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1.
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   

2.
《Applied Geochemistry》2006,21(6):1073-1082
In the lower part of the River Saale, Germany, U shows concentrations of up to 4 μg/L. Former mining activities and their still existing dewatering systems in the drainage basin of the River Saale are responsible for the high salt and trace metal concentrations in the water of some tributaries. An old adit from the Mansfeld mining district flowing into the Schlenze Stream with mean U concentrations of about 60 μg/L increases the U concentration of the River Saale by 0.5 μg/L. The U concentrations in the running waters of the study area can be explained by mixing processes. Uranium from the adit and the Schlenze is mainly transported in the <0.45 μm fraction as a carbonate complex.  相似文献   

3.
The solubility controls on vanadium (V) in groundwater were studied due to concerns over possible harmful health effects of ingesting V in drinking water. Vanadium concentrations in the northeastern San Joaquin Valley ranged from <3 μg/L to 70 μg/L with a median of 21 μg/L. Concentrations of V were highest in samples collected from oxic groundwater (49% > 25 μg/L) and lowest in samples collected from anoxic groundwater (70% < 0.8 μg/L). In oxic groundwater, speciation modeling (SM) using PHREEQC predicted that V exists primarily as the oxyanion H2VO4−. Adsorption/desorption reactions with mineral surfaces and associated oxide coatings were indicated as the primary solubility control of V5+ oxyanions in groundwater. Environmental data showed that V concentrations in oxic groundwater generally increased with increasing groundwater pH. However, data from adsorption isotherm experiments indicated that small variations in pH (7.4–8.2) were not likely as an important a factor as the inherent adsorption capacity of oxide assemblages coating the surface of mineral grains. In suboxic groundwater, accurate SM modeling was difficult since Eh measurements of source water were not measured in this study. Vanadium concentrations in suboxic groundwater decreased with increasing pH indicating that V may exist as an oxycationic species [e.g. V(OH)3+]. Vanadium may complex with dissolved inorganic and organic ligands under suboxic conditions, which could alter the adsorption behavior of V in groundwater. Speciation modeling did not predict the existence of V-inorganic ligand complexes and organic ligands were not collected as part of this study. More work is needed to determine processes governing V solubility under suboxic groundwater conditions. Under anoxic groundwater conditions, SM predicts that aqueous V exists as the uncharged V(OH)3 molecule. However, exceedingly low V concentrations show that V is sparingly soluble in anoxic conditions. Results indicated that V may be precipitating as V3+- or mixed V3+/Fe3+-oxides in anoxic groundwater, which is consistent with results of a previous study. The fact that V appears insoluble in anoxic (Fe reducing) redox conditions indicates that the behavior of V is different than arsenic (As) in aquifer systems where the reductive dissolution of Fe-oxides with As adsorbed to the surface is a well-documented mechanism for increasing As concentrations in groundwater. This hypothesis is supported by the relation of V to As concentrations in oxic versus anoxic redox conditions.Sequential extraction procedures (SEP) applied to aquifer material showed that the greatest amount of V was recovered by the nitric acid (HNO3) extract (37–71%), followed by the oxalate-ascorbic acid extract (19–60%) and the oxalate extract (3–14%). These results indicate that V was not associated with the solid phase as an easily exchangeable fraction. Although the total amount of V recovered was greatest for the HNO3 extract that targets V adsorbed to sorption sites of crystalline Al, Fe and Mn oxides, the greatest V saturation of sorption sites appeared to occur on the amorphous and poorly crystalline oxide solid phases targeted by the oxalate and oxalate-ascorbic acid extracts respectively. Adsorption isotherm experiments showed no correlation between V sorption and any of the fractions identified by the SEP. This lack of correlation indicates the application of an SEP alone is not adequate to estimate the sorption characteristics of V in an aquifer system.  相似文献   

4.
About a century of exploitation of the galena-arsenopyrite deposit of Baccu Locci in Sardinia (Italy) has caused a severe, persistent arsenic contamination that extends downstream from the mine for several kilometres. Differently from As, the contamination of lead in surface waters is only localised in the upper part of the mine despite very high Pb concentrations in geologic materials (waste rocks, tailings, stream sediments, soils) over the whole Baccu Locci stream catchment. The aqueous and solid speciation of Pb in various environmental media of the Baccu Locci system was determined by means of a combined analytical (ICP-MS, SEM-EDX, TEM-EDX, chemical extraction) and thermodynamic approach (PHREEQC). The study has pointed out that relatively little Pb (up to 30 µg/L) is initially released to surface waters (pH = 7–8, Eh = 0.4–0.6 V) very rapidly due to dissolution of anglesite that is the first product of galena oxidation. Subsequently, Pb is removed (down to 0.6 µg/L) by probable sorption onto hydrous ferric oxides (e.g. ferrihydrite) and/or possible precipitation of As-containing plumbojarosite that is the main secondary Pb-bearing phase in stream sediments/tailings along the Baccu Locci stream course. The latter hypothesis is controversial since it is reported from the literature that plumbojarosite is formed under acidic conditions, although there is contrary field evidence as well. Bearing in mind the uncertainties introduced from thermodynamic and analytical data, the solubility calculations indicate strong undersaturation of surface waters with respect to plumbojarosite (SI: ? 19.9 to ? 3.7). On the contrary arsenatian plumbojarosite is at or close to saturation (SI: ? 0.6 to 3.2) in most surface waters and beudantite is clearly above saturation (SI: 4.1 to 12.7). This suggests that the incorporation of As might increase the stability of plumbojarosite, extending it up to near-neutral conditions. As a consequence, Pb is prevented from being released downstream to surface waters, and dissolved Pb concentrations remain definitely below the Italian and WHO limits for drinking waters (50 µg/L and 10 µg/L, respectively).  相似文献   

5.
Contaminated drainage related to the leaching of soluble metals under near-neutral conditions, known as contaminated neutral drainage (CND), may arise when metal species are soluble at neutral pH. Such a phenomenon has been sporadically observed in effluent from the Tio mine waste-rock pile in Quebec, Canada, particularly from older sections of the pile, where Ni concentrations are increasing with time. It has been postulated that Ni is retained within the fresh waste rock as sorbed species, but as the rock ages, sorption sites become saturated and more Ni is released to the effluent. A field test program was initiated to evaluate the geochemical behavior of the waste rock. This paper presents a numerical analysis of CND generation from waste-rock field test cells including water flow and multi-component transport with geochemical reactions (e.g. sulfide oxidation, pH neutralization, and Ni sorption), using the code MIN3P. The model was able to represent the delay before Ni is seen in the effluent, as caused by sorption of Ni onto Fe-oxide particles. Once the sorption sites are saturated, the model allows Ni release into the effluent by millerite dissolution, expressed by the shrinking core model. A sensitivity analysis indicated that sorption parameters significantly affected the simulated results, so their selection should be based on sound independent field or experimental data.  相似文献   

6.
《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   

7.
《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   

8.
《Applied Geochemistry》2005,20(5):989-1016
Groundwater from the Quaternary loess aquifer of La Pampa, central Argentina, has significant problems with high concentrations of As (up to 5300 μg L−1) as well as other potentially toxic trace elements such as F, B, Mo, U, Se and V. Total As concentrations in 45 loess samples collected from the aquifer have a range of 3–18 mg kg−1 with a mean of 8 mg kg−1. These values are comparable to world-average sediment As concentrations. Five samples of rhyolitic ash from the area have As concentrations of 7–12 mg kg−1. Chemical analysis included loess sediments and extracted porewaters from two specially cored boreholes. Results reveal a large range of porewater As concentrations, being generally higher in the horizons with highest sediment As concentrations. The displaced porewaters have As concentrations ranging up to 7500 μg L−1 as well as exceptionally high concentrations of some other oxyanion species, including V up to 12 mg L−1. The highest concentrations are found in a borehole located in a topographic depression, which is a zone of likely groundwater discharge and enhanced residence time. Comparison of sediment and porewater data does not reveal unequivocally the sources of the As, but selective extract data (acid-ammonium oxalate and hydroxylamine hydrochloride) suggest that much of the As (and V) is associated with Fe oxides. Primary oxides such as magnetite and ilmenite may be partial sources but given the weathered nature of many of the sediments, secondary oxide minerals are probably more important. Extract compositions also suggest that Mn oxide may be an As source. The groundwaters of the region are oxidising, with dissolved O2, NO3 and SO4 normally present and As(V) usually the dominant dissolved As species. Under such conditions, the solubility of Fe and Mn oxides is low and As mobilisation is strongly controlled by sorption–desorption reactions. Desorption may be facilitated by the relatively high-pH conditions of the groundwaters in the region (7.0–8.8) and high concentrations of potential competitors (e.g. V, P, HCO3). PHREEQC modelling suggests that the presence of V at the concentrations observed in the Pampean porewaters can suppress the sorption of As to hydrous Fe(III) oxide (HFO) by up to an order of magnitude. Bicarbonate had a comparatively small competitive effect. Oxalate extract concentrations have been used to provide an upper estimate of the amount of labile As in the sediments. A near-linear correlation between oxalate-extractable and porewater As in one of the cored boreholes investigated has been used to estimate an approximate Kd value for the sediments of 0.94 L kg−1. This low value indicates that the sediments have an unusually low affinity for As.  相似文献   

9.
《Chemical Geology》2007,236(3-4):217-227
The association of arsenate, As(V), and arsenite, As(III), with disordered mackinawite, FeS, was studied in sulfide-limited (Fe:S = 1:1) and excess-sulfide (Fe:S = 1:2) batch experiments. In the absence of arsenic, the sulfide-limited experiments produce disordered mackinawite while the excess-sulfide experiments yield pyrite with trace amounts of mackinawite. With increasing initially added As(V) concentrations the transformation of FeS to mackinawite and pyrite is retarded. At S:As = 1:1 and 2:1, elemental sulfur and green rust are the end products. As(V) oxidizes S(-II) in FeS and (or) in solution to S(0), and Fe(II) in the solid phase to Fe(III). Increasing initially added As(III) concentrations inhibit the transformation of FeS to mackinawite and pyrite and no oxidation products of FeS or sulfide, other than pyrite, were observed. At low arsenic concentrations, sorption onto the FeS surface may be the reaction controlling the uptake of arsenic into the solid phase. Inhibition of iron(II) sulfide transformations due to arsenic sorption suggests that the sorption sites are crucial not only as sorption sites, but also in iron(II) sulfide transformation mechanisms.  相似文献   

10.
《Applied Geochemistry》2005,20(5):973-987
Due to liming of acid mine drainage, a calcite–gypsum sludge with high concentrations of Zn (24,400 ± 6900 μg g−1), Cu (2840 ± 680 μg g−1) and Cd (59 ± 20 μg g−1) has formed in a flooded tailings impoundment at the Kristineberg mine site. The potential metal release from the sludge during resuspension events and in a long-term perspective was investigated by performing a shake flask test and sequential extraction of the sludge. The sequentially extracted carbonate and oxide fractions together contained ⩾97% of the total amount of Cd, Co, Cu, Ni, Pb and Zn in the sludge. The association of these metals with carbonates and oxides appears to result from sorption and/or coprecipitation reactions at the surfaces of calcite and Fe, Al and Mn oxyhydroxides forming in the impoundment. If stream water is diverted into the flooded impoundment, dissolution of calcite, gypsum and presumably also Al oxyhydroxides can be expected during resuspension events. In the shake flask test (performed at a pH of 7–9), remobilisation of Zn, Cu, Cd and Co from the sludge resulted in dissolved concentrations of these metals that were significantly lower than those predicted to result from dissolution of the carbonate fraction of the sludge. This may suggest that cationic Zn, Cu, Cd and Co remobilised from dissolving calcite, gypsum and Al oxyhydroxides were readsorbed onto Fe oxyhydroxides remaining stable under oxic conditions. In a long-term perspective (≳102 a), ⩾97% of the Cd, Co, Cu, Ni, Pb and Zn content of the sludge potentially is available for release by dissolution of calcite and reductive dissolution of Fe oxyhydroxides if the sludge is subject to a soil environment with lower dissolved Ca concentrations, pH and redox than in the impoundment.  相似文献   

11.
《Applied Geochemistry》2006,21(10):1760-1780
Sulfide-rich mine tailings in Adak that are exposed to weathering cause acid mine drainage characterized by low pH (2–4) and high SO4 (up to 800 mg L−1). Surface water, sediment and soil samples collected in this study contain higher concentrations of As, Cu, Fe and Zn, compared to the target and/or intervention limits set by international regulatory agencies. In particular, high As concentrations in water (up to 2900 μg L−1) and sediment (up to 900 mg kg−1) are of concern. There is large variability in trace element concentrations, implying that both physical (grain size) and chemical factors (pH, secondary phases as sulfides, Al-oxides or clay minerals) play an important role in their distribution. The low pH keeps the trace elements dissolved, and they are transported farther downstream. Trace element partition coefficients are low (log Kd = 0.3–4.3), and saturation indices calculated with PHREEQC are <0 for common oxide and sulfidic minerals. The sediment and soil samples indicate an enhanced pollution index (up to 17), and high enrichment factors for trace elements (As up to 38,300; Zn up to 800). Finally, leaves collected from different plant types indicate bioaccumulation of several elements (As, Al, Cu, Fe and Zn). However, some of the plants growing in this area (e.g., Salix, Equisétum) are generally resistant to metal toxicity, and hence, liming and phytoremediation could be considered as potential on-site remediation methods.  相似文献   

12.
The Mokrsko Stream in the central Czech Republic is an oxic and slightly alkaline stream that drains a natural As geochemical anomaly. Although long-term monitoring has characterized the general seasonal trends in trace element concentrations (i.e., As, Mo, Cu, Zn) in this stream, little is known about solubility controls and sorption processes that influence diel cycles in trace element concentrations. Trace elements (including As species, Cu, Mn, Mo, Pb and Sb) and other parameters were monitored over two 24-h periods in unfiltered and filtered (0.1 μm) samples collected in August 2010 and June 2011. Copper and Pb were predominantly (>92% of the mass) associated with the particulate fraction (>0.1 μm). Arsenic, Mo and Sb were predominantly (>88% of the mass) in the “dissolved” (<0.1 μm) form. Particulate-associated elements displayed up to a factor of 13 differences between minimum and maximum concentrations, most likely due to increased streamflow related to rainfall events. Dissolved concentrations of the trace metal cations (Cu, Fe, Mn and Pb) were consistently low and displayed no diel trends. Dissolved As(V), Mo and Sb varied on a diel cycle, with increased concentrations (up to 36%) during the late afternoon and decreased concentrations during the nighttime. Diel trends in trace anionic elements are explained by temperature-dependent sorption, as the diel changes in pH during base flow were very small (0.07 std. units). Very low concentrations of As(III), which have been shown to vary in a diel cycle, were attributed to enhanced hydraulic exchange with As(III)-rich hyporheic water during rainfall events.  相似文献   

13.
The abandoned Sn-W Ribeira mine, northeast of Portugal, contained quartz veins with cassiterite, wolframite, scheelite, pyrite, arsenopyrite, sphalerite, chalcopyrite, manganocolumbite, bismuthinite, native bismuth, phosphates and carbonates. The exploration took place on the northern slope of the Viveiros stream, which is an affluent of the Sabor River. The waste-rock dumps and tailings were deposited on the hillside, close to the mine and are nowadays exposed to significant weathering and erosion, as they are not vegetated. The eroded material is transported by the Viveiros stream toward the Sabor River. A seasonal stream drains the tailings. The stream sediments samples were collected along the Viveiros stream, in the seasonal stream, in a seasonal spring at the bottom of the tailings, in the Sabor River and in other streams not affected by mine workings, following the mine influence along the Viveiros stream and in the Sabor River (1.2 km away from the mine workings). The data show that the degree of pollution increases along the Viveiros stream, especially in winter. The highest degree of pollution is for As, In, W, Sn and Bi. The sediments from the drainage of the main tailings are particularly polluted during winter, by Bi, In and Sn. The sedimentary precipitate from the spring is polluted in Cu, As, In, Sn, Ta, W, Bi, Zn, Nb, Ag, Sb and Ta. The sediments from the Sabor River are significantly polluted by As, Ag, In, Sn, W and Bi. The sediments from the regional streams, Viveiros stream and Sabor River have similar REE (NASC normalized) patterns (ΣREE = 131.7–185.9 mg/kg, LaN/LuN = 1.23–1.42 and Eu/Eu* = 1.02), while those from the seasonal stream, crossing the main tailings, are enriched in REE (ΣREE = 250.3–283.6 mg/kg, LaN/LuN = 1.6–2.09 and Eu/Eu* = 0.96). The general decrease in LaN/LuN values with increase in total Fe2O3 can be explained by the partitioning of HREE to the solid Fe-oxides phase. The sedimentary precipitate and coatings, which are mainly formed by Fe-oxy-hydroxides, but also contain jarosite, are impoverished in all REE. The impoverishment can be explained by the release of REE from the surface of the Fe-oxy-hydroxides, which occurs due to a local lowering of pH, caused by jarosite dissolution. During successive alternate cycles of wet and dry conditions, takes place the formation of Fe-oxy-hydroxides and jarosite in the sedimentary precipitate and coatings. The subsequent dissolution of jarosite releases acidity, thus promoting de-sorption of REE from the Fe-oxy-hydroxides mineral phases.  相似文献   

14.
《Applied Geochemistry》2006,21(10):1799-1817
Release of acid drainage from mine-waste disposal areas is a problem of international scale. Contaminated surface water, derived from mine wastes, orginates both as direct surface runoff and, indirectly, as subsurface groundwater flow. At Camp Lake, a small Canadian Shield lake that is in northern Manitoba and is ice-covered 6 months of the year, direct and indirect release of drainage from an adjacent sulfide-rich tailings impoundment has severely affected the quality of the lake water. Concentrations of the products from sulfide oxidation are extremely high in the pore waters of the tailings impoundment. Groundwater and surface water derived from the impoundment discharge into a semi-isolated shallow bay in Camp Lake. The incorporation of this aqueous effluent has altered the composition of the lake water, which in turn has modified the physical limnology of the lake. Geochemical profiles of the water column indicate that, despite its shallow depth (6 m), the bay is stratified throughout the year. The greatest accumulation of dissolved metals and SO4 is in the lower portion of the water column, with concentrations up to 8500 mg L−1 Fe, 20,000 mg L−1 SO4, 30 mg L−1 Zn, 100 mg L−1 Al, and elevated concentrations of Cu, Cd, Pb and Ni. Meromictic conditions and very high solute concentrations are limited to the bay. Outside the bay, solute concentrations are lower and some stratification of the water column exists. Identification of locations and composition of groundwater discharge relative to lake bathymetry is a fundamental aspect of understanding chemical evolution and physical stability of mine-impacted lakes.  相似文献   

15.
Hematite is a common primary/secondary mineral in mine drainage and mine waste settings that can adsorb dissolved metals and metalloids. This study explored the ability of synthetic hematite to retain one such contaminant, molybdate, on its surfaces under highly alkaline (pH = ∼10) conditions. X-ray diffraction (XRD), Raman spectroscopy (RS), scanning electron microscopy (SEM), and specific surface area (BET) analyses show that synthetic hematite particles are stable and able to adsorb molybdate. Raman spectra show that the hematite efficiently adsorbs molybdate and retains it on its surfaces via strong inner-sphere surface complexation. Inductively coupled plasma-mass spectrometry (ICP-MS) data indicate that hematite aged (7 and 9 days) at high and room temperatures (75 and 25 °C) retains adsorbed molybdate and that molybdate sorption increases with aging. SEM images show that aged hematite particles with adsorbed molybdate are similar in size and shape to pure hematite and exhibit no significant reduction in surface area. These findings are valuable for understanding the fate of Mo in mine wastes and mill tailings environments where the 2-line ferrihydrite to which it is adsorbed can transform to hematite.  相似文献   

16.
《Applied Geochemistry》2006,21(11):1969-1985
Gossan Creek, a headwater stream in the SE Upsalquitch River watershed in New Brunswick, Canada, contains elevated concentrations of total Hg (HgT up to 60 μg/L). Aqueous geochemical investigations of the shallow groundwater at the headwaters of the creek confirm that the source of Hg is a contaminated groundwater plume (neutral pH with Hg and Cl concentrations up to 150 μg/L and 20 mg/L, respectively), originating from the Murray Brook mine tailings, that discharges at the headwaters of the creek. The discharge area of the contaminant plume was partially delineated based on elevated pH and Cl concentrations in the groundwater. The local groundwater outside of the plume contains much lower concentrations of Hg and Cl (<0.1 μg/L and 3.8 mg/L, respectively) and displays the chemical characteristics of an acid-sulfate weathering system, with low pH (4.1–5.5) and elevated concentrations of Cu, Zn, Pb and SO4 (up to 5400 μg Cu/L, 8700 μg Zn/L, 70 μg Pb/L and 330 mg SO4/L), derived from oxidation of sulfide minerals in the Murray Brook volcanogenic massive sulfide deposit and surrounding bedrock. The HgT mass loads measured at various hydrologic control points along the stream system indicate that 95–99% of the dissolved HgT is attenuated in the first 3–4 km from the source. Analyses of creek bed sediments for Au, Ag, Cu, Zn, Pb and Hg indicate that these metals have partitioned strongly to the sediments. Mineralogical investigations of the contaminated sediments using analytical scanning electron microscopy (SEM), transmission electron microscopy (TEM) and scanning transmission electron microscopy (STEM), reveal discrete particles (<1–2 μm) of metacinnabar (HgS), mixed Au–Ag–Hg amalgam, Cu sulfide and Ag sulfide.  相似文献   

17.
《Applied Geochemistry》2006,21(7):1093-1108
Peña del Hierro is an abandoned mine site located in the catchment area of the Tinto river (Pyrite Belt, SW Spain). As leaching from the spoils affect the quality of the stream water, the waste dumps have been characterized for mineralogy, geochemistry and granulometry to obtain an estimate of the potential pollution. Waste rock dumps in Peña del Hierro are very heterogeneous and are mainly composed of acid volcanic tuffs > gossan > shales > roasted pyrite ashes > floated pyrite. The volcanic tuffs, the gossan and the shales coexist in the same piles. The roasted pyrite ashes and the floated pyrite form more homogeneous dumps. The dissolution of pyrite concentrated in pyrite ashes and floated pyrite units can generate acid mine drainage. Nevertheless, acid volcanic tuffs, which are rich in pyrite and have no neutralizing minerals, are the main source of these acidic effluents. Only muscovite might partially neutralize the acidity, but the dissolution of this mineral is too slow to compensate for acidity. The occurrence of jarosite in the <2 mm fraction indicates that extreme acid mine drainage occurs. The gossan and roasted pyrite ashes have high contents of trace elements. According to their concentration, As (46–1710 ppm), Pb (113–3455 ppm) and Hg (0–53) are some of the most important toxic trace elements in these wastes. In dumps mainly composed of volcanic tuffs most of the trace elements derive from the gossan mixed in the piles. Gossan is stable in an oxidizing environment, but acidic effluents (pH < 2) can dissolve Fe oxyhydroxides from them and release high amounts of trace elements to the stream water. This research contributes to estimating the production of acid mine drainage and the actual contamination risk of potentially toxic elements in soils and waters of this area, and could be the base for possible future mitigation actions in other areas affected by mining wastes.  相似文献   

18.
Arsenic species including arsenite, arsenate, and organic arsenic were measured in the porewaters collected from Poyang Lake, the largest freshwater lake of China. The vertical distributions of dissolved arsenic species and some diagenetic constituents [Fe(II), Mn(II), S(−II)] were also obtained in the same porewater samples in summer and winter. In sediments the concentration profiles of total As and As species bound to Fe–Mn oxyhydroxides and to organic matter were also determined along with the concentrations of Fe, Mn and S in different extractable fractions. Results indicate that, in the summer season, the concentrations of total dissolved As varying from 3.9 to 55.8 μg/L in sediments were higher than those (5.3–15.7 μg/L) measured in the winter season, while the concentrations of total As species in the solid phase varied between 10.97 and 25.32 mg/kg and between 7.84 and 30.52 mg/kg on a dry weight basis in summer and winter, respectively. Seasonal profiles of dissolved As suggest downward and upward diffusion, and the flux of dissolved As across the sediment–water interface (SWI) in summer and winter were estimated at 3.88 mg/m2 a and 0.79 mg/m2 a, respectively. Based on porewater profiles and sediment phase data, the main geochemical behavior of As was controlled by adsorption/desorption, precipitation and molecular diffusion. The solubility and migration of inorganic As are controlled by Fe–Mn oxyhydroxides in summer whereas they appear to be more likely controlled by both amorphous Fe–Mn oxyhydroxides and sulfides in winter. A better knowledge of the cycle of As in Poyang Lake is essential to a better management of its hydrology and for the environmental protection of biota in the lake.  相似文献   

19.
《Applied Geochemistry》2006,21(11):1986-1998
Elevated concentrations of Hg are present (averaging 36 μg/g), mainly as cinnabar, in the Murray Brook Au deposit, located in northern New Brunswick, Canada. After the mined ore was subjected to CN leaching, the tailings were deposited in an unsaturated pile, and 10 a after mine closure an estimated 4.7 × 103 kg of CN and 1.1 × 104 kg of Hg remain in the pile. Elevated Hg concentrations have been measured in the groundwater (up to 11,500 μg/L) and surface water (up to 32 μg/L) down-gradient of the tailings. To investigate the controls on Hg mobility and leaching persistence, laboratory experiments were conducted using unsaturated columns filled with tailings. Within the first 0.2 pore volumes (PV) eluted, the concentrations of Hg and CN increased to peak concentrations of 12,900 μg Hg/L and 16 mg CN/L, respectively. In the subsequent 0.9 PV, concentrations decreased to approximately 1300 μg Hg/L and 2.8 mg CN/L. Thermodynamic calculations demonstrate that >99.8% of the mobilized Hg in the tailings pore water is in the form of Hg–CN complexes, indicating that Hg mobility to the surrounding aquatic environment is directly dependent on the rate of CN leaching. One-dimensional transport simulations suggest that leached CN can be partitioned into conservative (24%) and non-conservative (76%) fractions. Extrapolation of simulation results to the field scale suggests that CN, and by extension Hg, will continue to elute from the tailings for at least an additional 130 a.  相似文献   

20.
In the present study, we investigated As behavior in a high-As hot spring (Sambe hot spring, Shimane, Japan) by coupling direct chemical speciation by synchrotron-based XAFS and HPLC–ICP-MS with microbial As-redox transformation gene analysis. The concentration of soluble As in the spring streamwater decreased immediately along the flow in correlation with Fe behavior, indicating that As in the streamwater was naturally attenuated in the streamwater. Iron XAFS analysis suggested deposition of Fe(III) oxyhydroxides along the flow. Thus, considering the strong affinity of As to Fe oxyhydroxides, the observed attenuation in As was possibly caused by sorption (or incorporation) of As on Fe(III) oxyhydroxides. Both dissolved As(III) and As(V) were present in the aqueous phase, and As(III) was rapidly oxidized to As(V) (<30 s) along the flow. The oxidation kinetics indicated the occurrence of biotic As(III) oxidation, because obtained As(III) oxidation rate (6.7–7.8 μM min−1) was much faster than the reported abiotic oxidation rates. Furthermore, the bacterial arsenite oxidase gene (aioA) was detected in DNA extracted from all samples (average of 2.0 × 105 copies dry g−1), which also supported potential attributes of biological As(III) oxidation in situ. In solid phase samples from sampling points analyzed by XAFS, most of the As existed as oxidized pentavalent form, As(V). This result indicated that this form was preferentially partitioned to the solid phase because of the much higher affinity of As(V) than of As(III) to Fe(III) oxyhydroxides. Considering the kinetic and microbiological findings, it is indicated that biotic process was predominantly responsible for As(III) oxidation at the present site, and this biotic As(III) oxidation to As(V) controlled the observed attenuation of As, because oxidized As(V) was removed from the aqueous phase by Fe(III) oxyhydroxides more efficiently.  相似文献   

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