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1.
Jarosite [KFe3(SO4)2(OH)6] is a mineral that is common in acidic, sulphate-rich environments, such as acid sulphate soils derived from pyrite-bearing sediments, weathering zones of sulphide ore deposits and acid mine or acid rock drainage (ARD/AMD) sites. The structure of jarosite is based on linear tetrahedral-octahedral-tetrahedral (T-O-T) sheets, made up from slightly distorted FeO6 octahedra and SO4 tetrahedra. Batch dissolution experiments carried out on synthetic jarosite at pH 2, to mimic environments affected by ARD/AMD, and at pH 8, to simulate ARD/AMD environments recently remediated with slaked lime (Ca(OH)2), suggest first order dissolution kinetics. Both dissolution reactions are incongruent, as revealed by non-ideal dissolution of the parent solids and, in the case of the pH 8 dissolution, because a secondary goethite precipitate forms on the surface of the dissolving jarosite grains. The pH 2 dissolution yields only aqueous K, Fe, and SO4. Aqueous, residual solid, and computational modelling of the jarosite structure and surfaces using the GULP and MARVIN codes, respectively, show for the first time that there is selective dissolution of the A- and T-sites, which contain K and SO4, respectively, relative to Fe, which is located deep within the T-O-T jarosite structure. These results have implications for the chemistry of ARD/AMD waters, and for understanding reaction pathways of ARD/AMD mineral dissolution.  相似文献   

2.
The net result of acid-generating and-neutralizing reactions within mining wastes is termed acid rock drainage (ARD). The oxidation of sulfide minerals is the major contributor to acid generation. Dissolution and alteration of various minerals can contribute to the neutralization of acid. Definitions of alkalinity, acidity, and buffer capacity are reviewed, and a detailed discussion of the dissolution and neutralizing capacity of carbonate and silicate minerals related to equilibium conditions, dissolution mechanism, and kinetics is provided. Factors that determine neutralization rate by carbonate and silicate minerals include: pH, PCO 2, equilibrium conditions, temperature, mineral composition and structure, redox conditions, and the presence of foreign ions. Similar factors affect sulfide oxidation. Comparison of rates shows sulfides react fastest, followed by carbonates and silicates. The differences in the reaction mechanisms and kinetics of neutralization have important implications in the prediction, control, and regulation of ARD. Current static and kinetic prediction methods upon which mine permitting, ARD control, and mine closure plans are based do not consider sample mineralogy or the kinetics of the acid-generating and-neutralizing reactions. Erroneous test interpretations and predictions can result. The importance of considering mineralogy for site-specific interpretation is highlighted. Uncertainty in prediction leads to difficulties for the mine operator in developing satisfactory and cost-effective control and remediation measures. Thus, the application of regulations and guidelines for waste management planning need to beflexible.  相似文献   

3.
Acid mine/rock drainage (AMD/ARD) is the biggest environmental threat facing the mining industry. This study investigates AMD/ARD possibilities in three mines in the Ashanti Belt, using acid base accounting (ABA) and net acid generation pH (NAGpH) tests. Twenty-eight samples of rock units and mine spoil from these mines were collected for ABA and NAGpH tests. Two tailing dumps at Prestea and Nsuta were confirmed by both methods as acid generating with NAGpH of 4.5 and 4.6 and neutralization potential ratio values of 4.38 and 4.60, respectively. Six other samples are classified as potentially acid generating using a variety of established classification criteria. The rest of the samples either exhibited very low sulphur and carbonate content or had excess carbonate over sulphur. Consistency between results from ABA and NAGpH tests validates these tests as adequate tools for preliminary evaluation of AMD/ARD possibilities in any mining project in the Ashanti Belt.  相似文献   

4.
《Applied Geochemistry》2005,20(10):1941-1964
The pH, alkalinity, and acidity of mine drainage and associated waters can be misinterpreted because of the chemical instability of samples and possible misunderstandings of standard analytical method results. Synthetic and field samples of mine drainage having various initial pH values and concentrations of dissolved metals and alkalinity were titrated by several methods, and the results were compared to alkalinity and acidity calculated based on dissolved solutes. The pH, alkalinity, and acidity were compared between fresh, unoxidized and aged, oxidized samples.Data for Pennsylvania coal mine drainage indicates that the pH of fresh samples was predominantly acidic (pH 2.5–4) or near neutral (pH 6–7);  25% of the samples had pH values between 5 and 6. Following oxidation, no samples had pH values between 5 and 6.The Standard Method Alkalinity titration is constrained to yield values >0. Most calculated and measured alkalinities for samples with positive alkalinities were in close agreement. However, for low-pH samples, the calculated alkalinity can be negative due to negative contributions by dissolved metals that may oxidize and hydrolyze.The Standard Method hot peroxide treatment titration for acidity determination (Hot Acidity) accurately indicates the potential for pH to decrease to acidic values after complete degassing of CO2 and oxidation of Fe and Mn, and it indicates either the excess alkalinity or that required for neutralization of the sample. The Hot Acidity directly measures net acidity (= −net alkalinity). Samples that had near-neutral pH after oxidation had negative Hot Acidity; samples that had pH < 6.3 after oxidation had positive Hot Acidity. Samples with similar pH values before oxidation had dissimilar Hot Acidities due to variations in their alkalinities and dissolved Fe, Mn, and Al concentrations. Hot Acidity was approximately equal to net acidity calculated based on initial pH and dissolved concentrations of Fe, Mn, and Al minus the initial alkalinity. Acidity calculated from the pH and dissolved metals concentrations, assuming equivalents of 2 per mole of Fe and Mn and 3 per mole of Al, was equivalent to that calculated based on complete aqueous speciation of FeII/FeIII. Despite changes in the pH, alkalinity, and metals concentrations, the Hot Acidities were comparable for fresh and most aged samples.A meaningful “net” acidity can be determined from a measured Hot Acidity or by calculation from the pH, alkalinity, and dissolved metals concentrations. The use of net alkalinity = (Alkalinitymeasured  Hot Aciditymeasured) to design mine drainage treatment can lead to systems with insufficient Alkalinity to neutralize metal and H+ acidity and is not recommended. The use of net alkalinity = −Hot Acidity titration is recommended for the planning of mine drainage treatment. The use of net alkalinity = (Alkalinitymeasured  Aciditycalculated) is recommended with some cautions.  相似文献   

5.
Many waters sampled in Yellowstone National Park, both high-temperature (30–94 °C) and low-temperature (0–30 °C), are acid–sulfate type with pH values of 1–5. Sulfuric acid is the dominant component, especially as pH values decrease below 3, and it forms from the oxidation of elemental S whose origin is H2S in hot gases derived from boiling of hydrothermal waters at depth. Four determinations of pH were obtained: (1) field pH at field temperature, (2) laboratory pH at laboratory temperature, (3) pH based on acidity titration, and (4) pH based on charge imbalance (at both laboratory and field temperatures). Laboratory pH, charge imbalance pH (at laboratory temperature), and acidity pH were in close agreement for pH < 2.7. Field pH measurements were predominantly used because the charge imbalance was <±10%. When the charge imbalance was generally >±10%, a selection process was used to compare acidity, laboratory, and charge balance pH to arrive at the best estimate. Differences between laboratory and field pH can be explained based on Fe oxidation, H2S or S2O3 oxidation, CO2 degassing, and the temperature-dependence of pK2 for H2SO4. Charge imbalances are shown to be dependent on a speciation model for pH values <3. The highest SO4 concentrations, in the thousands of mg/L, result from evaporative concentration at elevated temperatures as shown by the consistently high δ18O values (−10‰ to −3‰) and a δD vs. δ18O slope of 3, reflecting kinetic fractionation. Low SO4 concentrations (<100 mg/L) for thermal waters (>350 mg/L Cl) decrease as the Cl concentration increases from boiling which appears inconsistent with the hypothesis of H2S oxidation as a source of hydrothermal SO4. This trend is consistent with the alternate hypothesis of anhydrite solubility equilibrium. Acid–sulfate water analyses are occasionally high in As, Hg, and NH3 concentrations but in contrast to acid mine waters they are low to below detection in Cu, Zn, Cd, and Pb concentrations. Even concentrations of SO4, Fe, and Al are much lower in thermal waters than acid mine waters of the same pH. This difference in water chemistry may explain why certain species of fly larvae live comfortably in Yellowstone’s acid waters but have not been observed in acid rock drainage of the same pH.  相似文献   

6.
 Oxygen-18 (18O) and deuterium (D, or 2H) are routinely used in hydrologic, climatologic and geothermal studies. In hydrology, stable isotopes provide information on the type and topology (altitude and latitude) of the recharge waters and the historical effects on water, related to such physical processes as evaporation (in ponds), melting (of snow or ice), condensation, evapotranspiration and mixing. In geothermal studies, stable isotopes provide key information related to recharge and the various temperature-dependent water/rock isotope exchange reactions. The latter is assessed through the oxygen shift in the 18O/D correlation. At acid rock drainage (ARD) sites, water/rock interactions are primarily controlled by pH and oxidation potential. Using the isotopic characteristics of the rocks and the recharge waters as a basis, the relative oxygen shift of the ARD effluent can provide information on: (1) the residence time, (2) the rate of water/rock reactions, and (3) the actual pH at the rock/water interface. This paper offers a methodology for conducting oxygen and hydrogen isotope studies related to ARD and other mineral effluent problems. The methodology is based on: (1) comprehensive sampling of regional waters, ARD effluent and major contributing minerals and rocks, (2) isotopic and elemental analysis, and (3) data interpretation on the basis of a zero-dimensional (mass balance), multi-component mixing model. Received: 15 January 1999 · Accepted: 3 May 1999  相似文献   

7.
An ideal engineered soil cover can mitigate acid rock drainage (ARD) by limiting water and gaseous O2 ingress into an underlying waste rock pile. However, the barrier layer in the soil cover almost invariably tends to develop cracks or fractures after placement. These cracks may change water flow and O2 transport in the soil cover and decrease performance in the long run. The present study employed a 10-cm-wide sand-filled channel installed in a soil barrier layer (silty clay) to model the aggregate of cracks or fractures that may be present in the cover. The soil cover had a slope of 20%. Oxygen transport through the soil cover and oxidation of the underlying waste rock were investigated and compared to a controlled column test with bare waste rock (without soil cover). Moreover, gaseous O2 transport in the soil cover with channel and its sensitivity to channel location as well as the influence of the saturated hydraulic conductivity of the channel material were modeled using the commercial software VADOSE/W. The results indicted that the waste rock underlying the soil cover with channel had a lower oxidation rate than the waste rock without cover because of reduced O2 ingress and water flushing in the soil cover with channel, which meant a partial soil cover might still be effective to some extent in reducing ARD generation. Gaseous O2 ingress into the covered waste rock was more sensitive to the channel location than to the saturated hydraulic conductivity of the material filling the channel. Aqueous equilibrium speciation modeling and scanning electron microscopy with energy dispersive X-ray analysis indicated that secondary minerals formed as a result of the oxidation of the waste rock included gypsum and goethite in the covered waste rock and schwertmannite and other Fe oxides in the uncovered waste rock. The findings of the study provided insight into the effect of channel flow on O2 transport and oxidation of the covered waste rock, which may help to improve soil cover design and construction to minimise the generation of preferential flow in the barrier layer.  相似文献   

8.
Acid mine drainage predictive testwork associated with the Australian Mineral Industries Research Association (AMIRA) P387A Project: Prediction and Kinetic Control of Acid Mine Drainage (AMD) has critically examined static acid assessment and kinetic information from acid–base accounting techniques, including net acid production potential (NAPP), net acid generation (NAG) and column leach tests. This paper compares results on two waste rock samples that were obtained from the Kaltim Prima Coal mine (KPC) containing significant quantities of fine-grained framboidal pyrite. In agreement with other research, the authors' results indicated that framboidal pyrite is more reactive than euhedral forms due to the greater specific surface area of framboidal pyrite. This is evidenced by optical microscopy of reacted samples. Importantly, the results showed that NAPP testing is biased by the rapid acid generating oxidation of framboidal pyrite prior to, and during the acid neutralisation capacity (ANC) test. This can result in negative ANC values for samples containing significant framboidal pyrite (often “corrected” to zero kg H2SO4/t) when significant ANC is actually present in the sample. NAG testing using H2O2 indicated that samples containing a significant quantity of framboidal pyrite can result in the catalytic decomposition of the H2O2 prior to complete oxidation of the sulfide minerals present, requiring sequential addition of H2O2 for completion. A benefit of the NAG test, however, is that it assesses the net acid generation capacity of the sample without bias towards acid generation as is observed using NAPP methods. The kinetic NAG test also gives information on the reaction sequence of framboidal and euhedral pyrite. Periodic (kinetic) analysis of sub-samples from column leach tests indicated rapid oxidation of the framboidal pyrite compared to the euhedral pyrite, which was correlated with the greater framboidal pyrite surface area.Calculations to determine the sulfide/sulfate acidity derived from the oxidation of framboidal pyrite prior to; and during the ANC test have been developed to provide a better indication of the actual ANC (ANCActual) of the sample. Paste pH values of <pH 4–5 may be one suitable trigger mechanism for the implementation of this new method. This has led to an improved NAPP estimation of total acid production. Together with NAG and column leach testing this improved methodology has resulted in accurate AMD characterisation of samples containing acidic oxidation products and framboidal pyrite.  相似文献   

9.
《Applied Geochemistry》2002,17(8):987-1001
Surface (0–10 cm) samples of 7 soils from tropical coastal Queensland were incubated at room temperature and at field capacity with finely ground (<150 μ) basalt rock for 3 months. The amendment was applied at 0, 1, 5, 25 and 50 t/ha to cover situations of moderate application rates to that where the amendment might be banded to produce high local concentrations. Having an abrasion pH of about 9, the amendment was able to reduce both active acidity (as estimated by an increase in soil pH) and reserve acidity (reduction in % Al saturation of the CEC). Increases in soil pH resulted in increased CEC, depending on the variable charge nature of each soil, accompanied by increases in exchangeable Ca, Mg, and K supplied by the basalt. The amounts of basic cations converted to exchangeable form constituted only a fraction of the amounts applied. Thus the cations held in reserve ensure that the effect of cation enrichment will be prolonged. In some soils phosphate sorption was significantly reduced by crushed basalt application. Furthermore, ‘available’ P as measured by extraction with 0.005 M H2SO4 was increased. These effects appear to be due to the release of silicate from the basalt as well as modest amounts of phosphate in the rock. Three extractants commonly used for estimating Si availability in sugarcane production indicated that all 7 soils contained sub-optimal levels of the element. Application of crushed basalt rock increased extractable Si levels above what is considered sufficient for this crop. The incubated soils were placed in columns and leached with the equivalent of 2750-mm (average wet season) rainfall. Re-analysis showed that the favourable chemical soil properties imparted by the amendment were retained. These results add further support to the contention that the effects of amelioration will continue for some time.  相似文献   

10.
金属硫化物矿山的废石堆场受降水淋滤影响而发生硫化物氧化,产生硫酸并释放重金属,因此采矿工程产生的废石是水污染不可忽视的来源。前人关于金属硫化矿物氧化的机理研究大多集中在单一矿物的室内实验,与野外情况匹配度较低。本研究从岩样(矿石和废石)、水样(河水、地下水、废弃尾矿库渗滤液)的水化学、微量元素和锶同位素等方面,分析某铅锌矿废石堆场对水环境的影响,并讨论其产生的化学组分在野外环境中的变化规律及机理。研究结果显示,金属硫化物氧化造成了河水酸化,pH低至2.38,SO42-高达9421 mg·L-1,同时微量元素中Zn、Pb、Ni、Mn、Cd质量浓度远超饮用水限值,如Zn达到了582 mg·L-1(饮用水限值为1 mg·L-1),且浓度与pH负相关。河水酸化的主因是黄铁矿、磁黄铁矿的氧化作用,并贡献了河水中大部分的SO42-。闪锌矿等矿物在贡献了河水中少部分SO42-的同时,也是重金属元素的主要来源。地下水离子浓度较河水低,pH在中性左右。虽然主要是受到侧向山体地下水补给稀释,但碳酸盐和硅酸盐对酸起到的中和作用对酸性水的治理有很大启示价值。以上机理的认识对于废石对水土环境污染的防治具有重要意义。  相似文献   

11.
 Leaching of two contrasting types of sulphidic tailings in humidity cells has been performed. The release of heavy metals and the oxidation rate have been studied. Tailings from the Laver mine contain a few percent sulphides and lack carbonates, whereas tailings from the Stekenjokk mine are both sulphide- and carbonate-rich. The results showed that in the leachates from the Laver samples, the metal concentrations increased and pH decreased with time, indicating an increased oxidation rate. In the Stekenjokk samples, pH remained high during the experiment, thereby keeping the metal concentrations low in the leachates. The oxidation rate also decreased with time, probably due to Fe-hydroxide coatings on sulphide surfaces. The results show that addition of carbonates and the maintenance of a high pH not only reduce the solubility of heavy metals, but also decrease the oxidation rate of sulphides. Received: 20 January 1998 · Accepted: 2 April 1998  相似文献   

12.
Groundwater down-gradient from a mine rock dump in Dalarna, Sweden was sampled from the onset of snowmelt runoff (April) until October in order to investigate seasonal variations in groundwater composition. The results demonstrate that considerable variation in solute concentration (Al, Cu, Fe, SO42−, Zn) and acidity occurs in groundwater; the greatest change in solute concentrations occurs during the melting of the snow cover, when sulfide oxidation products are flushed from the rock dump. During this period, groundwater flow is concentrated near the soil surface with an estimated velocity of 1 m/day. Groundwater acidity varied by a factor of four closest to the rock dump during the sampling period, but these variations were attenuated with distance from the rock dump. Over a distance of 145 m, groundwater pH increases from 2.5 to 4.0 and acidity decreases from 3–13 to 0.8–1.1 meq/L, which is the combined effect of ferric iron precipitation and aluminosilicate weathering. As a result of flushing from the upper soil horizons, peaks in total organic carbon and ammonium concentrations in groundwater are observed at the end of snowmelt. In soils impacted by acidic surface runoff, the sequential extraction of C horizon soils indicates the accumulation of Cu in well-crystallized iron oxyhydroxides in the upper C horizon, while Cu, Fe, Ni and Zn accumulate in a well-crystallized iron oxyhydroxide hardpan that has formed 2.5m below the ground surface. Surface complexation modeling demonstrates that SO42− and Cu adsorb to the abundant iron oxyhydroxides at pH < 4, while Zn adsorption in this pH range is minimal.  相似文献   

13.
The ability to properly manage the oxidation of pyritic minerals and associated acid mine drainage is dependent upon understanding the chemistry of the disposal environment. One accepted disposal method is placing pyritic-containing materials in the groundwater environment. The objective of this study was to examine solubility relationships of Al and Fe minerals associated with pyritic waste disposed in a low leaching aerobic saturated environment. Two eastern oil shales were used in this oxidizing equilibration study, a New Albany Shale (unweathered, 4.6 percent pyrite), and a Chattanooga Shale (weathered, 1.5 percent pyrite). Oil shale samples were equilibrated with distilled-deionized water from 1 to 180 d with a 1∶1 solid-to-solution ratio. The suspensions were filtered and the clear filtrates were analyzed for total cations and anions. Ion activities were calculated from total concentrations. Below pH 6.0, depending upon SO 4 2− activity, Al3+ solubility was controlled by AlOHSO4 (solid phase) for both shales. Initially, Al3+ solubility for the New Albany Shale showed equilibrium with amorphous Al(OH)3. The pH decreased with time, and Al3+ solubility approached equilibrium with AlOHSO4(s). Below pH 6.0, Fe3+ solubility appeared to be regulated by a basic iron sulfate solid phase with the stoichiometric composition of FeOHSO4(s). The results of this study indicate that below pH 6.0, Al3+ solubilities, are limited by basic Al and Fe sulfate solid phases (AlOHSO4(s) and FeHSO4(s)). The results from this study further indicate that the acidity in oil shale waters is produced from the hydrolysis of Al3+ and Fe3+ activities in solution. These results indicate a fundamental change in the stoichiometric equations used to predict acidity from iron sulfide oxidation. The results of this study also indicate that water quality predictions associated with acid mine drainage can be based on fundamental thermodynamic relationships. As a result, waste management decisions can be based on waste-specific/site-specific test methods.  相似文献   

14.
Lead- and Pb-As-jarosites are minerals common to acidic, sulphate-rich environments, including weathering zones of sulphide ore deposits and acid rock or acid mine drainage (ARD/AMD) sites, and often form on or near galena. The structures of these jarosites are based on linear tetrahedral-octahedral-tetrahedral (T-O-T) sheets, comprised of slightly distorted FeO6 octahedra and SO42− (-AsO43− in Pb-As-jarosites) tetrahedra. To better understand the dissolution mechanisms and products of the break down of Pb- and Pb-As-jarosite, preliminary batch dissolution experiments were conducted on synthetic Pb- and Pb-As-jarosite at pH 2 and 20 °C, to mimic environments affected by ARD/AMD, and at pH 8 and 20 °C, to simulate ARD/AMD environments recently remediated with slaked lime (Ca(OH)2). All four dissolutions are incongruent. Dissolution of Pb-jarosite at pH 2 yields aqueous Pb, Fe and SO42−. The pH 8 Pb-jarosite dissolution yields aqueous Pb, SO42− and poorly crystalline Fe(OH)3, which does not appear to resorb Pb or SO42−, possibly due to the low solution pH (3.44-3.54) at the end of the experiment. The pH 2 and 8 dissolutions of Pb-As-jarosite result in the formation of secondary compounds (poorly crystalline PbSO4 for pH 2 dissolution; poorly crystalline PbSO4 and Fe(OH)3 for pH 8 dissolution), which may act as dissolution inhibitors after 250 to 300 h of dissolution. In the pH 2 dissolution, aqueous Fe, SO42− and AsO43− also form, and in the pH 8 dissolution, Fe(OH)3 precipitates then subsequently resorbs aqueous AsO43−. The dissolutions probably proceed by preferred dissolution of the A- and T-sites, which contain Pb, and SO42− and AsO43−, respectively, rather than Fe, which is sterically remote, within the T-O-T Pb- and Pb-As-jarosite structures. These data provide the foundation necessary for further, more detailed investigations into the dissolution of Pb- and Pb-As-jarosites.  相似文献   

15.
《Applied Geochemistry》2002,17(5):633-648
Acid rock drainage (ARD) solution from an abandoned ore mine (pH 2.7, SO2−4 concentration 411 mmol/l, Fe concentration 93.5 mmol/l) was investigated by photon correlation spectroscopy, centrifugation, filtration, ultrafiltration, scanning electron microscopy, ICP–MS, AAS, ion chromatography, TOC analysis, and extended X-ray absorption fine structure (EXAFS) spectroscopy. A colloid concentration of ⩾1 g/l was found. The prevailing particle size was <5 nm. Iron, As and Pb were the metal constituents of the colloidal particles. The most probable mineralogical composition of the particles is a mixture of hydronium jarosite and schwertmannite. A small amount of a relatively coarse precipitate was formed in the ARD solution during the months after sampling. The colloid particles are obviously an intermediate in the precipitate formation process. The results suggest that the arsenate is bound to the colloids by the formation of a bidentate binuclear inner-sphere surface complex. However, the transformation of the colloidal material to the more aggregated long-term precipitate results in the incorporation of the arsenate into the interior of the Fe hydroxy sulfate crystal structures. Lead seems to occur as anglesite.  相似文献   

16.
Oxidation of sulfides at the Leona Heights Sulfur Mine has resulted in the liberation of acid, SO4 and metals to Leona Creek. Previous research at the site has indicated Fe(II) oxidation at rates faster than would be predicted by abiotic oxidation alone, particularly in the segment of stream between the Adit and Leona Street sample stations. In order to assess the mechanisms responsible for sulfide oxidation, samples were collected for isotopic analysis of water and SO4, the results of which were used to develop a stoichiometric isotope-balance model. This exercise indicated that the percentage of water-derived oxygen in SO4 increased spatially from between 56% and 64% at the Adit to between 71% and 72% at Leona Street, illustrating that increased sulfide oxidation via Fe(III) was occurring within, or as water flows over, the waste rock, relative to water emanating directly from the former mine. The incorporation of water-derived oxygen in SO4 during pyrite oxidation is a process controlled by Fe oxidizing bacteria such as A. ferrooxidans at low pH. The role of bacteria was further supported by estimates of the rate constant for Fe oxidation between sampling stations, yielding values that were approximately 106 faster than abiotic Fe oxidation alone. Stable isotopic analysis of water further indicates a close correlation of adit spring water to the local meteoric water line, while 3H data indicate a groundwater apparent age, or time of travel from its primary zone of recharge, of <5–18 a. Additionally, the δ34S data, in conjunction with reported albitized feldspars within the Leona Rhyolite host rock, indicate a magmatic origin of ore sulfur, contrary to previous interpretations at the site.  相似文献   

17.
At the Kristineberg mine, northern Sweden, sulphidic mine tailings were remediated in an 8-year pilot-scale experiment using sewage sludge to evaluate its applicability as a sealing layer in a composite dry cover. Sediment, leachate water, and pore gas geochemistry were collected in the aim of determining if the sludge was an effective barrier material to mitigate acid rock drainage (ARD) formation. The sludge was an effective barrier to oxygen influx as it formed both a physical obstruction and functioned as an organic reactive barrier to prevent oxygen to the underlying tailings. Sulphide oxidation and consequential ARD formation did not occur. Sludge-borne trace elements accumulated in a reductive, alkaline environment in the underlying tailings, resulting in an effluent drainage geochemistry of Cd, Cu, Pb and Zn below 10 μg/L, high alkalinity (810 mg/L) and low sulphate (38 mg/L). In contrast, the uncovered reference tailings received a 0.35-m deep oxidation front and typical ARD, with dissolved concentrations of Cd, Zn and sulphate, 20.8 μg/L, 16,100 μg/L and 1,390 mg/L, respectively. Organic matter degradation in the sludge may be a limiting factor to the function of the sealing layer over time as 85 % loss of the organic fraction occurred over the 8-year experimental period due to aerobic and anaerobic degradation. Though the cover may function in the short to medium term (100 years), it is unlikely to meet the demands of a long-term remedial solution.  相似文献   

18.
《Applied Geochemistry》2004,19(11):1837-1853
Iron monosulfide formation and oxidation processes were studied in the extensively drained acid sulfate soil environment of the Tweed River floodplain in eastern Australia. Porewater profiles of pH, Eh, SO42−, Fe2+, Fe3+, Cl, HCO3, and metals (Cd, Co, Cr, Cu, Ni, Pb and Zn) were obtained using in situ dialysis membrane samplers (`peepers'). Concentrations of acid volatile S (AVS), pyrite, total S, reactive Fe, total and organic C, simultaneously extracted metals (SEMs) and total elemental composition by X-ray fluorescence, were determined on sediment samples. The oxidation of pyrite in the surrounding landscape provides a source of acidity, Fe, Al, SO4 and metals, which are exported into the drainage system where they accumulate in the sediments and porewaters. Negative porewater concentration gradients of SO42− and Fe2+, and large AVS concentrations in the sediments, indicate Fe monosulfides form rapidly under reducing conditions and consume acidity and metals. Oxidation of the sediments during previous drought episodes has resulted in the conversion of monosulfides and pyrite to oxidised Fe minerals and the release of acidity, SO42−, Fe3+, and metals to the surface waters. These formation and oxidation cycles show that Fe monosulfides play an important role in controlling water quality in the drainage system.  相似文献   

19.
《Applied Geochemistry》2004,19(7):1075-1084
The biogeochemical cycling of Fe in acid rock drainage (ARD) streams has presented ongoing challenges to reactive solute transport modeling. Previous studies have relied on the pH-dependent solubility of Fe oxides as the main control of the mid-day Fe(II) maxima concentration in ARD streams. In this study, the authors assess the potential for Fe(II)-oxidizing reactions, including the Fenton and microbial oxidation reactions, to constrain the mid-day Fe(II) maxima concentration. At mid-day, pseudo-equilibrium between Fe(II) oxidizing reactions and photoreduction was assumed in order to evaluate the observed Fe(II) maxima and develop an equation to represent this steady state scenario. This steady state condition is assumed only while light intensity, reactivity of oxides and dissolved organic matter (DOM), and microbial populations remain approximately constant. Three Rocky Mountain ARD streams with known values for Fe(II) were evaluated and average photoreduction rates ranging from 5.56×10−4 to 1.39×10−3 μM/s were found during mid-day steady state Fe(II) maxima. Application of Fe redox biogeochemistry to reactive solute transport modeling may improve predictive capabilities of various trace metal and solute interactions incorporated with the cycling of Fe within ARD streams. Further, model improvement of Fe cycling may enable more accurate remediation predictions for ARD streams.  相似文献   

20.
The Bralorne and Pioneer mines, now inactive, produced over 4 million ounces of Au from an orogenic lode Au deposit located on the eastern edge of the Coastal Mountains of SW British Columbia. Between 2007 and 2009, drainage from a recently developed exploration adit was investigated in order to better understand and anticipate potential environmental management issues associated with the development of this type of deposit in the future. Portal discharge rate and specific conductance were monitored continuously over a 14-month period during which 36 water samples were collected. Additional samples were collected from flooded workings within the adit. Concentrations of As and Sb at the portal range as high as 1738 and 316 μg/L, respectively, while those in the mine pool reach 3304 and 349 μg/L, respectively. Effluent chemistry is mildly alkaline (pH = 8.7) and is dominated by Na, Ca, Mg, HCO3 and SO4. Geochemical inverse modeling of effluent composition indicates weathering of albite (2515 kg/a), ferroan dolomite (718 kg/a), pyrite (456 kg/a), arsenopyrite (23 kg/a) and stibnite (2 kg/a). Modeled sulfide reaction coefficients, normalized by their corresponding host rock concentrations, suggest that oxidation of arsenopyrite is 25 times slower than that of pyrite whereas oxidation of stibnite is 1.5 times faster. Oxidative dissolution of arsenopyrite and stibnite releases 10.6 kg/a of As and 1.1 kg/a of Sb of which 57% and 46%, respectively, are sorbed to ferrihydrite and gibbsite on the bed of the shallow channel through which the mine pool drains to the portal. Although mass balance calculations predict the formation of sufficient ferrihydrite to sorb 100% of the As dissolved in the mine pool, this attenuation process was ineffective possibly because the precipitated sorbents settled to the bottom of the water column or because of competition for sorption sites from Ca and HCO3. The dissolved Sb/As molar ratio in portal effluent (0.082) is much greater than the Sb/As ratio of the mineralization (0.002) because of slower arsenopyrite oxidation and somewhat lesser sorption of Sb.  相似文献   

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