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Assessing Migration of Uranium through Chalk Substrate: Field Study and Reactive Transport Modelling
2012
Crançon, Pierre | Mangeret, Arnaud | De Windt, Laurent
The migration of uranium from polluted soil has been investigated in the field, and through modelling of thermodynamics and kinetics of uranium-water-rock interactions. Field monitoring following surface contamination by uranium deposits revealed up to 5 m deep uranium migration in soil and chalk substrate, as well as uranium concentrations in groundwater significantly higher than the geochemical background. Such observations can hardly be explained by a pure reactive transport dominated by reversible adsorption of uranium onto mineral phases. Therefore, a reactive transport model using the HYTEC code has been developed to better assess uranium migration through soil to the carbonate aquifer. Reactive transport modelling shows that adsorption of U (VI) at equilibrium on goethite at pH 7 is responsible for strong immobilization of uranium in the soil and carbonate matrix, matching uranium concentration profiles observed in boreholes. Simulations considering highly mobile ternary complex Ca2UO2(CO3)3(aq) in the aqueous phase cannot account alone for the rapid migration of uranium through the unsaturated zone. Without a mobile colloidal phase, the model clearly underestimates the concentration of aqueous U(VI) that reached groundwater underneath polluted soils.
Afficher plus [+] Moins [-]Main properties and origins of winter PM10 pollution events in France | Caractéristiques et origines principales des épisodes de pollution hivernaux aux PM10 en France
2012
Favez, Olivier | Petit, Jean-Eudes | Bessagnet, Bertrand | Meleux, Frédérik | Chiappini, Laura | Lemeur, Sébastien | Labartette, Claire | Chappaz, Claire | Guergnion, Pierre-Yves | Saison, Jean-Yves | Chretien, Eve | Pallares, Cyril | Verlhac, Stéphane | Aujay, Robin | Malherbe, Laure | Beauchamp, Maxime | Piot, Christine | Jaffrezo, Jean-Luc | Besombes, Jean-Luc | Sciare, Jean | Rouil, Laurence | Leoz-Garziandia, Eva | Institut National de l'Environnement Industriel et des Risques (INERIS) | Laboratoire des Sciences du Climat et de l'Environnement [Gif-sur-Yvette] (LSCE) ; Université de Versailles Saint-Quentin-en-Yvelines (UVSQ)-Commissariat à l'énergie atomique et aux énergies alternatives (CEA)-Institut national des sciences de l'Univers (INSU - CNRS)-Université Paris-Saclay-Centre National de la Recherche Scientifique (CNRS) | Air Normand ; Air Normand | Association pour la Surveillance et l'Etude la Pollution Atmosphérique en Alsace ; Association pour la Surveillance et l'Etude la Pollution Atmosphérique en Alsace | Laboratoire de glaciologie et géophysique de l'environnement (LGGE) ; Observatoire des Sciences de l'Univers de Grenoble (OSUG) ; Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS) | Laboratoire de Chimie Moléculaire et Environnement (LCME) ; Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])
National audience | This paper aims at gaining an insight into the PM10 daily threshold (50 micro g/m3) exceedances measured by French regional air quality monitoring networks for the last four years. As almost three quarter of these exceedances happens to occur between November and April, we focus here on such winter (broadly speaking) pollution episodes. The deployment of monitoring devices allowing for a proper account of semi-volatile material within PM10 was achieved concomitantly to the development particulate pollution episodes largely influenced by ammonium nitrate (which is semi-volatile) in March-April 2007. Since then, such pollution events are frequently observed at this period of the year, notably due to stable meteorological conditions favoring the condensation of semi-volatile material into the particulate phase along with the resumption of manure spreading, which constitutes a major source of ammonium nitrate gaseous precursors (at least at some points of the year). Such pollution events, which are also related to combustion emissions (among which mobile sources) are typically preceded, from November to February, by frequent daily threshold exceedances with potentially significant influences of biomass burning (e.g. residential wood burning). The winter period is also impacted by long range transport episodes, corresponding notably to increases of ammonium sulfate relative abundances within PM10. Moreover, as traffic sites are generally the first ones showing PM10 exceedances due the increment of direct emissions and resuspension processes, mobile sources are also considered as a major target for action plans. Finally, it is underlined that the occurrence of daily threshold exceedances is highly influenced by meteorological conditions, so that the yearly number of these exceedances shows well-marked inter-annual variations, with 2009 and 2011 (and 2012, but not shown here) being significantly more polluted than 2008 and 2010. The on-going development of efficient forecasting systems still suffer lacks of detailed emission inventories and strong knowledge on the physical and chemical transformation processes of particles and their gaseous precursors within the boundary layer. | Cette synthèse dresse une analyse non exhaustive des dépassements du seuil réglementaire journalier de 50 micro g/m3 pour les PM10 mesurés au niveau national par les Associations Agréées de Surveillance de la Qualité de l'Air (AASQA) au cours des quatre dernières années. Près des trois quarts de ces dépassements étant observés entre fin novembre et début avril, nous nous intéressons plus particulièrement ici à ces épisodes hivernaux (au sens large). La mise en oeuvre de techniques analytiques permettant une prise en compte correcte des espèces semi-volatiles dans la composition des PM10 a coïncidé en mars-avril 2007 à la survenue de nombreux dépassements de seuil journalier s'accompagnant d'importants niveaux de nitrate d'ammonium (composé semi-volatil). Ce type d'épisode est régulièrement observé à cette période. Il s'explique notamment par la conjonction de conditions atmosphériques stables et propices à la condensation en phase particulaire des espèces labiles, et de la reprise des épandages agricoles, constituant une source majeure, au moins ponctuellement, de précurseurs gazeux azotés du nitrate d'ammonium. Ce type d'épisode, mettant également en cause les émissions anthropiques de combustion (dont les transports), est typiquement précédé entre novembre et février de fréquents dépassements pour lesquels le rôle des combustions de biomasse (incluant notamment le chauffage au bois individuel) peut être important. La période hivernale est également marquée par l'occurrence de phénomènes de transport longue distance se caractérisant par une augmentation des contributions du sulfate d'ammonium. Les sites de proximité automobile étant généralement les premiers concernés par les dépassements du seuil journalier en raison du surplus de concentrations provenant des émissions à l'échappement et des phénomènes de remise en suspension, le transport routier est également considéré comme un levier incontournable pour le respect des valeurs limites. Enfin, il est souligné que l'occurrence des différents types d'épisodes de dépassements dépend fortement des conditions météorologiques, de sorte qu'on observe une forte variabilité interannuelle du nombre de dépassements hivernaux ? : 2009 et 2011 (et 2012) étant significativement plus impactées que 2008 et 2010. Une bonne prévision de ces épisodes passe encore par l'affinage des cadastres d'émission et une meilleure compréhension du devenir dans l'atmosphère des émissions primaires (gazeuses et particulaires).
Afficher plus [+] Moins [-]Chemical analysis of atmospheric PM and improvment of the knowledge on emissions sources | L'apport des méthodes d'analyses chimiques des PM pour la connaissance des sources d'émission
2012
Jaffrezo, Jean-Luc | Piot, Christine | Besombes, Jean-Luc | Marchand, Nicolas | El Haddad, I. | Favez, Olivier | Brulfert, G. | Laboratoire de glaciologie et géophysique de l'environnement (LGGE) ; Observatoire des Sciences de l'Univers de Grenoble (OSUG) ; Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Centre National de la Recherche Scientifique (CNRS) | Laboratoire de Chimie Moléculaire et Environnement (LCME) ; Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry]) | Laboratoire Chimie de l'environnement (LCE) ; Aix Marseille Université (AMU)-Institut de Chimie du CNRS (INC)-Centre National de la Recherche Scientifique (CNRS) | Institut National de l'Environnement Industriel et des Risques (INERIS)
National audience
Afficher plus [+] Moins [-]Occurrence and removal of benzotriazoles and ultraviolet filters in a municipal wastewater treatment plant
2012
Liu, You-Sheng | Ying, Guang-Guo | Shareef, Ali | Kookana, Rai S.
We investigated the occurrence and removal of four benzotriazoles (BTs) (benzotriazole: BT; 5-methyl-benzotriazole: 5-TTri; 5-chloro-benzotriazole: CBT; 5,6-dimethyl-benzotriazole: XTri) and six UV filters (benzophenone-3: BP-3; 3-(4-methylbenzylidene)camphor: 4-MBC; octyl 4-methoxycinnamate: OMC; 2-(3-t-butyl-2-hydroxy-5-methylphenyl)-5-chloro benzotriazole: UV-326; 2-(2′-Hydroxy-5′-octylphenyl)-benzotriazole: UV-329; octocrylene: OC) in a full scale municipal wastewater treatment in South Australia. BT, 5-TTri and BP-3 were found as the dominant compounds detected in the wastewater samples with average concentrations up to 5706 ± 928 ng/L, 6758 ± 1438 ng/L and 2086 ± 1027 ng/L in influent, and up to 2439 ± 233 ng/L, 610 ± 237 ng/L and 153 ± 121 ng/L in effluent, respectively. In the biosolid, 4-MBC and OC were found with the highest concentrations of 962 ± 135 ng/g and 465 ± 65 ng/g, respectively. Sorption onto sludge played a dominant role in the removal for UV filters, especially for 4-MBC, UV-326 and OC, which accounted for 54%–92% of influent loads, while biological degradation played a significant role for the other compounds.
Afficher plus [+] Moins [-]Phytochelatins play a key role in arsenic accumulation and tolerance in the aquatic macrophyte Wolffia globosa
2012
Zhang, Xin | Uroic, M Kalle | Xie, Wan-Ying | Zhu, Yong-Guan | Chen, Bao-Dong | McGrath, Steve P. | Feldmann, Jörg | Zhao, Fang-Jie
The rootless duckweed Wolffia globosa can accumulate and tolerate relatively large amounts of arsenic (As); however, the underlying mechanisms were unknown. W. globosa was exposed to different concentrations of arsenate with or without l-buthionine sulphoximine (BSO), a specific inhibitor of γ-glutamylcysteine synthetase. Free thiol compounds and As(III)–thiol complexes were identified and quantified using HPLC – high resolution ICP-MS – accurate mass ESI-MS. Without BSO, 74% of the As accumulated in the duckweed was complexed with phytochelatins (PCs), with As(III)–PC₄ and As(III)–PC₃ being the main species. BSO was taken up by the duckweed and partly deaminated. The BSO treatment completely suppressed the synthesis of PCs and the formation of As(III)–PC complexes, and also inhibited the reduction of arsenate to arsenite. BSO markedly decreased both As accumulation and As tolerance in W. globosa. The results demonstrate an important role of PCs in detoxifying As and enabling As accumulation in W. globosa.
Afficher plus [+] Moins [-]Application of XAD-resin based passive air samplers to assess local (roadside) and regional patterns of persistent organic pollutants
2012
Barthel, Paul | Thuens, Sabine | Shunthirasingham, Chubashini | Westgate, John N. | Wania, Frank | Radke, Michael
We used XAD-resin based passive air samplers (PAS) to measure atmospheric levels of polycyclic aromatic hydrocarbons (PAHs) and polychlorinated biphenyls (PCBs) at five ombrotrophic bogs in Eastern Canada. The aims of our study were to investigate the influence of local roads on contaminant levels in the bogs, to derive the regional pattern of atmospheric concentrations, and to assess the uncertainties of the method. Expanded uncertainties based on the duplicate PAS deployed at 24 sites were good for the PAHs, while the deployment period of approx. 100 days was too short to yield acceptable uncertainties for PCBs. The regional PAH distribution was in good agreement with the calculated source proximity of the sampled bogs. We conclude that XAD-resin based PAS deployed for comparatively short periods are well suited for measuring atmospheric concentrations of volatile PAHs, while in remote regions longer deployment is necessary for less volatile PAHs and for PCBs.
Afficher plus [+] Moins [-]High bacterial biodiversity increases degradation performance of hydrocarbons during bioremediation of contaminated harbor marine sediments
2012
Dell'Anno, Antonio | Beolchini, Francesca | Rocchetti, Laura | Luna, Gian Marco | Danovaro, Roberto
We investigated changes of bacterial abundance and biodiversity during bioremediation experiments carried out on oxic and anoxic marine harbor sediments contaminated with hydrocarbons. Oxic sediments, supplied with inorganic nutrients, were incubated in aerobic conditions at 20 °C and 35 °C for 30 days, whereas anoxic sediments, amended with organic substrates, were incubated in anaerobic conditions at the same temperatures for 60 days. Results reported here indicate that temperature exerted the main effect on bacterial abundance, diversity and assemblage composition. At higher temperature bacterial diversity and evenness increased significantly in aerobic conditions, whilst decreased in anaerobic conditions. In both aerobic and anaerobic conditions, biodegradation efficiencies of hydrocarbons were significantly and positively related with bacterial richness and evenness. Overall results presented here suggest that bioremediation strategies, which can sustain high levels of bacterial diversity rather than the selection of specific taxa, may significantly increase the efficiency of hydrocarbon degradation in contaminated marine sediments.
Afficher plus [+] Moins [-]Polybrominated diphenyl ethers and decabromodiphenylethane in sediments from twelve lakes in China
2012
Wu, Fengchang | Guo, Jianyang | Chang, Hong | Liao, Haiqing | Zhao, Xiaoli | Mai, Bixian | Xing, Baoshan
Sediment cores from 12 Chinese lakes were analyzed to investigate the historical inputs of polybrominated diphenyl ethers (PBDEs) and decabromodiphenylethane (DBDPE) during the past few decades. Concentrations of ΣPBDE₁ (sum of tri- to hepta-BDEs), ΣPBDE₂ (sum of nona- to deca-BDEs) and DBDPE in the surface sediments were 0.02–0.29 ng g⁻¹, 0.46–46.6 ng g⁻¹ and 1.02–3.64 ng g⁻¹, respectively. The temporal trends of PBDEs and DBDPE followed a general increase from the bottom to the surface. The calculated fluxes for ΣPBDE₁, ΣPBDE₂ and DBDPE were 0.001–0.09, 0.03–4.24, and 0.05–0.31 ng cm⁻² yr⁻¹, and the inventories were 0.09–7.86, 0.91–461, and 3.83–24.6 ng cm⁻², respectively. The urbanization and industrialization are highly related to the contamination of PBDEs and DBDPE in sediments. The DBDPE input in recent years was still lower than ΣPBDE₂ but the temporal trends indicated that the contamination would increase with the increasing usage of DBDPE in the future.
Afficher plus [+] Moins [-]Nitrate leaching, direct and indirect nitrous oxide fluxes from sloping cropland in the purple soil area, southwestern China
2012
Zhou, Minghua | Zhu, Bo | Butterbach-Bahl, Klaus | Wang, Tao | Bergmann, Jessica | Brüggemann, Nicolas | Wang, Zhenhua | Li, Taikui | Kuang, Fuhong
This study provides a combined dataset on N loss pathways and fluxes from sloping cropland in the purple soil area, southwestern China. A lysimeter experiment was conducted to quantify nitrate leaching (May 2004–May 2010) and N₂O emission (May 2009–May 2010) losses. Nitrate leaching was the dominant N loss pathway and annual leaching fluxes ranged from 19.2 to 53.4 kg N ha⁻¹, with significant differences between individual observation years (P < 0.05). Direct N₂O emissions due to N fertilizer use were 1.72 ± 0.34 kg N ha⁻¹ yr⁻¹, which corresponds to an emission factor of 0.58 ± 0.12%. However, indirect N₂O emissions caused by nitrate leaching and surface runoff N losses, may contribute another 0.15–0.42 kg N ha⁻¹ yr⁻¹. Our study shows that nitrate leaching lowered direct N₂O emissions, highlighting the importance for a better understanding of the tradeoff between direct and indirect N₂O emissions for the development of meaningful N₂O emission strategies.
Afficher plus [+] Moins [-]Effects of silicon on the distribution of cadmium compartmentation in root tips of Kandelia obovata (S., L.) Yong
2012
Ye, Juan | Yan, Chongling | Liu, Jingchun | Lu, Haoliang | Liu, Tao | Song, Zengfeng
The Effects of silicon (Si) on the distribution of cadmium (Cd) compartmentation in root tips of Kandelia obovata (S., L.) Yong were investigated by pot experiments. Cd concentrations in the apoplastic saps and symplastic fractions of the root tips of K. obovata seedlings were decreased at both Si-supplied treatments. Si addition reduced the concentrations of BaCl₂₋extractable cell-wall-Cd in root tips, but increased the concentrations of Na₃citrate-extractable cell-wall-Cd and HCl-extractable cell-wall-Cd in root tips. The total root-tip contents of Cd were mainly distributed in the apoplast and most of the Cd in the apoplast was bound to the cell wall. Our experiment found that Si increased the ratio of apoplast Cd (>87.08%) and reduced the ratio of Cd in the symplast (<12.92%). This suggested that Si enhanced binding of Cd to the cell walls and restricted the apoplastic transport of Cd.
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