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1.
To better understand reaction pathways of pyrite oxidation and biogeochemical controls on δ18O and δ34S values of the generated sulfate in acid mine drainage (AMD) and other natural environments, we conducted a series of pyrite oxidation experiments in the laboratory. Our biological and abiotic experiments were conducted under aerobic conditions by using O2 as an oxidizing agent and under anaerobic conditions by using dissolved Fe(III)aq as an oxidant with varying δ18OH2O values in the presence and absence of Acidithiobacillus ferrooxidans. In addition, aerobic biological experiments were designed as short- and long-term experiments where the final pH was controlled at ∼2.7 and 2.2, respectively. Due to the slower kinetics of abiotic sulfide oxidation, the aerobic abiotic experiments were only conducted as long term with a final pH of ∼2.7. The δ34SSO4 values from both the biological and abiotic anaerobic experiments indicated a small but significant sulfur isotope fractionation (∼−0.7‰) in contrast to no significant fractionation observed from any of the aerobic experiments. Relative percentages of the incorporation of water-derived oxygen and dissolved oxygen (O2) to sulfate were estimated, in addition to the oxygen isotope fractionation between sulfate and water, and dissolved oxygen. As expected, during the biological and abiotic anaerobic experiments all of the sulfate oxygen was derived from water. The percentage incorporation of water-derived oxygen into sulfate during the oxidation experiments by O2 varied with longer incubation and lower pH, but not due to the presence or absence of bacteria. These percentages were estimated as 85%, 92% and 87% from the short-term biological, long-term biological and abiotic control experiments, respectively. An oxygen isotope fractionation effect between sulfate and water (ε18OSO4-H2O) of ∼3.5‰ was determined for the anaerobic (biological and abiotic) experiments. This measured value was then used to estimate the oxygen isotope fractionation effects between sulfate and dissolved oxygen in the aerobic experiments which were −10.0‰, −10.8‰, and −9.8‰ for the short-term biological, long-term biological and abiotic control experiments, respectively. Based on the similarity between δ18OSO4 values in the biological and abiotic experiments, it is suggested that δ18OSO4 values cannot be used to distinguish biological and abiotic mechanisms of pyrite oxidation. The results presented here suggest that Fe(III)aq is the primary oxidant for pyrite at pH < 3, even in the presence of dissolved oxygen, and that the main oxygen source of sulfate is water-oxygen under both aerobic and anaerobic conditions.  相似文献   

2.
《Applied Geochemistry》2005,20(11):2116-2137
Samples of mine water from Butte, Montana were collected for paired geochemical and stable isotopic analysis. The samples included two sets of depth profiles from the acidic Berkeley pit lake, deep groundwater from several mine shafts in the adjacent flooded underground mine workings, and the acidic Horseshoe Bend Spring. Beginning in July-2000, the spring was a major surface water input into the Berkeley pit lake. Vertical trends in major ions and heavy metals in the pit lake show major changes across a chemocline at 10–20 m depth. The chemocline most likely represents the boundary between pre-2000 and post-2000 lake water, with lower salinity, modified Horseshoe Bend Spring water on top of higher salinity lake water below. Based on stable isotope results, the deep pit lake has lost approximately 12% of its initial water to evaporation, while the shallow lake is up to 25% evaporated. The stable isotopic composition of SO4 in the pit lake is similar to that of Horseshoe Bend Spring, but differs markedly from SO4 in the surrounding flooded mine shafts. The latter is heavier in both δ34S and δ18O, which may be due to dissolution of hypogene SO4 minerals (anhydrite, gypsum, barite) in the ore deposit. The isotopic and geochemical evidence suggests that much of the SO4 and dissolved heavy metals in the deep Berkeley pit lake were generated in situ, either by leaching of soluble salts from the weathered pit walls as the lake waters rose, or by subaqueous oxidation of pyrite on the submerged mine walls by dissolved Fe(III). Laboratory experiments were performed to contrast the isotopic composition of SO4 formed by aerobic leaching of weathered wallrock vs. SO4 from anaerobic pyrite oxidation. The results suggest that both processes were likely important in the evolution of the Berkeley pit lake.  相似文献   

3.
The study was carried out on the Sulejów dam reservoir (Central Poland). Water and sediment samples were collected between February and October 2006. Sulfur compounds in the sediment were chemically extracted and subjected to isotopic analysis.Large variability of SO42− concentration in the water column (from 10.3 to 36.2 mg/dm3) and the isotopic composition of sulfur (δ34S from 2.1 to 5.4‰) was observed. The main identified sources of SO42− were watercourses, surface runoff, and phosphorus fertilizers.Both oxidized sulfur species (SO42−) and its reduced forms were found in sediments. Particular sulfur forms were characterized by large variations in both, concentrations and the isotopic composition of sulfur. SO42− in the sediment and in the water column had different genesis. Bacterial oxidation of organic sulfur and its binding in SO42− were observed in the sediment. Under reducing conditions, oxidized and organic sulfur is converted to H2S which reacted with Fe or other metallic ions leading to metal sulfide precipitation. Monosulfides were shown to have a very low concentration, ranging up to 0.07 mg/g of sediment. The transformation of elemental sulfur from sulfides through their chemical oxidation occurred in the sediment.  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.
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   

6.
Climate change in the SW USA is likely to involve drier conditions and higher surface temperatures. In order to better understand the evolution of water chemistry and the sources of aqueous SO4 in these semi-arid settings, chemical and S isotope compositions were determined of springs, groundwater, and bedrock associated with a Permian fractured carbonate aquifer located in the southern Sacramento Mountains, New Mexico, USA. The results suggest that the evolution of water chemistry in the semi-arid carbonate aquifer is mainly controlled by dedolomitization of bedrock, which was magnified by increasing temperature and increasing dissolution of gypsum/anhydrite along the groundwater flow path. The δ34S of dissolved SO4 in spring and groundwater samples varied from +9.0‰ to +12.8‰, reflecting the mixing of SO4 from the dissolution of Permian gypsum/anhydrite (+12.3‰ to +13.4‰) and oxidation of sulfide minerals (−24.5‰ to −4.2‰). According to S isotope mass balance constraints, the contribution of sulfide-derived SO4 was considerable in the High Mountain recharge areas, accounting for up to ∼10% of the total SO4 load. However, sulfide weathering decreased in importance in the lower reaches of the watershed. A smaller SO4 input of ∼2–4% was contributed by atmospheric wet deposition. This study implies that the δ34S variation of SO4 in semi-arid environments can be complex, but that S isotopes can be used to distinguish among the different sources of weathering. Here it was found that H2SO4 dissolution due to sulfide oxidation contributes up to 5% of the total carbonate weathering budget, while most of the SO4 is released from bedrock sources during dedolomitization.  相似文献   

7.
《Applied Geochemistry》2003,18(1):25-36
The controls on the internal neutralization of low productivity, highly acidified waters by sulfide accumulation in sediments are yet poorly understood. It is demonstrated that the neutralization process is constrained by organic matter quality and thermodynamic effects which control the relative rates of SO4 and Fe reduction, and the fate of the reduced Fe and S in the sediments. The investigated sediments were rich in dissolved Fe(II) (0.005–12 mmol l−1) and SO4 (1.3–22 mmol l−1). The pH ranged from 3.0 to 6.8. Contents of reduced inorganic S (0.1–9.5%), molar C/N ratios of the organic matter (12–80) and metabolic turnover rates (1–110 μeq cm−3 a−1) varied strongly. Substantial amounts of Fe sulfides were only found at a simultaneous partial thermodynamic and solubility equilibrium of the involved biogeochemical processes. Sulfide oxidation was apparently inhibited, and SO4 and Fe reduction coexisted. In this type of sediment increases in C availability cause enhanced neutralization rates. In the absence of a partial equilibrium, the sediments were in a sulfide oxidizing and Fe reducing state, and did not accumulate Fe sulfides. The latter type of sediment will increase neutralization rates in response to decreasing deposition of reactive Fe oxides but not necessarily in response to increases in lake productivity by e.g. fertilization measures.  相似文献   

8.
The main terminal processes of organic matter mineralization in anoxic Black Sea sediments underlying the sulfidic water column are sulfate reduction in the upper 2-4 m and methanogenesis below the sulfate zone. The modern marine deposits comprise a ca. 1-m-deep layer of coccolith ooze and underlying sapropel, below which sea water ions penetrate deep down into the limnic Pleistocene deposits from >9000 years BP. Sulfate reduction rates have a subsurface maximum at the SO42−-CH4 transition where H2S reaches maximum concentration. Because of an excess of reactive iron in the deep limnic deposits, most of the methane-derived H2S is drawn downward to a sulfidization front where it reacts with Fe(III) and with Fe2+ diffusing up from below. The H2S-Fe2+ transition is marked by a black band of amorphous iron sulfide above which distinct horizons of greigite and pyrite formation occur. The pore water gradients respond dynamically to environmental changes in the Black Sea with relatively short time constants of ca. 500 yr for SO42− and 10 yr for H2S, whereas the FeS in the black band has taken ca. 3000 yr to accumulate. The dual diffusion interfaces of SO42−-CH4 and H2S-Fe2+ cause the trapping of isotopically heavy iron sulfide with δ34S = +15 to +33‰ at the sulfidization front. A diffusion model for sulfur isotopes shows that the SO42− diffusing downward into the SO42−-CH4 transition has an isotopic composition of +19‰, close to the +23‰ of H2S diffusing upward. These isotopic compositions are, however, very different from the porewater SO42− (+43‰) and H2S (−15‰) at the same depth. The model explains how methane-driven sulfate reduction combined with a deep H2S sink leads to isotopically heavy pyrite in a sediment open to diffusion. These results have general implications for the marine sulfur cycle and for the interpretation of sulfur isotopic data in modern sediments and in sedimentary rocks throughout earth’s history.  相似文献   

9.
Acid mine drainage (AMD) is a common pollution in mining areas due to the oxidation of pyrite and associated sulfide minerals at mines, tailings and mine dumps. Elevated metals (Fe, Mn, Al) and metalloids (As, Hg) in AMD would deteriorate the local aquatic environment and influence the water supply. A carbonate basin with deposits of high-arsenic coal in Xingren County, southwestern China, was chosen to study the behavior of As and other chemical constituents along a river receiving AMD. Heavy metals (Fe, Mn) and major ions such as (Ca2+, Mg2+, Cl−, SO4 2−) in surface water, and As in sediment and surface water were analyzed. It was found that high concentrations of SO4 2− (1,324–7,560 mg/L) and Fe (369–1,472 mg/L) in surface water were mainly controlled by the interactions between water and rocks such as the oxidation of pyrite in the local coal seams, precipitation and adsorption of iron minerals. Although ubiquitous carbonate minerals in the bedrock and the riverbeds, low pH (<3) water was maintained until 2 km downstream from the AMD source due to the Fe(hydro)oxide minerals coating on the surface of carbonate minerals to restrain the neutralization of acidic water. Moreover, the formation of Fe(hydro)oxide precipitations absorbed As was dominated the attenuation of As from water to sediment. Whereas, the dilution also played an important role in decrease of As in river water.  相似文献   

10.
Arsenic and Sb are common mine-water pollutants and their toxicity and fate are strongly influenced by redox processes. In this study, simultaneous Fe(II), As(III) and Sb(III) oxidation experiments were conducted to obtain rates under laboratory conditions similar to those found in the field for mine waters of both low and circumneutral pH. Additional experiments were performed under abiotic sterile conditions to determine the biotic and abiotic contributions to the oxidation processes. The results showed that under abiotic conditions in aerated Fe(III)–H2SO4 solutions, Sb(III) oxidizes slightly faster than As(III). The oxidation rates of both elements were accelerated by increasing As(III), Sb(III), Fe(III), and Cl− concentrations in the presence of light. For unfiltered circumneutral water from the Giant Mine (Yellowknife, NWT, Canada), As(III) oxidized at 15–78 μmol/L/h whereas Sb(III) oxidized at 0.03–0.05 μmol/L/h during microbial exponential growth. In contrast, As(III) and Sb(III) oxidation rates of 0.01–0.03 and 0.01–0.02 μmol/L/h, respectively, were obtained in experiments performed with acid unfiltered mine waters from the Iberian Pyritic Belt (SW Spain). These results suggest that the Fe(III) formed from microbial oxidation abiotically oxidized As(III) and Sb(III). After sterile filtration of both mine water samples, neither As(III), Sb(III), nor Fe(II) oxidation was observed. Hence, under the experimental conditions, bacteria were catalyzing As and Sb oxidation in the Giant Mine waters and Fe oxidation in the acid waters of the Iberian Pyrite Belt.  相似文献   

11.
Acid sulfate-chloride thermal water samples collected together with fumarolic gases from various volcanic areas in northeastern Japan were studied chemically and isotogdically. δ34S (COT) values of sulfate and hydrogen sulfide from these volcanic hot springs range from +4.0 to +31 and from ?15.0 to ?2.0% respectively, with δ34Sys value of +2.5 to +31. The δ34S of the sulfate in the more saline waters tends to become smaller with increasing ratio of SO4 to Cl, although the chemical and isotopic composition of acid thermal water within some areas may be altered by secondary processes during the discharge of the thermal waters. This trend can be explained by the reaction of the volcanic gases, having S/Cl of 4 ~ 7 and total sulfur of ~0% in δ34S, with ground water at 200°C, and/or the removal of sulfide phase depleted in 34S from the acid thermal water formed by the disproportionation of volcanic sulfur. The sulfur species in acid sulfate-chloride thermal water are shown to be volcanic exhalations.  相似文献   

12.
《Applied Geochemistry》2004,19(7):995-1009
Published literature on preservation procedures for stabilizing aqueous inorganic As(III/V) redox species contains discrepancies. This study critically evaluates published reports on As redox preservation and explains discrepancies in the literature. Synthetic laboratory preservation experiments and time stability experiments were conducted for natural water samples from several field sites. Any field collection procedure that filters out microorganisms, adds a reagent that prevents dissolved Fe and Mn oxidation and precipitation, and isolates the sample from solar radiation will preserve the As(III/V) ratio. Reagents that prevent Fe and Mn oxidation and precipitation include HCl, H2SO4, and EDTA, although extremely high concentrations of EDTA are necessary for some water samples high in Fe. Photo-catalyzed Fe(III) reduction causes As(III) oxidation; however, storing the sample in the dark prevents photochemical reactions. Furthermore, the presence of Fe(II) or SO4 inhibits the oxidation of As(III) by Fe(III) because of complexation reactions and competing reactions with free radicals. Consequently, fast abiotic As(III) oxidation reactions observed in the laboratory are not observed in natural water samples for one or more of the following reasons: (1) the As redox species have already stabilized, (2) most natural waters contain very low dissolved Fe(III) concentrations, (3) the As(III) oxidation caused by Fe(III) photoreduction is inhibited by Fe(II) or SO4.  相似文献   

13.
The sulfur cycle of Mariager Fjord was studied by following the pool of sulfide in the anoxic water and its isotopic composition during a period of 3 yr. Though most of the sulfide accumulating in the fjord was formed in the sediment, the isotopic composition of sulfide in the water was different from the isotopic composition of sulfide diffusing into the water from the sediment. The mean isotopic composition of the water column sulfide (δ34S) varied during the year between −13‰ and −21‰ with the most negative values reached during winter/early spring, while the sulfide diffusing into the water from the sediment had a mean isotope composition of −11.3‰. This annual pattern suggested that processes in the oxidative part of the sulfur cycle were responsible for the excess fractionation, and mass-balance considerations indicated that the excess fractionation of the sulfur isotopes could be accounted for by disproportionation of S0 or S2O32− in the water column, but not by water column sulfate reduction or sulfide oxidation alone. MPN counts demonstrated that a population of more than 3 × 104 cells mL−1 capable of growing by disproportionation of these two substrates was present in all depths of the fjord. The results presented in this communication demonstrate that the isotopic depletion of sulfide in anoxic systems may vary between periods of net sulfate reduction versus periods of net sulfide oxidation and indicate that disproportionation of sulfur compounds may be an important step in the sulfur cycle of euxinic basins.  相似文献   

14.
Hydrochemical data were gathered throughout the last 12 years from 57 sampling stations in the drainage basin of the Sarcheshmeh copper mine, Kerman Province, Iran. The mean values of these data for each sampling station were used to evaluate water quality and to determine processes that control water chemistry. Principal component analyses specified the oxidation of sulfide minerals, dissolution of carbonate and sulfate minerals and weathering of silicate minerals as the principal processes responsible for the chemical composition of water in the study area. Q-mode cluster analysis revealed three main water groups. The first group had a Ca-HCO3–SO4 composition whereas the second and third groups had Ca–SO4 and Ca–Mg–SO4 composition, respectively. The results of this study clearly indicated the role of sulfide minerals oxidation and the buffering processes in the geochemical evolution of water in the Sarcheshmeh area. Due to these processes, extensive changes occurred in the chemical composition of water by passage through the mining area or waste and low-grade dumps, so that the fresh water of the peripheral area of the pit evolved to an acid water rich in sulfate and heavy metals at the outlet of the pit and in the seepages of waste and low-grade dumps.  相似文献   

15.
Data on the decommissioned Degtyarka Cu sulfide deposit, Urals, confirm the hypothesis that the flooding of abandoned mine workings is associated with the synthesis of secondary sulfates. Numerical simulation of hydrogeochemical processes in the rock—water system imitating the flooding of an underground void makes it possible to evaluate the conditions under which kirovite (Fe,Mg)SO4 · 7H2O and melanterite are formed at the oxidation of ore sulfides. Secondary sulfates are formed when the redox potential of the system is transformed from reducing to oxidizing within the stability field of Fe(II) species. The Fe/Mg ratio of the kirovite (Fe,Mg)SO4 · 7H2O is controlled first of all by the percentage of sulfides in the rock—water system, the rock/water ratio, the openness of the system with respect to atmospheric gases, and the temperature.  相似文献   

16.
We have determined the extent of Se isotope fractionation induced by reduction of selenate by sulfate interlayered green rust (GRSO4), a Fe(II)-Fe(III) hydroxide-sulfate. This compound is known to reduce selenate to Se(0), and it is the only naturally relevant abiotic selenate reduction pathway documented to date. Se reduction reactions, when they occur in nature, greatly reduce Se mobility and bioavailability. Se stable isotope analysis shows promise as an indicator of Se reduction, and Se isotope fractionation by various Se reactions must be known in order to refine this tool. We measured the increase in the 80Se/76Se ratio of dissolved selenate as lighter isotopes were preferentially consumed during reduction by GRSO4. Six different experiments that used GRSO4 made by two methods, with varying solution compositions and pH, yielded identical isotopic fractionations. Regression of all the data yielded an instantaneous isotope fractionation of 7.36 ± 0.24‰. Selenate reduction by GRSO4 induces much greater isotopic fractionation than does bacterial selenate reduction. If selenate reduction by GRSO4 occurs in nature, it may be identifiable on the basis of its relatively large isotopic fractionation.  相似文献   

17.
Laboratory experiments were conducted to simulate chalcopyrite oxidation under anaerobic and aerobic conditions in the absence or presence of the bacterium Acidithiobacillus ferrooxidans. Experiments were carried out with 3 different oxygen isotope values of water (δ18OH2O) so that approach to equilibrium or steady-state isotope fractionation for different starting conditions could be evaluated. The contribution of dissolved O2 and water-derived oxygen to dissolved sulfate formed by chalcopyrite oxidation was unambiguously resolved during the aerobic experiments. Aerobic oxidation of chalcopyrite showed 93 ± 1% incorporation of water oxygen into the resulting sulfate during the biological experiments. Anaerobic experiments showed similar percentages of water oxygen incorporation into sulfate, but were more variable. The experiments also allowed determination of sulfate–water oxygen isotope fractionation, ε18OSO4–H2O, of ~ 3.8‰ for the anaerobic experiments. Aerobic oxidation produced apparent εSO4–H2O values (6.4‰) higher than the anaerobic experiments, possibly due to additional incorporation of dissolved O2 into sulfate. δ34SSO4 values are ~ 4‰ lower than the parent sulfide mineral during anaerobic oxidation of chalcopyrite, with no significant difference between abiotic and biological processes. For the aerobic experiments, a small depletion in δ34SSO4 of ~? 1.5 ± 0.2‰ was observed for the biological experiments. Fewer solids precipitated during oxidation under aerobic conditions than under anaerobic conditions, which may account for the observed differences in sulfur isotope fractionation under these contrasting conditions.  相似文献   

18.
The oxidation of sulfide minerals generates acidic waters containing high levels of SO4 and Fe. The study area has active Pb?CZn?CCu mining. It is thought that the surface/subsurface/underground sulfide minerals in the region generally contribute to the acidification of groundwater. Low pH values are also responsible for dissolved metals (Al, Fe, Mn, SO4, Pb, Zn) in the groundwater and river. Furthermore, current mining wastes have affected concentrations of trace elements in the water. High Fe and Mn concentrations are generally found in the spring which has acidic and low Eh values, while Al, Fe and Mn concentrations in the acidic waters show notable increases with the maximum values reaching 8,829, 19,084 and 1,708?ppb, respectively. These values exceed the Turkish drinking water standard of 200, 200 and 50?ppb, respectively.  相似文献   

19.
Previous geochemical and microbiological studies in the Cariaco Basin indicate intense elemental cycling and a dynamic microbial loop near the oxic-anoxic interface. We obtained detailed distributions of sulfur isotopes of total dissolved sulfide and sulfate as part of the on-going CARIACO time series project to explore the critical pathways at the level of individual sulfur species. Isotopic patterns of sulfate (δ34SSO4) and sulfide (δ34SH2S) were similar to trends observed in the Black Sea water column: δ34SH2S and δ34SSO4 were constant in the deep anoxic water (varying within 0.6‰ for sulfide and 0.3‰ for sulfate), with sulfide roughly 54‰ depleted in 34S relative to sulfate. Near the oxic-anoxic interface, however, the δ34SH2S value was ∼3‰ heavier than that in the deep water, which may reflect sulfide oxidation and/or a change in fractionation during in situ sulfide production through sulfate reduction (SR). δ34SH2S and Δ33SH2S data near the oxic-anoxic interface did not provide unequivocal evidence to support the important role of sulfur-intermediate disproportionation suggested by previous studies. Repeated observation of minimum δ34SSO4 values near the interface suggests ‘readdition’ of 34S-depleted sulfate during sulfide oxidation. A slight increase in δ34SSO4 values with depth extended over the water column may indicate a reservoir effect associated with removal of 34S-depleted sulfur during sulfide production through SR. Our δ34SH2S and Δ33SH2S data also do not show a clear role for sulfur-intermediate disproportionation in the deep anoxic water column. We interpret the large difference in δ34S between sulfate and sulfide as reflecting fractionations during SR in the Cariaco deep waters that are larger than those generally observed in culturing studies.  相似文献   

20.
《Applied Geochemistry》2004,19(3):343-358
Ion-exchange batch experiments were run on Cretaceous (Magothy aquifer) clay cores from a nearshore borehole and an inland borehole on Long Island, NY, to determine the origin of high SO42− concentrations in ground water. Desorption batch tests indicate that the amounts of SO42− released from the core samples are much greater (980–4700 μg/g of sediment) than the concentrations in ground-water samples. The locally high SO42− concentrations in pore water extracted from cores are consistent with the overall increase in SO42− concentrations in ground water along Magothy flow paths. Results of the sorption batch tests indicate that SO42− sorption onto clay is small but significant (40–120 μg/g of sediment) in the low-pH (<5) pore water of clays, and a significant part of the SO42− in Magothy pore water may result from the oxidation of FeS2 by dissolved Fe(III). The acidic conditions that result from FeS2 oxidation in acidic pore water should result in greater sorption of SO42− and other anions onto protonated surfaces than in neutral-pH pore water. Comparison of the amounts of Cl− released from a clay core sample in desorption batch tests (4 μg/g of sediment) with the amounts of Cl− sorbed to the same clay in sorption tests (3.7–5 μg/g) indicates that the high concentrations of Cl− in pore water did not originate from connate seawater but were desorbed from sediment that was previously in contact with seawater. Furthermore, a hypothetical seawater transgression in the past is consistent with the observed pattern of sorbed cation complexes in the Magothy cores and could be a significant source of high SO42− concentrations in Magothy ground water.  相似文献   

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