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Contrasted fate of zinc sulfide nanoparticles in soil revealed by a combination of X-ray absorption spectroscopy, diffusive gradient in thin films and isotope tracing
2022
Le Bars, Maureen | Legros, Samuel | Levard, Clément | Chevassus-Rosset, Claire | Montes, Mélanie | Tella, Marie | Borschneck, Daniel | Guihou, Abel | Angeletti, Bernard | Doelsch, Emmanuel
Incidental zinc sulfide nanoparticles (nano-ZnS) are spread on soils through organic waste (OW) recycling. Here we performed soil incubations with synthetic nano-ZnS (3 nm crystallite size), representative of the form found in OW. We used an original set of techniques to reveal the fate of nano-ZnS in two soils with different properties. 68Zn tracing and nano-DGT were combined during soil incubation to discriminate the available natural Zn from the soil, and the available Zn from the dissolved nano-68ZnS. This combination was crucial to highlight the dissolution of nano-68ZnS as of the third day of incubation. Based on the extended X-ray absorption fine structure, we revealed faster dissolution of nano-ZnS in clayey soil (82% within 1 month) than in sandy soil (2% within 1 month). However, the nano-DGT results showed limited availability of Zn released by nano-ZnS dissolution after 1 month in the clayey soil compared with the sandy soil. These results highlighted: (i) the key role of soil properties for nano-ZnS fate, and (ii) fast dissolution of nano-ZnS in clayey soil. Finally, the higher availability of Zn in the sandy soil despite the lower nano-ZnS dissolution rate is counterintuitive. This study demonstrated that, in addition to nanoparticle dissolution, it is also essential to take the availability of released ions into account when studying the fate of nanoparticles in soil.
Show more [+] Less [-]Long-term pollution by chlordecone of tropical volcanic soils in the French West Indies: New insights and improvement of previous predictions
2022
Comte, Irina | Pradel, Alice | Grabit, Armand | Mottes, Charles | Pak, Lai-Ting | Cattan, Philippe
Chlordecone (CLD), was widely applied in banana fields in the French West Indies from 1972 to 1993. The WISORCH model was constructed to assess soil contamination by CLD and estimated that it lasts from 100 to 600 years, depending on leaching intensity and assuming no degradation. However, recent studies demonstrated that CLD is degraded in the environment, hence questioning the reliability of previous estimations. This paper shows how to improve the model and provides insights into the long-term dissipation of CLD. In-situ observations were made in nearly 2545 plots between 2001 and 2020, and 17 plots were sampled at two dates. Results of soil analyses showed an unexpected 4-fold decrease in CLD concentrations in the soil, in contrast to simulations made using the first version of WISORCH at the time. Neither erosion, nor CLD leaching explained these discrepancies. In a top-down modeling approach, these new observations of CLD concentrations led us to implement a new dissipation process in the WISORCH model that corresponds to a DT50 dissipation half-life of 5 years. The new version of the improved model allowed us to update the prediction of the persistence of soil pollution, with soil decontamination estimated for the 2070s. This development calls for re-evaluation of soil pollution status. Further validation of the new version of WISORCH is needed so it can contribute to crop management on contaminated soil.
Show more [+] Less [-]Analysis of surface water reveals land pesticide contamination: An application for the determination of chlordecone-polluted areas in Guadeloupe, French West Indies
2020
Rochette, Romain | Bonnal, Vincent | Andrieux, Patrick | Cattan, Philippe
In Guadeloupe, the use between 1972 and 1993 of chlordecone, an organochlorine insecticide, has permanently contaminated the island's soil, thus contaminating the food chain at its very beginning. There is today a strong societal requirement for an improved mapping of the contaminated zones. Given the extent of the areas to be covered, carrying out soil tests on each plot of the territory would be a long and expensive process. In this article, we explore a method of demarcating polluted areas. The approach adopted consists in carrying out, using surface water analyses, a hydrological delimitation that makes it possible to distinguish contaminated watersheds from uncontaminated ones. The selection of sampling points was based on the spatial analysis of the actual and potential contamination data existing at the beginning of the study. The approach was validated by soil analyses, after having compared the contamination data of the watersheds with the soil contamination data of the plots within them. The study thus made it possible to highlight new contaminated areas and also those at risk of contamination and to identify the plots to be targeted as a priority during future analysis campaigns by State services.
Show more [+] Less [-]Assessing ecotoxicity and uptake of metals and metalloids in relation to two different earthworm species (Eiseina horterzsis and Lumbricus terrestris)
2013
Leveque , Thibaut (Université de ToulouseEcolab Laboratoire d'écologie fonctionnelle, Castanet-Tolosan31326 Castanet-Tolosan (France). INP-ENSATUMR 5245 CNRS-INP-UPS) | Capowiez , Yvan (INRA , Avignon (France). UR 1115 Unité de recherche Plantes et Systèmes de Culture Horticoles) | Schreck , Eva (Géosciences Environnement Toulouse, Toulouse(France). UMR 5563 CNRS/UPS/IRD/CNES) | Mazzia , Christophe (Institut Méditerranéen de Biodiversité et d'Écologie Marine et Continentale(France). UMR CNRS 7263) | Auffan , Mélanie (Centre Européen de Recherche et d'Enseignement des Géosciences de l'Environnement, Aix-en-Provence(France). Europôle méditerranéen de l’Arbois) | Foucault , Yann (Université de ToulouseEcolab Laboratoire d'écologie fonctionnelleSociété de Traitement Chimique des Métaux, Castanet-Tolosan31326 Castanet-Tolosan Toulouse(France). INP-ENSATUMR 5245 CNRS-INP-UPS) | Austruy , Annabelle (Université de ToulouseEcolab Laboratoire d'écologie fonctionnelle, Castanet-Tolosan31326 Castanet-Tolosan (France). INP-ENSATUMR 5245 CNRS-INP-UPS) | Dumat , Camille (auteur de correspondance) (Université de ToulouseEcolab Laboratoire d'écologie fonctionnelle, Castanet-Tolosan31326 Castanet-Tolosan (France). INP-ENSATUMR 5245 CNRS-INP-UPS)
Due to diffuse atmospheric fallouts of process particles enriched by metals and metalloids, polluted soils concern large areas at the global scale. Useful tools to assess ecotoxicity induced by these polluted soils are therefore needed. Earthworms are currently used as biotest, however the influence of specie and earthworm behaviour, soil characteristics are poorly highlighted. Our aim was therefore to assess the toxicity of various polluted soils with process particles enriches by metals and metalloids (Pb, Cd, Cu, Zn, As and Sb) collected from a lead recycling facility on two earthworm species belonging to different ecological types and thus likely to have contrasted behavioural responses (Eiseina hortensis and Lumbricus terrestris). The combination of behavioural factors measurements (cast production and biomass) and physicochemical parameters such as metal absorption, bioaccumulation by earthworms and their localization in invertebrate tissues provided a valuable indication of pollutant bioavailability and ecotoxicity. Soil characteristics influenced ecotoxicity and metal uptake by earthworms, as well as their soil bioturbation.
Show more [+] Less [-]Using a two site-reactive model for simulating one century changes of Zn and Pb concentration profiles in soils affected by metallurgical fallout
2012
Mallmann , Fábio Joel Kochem (Universidade Federal de Santa Maria, Santa Maria(Brésil). Departamento de Solos) | Rheinheimer , Danilo dos Santos (Universidade Federal de Santa Maria, Santa Maria(Brésil). Departamento de Solos) | Labanowski , Jérôme (Centre National de la Recherche Scientifique, Poitiers(France). UMR 6008, LCME, Université de Poitiers-ESIP) | Cambier , Philippe (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Lamy , Isabelle (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Santanna , Maria Alice (Universidade Federal de Santa Maria, Santa Maria(Brésil). Departamento de Física) | Tessier , Daniel (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Van Oort , Folkert (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés)
Predicting the transfer of contaminants in soils is often hampered by lacking validation of mathematical models. Here, we applied Hydrus-2D software to three agricultural soils for simulating the 1900–2005 changes of zinc and lead concentration profiles derived from industrial atmospheric deposition, to validate the tested models with plausible assumptions on past metal inputs to reach the 2005 situation. The models were set with data from previous studies on the geochemical background, estimated temporal metal deposition, and the 2005 metal distributions. Different hypotheses of chemical reactions of metals with the soil solution were examined: 100% equilibrium or partial equilibrium, parameterized following kinetic chemical extractions. Finally, a two-site model with kinetic constant values adjusted at 1% of EDTA extraction parameters satisfactory predicted changes in metal concentration profiles for two arable soils. For a grassland soil however, this model showed limited applicability by ignoring the role of earthworm activity in metal incorporation.
Show more [+] Less [-]Long-term pollution by chlordecone of tropical volcanic soils in the French West Indies: A simple leaching model accounts for current residue
2009
Cabidoche , Yves-Marie (INRA , Petit-Bourg (France). UR 0135 Unité de Recherche AgroPédoClimatique de la zone caraïbe) | Achard , Raphaël (Centre de Coopération Internationale en Recherche Agronomique pour le DéveloppementPôle de Recherche Agro-Environnementale de la Martinique, Le LamentinLe Lamentin(France). UPR Systemes Bananes et Ananas) | Cattan , Philippe (Centre de Coopération Internationale en Recherche Agronomique pour le Développement, Capesterre-Belle-Eau(France). UPR Systèmes Bananes et Ananas (Guadeloupe)) | Clermont-Dauphin , Claridge (INRA , Petit-Bourg (France). UR 0135 Unité de Recherche AgroPédoClimatique de la zone caraïbe) | Massat , Félix (Laboratoire Départemental d’Analyses de la Drôme, Valence(France).) | Sansoulet , Julie (INRA , Petit-Bourg (France). UR 0135 Unité de Recherche AgroPédoClimatique de la zone caraïbe)
Chlordecone was applied between 1972 and 1993 in banana fields of the French West Indies. This resulted in long-term pollution of soils and contamination of waters, aquatic biota, and crops. To assess pollution level and duration according to soil type, WISORCH, a leaching model based on first-order desorption kinetics, was developed and run. Its input parameters are soil organic carbon content (SOC) and SOC/water partitioning coefficient (Koc). It accounts for current chlordecone soil contents and drainage water concentrations. The model was valid for andosol, which indicates that neither physicochemical nor microbial degradation occurred. Dilution by previous deep tillages makes soil scrapping unrealistic.Lixiviation appeared the main way to reduce pollution. Besides the SOC and rainfall increases, Koc increased from nitisol to ferralsol and then andosol while lixiviation efficiency decreased. Consequently, pollution is bound to last for several decades for nitisol, centuries for ferralsol, and half a millennium for andosol.
Show more [+] Less [-]Kinetic extractions to assess mobilization of Zn, Pb, Cu, and Cd in a metal-contaminated soil: EDTA vs. citrate.
2008
Labanowski , Jérome (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Monna , Fabrice (Centre National de la Recherche Scientifique, Dijon(France). Univ. de Bourgogne Centre des Sciences de la Terre) | Bermond , Alain (INRA , Thiverval-Grignon (France). UMR 1091 Environnement et Grandes Cultures) | Cambier , Philippe (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Fernandez , Christelle (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Lamy , Isabelle (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Van Oort , Folkert (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés)
Kinetic EDTA and citrate extractions were used to mimic metal mobilization in a soil contaminated by metallurgical fallout. Modeling of metal removal rates vs. time distinguished two metal pools: readily labile (QM1) and less labile (QM2). In citrate extractions, total extractability (QM1 + QM2) of Zn and Cd was proportionally higher than for Pb and Cu. Proportions of Pb and Cu extracted with EDTA were three times higher than when using citrate. We observed similar QM1/QM2 ratios for Zn and Cu regardless of the extractant, suggesting comparable binding energies to soil constituents. However, for Pb and Cd, more heterogeneous binding energies were hypothesized to explain different kinetic extraction behaviors. Proportions of citrate-labile metals were found consistent with their short-term, in-situ mobility assessed in the studied soil, i.e., metal amount released in the soil solution or extracted by cultivated plants. Kinetic EDTA extractions were hypothesized to be more predictive for long-term metal migration with depth.
Show more [+] Less [-]Anthropogenic lead distribution in soils under arable land and permanent grassland estimated by Pb isotopic compositions
2008
Fernandez , Christelle (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Monna , Fabrice (Centre National de la Recherche Scientifique, Dijon(France). Centre des Sciences de la Terre) | Labanowski , Jérome (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés) | Loubet , Michel (Université Toulouse 3, Toulouse(France). Laboratoire de Géochimie) | Van Oort , Folkert (INRA , Versailles (France). UR 0251 Physico-chimie et Ecotoxicologie des Sols d'agrosystèmes contaminés)
The role of land use on fate of metals in soils is poorly understood. In this work, we studied the incorporation of lead in two neighboring soils with comparable pedogenesis but under long-term different agricultural management. Distributions of anthropogenic Pb were assessed from concentrations and isotopic compositions determined on bulk horizon samples, systematical 5–10 cm increment samples, and on 24-h EDTA extracts. Minor amounts of anthropogenic lead were detected until 1-m depth under permanent grassland, linked to high earthworm activity. In arable land, exogenous Pb predominantly accumulated at depths <60 cm. Although the proximity between the two sites ensured comparable exposition regarding atmospheric Pb deposition, the isotopic compositions clearly showed the influence of an unidentified component for the cultivated soil. This work highlights the need for exhaustive information on historical human activities in such anthropized agrosystems when fate of metal pollution is considered.
Show more [+] Less [-]The pesticide chlordecone is trapped in the tortuous mesoporosity of allophane clays
2018
Woignier, Thierry | Clostre, Florence | Fernandes, Paula | Soler, Alain | Rangon, Luc | Sastre-Conde, Maria Isabel | Jannoyer-Lesueur, Magalie
Some volcanic soils like andosols contain short-range order nanoclays (allophane) which build aggregates with a tortuous and fractal microstructure. The aim of the work was to study the influence of the microstructure and mesoporosity of the allophane aggregates on the pesticide chlordecone retention in soils. Our study shows that the allophane microstructure favors pollutants accumulation and sequestration in soils. We put forth the importance of the mesoporous microstructure of the allophane aggregates for pollutant trapping in andosols. We show that the soil contamination increases with the allophane content but also with the mesopore volume, the tortuosity, and the size of the fractal aggregate. Moreover, the pore structure of the allophane aggregates at nanoscale favors the pesticide retention. The fractal and tortuous aggregates of nanoparticles play the role of nanolabyrinths. It is suggested that chlordecone storage in allophanic soils could be the result of the low transport properties (permeability and diffusion) in the allophane aggregates. The poor accessibility to the pesticide trapped in the mesopore of allophane aggregates could explain the lower pollutant release in the environment. (Résumé d'auteur)
Show more [+] Less [-]Competitive sorption of heavy metal by soils. Isotherms and fractional factorial experiments
1998
Echevarria, Guillaume | Morera, M.T. | Mazkiaran, C. | Garrido, J.J. | Laboratoire Sols et Environnement (LSE) ; Institut National de la Recherche Agronomique (INRA)-Université de Lorraine (UL) | Universidad Pública de Navarra [Espagne] = Public University of Navarra (UPNA)
Competing ions strongly affect heavy metal sorption onto the solid surfaces of soil. This study evaluated competitive sorption of Cd, Cu, Ni, Pb and Zn on three soils: Calcixerollic Xerochrept, Paralithic Xerorthent and Lithic Haplumbrept. Monometal and competitive sorption isotherms were obtained at 25°C. The individual effect of ions on retention of the others was ascertained by a fractional factorial analysis design. Most of the sorption isotherms belonged to type L subtype 2 in the classification of Giles. In competitive sorption the initial linear part was shorter and the knee sharper when compared with monometal sorption isotherms. Parameters related to sorptive capacity, such as Point B, Langmuir monolayer and Freundlich distribution coefficient, were higher in monometal than in competitive sorption, and in basic soils than in acidic soil. Calcium desorbed at different points of the sorption isotherms indicated that cationic exchange with Ca was the main retention mechanism in calcareous soils. For Pb, the ratio Ca desorbed/Pb sorbed was close to one; for Cu, Ni and Zn the ratio ranged from 1.20 to 1.37, probably due to partial dissolution of calcium carbonates by hydrolytic processes during retention. On the other hand, Cd had a ratio around 0.6 reflecting another additional retention mechanism, probably surface complexation. Fractional factorial design confirmed that the presence of the cations investigated reduced the amount of the five metals retained, but the presence of Cu and Pb in the system depressed Ni, Cd and Zn sorption more than the inverse. Cation mobility was enhanced when equilibrium concentration increased and the effect was higher in Ca-saturated soils.
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