International audience | 30 years after the Chernobyl Nuclear Power Plant (CNPP) accident, its radioactive releases still remain of great interest mainly due to the long half-lives of many radionuclides emitted. Observations from the terrestrial environment, which hosts radionuclides for many years after initial deposition, are important for health and environmental assessments. Furthermore, such measurements are the basis for validation of atmospheric transport models and can be used for constraining the still not accurately known source terms. However, although the "Atlas of cesium deposition on Europe after the Chernobyl accident" (hereafter referred to as "Atlas") has been published since 1998, less than 1% of the direct observations of 137 Cs deposition has been made publicly available. The remaining ones are neither accessible nor traceable to specific data providers and a large fraction of these data might have been lost entirely. The present paper is an effort to rescue some of the data collected over the years following the CNPP accident and make them publicly available. The database includes surface air activity concentrations and depo-sition observations for 131 I, 134 Cs and 137 Cs measured and provided by Former Soviet Union authorities the years that followed the accident. Using the same interpolation tool as the official authorities, we have reconstructed a deposition map of 137 Cs based on about 3% of the data used to create the Atlas map. The reconstructed deposition map is very similar to the official one, but it has the advantage that it is based exclusively on documented data sources, which are all made available within this publication. In contrast to the official map, our deposition map is therefore reproducible and all underlying data can be used also for other purposes. The efficacy of the database was proved using simulated activity concentrations and deposition of 137 Cs from a Langrangian and a Euleurian transport model.

30 years after the Chernobyl Nuclear Power Plant (CNPP) accident, its radioactive releases still remain of great interest mainly due to the long half-lives of many radionuclides emitted. Observations from the terrestrial environment, which hosts radionuclides for many years after initial deposition, are important for health and environmental assessments. Furthermore, such measurements are the basis for validation of atmospheric transport models and can be used for constraining the still not accurately known source terms. However, although the “Atlas of cesium deposition on Europe after the Chernobyl accident” (hereafter referred to as “Atlas”) has been published since 1998, less than 1% of the direct observations of 137Cs deposition has been made publicly available. The remaining ones are neither accessible nor traceable to specific data providers and a large fraction of these data might have been lost entirely. The present paper is an effort to rescue some of the data collected over the years following the CNPP accident and make them publicly available. The database includes surface air activity concentrations and deposition observations for 131I, 134Cs and 137Cs measured and provided by Former Soviet Union authorities the years that followed the accident. Using the same interpolation tool as the official authorities, we have reconstructed a deposition map of 137Cs based on about 3% of the data used to create the Atlas map. The reconstructed deposition map is very similar to the official one, but it has the advantage that it is based exclusively on documented data sources, which are all made available within this publication. In contrast to the official map, our deposition map is therefore reproducible and all underlying data can be used also for other purposes. The efficacy of the database was proved using simulated activity concentrations and deposition of 137Cs from a Langrangian and a Euleurian transport model.

International audience | Mining and smelting activities have contaminated the environment with trace metals (TMs) at a worldwide scale for at least two millennia. A combination of chemical approaches and active biomonitoring was performed to analyse the environmental availability and bioavailability of TM palaeo-pollution in a former Pb-Ag mining district in the Vosges Mountains, France. Along a soil TM contamination gradient that covered eight stations, including two archaeological mining sites, the toxicokinetics of six TMs (Pb, Cd, As, Ag, Co, Sb) in the snail Cantareus aspersus revealed that palaeo-pollution from the studied sites remains bioavailable. This study provides the first data on the accumulation kinetics of Ag and Co for C. aspersus. The environmental availability of the TMs was estimated with three chemical extraction methods (aqua regia, EDTA 50 mM, CaCl2 10 mM). Univariate regression analyses showed that EDTA extraction is the best method for estimating the bioavailability of Pb, As, Ag, Co and Sb to snails. None of the three extractants was efficient for Cd. A multivariate analysis of bioaccumulation data revealed that TM bioavailability and transfer were modulated by exposure sources (soil, humus and vegetation) rather than by soil physico-chemical characteristics. Hence, although the deposition of mining wastes dates back several centuries, these wastes still represent a source of contamination that must be considered to develop relevant site management and environmental risk assessment. (C) 2016 Elsevier Ltd. All rights reserved.

Mining and smelting activities have contaminated the environment with trace metals (TMs) at a worldwide scale for at least two millennia. A combination of chemical approaches and active biomonitoring was performed to analyse the environmental availability and bioavailability of TM palaeo-pollution in a former PbAg mining district in the Vosges Mountains, France. Along a soil TM contamination gradient that covered eight stations, including two archaeological mining sites, the toxicokinetics of six TMs (Pb, Cd, As, Ag, Co, Sb) in the snail Cantareus aspersus revealed that palaeo-pollution from the studied sites remains bioavailable. This study provides the first data on the accumulation kinetics of Ag and Co for C. aspersus. The environmental availability of the TMs was estimated with three chemical extraction methods (aqua regia, EDTA 50 mM, CaCl2 10 mM). Univariate regression analyses showed that EDTA extraction is the best method for estimating the bioavailability of Pb, As, Ag, Co and Sb to snails. None of the three extractants was efficient for Cd. A multivariate analysis of bioaccumulation data revealed that TM bioavailability and transfer were modulated by exposure sources (soil, humus and vegetation) rather than by soil physico-chemical characteristics. Hence, although the deposition of mining wastes dates back several centuries, these wastes still represent a source of contamination that must be considered to develop relevant site management and environmental risk assessment.

International audience | This study aimed at determining the fate of trace elements (TE) following soil organic waste (OW) application. We used a unique combination of X-ray absorption spectroscopy analyses, to determine TE speciation, with incubation experiments for in situ monitoring of TE availability patterns over a time course with the technique of the diffusive gradients in thin films (DGT). We showed that copper (Cu) and zinc (Zn) availability were both increased in OW-amended soil, but their release was controlled by distinct mechanisms. Zn speciation in OW was found to be dominated by an inorganic species, i.e. Zn sorbed on Fe oxides. Zn desorption from Fe oxides could explain the increase in Zn availability in OW amended soil. Cu speciation in OW was dominated by organic species. Cu release through the mineralization of organic carbon from OW was responsible for the increase in Cu availability. (C) 2016 Elsevier Ltd. All rights reserved.

This study aimed at determining the fate of trace elements (TE) following soil organic waste (OW) application. We used a unique combination of X-ray absorption spectroscopy analyses, to determine TE speciation, with incubation experiments for in situ monitoring of TE availability patterns over a time course with the technique of the diffusive gradients in thin films (DGT). We showed that copper (Cu) and zinc (Zn) availability were both increased in OW-amended soil, but their release was controlled by distinct mechanisms. Zn speciation in OW was found to be dominated by an inorganic species, i.e. Zn sorbed on Fe oxides. Zn desorption from Fe oxides could explain the increase in Zn availability in OW-amended soil. Cu speciation in OW was dominated by organic species. Cu release through the mineralization of organic carbon from OW was responsible for the increase in Cu availability.

This study aimed at determining the fate of trace elements (TE) following soil organic waste (OW) application. We used a unique combination of X-ray absorption spectroscopy analyses, to determine TE speciation, with incubation experiments for in situ monitoring of TE availability patterns over a time course with the technique of the diffusive gradients in thin films (DGT). We showed that copper (Cu) and zinc (Zn) availability were both increased in OW-amended soil, but their release was controlled by distinct mechanisms. Zn speciation in OW was found to be dominated by an inorganic species, i.e. Zn sorbed on Fe oxides. Zn desorption from Fe oxides could explain the increase in Zn availability in OW-amended soil. Cu speciation in OW was dominated by organic species. Cu release through the mineralization of organic carbon from OW was responsible for the increase in Cu availability. (Résumé d'auteur)

International audience | Studying long-term trends of contaminants in Arctic biota is essential to better understand impacts of anthropogenic activities and climate change on the exposure of sensitive species and marine ecosystems. We concurrently measured temporal changes (2006e2014) in mercury (Hg) contamination of little auks (Alle alle; the most abundant Arctic seabird) and in their major zooplankton prey species (Calanoid copepods, Themisto libellula, Gammarus spp.). We found an increasing contamination of the food-chain in East Greenland during summer over the last decade. More specifically, bird contamination (determined by body feather analyses) has increased at a rate of 3.4% per year. Conversely, bird exposure to Hg during winter in the northwest Atlantic (determined by head feather analyses) decreased over the study period (at a rate of 1.5% per year), although winter concentrations remained consistently higher than during summer. By combining mercury levels measured in birds and zooplankton to isotopic analyses, our results demonstrate that inter-annual variations of Hg levels in little auks reflect changes in food-chain contamination, rather than a reorganization of the food web and a modification of seabird trophic ecology. They therefore underline the value of little auks, and Arctic seabirds in general, as bio-indicators of long-term changes in environmental contamination.

Studying long-term trends of contaminants in Arctic biota is essential to better understand impacts of anthropogenic activities and climate change on the exposure of sensitive species and marine ecosystems. We concurrently measured temporal changes (2006–2014) in mercury (Hg) contamination of little auks (Alle alle; the most abundant Arctic seabird) and in their major zooplankton prey species (Calanoid copepods, Themisto libellula, Gammarus spp.). We found an increasing contamination of the food-chain in East Greenland during summer over the last decade. More specifically, bird contamination (determined by body feather analyses) has increased at a rate of 3.4% per year. Conversely, bird exposure to Hg during winter in the northwest Atlantic (determined by head feather analyses) decreased over the study period (at a rate of 1.5% per year), although winter concentrations remained consistently higher than during summer. By combining mercury levels measured in birds and zooplankton to isotopic analyses, our results demonstrate that inter-annual variations of Hg levels in little auks reflect changes in food-chain contamination, rather than a reorganization of the food web and a modification of seabird trophic ecology. They therefore underline the value of little auks, and Arctic seabirds in general, as bio-indicators of long-term changes in environmental contamination.

International audience | Microplastics have been reported everywhere around the globe. With very limited human activities, the Arctic is distant from major sources of microplastics. However, microplastic ingestions have been found in several Arctic marine predators, confirming their presence in this region. Nonetheless, existing information for this area remains scarce, thus there is an urgent need to quantify the contamination of Arctic marine waters. In this context, we studied microplastic abundance and composition within the zooplankton community off East Greenland. For the same area, we concurrently evaluated microplastic contamination of little auks (Alle alle), an Arctic seabird feeding on zooplankton while diving between 0 and 50 m. The study took place off East Greenland in July 2005 and 2014, under strongly contrasted sea-ice conditions. Among all samples, 97.2% of the debris found were filaments. Despite the remoteness of our study area, microplastic abundances were comparable to those of other oceans, with 0.99 ± 0.62 m−3 in the presence of sea-ice (2005), and 2.38 ± 1.11 m−3 in the nearby absence of sea-ice (2014). Microplastic rise between 2005 and 2014 might be linked to an increase in plastic production worldwide or to lower sea-ice extents in 2014, as sea-ice can represent a sink for microplastic particles, which are subsequently released to the water column upon melting. Crucially, all birds had eaten plastic filaments, and they collected high levels of microplastics compared to background levels with 9.99 and 8.99 pieces per chick meal in 2005 and 2014, respectively. Importantly, we also demonstrated that little auks took more often light colored microplastics, rather than darker ones, strongly suggesting an active contamination with birds mistaking microplastics for their natural prey. Overall, our study stresses the great vulnerability of Arctic marine species to microplastic pollution in a warming Arctic, where sea-ice melting is expected to release vast volumes of trapped debris.

Microplastics have been reported everywhere around the globe. With very limited human activities, the Arctic is distant from major sources of microplastics. However, microplastic ingestions have been found in several Arctic marine predators, confirming their presence in this region. Nonetheless, existing information for this area remains scarce, thus there is an urgent need to quantify the contamination of Arctic marine waters. In this context, we studied microplastic abundance and composition within the zooplankton community off East Greenland. For the same area, we concurrently evaluated microplastic contamination of little auks (Alle alle), an Arctic seabird feeding on zooplankton while diving between 0 and 50 m. The study took place off East Greenland in July 2005 and 2014, under strongly contrasted sea-ice conditions. Among all samples, 97.2% of the debris found were filaments. Despite the remoteness of our study area, microplastic abundances were comparable to those of other oceans, with 0.99 ± 0.62 m−3 in the presence of sea-ice (2005), and 2.38 ± 1.11 m−3 in the nearby absence of sea-ice (2014). Microplastic rise between 2005 and 2014 might be linked to an increase in plastic production worldwide or to lower sea-ice extents in 2014, as sea-ice can represent a sink for microplastic particles, which are subsequently released to the water column upon melting. Crucially, all birds had eaten plastic filaments, and they collected high levels of microplastics compared to background levels with 9.99 and 8.99 pieces per chick meal in 2005 and 2014, respectively. Importantly, we also demonstrated that little auks took more often light colored microplastics, rather than darker ones, strongly suggesting an active contamination with birds mistaking microplastics for their natural prey. Overall, our study stresses the great vulnerability of Arctic marine species to microplastic pollution in a warming Arctic, where sea-ice melting is expected to release vast volumes of trapped debris.

International audience | Once released into the environment, pesticides generate transformation products (TPs) which may be of (eco-)toxicological importance. Past studies have demonstrated the difficulty to predict pesticide TP occurrence and their environmental risk by monitoring-driven approaches mostly used in current regulatory frameworks targeting only known toxicologically relevant TPs. We present a novel combined approach which identifies and categorizes known and unknown pesticide TPs in soil by combining suspect screening time-of-flight mass spectrometry with in silico molecular typology. This approach applies an empirical and theoretical pesticide TP library for compound identification by both non-target and target time-of-flight (tandem) mass spectrometry and structural elucidation through a molecular structure correlation program. In silico molecular typology was then used to group the detected TPs according to common molecular descriptors and to indirectly elucidate their environmental properties by analogy to known pesticide compounds having similar molecular descriptors. This approach was evaluated via the identification of TPs of the triazole fungicide tebuconazole occurring in a field dissipation study. Overall, 22 empirical and 12 yet unknown TPs were detected and categorized into three groups with defined environmental properties. This approach combining suspect screening time-of-flight mass spectrometry with molecular typology could be extended to other organic pollutants and used to rationalize the choice of TPs to be intensively studied towards a more comprehensive environmental risk assessment scheme.

International audience | Once released into the environment, pesticides generate transformation products (TPs) which may be of (eco-)toxicological importance. Past studies have demonstrated the difficulty to predict pesticide TP occurrence and their environmental risk by monitoring-driven approaches mostly used in current regulatory frameworks targeting only known toxicologically relevant TPs. We present a novel combined approach which identifies and categorizes known and unknown pesticide TPs in soil by combining suspect screening time-of-flight mass spectrometry with in silico molecular typology. This approach applies an empirical and theoretical pesticide TP library for compound identification by both non-target and target time-of-flight (tandem) mass spectrometry and structural elucidation through a molecular structure correlation program. In silico molecular typology was then used to group the detected TPs according to common molecular descriptors and to indirectly elucidate their environmental properties by analogy to known pesticide compounds having similar molecular descriptors. This approach was evaluated via the identification of TPs of the triazole fungicide tebuconazole occurring in a field dissipation study. Overall, 22 empirical and 12 yet unknown TPs were detected and categorized into three groups with defined environmental properties. This approach combining suspect screening time-of-flight mass spectrometry with molecular typology could be extended to other organic pollutants and used to rationalize the choice of TPs to be intensively studied towards a more comprehensive environmental risk assessment scheme.

Pesticides generate transformation products (TPs) when they are released into the environment. These TPs may be of ecotoxicological importance. Past studies have demonstrated how difficult it is to predict the occurrence of pesticide TPs and their environmental risk. The monitoring approaches mostly used in current regulatory frameworks target only known ecotoxicologically relevant TPs. Here, we present a novel combined approach which identifies and categorizes known and unknown pesticide TPs in soil by combining suspect screening time-of-flight mass spectrometry with in silico molecular typology. We used an empirical and theoretical pesticide TP library for compound identification by both non-target and target time-of-flight (tandem) mass spectrometry, followed by structural proposition through a molecular structure correlation program. In silico molecular typology was then used to group TPs according to common molecular descriptors and to indirectly elucidate their environmental parameters by analogy to known pesticide compounds with similar molecular descriptors. This approach was evaluated via the identification of TPs of the triazole fungicide tebuconazole occurring in soil during a field dissipation study. Overall, 22 empirical and 12 yet unknown TPs were detected, and categorized into three groups with defined environmental properties. This approach combining suspect screening time-of-flight mass spectrometry with molecular typology could be extended to other organic pollutants and used to rationalize the choice of TPs to be investigated towards a more comprehensive environmental risk assessment scheme.

The aim of this study was to link the concentrations of particulate matter with an aerodynamic diameter below 2.5 μm (PM₂.₅) and associated heavy metals with occurrence of wheezing and hospitalizations due to wheezing in 111 children who live near metallurgical plants in Targoviste City, Romania. A group of 72 children with high levels of immunoglobulin E (IgE) and eosinophils, as well as frequent wheezing episodes, was geolocated on digital thematic maps. Monitoring campaigns and medical assessments were performed over two consecutive years (2013–2014). The multiannual average concentrations of PM₂.₅ ranged from 4.6 to 22.5 μg m⁻³, up to a maximum value of 102 μg m⁻³. Significant correlations (p < 0.01) were observed between the locations of the children with respiratory issues and the PM₂.₅ multiannual average (r = 0.985) and PM₂.₅ maximum (r = 0.813). Fe, Ni, Cd, and Cr were the main marker elements of the emissions from steel production and metal-working facilities in the Targoviste area. The results support the hypothesis that increased PM₂.₅ levels directly influence wheezing symptom and asthma attacks in the analyzed group. IgE, eosinophils, and wheezing episodes may be considered key indicators with which to evaluate the adverse effects of PM₂.₅ air pollution on children’s health.