Retention of arsenic and phosphorus in iron-rich concretions of Tagus salt marshes   总被引：1，自引：0，他引：1  

Miguel Caetano  Carlos Vale 《Marine Chemistry》2002,79(3-4)

Iron-rich concretions are frequently found around plant roots in Tagus estuary (Portugal) where radial delivery of O₂ takes place. Salt marsh sediments exhibit cracks that are an additional feature to introduce O₂ and other solutes in the upper sediments. Metal concentrations in salt marsh sediments are clearly above the background levels reflecting the anthropogenic sources from a large city with 2.5 million inhabitants, and several industrial centres. In order to evaluate how both oxidised structures influences the redistribution of redox sensitive elements in salt marsh sediments, concretions were collected from roots of Halimione portucaloides below the oxygenated zone. These tubular cylindrical structures were analysed for Fe, Al, Mn, As, and P along 1-cm radial transect in a millimetre scale from the inner part to the adjacent anoxic sediment. In addition, oxidised cracks were analysed for the same spatial resolution, from the sediment–water interface to anoxic layers (2-cm transept). The parallelism between Fe, As, and P concentrations at this microscale is the most noticeable aspect. Iron and As presented very high concentrations in the 4-mm concretions (3.4 mmol g⁻¹ and 3.1 μmol g⁻¹, respectively) and decreased sharply to the host sediment. Oxygen released from roots oxidise the solid sulphides, and the reduced Fe and As are transported towards the root by both diffusion and pore water flow associated with the root water uptake. Subsequently, Fe(III) precipitates and As is retained by sorption and/or coprecipitation. These elements are also enriched in the first 2-mm of oxidised cracks, but in lower concentrations (50% and 30%, respectively). Manganese concentrations in concretions were low (11.8 μmol g⁻¹), indicating that Fe dominates the sediment chemistry. Phosphorus and iron concentrations in the ascorbate fraction were higher in the oxidising surfaces of concretions (10.7 μmol g⁻¹ and 1.6 mmol g⁻¹, respectively) and of cracks (5.1 μmol g⁻¹ and 0.47 mmol g⁻¹). The parallelism of Fe and As distributions includes not only their similar redox chemistries, but also that to phosphate, including control by coprecipitation of the host iron phases. The mechanisms involved in the mobilisation of As and P are however different, whereas As comes from the oxidation of iron sulphides; dissolved P derives from reduction of ferri-hydroxide phases.  相似文献   

Distribution of dissolved species and suspended particulate copper in an intertidal ecosystem affected by copper mine tailings in Northern Chile   总被引：1，自引：0，他引：1  

Santiago Andrade  James Moffett  Juan A. Correa   《Marine Chemistry》2006,101(3-4):203-212

The coastline near Chañaral in Northern Chile is one of the most highly Cu-contaminated zones in the world due to discharges from mining activities for more than 60 years. The speciation of Cu has been studied to determine the importance of organic complexation in highly contaminated areas, and to assess the likely physiological impacts of Cu on marine organisms. Dissolved Cu concentrations of up to 500 nM were measured, completely saturating organic ligands and leading to free Cu²⁺ concentrations in excess of 10^− 8 M. These values are higher than those reported in any other marine environment, and because they occur over an extensive area, provide a unique opportunity to study the effects of Cu on marine ecosystems and to see how Cu behaves when its speciation is predominantly inorganic. We found strong gradients in free Cu²⁺ between Chañaral and adjacent areas with lower Cu, where speciation is dominated by organic complexation. There is also a significant increase in the partitioning of Cu onto suspended particles in the contaminated areas, consistent with previous studies that showed that organic ligands stabilize Cu in the dissolved phase, whilst “excess” Cu is rapidly scavenged. Those high dissolved Cu concentrations persist in spite of solid phase partitioning and advective processes along this open-ocean coastline, suggesting that Cu inputs into the system are still very large. Measurements were made using anodic stripping voltammetry with a thin mercury film coated with Nafion, which previous workers have shown can mitigate ambiguity in the data arising from inadvertent reduction of organic complexes. Our findings suggest that this is a useful methodology for contaminated systems.  相似文献   

滇西沘江流域水体中重金属元素的地球化学特征   总被引：6，自引：1，他引：5  

李瑞萍  王安建  曹殿华  王高尚  李以科  耿诺 《地质通报》2008,27(7):1071-1078

通过测定流经兰坪金顸铅锌矿区的沘江水体中Pb、Zn、Cd、As的含量和底泥中重金属元素的化学形态的含量,分析了重金属元素的分布和化学形态的变化。结果表明,沘江水遭到了Cd污染,底泥已经成为重金属元素的蓄积库,以国家土壤环境质量标准（Ⅲ级）衡量,Pb、Zn、Cd和舡分别超标3．4倍、15．8倍、106倍和2．6倍。沘江水中重金属元素含量的峰值在矿山附近的下游,而底泥中重金属元素的峰值在矿山下游30-50km的地方,矿业活动、水流变缓、pH等水体环境条件的变化都能影响水和底泥中重金属元素的含量。底泥中的Pb以碳酸盐结合态为主,Zn和Cd以铁锰氧化物结合态为主,而As以残渣态为主。Pb、Cd、Zn三种元素的环境有效态含量比较高,对沘江流域生态环境具有潜在的巨大的危害。  相似文献   

Geostatistical analysis of arsenic concentration in the groundwater of Malda district of West Bengal, India     

Barendra Purkait  Amitava Mukherjee 《Frontiers of Earth Science》2008,2(3):292-301

The problem of arsenic (As) poisoning in the upper deltaic plain of the Ganga-Bhagirathi river system in the Bengal Basin of West Bengal, India is an alarming issue. Four blocks (Kaliachak-1, 2, 3 and English Bazar) of Malda district, West Bengal were critically studied. Geomorphologically, the area exhibits three terraces: the present Youngest terrace (T₀-terrace), the Older Shaugaon Surface (T₁-terrace) and the Oldest Baikunthapur Surface (T₂-terrace). On the basis of numerous measurements, including As-content, pH, DO, specific conductivity and salinity, it was observed that maximum As-content beyond the permissible limit (0.05 mg/L, Indian standard) occurs within a depth range of 10–30 m with a non-linear distribution pattern. Variance test also found that a block effect was highly significant in an As-distribution pattern. Mean arsenic level of Kaliachak block-1 is 0.2253 mg/L, followed by Kaliachak-2 with arsenic level 0.1923, Kaliachak-3 with arsenic level 0.1755 and English Bazar with arsenic level 0.1324. The arsenious belt lies mainly within the Older terrace (T₁). The very recent flood plain deposits of silvery white, fine sands lying very close to the Ganga River margin do not contain significant amounts of As. Elevated As-concentration in the ground water was observed in alluvial sands, grayish white to brownish in color and occurring away from the Ganga margin. The Oldest terrace (T2) further away from the Ganga margin (e.g. English Bazar) and Barind surface contains less arsenic. Barind surface acts as a hard capping with ferruginous sands and lateritic concretions-chocolate, mottled and purple brown in color-occurring northeast of the studied area. Arsenic content of ground water in the same locality within a radius of ∼ 20 m varies within wide limits. Thus, it poses problem to delineate its distribution pattern. Such a patchy occurrence possibly could not be explained satisfactorily solely by geomorphology. Chemical analysis of aquifer clay samples of the cores shows a maximum Ascontent of up to 3 mg/kg, whereas the bulk samples (sandclay mixture) of the cores contain a maximum of 17 mg/kg As-value. Therefore, it is not always true that clay contains elevated As-value.  相似文献   

Visualization experiments of iron precipitates: Application for in-situ arsenic remediation     

M.I.M. Darwish  V.M. van Beek  J. Bruining 《Journal of Geochemical Exploration》2006,88(1-3):19

Laboratory experiments were carried out to acquire more insight and understanding of the phenomena associated with the in-situ arsenic remediation. Visualization techniques are the most informative for the detection of Fe(II) while flowing in soils. Green Rust (GR) was considered as representative of in-situ iron precipitates. In a visualization flat cell, the change in color of GR to orange, due to oxidation, was monitored by a digital camera and the images were analyzed giving the spatial and temporal distribution of Fe(II). Moreover, both oxygen and pH changes in time were recorded in two sections along the flow direction in the cell. The measured and calculated concentration profiles were compared and the actual reaction rates were predicted. The reaction rate constants measured in this study, under flowing conditions, are in a good agreement with the values obtained from batch experiments reported in the literature.  相似文献   

Speciation of adsorbed arsenate on the surface of hydrous iron oxide     

Yongfeng JIA Xin WANG George Demopoulos 《中国地球化学学报》2006,25(B08):35-35

Adsorption of arsenate on hydrous iron oxide is an important process controlling geochemical cycling of arsenic in environment as well as the fate of arsenic-bearing mining wastes. The widely accepted view on the mechanism of adsorption is that arsenate is adsorbed via bidentate binuclear inner-sphere complexation. In this study, we characterized the arsenate-hydrous iron oxide sorption solids synthesized at pH=3-8 using Fourier transformed infrared spectroscopy （FTIR） and X-ray diffraction （XRD）. It has been determined that poorly crystalline ferric arsenate developed on the surface of iron oxide when arsenate was sorbed at acidic pH, while at alkaline pH the adsorption of arsenate was via bidentate complexation.  相似文献   

Flotation and depression control of arsenopyrite through pH and pulp redox potential using xanthate as the collector     

A. López Valdivieso  A.A. Sánchez López  C. Ojeda Escamilla  M.C. Fuerstenau 《International Journal of Mineral Processing》2006

The role of pH and pulp redox potential (E_H) to control the flotation and depression of arsenopyrite has been investigated through studies on microflotation of arsenopyrite crystals and batch flotation of an arsenopyritic ore using isopropyl xanthate as collector. The transition between flotation and depression of arsenopyrite is established by the reversible potential of the xanthate/dixanthogen couple. Adsorption of arsenate ions on ferric hydroxide has been studied through electrokinetics to delineate mechanisms involved in the depression of arsenopyrite using oxidants. Chemical binding between arsenate species and ferric hydroxide sites on arsenopyrite is suggested as the mechanism responsible for depression of arsenopyrite. E_H conditions are given for the flotation and depression of arsenopyite at various pH values for the arsenopyritic ore.  相似文献   

Speciation analysis and significance of ecological geochemistry     

Yaping WANG Chunxue XU Ziyi AN Suming WANG 《中国地球化学学报》2006,25(B08):205-205

Different species of one element have different activities, so it has different effects on environment and human health. To analyze qualitatively and quantitatively the speciation of a special element in sample, which is the important basis for appraising the toxicity and studying the rule of transfer and translation of elements. Since the 1970＇s, the scheme of sequential extraction has already been used at many laboratories both at home and abroard, to get the information about heavy metals＇ activity in polluted soils. Because this method has the experimental nature, many schemes of problem has taken place, the absence of consistency of these sequential extraction have been formed. Thus the complexity of the schemes, the lack of selectivity of reagent, the lack of quality control, the result mainly related to the extraction scheme used, and so on. In the face of these problems, the study of experimental methods of sequential extraction on three different soils, sediment in Dongting Lake, soil in Jiangsu Province and loess in Shanxi Province was made. Reference materials of heavy metal speciation following sequential extraction in soil and sediment had been developed. Nowadays two kinds of sequential extraction methods which are widely used are BCR （three steps） and improved Tessier methods （seven steps）. Based on three steps of BCR, water-soluble speciation and the residual speciation were increased in our research. BCR701 was determined eight times at different laboratories using BCR three steps. The results showed that determined data obtained eight times were identical to the standard value, and it is indicated that this method has good reproducibility. The stability and homogeneity experiments indicated that the preparation of three types of candidates accorded with our requirements. Eight laboratories had afforded the determined values of 12 heavy metal elements （Cu, Pb, Zn, Mn, Co, Ni, Cd, Cr, Mo, As, Sb, Hg, Se et al.） using BCR three steps. Also, these three candidates afforded the determined values by seven steps, and 12 laboratories had participated.  相似文献   

Speciation of sulfate components in size-fractionated aerosol particles using sulfur K-edge X-ray absorption near-edge structure （XANES）     

Yoshio Takahashi Yutaka Kanai Hikari Kamioka Atsuyuki Ohta Takuro Miyoshi Hiroshi Shimizu 《中国地球化学学报》2006,25(B08):222-222

Sulfates are a main constituent of aerosols, which sulfate aerosols, it is necessary to determine what can cause various environmental problems sulfate ions are contained in these aerosols In the evaluation of the influence of In this study, sulfur K-edge XANES was used to determine sulfate species present in size-fractionated aerosol particles based on the post-edge structure after the main absorption peak in the XANES region. Aerosol samples were collected as part of the Japan-China joint project, ＂Asian Dust Experiment on Climate Impact＂ using a low-volume Andersen-type air sampler. XANES was measured at Beamline BL-9A at Photon Factory, Japan. A comparison of the XANES spectra of reference sulfate materials and aerosol samples collected in Tsukuba in Japan clearly showed that （NH4）2SO4 was the main sulfur species in particles with a smaller diameter and gypsum was the main sulfur species in particles with a larger diameter. A simulation of the XANES spectra by reference materials allows us to obtain the quantitative mixing ratios of the different sulfate species present in the aerosol samples. The presence of minor sulfur species other than （NH4）2SO4 and gypsum at the surface of mineral aerosols is suggested in our simulations and by a surface-sensitive conversion electron/He-ion yield XANES. In the absence of a contribution from a large dust event, the mole concentration of gypsum in the mineral aerosol fraction determined by XANES is similar to that of Ca which is determined independently using ion chromatography. This shows that the Ca and sulfate in the mineral aerosols are present only as gypsum. Considering that calcite is the main Ca mineral in the original material arising from an arid and semi-arid area in China, it is strongly suggested that gypsum is formed in aerosol during its long-range transportation by a reaction between calcite and sulfate ions.  相似文献   

Distribution of cadmium, chromium, copper, lead and zinc in marine sediments in Hong Kong waters     

S. C. Choi  Onyx W. H. Wai  Thomas W. H. Choi  X. D. Li  C. W. Tsang 《Environmental Geology》2006,51(3):455-461

Partitioning of heavy metals (Cd, Cr, Cu, Pb, Zn) in marine sediments collected from various sites in Hong Kong waters were determined using sequential extraction method. Sediments from Kellette Bank, located in Victoria Harbour, had higher metal concentrations especially Cu and Zn than most other sites. Slightly over 20% of total Cu and Cr existed as readily available forms in Peng Chau and Kellette Bank. At most sampling sites, over 15% of the Cu existed as the exchangeable form indicating that Cu could be readily released into the aqueous phase from sediments. A significantly higher percentage of Pb and Zn was associated with the three non-residual fractions. Hence, there is a greater environmental concern for remobilization of Pb and Zn compared with Cr. The high amount of residual Cd (>50%) and the relatively lower Cd content indicate that little environmental concern is warranted for the remobilization of Cd. Distribution of metals in sediments collected from different depth at Kellette Bank shows that metal concentrations decreased with profile depth. The levels of Pb and Zn associated with the two readily available fractions increased sharply in the surface sediment. These metals represented the pollutants, which were introduced into the area in the mid-eighties through early nineties as a result of rapid economic and industrial development in the territory. As significant portions of these metals were bound to the readily available phases in the surface sediments, metal remobilization could be a concern. An erratum to this article can be found at  相似文献