1. |
- Bouchet, Sylvain, et al.
(författare)
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Mercury sources and fate in a large brackish ecosystem (the Baltic Sea) depicted by stable isotopes
- 2023
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 57:38, s. 14340-14350
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Tidskriftsartikel (refereegranskat)abstract
- Identifying Hg sources to aquatic ecosystems and processes controlling the levels of monomethylmercury (MMHg) is critical for developing efficient policies of Hg emissions reduction. Here we measured Hg concentrations and stable isotopes in sediment, seston, and fishes from the various basins of the Baltic Sea, a large brackish ecosystem presenting extensive gradients in salinity, redox conditions, dissolved organic matter (DOM) composition, and biological activities. We found that Hg mass dependent fractionation (Hg-MDF) values in sediments mostly reflect a mixing between light terrestrial Hg and heavier industrial sources, whereas odd Hg isotope mass independent fractionation (odd Hg-MIF) reveals atmospheric inputs. Seston presents intermediate Hg-MDF and odd Hg-MIF values falling between sediments and fish, but in northern basins, high even Hg-MIF values suggest the preferential accumulation of wet-deposited Hg. Odd Hg-MIF values in fish indicate an overall low extent of MMHg photodegradation due to limited sunlight exposure and penetration but also reveal large spatial differences. The photodegradation extent is lowest in the central basin with recurrent algal blooms due to their shading effect and is highest in the northern, least saline basin with high concentrations of terrestrial DOM. As increased loads of terrestrial DOM are expected in many coastal areas due to global changes, its impact on MMHg photodegradation needs to be better understood and accounted for when predicting future MMHg concentrations in aquatic ecosystems.
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2. |
- Bravo, Andrea Garcia, et al.
(författare)
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Cleaning and sampling protocol for analysis of mercury and dissolved organic matter in freshwater systems
- 2018
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Ingår i: MethodsX. - : Elsevier BV. - 1258-780X .- 2215-0161. ; 5, s. 1017-1026
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Tidskriftsartikel (refereegranskat)abstract
- Mercury (Hg), and in particular its methylated form (methylmercury, MeHg), is a hazardous substance with the potential to produce significant adverse neurological and other health effects. Enhanced anthropogenic emissions and long-range transport of atmospheric Hg have increased Hg concentrations above background levels in aquatic systems. In this context, the Minamata Convention, a global legally binding agreement that seeks to prevent human exposure to Hg, was signed and enforced by 128 countries, and today more than 90 Parties have ratified it. All these Parties have committed to develop Hg monitoring programs to report the effectiveness of the convention. For this purpose, we provide a standardized cleaning and water sampling protocol for the determination of total-Hg and MeHg in freshwaters at ambient levels. As Hg and organic matter are tightly bound, the protocol also describes sample collection for dissolved organic carbon (DOC) concentration and characterization of dissolved organic matter (DOM) composition by fluorescence spectroscopy. This protocol is highly useful to non-experts without a prior background in Hg sampling and analysis, and can serve as a useful basis for national monitoring programs. Furthermore, this protocol should help increase quantitative inventories of DOC, inorganic-Hg (IHg) and MeHg concentrations and DOM composition in freshwater, which are severely lacking at a global scale. • Provides a standardized method to collect water samples for IHg, MeHg, DOC and DOM composition from freshwater ecosystems.
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3. |
- Bravo, Andrea Garcia, et al.
(författare)
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High methylmercury production under ferruginous conditions in sediments impacted by sewage treatment plant discharges
- 2015
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Ingår i: Water Research. - : Elsevier BV. - 0043-1354 .- 1879-2448. ; 80, s. 245-255
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Tidskriftsartikel (refereegranskat)abstract
- Sewage treatment plants (STPs) are important point sources of mercury (Hg) to the environment. STPs are also significant sources of iron when hydrated ferric oxide (HFO) is used as a dephosphatation agent during water purification. In this study, we combined geochemical and microbiological characterization with Hg speciation and sediment amendments to evaluate the impact of STP's effluents on monomethylmercury (MMHg) production. The highest in-situ Hg methylation was found close to the discharge pipe in subsurface sediments enriched with Hg, organic matter, and iron. There, ferruginous conditions were prevailing with high concentrations of dissolved Fe2+ and virtually no free sulfide in the porewater. Sediment incubations demonstrated that the high MMHg production close to the discharge was controlled by low demethylation yields. Inhibition of dissimilatory sulfate reduction with molybdate led to increased iron reduction rates and Hg-methylation, suggesting that sulfate-reducing bacteria (SRB) may not have been the main Hg methylators under these conditions. However, Hg methylation in sediments amended with amorphous Fe(III)-oxides was only slightly higher than control conditions. Thus, in addition to iron-reducing bacteria, other non-SRB most likely contributed to Hg methylation. Overall, this study highlights that sediments impacted by STP discharges can become local hot-spots for Hg methylation due to the combined inputs of i) Hg, ii) organic matter, which fuels bacterial activities and iii) iron, which keeps porewater sulfide concentration low and hence Hg bioavailable.
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4. |
- Bravo, Andrea G., et al.
(författare)
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The interplay between total mercury, methylmercury and dissolved organic matter in fluvial systems : A latitudinal study across Europe
- 2018
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Ingår i: Water Research. - : Elsevier. - 0043-1354 .- 1879-2448. ; 144, s. 172-182
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Tidskriftsartikel (refereegranskat)abstract
- Large-scale studies are needed to identify the drivers of total mercury (THg) and monomethyl-mercury (MeHg) concentrations in aquatic ecosystems. Studies attempting to link dissolved organic matter (DOM) to levels of THg or MeHg are few and geographically constrained. Additionally, stream and river systems have been understudied as compared to lakes. Hence, the aim of this study was to examine the influence of DOM concentration and composition, morphological descriptors, land uses and water chemistry on THg and MeHg concentrations and the percentage of THg as MeHg (%MeHg) in 29 streams across Europe spanning from 41°N to 64°N. THg concentrations (0.06–2.78 ng L−1) were highest in streams characterized by DOM with a high terrestrial soil signature and low nutrient content. MeHg concentrations (7.8–159 pg L−1) varied non-systematically across systems. Relationships between DOM bulk characteristics and THg and MeHg suggest that while soil derived DOM inputs control THg concentrations, autochthonous DOM (aquatically produced) and the availability of electron acceptors for Hg methylating microorganisms (e.g. sulfate) drive %MeHg and potentially MeHg concentration. Overall, these results highlight the large spatial variability in THg and MeHg concentrations at the European scale, and underscore the importance of DOM composition on mercury cycling in fluvial systems.
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5. |
- Bravo, Andrea G., et al.
(författare)
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The interplay between total mercury, methylmercury and dissolved organic matter in fluvial systems : A latitudinal study across Europe
- 2018
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Ingår i: Water Research. - : Pergamon. - 0043-1354 .- 1879-2448. ; 144, s. 172-182
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Tidskriftsartikel (refereegranskat)abstract
- Large-scale studies are needed to identify the drivers of total mercury (THg) and monomethyl-mercury (MeHg) concentrations in aquatic ecosystems. Studies attempting to link dissolved organic matter (DOM) to levels of THg or MeHg are few and geographically constrained. Additionally, stream and river systems have been understudied as compared to lakes. Hence, the aim of this study was to examine the influence of DOM concentration and composition, morphological descriptors, land uses and water chemistry on THg and MeHg concentrations and the percentage of THg as MeHg (%MeHg) in 29 streams across Europe spanning from 41°N to 64 °N. THg concentrations (0.06–2.78 ng L−1) were highest in streams characterized by DOM with a high terrestrial soil signature and low nutrient content. MeHg concentrations (7.8–159 pg L−1) varied non-systematically across systems. Relationships between DOM bulk characteristics and THg and MeHg suggest that while soil derived DOM inputs control THg concentrations, autochthonous DOM (aquatically produced) and the availability of electron acceptors for Hg methylating microorganisms (e.g. sulfate) drive %MeHg and potentially MeHg concentration. Overall, these results highlight the large spatial variability in THg and MeHg concentrations at the European scale, and underscore the importance of DOM composition on mercury cycling in fluvial systems.
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6. |
- Dominik, Janusz, et al.
(författare)
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Mercury in the food chain of the Lagoon of Venice, Italy
- 2014
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Ingår i: Marine Pollution Bulletin. - : Elsevier BV. - 0025-326X .- 1879-3363. ; 88:1-2, s. 194-206
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Tidskriftsartikel (refereegranskat)abstract
- Sediments and biota samples were collected in a restricted area of the Lagoon of Venice and analysed for total mercury, monomethyl mercury (MMHg), and nitrogen and carbon isotopes. Results were used to examine mercury biomagnification in a complex food chain. Sedimentary organic matter (SOM) proved to be a major source of nutrients and mercury to primary consumers. Contrary to inorganic mercury, MMHg was strongly biomagnified along the food chain, although the lognormal relationship between MMHg and δ15N was less constrained than generally reported from lakes or coastal marine ecosystems. The relationship improved when log MMHg concentrations were plotted against trophic positions derived from baseline δ15N estimate for primary consumers. From the regression slope a mean MMHg trophic magnification factor of 10 was obtained. Filter-feeding benthic bivalves accumulated more MMHg than other primary consumers and were probably important in MMHg transfer from sediments to higher levels of the food chain.
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7. |
- Garcia Bravo, Andrea, et al.
(författare)
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Extremely elevated methyl mercury levels in water, sediment and organisms in a Romanian reservoir affected by release of mercury from a chlor-alkali plant
- 2014
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Ingår i: Water Research. - : Elsevier BV. - 0043-1354 .- 1879-2448. ; 49, s. 391-405
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Tidskriftsartikel (refereegranskat)abstract
- We examined mercury (Hg) biogeochemistry and biomagnification in the Babeni Reservoir, a system strongly affected by the release of Hg from a chlor-alkali plant. Total mercury (THg) concentrations in river water reached 88 ng L−1 but decreased rapidly in the reservoir (to 9 ng L−1). In contrast, monomethylmercury (MMHg) concentrations increased from the upstream part of the reservoir to the central part (0.7 ng L−1), suggesting high methylation within the reservoir. Moreover, vertical water column profiles of THg and MMHg indicated that Hg methylation mainly occurred deep in the water column and at the sediment–water interface. The discharge of Hg from a chlor-alkali plant in Valcea region caused the highest MMHg concentrations ever found in non-piscivorous fish worldwide. MMHg concentrations and bioconcentration factors (BCF) of plankton and macrophytes revealed that the highest biomagnification of MMHg takes place in primary producers.
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8. |
- Gascon Diez, Elena, et al.
(författare)
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Influence of a wastewater treatment plant on mercury contamination and sediment characteristics in Vidy Bay (Lake Geneva, Switzerland)
- 2014
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Ingår i: Aquatic Sciences. - : Springer Science and Business Media LLC. - 1015-1621 .- 1420-9055. ; 76:S1, s. S21-S32
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Tidskriftsartikel (refereegranskat)abstract
- Previous direct observations of the sediment surface in Vidy Bay, Lake Geneva (Switzerland), revealed a range of sediment characteristics in terms of colour, texture and morphology. Dives with the MIR submersibles during the éLEMO project permitted the exploration of a large portion of Vidy Bay. It is the most contaminated part of Lake Geneva, due to inputs of treated and untreated waters from a large wastewater treatment plant (WWTP). To evaluate the influence of WWTP effluent on mercury contamination and sediment characteristics, 14 sediment cores were retrieved in the vicinity of the wastewater treatment plant effluent. Total mercury concentrations in sediments ranged between 0.32 and 10.1 mg/kg. Inorganic mercury and monomethylmercury concentrations in overlying and pore waters were also measured. The total partition coefficients of mercury (logK d) ranged from 3.6 to 5.8. The monomethylmercury concentration in pore waters of surface sediments was a large proportion of the total mercury concentration (44 ± 25 %). A Spearman test showed a negative correlation between the distance to the wastewater treatment plant outlet and the concentrations of total mercury in sediments and pore waters. Visual observations from the submersible allowed recognizing six different types of sediment. The areal distribution of these different sediment types clearly showed the influence of the wastewater treatment plant outlet on the sediment surface patterns. However, no relationship with mercury concentrations could be established.
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9. |
- Gascon Diez, Elena, et al.
(författare)
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Role of settling particles on mercury methylation in the oxic water 1 column of freshwater systems
- 2016
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 50:21, s. 11672-11679
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Tidskriftsartikel (refereegranskat)abstract
- As the methylation of inorganic divalent mercury (HgII) to neurotoxic methylmercury (MeHg) has been attributed to the activity of anaerobic bacteria, the formation of MeHg in the oxic water column of marine ecosystems has puzzled scientists over the past years. Here we show for the first time that MeHg can be produced in particles sinking through oxygenated water column of lakes. Total mercury (THg) and MeHg concentrations were measured in settling particles and in surface sediments of the largest freshwater lake in Western Europe (Lake Geneva). Whilst THg concentration differences between sediments and settling particles were not significant, MeHg concentrations were up to ten-fold greater in settling particles. MeHg demethylation rate constants (kd) were of similar magnitude in both compartments. In contrast, Hg methylation rate constants (km) were one order of magnitude greater in settling particles. The net potential for MeHg formation, assessed by the ratio between the two rate constants (km kd-1), was therefore up to ten times higher in settling particles, denoting that in situ transformations likely contributed to the high MeHg concentrations found in settling particles. Hg methylation was inhibited ( 80 %) in settling particles amended with molybdate, demonstrating the prominent role of biological sulfate-reduction in the process.
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10. |
- Hu, Haiyan, et al.
(författare)
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Shifts in mercury methylation across a peatland chronosequence : From sulfate reduction to methanogenesis and syntrophy
- 2020
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Ingår i: Journal of Hazardous Materials. - : Elsevier. - 0304-3894 .- 1873-3336. ; 387
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Tidskriftsartikel (refereegranskat)abstract
- Peatlands are globally important ecosystems where inorganic mercury is converted to bioaccumulating and highly toxic methylmercury, resulting in high risks of methylmercury exposure in adjacent aquatic ecosystems. Although biological mercury methylation has been known for decades, there is still a lack of knowledge about the organisms involved in mercury methylation and the drivers controlling their methylating capacity. In order to investigate the metabolisms responsible for mercury methylation and methylmercury degradation as well as the controls of both processes, we studied a chronosequence of boreal peatlands covering fundamentally different biogeochemical conditions. Potential mercury methylation rates decreased with peatland age, being up to 53 times higher in the youngest peatland compared to the oldest. Methylation in young mires was driven by sulfate reduction, while methanogenic and syntrophic metabolisms became more important in older systems. Demethylation rates were also highest in young wetlands, with a gradual shift from biotic to abiotic methylmercury degradation along the chronosequence. Our findings reveal how metabolic shifts drive mercury methylation and its ratio to demethylation as peatlands age.
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11. |
- Pokrovsky, Oleg S., et al.
(författare)
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Dissolved organic matter controls seasonal and spatial selenium concentration variability in thaw lakes across a permafrost gradient
- 2018
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Ingår i: Environmental Science and Technology. - : American Chemical Society (ACS). - 0013-936X .- 1520-5851. ; 52:18, s. 10254-10262
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Tidskriftsartikel (refereegranskat)abstract
- Little is known about the sources and processing of selenium, an important toxicant and essential micronutrient, within boreal and sub-arctic environments. Upon climate warming and permafrost thaw, the behavior of Se in northern peatlands becomes an issue of major concern, because a sizable amount of Se can be emitted to the atmosphere from thawing soils and inland water surfaces and exported to downstream waters, thus impacting the Arctic biota. Working toward providing a first-order assessment of spatial and temporal variation of Se concentration in thermokarst waters of the largest frozen peatland in the world, we sampled thaw lakes and rivers across a 750-km latitudinal profile. This profile covered sporadic, discontinuous, and continuous permafrost regions of western Siberia Lowland (WSL), where we measured dissolved (<0.45 mu m) Se concentration during spring (June), summer (August), and autumn (September). We found maximum Se concentration in the discontinuous permafrost zone. Considering all sampled lakes, Se exhibited linear relationship (R-2 = 0.7 to 0.9, p < 0.05, n approximate to 70) with dissolved organic carbon (DOC) concentration during summer and autumn. Across the permafrost gradient, the lakes in discontinuous permafrost regions demonstrated stronger relationship with DOC and UV-absorbance compared to lakes in sporadic/isolated and continuous permafrost zones. Both seasonal and spatial features of Se distribution in thermokarst lakes and ponds suggest that Se is mainly released during thawing of frozen peat. Mobilization and immobilization of Se within peat-lake-river watersheds likely occurs as organic and organo-Fe, Al colloids, probably associated with reduced and elemental Se forms. The increase of active layer thickness may enhance leaching of Se in the form of organic complexes with aromatic carbon from the deep horizons of the peat profile. Further, the northward shift of permafrost boundaries in WSL may sizably increase Se concentration in lakes of continuous permafrost zone.
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12. |
- Rincón-Tomás, Blanca, et al.
(författare)
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Revisiting the mercury cycle in marine sediments : A potential multifaceted role for Desulfobacterota
- 2024
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Ingår i: Journal of Hazardous Materials. - : Elsevier. - 0304-3894 .- 1873-3336. ; 465
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Tidskriftsartikel (refereegranskat)abstract
- Marine sediments impacted by urban and industrial pollutants are typically exposed to reducing conditions and represent major reservoirs of toxic mercury species. Mercury methylation mediated by anaerobic microorganisms is favored under such conditions, yet little is known about potential microbial mechanisms for mercury detoxification. We used culture-independent (metagenomics, metabarcoding) and culture-dependent approaches in anoxic marine sediments to identify microbial indicators of mercury pollution and analyze the distribution of genes involved in mercury reduction (merA) and demethylation (merB). While none of the isolates featured merB genes, 52 isolates, predominantly affiliated with Gammaproteobacteria, were merA positive. In contrast, merA genes detected in metagenomes were assigned to different phyla, including Desulfobacterota, Actinomycetota, Gemmatimonadota, Nitrospirota, and Pseudomonadota. This indicates a widespread capacity for mercury reduction in anoxic sediment microbiomes. Notably, merA genes were predominately identified in Desulfobacterota, a phylum previously associated only with mercury methylation. Marker genes involved in the latter process (hgcAB) were also mainly assigned to Desulfobacterota, implying a potential central and multifaceted role of this phylum in the mercury cycle. Network analysis revealed that Desulfobacterota were associated with anaerobic fermenters, methanogens and sulfur-oxidizers, indicating potential interactions between key players of the carbon, sulfur and mercury cycling in anoxic marine sediments.
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13. |
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