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1.
Sci Rep ; 14(1): 14213, 2024 Jun 20.
Article in English | MEDLINE | ID: mdl-38902351

ABSTRACT

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.

2.
Proc Natl Acad Sci U S A ; 120(43): e2301811120, 2023 10 24.
Article in English | MEDLINE | ID: mdl-37844225

ABSTRACT

In the context of elevated concerns related to nuclear accidents and warfare, the lessons learnt from the Fukushima Daiichi Nuclear Power Plant accident in 2011 are important. In particular, Japanese authorities implemented an ambitious decontamination program to reduce the air dose rate in order to facilitate the return of the local inhabitants to previously evacuated areas. This approach contrasts the strategy adopted in Chernobyl, where the most contaminated areas remain off limits. Nonetheless, the effectiveness of the Japanese decontamination strategy on the dispersion of radioactive contaminant fluxes across mountainous landscapes exposed to typhoons has not been quantified. Based on the unique combination of river monitoring and modeling in a catchment representative of the most impacted area in Japan, we demonstrate that decontamination of 16% of the catchment area resulted in a decrease of 17% of sediment-bound radioactive fluxes in rivers. Decontamination operations were therefore relatively effective, although they could only be conducted in a small part of the area due to the dominance of steep forested slopes. In fact, 67% of the initial radiocesium contamination was calculated to remain stored in forested landscapes, which may contribute to future downstream radiocesium dispersion during erosive events. Given that only a limited proportion of the initial population had returned in 2019 (~30%), it raises the question as to whether decontaminating a small percentage of the contaminated area was worth the effort, the price, and the amount of waste generated?


Subject(s)
Fukushima Nuclear Accident , Radiation Monitoring , Soil Pollutants, Radioactive , Water Pollutants, Radioactive , Cesium Radioisotopes/analysis , Decontamination , Water Pollutants, Radioactive/analysis , Soil Pollutants, Radioactive/analysis , Japan
3.
Anal Chem ; 95(17): 6923-6930, 2023 May 02.
Article in English | MEDLINE | ID: mdl-37071760

ABSTRACT

The 135Cs/137Cs isotopic ratio is a powerful tool for tracing the origin of radioactive contamination. Since the Fukushima accident, this ratio has been measured by mass spectrometry in several highly contaminated environmental matrices mainly collected near nuclear accident exclusion zones and former nuclear test areas. However, few data were reported at 137Cs environmental levels (<1 kBq kg-1). This is explained by the occurrence of analytical challenges related to the very low radiocesium content at the environmental level with the large presence of mass interferences, making 135Cs and 137Cs measurements difficult. To overcome these difficulties, a highly selective procedure for Cs extraction/separation combined with an efficient mass spectrometry measurement must be applied on a quantity of ca. 100 g of soil. In the current research, an innovative inductively coupled plasma-tandem mass spectrometry (ICP-MS/MS) method has been developed for the 135Cs/137Cs ratio measurement in low activity environmental samples. The use of ICP-MS/MS led to a powerful suppression of 135Cs and 137Cs interferences by introducing N2O, He, and, for the first time, NH3, into the collision-reaction cell. By adjusting the flow rates of these gases, the best compromise between a maximum signal in Cs and an effective interference elimination was achieved allowing a high Cs sensitivity of more than 1.105 cps/(ng g-1) and low background levels at m/z 135 and 137 lower than 0.6 cps. The accuracy of the developed method was successfully verified by analyzing two certified reference materials (IAEA-330 and IAEA-375) commonly used in the literature as validation samples and three sediment samples collected in the Niida River catchment (Japan) impacted by the Fukushima fallout.

4.
Environ Pollut ; 329: 121606, 2023 Jul 15.
Article in English | MEDLINE | ID: mdl-37087087

ABSTRACT

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).


Subject(s)
Fukushima Nuclear Accident , Military Personnel , Radiation Monitoring , Radioactive Fallout , Radioactive Hazard Release , Soil Pollutants, Radioactive , Water Pollutants, Radioactive , Humans , Soil Pollutants, Radioactive/analysis , Tandem Mass Spectrometry , Radiation Monitoring/methods , Cesium Radioisotopes/analysis , Water Pollutants, Radioactive/analysis , Radioactive Fallout/analysis
5.
Environ Pollut ; 324: 121283, 2023 May 01.
Article in English | MEDLINE | ID: mdl-36804884

ABSTRACT

Recently, Comte et al. (2022) re-examined the natural degradation of chlordecone (CLD) in the soils of the French West Indies (FWI) by introducing an additional 'dissipation parameter' into the WISORCH model developed by Cabidoche et al. (2009). Recent data sets of CLD concentrations in FWI soils obtained by Comte et al. enabled them optimizing the model parameters, resulting in significantly shorter estimates of pollution persistence than in the original model. Their conclusions jeopardize the paradigm of a very limited degradation of CLD in FWI soils, which may lead to an entire revision of the management of CLD contamination. However, we believe that their study is questionable on several important aspects. This includes potential biases in the data sets and in the modeling approach. It results in an inconsistency between the estimated dissipation half-life time (DT50) of five years that the authors determined for CLD and the fate of CLD in soil from the application period 1972-1993 until nowadays. Most importantly, a rapid dissipation of CLD in the field as proposed by Comte et al. is not sufficiently supported by data and estimates. Hence, the paradigm of long-term persistence of CLD in FWI soils is still to be considered.


Subject(s)
Chlordecone , Insecticides , Soil Pollutants , Chlordecone/analysis , Chlordecone/metabolism , Insecticides/analysis , Soil , Half-Life , Soil Pollutants/analysis , West Indies
6.
Environ Pollut ; 319: 120963, 2023 Feb 15.
Article in English | MEDLINE | ID: mdl-36587785

ABSTRACT

In 2011, the Fukushima Dai-Ichi Nuclear Power Plant (FDNPP) accident released significant quantities of radionuclides into the environment. Japanese authorities decided to progressively reopen the Difficult-To-Return Zone after the decontamination of priority reconstruction zones. These areas include parts of the initially highly contaminated municipalities located to the north of the FDNPP, including Namie Town, an area drained by the Ukedo and Takase Rivers. Eleven years after the accident, research focused on the spatial distribution of plutonium (Pu) and radiocesium (Cs) isotopes at contrasted individual locations. To complement previous results, the current research was conducted on flood sediment deposits collected at the same locations after major flooding events during eleven fieldwork campaigns organised between 2013 and 2020 at the outlet of the Ukedo and Takase Rivers (n = 22). The results highlighted a global decrease of the Pu and 137Cs contents in sediment with time during the abandonment phase in the region, from 2013 (238.20 fg g-1) to 2020 (4.28 fg g-1). Furthermore, based on the analysis of the 240Pu/239Pu isotopic ratios, the plutonium transiting these rivers (range: 0.166 - 0.220) essentially originated from the global fallout (0.180 ± 0.014 (Kelley et al., 1999)). Sediment showed contrasted properties in the two investigated rivers, which is likely mainly the result of the occurrence of Ogaki Dam on upper sections of the Ukedo River as it strongly impacts the material supply from this river to the Pacific Ocean. A statistical analysis highlighted the strong correlation between Pu activity concentrations and 137Cs activities in both rivers, confirming that both radionuclides are transported with a similar pathway. Despite it was detected early after the accident (2011-2013), the current research demonstrates that plutonium originating from FDNPP is no longer detected in these rivers draining the Difficult-To-Return Zone at the onset of the reopening of the area to its former inhabitants.


Subject(s)
Fukushima Nuclear Accident , Plutonium , Radiation Monitoring , Water Pollutants, Radioactive , Plutonium/analysis , Radiation Monitoring/methods , Japan , Rivers , Water Pollutants, Radioactive/analysis , Cesium Radioisotopes/analysis
7.
Talanta ; 252: 123848, 2023 Jan 15.
Article in English | MEDLINE | ID: mdl-36037768

ABSTRACT

Every accident affecting industrial or nuclear facilities emits micrometric fragments of material into the environment whose elemental and isotopic compositions are characteristic of the process or event. Particle analysis, mainly implemented in the framework of the Non Proliferation Treaty to detect clandestine nuclear activities, provides a powerful tool to identify the origin of the nuclear particulate matter and to assess the environmental impact of nuclear accidents. Initially, particle-scale isotopic analyses aimed at the determination of the U isotopic composition. Now, focus is increasingly given on Pu isotopic measurements to address its origin and potential use. Such measurements are more challenging because of isobaric interferences, including those induced by hydride ions, like 239PuH+ on 240Pu+ and 238UH+ on 239Pu+ in Mixed Oxide (MOX). Such ions are generated during ionization processes by Secondary Ion Mass Spectrometry. Based on a parametric study aiming at the measurement of uranium oxide, uranium carbide and uranium single and double hydride rates, we determined that Pu and U should be detected as elementary ions to limit the impact of such interferences, although mono-oxide ions are more abundant. Thus, we developed an analytical methodology to obtain accurate 240Pu/239Pu atomic ratios both for weapon grade Pu and MOX materials. Hydride rate is first measured in U oxide particles and then applied to correct 240Pu+ and 239Pu+ signals. The relative difference of corrected 240Pu/239Pu isotopic ratios with expected values is reduced by a factor of 4 when measuring weapon grade Pu particles and by a factor of 10-100 when measuring MOX particles containing 1 to 10 wt% of Pu. We also proposed a method to determine the Relative Sensitivity Factor (RSF) based on the decay of Pu in order to quantify the Pu content in MOX samples. The estimated lowest measurable 239Pu/238U atomic ratio in MOX particles is ∼1.6 × 10-3.


Subject(s)
Plutonium , Uranium , Uranium/analysis , Plutonium/analysis , Spectrometry, Mass, Secondary Ion
8.
Sci Total Environ ; 843: 156943, 2022 Oct 15.
Article in English | MEDLINE | ID: mdl-35753489

ABSTRACT

Atmospheric nuclear tests (1945-1980) have led to radioactive fallout across the globe. French tests in Polynesia (1966-1974) may influence the signature of fallout in South America in addition to those conducted by USA and former USSR until 1963 in the Northern hemisphere. Here, we compiled the 240Pu/239Pu atom ratios reported for soils of South America and conducted additional measurements to examine their latitudinal distributions across this continent. Significantly lower ratio values were found in the 20-45° latitudinal band (0.04 to 0.13) compared to the rest of the continent (up to 0.20) and attributed to the contribution of the French atmospheric tests to the ultra-trace plutonium levels found in these soils. Based on sediment cores collected in lakes of Chile and Uruguay, we show the added value of measuring 240Pu/239Pu atom ratios to refine the age models of environmental archives in this region of the world.


Subject(s)
Plutonium , Radiation Monitoring , Soil Pollutants, Radioactive , Water Pollutants, Radioactive , Chile , Plutonium/analysis , Radioisotopes/analysis , Soil , Soil Pollutants, Radioactive/analysis , Water Pollutants, Radioactive/analysis
9.
J Soils Sediments ; 22(6): 1648-1661, 2022.
Article in English | MEDLINE | ID: mdl-35495078

ABSTRACT

Purpose: Identifying best practices for sediment fingerprinting or tracing is important to allow the quantification of sediment contributions from catchment sources. Although sediment fingerprinting has been applied with reasonable success, the deployment of this method remains associated with many issues and limitations. Methods: Seminars and debates were organised during a 4-day Thematic School in October 2021 to come up with concrete suggestions to improve the design and implementation of tracing methods. Results: First, we suggest a better use of geomorphological information to improve study design. Researchers are invited to scrutinise all the knowledge available on the catchment of interest, and to obtain multiple lines of evidence regarding sediment source contributions. Second, we think that scientific knowledge could be improved with local knowledge and we propose a scale of participation describing different levels of involvement of locals in research. Third, we recommend the use of state-of-the-art sediment tracing protocols to conduct sampling, deal with particle size, and examine data before modelling and accounting for the hydro-meteorological context under investigation. Fourth, we promote best practices in modelling, including the importance of running multiple models, selecting appropriate tracers, and reporting on model errors and uncertainty. Fifth, we suggest best practices to share tracing data and samples, which will increase the visibility of the fingerprinting technique in geoscience. Sixth, we suggest that a better formulation of hypotheses could improve our knowledge about erosion and sediment transport processes in a more unified way. Conclusion: With the suggested improvements, sediment fingerprinting, which is interdisciplinary in nature, could play a major role to meet the current and future challenges associated with global change. Supplementary information: The online version contains supplementary material available at 10.1007/s11368-022-03203-1.

10.
Sci Total Environ ; 805: 149778, 2022 Jan 20.
Article in English | MEDLINE | ID: mdl-34818795

ABSTRACT

Since 1945, a large amount of heterogeneous data has been acquired to survey river sediment quality, especially concerning regulatory metals such as Cd, Cr, Cu, Hg, Ni, Pb, and Zn. Large-scale syntheses are critical to assess the effectiveness of public regulations and the resiliency of the river systems. Accordingly, this data synthesis proposes a first attempt to decipher spatio-temporal trends of metal contamination along seven major continental rivers in Western Europe (France, Belgium, Germany, and the Netherlands). A large dataset (>12,000 samples) from various sediment matrices (bed and flood deposits - BFD, suspended particulate matter - SPM, dated sediment cores - DSC) was set up based on monitoring and scientific research from the 1950s to the 2010s. This work investigates the impact of analytical protocols (matrix sampling, fractionation, extraction), location and time factors (related to geology and anthropogenic activities) on metal concentration trends. Statistical analyses highlight crossed-interactions in space and time, as well as between sediment matrices (metal concentrations in SPM ≃ DSC > BFD) and extraction procedures (also related to river lithology). Major spatio-temporal trends are found along several rivers such as (i) an increase of metal concentrations downstream of the main urban industrial areas (e.g. Paris-Rouen corridor on the Seine River, Bonn-Duisburg corridor on the Rhine River), (ii) a long-term influence of former mining areas located in crystalline zones, releasing heavily contaminated sediments for decades (Upper Loire River, Middle Meuse section), (iii) a decrease of metal concentrations since the 1970s (except for Cr and Ni, rather low and stable over time). The improvement of sediment quality in the most recent years in Europe reflects a decisive role of environment policies, such as more efficient wastewater treatments, local applications of the Water Framework Directive and urban industrial changes in the river valleys.


Subject(s)
Metals, Heavy , Water Pollutants, Chemical , Environmental Monitoring , Geologic Sediments , Metals, Heavy/analysis , Rivers , Water Pollutants, Chemical/analysis
11.
Environ Sci Pollut Res Int ; 28(29): 39370-39386, 2021 Aug.
Article in English | MEDLINE | ID: mdl-33755887

ABSTRACT

Brazil is one of the largest consumers of pesticides in the world, and these chemicals present a high contamination risk for the country's water bodies. The mechanisms of mobilization and transport of pesticides from cropland to river systems are controlled by runoff and erosion processes occurring at the catchment scale. In addition to the excessive use of pesticides, the transport processes of these substances are also accelerated by inadequate soil management and the absence of soil conservation measures at the catchment scale. The current research relied on hydrological monitoring to investigate the transport and persistence of pesticides in response to hydrological dynamics. The study was conducted in the Conceição River watershed where runoff and suspended sediment fluxes are continuously monitored at the outlet. This study area is representative of the grain production system in southern Brazil including the application of large amounts of pesticides combined with extensive runoff and erosion problems. Sample collection in the river for pesticide analysis included the analysis of both water and suspended sediment. The sediment deposit analysis was performed in a single location at 4 depths. Results demonstrate the occurrence of pesticides including simazine, 2,4-D, carbendazim, imidacloprid, tebuconazole, propiconazole, tetraconazole, and trifloxystrobin in water, while glyphosate and AMPA were detected in suspended sediments, and AMPA and carbendazim were found in sediment deposits. The study demonstrated the strong dependence of the mechanisms of pesticide mobilization and transport in the catchment with the intra- and interevent variability of hydro-sedimentary processes. Pesticide detections can be related to several factors, including the magnitude of the rainfall event, the period of pesticide application, or the transport of suspended sediment. All these factors are correlated, and the mechanisms of transportation play an important role in the connections between sink and sources. The results suggest that pesticide monitoring should take into account the runoff and erosion pathways in each particular catchment, and it should especially include the monitoring of major rainfall events for identifying and quantifying the occurrence of pesticides in the environment. The transport of pesticides indicates to be potentiated by intensive pesticide use, the magnitude of rainfall-runoff events, and the absence of runoff control measures (e.g., terracing). These results demonstrate that water and soil conservation techniques should be planned and coordinated at the watershed scale to reduce the connectivity of water and sediment flows from agricultural areas to river systems with the implementation of effective runoff control practices. This will control the mobilization agents (runoff), as well as limit the connection between the sources and the water bodies.


Subject(s)
Pesticides , Agriculture , Brazil , Environmental Monitoring , Geologic Sediments , Pesticides/analysis
12.
Environ Sci Technol ; 55(4): 2296-2306, 2021 02 16.
Article in English | MEDLINE | ID: mdl-33507080

ABSTRACT

The widespread use of pesticides in agriculture during the last several decades has contaminated soils and different Critical Zone (CZ) compartments, defined as the area extended from the top of the vegetation canopy to the groundwater table, and it integrates interactions of the atmosphere, lithosphere, biosphere, and hydrosphere. However, the long-term fate, storage, and transfer dynamics of persistent pesticides in CZ in a changing world remain poorly understood. In the French West Indies, chlordecone (CLD), a toxic organochlorine insecticide, was extensively applied to banana fields to control banana weevil from 1972 to 1993 after which it was banned. Here, to understand CZ trajectories we apply a retrospective observation based on marine sediment core analyses to monitor long-term CLD transfer, fate, and consequences in Guadeloupe and Martinique islands. Both CLD profiles show synchronous chronologies. We hypothesized that the use of glyphosate, a postemergence herbicide, from the late 1990s onward induced CZ modification with an increase in soil erosion and led to the release of the stable CLD stored in the soils of polluted fields. CLD fluxes drastically increased when glyphosate use began, leading to widespread ecosystem contamination. As glyphosate is used globally, ecotoxicological risk management strategies should consider how its application affects persistent pesticide storage in soils, transfer dynamics, and widespread contamination.


Subject(s)
Chlordecone , Insecticides , Soil Pollutants , Chlordecone/analysis , Ecosystem , Glycine/analogs & derivatives , Guadeloupe , Insecticides/analysis , Retrospective Studies , Soil Pollutants/analysis , West Indies , Glyphosate
13.
J Soils Sediments ; 20(12): 4160-4193, 2020.
Article in English | MEDLINE | ID: mdl-33239964

ABSTRACT

PURPOSE: This review of sediment source fingerprinting assesses the current state-of-the-art, remaining challenges and emerging themes. It combines inputs from international scientists either with track records in the approach or with expertise relevant to progressing the science. METHODS: Web of Science and Google Scholar were used to review published papers spanning the period 2013-2019, inclusive, to confirm publication trends in quantities of papers by study area country and the types of tracers used. The most recent (2018-2019, inclusive) papers were also benchmarked using a methodological decision-tree published in 2017. SCOPE: Areas requiring further research and international consensus on methodological detail are reviewed, and these comprise spatial variability in tracers and corresponding sampling implications for end-members, temporal variability in tracers and sampling implications for end-members and target sediment, tracer conservation and knowledge-based pre-selection, the physico-chemical basis for source discrimination and dissemination of fingerprinting results to stakeholders. Emerging themes are also discussed: novel tracers, concentration-dependence for biomarkers, combining sediment fingerprinting and age-dating, applications to sediment-bound pollutants, incorporation of supportive spatial information to augment discrimination and modelling, aeolian sediment source fingerprinting, integration with process-based models and development of open-access software tools for data processing. CONCLUSIONS: The popularity of sediment source fingerprinting continues on an upward trend globally, but with this growth comes issues surrounding lack of standardisation and procedural diversity. Nonetheless, the last 2 years have also evidenced growing uptake of critical requirements for robust applications and this review is intended to signpost investigators, both old and new, towards these benchmarks and remaining research challenges for, and emerging options for different applications of, the fingerprinting approach.

14.
Sci Total Environ ; 748: 141345, 2020 Dec 15.
Article in English | MEDLINE | ID: mdl-32810806

ABSTRACT

Solute and particulate elemental concentrations (C) exhibit different responses to changes in discharge (Q), and those relationships are not well understood in subtropical agricultural environments. The objective is to describe the transport processes of different chemical elements during a set of contrasted rainfall events (2011-2015) that occurred in a small rural catchment under subtropical climate. The study was carried out in the Lajeado Ferreira Creek catchment (1.23 km2), southern Brazil. To this end, the concentrations in dissolved organic carbon (DOC), Cl-, NO3-, SO4-, ten chemical elements (in either dissolved or particulate forms) and suspended sediment concentrations (SSC) were determined. Metric indices were then calculated to characterize their transport patterns: (i) the best fit slope between log-C and log-Q (ß), (ii) the coefficient of variation of C and Q, (iii) shape of the hysteresis loop and hysteresis index, and (iv) the flushing index. All particulate elements along with the dissolved inorganic phosphorus (PO4-3) were shown to be controlled by the sediment dynamics. Geogenic elements (Fe2+, Zn2+, Cu2+, Mn2+, Si4+) showed a dilution effect with increasing Q values, likely because they were mainly transported with subsurface and base flow. Dissolved elements that are mainly supplied with fertilizers (Na+ and Cl-) as well as DOC showed a dilution effect, although they were mainly transported by surface runoff. Finally, a chemostatic behavior was found for those chemical elements (Mg2+, K+, Ca2+, NO3- and SO42-) that are supplied by more than one flow pathways. The results demonstrate that under subtropical climate conditions, the transport of essential nutrients including PO4-3 and metals (in particulate form), are mainly transported with surface runoff. Accordingly, runoff control on cultivated hillslopes should be improved to reduce the potential contaminant supply to the river and to reduce the potentially deleterious impacts that they may cause in downstream regions.

15.
Sci Rep ; 10(1): 11858, 2020 07 16.
Article in English | MEDLINE | ID: mdl-32678221

ABSTRACT

Global nuclear weapon testing and the Chernobyl accident have released large amounts of radionuclides into the environment. However, to date, the spatial patterns of these fallout sources remain poorly constrained. Fallout radionuclides (137Cs, 239Pu, 240Pu) were measured in soil samples (n = 160) collected at flat, undisturbed grasslands in Western Europe in the framework of a harmonised European soil survey. We show that both fallout sources left a specific radionuclide imprint in European soils. Accordingly, we used plutonium to quantify contributions of global versus Chernobyl fallout to 137Cs found in European soils. Spatial prediction models allowed for a first assessment of the global versus Chernobyl fallout pattern across national boundaries. Understanding the magnitude of these fallout sources is crucial not only to establish a baseline in case of future radionuclide fallout but also to define a baseline for geomorphological reconstructions of soil redistribution due to soil erosion processes.

16.
Sci Rep ; 10(1): 10502, 2020 06 29.
Article in English | MEDLINE | ID: mdl-32601368

ABSTRACT

eDNA refers to DNA extracted from an environmental sample with the goal of identifying the occurrence of past or current biological communities in aquatic and terrestrial environments. However, there is currently a lack of knowledge regarding the soil memory effect and its potential impact on lake sediment eDNA records. To investigate this issue, two contrasted sites located in cultivated environments in France were studied. In the first site, soil samples were collected (n = 30) in plots for which the crop rotation history was documented since 1975. In the second site, samples were collected (n = 40) to compare the abundance of currently observed taxa versus detected taxa in cropland and other land uses. The results showed that the last cultivated crop was detected in 100% of the samples as the most abundant. In addition, weeds were the most abundant taxa identified in both sites. Overall, these results illustrate the potential of eDNA analyses for identifying the recent (< 10 years) land cover history of soils and outline the detection of different taxa in cultivated plots. The capacity of detection of plant species grown on soils delivering sediments to lacustrine systems is promising to improve our understanding of sediment transfer processes over short timescales.


Subject(s)
DNA, Environmental/analysis , Geologic Sediments/chemistry , Soil/chemistry , DNA, Plant/genetics , France , Lakes , Plants/genetics
17.
Talanta ; 206: 120221, 2020 Jan 01.
Article in English | MEDLINE | ID: mdl-31514872

ABSTRACT

The 236U/238U isotope ratio is a widely used tracer, which provides information on source identification for safeguard purposes, nuclear forensic studies and environmental monitoring. This paper describes an original approach to determine 236U/238U ratios, below 10-8, in environmental samples by combination of ICP-MS/MS for 236U/238U ratio and multiple collector ICPMS measurements for 235U/238U and 234U/235U isotope ratios. Since the hydride form of UO+ (UOH+) is less prone to occur than UH+, we were focused on the oxidised forms of uranium in order to reduce hydride based-interferences in ICP-MS/MS. Then, in-cell ion-molecule reactions with O2 and CO2 were assessed to detect the uranium isotopes in mass-shift mode (Q1: U+ → Q2: UO+). The performances in terms of UO+ sensitivity and minimisation of hydride form of UO+ were evaluated using five different desolvating systems. The best conditions, using an Apex Ω or an Aridus system, produced uranium oxide hydride rate (235U16O1H+/235U16O+) of about 10-7 with O2 in the collision cell. The method was validated through measurements of two certified IRMM standards with 236U/238U isotope ratio of 1.245 × 10-7 and 1.052 × 10-8, giving results in agreement with certified reference values. The relative standard deviations on seven independent measurements for each standard were respectively of 1.5% and 6.2%. Finally, environmental samples corresponding to sediments from the radioactive contamination plume emitted by the Fukushima Daiichi Nuclear Power Plant accident were analysed after a well-established uranium chemical separation procedure. 236U/238U atomic ratios between 1.5 × 10-8 and 7 × 10-9 were obtained with a level accuracy lower than 20%.

18.
Philos Trans R Soc Lond B Biol Sci ; 374(1780): 20180434, 2019 09 02.
Article in English | MEDLINE | ID: mdl-31303171

ABSTRACT

In matrilineal populations, the descent group affiliation is transmitted by women whereas the socio-political power frequently remains in the hands of men. This situation, named the 'matrilineal puzzle', is expected to promote local endogamy as a coping mechanism allowing men to maintain their decision-making power over their natal descent group. In this paper, we revisit this 'matrilineal puzzle' from a population genetics' point of view. Indeed, such tendency for local endogamy in matrilineal populations is expected to increase their genetic inbreeding and generate isolation-by-distance patterns between villages. To test this hypothesis, we collected ethno-demographic data for 3261 couples and high-density genetic data for 675 individuals from 11 Southeast Asian populations with a wide range of social organizations: matrilineal and matrilocal populations (M), patrilineal and patrilocal populations (P) or cognatic populations with predominant matrilocal residence (C). We observed that M and C populations have higher levels of village endogamy than P populations, and that such higher village endogamy leads to higher genetic inbreeding. M populations also exhibit isolation-by-distance patterns between villages. We interpret such genetic patterns as the signature of the 'matrilineal puzzle'. Notably, our results suggest that any form of matrilocal marriage (whatever the descent rule is) increases village endogamy. These findings suggest that male dominance, when combined with matrilocality, constrains inter-village migrations, and constitutes an underexplored cultural process shaping genetic patterns in human populations. This article is part of the theme issue 'The evolution of female-biased kinship in humans and other mammals'.


Subject(s)
Asian People/genetics , Genetic Variation , Mothers/psychology , Asian People/psychology , Family , Family Relations , Fathers/psychology , Female , Genetics, Population , Humans , Male , Marriage/psychology , Rural Population
19.
Sci Total Environ ; 669: 448-458, 2019 Jun 15.
Article in English | MEDLINE | ID: mdl-30884267

ABSTRACT

Polycyclic aromatic hydrocarbons (PAH) have been released by human activities during more than a century, contaminating the entire atmosphere - soil - river continuum. Due to their ubiquity in the environment and their potential severe biological impacts, PAH became priority pollutants and were targeted by environmental public agencies. To better manage PAH pollution, it is necessary to identify unambiguously the sources and pathways of those compounds at the catchment scale, and to evaluate the persistence of historical PAH pollution in the environment especially in those urban contexts concentrating multiple PAH sources. Accordingly, the current research monitored the contamination in atmospheric fallout, soils and rivers of a 950-km2 catchment (Orge River) characterized by an increasing urban gradient in downstream direction, and located in the Seine River basin characterized by a high level of PAH legacy contamination. A combination of various approaches was used, including the widely used PAH diagnostic ratios, together with innovative methods such as PAH correlations and sediment fingerprinting using fallout radionuclides to clearly identify both the origin of PAH and their main PAH pathways to the river. The results demonstrated the persistence of legacy PAH contamination in the catchment, responsible for the signature of the suspended particulate matter currently transiting in the Orge River. They underlined the conservation of PAH through the soil - river continuum. Finally, urban runoff was demonstrated to provide the main PAH source to the river in the densely urbanized area by both PAH correlations and sediment fingerprinting. These results were used to model PAH concentrations in those particles supplied from urban areas to the river.

20.
Chemosphere ; 225: 849-858, 2019 Jun.
Article in English | MEDLINE | ID: mdl-30904765

ABSTRACT

The Fukushima Dai-ichi Nuclear Power Plant (FDNPP) accident in Japan resulted in a major release of radionuclides into the environment. Compared to other radionuclides, few studies have investigated the fate of actinides in the environment. Accordingly, this research investigates the Pu composition in soil samples collected in paddy fields before and after the accident. Furthermore, the vertical distributions of Pu and U isotopic signatures, along with 137Cs activities, were measured in a sediment core collected in the Mano Dam reservoir, in the Fukushima Prefecture. Changes in the relative contributions of the major actinide sources (global fallout or FDNPP derived fallout) were investigated in sediment deposited in the reservoir. The distinct peak observed for all Pu isotope ratios (240Pu/239Pu, 241Pu/239Pu and 242Pu/239Pu) and for 137Cs concentrations in the sediment core was attributed to the Fukushima fallout, and coincided with the maximum atomic contribution of only 4.8 ±â€¯1.0% of Pu from the FDNPP. Furthermore, 236U/238U ratios measured in the sediment core remained close to the global fallout signature indicating there was likely no U from the FDNPP accident detected in the sediment core. More research is required on the environmental dynamics of trace actinides in landscapes closer to the FDNPP where there are likely to be greater abundances of FDNPP-derived Pu and U.


Subject(s)
Fukushima Nuclear Accident , Geologic Sediments/chemistry , Plutonium/analysis , Radiation Monitoring/methods , Soil Pollutants, Radioactive/analysis , Uranium/analysis , Cesium Radioisotopes/analysis , Japan , Nuclear Power Plants , Water Pollutants, Radioactive/analysis
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