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1.
Metals released from oxidation and weathering of sulphide minerals in mine tailings are to a high degree retained at deeper levels within the tailings themselves. To be able to predict what could happen in the future with these secondarily retained metals, it is important to understand the retention mechanisms. In this study an attempt to use laser ablation high-resolution ICP-MS (LA-ICP-SMS) to quantify enrichment of trace elements on pyrite surfaces in mine tailings was performed. Pyrite grains were collected from a profile through the pyrite-rich tailings at the Kristineberg mine in northern Sweden. At each spot hit by the laser, the surface layer was analyzed in the first shot, and a second shot on the same spot gave the chemical composition of the pyrite immediately below. The crater diameter for a laser shot was known, and by estimating the crater depth and total pyrite surface, the total enrichment on pyrite grains was calculated. Results are presented for As, Cd, Co, Cu, Ni and Zn. The results clearly show that there was an enrichment of As, Cd, Cu and Zn on the pyrite surfaces below the oxidation front in the tailings, but not of Co and Ni. Arsenic was also enriched on the pyrite grains that survived in the oxidized zone. Copper has been enriched on pyrite surfaces in unoxidized tailings in the largest amount, followed by Zn and As. However, only 1.4 to 3.1% of the Cd and Zn released by sulphide oxidation in the oxidized zone have been enriched on the pyrite surfaces in the unoxidized tailings, but for As and Cu corresponding figures are about 64 and 43%, respectively. There were many uncertainties in these calculations, and the results shall not be taken too literally but allowed the conclusion that enrichment on pyrite surfaces is an important process for retention of As and Cu below the oxidation front in pyrite rich tailings. Laser ablation is not a surface analysis technique, but more of a thin layer method, and gives no information on the type of processes resulting in enrichment on the pyrite surfaces. Although only pyrite grains that appeared to be fresh and without surface coatings were used in this study, the possibility that a thin layer of Fe-hydroxides occurred must be considered. Both adsorption to the pyrite directly or to Fe-oxyhydroxides may explain the enrichment of As, Cd, Cu and Zn on the pyrite surfaces, and, in the case of Cu, also the replacement of Fe(II) by Cu(II) in pyrite.  相似文献   

2.
Redistribution of potentially harmful metals and As was studied based on selective extractions in two active sulphide mine tailings impoundments in Finland. The Hitura tailings area contains residue from Ni ore processing, while the Luikonlahti site includes tailings from the processing of Cu–Co–Zn–Ni and talc ores. To characterize the element solid-phase speciation with respect to sulphide oxidation intensity and the water saturation level of the tailings, drill cores were collected from border zones and mid-impoundment locations. The mobility and solid-phase fractionation of Ni, Cu, Co, Zn, Cr, Fe, Ca, Al, As, and S were analysed using a 5-step non-sequential (parallel) selective extraction procedure. The results indicated that metal redistribution and sulphide oxidation intensity were largely controlled by the disposal history and strategy of the tailings (sorting, exposure of sulphides due to delayed burial), impoundment structure and water table, and reactivity of the tailings. Metal redistribution suggested sulphide weathering in the tailings surface, but also in unsaturated proximal areas beside the earthen dams, and in water-saturated bottom layers, where O2-rich infiltration is possible. Sulphide oxidation released trace metals from sulphide minerals at both locations. In the Hitura tailings, with sufficient buffering capacity, pH remained neutral and the mobilized metals were retained by secondary Fe precipitates deeper in the oxidized zone. In contrast, sulphide oxidation-induced acidity and rise in the water table after oxidation apparently remobilized the previously retained metals in Luikonlahti. In general, continuous disposal of tailings decreased the sulphide oxidation intensity in active tailings, unless there was a delay in burial and the reactive tailings were unsaturated after deposition.  相似文献   

3.
Weathering of Hitura (W Finland) nickel sulphide mine tailings and release of heavy metals into pore water was studied with mineralogical (optical and electron microscopy, X-ray diffraction) and geochemical methods (selective extractions). Tailings were composed largely of serpentine, micas and amphiboles with only minor carbonates and sulphides. Sulphides, especially pyrrhotite, have oxidized intensively in the shallow tailings in 10–15 years, but a majority of the tailings have remained unchanged. Oxidation has resulted in depletion of carbonates, slightly decreased pH, and heavy metal (Ni, Zn) release in pore water as well as in the precipitation of secondary Fe precipitates. Nevertheless, in the middle of the tailings area, where the oxidation front moves primarily downward, released heavy metals have been adsorbed and immobilized with these precipitates deeper in the oxidation zone. In contrast to what was seen in pore water pH, but in accordance with static tests of the previous studies, the neutralisation potential ratio (NPR) calculated based on the mineralogical composition and the total sulphur content suggested that tailings are ‘not potentially acid mine drainage (AMD) generating’. However, the calculated buffering capacity of the tailings resulted largely from the abundant serpentine because of the low carbonate content. Despite its slow weathering rate, serpentine may buffer the acidity to some extent through ion exchange processes in fine ground tailings. Nevertheless, in practice, acid production capacity of the tailings depends primarily on the balance between Ca–Mg carbonates and iron sulphides. NPR calculation based on carbonate and sulphur contents suggested, that the Hitura tailings are ‘likely AMD generating’. The study shows that sulphide oxidation can be significant in mobilisation of heavy metals even in apparently non-acid producing, low sulphide tailings. Therefore, prevention of oxygen diffusion into tailings is also essential in this type of sulphide tailings.  相似文献   

4.
《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   

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 distribution of arsenic (As(III), As(V)) and iron (Fe(II), Fe(III)) species was monitored during 1 year in a borehole drilled in the Carnoulès tailings impoundment which contains As-rich pyrite. The concentrations of total As and Fe in subsurface waters exhibited strong variations over one year, which were controlled by dissolved oxygen concentrations. At high oxygen levels, extremely high As (up to 162 mM) and Fe (up to 364 mM) concentrations were reached in the borehole, with the oxidised species predominant. As and Fe concentrations decreased 10-fold under oxygen-deficient conditions, as a result of pH increase and subsequent precipitation of As(V) and Fe(III). From drill core sections, it appeared that at low dissolved oxygen levels, As(III) was primarily released into water by the oxidation of As-rich pyrite in the unsaturated zone. Subsequent As and Fe precipitation was promoted during transport to the saturated zone; this reaction resulted in As enrichments in the sediment below the water table compared to the original content in pyrite, together with the formation of As-rich (up to 35 wt% As) ferruginous material in the unsaturated zone. High amounts of As(V) were released from these secondary phases during leaching experiments with oxygenated acid sulfate-rich waters; this process is believed to contribute to As(V) enrichment in the subsurface waters of the Carnoulès tailings during periods of high dissolved oxygen level.  相似文献   

7.
In the old mining area of Rodalquilar, mine wastes, soil and sediments were characterized and the results revealed high concentration of Au, Ag, As, Bi, Cu, Fe, Mn, Pb, Se, Sb and Zn in tailings and sediments. The contaminant of greatest environmental concern is As. The mean concentration in the tailings was 679.9, and 345 mg/kg in the sediments of Playazo creek. The groundwater samples from the alluvial aquifer showed high concentration of Al, As, Cd, Fe, Hg, Mn, Ni, Pb, Se, Sb and Zn and very high concentration of chloride and sulfate, which were above the concentration defined in the European standards for drinking water. The presence of As in groundwater may be caused by the oxidation of arsenian pyrite, the possible As desorption from goethite and ferrihydrite and the jarosite dissolution. Groundwater concentrations of Cd, Fe, Mn, and possibly Cu, were associated with low values of Eh, indicating the possible dissolution of oxy-hydroxides of Fe and Mn. The mobility of metals in the column experiments show the release of Al, Fe, Mn, Cr, Cu, Ni, V and Zn in significant concentrations but below the detected values in groundwater. However, As, Cd, Sb, Se Pb and Au, are generally mobilized in concentrations above the detected values in groundwater. The possible mass transfer processes that could explain the presence of the contaminants in the aquifer and the leachates was simulated with the PHREEQC numerical code and revealed the possible dissolution of the following mineral phases: jarosite, natrojarosite, arsenian pyrite, alunite, chlorite, kaolinite and calcite.  相似文献   

8.
《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   

9.
The Haveri tailings area contains 1.5 Mt of sulfide-bearing waste from the Au–Cu mine that operated during 1942–1961. Geophysical and geochemical methods were used to evaluate and characterize the generation of acid mine drainage (AMD). Correlations were examined among the electrical resistivity tomography (ERT) data, the total sulfide content and concentrations of sulfide-bound metals (Cu, Co, Fe, Mn, Ni, Pb and Zn) of tailings samples, and the resistivity and geochemistry of surface water. The resulting geophysical–geochemical model defines an area in the vadose tailings, where a low resistivity anomaly (<10 Ohm m) is correlated with the highest sulfide content, extensive sulfide oxidation and low pH (average 3.1). The physical and geochemical conditions, resulting from the oxidation of the sulfide minerals, suggest that the low resistivity anomaly is associated with acidic and metal-rich porewater (i.e., AMD). The lower resistivity values in the saturated zone of the central impoundment suggest the formation of a plume of AMD. The natural subsoil layer (silt and clay) and the bedrock surface below the tailings area were well mapped from the ERT data. The detected fracture zones of the bedrock that could work as leakage pathways for AMD were consistent with previous geological studies. The integrated methodology of the study offers a promising approach to fast and reliable monitoring of areas of potential AMD generation and its subsurface movement over large areas (ca. 9 ha). This methodology could be helpful in planning drill core sampling locations for geochemical and mineralogical analysis, groundwater sampling, and choosing and monitoring remedial programs.  相似文献   

10.
This study evaluates the pollution load on a creek based on the physicochemical and mineralogical properties of old tailings. The Sanggok mine is one of the largest lead–zinc producers in the Hwanggangri mining district, Republic of Korea. The vertical profile of the old tailings in the mine area can be divided into three units based on color change, and mineralogical and textural variations, as well as physical and chemical properties. Unit I (surface accumulation and oxidized heterogeneous tailing soil) has lower pH and higher Eh than unit II (originally unoxidized dumped tailing soil) and unit III (pebble-bearing bottom soil). The conductivity data indicates that unit I and II have very high values compared to unit III and basement. The mine area consists mainly of carbonate rocks; however, mineral constituents of tailing soil and sediments near the mine were mainly composed of quartz, mica, feldspar, amphibole, calcite, dolomite, magnesite, and clay minerals. Units I and II are characterized by high abundances of siderite, locally pyrite, and dolomite. Precipitates in the mining drainage mainly included: smectite, illite, berthierine, quartz, siderite, hexahydrite, and Ca-ferrate. Among the separated metallic minerals, tailing soils and sediments of highly concentrated toxic metals are found: some pyrite, arsenopyrite, chalcopyrite, sphalerite, galena, malachite, goethite, various hydroxide, and uncertain secondary minerals. Units I and II are characterized by relatively high concentrations of Ca, Fe, Mn and low contents of Al, Mg, K, Na, Ti, rare earth elements (REEs) that correlated with the proportion of secondary minerals. Potentially toxic elements such as Ag, As, Cd, Cu, Pb, Sb, and Zn are highly enriched in the upper two units. This metal concentration can be influenced by changes in the depth because of oxic and suboxic zonal distribution. The removal zone (unit I) has probably migrated below the elevation of the maximum enrichment layer due to deepening of the oxic/suboxic boundary. In most of the materials, the enrichment index is higher than 3.62. The highest value of 42.55 is found in the oxidation surface soils of the tailing pile. An average enrichment index of the profiles and precipitates are 27.62 and 22.62, respectively. Rocky basement soils have an average enrichment index of 6.63, which is influenced by overlying the tailing pile. The water quality and habitat of the Sanggok creek are severely polluted. Polluted surface water may also negatively impact the agricultural soil and groundwater.  相似文献   

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