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1.
Tailings generated during processing of sulfide ores represent a substantial risk to water resources. The oxidation of sulfide minerals within tailings deposits can generate low-quality water containing elevated concentrations of SO4, Fe, and associated metal(loid)s. Acid generated during the oxidation of pyrite [FeS2], pyrrhotite [Fe(1−x)S] and other sulfide minerals is neutralized to varying degrees by the dissolution of carbonate, (oxy)hydroxide, and silicate minerals. The extent of acid neutralization and, therefore, pore-water pH is a principal control on the mobility of sulfide-oxidation products within tailings deposits. Metals including Fe(III), Cu, Zn, and Ni often occur at high concentrations and exhibit greater mobility at low pH characteristic of acid mine drainage (AMD). In contrast, (hydr)oxyanion-forming elements including As, Sb, Se, and Mo commonly exhibit greater mobility at circumneutral pH associated with neutral mine drainage (NMD). These differences in mobility largely result from the pH-dependence of mineral precipitation–dissolution and sorption–desorption reactions. Cemented layers of secondary (oxy)hydroxide and (hydroxy)sulfate minerals, referred to as hardpans, may promote attenuation of sulfide-mineral oxidation products within and below the oxidation zone. Hardpans may also limit oxygen ingress and pore-water migration within sulfide tailings deposits. Reduction–oxidation (redox) processes are another important control on metal(loid) mobility within sulfide tailings deposits. Reductive dissolution or transformation of secondary (oxy)hydroxide phases can enhance Fe, Mn, and As mobility within sulfide tailings. Production of H2S via microbial sulfate reduction may promote attenuation of sulfide-oxidation products, including Fe, Zn, Ni, and Tl, via metal-sulfide precipitation. Understanding the dynamics of these interrelated geochemical and mineralogical processes is critical for anticipating and managing water quality associated with sulfide mine tailings.  相似文献   

2.
The evolution of pore-water and the composition of solid phases in the vadose zone of pyritic tailings was studied by means of unsaturated column experiments. Several columns of water-saturated mine tailings were dried during 125 days under controlled laboratory conditions. The columns were dismantled at four successive drying stages and the evolution of pore-water, mineralogy, water content and temperature was characterized.Sulfide and aluminosilicate minerals present in the waste dissolved, releasing sulfate and other solutes (mainly Fe, Zn, Cu, Al, Mg and Ca) to the pore-water. Evaporation caused a crust of efflorescent, water-soluble sulfates to develop over the complete top surface of the columns and into the pores of the underlying waste material. This crust, which has also been identified in the field, changed the hydraulic properties of the tailings and produced a decrease in the evaporation rate of the columns. Moreover, these water-soluble precipitates (mainly rozenite, szomolnokite, halotrichite, hexahydrite, mirabilite and gypsum) acted as temporary sinks for Cd, Pb, Co and Ni, which could be released to the surface run-off or the groundwaters during rainfall events under field conditions.Pore-water evolution was determined not only by geochemical processes (dissolution of sulfides and aluminosilicates, precipitation of secondary phases) but also by thermal and hydraulic processes. Progressive dilution was observed in the lower part of the columns. Dilution was caused by the thermally driven vapor flux from the top of the column to its colder bottom and subsequent condensation therein. This process, which may also occur in tailings under sub-arid climate, played a key role on the evolution of pore-water with increasing drying.  相似文献   

3.
《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   

4.
 The oxidation and the subsequent dissolution of sulfide minerals within the Copper Cliff tailings area have led to the release of heavy metals such as Fe, Ni, and Co to the tailings pore water. Dissolved concentrations in excess of 10 g/l Fe and 2.2 g/l Ni have been detected within the shallow pore water of the tailings, with increasing depth these concentrations decrease to or near analytical detection limits. Geochemical modelling of the pore-water chemistry suggests that pH-buffering reactions are occurring within the shallow oxidized zones, and that secondary phases are precipitating at or near the underlying hardpan and transition zones. Mineralogical study of the tailings confirmed the presence of goethite, jarosite, gypsum, native sulfur, and a vermiculite-type clay mineral. Goethite, jarosite, and native sulfur form alteration rims and pseudo-morphs of the sulfide minerals. Interstitial cements, composed of goethite, jarosite, and gypsum, locally bind the tailings particles, forming hardpan layers. Microprobe analyses of the goethite indicate that it contains up to 0.6 weight % Ni, suggesting that the goethite is a repository for Ni. Other sinks detected for heavy metals include jarosite and a vemiculite-type clay mineral which locally contains up to 1.6 weight % Ni. To estimate the mass and distribution of heavy metals associated with the secondary phases within the shallow tailings, a series of chemical extractions was completed. The experimental design permitted four fractions of the tailings to be evaluated independently. These four fractions consisted of a water-soluble, an acid-leachable, and a reducible fraction, as well as the whole-rock total. Twenty-five percent of the total mass of heavy metals was removed in the acid-leaching experiments, and 100% of the same components were removed in the reduction experiments. The data suggest that precipitation/coprecipitation reactions are providing an effective sink for most of the heavy metals released by sulfide mineral oxidation. In light of these results, potential decommissioning strategies should be evaluated with the recognition that changing the geochemical conditions may alter the stability of the secondary phases within the shallow tailings. Received: 9 April 1997 · Accepted: 21 July 1997  相似文献   

5.
Mining and milling of base metal ore deposits can result in the release of metals to the environment. When sulfide minerals contained in mine tailings are exposed to oxygen and water, they oxidize and dissolve. Two principal antagonistic geochemical processes affect the migration of dissolved metals in tailings impoundments: sulfide oxidation and acid neutralization. This study focuses on acid neutralization reactions occurring in the saturated zone of tailings impoundments. To simulate conditions prevailing in many tailings impoundments, 0.1 mol/L sulfuric acid was passed continuously through columns containing fresh, unoxidized tailings, collected at Kidd Creek metallurgical site. The results of this column experiment represent a detailed temporal observation of pH, Eh, and metal concentrations. The results are consistent with previous field observations, which suggest that a series of mineral dissolution-precipitation reactions control pH and metal mobility. Typically, the series consists of carbonate minerals, Al and Fe(III) hydroxides, and aluminosilicates. In the case of Kidd Creek tailings, the dissolution series consists of ankerite-dolomite, siderite, gibbsite, and aluminosilicates. In the column experiment, three distinct pH plateaus were observed: 5.7, 4.0, and 1.3. The releases of trace elements such as Cd, Co, Cr, Cu, Li, Ni, Pb, V, and Zn were observed to be related to the pH buffering zones. High concentrations of Zn, Ni, and Co were observed at the first pH plateau (pH 5.7), whereas Cd, Cr, Pb, As, V, and Al were released as the pH of the pore water decreased to 4.0 or less.  相似文献   

6.
The chemistry of pore water is an important property of clayrocks being considered as host rocks for long-term storage of radioactive waste. It may be difficult, if not impossible, to obtain water samples for chemical analysis from such rocks because of their low hydraulic conductivity. This paper presents an approach for calculating the pore-water compositions of clayrocks from laboratory-measured properties of core samples, including their leachable Cl and SO4 concentrations and analysed exchangeable cations, and from mineral and cation exchange equilibria based on the formation mineralogy. New core sampling and analysis procedures are presented that reduce or quantify side reactions such as sample oxidation (e.g. pyrite) and soluble mineral dissolution (celestite, SrSO4) that affect measured SO4 concentrations and exchangeable cation distributions. The model considers phase equilibria only with minerals that are observed in the formation including the principal clay phases. The model has been used to calculate the composition of mobile pore water in the Callovo-Oxfordian clayrock and validated against measurements of water chemistry made in an underground research laboratory in that formation. The model reproduces the measured, in situ pore-water composition without any estimated parameters. All required parameters can be obtained from core sample analysis. We highlight the need to consider only those mineral phases which can be shown to be in equilibrium with contacting pore water. The consequence of this is that some conceptual models available in the literature appear not to be appropriate for modelling clayrocks, particularly those considering high temperature and/or high pressure detrital phases as chemical buffers of pore water. The robustness of our model with respect to uncertainties in the log K values of clay phases is also demonstrated. Large uncertainties in log K values for clay minerals have relatively small effects on modelled pore-water compositions.  相似文献   

7.
A field-scale experiment was conducted to evaluate various organic C sources as amendments for passive treatment of tailings pore water. Varied mixtures of peat, spent-brewing grain (SBG) and municipal biosolids (MB) were assessed for the potential to promote dissimilatory sulfate reduction (DSR) and metal-sulfide precipitation. Five amended cells and one control were constructed in the vadose zone of a sulfide- and carbonate-rich tailings deposit, and the geochemistry, microbiology and mineralogy were monitored for 4 a. Increases in pore-water concentrations of dissolved organic C (DOC) and decreases in aqueous SO4 concentrations of >2500 mg L−1 were observed in cells amended with peat + SBG and peat + SBG + MB. Removal of SO4 was accompanied by shifts in δ34S-SO4 values of >+30‰, undersaturation of pore water with respect to gypsum [CaSO4·2H2O], and increased populations of SO4-reducing bacteria (SRB). Decreases in aqueous concentrations of Zn, Mn, Ni, Sb and Tl were observed for these cells relative to the control. Organic C introduction also supported growth of Fe-reducing bacteria (IRB) and increases in Fe and As concentrations. Enhanced Fe and As mobility occurred in all cells; however, maximum concentrations were observed in cells amended with MB. Subsequent decreases in Fe and As concentrations were attributed to DSR and metal-sulfide precipitation. The common presence of secondary Zn-S and Fe-S phases was observed by field emission-scanning electron microscopy (FE-SEM) and energy dispersive X-ray (EDS) spectroscopy. Selective extractions indicated that large decreases in water-soluble SO4 occurred in cells that supported DSR. Furthermore, amendments that supported DSR generally were characterized by slight decreases in solid-phase concentrations of extractable metal(loid)s. Amendment of tailings with organic C amendments that supported ongoing DOC production and DSR was essential for sustained treatment.  相似文献   

8.
Formation and dissolution of secondary arsenic minerals often play significant roles in controlling arsenic mobility in contaminated environments, especially in sulfide mines. Weathering of the orpiment and realgar-bearing tailings from the Shimen realgar deposit, the largest realgar deposit in Asia, were studied. An integrated mineralogical analysis by using X-ray powder diffraction (XRD), Raman spectrum, scanning electron microscope (SEM) and transmission electron microscope (TEM) reveals four kinds of As-bearing secondary minerals including arsenic oxides, arsenates, As-gypsum, and As-Fe minerals. The precipitation of arsenates is due to interaction of As-bearing run-off waters and the underlying carbonate rocks, or the transformation of gypsum into arsenates or As-bearing gypsum through SO42-/HAsO42- substitution. Ca-arsenates are mainly weilite and pharmacolite with Ca/As atomic ratio of 1. Scanning transmission X-ray microscope (STXM) and X-ray absorption fine structure (XAFS) reveal that the valence of arsenic is mainly +3 and +5.  相似文献   

9.
《Applied Geochemistry》1999,14(4):485-498
Fine grained (ca. 15 μm), arsenopyrite-bearing mine tailings have been exposed to drying and oxidation for 4 a pending relocation. The tailings are still partly covered by a pond of decanted pore waters. The water table in drying tailings has lowered by 1–3 m and desiccation cracks up to 2 cm wide have formed on the 1 m scale, extending through the unsaturated zone. Tailings in the unsaturated zone have similar pore water contents to saturated tailings: typically 16–32 wt% water. Saturated tailings retain alkaline pH (ca. 10) from the mine cyanidation plant, but pH lowers progressively towards ca. 7 near the surface, or near desiccation cracks, in the unsaturated zone. The redox state of the tailings changes in parallel with pH, with an empirical relationship: Eh(mV)=−55 pH+290. Water in the remnant decant pond reflects this relationship also. Unsaturated tailings have variable but low permeabilities, typically 10−3 to 10−4 m/day, and more permeable horizons have allowed incursion of oxygenated air and/or rain water from desiccation cracks. Sulphide grains in all tailings examined are unaltered. Sulphides and solutions in the tailings are out of thermodynamic equilibrium predicted from the redox–pH conditions, due to kinetic constraints. Incursion of rain water locally facilitates deposition from pore waters of insoluble Fe oxide and arsenate minerals, thus fixing As in the dry unsaturated tailings.  相似文献   

10.
Mineralogical, geochemical and microbial characterization of tailings solids from the Greens Creek Mine, Juneau, Alaska, was performed to evaluate mechanisms controlling aqueous geochemistry of near-neutral pH pore water and drainage. Core samples of the tailings were collected from five boreholes ranging from 7 to 26 m in depth. The majority of the 51 samples (77%) were collected from the vadose zone, which can extend >18 m below the tailings surface. Mineralogical investigation indicates that the occurrence of sulfide minerals follows the general order: pyrite [FeS2] >> sphalerite [(Zn,Fe)S] > galena [PbS], tetrahedrite [(Fe,Zn,Cu,Ag)12Sb4S13] > arsenopyrite [FeAsS] and chalcopyrite [CuFeS2]. Pyrite constitutes <20 to >35 wt.% of the tailings mineral assemblage, whereas dolomite [CaMg(CO3)2] and calcite [CaCO3] are present at ?30 and 3 wt.%, respectively. The solid-phase geochemistry generally reflects the mineral assemblage. The presence of additional trace elements, including Cd, Cr, Co, Mo, Ni, Se and Tl, is attributed to substitution into sulfide phases. Results of acid–base accounting (ABA) underestimated both acid-generating potential (AP) and neutralization potential (NP). Recalculation of AP and NP based on solid-phase geochemistry and quantitative mineralogy yielded more representative results. Neutrophilic S-oxidizing bacteria (nSOB) and SO4-reducing bacteria (SRB) are present with populations up to 107 and 105 cells g−1, respectively. Acidophilic S-oxidizing bacteria (aSOB) and iron-reducing bacteria (IRB) were generally less abundant. Primary influences on aqueous geochemistry are sulfide oxidation and carbonate dissolution at the tailings surface, gypsum precipitation–dissolution reactions, as well as Fe reduction below the zone of sulfide oxidation. Pore-water pH values generally ranged from 6.5 to 7.5 near the tailings surface, and from approximately 7–8 below the oxidation zone. Elevated concentrations of dissolved SO4, S2O3, Fe, Zn, As, Sb and Tl persisted under these conditions.  相似文献   

11.
Variations in arsenic (As) mineralogy and geochemical controls on its mobility were evaluated in subsurface tailings at the historical Montague and Goldenville mine sites in Nova Scotia, Canada. Tailings at these sites contain some of the highest As concentrations in Nova Scotia and are located in close proximity to local communities. Pore water in the subsurface tailings is characterized by circumneutral to alkaline pH (6.2 to 8.7) and mildly reducing to oxidizing redox conditions (+130 mV to +347 mV). Bulk chemistry, scanning electron microscopy, and synchrotron micro-X-ray diffraction analyses showed As mineral hosts differ with depth. The deepest tailings (max. 2 m) are in direct contact with partially decomposed vegetation, which supports reducing conditions and the precipitation of authigenic As and Fe sulfides. Under reducing conditions, dissolved As concentrations are also controlled by desorption of As from dissolution of Fe and Mn oxides and the sorption or co-precipitation of As with carbonates. These geochemical controls differ from those influencing dissolved As concentrations under oxidizing conditions. In the near surface, As mobility is controlled by oxidative dissolution of primary arsenopyrite, precipitation of secondary Fe arsenates, Fe oxyhydroxides and Mn oxides, secondary Ca-Fe arsenates, and sorption onto Fe oxyhydroxides and gangue minerals. Some of these mineral species are stable under different conditions yet occur in close association, indicating the importance of microenvironments. The results of this study show that the weathering characteristics of these tailings vary with depth, leading to the formation of new As hosts that are distinct from those observed in the near surface. Identification of these As hosts provides an understanding of current controls on As mobility and has implications for future reprocessing and/or remediation efforts.  相似文献   

12.
Models of geochemical controls on elements of concern (EOCs; e.g., As, Se, Mo, Ni) in U tailings are dominated by ferrihydrite. However, the evolution of aqueous concentrations of Al and Mg through the Key Lake (KL) U mill bulk neutralization process indicates that secondary Al and Mg minerals comprise a large portion of the tailings solids. X-ray diffraction, Al K-edge XAS, and TEM elemental mapping of solid samples collected from a pilot-scale continuous-flow synthetic raffinate neutralization system of the KL mill indicate the secondary Al–Mg minerals present include Mg–Al hydrotalcite, amorphous Al(OH)3, and an amorphous hydrobasaluminite-type phase. The ferrihydrite present contains Al and may be more accurately described as Al–Fe(OH)3. In the final combined tailings sample (pH 10.5) collected from the model experiments using raffinate with Al, Mg, and Fe, solid phase EOCs were associated with Al–Fe(OH)3 and Mg–Al hydrotalcite. In model experiments using raffinate devoid of Fe, aqueous EOC concentrations decreased greatly at pH 4.0 (i.e., where ferrihydrite would precipitate) and largely remained in the solid phase when increased to the terminal pH of 10.5; this suggests Al–Mg minerals can control aqueous concentrations of EOCs in the raffinate in the absence of Fe. Maximum adsorption capacities for individual and mixtures of adsorbates by Mg–Al hydrotalcite were determined. A revised model of the geochemical controls in U mill tailings is presented in which Al and Mg minerals co-exist with Fe minerals to control EOC concentrations.  相似文献   

13.
《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   

14.
The oxidation and subsequent dissolution of sulfide minerals within mine tailings impoundments releases H+, Fe(II), SO4 and trace elements to the tailings pore water. Subsequent pH-buffering and hydrolysis reactions result in the precipitation of secondary phases such as gypsum, goethite and jarosite. In areas of intense precipitation, cemented layers or “hardpans” often form within the shallow tailings. Three cemented layers within pyrrhotite-bearing mine tailings at the Fault Lake, Nickel Rim and East Mine impoundments located near Sudbury, Canada, were examined. The location of the three cemented layers within the tailings stratigraphy varies as does their location relative to the water table. The morphology, mineralogy and chemical composition of the cemented layers also vary between sites. The bulk density within the three cemented layers all showed an increase relative to the surrounding uncemented tailings ranging from 9% to 29%. The porosity of each cemented layer decreased relative to the surrounding uncemented tailings ranging from an 8% to 18% decrease. The cemented layers also showed relative enrichment of total sulfur, carbon and trace elements relative to the surrounding uncemented tailings. Arsenic concentrations showed an enrichment in the cemented layers of up to 132%, Cd up to 99%, Co up to 84%, Cu up to 144%, Ni up to 693% and Zn up to 145% relative to the surrounding uncemented tailings. All the cemented layers studied show an evolution of the secondary phases with time from a gypsum–jarosite-based cement to a goethite-rich cement. The formation of these layers could potentially have a significant effect on the environmental impacts of sulfide-bearing mine waste.  相似文献   

15.
Arsenic and antimony contamination is found at the Pezinok mining site in the southwest of the Slovak Republic. Investigation of this site included sampling and analysis of water, mineralogical analyses, sequential extraction, in addition to flow and geochemical modeling. The highest dissolved arsenic concentrations correspond to mine tailings (up to 90,000 μg/L) and the arsenic is present predominately as As(V). The primary source of the arsenic is the dissolution of arsenopyrite. Concentration of antimony reaches 7,500 μg/L and its primary source is the dissolution of stibnite. Pore water in mine tailings is well-buffered by the dissolution of carbonates (pH values between 6.6 and 7.0) and arsenopyrite grains are surrounded by reaction rims composed of ferric iron minerals. Based on sequential extraction results, most solid phase arsenic is in the reducible fraction (i.e. ferric oxyhydroxides), sulfidic fraction, and residual fraction. Distribution of antimony in the solid phase is similar, but contents are lower. The principal attenuation mechanism for As(V) is adsorption to ferric oxide and hydroxides, but the adsorption seems to be limited by the competition with Sb(V) produced by the oxidation of stibnite for adsorption sites. Water in mine tailings is at equilibrium with gypsum and calcite, but far from equilibrium with any arsenic and antimony minerals. The concentrations of arsenic and antimony in the surrounding aquifer are much lower, with maximum values of 215 and 426 μg/L, respectively. Arsenic and antimony are transported by ground water flow towards the Blatina Creek, but their loading from ground water to the creek is much lower compared with the input from the mine adits. In the Blatina Creek, arsenic and antimony are attenuated by dilution and by adsorption on ferric iron minerals in stream sediments with resulting respective concentrations of 93 and 45 μg/L at the site boundary south of mine tailing ponds.  相似文献   

16.
Nearly half a century after mine closure, release of As from the Ylöjärvi Cu–W–As mine tailings in groundwater and surface water run-off was observed. Investigations by scanning electron microscopy (SEM), electron microprobe analysis (EMPA), synchrotron-based micro-X-ray diffraction (μ-XRD), micro-X-ray absorption near edge structure (μ-XANES) and micro-extended X-ray absorption fine structure (μ-EXAFS) spectroscopy, and a sequential extraction procedure were performed to assess As attenuation mechanisms in the vadose zone of this tailings deposit. Results of SEM, EMPA, and sequential extractions indicated that the precipitation of As bearing Fe(III) (oxy)hydroxides (up to 18.4 wt.% As2O5) and Fe(III) arsenates were important secondary controls on As mobility. The μ-XRD, μ-XANES and μ-EXAFS analyses suggested that these phases correspond to poorly crystalline and disordered As-bearing precipitates, including arsenical ferrihydrite, scorodite, kaňkite, and hydrous ferric arsenate (HFA). The pH within 200 cm of the tailings surface averaged 5.7, conditions which favor the precipitation of ferrihydrite. Poorly crystalline Fe(III) arsenates are potentially unstable over time, and their transformation to ferrihydrite, which contributes to As uptake, has potential to increase the As adsorption capacity of the tailings. Arsenic mobility in tailings pore water at the Ylöjärvi mine will depend on continued arsenopyrite oxidation, dissolution or transformation of secondary Fe(III) arsenates, and the As adsorption capacity of Fe(III) (oxy)hydroxides within this tailings deposit.  相似文献   

17.
《Applied Geochemistry》2000,15(8):1219-1244
Arsenian pyrite, formed during Cretaceous gold mineralization, is the primary source of As along the Melones fault zone in the southern Mother Lode Gold District of California. Mine tailings and associated weathering products from partially submerged inactive gold mines at Don Pedro Reservoir, on the Tuolumne River, contain ∼20–1300 ppm As. The highest concentrations are in weathering crusts from the Clio mine and nearby outcrops which contain goethite or jarosite. As is concentrated up to 2150 ppm in the fine-grained (<63 μm) fraction of these Fe-rich weathering products.Individual pyrite grains in albite-chlorite schists of the Clio mine tailings contain an average of 1.2 wt.% As. Pyrite grains are coarsely zoned, with local As concentrations ranging from ∼0 to 5 wt.%. Electron microprobe, transmission electron microscope, and extended X-ray absorption fine-structure spectroscopy (EXAFS) analyses indicate that As substitutes for S in pyrite and is not present as inclusions of arsenopyrite or other As-bearing phases. Comparison with simulated EXAFS spectra demonstrates that As atoms are locally clustered in the pyrite lattice and that the unit cell of arsenian pyrite is expanded by ∼2.6% relative to pure pyrite. During weathering, clustered substitution of As into pyrite may be responsible for accelerating oxidation, hydrolysis, and dissolution of arsenian pyrite relative to pure pyrite in weathered tailings. Arsenic K-edge EXAFS analysis of the fine-grained Fe-rich weathering products are consistent with corner-sharing between As(V) tetrahedra and Fe(III)-octahedra. Determinations of nearest-neighbor distances and atomic identities, generated from least-squares fitting algorithms to spectral data, indicate that arsenate tetrahedra are sorbed on goethite mineral surfaces but substitute for SO4 in jarosite. Erosional transport of As-bearing goethite and jarosite to Don Pedro Reservoir increases the potential for As mobility and bioavailability by desorption or dissolution. Both the substrate minerals and dissolved As species are expected to respond to seasonal changes in lake chemistry caused by thermal stratification and turnover within the monomictic Don Pedro Reservoir. Arsenic is predicted to be most bioavailable and toxic in the reservoir’s summer hypolimnion.  相似文献   

18.
谭凯旋  谢焱石  刘永 《矿物学报》2004,24(4):398-404
从硫化物的氧化、脉石矿物的溶解、氧的扩散、水的流动和溶质质量迁移等过程的耦合作用建立了尾矿-水相互作用的动力学模型。对湖南湘西金矿尾矿库的数学模拟表明：早期尾矿-水的相互作用可以引起酸水的产生和重金属的释放及对环境的污染，影响较大的主要是前30年，随着时间增加，尾矿孔隙水逐渐中性化，污染元素含量显著降低。脉石矿物的溶解和有机物反应可降低尾矿中氧的扩散和产生酸的中和作用。尾矿库上部孔隙水中各组分含量明显高于尾矿库下部，并在约6m深处存在突变带。尾矿库的水文分带是导致地球化学分带的主要原因。  相似文献   

19.
金属矿山生产产生大量的尾矿,不但危害周围生态环境,而且对资源造成极大浪费。金川镍矿尾矿砂Ni、Cu和Co的平均含量分别达到0.21%、0.19%和0.01%,是够得上二次开发利用的宝贵资源。文中对金川镍矿尾矿砂矿物组成特征及酸溶特性进行了详细的研究,目的是为工业化高效回收尾矿砂中Ni、Cu和Co等有价金属提供科学依据与技术支撑。矿物学研究表明,金川镍矿尾矿砂主要由蛇纹石、绿泥石、橄榄石、辉石、透闪石、磁铁矿、白云石及少量磁黄铁矿、镍黄铁矿和黄铜矿等组成。经多年露天堆存,金川镍矿老尾矿库尾矿砂已发生不同程度的氧化作用。尾矿库3 m以上为强烈氧化带,金属硫化物矿物颗粒边缘、裂缝处基本都有强烈的氧化作用发生。碳酸盐等易溶矿物被大量消耗。硫酸溶解实验表明,金川镍矿老尾矿库尾矿砂中有价金属Cu、Ni和Co的平均浸出率分别可达88.6%、75.3% 和70.8%。尾矿砂中Cu、Ni和Co有价金属的浸出效果不但清楚直观地反映了尾矿库中尾矿砂的氧化程度,而且表明金属硫化物尾矿砂的风化作用,极大地促进了硫化物矿物中有价金属的酸溶浸出。  相似文献   

20.
The Lavrion carbonate-hosted Pb-Ag-Zn deposit in southeast Attica, Greece, consisted of significant non-sulfide ore bodies. The polymetallic sulfide mineralization was subjected to supergene oxidation, giving rise to gossan. The principal non-sulfide minerals of past economic importance were smithsonite, goethite and hematite. The supergene mineral assemblages occupy secondary open spaces and occur as replacement pods within marble. Calamine and iron ore mainly filled open fractures. X-ray diffraction and scanning electron microscopy of samples of oxidized ore indicate complex gossan mineralogy depending on the hypogene mineralogy, the degree of oxidation and leaching of elements, and the local hydrologic conditions. Bulk chemical analysis of the samples indicated high ore-grade variability of the supergene mineralization. On multivariate cluster analysis of geochemical data the elements were classified into groups providing evidence for their differential mobilization during dissolution, transport and re-precipitation. The mode of occurrence, textures, mineralogy and geochemistry of the non-sulfide mineralization confirm that it is undoubtedly of supergene origin: the product of influx into open fractures in the country rock of highly acidic, metal-rich water resulting from the oxidation of pyrite-rich sulfide protore. Dissolution of carbonates led to opening of the fractures. Mineral deposition in the supergene ore took place under near-neutral to mildly acidic conditions. The supergene dissolution and re-precipitation of Fe and Zn in the host marble increased metal grades and separated iron and zinc from lead, thereby producing economically attractive deposits; it further contributed to minimization of pollution impact on both soil and ground water.  相似文献   

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