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1.
Methylation of mercury (Hg) is the crucial process that controls Hg biomagnification along the aquatic food chains. Aquatic sediments are of particular interest because they constitute an essential reservoir where inorganic divalent Hg (HgII) is methylated. Methylmercury (MeHg) concentrations in sediments mainly result from the balance between methylation and demethylation reactions, two opposite natural processes primarily mediated by aquatic microorganisms. Thus, Hg availability and the activity of methylating microbial communities control the MeHg abundance in sediments. Consistently, some studies have reported a significant positive correlation between MeHg and HgII or total Hg (HgT), taken as a proxy for HgII, in aquatic sediments using enzyme-catalyzed methylation/demethylation mechanisms. By compiling 1,442 published and unpublished HgT–MeHg couples from lacustrine, riverine, estuarine and marine sediments covering various environmental conditions, from deep pristine abyssal to heavily contaminated riverine sediments, we show that a Michaelis–Menten type relationship is an appropriate model to relate the two parameters: MeHg = aHgT/(K m  + HgT), with a = 0.277 ± 0.011 and K m  = 188 ± 15 (R 2 = 0.70, p < 0.001). From K m variations, which depend on the various encountered environmental conditions, it appears that MeHg formation and accumulation are favoured in marine sediments compared to freshwater ones, and under oxic/suboxic conditions compared to anoxic ones, with redox potential and organic matter lability being the governing factors.  相似文献   

2.
Mercury inputs and outputs at a small lake in northern Minnesota   总被引:1,自引:0,他引:1  
Storages and cycling of total mercury (HgT), methylmercury (MeHg), and Hg0 are described for Spring Lake, a small bog lake in the Marcell Experimental Forest in north-central Minnesota. We quantified photoredox transformations, MeHg photolysis, burial to the sediments, and internal and external loadings of HgT and MeHg. Atmospheric deposition was the main input of HgT; MeHg was supplied by a combination of atmospheric, near-shore wetland, and biotic (methylation) sources. HgT outputs were dominated by burial (67%), and Hg0 evasion accounted for 26% of HgT outputs. The watershed of Spring Lake is small (3.7× lake surface area), and accordingly, bog and upland runoff were minor contributors to both HgT and MeHg inputs. Wet deposition was ∼9% of total MeHg input, and other external inputs (runoff, sediment porewater) provided only an additional 7%, indicating that internal production of MeHg was occurring in the lake. Photolysis of MeHg, measured in the field and laboratory, removed ∼3× the lake mass of MeHg (20 mg) annually, and was the dominant sink for MeHg. Residence times of MeHg and HgT in the lake were 48 and 61 days, respectively, during the open-water season, compared with only 8 days for the residence time of MeHg on settling particles (seston). Photoreduction of Hg2+ to Hg0 was greater than the reverse reaction (Hg0 photooxidation), and the residence time of Hg0 in the photic zone was short (hours). Data from this study show active cycling of all the measured species of mercury (HgT, MeHg, and Hg0) and the importance of MeHg photolysis and photo-redox processes.  相似文献   

3.
Behavior of mercury in the Patuxent River estuary   总被引:12,自引:0,他引:12  
An overview of a comprehensive study of the behavior and fate of mercury in the estuarine Patuxent River is presented. Total Hg (HgT) and methylmercury (MeHg) exhibited weakly non-conservative behavior in the estuary. Total Hg concentrations ranged from 6 ng L-1 in the upper reaches of the sub-urbanized tidal freshwater river to <0.5 ng L-1 in the mesohaline lower estuary. Filterable (0.2 µm) HgT ranged from 0.2 to 1.5 ng L-1. On average, MeHg accounted for <5% of unfiltered HgT and <2% of filterable HgT. Dissolved gaseous section Hg (DGHg) concentrations were highest (up to 150 pg L-1) in the summer in the mesohaline, but were not well correlated with primary production or chlorophyll a, demonstrating the complex nature of Hg0 formation and cycling in an estuarine environment. Organic matter content appeared to control the HgT content of sediments, while MeHg in sediments was positively correlated with HgT and organic matter, and negatively correlated with sulfide. MeHg in sediments was low (0.1 to 0.5% of HgT). Preliminary findings suggest that net MeHg production within sediments exceeds net accumulation. Although HgT in pore waters increased with increasing sulfide, bulk MeHg concentrations decreased. The concentration of MeHg in sediments was not related to the concentration of HgT in pore waters. These observations support the hypothesis that sulfide affects the speciation and therefore bioavailability of dissolved and/or solid-phase Hg for methylation. Comparison with other ecosystems, and the negative correlation between pore water sulfide and sediment MeHg, suggest that sulfide limits production and accumulation of MeHg in this system.  相似文献   

4.
Summary Selenium has been suggested to enhance the histochemical staining of mercury when sections of tissue are subjected to the silver-enhancement method. In the present study, histochemical staining patterns of mercury in tissue sections of rat livers were compared with the actual content of organic and inorganic Hg in the livers, in both the presence and the absence of Se. Rats were injected intravenously with 5g of Hgg–1 body weight as methyl [203Hg] mercury chloride (MeHg) or as [203Hg]mercuric chloride (Hg2+). After 2h, half the rats received an additional intraperitoneal injection of 2g of Se g–1 body weight as sodium [75Se]selenite. All the rats were killed 1h later. Homogenized liver samples were prepared for mercury analysis by two different methods: alkaline digestion and ultrasonic disintegration. Quantitative chemical analysis based on benzene extrction of the radioactively labelled Hg compounds showed that the chemical form of mercury, either organic or inorganic, was preserved from its administration to its deposition in the liver. Light and electron microscopy demonstrated that no silver enhancement of Hg occurred when MeHg alone was present in the sections of tissue, whereas MeHg accompanied by Se induced a moderate deposition of silver grains. In contrast, sections containing Hg2+ alone yielded some staining, and the addition of Se increased the staining dramatically. The results of the present study show that acute selenite pretreatment is a prerequisite for the histochemical demonstration of methyl mercury, and greatly increases the staining of inorganic mercury when applying the silver-enhancement method.  相似文献   

5.
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7.
A novel integrated dynamic model, the Integrated Fish Model (INTFISH), incorporating mercury (Hg) dynamics at non-steady state in marine organisms, is presented and is applied to the benthic food web in a polluted area. The integrated Fish model represents the dynamics of inorganic mercury (HgII) and methyl‑mercury (MeHg) in a real marine ecosystem including environmental (seawater and sediments) and biota compartments. Mercury concentration in fish is estimated using the INTFISH model coupled, in real-time, with results from i) the seawater and sediments modules computed using the HR3DHG model, ii) a dedicated Phytoplankton model and iii) six modules for Hg fluxes within the invertebrate compartment, incorporating the main organisms included in fish diet preferences, whose variations during the whole life cycle are also taken into account to verify the sensitivity of the integrated model to the core set of parameters. The simulated total mercury concentrations (HgTOT) in specimens of red mullet (Mullus barbatus), selected as target species for the Fish model, are in excellent agreement with field observations reported from the investigated area. The intrinsic modularity of the model offers the opportunity to extend simulations to other fish species (which are part of the diet of human populations of interest) and predict Hg concentration in food. A natural extension of the model will allow to evaluate the health risks related to human consumption of contaminated fish.  相似文献   

8.
BackgroundMethylmercury (MeHg) and ethylmercury (EtHg) are potent toxicants affecting the environment and human healthy. In this way, the present study aimed to investigate and compare the effects of MeHg and EtHg exposure on human peripheral blood mononuclear cells (PBMCs), which are critical components of the mammalian immune system.MethodsPBMCs were exposed to 2.5 μM MeHg or 2.5 μM EtHg. The number of cells and incubation times varied according to each assay. After exposures, the PBMCs were subjected to different evaluations, including cell viability, morphological aspects, cell cycle phases, indices of apoptosis and necrosis, reactive species (RS) production, and mitochondrial functionality.ResultsPBMCs exposed to EtHg were characterized by decreased viability and size, increased granularity, RS production, and apoptotic indexes accompanied by an intensification of Sub-G1 and reduction in G0-G1 cell cycle phases. Preceding these effects, we found mitochondrial dysfunctions, namely a reduction in the electron transport system related to mitochondrial complex I. In contrast, PBMCs exposed to MeHg showed only reduced viability. By ICP-MS, we found that PBMCs treated with EtHg accumulated Hg + levels ∼1.8-fold greater than MeHg-exposed cells.Conclusions and significanceTaken together, our findings provide important insights about mercury immunotoxicity, showing that EtHg is more immunotoxic to human PBMCs than MeHg.  相似文献   

9.
Seven Wisconsin rivers with contrasting, relativelyhomogeneous watershed composition were selected toassess the factors controlling mercury transport.Together, these watersheds allow comparisons ofwetland, forest, urban and agricultural land-uses.Each site was sampled nine times between September1993 and September 1994 to establish seasonalsignatures and transport processes of total mercury(HgT) and methylmercury (MeHg). Our resultsclearly show that land use and land cover stronglyinfluence mercury transport processes. Under base-flowconditions, unfiltered MeHg yield varies by a factorof sixteen (12–195 mg km-2 d-1), andincreases with the fraction of wetland area in thewatershed. Elevated mercury yields during high floware particle-phase associated in agricultural sites,but filtered-phase associated in wetland sites.Methylmercury represented less than 5% of totalmercury mobilized during the spring thaw across allwatersheds. Autumn MeHg yield was generally 11–15%of HgT in wetland influenced watersheds, thougha maximum of 51% was observed. In some cases, singlehigh-flow events may dominate the annual export ofmercury from a watershed. For example, one high-flowevent on the agricultural Rattlesnake Creek had thelargest HgT and MeHg yield in the study (107 and2.32 mg km-2 d-1, respectively). The mass ofmercury transported downstream by this single eventwas an order of magnitude larger than the eight other(non-event) sampling dates combined. These resultsunderscore the importance of watershed characteristicsand seasonal events on the fate of mercury in freshwater rivers.  相似文献   

10.
The accumulation of total mercury (HgT) andmethylmercury (MeHg) was evaluated in sediments ofTivoli South Bay, a freshwater tidal mudflat wetlandin the Hudson River National Estuarine ResearchReserve system. HgT concentrations in sedimentcores were measured to evaluate the spatialvariability of HgT deposition, and to establisha chronology of HgT accumulation. Cores takenfrom the northern, middle, and southern sections ofthe bay had similar distribution patterns andconcentrations of HgT, suggesting a common sourceof HgT throughout the bay. Sedimentconcentrations ranged from 190 to 1040 ng Hg g–1,2 to 10 times greater than concentrations expected insediments from non-anthropogenic sources. HgTdeposition rates were similar in different regions ofthe bay, and increased from 200 ng Hg cm–2yr–1in the 1930s to a maximum of 300 ngHg cm–2 yr–1 in the 1960s. Deposition rateshave steadily declined since the 1970s and arecurrently at 80 ng Hg cm–2 yr–1. Transportof HgT by tidal waters from the Hudson River islikely the main source of HgT in the bay.Distribution patterns and absolute concentrations ofMeHg in sediment cores were similar throughout thebay, with concentrations ranging from 0.43 to 2.95ng g–1. Maxima in MeHg concentration profilesoccurred just below the sediment-water interface andat a depth of 30 cm. The maximum at 30 cm wascoincident with maximum HgT concentrations. MeHgconcentrations in suspended particulate matter (SPM)from the Hudson River suggest that MeHg in the baycould be derived from riverine SPM rather than formedin situ.  相似文献   

11.
We have previously hypothesized that sulfide inhibits Hg methylation by decreasing its bioavailability to sulfate-reducing bacteria (SRB), the important methylators of Hg in natural sediments. With a view to designing a bioassay to test this hypothesis, we investigated a number of aspects of Hg methylation by the SRB Desulfobulbus propionicus, including (i) the relationship between cell density and methylmercury (MeHg) production, (ii) the time course of Hg methylation relative to growth stage, (iii) changes in the bioavailability of an added inorganic Hg (HgI) spike over time, and (iv) the dependence of methylation on the concentration of dissolved HgI present in the culture. We then tested the effect of sulfide on MeHg production by this microorganism. These experiments demonstrated that under conditions of equal bioavailability, per-cell MeHg production was constant through log-phase culture growth. However, the methylation rate of a new Hg spike dramatically decreased after the first 5 h. This result was seen whether methylation rate was expressed as a fraction of the total added Hg or the filtered HgI concentration, which suggests that Hg bioavailability decreased through both changes in Hg complexation and formation of solid phases. At low sulfide concentration, MeHg production was linearly related to the concentration of filtered HgI. The methylation of filtered HgI decreased about fourfold as sulfide concentration was increased from 10−6 to 10−3 M. This decline is consistent with a decrease in the bioavailability of HgI, possibly due to a decline in the dissolved neutral complex, HgS0.  相似文献   

12.

Background

Mercury-polluted environments are often contaminated with other heavy metals. Therefore, bacteria with resistance to several heavy metals may be useful for bioremediation. Cupriavidus metallidurans CH34 is a model heavy metal-resistant bacterium, but possesses a low resistance to mercury compounds.

Methodology/Principal Findings

To improve inorganic and organic mercury resistance of strain CH34, the IncP-1β plasmid pTP6 that provides novel merB, merG genes and additional other mer genes was introduced into the bacterium by biparental mating. The transconjugant Cupriavidus metallidurans strain MSR33 was genetically and biochemically characterized. Strain MSR33 maintained stably the plasmid pTP6 over 70 generations under non-selective conditions. The organomercurial lyase protein MerB and the mercuric reductase MerA of strain MSR33 were synthesized in presence of Hg2+. The minimum inhibitory concentrations (mM) for strain MSR33 were: Hg2+, 0.12 and CH3Hg+, 0.08. The addition of Hg2+ (0.04 mM) at exponential phase had not an effect on the growth rate of strain MSR33. In contrast, after Hg2+ addition at exponential phase the parental strain CH34 showed an immediate cessation of cell growth. During exposure to Hg2+ no effects in the morphology of MSR33 cells were observed, whereas CH34 cells exposed to Hg2+ showed a fuzzy outer membrane. Bioremediation with strain MSR33 of two mercury-contaminated aqueous solutions was evaluated. Hg2+ (0.10 and 0.15 mM) was completely volatilized by strain MSR33 from the polluted waters in presence of thioglycolate (5 mM) after 2 h.

Conclusions/Significance

A broad-spectrum mercury-resistant strain MSR33 was generated by incorporation of plasmid pTP6 that was directly isolated from the environment into C. metallidurans CH34. Strain MSR33 is capable to remove mercury from polluted waters. This is the first study to use an IncP-1β plasmid directly isolated from the environment, to generate a novel and stable bacterial strain useful for mercury bioremediation.  相似文献   

13.
Adsorption of Hg2+ and methylmercury (MeHg) to multi-walled carbon nanotubes (MWCNTs) modified, respectively, with hydroxyl, amine and carboxyl groups was studied. The effect of various factors like the initial pH, natural organic matter (NOM), Cl- and adsorbent dose on the sorption efficiency were evaluated. It was found that amine-modified MWCNTs showed a strong adsorption capacity to Hg2+ and MeHg, and the removal efficiency could reach up to 92% (0.5 g/L MWCNTs, and 100 μg/L Hg2+ and MeHg) which is independent of pH. NOM had complex effects on the adsorption of Hg2+ and MeHg to MWCNTs. Cl- inhibited the adsorption of Hg2+ and MeHg to MWCNTs. The adsorption of Hg2+ and MeHg was found to be inhomogeneous and homogeneous chemisorption, respectively. Our results suggested that MWCNTs modified with different functional groups can efficiently adsorb both Hg2+ and MeHg in aqueous environment.  相似文献   

14.
Abstract

Mature starfish Leptasterias polaris were exposed to labelled mercury (II) species via food contaminated at a level of 5.0 μg g?1. The distribution of inorganic Hg and methylmercury (MeHg) in starfish organs and tissues and the effect of a series of complexing agents on mercury translocation between organs and tissues were examined over a 24-h period. The distribution of mercury species in coelomic fluid components, ammonia excretion rate and mercury excretion were also measured. The highest concentrations were observed in the stomach (the source organ) and in pyloric caecum (up to 0.32 μg g?1 wet weight for inorganic Hg and 0.22 μg g?1 for MeHg). Concentrations of MeHg in gonads ranged from ≤ 0.01 to 0.08 μg g?1 whereas concentrations of inorganic Hg never exceeded 0.06 μg g?1. In all studied cases, mercury concentration was very low the coelomic fluid (≤ 0.01 μg g?1). The short-term distribution of Hg species via contaminated food in starfish L. polaris seems to be controlled by the haemal system, a primitive circulatory system responsible for the transport of soluble nutrients from the digestive track towards organs and tissues, but a possible role of the coelomic fluid can not be excluded. Very low Hg contents were observed in gonads and in the coelomic fluid which fills the general cavity. Except for mercaptoethanol (merOH) and dimercaptosuccinic acid (DMSA), the addition of complexing agents to the food had little effect on the distribution of Hg species. MerOH appeared as an efficient carrier for methylmercury transport through the digestive system. DMSA enhanced the translocation of inorganic mercury from stomach and pyloric caecum toward external tissues and markedly increased its excretion.  相似文献   

15.
A biosorbent prepared by alkaline extraction of Aspergillus niger biomass was evaluated for its potential to remove mercury species – inorganic (Hg2+) and methyl mercury (CH3Hg+) – from aqueous solutions. Batch experiments were carried out to determine the pH and time profile of sorption for both species in the pH range 2–7. The Hg2+ exhibited more rapid sorption and higher capacity than the CH3Hg+. Further, removal of both mercury species from spiked ground water samples was efficient and not influenced by other ions. Sorption studies with esterified biosorbent indicated loss of binding of both mercury species (>80%), which was regained when the ester groups were removed by alkaline hydrolysis, suggesting the involvement of carboxyl groups in binding. Further, no interconversion of sorbed species occurred on the biomass. The biosorbent was reusable up to six cycles without serious loss of binding capacity. Our results suggest that the biosorbent from Aspergillus niger can be used for removal of mercury and methyl mercury ions from polluted aqueous effluents.  相似文献   

16.
Litterfall from trees has been identified as an important pathway for deposition of mercury (Hg) and methylmercury (MeHg) in forested catchments, but very little is known about the role of ground vegetation in deposition and cycling of Hg compounds. This study was conducted to identify the origin of Hg compounds in the ground vegetation, and to estimate the role of its litterfall with respect to pools and fluxes of Hg in a coniferous forest in the German Fichtelgebirge mountains. Above and below ground biomass of the dominant ground vegetation (Vaccinium myrtillus, Deschampsia flexuosa and Calamagrostis villosa) were sampled at several plots successively during the growing season. The fluxes to the soil via litterfall of the ground vegetation were calculated using contents of Hg and MeHg in the annual fractions of aboveground biomass. With fluxes of 0.4 – 7.8 mg Hgtotal ha–1 a–1 and 0.01 – 0.04 mg MeHg ha–1 a–1 (depending on the plant species) this pathway contributes only a few percent to the total deposition of both compounds in the catchment. To identify the uptake pathways of Hg compounds, the same plant species were grown in a pot experiment with addition of isotope labelled Hg compounds (202Hg2+, Me198Hg) to a clean sand substrate. Only small proportions of 202Hg and Me198Hg in the substrate were taken up by the plants, but in all cases the proportion translocated into aboveground biomass after uptake was greater in case of Me198Hg. Thus, internal recycling in the plant-soil system is a source especially for MeHg in the ground vegetation. However, as compared to the input of Hg compounds by tree litterfall and storage in the forest floor, Hgtotal and MeHg in ground vegetation are of minor importance. High volatilization of added Hg isotopes raises the question of a re-emission of Hg compounds by the transpiration flux of the ground vegetation.  相似文献   

17.
The biotransformation of HgII in pH-controlled and aerated algal cultures was investigated. Previous researchers have observed losses in Hg detection in vitro with the addition of cysteine under acid reduction conditions in the presence of SnCl2. They proposed that this was the effect of Hg-thiol complexing. The present study found that cysteine-Hg, protein and nonprotein thiol chelates, and nucleoside chelates of Hg were all fully detectable under acid reduction conditions without previous digestion. Furthermore, organic (R-Hg) mercury compounds could not be detected under either the acid or alkaline reduction conditions, and only β-HgS was detected under alkaline and not under acid SnCl2 reduction conditions. The blue-green alga Limnothrix planctonica biotransformed the bulk of HgII applied as HgCl2 into a form with the analytical properties of β-HgS. Similar results were obtained for the eukaryotic alga Selenastrum minutum. No evidence for the synthesis of organomercurials such as CH3Hg+ was obtained from analysis of either airstream or biomass samples under the aerobic conditions of the study. An analytical procedure that involved both acid and alkaline reduction was developed. It provides the first selective method for the determination of β-HgS in biological samples. Under aerobic conditions, HgII is biotransformed mainly into β-HgS (meta-cinnabar), and this occurs in both prokaryotic and eukaryotic algae. This has important implications with respect to identification of mercury species and cycling in aquatic habitats.  相似文献   

18.
In the aquatic environment, mercury is readily methylated into its most toxic form of methylmercury. In this form, it enters the aquatic food chain and its concentrations increase in subsequent links, which decreases the quality of fish meat and poses risks to consumer health. Concentrations of methylmercury (MeHg) and total mercury (THg) were determined in the muscle tissues of 64 eel specimens measuring from 59 to 95 cm in length as functions of specimen size and weight. Risks posed to consumers by eel from different length classes were also assessed. The mean concentration of THg in all of the eel examined was 0.179 mg kg?1, but the range was from 0.028 to 0.487 mg kg?1. The mean concentration of MeHg was 0.147 mg kg?1, and the range was also wide from 0.023 to 0.454 mg kg?1. Accumulated MeHg and THg increased with eel body length. The percentage share of MeHg in THg also changed with specimen length, and there was a positive correlation between the concentrations of MeHg and THg. Risk assessment was performed based on the doses of THg and MeHg ingested with fish for several specimen length classes. Consuming the meat of eel measuring 80 cm in length increased the estimated weekly intake (EWI) of THg and MeHg twofold in comparison to that from specimens 60 cm in length and fourfold in specimens exceeding 90 cm in length. The percentage shares of the EWI in the tolerable weekly intake and the target hazard quotient coefficient also increased proportionally. Generally, concentrations of MeHg and THg in eel are below current limits and pose no risk to consumer health as long as the consumption of larger specimens is avoided.  相似文献   

19.
As top predators in the Pearl River Estuary (PRE) of China, Indo-Pacific humpback dolphins (Sousa chinensis) are bioindicators for examining regional trends of environmental contaminants in the PRE. We examined samples from stranded S. chinensis in the PRE, collected since 2004, to study the distribution and fate of total mercury (THg), methylmercury (MeHg) and selenium (Se) in the major tissues, in individuals at different ages and their prey fishes from the PRE. This study also investigated the potential protective effects of Se against the toxicities of accumulated THg. Dolphin livers contained the highest concentrations of THg (32.34±58.98 µg g−1 dw) and Se (15.16±3.66 µg g−1 dw), which were significantly different from those found in kidneys and muscles, whereas the highest residue of MeHg (1.02±1.11 µg g−1 dw) was found in dolphin muscles. Concentrations of both THg and MeHg in the liver, kidney and muscle of dolphins showed a significantly positive correlation with age. The biomagnification factors (BMFs) of inorganic mercury (Hginorg) in dolphin livers (350×) and MeHg in muscles (18.7×) through the prey fishes were the highest among all three dolphin tissues, whereas the BMFs of Se were much lower in all dolphin tissues. The lower proportion of MeHg in THg and higher Se/THg ratios in tissues were demonstrated. Our studies suggested that S. chinensis might have the potential to detoxify Hg via the demethylation of MeHg and the formation of tiemannite (HgSe) in the liver and kidney. The lower threshold of hepatic THg concentrations for the equimolar accumulation of Se and Hg in S. chinensis suggests that this species has a greater sensitivity to THg concentrations than is found in striped dolphins and Dall’s porpoises.  相似文献   

20.
Bacterially mediated ionic mercury reduction to volatile Hg0 was shown to play an important role in the geochemical cycling of mercury in a contaminated freshwater pond. This process, and the degradation of methylmercury, could be stimulated to reduce the concentration of methylmercury that is available for accumulation by biota. A study testing the utility of this approach is described.Abbreviations HgR inorganic mercury resistance - Org-Hg organomercury - Org-HgR organomercury resistance - SRB sulfate reducing bacteria - Methyl-B12 methylcobalamine  相似文献   

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