivers were established using sediment coring. Our results show that 137Cs contents in sediments of the studied rivers display a large spatial and temporal variability in response to the various anthropogenic pressures exerted on their catchment. The Loire, Rhone, and Rhine rivers were the most affected by atmospheric fallout from the global deposition from nuclear tests. Rhine and Rhone also received significant fallout from the Chernobyl accident in 1986 and recorded significant 137Cs concentrations in their sediments over the 1970-1985 period due to the regulatory releases from the nuclear industries. The Meuse River was notably impacted in the early 1970s by industrial releases. In contrast, the Seine River display the lowest 137Cs concentrations regardless of the period. All the rivers responded similarly over time to atmospheric fallout on their catchment, underlying a rather homogeneous resilience capacity of these river systems to this source of contamination.

Identification of the origin of radiocesium released into the environment in areas remote from nuclear accident and military test sites using the 135Cs/137Cs isotopic signature.

The isotopic signature of radionuclides provides a powerful tool for discriminating radioactive contamination sources and estimating their respective contributions in the environment. In this context, the 135Cs/137Cs ratio has been tested as a very promising isotopic ratio that had not been explored yet in many countries around the world including France. To quantify the levels of radioactivity found in the environment, a new method combining a thorough radiochemical treatment of the sample and an efficient measurement by ICP-MS/MS has been recently developed. This method was successfully applied, for the first time, to soil and sediment samples collected in France in two mountainous regions preferentially impacted either by global fallout from nuclear weapons testing (i.e., the Pyrenees) or by the Chernobyl accident (i.e., the Southern Alps). The 135Cs/137Cs ratios measured on twenty-one samples ranged from 0.66 ± 0.04 and 4.29 ± 0.21 (decay-corrected to January 1st, 2022) corresponding to the characteristic signatures of the fallout from Chernobyl and global fallout associated with the nuclear weapons testing, respectively. Moreover, large variations of both the 137Cs mass activity and the studied isotopic ratio recorded by most samples from the southern Alps suggest varying proportions of these two 137Cs sources. For these samples, the contribution of each source was estimated using this new tracer (135Cs/137Cs) and compared with the mixing contribution given by activity ratio: 239+240Pu/137Cs. This work has successfully demonstrated the applicability of the 135Cs/137Cs isotopic signature to nuclear forensic studies and could be extended to better evaluate the environmental impact of nuclear facilities (i.e., NPP, waste reprocessing).

Depositional environments and historical contamination as a framework to reconstruct fluvial sedimentary evolution.

In this study, we explore the variability of sedimentation conditions (e.g., grain-size, accumulation rate, contamination) according to fluvial depositional environments. Indeed, sediment cores are commonly used as archives of natural and anthropogenic activities in hydrosystems, but their interpretation is often complex, especially in a fluvial context where many factors may affect the quality, continuity, and resolution of the record. It is therefore critical to thoroughly understand the nature and dynamics of an environment in which a sediment core is sampled to be able to interpret it. To that end, four depositional environments from a bypassed reach of the Rhône River were comparatively investigated through geophysics in order to assess the range of sedimentation conditions: a floodplain, a semi-active secondary channel, an active secondary channel, and a dam reservoir. Sediment cores were retrieved from each environment and thoroughly characterised (e.g., grain-size, Total Organic Carbon, organic contaminants). Robust age-depth models were elaborated for each core based on 137Cs, 210Pbex, and Persistent Organic Pollutants (POPs) trends. The results show that each depositional environment recorded a different time-period, and therefore different contamination levels and trends. In particular, a shift from polychlorinated biphenyls (PCBs) to polybrominated diphenyl ethers (PBDEs) as the predominant POP in the sediments can be observed, the tipping point being set in the 1970s. Two types of infrastructure-induced legacy sediments related to two periods of river engineering in the reach were also identified using grain-size analysis. The combination of geophysical methods (Ground Penetrating Radar) and sediment cores is therefore confirmed as a relevant methodology that should be promoted in fluvial contexts in order to reconstruct the sedimentary evolution of fluvial corridors. The study also highlights the challenges of dating recent fluvial sediments and proposes a multi-proxy dating methodology using POPs contamination trends.

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.