首页 | 本学科首页   官方微博 | 高级检索  
相似文献
 共查询到20条相似文献，搜索用时 31 毫秒
1.
《Applied Geochemistry》2005,20(2):383-396
Potential contamination of rivers by trace elements can be controlled, among others, by the precipitation of oxyhydroxides. The streambed of the studied area, located in “La Châtaigneraie” district (Lot River Basin, France), is characterised by iron-rich ochreous deposits, acidic pH (2.7–4.8) and SO4–Mg waters. Beyond the acid mine drainage, the presence of As both in the dissolved fraction and in the deposits is also a problem. Upstream, at the gallery outlet, As concentrations are high (Asmax = 2.6 μmol/l and up to 5 wt% locally, respectively, in the dissolved and in the solid fractions). Downstream, As concentrations decrease below 0.1 μmol/l in the dissolved fraction and to 1327 mg/kg in the solid fraction. This natural attenuation is related to the As retention within ochreous precipitates (amorphous to poorly crystalline Fe oxyhydroxides, schwertmannite and goethite), which have great affinities for this metalloid. Upstream, schwertmannite is dominant while downstream, goethite becomes the main mineral. The transformation of schwertmannite into goethite is observed in the upstream deposits as schwertmannite is unstable relative to goethite. Furthermore, thermodynamic calculations indicate that the downstream goethite is not able to precipitate in situ according to the water chemistry. Goethite mainly results from the transformation of schwertmannite and its solid transport downstream.Moreover, as highlighted by leaching experiments carried out on the ochreous precipitates, this transformation does not seem to affect the As-retention in solids as no release of As was observed in the solution. Arsenic may either be strongly trapped by co-precipitation in the present minerals or it may be quickly released and re-adsorbed on the precipitate surface.  相似文献   

2.

Sulfide‐rich materials comprising the waste at the abandoned Montalbion silver mine have undergone extensive oxidation prior to and after mining. Weathering has led to the development of an abundant and varied secondary mineral assemblage throughout the waste material. Post‐mining minerals are dominantly metal and/or alkali (hydrous) sulfates, and generally occur as earthy encrustations or floury dustings on the surface of other mineral grains. The variable solubility of these efflorescences combined with the irregular rainfall controls the chemistry of seepage waters emanating from the waste dumps. Irregular rainfall events dissolve the soluble efflorescences that have built up during dry periods, resulting in ‘first‐flush’ acid (pH 2.6–3.8) waters with elevated sulfate, Fe, Cu and Zn contents. Less‐soluble efflorescences, such as anglesite and plumbojarosite, retain Pb in the waste dump. Metal‐rich (Al, Cd, Co, Cu, Fe, Mn, Ni, Zn) acid mine drainage waters enter the local creek system. Oxygenation and hydrolysis of Fe lead to the formation of Fe‐rich precipitates (schwertmannite, goethite, amorphous Fe compounds) that, through adsorption and coprecipitation, preferentially incorporate As, Sb and In. Furthermore, during dry periods, evaporative precipitation of hydrous alkali and metal sulfate efflorescences occurs on the perimeter of stagnant pools. Flushing of the streambed by neutral pH waters during heavy rainfall events dissolves the efflorescences resulting in remobilisation and transport of sulfate and metals (particularly Cd, Zn) downstream. Thus, in areas of seasonal or irregular rainfall, secondary efflorescent minerals present in waste materials or drainage channels have an important influence on the chemistry of surface waters.  相似文献   

3.
Schwertmannite is a ubiquitous mineral formed from acid rock drainage (ARD), and plays a major role in controlling the water chemistry of many acid streams. The formation of schwertmannite was investigated in the acid discharge of the Monte Romero abandoned mine (Iberian Pyrite Belt, SW, Spain). Schwertmannite precipitated from supersaturated solutions mainly owing to the oxidation of Fe(II) to Fe(III) and transformed with time into goethite and jarosite. In a few hours, schwertmannite precipitation removed more than half of the arsenic load from solution, whereas the concentration of divalent trace metals (Zn, Cu, Pb, Cd, Ni, and Co) remained almost unchanged. In the laboratory, natural schwertmannite was kept in contact with its coexisting acid water in a flask with a solid-liquid mass ratio of 1:5 for 353 days. During this time, the pH of the solution dropped from 3.07 to 1.74 and the concentrations of sulfate and Fe increased. During the first 164 days, schwertmannite transformed into goethite plus H3O-jarosite but, subsequently, goethite was the only mineral to form. Some of the trace elements, such as Al, Cu, Pb, and As were depleted in solution during the first stage as schwertmannite transformed into goethite plus H3O-jarosite. On the contrary, the transformation of schwertmannite to goethite (with no jarosite) during the second stage released Al, Cu, and As to the solution. Despite the variation in their concentrations in solution, approximately 80% of the total Al and Cu inventories and more than 99% As and Pb remained in the solid phase throughout the entire aging process.  相似文献   

4.
The mineralogical and chemical evolution of ochreous precipitates forming from acid mine drainage (AMD) from the abandoned Libiola Fe–Cu-sulfide mine (Eastern Liguria, Italy) was followed through a multianalytical approach (XRD, TEM, XRF, ICP) applied to surface precipitates and associated waters collected from several mine adits. The mineralogy of the precipitates changed significantly as a consequence of the variations of the chemical parameters of the circulating solutions (mainly pH, Eh, and sulfate concentrations) which, in turn, were mainly controlled by mixing with unpolluted stream and rill waters of the mining area. A progressive transition from jarosite-, to schwertmannite-, to goethite-, to ferrihydrite-, to amorphous-dominated precipitates was observed, mainly as a consequence of an increase in the pH of the associated solutions. This mineralogical evolution agrees well with the aqueous speciation and Eh–pH stability calculations performed on the waters associated with the different precipitate types. Furthermore, TEM analysis indicated that metastable pristine phases (schwertmannite) tend to transform progressively to well-crystallized more stable species, here represented by goethite. The comparison of the water chemistry and the crystal chemistry of the different precipitates showed a significant decrease in the Zn, Cu, Ni, Co contents in waters where the coexisting precipitates were almost exclusively composed of goethite. The distribution of V, Sr, As concentrations within the different precipitates showed that the most efficient scavenging phase for these elements was jarosite, whereas ferrihydrite efficiently took up Pb ions, and schwermannite acted as a natural sink for Cr.  相似文献   

5.
Simultaneous analysis of micro-X-ray diffraction (μ-XRD) and micro-X-ray fluorescence (μ-XRF) based on synchrotron light sources, and electron microprobe (EMP) analyses, were performed on iron terrace samples taken from Tinto-Odiel river system from the Iberian Pyrite Belt (IBP, SW Iberian Peninsula). Iron terraces are formed during the oxidation and precipitation of dissolved iron along the riverbeds impacted by acid mine drainage (AMD). This paper includes the study of actively-forming current terraces and fossil terraces isolated from the stream courses due to the river migration over time. The results of the study of current terrace samples from AMD-affected streams of two IPB abandoned mines (Tinto Santa Rosa and Cueva de la Mora) showed that fresh precipitates at the surface are composed primarily of metastable schwertmannite, which is gradually transformed at depth over short-time scales into goethite. Sediments of ancient terraces are composed mainly of goethite, which most likely originated from the re-crystallization of a precursor schwertmannite. However, at century-time scale, goethite partially re-crystallizes to hematite due to diagenetic processes. The transformation rate of goethite into hematite is negatively correlated with grain size and the crystallinity of goethite. Moreover, this transformation is accompanied by an increase in grain size and a decrease in surface area of hematite, and a concomitant decrease in arsenic trapped in the solid. This increase in the arsenic mobility during the diagenetic maturation should be considered in the development of conceptual and analytical models describing long-term fate, transport and bioavailability of arsenic in environmental systems.  相似文献   

6.
《Applied Geochemistry》2007,22(4):760-777
Ochreous precipitate and water samples were collected from the surroundings of seven closed sulphide mines in Finland. In the Hammaslahti Zn–Cu–Au mine, Otravaara pyrite mine and Paroistenjärvi Cu–W–As mine, the collection was repeated in different seasons to study mineralogical and geochemical variations of precipitates. The sampling was done in 1999–2002 from the ditches and drainage ponds of the tailings and waste rock piles that are susceptible to seasonal changes. Mineralogy of the precipitates was evaluated by X-ray diffraction (XRD) and infrared spectroscopy (IR), and precipitate geochemistry was examined by selective extractions. Schwertmannite (Fe8O8(OH)6SO4) was the most typical Fe hydroxide mineral found. Goethite was almost as common as schwertmannite, was often poorly ordered, and contained up to 10 wt.% of SO4. Goethite and schwertmannite were commonly found as mixtures, and they occurred in similar pH and SO4 concentrations. Ferrihydrite (nominally Fe5HO8 · 4H2O) was typically found in areas not influenced by acid mine drainage, and also in acid mine waters with high organic matter or As content. Jarosite (KFe3(SO4)2(OH)6) was found only in one site. In addition, some gypsum (CaSO4 · 2H2O) and aluminous sulphate precipitates (presumably basaluminite, Al4(SO4)(OH)10 · 5H2O) were identified. Selective extractions showed that acid extracts Fetot/Stot-ratios of schwertmannite and goethite samples were similar, but the ratio of oxalate-extractable to total Fe, Feox/Fetot, of goethite samples were lower than those of the schwertmannite samples. Only Al, Si and As were bound to precipitates in substantial amounts, up to several wt.%. In schwertmannites and goethites, Al, Cu, Co, Mn and Zn were mostly structural, substituting for Fe in an Fe oxyhydroxide structure or bound to surface adsorption sites in pores limited by diffusion. In ferrihydrites, heavy metals were also partly bound in adsorbed form dissolving in acid ammonium acetate. Ferrihydrites and goethites were more enriched in Co, Mn and Zn than schwertmannites, but schwertmannites and ferrihydrites were more enriched in As than goethites. Mineralogical and geochemical evidence showed that in the spring, after the snowmelt, the acid mine drainage precipitates were predominantly schwertmannite, and were partly transformed during warm summer months to goethite. The phase transformation of precipitates was followed by a decrease in pH values and increase in SO4 concentrations of waters. Adsorbed As retarded the phase transformation.  相似文献   

7.
This work focuses on the geochemical processes taking place in the acid drainage in the Ribeira da Água Forte, located in the Aljustrel mining area in the Iberian Pyrite Belt. The approach involved water and stream sediment geochemical analyses, as well as other techniques such as sequential extraction, Mössbauer spectroscopy, and X-ray diffraction. Ribeira da Água Forte is a stream that drains the area of the old mine dumps of the Aljustrel mine, which have for decades been a source of acid waters. This stream flows to the north for a little over than 10 km, but mixes with a reduced, organic-rich, high pH waste water from the municipal waste water pools of the village. This water input produces two different results in the chemistry of the stream depending upon the season: (i) in the winter season, effective water mixing takes place, and the flux of acid water from the mine dumps is continuous, resulting in the immediate precipitation of the Fe from the acid waters; (ii) during the summer season, acid drainage is interrupted and only the waste water feeds the stream, resulting in the reductive dissolution of Fe hydroxides and hydroxysulfates in the stream sediments, releasing significant quantities of metals into solution. Throughout the year, water pH stays invariably within 4.0–4.5 for several meters downstream of this mixing zone even when the source waters come from the waste water pools, which have a pH around 8.4. The coupled interplay of dissolution and precipitation of the secondary minerals (hydroxides and sulfates), keeps the system pH between 3.9 and 4.5 all along the stream. In particular, evidence suggests that schwertmannite may be precipitating and later decomposing into Fe hydroxides to sustain the stream water pH at those levels. While Fe content decreases by 50% from solution, the most important trace metals are only slightly attenuated before the solution mixes with the Ribeira do Rôxo stream waters. Concentrations of As are the only ones effectively reduced along the flow path. Partitioning of Cu, Zn and Pb in the contaminated sediments also showed different behavior. Specific/non-specific adsorption is relevant for Cu and Zn in the upstream branch of Ribeira da Água Forte with acid drainage conditions, whereas the mixture with the waste water causes that the association of these metals with oxyhydroxide to be more important. Metals bound to oxyhydroxides are on the order of 60–70% for Pb, 50% for Cu and 30–60% for Zn. Organic matter is only marginally important around the waste water input area showing 2–8% Cu bound to this phase. These results also show that, although the mixing process of both acid and organic-rich waters can suppress and briefly mitigate some adverse effects of acid drainage, the continuing discharge of these waste waters into a dry stream promotes the remobilization of metals fixed in the secondary solid phases in the stream bed back into solution, a situation that can hardly be amended back to its original state.  相似文献   

8.
酸性矿山废水(acid mine drainage,AMD)是一类pH低并含有大量有毒金属元素的废水。AMD及受其影响的环境中次生高铁矿物类型主要包括羟基硫酸高铁矿物(如黄铁矾和施威特曼石等)和一些含水氧化铁矿物(如针铁矿和水铁矿等),而且这些矿物在不同条件下会发生相转变,如施氏矿物向针铁矿或黄铁矾矿物相转化。基于酸性环境中生物成因次生矿物的形成会"自然钝化"或"清除"废水中铁和有毒金属这一现象所获得的启示,提出利用这些矿物作为环境吸附材料去除地下水中砷,不但吸附量大(如施氏矿物对As的吸附可高达120mg/g),而且可直接吸附As(III),还几乎不受地下水中其他元素影响。利用AMD环境中羟基硫酸高铁矿物形成的原理,可将其应用于AMD石灰中和主动处理系统中,构成"强化微生物氧化诱导成矿-石灰中和"的联合主动处理系统,以提高AMD处理效果和降低石灰用量。利用微生物强化氧化与次生矿物晶体不断生长的原理构筑生物渗透性反应墙(PRB)并和石灰石渗透沟渠耦联,形成新型的AMD联合被动处理系统,这将有助于大幅度增加处理系统的寿命和处理效率。此外,文中还探讨了上述生物成因矿物形成在AMD和地下水处理方面应用的优点以及今后需要继续研究的问题。  相似文献   

9.
Oxidation of mackinawite (FeS) and concurrent mobilization of arsenic were investigated as a function of pH under oxidizing conditions. At acidic pH, FeS oxidation is mainly initiated by the proton-promoted dissolution, which results in the release of Fe(II) and sulfide in the solution. While most of dissolved sulfide is volatilized before being oxidized, dissolved Fe(II) is oxidized into green rust-like precipitates and goethite (α-FeOOH). At basic pH, the development of Fe(III) (oxyhydr)oxide coating on the FeS surface inhibits the solution-phase oxidation following FeS dissolution. Instead, FeS is mostly oxidized into lepidocrocite (γ-FeOOH) via the surface-mediated oxidation without dissolution. At neutral pH, FeS is oxidized via both the solution-phase oxidation following FeS dissolution and the surface-mediated oxidation mechanisms. The mobilization of arsenic during FeS oxidation is strongly affected by FeS oxidation mechanisms. At acidic pH (and to some extent at neutral pH), the rapid FeS dissolution and the slow precipitation of Fe (oxyhydr)oxides results in arsenic accumulation in water. In contrast, the surface-mediated oxidation of FeS at basic pH leads to the direct formation of Fe (oxyhydr)oxides, which provides effective adsorbents for As under oxic conditions. At acidic and neutral pH, the solution-phase oxidation of dissolved Fe(II) accelerates the oxidation of the less adsorbing As(III) to the more adsorbing As(V). This study reveals that the oxidative mobilization of As may be a significant pathway for arsenic enrichment of porewaters in sulfidic sediments.  相似文献   

10.
《Applied Geochemistry》2002,17(10):1273-1286
The pH of mine impacted waters was estimated from the spectral reflectance of resident sediments composed mostly of chemical precipitates. Mine drainage sediments were collected from sites in the Anthracite Region of eastern Pennsylvania, representing acid to near neutral pH. Sediments occurring in acidic waters contained primarily schwertmannite and goethite while near neutral waters produced ferrihydrite. The minerals comprising the sediments occurring at each pH mode were spectrally separable. Spectral angle difference mapping was used to correlate sediment color with stream water pH (r2=0.76). Band-center and band-depth analysis of spectral absorption features were also used to discriminate ferrihydrite and goethite and/or schwertmannite by analyzing the 4T1←6A1 crystal field transition (900–1000 nm). The presence of these minerals accurately predicted stream water pH (r2=0.87) and provided a qualitative estimate of dissolved SO4 concentrations. Spectral analysis results were used to analyze airborne digital multispectral video (DMSV) imagery for several sites in the region. The high spatial resolution of the DMSV sensor allowed for precise mapping of the mine drainage sediments. The results from this study indicate that airborne and space-borne imaging spectrometers may be used to accurately classify streams impacted by acid vs. neutral-to-alkaline mine drainage after appropriate spectral libraries are developed.  相似文献   

11.
煤矿酸性水中亚稳态矿物Schwertmannite的形成与转变   总被引：1，自引：0，他引：1  
斯沃特曼矿是一种形成于煤矿酸性水环境中的铁的含水硫酸盐矿物,具有很高的比表面积和不稳定性,对煤矿酸性水中有害微量元素的吸附和迁移活性具有重要影响。运用扫描电镜(SEM/EDX)和粉末X射线衍射等手段,通过测定和对比,鉴别了中国的煤矿酸性矿排水渠中存在斯沃特曼矿物,在实验室中模拟酸性水环境对煤中非均质黄铁矿进行氧化反应试验,结果显示,反应产物中存在斯沃特曼矿物,并且认为随着反应时间的延长,斯沃特曼矿物逐渐向针铁矿转变。  相似文献   

12.
Abstract: To determine the geochemical characteristics of the Imgok creek impacted by acid mine drainage (AMD) generated from the abandoned Youngdong coal mine in Korea, chemical analyses of water samples and precipitates and the geochemical modelling of the precipitates were conducted. Acid mine drainage drained from the mine adit and coal refuse piles shows a low pH, high conductivity and high concentrations of Fe, Al, SO4 and heavy metals such as Co, Cu, Ni and Zn. In the Imgok creek, the concentrations of heavy metals and major cations besides Fe are decreased by dilution, but concentrations of Fe are decreased by the formation of precipitates as well as dilution. From the results of geochemical modelling, goethite is oversaturated, and schwertmannite is the most stable solid phase in the Imgok creek. Yellowish red Fe-precipitates collected at the Imgok creek are recognized as amorphous or poorly crystallized minerals from XRD patterns and Feox/Fetotratios, and as containing chemically bonded SO4 and OH by an IR analysis. The mole ratios of Fe/S in these precipitates, which are determined by EPMA, are 5. 1 and 6. 1.  相似文献   

13.
《Applied Geochemistry》2002,17(8):1081-1092
Different types of fine-grained chemical precipitates were characterized in the surroundings of the pyrite-chalcopyrite mine of Libiola (Northern Italy). Both water chemistry and sediment composition were used to investigate metal mobility near the mine area. Local drainage waters were very acidic (with a pH as low as 2.5) and were rich in dissolved metals (Fe, Al, Cu, Zn, Mn, Ni). Sediments associated with low pH water (pH <4.5) were ochreous mixtures of schwertmannite and goethite with traces of jarosite. Their chemistry was dominated by Fe and they had, compared to other sediments investigated, low concentrations of other metals. When the acidity decreased gradually, other precipitates formed. At a pH of approximately 5, a poorly crystalline, whitish, Al-rich precipitate occurred. At a pH between 6 and 7, a poorly crystalline, blue, Cu (Zn) rich phase was present. These “sequential” precipitation events progressively reduced the metal loading typical of the acidic mine water when there was a gradual mixing with normal water. When a sudden mixing between normal waters (pH ∼8, Ca–HCO3, low metal bearing) and acidic waters took place, a rapid flocculation occurred of mixed precipitates containing Fe, Al and trace elements.  相似文献   

14.
Acid mine drainage discharged from the abandoned Daduk mine towards the Daduk creek has a pH of 3.3, and concentrations of Al, Mn, Fe, Zn and SO4 of 18, 41, 45, 38 and 1940 mg/L, respectively. In particular, As concentration in acid mine drainage is 1000 μg/L. Removing order of metal ions normalized by SO4 concentration downstream from discharge point is Fe > As > Al > Cu > Zn > Mn > Cd > Pb. In the Daduk creek, Fe and As are the most rapidly depleted downstream from acid mine drainage because As adsorbs, coprecipitates and forms compounds with ferric oxyhydroxide. From the results of geochemical modeling using the Phreeq C program, goethite (FeOOH) is oversaturated, and schwertmannite (Fe8O8(OH)4.5(SO4)1.75) is the most stable solid phase at low pH in the Daduk creek. Yellowish red (orange ochre) precipitates that occurred in the study area are probably composed of goethite or schwertmannite.  相似文献   

15.
This paper reports the results of a laboratory experiment conducted to investigate the effects of wollastonite dissolution on removal of potentially toxic trace elements from stream waters affected by acid mine drainage (AMD). Nearly pure wollastonite was treated with natural acid mine water (pH 2.1) for different lengths of time (15, 30, 50 and 80 days). The compositional and textural characterization of the solid reaction products suggests that wollastonite was incongruently dissolved leaving a residual amorphous silica-rich phase that preserved the prismatic morphology of the parent wollastonite. The release of Ca into solution resulted in a pH increase from 2.1 to 3.5, and subsequent precipitation of gypsum as well as poorly crystallized Fe–Al oxy-hydroxides and oxy-hydroxysulfates whose components derived from the AMD solution. A geochemical modeling approach of the wollastonite–AMD interaction using the PHREEQC code indicated supersaturation with respect to schwertmannite (saturation index = 10.7–15.7), jarosite (SI = 8.7–10.2), alunite (SI = 5.1), goethite (SI = 4.7) and jurbanite (SI = 2.2). These secondary phases developed a thin coating on the reacted wollastonite surface, readily cracked and flaked off upon drying, that acted as a sink for trace elements, especially As, Cu and Zn, as indicated by their enrichment relative to the starting wollastonite. At such low pH values, adsorption of As oxyanions on the positively charged solid particles and coprecipitation of metals (mainly Cu and Zn) with the newly formed Fe oxy-hydroxides and oxy-hydroxysulfates seem to be the dominant processes controlling the removal of trace elements.  相似文献   

16.
Oxidation of As(III) by natural manganese (hydr)oxides is an important geochemical reaction mediating the transformation of highly concentrated As(III) in the acidic environment such as acid mine drainage (AMD) and industrial As-contaminated wastewater, however, little is known regarding the presence of dissolved Fe(II) on the oxidation process. In this study, oxidation of As(III) in the absence and presence of Fe(II) by MnO2 under acidic conditions was investigated. Kinetic results showed that the presence of Fe(II) significantly inhibited the removal of As(III) (including oxidation and sorption) by MnO2 in As(III)-Fe(II) simultaneous oxidation system even at the molar ratio of Fe(II):As(III) = 1/64:1, and the inhibitory effects increased with the increasing ratios of Fe(II):As(III). Such an inhibition could be attributed to the formation of Fe(III) compounds covering the surface of MnO2 and thus preventing the oxidizing sites available to As(III). On the other hand, the produced Fe(III) compounds adsorbed more As(III) and the oxidized As(V) on the MnO2 surface with an increasing ratio of Fe(II):As(III) as demonstrated in kinetic and XPS results. TEM and EDX results confirmed the formation of Fe compounds around MnO2 particles or separated in solution in Fe(II) individual oxidation system, Fe(II) pre-treated and simultaneous oxidation processes, and schwertmannite was detected in Fe(II) individual and Fe pre-treated oxidation processes, while a new kind of mineral, probably amorphous FeOHAs or FeAsO4 particles were detected in Fe(II)-As(III) simultaneous oxidation process. This suggests that the mechanisms are different in Fe pre-treated and simultaneous oxidation processes. In the Fe pre-treated and MnO2-mediated oxidation pathway, As(III) diffused through a schwertmannite coating formed around MnO2 particles to be oxidized. The newly formed As(V) was adsorbed onto the schwertmannite coating until its sorption capacity was exceeded. Arsenic(V) then diffused out of the coating and was released into the bulk solution. The diffusion into the schwertmannite coating and the oxidation of As(III) and sorption of both As(V) and As(III) onto the coating contributed to the removal of total As from the solution phase. In the simultaneous oxidation pathway, the competitive oxidation of Fe(II) and As(III) on MnO2 occurred first, followed by the formation of FeOHAs or FeAsO4 around MnO2 particles, and these poorly crystalline particles of FeOHAs and FeAsO4 remained suspended in the bulk solution to adsorb As(III) and As(V). The present study reveals that the formation of Fe(III) compounds on mineral surfaces play an important role in the sorption and oxidation of As(III) by MnO2 under acidic conditions in natural environments, and the mechanisms involved in the oxidation of As(III) depend upon how Fe(II) is introduced into the As(III)-MnO2 system.  相似文献   

17.
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   

18.
Schwertmannite stability in acidified coastal environments   总被引：1，自引：0，他引：1  
A combination of analytical and field measurements has been used to probe the speciation and cycling of iron in coastal lowland acid sulfate soils. Iron K-edge EXAFS spectroscopy demonstrated that schwertmannite dominated (43-77%) secondary iron mineralization throughout the oxidized and acidified soil profile, while pyrite and illite were the major iron-bearing minerals in the reduced potential acid sulfate soil layers. Analyses of contemporary precipitates from shallow acid sulfate soil groundwaters indicated that 2-line ferrihydrite, in addition to schwertmannite, is presently controlling secondary Fe(III) mineralization. Although aqueous pH values and concentrations of Fe(II) were seasonally high, no evidence was obtained for the Fe(II)-catalyzed crystallization of either mineral to goethite. The results of this study indicate that: (a) schwertmannite is likely to persist in coastal lowland acid sulfate soils on a much longer time-scale than predicted by laboratory experiments; (b) this mineral is less reactive in these types of soils due to surface-site coverage by components such as silicate and possibly, to a lesser extent, natural organic matter and phosphate and; (c) active water table management to promote oxic/anoxic cycles around the Fe(II)-Fe(III) redox couple, or reflooding of these soils, will be ineffective in promoting the Fe(II)-catalyzed transformation of either schwertmannite or 2-line ferrihydrite to crystalline iron oxyhydroxides.  相似文献   

19.
Mining residues from the Sb mine of Bournac in the upper Orb River valley (Southern France), constitute an important source of As and Sb pollution. Arsenic concentrations are as high as 78 μg/L and Sb reaches 32 μg/L in the small creek draining the tailings impoundment. Although both metalloids occur mainly in oxidized form in the creek water, their behaviour differs significantly. Iron oxides are the main carrier phases for both elements in the suspended particulate matter. In oxic conditions the two elements are mainly present in water in oxidised form As(V) and Sb(V) and both field studies and laboratory experiments indicate a higher affinity of As(V) than Sb(V) for the solid phase. In the pool, which receives the water from Bournac Creek, the reductive dissolution of Fe-oxides is linked to the oxidation of small pyrite grains transported from the tailings dump. In oxic conditions Sb is released to solution more efficiently than As. Conversely, in anoxic conditions, mobilisation of As is greater than that of Sb. This is attributed to the reduction of As, which favours its mobility. Whatever the conditions, the activity of bacteria naturally present in the sediments enhances the remobilization of Sb in oxidizing conditions and that of As in reducing conditions.  相似文献   

20.
酸性条件下Fe(II)的生物氧化过程可以被有效应用于煤矿酸性矿井水修复中,但是Fe行为与归宿的不确定性增加了应用难度。本研究通过对某煤矿酸性矿井水场地发生的生物地球化学过程进行监测,富集培养场地沉积物嗜酸微生物群落,进行室内恒化生物反应器连续流实验,探究微生物作用下Fe及其他金属离子的行为与归宿。研究表明,Fe的形态转化是场地和反应器中最主要的生物地球化学过程。当pH<2.7时,反应更倾向于产生溶解性Fe(III);当2.7相似文献   

设为首页 | 免责声明 | 关于勤云 | 加入收藏

Copyright©北京勤云科技发展有限公司  京ICP备09084417号