Shifts in sediment bacterial communities reflect changes in depositional environments in a fluviatile context.

Sediments are complex heterogeneous matrices allowing to some extent the recording of past environmental conditions by integrating sediment characteristics, contamination and the microbial community assembly. In aquatic environments, abiotic environmental filtering is considered the primary deterministic mechanism shaping microbial communities in sediments. However, the number and relative contributions of geochemical and physical factors associated with biotic parameters (reservoir of microorganisms) complicate our understanding of community assembly dynamics. In this study, the sampling of a sedimentary archive in a site alternately subjected to contrasting inputs from the Eure and the Seine Rivers allowed us to study the response of microbial communities to changes in depositional environment over time. The coupling of the quantification and sequencing of the gene encoding the 16S rRNA with analyses of grain size, organic matter and major and trace metal contents demonstrated that microbial communities reflected contrasting sedimentary inputs over time. Total organic carbon (TOC) was the main factor influencing microbial biomass, while the quantity and quality of organic matter (R400, RC/TOC), major elements (i.e. Al, Fe, Ti) and trace metals (i.e. Zn, Pb, Cu, Cr, Ni, As, Co, Ag, Sb) shaped the structure of the microbial community. Besides the effect of geochemical factors, a specific microbial signature was associated with the contrasting sedimentary sources, highlighting the importance of the microbial reservoir in the assembly of microbial communities. Indeed, the main genera identified in the facies influenced by the Eure River were affiliated with the phyla Desulfobacterota (Syntrophus, Syntrophorhabdus, Smithella, Desulfatiglans), Firmicutes (Clostridium_sensu_stricto_1), Proteobacteria (Crenothrix), Verrucomicrobiota (Luteolibacter), while the contributions of the Seine River were characterised by some halophilic genera Salirhabdus (Firmicutes), Haliangium (Myxococcota) and SCGC-AB-539-J10 (Chloroflexi). This study sheds light on the overall processes determining the assembly of microbial communities in sediments and the importance of associating geochemical factors with reservoirs of microorganisms inherited from sediment sources.

Determining the geochemical fingerprint of the lead fallout from the Notre-Dame de Paris fire: Lessons for a better discrimination of chemical signatures.

On 2019, the fire of Notre-Dame de Paris cathedral ("NDdP") spread an unknown amount of lead (Pb) dust from the roof of the cathedral over Paris. No data describing the geochemical fingerprint of the roof lead, as well as no particle collected during the fire, were available: a post-hoc sampling was performed. To discriminate the potential environmental impact of the fire from multiple Pb sources in Paris, it was mandatory to define unequivocally the fire dust geochemical signature. A dedicated and in hindsight geochemistry-based strategy was developed to eliminate any source of potential contamination due to sampling substrates or previously deposited dust. Radiogenic Pb isotopic signatures (206Pb/207Pb and 208Pb/206Pb ratios) and elemental ratios were determined in 23 Pb-rich samples collected inside NDdP. We determined that the dust collected on wood substrates on the first floor was most representative of fire emissions. These samples were the analyzed for the 4 Pb isotopes (204, 206, 207, 208) and the fire dust signature is characterized by ratio values of 206Pb/207Pb: 1.1669-1.1685, 208Pb/206Pb: 2.0981-2.1095, 208Pb/204Pb: 38.307-38.342, 207Pb/204Pb: 15.633-15.639 and 206Pb/204Pb: 18.242-18.275. In addition, the fire dust presents typical element-to-Pb ratio. This fingerprint was compared to the signatures of the known local Pb sources. The geochemical fingerprint of the fire is significantly different from that of the dominant urban Pb source. This will allow future evaluation of the contribution of the fire to Paris Pb pollution and of the real extent of the area affected by the Pb-containing dust plume. Moreover, the geographical origin of Pb used for the roof restauration and the spire building was identified. These findings open new ways to study the Pb sources in historical monuments for environmental impacts evaluation, as well as for historical perspectives.

The stress sigma factor σS/RpoS counteracts Fur repression of genes involved in iron and manganese metabolism and modulates the ionome of Salmonella enterica serovar Typhimurium.

In many Gram-negative bacteria, the stress sigma factor of RNA polymerase, σS/RpoS, remodels global gene expression to reshape the physiology of quiescent cells and ensure their survival under non-optimal growth conditions. In the foodborne pathogen Salmonella enterica serovar Typhimurium, σS is also required for biofilm formation and virulence. We have previously identified sRNAs genes positively controlled by σS in Salmonella, including the two paralogous sRNA genes, ryhB1 and ryhB2/isrE. Expression of ryhB1 and ryhB2 is repressed by the ferric uptake regulator Fur when iron is available. In this study, we show that σS alleviates Fur-mediated repression of the ryhB genes and of additional Fur target genes. Moreover, σS induces transcription of the manganese transporter genes mntH and sitABCD and prevents their repression, not only by Fur, but also by the manganese-responsive regulator MntR. These findings prompted us to evaluate the impact of a ΔrpoS mutation on the Salmonella ionome. Inductively coupled plasma mass spectrometry analyses revealed a significant effect of the ΔrpoS mutation on the cellular concentration of manganese, magnesium, cobalt and potassium. In addition, transcriptional fusions in several genes involved in the transport of these ions were regulated by σS. This study suggests that σS controls fluxes of ions that might be important for the fitness of quiescent cells. Consistent with this hypothesis, the ΔrpoS mutation extended the lag phase of Salmonella grown in rich medium supplemented with the metal ion chelator EDTA, and this effect was abolished when magnesium, but not manganese or iron, was added back. These findings unravel the importance of σS and magnesium in the regrowth potential of quiescent cells.

Key factors influencing metal concentrations in sediments along Western European Rivers: A long-term monitoring study (1945-2020).

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.

Increasing the power of interpretation for soil metaproteomics data.

BACKGROUND: Soil and sediment microorganisms are highly phylogenetically diverse but are currently largely under-represented in public molecular databases. Their functional characterization by means of metaproteomics is usually performed using metagenomic sequences acquired for the same sample. However, such hugely diverse metagenomic datasets are difficult to assemble; in parallel, theoretical proteomes from isolates available in generic databases are of high quality. Both these factors advocate for the use of theoretical proteomes in metaproteomics interpretation pipelines. Here, we examined a number of database construction strategies with a view to increasing the outputs of metaproteomics studies performed on soil samples. RESULTS: The number of peptide-spectrum matches was found to be of comparable magnitude when using public or sample-specific metagenomics-derived databases. However, numbers were significantly increased when a combination of both types of information was used in a two-step cascaded search. Our data also indicate that the functional annotation of the metaproteomics dataset can be maximized by using a combination of both types of databases. CONCLUSIONS: A two-step strategy combining sample-specific metagenome database and public databases such as the non-redundant NCBI database and a massive soil gene catalog allows maximizing the metaproteomic interpretation both in terms of ratio of assigned spectra and retrieval of function-derived information. Video abstract.

The Isotopic Signature of Lead Emanations during the Fire at Notre Dame Cathedral in Paris, France.

When Notre Dame de Paris cathedral caught fire on 15 April 2019, lead particles were deposited in its surroundings. Our objective was to determine whether the lead plume had a homogeneous isotopic signature (i.e., a set of homogenous isotopic ratios), and whether, if so, this was different from common sources. In January 2020, dust samples were collected from six areas inside the cathedral, downwind of the fire, as well as from eight roof debris fragments. These samples were mineralized and analyzed using ICP-MS. Their isotopic ratios (207Pb/206Pb and 206Pb/204Pb) were determined and then compared both to each other and to previous published ratios measured in home dusts and blood samples collected in France. The isotopic ratios of dust samples collected inside the cathedral were compatible with each other and with the roof fragments. These isotopic ratios are common and differ neither from those of many other dusts collected in France during the period 2008-2009, nor from those of blood samples collected from children in France during the same period. Moreover, the fire's isotopic signature is close to the overall signature for Paris. Indeed, it would be difficult to attribute the fire at the cathedral to either lead poisoning or environmental contamination.

Investigating the relationships between chemical element concentrations and discharge to improve our understanding of their transport patterns in rural catchments under subtropical climate conditions.

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.

Innovative combination of tracing methods to differentiate between legacy and contemporary PAH sources in the atmosphere-soil-river continuum in an urban catchment (Orge River, France).

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.

Impact of urban pressure on the spatial and temporal dynamics of PAH fluxes in an urban tributary of the Seine River (France).

Polycyclic aromatic hydrocarbons (PAHs) produced by numerous anthropogenic activities are ubiquitous in the environment and have become a priority concern due to their potential severe biological impacts. A better understanding of PAH transfer at the catchment scale is therefore necessary to improve the management of PAH contaminants and protect rivers. Furthermore, the impact of changes in hydrological regimes and land uses on PAH fluxes should be specifically investigated. Accordingly, the current research monitors the contamination in atmospheric fallout, soils and rivers in a 950-km2 catchment (Orge River) characterized by an increasing urban gradient in downstream direction. During an entire hydrological year, river water contamination was quantified through regular sampling of both particulate and dissolved material at four river-monitoring stations, reflecting the increasing urbanization gradient. The significant input of PAHs from urban areas in downstream river sections corresponded to a specific PAH flux that reached 23 g km-2 y-1 despite the low sediment yield. Moreover, the comparison with runoff-specific fluxes reported in the literature underlined the major impact of urban runoff on the Orge River water and sediment quality. Nevertheless, the annual PAH load exported by the river (21 kg y-1) remained lower than the PAH inputs from atmospheric fallout (173 kg y-1), demonstrating the continuous accumulation of PAH from atmospheric fallout in the catchment soils. Consequently, the notably large PAH stock (close to 1000 tons) resulting from historical contamination of this early-industrialized region continues to increase due to ongoing atmospheric inputs.

Tracing the sources of suspended sediment and particle-bound trace metal elements in an urban catchment coupling elemental and isotopic geochemistry, and fallout radionuclides.

The excessive supply of contaminants from urban areas to rivers during the last centuries has led to deleterious impacts on aquatic ecosystems. The sources, the behavior, and the dynamics of these contaminants must be better understood in order to reduce this excessive anthropogenic pollution. Accordingly, the current research investigated the particle-bound trace element (TE) contamination of the 900-km2 Orge River (Seine basin, France) and the potential sources of these particles (agricultural or forest soils, channel banks, road deposited sediments), through the analysis of multiple fallout radionuclides, elemental geochemistry, and lead isotopic composition on suspended particulate matter (SPM) collected during a hydrological year at four stations following an increasing urbanization gradient (300 to 5000 inhab.km-2). Fallout radionuclide measurements showed an increasing contribution of recently eroded particles from urban areas to the SPM in downstream direction. However, this contribution varied depending on hydrological conditions. A greater contribution of particles originating from urban areas was observed during low stage periods. On the contrary, the contribution of agricultural soils and channel banks that are less enriched in contaminants and fallout radionuclides was higher during seasonal floods, which explained the dilution of radionuclide contents in sediment transiting the river during those events. Trace element contamination of SPM in Cu, Zn, Pb, and Sb increased from moderate to significant levels with urban pressure in downstream direction (with corresponding enrichment factors raising from 2 to 6). In addition, Pb isotopic ratios indicated that the main source of Pb corresponded to the "urban" signature found in road deposited sediments. The low variations in lead isotope ratios found in the SPM for contrasting hydrological conditions demonstrated the occurrence of a single source of Pb contamination. These results demonstrate the need to better manage urban runoff during both flood and low precipitation events to prevent the supply of diffuse particle-bound contamination to rivers draining urban areas.

Investigating the metal contamination of sediment transported by the 2016 Seine River flood (Paris, France).

Fine sediment transport in rivers is exacerbated during flood events. These particles may convey various contaminants (i.e. metals, pathogens, industrial chemicals, etc.), and significantly impact water quality. The exceptional June 2016 flood of the Seine River (catchment area: 65 000 km2, France), potentially mobilized and deposited contaminated materials throughout the Paris region. Flood sediment deposits (n = 29) were collected along the Seine River and its main tributaries upstream (Yonne, Loing and Marne Rivers) and downstream of Paris (Oise and Eure Rivers). Fallout radionuclides (137Cs, 7Be) were measured to characterize the sources of the material transiting the river, while trace elements (e.g. Cr, Ni, Zn, Cu, As, Cd, Sb, Pb, Tl, Ag) and stable lead isotopes (206Pb/207Pb) were analyzed to quantify the contamination of sediment transported during the flood. In upper sections of the Seine River, sediment mainly originated from the remobilization of particles with a well-balanced contribution of surface and subsurface sources. In the upstream tributaries, sediment almost exclusively originated from the remobilization of subsurface particles. In Paris and downstream of Paris, recently eroded particles and surface sources dominated, suggesting particles were mainly supplied by urban runoff and the erosion of agricultural soils. The highest metal concentrations and Enrichment Factors (EF) were found in the sediment collected in the Loing, Orge and Yvette upstream tributaries. Although these inputs were diluted in the Seine River, an increase in elemental concentrations was observed, progressing downstream through Paris. However, EFs in sediment collected along the Seine River were lower or in the same range of values sampled over the last several decades, reflecting the progressive decontamination of the urbanized Seine River basin.

Application of a multidisciplinary and integrative weight-of-evidence approach to a 1-year monitoring survey of the Seine River.

Quality assessment of environments under high anthropogenic pressures such as the Seine Basin, subjected to complex and chronic inputs, can only be based on combined chemical and biological analyses. The present study integrates and summarizes a multidisciplinary dataset acquired throughout a 1-year monitoring survey conducted at three workshop sites along the Seine River (PIREN-Seine program), upstream and downstream of the Paris conurbation, during four seasonal campaigns using a weight-of-evidence approach. Sediment and water column chemical analyses, bioaccumulation levels and biomarker responses in caged gammarids, and laboratory (eco)toxicity bioassays were integrated into four lines of evidence (LOEs). Results from each LOE clearly reflected an anthropogenic gradient, with contamination levels and biological effects increasing from upstream to downstream of Paris, in good agreement with the variations in the structure and composition of bacterial communities from the water column. Based on annual average data, the global hazard was summarized as "moderate" at the upstream station and as "major" at the two downstream ones. Seasonal variability was also highlighted; the winter campaign was least impacted. The model was notably improved using previously established reference and threshold values from national-scale studies. It undoubtedly represents a powerful practical tool to facilitate the decision-making processes of environment managers within the framework of an environmental risk assessment strategy.

Contamination of soils by metals and organic micropollutants: case study of the Parisian conurbation.

Soils are playing a central role in the transfer and accumulation of anthropogenic pollutants in urbanized regions. Hence, this study aimed at examining the contamination levels of selected soils collected within and around the Paris conurbation (France). This also evaluated factors controlling contamination. Twenty-three trace and major elements as well as 82 organic micropollutants including polycyclic aromatic hydrocarbons (PAHs), polychlorinated biphenyls (PCBs), phthalates (PAEs), polybrominated diphenyl ethers (PBDEs), alkylphenols (APs), and perfluoroalkylated substances (PFASs) were analyzed. Results reinforced the concern raised by the occurrence and levels of metals such as Zn, Pb, Cu, and Hg, identified as metallic markers of anthropogenic activities, but also pointed out the ubiquitous contamination of soils by organic micropollutants in the 0.2-55,000-µg/kg dw range. For well-documented compounds like PAHs, PCBs, and to a lesser extent PBDEs, contents were in the range of background levels worldwide. The pollutant stock in tested soil was compared to the annual atmospheric input. For PAHs; Pb; and to a lesser extent Zn, Cu, Cd, Hg, Sb, PAEs, and APs, a significant stock was observed, far more important than the recent annual atmospheric fluxes. This resulted from both (i) the persistence of a fraction of pollutants in surface soils and (ii) the cumulative atmospheric inputs over several decades. Regarding PBDEs and PFASs, stronger atmospheric input contributions were observed, thereby highlighting their recent dispersal into the environment.

Investigating the temporal dynamics of suspended sediment during flood events with 7Be and 210Pbxs measurements in a drained lowland catchment.

Soil erosion is recognized as one of the main processes of land degradation in agricultural areas. High suspended sediment loads, often generated from eroding agricultural landscapes, are known to degrade downstream environments. Accordingly, there is a need to understand soil erosion dynamics during flood events. Suspended sediment was therefore sampled in the river network and at tile drain outlets during five flood events in a lowland drained catchment in France. Source and sediment fallout radionuclide concentrations (7Be, 210Pbxs) were measured to quantify both the fraction of recently eroded particles transported during flood events and their residence time. Results indicate that the mean fraction of recently eroded sediment, estimated for the entire Louroux catchment, increased from 45 ± 20% to 80 ± 20% between December 2013 and February 2014, and from 65 ± 20% to 80 ± 20% in January 2016. These results demonstrate an initial flush of sediment previously accumulated in the river channel before the increasing supply of sediment recently eroded from the hillslopes during subsequent events. This research highlights the utility of coupling continuous river monitoring and fallout radionuclide measurements to increase our understanding of sediment dynamics and improve the management of soil and water resources in agricultural catchments.

Quantifying sediment sources in a lowland agricultural catchment pond using (137)Cs activities and radiogenic (87)Sr/(86)Sr ratios.

Soil erosion often supplies high sediment loads to rivers, degrading water quality and contributing to the siltation of reservoirs and lowland river channels. These impacts are exacerbated in agricultural catchments where modifications in land management and agricultural practices were shown to accelerate sediment supply. In this study, sediment sources were identified with a novel tracing approach combining cesium ((137)Cs) and strontium isotopes ((87)Sr/(86)Sr) in the Louroux pond, at the outlet of a lowland cultivated catchment (24km(2), Loire River basin, France) representative of drained agricultural areas of Northwestern Europe. Surface soil (n=36) and subsurface channel bank (n=17) samples were collected to characterize potential sources. Deposited sediment (n=41) was sampled across the entire surface of the pond to examine spatial variation in sediment deposits. In addition, a 1.10m sediment core was sampled in the middle of the pond to reconstruct source variations throughout time. (137)Cs was used to discriminate between surface and subsurface sources, whereas (87)Sr/(86)Sr ratios discriminated between lithological sources. A distribution modeling approach quantified the relative contribution of these sources to the sampled sediment. Results indicate that surface sources contributed to the majority of pond (µ 82%, σ 1%) and core (µ 88%, σ 2%) sediment with elevated subsurface contributions modeled near specific sites close to the banks of the Louroux pond. Contributions of the lithological sources were well mixed in surface sediment across the pond (i.e., carbonate sediment contribution, µ 48%, σ 1% and non-carbonate sediment contribution, µ 52%, σ 3%) although there were significant variations of these source contributions modeled for the sediment core between 1955 and 2013. These fluctuations reflect both the progressive implementation of land consolidation schemes in the catchment and the eutrophication of the pond. This original sediment fingerprinting study demonstrates the potential of combining radionuclide and strontium isotopic geochemistry measurements to quantify sediment sources in cultivated catchments.

Metal exposure in cows grazing pasture contaminated by iron industry: Insights from magnetic particles used as tracers.

Magnetic particles (MP) emitted by an iron smelter were used to investigate the exposure of cows grazing on a grassland polluted by these MP and by large amounts of potentially toxic elements (PTE). The morphology as well as the chemical composition of the MP separated from cow dung were studied. Large amounts of typical MP were found (1.1 g kg(-1) dry weight) in the cow dung sampled from the exposed site, whereas these particles were absent from the reference unpolluted site. The ingested MP were mainly technogenic magnetic particles (TMP) emitted by the smelter. Considering the MP concentration in the grazed grass on the exposed site, it was concluded that cows absorb the MP not only from the grass but also from the soil surface. The results of a mild acidic leaching of the MP suggested that the particles were possibly submitted to a superficial dissolution in the abomasum, pointing at a potential route of transfer of the PTE originating from the TMP and leading into food chains. TMP were only a small part of the anthropogenic contamination having affected the soil and the dung. However, due to their unequivocal signature, TMP are a powerful tracer of the distribution of PTE in the different compartments constituting the food chains and the ecosystems. Furthermore, the measurement of the particle sizes gave evidence that a noticeable proportion of the MP could enter the respiratory tract.

Radiocesium transfer from hillslopes to the Pacific Ocean after the Fukushima Nuclear Power Plant accident: A review.

The devastating tsunami triggered by the Great East Japan Earthquake on March 11, 2011 inundated the Fukushima Dai-ichi Nuclear Power Plant (FDNPP) resulting in a loss of cooling and a series of explosions releasing the largest quantity of radioactive material into the atmosphere since the Chernobyl nuclear accident. Although 80% of the radionuclides from this accidental release were transported over the Pacific Ocean, 20% were deposited over Japanese coastal catchments that are subject to frequent typhoons. Among the radioisotopes released during the FDNPP accident, radiocesium ((134)Cs and (137)Cs) is considered the most serious current and future health risk for the local population. The goal of this review is to synthesize research relevant to the transfer of FDNPP derived radiocesium from hillslopes to the Pacific Ocean. After radiocesium fallout deposition on vegetation and soils, the contamination may remain stored in forest canopies, in vegetative litter on the ground, or in the soil. Once radiocesium contacts soil, it is quickly and almost irreversibly bound to fine soil particles. The kinetic energy of raindrops instigates the displacement of soil particles, and their bound radiocesium, which may be mobilized and transported with overland flow. Soil erosion is one of the main processes transferring particle-bound radiocesium from hillslopes through rivers and streams, and ultimately to the Pacific Ocean. Accordingly this review will summarize results regarding the fundamental processes and dynamics that govern radiocesium transfer from hillslopes to the Pacific Ocean published in the literature within the first four years after the FDNPP accident. The majority of radiocesium is reported to be transported in the particulate fraction, attached to fine particles. The contribution of the dissolved fraction to radiocesium migration is only relevant in base flows and is hypothesized to decline over time. Owing to the hydro-meteorological context of the Fukushima region, the most significant transfer of particulate-bound radiocesium occurs during major rainfall and runoff events (e.g. typhoons and spring snowmelt). There may be radiocesium storage within catchments in forests, floodplains and even within hillslopes that may be remobilized and contaminate downstream areas, even areas that did not receive fallout or may have been decontaminated. Overall this review demonstrates that characterizing the different mechanisms and factors driving radiocesium transfer is important. In particular, the review determined that quantifying the remaining catchment radiocesium inventory allows for a relative comparison of radiocesium transfer research from hillslope to catchment scales. Further, owing to the variety of mechanisms and factors, a transdisciplinary approach is required involving geomorphologists, hydrologists, soil and forestry scientists, and mathematical modellers to comprehensively quantify radiocesium transfers and dynamics. Characterizing radiocesium transfers from hillslopes to the Pacific Ocean is necessary for ongoing decontamination and management interventions with the objective of reducing the gamma radiation exposure to the local population.

Depth distribution of cesium-137 in paddy fields across the Fukushima pollution plume in 2013.

Large quantities of radiocesium were deposited across a 3000 km(2) area northwest of the Fukushima Dai-ichi nuclear power plant after the March 2011 accident. Although many studies have investigated the fate of (137)Cs in soil in the months following the accident, the depth distribution of this radioactive contaminant in rice paddy fields requires further examination after the typhoons that occurred in this region. Such investigations will help minimize potential human exposure in rice paddy fields. Radionuclide activity concentrations, organic content and particle size were analysed in 10 soil cores sampled from paddy fields in November 2013, 20 km north of the Fukushima power plant. Our results demonstrate limited depth migration of (137)Cs with the majority concentrated in the uppermost layers of soils (<5 cm). More than 30 months after the accident, between 46.8 and 98.7% of the total (137)Cs inventories was found within the top 5 cm of the soil surface, despite cumulative rainfall totalling 3300 mm. Furthermore, there were no significant correlations between (137)Cs depth distribution and the other parameters. We attributed the maximum depth penetration of (137)Cs to grass cutting (73.6-98.5% of (137)Cs in the upper 5 cm) and farming operations (tillage - 46.8-51.6% of (137)Cs in the upper 5 cm). As this area is exposed to erosive events, ongoing decontamination works may increase soil erodibility. We therefore recommend the rapid removal of the uppermost - contaminated - layer of the soil after removing the vegetation to avoid erosion of contaminated material during the subsequent rainfall events. Further analysis is required to thoroughly understand the impacts of erosion on the redistribution of radiocesium throughout the Fukushima Prefecture.

Three centuries of heavy metal pollution in Paris (France) recorded by urban speleothems.

The first record of urban speleothems used to reconstruct the history of heavy metal pollution of shallow groundwaters is presented. Two speleothems grew during the last 300 years in an underground aqueduct in the north-eastern part of Paris. They display high Pb, Mn V, Cu, Cd and Al concentrations since 1900 due to the urbanization of the site which triggered anthropogenic contamination of the water feeding the speleothems. Surprisingly, these heavy metal concentrations are also high in the oldest part. This early pollution could come from the use of Parisian waste as fertilizers in the orchards and vineyards cultivated above the aqueduct before urbanization. Lead isotopes were measured in these carbonates as well as in lead artifacts from the 17th-18th centuries ((206)Pb/(207)Pb=1.180+/-0.003). The mean (206)Pb/(207)Pb ratio, for one of the speleothems is 1.181+/-0.003 unvarying with time. These lead signatures are close to those of coal and old lead from northern European mines, lower than the natural background signature. It confirms that the high metal concentrations found come from anthropogenic pollution. Conversely, the lead isotopic composition of the second speleothem presents two temporal trends: for the oldest levels, the mean value (1.183+/-0.003) is similar to the first speleothem. For the youngest part, a lower value (1.172+/-0.005) is recorded, evidencing the contribution of a new lead source at the beginning of the industrial revolution. Pb isotopes were also measured in recent samples from a nearby superficial site. The first sample is a recent (AD 1975+/-15 years) deposit ((206)Pb/(207)Pb=1.148+/-0.003), and the second, a thin subactual layer ((206)Pb/(207)Pb=1.181+/-0.002). These data are compatible with the adding of anthropogenic sources (leaded gasoline and industrial lead from Rio Tinto ore).

Quantifying diet-borne metal uptake in Gammarus pulex using stable isotope tracers.

Gammarids are aquatic amphipods widely used for water quality monitoring. To investigate the copper and cadmium diet-borne metal uptake in Gammarus pulex, we adapted the pulse-chase stable isotopes-based approach to determine the food ingestion rate (IR), the gut retention time (GRT) and the metal assimilation efficiencies (AE). G. pulex were fed with (65)Cu-, (106)Cd-, and (53)Cr-labeled alder leaves for 7.5h and then with unlabeled leaves for 5d. The metal stable isotope contents in the gammarids, leaves, filtered water and periodically collected feces were determined. Chromium was poorly assimilated by the gammarids; thus, Cr was used as an unassimilated tracer. The first tracer defecation occurred before the first feces harvest, indicating a gut passage time of less than 9h. A 24-h GRT and a 0.69gg(-1)d(-1) IR were estimated. The Cd AE value was estimated as 5-47%, depending on the assimilation determination method applied. The Cu AE value could not be evaluated regardless of the determination method used, most likely because of the rapid Cu regulation in gammarids in addition to analytical uncertainties when determining the Cu content in leaves. Application of the Cd AE value in the framework of the biodynamic bioaccumulation model shows that the diet-borne uptake of Cd significantly contributes (66-95%) to the metal bioaccumulation in G. pulex fed with alder leaves.