Mobility of some potentially toxic trace elements in the coal of Guizhou, China   总被引：5，自引：0，他引：5  

X. Feng  Y. Hong  B. Hong  J. Ni 《Environmental Geology》2000,39(3-4):372-377

 The mobility of 10 potentially toxic trace elements (PTTE), As, Cd, Cr, Cu, Hg, Ni, Pb, Se, Tl, and Zn from 32 coals of the Longtan Group formed in Permian Period in Guizhou Province, China was investigated using sequential extraction procedures. The results demonstrate that PTTEs such as Hg, As, Se, Cd, Cu, and Pb have the highest mobility at surface conditions, and the average extractable fractions of them are 86%, 95%, 79%, 76%, 69%, and 69% of the total amount in coal, respectively. The elements in coal with the lowest leachability include Tl, Cr, and Ni, and the average extractable fractions of them are 30%, 20%, and 29% of the total amount in coal respectively. Zinc has an intermediate behavior, and the average leachable fraction of it accounts for 46% of the total amount in coal. The results demonstrate that mobility of PTTE in coal depends on the speciation of these elements. The elements associated with sulfates, carbonates, sulfides and some organic matter in coal show the highest extraction rates during the weathering process, while elements with silicate affinities are inert at surface conditions. Received: 29 December 1998 · Accepted: 10 November 1998  相似文献   

Influence of salinity and humic substances on the uptake of trace metals by the marine macroalga, Ulva lactuca: Experimental observations and modelling using WHAM     

Andrew Turner  Silvia S. Pedroso  Murray T. Brown 《Marine Chemistry》2008,110(3-4):176-184

Uptake of the trace metals, Pd, Cd, Hg and Pb, by the marine macroalga, Ulva lactuca, has been studied along a salinity gradient (S = 15–35; pH ~ 8.3) created by batch mixing of synthetic sea water and pure water, both in the absence and presence of humic substances. Factors defining the concentration ratio of metal taken up (w/w) to metal remaining in solution ranged from about 10² mL g^− 1 for Cd to 10³ mL g^− 1 for Pd and Hg. Within experimental error, only the biouptake of Cd appeared to exhibit a dependence on salinity, while the addition of 3 mg L^− 1 of humics resulted in a small suppression of Pd and Hg uptake and a moderate enhancement of Pb uptake compared with the humic-free system. Metal internalisation, evaluated from an EDTA wash of the alga, followed the sequence: Hg > Pd > Cd > Pb; and was notably inhibited in the presence of humics for Pb. Metal uptake (as adsorption and internalisation) was modelled using the Windermere Humic Aqueous Model (WHAM, v6) by encoding the macroalga as a polyelectrolytic binding phase whose properties were defaulted to those of aqueous humics in the software database. By setting the “activity” of the binding phase to about 0.1 and systematically reducing the default constants for metal binding, the magnitude of metal uptake by U. lactuca was reproduced. However, for all metals the model predicted a reduction in algal uptake as a function of salinity that was not always observed experimentally. Moreover, calculations performed in the presence of aqueous humic substances and using the earlier fitted constants significantly underestimated metal uptake by U. lactuca. Discrepancies between experimental observations and model calculations, which are attributed to the formation of ternary complexes at the algal surface, suggest that conventional equilibrium speciation considerations alone are not applicable for modelling metal interactions with marine macroalgae.  相似文献   

Chromium speciation and existing natural attenuation conditions in lagoonal and pond sediments in the former chemical plant of Porto-Romano (Albania)     

A. Shtiza  R. Swennen  A. Tashko 《Environmental Geology》2008,53(5):1107-1128

Near the outskirts of the Albanian port of Durres on the Adriatic Coast, at a place called Porto Romano, an old chemical complex has been producing chromate salts for a period of ∼20 years (1972–1993). As a result large quantities of chromite ore processing residue (COPR) waste were released mainly as suspended particles and/or dissolved species in effluents, which settled in a decantation pond area, 200 × 250 m in size, east of the industrial plant. Unfortunately, pollutants were spread out with time. Knowing that chromium mobility and toxicity in natural settings is species dependent, the species characterization has been carried out in different sampling media (pond sediments, lagoonal sediments and water samples). Five pond profiles were sampled within the decantation area up to a depth of ∼1 m, till the underlying Quaternary lagoonal silty-clays were reached. Total Cr content is highly variable with values between 1,130 and 24,409 mg/kg which is clearly higher than the defined local background values for lagoonal silty-clays (198 mg/kg of Cr). Leaching of Cr(VI) especially occurs in the pond sediments, which are low in OC, CEC and clay content, under acidic and neutral pH conditions (e.g. up to ∼2,230 mg/kg Cr(VI) leached from a sample containing a total concentration of Cr 12,200 mg/kg). Moreover, leaching of the Cr(III) occurs only under strictly acidic conditions (maximum 1,144 mg/kg leached from a sample containing a total Cr-concentration of 17,608 mg/kg). In this study also a number of natural attenuation conditions (i.e. reaction with lagoonal clays rich in organic matter and iron as well as isomorphous substitution) have been recognized.  相似文献   

Copper complexation by fulvic acid affects copper toxicity to the larvae of the polychaete Hydroides elegans   总被引：1，自引：0，他引：1  

Qiu JW  Tang X  Zheng C  Li Y  Huang Y 《Marine environmental research》2007,64(5):563-573

Copper toxicity is influenced by a variety of environmental factors including dissolved organic matter (DOM). We examined the complexation of copper by fulvic acid (FA), one of the major components of DOM, by measuring the decline in labile copper by anodic stripping voltammetrically (ASV). The data were described using a one-site ligand binding model, with a ligand concentration of 0.19micromol site mg(-1) C, and a logK' of 6.2. The model was used to predict labile copper concentration in a bioassay designed to quantify the extent to which Cu-FA complexation affected copper toxicity to the larvae of marine polychaete Hydroides elegans. The toxicity data, when expressed as labile copper concentration causing abnormal development, were independent of FA concentration and could be modeled as a logistic function, with a 48-h EC(50) of 58.9microgl(-1). However, when the data were expressed as a function of total copper concentration, the toxicity was dependent on FA concentration, with a 48-h EC(50) ranging from 55.6microgl(-1) in the no-FA control to 137.4microgl(-1) in the 20mgl(-1) FA treatment. Thus, FA was protective against copper toxicity to the larvae, and such an effect was caused by the reduction in labile copper due to Cu-FA complexation. Our results demonstrate the potential of ASV as a useful tool for predicting metal toxicity to the larvae in coastal environment where DOM plays an important role in complexing metal ions.  相似文献   

Improved thermodynamic calculations for concentrated mixed electrolyte systems including ion pairing (or the absence of it)     

Peter M. May   《Marine Chemistry》2006,99(1-4):62

Knowledge of the activity coefficients of solutes under temperature and pressure ranges of interest is generally required for calculations of the physicochemical properties of aqueous multicomponent electrolyte solutions such as seawater. Whilst these activity coefficients are well characterized for the predominant salts individually, fewer data are available for minor components under a sufficiently wide range of conditions and there are significant interactions between some of the chemical species involved which can substantially alter the required activity coefficients in mixtures.For these reasons, accurate thermodynamic predictions for seawater and other multi-electrolyte solutions in moderate or high concentration are more difficult than is often supposed. In particular, progress in this area has been slowed by uncertainty regarding the nature and extent of ion pairing in concentrated strong electrolyte solutions, a problem that has been debated for decades. Zdanovskii's rule, described originally almost a century ago but widely neglected, provides a fundamentally sound method for calculating the properties of mixed electrolyte solutions. Modelling developments are described, which accord with various types of experiment, from our laboratory and from the chemical literature. It has become clear that, when treated in an appropriate way based on solvent activity, linear mixing behaviour of strong electrolyte solutions can be considered the norm. This is an inevitable consequence, first recognized by Guggenheim, of the cancellation of ion pairing and other interactions as, conceptually, one ion replaces another. Stronger solute–solute interactions, described by equilibrium constants, can then easily be coupled in a thermodynamically consistent manner.  相似文献   

Mercury speciation in sediments at a municipal sewage sludge marine disposal site   总被引：3，自引：0，他引：3  

Shoham-Frider E  Shelef G  Kress N 《Marine environmental research》2007,64(5):601-615

Mercury speciation was performed in excess activated sewage sludge (ASS) and in marine sediments collected at the AAS disposal site off the Mediterranean coast of Israel in order to characterize the spatial and vertical distribution of different mercury species and assess their environmental impact. Total Hg (HgT) concentrations ranged between 0.19 and 1003ng/g at the polluted stations and 5.7 and 72.8ng/g at the background station, while the average concentration in ASS was 1181+/-273ng/g. Only at the polluted stations did HgT concentrations decrease exponentially with sediment depth, reaching background values at 16-20cm, the vertical distribution resulting from mixing of natural sediment with ASS solids and bioturbation by large populations of polycheates. Average Methyl Hg (MeHg) concentration in ASS was 39.7+/-7.1ng/g, ca. 3% of the HgT concentration, while the background concentrations ranged between 0.1 and 0.61ng/g. MeHg concentrations in surficial polluted sediments were 0.7-5.9ng/g (ca. 0.5% of the HgT) and decreased vertically, similar to HgT. A positive correlation between MeHg and Hg only at the polluted stations, higher MeHg concentrations at the surface of the sediment and not below the redoxline, and no seasonality in the concentrations suggest that the MeHg originated from the ASS and not from in situ methylation. By doing selective extractions, we found that ca. 80% of the total Hg in ASS and polluted sediments was strongly bound to amorphous organo-sulfur and to inorganic sulfide species that are not bioavailable. The fractions with potential bioaccessible Hg had maximal concentrations in the range in which biotic effects should be expected. Therefore, although no bioaccumulation was found in the biota in the area, the concentration in the polluted sediments are not negligible and should be carefully monitored.  相似文献   

Geochemistry of barium in soils supplied with carbonatite rock powder and barium uptake to plants     

《Applied Geochemistry》2016

Apatite-biotite-carbonatite (short form: carbonatite) rock powder originating from Lillebukt alkaline complex, N-Norway is a potential liming and multi-nutrient fertilizer. However, the elevated contents of potentially bio-toxic barium (Ba) (up to 5.5 g kg⁻¹) is a matter of concern. A pot experiment was conducted in order to investigate the geochemistry of Ba in a sandy peat-containing growth media treated with carbonatite, with special focus on Ba-speciation in the pore water. These results were correlated with Ba uptake in Trifolium repens L. (white clover) and Fesctua arundinácea L. (tall fescue). The Ba-speciation and bioavailability as affected by treatment and plant growth was conducted using WHAM/Model VI version 7.0.4 and the diffusive gradients in thin films (DGT) technique, respectively. The increasing cation exchange capacity (CEC) in the growth media, and colloidal fulvic acids (FA) decreased the Ba²⁺ concentration in pore water. Both the Ba detected in DGT (Ba_dgt), and exchangeable Ba (Ba_exc) were higher in pots containing rock powder. A strong relationship between Ba_exc and diffusively bound Ba to FA (Ba_dfa) with plant uptake was evident. The latter was likely initiated by organic material mobilization of Ba from carbonatite. The mobilized Ba bound to FA (Ba_fa) in pore water was mainly bound diffusively, and the Ba_dfa fraction was thus made available to plants. Finally, the Ba_dgt was increased in pots grown with white clover compared to tall fescue. Further investigation is required to determine if this is related to increased rhizosphere activity by plants or to the nitrogen fixating plant-microbe relationship.  相似文献   

Distribution and speciation of metals,phosphorus, sulfate and organic material in brackish estuary water affected by acid sulfate soils     

《Applied Geochemistry》2016

Dissolved (<1 kDa) and colloidal (1 kDa-0.45 μm) size fractions of sulfate, organic carbon (OC), phosphate and 17 metals/metalloids were investigated in the acidic Vörå River and its estuary in Western Finland. In addition, geochemical modelling was used to predict the formation of free ions and complexes in these waters. The sampling was carried out during high-water flow in autumn and in spring when the abundantly occurring acid sulfate (AS) soils in the catchment area are extensively flushed. Based on the high concentrations of sulfate, acidity and several metals, it is clear that the Vörå River and its estuary is strongly affected by AS soils. The high dissolved form of metals limits also the existence of fish and other organisms in this estuary, and certainly also in other similar shallow brackish estuaries elsewhere in the Gulf of Bothnia. However, generally already <20% saline sea water reduces the concentration for OC and several elements (Al, Cu, Cr, Fe, Pb, PO₄ and U) by half and c. 20–30% saline sea water is needed to halve concentrations of Cd, Co, Mn, Ni and Zn. Consequently, these elements as well as organic matters were rapidly precipitated in the estuary, even after mixing with fairly small amounts of the alkaline brackish sea water. Aluminium, Cu, Fe and U most likely precipitate together with organic matter closest to the river mouth. Manganese is relatively persistent in solution and, thus, precipitates further down the estuary as Mn oxides, which concomitantly capture Ba, Cd, Co, Cu, Ni and Zn. In the inner estuary, the high contents of Al is as important than Fe in removing PO₄ and, thus, also reducing the risk of algae blooms in near coastal areas influenced by AS soils in the Gulf of Bothnia. Moreover, the dispersion of metals far out in the estuary is dependent on hydrological conditions, i.e. with high flows the plume of metal-rich water will spread further out in the estuary. Furthermore, the extensive drainage of the catchment and subsequent artificial enlargement of the river channel during recent decades has not only enabled oxidation of sulfidic sediments, but strongly increased flow peaks that reach further out in the estuary.  相似文献   

Geochemical behavior and speciation modeling of rare earth elements in acid drainages at Sarcheshmeh porphyry copper deposit,Kerman Province,Iran     

Reza Sharifi  Farid MooreBehnam Keshavarzi 《Chemie der Erde / Geochemistry》2013

Acid mine drainage is a major source of water pollution in the Sarcheshmeh porphyry copper mine area. The concentrations of heavy metals and rare earth elements (REEs) in the host rocks, natural waters and acid mine drainage (AMD) associated with mining and tailing impoundments are determined. Contrary to the solid samples, AMDs and impacted stream waters are enriched in middle rare earth elements (MREEs) and heavy rare earth elements (HREEs) relative to light rare earth elements (LREEs). This behavior suggests that REE probably fractionate during sulfide oxidation and acid generation and subsequent transport, so that MREE and HREE are preferentially enriched. Speciation modeling predict that the dominant dissolved REE inorganic species are Ln³⁺, Ln(SO₄)₂⁻, LnSO₄⁺, LnHCO₃²⁺, Ln(CO₃)₂⁻ and LnCO₃⁺. Compared to natural waters, Sarcheshmeh AMD is enriched in REEs and SO₄²⁻. High concentrations of SO₄²⁻ lead to the formation of stable LnSO₄⁺, thereby resulting in higher concentrations of REEs in AMD samples. The model indicates that LnSO₄⁺ is the dissolved form of REE in acid waters, while carbonate and dicarbonate complexes are the most abundant dissolved REE species in alkaline waters. The speciation calculations indicate that other factors besides complexation of the REE's, such as release of MREE from dissolution and/or desorption processes in soluble salts and poorly crystalline iron oxyhydroxy sulfates as well as dissolution of host rock MREE-bearing minerals control the dissolved REE concentrations and, hence, the MREE-enriched patterns of acid mine waters.  相似文献   

The Chemical Speciation of Fe(III) in Freshwaters   总被引：1，自引：0，他引：1  

Stephen Lofts  Edward Tipping  John Hamilton-Taylor 《Aquatic Geochemistry》2008,14(4):337-358

Dialysis and chemical speciation modelling have been used to calculate activities of Fe³⁺ for a range of UK surface waters of varying chemistry (pH 4.3–8.0; dissolved organic carbon 1.7–40.3 mg l⁻¹) at 283 K. The resulting activities were regressed against pH to give the empirical model: . Predicted Fe³⁺ activities are consistent with a solid–solution equilibrium with hydrous ferric oxide, consistent with some previous studies on Fe(III) solubility in the laboratory. However, as has also sometimes been observed in the laboratory, the slope of the solubility equation is lower than the theoretical value of 3. The empirical model was used to predict concentrations of Fe in dialysates and ultrafiltrates of globally distributed surface and soil/groundwaters. The predictions were improved greatly by the incorporation of a temperature correction for , consistent with the temperature dependence of previously reported hydrous ferric oxide solubility. The empirical model, incorporating temperature effects, may be used to make generic predictions of the ratio of free and complexed Fe(III) to dissolved organic matter in freshwaters. Comparison of such ratios with observed Fe:dissolved organic matter ratios allows an assessment to be made of the amounts of Fe present as Fe(II) or colloidal Fe(III), where no separate measurements have been made. Electronic supplementary material  The online version of this article (doi:) contains supplementary material, which is available to authorized users.  相似文献