The legacy of metallurgical atmospheric contamination in a mountainous catchment: A delayed response of Pb contamination.

Metal-rich fumes emitted during ore smelting contribute to widespread anthropogenic contamination. Environmental archives (such as lake sediments) record fallouts deposited on lake and terrestrial surfaces during ancient mining and smelting activities. However, very few is known about the potential buffering effect of soils upon which metal falls out, prior to be released through runoff and or/erosion, hence leading to pervasive contamination fluxes long after the ceasing of metallurgical activities. Here we aim at assessing this long-term remobilisation in a mountainous catchment area. Lake sediments and soils were collected 7 km upward a 200-year-old historic mine. The PbAg mine of Peisey-Nancroix was operated between the 17th and the 19th centuries with a documented smelting period of 80 years. In lake sediments, the total Pb content varies from 29 mg.kg-1 prior smelting to 148 mg.kg-1 during ore smelting. Pb isotopes in lake sediments and soils provide evidence of anthropogenic Pb from the local ore (206Pb/207Pb = 1.173; 208Pb/206Pb = 2.094) during and after smelting, suggesting anthropogenic Pb remobilisation for 200 years. The accumulation rates of anthropogenic Pb calculated in lake sediments after the smelting period confirm such a remobilisation. Despite a decrease in this accumulation rate through time, soils still contain significant stocks of anthropogenic Pb (54-89 % of PbANTH). The distribution of present-day anthropogenic Pb in the catchment area depends mainly on topographic characteristics. Coupling lake sediments and soils investigations is thus necessary to constrain the long-term persistence and remobilisation of a diffuse contamination related to mining activities.

Climate-driven fluxes of organic-bound uranium to an alpine lake over the Holocene.

Uranium (U) isotopic signatures and concentration in sediments are widely used as paleo-redox proxies, as the behavior of U is often controlled by bottom water oxygenation. Here, we investigated the processes controlling U accumulation in the sediments of Lake Nègre (Mediterranean Alps, South-East France) over the past 9200 years. Exceptionally high natural U concentrations (350-1250 µg·g-1) allowed the measurement of U along with other elements by high-resolution X-Ray Fluorescence core-scanning. Weathering and erosion proxies (Ti content, Zr/Al and K/Ti ratios) indicate that sedimentary inputs were controlled by Holocene climatic variations. After a period of low erosion during the Holocene Climatic Optimum, a major regime shift was recorded at 4.2 kyr BP when terrigenous fluxes consistently increased until present with high sensitivity to centennial-scale climatic events. Sedimentary organic matter (OM) inputs were dominated by terrigenous OM from the catchment soils until 2.4 kyr BP, as attested by carbon to nitrogen (C/N) and bromine to organic carbon (Br/TOC) ratios. From 2.4 kyr BP to present, lake primary production and soils equally contributed to sedimentary OM. Uranium fluxes to the sediments were well correlated to terrigenous OM fluxes from 7 kyr BP to present, showing that U supply to the lake was controlled by U scavenging in the soils of the watershed followed by transport of U bound to detrital organic particles. Higher U/OM ratios before 7 kyr BP likely reflect the development of the upstream wetland. The fluctuations of U sedimentary inputs appear to be independent of bottom water oxygenation, as estimated from constant Fe/Mn ratios and δ238U isotopic signatures, and rather controlled by the production, erosion and sedimentation of terrigenous OM. This finding confirms that the use of U (and potentially other metals with high affinity to OM) concentrations alone should be used with caution for paleo-redox reconstructions.

Evidence of Chlordecone Resurrection by Glyphosate in French West Indies.

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.

Flux estimation, temporal trends and source determination of trace metal contamination in a major tributary of the Seine estuary, France.

Anthropogenic impacts on rivers have increased significantly over the past ~150 years, particularly at the beginning of the industrial revolution. Among other signs, this impact is manifested through the addition of trace metals and metalloid elements to rivers. The Eure River watershed in France covers an area of 6017 km2 and is a major tributary of the Seine estuary. It is not exempt from anthropogenic pressures and has been exposed to significant metal discharges over the last 80 years. The average concentrations of metals (i.e., Cr, Co, Ni, Cu, Zn, Ag, Cd, Sb, and Pb), in suspended particulate matter currently transported by the river are high compared to the local geochemical background. Moreover, the lack of correlation between concentration variations and the hydrosedimentary behaviour of the Eure River suggests that the river is currently under anthropogenic pressure. Analysis of sediment cores indicate strong As contamination during the 1940s, Cr, Co, Ni, Cu, Zn, Ag, and Cd contamination during the 1960s and 1970s, and Sb and Pb contamination during the 1990s and 2000s. The enrichment factors calculation suggests that total anthropogenic pressure within the Eure River watershed since the 1940s was comparable or higher than those in many other French watersheds. An estimation of particulate metal flux in 2017 shows that the Eure River watershed contributed to 7, 8, 9, 10 and 16% of total inputs to the Seine estuary in Cr, Cu, Zn, Cd and Pb respectively. Moreover, the estimation of past theoretical flux indicates that during the 1990s the Eure River watershed was the main contributor of particulate Pb to the estuary. The use of Pb isotopes has revealed that this contamination was primarily of industrial origin.

When archives are missing, deciphering the effects of public policies and climate variability on the Brazilian semi-arid region using sediment core studies.

The northeastern region of Brazil is the most densely populated and biodiverse semi-arid regions of the planet. Effects of the natural climate variability and colonization on the landscape have been described since the beginning of the 16th century but little is known about their effects on natural resources. Climate projections predict temperatures above 40 °C and an increase in the number and duration of droughts at the end of the 21st century with strong societal impacts. Here, we analyze the influence of public policies, human activities and natural climate variability on the environment over the last 60 years. Our study is based on sedimentological and environmental reconstructions from two sediment cores collected in two dam lakes on the river Acaraú in the State of Ceará. Multiproxy analyses of both cores (inorganic geochemistry, pollen, charcoal, remote sensing) at an annual resolution showed that 1) at interannual scale composition and distribution of the dry forest (known as Caatinga) were not affected by the alternance of drought and high moisture episodes; 2) at decadal scale human activities such as agriculture were reflected by changes in vegetation cover and fishery by progressive changes in lake trophic status; 3) public policies were able to promote changes in the landscape e.g., land colonization with the regression of the dry forest and irrigation plan able to amplify the deforestation and change the floristic composition. Thanks to paleo-science approach, our environmental diagnosis should help future decision-making and provide guidelines for preservation of resources and wellbeing of the inhabitants.

Long-term dynamics in microbial eukaryotes communities: a palaeolimnological view based on sedimentary DNA.

Assessing the extent to which changes in lacustrine biodiversity are affected by anthropogenic or climatic forces requires extensive palaeolimnological data. We used high-throughput sequencing to generate time-series data encompassing over 2200 years of microbial eukaryotes (protists and Fungi) diversity changes from the sedimentary DNA record of two lakes (Lake Bourget in French Alps and Lake Igaliku in Greenland). From 176 samples, we sequenced a large diversity of microbial eukaryotes, with a total 16 386 operational taxonomic units distributed within 50 phylogenetic groups. Thus, microbial groups, such as Chlorophyta, Dinophyceae, Haptophyceae and Ciliophora, that were not previously considered in lacustrine sediment record analyses appeared to be potential biological markers of trophic status changes. Our data suggest that shifts in relative abundance of extant species, including shifts between rare and abundant taxa, drive ecosystem responses to local and global environmental changes. Community structure shift events were concomitant with major climate variations (more particularly in Lake Igaliku). However, this study shows that the impacts of climatic fluctuations may be overpassed by the high-magnitude eutrophication impacts, as observed in the eutrophicated Lake Bourget. Overall, our data show that DNA preserved in sediment constitutes a precious archive of information on past biodiversity changes.

Long-term relationships among pesticide applications, mobility, and soil erosion in a vineyard watershed.

Agricultural pesticide use has increased worldwide during the last several decades, but the long-term fate, storage, and transfer dynamics of pesticides in a changing environment are poorly understood. Many pesticides have been progressively banned, but in numerous cases, these molecules are stable and may persist in soils, sediments, and ice. Many studies have addressed the question of their possible remobilization as a result of global change. In this article, we present a retro-observation approach based on lake sediment records to monitor micropollutants and to evaluate the long-term succession and diffuse transfer of herbicides, fungicides, and insecticide treatments in a vineyard catchment in France. The sediment allows for a reliable reconstruction of past pesticide use through time, validated by the historical introduction, use, and banning of these organic and inorganic pesticides in local vineyards. Our results also revealed how changes in these practices affect storage conditions and, consequently, the pesticides' transfer dynamics. For example, the use of postemergence herbicides (glyphosate), which induce an increase in soil erosion, led to a release of a banned remnant pesticide (dichlorodiphenyltrichloroethane, DDT), which had been previously stored in vineyard soil, back into the environment. Management strategies of ecotoxicological risk would be well served by recognition of the diversity of compounds stored in various environmental sinks, such as agriculture soil, and their capability to become sources when environmental conditions change.