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1.
Al is a critical ecotoxicant in surface waters impacted by acidic deposition. Apart from the most acidic surface waters, Al concentrations are often considered to be controlled by Al(OH)(3) or aluminosilicate (clay) solubility for modelling studies. For many UK rivers there is no clear evidence for such solubility controls even though there is the potential under moderately acidic/alkaline conditions. Here, Al solubility in ground and river water is compared for acid sensitive catchments in mid-Wales. The results reveal that there may be a solubility control within the groundwater but a more complex state of affairs within the river. The groundwater is of high CO(2) content and once in the river it degasses to raise pH. However, there is limited change in Al concentration and hence the solubility relationship is lost. The results flag the potential importance of groundwater solubility controls for Al and the potential for the groundwater zone to act as an Al filter. For positive alkalinity groundwaters, the high CO(2) levels depress the pH to near the value for minimum Al solubility. However, there is no simple groundwater end-member. Examining Al solubility controls solely within the rivers provides cryptic and misleading clues to the hydrogeological controls for Al within catchments. Assessing the within-catchment processes requires direct measurement with full consideration of both inorganic and organic attenuation.  相似文献   

2.
Episodic events may be critical with respect to aluminium (Al) toxicity in moderately acidified salmon rivers. The present work demonstrates that sea salt episodes enhance the toxicity of Al in acidic rivers. The documented sea salt episode (300 [micro sign]M Cl) mobilized positively charged Al species (0.4 to 1.1 [micro sign]M Al(i)), enhanced the Al accumulation on fish gills (0.9 to 10 [micro sign]mol g(-1) dw) and caused increased stress responses (6 to15 mM blood glucose) in fish. Accumulated Al on gills remained high several days after the episode. The presented results are based on a six-week field study in two tributary rivers on the west coast of Norway. Changes in the river water qualities and Al speciation were followed using in situ fractionation techniques. Al accumulation on gills and stress responses were followed for Atlantic salmon (Salmo salar) kept in tanks continually exposed to the changing water quality. The potential mobilization of Al from the two catchments was studied by extracting soils with diluted seawater (salinity of 3). To counteract Al toxicity, one of the tributary catchments has been limed. The potential mobility of Al by sea salt was lower in limed soils compared to acid soils, and the Al deposition on fish gills (<3.5 [micro sign]mol g(-1) dw) and associated stress responses stayed low during the sea salt episode in the river draining the limed catchment. Thus, for acid river systems in coastal areas, catchment liming should be considered as a useful countermeasure for Al toxicity.  相似文献   

3.
Ten years of monitoring of rainfall and streams in the remote acidic and acid sensitive moorland and afforested moorland of upland mid-Wales reveals concentrations of arsenic (As) typically <1 μg L(-1). On average, the lowest concentrations occur within rainfall and they have declined over time probably in response to reductions in global emissions. There is a corresponding reduction within the streams except for forested systems where concentrations up to doubled following clear-fell. Within the streams there are both annual cycling and diurnal cycling of As. The annual cycling gives maxima during the summer months and this probably reflects the importance of groundwater inputs and mineralisation/desorption from the surface soil layers. Correspondingly, the diurnal cycling occurs during the summer months at low flow periods with As concentrations highest in the afternoon/evening. For the urban/industrial basins of northern England with historically a much higher As deposition, land contamination and effluent discharges, comparative data indicate As concentrations around three fold higher: strong seasonal patterns are observed for the same reasons as with the uplands. Across the sites, the As concentrations are over an order of magnitude lower than that of environmental concern. Nonetheless, the results clearly show the effects of declining emissions on rainfall deposition and some indication of areas of historic contamination. Arsenic is mainly present in the <0.45 fraction, but cross-flow filtration indicates that approx. 43% is in the colloidal phase at the clean water sites, and 16% in the colloidal phase at the contaminated sites. Part of this colloidal component may well be associated with organic carbon.  相似文献   

4.
The environmental risk of aquatic phosphorus (P) critically depends on its mobility and bioavailability, both of which are greatly affected by the size distribution and composition of P. The size distribution (particulate, colloidal and truly dissolved phase) of P, composed of molybdate reactive P (MRP) and molybdate unreactive P (MUP), was determined at twenty-three typical sections of the East Tiao River, China in the plum rain season. Results indicated particulate P was dominant followed by the truly dissolved P, while colloidal P was quantitatively the lowest in the whole river. From upstream to downstream, particulate P sharply increased, along with a slight decrease of truly dissolved P. However, colloidal P remained at a relatively stable level in the whole river, ranging from below detection limit to 0.025 mg L(-1), 0 to 13.4% of total P (TP). Furthermore, colloidal MRP exhibited a rising trend downriver as compared to upriver, with the notable transfer of MRP from the truly dissolved phase to particulate and colloidal phases. Particle concentration effect for colloids, observed in the study of MRP distribution, further corroborated the role of colloids in MRP solid/liquid partitioning. These observations, in this large-scale field investigation, fitted the "colloidal pumping" hypothesis. It may be concluded that colloids act as the intermediate and buffer in the dynamically balanced transfer of P from truly dissolved phase to large particulate phase, having a significant role in size distribution of P.  相似文献   

5.
The background levels, variability, partitioning and transport of eleven trace elements-Ag, Al, As, Cd, Co, Cr, Cu, Mn, Pb, Zn and U-were investigated in a mountain range river system (Adour River, France). This particular river system displayed a turbulent hydrodynamic regime, characterized by flash-transient discharge conditions leading to fast shifts in suspended particulate matter (SPM) concentrations as high as two orders of magnitude (12 to 600 mg l(-1)). The distribution of SPM was accurately predicted with a "hysteresis" transport model, indicating that about 75% of the annual solids load was exported within 20 to 40 days. Dissolved and particulate concentrations of most trace elements were low compared to their concentrations in other reference river systems expect for Pb and Cr, associated with historical anthropogenic activities. Although dissolved and particulate metal concentrations were steady for most elements during low and average discharge conditions, significant changes were observed with increasing river discharge. The changes in trace element concentrations in the two compartments was found to induce a partitioning anomaly referred to as the particulate concentration effect. This anomaly was significant for Cr, Mn, Pb, Zn, Cu and organic carbon (p < 0.03). The processes driving this anomaly were possibly linked to the modification and/or increase of colloidal organic and inorganic vectors, suggested by the significant increase of DOC (p < 0.001) and dissolved Al concentrations (p < 0.05) during flood conditions. A complementary process linked to the influence of coarse particles of low complexation capacity and transported mainly during high discharge may also effect trace element concentrations. Annual metal fluxes transported by this river system were estimated using the hysteresis SPM model with consideration of these fate processes. Metals in the Adour River system are primarily exported into the Bay of Biscay (Atlantic Ocean).  相似文献   

6.
Newly developed methods involving an on-line combination of sedimentation field-flow fractionation-inductively coupled plasma-high resolution mass spectrometry (SdFFF-ICP-HRMS) have been used to study the distributions of extractable heavy metals in a soil which had been treated with sewage sludge contaminated with Cu or Pb. The relationship of these metals with other elements in the colloidal fraction was also investigated. The colloidal fraction from the soil was obtained by repeated gravitational sedimentation and extracted with 0.11 M acetic acid, 0.1 M hydroxylamine hydrochloride, 0.05 M ethylenediaminetetraacetic acid disodium salt (EDTA) or aqua regia to assess the potential availability of the metals Cu and Pb. Large proportions of the Cu and Pb were extracted by EDTA, approaching that removed by aqua regia, whereas < 10% of the aqua regia extractable metals were removed by acetic acid and hydroxylamine chloride. The distributions of the heavy metals, the major mineral forming element (Al) and the elements forming sesquioxides (Fe and Mn) within different size classes (0.05-1 microm) of the colloidal fraction were measured using SdFFF-ICP-HRMS before and after extraction with EDTA. This information provides an insight into the composition of the colloids and the distributions of metal contaminants. In the contaminated soil colloids, the concentration of Fe, Mn and Pb is greatest in the smaller particles (<0.2 microm). In contrast, the Cu concentration is constant over the size range studied. Iron oxide surface coatings probably play a significant role in Pb adsorption on soil particles, but may be less important for Cu. The combination of selective chemical extraction, SdFFF and ICP-HRMS provides a means of determining the distribution of potentially available heavy metals within the colloidal fraction of contaminated soils.  相似文献   

7.
Previous studies have shown that the application of soil amendments is efficient in reducing acidity and heavy metal bioavailability in mine soils. However, it remains a challenge for environmentalists to predict accurately and control economically the re-acidification in re-vegetated mine soils. In this study, net acid generation (NAG) test and bioassay technique were employed to assess the effectiveness of the amendments [including lime, N-P-K (nitrogen, phosphorous and potassium) fertilizer, phosphate and river sediment] on re-acidification and heavy metal immobilization in an extremely acid (pH < 3) mine soil. Our results suggested that NAG test was a rapid and accurate approach to assess the effectiveness of the amendments on re-acidification potential of the mine soil. Interestingly, it was found that phosphate and river sediment played quite specific roles in preventing the re-acidification in the mine soil. In addition, the results also indicated that the addition of 25 t ha(-1) lime combined with river sediment (30%) might be an economical method to successfully control the acidification and re-acidification in the extremely acid mine soil, allowing the re-establishment of the plants. Collectively, our results implied that the combined use of NAG test and bioassay assessment was effective in evaluating a reclamation strategy for extremely acidic mine soils.  相似文献   

8.
The distribution of 152Eu between magnesium hydroxide bulk, colloids and solution has been assessed under alkaline conditions, such as those in nuclear fuel storage ponds. The colloidal phase has been characterised by two complementary methods: coupled ultrafiltration-ICP-AES and scanning electron microscopy. The quantity and the size distribution of the colloidal phase is strongly ionic strength-dependent. A decrease of the quantity of colloids, in particular the larger size ranges, has been observed with increasing ionic strength. Small colloids (1 kDa-10 kDa fraction) are predominant at all ionic strengths. The morphology of colloids, observed by field-emission gun scanning electron microscopy, appears to change from hexagonal prismatic (characteristic to the mineral) to spherical (energetically more favourable) as size decreases. The distribution of 152Eu between the solid and liquid/colloidal phases has been investigated at carbonate concentrations ranging from 0 to 10(-2) M by coupled ultrafiltration and gamma-spectrometry. Mg(OH)2 bulk appears to be a very strong sorbent for 152Eu, since complete sorption onto the bulk happens for carbonate concentrations as high as 10(-3) M. Scavenging of 152Eu by Mg(OH)2 colloids is negligible in the presence of Mg(OH)2 bulk. The distribution of 152Eu between liquid and colloidal phases has been investigated in the absence of bulk at various carbonate concentrations. A significant uptake of 152Eu by the colloids in solution has been observed, which decreases with increasing carbonate concentration. 152Eu appears to be mainly associated to the smallest colloids (1 kDa-10 kDa fraction). There is a strong correlation between the sorption properties and the surface area of the colloids.  相似文献   

9.
Mercury (Hg) in estuarine water is distributed among different physical phases (i.e. particulate, colloidal, and truly dissolved). This phase speciation influences the fate and cycling of Hg in estuarine systems. However, limited information exists on the estuarine distribution of colloidal phase Hg, mainly due to the technical difficulties involved in measuring it. In the present study, we determined Hg and organic carbon levels from unfiltered, filtered (<0.45 μm), colloidal (10 kDa-0.45 μm), and truly dissolved (<10 kDa) fractions of Galveston Bay surface water in order to understand the estuarine mixing behavior of Hg species as well as interactions of Hg with colloidal organic matter. For the riverine end-member, the colloidal fraction comprised 43 ± 11% of the total dissolved Hg pool and decreased to 17 ± 8% in brackish water. In the estuarine mixing zone, dissolved Hg and colloidal organic carbon showed non-conservative removal behavior, particularly in the low salinity (<15 ppt) region. This removal may be caused by salt-induced coagulation of colloidal matter and consequent removal of dissolved Hg. The particle-water interaction, K(d) ([particulate Hg (mol kg(-1))]/[dissolved Hg (mol L(-1))]) of Hg decreased as particle concentration increased, while the particle-water partition coefficient based on colloidal Hg and the truly dissolved Hg fraction, K(c) ([colloidal Hg (mol kg(-1))]/[truly dissolved Hg (mol L(-1))]) of Hg remained constant as particle concentration increased. This suggests that the particle concentration effect is associated with the amount of colloidal Hg, increasing in proportion to the amount of suspended particulate matter. This work demonstrates that, colloidal organic matter plays an important role in the transport, particle-water partitioning, and removal of dissolved Hg in estuarine waters.  相似文献   

10.
The validity of a steady-state massbalance model (Arp et al., 1996; referred to asARP) was tested using physicochemical soil data fromthe Monitoring Acid Rain Youth Program (MARYP). FourARP sites were matched with ten MARYP sites accordingto proximity, bedrock type and subsoil pH to test thevalidity of the ARP model for critical loadexceedances. Soil solution pH, base concentration andAl concentration from MARYP sites, which were wellmatched to ARP sites, validated the modelled criticalload exceedances. Higher exceedance areas wereassociated with more acidic pH and lower base andhigher Al concentrations from matched MARYP sites andvice versa. One ARP site was inappropriately matchedwith MARYP sites and could not be validated using baseand Al concentrations. This study also confirmed thesouthern limit of the zero critical load exceedanceisopleth from the model. However, variability of theother exceedance isopleths was noted due to thelimited number of sites used in the model. Thevalidation of these sites in the ARP model and thezero critical load exceedance isopleth nonethelessallows greater confidence in using this model as amanagement tool for acidic deposition.  相似文献   

11.
The purpose of this paper are to determine the concentration of heavy metals namely cadmium (Cd), copper (Cu) and lead (Pb) in water and sediment; and to investigate the effect of sediment pH and sediment organic matter on concentration of cadmium, copper and lead in sediment at oxidation fraction. For this purpose the concentration of heavy metals were measured in water and sediments at 15 sites from Tasik Chini, Peninsular Malaysia. The sequential extraction procedure used in this study was based on defined fractions: exchangeable, acid reduction, oxidation, and residual. The concentration of heavy metals in residual fraction was higher than the other fractions. Among the non-residual fractions, the concentration of heavy metals in organic matter fraction was much higher than other fractions collected from all sampling sites. The pH of the sediment in all sites was acidic. The mean pH ranges from 4.8 to 5.5 with the higher value observed at site 15. Results of organic matter analysis showed that the percentage of organic matter present in sediment samples varies throughout the lake and all sites of sediments were relatively rich in organic matter ranging from 13.0% to 34.2%. The highest mean percentage of organic matter was measured at sampling site 15, with value of 31.78%.  相似文献   

12.
Total mercury (T-Hg) concentrations in rivers are described across a rural to urban/industrial and agricultural landscape gradient in NW England. T-Hg ranges between 0.2 and 230 ng L(-1). The regional median was 3.6 ng L(-1) with individual river medians ranging between 1.9 and 8.3 ng L(-1). Median T-Hg concentrations were sometimes moderately higher for the lowland areas and at higher flows. Our estimates suggest that the Ribble estuary receives 9.2 kg y(-1) and the Wyre estuary 0.7 kg y(-1). In order to examine regional inputs from urban/industrial components, regression analysis was undertaken by comparing three types of hydrochemical signature: suspended sediments (SS), which provide a measure of the particulate component, dissolved organic carbon (DOC) that provides an indication of humic/fulvic acids that are part of the organic colloids and strong chelating agents, and boron a marker of sewage effluents and population density. The results show high positive relationships of T-Hg with both SS and DOC, but no relationship with the urban/industrial signal. The regression analysis with T-Hg indicated on average a gradient of 0.33 ng mg(-1) for DOC and 0.2 ng mg(-1) for SS. They indicate the primary importance of a diffuse source of T-Hg. For the upland areas and cleaner river systems, the linkages between T-Hg and DOC were particularly strong, while for the lowland areas, the linkage with SS proved stronger. Analysis of a latter subset of data that partition the SS into organic and inorganic fractions indicated that the T-Hg was primarily linked with the organic fraction. Indeed, multiple regression of T-Hg with DOC and POM reveals gradients similar to other parts of the World.  相似文献   

13.
Aluminium (Al) toxicity is usually associated with acid rain and acidified freshwater systems. The present work demonstrates that acute fish mortality (50%) also occurs in moderate acidified salmon rivers during sea salt episodes. Furthermore, catchment liming was proved to be an efficient measure to counteract the fish toxicity. The impact of sea salt episodes on river water qualities and on Atlantic Salmon (Salmo salar L.) was studied in two rivers situated at the west coast of Norway. During February-May 2002, fish were kept in tanks and continually exposed to the changing water qualities. Changes in Al-species were followed using in situ fractionation techniques. During storm events and high sea salt deposition, the sea salt concentration increased (190 to 580 microM Cl), pH decreased (pH 5.3 to 4.6) and the concentration of low molecular mass (LMM) cationic Al-species (Al(i)) increased (0.7 to 3.0 microM) in the river. Subsequently, Al accumulated in fish gills (6 to 19 micromol g(-1) dw) causing ionoregulatory and respiratory failures as well as mortality. In water the concentration of LMM Al(i) stayed enhanced during four weeks, while the physiological stress responses in surviving fish remained high for a longer time (>eight weeks). To counteract Al toxicity, one of the tributary catchments had been limed four years earlier. Due to catchment liming (1000 kg ha(-1)) the water concentration of LMM Al(i)(<0.7 microM) and the Al accumulation in gills remained relatively low (<7 micromol g(-1) dw) during the storm and no fish mortality occurred.  相似文献   

14.
An on-line method has been developed for separating inorganic and organic bound uranium species present in river water samples. The method utilised a small chelating resin (Hyphan) column incorporated into the sample introduction manifold of an ICP-MS instrument. The method was evaluated for samples from rivers on Dartmoor (Devon, UK), an area of granite overlain with peat bogs. The results indicate that organic-uranium species form a major proportion (80%) of the total dissolved uranium present. Further work with synthetic water samples indicated that the level of dissolved organic carbon played a greater role in determining the level of organic-uranium species than did sample pH. Computer models for the water samples were constructed using the WHAM program (incorporating uranium data from the Nuclear Energy Agency Thermochemical Database project) in order to predict the levels of organic-uranium species that would form. By varying the proportion of humic and fulvic acids used in the humic component, predictions within 10% of the experimental results were obtained. The program did exhibit a low bias at higher pH values (7.5) and low organic carbon concentrations (0.5 microg ml(-1)), but under the natural conditions prevalent in the Dartmoor water samples, the model predictions were successful.  相似文献   

15.
16.
Soil acidification, caused by elevated anthropogenic deposition, has led to concerns over nutrient imbalances in Ontario's sugar maple (Acer saccharum Marsh.) forests. In this study, soil chemistry, foliar chemistry, crown condition, and tree growth were measured at 36 sugar maple stands that included acidic (pH?相似文献   

17.
The seasonal variability of inorganic and organic nutrients and stable isotopes and their relations with plankton and environmental conditions were monitored in Lake Chasicó. Principal component analysis evidenced the strong influence of the river runoff on several biogeochemical variables. Silicate concentrations were controlled by diatom biomass and river discharge. Higher values of nitrate and soluble reactive phosphorus (SRP) indicated agricultural uses in the river basin. Elevated pH values (~9) inhibiting nitrification in the lake explained partially the dominance of ammonium: ~83 % of dissolved inorganic nitrogen (DIN). The low DIN/SRP ratio inferred nitrogen limitation, although the hypotheses of iron and CO2 limitation are relevant in alkaline lakes. Particulate organic matter (POM) and dissolved organic matter (DOM) were mainly of autochthonous origin. The main allochthonous input was imported by the river as POM owning to the arid conditions. Dissolved organic carbon was likely top-down regulated by the bacterioplankton grazer Brachionus plicatilis. The δ13C signature was a good indicator of primary production and its values were influenced probably by CO2 limitation. The δ15N did not evidence nitrogen fixation and suggested the effects of anthropogenic activities. The preservation of a good water quality in the lake is crucial for resource management.  相似文献   

18.
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   

19.
Large-scale exposure of acid sulfate soils during a hydrological drought in the Lower Lakes of South Australia resulted in acidification of surface water in several locations. Our aim was to describe the techniques used to monitor, assess and manage these acidification events using a field and laboratory dataset (n?=?1,208) of acidic to circum-neutral pH water samples. The median pH of the acidified (pH?<?6.5) samples was 3.8. Significant (p?<?0.05) increases in soluble metals (Al, Co, Mn, Ni and Zn above guidelines for ecosystem protection), SO4 (from pyrite oxidation), Si (from aluminosilicate dissolution) and Ca (from carbonate dissolution and limestone addition), were observed under the acidic conditions. The log of the soluble metal concentrations, acidity and SO4/Cl ratio increased linearly with pH. The pH, alkalinity and acidity measurements were used to inform aerial limestone dosing events to neutralise acidic water. Field measurements correlated strongly with laboratory measurements for pH, alkalinity and conductivity (r 2?≥?0.97) but only moderately with acidity (r 2?=?0.54), which could be due to difficulties in determining the indicator-based field titration endpoint. Laboratory measured acidity correlated well with calculated acidity (r 2?=?0.87, acidity present as AlIII?>>?H+?≈?MnII?>?FeII/III) but was about 20 % higher on average. Geochemical speciation calculations and XRD measurements indicated that solid phase minerals (schwertmannite and jarosite for Fe and jurbanite for Al) were likely controlling dissolved metal concentrations and influencing measured acidity between pH 2 and 5.  相似文献   

20.
Increasing urbanization and changes in land use in Langat river basin lead to adverse impacts on the environment compartment. One of the major challenges is in identifying sources of organic contaminants. This study presented the application of selected chemometric techniques: cluster analysis (CA), discriminant analysis (DA), and principal component analysis (PCA) to classify the pollution sources in Langat river basin based on the analysis of water and sediment samples collected from 24 stations, monitored for 14 organic contaminants from polycyclic aromatic hydrocarbons (PAHs), sterols, and pesticides groups. The CA and DA enabled to group 24 monitoring sites into three groups of pollution source (industry and urban socioeconomic, agricultural activity, and urban/domestic sewage) with five major discriminating variables: naphthalene, pyrene, benzo[a]pyrene, coprostanol, and cholesterol. PCA analysis, applied to water data sets, resulted in four latent factors explaining 79.0% of the total variance while sediment samples gave five latent factors with 77.6% explained variance. The varifactors (VFs) obtained from PCA indicated that sterols (coprostanol, cholesterol, stigmasterol, β-sitosterol, and stigmastanol) are strongly correlated to domestic and urban sewage, PAHs (naphthalene, acenaphthene, pyrene, benzo[a]anthracene, and benzo[a]pyrene) from industrial and urban activities and chlorpyrifos correlated to samples nearby agricultural sites. The results demonstrated that chemometric techniques can be used for rapid assessment of water and sediment contaminations.  相似文献   

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