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1.
《Applied Geochemistry》2006,21(8):1301-1321
Low-quality pore waters containing high concentrations of dissolved H+, SO4, and metals have been generated in the East Tailings Management Area at Lynn Lake, Manitoba, as a result of sulfide-mineral oxidation. To assess the abundance, distribution, and solid-phase associations of S, Fe, and trace metals, the tailings pore water was analyzed, and investigations of the geochemical and mineralogical characteristics of the tailings solids were completed. The results were used to delineate the mechanisms that control acid neutralization, metal release, and metal attenuation. Migration of the low-pH conditions through the vadose zone is limited by acid-neutralization reactions, resulting in the development of distinct pore-water pH zones at depth; the neutralization reactions involve carbonate (pH ⩾ 5.7), Al-hydroxide (pH ⩾ 4.0), and aluminosilicate solids. As the zone of low-pH pore water expands, the pH will then be primarily controlled by less soluble solids, such as Fe(III) oxyhydroxides (pH < 3.5) and the relatively more recalcitrant aluminosilicates (pH ⩾ 1.3). Precipitation/dissolution reactions involving secondary Fe(III) oxyhydroxides and hydroxysulfates control the concentrations of dissolved Fe(III). Concentrations of dissolved SO4 are principally controlled by the formation of gypsum and jarosite. Geochemical extractions indicate that the solid-phase concentrations of Ni, Co, and Zn are associated predominantly with reducible and acid-soluble fractions. The concentrations of dissolved trace metals are therefore primarily controlled by adsorption/complexation and (or) co-precipitation/dissolution reactions involving secondary Fe(III) oxyhydroxide and hydroxysulfate minerals. Concentrations of dissolved metals with relatively low mobility, such as Cu, are also controlled by the precipitation of discrete minerals. Because the major proportion of metals is sequestered through adsorption and (or) co-precipitation, the metals are susceptible to remobilization if low-pH or reducing conditions develop within the tailings. 相似文献
2.
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
3.
《Journal of Geochemical Exploration》2005,85(3):119-137
This study reports on the seepage of metals, metalloids and radionuclides from the Mary Kathleen uranium mill tailings repository. Since rehabilitation in the 1980s, the capped tailings have developed a stratified hydrochemistry, with acid (pH 3.7), saline, metal-rich (Fe, Mn, Ni, U ± As, Pb, Zn), oxygenated (1.05 mg L−1 DO), radioactive waters in the upper tailings pile and near-neutral pH (pH 7.57), metal-poor, reduced (0.08 mg L−1 DO) waters at depth. Seepage (∼0.5 L s−1) of acid (pH 5.5), metal-rich (Fe, Mn ± Ni, U, Zn), radioactive (U-235, U-238, Ra-226, Ra-228, Ac-227) waters occurs from the base of the tailings dam retaining wall into the former evaporation pond and local drainage system. Oxygenation of the seepage waters causes the precipitation of Fe and coprecipitation and adsorption of other metals (U, Y), metalloids (As), rare earth elements (Ce, La) and radionuclides (U-235, U-238). By contrast, alkalis and alkaline–earth elements (Ca, K, Mg, Na, Sr), Mn, sulfate and to some degree metals (U, Zn, Ni), rare earth elements (Ce, La) and radionuclides (U-235, U-238, Ra-226, Ra-228) remain in solution until pH neutralisation and evaporation lead to their precipitation in efflorescences and sulfate-rich evaporative sediments. While the release of contaminant loads from the waste repository through seepage is insignificant (e.g. ∼5 kg of U per year), surface waters downstream of the tailings impoundment possess TDS, U and SO4 concentrations that exceed Australian water quality guideline values in livestock drinking water. Thus, in areas with a semi-arid climate, even insignificant load releases of contaminants from capped tailings repositories can still cause the deterioration of water quality in ephemeral creek systems. 相似文献
4.
In the present study, we investigated As behavior in a high-As hot spring (Sambe hot spring, Shimane, Japan) by coupling direct chemical speciation by synchrotron-based XAFS and HPLC–ICP-MS with microbial As-redox transformation gene analysis. The concentration of soluble As in the spring streamwater decreased immediately along the flow in correlation with Fe behavior, indicating that As in the streamwater was naturally attenuated in the streamwater. Iron XAFS analysis suggested deposition of Fe(III) oxyhydroxides along the flow. Thus, considering the strong affinity of As to Fe oxyhydroxides, the observed attenuation in As was possibly caused by sorption (or incorporation) of As on Fe(III) oxyhydroxides. Both dissolved As(III) and As(V) were present in the aqueous phase, and As(III) was rapidly oxidized to As(V) (<30 s) along the flow. The oxidation kinetics indicated the occurrence of biotic As(III) oxidation, because obtained As(III) oxidation rate (6.7–7.8 μM min−1) was much faster than the reported abiotic oxidation rates. Furthermore, the bacterial arsenite oxidase gene (aioA) was detected in DNA extracted from all samples (average of 2.0 × 105 copies dry g−1), which also supported potential attributes of biological As(III) oxidation in situ. In solid phase samples from sampling points analyzed by XAFS, most of the As existed as oxidized pentavalent form, As(V). This result indicated that this form was preferentially partitioned to the solid phase because of the much higher affinity of As(V) than of As(III) to Fe(III) oxyhydroxides. Considering the kinetic and microbiological findings, it is indicated that biotic process was predominantly responsible for As(III) oxidation at the present site, and this biotic As(III) oxidation to As(V) controlled the observed attenuation of As, because oxidized As(V) was removed from the aqueous phase by Fe(III) oxyhydroxides more efficiently. 相似文献
5.
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
6.
The linkage between the iron and the carbon cycles is of paramount importance to understand and quantify the effect of increased CO2 concentrations in natural waters on the mobility of iron and associated trace elements. In this context, we have quantified the thermodynamic stability of mixed Fe(III) hydroxo-carbonate complexes and their effect on the solubility of Fe(III) oxihydroxides. We present the results of carefully performed solubility measurements of 2-line ferrihydrite in the slightly acidic to neutral–alkaline pH ranges (3.8–8.7) under constant pCO2 varying between (0.982–98.154 kPa) at 25 °C.The outcome of the work indicates the predominance of two Fe(III) hydroxo carbonate complexes FeOHCO3 and Fe(CO3)33−, with formation constants log*β°1,1,1 = 10.76 ± 0.38 and log β°1,0,3 = 24.24 ± 0.42, respectively.The solubility constant for the ferrihydrite used in this study was determined in acid conditions (pH: 1.8–3.2) in the absence of CO2 and at T = (25 ± 1) °C, as log*Ks,0 = 1.19 ± 0.41.The relative stability of the Fe(III)-carbonate complexes in alkaline pH conditions has implications for the solubility of Fe(III) in CO2-rich environments and the subsequent mobilisation of associated trace metals that will be explored in subsequent papers. 相似文献
7.
Toxic metal(loid) speciation during weathering of iron sulfide mine tailings under semi-arid climate
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
8.
《Chemical Geology》2007,236(3-4):217-227
The association of arsenate, As(V), and arsenite, As(III), with disordered mackinawite, FeS, was studied in sulfide-limited (Fe:S = 1:1) and excess-sulfide (Fe:S = 1:2) batch experiments. In the absence of arsenic, the sulfide-limited experiments produce disordered mackinawite while the excess-sulfide experiments yield pyrite with trace amounts of mackinawite. With increasing initially added As(V) concentrations the transformation of FeS to mackinawite and pyrite is retarded. At S:As = 1:1 and 2:1, elemental sulfur and green rust are the end products. As(V) oxidizes S(-II) in FeS and (or) in solution to S(0), and Fe(II) in the solid phase to Fe(III). Increasing initially added As(III) concentrations inhibit the transformation of FeS to mackinawite and pyrite and no oxidation products of FeS or sulfide, other than pyrite, were observed. At low arsenic concentrations, sorption onto the FeS surface may be the reaction controlling the uptake of arsenic into the solid phase. Inhibition of iron(II) sulfide transformations due to arsenic sorption suggests that the sorption sites are crucial not only as sorption sites, but also in iron(II) sulfide transformation mechanisms. 相似文献
9.
《Applied Geochemistry》2006,21(3):528-545
High mean As concentrations of up to 26.6 μmol/L (1990 μg/L) occur in ground water collected from a fractured-bedrock system composed of sulfidic schist with granitic to dioritic intrusions. Sulfides in the bedrock are the primary source of the As in the ground water, but the presence of arsenopyrite in rock core retrieved from a borehole with As concentrations in the ground water barely above the detection limit of 2.0 μmol/L, shows that there are complicating factors. Chemical analyses of water from 35 bedrock wells throughout a small watershed reveal spatial clustering of wells with high As concentrations. Stiff diagrams and box plots distinguish three distinct types; calcium-bicarbonate-dominated water with low As concentrations (CaHCO3 type), sodium-bicarbonate-dominated water with moderately high As concentrations (NaHCO3 type), and calcium-bicarbonate-dominated water with very high As concentrations (High-As type). It is proposed that differences in recharge area and ground-water evolution, and possible bedrock composition difference are responsible for the chemical distinctions within the watershed. Lack of correlation of As concentrations with pH indicates that desorption of As is an insignificant control on As concentration. Correlations of As concentrations with Fe and redox parameters indicates that reductive dissolution of Fe(III) oxyhydroxides may play a role in the occurrence of high As concentrations in the NaHCO3 and High-As type water. The oxidation of sulfide minerals occurs within the ground-water system and is ultimately responsible for the existence of As in the ground water, but there is no correlation between As and SO4 concentrations, probably due to precipitation of Fe(III) oxyhydroxides and adsorption of As under oxidizing conditions. 相似文献
10.
《Applied Geochemistry》2005,20(5):989-1016
Groundwater from the Quaternary loess aquifer of La Pampa, central Argentina, has significant problems with high concentrations of As (up to 5300 μg L−1) as well as other potentially toxic trace elements such as F, B, Mo, U, Se and V. Total As concentrations in 45 loess samples collected from the aquifer have a range of 3–18 mg kg−1 with a mean of 8 mg kg−1. These values are comparable to world-average sediment As concentrations. Five samples of rhyolitic ash from the area have As concentrations of 7–12 mg kg−1. Chemical analysis included loess sediments and extracted porewaters from two specially cored boreholes. Results reveal a large range of porewater As concentrations, being generally higher in the horizons with highest sediment As concentrations. The displaced porewaters have As concentrations ranging up to 7500 μg L−1 as well as exceptionally high concentrations of some other oxyanion species, including V up to 12 mg L−1. The highest concentrations are found in a borehole located in a topographic depression, which is a zone of likely groundwater discharge and enhanced residence time. Comparison of sediment and porewater data does not reveal unequivocally the sources of the As, but selective extract data (acid-ammonium oxalate and hydroxylamine hydrochloride) suggest that much of the As (and V) is associated with Fe oxides. Primary oxides such as magnetite and ilmenite may be partial sources but given the weathered nature of many of the sediments, secondary oxide minerals are probably more important. Extract compositions also suggest that Mn oxide may be an As source. The groundwaters of the region are oxidising, with dissolved O2, NO3 and SO4 normally present and As(V) usually the dominant dissolved As species. Under such conditions, the solubility of Fe and Mn oxides is low and As mobilisation is strongly controlled by sorption–desorption reactions. Desorption may be facilitated by the relatively high-pH conditions of the groundwaters in the region (7.0–8.8) and high concentrations of potential competitors (e.g. V, P, HCO3). PHREEQC modelling suggests that the presence of V at the concentrations observed in the Pampean porewaters can suppress the sorption of As to hydrous Fe(III) oxide (HFO) by up to an order of magnitude. Bicarbonate had a comparatively small competitive effect. Oxalate extract concentrations have been used to provide an upper estimate of the amount of labile As in the sediments. A near-linear correlation between oxalate-extractable and porewater As in one of the cored boreholes investigated has been used to estimate an approximate Kd value for the sediments of 0.94 L kg−1. This low value indicates that the sediments have an unusually low affinity for As. 相似文献
11.
《Applied Geochemistry》2006,21(7):1240-1247
This paper reports the abundance of elemental S in drain sediments associated with acid sulfate soils. The sediments exhibited near-neutral pH (5.97–7.27), high concentrations of pore-water Fe2+ (1.37–15.9 mM) and abundant oxalate-extractable Fe (up to 4300 μmol g−1). Maximum acid-volatile sulfide (AVS) concentrations in each sediment profile were high (118–1019 μmol g−1), with AVS often exceeding pyrite-S. Elemental S occurred at concentrations of 13–396 μmol g−1, with the higher concentrations exceeding previous concentrations reported for other sedimentary systems. Up to 62% of reduced inorganic S near the sediment/water interface was present as elemental S, due to reaction between AVS and oxidants such as O2 and Fe(III). Significant correlation (r = 0.74; P < 0.05) between elemental S and oxalate-extractable Fe(III) is indicative of elemental S formation by in situ oxidation of AVS. The results indicate that AVS oxidation in near-surface sediments is dynamic in acidified coastal floodplain drains, causing elemental S to be a quantitatively important intermediate S fraction. Transformations of elemental S may therefore strongly influence water quality in ASS landscapes. 相似文献
12.
The solubility controls on vanadium (V) in groundwater were studied due to concerns over possible harmful health effects of ingesting V in drinking water. Vanadium concentrations in the northeastern San Joaquin Valley ranged from <3 μg/L to 70 μg/L with a median of 21 μg/L. Concentrations of V were highest in samples collected from oxic groundwater (49% > 25 μg/L) and lowest in samples collected from anoxic groundwater (70% < 0.8 μg/L). In oxic groundwater, speciation modeling (SM) using PHREEQC predicted that V exists primarily as the oxyanion H2VO4−. Adsorption/desorption reactions with mineral surfaces and associated oxide coatings were indicated as the primary solubility control of V5+ oxyanions in groundwater. Environmental data showed that V concentrations in oxic groundwater generally increased with increasing groundwater pH. However, data from adsorption isotherm experiments indicated that small variations in pH (7.4–8.2) were not likely as an important a factor as the inherent adsorption capacity of oxide assemblages coating the surface of mineral grains. In suboxic groundwater, accurate SM modeling was difficult since Eh measurements of source water were not measured in this study. Vanadium concentrations in suboxic groundwater decreased with increasing pH indicating that V may exist as an oxycationic species [e.g. V(OH)3+]. Vanadium may complex with dissolved inorganic and organic ligands under suboxic conditions, which could alter the adsorption behavior of V in groundwater. Speciation modeling did not predict the existence of V-inorganic ligand complexes and organic ligands were not collected as part of this study. More work is needed to determine processes governing V solubility under suboxic groundwater conditions. Under anoxic groundwater conditions, SM predicts that aqueous V exists as the uncharged V(OH)3 molecule. However, exceedingly low V concentrations show that V is sparingly soluble in anoxic conditions. Results indicated that V may be precipitating as V3+- or mixed V3+/Fe3+-oxides in anoxic groundwater, which is consistent with results of a previous study. The fact that V appears insoluble in anoxic (Fe reducing) redox conditions indicates that the behavior of V is different than arsenic (As) in aquifer systems where the reductive dissolution of Fe-oxides with As adsorbed to the surface is a well-documented mechanism for increasing As concentrations in groundwater. This hypothesis is supported by the relation of V to As concentrations in oxic versus anoxic redox conditions.Sequential extraction procedures (SEP) applied to aquifer material showed that the greatest amount of V was recovered by the nitric acid (HNO3) extract (37–71%), followed by the oxalate-ascorbic acid extract (19–60%) and the oxalate extract (3–14%). These results indicate that V was not associated with the solid phase as an easily exchangeable fraction. Although the total amount of V recovered was greatest for the HNO3 extract that targets V adsorbed to sorption sites of crystalline Al, Fe and Mn oxides, the greatest V saturation of sorption sites appeared to occur on the amorphous and poorly crystalline oxide solid phases targeted by the oxalate and oxalate-ascorbic acid extracts respectively. Adsorption isotherm experiments showed no correlation between V sorption and any of the fractions identified by the SEP. This lack of correlation indicates the application of an SEP alone is not adequate to estimate the sorption characteristics of V in an aquifer system. 相似文献
13.
《Applied Geochemistry》2005,20(4):789-805
Mineralogical, hydrochemical and S isotope data were used to constrain hydrogeochemical processes that produce acid mine drainage from sulfidic waste at the historic Mount Morgan Au–Cu mine, and the factors controlling the concentration of SO4 and environmentally hazardous metals in the nearby Dee River in Queensland, Australia. Some highly contaminated acid waters, with metal contents up to hundreds of orders of magnitude greater than the Australia–New Zealand environmental standards, by-pass the water management system at the site and drain into the adjacent Dee River.Mine drainage precipitates at Mt. Morgan were classified into 4 major groups and were identified as hydrous sulfates and hydroxides of Fe and Al with various contents of other metals. These minerals contain adsorbed or mineralogically bound metals that are released into the water system after rainfall events. Sulfate in open pit water and collection sumps generally has a narrow range of S isotope compositions (δ34S = 1.8–3.7‰) that is comparable to the orebody sulfides and makes S isotopes useful for tracing SO4 back to its source. The higher δ34S values for No. 2 Mill Diesel sump may be attributed to a difference in the source. Dissolved SO4 in the river above the mine influence and 20 km downstream show distinctive heavier isotope compositions (δ34S = 5.4–6.8‰). The Dee River downstream of the mine is enriched in 34S (δ34S = 2.8–5.4‰) compared with mine drainage possibly as a result of bacterial SO4 reduction in the weir pools, and in the water bodies within the river channel. The SO4 and metals attenuate downstream by a combination of dilution with the receiving waters, SO4 reduction, and the precipitation of Fe and Al sulfates and hydroxides. It is suggested here that in subtropical Queensland, with distinct wet and dry seasons, temporary reducing environments in the river play an important role in S isotope systematics. 相似文献
14.
《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
15.
《Applied Geochemistry》1998,13(6):687-705
The results of an integrated geochemical and mineralogical study conducted at the Agnico-Eagle gold-mine tailings impoundment, Joutel, Québec, are correlated with bacterial populations determined from an enumeration of 3 groups of Thiobacilli. The tailings were determined to contain approximately 5 wt.% sulphide–S, predominantly as pyrite, and up to 30 wt.% carbonate minerals, chiefly as dolomite–ankerite and siderite. The objective of the study was to evaluate the potential for the development of acidic drainage and dissolved-metal migration in carbonate-rich tailings impoundments, and to compare the results of the geochemical and microbiological characterization of the tailings. Sulphide-oxidation reactions have proceeded to a depth of 20–100 cm below the tailings surface. Pyrrhotite consistently shows more alteration than pyrite and arsenopyrite. Pyrrhotite is altered mainly through the replacement by goethite. The most abundant Thiobacilli are neutrophilic bacteria of the Thiobacillus thioparus type. The maximum most probable number values for these bacteria occur 20–40 cm below the tailings surface, a depth that coincides with the disappearance of oxide coatings. This observation, coupled with the sharp decline in gas-phase O2 concentration, suggests that rapid bacterially-mediated S–oxidation is occurring at this depth. The pore-water pH throughout the tailings varies between 6.5 and 8.5; no low-pH waters were observed in the impoundment. These neutral pH conditions are attributed to the effect of acid-consuming carbonate-mineral dissolution reactions, which are also indicated by increased concentrations of Mg and Ca and alkalinity in the shallow zone of the tailings. As a result of these acid-neutralization reactions, dissolved metal concentrations are low. 相似文献
16.
The Baogutu gold deposit, West Junggar (Xinjiang, NW China), is composed of quartz–sulfide veins and their stockworks and is hosted within an Early Carboniferous volcanic–sedimentary sequence. Three ore-forming paragenetic stages can be identified: coarse-grained quartz–sulfide vein (stage I), gold-bearing fine-grained quartz–sulfide vein (stage II), and native antimony-bearing calcite–sulfide veinlets (stage III). The estimated formation temperatures (approximately 360 to 220 °C), fS2 (? 7 to ? 15 log units), and fO2 (? 26 to ? 43 log units) decrease from stage I, through stage II, to stage III. The nature of the hydrothermal fluid changed from weakly acidic (pH: 5 to 6 at stage I) to alkaline (pH: > 7 at stage III).Two different occurrences of native antimony could be identified: one coexists with chalcopyrite and pyrrhotite, whereas the other occurs as isolate grains within calcite veins. Native antimony (up to 100 μm in size) contains minor amounts of As (2.0 to 2.7 wt.%); empirical formula Sb0.95–0.96As0.03–0.04. Decrease of temperature and fO2 at high pH and low fS2 conditions favored co-precipitation of native antimony–ullmannite assemblages and the decomposition of tetrahedrite. Native antimony crystallized later than the native gold, suggesting fractionation between Au and Sb during the hydrothermal evolution of the deposit. 相似文献
17.
This study investigated the efficiency of a constructed wetland/filter basin (CW/FB) treatment system to improve the chemical composition of waste and surface waters. The system was constructed in closed phosphate mines used for clay settling and sand tailings. Monitoring was carried out for 18 months to evaluate the CW/FB performance under a variety of climatic conditions. Water samples were taken bi-monthly. To evaluate possible groundwater input into and water leaking out of the wetland 6 monitor wells were installed along the flow path and sampled monthly. In order to estimate the change of water chemistry along the wetland flow path, water samples along a transect were taken during the dry and rainy seasons. The samples were analyzed for pH, T, oxidation–reduction potential (ORP), conductivity, total dissolved solids (TDS), dissolved oxygen (DO), Fe(II), H2S, major anions, major cations, arsenic, fecal and total coliform.The study showed the following changes in water quality between the input and output: (1) Substantial decrease of water temperature (up to 10 °C); (2) Significant change in pH from about 9 to 6.5–7; (3) Negative ORP confirming the reducing conditions of the treatment system; (4) Substantial increase of H2S (up to 1060 µg/L); (5) Reduction of As from 5 to <2 µg/L (mostly <0.5); (6) Substantial reduction of SO4, F, Cl, NO3, NO2, Br, Na, K, Ca, and Mg; (7) Reduction of fecal and total coliform from 30–730 and 1000–7000 to <2 and <100 count/100 mL, respectively. In general, the performance of the CW/FB treatment system showed great potential to improve the water quality of industrial and municipal wastewater. Despite significant seasonal variations with respect to temperature, rainfall and humidity, the chemical/microbiological composition of the wetland output remained relatively constant. 相似文献
18.
Cu-Fe-sulphide mineral assemblages from the Olympic Dam (OD) Fe-oxide Cu-U-Au-Ag deposit, South Australia, are studied down to the nanoscale to explore the potential these minerals have for understanding genetic processes such as primary deposit zonation. Cu-Fe-sulphide pairs: ‘brown’ bornite associated with chalcopyrite (bornite-chalcopyrite zone); and symplectites of ‘purple’ bornite with species from the chalcocite group, Cu2 − xS (bornite-chalcocite zone), co-define an upwards and inwards deposit-scale zonation at OD. In the bornite-chalcocite zone, there is also an increase in the proportion of chalcocite relative to bornite within the symplectites towards upper levels. In this case, two-phase Cu2 − xS assemblages are also present, as anisotropic, hexagonal chalcocite (CcH) with lamellar exsolutions of digenite, distinguishable at the μm-scale. Using compositional data (electron microprobe) combined with Transmission Electron Microscopy (TEM) study of foils prepared in–situ via Focused Ion Beam (FIB)-SEM, we show that Cu-Fe-sulphides from different ore zones feature nanoscale intergrowths, lattice defects, superstructure domains (na) and antiphase boundary domains (APBs) that can be interpreted as due to exsolution, coarsening and phase transformation during cooling from high-T solid solutions in the system Cu-Fe-S and sub-systems according to published phase diagrams. ‘Brown’ bornite [(Cu + Fe)/S > 5] contains pervasive lamellae of chalcopyrite which extend down to the nanoscale; such specimens appear homogeneous at the μm-scale. ‘Purple bornite’ [(Cu + Fe)/S < 5] in high-bornite symplectites is associated with chalcocite that shows APBs with 6a digenite and low-T chalcocite. Comparable APBs are also found in the ‘chalcocite’ zone with apparent homogeneity at the μm-scale. Both bornites contain exsolutions of djurleite. Systematic variation of Me/S and Cu/Fe in the two types of bornite points, however, to distinct origins from different bornite solid-solutions in the system Cu-Fe-S. Both show 2a and 4a intermediate superstructures. High-order superstructures (6a and incommensurate na) are restricted to the ‘purple’ bornite whereas the 2a4a low-T superstructure is found in both cases. Me/S ratios in the chalcocite group are variable; lower ratios (down to 1.8; digenite) are more common in chalcocite from symplectites with ‘purple’ bornite. Me/S can be as low as 1.4 where associated with ‘blue’ varieties (‘blaubleibender covellin’) of replacement origin. The two-phase Cu2 − xS associations contain hexagonal chalcocite (Me/S = 1.95), lamellae of Cu-rich digenite (Me/S = 1.92), and anilite (Cu7S4) as nm-scale lamellae. Digenite shows 3a and 6a superstructures and CcH shows transition to pseudo-orthorhombic chalcocite. The presence of superstructures, high-T species and APBs is evidence for Cu-(Fe)-sulphide formation from high-T solid solutions at T > 300 °C (high-T phases, Cu-poor digenite), followed by cooling along distinct paths down to < 120 °C (APBs). The scenario of ‘exsolution from primary solid-solution’, corroborated by the consistency in phase relations within each zone across different scales of observation from deposit scale to nanoscale, backs up a model of primary hypogene ore precipitation rather than replacement, and accounts for the observed vertical zoning at OD. The FIB-TEM approach here is readily applicable to other deposits and shows that nanoscale observations are a valuable, although often overlooked, source of information to constrain ore genesis. 相似文献
19.
T. Allard T. Weber C. Bellot C. Damblans M. Bardy G. Bueno N.R. Nascimento E. Fritsch M.F. Benedetti 《Chemical Geology》2011,280(1-2):79-88
Suspended solids found in porewaters obtained in waterlogged soil sequences that included representative laterite–podzol transitions, associated brooks and major rivers of the Rio Negro watershed (Brazil) were studied using electron paramagnetic resonance (EPR) and Fourier-transform infrared spectroscopies. The main goal was to ascertain sources and track the evolution of suspended matter using a ubiquitous chemical species, FeIII complexed to organic matter (FeOM). Three size fractions were separated by tangential-flow (ultra)filtration: particulate (> 0.2 μm), dense (P) and light (Ps), and colloidal (5 kD < Col. < 0.2 μm) fractions. Quantitative results were acquired for Col. and Ps fractions which are predominantly organic in nature.FeOM concentration (in ‰ dry weight) was determined to be relatively low in suspended solids found in black waters from podzol porewaters and brooks whereas in the main rivers it was several times higher. FeOM concentrations were also correlated with Fe(II)/Fe(III) ratios in solution; these ratios were high in podzol porewaters and low in the rivers. Considering that organic complexation of Fe(II) is minor when compared to that of Fe(III), two interpretations were proposed to account for the above observation. First, [FeOM] was assumed to be distributed along a mixing line, with the clear waters from laterites and the black waters from podzols being its end-members. Consequently, [FeOM] can be used to trace the source of suspended material. Second, dissolved Fe(II) from podzol areas was considered to be progressively oxidized as pore waters move towards the mainstream. According to this mechanism, iron is complexed by organic matter or precipitated as oxides, thus producing an evolution of colloidal matter. As a result of these mechanisms' action, both the high production of Fe(II) and organic matter at the waterlogged podzol–laterite transition areas are major factors affecting iron export in the Rio Negro watershed. 相似文献
20.
《Applied Geochemistry》2006,21(6):949-963
In the central part of the Pannonian Basin, factors controlling the distribution of As in sediments and groundwater of the upper 500 m were studied. In core samples, the amounts of As, Fe and Mn extractable with hydroxylamine hydrochloride (NH2OH · HCl) in 25% acetic acid, the proportion of the <0.063 mm size fraction, and the sediment organic C (Corg) contents were measured. In the groundwaters concentrations of As, humic substances, and selected major chemical components were determined. In most core samples extractable Fe, as FeOOH, and Corg are correlated, but some samples have excess Fe, or organic matter. In cases where either excess Fe or excess organic matter is found, the amount of As is also elevated. The spatial distribution of As in the groundwater and the lack of a consistent correlation of As with a single component indicate that there is no single factor controlling the concentration of dissolved As over the entire study area. The only consistent feature is enrichment of As relative to Fe in the groundwater, compared to the sediments. This suggests that the dissolution of Fe minerals, which primarily adsorb As, is not congruent. In reducing conditions Fe(III) oxyhydroxides together with adsorbed As dissolve, and siderite with little or no As precipitates. When sub-regions are separated and studied individually, it can be shown that hydrogeological features of the sediments, the proportions of Fe minerals and sedimentary organic matter, and the concentration of dissolved humic materials, all influence the accumulation and mobilization of As. The significance of the different mobilizing processes, however, and the mean concentration of As, is different in the recharge, through-flow and discharge areas. 相似文献