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1.
The River Nura in Central Kazakhstan has been heavily polluted by Hg originating from an acetaldehyde plant. A number of studies were undertaken to investigate the transport, fate and bioavailability of Hg in this river system. The sediments within a 20 km section of the river downstream of the effluent outfall canal are highly polluted and are acting as a strong source of surface water contamination. Mercury transport in the river is dominated by the remobilization of contaminated bed sediments and river bank erosion during the annual spring flood. Peak Hg concentrations in unfiltered surface water samples during a larger than usual flood event in 2004 were in the order of 1600–4300 ng L−1. The majority of the particulate-bound Hg appears to be sedimented in the shallow Intumak reservoir 75 km downstream of the source of the pollution, leading to a drop in aqueous Hg concentrations by an order of magnitude. Nevertheless, background concentrations of Hg in surface water are not reached until at least 200 km downstream, and during the flood period Hg is also detected in the terminal wetlands of the river.Mercury concentrations in sediment cores taken from the river bed in the most contaminated section of the Nura ranged from 9.95 to 306 mg kg−1. Methylmercury (MeHg) levels in shallow sediment cores were highest in surface sediments and ranged between 4.9 and 39 μg kg−1, but were generally less than 0.1% of total Hg (THg). A significant inverse relationship was found between THg concentrations and the percentage of MeHg formed in the sediments, irrespective of the sampling depth. The observed relationship was confirmed by comparison with results from a different river system, indicating that it may be true also for other highly contaminated aquatic systems. It is hypothesized that at high THg levels in severely contaminated sediments, the accumulation of MeHg may be limited by increasingly efficient demethylation processes, and that this underlying trend in sediments is the reason why MeHg levels in surface water are often found to be higher at less contaminated sites compared to upstream sites.Mercury concentrations in biota in the most contaminated section of the river were 15–20 times higher than background levels. Fish were found to be impacted for more than 125 km downstream from the source, indicating significant transport of dissolved MeHg to downstream areas and/or in-situ MeHg production in less contaminated downstream reaches. There were also indications that impoundments may increase the bioavailability of Hg.  相似文献   

2.
Historic Hg mining in the Cache Creek watershed in the Central California Coast Range has contributed to the downstream transport of Hg to the San Francisco Bay-Delta. Different aspects of Hg mobilization in soils, including pedogenesis, fluvial redistribution of sediment, volatilization and eolian transport were considered. The greatest soil concentrations (>30 mg Hg kg−1) in Cache Creek are associated with mineralized serpentinite, the host rock for Hg deposits. Upland soils with non-mineralized serpentine and sedimentary parent material also had elevated concentrations (0.9–3.7 mg Hg kg−1) relative to the average concentration in the region and throughout the conterminous United States (0.06 mg kg−1). Erosion of soil and destabilized rock and mobilization of tailings and calcines into surrounding streams have contributed to Hg-rich alluvial soil forming in wetlands and floodplains. The concentration of Hg in floodplain sediment shows sediment dispersion from low-order catchments (5.6–9.6 mg Hg kg−1 in Sulphur Creek; 0.5–61 mg Hg kg−1 in Davis Creek) to Cache Creek (0.1–0.4 mg Hg kg−1). These sediments, deposited onto the floodplain during high-flow storm events, yield elevated Hg concentrations (0.2–55 mg Hg kg−1) in alluvial soils in upland watersheds. Alluvial soils within the Cache Creek watershed accumulate Hg from upstream mining areas, with concentrations between 0.06 and 0.22 mg Hg kg−1 measured in soils 90 km downstream from Hg mining areas. Alluvial soils have accumulated Hg released through historic mining activities, remobilizing this Hg to streams as the soils erode.  相似文献   

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

4.
《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   

5.
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   

6.
Surface sediments from the subtropical Pearl River estuary and adjacent South China Sea were investigated by molecular organic geochemical methods to determine the composition, distribution and origin of extractable lipids (n-alkanes, n-alkanols and sterols). The absolute and organic C normalized concentrations of total alkane, n-alkanol, and sterol ranged from 0.16 to 2.67 μg g−1 and 0.9 to 12.3 μg g−1 OC, 24.4 to 427.3 ng g−1 and 63.2 to 1966.7 ng g−1 OC, and 9.0 to 493.5 ng g−1 and 58.4 to 1042.4 ng g−1 OC, respectively. The spatial distributions of these biomarkers indicated that terrestrial-derived molecular biomarkers such as long-chain n-alkanes, n-alkanols and plant-derived sterols were higher at the river mouth and along the coastline, suggesting that a higher proportion of terrestrial particulate organic matter was deposited there. Relatively lower amounts of marine-derived biomarkers such as short-chain n-alkanes, algal sterols at the river mouth reflected the lower primary productivity due to high turbidity. The spatial patterns of these biomarkers were partially related to the estuarine processes and conditions, evidencing an increased terrestrial signal from the Pearl River mouth to the inner estuary, and enhanced marine conditions further offshore.  相似文献   

7.
For a period of 2 a, pore water composition in a heavily contaminated river floodplain soil was monitored in situ. Pore water samples were collected 12 times over all seasons in a profile ranging from aerobic to sulphidic redox conditions, and As, Cd, Cr, Cu, Pb, Zn, Mn, Fe, Ca, Cl, SO4, DOC, IOC and pH were determined. The variability of pH, IOC, DOC and Ca was found to be rather small during the year and within the profile (rsd < 0.04, 0.16, 0.24 and 0.22, respectively). The temporal variability of the metal and As concentrations was small, too, whereas changes with depth were distinct. Under sulphidic conditions, concentrations were below 1 μg L−1 (Cd, Cu, Pb) or 10 μg L−1 (Zn, As). The data set was compared with results from a geochemical model that was fully parameterised from literature data and included equilibrium speciation, sorption and mineral dissolution. The general pattern of the solid–solution partitioning of Cd, Cu, Zn and As in the profile was predicted well by mechanistic geochemical modelling on the basis of solid phase composition. Metals strongly bound to organic matter such as Cd and Cu were predicted better than metals mainly present within a mineral. Detailed information regarding the presence of colloidal Fe and Mn in pore water might improve the prediction of the solid–solution partitioning of a number of metals. The study also indicates that the chemical behaviour of Pb is still not understood sufficiently.  相似文献   

8.
The Mapocho river, which crosses downtown Santiago, is one of the most important rivers in contact with a population of about six million inhabitants. Anthropogenic activities, industrialization, farming activities, transport, urbanization, animal and human excretions, domestic wastes and copper mining have affected the river, contaminating it and its sediments with heavy metals. Concentration and distribution of Cu, Zn, Pb and Cd were studied with the purpose of determining their bioavailability and their relation with the characteristics of the sediments. Freshly deposited seasonal sediments were collected from 0–8 cm depths from 6 locations (S1 to S6) along the 30-km long channel length, in the four seasons of year on the following dates: May 2001 (D1, autumn); August 2001 (D2, winter); October 2001 (D3, spring) and January 2002 (D4, summer). The dried samples were sifted to obtain the < 63-μm sediment fraction, since it has been shown that large amounts of heavy metals are bound in the fine-grained fraction of the sediment. Cu and Zn were analyzed by atomic absorption spectrophotometry and Pb and Cd by square wave anodic stripping voltammetry. The highest concentrations of Cu (2850 μg g− 1) were found in the northern part of the river (S1, average D1–D4), near the mountains and a copper mine, and then decreased downstream to 209 μg g− 1 (S6). Total Zn showed an irregular variation, with higher values at S1 (1290 μg g− 1) and high values in some winter sampling (1384 μg g− 1 S4, S5–D2). Pb showed different trends, increasing from S1 to S6 (17 to 61 μg g− 1), with the highest values in the summer samples (83 μg g− 1, S4–S6, D4), and total Cd increased slightly from mean values of 0.2 and 0.5 μg g− 1. Partition into five fractions was made using Tessier's analytical sequential extraction technique; the residue was treated with aqua regia for recovery studies, although this step is not part of the Tessier procedure. The results show that Cu, Zn and Pb in the sediments were dependent on the sampling places along the river, and variation in two years was low (D1–D4). The highest values of total organic matter, carbonate and conductivity were found in S6, which has the smallest size particles, while at S1 the sediments were predominantly sand and contain larger amounts of silica. Cu associated with carbonate decreased gradually from 58% (1771 μg g− 1, S1) to 16% (32 μg g− 1, S6); Cu bonded to reducible fraction was almost constant (33% to 37%), and Cu associated with oxidizable fraction increased from 7% (S1) to 34% (S6), but copper content was lower (214 to 68 μg g− 1). Zn had a similar fractionation profile. However, Pb bound to oxidizable fraction did not show significant percent variation along the river (20% to 19%), but the amount bounded was 4 to 12 μg g− 1. The residual fraction increased from 24% to 41% (5 to 25 μg g− 1, S1 to S6). The distribution of Cd in the sediment was almost independent of the sampling stations and was bound to carbonate, reducible and residual fraction in similar proportion. Cu and Zn at S1 were mainly bound to carbonates and reducible phases with 91% and 73% (2779 and 965 μg g− 1, respectively), and with a change in the pH and/or the redox potential of the sediment–water system, these contaminants could easily enter the food chain. In S6 the amount of Cu and Zn in these phases was 50% and 53% (100 to 313 μg g− 1, respectively).  相似文献   

9.
The distribution and nature of sedimentary organic matter (OM) have been examined in sediment cores collected from the lower reaches, including estuary, of the Godavari River in order to understand sedimentation patterns, sources, and diagenesis of OM. The samples were analyzed for organic carbon (Corg), total nitrogen, amino acids and hexosamines. The observed irregular trends in Corg distribution with depth indicate the unstable nature of bed sediment in the lower reaches of the river. Yet, in the lower estuarine region, regular trends in Corg distribution with depth reflect the deposition of sediment. The atomic ratio of Corg and total nitrogen (C/N; 10.5–16.1) also supported this observation. The distribution of amino acids and diagenetic indicators (β-ala+γ-aba mol.%, AA/HA and Glc-NH2/Gal-NH2) in individual cores revealed the post-depositional changes in the OM. In the core sediment from the lower reaches, there was no clear cut trend in amino acid content with depth. In the estuarine region, however, amino acid content was very low (50.5 and 186.5 μg g−1) in the upper layers compared to that in the lower layers (558.5 and 1099.3 μg g−1). Reactivity index (range 0.3–3.7) revealed that OM in the upper few centimeters, especially in the lower estuarine region, was more reactive relative to that in the deeper layers.  相似文献   

10.
This study reports on the behavior of two redox-sensitive elements, As and Sb, along the turbidity gradient in the freshwater reaches of the turbid Gironde Estuary. During a 17-month survey, surface water and suspended particulate matter (SPM) were sampled monthly at six sites representing both fluvial branches of the Gironde Estuary. Additionally, two longitudinal high resolution profiles were sampled along the fluvial estuary of the Garonne Branch during two contrasted seasons, i.e. with and without the presence of the maximum turbidity zone (MTZ). Seasonal variability and spatial distribution of dissolved (<0.2 μm; <0.02 μm) and particulate As, Sb and Fe were measured and combined with SPM data to understand metalloid behavior in the estuarine freshwater turbidity gradient.At the two main fluvial entries of the Gironde Estuary, dissolved As and Sb concentrations showed strong (by a factor of 2–4) seasonal variations, that were only partly controlled by discharge-related dilution. Seasonal addition of dissolved As and Sb was attributed to the degradation of particulate As and Sb carrier phases in bottom sediment and/or in the adjacent aquifers, rather than release from SPM. In the surface freshwater reaches of the Gironde Estuary, Sb behaved conservatively under all hydrological conditions. In contrast, As was strongly reactive in the presence of the MTZ, with opposite behaviors in the two fluvial branches of the estuary: in the Garonne Branch As was removed from the dissolved phase, whereas in the Dordogne Branch As was added. Redistribution of As between the dissolved and the particulate phases along the turbidity gradient in estuarine freshwater only affected the <0.02 μm fraction, as the 0.02–0.2 μm fraction remained constant (300 ng L−1 in September 2005). Accordingly, As removal seemed to be decoupled from concomitant “colloidal” (0.02–0.2 μm) Fe flocculation in the turbidity gradient. The contrasting behavior of dissolved As in the fluvial estuaries of the Garonne and Dordogne Branches was attributed to sorption processes during equilibration of river-borne dissolved As with estuarine SPM forming the MTZ. This equilibrium, described by a distinct distribution coefficient Kd(As)  11,000 L kg−1 in the MTZ, resulted in either As release (desorption; Dordogne Branch) or removal (adsorption; Garonne Branch) in the respective fluvial estuaries. A mixing experiment under controlled laboratory conditions tended to support that equilibration between the dissolved phase and MTZ particles may induce both As release and removal in the estuarine freshwater reaches, with As distribution evolving towards a distinct Kd value for increasing SPM concentrations. The long-term survey allowed estimating annual (2004) dissolved fluxes of As and, for the first time Sb, at the main fluvial entries of the Gironde Estuary at 30.7 t a−1 and 3.2 t a−1 (Garonne River) and at 8.0 t a−1 and 2.3 t a−1 (Dordogne River), respectively.  相似文献   

11.
Xiamen Bay (XMB) has received substantial loadings of pollutants from industrial and municipal wastewater discharged since the 1980s. To assess ecological risks and the current spatial changes of metal contaminants in bottom surface sediments, 12 samples were collected. Samples were subjected to a total digestion technique and analyzed by ICP–OES for Cu, Pb, Zn, Cr, and Cd, and by AFS for Hg and As. Among these metals, Zn had the highest values (68–268 mg kg−1), followed by Pb (27–71 mg kg−1), and lower concentrations were found for Cd (42–1,913 μg kg−1) and Hg (0–442 μg kg−1). In comparison with the average crustal abundance values, the results indicated that nearly half of the sediment samples of XMB and its adjacent areas were contaminated by Cd, Pb, Zn, and As. Furthermore, based on the modified BCR sequential extraction procedure, the chemical speciation of heavy metals (Cd, Cr, Cu, Pb, Zn, Hg, and As) in selected sediment samples were evaluated in this study. Data from BCR sequential extractions indicated that Cd posed a medium ecological risk, whereas, Cr posed low risk since its exchangeable and carbonate fractions were below 4%, and the mobility of heavy metals in XMB decreased in the order Cd > Pb > Cu > Zn > Hg > As > Cr. By applying mean effects range median quotients (mERMQ), the results showed that Yuandang Lagoon with mERMQ value >0.5 would be expected to have the greatest potential toxic risk in amphipod within XMB and its adjacent areas.  相似文献   

12.
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   

13.
The Wanshan Hg mining area in Guizhou, China, was one of the world’s largest Hg producing regions. Numerous mine-waste and calcines still remain, leaching Hg to local rivers and streams and potentially impacting the local population. Several studies have been published on local environmental impacts of these mining and retorting residues, but a comprehensive, regional survey on the distribution of Hg in the rivers in the region, as presented in this paper, has not previously been conducted. This study focuses on the regional distribution and temporal variation of aqueous Hg fractions in the five main watercourses draining the Wanshan Hg mining and retorting area, covering more than 700 km2. Three sampling campaigns were carried out in 2007 and 2008, covering high flow, normal flow and low flow periods. Total (THg), particulate (PHg), dissolved (DHg) and reactive (RHg) Hg fractions were determined. All rivers had the highest Hg concentrations at sample sites about 100–500 m downstream of the mine wastes. Total Hg concentrations ranged from extremely high (up to 12,000 ng L−1) at the sample site just 100 m below mine wastes, to quite low in tributary streams (1.9 ng L−1, about 14 km downstream of the mine wastes). Total Hg and PHg concentrations were usually highest during high flow periods in the Hg-contaminated areas (i.e. THg ? 50 ng L−1), while in the less-impacted downstream areas (with THg < 50 ng L−1) the Hg concentrations were usually lowest during high flow periods. Although highly elevated concentrations of Hg in water samples were found just downstream of the mine wastes, the concentrations decreased sharply to well below 50 ng L−1 (US EPA Hg concentration standard for protection of fresh water), within only 6–8 km downstream. Concentrations of THg were highly dominated by and correlated with PHg (R2 = 0.996–0.999, P < 0.001); PHg constituted more than 80% of THg in Hg-contaminated areas, and could account for 99.6% of the THg close to the mine wastes.  相似文献   

14.
M. Doi  G. Warren  M.E. Hodson   《Applied Geochemistry》2005,20(12):2207-2216
Ochre is an unwanted waste product that accumulates in wetlands and streams draining abandoned coal and metal mines. A potential commercial use for ochre is to remediate As contaminated soil. Arsenic contaminated soil (605 mg kg−1) was mixed with different ochres (A, B and C) in a mass ratio of 1:1 and shaken in 20 mL of deionised water. After 72 h As concentration in solution was ca. 500 μg kg−1 in the control and 1–2.5 μg kg−1 in the ochre treated experiments. In a second experiment soil:ochre mixtures of 0.05–1:1 were shaken in 20 mL of deionised water for 24 h. For Ochres A and C, as solution concentration was reduced to ca. 1 μg kg−1 by 0.2–1:1 ochre:soil mixtures. For Ochre B, as concentration only reached ca. 1 μg kg−1 in the 1:1 ochre:soil mix. Sorption of As was best modelled by a Freundlich isotherm using As sorption per mass of goethite in the ochre (log K = 1.64, n = 0.79, R2 = 0.76, p 0.001). Efficiency of ochre in removing As from solution increased with increasing total Fe, goethite, citrate dithionite extractable Fe and surface area.  相似文献   

15.
Cinnabar (α-HgS) and metacinnabar (β-HgS) dissolved at environmentally significant rates in oxygenated slurry experiments simulating a low-flow fluvial system. Based on SO42− production, cinnabar dissolution rates were 2.64 to 6.16 μmol (SO42−) m− 2 day− 1, and metacinnabar dissolution rates were 1.20 to 1.90 μmol (SO42−) m− 2 day− 1. Monodentate-bound thiosulfate (S2O32−) was identified as an oxidation product on the HgS surface by ATR-IR spectroscopy based on strong infrared absorption bands in the 1140–1145 cm− 1 and 1006–1014 cm− 1 regions. The presence of sulfide oxidation intermediates on the HgS surface indicates that SO42− concentration underestimates α-HgS and β-HgS dissolution in this setting. Mercury release rates during dissolution were more than two orders of magnitude less than SO42− production, but were significant: 0.47 mg (Hg) m− 2 y− 1 from cinnabar [6.45 nmol (Hg) m− 2 day− 1], and 0.17 mg (Hg) m− 2 y− 1 from metacinnabar [2.29 nmol (Hg) m− 2 day− 1]. The Hg mobilized during α-HgS and β-HgS dissolution is sufficient to form natural Au–Hg amalgam in downstream placer settings. The proportion of mercury that is not remobilized during α-HgS and β-HgS dissolution likely adsorbs to the dissolving mercuric sulfide. Adsorption of Hg2+ to cinnabar was detected in situ by anodic stripping voltammetry using a cinnabar-modified carbon paste electrode following accumulation of Hg2+ on the electrode at open circuit potential.  相似文献   

16.
The Minqin Basin is a type area for examining stress on groundwater resources in the Gobi Desert, and has been investigated here using a combination of isotopic, noble gas and chemical indicators. The basin is composed of clastic sediments of widely differing grain size and during the past half century over 10 000 boreholes have been drilled with a groundwater decline of around 1 m a−1. Modern diffuse recharge is unlikely to exceed 3 mm a−1, as determined using unsaturated zone profiles and Cl− mass balance. A small component of modern (<50 a) groundwater is identified in parts of the basin from 3H–3He data, probably from irrigation returns. A clear distinction is found between modern waters with median δ18O values of 6.5 ± 0.5‰ and most groundwaters in the basin with more depleted isotopic signatures. Radiocarbon values as pmc range from 0.6% to 85% modern, but it is difficult to assign absolute ages to these, although a value of 20% modern C probably represents the late Pleistocene to Holocene transition. The δ13C compositions remain near-constant throughout the basin (median value of −8.1‰ δ13C) and indicate that carbonate reactions are unimportant and also that little reaction takes place. There is a smooth decrease in 14C activity accompanied by a parallel increase in 4He accumulations from S–N across the basin, which define the occurrence of a regional flow system. Noble gas temperatures indicate recharge temperatures of about 5.6 °C for late Pleistocene samples, which is some 2–3 °C cooler than the modern mean annual air temperature and the recharge temperature obtained from several Holocene samples. Groundwaters in the Minqin Basin have salinities generally below 1 g/L and are aerobic, containing low Fe but elevated concentrations of U, Cr and Se (mean values of 27.5, 5.8 and 5.3 μg L−1, respectively). Nitrate is present at baseline concentrations of around 2 mg L−1 but there is little evidence of impact of high NO3 from irrigation returns. Strontium isotope and major ion ratios suggest that silicate reactions predominate in the aquifer. The results have important implications for groundwater management in the Minqin and other water-stressed basins in NW China – a region so far destined for rapid development. The large proportion of the water being used at present is in effect being mined and significant changes are urgently needed in water use strategy.  相似文献   

17.
The geochemistry of Sepetiba Bay was studied in four sediment cores using a multi-element approach. Two cores were sampled in the more contaminated eastern part of the bay and two cores were sampled in the western region. The aim was to determine whether less common elements like the rare earths or the actinides are associated with contaminant metals like zinc in the Bay. Samples were analysed by instrumental neutron activation analysis that permits the quantification of total concentrations of metals (Ba, Co, Cr, Cs, Fe, Hf, Rb, Sc, Zn), rare earth elements (Ce, Eu, La, Lu, Sm and Yb), actinides (Th, U), non-metals and semi-metals (As, Br). Organic carbon and total sulphur were also analysed. The results show very strong zinc contamination in the top layers (more than 1000 μg g−1) and background concentrations in the bottom (15 μg g−1). Elements like chromium which would be expected to be released by the heavy industries of Sepetiba Bay, did not show a contamination profile, and concentrations remained close to those of natural environments. No evidence of any association between the zinc and other potential contaminant elements could be identified in this work.  相似文献   

18.
A soil geochemical survey was conducted in a 27,000-km2 study area of northern California that includes the Sierra Nevada Mountains, the Sacramento Valley, and the northern Coast Range. The results show that soil geochemistry in the Sacramento Valley is controlled primarily by the transport and weathering of parent material from the Coast Range to the west and the Sierra Nevada to the east. Chemically and mineralogically distinctive ultramafic (UM) rocks (e.g. serpentinite) outcrop extensively in the Coast Range and Sierra Nevada. These rocks and the soils derived from them have elevated concentrations of Cr and Ni. Surface soil samples derived from UM rocks of the Sierra Nevada and Coast Range contain 1700–10,000 mg/kg Cr and 1300–3900 mg/kg Ni. Valley soils west of the Sacramento River contain 80–1420 mg/kg Cr and 65–224 mg/kg Ni, reflecting significant contributions from UM sources in the Coast Range. Valley soils on the east side contain 30–370 mg/kg Cr and 16–110 mg/kg Ni. Lower Cr and Ni concentrations on the east side of the valley are the result of greater dilution by granitic sources of the Sierra Nevada.Chromium occurs naturally in the Cr(III) and Cr(VI) oxidation states. Trivalent Cr is a non-toxic micronutrient, but Cr(VI) is a highly soluble toxin and carcinogen. X-ray diffraction and scanning electron microscopy of soils with an UM parent show Cr primarily occurs within chromite and other mixed-composition spinels (Al, Mg, Fe, Cr). Chromite contains Cr(III) and is highly refractory with respect to weathering. Comparison of a 4-acid digestion (HNO3, HCl, HF, HClO4), which only partially dissolves chromite, and total digestion by lithium metaborate (LiBO3) fusion, indicates a lower proportion of chromite-bound Cr in valley soils relative to UM source soils. Groundwater on the west side of the Sacramento Valley has particularly high concentrations of dissolved Cr ranging up to 50 μg L−1 and averaging 16.4 μg L−1. This suggests redistribution of Cr during weathering and oxidation of Cr(III)-bearing minerals. It is concluded that regional-scale transport and weathering of ultramafic-derived constituents have resulted in enrichment of Cr and Ni in the Sacramento Valley and a partial change in the residence of Cr.  相似文献   

19.
The Okchon black shale in Korea provides a typical example of natural geological materials enriched with potentially toxic elements. The Chung-Joo, Duk-Pyung, Geum-Kwan, I-Won, Bo-Eun and Chu-Bu areas are underlain by these black shales and slates of the Guryongsan Formation or the Changri Formation, which are parts of the Okchon Group in the central part of the southern Korean Peninsula. In order to investigate the enrichment levels and dispersion patterns of potentially toxic elements in the rock–soil–plant system, environmental geochemical surveys were undertaken in the above six study areas in the Okchon Zone. After appropriate preparation, rock and soil samples were analyzed for potentially toxic elements by instrumental neutron activation analysis (INAA) and inductively coupled plasma atomic emission spectrometry (ICP-AES), and plant samples by atomic absorption spectrometry (AAS). In particular, Ba, Cd, Mo, V and U in Okchon black shales are highly enriched, and their mean concentrations are significantly higher than those in black slates. These elements are geochemically associated, and might be enriched simultaneously. The highest mean concentrations of 42.0 μg g−1 As, 2100 μg g−1 Ba, 10.9 μg g−1 Cd, 213 μg g−1 Mo, 83 μg g−1 U, 938 μg g−1 V and 394 μg g−1 Zn are found in black shales from the Duk-Pyung area. Mean concentrations of As, Mo and U in soils overlying black shales occurring in the Duk-Pyung area (30 μg g−1 As, 24 μg g−1 Mo and 50 μg g−1 U) and Chu-Bu area (39 μg g−1 As, 15 μg g−1 Mo and 27 μg g−1 U) are higher than the permissible level. Enrichment index values of the six study areas decrease in the order of Duk-Pyung > Chu-Bu > Bo-Eun > Chung-Joo > Geum-Kwan = I-Won areas. Relationships between trace element concentrations in soils and plants are significantly correlated, and the biological absorption coefficients (BAC) in plants are in the order of Cd > Zn = Cu > Pb, which suggests that Cd is more bioavailable to plants than the other elements. Cadmium concentrations in plant species decrease in the order of chinese cabbage > red pepper > soybean = sesame > rice stalk > corn > rice grain. From the result of sequential extraction analysis of soils, relatively high proportions of Cu, Pb and Zn are present as residual fractions, and that of Cd as non-residual fractions. Cadmium occurs predominantly as exchangeable/water-acid soluble phase in soils, and this is in agreement with the findings of high Cd concentrations in plants.  相似文献   

20.
Radiocaesium (137Cs) dispersion and Cs+ fixation were studied in the sediments collected from the lagoon systems of “Ria de Aveiro”. The Cs+ sorption was tested for the fine mica grains and for the < 2 μm clay fractions extracted from silty clays. The Cs+ exchange is found strongly onto mica-rich fractions than smectite-rich fractions. The distribution coefficient increases if the silty material is constituted by rich-mica clay fractions or if the non-clay minerals are removed from the silty-clay material. The samples studied behave as multisite ion exchange, where Cs+ engages in ion-exchange reactions with hydrated cations on planar sites on expansible layer silicates. Higher concentrations of the 137Cs were found associated with mica-rich silty clays. The 137Cs ranges from 3.2 to 3.9 Bq kg− 1 in the < 38 μm fractions and from 2.9 to 3.3 Bq kg− 1 in the < 64 μm fractions.  相似文献   

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