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1.
Mine tailings at the former Delnite gold mine in northern Ontario were characterized to assess the impact of a biosolids cover on the stability of As species and evaluate options for long-term management of the tailings. Arsenic concentrations in the tailings range from 0.15 to 0.36 wt% distributed among goethite, pyrite and arsenopyrite. Pyrite and arsenopyrite occur as small and liberated particles that are enveloped by goethite in the uncovered tailings and the deeper portions of the biosolids-covered tailings. Sulfide particles in the shallower portions of the biosolids-covered tailings are free of goethite rims. Arsenic occurs predominantly as As5+ with minor amount of As1− in the uncovered tailings. Coinciding with the disappearence of goethite rims on sulfide particles, the biosolids-covered tailings have As3+ species gradually increasing in proportion towards the cover. Leaching tests indicated that the As concentrations in the leachate gradually increase from less than 0.085 to 13 mg/L and Fe from 28 to 179 mg/L towards the biosolids cover. These are in sheer contrast to the leachate concentrations of less than 0.085 mg/L As and 24–64 mg/L Fe obtained from the uncovered tailings confirming the role of biosolids-influenced reduction and mobilization of As in the form of As3+ species. The evidence suggests that reductive dissolution of goethite influenced by the biosolids-cover caused the mobilization of As as As3+ species.  相似文献   

2.
An exploratory study has been conducted to test the utility of automated mineral analysis observations to identify flue dust particles in topsoils exposed for several decades to emissions of a copper smelter. The methods used are readily available in mining countries. To identify the most impacted sites, the Cu, Zn, Pb, Mo and As levels in water and diluted sulphuric acid extractions of four topsoil size fractions (833–495 μm, 246–148 μm; 74–38 μm; <38 μm) were analysed. X-ray diffraction analyses were used to demonstrate the mineralogical degradation of smectite phases when approaching the smelter. Flue dust particles in different states of conservation in topsoils were directly observed by scanning electron microscopy (SEM) aided by energy dispersive detection of X-rays. Qemscan® scanning of dispersed topsoil preparations (10,000 particles) pinpoints smelter particles by their density; flue dust pearls can be tracked by sorting particles according to their sphericity, clearly identifying them as pyrometallurgical products. When sorting soil particles by mineral groups (e.g. sulphides), an increase in this phase group can be observed when approaching the smelter. SEM resolution limits observations to particles larger than 2–3 μm. Smaller particles can be observed by transmission electron microscopy, although observer experience and the availability of equipment time are essential as is the case for SEM.  相似文献   

3.
Toxic metalliferous mine-tailings pose a significant health risk to ecosystems and neighboring communities from wind and water dispersion of particulates containing high concentrations of toxic metal(loid)s (e.g., Pb, As, Zn). Tailings are particularly vulnerable to erosion before vegetative cover can be reestablished, i.e., decades or longer in semi-arid environments without intervention. Metal(loid) speciation, linked directly to bioaccessibility and lability, is controlled by mineral weathering and is a key consideration when assessing human and environmental health risks associated with mine sites. At the semi-arid Iron King Mine and Humboldt Smelter Superfund site in central Arizona, the mineral assemblage of the top 2 m of tailings has been previously characterized. A distinct redox gradient was observed in the top 0.5 m of the tailings and the mineral assemblage indicates progressive transformation of ferrous iron sulfides to ferrihydrite and gypsum, which, in turn weather to form schwertmannite and then jarosite accompanied by a progressive decrease in pH (7.3–2.3).Within the geochemical context of this reaction front, we examined enriched toxic metal(loid)s As, Pb, and Zn with surficial concentrations 41.1, 10.7, 39.3 mmol kg−1 (3080, 2200, and 2570 mg kg−1), respectively. The highest bulk concentrations of As and Zn occur at the redox boundary representing a 1.7 and 4.2-fold enrichment relative to surficial concentrations, respectively, indicating the translocation of toxic elements from the gossan zone to either the underlying redox boundary or the surface crust. Metal speciation was also examined as a function of depth using X-ray absorption spectroscopy (XAS). The deepest sample (180 cm) contains sulfides (e.g., pyrite, arsenopyrite, galena, and sphalerite). Samples from the redox transition zone (25–54 cm) contain a mixture of sulfides, carbonates (siderite, ankerite, cerrusite, and smithsonite) and metal(loid)s sorbed to neoformed secondary Fe phases, principally ferrihydrite. In surface samples (0–35 cm), metal(loid)s are found as sorbed species or incorporated into secondary Fe hydroxysulfate phases, such as schwertmannite and jarosites. Metal-bearing efflorescent salts (e.g., ZnSO4·nH2O) were detected in the surficial sample. Taken together, these data suggest the bioaccessibility and lability of metal(loid)s are altered by mineral weathering, which results in both the downward migration of metal(loid)s to the redox boundary, as well as the precipitation of metal salts at the surface.  相似文献   

4.
The aim of this study was to investigate the accumulation of arsenic (As) in and on roots of Zea mays (maize) and Helianthus annuus (sunflower) by means of synchrotron-based micro-focused X-ray fluorescence imaging (μ-XRF). Plant and soil samples were collected from two field sites in the Hetao Plain (Inner Mongolia, China) which have been regularly irrigated with As-rich groundwater. Detailed μ-XRF element distribution maps were generated at the Fluo-beamline of the Anka synchrotron facility (Karlsruhe Institute of Technology) to assess the spatial distribution of As in thin sections of plant roots and soil particles. The results showed that average As concentrations in the roots (14.5–27.4 mg kg−1) covered a similar range as in the surrounding soil, but local maximum root As concentrations reached up to 424 mg kg−1 (H. annuus) and 1280 mg kg−1 (Z. mays), respectively. Importantly, the results revealed that As had mainly accumulated at the outer rhizodermis along with iron (Fe). We therefore conclude that thin crusts of Fe-(hydr)oxides cover the roots and act as an effective barrier to As, similar to the formation of Fe plaque in rice roots. In contrast to permanently flooded rice paddy fields, regular flood irrigation results in variable redox conditions within the silty and loamy soils at our study site and fosters the formation of Fe-(hydr)oxide plaque on the root surfaces.  相似文献   

5.
Temporal changes of As concentration in surface waters were observed in some areas of the Czech Republic. Mobilized As originates from past atmospheric deposition. To understand the factors influencing As aqueous concentration and mobility the chemistry and runoff generation of a number of brooks, springs and rivers in the central part of the Elbe River catchment, Czech Republic, were monitored. Seasonal variations of As (from 0.5 to 10.5 μg L−1), Fe (from 0.05 to 3.9 mg L−1) and DOC (dissolved organic C – from 1.2 to 17.5 mg L−1) were observed in monitored stream waters with maximum values of As and Fe in the summer months at pH values 7.6–7.8. The concentration of As in particles with a diameter < 60 μm correlates with the Fe concentration. There is no correlation between Fe and As in filtered samples (<0.45 μm). The As concentration in stream water colloids depends on an increase in DOC concentration and a decrease in ionic strength. The DOC stabilizes As in solution and reduces its re-adsorption on Fe colloids and consequently As concentration in the stream increases.  相似文献   

6.
We evaluated the concentration, size and distribution, and temporal variation of insoluble dust micro-particles in the snow, rainfall and water taken from the areas surrounding the Mt. Yulong to define the characteristics of modern atmospheric dust deposition and the contributions of different dust sources. The mean mass concentration (4511 μg kg−1) of micro-particles with 0.57 < d < 26 μm, and the diameter (11.5 μm) of dust contained in the water bodies of the Mt. Yulong are roughly similar to those observed in other sites, implying that dust is primarily supplied through short-range transport from proximal source regions (several or hundreds of km distances). The mean mass concentrations of micro-particles with 0.57 < d < 26 μm is lower in the rainfall than in the snow and the river water, suggesting the rain water is an ideal source/carrier for detecting the characteristics of modern atmospheric micro-particles. Volume size distributions of micro-particles in the snow and water showed single modal structures having volume median diameters from 3 to 26 μm. Number concentrations of micro-particles in the snow were higher than that in the rainfall, the river water contains the least amount of micro-particles. Vertical profiles of the snowpits show that there is a strong lateral correlation among the dust peaks, indicating a regional uniformity of dust deposition and suitability of snow analysis for dust deposition. In addition, the bare rock of snow-free terrain in the Mt. Yulong region and the mineral particles from local rock weathering are also important sources for the dust deposition.  相似文献   

7.
Hematite is a common primary/secondary mineral in mine drainage and mine waste settings that can adsorb dissolved metals and metalloids. This study explored the ability of synthetic hematite to retain one such contaminant, molybdate, on its surfaces under highly alkaline (pH = ∼10) conditions. X-ray diffraction (XRD), Raman spectroscopy (RS), scanning electron microscopy (SEM), and specific surface area (BET) analyses show that synthetic hematite particles are stable and able to adsorb molybdate. Raman spectra show that the hematite efficiently adsorbs molybdate and retains it on its surfaces via strong inner-sphere surface complexation. Inductively coupled plasma-mass spectrometry (ICP-MS) data indicate that hematite aged (7 and 9 days) at high and room temperatures (75 and 25 °C) retains adsorbed molybdate and that molybdate sorption increases with aging. SEM images show that aged hematite particles with adsorbed molybdate are similar in size and shape to pure hematite and exhibit no significant reduction in surface area. These findings are valuable for understanding the fate of Mo in mine wastes and mill tailings environments where the 2-line ferrihydrite to which it is adsorbed can transform to hematite.  相似文献   

8.
The historical (1932–1971) Bralorne mine produced over 87 million grams of Au from an archetypal orogenic lode gold deposit in southwest British Columbia. High concentrations of As in mine drainage, however, represent an on-going environmental concern prompting a detailed study of effluent chemistry. The discharge rate at the mine portal was monitored continuously over a fourteen-month period during which effluent samples were collected on a quasi-weekly basis. Water samples were also collected on synoptic surveys of the adit between the portal and the main source of flow in the flooded workings. Total concentrations of As in the mildly alkaline (pH = 8.7) portal drainage average 3034 μg/L whereas at the source they average 5898 μg/L. As emergent waters from the flooded workings flow toward the portal, their dissolved oxygen content and pH increase from 0 to 10 mg/L and from 7.7 to 9, respectively. Near the emergence point, dissolved Fe precipitates rapidly, sorbing both As(III) and As(V). With increasing distance from the emergence point, dissolved As(III) concentrations drop to detection limits through sorption on hydrous ferric oxide and through oxidation to As(V). Concentrations of dissolved As(V), on the other hand, increase and stabilize, reflecting lower sorption at higher pH and the lack of available sorbent. Nonetheless, based on synoptic surveys, approximately 35% of the source As load is sequestered in the adit resulting in As sediment concentrations averaging 8.5 wt%. The remaining average As load of 1.34 kg/d is discharged from the portal. Partitioning of As(V) between dissolved and particulate phases in portal effluent is characterized by a sorption density of 0.37 mol As (mol Fe)−1 and by a distribution coefficient (Kd) of 130 L/g HFO. The relatively high sorption density may reflect co-precipitation of As with Fe oxyhydroxides rather than a purely adsorption-controlled process. Results of this study show that the As self-mitigating capacity of drainage from orogenic lode gold deposits may be poor in high-pH and Fe-limited settings.  相似文献   

9.
《Applied Geochemistry》2006,21(10):1760-1780
Sulfide-rich mine tailings in Adak that are exposed to weathering cause acid mine drainage characterized by low pH (2–4) and high SO4 (up to 800 mg L−1). Surface water, sediment and soil samples collected in this study contain higher concentrations of As, Cu, Fe and Zn, compared to the target and/or intervention limits set by international regulatory agencies. In particular, high As concentrations in water (up to 2900 μg L−1) and sediment (up to 900 mg kg−1) are of concern. There is large variability in trace element concentrations, implying that both physical (grain size) and chemical factors (pH, secondary phases as sulfides, Al-oxides or clay minerals) play an important role in their distribution. The low pH keeps the trace elements dissolved, and they are transported farther downstream. Trace element partition coefficients are low (log Kd = 0.3–4.3), and saturation indices calculated with PHREEQC are <0 for common oxide and sulfidic minerals. The sediment and soil samples indicate an enhanced pollution index (up to 17), and high enrichment factors for trace elements (As up to 38,300; Zn up to 800). Finally, leaves collected from different plant types indicate bioaccumulation of several elements (As, Al, Cu, Fe and Zn). However, some of the plants growing in this area (e.g., Salix, Equisétum) are generally resistant to metal toxicity, and hence, liming and phytoremediation could be considered as potential on-site remediation methods.  相似文献   

10.
《Applied Geochemistry》2006,21(11):1986-1998
Elevated concentrations of Hg are present (averaging 36 μg/g), mainly as cinnabar, in the Murray Brook Au deposit, located in northern New Brunswick, Canada. After the mined ore was subjected to CN leaching, the tailings were deposited in an unsaturated pile, and 10 a after mine closure an estimated 4.7 × 103 kg of CN and 1.1 × 104 kg of Hg remain in the pile. Elevated Hg concentrations have been measured in the groundwater (up to 11,500 μg/L) and surface water (up to 32 μg/L) down-gradient of the tailings. To investigate the controls on Hg mobility and leaching persistence, laboratory experiments were conducted using unsaturated columns filled with tailings. Within the first 0.2 pore volumes (PV) eluted, the concentrations of Hg and CN increased to peak concentrations of 12,900 μg Hg/L and 16 mg CN/L, respectively. In the subsequent 0.9 PV, concentrations decreased to approximately 1300 μg Hg/L and 2.8 mg CN/L. Thermodynamic calculations demonstrate that >99.8% of the mobilized Hg in the tailings pore water is in the form of Hg–CN complexes, indicating that Hg mobility to the surrounding aquatic environment is directly dependent on the rate of CN leaching. One-dimensional transport simulations suggest that leached CN can be partitioned into conservative (24%) and non-conservative (76%) fractions. Extrapolation of simulation results to the field scale suggests that CN, and by extension Hg, will continue to elute from the tailings for at least an additional 130 a.  相似文献   

11.
Previous research has shown that Cu and Fe isotopes are fractionated by dissolution and precipitation reactions driven by changing redox conditions. In this study, Cu isotope composition (65Cu/63Cu ratios) was studied in profiles through sulphide-bearing tailings at the former Cu mine at Laver and in a pilot-scale test cell at the Kristineberg mine, both in northern Sweden. The profile at Kristineberg was also analysed for Fe isotope composition (56Fe/54Fe ratios). At both sites sulphide oxidation resulted in an enrichment of the lighter Cu isotope in the oxidised zone of the tailings compared to the original isotope ratio, probably due to preferential losses of the heavier Cu isotope into the liquid phase during oxidation of sulphides. In a zone with secondary enrichment of Cu, located just below the oxidation front at Laver, δ65Cu (compared to ERM-AE633) was as low as −4.35 ± 0.02‰, which can be compared to the original value of 1.31 ± 0.03‰ in the unoxidised tailings. Precipitation of covellite in the secondary Cu enrichment zone explains this fractionation. The Fe isotopic composition in the Kristineberg profile is similar in the oxidised zone and in the unoxidised zone, with average δ56Fe values (relative to the IRMM-014) of −0.58 ± 0.06‰ and −0.49 ± 0.05‰, respectively. At the well-defined oxidation front, δ56Fe was less negative, −0.24 ± 0.01‰. Processes such as Fe(II)–Fe(III) equilibrium and precipitation of Fe-(oxy)hydroxides at the oxidation front are assumed to cause this Fe isotope fractionation. This field study provides additional support for the importance of redox processes for the isotopic composition of Cu and Fe in natural systems.  相似文献   

12.
《Applied Geochemistry》2005,20(5):973-987
Due to liming of acid mine drainage, a calcite–gypsum sludge with high concentrations of Zn (24,400 ± 6900 μg g−1), Cu (2840 ± 680 μg g−1) and Cd (59 ± 20 μg g−1) has formed in a flooded tailings impoundment at the Kristineberg mine site. The potential metal release from the sludge during resuspension events and in a long-term perspective was investigated by performing a shake flask test and sequential extraction of the sludge. The sequentially extracted carbonate and oxide fractions together contained ⩾97% of the total amount of Cd, Co, Cu, Ni, Pb and Zn in the sludge. The association of these metals with carbonates and oxides appears to result from sorption and/or coprecipitation reactions at the surfaces of calcite and Fe, Al and Mn oxyhydroxides forming in the impoundment. If stream water is diverted into the flooded impoundment, dissolution of calcite, gypsum and presumably also Al oxyhydroxides can be expected during resuspension events. In the shake flask test (performed at a pH of 7–9), remobilisation of Zn, Cu, Cd and Co from the sludge resulted in dissolved concentrations of these metals that were significantly lower than those predicted to result from dissolution of the carbonate fraction of the sludge. This may suggest that cationic Zn, Cu, Cd and Co remobilised from dissolving calcite, gypsum and Al oxyhydroxides were readsorbed onto Fe oxyhydroxides remaining stable under oxic conditions. In a long-term perspective (≳102 a), ⩾97% of the Cd, Co, Cu, Ni, Pb and Zn content of the sludge potentially is available for release by dissolution of calcite and reductive dissolution of Fe oxyhydroxides if the sludge is subject to a soil environment with lower dissolved Ca concentrations, pH and redox than in the impoundment.  相似文献   

13.
The abandoned Sn-W Ribeira mine, northeast of Portugal, contained quartz veins with cassiterite, wolframite, scheelite, pyrite, arsenopyrite, sphalerite, chalcopyrite, manganocolumbite, bismuthinite, native bismuth, phosphates and carbonates. The exploration took place on the northern slope of the Viveiros stream, which is an affluent of the Sabor River. The waste-rock dumps and tailings were deposited on the hillside, close to the mine and are nowadays exposed to significant weathering and erosion, as they are not vegetated. The eroded material is transported by the Viveiros stream toward the Sabor River. A seasonal stream drains the tailings. The stream sediments samples were collected along the Viveiros stream, in the seasonal stream, in a seasonal spring at the bottom of the tailings, in the Sabor River and in other streams not affected by mine workings, following the mine influence along the Viveiros stream and in the Sabor River (1.2 km away from the mine workings). The data show that the degree of pollution increases along the Viveiros stream, especially in winter. The highest degree of pollution is for As, In, W, Sn and Bi. The sediments from the drainage of the main tailings are particularly polluted during winter, by Bi, In and Sn. The sedimentary precipitate from the spring is polluted in Cu, As, In, Sn, Ta, W, Bi, Zn, Nb, Ag, Sb and Ta. The sediments from the Sabor River are significantly polluted by As, Ag, In, Sn, W and Bi. The sediments from the regional streams, Viveiros stream and Sabor River have similar REE (NASC normalized) patterns (ΣREE = 131.7–185.9 mg/kg, LaN/LuN = 1.23–1.42 and Eu/Eu* = 1.02), while those from the seasonal stream, crossing the main tailings, are enriched in REE (ΣREE = 250.3–283.6 mg/kg, LaN/LuN = 1.6–2.09 and Eu/Eu* = 0.96). The general decrease in LaN/LuN values with increase in total Fe2O3 can be explained by the partitioning of HREE to the solid Fe-oxides phase. The sedimentary precipitate and coatings, which are mainly formed by Fe-oxy-hydroxides, but also contain jarosite, are impoverished in all REE. The impoverishment can be explained by the release of REE from the surface of the Fe-oxy-hydroxides, which occurs due to a local lowering of pH, caused by jarosite dissolution. During successive alternate cycles of wet and dry conditions, takes place the formation of Fe-oxy-hydroxides and jarosite in the sedimentary precipitate and coatings. The subsequent dissolution of jarosite releases acidity, thus promoting de-sorption of REE from the Fe-oxy-hydroxides mineral phases.  相似文献   

14.
Arsenic species including arsenite, arsenate, and organic arsenic were measured in the porewaters collected from Poyang Lake, the largest freshwater lake of China. The vertical distributions of dissolved arsenic species and some diagenetic constituents [Fe(II), Mn(II), S(−II)] were also obtained in the same porewater samples in summer and winter. In sediments the concentration profiles of total As and As species bound to Fe–Mn oxyhydroxides and to organic matter were also determined along with the concentrations of Fe, Mn and S in different extractable fractions. Results indicate that, in the summer season, the concentrations of total dissolved As varying from 3.9 to 55.8 μg/L in sediments were higher than those (5.3–15.7 μg/L) measured in the winter season, while the concentrations of total As species in the solid phase varied between 10.97 and 25.32 mg/kg and between 7.84 and 30.52 mg/kg on a dry weight basis in summer and winter, respectively. Seasonal profiles of dissolved As suggest downward and upward diffusion, and the flux of dissolved As across the sediment–water interface (SWI) in summer and winter were estimated at 3.88 mg/m2 a and 0.79 mg/m2 a, respectively. Based on porewater profiles and sediment phase data, the main geochemical behavior of As was controlled by adsorption/desorption, precipitation and molecular diffusion. The solubility and migration of inorganic As are controlled by Fe–Mn oxyhydroxides in summer whereas they appear to be more likely controlled by both amorphous Fe–Mn oxyhydroxides and sulfides in winter. A better knowledge of the cycle of As in Poyang Lake is essential to a better management of its hydrology and for the environmental protection of biota in the lake.  相似文献   

15.
The present study investigates the bioavailability, soil to plant transfer and health risks of arsenic (As) in the coastal part of Chianan Plain in southwestern Taiwan. Groundwater used for irrigation, surface soils from agricultural lands and locally grown foodstuffs were collected from eight locations and analyzed for As to assess the risks associated with consuming these items. The concentration of As in groundwater ranged from 13.8 to 881 μg/L, whereas surface soil showed total As content in the range of 7.92–12.7 mg/kg. The available As content in surface soil accounted for 0.06–6.71% of the total As content, and was significantly correlated with it (R2 = 0.65, p < 0.05). Among the leachable fraction, the organic matter (3.23–54.8%) and exchangeable portions of oxides (6.03–38.4%) appear to be the major binding phases of As. The average As content in fourteen studied crops and vegetables varied from 10.3 to 151 μg/kg with maximum in mustard and minimum in radish. All the plants showed considerably higher As content (21.5 ± 3.64–262 ± 36.2 μg/kg) in their roots compared to the edible parts (9.15 ± 1.44–75.8 ± 22.9 μg/kg). The bioaccumulation factor (BAF) based on total As (ranging from 0.0009 to 0.144) and available As in soil (ranging from 0.039 to 0.571) indicate that mustard, rice, amaranth and spinach are the highest accumulators of As. Although the health risk index (HRI) of the studied crops and vegetables ranged from only 0.0068–0.454, with the maximum in rice, the combined HRI indicates an alarming value of 0.88. Therefore, the possible health risks due to long-term consumption of rice and other As-rich foodstuffs could be overcome by controlling the contamination pathways in the water–soil–plant system.  相似文献   

16.
The petrological, geochemical, and mineralogical compositions of the coal-hosted Jurassic uranium ore deposit in the Yili Basin of Xinjiang province, northwestern China, were investigated using optical microscopy and field emission-scanning electron microscopy in conjunction with an energy-dispersive X-ray spectrometer, as well as X-ray powder diffraction, X-ray fluorescence, and inductively coupled plasma mass spectrometry. The Yili coal is of high volatile C/B bituminous rank (0.51–0.59% vitrinite reflectance) and has a medium sulfur content (1.32% on average). Fusinite and semifusinite generally dominate the maceral assemblage, which exhibits forms suggesting fire-driven formation of those macerals together with forms suggesting degradation of wood followed by burning. The Yili coals are characterized by high concentrations of U (up to 7207 μg/g), Se (up to 253 μg/g), Mo (1248 μg/g), and Re (up to 34 μg/g), as well as As (up to 234 μg/g) and Hg (up to 3858 ng/g). Relative to the upper continental crust, the rare earth elements (REEs) in the coals are characterized by heavy or/and medium REE enrichment. The minerals in the Yili coals are mainly quartz, kaolinite, illite and illite/smectite, as well as, to a lesser extent, K-feldspar, chlorite, pyrite, and trace amounts of calcite, dolomite, amphibole, millerite, chalcopyrite, cattierite, siegenite, ferroselite, krutaite, eskebornite, pitchblende, coffinite, silicorhabdophane, and zircon. The enrichment and modes of occurrence of the trace elements, and also of the minerals in the coal, are attributed to derivation from a sediment source region of felsic and intermediate petrological composition, and to two different later-stage solutions (a U–Se–Mo–Re rich infiltrational and a Hg–As-rich exfiltrational volcanogenic solution). The main elements with high enrichment factors, U, Se, As, and Hg, overall exhibit a mixed organic–inorganic affinity. The uranium minerals, pitchblende and coffinite, occur as cavity-fillings in structured inertinite macerals. Selenium, As, and Hg in high-pyrite samples mainly show a sulfide affinity.  相似文献   

17.
《Applied Geochemistry》2005,20(3):639-659
The oxidation of sulfide minerals from mine wastes results in the release of oxidation products to groundwater and surface water. The abandoned high-sulfide Camp tailings impoundment at Sherridon, Manitoba, wherein the tailings have undergone oxidation for more than 70 a, was investigated by hydrogeological, geochemical, and mineralogical techniques. Mineralogical analysis indicates that the unoxidized tailings contain nearly equal proportions of pyrite and pyrrhotite, which make up to 60 wt% of the total tailings, and which are accompanied by minor amounts of chalcopyrite and sphalerite, and minute amounts of galena and arsenopyrite. Extensive oxidation in the upper 50 cm of the tailings has resulted in extremely high concentrations of dissolved SO4 and metals and As in the tailings pore water (pH < 1, 129,000 mg L−1 Fe, 280,000 mg L−1 SO4, 55,000 mg L−1 Zn, 7200 mg L−1 Al, 1600 mg L−1 Cu, 260 mg L−1 Mn, 110 mg L−1 Co, 97 mg L−1 Cd, 40 mg L−1 As, 15 mg L−1 Ni, 8 mg L−1 Pb, and 3 mg L−1 Cr). The acid released from sulfide oxidation has been extensive enough to deplete carbonate minerals to 6 m depth and to partly deplete Al-silicate minerals to a 1 m depth. Below 1 m, sulfide oxidation has resulted in the formation of a continuous hardpan layer that is >1 m thick. Geochemical modeling and mineralogical analysis indicate that the hardpan layer consists of secondary melanterite, rozenite, gypsum, jarosite, and goethite. The minerals indicated mainly control the dissolved concentrations of SO4, Fe, Ca and K. The highest concentrations of dissolved metals are observed directly above and within the massive hardpan layer. Near the water table at a depth of 4 m, most metals and SO4 sharply decline in concentration. Although dissolved concentrations of metals and SO4 decrease below the water table, these concentrations remain elevated throughout the tailings, with up to 60,600 mg L−1 Fe and 91,600 mg L−1 SO4 observed in the deeper groundwater. During precipitation events, surface seeps develop along the flanks of the impoundment and discharge pore water with a geochemical composition that is similar to the composition of water directly above the hardpan. These results suggest that shallow lateral flow of water from a transient perched water table is resulting in higher contaminant loadings than would be predicted if it were assumed that discharge is derived solely from the deeper primary water table. The abundance of residual sulfide minerals, the depletion of aluminosilicate minerals in the upper meter of the tailings and the presence of a significant mass of residual sulfide minerals in this zone after 70 a of oxidation suggest that sulfide oxidation will continue to release acid, metals, and SO4 to the environment for decades to centuries.  相似文献   

18.
《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   

19.
《Applied Geochemistry》2006,21(9):1613-1624
Ingestion of soil is a common behaviour in young children as a means of exploring their surroundings. Much attention has been given to remediation of point-source polluted sites with regard to potential health risks for children. However, because of diffuse pollution and long-range atmospheric deposition, soil contaminant levels are generally increased in urban areas compared to their rural counterparts, even in areas located away from any point sources of pollution. Intake of urban soil can thereby result in significant amounts of the child’s daily metal intake. In the present study, soil samples were collected from 25 playgrounds around urban Uppsala, Sweden and analysed for contents of Al, As, Fe, Cr, Cu, Cd, Hg, Mn, Ni, Pb, W and Zn. Prior to aqua regia digestion, the samples were wet-sieved in order to separate soil particle fractions representing deliberate (<4 mm) and involuntary (<50 μm) soil ingestion by children, as well as a third size fraction of 50–100 μm representing soil that is easily transported by suspension. While the metal and As contents in the 50–100 μm fraction were similar to those of the <4 mm fraction, the <50 μm fraction had metal and As contents on average one and a half times higher than those of the <4 mm fraction. The metal and As contents correlated negatively with the sand content in both particle size fractions <4 mm and 50–100 μm, suggesting a general decrease in metal and As content with increasing sand content. However, a positive correlation was found between sand content and the metal and As contents of the finest fraction (<50 μm), suggesting that when the sand content is high, the bulk of the sorbed elements are on the finest particles. The difference between metal and As contents in the different size fractions was greater in the soil sample with the highest sand content than in the sample with the lowest sand content. This implies that texture is a significant factor in metal and As distribution in soils with moderate metal and As contents, when the number of binding sites associated with small particles is low. Tolerable daily intake (TDI) values for Pb and As were exceeded at all sites, and at two sites for Cd, for children with pica behaviour. A high ingestion rate of mainly small particles could also result in the TDI value for Pb being exceeded at 10 sites and that for As at one site. This study also found that soil analysis by the procedure recommended by Swedish authorities accurately represents the metal intake from deliberate soil ingestion, whereas involuntary soil ingestion of mainly small particles could result in metal intakes which are up to twice as high.  相似文献   

20.
Thick ferromanganese (Fe-Mn) crusts from four Cretaceous seamounts (The Paps, Tropic, Echo and Drago) at the southern Canary Island Seamount Province (CISP) in the northeastern tropical Atlantic were recovered along the flanks and summits from 1700 to 3000 m water depths. CISP is composed of > 100 seamounts and submarine hills, is likely the oldest hotspot track in the Atlantic Ocean, and is the most long-lived of known hotspots globally. The Fe-Mn crusts grow on basalt-sedimentary rock substrates below the northeastern tropical Atlantic core of the oxygen minimum zone (OMZ) with a maximum thickness of 250 mm at a water depth of 2400 m. The mineralogical and chemical composition of these Fe-Mn crusts indicate a hydrogenetic origin. The main Mn minerals are vernadite with minor interlayered todorokite and asbolane-buserite. Fe oxides are essentially ferroxyhyte and goethite. The Fe-Mn crusts show high average contents in Fe (23.5 wt%), Mn (16.1 wt%), and trace elements like Co (4700 μg/g), Ni (2800 μg/g), V (2400 μg/g) and Pb (1600 μg/g). Rare earth elements plus yttrium (REY) averages 2800 μg/g with high proportions of Ce (1600 μg/g). Total platinum group elements (PGEs) average 230 ng/g, with average Pt of 182 ng/g. Two main types of growth layers form the crusts: 1) a dense laminae of oxides with high contents in Mn, Co and Ni associated with vernadite and Cu, Ni, and Zn associated with todorokite; 2) botryoidal layers with high contents in Fe, Ti, V and REY associated with goethite. The Fe-Mn crusts from the CISP region show higher contents in Fe, V, Pb and REY but lower Mn, Co, Ni and PGEs contents than Pacific or Indian ocean seamount crusts. The oldest maximum age of initiation of crust growth was at 76 Ma (Campanian, Late Cretaceous). Using a combination of high resolution Co-chronometer and geochemical data along an Electron Probe Micro Analysis (EPMA) transect, four stages in morphology, chemical contents and growth rates can be differentiated in the the Cenozoic crusts since 28 Ma, which we interpret as due to changes in the ventilation of the North Atlantic OMZ and to the increase of Saharian dust inputs. An earliest growth period, characterized by similar contents of Fe and Mn in the interval 27.8–24.45 Ma (late Oligocene-early Miocene) reflects slow precipitation related to a thick OMZ. An intermediate laminated zone with higher contents of Fe, Si and P, high growth rates reaching 4.5 mm/Ma, and precipitation of Fe-Mn oxides during the interval 24.5–16 Ma is related to periods of ventilation of the OMZ by intrusion of deep upwelling currents. Significant increase in Fe contents at ca. 16 Ma correlates with the onset of incursions of Northern Component Waters into the North Atlantic. Finally, since 12 Ma, the very low growth rates (< 0.5 mm/Ma) of the crust are related to a thick North Atlantic OMZ, an increase in Sahara dust input and a stable thermohaline circulation.  相似文献   

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