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1.
《Applied Geochemistry》2005,20(2):383-396
Potential contamination of rivers by trace elements can be controlled, among others, by the precipitation of oxyhydroxides. The streambed of the studied area, located in “La Châtaigneraie” district (Lot River Basin, France), is characterised by iron-rich ochreous deposits, acidic pH (2.7–4.8) and SO4–Mg waters. Beyond the acid mine drainage, the presence of As both in the dissolved fraction and in the deposits is also a problem. Upstream, at the gallery outlet, As concentrations are high (Asmax = 2.6 μmol/l and up to 5 wt% locally, respectively, in the dissolved and in the solid fractions). Downstream, As concentrations decrease below 0.1 μmol/l in the dissolved fraction and to 1327 mg/kg in the solid fraction. This natural attenuation is related to the As retention within ochreous precipitates (amorphous to poorly crystalline Fe oxyhydroxides, schwertmannite and goethite), which have great affinities for this metalloid. Upstream, schwertmannite is dominant while downstream, goethite becomes the main mineral. The transformation of schwertmannite into goethite is observed in the upstream deposits as schwertmannite is unstable relative to goethite. Furthermore, thermodynamic calculations indicate that the downstream goethite is not able to precipitate in situ according to the water chemistry. Goethite mainly results from the transformation of schwertmannite and its solid transport downstream.Moreover, as highlighted by leaching experiments carried out on the ochreous precipitates, this transformation does not seem to affect the As-retention in solids as no release of As was observed in the solution. Arsenic may either be strongly trapped by co-precipitation in the present minerals or it may be quickly released and re-adsorbed on the precipitate surface.  相似文献   

2.
Acid mine drainage discharged from the abandoned Daduk mine towards the Daduk creek has a pH of 3.3, and concentrations of Al, Mn, Fe, Zn and SO4 of 18, 41, 45, 38 and 1940 mg/L, respectively. In particular, As concentration in acid mine drainage is 1000 μg/L. Removing order of metal ions normalized by SO4 concentration downstream from discharge point is Fe > As > Al > Cu > Zn > Mn > Cd > Pb. In the Daduk creek, Fe and As are the most rapidly depleted downstream from acid mine drainage because As adsorbs, coprecipitates and forms compounds with ferric oxyhydroxide. From the results of geochemical modeling using the Phreeq C program, goethite (FeOOH) is oversaturated, and schwertmannite (Fe8O8(OH)4.5(SO4)1.75) is the most stable solid phase at low pH in the Daduk creek. Yellowish red (orange ochre) precipitates that occurred in the study area are probably composed of goethite or schwertmannite.  相似文献   

3.
《Applied Geochemistry》2005,20(6):1226-1239
High concentrations of Cr (up to 812 ppm) and As (up to 6740 ppm) were detected in precipitates of the mineral schwertmannite in areas influenced by acid mine drainage. Schwertmannite may act as well as a natural filter for these elements in water as well as their source by releasing the previously bound elements during its dissolution or mineral-transformation. The mechanisms of uptake and potential release for the species arsenate and chromate were investigated by performing synthesis and stability experiments with schwertmannite.Schwertmannite, synthesized in solutions containing arsenate in addition to sulphate, was enriched by up to 10.3 wt% arsenate without detectable structural changes as demonstrated by powder X-ray diffraction (XRD). In contrast to arsenate, a total substitution of sulphate by chromate was possible in sulphate-free solutions. Thereby, the chromate content in schwertmannite could reach 15.3 wt%.To determine the release of oxyanions from schwertmannite over time, synthetic schwertmannite samples containing varying amounts of sulphate, chromate and arsenate were kept at a stable pH of either 2 or 4 over 1 year in suspension. At several time intervals Fe and the oxyanions were measured in solution and alterations of the solid part were observed by XRD and Fourier-Transform infrared (FT-IR) spectroscopy. At pH 2 schwertmannite partly dissolved and the total release of arsenate (24%) was low in contrast to chromate (35.4–57.5%) and sulphate (67–76%). Accordingly, the ionic activity product (log IAP) of arsenated schwertmannite was lowest (13.5), followed by the log IAP for chromated schwertmannite (16.2–18.5) and the log IAP for regular (=non-substituted) schwertmannite (18). At pH 4 schwertmannite transformed to goethite, an effect which occurred at the fastest rate for regular schwertmannite (=arsenate- and chromate-free), followed by chromate and arsenate containing schwertmannite. Both chromate and more evidently arsenate have a stabilizing effect on the schwertmannite structure, because they retarded the dissolution and transformation reactions.These kinetic investigations as well as crystallographic considerations demonstrated that the strength of the Fe(III) complexes with the anions controls the formation process and the stability of schwertmannite: with increasing affinity of the oxyanions to form complexes with Fe(III), the strength of the resulting binding and thus the stability and substitution preference increases.  相似文献   

4.
《Applied Geochemistry》2005,20(8):1445-1460
Changes in precipitate mineralogy, morphology, and major and trace element concentrations and associations throughout 5 coal mine drainage (CMD) remediation systems treating discharges of varying chemistries were investigated in order to determine the factors that influence the characteristics of precipitates formed in passive systems. The 5 passive treatment systems sampled in this study are located in the bituminous coal fields of western Pennsylvania and northern Maryland, and treat discharges from Pennsylvanian age coals. The precipitates are dominantly (>70%) goethite. Crystallinity varies throughout an individual system, and lower crystallinity is associated with enhanced sorption of trace metals. Degree of crystallinity (and subsequently morphology and trace metal associations) is a function of the treatment system and how rapidly Fe(II) is oxidized, forms precipitates, aggregates and settles. Precipitates formed earlier in the passive treatment systems tend to have the highest crystallinity and the lowest concentrations of trace metal cations. High surface area and cation vacancies within the goethite structure enable sorption and incorporation of metals from coal mine drainage-polluted waters. Sorption affinities follow the order of Zn > Co ≈ Ni > Mn. Cobalt and Ni are preferentially sorbed to Mn oxide phases when these phases are present. As pH increases in the individual CMD treatment systems toward the pHpzc of goethite, As sorption decreases and transition metal (Co, Mn, Ni and Zn) sorption increases. Sulfate, Na and Fe(II) concentrations may all influence the sorption of trace metals to the Fe hydroxide surface. Results of this study have implications not only for solids disposal and resource recovery but also for the optimization of passive CMD treatment systems.  相似文献   

5.
《Applied Geochemistry》2001,16(11-12):1387-1396
The purposes of this study are to (i) determine the geochemical characteristics of Imgok creek impacted by acid mine drainage (AMD) generated from abandoned coal mines, (ii) to assess the pollution of heavy metals in the stream sediments and soils, and (iii) to identify the chemical form of Fe precipitates collected in the study area where there are 4 abandoned coal mines, which belong to the Grangreung coal field at the eastern part of Korea. AMD generated from mine adits and coal refuse piles shows low pH, and high concentrations of Fe, Al and SO4, especially in the Youngdong coal mine. In Imgok creek, pH values increased, and total dissolved solids (TDS) values decreased with distance. The concentrations of toxic heavy metals and major cations except Fe decreased by dilution, but the concentration of Fe decreased rapidly due to the formation of precipitates. The quality of groundwater samples did not exceed the Korean drinking-water standard. In the stream sediments, the concentrations of Fe are relatively high in the Youngdong tributary and Imgok creek, but the concentrations of heavy metals are similar to those of unpolluted sediments. Pollution indices of agricultural soils range from 0.28 to 0.47. Yellowish red Fe precipitates collected in the study area turned out to be amorphous or poorly crystallized minerals (determined by X-ray diffraction patterns and Feox/Fetot ratios) and to contain chemically bonded SO4 and OH [determined by infra-red (IR) spectral analysis]. With these, the mol ratios of Fe/S ranging from 4.6 to 6.1 determined by electron probe micro-analysis (EPMA) in precipitates strongly support the existence of schwertmannite.  相似文献   

6.
Tidal inundation is a new technique for remediating coastal acid sulfate soils (CASS). Here, we examine the effects of this technique on the geochemical zonation and cycling of Fe across a tidally inundated CASS toposequence, by investigating toposequence hydrology, in situ porewater geochemistry, solid-phase Fe fractions and Fe mineralogy. Interactions between topography and tides exerted a fundamental hydrological control on the geochemical zonation, redistribution and subsequent mineralogical transformations of Fe within the landscape. Reductive dissolution of Fe(III) minerals, including jarosite (KFe3(SO4)2(OH)6), resulted in elevated concentrations of porewater Fe2+ (> 30 mmol L?1) in former sulfuric horizons in the upper-intertidal zone. Tidal forcing generated oscillating hydraulic gradients, driving upward advection of this Fe2+-enriched porewater along the intertidal slope. Subsequent oxidation of Fe2+ led to substantial accumulation of reactive Fe(III) fractions (up to 8000 μmol g?1) in redox-interfacial, tidal zone sediments. These Fe(III)-precipitates were poorly crystalline and displayed a distinct mineralisation sequence related to tidal zonation. Schwertmannite (Fe8O8(OH)6SO4) was the dominant Fe mineral phase in the upper-intertidal zone at mainly low pH (3–4). This was followed by increasing lepidocrocite (γ-FeOOH) and goethite (α-FeOOH) at circumneutral pH within lower-intertidal and subtidal zones. Relationships were evident between Fe fractions and topography. There was increasing precipitation of Fe-sulfide minerals and non-sulfidic solid-phase Fe(II) in the lower intertidal and subtidal zones. Precipitation of Fe-sulfide minerals was spatially co-incident with decreases in porewater Fe2+. A conceptual model is presented to explain the observed landscape-scale patterns of Fe mineralisation and hydro-geochemical zonation. This study provides valuable insights into the hydro-geochemical processes caused by saline tidal inundation of low lying CASS landscapes, regardless of whether inundation is an intentional strategy or due to sea-level rise.  相似文献   

7.
《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   

8.
We examined the transformations of Fe and S associated with schwertmannite (Fe8O8(OH)6SO4) reduction in acidified coastal lowlands. This was achieved by conducting a 91 day diffusive-flux column experiment, which involved waterlogging of natural schwertmannite- and organic-rich soil material. This experiment was complemented by short-term batch experiments utilizing synthetic schwertmannite. Waterlogging readily induced bacterial reduction of schwertmannite-derived Fe(III), producing abundant pore-water FeII, SO4 and alkalinity. Production of alkalinity increased pH from pH 3.4 to pH ∼6.5 within the initial 14 days, facilitating the precipitation of siderite (FeCO3). Interactions between schwertmannite and FeII at pH ∼6.5 were found, for the first time, to catalyse the transformation of schwertmannite to goethite (αFeOOH). Thermodynamic calculations indicate that this FeII-catalysed transformation shifted the biogeochemical regime from an initial dominance of Fe(III)-reduction to a subsequent co-occurrence of both Fe(III)- and SO4-reduction. This lead firstly to the formation of elemental S via H2S oxidation by goethite, and later also to formation of nanoparticulate mackinawite (FeS) via H2S precipitation with FeII. Pyrite (FeS2) was a quantitatively insignificant product of reductive Fe and S mineralization. This study provides important new insights into Fe and S geochemistry in settings where schwertmannite is subjected to reducing conditions.  相似文献   

9.
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10.
Oxygenation of the Earth's atmosphere occurred in two major steps, near the beginning and near the end of the Proterozoic Eon (2500 to 542 Ma ago), but the details of this history are unclear. Chromium isotopes in iron-rich chemical sediments offer a potential to highlight fine-scale fluctuations in the oxygenation of the oceans and atmosphere and to add a further dimension in the use of redox-sensitive tracers to solve the question regarding fluctuations of atmospheric oxygen levels and their consequences for Earth's climate. We observe strong positive fractionations in Cr isotopes (δ53Cr up to + 5.0‰) in iron-rich cherts and banded iron formation horizons within the Arroyo del Soldado Group (Ediacaran; Uruguay) that can be explained by rapid, effective oxidation of Fe(II)-rich surface waters. These fluctuations are correlated with variations in ratios of highly reactive iron (FeHR) to total iron (Fetot) which indicate a predominance of anoxic water columns (FeHR/Fetot > 0.38) during the onset of oxidation pulses. We favor the scenario by which isotopically heavy Cr(VI) entered the basin after pulses of oxidative weathering on land and in which Fe(II) accumulated in the water column. Neodymium isotopes reveal that these oxygenation pulses were followed by increased influxes to the basin of continental crust-derived detrital components of Paleoproterozoic (Nd TDM model ages = 2.1–2.2 Ga) provenance typical of the Rio de la Plata Craton. The association of positive δ53Cr–ferruginous (FeHR/Fetot > 0.38) stratigraphic intervals with low-diversity acritarch assemblages dominated by Bavlinella faveolata strongly support models postulating a stratified, eutrophic Neoproterozoic ocean. Thus, even within a few million years of the Precambrian–Cambrian boundary, paleoceanographic conditions resembled more those of Paleoproterozoic oceans than Phanerozoic and present oceans. This highlights the sheer magnitude of ecological changes at the Precambrian–Cambrian transition, changes which ultimately led to the demise of the Precambrian world and the birth of the metazoan-dominated Phanerozoic.  相似文献   

11.
This is the first detailed account of the copper sulfate posnjakite (Cu4(SO4)(OH)6·H2O) coating cm-long filaments of a microbial consortium of four cyanobacteria and Herminiimonas arsenicoxydans. It was first observed on immersed plant leaves and stalks in a quarry sump of the abandoned Yanqul gold mine in the northern region of Oman; rock surfaces in the immediate vicinity show no immediate evidence of posnjakite. However, a thin unstructured layer without filaments but also containing the brightly coloured turquoise posnjakite covers ferruginous muds in the sump. Although copper is a potent bactericide, the microbes seem to survive even at the extreme heavy metal concentrations that commonly develop in the sump during the dry season (Cu2+ ≈ 2300 ppm; Zn2+ = 750 ppm; Fe2+ ≈ 120 ppm; Ni2+ = 37 ppm; Crtotal = 2.5 ppm; Cl− = 8250 ppm; and SO42− = 12,250 ppm; pH ∼2.6), thus leading to the precipitation of posnjakite over a large range of physicochemical conditions. Upon exposure to the prevailing arid climate, dehydration and carbonation quickly replace posnjakite with brochantite (Cu4(SO4)(OH)6) and malachite (Cu2(CO3)(OH)2). To characterise and understand the geochemical conditions in which posnjakite precipitates from undersaturated fluids (according to our thermodynamic modelling of the dominant elements), waters from rainy and dry periods were analysed together with various precipitates and compared with the observed field occurrences. The findings imply that posnjakite should not form in the examined environment through purely inorganic mechanisms and its origin must, therefore, be linked to the encountered microbial activities.  相似文献   

12.
《Applied Geochemistry》2005,20(5):907-917
Solutions draining the Alta Mine, Jefferson County, MT, were contaminated by acid sulfate waters (ASW) generated from anthropogenic exposure of meteoric waters to sulfidic underground mine workings and a waste-rock pile. In 1999, a remediation effort was initiated in an attempt to improve the quality of water draining the site through removal of the waste-rock pile with which these solutions come in contact. ASW were sampled in the mineshaft prior to entering the waste-rock pile and upon discharge from the waste-rock pile aquifer near the pile toe. ASW composition changed as solutions flowed through the waste-rock pile due to sulfide and silicate weathering and schwertmannite precipitation.Schwertmannite and goethite were both sampled in the waste-rock pile where a distinct field relation was observed between the two minerals. Schwertmannite was always in contact with actively flowing ASW, while goethite was never in direct contact with ASW and was generally above the waste-rock water table. Goethite is hypothesized to be re-dissolved/re-precipitated schwertmannite that was deposited under higher flow conditions and subsequently transformed to goethite through exposure to wet/dry cycling associated with seasonal fluctuations in the amount of water moving through the hydrogeologic system. Trace metal concentrations in ammonium oxalate extracts of these minerals provides the first published data on the behavior of multiple trace metals through this phase transformation, which has important ramifications for considering schwertmannite as a long term metal sink due to its known metastability with respect to goethite. A relative retention scale through this phase transformation of Pb > Zn, Mn > As, Al, Cu is potentially applicable to other ASW systems.  相似文献   

13.
《Applied Geochemistry》2005,20(11):2038-2048
Thermodynamic simulations of reactions among SO2-bearing CO2-dominated gas, water and mineral phases predict that FeIII in sediments should be converted almost entirely to dissolved FeII and siderite (FeCO3), and that SO2 should simultaneously be oxidized to dissolved sulfate. The reactions are however, subject to kinetic constraints which may result in deviation from equilibrium and the precipitation of other metastable mineral phases. To test the prediction, a laboratory experiment was carried out in a well stirred hydrothermal reactor at 150 °C and 300 bar with hematite, 1.0 m NaCl, 0.5 m NaOH, SO2 in quantity sufficient to reduce much of the iron, and excess CO2. The experiment produced stable siderite and metastable pyrite and elemental S. Changes in total dissolved Fe are consistent with nucleation of pyrite at ∼17 h, and nucleation of siderite at ∼600 h. Dissolution features present on elemental S at the conclusion of the experiment suggest nucleation early in the experiment. The experiment did not reach equilibrium after ∼1400 h, as indicated by coexistence of hematite with metastable pyrite and elemental sulfur. However, the results confirm that FeIII can be used to trap CO2 in siderite if partly oxidized S, as SO2, is present to reduce the Fe with CO2 in the gas phase.  相似文献   

14.
《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   

15.
《Applied Geochemistry》2005,20(6):1180-1194
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16.
《Applied Geochemistry》2006,21(8):1251-1258
Computer modelling techniques involving a rigid ion model have been used to investigate the defect structure and impurity site preferences in end-member K-jarosite. Calculated intrinsic vacancy energies show that the K2SO4 neutral cluster, with an energy per species of 1.34 eV, will be the most common defect in the pure phase. Defect reactions leading to vacancies on the Fe site have high energies, in excess of 4.0 eV per species, and are thus unlikely to occur in great numbers. However, the calculations show that divalent metal cations can be incorporated onto the Fe site via solution reactions with oxides leading to the formation of goethite. Calculated solution reactions are exothermic and thus predicted to be highly favourable. At K sites substitutions occur in the order Cd > Zn > Cu, but will be limited due to endothermic solution energies and structural considerations.  相似文献   

17.
《Geochimica et cosmochimica acta》1999,63(19-20):3407-3416
The apparent solubilities of schwertmannite and ferrihydrite were estimated from the H+, OH−, Fe3+, and SO42− activities of the natural stream waters in Korea and mine drainage in Ohio, USA. Both chemical composition of the stream waters and the mineralogy of the precipitates were determined for samples from two streams polluted by coal mine drainage. This study combines these new results with previous data from Ohio, USA to redetermine solubilities. The activities of the dissolved species necessary for the solubility determinations were calculated from the chemical compositions of the waters with the WATEQ4F computer code.Laboratory analyses of precipitates indicated that the main minerals present in Imgok and Osheep creek were schwertmannite and ferrihydrite, respectively. The schwertmannite from Imgok creek had a variable chemical formula of Fe8O8(OH)8−2x(SO4)x· nH2O, where 1.74 ≤ x ≤ 1.86 and 8.17 ≤ n ≤ 8.62. The chemical formula of ferrihydrite was Fe2O3· 1.6H2O. With known mineralogy of the precipitates from each stream, the activities of H+, OH−, Fe3+, and SO42− in the waters were plotted on logarithmic activity-activity diagrams to determine apparent solubilities of schwertmannite and ferrihydrite. The best estimate for the logarithm of the solubility product of schwertmannite, logKs, was 10.5 ± 2.5 around 15°C. This value of logKs constrains the logarithm of the solubility product of ferrihydrite, logKf, to be 4.3 ± 0.5 to maintain the stability boundary with schwertmannite observed in natural waters.  相似文献   

18.
《Applied Geochemistry》2003,18(8):1267-1278
At the abandoned As mine in Nishinomaki, Japan, discharged water from the mining and waste dump area is acidic and rich in As. However, the As concentration in the drainage has been decreased to below the maximum contaminant level (0.01 mg/l for drinking water, Japan) without any artificial treatments before mixing with a tributary to populated areas. This implies that the As concentration in water from the waste dump area has been naturally attenuated. To elucidate the reaction mechanisms of the natural attenuation, analysis of water quality and characterization of the precipitates from the stream floor were performed by measuring pH, ORP and electric conductivity on-site, as well as X-ray diffraction, ICP-mass spectrometry and ion-chromatography. Selective extractions and mineral alteration experiments were also conducted to estimate the distribution of As in constituent phases of the precipitates and to understand the stability of As-bearing phases, respectively. The water contamination resulted from oxidation of sulfide minerals in the waste rocks, i.e., the oxidation of pyrite and realgar and subsequent release of Fe, SO4, As(V) and proton. The released Fe(II) transformed to Fe(III) by bacterial oxidation; schwertmannite then formed immediately. While the As concentrations in the stream were lowered nearly to background level downstream, those in the ochreous precipitates were up to several tens of mg/g. The As(V) was effectively removed by the formed schwertmannite and had been naturally attenuated. Although schwertmannite is metastable with respect to goethite, the experiments show that the transformation of schwertmannite to goethite may be retarded by the presence of absorbed As(V) in the structure. Therefore, the attenuation of As in the drainage and the retention of As by schwertmannite are expected to be maintained for the long term.  相似文献   

19.
《Applied Geochemistry》2005,20(7):1320-1356
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20.
Schwertmannite (Fe8O8(OH)6SO4) is a common Fe(III)-oxyhydroxysulfate mineral in acid-sulfate systems, where its formation and fate strongly influence water quality. The present study examines transformation of schwertmannite to goethite (FeOOH), as catalyzed by interactions with Fe(II) in anoxic aquatic environments. This study also evaluates the role of the Fe(II) pathway in influencing the formation of iron-sulfide minerals in such environments. At pH > 5, the rates of Fe(II)-catalyzed schwertmannite transformation were several orders of magnitude faster than transformation in the absence of Fe(II). Complete transformation of schwertmannite occurred within only 3-5 h at pH > 6 and Fe(II)(aq) ? 5 mmol L−1. Model calculations indicate that the Fe(II)-catalyzed transformation of schwertmannite to goethite greatly decreases the reactivity of the Fe(III) pool, thereby favoring SO4-reduction and facilitating the formation of iron-sulfide minerals (particularly mackinawite, tetragonal FeS). Examination of in situ sediment geochemistry in an acid-sulfate system revealed that the rapid Fe(II)-catalyzed transformation was consistent with an abrupt shift from an acidic Fe(III)-reducing regime with abundant schwertmannite near the sediment surface, to a near-neutral mackinawite-forming regime where goethite was dominant. This study demonstrates that the Fe(II) pathway exerts a major influence on schwertmannite transformation and iron-sulfide formation in anoxic acid-sulfate systems. These findings have important implications for understanding acidity dynamics and trace element mobility in such systems.  相似文献   

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