The role of particulate organic matter in radiocesium transfers from soils to rivers was investigated in areas contaminated by the Fukushima Daiichi Nuclear Power Plant accident. Suspended and ...deposited sediments, filtered water, macro organic debris and dead leaves were sampled along the six most contaminated coastal river catchments of the Fukushima prefecture in the early autumns 2013 and 2014. Radiocesium concentrations of river samples and total organic carbon concentrations in suspended and deposited sediments were measured. Radiocesium concentrations of suspended and deposited sediments were significantly correlated to 137Cs inventories in soils and total organic carbon. The distributions of radiocesium between the organic and mineral phases of both types of sediment were assessed by using a modelling approach. The results suggest that, during the early autumn season, the organic fraction was the main phase that carried the radiocesiums in deposited sediments and in suspended sediments for suspended loads <25mg·L−1. For higher suspended loads like those occurring during typhoon periods, the mineral fraction was the main carrier phase. Thus, high apparent distribution coefficient values noted by various authors in Fukushima could be attributed to the high radiocesium contents of particulate organic matter. Since it is well known that organic compounds generally do not significantly adsorb radiocesium onto specific sites, several hypotheses are suggested: 1) Radiocesiums may have been absorbed into organic components at the early stage of atmospheric radioactive deposits and/or later due to biomass recycling and 2) Those elements would be partly carried by glassy hot particles together with organic matter transported by rivers in Fukushima. Both hypotheses would lead to conserve the amount of radiocesiums associated with particles during their transfers from the contaminated areas to the marine environment. Finally, such organically bound radiocesium would lead to significant deliveries of bioavailable radiocesium for living organisms at Fukushima.
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•Unexpected role of organic particles on 137Cs transfer within Fukushima rivers.•137Cs exported by organic matter in rivers depends on 137Cs soil inventories.•Particulate organic matter is more contaminated than the particulate mineral matter.•Particulate organic matter is the main 137Cs carrier at low suspended loads.•137Cs in organic particles would explain high apparent Kd values at Fukushima.
Abstract 137 Cs 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 137 Cs 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 137 Cs 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 137 Cs 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.
This Research Topic focused on the advancements in our understanding of theenvironmental processes governing the transport and fate of several elements within naturalbiogeochemical cycles. The target ...elements were a group characterized by potentialenvironmental impacts, including emerging contaminants (e.g., critical elements) andradionuclides.
Effective, post-accidental management needs an accurate understanding of the biogeochemical behavior of radionuclides in surface environments at a regional scale. Studies on stable isotopes (element ...homologs) can improve this knowledge. This work focuses on the biogeochemical behavior of stable cesium (Cs) along a major European fluvial-estuarine system, the Gironde Estuary (SW France). We present results obtained from (i) a long-term monitoring (2014–2017) of dissolved (Csd) and particulate (Csp) Cs concentrations at five sites along the freshwater continuum of the Garonne watershed, (ii) Csd and Csp concentrations during four oceanographic campaigns at contrasting hydrological conditions along longitudinal profiles of the estuarine system, (iii) a 24 h cycle of Csp at the estuary mouth, and (iv) a historical trend of Cs bioconcentration in wild oysters at the estuary mouth (RNO/ROCCH, 1984–2017). In addition, we model the partitioning of Cs within the estuarine environment for clay mineral interactions via PhreeqC. At fluvial sites, we observe a geogenic dependence of the Csp and a seasonal variability of Csd, with a downstream increase of the solid-liquid partitioning (log10 Kd values from 3.64 to 6.75 L kg−1) for suspended particulate matter (SPM) < 200 mg L−1. Along the estuarine salinity gradients, Cs shows a non-conservative behavior where fresh SPM (defined as Cs-depleted particles recently put in contact with Csd) act as a Cs sink during both flood and low discharge (drought) conditions. This sorption behavior was explained by the geochemical model, highlighting the relevance of ionic strength, water and SPM residence times. However, at high salinities, the overall log10 Kd value decreases from 6.02 to 5.20 for SPM ∼300–350 mg L−1 due to the Csd oceanic endmember. Despite wild oysters showing low bioconcentration factors (∼1220 L kg−1) at the estuary mouth, they are sensitive organisms to Cs fluxes.
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•Unique comprehensive work on stable Cs in continent-ocean transition system.•Watershed reactivity depends on geological source and seasonal processes.•Non-conservative estuarine behavior, driven by SPM age and salinity.•Modeled conditions show main sorption driver is cation-exchange with clay fraction.•Low BCFs in oysters but general natural origin of Cs related to water discharge.
The Rhone River is one of the most nuclearized river in the world. Radionuclide concentrations in water and suspended sediments transferred to the marine environment were intensively monitored in ...this river over the last decades (2002–2018). Over this period of time, >12 and 25 time integrating samples were collected each year in filtered waters and suspended sediments, respectively, and analyzed for their radionuclide contents at ultra-trace levels by using top performance analytical tools. While >60% of plutonium, americium, cesium, cobalt, silver, beryllium and actinium radioisotopes are carried by sedimentary particles, sodium, tritium, antimony and strontium are mainly exported as dissolved species (>90%) due to their low affinity with particles. Most natural radionuclides contents show low seasonal variation. No significant trends are observed over the last two decades for these elements, even for 40K widely used in fertilizers after the middle of the last century, indicating that the basin has currently converged towards geochemical equilibrium for all of them. In contrast, the concentrations of numerous anthropogenic radionuclides originating from nuclear industries significantly declined since the beginning of the 2000s. Assuming no change of the current anthropic and climatic pressures over the next decades, apparent periods, i.e. the time required for a reduction by half the concentrations in the downstream part of the Rhône River, would be close to 6 years for most artificial radionuclides, except for tritium and other artificial radionuclides conveyed to the river by soil leaching and erosion (90Sr, 241Am, plutonium isotopes) which would be far longer. Referring to regional referential backgrounds, only few anthropogenic radionuclides specifically produced by nuclear industries are still detectable at the downstream part of the Rhone River and excess contents of tritium, 238Pu and 241Am are observed in filtered waters.
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•Contents of natural and anthropogenic radionuclides were monitored over the two last decades.•In filtered waters tritium contents are significantly higher than those of all other radionuclides.•Naturally occurring radionuclides contents show seasonal variation.•Most anthropogenic radionuclides contents declined over the two last decades, except for tritium, OBT, 90Sr and transuranium elements.•Resiliency of the river regarding this family of contaminant is going on for most of them.
Sediment cores from three major French watersheds (Loire, Meuse and Moselle) have been dated by 137Cs and 210Pbxs from 1910 (Loire), 1947 (Meuse) and 1930 (Moselle) until the present in order to ...reconstruct trajectories of plastic additive contaminants including nine phthalate esters (PAEs) and seven organophosphate esters (OPEs), measured by gas chromatography–mass spectrometer (GC–MS–MS). Historical levels of ∑PAEs were higher than those of ∑OPEs in the Loire and the Moselle sediments, while ∑PAEs and ∑OPEs contents were of the same order of magnitude in the Meuse sediments. Although increases in concentrations do not evolve linearly, our results clearly indicate an increase in OPEs and PAEs concentrations from the 1950–1970 period onwards, compared with the first half of the 20th century. Our results show that, ∑OPE contents increase gradually over time in the Loire and Meuse rivers but evolve more randomly in the Moselle River. Trajectories of ∑PAEs depend on the river and no generality can be established, suggesting sedimentary reworking and/or local contamination. Data from this study allowed comparisons of contents of ∑OPEs and ∑PAEs between rivers, with ∑OPE concentrations in the Moselle River > Meuse River > Loire River, and concentrations of ∑PAEs in the Loire River > Moselle River > Meuse River. Among all PAEs, di(2-ethylhexyl) phthalate (DEHP) was the most abundant in all sediment samples, followed by diisobutyl phthalate (DiBP). Tris (2-chloroisopropyl) phosphate (TCPP) was the most abundant OPE in sediments of the three rivers. In addition, strong positive Pearson correlations were observed between organic matter (OM) parameters and OPE concentrations, and to a lesser extent, between OM parameters and PAE concentrations. This is particularly true for the Moselle River and for the Loire River, but less so for the Meuse River.
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•Sediment phthalate (PAE) levels were higher than organophosphate ester (OPE) ones.•PAE and OPE levels increased from the second part of the century until today.•These increases are likely due to European chemical production at the same period.•Tris(2-chloroisopropyl) phosphate (TCPP) was the dominant OPE in sediment cores.•Di(2-ethylhexyl) phthalate (DEHP) was the dominant PAE in sediment cores.
Tritium is a radionuclide commonly observed worldwide in riverine systems. In the Rhône River downstream the Lake Geneva (Switzerland and France), its occurrence is also related to its use for its ...luminescent properties in watchmaking paints. In fact, tritium is regularly observed at anomalous levels in this river and extreme events such as flushing operations might conduct to its transport downstream. In the Rhône River, characterized by 21 dams downstream the Geneva Lake, such operations are regularly organized to remove the sediments and limit problematic consequences such as siltation and increased flooding hazards. The consequences of dam flushing operations on tritium concentrations were thus investigated. Samples of Suspended Particulate Matter (SPM) and water were collected in the Rhone River downstream of Geneva in June 2012, during a planned flushing operation of three upstream reservoirs (Verbois, Chancy-Pougny and Génissiat). The concentrations of tritiated water (HTO) and organically bound Tritium (OBT) were measured and compared to reference concentrations. The flushing operations had no impact on the HTO concentration while the increases observed were related to the authorized releases of HTO from a nuclear power plant located downstream the dams. High increases of OBT concentrations in SPM were observed at two stations (Creys-Malville and Jons) without clear spatial or temporal trends. These anomalous peaks could be explained by the heterogeneous spatial distribution of technogenic tritium leading to large variations of tritium concentrations within the samples even though collected in areas close to each other. The results highlight the need to investigate the amount of such technogenic tritium currently stored in the upstream Rhone River as it might be significant.
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•Tritium were monitored during dam regulations in the Rhone River.•Dam flushing operations had no impact on HTO concentration in water.•Increase of HTO contents were only related to the releases from a nuclear plant.•Flushing operations resuspended contaminated sediments by watches industries.•Sporadic high OBT contents in SPM reflect its heterogeneous distribution.
Although global plastic distribution is at the heart of 21st century environmental concerns, little information is available concerning how organic plastic additives contaminate freshwater sediments, ...which are often subject to strong anthropogenic pressure. Here, sediment core samples were collected in the Rhone and the Rhine watersheds (France), dated using 137Cs and 210Pbxs methods and analysed for nine phthalates (PAEs) and seven organophosphate esters (OPEs). The distribution of these organic contaminants was used to establish a chronological archive of plastic additive pollution from 1860 (Rhine) and 1930 (Rhone) until today. Sediment grain size and parameters related to organic matter (OM) were also measured as potential factors that may affect the temporal distribution of OPEs and PAEs in sediments. Our results show that OPE and PAE levels increased continuously in Rhone and Rhine sediments since the first records. In both rivers, ∑PAEs levels (from 9.1 ± 1.7 to 487.3 ± 27.0 ng g−1 dry weight (dw) ± standard deviation and from 4.6 ± 1.3 to 65.2 ± 11.2 ng g−1 dw, for the Rhine and the Rhone rivers, respectively) were higher than ∑OPEs levels (from 0.1 ± 0.1 to 79.1 ± 13.7 ng g−1 dw and from 0.6 ± 0.1 to 17.8 ± 2.3 ng g−1 dw, for Rhine and Rhone rivers, respectively). In both rivers, di(2-ethylhexyl) phthalate (DEHP) was the most abundant PAE, followed by diisobutyl phthalate (DiBP), while tris (2-chloroisopropyl) phosphate (TCPP) was the most abundant OPE. No relationship was found between granulometry and additives concentrations, while organic matter helps explain the vertical distribution of PAEs and OPEs in the sediment cores. This study thus establishes a temporal trajectory of PAEs and OPEs contents over the last decades, leading to a better understanding of historical pollution in these two Western European rivers.
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•Phthalates (PAEs) appeared in riverine sediments before the 1900s.•Higher concentrations of PAEs than OPEs were observed in sediments of both rivers.•Tris(2-chloroisopropyl) phosphate (TCPP) was the dominant OPE in sediments.•Di(2-ethylhexyl) phthalate (DEHP) was the dominant PAE in sediments.•A positive correlation was found between plastic additive level and organic matter.
An updated review on tritium in the environment Eyrolle, Frédérique; Ducros, Loïc; Le Dizès, Séverine ...
Journal of environmental radioactivity,
January 2018, 2018-Jan, 2018-01-00, 2018-01-01, Letnik:
181
Journal Article
Recenzirano
Various studies indicated more or less recently that organically bound tritium (OBT) formed from gaseous or liquid tritium releases into the environment potentially accumulates in organisms ...contradicting hypotheses associated to methods used to assess the biological impact of tritium on humans (ASN, 2010). Increasing research works were then performed during the last decade in order to gain knowledge on this radionuclide expected to be increasingly released by nuclear installations in the near future within the environment. This review focusses on publications of the last decade. New unpublished observations revealing the presence of technogenic tritium in a sedimentary archive collected in the upper reaches of the Rhône river and findings from the Northwestern Mediterranean revealing in all likelihood the impact of terrigenous tritium inputs on OBT levels recorded in living organisms are also presented. Identifying and understanding the physicochemical forms of tritium and the processes leading to its persistence in environmental compartments would explain most observations regarding OBT concentrations in organisms and definitively excludes that tritium would “bio accumulate” within living organisms.
•Tritium exhibits numerous physico-chemical forms and complex behavior.•Organically bound tritium (OBT) persists in numerous environmental components.•Kinetic gaps lead to apparent disequilibrium between bound (OBT) and free (HTO) forms.•Persistence of technogenic tritium is observed in the Rhône River.•Tritium delivered by coastal rivers could explain OBT in marine organisms.
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