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1.
《Applied Geochemistry》2000,15(4):513-530
Soil samples taken from excavated pits on traverses across New Zealand’s Scott Base, Antarctica, were leached with water and 0.01 M HNO3 and the leachates analysed for Ag, Al, As, Cd, Cr, Cu, Fe, Mn, Ni, Pb and Zn. The soils had high conductivity and pH values generally increasing with depth and in the range 8.3–10.1. The water leachate generally contained most of the extractable metals except Mn and Cd, and As. Linear relationships were observed between some metals leached into alkaline solution and the Fe in those solutions. The ratios to Fe were comparable to those of the host basanite, and this observation is interpreted as showing that these metals are incorporated in fine mineral particulates derived directly from the rock mass. Outliers in leachable metal concentrations in the soils indicated appreciable contamination of the soil from anthropogenic sources with Ag, Cd, Cu, Pb and Zn as well as As. In some locations high concentrations of Ag and Cd correspond to specific sources and drainage channels. High concentrations of Pb were widely spread and in the top soil layers whereas the elevated concentrations of Zn were distributed throughout the soil profiles indicating atmospheric sources and different mobilities within the soils. Transport within the soils is evident for some metals, as is lateral movement over and through the soils.  相似文献   

2.
Primary and placer gold mining sites in southern Ethiopia were studied to see the contribution of mining to the accumulation of metals in different environmental media. Sediment, water and plant samples were analyzed for Al, Mn, Fe, As, Ni, Cr, Cu, Co, Pb, W, Sb, Mo, Zn and V. Water parameters (pH, Eh, TDS, anions and cations) were also measured. The sediment analyses results show that the most abundant metals are Ni (average 224.7 mg/kg), Cr (199 mg/kg), Cu (174.2 mg/kg), V (167.3 mg/kg), Zn (105.5 mg/kg), Pb (61.5 mg/kg) and As (59.7 mg/kg) in the primary gold mining sites while the placer sites show high concentration of V (average 301.2 mg/kg), Cr (260.4 mg/kg), Zn (179 mg/kg), Ni (113.4 mg/kg), Cu (46.7 mg/kg), As (32.2 mg/kg) and Co (31 mg/kg). The metals Cu, Ni, W, Cr, As and Pb in primary and Sb, W, Cr, Ni, Zn, As and Mo in placer gold mining sites have geoaccumulation indexes (I geo) from one to four indicating considerable accumulation of these metals. Waters from both primary and placer mining sites are near neutral to alkaline. Arsenic (average 92.8 μg/l), Ni (276.6 μg/l), Pb (18.7 μg/l), Sb (10.7 μg/l), Mn (1 mg/l), Fe (8.3 mg/l) and Al (23.8 mg/l) exceeded the guideline value for drinking water. Plants show high concentration of Cr (average 174.5 mg/kg), Ni (163.5 mg/kg), Zn (96 mg/kg) and W (48 mg/kg). Zinc, W, Mo, Ni and Cr show the maximum biological absorption coefficient (BAC) ranging 0.4–1.7, 0.1–104.6, 1.1–2.6, 0.2–1.6 and 0.2–3.6, respectively, and the results suggest bioaccumulation of these elements in plants. The minerals especially sulfides in the ore aggregate are the ultimate source of the metals. The release of the metals into the environmental media is facilitated (in addition to normal geologic processes) by human activities related to gold mining.  相似文献   

3.
《Applied Geochemistry》2002,17(5):569-581
This study examined the sorption of trace metals to precipitates formed by neutralization of 3 natural waters contaminated with acid mine drainage (AMD) in the former Ducktown Mining District, Tennessee. The 3 water samples were strongly acidic (pH 2.2 to 3.4) but had distinctively different chemical signatures based on the mole fractions of dissolved Fe, Al and Mn. One sample was Fe-rich (Fe=87.5%, Al=11.3%, and Mn=1.3%), another was Al-rich (Al=79.4%, Mn=18.0%, and Fe=2.5%), and the other was Mn-rich (Mn=51.4%, Al=25.7%, and Fe=22.9%). In addition, these waters had high concentrations of trace metals including Zn (37,700 to 17,400 μg/l), Cu (13,000 to 270 μg/l), Co (1,500 to 520 μg/l), Ni (360 to 75 μg/l), Pb (30 to 8 μg/l), and Cd (30 to 6 μg/l). Neutralization of the AMD-contaminated waters in the laboratory caused the formation of either schwertmannite at pH<4 or ferrihydrite at pH>4. Both phases were identified by XRD analyses of precipitates from the most Fe-rich water. At higher pH values (∼5) Al-rich precipitates were formed. Manganese compounds were precipitated at pH∼8. The removal of trace metals depended on the precipitation of these compounds, which acted as sorbents. Accordingly, the pH for 50% sorption (pH50) ranged from 5.6 to 7.5 for Zn, 4.6 to 6.1 for Cu, 5.4 to 7.7 for Ni, 5.9 to 7.9 for Co, 3.1 to 4.3 for Pb, and 5.5 to 7.7 for Cd. The pH dependence of sorption arose not only because of changes in the sorption coefficients of the trace metals but also because the formation and composition of the sorbent was controlled by the pH, the chemical composition of the water, and the solubilities of the oxyhydroxide-sulfate complexes of Fe, Al, and Mn.  相似文献   

4.
针对金铜精矿采用中性催化加压预处理工艺,经试验,在温度180 ℃、氧分压1.8 MPa、催化剂0.14 mol/L的基本条件下,Cu浸出率为99.4%,浸液中残留∑Fe质量浓度仅为3.52 g/L,对后续回收Cu的精炼工艺非常有利。氧化渣以氯化浸金工艺浸出Au、Ag,浸出率分别为98.2%、90.3%,有价元素回收率高,工艺简单,环境效益好。  相似文献   

5.
《Applied Geochemistry》1988,3(3):345-356
Suspended particulate matter was recovered by filtration (0.40 μm) of water from a stream receiving acidic effluents from a mine tailings deposit. This solid phase formed rapidly as pH increased from 3.5 at the release point to 6.5, approximately 2 km downstream. The suspended solid was present in concentrations that ranged from 10–20 mg/l for anoxic conditions (winter) to 30–120 mg/l for oxic conditions (early spring). The solid consisted of FeOOH + Fe(OH)3(am) and AlOOH + Al(OH)3(am), as well as silicates. The organic content (of natural origin) was up to 30% (dry wt). Most of the Fe and Al from the leachate was precipitated in the particulate phase, approximately 98% of total metal content in the aqueous phase, as well as ∼50% of Mn, Cu, Zn, Cd and Pb. These elements were predominantly adsorbed on the hydrous oxide precipitate, or to some extent (Mn and Pb) coprecipitated, as indicated from a sequential leaching procedure and powder X-ray diffractometry. All the elements, particularly Cu, were to a significant degree associated with organic matter.  相似文献   

6.
The technique of diffusive gradients in thin films (DGT) was applied to obtain high-resolution vertical profiles of trace metals in sediment porewater of a eutrophic lake, Lake Chaohu. All sampling sediments were under anaerobic conditions with Eh values below 0, the redox potential profile in M4 was relatively stable, and higher Eh values in M4 than that in M1 were observed due to hydrodynamic effects. Fe, Mn and As exhibited closely corresponding profiles due to the co-release of Fe and Mn oxides and the reduction of As. Higher Fe and Mn concentrations and lower As concentrations were observed in M1 of the western half-lake than those in M4 of the eastern half-lake due to different sources and metal contamination levels in the two regions. Cu and Zn showed increasing concentrations similar to Mn and Fe at 1–2 cm depth of sediments, while DGT measured Co, Ni, Cd and Pb concentrations decreased down to 3–4 cm in the profiles. Co, Ni, Cu, Zn, Cd and Pb showed insignificant regional concentration variances in the western and eastern half-lakes. According to the R(C DGT/C centrifugation) values, the rank order of metal labilities decrease as follows: Fe (>1) > Cu, Pb, Zn (>0.9) > Co, Ni, Cd (>0.3) > Mn, As (>0.1).  相似文献   

7.
《Applied Geochemistry》2004,19(7):1039-1064
Slag collected from smelter sites associated with historic base-metal mines contains elevated concentrations of trace elements such as Cu, Zn and Pb. Weathering of slag piles, many of which were deposited along stream banks, potentially may release these trace elements into the environment. Slags were sampled from the Ely and Elizabeth mines in the Vermont copper belt, from the copper Basin mining district at Ducktown, Tennessee and from the Clayton silver mine in the Bayhorse mining district, Idaho, in the USA. Primary phases in the slags include: olivine-group minerals, glass, spinels, sulfide minerals and native metals for Vermont samples; glass, sulfide minerals and native metals for the Ducktown sample; and olivine-group minerals, clinopyroxenes, spinels, sulfide minerals, native metals and other unidentified metallic compounds for Clayton slag. Olivine-group minerals and pyroxenes are dominantly fayalitic and hedenbergitic in composition, respectively and contain up to 1.25 wt.% ZnO. Spinel minerals range between magnetite and hercynite in composition and contain Zn (up to 2.07 wt.% ZnO), Ti (up to 4.25 wt.% TiO2) and Cr (up to 1.39 wt.% Cr2O3). Cobalt, Ni, Cu, As, Ag, Sb and Pb occur in the glass phase, sulfides, metallic phases and unidentified metallic compounds. Bulk slag trace-element chemistry shows that the metals of the Vermont and Tennessee slags are dominated by Cu (1900–13,500 mg/kg) and Zn (2310–10,200 mg/kg), whereas the Clayton slag is dominated by Pb (63,000 mg/kg), Zn (19,700 mg/kg), Cu (7550 mg/kg), As (555 mg/kg), Sn (363 mg/kg) and Ag (200 mg/kg). Laboratory-based leach tests indicate metals can be released under simulated natural conditions. Leachates from most slags were found to contain elevated concentrations of Cu and Zn (up to 1800 and 470 μg/l, respectively), well in excess of the acute toxicity guidelines for aquatic life. For the Idaho slag, the concentration of Pb in the leachate (11,000 μg/l) is also in excess of the acute toxicity guideline. Geochemical modeling of the leachate chemistry suggests that leachates from the Vermont, Tennessee and Clayton slags are saturated with amorphous silica and Al hydroxide. Therefore, the dissolution of silicate and oxide phases, the oxidation of sulfide phases, as well as the precipitation of secondary phases may control the composition of leachate from slags. The presence of secondary minerals on slag deposits in the field is evidence that these materials are reactive. The petrographic data and results of leaching tests from this study indicate slag may be a source of potentially toxic metals at abandoned mine sites.  相似文献   

8.
Processing of arsenopyrite ore took place at Blackwater Au mine, New Zealand, between 1908 and 1951 and no rehabilitation was undertaken after mine closure. High As concentrations in solid processing residues (up to 40 wt% As) are due to secondary As minerals. Site pH regimes vary from 4.1 to circum-neutral. Originally, all processed As was present as arsenolite (arsenic trioxide polymorph, AsIII), a by-product of arsenopyrite roasting. Near the roaster, scorodite precipitated as a result of the high dissolved As concentration during arsenolite dissolution. The formation of scorodite has two major consequences. Firstly, the scorodite precipitate cements the ground in the vicinity of the roaster area, thereby creating an impermeable surface crust (up to 30 wt% As) and encapsulating weathered arsenolite grains within the cement. Secondly, formation of scorodite temporarily immobilizes some of the dissolved As that is generated during nearby arsenolite dissolution. Where all the available arsenolite has dissolved, scorodite becomes soluble, and the dissolved As concentrations are controlled by scorodite solubility, which is at least two orders of magnitudes lower than arsenolite solubility. Downstream Eh conditions fall below the AsV/AsIII boundary, so that scorodite does not precipitate and dissolved As concentrations are controlled by arsenolite solubility. Dissolved As reaches up to 52 mg/L in places, and exceeds the current WHO drinking water guideline of 0.01 mg/L by 5200 times. This study shows that dissolved As concentrations in discharge waters at historic mine sites are dependent on the processing technology and associated mineralogy.  相似文献   

9.
The hydrogeochemistry of methane: Evidence from English groundwaters   总被引:2,自引:0,他引:2  
The presence of methane (CH4) in groundwater is usually only noticed when it rises to high concentrations; to date rather little is known about its production or natural ‘baseline’ conditions. Evidence from a range of non-polluted groundwater environments in England, including water supply aquifers, aquicludes and thermal waters, reveals that CH4 is almost always detectable, even in aerobic conditions. Measurements of potable waters from Cretaceous, Jurassic and Triassic carbonate and sandstone aquifers reveal CH4 concentrations of up to 500 μg/l, but a mean value of < 10 μg/l. However, aquiclude and thermal waters from the Carboniferous and Triassic typically contain in excess of 1500 μg/l. Such high concentrations have so far only been found at redox (Eh) potentials below 0 mV, but in general CH4 concentration and Eh value are poorly correlated. This suggests a lack of thermodynamic equilibrium, which is confirmed by comparing pe values calculated from the redox couple C(4)/C(− 4) with those derived from Eh. Genesis of CH4 appears to occur on two timescales: a rapid if low rate of production from labile carbon in anaerobic microsites in the soil, and a much longer, millennium scale of production from more refractory carbon. Methane is rarely measured in groundwater; there is no single ionic determinand which acts universally as a proxy, but a combination of high HCO3 and low SO4 concentrations, or the reverse, is an indication that high amounts of CH4 may be present.  相似文献   

10.
In this work we have studied the geochemistry of stream waters arising from waste dumps at the Peña de Hierro mine (Iberian Pyrite Belt, SW Spain), and we have correlated them with the mineralogical and geochemical characteristics of the wastes to asses the source and factors affecting the release of trace elements. The mineralogical composition and geochemistry of 58 borehole samples of waste dumps were studied in the <2 mm fraction. Twenty-eight water samples collected in winter and summer from streams emerging from the waste dumps were analysed for pH, Eh, conductivity, temperature, sulphates and major and trace elements. The leachates from pyrite-rich volcanic tuffs produced very acidic waters, usually with pHs below 2 and reaching values as low as 0.7. The partial dissolution of gossan, which is mainly composed of Fe oxy-hydroxides and is rich in trace elements, released high concentrations of Fetot (up to 33 g/L), As (up to 72), Mo (up to 11 mg/L). On the other hand Cd, Zn and Pb reached up to 0.85, 142 and 0.42 mg/L, respectively, in the stream arising from roasted pyrite ashes and other pyritic wastes. Several elements such as Al, Fe, As, Co, Cu and Mo were strongly correlated with the pH, but Cd and Zn were not correlated under such acidic conditions. The precipitation of jarosite seems to be an important factor in the retention of Pb. The mobility sequence of trace elements shows that Co, Zn and Cd were among the most mobile elements; Cu, As and Mo had intermediate mobility, and Pb was the most immobile. This work shows that uncontrolled waste dumping increases the pollution potential, and a selective management could reduce the release of trace elements into stream waters and mitigate the contamination.  相似文献   

11.
The leaching behaviour of electrostatic precipitator dust from the Mufulira Cu smelter (Copperbelt, Zambia) was studied using a 48-h pH-static leaching experiment (CEN/TS 14997). The release of metals (Cd, Co, Cu, Ni, Pb and Zn) and changes in mineralogical composition using X-ray diffraction and PHREEQC-2 modelling were investigated in the pH range of 3–7. The highest concentrations of metals were released at pH 3–4.5, which encompasses the natural pH of the dust suspension (~4.3). About 40% of the total Cu was leached at pH 3, yielding 107 g/kg. Chalcanthite (CuSO4·5H2O), magnetite (Fe3O4) and delafossite (CuFeO2) represented the principal phases of the studied dust. In contact with water, chalcanthite was dissolved and hydrated Cu sulphates precipitated at pH 4–7. Gypsum (CaSO4·2H2O) and secondary Fe or Al phases were observed in the leached residues. Serious environmental impact due to leaching may occur in dust-contaminated soil systems in the vicinity of the smelting plants.  相似文献   

12.
This study reexamines the notion that extensive As mobilization in anoxic groundwater of Bangladesh is intimately linked to the dissolution of Fe oxyhydroxides on the basis of analyses performed on a suite of freshly collected samples of aquifer material. Detailed sediment profiles extending to 40 to 70 m depth below the surface were obtained at six sites where local groundwater As concentrations were known to span a wide range. The sediment properties that were measured include (1) the proportion of Fe(II) in the Fe fraction leached in hot 1.2 N HCl, (2) diffuse spectral reflectance, and (3) magnetic susceptibility.In parallel with local concentrations of dissolved As ranging from <5 to 600 μg/L, Fe(II)/Fe ratios in shallow (gray) Holocene sands tended to gradually increase with depth from values of 0.3 to 0.5 to up to 0.9. In deeper (orange) aquifers of presumed Pleistocene age that were separated from shallow sands by a clay layer and contained <5 μg/L dissolved As, leachable Fe(II)/Fe ratios averaged ∼0.2. There was no consistent relation between sediment Fe(II)/Fe and dissolved Fe concentrations in groundwater in nearby wells. The reflectance measurements indicate a systematic linear relation (R2 of 0.66; n = 151) between the first derivative transform of the reflectance at 520 nm and Fe(II)/Fe. The magnetic susceptibility of the shallow aquifer sands ranged from 200 to 3600 (x 10−9 m3/kg SI) and was linearly related (R2 of 0.75; n = 29) to the concentrations of minerals that could be magnetically separated (0.03 to 0.79% dry weight). No systematic depth trends in magnetic susceptibility were observed within the shallow sands, although the susceptibility of deeper low-As aquifers was low (up to ∼200 × 10−9 m3/kg SI).This set of observations, complemented by incubation results described in a companion paper by van Geen et al. (this volume), suggests that the release of As is linked to the transformation of predominantly Fe (III) oxyhydroxide coatings on sand particles to Fe(II) or mixed Fe(II/III) solid phases with a flatter reflectance spectrum such as siderite, vivianite, or magnetite, without necessarily resulting in the release of Fe to groundwater. The very low As/Fe ratio of magnetically separated minerals compared to the As/Fe of bulk acid leachate (2 vs. 40 10−6, respectively) suggests that such a transformation could be accompanied by a significant redistribution of As to a mobilizable phase on the surface of aquifer particles.  相似文献   

13.
On the basis of investigations on the composition and contents of heavy metals in the domestic refuse in the Three-Gorges region of the Yangtze River, in combination with the experimental results, this paper deals with the distribution rule of heavy metals in the various compartments of an incineration system: leachate pool, fly ash and residue. It is concluded that in the leachate pool heavy metals should not be neglectable since about 30% of Pb and 10% of Cr are leached here; in the incineration system, above 74% of Cr, As and Pb exists in residue; above 96% of Hg exists in fly ash and the contents of Cd in fly ash are close to those of residue. It is also concluded that the physical conditions of incineration have a significant influence on the distribution of heavy metals in the incineration system.  相似文献   

14.
《Applied Geochemistry》1998,13(2):213-233
Porewater concentration profiles were determined for Fe, trace elements (As, Cd, Co, Cu, Mn, Ni, Pb, Zn), sulfide, SO4 and pH in two Canadian Shield lakes (Chevreuil and Clearwater). Profiles of pyrite, sedimentary trace elements associated with pyrite and AVS were also obtained at the same sites. Thermodynamic calculations are used, for the anoxic porewaters where sulfide was measured, to characterize diagenetic processes involving sulfide and trace elements and to illustrate the importance of sulfide, and possibly polysulfides and thiols, in binding trace elements. The ion activity products (IAP) of Fe sulfide agree with the solubility products (Ks) of greigite or mackinawite. For Co, Ni and Zn, IAP values are close to the KS values of their sulfide precipitates; for Cu and Pb, IAP/Ks indicate large oversaturations, which can be explained by the presence of other ligands (not measured) such as polysulfides (Cu) and thiols (Pb). Cobalt, Cu, Ni and Zn porewater profiles generally display a decrease in concentration with increasing ΣH2S, as expected for transition metals, whereas Cd, Pb and Zn show an increase (mobilisation). The results suggest that removal of trace elements from anoxic porewaters occurs by coprecipitation (As and Mn) with FeS(s) and/or adsorption (As and Mn) on FeS(s), and by formation of discrete solid sulfides (Cd, Cu, Ni, Pb, Zn and Co). Reactive Fe is extensively sulfidized (51–65%) in both lakes, mostly as pyrite, but also as AVS. Similarities between As, Co, Cu and Ni to Fe ratios in pyrite and their corresponding mean diffusive flux ratios suggest that pyrite is an important sink at depth for these trace elements. High molar ratios of trace elements to Fe in pyrite from Clearwater Lake correspond chronologically to the onset of smelting activities. AVS can be an important reservoir of reactive As, Cd and Ni and, to a lesser extent, of Co, Cu and Pb. Overall, the trace elements most extensively sulfidized were Ni, Cd and As (maximum of 100%, 81% and 49% of the reactive fraction, respectively), whereas Co, Cu, Mn, Pb and Zn were only moderately sulfidized (11–16%).  相似文献   

15.
The purpose of this work is to characterize the hydrochemical behavior of acid mine drainages (AMD) and superficial waters from the Adoria mine area (Northern Portugal). Samples of superficial and mine drainage water were collected for one year, bi-monthly, with pH, temperature, Eh, conductivity and HCO3 determined in situ with chemical analyses of SO4, Ca, K, Mg, Na, Cl, Ag, As, Bi, Co, Cu, Fe, Mn, Ni, Pb, Zn and Cd. In the mine, there are acidic waters, with low pH and significant concentrations of SO4, and metals (Fe, Mn, Zn, Cu, Pb, Cd and Ni), while in the superficial natural stream waters outside the mine, the pH is close to neutral, with low conductivity and lower metal concentrations. The stream waters inside the mine influence are intermediate in composition between AMD and natural stream waters outside the mine influence. Principal Component Analysis (PCA) shows a clear separation between AMD galleries and AMD tailings, with tailings having a greater level of contamination.  相似文献   

16.
Scorodite, ferric arsenate and arsenical ferrihydrite are important arsenic carriers occurring in a wide range of environments and are also common precipitates used by metallurgical industries to control arsenic in effluents. Solubility and stability of these compounds are controversial because of the complexities in their identification and characterization in heterogeneous media. To provide insights into the formation of scorodite, ferric arsenate and ferrihydrite, series of synthesis experiments were carried out at 70 °C and pH 1, 2, 3 and 4.5 from 0.2 M Fe(SO4)1.5 solutions also containing 0.02-0.2 M Na2HAsO4. The precipitates were characterized by transmission electron microscopy, X-ray diffraction and X-ray absorption fine structure techniques. Ferric arsenate, characterized by two broad diffuse peaks on the XRD pattern and having the structural formula of FeAsO4·4-7H2O, is a precursor to scorodite formation. As defined by As XAFS and Fe XAFS, the local structure of ferric arsenate is profoundly different than that of scorodite. It is postulated that the ferric arsenate structure is made of single chains of corner-sharing Fe(O,OH)6 octahedra with bridging arsenate tetrahedra alternating along the chains. Scorodite was precipitated from solutions with Fe/As molar ratios of 1 over the pH range of 1-4.5. The pH strongly controls the kinetics of scorodite formation and its transformation from ferric arsenate. The scorodite crystallite size increased from 7 to 33 nm by ripening and aggregation. Precipitates, resulting from continuous synthesis at pH 4.5 from solutions having Fe/As molar ratios ranging from 1 to 4 and resembling the compounds referred to as ferric arsenate, arsenical ferrihydrite and As-rich hydrous ferric oxide in the literature, represent variable mixtures of ferric arsenate and ferrihydrite. When the Fe/As ratio increases, the proportion of ferrihydrite increases at the expense of ferric arsenate. Arsenate adsorption appears to retard ferrihydrite growth in the precipitates with molar Fe/As ratios of 1-4, whereas increased reaction gradually transforms two-line ferrihydrite to six-line ferrihydrite at Fe/As ratios of 5 and greater.  相似文献   

17.
The distribution of arsenic (As) in shallow groundwater of eastern Chancheng District in Foshan City as a function of season and water table was investigated, and the influence of hydrochemical factors on the As distribution was discussed. The groundwater samples were collected from 20 sites in dry season and 9 sites in wet season. As concentrations in 20% groundwater samples exceeded value of the WHO guideline (10 μg/L), and the highest As concentration of 23.5 μg/L occurred in dry season. It is observed that groundwater As concentration decreased with the increase of depth of water table in dry season, and were generally higher in wet season than that in dry season, indicating that ground surface As might be one of the main sources for shallow groundwater As in study area, especially in wet season. Groundwater As concentration in study area had significantly positive correlation with the concentration of Fe, Mn, NH4, F, and COD, and was positively correlated to pH, but negatively correlated to Eh and K, indicating that reductive dissolution of Fe and Mn (oxy)hydroxides might be one of the main control mechanisms for groundwater As mobilization, while pH and F also played an important role in controlling the groundwater As mobilization in study area.  相似文献   

18.
The degree of metal contamination (Zn, Pb, Cu, Ni, Cd) has been investigated in the vicinity of an old unmonitored municipal landfill in Prague, Czech Republic, where the leachate is directly drained into a surface stream. The water chemistry was coupled with investigation of the stream sediment (aqua regia extract, sequential extraction, voltammetry of microparticles) and newly formed products (SEM/EDS, XRD). The MINTEQA2 speciation-solubility calculation showed that the metals (Zn, Pb, Cu, Ni) are mainly present as carbonate complexes in leachate-polluted surface waters. These waters were oversaturated with respect to Fe(III) oxyhydroxides, calcite (CaCO3) and other carbonate phases. Three metal attenuation mechanisms were identified in leachate-polluted surface waters: (i) spontaneous precipitation of metal-bearing calcite exhibiting significant concentrations of trace elements (Fe, Mn, Mg, Sr, Ba, Pb, Zn, Ni); (ii) binding to Fe(III) oxyhydroxides (mainly goethite, FeOOH) (Pb, Zn, Cu, Ni); and (iii) preferential bonding to sediment organic matter (Cu). These processes act as the key scavenging mechanisms and significantly decrease the metal concentrations in leachate-polluted water within 200 m from the direct leachate outflow into the stream. Under the near-neutral conditions governing the sediment/water interface in the landfill environment, metals are strongly bound in the stream sediment and remain relatively immobile.  相似文献   

19.
Reducing heavy metal concentrations to allowable levels in landfill leachate before discharge is an extremely important process to prevent environmental pollution. Iron oxide-coated gravel was used in order to remove Cd(II), Cu(II), Pb(II), Fe(III) and Al(III) simultaneously in high-strength synthetic leachate samples. Batch and column studies were performed to determine the kinetics and mechanism of adsorption process. The experimental data obtained from batch study satisfactorily fitted to the Freundlich model indicating surface heterogeneity and multilayer adsorption process. The data obtained from kinetic studies followed the pseudo-second-order kinetics indicating adsorption governed by chemisorption. The metal adsorption order observed in the batch study was Pb(II)(99.72%) ≈ Cu(II)(99.61%) ≈ Cd(II)(99.51%) ≈ Fe(III)(99.3%) > Al(III)(93.3%) at pH 7. Average metal removals in the fixed-bed column were found to be 96.5% for Cu(II), 94.8% for Pb(II), 90% for Cd(II), 84% for Fe(III) and 67% for Al(III). Iron oxide-coated gravel column adsorption capacity ranged from 0.56 to 66.82 mg/g. Recovery efficiency of adsorbed metals via desorption was between 5–97.75% in first cycle and 2–80.3% in second cycle.  相似文献   

20.
X-ray absorption fine structure (XAFS) is used to characterize the mineralogy of the iron(III)-arsenate(V) precipitates produced during the raffinate (aqueous effluent) neutralization process at the McClean Lake uranium mill in northern Saskatchewan, Canada. To facilitate the structural characterization of the precipitated solids derived from the neutralized raffinate, a set of reference compounds were synthesized and analyzed. The reference compounds include crystalline scorodite, poorly-crystalline scorodite, iron(III)-arsenate co-precipitates obtained under different pH conditions, and arsenate-adsorbed on goethite. The poorly-crystalline scorodite (prepared at pH 4 with Fe/As = 1) has similar As local structure as that of crystalline scorodite. Both As and Fe K-edge XAFS of poorly-crystalline scorodite yield consistent results on As-Fe (or Fe-As) shell. From As K-edge analysis the As-Fe shell has an inter-atomic distance of 3.33 ± 0.02 Å and coordination number of 3.2; while from Fe K-edge analysis the Fe-As distance and coordination number are 3.31 ± 0.02 Å and 3.8, respectively. These are in contrast with the typical arsenate adsorption on bidentate binuclear sites on goethite surfaces, where the As-Fe distance is 3.26 ± 0.03 Å and coordination number is close to 2. A similar local structure identified in the poorly-crystalline scorodite is also found in co-precipitation solids (Fe(III)/As(V) = 3) when precipitated at the same pH (pH = 4): As-Fe distance 3.30 ± 0.03 Å and coordination number 3.9; while at pH = 8 the co-precipitate has As-Fe distance of 3.27 ± 0.03 Å and coordination number about 2, resembling more closely the adsorption case. The As local structure in the two neutralized raffinate solid series (precipitated at pH values up to 7) closely resembles that in the poorly-crystalline scorodite. All of the raffinate solids have the same As-Fe inter-atomic distance as that in the poorly-crystalline scorodite, and a systematic decrease in the As-Fe coordination is observed when pH is progressively increased; the basic poorly-crystalline scorodite structural feature remains in the raffinate solid up to pH 7.  相似文献   

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