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1.
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   

2.
Mass independent fractionation (MIF) of stable isotopes associated with terrestrial geochemical processes was first observed in the 1980s for oxygen and in the 1990s for sulfur isotopes. Recently mercury (Hg) was added to this shortlist when positive odd Hg isotope anomalies were observed in biological tissues. Experimental work identified photoreduction of aquatic inorganic divalent HgII and photodegradation of monomethylmercury species as plausible MIF inducing reactions. Observations of continental receptors of atmospheric Hg deposition such as peat, lichens, soils and, indirectly, coal have shown predominantly negative MIF. This has led to the suggestion that atmospheric Hg has negative MIF signatures and that these are the compliment of positive Hg MIF in the aquatic environment. Recent observations on atmospheric vapor phase Hg0 and HgII in wet precipitation reveal zero and positive Hg MIF respectively and are in contradiction with a simple aquatic HgII photoreduction scenario as the origin for global Hg MIF observations.This study presents a synthesis of all terrestrial Hg MIF observations, and these are integrated in a one-dimensional coupled continent-ocean-atmosphere model of the global Hg cycle. The model illustrates how Hg MIF signatures propagate through the various Earth surface reservoirs. The scenario in which marine photoreduction is the main MIF inducing process results in negative atmospheric Δ199Hg and positive ocean Δ199Hg of −0.5‰ and +0.25‰, yet does not explain atmospheric Hg0 and HgII wet precipitation observations. Alternative model scenarios that presume in-cloud aerosol HgII photoreduction and continental HgII photoreduction at soil, snow and vegetation surfaces to display MIF are necessary to explain the ensemble of natural observations. The model based approach is a first step in understanding Hg MIF at a global scale and the eventual incorporation of Hg stable isotope information in detailed global mercury chemistry and transport models.  相似文献   

3.
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   

4.
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   

5.
In order to examine the transportation and deposition mechanisms of Hg, we investigated the ore and hydrothermal alteration minerals and solid organic matters from Itomuka mercury mine located in the eastern part of central Hokkaido. In addition to the ore minerals, native mercury and cinnabar, quartz, marcasite, alunite, kaolinite, and minor amounts of pyrite and smectite were identified in the Hg ore by powder X‐ray diffraction (XRD) analysis. This mineral assemblage of acid sulfate alteration was likely developed under the conditions of low temperature (≤100°C) and low pH (≤2) in the steam‐heated environment. The H2SO4 was produced above the water table by the oxidation of H2S separated from deep, near‐neutral fluids by boiling. The dominance of native mercury over cinnabar in Hg ore indicates that the greater part of mineralized Hg was transported as Hg0 in aqueous solution and vapor with low sulfur fugacity. The solid organic matters found in the Hg ore were analyzed with SEM‐EDS, micro‐XRD, and micro‐Fourier transform infrared (FTIR) spectroscopy, and these results suggest that the organic matters contributed to keeping the low fO2 of the Hg‐bearing fluid and transportation of Hg as Hg0 in S‐poor condition. Because the solubility of Hg in acidic fluid is low, neutral to alkaline fluid seems to have leached Hg from the basement sedimentary rocks of Hidaka Group which also supplied the organic matters to the fluid. The oxidation and cooling of Hg‐bearing solution and vapor triggered the deposition of liquid Hg as a primary phase.  相似文献   

6.
Aqueous production and water-air exchange of elemental mercury (Hg0) are important features of the environmental cycling of Hg. We investigated Hg0 cycling in ten Arctic Alaskan lakes that spanned a wide range in physicochemical characteristics. Dissolved gaseous Hg (DGM, dominated by Hg0) varied from 40 to 430 fM and averaged 200 fM. All surface waters were supersaturated relative to the atmosphere. DGM averaged 3 ± 2% of dissolved (i.e., filter passing) dissolved total mercury (DTM) and 15 ± 6% of dissolved labile Hg (DLM). In-lake DGM profiles generally followed the vertical distribution of light, indicating photoreduction of Hg(II) complexes as a source of Hg0. Additionally, DGM correlated linearly with DLM (r2 = 0.82, p < 0.0001) in the lake surface, signifying that Hg complexes (mostly organic Hg associations) in dissolved phase are photoreducible and contribute to production of DGM. Further, a positive relation between DGM/DTM and both Ka (light attenuation coefficient; r2 = 0.73, p < 0.02) and DOC (r2 = 0.60, p = 0.02) suggests that solar radiation and dissolved organic matter control DGM production and its cycling. An average rate of DGM formation (0.6 ± 0.2% of DTM d−1; range, 0.20.8) was estimated by assuming steady state with the evasional rate. In-lake DGM formation occurs at lower rates in waters with greater suspended particulate matter and dissolved organic carbon (DOC), pointing to the significant role of organic matter plays in controlling DGM formation in these aquatic systems. Estimated evasional fluxes of Hg0 (average, 140 ± 50 pmol m−2 d−1; range, 60-200) were comparable to those of temperate lakes (e.g., Wisconsin, Michigan). In arctic lakes, the rate of evasion during ice-free periods (7 ± 3 nmol m−2 yr−1) is similar to the atmospheric input of Hg (wet + dry) to the lakes based on levels in summertime precipitation but not including additional sources, e.g., springtime depletion.  相似文献   

7.
The solubility metallic mercury in water and its dominating forms were studied. The prevalence of the Hgaq0 form in the high-temperature range was confirmed and the reaction constant Hgliq0 ai Hgaq0 (logK = logm = −8.01) at 25°C with the predominance of oxidized forms of mercury for the 20–80°C area of low temperatures was found.  相似文献   

8.
Vegetation plays a significant role in the biogeochemical cycling of mercury. This conclusion is drawn from data presented here on bioaccumulation and subsequent release of volatile mercury from non-vascular plants together with the results of previous work. There is no obvious relation between total plant Hg or soil Hg and rate of release from the plant. Heat of vaporization for Hg0 was calculated at 13.99 kcal/g-atom; from soil it was experimentally determined at 13.81 kcal/g-atom but from the most active vascular plant was only 9.49 kcal/g-atom.  相似文献   

9.
Mercury vapor (Hg0) emission from plants contributes to the atmospheric Hg cycle. Young barley (Hordeum vulgare L.) plants grown on a hydroponic cultivation medium containing Hg(II) have previously been shown to increase their Hg0 emission significantly by reduction of Hg(II) with endogenous ascorbic acid. Regarding the potential contribution to the Hg cycle from the vast forest-covered areas, it was important to investigate this mechanism in trees. The increase in Hg0 emission from young European beech plants cultivated on a HgCl2 medium exceeded that from controls by ca. tenfold and was proportional to the Hg(II) concentration. From these experiments, a flux of 12.8 μg Hg0/h/m2 was estimated at an exposure of the roots to 20 μM Hg(II). Mercury vapor release from homogenates of Norway spruce needles exceeded that from European beech leaves by a factor of 2.3–4, i.e. in proportion to the reported AA concentrations; the reduction was maximal at alkaline pH which is typical for AA. The 8.4-fold difference in Hg0 release between homogenates from wild-type Arabidopsis thaliana and from its AA-deficient mutant vtc 1-1 also paralleled the reported difference in AA levels of both species. It is concluded that the phytoreduction and vaporization of Hg by AA is an important mechanism as much for Hg detoxification in trees as for Hg emission to the atmosphere. The efficiency of this process seems to result from the optimal coordination of transfer and biochemical transformation of mercuric ions and Hg vapor. There is no evidence for a relevant difference in the mechanisms of biogenic Hg(II) reduction between grass plants and trees.  相似文献   

10.
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   

11.
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   

12.
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   

13.
 Understanding the mechanisms of mercury evaporation from soil to the atmosphere is necessary for tracing the fate of mercury in the biological environment and for assessing potential health effects and the impact of anthropogenic mercury emissions on the environment. In this article an integrating overview of the current knowledge of the mechanisms of mercury evaporation is presented. Abiological and biological formation of Hg(0) and/or (CH3)2Hg in the uppermost soil layers are the rate limiting processes of mercury evaporation from soils in background areas; the evaporation rate in background areas is probably strongly influenced by deposited airborne mercury. The evaporation rate limiting factors in mercury enriched mineralized areas with large fractions of total mercury being volatile mercury species (relative to background soil in the non-mineralized vicinity) meteorological variations and the transport characteristics of soils for volatile mercury species. Mercury evaporation rates from background soils are usually <0.2 μg·m–2·h–1 and significantly smaller than from mercury-enriched mineralized areas. Received: 20 November 1995 / Accepted: 24 July 1996  相似文献   

14.
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   

15.
Mercury is a global contaminant of concern due to its transformation by microorganisms to form methylmercury, a toxic species that accumulates in biological tissues. The effect of dissolved organic matter (DOM) isolated from natural waters on reactions between mercury(II) (Hg) and sulfide (S(-II)) to form HgS(s) nanoparticles across a range of Hg and S(-II) concentrations was investigated. Hg was equilibrated with DOM, after which S(-II) was added. Dissolved Hg (Hgaq) was periodically quantified using ultracentrifugation and chemical analysis following the addition of S(-II). Particle size and identity were determined using dynamic light scattering and X-ray absorption spectroscopy. S(-II) reacts with Hg to form 20 to 200 nm aggregates consisting of 1-2 nm HgS(s) subunits that are more structurally disordered than metacinnabar in the presence of 2 × 10−9 to 8 × 10−6 M Hg and 10 (mg C) L−1 DOM. Some of the HgS(s) nanoparticle aggregates are subsequently dissolved by DOM and (re)precipitated by S(-II) over periods of hours to days. At least three fractions of Hg-DOM species were observed with respect to reactivity toward S(-II): 0.3 μmol reactive Hg per mmol C (60 percent), 0.1 μmol per mmol C (20 percent) that are kinetically hindered, and another 0.1 μmol Hg per mmol C (20 percent) that are inert to reaction with S(-II). Following an initial S(-II)-driven precipitation of HgS(s), HgS(s) was dissolved by DOM or organic sulfur compounds. HgS(s) formation during this second phase was counterintuitively favored by lower S(-II) concentrations, suggesting surface association of DOM moieties that are less capable of dissolving HgS(s). DOM partially inhibits HgS(s) formation and mediates reactions between Hg and S(-II) such that HgS(s) is susceptible to dissolution. These findings indicate that Hg accessibility to microorganisms could be controlled by kinetic (intermediate) species in the presence of S(-II) and DOM, undermining the premise that equilibrium Hg species distributions should correlate to the extent or rate of Hg methylation in soils and sediments.  相似文献   

16.
Equilibrium stable isotope fractionations of mercury and thallium are estimated for molecules, atoms and ions using first-principles vibrational frequency and electronic structure calculations. These calculations suggest that isotopic variation in nuclear volume is the dominant cause of equilibrium fractionation, driving 205Tl/203Tl and 202Hg/198Hg fractionations of up to 3‰ at room temperature. Mass-dependent fractionations are smaller, ca. 0.5-1‰ for the same isotopes. Both fractionation mechanisms tend to enrich the neutron-rich isotopes in oxidized mercury- and thallium-bearing phases (Tl3+ and Hg2+) relative to reduced phases (Tl+ and Hg0). Among Hg2+-bearing species, inorganic molecules and complexes like HgCl2, and will have higher 202Hg/198Hg than coexisting methylmercury species, suggesting a possible application of Hg-isotope measurements to understanding mercury methylation and increasing methylmercury concentrations at the top of the food chain. Estimated 205Tl/203Tl fractionation between and is in reasonable agreement with the fractionations previously observed between seawater and Fe-Mn crusts, supporting an equilibrium-like reduction/oxidation fractionation mechanism.More generally, nuclear-volume isotope fractionation will concentrate larger (heavier) nuclei in species where the electron density at the nucleus is small—due to lack of s-electrons (e.g., Hg2+—[Xe]4f145d106s0 vs. Hg0—[Xe]4f145d106s2) or enhanced s-electron screening by extra p, d, or f electrons (e.g., Tl0—[Xe]4f145d106s26p1 vs. Tl+—[Xe]4f145d106s26p0). Nuclear-volume fractionations become much smaller for lighter elements, declining from ∼1‰/amu for thallium and mercury to ∼0.2‰/amu for ruthenium and ∼0.02‰/amu for sulfur.  相似文献   

17.
The giant Almadén mercury deposit (Spain) is hosted by the Lower Silurian Criadero Quartzite; in turn this ore-bearing rock unit is cross-cut by the so-called Frailesca unit, a diatreme body of basaltic composition. The geochemical characteristics of the Silurian to Devonian Almadén District volcanic units indicate that these rocks originated from an enriched, evolving mantle source that ultimately yielded basanites–nephelinites to rhyolites, through olivine-basalts, pyroxene-basalts, trachybasalts, trachytes, very scarce rhyolites, and quartz-diabases. The Silurian intraplate alkaline volcanism developed in submarine conditions which triggered widespread hydrothermal activity resulting in Hg ore formation and pervasive alteration to carbonates. The δ18O, δ13C, and δ34S isotopic signatures for carbonates and pyrite suggest different sources for carbon and sulfur, including magmatic and organic for the former and magmatic and sea water for the latter. The most important and efficient natural source of mercury on Earth is by far the volcanic activity, which liberates mercury via quiescent degassing and catastrophic (Plinian) events when eruptions can overwhelm the atmospheric budget of Hg. Thus, we suggest that CO2 degasification and coeval distillation of mercury from the volcanic rocks fed the huge hydrothermal system that led to massive deposition of mercury at Almadén. Build up of Hg0gas in magmatic chambers during waning rifting in the Late Ordovician, followed by renewed volcanism in the Early Silurian, would have resulted in massive degasification of the accumulated mercury. Part of this mercury went into the Criadero Quartzite leading to formation of the huge Almadén deposit and others (e.g., El Entredicho) along the same stratigraphic level. Progressive depletion of the deep seated magmatic Hg stock would have resulted in a drastic reduction in ore deposit size after the Lower Silurian when smaller deposits formed (e.g., Las Cuevas).  相似文献   

18.
Mercury (Hg) concentrations and isotopic compositions were examined in shallow-water surface sediment (0-2 cm) from San Francisco (SF) Bay to determine the extent to which historic Hg mining contributes to current Hg contamination in SF Bay, and to assess the use of Hg isotopes to trace sources of contamination in estuaries. Inter-tidal and wetland sediment had total Hg (HgT) concentrations ranging from 161 to 1529 ng/g with no simple gradients of spatial variation. In contrast, inter-tidal and wetland sediment displayed a geographic gradient of δ202Hg values, ranging from −0.30‰ in the southern-most part of SF Bay (draining the New Almaden Hg District) to −0.99‰ in the northern-most part of SF Bay near the Sacramento-San Joaquin River Delta. Similar to SF Bay inter-tidal sediment, surface sediment from the Alviso Slough channel draining into South SF Bay had a δ202Hg value of −0.29‰, while surface sediment from the Cosumnes River and Sacramento-San Joaquin River Delta draining into north SF Bay had lower average δ202Hg values of −0.90‰ and −0.75‰, respectively. This isotopic trend suggests that Hg-contaminated sediment from the New Almaden Hg District mixes with Hg-contaminated sediment from a low δ202Hg source north of SF Bay. Tailings and thermally decomposed ore (calcine) from the New Idria Hg mine in the California Coast Range had average δ202Hg values of −0.37 and +0.03‰, respectively, showing that Hg calcination fractionates Hg isotopes resulting in Hg contamination from Hg(II) mine waste products with higher δ202Hg values than metallic Hg(0) produced from Hg mines. Thus, there is evidence for at least two distinct isotopic signals for Hg contamination in SF Bay: Hg associated with calcine waste materials at Hg mines in the Coast Range, such as New Almaden and New Idria; and Hg(0) produced from these mines and used in placer gold mines and/or in other industrial processes in the Sierra Nevada region and SF Bay area.  相似文献   

19.
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   

20.
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   

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