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1.
It is widely recognized that wetlands, especially those rich in organic matter and receiving appreciable atmospheric mercury (Hg) inputs, are important sites of methylmercury (MeHg) production. Extensive wetlands in the southeastern United States have many ecosystem attributes ideal for promoting high MeHg production rates; however, relatively few mercury cycling studies have been conducted in these environments. We conducted a landscape scale study examining Hg cycling in coastal Louisiana (USA) including four field trips conducted between August 2003 and May 2005. Sites were chosen to represent different ecosystem types, including: a large shallow eutrophic estuarine lake (Lake Pontchartrain), three rivers draining into the lake, a cypress-tupelo dominated freshwater swamp, and six emergent marshes ranging from a freshwater marsh dominated by Panicum hemitomon to a Spartina alterniflora dominated salt marsh close to the Gulf of Mexico. We measured MeHg and total Hg (THg) concentrations, and ancillary chemical characteristics, in whole and filtered surface water, and filtered porewater. Overall, MeHg concentrations were greatest in surface water of freshwater wetlands and lowest in the profundal (non-vegetated) regions of the lake and river mainstems. Concentrations of THg and MeHg in filtered surface water were positively correlated with the highly reactive, aromatic (hydrophobic organic acid) fraction of dissolved organic carbon (DOC). These results suggest that DOC plays an important role in promoting the mobility, transport and bioavailability of inorganic Hg in these environments. Further, elevated porewater concentrations in marine and brackish wetlands suggest coastal wetlands along the Gulf Coast are key sites for MeHg production and may be a principal source of MeHg to foodwebs in the Gulf of Mexico. Examining the relationships among MeHg, THg, and DOC across these multiple landscape types is a first step in evaluating possible links between key zones for Hg(II)-methylation and the bioaccumulation of mercury in the biota inhabiting the Gulf of Mexico region.  相似文献   

2.
The Diffusive Gradients in Thin films (DGT) technique is an operationally defined method to determine the dissolved fraction of trace elements in water. The aim of this study was to develop this technique for the measurement of the bioavailable mercury species in natural waters. For that purpose, three types of DGT units (commercial, manufactured with agarose diffusive gel (DG) and manufactured with polyacrylamide DG) were tested under controlled conditions using an Hg(II) solution both with and without dissolved organic matter (DOM). An acid digestion method using aqua regia was optimised to efficiently digest the resin gel discs prior to analysis. A good performance was obtained for the three DGT types when deployed in a DOM-free mercury solution in the laboratory, and it was demonstrated that polyacrylamide gel can be used as diffusive layer for mercury sampling. However, when the DGT units were deployed in a mercury solution containing DOM, performance differences were observed. Furthermore, the mass of background mercury (blanks) varied among the different DGT types. In the light of the results, the devices manufactured with polyacrylamide DG seemed to be the best choice for dissolved mercury determination.  相似文献   

3.
Characteristics of mercury speciation in Minnesota rivers and streams   总被引:2,自引:0,他引:2  
Patterns of mercury (Hg) speciation were examined in four Minnesota streams ranging from the main-stem Mississippi River to small tributaries in the basin. Filtered phase concentrations of methylmercury (MeHg), inorganic Hg (IHg), and dissolved organic carbon (DOC) were higher in all streams during a major summertime runoff event, and DOC was enriched with MeHg but not with IHg. Particulate-phase MeHg and IHg concentrations generally increased with total suspended solids (TSS) concentrations but the event data did not diverge greatly from the non-event data, suggesting that sources of suspended sediments in these streams did not vary significantly between event and non-event samplings. The dissolved fractions (filtered concentration/unfiltered concentration) of both MeHg and IHg increased with increasing DOC concentrations, but varied inversely with TSS concentrations. While MeHg typically constitutes only a minor portion of the total Hg (THg) in these streams, this contribution is not constant and can vary greatly over time in response to watershed inputs.  相似文献   

4.
The interaction of Cu with dissolved organic matter (DOM, extracted from an organic forest floor) was investigated and the resulting data was evaluated in terms of their uncertainty. The speciation of Cu over ‘free’ Cu (as analysed by diffusive gradients in thin films (DGT)), dissolved Cu–DOM complexes and precipitated Cu–DOM was determined as a function of pH (3.5, 4.0 and 4.5) and Cu/C ratio. The dissolved organically bound fraction was highest at pH 4.5, but this fraction decreased with increasing Cu/C ratio, which was observed for all pH levels. In the range of Cu/C=7×10−5–2.3×10−2 (mol/mol) the precipitated fraction was very small. The speciation of both Al and Fe was not affected by increasing Cu concentrations. From a continuous distribution model using the Scatchard approach, we calculated the optimal fit and corresponding upper and lower 95% uncertainty bounds of the overall stability constants (Ko) with the shuffled complex evolution Metropolis (SCEM) algorithm. Although the optimal equation fitted the data very well, the uncertainty of the, according to literature, most reliable approach to establish stability constants, was still large. Accordingly, the usually reported intrinsic stability constants exhibited large uncertainty ranging from logKi=6.0–7.1 (optimal 6.7) for pH 3.5, logKi=6.5–7.1 (optimal 6.8) for pH 4.0, and logKi=6.4–7.2 (optimal 6.8) for pH 4.5 and showed only little effect of pH.  相似文献   

5.
Bioavailability of mercury (Hg) to Selenastrum capricornutum was assessed in bioassays containing field-collected freshwater of varying dissolved organic carbon (DOC) concentrations. Bioconcentration factor (BCF) was measured using stable isotopes of methylmercury (MeHg) and inorganic Hg(II). BCFs for MeHg in low-DOC lake water were significantly larger than those in mixtures of lake water and high-DOC river water. The BCF for MeHg in rainwater (lowest DOC) was the largest of any treatment. Rainwater and lake water also had larger BCFs for Hg(II) than river water. Moreover, in freshwater collected from several US and Canadian field sites, BCFs for Hg(II) and MeHg were low when DOC concentrations were >5mg L(-1). These results suggest high concentrations of DOC inhibit bioavailability, while low concentrations may provide optimal conditions for algal uptake of Hg. However, variability of BCFs at low DOC indicates that DOC composition or other ligands may determine site-specific bioavailability of Hg.  相似文献   

6.

Purpose

Due to the fast development of industry and the overuse of agrichemicals in past decades, Lake Taihu, an important source of aquatic products for Eastern China, has simultaneously suffered mercury (Hg) contamination and eutrophication. The objectives of this study are to understand Hg transfer in the food web in this eutrophic, shallow lake and to evaluate the exposure risk of Hg through fish consumption.

Methods

Biota samples including macrophytes, sestons, benthic animals, and fish were collected from Lake Taihu in the fall of 2009. The total mercury (THg), methyl mercury (MeHg), ??13C and ??15N in the samples were measured.

Results and discussion

The signature for ??15N increased with the trophic levels. Along with a diet composed of fish, the significant relationship between the ??13C and ??15N indicated that a pelagic foraging habitat is the dominant pathway for energy transfer in Lake Taihu. The concentrations of THg and MeHg in the organisms varied dramatically by ??3 orders of magnitude from primary producers (macrophytes and sestons) to piscivorous fish. The highest concentrations of both THg (100 ng g?1) and MeHg (66 ng g?1), however, were lower than the guideline of 200 ng g?1 of MeHg for vulnerable populations that is recommended by the World Health Organization (WHO). The daily intake of THg and MeHg of 92 and 56 ng day?1 kg?1 body weight, respectively, was generally lower than the tolerable intake of 230 ng day?1 kg?1 body weight for children recommended by the Joint FAO/WHO Expert Committee on Food Additives. Significant relationships between the ??15N and the logarithm of THg and MeHg showed an obvious biomagnification of Hg along the food web. The logarithmic bioaccumulation factor of MeHg in the fish (up to 5.7) from Lake Taihu, however, was relatively low compared to that of other aquatic ecosystems.

Conclusion

Health risk of exposure to Hg by consumption of fish for local residents is relatively low in the Lake Taihu area. Dilution of Hg levels in the phytoplankton induced by eutrophication is a possible factor inhibiting accumulation of MeHg in fish in eutrophic Lake Taihu.  相似文献   

7.
Total mercury (HgT), methylmercury (MeHg), and other operationally defined Hg species were determined on water samples collected from a river-reservoir system impacted by historic mine wastes. Simultaneously, a comprehensive study was undertaken to determine the influence of some major physico-chemical parameters on the fate of Hg within the system. Total Hg levels showed an increase from background concentrations of 4 ng liter(-1) upstream of mining activity, to peak values of 1500-2100 ng liter(-1) downstream of Hg contaminated mine tailings piles. MeHg concentrations varied from 0.1 to 7 ng liter(-1) in surface waters. In both cases, peak values were associated with the highest concentrations of total suspended solids (TSS). Particulate Hg (HgP) was typically >50% of HgT and increased downstream. The dissolved fraction of MeHg (MeHgD) always constituted a large portion of total methylmercury (MeHgT). The [MeHgT]/[HgT] ratio decreased downstream suggesting either a high percentage of inorganic Hg input from point sources, or low specific rates of MeHg production within the aquatic system. The latter could be due to the combined effects on microbial populations of both high levels of Hg concentrations found in water and sediments, and other factors related to the aqueous geochemistry of the system. Concentrations of HgT in the water column appeared to be enhanced by inputs of contaminated particles from the watershed during spring snow melt. In the reservoir, significant losses of Hg from the water column were observed. In addition to losses of Hg bound to particles by sedimentation, the removal through volatilization of dissolved gaseous Hg could be an important pathway.  相似文献   

8.
Selected water quality parameters and spectroscopic characteristics of dissolved organic matter (DOM) were examined during two different seasons for an artificial coastal lake (Shiwha Lake in South Korea), which are affected by seawater exchange due to the operation of a tidal power plant and external organic loadings from the upstream catchments. The coastal lake exhibited much lower concentrations of organic matter and nutrients than the upstream sources. The spectroscopic properties of the lake DOM were easily distinguished from those of the catchment sources as revealed by a lower absorption coefficient, lower degree of humification, and higher spectral slopes. The observed DOM properties suggest that the lake DOM may be dominated by smaller molecular size and less condensed structures. For the lake and the upper streams, higher absorption coefficients and fluorescence peak intensities but lower spectral slopes and humification index were found for the premonsoon versus the monsoon season. However, such seasonal differences were less pronounced for the industrial channels in the upper catchments. Three distinctive fluorophore groups including microbial humic-like, tryptophan-like, and terrestrial humic-like fluorescence were decomposed from the fluorescence excitation-emission matrix (EEM) of the DOM samples by parallel factor analysis (PARAFAC) modeling. The microbial humic-like component was the most abundant for the industrial channels, suggesting that the component may be associated with anthropogenic organic pollution. The terrestrial humic-like component was predominant for the upper streams, and its relative abundance was higher for the rainy season. Our principal component analysis (PCA) results demonstrated that exchange of seawater and seasonally variable input of allochthonous DOM plays important roles in determining the characteristics of DOM in the lake.  相似文献   

9.
Bonzongo JC  Lyons WB 《Ambio》2004,33(6):328-333
Mercury (Hg) concentrations above levels that could pose health risks have been measured recently in predatory fish from many aquatic systems in the southeastern region of the United States. Based on hypotheses derived from published experimental data on the aqueous geochemistry of Hg, we investigated the effect of certain natural and human-imposed conditions on in situ levels of methylmercury (MeHg) in the Mobile-Alabama River System (MARS). Water samples were collected from different types of environments, hypothesized to have contrasting levels of MeHg in the aqueous phase, and were analyzed for total-Hg (THg) and MeHg concentrations, as well as some key geochemical parameters. The results showed the following. i) Overall, total Hg concentrations in waters of the MARS are quite uniformly distributed and vary from 0.2 to 6 ng L(-1), suggesting that besides geological sources, atmospheric deposition is certainly the main source of Hg inputs in the studied system. ii) In locations with comparable THg levels, the Hg fraction present as MeHg was consistently higher in samples collected from the Coastal Plain portion of the MARS as compared to those from other geological provinces. iii) Our in situ observations confirmed conclusions derived from laboratory experiments, in that, MeHg abundance in aquatic systems correlates with sulfate (but only within a narrow range of concentrations); decreasing pH; and has no direct relationships with either nitrate or phosphate. iv) The investigation of Hg accumulation in biota at a single site showed that an aquatic system with low THg concentrations but a high MeHg:THg ratios, could have organisms with Hg content above safe levels. Therefore, potential health risks to fish eating populations can exist even when the aqueous phase does not show signs of significant Hg enrichment.  相似文献   

10.
Methyl-mercury (CH3Hg+) production was studied in freshwaters from lake Moreno, an ultraoligotrophic system belonging to Northern Patagonia. Hg2+ labelled with high specific activity 197Hg was spiked to water samples in concentrations of 10 ng l(-1), and incubated in laboratory for 3d time trends under different conditions. Experimental water was sampled daily to evaluate CH3(197)Hg+ production. Lake water used in the experiments was sampled just below the upper limit of the metalimnion ( approximately 30 m depth), where maximum values of chlorophyll a have been measured previously. Sampling was performed in late autumn, when the plankton fraction <50 microm exhibited mercury concentrations up to 260 microg g(-1) dry weight. The experiments analysed lake water filtered through 50, 20, and 0.2 microm (filter-sterilized) mesh nets. ASTM grade 1 water was also incubated for control. All the experiments were run in an environmental chamber under controlled temperature and light regime. High Hg2+ conversion to CH3Hg+, up to 50%, was measured in lake water, in a process stimulated by light. CH3Hg+ production was two-fold higher after 3d of incubation with illumination compared to total darkness. Sterile lake water showed conversions up to 30%, while the planktonic components seem to enhance the CH3Hg+ production. Overall, our results provide evidence that lake Moreno waters favour CH3Hg+ production in processes stimulated by light. Although biotic components certainly contribute to enhance mercury methylation, water chemistry plays a key role in this process. We hypothesize that dissolved organic matter, particularly its quality, could be decisive.  相似文献   

11.
Yao X  Zhang Y  Zhu G  Qin B  Feng L  Cai L  Gao G 《Chemosphere》2011,82(2):145-155
Taihu Basin is the most developed area in China, which economic development has resulted in pollutants being produced and discharged into rivers and the lake. Lake Taihu is located in the center of the basin, which is characterized by a complex network of rivers and channels. To assess the sources and fate of dissolved organic matter (DOM) in surface waters, we determined the components and abundance of chromophoric dissolved organic matter (CDOM) within Lake Taihu and 66 of its tributaries, and 22 sites along transects from two main rivers. In Lake Taihu, there was a relative less spatial variation in CDOM absorption aCDOM(355) with a mean of 2.46 ± 0.69 m−1compared to the mean of 3.36 ± 1.77 m−1 in the rivers. Two autochthonous tryptophan-like components (C1 and C5), two humic-like components (C2 and C3), and one autochthonous tyrosine-like component (C4) were identified using the parallel factor analysis (PARAFAC) model. The C2 and C3 had a direct relationship with aCDOM(355), dissolved organic carbon (DOC), and chemical oxygen demand (COD). The separation of lake samples from river samples, on both axes of the Principal Component Analysis (PCA), showed the difference in DOM fluorophores between these various environments. Components C1 and C5 concurrently showed positive factor 1 loadings, while C4 was close to the negative factor 1 axis. Components C2 and C3 showed positive second factor loadings. The major contribution of autochthonous tryptophan-like components to lake samples is due to the autochthonous production of CDOM in the lake ecosystems. The results also showed that the differences in geology and associated land use control CDOM dynamics, such as the high levels of CDOM with terrestrial characteristics in the northwestern upstream rivers and low levels of CDOM with increased microbial characteristics in the southwestern upstream rivers. Most of river samples from the downstream regions in the eastern and southeastern plains had a similar relative abundance of humic-like fluorescence, with less of the tryptophan-like and more of the tyrosine-like contributions than did samples from upstream regions.  相似文献   

12.
Mercury (Hg) can be strongly accumulated and biomagnified along aquatic food chain, but the exposure pathway remains little studied. In this study, we quantified the uptake and elimination of both inorganic mercury [as Hg(II)] and methylmercury (as MeHg) in an important farmed freshwater fish, the tilapia Oreochromis niloticus, using 203Hg radiotracer technique. The dissolved uptake rates of both mercury species increased linearly with Hg concentration (tested at ng/L levels), and the uptake rate constant of MeHg was 4 times higher than that of Hg(II). Dissolved uptake of mercury was highly dependent on the water pH and dissolved organic carbon concentration. The dietborne assimilation efficiency of MeHg was 3.7-7.2 times higher than that of Hg(II), while the efflux rate constant of MeHg was 7.1 times lower. The biokinetic modeling results showed that MeHg was the greater contributor to the overall mercury bioaccumulation and dietary exposure was the predominant pathway.  相似文献   

13.
Our objective was to examine how the behavior of atmospheric mercury (Hg) deposited to boreal lake mesocosms changed over time. We added inorganic Hg enriched in a different stable isotope in each of two years, which allowed us to differentiate between Hg added in the first and second year. Although inorganic Hg and methylmercury (MeHg) continued to accumulate in sediments throughout the experiment, the availability of MeHg to the food web declined within one year. This decrease was detected in periphyton, zooplankton, and water mites, but not in gomphid larvae, amphipods, or fish. We suggest that reductions in atmospheric Hg deposition should lead to decreases in MeHg concentrations in biota, but that changes will be more easily detected in short-lived pelagic species than long-lived species associated with benthic food webs.  相似文献   

14.
Speciation of zinc in contaminated soils   总被引:1,自引:0,他引:1  
The chemical speciation of zinc in soil solutions is critical to the understanding of its bioavailability and potential toxic effects. We studied the speciation of Zn in soil solution extracts from 66 contaminated soils representative of a wide range of field conditions in both North America and Europe. Within this dataset, we evaluated the links among the dissolved concentrations of zinc and the speciation of Zn(2+), soil solution pH, total soil Zn, dissolved organic matter (DOM), soil organic matter (SOM) and the concentrations of different inorganic anions. The solid-liquid partitioning coefficient (K(d)) for Zn ranged from 17 to 13,100Lkg(-1) soil. The fraction of dissolved Zn bound to DOM varied from 60% to 98% and the soil solution free Zn(2+) varied from 40% to 60% of the labile Zn. Multiple regression equations to predict free Zn(2+), dissolved Zn and the solid-liquid partitioning of Zn are given for potential use in environmental fate modeling and risk assessment. The multiple regressions also highlight some of the most important soil properties controlling the solubility and chemical speciation of zinc in contaminated soils.  相似文献   

15.
Jiang S  Liu X  Chen Q 《Chemosphere》2011,83(8):1108-1116
The toxicities and bioavailabilities of total mercury (THg) and methylmercury (MeHg) in aquatic systems have made them the subjects of recent research. In this study, we collected a lake sediment core from Ny-Ålesund in Svalbard and analyzed the distributions of THg and MeHg in the sediments. The increased trend of THg was caused by anthropogenic contamination since the 14th century through long-range transportation, especially after the industrial era. However, the peak values of Hg in surface sediment samples could be explained by the increased algal scavenging process in recent decades. All the biogeochemical proxies (e.g., pigments and diatom biomass) revealed recent sharp increases in aquatic primary production due to the current climate warming. Rock-Eval analyses indicated that algal-derived organic matter took up a large portion, and quantitative calculation showed that 89.6-95.8% of the Hg in post-1950 could be explained by scavenging. The distribution of MeHg has a close relationship with total Hg and organic matter. The oxidation-reduction condition is one of the possible factors affecting the methylation rates in H2 lake sediments. Higher algal productivity and organic matter actually led to the increased trend of methylation in the uppermost sediment. This study supports some new key hypotheses on climate-driven factors affecting Hg and MeHg cycling in High Arctic lake sediments.  相似文献   

16.
We analyzed Hg species distribution patterns among ecosystem compartments in the Everglades at the landscape level in order to explore the implications of Hg distribution for Hg bioaccumulation and to investigate major biogeochemical processes that are pertinent to the observed Hg distribution patterns. At an Everglade-wide scale, THg concentrations were significantly increased in the following order: periphyton相似文献   

17.
The effects of environmental and maternally derived methylmercury (MeHg) on the embryonic and larval stages of walleye (Stizostedion vitreum) were investigated using eggs collected during two successive spawning seasons. Eggs were collected from fish in a mercury (Hg)-polluted environment (Clay Lake, Ontario, Canada), and from fish in two relatively pristine lakes (Lakes Manitoba and Winnipeg, in the province of Manitoba). Both bioaccumulation of Hg into muscle and its mobilization into eggs was significantly higher in Clay Lake females. Maternal muscle MeHg concentration was positively correlated with female length and egg MeHg was positively correlated with muscle MeHg concentration in all three populations. Hatching success of eggs from all three stocks declined significantly with increasing waterborne MeHg (0.1-7.8 ng l-1). Hatching success was not significantly affected by egg MeHg concentration. Embryonic heart rate declined with increasing waterborne MeHg concentration, but larval growth was not affected. Occurrence of larval deformities was negatively correlated with size of female, but was not significantly correlated with MeHg in either eggs or water. Larval MeHg was positively correlated with the concentrations of MeHg in eggs demonstrating transmission of MeHg from females. Uptake of ambient MeHg was higher in larvae exposed to higher waterborne MeHg concentrations.  相似文献   

18.
Litterfall is a major source of mercury (Hg) and toxic methylmercury (MeHg) to forest soils and influences exposures of wildlife in terrestrial and aquatic ecosystems. However, the origin of MeHg associated with tree foliage is largely unknown. We tested the hypothesis that leaf MeHg is influenced by root uptake and thereby related to MeHg levels in soils. Concentrations of MeHg and total Hg in deciduous and coniferous foliage were unrelated to those in soil at 30 urban and rural forested locations in southwest Ohio. In contrast, tree genera and trunk diameter were significant variables influencing Hg in leaves. The fraction of total Hg as MeHg averaged 0.4% and did not differ among tree genera. Given that uptake of atmospheric Hg(0) appears to be the dominant source of total Hg in foliage, we infer that MeHg is formed by in vivo transformation of Hg in proportion to the amount accumulated.  相似文献   

19.
We determined total mercury (Hg) concentrations in 50 female lake trout (Salvelinus namaycush) and 69 male lake trout from Lake Ontario (Ontario, Canada and New York, United States). Results showed that, on average, males were 8% higher in Hg concentration than females in Lake Ontario. We also used bioenergetics modeling to determine whether a sexual difference in gross growth efficiency (GGE) could explain the observed sexual difference in Hg concentrations. According to the bioenergetics modeling results, male GGE was about 3% higher than female GGE, on average. Although the bioenergetics modeling could not explain the higher Hg concentrations exhibited by the males, a sexual difference in GGE remained a plausible explanation for the sexual difference in Hg concentrations of the lake trout. In an earlier study, male lake trout from Lake Ontario were found to be 22% higher in polychlorinated biphenyl (PCB) concentration than females from Lake Ontario. Thus, although males were higher in both Hg and PCB concentrations, the degree of the sexual difference in concentration varied between the two contaminants. Further research on sexual differences in Hg excretion rates and Hg direct uptake rates may be needed to resolve the disparity in results between the two contaminants.  相似文献   

20.
为探究台特玛湖水体水质超标原因,结合流域自然条件,以水中溶解性有机质(DOM)为研究对象,分析DOM的光谱特征和来源,通过平行因子分析(PARAFAC)和荧光区域积分分析(FRI)对台特玛湖流域水体DOM进行定性与定量分析。结果表明:PARAFAC识别出台特玛湖流域DOM中 4种主要荧光组分,分别为腐殖酸、类色氨酸、类酪氨酸(B峰和D峰),水体DOM主要组分为色氨酸类蛋白质和酪氨酸类蛋白质,占总体比例为66.57%,说明DOM来源主要以内源输入为主,腐殖化程度低;台特玛湖流域水体水质超标主要是因为尾闾湖的封闭性、面积大、高蒸发量且为浅水湖泊,导致个别水质指标不断富集;水体DOM各组分与TN和COD呈显著正相关,氟化物与矿化度之间呈显著正相关。本研究为台特玛湖水质超标提出的原因分析及建议措施可为台特玛湖流域水环境保护提供依据。  相似文献   

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