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1.
《Applied Geochemistry》2006,21(11):1940-1954
Speciation and microbial transformation of Hg was studied in mine waste from abandoned Hg mines in SW Texas to evaluate the potential for methyl-Hg production and degradation in mine wastes. In mine waste samples, total Hg, ionic Hg2+, Hg0, methyl-Hg, organic C, and total S concentrations were measured, various Hg compounds were identified using thermal desorption pyrolysis, and potential rates of Hg methylation and methyl-Hg demethylation were determined using isotopic-tracer methods. These data are the first reported for Hg mines in this region. Total Hg and methyl-Hg concentrations were also determined in stream sediment collected downstream from two of the mines to evaluate transport of Hg and methylation in surrounding ecosystems. Mine waste contains total Hg and methyl-Hg concentrations as high as 19,000 μg/g and 1500 ng/g, respectively, which are among the highest concentrations reported at Hg mines worldwide. Pyrolysis analyses show that mine waste contains variable amounts of cinnabar, metacinnabar, Hg0, and Hg sorbed onto particles. Methyl-Hg concentrations in mine waste correlate positively with ionic Hg2+, organic C, and total S, which are geochemical parameters that influence processes of Hg cycling and methylation. Net methylation rates were as high as 11,000 ng/g/day, indicating significant microbial Hg methylation at some sites, especially in samples collected inside retorts. Microbially-mediated methyl-Hg demethylation was also observed in many samples, but where both methylation and demethylation were found, the potential rate of methylation was faster. Total Hg concentrations in stream sediment samples were generally below the probable effect concentration of 1.06 μg/g, the Hg concentration above which harmful effects are likely to be observed in sediment dwelling organisms; whereas total Hg concentrations in mine waste samples were found to exceed this concentration, although this is a sediment quality guideline and is not directly applicable to mine waste. Although total Hg and methyl-Hg concentrations are locally high in some mine waste samples, little Hg appears to be exported from these Hg mines in stream sediment primarily due to the arid climate and lack of precipitation and mine runoff in this region. 相似文献
2.
Narraguinnep Reservoir in southwestern Colorado is one of several water bodies in Colorado with a mercury (Hg) advisory as Hg in fish tissue exceed the 0.3 μg/g guideline to protect human health recommended by the State of Colorado. Concentrations of Hg and methyl-Hg were measured in reservoir bottom sediment and pore water extracted from this sediment. Rates of Hg methylation and methyl-Hg demethylation were also measured in reservoir bottom sediment. The objective of this study was to evaluate potential sources of Hg in the region and evaluate the potential of reservoir sediment to generate methyl-Hg, a human neurotoxin and the dominant form of Hg in fish. Concentrations of Hg (ranged from 1.1 to 5.8 ng/L, n = 15) and methyl-Hg (ranged from 0.05 to 0.14 ng/L, n = 15) in pore water generally were highest at the sediment/water interface, and overall, Hg correlated with methyl-Hg in pore water (R2 = 0.60, p = 0007, n = 15). Net Hg methylation flux in the top 3 cm of reservoir bottom sediment varied from 0.08 to 0.56 ng/m2/day (mean = 0.28 ng/m2/day, n = 5), which corresponded to an overall methyl-Hg production for the entire reservoir of 0.53 g/year. No significant point sources of Hg contamination are known to this reservoir or its supply waters, although several coal-fired power plants in the region emit Hg-bearing particulates. Narraguinnep Reservoir is located about 80 km downwind from two of the largest power plants, which together emit about 950 kg-Hg/year. Magnetic minerals separated from reservoir sediment contained spherical magnetite-bearing particles characteristic of coal-fired electric power plant fly ash. The presence of fly-ash magnetite in post-1970 sediment from Narraguinnep Reservoir indicates that the likely source of Hg to the catchment basin for this reservoir has been from airborne emissions from power plants, most of which began operation in the late-1960s and early 1970s in this region. 相似文献
3.
Richard R. Goulet Jonathan Holmes Laurier Poissant David R.S. Lean Marc Amyot 《Geochimica et cosmochimica acta》2007,71(14):3393-3406
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
4.
《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
5.
6.
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
7.
Two new methods for analysis of sedimentary sulfur employing sensitive flame photometric detection have been developed and applied to a study of marine, estuarine and freshwater sediments. Volatile organosulfur compounds generated from freeze-dried sediments upon heating in a H2 atmosphere reflect the distribution and extent of degradation of detrital organic matter. Regions of biogeochemical sulfur transformations, as characterized by the presence of SO2 progenitors, sulfite and thiosulfate, are also depicted. Scrubbing of sediment slurries treated with the reducing agent, acidic Cr(II) solution, releases H2S and CH2SH from their metal-complexed forms. CH3SH is a common constituent of marine and estuarine sediments at sub-ppm concentrations. 相似文献
8.
《Applied Geochemistry》2005,20(3):627-638
Concentrations of total Hg and methylmercury (MMHg) in riparian soil, mine-waste calcine, sediment, and moss samples collected from abandoned Hg mines in Wanshan district, Guizhou province, China, were measured to show regional dispersion of Hg-contamination. High total Hg and MMHg concentrations obtained in riparian soils from mined areas, ranged from 5.1 to 790 mg kg−1 and 0.13 to 15 ng g−1, respectively. However, total Hg and MMHg concentrations in the soils collected from control sites were significantly lower varying from 0.1 to 1.2 mg kg−1 and 0.10 to 1.6 ng g−1, respectively. Total Hg and MMHg concentrations in sediments varied from 90 to 930 mg kg−1 and 3.0 to 20 ng g−1, respectively. Total Hg concentrations in mine-waste calcines were highly elevated ranging from 5.7 to 4400 mg kg−1, but MMHg concentrations were generally low ranging from 0.17 to 1.1 ng g−1. Similar to the high Hg concentrations in soil and sediments, moss samples collected from rocks ranged from 1.0 to 95 mg kg−1 in total Hg and from 0.21 to 20 ng g−1 in MMHg. Elevated Hg concentrations in mosses suggest that atmospheric deposition might be an important pathway of Hg to the local terrestrial system. Moreover, the spatial distribution patterns of Hg contamination in the local environment suggest derivation from historic Hg mining sites in the Wanshan area. 相似文献
9.
《Applied Geochemistry》2006,21(3):515-527
Dissolved and particulate Hg fluxes in the Lot–Garonne–Gironde fluvial-estuarine system were obtained from observation of daily discharge and suspended particulate matter (SPM) concentrations. In addition to the measurements of the total dissolved (<0.45 μm) and particulate Hg (>0.45 μm), called HgTD and HgTP respectively, the dissolved inorganic Hg species (HgRD) were determined monthly. Geochemical background values for HgTP in sediments and SPM were similar to crustal values and to typical concentrations in SPM of non-contaminated river systems, respectively. The Riou Mort watershed already known as the origin of important historical polymetallic (e.g., Cd, Zn) pollution was identified as an important Hg point source. In the downstream Lot River, Hg concentrations were clearly higher than those in other moderately contaminated systems. The mean relative contribution of HgRD to HgTD in the Lot River and in the Garonne River was close to 25% and 50%, respectively, and showed no correlation with water discharge or SPM concentration. Depending on the origin and nature of SPM, HgTP concentrations were correlated or not with particulate organic C (POC). Maximum HgTP concentrations were measured in samples containing low POC concentrations and were attributed to sediment resuspension. In contrast, high POC concentrations (6–17%) during algal blooms were associated with low/moderate HgTP concentrations (<0.5 mg kg−1) at different sites, suggesting that Hg concentrations in fluvial phytoplankton may be limited by bioavailability of dissolved Hg and/or physiologically controlled Hg accumulation. Mercury was mostly (up to 98%) transported in the particulate phase with estimated annual Hg fluxes at the outlet of the Lot River system ranging from 35 to 530 kg a−1 for the past decade. The minimum anthropogenic component (58–84% of total Hg fluxes) could not be explained by present Riou Mort point source contributions, suggesting important Hg release from contaminated sediment as a major source and from downstream point sources (e.g., coal-fired power plants and/or metal processing industries). HgTP concentrations and fluxes were strongly related to hydrologic variations and were clearly increased by riverbed dredging during lock construction. Therefore, the estimated Hg stocks in the Lot River sediment (5–13 tons) represent an important potential Hg source for the downstream fluvial-estuarine system. 相似文献
10.
In the Patía River delta, the best-developed delta on the western margin of South America, a major water diversion started in 1972. The diversion of the Patía flow to the Sanquianga River, the latter a small stream draining internal lakes from the Pacific lowlands, shifted the active delta plain from the south to the north and changed the northern estuarine system into an active delta plain. The Sanquianga Mangrove National Park, a mangrove reserve measuring 800 km2, lies in this former estuary, where major hydrologic and sedimentation changes are occurring. Overall, major environmental consequences of this discharge diversion in terms of geomorphic changes along distributary channels and ecological impacts on mangrove ecosystems are evidenced by: (1) distributary channel accretion by operating processes such as sedimentation, overbank flow, increasing width of levees, sedimentation in crevasses, interdistributary channel fill, and colonization of pioneer mangrove; (2) freshening conditions in the Sanquianga distributary channel, a hydrologic change that has shifted the upper estuarine region (salinity <1%) downstream; (3) downstream advance of freshwater vegetation, which is invading channel banks in the lower and mixing estuarine zones; (4) die-off of approximately 5200 ha of mangrove near the delta apex at Bocas de Satinga, where the highest sediment accumulation rates occur; and (5) recurrent periods of mangrove defoliation due to a worm plague. Further analyses indicate strong mangrove erosion along transgressive barrier islands on the former delta plain. Here tectonic-induced subsidence, relative sea-level rise, and sediment starving conditions due to the channel diversion, are the main causes of the observed retreating conditions of mangrove communities. Our data also indicate that the Patía River has the highest sediment load (27 × 106 t yr−1) and basin-wide sediment yield (1500 t km−2 yr−1) on the west coast of South America. Erosion rates from the Patía catchment have been more pronounced during the decades of 1970–1980 and 1990–2000, as a result of land degradation and deforestation. The high sediment and freshwater inputs into the mangrove ecosystem create additional stress (both at ongoing background levels and, occasionally, at dramatic levels), which may periodically push local environmental parameters beyond the thresholds for mangrove survival. The future environmental state of the Sanquianga Mangrove National Reserve deserves more scientific and governmental attention. 相似文献
11.
《Chemie der Erde / Geochemistry》2013,73(3):249-259
In total 27 short and one long sediment core, and 278 surface sediment samples from the Baltic Sea were analyzed for mercury (Hg), and organic carbon contents. Thirteen short cores and the long core were dated by radionuclide methods (210Pb, 137Cs, AMS14C). The dataset allows discriminating between natural and human induced changes on the Hg levels in Baltic Sea sediments. Preindustrial Holocene background concentrations vary between 20 and 50 μg Hg per kg dry sediment and are positively correlated with organic carbon changes. Strong human induced pollution is recorded for the second half of the past century and caused high Hg concentrations of up to several hundred μg Hg per kg dry sediment even in Baltic Sea basins. Maximum concentrations are found at industrial and war waste dumping sites (local hot spots). An Hg concentration decreasing trend toward the present day is observed at most coring sites, a result of environmental measures undertaken during the last two decades. At sites where it is possible to calculate Hg fluxes, the natural accumulation rates vary between 2.1 and 5.4 μg Hg per m2 per year. Anthropogenically sourced Hg accumulation rates vary in a wide range of 30 and 300 μg Hg per m2 per year for the time span of maximum pollution. In areas characterized by discontinuous sedimentation only “inventories” of human sourced Hg expressed as the total amount of deposited Hg (above the natural background) per m2 can be calculated. The inventories of the investigated cores vary in the range of 1 and 8 mg Hg per m2. Additionally, influences of sediment dynamics on spatial distribution pattern of Hg concentrations in surface and subsurface sediments are discussed. 相似文献
12.
Kathleen Gosnell Prentiss Balcom Veronica Ortiz Brian DiMento Amina Schartup Richard Greene Robert Mason 《Aquatic Geochemistry》2016,22(4):313-336
The Delaware River Estuary (DRE) is a cornerstone of industrialization, shipping, and urban usage, and has a long history of human impact on pollution and recovery. Mercury (Hg) is a contaminant of concern in the DRE based upon concentrations in some fish samples that were found to exceed State and Federal fish tissue criteria. Methylation of Hg often follows a seasonal pattern as its production is biologically mediated. Surveys were conducted in November 2011, April 2012, and July 2012 to assess this effect. We sampled surface and bottom water at six sites spanning the estuarine turbidity maximum (ETM) in the main channel of the river, plus three sediment sites at shallow, subtidal locations. Our results indicate there is a clear seasonal increase in both water column and sediment methylmercury (MeHg) and %MeHg concentrations in the ETM during July. Water-column-filtered total mercury (HgT), suspended particle HgT, and MeHg concentrations were found to fluctuate little with location or season in the ETM. In contrast, sediment MeHg, water-column-filtered MeHg, and pore water HgT varied seasonally. Furthermore, pore water MeHg levels were elevated in concert with increased k meth rates in July. Estimated river input and sediment and atmospheric depositional MeHg flux were compared seasonally. River flux was more than an order of magnitude higher than sediment flux in April, coinciding with higher fluvial transport. However, during July, river flux decreases and sediment flux becomes a larger relative source. This trend has potential implications for fish and other biota residing in the DRE during summer. 相似文献
13.
Microbial cycling of mercury in contaminated pelagic and wetland sediments of San Pablo Bay,California 总被引：4，自引：0，他引：4
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
14.
《Applied Geochemistry》2006,21(11):1999-2009
The Carson River flows in a closed basin system and the total flow of the river water decreases downstream due to both evaporation and consumptive uses. This river system is fed primarily by snow pack in the Sierra Nevada during the winter, which flows down gradient following melting in spring and summer. Water loss through evaporation in the Carson River results in a downstream buildup of conservative elements such as Cl− and certain oxyanion forming elements including Se, Mo and W, which are known to interfere with the transformation of Hg within the S cycle. In addition to these naturally occurring hydrologic processes and the resulting affects on water chemistry, the Carson River Basin has been historically impacted by Au and Ag mining that used Hg amalgamation techniques. Contamination of Hg in the Carson River system is now well documented and published Hg concentrations in different environmental compartments are extremely high. In this study, hydrologically driven changes in water chemistry of the river system and the resulting effects on Hg cycling were examined. Results show that periods of low water flow correspond to high water pH (up to 8.3), relatively high concentrations of oxyanion forming elements (e.g., As, Se, Mo and W), and low Hg methylation potential in sediment. In contrast, periods of high flow bring about dilution, which results in lower pH (∼7), lower concentrations of oxyanion forming elements, but higher Hg methylation potential. Overall, changes in flow regimes likely affect rates of methyl-Hg (MeHg) production through a combination of factors such as high pH, which favors MeHg demethylation, and the occurrence of relatively high concentrations of Group VI oxyanions that could interfere with microbial SO4 reduction and MeHg production. 相似文献
15.
《Applied Geochemistry》2006,21(11):1868-1879
Ultra-clean sampling methods and approaches typically used in pristine environments were applied to quantify concentrations of Hg species in water and microbial biomass from hot springs of Yellowstone National Park, features that are geologically enriched with Hg. Microbial populations of chemically-diverse hot springs were also characterized using modern methods in molecular biology as the initial step toward ongoing work linking Hg speciation with microbial processes. Molecular methods (amplification of environmental DNA using 16S rDNA primers, cloning, denatured gradient gel electrophoresis (DGGE) screening of clone libraries, and sequencing of representative clones) were used to examine the dominant members of microbial communities in hot springs. Total Hg (THg), monomethylated Hg (MeHg), pH, temperature, and other parameters influential to Hg speciation and microbial ecology are reported for hot springs water and associated microbial mats.Several hot springs indicate the presence of MeHg in microbial mats with concentrations ranging from 1 to 10 ng g−1 (dry weight). Concentrations of THg in mats ranged from 4.9 to 120,000 ng g−1 (dry weight). Combined data from surveys of geothermal water, lakes, and streams show that aqueous THg concentrations range from l to 600 ng L−1. Species and concentrations of THg in mats and water vary significantly between hot springs, as do the microorganisms found at each site. 相似文献
16.
Kate Buckman Vivien Taylor Hannah Broadley Daniel Hocking Prentiss Balcom Rob Mason Keith Nislow Celia Chen 《Estuaries and Coasts》2017,40(5):1358-1370
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
17.
《Applied Geochemistry》2006,21(11):1837-1854
Total dissolved and total particulate Hg mass balances were estimated during one hydrological period (July 2001–June 2002) in the Thur River basin, which is heavily polluted by chlor-alkali industrial activity. The seasonal variations of the Hg dynamics in the aquatic environment were assessed using total Hg concentrations in bottom sediment and suspended matter, and total and reactive dissolved Hg concentrations in the water. The impact of the chlor-alkali plant (CAP) remains the largest concern for Hg contamination of this river system. Upstream from the CAP, the Hg partitioning between dissolved and particulate phases was principally controlled by the dissolved fraction due to snow melting during spring high flow, while during low flow, Hg was primarily adsorbed onto particulates. Downstream from the CAP, the Hg partitioning is controlled by the concentration of dissolved organic and inorganic ligands and by the total suspended sediment (TSS) concentrations. Nevertheless, the particulate fluxes were five times higher than the dissolved ones. Most of the total annual flux of Hg supplied by the CAP to the river is transported to the outlet of the catchment (total Hg flux: 70 μg m−2 a−1). Downstream from the CAP, the bottom sediment, mainly composed of coarse sediment (>63 μm) and depleted in organic matter, has a weak capacity to trap Hg in the river channel and the stock of Hg is low (4 mg m−2) showing that the residence time of Hg in this river is short. 相似文献
18.
Benthic fluxes of mercury species in a lagoon environment (Grado Lagoon,Northern Adriatic Sea,Italy)
Stefano Covelli Jadran Faganeli Cinzia De Vittor Sergio Predonzani Alessandro Acquavita Milena Horvat 《Applied Geochemistry》2008
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
19.
The distribution of total mercury and methyl mercury in a shallow hypereutrophic lake (Lake Taihu) in two seasons 总被引：1，自引：0，他引：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
20.
Kinetics of microbial sulfate reduction in estuarine sediments 总被引：2，自引：0，他引：2
Kinetic parameters of microbial sulfate reduction in intertidal sediments from a freshwater, brackish and marine site of the Scheldt estuary (Belgium, the Netherlands) were determined. Sulfate reduction rates (SRR) were measured at 10, 21, and 30 °C, using both flow-through reactors containing intact sediment slices and conventional sediment slurries. At the three sites, and for all depth intervals studied (0-2, 2-4, 4-6 and 6-8 cm), the dependence of potential SRR on the sulfate concentration followed the Michaelis-Menten rate equation. Apparent sulfate half-saturation concentrations, Km, measured in the flow-through reactor experiments were comparable at the freshwater and marine sites (0.1-0.3 mM), but somewhat higher at the brackish site (0.4-0.9 mM). Maximum potential SRR, Rmax, in the 0-4 cm depth interval of the freshwater sediments were similar to those in the 0-6 cm interval of the marine sediments (10-46 nmol cm−3 h−1 at 21 °C), despite much lower in situ sulfate availability and order-of-magnitude lower densities of sulfate-reducing bacteria (SRB), at the freshwater site. Values of Rmax in the brackish sediments were lower (3.7-7.6 nmol cm−3 h−1 at 21 °C), probably due to less labile organic matter, as inferred from higher Corg/N ratios. Inflow solutions supplemented with lactate enhanced potential SRR at all three sites. Slurry incubations systematically yielded higher Rmax values than flow-through reactor experiments for the freshwater and brackish sediments, but similar values for the marine sediments. Transport limitation of potential SRR at the freshwater and brackish sites may be related to the lower sediment porosities and SRB densities compared to the marine site. Multiple rate controls, including sulfate availability, organic matter quality, temperature, and SRB abundance, modulate in situ sulfate-reducing activity along the estuarine salinity gradient. 相似文献