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1.
Porewater samples were obtained on five occasions during spring, summer and fall by in situ dialysis from three sites of a large freshwater wetland situated along the St. Lawrence River. These samples were analysed for total dissolved mercury ([Hg]T) and methylmercury ([MeHg]) concentrations and for complementary variables including dissolved sulfate, sulfide and elemental sulfur concentrations. Sediment cores were obtained on three occasions from one of these sites for the determination of total mercury ({Hg}T) and methylmercury ({MeHg}) concentration as well as mercury methyltransferase (HgMT) activity profiles. {MeHg} and HgMT activity varied with time and sediment depth. The porewater [Hg]T and [MeHg] depth profiles varied with time and among sites. Modeling the porewater [MeHg] profiles with a one-dimensional reaction-transport equation allowed identification of the sediment depths where MeHg is produced or consumed, as well as an estimate of the net in situ MeHg production rates in the sediments. The model-predicted depths of MeHg production, as well as the sulfate concentration and the HgMT activity depth distributions are all consistent with the involvement of sulfate reducing bacteria in the production of MeHg.  相似文献   

2.
The first advisory to limit consumption of Florida Bay fish due to mercury was issued in 1995. Studies done by others in the late 1990s found elevated water column concentrations of both total Hg (THg) and methylmercury (MeHg) in creeks discharging from the Everglades, which had its own recognized mercury problem. To investigate the significance of allochthonous MeHg discharging from the upstream freshwater Everglades, we collected surface water and sediment along two transects from 2000 to 2002. Concentrations of THg and MeHg, ranging from 0.36 ng THg/L to 5.98 ng THg/L and from <0.02 ng MeHg/L to 1.79 ng MeHg/L, were elevated in the mangrove transition zone when compared both to upstream canals and the open waters of Florida Bay. Sediment concentrations ranged from 5.8 ng THg/g to 145.6 ng THg/g and from 0.05 ng MeHg/g to 5.4 ng MeHg/g, with MeHg as a percentage of THg occasionally elevated in the open bay. Methylation assays indicated that sediments from Florida Bay have the potential to methylate Hg. Assessment of mass loading suggests that canals delivering stormwater from the northern Everglades are not as large a source as direct atmospheric deposition and in situ methylation, especially within the mangrove transition zone.  相似文献   

3.
This study investigated the contamination levels and profiles of polychlorinated biphenyls (PCBs), polybrominated diphenyl ethers (PBDEs), organochlorine pesticides (OCPs) including dichlorodiphenyltrichloroethane and its metabolites (DDTs), hexachlorocyclohexanes (HCHs) and hexachlorobenzene (HCB) in fish from the Niyang River, Tibetan Plateau. The total concentrations of ∑PCB, ∑PBDE and ∑OCP were in the range of 0.246–1.056 ng/g (mean 0.540 ± 0.289 ng/g), 0.280–2.220 ng/g (mean 0.914 ± 0.643 ng/g) and 7.24–13.80 ng/g (mean 10.70 ± 2.31 ng/g), respectively. The total mercury concentration (HgT) in fish ranged from 85 to 217 ng/g dw with an average of 129 ng/g dw, and the concentrations of methyl mercury (MeHg) ranged from 61 to 160 ng/g dw with an average of 102 ng/g dw. The proportion of MeHg contributed to 66–91 % (average 80 %) of HgT for all samples, indicating that organic mercury was the predominant form of mercury in fish muscle. The results revealed that the fish from the Niyang River were contaminated with various persistent toxic pollutants and the potential influencing factors on the bioaccumulation concentration in fish were analyzed using Pearson’s correlation analysis.  相似文献   

4.
Concentrations of total Hg in sediments near six drilling sites in the Gulf of Mexico were elevated well above average background values of 40–80 ng/g. The excess Hg was associated with barite from discharged drilling mud. In contrast with total Hg, concentrations of methylmercury (MeHg) in these sediments did not vary significantly at nearfield (<100 m) versus farfield (>3 km) distances from the drilling sites. Observed variability in concentrations of MeHg were related to local differences in redox state in the top 10 cm of sediment. Low to non-detectable concentrations of MeHg were found in nearfield sediments that were anoxic, highly reducing and contained abundant H2S. At most drilling sites, nearfield samples with high concentrations of total Hg (>200 ng/g) had similar or lower amounts of MeHg than found at background (farfield) stations. Higher values of MeHg were found in a few nearfield sediments at one site where concentrations of TOC were higher and where sediments were anoxic and moderately reducing. Overall, results from this study support the conclusion that elevated concentrations of MeHg in sediments around drilling sites are not a common phenomenon in the Gulf of Mexico.  相似文献   

5.
The water, pore water, sediment, and fish samples were collected from the Hongfeng Reservoir in November 2003 and February 2004 in accordance with trace metal protocols. The average concentrations of total mercury （THg）, dissolved mercury （DHg）, reactive mercury, dissolved gaseous mercury, total methylmercury, and dissolved methylmercury in the water columns were 8.00, 5.70, 0.63, 0.05, 0.16, and 0.07 ng/L, respectively. THg and DHg in the water columns, THg in pore water and THg in lake sediments of the Hongfeng Reservoir showed the level of mercury in the Hongfeng Reservoir was higher than in other natural waters in the world due to the loading of a lot of waste water with relatively high concentrations of mercury, whereas methylmercury concentrations in fish （wet weight） varied from 1.73-51.00 ng/g, much lower than in most remote lakes and reservoirs reported in northern Europe and North America. Methylmercury distributions in pore water and sediments showed methylation occurred mainly in the upper several centimeters of sediment cores in the Hongfeng Reservoir. The concentrations of dissolved organic carbon, total suspended particles, total Hg, and methylmercury were higher at Houwu than those at Daba in November 2003. It is suggested that other pollutants such as N and P from fishing farm and other waste water at Houwu, which resulted in deterioration of water quality, affected the concentrations and distributions of mercury species in the reservoir.  相似文献   

6.
The characteristics of mercury in the aquatic environment have been intensively studied in mining areas with heavy mercury pollution but little work has been conducted in urban areas, with no significant Hg source. This paper presents a study of the Haihe River, which flows through an urban area in North China. The concentrations of total mercury (THg) and methylmercury (MeHg) in the river water were 3.6–31.2 and 0.12–3.21 ng/l, and the corresponding values in river sediment were 22.9–374.8 and 0.03–0.46 μg/kg. These values are lower than the reported values from mining areas. The THg concentration in sediment samples collected from the urban areas was higher than that from the rural areas and the global background levels, indicating the influence of urbanization on mercury contamination. Samples of typical riparian and floating plants, reed and hornwort, were collected. Correlation analysis showed that sediment is the major source of THg and MeHg in reed and water is the major source of MeHg in hornwort. The higher bioaccumulation factor of reed indicates its higher potential to accumulate MeHg from the environment.  相似文献   

7.
Karen A. Merritt  Aria Amirbahman   《Earth》2009,96(1-2):54-66
Considerable recent research has focused on methylmercury (MeHg) cycling within estuarine and coastal marine environments. Because MeHg represents a potent neurotoxin that may magnify in marine foodwebs, it is important to understand the mechanisms and environmental variables that drive or constrain methylation dynamics in these environments. This critical review article explores the mechanisms hypothesized to influence aqueous phase and sediment solid phase MeHg concentrations and depth-specific inorganic Hg (II) (Hgi) methylation rates (MMR) within estuarine and coastal marine environments, and discusses issues of terminology or methodology that complicate mechanism-oriented interpretation of field and laboratory data. Mechanisms discussed in this review article include: 1) the metabolic activity of sulfate reducing bacteria (SRB), the microbial group thought to dominate mercury methylation in these environments; 2) the role that Hgi concentration and/or speciation play in defining depth-specific Hgi methylation rates; and 3) the depth-dependent balance between MeHg production and consumption within the sedimentary environment. As discussed in this critical review article, the hypothesis of SRB community control on the Hgi methylation rate in estuarine and coastal marine environments is broadly supported by the literature. Although Hgi speciation, as a function of porewater inorganic sulfide and/or dissolved organic matter concentration and/or pH, may also play a role in observed variations in MMR, the nature and function of the controlling ligand(s) has not yet been adequately defined. Furthermore, although it is generally recognized that the processes responsible for MeHg production and consumption overlap spatially and/or kinetically in the sedimentary environment, and likely dictate the extent to which MeHg accumulates in the aqueous and/or sediment solid phase, this conceptual interpretation requires refinement, and would benefit greatly from the application of kinetic modeling.  相似文献   

8.
San Pablo Bay is an estuary, within northern San Francisco Bay, containing elevated sediment mercury (Hg) levels because of historic loading of hydraulic mining debris during the California gold-rush of the late 1800s. A preliminary investigation of benthic microbial Hg cycling was conducted in surface sediment (0-4 cm) collected from one salt-marsh and three open-water sites. A deeper profile (0-26 cm) was evaluated at one of the open-water locations. Radiolabeled model Hg-compounds were used to measure rates of both methylmercury (MeHg) production and degradation by bacteria. While all sites and depths had similar total-Hg concentrations (0.3-0.6 ppm), and geochemical signatures of mining debris (as )Nd, range: -3.08 to -4.37), in-situ MeHg was highest in the marsh (5.4Dž.5 ppb) and А.7 ppb in all open-water sites. Microbial MeHg production (potential rate) in 0-4 surface sediments was also highest in the marsh (3.1 ng g-1 wet sediment day-1) and below detection (<0.06 ng g-1 wet sediment day-1) in open-water locations. The marsh exhibited a methylation/demethylation (M/D) ratio more than 252 that of all open-water locations. Only below the surface 0-4-cm horizon was significant MeHg production potential evident in the open-water sediment profile (0.2-1.1 ng g-1 wet sediment day-1). In-situ Hg methylation rates, calculated from radiotracer rate constants, and in-situ inorganic Hg(II) concentrations compared well with potential rates. However, similarly calculated in-situ rates of MeHg degradation were much lower than potential rates. These preliminary data indicate that wetlands surrounding San Pablo Bay represent important zones of MeHg production, more so than similarly Hg-contaminated adjacent open-water areas. This has significant implications for this and other Hg-impacted systems, where wetland expansion is currently planned.  相似文献   

9.
Ambient air and coarse, fine and particulate-bound mercury (Hg(p)) pollutants were collected and analyzed from March 17 to May 22 and September 3, 2009 to March 5, 2010 at a highway traffic site located in Sha-Lu, central Taiwan. This study has the following objectives: (1) to measure the coarse and fine particulates concentrations and the particulate-bound mercury Hg(p) which was attached to these particulate; (2) to determine the average Hg(p) compositions in coarse and fine particulates and (3) to compare the Hg(p) concentrations and compositions particulate in this study to the those obtained in other studies. The results obtained in this study indicated that the average ambient air PM2.5, PM2.5–10 and PM10 were 18.79 ± 6.71, 11.22 ± 4.93 and 30.01 ± 10.27 μg/m3, respectively. The ranges of concentrations for Hg(p) in PM2.5 were from 0.0016 to 0.0557 ng/m3, from 0.0006 to 0.0364 ng/m3 in PM2.5–10 and from 0.0022 to 0.0862 ng/m3 in PM10. In addition, the highest particle-bound mercury compositions in PM2.5 were 16.85 ng/g and the lowest particle-bound mercury concentrations were 0.55 ng/g. The highest particle-bound mercury compositions in PM2.5–10 were 13.88 ng/g and the lowest particle-bound mercury in PM2.5–10 were 0.22 ng/g.  相似文献   

10.
Microbial mercury (Hg) methylation and methylmercury (MeHg) degradation processes were examined using radiolabled model Hg compounds in San Francisco Bay-Delta surface sediments during three seasonal periods: late winter, spring, and fall. Strong seasonal and spatial differences were evident for both processes. MeHg production rates were positively correlated with microbial sulfate reduction rates during late winter only. MeHg production potential was also greatest during this period and decreased during spring and fall. This temporal trend was related both to an increase in gross MeHg degradation, driven by increasing temperature, and to a build-up in pore water sulfide and solid phase reduced sulfur driven by increased sulfate reduction during the warmer seasons. MeHg production decreased sharply with depth at two of three sites, both of which exhibited a corresponding increase in reduced sulfur compounds with depth. One site that was comparatively oxidized and alkaline exhibited little propensity for net MeHg production. These results support the hypothesis that net MeHg production is greatest when and where gross MeHg degradation rates are low and dissolved and solid phase reduced sulfur concentrations are low.  相似文献   

11.
In this paper, the relationship between sulfate reduction potential and mercury methylation potential was studied in the Aha, Baihua and Hongfeng reservoirs from Guiyang City. The methylmercury (MeHg) concentrations of lake water in the Aha Reservoir were greatly elevated as compared to those of the Hongfeng and Baihua reservoirs, which was correlated with its distinctly high SRB abundance, SO42-, and S2- concentrations. Among the three reservoirs, however, the highest MeHg was observed in in the top several centimenters of pore water profile in the Hongfeng Reservoir where the lowest S2- in pore water occurred. The distributions of MeHg in lake water and pore water showed the highest methylation potential occurred at water-sediment surface for the Aha Reservoir and the in the top several centimenters of sediments for the Hongfeng Reservoir. It is guessed that the highest mercury methylation only occurs at the sites with certain sulfide concentrations.  相似文献   

12.
The 26 December 2004 tsunami covered significant portion of a coastal zone with a blanket of potentially contaminated sediments. In this report are presented results on mercury concentrations in sediments deposited by the tsunami in a coastal zone of Thailand. Since the total mercury concentrations are insufficient to assess mercury mobility and bioavailability in sediment, its fractionation was applied. Sediments were sampled within 50 days after the event and analyzed by sequential extraction method. The procedure of sequential extraction involved five subsequent stages performed with solutions of chloroform, deionized water, 0.5 M HCl, 0.2 M NaOH, and aqua regia. The mean concentration of total mercury in sediments was 119 ± 50 ng g−1 dry mass (range 66–230). The fractionation revealed that mercury is mainly bound to the least bioavailable sulphides 75 ± 6% (range 62–86), organomercury compounds 14 ± 7% (range 4–26), and humic matter 9 ± 7% (range 1–27). The lowest contributions bring fractions of water-soluble mercury 0.8 ± 1.0% (range 0.1–3.6) and acid soluble mercury 0.9 ± 0.5% (range 0.2–2.1). Although, the total mercury content is similar in a reference sample and in the tsunami sediments, the highly toxic organomercury fraction contribution is higher in the latter. The results were compared with chemical and sedimentological properties of the sediments but no significant correlations were obtained between them.  相似文献   

13.
Mercury (Hg) and methylmercury (CH3Hg+) concentrations in streambed sediment and water were determined at 27 locations throughout the Sacramento River Basin, CA. Mercury in sediment was elevated at locations downstream of either Hg mining or Au mining activities where Hg was used in the recovery of Au. Methylmercury in sediment was highest (2.84 ng/g) at a location with the greatest wetland land cover, in spite of lower total Hg at that site relative to other river sites. Mercury in unfiltered water was measured at 4 locations on the Sacramento River and at tributaries draining the mining regions, as well as agricultural regions. The highest levels of Hg in unfiltered water (2248 ng/l) were measured at a site downstream of a historic Hg mining area, and the highest levels at all sites were measured in samples collected during high streamflow when the levels of suspended sediment were also elevated. Mercury in unfiltered water exceeded the current federal and state recommended criterion for protection of aquatic life (50 ng/l as total Hg in unfiltered water) only during high streamflow conditions. The highest loading of Hg to the San Francisco Bay system was attributed to sources within the Cache Creek watershed, which are downstream of historic Hg mines, and to an unknown source or sources to the mainstem of the Sacramento River upstream of historic Au mining regions. That unknown source is possibly associated with a volcanic deposit. Methylmercury concentrations also were dependent on season and hydrologic conditions. The highest levels (1.98 ng/l) in the Sacramento River, during the period of study, were measured during a major flood event. The reactivity of Hg in unfiltered water was assessed by measuring the amount available for reaction by a strong reducing agent. Although most Hg was found to be nonreactive, the highest reactivity (7.8% of the total Hg in water) was measured in the sample collected from the same site with high CH3Hg+ in sediment, and during the time of year when that site was under continual flooded conditions. Although Hg concentrations in water downstream of the Hg mining operations were measured as high as 2248 ng/l during stormwater runoff events, the transported Hg was found to have a low potential for geochemical transformations, as indicated by the low reactivity to the reducing agent (0.0001% of the total), probably because most of the Hg in the unfiltered water sample was in the mercury sulfide form.  相似文献   

14.
Spatial variation in mercury (Hg) and methylmercury (MeHg) bioaccumulation in urban coastal watersheds reflects complex interactions between Hg sources, land use, and environmental gradients. We examined MeHg concentrations in fauna from the Delaware River estuary, and related these measurements to environmental parameters and human impacts on the waterway. The sampling sites followed a north to south gradient of increasing salinity, decreasing urban influence, and increasing marsh cover. Although mean total Hg in surface sediments (top 4 cm) peaked in the urban estuarine turbidity maximum and generally decreased downstream, surface sediment MeHg concentrations showed no spatial patterns consistent with the examined environmental gradients, indicating urban influence on Hg loading to the sediment but not subsequent methylation. Surface water particulate MeHg concentration showed a positive correlation with marsh cover whereas dissolved MeHg concentrations were slightly elevated in the estuarine turbidity maximum region. Spatial patterns of MeHg bioaccumulation in resident fauna varied across taxa. Small fish showed increased MeHg concentrations in the more urban/industrial sites upstream, with concentrations generally decreasing farther downstream. Invertebrates either showed no clear spatial patterns in MeHg concentrations (blue crabs, fiddler crabs) or increasing concentrations further downstream (grass shrimp). Best-supported linear mixed models relating tissue concentration to environmental variables reflected these complex patterns, with species specific model results dominated by random site effects with a combination of particulate MeHg and landscape variables influencing bioaccumulation in some species. The data strengthen accumulating evidence that bioaccumulation in estuaries can be decoupled from sediment MeHg concentration, and that drivers of MeHg production and fate may vary within a small region.  相似文献   

15.
The concentrations of typical organochlorine pesticides (OCPs) (DDTs, HCHs, PCP-Na, and HCB) were measured to understand distribution and source of OCPs in surface and columnar sediments of Poyang Lake in 2006. And OCPS concentrations in surface sediment in 2017 were made a comparison with those in 2006 at several same sampling sites. OCPs showed higher concentrations in main stream than in river mouths (entrance of river flow into lake) of the lake. The average concentrations of HCHs and DDTs were 4.63 ± 3.86 and 20.15 ± 26.86 ng/g in surface sediments in 2006, respectively. Concentrations of OCPs in 2017 were lower than in 2006, such as HCHs average 1.98 ± 2.04 ng/g and DDTs average 4.87 ± 1.48 ng/g in 2017, indicating historical residual and degradation. The primary isomers of HCHs and DDTs in the lake were α-HCH, γ-HCH and p,p′-DDD, respectively. HCHs were from historical residual and lindane application. DDTs were from historical residual. PCP-Na total concentrations in surface sediment were 77.36 ng/g in 2006 and 44.04 ng/g in 2017. The concentration of HCB residues in surface sediment was 0.92 ± 0.90 ng/g in 2006 and 0.42 ± 0.38 ng/g in 2017. The concentrations of OCPs in columnar sediments showed annual variations, and the peak concentrations occurred in 1953, 1961, 1974, 1982, and 1995, showing close relations with onset of production OCPs pesticide in 1950s and its later prohibition in 1980s and a large number agricultural cultivated land decrease in 1990s in China. The concentrations of HCB in columnar sediments were average 2.33 ± 1.26 ng/g. OCPs of columnar sediments were from historical residues and lindane input. The main contamination of OCPs was PCP-Na and p,p′-DDD in Poyang Lake. On the whole, the combination of surface samples (0–5 cm in depth) and columnar samples (0–38 cm in depth) in a single study would give insight into OCPs pollution levels in different years (temporal resolution) and in different regions (spatial resolution) in Poyang Lake.  相似文献   

16.
The aim of this study was to evaluate Hg distribution in mangrove plants and changes of Hg content during leaf aging; the contribution of litterfall to Hg enrichment in mangrove ecosystems is also discussed. Contents of total Hg (THg) and methylmercury (MeHg) in mangrove plants and sediments were determined. Contents of THg and MeHg in the sediments were 225 ± 157 ng/g and 0.800 ± 0.600 ng/g. Concentrations of THg and MeHg in the mangrove plants were 1760 ± 1885 ng/g and 0.721 ± 0.470 ng/g (dry weight), respectively, which were much higher than those in terrestrial plants. Enrichment of THg in mangrove plants was different, following the order Rhizophra apiculata > Rhizophora stylosa > Kandelia candel > Aegiceras corniculatum > Avicennia marina; while MeHg contents in mangrove plants decreased in the order of R. stylosa > K. candel > A. corniculatum > R. apiculata > A. marina. There were obvious interspecies differences, regional differences, individual differences and tissue differences between THg and MeHg contents of mangrove plants, all of which were closely related to the environmental and the physiological characteristics of mangrove plants. In juvenile leaves, mature leaves and leaf litter, THg contents ranged 55.3-1760 ng/g, 204-1800 ng/g, and 385-2130 ng/g (dry weight), respectively; MeHg contents ranged 0.17-2.39 ng/g, 0.01-1.28 ng/g, and 0.13-1.47 ng/g (dry weight), respectively. Except for A. corniculatum and Bruguier gymnorrhiza, THg content of mature leaves was always higher than that in juvenile leaves, but MeHg showed a contrasting trend. THg content of litter leaves was between that of juvenile leaves and mature leaves, while MeHg content was generally lower than that of juvenile leaves and mature leaves. In the mangrove ecosystem, Hg enrichment contributed by the litterfall decreased in the order of K. candel > A. corniculatum > A. marina.  相似文献   

17.
The role of the major biogeochemical processes in Hg cycling at the sediment–water interface was investigated in the Grado Lagoon (Northern Adriatic Sea). This wetland system has been extensively contaminated from the Idrija Hg Mine (Slovenia) through the Isonzo River suspended load carried by tidal fluxes. Three approaches were used to study the sediment–water exchange of total Hg (THg), methylmercury (MeHg), reactive Hg (RHg) and dissolved gaseous Hg (DGHg): (1) estimation of diffusive fluxes from porewater and overlying water concentrations, (2) measurements of benthic fluxes using a deployed light benthic chamber in situ and (3) measurements of benthic fluxes during oxic–anoxic transition with a laboratory incubation experiment. The THg solid phase, ranging between 9.5 and 14.4 μg g−1, showed slight variability with depth and time. Conversely, MeHg contents were highest (up to 21.9 ng g−1) at the surface; they tended to decrease to nearly zero concentration with depth, thus suggesting that MeHg production and accumulation occur predominantly just below the sediment–water interface. Porewater MeHg concentrations (0.9–7.9 ng L−1, 0.15–15% of THg) varied seasonally; higher contents were observed in the warmer period. The MeHg diffusive fluxes (up to 17 ng m−2 day−1) were similar to those in the nearby Gulf of Trieste [Covelli, S., Horvat, M., Faganeli, J., Brambati, A., 1999. Porewater distribution and benthic flux of mercury and methylmercury in the Gulf of Trieste (Northern Adriatic Sea). Estuar. Coast. Shelf Sci. 48, 415–428], although the lagoon sediments contained four-fold higher THg concentrations. Conversely, the THg diffusive fluxes in the lagoon (up to 110 ng m−2 day−1) were one- to two-fold higher than those previously estimated for the Gulf of Trieste. The diurnal MeHg benthic fluxes were highest in summer at both sites (41,000 and 33,000 ng m−2 day−1 at the fishfarm and in the open lagoon, respectively), thus indicating the influence of temperature on microbial processes. The diurnal variations of dissolved THg and especially MeHg were positively correlated with O2 and inversely with DIC, suggesting an important influence of benthic photosynthetic activities on lagoon benthic Hg cycling, possibly through the production of organic matter promptly available for methylation. The results from the dark chamber incubated in the laboratory showed that the regeneration of dissolved THg was slightly affected by the oxic–anoxic transition. Conversely, the benthic flux of MeHg was up to 15-fold higher in sediments overlain by O2 depleted waters. In the anoxic phase, the MeHg fluxes proceeded in parallel with Fe fluxes and the methylated form reached approximately 100% of dissolved THg. The MeHg is mostly released into overlying water (mean recycling efficiency of 89%) until the occurrence of sulphide inhibition, due to scavenging of the available Hg substrate for methylation. The results suggest that sediments in the Grado Lagoon, especially during anoxic events, should be considered as a primary source of MeHg for the water column.  相似文献   

18.
《Applied Geochemistry》2006,21(11):1969-1985
Gossan Creek, a headwater stream in the SE Upsalquitch River watershed in New Brunswick, Canada, contains elevated concentrations of total Hg (HgT up to 60 μg/L). Aqueous geochemical investigations of the shallow groundwater at the headwaters of the creek confirm that the source of Hg is a contaminated groundwater plume (neutral pH with Hg and Cl concentrations up to 150 μg/L and 20 mg/L, respectively), originating from the Murray Brook mine tailings, that discharges at the headwaters of the creek. The discharge area of the contaminant plume was partially delineated based on elevated pH and Cl concentrations in the groundwater. The local groundwater outside of the plume contains much lower concentrations of Hg and Cl (<0.1 μg/L and 3.8 mg/L, respectively) and displays the chemical characteristics of an acid-sulfate weathering system, with low pH (4.1–5.5) and elevated concentrations of Cu, Zn, Pb and SO4 (up to 5400 μg Cu/L, 8700 μg Zn/L, 70 μg Pb/L and 330 mg SO4/L), derived from oxidation of sulfide minerals in the Murray Brook volcanogenic massive sulfide deposit and surrounding bedrock. The HgT mass loads measured at various hydrologic control points along the stream system indicate that 95–99% of the dissolved HgT is attenuated in the first 3–4 km from the source. Analyses of creek bed sediments for Au, Ag, Cu, Zn, Pb and Hg indicate that these metals have partitioned strongly to the sediments. Mineralogical investigations of the contaminated sediments using analytical scanning electron microscopy (SEM), transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM), reveal discrete particles (<1–2 μm) of metacinnabar (HgS), mixed Au–Ag–Hg amalgam, Cu sulfide and Ag sulfide.  相似文献   

19.
Density stratification in saline and hypersaline water bodies from throughout the world can have large impacts on the internal cycling and loading of salinity, nutrients, and trace elements. High temporal resolution hydroacoustic and physical/chemical data were collected at two sites in Great Salt Lake (GSL), a saline lake in the western USA, to understand how density stratification may influence salinity and mercury (Hg) distributions. The first study site was in a causeway breach where saline water from GSL exchanges with less saline water from a flow restricted bay. Near-surface-specific conductance values measured in water at the breach displayed a good relationship with both flow and wind direction. No diurnal variations in the concentration of dissolved (<0.45 μm) methylmercury (MeHg) were observed during the 24-h sampling period; however, the highest proportion of particulate Hgtotal and MeHg loadings was observed during periods of elevated salinity. The second study site was located on the bottom of GSL where movement of a high-salinity water layer, referred to as the deep brine layer (DBL), is restricted to a naturally occurring 1.5-km-wide “spillway” structure. During selected time periods in April/May, 2012, wind-induced flow reversals in a railroad causeway breach, separating Gunnison and Gilbert Bays, were coupled with high-velocity flow pulses (up to 55 cm/s) in the DBL at the spillway site. These flow pulses were likely driven by a pressure response of highly saline water from Gunnison Bay flowing into the north basin of Gilbert Bay. Short-term flow reversal events measured at the railroad causeway breach have the ability to move measurable amounts of salt and Hg from Gunnison Bay into the DBL. Future disturbance to the steady state conditions currently imposed by the railroad causeway infrastructure could result in changes to the existing chemical balance between Gunnison and Gilbert Bays. Monitoring instruments were installed at six additional sites in the DBL during October 2012 to assess impacts from any future modifications to the railroad causeway.  相似文献   

20.
We present here the first mercury speciation study in the water column of the Southern Ocean, using a high-resolution south-to-north section (27 stations from 65.50°S to 44.00°S) with up to 15 depths (0-4440 m) between Antarctica and Tasmania (Australia) along the 140°E meridian. In addition, in order to explore the role of sea ice in Hg cycling, a study of mercury speciation in the “snow-sea ice-seawater” continuum was conducted at a coastal site, near the Australian Casey station (66.40°S; 101.14°E). In the open ocean waters, total Hg (HgT) concentrations varied from 0.63 to 2.76 pmol L−1 with “transient-type” vertical profiles and a latitudinal distribution suggesting an atmospheric mercury source south of the Southern Polar Front (SPF) and a surface removal north of the Subantartic Front (SAF). Slightly higher mean HgT concentrations (1.35 ± 0.39 pmol L−1) were measured in Antarctic Bottom Water (AABW) compared to Antarctic Intermediate water (AAIW) (1.15 ± 0.22 pmol L−1). Labile Hg (HgR) concentrations varied from 0.01 to 2.28 pmol L−1, with a distribution showing that the HgT enrichment south of the SPF consisted mainly of HgR (67 ± 23%), whereas, in contrast, the percentage was half that in surface waters north of PFZ (33 ± 23%). Methylated mercury species (MeHgT) concentrations ranged from 0.02 to 0.86 pmol L−1. All vertical MeHgT profiles exhibited roughly the same pattern, with low concentrations observed in the surface layer and increasing concentrations with depth up to an intermediate depth maximum. As for HgT, low mean MeHgT concentrations were associated with AAIW, and higher ones with AABW. The maximum of MeHgT concentration at each station was systematically observed within the oxygen minimum zone, with a statistically significant MeHgTvs Apparent Oxygen Utilization (AOU) relationship (p < 0.001). The proportion of HgT as methylated species was lower than 5% in the surface waters, around 50% in deep waters below 1000 m, reaching a maximum of 78% south of the SPF. At Casey coastal station HgT and HgR concentrations found in the “snow-sea ice-seawater” continuum were one order of magnitude higher than those measured in open ocean waters. The distribution of HgT there suggests an atmospheric Hg deposition with snow and a fractionation process during sea ice formation, which excludes Hg from the ice with a parallel Hg enrichment of brine, probably concurring with the Hg enrichment of AABW observed in the open ocean waters. Contrastingly, MeHgT concentrations in the sea ice environment were in the same range as in the open ocean waters, remaining below 0.45 pmol L−1. The MeHgT vertical profile through the continuum suggests different sources, including atmosphere, seawater and methylation in basal ice. Whereas HgT concentrations in the water samples collected between the Antarctic continent and Tasmania are comparable to recent measurements made in the other parts of the World Ocean (e.g., Soerensen et al., 2010), the Hg species distribution suggests distinct features in the Southern Ocean Hg cycle: (i) a net atmospheric Hg deposition on surface water near the ice edge, (ii) the Hg enrichment in brine during sea ice formation, and (iii) a net methylation of Hg south of the SPF.  相似文献   

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