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 15 毫秒
1.
Flow field flow fractionation (FlFFF) in combination with inductively coupled plasma mass spectrometry (ICP-MS) was used to study the chemical speciation of U and trace metals in depleted uranium (DU) contaminated soils. A chemical extraction procedure using sodium pyrophosphate, followed by isolation of humic and fulvic substances was applied to two dissimilar DU contaminated sample types (a sandy soil and a clay-rich soil), in addition to a control soil. The sodium pyrophosphate fractions of the firing range soils (Eskmeals and Kirkcudbright) were found to contain over 50% of the total U (measured after aqua regia digestion), compared to approximately 10% for the control soil. This implies that the soils from the contaminated sites contained a large proportion of the U within more easily mobile soil fractions. Humic and fulvic acid fractions each gave characteristic peak maxima for analytes of interest (Mn, Fe, Cu, Zn, Pb and U), with the fulvic acid fraction eluting at a smaller diameter (approximately 2.1 nm on average) than the humic fraction (approximately 2.4 nm on average). DU in the fulvic acid fraction gave a bimodal peak, not apparent for other trace elements investigated, including natural U. This implies that DU interacts with the fulvic acid fraction in a different way to all other elements studied.  相似文献   

2.
Solid speciation of some trace metals (Pb, Cd, Fe, Mn, Cu) having environmental relevance was studied in coastal particulate sampled during the Austral Spring 2000/2001. A nearshore station situated in the Gerlache Inlet of Terra Nova Bay (Ross Sea, Antarctica) was sampled from November to February. Samples were collected using the in situ filtration system FIS500, equipped with polycarbonate membrane filters having different pore sizes (10 microm, 2 microm and 0.4 microm) for the size fraction analysis of particles. The total concentration of metals was determined both in dissolved and particulate fractions, while speciation was determined on particulate by applying a sequential extraction procedure. Concerning the surface and sub-surface layers, it has been observed that concentration of elements is mainly affected by the dynamic of the pack ice melting and by phytoplankton activity.The solid speciation in November and December is similar for all the studied elements, while some differences can be noted in February, when the pack has completely melted and phytoplankton bloom occurs. With the exception of iron, during this sampling period the quantity of metal associated to the labile fraction increases.  相似文献   

3.
The introduction of catalytic converters has led to a new environmental problem since catalysts emit platinum group elements (PGEs) which are among the least distributed elements in nature. Along with PGEs the vehicle exhaust catalysts contain also a number of stabilizers, commonly oxides of rare earth elements and alkaline earth elements such as Ce, La and Zr. Since vehicular emission of these elements has received little attention so far this work attempts to offer insight into their distribution and fate in the environment by measuring their speciation in road dust samples collected along several highways in Germany and a city centre (Saarbrücken). Speciation of the elements (fractionation into associated mineralogical phases) was carried out via a conventional sequential extraction protocol and the complexing abilities of humic substances in the organic matter were investigated by selective extraction methods in combination with size segregation. For evaluation purposes soil samples spiked with catalytic converter material were analyzed, showing a much lower fraction of Ce, La and Zr mobilized in comparison to the road dust samples. It was found that the elements were effectively bound to humic substances in road dust with a preference for complexation with low molecular weight compounds (<1600 Da).  相似文献   

4.
Marine sediment cores sampled in three different areas, during the 1997/98 Italian Antarctic Expedition, were studied. The cores (40 cm) were immediately subdivided into 13 or 14 layers (2-4 cm) in order to obtain a high-depth resolution in the metal content and humic substance analyses. The results obtained for the amount of metals strongly bound to humic acids showed the following order: Cu > Zn > Co > As >or= Mn. The fraction of Cu, Zn and As bound to humic acid (microg g(-1) of HA) increases in the first 10-12 cm of cores, then a decrease is observed. This observation could be related both to the presence of a mobile fraction of metals in sediments successively bound to humic acids and to different structural features showed by humic acids along the cores, due to transformation processes. For the other metals a variable pattern along the cores was found.  相似文献   

5.
Urban wastewater treatment leads to the generation of large quantities of biosolids. Accumulation of biosolids is a problem of environmental relevance due to the existence of heavy metals in the biosolids. Determination of total metal in biosolid provides information relating pollution levels. Determination of their mobilization capacity and behaviour in the environment is an important task. An experimental approach commonly used for studying the mobility, transport and bioavailability of metal in biosolids is the use of selective sequential extraction procedure. In the present study an attempt has been made to study the heavy metal properties in biosolid samples collected from urban wastewater treatment plants located at Mysore, Karnataka. Few heavy metals selected for the present study are cadmium, chromium, copper, iron, nickel and zinc. The concentration of these metals in biosolids and their partition in different fractions are studied. The speciation of metals based on the sequential extraction scheme was carried out. The concentration of heavy metals is lower than that established by European legislation. The residual fraction has the maximum percentage of heavy metals whereas, only a small fraction of heavy metals (Fe, Zn and Cd) are extracted in the most soluble fractions, exchangeable and carbonate fractions.  相似文献   

6.
Atmospheric deposition of nitrogen (N) and sulfur (S) containing compounds affects soil chemistry in forested ecosystems through (1) acidification and the depletion of base cations, (2) metal mobilization, particularly aluminum (Al), and iron (Fe), (3) phosphorus (P) mobilization, and (4) N accumulation. The Bear Brook Watershed in Maine (BBWM) is a long-term paired whole-watershed experimental acidification study demonstrating evidence of each of these acidification characteristics in a northeastern U.S. forested ecosystem. In 2003, BBWM soils were studied using the Hedley fractionation procedure to better understand mechanisms of response in soil Al, Fe, and P chemistry. Soil P fractionation showed that recalcitrant P was the dominant fraction in these watersheds (49%), followed by Al and Fe associated P (24%), indicating that a majority of the soil P was biologically unavailable. Acidification induced mobilization of Al and Fe in these soils holds the potential for significant P mobilization. Forest type appears to exert important influences on metal and P dynamics. Soils supporting softwoods showed evidence of lower Al and Fe in the treated watershed, accompanied by lower soil P. Hardwood soils had higher P concentrations in surface soils as a result of increased biocycling in response to N additions in treatments. Accelerated P uptake and return in litterfall overshadowed acidification induced P mobilization and depletion mechanisms in hardwoods.  相似文献   

7.
Determination of only total element in sediments does not give an accurate estimate of the likely environmental impacts. Speciation study of metals in sediment provides information on the potential availability of metals (toxic) to biota under various environmental conditions. In water, the toxic metal specie is the free hydrated metal ion. The toxicity of metals depends especially on their chemical forms rather than their total metal content. The present study focuses on Qaraaoun Reservoir, Lebanon. Earlier studies focused only on total metal concentrations in sediment and water. The objective of this study was to determine metal speciation (Fe, Cr, Ni, Zn, Cu, Pb, Cd) in the (operationally defined) sediment chemical fractions and metal speciation in reservoir water. This would reflect on metal bioavailability and toxicity. Water samples and bed sediments were collected from nine sites during the dry season and a sequential chemical fraction scheme was applied to the <75-??m sieve sediment fraction. Metal content in each fraction was determined by the FAAS technique. The data showed that the highest percentages of total metal content in sediment fractions were for: Fe in residual followed by reducible, Cr and Ni in residual and in reducible, Cu in organic followed by exchangeable, Zn in residual and in organic, Pb in organic and carbonate, Cd was mainly in carbonate. Total metal content in water was determined by ICP-MS technique and aqueous metal speciation was predicted using AQUACHEM software interfaced to PHREEQC geochemical computer model. The water speciation data predicted that a high percentage of Pb and Ni were present as carbonate complex species and low percentages as free hydrated ions, highest percentage of Zn as carbonate complex species followed by free hydrated ion, highest percentage of Cd as free hydrated ion followed by carbonate complex species. The sensitivity attempt of free hydrated ion of Ni, Zn, Pb, and Cd in reservoir water revealed dependence of Zn and Cd on pH and alkalinity, while Ni and Pb were only dependent on pH.  相似文献   

8.
This study investigates the stabilization of As in the contaminated sludge after treatment with MnO(2) or Ca(OH)(2), and the influence of the stabilizing materials on the leachability of the co-existing elements Pb and Zn. By exploiting a continuous-flow assembly facilitating a modified Wenzel's sequential extraction scheme (designed for the fractionation of arsenic), it is possible to ascertain the leachability, mobility and fractional alteration of these elements under stimulated natural (flow-through) leaching conditions. The fractionation data show that more than 80% of As, Pb and Zn in the untreated sludge are bound in the amorphous Fe oxides fraction and residual fraction. The addition of MnO(2) has only an insignificant effect on As fractional transformation, while Ca(OH)(2) caused an increase in As mobility. For Pb, the decrease in leachability was clearly visible. The extractable Pb was reduced by 18% and 40% in stabilized MnO(2) and Ca(OH)(2) sludge samples, respectively. Unlike that of Pb, the mobility of Zn was not affected by the additives used. Their fractional distribution patterns before and after the stabilization process remained the same. The ability to produce detailed leaching profiles for As and other elements (Pb, Zn, Ca, Mn and Fe) meant that elemental associations in individual fractions could be examined. From the MnO(2)-treated sludge, the coincidence of the As, Pb, Zn, Fe, and Mn peaks seems to indicate a close association of these elements in the Fe-oxides-bound fraction. Furthermore, the leaching profiles may be used as evidence of a strong affinity between these elements and added MnO(2).  相似文献   

9.
A long-term study of the effect of artificial aeration (destratification) of a water storage dam upon the speciation of iron and manganese in the dam waters has been undertaken. Separation of dam samples into soluble and insoluble forms by selective membrane filtration was undertaken before using the techniques of EPR spectroscopy, ion chromatography and gel filtration to assess the speciation of soluble species, and selective extraction and surface analysis (ESCA, SIMS and SEM) techniques to determine the speciation of particulate iron and manganese species. The percentages of soluble iron and manganese before (1983–85) and after (1986–88) artificial aeration are compared for the periods Jan–Dec, Jan–Mar, and Jun–Aug at three depths 6 m, 15 m and 0.5 m above the dam base, to assess the importance of seasonal changes in the various depths of the dam. Although aeration had an initial marked reduction in levels of soluble iron and manganese at all depths of the dam, the concentrations of these mtals showed a steady increase over succeeding years. Analysis of the figures over summer and winter periods shows that the reduction of soluble iron was maintained in summer, but not during winter. Upon aeration, the initial reduction of soluble manganese concentration was maintained in succeeding years in the epilimnic regions of the dam, but not in the hypolimnion. Statistical analysis of data has been undertaken to correlate the changes in relationship between the various forms of iron and manganese with the advent of aeration.  相似文献   

10.
Sulfur speciation was determined in real time in salt marsh microbial mats, subtidal sediments and hydrothermal vent diffuse flow waters using solid state gold-amalgam voltammetric microelectrodes. Chemical species were measured in situ without any sample manipulation or processing. The partially oxidized sulfur species detected were polysulfides, thiosulfate, elemental sulfur and tetrathionate. Fe(III) oxidation of hydrogen sulfide does not occur within the mats where microbially mediated processes are responsible for oxidation of H2S. In sediments and diffuse flow vent waters, Fe(III) phases are the direct oxidant of H2S. Sulfur speciation determined in this work is due to in situ biogeochemical processes and is not due to artefacts of sample manipulation. The voltammetric data show that polysulfides are the first detectable intermediate during sulfide oxidation which is consistent with previous laboratory studies.  相似文献   

11.
Sequential chemical extraction using chelating agents were used to study the P dynamics and its bioavailability along the surface sediments of the Cochin estuary (southwest coast of India). Sediments were analyzed for major P species (iron bound P, calcium bound P, acid soluble organic P, alkali soluble organic P and residual organic P), Fe, Ca, total carbon, organic carbon, total nitrogen and total sulfur contents. An abrupt increase in the concentration of dissolved inorganic P with increasing salinity was observed in the study region. Iron-bound P exhibited a distinct seasonal pattern with maximum values in the monsoon season when fresh water condition was prevailed in the estuary. As salinity increased, the percentage of iron-bound P decreased, while that of calcium-bound P and total sedimentary sulfur increased. C/P and N/P ratios were low which indicate that large amounts of organic matter enriched with P tend to accumulate in surface sediments. The high organic P contribution in the sedimentary P pool may indicate high organic matter load with incomplete mineralization, as well as comparatively greater percentage of humic substance and resistant organic compounds. Principal component analysis is employed to find the possible processes influencing the speciation of P in the study region and indicate the following processes: (1) the spatial and seasonal variations of calcium bound P and acid soluble organic P was mainly controlled by sediment texture and organic carbon content, (2) sediment redox conditions control the distribution of iron bound P and (3) the terrigenous input of organic P is a significant processes controlling total P content in surface sediments. The bioavailable P was very high in the surface sediments which on an average accounts for 59 % in the pre-monsoon, 65 % in the monsoon and 53 % in the post-monsoon seasons. The surface sediments act as a potential internal source of P in the Cochin estuary.  相似文献   

12.
Chromium speciation in groundwater of a tannery polluted area was investigated for the distribution of chromium species and the influence of redox couples such as Fe(III)/Fe(II) and Mn(IV)/Mn(II). Speciation analysis was carried out by ammonium pyrolidinedithiocarbamate (APDC)–methylisobutylketone (MIBK) procedure. The groundwater samples were analyzed for Cr(III), Cr(VI), and Cr(III)-organic complexes. The APDC could not extract the Cr(III)-organic complexes, but HNO3 digestion of the groundwater samples released the Cr(III)-organic complexes. The groundwater of the area is relatively oxidizing with redox potential (E h) and dissolved oxygen (DO) ranged between 65 and 299 mV and 0.25 and 4.65 mg L???1, respectively. The Fe(II) reduction of Cr(VI) was observed in some wells, but several wells that had Fe(II)/Cr(VI) concentrations more than the stoichiometric ratio (3:1) of the reduction reaction also had appreciable concentration of Cr(VI). This could partly be due to the oxidation of Fe(II) to Fe(III) by DO. It appears that the occurrence of Mn more than the Fe(II) concentration was also responsible for the presence of Cr(VI). Other reasons could be the Fe(II) complexation by organic ligands and the loss of reducing capacity of Fe(II) due to aquifer materials, but could not be established in this study.  相似文献   

13.
The Juru River flows through largely urbanized areas and is grossly polluted by domestic wastes and discharges from pig farms. Other than carrying highly polluting organic materials, these wastes are also contaminated with heavy metals. To ascertain the extent of heavy metal pollution in the river, total and non-residual concentrations of Cu, Pb, Zn, Mn and Fe in sediment samples collected along the river were determined. The results indicate that both the total and non-residual metal concentrations in sediments can successfully be used to identify heavy metal pollution sources. The speciation of Zn, Mn and Fe in the sediment samples were investigated using a sequential leaching technique which identifies the elements among six operationally defined host fractions: (1) exchangeable, (2) carbonate and surface-associated, (3) easily reducible, (4) moderately reducible, (5) bound to organic matter and sulphides and (6) residual. The results indicate that Zn is mainly associated with the reducible fractions. Zn and Fe found in the moderately reducible fraction are significantly correlated, indicating that iron oxides is the preferred host phase by Zn.  相似文献   

14.
The native distribution of As(III) and As(v) in drinking water supplies can influence the treatment removal strategy. The stability of As(III) and As(v) in iron-rich drinking waters can be affected by the formation of Fe precipitates (Fe oxides and/or hydroxides designated by "FeOOH"). These precipitates (ppts) can form during the transport of the sample to the laboratory for arsenic speciation analysis. The analysis of the ppt indicates considerable loss of the aqueous arsenic species (As(aq)) to the solid phase "FeOOH" ppt. Studies of laboratory reagent water containing both As(III) and Fe(III) indicate that the resulting "FeOOH" ppt contained a mixture of As(III) and As(v) with near quantitative removal of the As(aq) in 18 hr. The corresponding aqueous fraction after filtration through a 0.45 microm filter was composed primarily of As(v). The formation of "FeOOH" ppt and the loss of As(aq) to the ppt can be virtually eliminated by the use of EDTA, which sequesters the FeIII). Reagent water fortified with Fe(III), As(III) and EDTA produced less than a 1 ppb change in the As(III)aq concentration over 16 d. The EDTA treatment was also tested on three well waters with different native As(III )/As(v) ratios. The native distribution of As(III)/As(v) was stabilized over a period of 10 d with a worst case conversion of As(III) to As(v) of 2 ppb over a 30 d period. All well waters not treated with EDTA had dramatic losses (a factor of 2-5) of As(aq) in less than 1 d. These results indicated that EDTA preservation treatment can be used to preserve As(aq) in waters where the predominant species is the reduced form [As(III)] or in waters which the predominant species is the oxidized form [As(v)]. This preliminary investigation of EDTA to preserve As species in Fe-rich waters indicates stability can be achieved for greater than 14 d.  相似文献   

15.
In order to investigate the metal distribution, speciation, correlation and origin, risk assessment, 86 surface soil samples from the catchment area around the Miyun Reservoir, Beijing, including samples from gold and iron mine areas, were monitored for fractions of heavy metal and total contents. Most of the metal concentrations in the gold and iron mine soil samples exceeded the metal background levels in Beijing. The contents of most elements in the gold mine tailings were noticeably higher than those in the iron mine tailings. Geochemical speciation data of the metals showed that the residual fraction dominated most of the heavy metals in both mines. In both mine areas, Mn had the greatest the acid-soluble fraction (F1) per portion. The high secondary-phase fraction portion of Cd in gold mine samples indicated that there was a direct potential hazard to organisms in the tested areas. Multivariate analysis coupled with the contents of selected metals, showed that Hg, Pb, Cr, and Ni in gold mine areas represented anthropogenic sources; Cd, Pb, and Cr in iron mine areas represented industrial sources. There was moderate to high contamination of a few metals in the gold and iron soil samples, the contamination levels were relatively higher in gold mine than in iron mine soils.  相似文献   

16.
The main pool of dissolved organic carbon in tropical aquatic environments, notably in dark-coloured streams, is concentrated in humic substances (HS). Aquatic HS are large organic molecules formed by micro-biotic degradation of biopolymers and polymerization of smaller organic molecules. From an environmental point of view, the study of metal humic interactions is often aimed at predicting the effect of aquatic HS on the bioavailability of heavy metal ions in the environment. In the present work the aquatic humic substances (HS) isolated from a dark-brown stream (located in an environmental protection area near Cubat?o city in S?o Paulo-State, Brazil) by means of the collector XAD-8 were investigated. FTIR studies showed that the carboxylic carbons are probably the most important binding sites for Hg(II) ions within humic molecules. 13C-NMR and 1H-NMR studies of aquatic HS showed the presence of constituents with a high degree of aromaticity (40% of carbons) and small substitution. A special five-stage tangential-flow ultrafiltration device (UF) was used for size fractionation of the aquatic HS under study and for their metal species in the molecular size range 1-100 kDa (six fractions). The fractionation patterns showed that metal traces remaining in aquatic HS after their XAD-8 isolation have different distributions. Generally, the major percentage of traces of Mn, Cd and Ni (determined by ICP-AES) was preferably complexed by molecules with relatively high molecular size. Cu was bound by fractions with low molecular size and Co showed no preferential binding site in the various humic fractions. Moreover, the species formed between aquatic HS and Hg(II), prepared by spiking (determined by CVAAS), appeared to be concentrated in the relatively high molecular size fraction F1 (> 100 kDa).  相似文献   

17.
Antimony (Sb) emissions to the environment are increasing, and there is a dearth of knowledge regarding Sb fate and behaviour in natural systems. In particular, there is a lack of understanding of sorption of the oxidised Sb(V) species onto soils and soil phases. In this study sorption of Sb(V) by two organic rich soils with high levels of oxalate extractable Fe was examined over the pH range of 2.5-7. Furthermore, the sorption behaviour of Sb(V) was examined in two phases mimicking those dominant in the experimental soils, namely a solid humic acid and an amorphous Fe(OH)3, across the same pH range. Sorption of Sb by the soils and the humic acid fitted a Freundlich type isotherm, with the equation parameters reflecting changes in bonding affinity corresponding to pH changes. The soils sorbed >75% of the added Sb in all trials, and 80-100% at pH values less than approximately 6.5. The Fe(OH)3 retained >95% of the added Sb in all experiments. The humic acid sorbed up to 60% of the added Sb at acidic pH values, but sorption decreased to zero at higher pH values. Further adsorption studies are recommended, such as examining the effects of ion competition and changes in ionic strength.  相似文献   

18.
Chemical and physical size fractionation of heavy metals were carried out on 20 soil samples from the scrap yard area. Tessier method was used in sequential extraction. Cadmium showed the highest levels among the other elements studied in the exchangeable fraction (about 33%), while other elements showed low levels in this fraction (≥1%). Lead and manganese were mostly found in the Fe–Mn oxide fraction, zinc and iron were mostly in residual fraction, while copper was mostly found in the organic fraction of the soil. Soil samples were size-fractionated into four sizes: 1000–500, 500–125, 125–53, and less than 53 μm. The highest levels of Fe, Cu, Pb, Mn, and Cd were found in the medium fraction (500–125 μm), while zinc showed its highest levels in the fine fraction (125–53 μm). The order of heavy metal load in the size fractions was found to be medium > fine > coarse > silt for Fe, Mn, Cu, Pb, and Cd, where it was found as fine > medium > coarse > silt for zinc.  相似文献   

19.
One hundred workers carried personal air sampling equipment during three days to assess exposure to inhalable and respirable Mn. A novel four-step chemical fractionation procedure developed for the speciation of Mn in workroom aerosols was applied for selected aerosol filters. Blood and urine samples were analysed for Mn. The geometric mean (GM) concentrations of inhalable (n = 265) and respirable (n = 167) Mn determined in all filters were 254 microg m(-3) and 28 microg m(-3) respectively. Only 10.6% (95% CI 8.9-12.5) respirable Mn was found in the inhalable fraction when inhalable and respirable samples collected in parallel were considered (n = 153 pairs). There was a high correlation (Pearson's r = 0.70; p < 0.001) between respirable and inhalable Mn. The largest amounts of Mn in the inhalable aerosol fraction were found as Mn0 and Mn2+ (47.4%), whereas 28% was practically "insoluble". The associations between B-Mn and aerosol concentrations of Mn were weak, but an association was found between U-Mn and respirable Mn; Pearson's r being 0.38 between "soluble" respirable Mn and U-Mn. No significant association was found between the "insoluble" components (probably SiMn) and Mn in biological samples.  相似文献   

20.
One possible impact of large accumulations of decaying wood on forest sites is an increase in (1) eluviation, podzolization and acidification of, and (2) leaching and loss of nutrients from, the soil directly under decaying wood. As an exploratory investigation, we sampled soils beneath forest floors with and without large accumulations of decaying wood (lignic and algnic forest floors respectively) on three soil moisture regimes. Nine sites were located, three in each of central British Columbia, east Vancouver Island, and east of Vancouver. Among the moist sites, there were no differences in Ae horizon thickness between the alignic and lignic forest floors. However, the Ae horizon was thicker beneath the lignic forest floors (mean 4.2 cm) compared to the alignic forest floors (mean 0.7 cm) in slightly dry and fresh sites. Lignic and alignic forest floors differed (p<0.01) in pH, total C, total N, mineralizable N, available S, available P, extractable Mg, K and Ca, lipids, C in fraction B (soluble polysaccharide fraction), C in humic acid, C in fulvic acid, and polyphenol C in fulvic acid for all soil moisture regimes. There were no significant differences in the measures of nutrients or indicators of podzolization as measured by organically complexed Fe and Al, the total non-crystalline Fe and Al, and the poorly crystalline Fe and Al, in the underlying 10 cm of the Bf horizon between the two substrates regardless of the soil moisture regime. Further investigations are needed to establish the relationships between soil productivity and the observed soil chemical measures.  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