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1.
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   

2.
Age-dated sediment cores from 4 remote lakes across California were analyzed for total Hg (HgT) concentration as a function of pre- and post-industrialization. Particle size, magnetic susceptibility and organic C and N, were measured to determine if the Hg concentration in sediment cores could be related to atmospheric deposition and/or watershed processes. Results indicate that (a) for each lake modern (1970–2004) HgT lake sediment concentrations have increased by an average factor of 5 times more than historic (pre-1850) HgT concentrations; (b) the ratio of modern to pre-industrial lake sediment HgT for these lakes are higher than estimated for other locations where atmospheric deposition is presumed to be the main source of Hg; (c) 2 of the 4 studied lakes demonstrated significant relationships between HgT concentrations and percentage organic material (r2 = 0.68 and p < 0.01; r2 = 0.67 and p < 0.01) whereas the other two indicated no significant relationship (r2 = 0.05 and p = 0.51; r2 = 0.12 and p = 0.36).  相似文献   

3.
Reactive dissolved Hg (HgR), non-reactive dissolved Hg (HgNR), particulate Hg (HgP), dissolved organic C (DOC), particulate organic C (POC), salinity and other interpretative parameters were determined in water samples collected in the North Channel and in adjacent areas of the Tagus estuary (Portugal). Higher concentrations of both dissolved and particulate Hg in the North Channel indicate a pollution source and raise the possibility of Hg escaping to adjacent areas by tidal action. This transport was confirmed by the increase of HgR with salinity and HgNR with DOC, along a longitudinal axis paralleling the North Channel. Apparently, Hg leaving this channel is progressively complexed by inorganic and organic ligands. Near the mouth of the estuary, values decreased reflecting dilution with seawater. Moreover the HgP:POC ratio also increased seaward, suggesting mixing with Hg enriched particles that escaped the North Channel, or incorporation of dissolved Hg species in river-derived particles. These results suggest that the pathway of anthropogenic Hg in contaminated waters may be identified by their enrichment in organic matter, both in the dissolved and particulate fraction.  相似文献   

4.
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   

5.
In 2002, metallic Hg was found buried in a rural area of Descoberto city, Brazil. The origin of the Hg was a gold mining explotation plant established nearly one century ago. Although a number of studies have been conducted in order to assess the contamination of the area, none of them investigated the presence of methylated Hg in the hydric system. In this work methylmercury (CH3Hg+) was determined using gas chromatography-pyrolysis-atomic fluorescence detection (CG-pyro-AFS) in material from rain sedimentation boxes and stream sediments near the contaminated area. Total Hg concentration (HgT) along with the chemical speciation by thermo-desorption were performed. HgT in material from the sedimentation boxes was found to be very high, up to 41,580 μg kg−1, even in the rainy season, when in general HgT were much lower than in dry season. The samples from the Grama and Rico streams show a range of HgT from 5.8 to 266 μg kg−1. The thermo-desorption analysis showed predominance of Hg2+, possibly linked to organic sulfur, suggested by a good positive correlation between Hg2+, HgT, organic mater (OM) and total S. The CH3Hg+ concentration in stream sediment samples ranged from <0.07 to 1.87 μg kg−1 and in the samples of sedimentation boxes the concentrations were 1.33 and 8.0 μg kg−1 during dry season. The sample with the highest percentage of HgT as Hg2+ (98%) presented also the highest percentage of CH3Hg+ (0.7%). These are high values, showing that care should be taken to avoid the transport of this material to the hydrological system. Further studies on the transfer through the food chain would be very important.  相似文献   

6.
Two sampling campaigns were carried out in March and August 2005 representing dry and wet seasons, respectively, to investigate the distribution patterns of Hg species in the water column and sediment profiles at two sampling stations in Aha Reservoir located in Guiyang, Southwestern China. Aha Reservoir has been contaminated by Hg due to small scale coal mining activities. Mercury concentrations in both water and sediment were elevated. A clearly seasonal variation of dissolved Hg (DHg), particulate Hg (PHg) and total Hg (THg) concentrations in the water column was observed. The concentrations of these Hg species in the wet season were significantly higher than in the dry season. Runoff input and diffusion of Hg from sediments could be the reasons for elevated concentrations of these Hg species in the wet season. The contaminated sediment is acting as a secondary contamination source for both inorganic Hg (IHg) and methylmercury (MeHg) to the overlying water. The cycling of Mn in the sediment governs the diffusion process of IHg to the water column. In the dry season (winter and spring), Mn occurs as MnO2 because the uppermost part of sediment is in an oxic condition and Hg ions are absorbed by MnO2. In the wet season (summer and fall), the uppermost part of the sediment profile is in a reduced condition because of stratification of the water column and MnO2 is reduced to Mn2+, which results in transformation of Hg2+ into porewater as Mn2+ became soluble. This causes a higher diffusive flux of IHg from sediment to overlying water in the wet season. Both sampling stations showed a consistent trend that THg concentrations decreased in the uppermost part of sediment cores. This demonstrated that the measures taken to reduce ADM contamination to Aha Reservoir also reduced Hg input to the reservoir. Methyl Hg diffusive fluxes from sediment to overlying water were higher in the wet season than the dry season demonstrating that high temperatures favor Hg methylation processes in sediment.  相似文献   

7.
Hg in hydrothermal systems is generally thought to be transported as Hg-S complexes. However, the abundance of Hg0vap, in geothermal emissions suggests that Hg0eq, is present in the liquid phase of geothermal systems. Calculations for reducing fluids (HS? dominant over SO=4) in equilibrium with cinnabar indicate that Hg0eq, can be quite abundant relative to other species at temperatures above 200°C. Increasing pH and temperature, and decreasing total S, ionic strength, and pO2 all promote the abundance of Hg0eq. When a vapor phase develops from a geothermal liquid, Hg partitions strongly into the vapor as Hg0vap. Vapor transport at shallow level then results in the formation of Hg halos around shallow aquifers as well as in a flux of Hg to the atmosphere. Hg deposition may occur in response to mixing with oxidizing or acidic water, turning Hg0eq, into Hg++, with subsequent cinnabar precipitation. When pyrite is the stable Fe-sulfide, cinnabar solubility is at its lowest, so cinnabar + pyrite assemblages are common. Cinnabar + hematite ± pyrite can precipitate from more oxidized or S-poor water. Hg0liq, can occur as a primary mineral, in coexistence with all common Fe-sulfides and oxides. Cinnabar ± Hg0liq cannot coexist with pyrrhotite or magnetite at temperatures between 100° and 250°C. Evidence from Hg deposits indicates that many formed from dilute hydrothermal fluids in which Hg probably occurred as Hg0eq. In S-rich systems, Hg may occur as Hg-S complexes, and in saline waters it can occur as Hg-Cl complexes.  相似文献   

8.
《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   

9.
Mercury concentrations were determined in stream sediments from the Camaquã River Basin, located in the shield region of the state of Rio Grande do Sul, southern Brazil. The resulting geochemical data show that overbank floodplain deposits exhibit higher concentrations than sediments collected from the active channel bed. In addition, higher Hg concentrations were measured in the fine(<63 μm) sediment fraction of the samples. Total Hg concentrations in the fine fraction of active stream sediments from Lavras do Sul County, which have been influenced by past gold mining activities, have decreased during the last five years to values ≤142 ng g−1. However, in a settling pond containing abandoned mine wastes, the Hg concentration of a bulk sample remained exceptionally high (5220 ng g−1). Preliminary speciation results show that Hg0 is the predominant species in most of the samples. This was the form of Hg released by the gold amalgamation activities in the area, and appears to be relatively stable under the existing Eh and pH conditions.  相似文献   

10.
Mining wastes and calcines from two abandoned mining areas (Valle del Azogue and Bayarque in Almería) have been characterized. In the mining wastes, the dominant mercury phases are cinnabar and elemental mercury in the matrix. In the calcines, however, the dominant mercury phase is elemental mercury bounded to the matrix. Water-leaching experiments were conducted on low-grade stockpiles and calcines in order to simulate the mobilization of mercury by runoff under environmental conditions. The laboratory column-leaching experiments show a possible mobilization of mercury from Hg0 dissolution, colloid transport and a possible dissolution of calomel and other soluble phases in the mine wastes from the Valle del Azogue and Bayarque mines. Equilibrium speciation modeling of Hg, conducted using the numerical code MINTEQ, showed that the theoretical dominant mercury species in the calcine and mining wastes samples are Hg(OH)2, HgCl2, HgClOH and Hg0. In some leachates obtained from the Valle del Azogue mining wastes (sample A06), the high Hg concentrations may indicate the possible dissolution of mineral phases such as calomel and other soluble phases, which are subsaturated. The environmental results indicate a great environmental mobility of mercury, especially during wet episodes associated with intense precipitation events, when there are significative amounts of secondary soluble minerals.  相似文献   

11.
Considerable fractions of the Hg content of lake and river systems in Scandinavia are discharged from the soil of the catchments. An important soil type in Scandinavia is the iron–humus podzol. The sorption characteristics of this soil type for inorganic Hg(II) and monomethyl mercury were investigated by batch experiments. The solubility of Hg2+ and CH3Hg+ in the soil horizons containing organic matter increases with increasing pH of the soil solution by favoring the formation of solute organic matter–mercury complexes. While the solubility of Hg2+ is strongly dependent on complexation to dissolved organic matter, the solubility of CH3Hg+ is more dependent on ion exchange. The concentration of solute inorganic Hg(II) increased with increasing temperature probably because of an increase in the concentration of dissolved organic carbon. There was no effect of temperature on the concentration of solute CH3Hg+. At pH values where inorganic mercury–hydroxo complexes are formed, inorganic Hg(II) is efficiently sorbed to the metal oxides of the mineral soil. The soil–water distributions of inorganic Hg(II) in the different soil horizons were described by Freundlich isotherms or linear isotherms for common and contaminated mercury contents in the soils.  相似文献   

12.
《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   

13.
Mercury concentrations (HgT) in fine-grained fraction (<63 μm) of core sediments of the Hugli–Matla–Bidyadhari estuarine complex, India were analyzed. Results revealed a wide range of spatial variations (<4–93 ng g−1 dry weight) with a definite enhancement level at the lower stretch of the estuarine complex infested with mangrove plants, which might act as a sink to HgT. An elevated concentration of Hg was encountered in surface/subsurface layer of the core in majority of the cases resulting from physical, biogenic and postdepositional diagenetic processes that remobilized and resuspended the metal from deeper sediments. A strong positive correlation was observed between the Hg and clay fraction content of the sediments, while the correlations of Hg with Al, Fe and Mn were poor. Based on the index of geoaccumulation (I geo) and effects range-low (ER-L) value, it is considered that the sediments are less polluted and thus there is less chance of ecotoxicological risk to organisms living in sediments.  相似文献   

14.
Waters from abandoned Sb-Au mining areas have higher Sb (up to 2138 μg L−1), As (up to 1252 μg L−1) and lower Al, Zn, Li, Ni and Co concentrations than those of waters from the As-Au mining area of Banjas, which only contain up to 64 μg L−1 As. In general, Sb occurs mainly as SbO3− and As H2AsO4−. In general, waters from old Sb-Au mining areas are contaminated in Sb, As, Al, Fe, Cd, Mn, Ni and NO2−, whereas those from the abandoned As-Au mining area are contaminated in Al, Fe, Mn, Ni, Cd and rarely in NO2−. Waters from the latter area, immediately downstream of mine dumps are also contaminated in As. In stream sediments from Sb-Au and As-Au mining areas, Sb (up to 5488 mg kg−1) and As (up to 235 mg kg−1) show a similar behaviour and are mainly associated with the residual fraction. In most stream sediments, the As and Sb are not associated with the oxidizable fraction, while Fe is associated with organic matter, indicating that sulphides (mainly arsenopyrite and pyrite) and sulphosalts containing those metalloids and metal are weathered. Arsenic and Sb are mainly associated with clay minerals (chlorite and mica; vermiculite in stream sediments from old Sb-Au mining areas) and probably also with insoluble Sb phases of stream sediments. In the most contaminated stream sediments, metalloids are also associated with Fe phases (hematite and goethite, and also lepidocrocite in stream sediments from Banjas). Moreover, the most contaminated stream sediments correspond to the most contaminated waters, reflecting the limited capacity of stream sediments to retain metals and metalloids.  相似文献   

15.
The composition of waters from 10 thermal springs located in western Virginia near the 38th parallel lineament have been analysed for major dissolved components and for Sr, Fe, Cu, Zn and Cd; from these analyses, free ion activities have been calculated. The temperatures of the springs range from 17° to 39°C, the heat apparently being derived simply from deep circulation along synclinal, Middle Ordovician limestones. More than 95 per cent of the dissolved solids consist of Ca2+, Mg2+ HCO3?, and SO42?. The concentrations of these components, as well as the spring temperatures, have not changed appreciably in 140 yr in some springs. The waters that have temperatures below 25° are all undersaturated with respect to calcite and dolomite, possibly because they have been contaminated by shallow ground waters. The waters with temperatures above 25° are in equilibrium with calcite and dolomite. Furthermore, in this latter group, the calcium-sulfate activity product and the sulfate-carbonate activity ratio are nearly constant, even though the waters are under saturated with respect to gypsum, anhydrite, celestite and strontianite. This can be explained if CaSO4 is coprecipitated in a mineral such as aragonite. The waters have absorbed some dissolved oxygen near the surface, but at depth they may be anoxic with Eh controlled by the oxidation of pyrite to goethite. The extremely low chloride concentrations of these waters clearly distinguish them from the brines which deposited Mississippi Valley and Appalachian type epithermal ore deposits.  相似文献   

16.
Pristine water bodies in the Negro River basin, Brazilian Amazon, show relatively high concentrations of mercury. These waters are characterized by acidic pH, low concentrations of suspended solids, and high amounts of dissolved organic matter and are exposed to intense solar radiation throughout the year. This unique environment creates a very dynamic redox chemistry affecting the mobility of mercury due to the formation of the dissolved elemental species (Hg0). It has been shown that in this so-called black water, labile organic matter from flooded forest is the major scavenger of photogenerated H2O2. In the absence of hydrogen peroxide, these black waters lose their ability to oxidize Hg0 to Hg2+, thus increasing Hg0 evasion across the water/atmosphere interface, with average night time values of 3.80 pmol m?2 h?1. When the dry period starts, labile organic matter inputs gradually diminish, allowing the increasing concentration of H2O2 to re-establish oxidative water conditions, inhibiting the metal flux across the water/atmosphere interface and contributing to mercury accumulation in the water column.  相似文献   

17.
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   

18.
Floodplain soil-paleosol successions are valuable archives for reconstructing Pleistocene-Holocene climate changes but have been relatively unstudied in the southern Appalachian region. Two soil profiles on a small floodplain in southeastern Tennessee, USA were described and sampled in detail using both pedological and geological approaches, including stable carbon isotope analysis of soil organic matter (SOM). Correlation between the 2 profiles was constrained by uncalibrated AMS 14C ages of bulk humates, and using SOM δ13C values, both mobile and immobile elements. Four distinct 2.5-4‰ shifts towards less negative δ13C values for SOM suggest ∼ 300-yr cyclicity and transient warmer and drier climate events, with either water-stressed C3 vegetation or as much as 35% C4 plants present during the mid-Holocene. These postulated multi-episodic drier climate conditions have never before been documented in the southern Appalachian region and are tentatively correlated with mid-Holocene warming and drying in the eastern US, the nearly time-equivalent mid-Holocene events documented in Texas, the US High Plains and in the Gulf of Mexico. High rates of floodplain sediment accumulation (0.5-3 mm/yr), high clay content and maintenance of poorly drained soil conditions favor preservation of high-resolution climate archives in floodplain deposits by inhibiting oxidation and translocation of organic C.  相似文献   

19.
Five hundred years of mercury (Hg) mining activity in Idrija, Slovenia caused widespread Hg contamination. Besides Hg emissions from the ore smelter, tailings have been found to be the major source of river sediment contamination. In the present study, solid phase binding forms and the aqueous mobility of Hg have been investigated in tailings of the Idrija Hg mine by means of a pyrolysis technique and aqueous Hg speciation. Results show that Hg binding forms differ with the age of the tailings due to the processing of different ores with different roasting techniques. In older tailings, the predominant Hg species is cinnabar (HgS), due to incomplete roasting, whereas in tailings of the 20th century the amount of cinnabar in the material decreased due to a higher efficiency of the roasting process and the increasing use of ores bearing native Hg. In younger tailings, metallic Hg (Hg0) sorbed to mineral matrix components such as dolomite and Fe-oxyhydroxides became the predominant Hg binding form in addition to unbound Hg0 and traces of HgO. Leaching tests show that in younger tailings high amounts of soluble Hg exist in reactive form. In older tailings most of the soluble Hg occurs bound to soluble complexes. It might be assumed that in the long term, matrix-bound Hg0 could be bound to humic acids derived from soils covering the tailings. This means that, despite the lower total Hg concentrations found in the younger tailings, the long-term risk potential of its mobile matrix-bound Hg0 is higher than that of older tailings bearing mostly immobile cinnabar.  相似文献   

20.
Contaminated fluvial sediments represent both temporary sinks for river-borne pollutants and potential sources in case of natural and/or anthropogenic resuspension. Reservoir lakes play a very important role in sediment dynamics of watersheds and may offer great opportunities to study historical records of river-borne particles and associated elements transported in the past. The fate and potential environmental impact of Hg depends on its abundance, its carrier phases and its chemical speciation. Historical Hg records and solid state Hg speciation were compared in sediments from two contrasting reservoirs of the Lot River (France) upstream and downstream from a major polymetallic pollution (e.g. Cd, Zn) source. Natural (geochemical background) and anthropogenic Hg concentrations and their relationships with predominant carrier phases were determined. The results reveal important historical Hg contamination (up to 35 mg kg−1) of the downstream sediment, reflecting the historical evolution of industrial activity at the point source, i.e. former coal mining, Zn ore treatment and post-industrial remediation work. Single chemical extractions (ascorbate, H2O2, KOH) suggest that at both sites most (∼75%) of the Hg is bound to organic and/or reactive sulphide phases. Organo-chelated (KOH-extracted) Hg, representing an important fraction in the uncontaminated sediment, shows similar concentrations (∼0.02 mg kg−1) at both sites and may be mainly attributed to natural inputs and/or processes. Although, total Hg concentrations in recent surface sediments at both sites are still very different, similar mono-methylmercury concentrations (up to 4 μg kg−1) and vertical distributions were observed, suggesting comparable methylation-demethylation processes. High mono-methylmercury concentrations (4–15 μg kg−1) in 10–40 a-old, sulphide-rich, contaminated sediment suggest long-term persistence of mono-methylmercury. Beyond historical records of total concentrations, the studied reservoir sediments provided new insights in solid state speciation and carrier phases of natural and anthropogenic Hg. In case of sediment resuspension, the major part of the Hg historically stored in the Lot River sediments will be accessible to biogeochemical recycling in the downstream fluvial-estuarine environment.  相似文献   

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