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1.
To understand the geochemical cycle of Hg in hypereutrophic freshwater lake, two sampling campaigns were conducted in Lake Taihu in China during May and September of 2009. The concentrations of unfiltered total Hg (unfTHg) were in the range of 6.8–83 ng L−1 (28 ± 18 ng L−1) in the lake water and total Hg in the sediment was 12–470 ng g−1, both of which are higher than in other background lakes. The concentration of unfTHg in ∼11% of the lake water samples exceeded the second class of the Chinese environmental standards for surface water of 50 ng L−1 (GB 3838-2002), indicating that a high ecological risk is posed by the Hg in Lake Taihu. However, the concentrations of unfiltered total MeHg (unfMeHg) were relatively low in the lake water (0.14 ± 0.05 ng L−1, excluding two samples with 0.81 and 1.0 ng L−1). Lake sediment MeHg varied from 0.2–0.96 ng g−1, with generally low ratios of MeHg/THg of <1%. The low concentrations of TMeHg in the lake water may have resulted from a strong uptake by the high primary productivity and the demethylation of MeHg in oxic conditions. In addition, contrary to the results of previous research conducted in deep-water lakes and reservoirs, the low concentrations of MeHg and low ratio of MeHg/THg in the lake sediment indicates that the net methylation of Hg was not accelerated by the elevated organic matter load created by the eutrophication of Lake Taihu. The results also showed that sediments were a source of THg and MeHg in the water. Higher diffusion fluxes of THg and MeHg may be partly responsible for the higher concentrations of THg in the lake water in May, 2009.  相似文献   

2.
The Xunyang Hg mine (XMM) situated in Shaanxi Province is an active Hg mine in China. Gaseous elemental Hg (GEM) concentrations in ambient air were determined to evaluate its distribution pattern as a consequence of the active mining and retorting in the region. Total Hg (HgT) and methylmercury (MeHg) concentrations in riparian soil, sediment and rice grain samples (polished) as well as Hg speciation in surface water samples were measured to show local dispersion of Hg contamination. As expected, elevated concentrations of GEM were found, ranging from 7.4 to 410 ng m−3. High concentrations of HgT and MeHg were also obtained in riparian soils, ranged from 5.4 to 120 mg kg−1 and 1.2 to 11 μg kg−1, respectively. Concentrations of HgT and MeHg in sediment samples varied widely from 0.048 to 1600 mg kg−1 and 1.0 to 39 μg kg−1, respectively. Surface water samples showed elevated HgT concentrations, ranging from 6.2 to 23,500 ng L−1, but low MeHg concentrations, ranging from 0.022 to 3.7 ng L−1. Rice samples exhibited high concentrations of 50–200 μg kg−1 in HgT and of 8.2–80 μg kg−1 in MeHg. The spatial distribution patterns of Hg speciation in the local environmental compartments suggest that the XMM is the source of Hg contaminations in the study area.  相似文献   

3.
Water samples were collected during normal flow (2007) and during a drought period (2008) from five rivers and tributaries draining the Wanshan Hg mining district, Guizhou, China. Unfiltered methylmercury (MeHg) as well as particulate and dissolved fractions of MeHg (P-MeHg, D-MeHg) were measured to assess the spatial and temporal variation of MeHg contamination in the local river system. Most locations (about 80%) displayed higher MeHg concentrations during drought period than during normal discharge conditions. Concentrations of MeHg during the drought period ranged from <0.035 to 11 ng L−1 (geometric mean: 0.43), while during normal flow the concentrations ranged from <0.035 to only 3.4 ng L−1 (geometric mean: 0.21). Concentrations of MeHg were positively correlated with total Hg (THg) concentrations (R2 = 0.20–0.58, P < 0.001) and inversely related to distance from the calcines, during both sampling periods (R2 = 0.34 and 0.23, P < 0.001, for low and normal flow, respectively) indicating that calcines may be important sources of MeHg to the downstream environment. Approximately 39% of MeHg was bound to particulates and the rest was transported in the dissolved phase along stretches of the entire river, which was different from THg, as this was mainly transported bound to particulates (commonly more than 80%).  相似文献   

4.
The Wanshan Hg mining area in Guizhou, China, was one of the world’s largest Hg producing regions. Numerous mine-waste and calcines still remain, leaching Hg to local rivers and streams and potentially impacting the local population. Several studies have been published on local environmental impacts of these mining and retorting residues, but a comprehensive, regional survey on the distribution of Hg in the rivers in the region, as presented in this paper, has not previously been conducted. This study focuses on the regional distribution and temporal variation of aqueous Hg fractions in the five main watercourses draining the Wanshan Hg mining and retorting area, covering more than 700 km2. Three sampling campaigns were carried out in 2007 and 2008, covering high flow, normal flow and low flow periods. Total (THg), particulate (PHg), dissolved (DHg) and reactive (RHg) Hg fractions were determined. All rivers had the highest Hg concentrations at sample sites about 100–500 m downstream of the mine wastes. Total Hg concentrations ranged from extremely high (up to 12,000 ng L−1) at the sample site just 100 m below mine wastes, to quite low in tributary streams (1.9 ng L−1, about 14 km downstream of the mine wastes). Total Hg and PHg concentrations were usually highest during high flow periods in the Hg-contaminated areas (i.e. THg ? 50 ng L−1), while in the less-impacted downstream areas (with THg < 50 ng L−1) the Hg concentrations were usually lowest during high flow periods. Although highly elevated concentrations of Hg in water samples were found just downstream of the mine wastes, the concentrations decreased sharply to well below 50 ng L−1 (US EPA Hg concentration standard for protection of fresh water), within only 6–8 km downstream. Concentrations of THg were highly dominated by and correlated with PHg (R2 = 0.996–0.999, P < 0.001); PHg constituted more than 80% of THg in Hg-contaminated areas, and could account for 99.6% of the THg close to the mine wastes.  相似文献   

5.
Mercury fluxes from air/surface interfaces in paddy field and dry land   总被引：3，自引：0，他引：3  
In order to provide insight into the characteristics of Hg exchange in soil/water-air surface from cropland (including paddy field and dry land), Hg fluxes were measured in Chengjiang. Mercury fluxes were measured using the dynamic flux chamber method, coupled with a Lumex® multifunctional Hg analyzer RA-915+ (Lumex Ltd., Russia). The Hg fluxes from paddy field and dry land were alternatively measured every 30 min. Data were collected for 24-48 h once per month for 5 months. Mercury fluxes in both fields were synchronously measured under the same conditions to compare Hg emissions between paddy field and dry land over diurnal and seasonal periods and find out what factors affect Hg emission on each surface. These results indicated that air Hg concentrations at the monitoring site was double the value observed at the global background sites in Europe and North America. The Hg release fluxes were 46.5 ± 22.8 ng m−2 h−1 in the warm season, 15.5 ± 18.8 ng m−2 h−1 in the cold season for dry land, and 23.8 ± 15.6 ng m−2 h−1 in the warm season, 6.3 ± 11.9 ng m−2 h−1 in the cold season for paddy field. Solar radiation is important in the emission of Hg over both sites. Hg exchange at the soil/air and water/air interfaces showed temporal variations. The amount of Hg emission from dry land was higher than that from the paddy field, and the emission in daytime was higher than that at night. Moreover, Hg emissions from land covered by crops, was lower than that for bare land.  相似文献   

6.
Mercury air/surface exchange was measured over litter-covered soils with low Hg concentrations within various types of forests along the eastern seaboard of the USA. The fieldwork was conducted at six forested sites in state parks in South Carolina, North Carolina, New Jersey, Pennsylvania, New York and Maine from mid-May to early June 2005. The study showed that the Hg air/surface exchange was consistently very low and similar (overall daytime mean flux = 0.2 ± 0.9 ng m−2 h−1, n = 310, for all six sites monitored) with the various forest types. These flux values are comparable with those found in a year-long study in Tennessee (yearly daytime mean = 0.4 ± 0.5 ng m−2 h−1), but lower than many previous flux results reported for background soils. The Hg fluxes at all sites oscillated around zero, with many episodes of deposition (negative fluxes) occurring in both daytime and nighttime. While there were particular days showing significant correlations among the Hg air/surface exchange and certain environmental parameters, perhaps because of the low fluxes encountered, few significant correlations were found for any particular day of sampling between the Hg flux and environmental parameters such as solar radiation, soil temperature, air temperature (little variability seen), relative humidity, and ambient air Hg concentrations. Factors driving the Hg exchange as previously found for enriched soils may not hold for these background litter-covered forest soils. The results suggest that spatial variations of the Hg air/surface exchange were small among these different forest types for this particular time of year.  相似文献   

7.
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   

8.
The Dvurechenskii mud volcano (DMV) is located in permanently anoxic waters at 2060 m depth (Sorokin Trough, Black Sea). The DMV was studied during the RV Meteor expedition M72/2 as an example of an active mud volcano system, to investigate the significance of submarine mud volcanism for the methane and sulfide budget of the anoxic Black Sea hydrosphere. Our studies included benthic fluxes of methane and sulfide, as well as the factors controlling transport, consumption and production of both compounds within the sediment. The pie-shaped mud volcano showed temperature anomalies as well as solute and gas fluxes indicating high fluid flow at its summit north of the geographical center. The anaerobic oxidation of methane (AOM) coupled to sulfate reduction (SR) was repressed in this zone due to the upward flow of sulfate-depleted fluids through recently deposited subsurface muds, apparently limiting microbial methanotrophic activity. Consequently, the emission of dissolved methane into the water column was high, with an estimated rate of 0.46 mol m−2 d−1. On the wide plateau and edge of the mud volcano surrounding the summit, fluid flow and total methane flux were lower, allowing higher SR and AOM rates correlated with an increase in sulfate penetration into the sediment. Here, between 50% and 70% of the methane flux (0.07-0.1 mol m−2 d−1) was consumed within the upper 10 cm of the sediment. The overall amount of dissolved methane released from the entire mud volcano structure into the water column was significant with a discharge of 1.3 × 107 mol yr−1. The DMV maintains also high areal rates of methane-fueled sulfide production and emission of on average 0.05 mol m−2 d−1. This is a difference to mud volcanoes in oxic waters, which emit similar amounts of methane, but not sulfide. However, based on a comparison of this and other mud volcanoes of the Black Sea, we conclude that sulfide and methane emission into the hydrosphere from deep-water mud volcanoes does not significantly contribute to the sulfide and methane inventory of the Black Sea.  相似文献   

9.
Gaseous elemental mercury (GEM) and reactive gaseous mercury (RGM) were measured over 2-week seasonal field campaigns near Salmon Falls Creek Reservoir in south-central Idaho from the summer of 2005 through the fall of 2006 and over the entire summer of 2006 using automated Tekran Hg analyzers. GEM, RGM, and particulate Hg (HgP) were also measured at a secondary site 90 km to the west in southwestern Idaho during the summer of 2006. The study was performed to characterize Hg air concentrations in the southern Idaho area for the first time, estimate Hg dry deposition rates, and investigate the source of observed elevated concentrations. High seasonal variability was observed with the highest GEM (1.91 ± 0.9 ng m−3) and RGM (8.1 ± 5.6 pg m−3) concentrations occurring in the summer and lower values in the winter (1.32 ± 0.3 ng m−3, 3.2 ± 2.9 pg m−3 for GEM, RGM, respectively). The summer-average HgP concentrations were generally below detection limit (0.6 ± 1 pg m−3). Seasonally averaged deposition velocities calculated using a resistance model were 0.034 ± 0.032, 0.043 ± 0.040, 0.00084 ± 0.0017 and 0.00036 ± 0.0011 cm s−1 for GEM (spring, summer, fall and winter, respectively) and 0.50 ± 0.39, 0.40 ± 0.31, 0.51 ± 0.43 and 0.76 ± 0.57 cm s−1 for RGM. The total annual RGM + GEM dry deposition estimate was calculated to be 11.9 ± 3.3 μg m−2, or about 2/3 of the total (wet + dry) deposition estimate for the area. Periodic elevated short-term GEM (2.2–12 ng m−3) and RGM (50–150 pg m−3) events were observed primarily during the warm seasons. Back-trajectory modeling and PSCF analysis indicate predominant source directions to the SE (western Utah, northeastern Nevada) and SW (north-central Nevada) with fewer inputs from the NW (southeastern Oregon and southwestern Idaho).  相似文献   

10.
Atmospheric mercury deposition on snow at springtime has been reported in polar regions, potentially posing a threat to coastal and inland ecosystems receiving meltwaters. However, the post-depositional fate of Hg in snow is not well known, and no data are available on Hg partitioning in polar snow. During snowmelt, we conducted a survey of Hg concentrations, partitioning and speciation in surface snow and at depth, over sea ice and over land along a 100 km transect across Cornwallis Island, NU, Canada. Total Hg concentrations [THg] in surface snow were low (less than 20 pmol L−1) and were significantly higher in marine vs. inland environments. Particulate Hg in surface snow represented up to 90% of total Hg over sea ice and up to 59% over land. At depth, [THg] at the snow/sea ice interface (up to 300 pmol L−1) were two orders of magnitude higher than at the snow/lake ice interface (ca. 2.5 pmol L−1). Integrated snow columns, sampled over sea-ice and over land, showed that particulate Hg was mostly bound to particles ranging from 0.45 to 2.7 μm. Moreover, melting snowpacks over sea ice and over lake ice contribute to increase [THg] at the water/ice interfaces. This study indicates that, at the onset of snowmelt, most of the Hg in snow is in particulate form, particularly over sea ice. Low Hg levels in surface snow suggest that Hg deposited through early spring deposition events is partly lost to the atmosphere from the snowpack before snowmelt. The sea ice/snow interface may constitute a site for Hg accumulation, however. Further understanding of the cycling of mercury at the sea ice/snow and sea ice/seawater interfaces is thus warranted to fully understand how mercury enters the arctic food webs.  相似文献   

11.
《Applied Geochemistry》2006,21(11):1855-1867
Methylmercury (MeHg) and total Hg (THg) concentrations in soil profiles were monitored in the Thur River basin (Alsace, France), where a chlor-alkali plant has been located in the city of Vieux-Thann since the 1930s. Three soil types were studied according to their characteristics and location in the catchment: industrial soil, grassland soil and alluvial soil. Contamination of MeHg and THg in soil was important in the vicinity of the plant, especially in industrial and alluvial soil. Concentrations of MeHg reached 27 ng g−1 and 29,000 ng g−1 for THg, exceeding the predictable no effect concentration. Significant ecotoxicological risk exists in this area and remedial actions on several soil types are suggested. In each type of soil, MeHg concentrations were highest in topsoil, which decreased with depth. Concentrations of MeHg were negatively correlated with soil organic matter and total S, particularly when MeHg concentrations exceeded 8 ng g−1. Under these conditions, MeHg concentrations in soil seemed to be influenced by THg, soil organic matter and total S concentrations. It was found that high MeHg/THg ratios (near 2%) in soil were mainly related to the combined soil environmental conditions such as low THg concentrations, low organic C/N ratios (<11) and relatively low pH (5–5.5). Nevertheless, even when the MeHg/THg ratio was low (∼0.04%), MeHg and THg concentrations were elevated, up to 13 ng g−1 and to 29,000 ng g−1, respectively. Thus, both THg and MeHg concentrations should be taken into account to assess potential environmental risks of Hg.  相似文献   

12.
Brazil has extensive sugar cane monocultures, which significantly alter hydrogeochemical material fluxes. We studied dissolved organic matter (OM) fluxes in the Manguaba lagoon-estuary system, which drains a sugar cane monoculture-dominated hinterland and discharges into the Atlantic coastal ocean. The OM fluxes into the lagoon originate from baseflow, field runoff and sugar cane factory effluents. In the study, dissolved organic carbon (DOC) concentration, δ13C DOC and UV absorbance were analysed along a freshwater-seawater salinity gradient that encompasses river (DOC 9-11 mg l−1, δ13C −22.2‰ to −25.5‰); lagoon (4-11 mg l−1, −20.5‰ to −24.8‰); estuary (3-9 mg l−1, −22.6‰ to −25.3‰) and coastal waters (1.64 mg l−1, −21‰) with different intra-seasonal runoff conditions. We used the carbon isotope data to quantify the sugar cane derived DOC. Where river water meets brackish lagoon water, substantial loss of DOC occurs during rainy conditions, when suspended sediment from eroded fields in the river is very high. During dry weather, at much lower suspension levels, DOC increases, however, presumably from addition of photolysed resuspended sedimentary OM. In the estuary, mixing of DOC is strictly conservative. Ca. 1/3 of riverine DOM discharged into the lagoon has a sugar cane source. Within the lagoon on avg. 20% of the bulk DOM is comprised of sugar cane DOM, whereas during heavy rainfall the amount increases to 31%, due to intensified drainage flow and soil erosion. In the estuary, 14-26% is of sugar cane origin. The sugar cane-derived component follows the mixing patterns of bulk DOM.  相似文献   

13.
Complete hydrochemical data are rarely reported for coal-mine discharges (CMD). This report summarizes major and trace-element concentrations and loadings for CMD at 140 abandoned mines in the Anthracite and Bituminous Coalfields of Pennsylvania. Clean-sampling and low-level analytical methods were used in 1999 to collect data that could be useful to determine potential environmental effects, remediation strategies, and quantities of valuable constituents. A subset of 10 sites was resampled in 2003 to analyze both the CMD and associated ochreous precipitates; the hydrochemical data were similar in 2003 and 1999. In 1999, the flow at the 140 CMD sites ranged from 0.028 to 2210 L s−1, with a median of 18.4 L s−1. The pH ranged from 2.7 to 7.3; concentrations (range in mg/L) of dissolved (0.45-μm pore-size filter) SO4 (34–2000), Fe (0.046–512), Mn (0.019–74), and Al (0.007–108) varied widely. Predominant metalloid elements were Si (2.7–31.3 mg L−1), B (<1–260 μg L−1), Ge (<0.01–0.57 μg L−1), and As (<0.03–64 μg L−1). The most abundant trace metals, in order of median concentrations (range in μg/L), were Zn (0.6–10,000), Ni (2.6–3200), Co (0.27–3100), Ti (0.65–28), Cu (0.4–190), Cr (<0.5–72), Pb (<0.05–11) and Cd (<0.01–16). Gold was detected at concentrations greater than 0.0005 μg L−1 in 97% of the samples, with a maximum of 0.0175 μg L−1. No samples had detectable concentrations of Hg, Os or Pt, and less than half of the samples had detectable Pd, Ag, Ru, Ta, Nb, Re or Sn. Predominant rare-earth elements, in order of median concentrations (range in μg/L), were Y (0.11–530), Ce (0.01–370), Sc (1.0–36), Nd (0.006–260), La (0.005–140), Gd (0.005–110), Dy (0.002–99) and Sm (<0.005–79). Although dissolved Fe was not correlated with pH, concentrations of Al, Mn, most trace metals, and rare earths were negatively correlated with pH, consistent with solubility or sorption controls. In contrast, As was positively correlated with pH.  相似文献   

14.
The continental shelf benthic iron flux and its isotope composition   总被引：1，自引：0，他引：1  
Benthic iron fluxes from sites along the Oregon-California continental shelf determined using in situ benthic chambers, range from less than 10 μmol m−2 d−1 to values in excess of ∼300 μmol m−2 d−1. These fluxes are generally greater than previously published iron fluxes for continental shelves contiguous with the open ocean (as opposed to marginal seas, bays, or estuaries) with the highest fluxes measured in the regions around the high-sediment discharge Eel River and the Umpqua River. These benthic iron fluxes do not covary with organic carbon oxidation rates in any systematic fashion, but rather seem to respond to variations in bottom water oxygen and benthic oxygen demand. We hypothesize that the highest rates of benthic iron efflux are driven, in part, by the greater availability of reactive iron deposited along these river systems as compared to other more typical continental margin settings. Bioirrigation likely plays an important role in the benthic Fe flux in these systems as well. However, the influence of bottom water oxygen concentrations on the iron flux is significant, and there appears to be a threshold in dissolved oxygen (∼60-80 μM), below which sediment-ocean iron exchange is enhanced. The isotope composition of this shelf-derived benthic iron is enriched in the lighter isotopes, and appears to change by ∼3‰ (δ56Fe) during the course of a benthic chamber experiment with a mean isotope composition of −2.7 ± 1.1‰ (2 SD, n = 9) by the end of the experiment. This average value is slightly heavier than those from two high benthic Fe flux restricted basins from the California Borderland region where δ56Fe is −3.4 ± 0.4‰ (2 SD, n = 3). These light iron isotope compositions support previous ideas, based on sediment porewater analyses, suggesting that sedimentary iron reduction fractionates iron isotopes and produces an isotopically light iron pool that is transferred to the ocean water column. In sum, our data suggest that continental shelves may export a higher efflux of iron than previously hypothesized, with the likelihood that along river-dominated margins, the benthic iron flux could well be orders of magnitude larger than non-river dominated shelves. The close proximity of the continental shelf benthos to the productive surface ocean means that this flux is likely to be essential for maintaining ecosystem micronutrient supply.  相似文献   

15.
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16.
This study focused on the development of a seasonal data set of the Hg air/surface exchange over soils associated with low Hg containing surfaces in a deciduous forest in the southern USA. Data were collected every month for 11 months in 2004 within Standing Stone State Forest in Tennessee using the dynamic flux chamber method. Mercury air/surface exchange associated with the litter covered forest floor was very low with the annual mean daytime flux being 0.4 ± 0.5 ng m−2 h−1 (n = 301). The daytime Hg air/surface exchange over the year oscillated between emission (81% of samples with positive flux) and deposition (19% of samples with negative flux). A seasonal trend of lower emission in the spring and summer (closed canopy) relative to the fall and winter (open canopy) was observed. Correlations were found between the air/surface exchange and certain environmental factors on specific days sampled but not collectively over the entire year. The very low magnitude of Hg air/surface exchange as observed in this study suggests that an improved methodology for determining and reporting emission fluxes is needed when the values of fluxes and chamber blanks are both very low and comparable. This study raises questions and points to a need for more research regarding how to scale the Hg air/surface exchange for surfaces with very low emissions.  相似文献   

17.
《Applied Geochemistry》2006,21(11):1924-1939
The Idrija Mine, the second largest Hg mine in the world, ceased operation in 1995, but still delivers large quantities of Hg downstream including into the northern Adriatic Sea, 100 km away. Transformation of Hg species in sediment in sites over 60 km from the mine, including marine sites in the Adriatic Sea, was measured to determine the ability of the system to transform and mobilize Hg and to produce methylmercury (MeHg). Cores from a freshwater impoundment, a brackish estuarine site, and three marine sites in the Gulf of Trieste were sectioned anaerobically, and Hg methylation and MeHg demethylation activities determined using radio-techniques (203Hg for methylation and 14C-MeHg for demethylation). Total and dissolved Hg and MeHg were determined as were other geochemical parameters. In addition, rates of SO4 reduction were determined in marine sediment using a 35S technique. Mercury was readily methylated and demethylated at all sites. Marine sediment was investigated in winter and summer with rates of Hg transformation and SO4 reduction corresponding only in winter. Methylation of Hg in summer displayed subsurface peaks that may have been influenced by bioturbation. Total Hg and MeHg were most abundant in the freshwater, estuarine, and near-shore marine sites, but dissolved pore water Hg and MeHg were highest in the estuarine region where S cycling appeared ideal for the mobilization of Hg. The impoundment sediment also seemed to be a ‘hotspot’ of Hg transformations. MeHg demethylation occurred via the oxidative demethylation pathway (CO2 produced from MeHg), except in surficial sediment offshore in the Gulf during winter, where sediment was more oxidizing and significant amounts of CH4 were liberated during MeHg degradation via reductive demethylation. The CH4 formation was likely due to an increased influence from the expression of MeHg degradative enzymes encoded by the mer detoxification bacterial genetic system. The freshwater site also liberated CH4 from MeHg, but it appeared to be due to oxidative demethylation by methanogenic bacteria.  相似文献   

18.
Methylmercury can accumulate in fish to concentrations unhealthy for humans and other predatory mammals. Most sources of mercury (Hg) emit inorganic species to the environment. Therefore, ecological harm occurs when inorganic Hg is converted to methylmercury. Sulfate- and iron-reducing bacteria (SRB and FeRB) methylate Hg, but the effects of processes involving oxidized and reduced forms of sulfur and iron on the reactivity of Hg, including the propensity of inorganic Hg to be methylated, are poorly understood. Under abiotic conditions, using a laboratory flow reactor, bisulfide (HS−) was added at 40 to 250 μM h−1 to 5 g L−1 goethite (α-FeOOH) suspensions to which Hg(II) was adsorbed (30-100 nmol m−2) at pH 7.5. Dissolved Hg initially decreased from 103 or 104 nM (depending on initial conditions) to 10−1 nM, during which the concentration of Hg(II) adsorbed to goethite decreased by 80% and metacinnabar (β-HgS(s)) formed, based on identification using Hg LIII-edge extended X-ray absorption fine structure (EXAFS) spectroscopic analysis. The apparent coordination of oxygens surrounding Hg(II), measured with EXAFS spectroscopy, increased during one flow experiment, suggesting desorption of monodentate-bound Hg(II) while bidentate-bound Hg(II) persisted on the goethite surface. Further sulfidation increased dissolved Hg concentrations by one to two orders of magnitude (0.5 to 10 nM or 30 nM), suggesting that byproducts of bisulfide oxidation and Fe(III) reduction, primarily polysulfide and potentially Fe(II), enhanced the dissolution of β-HgS(s) and/or desorption of Hg(II). Rapid accumulation of Fe(II) in the solid phase (up to 40 μmol g−1) coincided with faster elevation of dissolved Hg concentrations. Fe(II) served as a proxy for elemental sulfur [S(0)], as S(0) was the dominant bisulfide oxidation product coupled to Fe(III) reduction, based on sulfur K-edge X-ray absorption near edge structure (XANES) spectroscopy. In one experiment, dissolved Hg concentrations tracked those of all sulfide species [S(-II)]. These results suggest that S(-II) reacted with S(0) to form polysulfide, which then caused the dissolution of β-HgS(s). A secondary Fe-bearing phase resembling poorly formed green rust was observed in sulfidized solids with scanning electron microscopy, although there was no clear evidence that either surface-bound or mineralized Fe(II) strongly affected Hg speciation. Examination of interrelated processes involving S(-II) and Fe(III) revealed new modes of Hg solubilization previously not considered in Hg reactivity models.  相似文献   

19.
Concentrations of atmospheric Hg species, elemental Hg (Hg°), reactive gaseous Hg (RGM), and fine particulate Hg (Hg-PM2.5) were measured at a coastal site near Weeks Bay, Alabama from April to August, 2005 and January to May, 2006. Mean concentrations of the species were 1.6 ± 0.3 ng m−3, 4.0 ± 7.5 pg m−3 and 2.7 ± 3.4 pg m−3, respectively. A strong diel pattern was observed for RGM (midday maximum concentrations were up to 92.7 pg m−3), but not for Hg° or Hg-PM2.5. Elevated RGM concentrations (>25 pg m−3) in April and May of 2005 correlated with elevated average daytime O3 concentrations (>55 ppbv) and high light intensity (>500 W m−2). These conditions generally corresponded with mixed continental-Gulf and exclusively continental air mass trajectories. Generally lower, but still elevated, RGM peaks observed in August, 2005 and January–March, 2006 correlated significantly (p < 0.05) with peaks in SO2 concentration and corresponded to periods of high light intensity and lower average daytime O3 concentrations. During these times air masses were dominated by trajectories that originated over the continent. Elevated RGM concentrations likely resulted from photochemical oxidation of Hg° by atmospheric oxidants. This process may have been enhanced in and by the near-shore environment relative to inland sites. The marine boundary layer itself was not found to be a significant source of RGM.  相似文献   

20.
This study combines sediment geochemical analysis, in situ benthic lander deployments and numerical modeling to quantify the biogeochemical cycles of carbon and sulfur and the associated rates of Gibbs energy production at a novel methane seep. The benthic ecosystem is dominated by a dense population of tube-building ampharetid polychaetes and conspicuous microbial mats were unusually absent. A 1D numerical reaction-transport model, which allows for the explicit growth of sulfide and methane oxidizing microorganisms, was tuned to the geochemical data using a fluid advection velocity of 14 cm yr−1. The fluids provide a deep source of dissolved hydrogen sulfide and methane to the sediment with fluxes equal to 4.1 and 18.2 mmol m−2 d−1, respectively. Chemosynthetic biomass production in the subsurface sediment is estimated to be 2.8 mmol m−2 d−1 of C biomass. However, carbon and oxygen budgets indicate that chemosynthetic organisms living directly above or on the surface sediment have the potential to produce 12.3 mmol m−2 d−1 of C biomass. This autochthonous carbon source meets the ampharetid respiratory carbon demand of 23.2 mmol m−2 d−1 to within a factor of 2. By contrast, the contribution of photosynthetically-fixed carbon sources to ampharetid nutrition is minor (3.3 mmol m−2 d−1 of C). The data strongly suggest that mixing of labile autochthonous microbial detritus below the oxic layer sustains high measured rates of sulfate reduction in the uppermost 2 cm of the sulfidic sediment (100-200 nmol cm−3 d−1). Similar rates have been reported in the literature for other seeps, from which we conclude that autochthonous organic matter is an important substrate for sulfate reducing bacteria in these sediment layers. A system-scale energy budget based on the chemosynthetic reaction pathways reveals that up to 8.3 kJ m−2 d−1 or 96 mW m−2 of catabolic (Gibbs) energy is dissipated at the seep through oxidation reactions. The microorganisms mediating sulfide oxidation and anaerobic oxidation of methane (AOM) produce 95% and 2% of this energy flux, respectively. The low power output by AOM is due to strong bioenergetic constraints imposed on the reaction rate by the composition of the chemical environment. These constraints provide a high potential for dissolved methane efflux from the sediment (12.0 mmol m−2 d−1) and indicates a much lower efficiency of (dissolved) methane sequestration by AOM at seeps than considered previously. Nonetheless, AOM is able to consume a third of the ascending methane flux (5.9 mmol m−2 d−1 of CH4) with a high efficiency of energy expenditure (35 mmol CH4 kJ−1). It is further proposed that bioenergetic limitation of AOM provides an explanation for the non-zero sulfate concentrations below the AOM zone observed here and in other active and passive margin sediments.  相似文献   

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