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1.
Distribution of colloidal trace metals in the San Francisco Bay estuary 总被引：11，自引：0，他引：11
Sergio A. Sañudo-Wilhelmy Ignacio Rivera-Duarte A. Russell Flegal 《Geochimica et cosmochimica acta》1996,60(24):4933-4944
The size distribution of trace metals (Al, Ag, Cd, Cu, Fe, Mn, Ni, Sr, and Zn) was examined in surface waters of the San Francisco Bay estuary. Water samples were collected in January 1994 across the whole salinity gradient and fractionated into total dissolved (<0.2 μm colloidal (10 KDa–0.2 μm) and < 10 kDa molecular weight phases. In the low salinity region of the estuary, concentrations of colloidal A1, Ag, and Fe accounted for ≥84% of the total dissolved fraction, and colloidal Cu and Mn accounted for 16–20% of the total. At high salinities, while colloidal Fe was still relatively high (40% of the dissolved), very little colloidal Al, Mn, and Cu (<10%) and no colloidal Ag was detectable. Colloidal Zn accounted for <3% of the total dissolved along the estuary, and colloidal Ni was only detectable (<2%) at the river endmember. All of the total dissolved Cd and Sr throughout the estuary consisted of relatively low molecular weight (<10 kDa) species. The relative affinity of metals for humic substances and their reactivity with particle surfaces appear to determine the amounts of metal associated with colloids. The mixing behavior of metals along the estuary appears to be determined by the relative contribution of the colloidal phase to the total dissolved pool. Metals with a small or undetectable colloidal fraction showed a nonconservative excess (Cd, Cu, Ni, and Mn) or conservative mixing (Sr) in the total dissolved fraction, relative to ideal dilution of river water and seawater along the estuary.
The salt-induced coagulation of colloidal A1, Fe, and Cu is indicated by their highly nonconservative removal along the salinity gradient. However, colloidal metals with low affinity for humic substances (Mn and Zn) showed conservative mixing behavior, indicating that some riverine colloids are not effectively aggregated during their transport to the sea. While colloidal metal concentrations correlated with dissolved organic carbon, they also covaried with colloidal Al, suggesting that colloids are a mixture of organic and inorganic components. Furthermore, the similarity between the colloidal metal:A1 ratios with the crustal ratios indicated that colloids could be the product of weathering processes or particle resuspension. Distribution coefficients for colloidal particles (Kc) and for large, filter-retained particles (Kd) were of the same magnitude, suggesting similar binding strength for the two types of particles. Also, the dependence of the distribution coefficients on the amount of suspended particulate matter (the so-called particle concentration effect) was still evident for the colloids-corrected distribution coefficient (Kp+c) and for metals (e.g., Ni) without affinity for colloidal particles. 相似文献
2.
Changes in size distribution of fresh water nanoscale colloidal matter and associated elements on mixing with seawater 总被引：1，自引：0，他引：1
Changes in size distribution and elemental composition of 0.5-50 nm fresh water colloids during estuarine mixing have been studied by in-laboratory mixing of natural creek water and synthetic seawater, followed by size fractionation with Asymmetrical Flow Field-Flow Fractionation, and online elemental quantification by High-Resolution ICPMS. At least two types of colloids were present in the studied size region; 0.5-3 nm fluorescent dissolved organic matter (FDOM), and >3 nm colloids that were rich in Fe and colored dissolved organic matter (CDOM). Most trace elements were associated in different proportions to these two populations of colloids. Following mixing with synthetic seawater, the >3 nm Fe-rich colloids and CDOM were extensively removed from the studied size region by salt induced aggregation. The degree of removal with increasing salinity was greatest below 2.5‰ salinity, continued to a lesser degree between 2.5‰ and 15‰ salinity, above which only very small additional removal could be distinguished. At 25‰ salinity, the Fe concentration in the 0.5-50 size region had been reduced down to 15% of its original value in freshwater, while the amount of CDOM had been reduced to 55%. On the contrary, the concentration of the 0.5-3 nm FDOM was unchanged by the increased concentration of sea salt. Therefore, colloidally associated Al, P, Co, Cu, Zn, Ce, Lu and Pb were removed from the 0.5-50 nm size region according to their relative distributions between the FDOM and the Fe-rich colloids. Consequently, at 25‰ salinity, the 0.5-50 nm concentrations of Al, Mn, P and Pb, (mainly associated with the Fe-rich colloids) had been reduced down to 13-26 % of their values in freshwater, while the concentrations of Co and Cu (with higher preferences for FDOM) were less reduced, down to 46% and 57%, respectively. Changes in the elemental composition of the remaining colloidal matter were observed, the most pronounced were increased contents of P, Al and Pb in Fe-rich colloidal matter of medium size (∼3-15 nm) and increased Pb content in Fe-rich colloidal matter of larger size (∼5-50 nm). 相似文献
3.
4.
《Applied Geochemistry》2000,15(5):655-666
A process model was used to better understand the controls on the chemical evolution of drainage in a historic mining district. At the Pecos Mine Operable Unit, New Mexico, drainage near the waste rock pile is acidic (pH varies from 3.0–5.0) and carries high concentrations of Zn, Al, Cu and Pb. As drainage flows toward the Pecos River, pH increases to greater than 7 and heavy metal content decreases. A process model of natural attenuation in this drainage shows the main controls on pH are reaction with a local bedrock that contains limestone, and concurrent mixing with tributary streams. Models that account for both calcite dissolution and mixing reproduce the observed decrease in aqueous metal concentrations with increasing pH. Contaminant concentrations attenuate primarily via two distinct pathways: Al, Cu, Fe and Pb precipitate directly from solution, whereas Zn, Mg, Mn and SO4 concentrations decrease primarily through dilution. Additionally, Pb adsorbs to precipitating hydroxide surfaces. 相似文献
5.
The authors determine the composition of a river that is impacted by acid-mine drainage, evaluate dominant physical and geochemical processes controlling the composition, and assess dissolved metal speciation and toxicity using a combination of laboratory, field and modeling studies. Values of pH increase from 3.3 to 7.6 and the sum of dissolved base metal (Cd + Co + Cu + Ni + Pb + Zn) concentrations decreases from 6270 to 100 μg/L in the dynamic mixing and reaction zone that is downstream of the river’s confluence with acid-mine drainage. Mixing diagrams and PHREEQC calculations indicate that mixing and dilution affect the concentrations of all dissolved elements in the reach, and are the dominant processes controlling dissolved Ca, K, Li, Mn and SO4 concentrations. Additionally, dissolved Al and Fe concentrations decrease due to mineral precipitation (gibbsite, schwertmannite and ferrihydrite), whereas dissolved concentrations of Cd, Co, Cu, Ni, Pb and Zn decrease due to adsorption onto newly formed Fe precipitates. 相似文献
6.
《Applied Geochemistry》1995,10(3):285-306
Inflows of metal-rich, acidic water that drain from mine dumps and tailings piles in the Leadville, Colorado, area enter the non-acidic water in the upper Arkansas River. Hydrous iron oxides precipitate as colloids and move downstream in suspension, particularly downstream from California Gulch, which has been the major source of metal loads. The colloids influence the concentrations of metals dissolved in the water and the concentrations in bed sediments. To determine the role of colloids, samples of water, colloids, and fine-grained bed sediment were obtained at stream-gaging sites on the upper Arkansas River and at the mouths of major tributaries over a 250-km reach. Dissolved and colloidal metal concentrations in the water column were operationally defined using tangential-flow filtration through 0.001-pm membranes to separate the water and the colloids. Surface-extractable and total bed sediment metal concentrations were obtained on the <60-μm fraction of the bed sediment. The highest concentrations of metals in water, colloids, and bed sediments occurred just downstream from California Gulch. Iron dominated the colloid composition, but substantial concentrations of As, Cd, Cu, Mn, Pb, and Zn also occurred in the colloidal solids. The colloidal load decreased by one half in the first 50 km downstream from the mining inflows due to sedimentation of aggregated colloids to the streambed. Nevertheless, a substantial load of colloids was transported through the entire study reach to Pueblo Reservoir. Dissolved metals were dominated by Mn and Zn, and their concentrations remained relatively high throughout the 250-km reach. The composition of extractable and total metals in bed sediment for several kilometers downstream from California Gulch is similar to the composition of the colloids that settle to the bed. Substantial concentrations of Mn and Zn were extractable, which is consistent with sediment-water chemical reaction. Concentrations of Cd, Pb, and Zn in bed sediment clearly result from the influence of mining near Leadville. Concentrations of Fe and Cu in bed sediments are nearly equal to concentrations in colloids for about 10 km downstream from California Gulch. Farther downstream, concentrations of Fe and Cu in tributary sediments mask the signal of mining inflows. These results indicate that colloids indeed influence the occurrence and transport of metals in rivers affected by mining. 相似文献
7.
《Applied Geochemistry》1997,12(4):447-464
The controls on metal concentrations in a plume of acidic (pH 3.29–5.55) groundwater in the Moon Creek watershed in Idaho, U.S.A., were investigated with the use of property-property plots. A plot of Ca vs S demonstrated that a plume of contaminated groundwater was being diluted by infiltration of rain and creek water at shallow depths and by ambient groundwater near bedrock. The small amount of dissolved Fe (2.1 mg/l) was removed while dissolved Pb was added, reaching a maximum concentration of 0.37 mg/l. The other metals (Zn ≤ 16, Al ≤ 6.2, Cu ≤ 2.1 and Cd ≤ 0.077 mg/l) in the shallow groundwater were essentially conserved until they emerged as a seep along the creek bank. Upon mixing with the creek water, groundwater was diluted by factors between 11 and 50, and the pH of the mixture became neutral. Metals originating from the contaminated groundwater were removed in the creek in the following order: Fe > Al > Pb ≫ Cu > Mn > Zn = Cd.Pb and Cu continued to be removed from solution even as the creek passed adjacent to a tailings pile. In contrast, Zn concentrations in the creek increased adjacent to the tailings area, presumably as a result of the reemergence of the upgradient plume as the creek lost elevation.Below the tailings dam, contaminated creek water (400–800 μg Zn/l) was diluted by both smaller side streams and a creek of equal flow. The presence of 3 distinctive water masses required the use of two tracers (dissolved Si and S) to distinguish between mixing and geochemical reactions. The removal of metals was greater during low flow conditions. Pb was removed to the greatest extent, falling below detection limits (0.5 μ/l) at the first sampling location. Copper and Mn were removed to a lesser extent during low flow conditions and approached conservative behavior during high flow conditions. During a 5-km journey through two hydrological regimes, less than 10% of the dissolved Zn and Cd was lost. 相似文献
8.
Arctic rivers typically transport more than half of their annual amounts of water and suspended sediments during spring floods. In this study, the Sagavanirktok, Kuparuk and Colville rivers in the Alaskan Arctic were sampled during the spring floods of 2001 to determine levels of total suspended solids (TSS) and dissolved and particulate metals and organic carbon. Concentrations of dissolved organic carbon (DOC) increased from 167 to 742 μmol/L during peak discharge in the Sagavanirktok River, at about the same time that river flow increased to maximum levels. Concentrations of dissolved Cu, Pb, Zn and Fe in the Sagavanirktok River followed trends observed for DOC with 3- to 25-fold higher levels at peak flow than during off-peak discharge. Similar patterns were found for the Kuparuk and Colville rivers, where average concentrations of dissolved trace metals and DOC were even higher. These observations are linked to a large pulse of DOC and dissolved metals incorporated into snowmelt from thawing ponds and upper soil layers. In contrast with Cu, Fe, Pb and Zn, concentrations of dissolved Ba did not increase in response to increased discharge of water, TSS and DOC. Concentrations of particulate Cu, Fe, Pb and Zn were more uniform than observed for their respective dissolved species and correlated well with the Al content of the suspended particles. However, concentrations of particulate Al were poorly correlated with particulate organic carbon. Results from this study show that >80% of the suspended sediment and more than one-third of the annual inputs of dissolved Cu, Fe, Pb, Zn and DOC were carried to the coastal Beaufort Sea in 3 and 12 d, respectively, by the Kuparuk and Sagavanirktok rivers. 相似文献
9.
The chemical status of major and trace elements (TE) in various boreal small rivers and watershed has been investigated along a 1500-km transect of NW Russia. Samples were filtered in the field through a progressively decreasing pore size (5, 0.8 and 0.22 μm; 100, 10, and 1 kD) using a frontal filtration technique. All major and trace elements and organic carbon (OC) were measured in filtrates and ultrafiltrates. Most rivers exhibit high concentration of dissolved iron (0.2–4 mg/l), OC (10–30 mg/l) and significant amounts of trace elements usually considered as immobile in weathering processes (Ti, Zr, Th, Al, Ga, Y, REE, V, Pb). In (ultra)filtrates, Fe and OC are poorly correlated: iron concentration gradually decreases upon filtration from 5 μm to 1 kD whereas the major part of OC is concentrated in the <1–10 kD fraction. This reveals the presence of two pools of colloids composed of organic-rich and Fe-rich particles. According to their behavior during filtration and association with these two types of colloids, three groups of elements can be distinguished: (i) species that are not affected by ultrafiltration and are present in the form of true dissolved inorganic species (Ca, Mg, Li, Na, K, Sr, Ba, Rb, Cs, Si, B, As, Sb, Mo) or weak organic complexes (Ca, Mg, Sr, Ba), (ii) elements present in the fraction smaller than 1–10 kD prone to form inorganic or organic complexes (Mn, Co, Ni, Zn, Cu, Cd, and, for some rivers, Pb, Cr, Y, HREE, U), and (iii) elements strongly associated with colloidal iron in all ultrafiltrates (P, Al, Ga, REE, Pb, V, Cr, W, Ti, Ge, Zr, Th, U). Based on size fractionation results and taking into account the nominal pore size for membranes, an estimation of the effective surface area of Fe colloids was performed. Although the total amount of available surface sites on iron colloids (i.e., 1–10 μM) is enough to accommodate the nanomolar concentrations of dissolved trace elements, very poor correlation between TE and surface sites concentrations was observed in filtrates and ultrafiltrates. This strongly suggests a preferential transport of TE as coprecipitates with iron oxy(hydr)oxides. These colloids can be formed on redox boundaries by precipitation of Fe(III) from inflowing Fe(II)/TE-rich anoxic ground waters when they meet well-oxygenated surface waters. Dissolved organic matter stabilizes these colloids and prevents their aggregation and coagulation. Estuarine behavior of several trace elements was studied for two small iron- and organic-rich rivers. While Si, Sr, Ba, Rb, and Cs show a clear conservative behavior during mixing of freshwaters with the White sea, Al, Pb and REE are scavenged with iron during coagulation of Fe hydroxide colloids. 相似文献
10.
A dialysis procedure was used to assess the distribution coefficients of ∼50 major and trace elements (TEs) between colloidal (1 kDa–0.22 μm) and truly dissolved (<1 kDa) phases in Fe- and organic-rich boreal surface waters. These measurements allowed quantification of both TE partitioning coefficients and the proportion of colloidal forms as a function of solution pH (from 3 to 8). Two groups of elements can be distinguished according to their behaviour during dialysis: (i) elements which are strongly associated with colloids and exhibit significant increases of relative proportion of colloidal forms with pH increase (Al, Ba, Cd, Co, Cr, Cu, Fe, Ga, Hf, Mn, Ni, Pb, rare earth elements (REEs), Sr, Th, U, Y, Zn, Zr and dissolved organic C) and (ii) elements that are weakly associated with colloids and whose distribution coefficients between colloidal and truly dissolved phases are not significantly affected by solution pH (As, B, Ca, Cs, Ge, K, Li, Mg, Mo, Na, Nb, Rb, Sb, Si, Sn, Ti, V). Element speciation was assessed using the Visual MINTEQ computer code with an implemented NICA-Donnan humic ion binding model and database. The model reproduces quantitatively the pH-dependence of colloidal form proportion for alkaline-earth (Ba, Ca, Mg, Sr) and most divalent metals (Co, Cd, Mn, Ni, Pb, Zn) implying that the complexation of these metals with low molecular weight organic matter (<1 kDa fraction) is negligible. In contrast, model prediction of colloidal proportion (fraction of 1 kDa–0.22 μm) of Cu2+ and all trivalent and tetravalent metals is much higher than that measured in the experiment. This difference may be explained by (i) the presence of strong metal-binding organic ligands in the <1 kDa fraction whose stability constants are several orders of magnitude higher than those of colloidal humic and fulvic acids and/or (ii) coprecipitation of TE with Fe(Al) oxy(hydr)oxides in the colloidal fraction, whose dissolution and aggregation controls the pH-dependent pattern of TE partitioning. Quantitative modeling of metal – organic ligand complexation and empirical distribution coefficients corroborate the existence of two colloidal pools, formerly reported in boreal surface waters: “classic” fulvic or humic acids binding divalent transition metals and alkaline-earth elements and large-size organo-ferric colloids transporting insoluble trivalent and tetravalent elements. 相似文献
11.
《Applied Geochemistry》2002,17(5):569-581
This study examined the sorption of trace metals to precipitates formed by neutralization of 3 natural waters contaminated with acid mine drainage (AMD) in the former Ducktown Mining District, Tennessee. The 3 water samples were strongly acidic (pH 2.2 to 3.4) but had distinctively different chemical signatures based on the mole fractions of dissolved Fe, Al and Mn. One sample was Fe-rich (Fe=87.5%, Al=11.3%, and Mn=1.3%), another was Al-rich (Al=79.4%, Mn=18.0%, and Fe=2.5%), and the other was Mn-rich (Mn=51.4%, Al=25.7%, and Fe=22.9%). In addition, these waters had high concentrations of trace metals including Zn (37,700 to 17,400 μg/l), Cu (13,000 to 270 μg/l), Co (1,500 to 520 μg/l), Ni (360 to 75 μg/l), Pb (30 to 8 μg/l), and Cd (30 to 6 μg/l). Neutralization of the AMD-contaminated waters in the laboratory caused the formation of either schwertmannite at pH<4 or ferrihydrite at pH>4. Both phases were identified by XRD analyses of precipitates from the most Fe-rich water. At higher pH values (∼5) Al-rich precipitates were formed. Manganese compounds were precipitated at pH∼8. The removal of trace metals depended on the precipitation of these compounds, which acted as sorbents. Accordingly, the pH for 50% sorption (pH50) ranged from 5.6 to 7.5 for Zn, 4.6 to 6.1 for Cu, 5.4 to 7.7 for Ni, 5.9 to 7.9 for Co, 3.1 to 4.3 for Pb, and 5.5 to 7.7 for Cd. The pH dependence of sorption arose not only because of changes in the sorption coefficients of the trace metals but also because the formation and composition of the sorbent was controlled by the pH, the chemical composition of the water, and the solubilities of the oxyhydroxide-sulfate complexes of Fe, Al, and Mn. 相似文献
12.
Heavy metal pollution in the surrounding ore deposits and mining activity: a case study from Koyulhisar (Sivas-Turkey) 总被引：1，自引：1，他引：0
The oxidation of sulfide minerals generates acidic waters containing high levels of SO4 and Fe. The study area has active Pb?CZn?CCu mining. It is thought that the surface/subsurface/underground sulfide minerals in the region generally contribute to the acidification of groundwater. Low pH values are also responsible for dissolved metals (Al, Fe, Mn, SO4, Pb, Zn) in the groundwater and river. Furthermore, current mining wastes have affected concentrations of trace elements in the water. High Fe and Mn concentrations are generally found in the spring which has acidic and low Eh values, while Al, Fe and Mn concentrations in the acidic waters show notable increases with the maximum values reaching 8,829, 19,084 and 1,708?ppb, respectively. These values exceed the Turkish drinking water standard of 200, 200 and 50?ppb, respectively. 相似文献
13.
The flood zone of the Ob River, the largest (in watershed area) river of the Arctic Ocean basin, is tens of km wide and, after the Amazon's Varzea, is the world's second largest flooding territory. To better understand the biogeochemistry of the Ob River and adjacent surface waters, we studied, in May and July 2014, the dissolved and colloidal organic carbon and trace metals in small rivers, lakes, and flooded water bodies connected and disconnected with the mainstream as well as the Ob River itself. All major and trace elements were distributed among two major categories depending on their pattern of dependence on the dissolved organic carbon (DOC) concentration. Dissolved inorganic carbon (DIC), Na, Mg, Ca, sulfate, Sr, Mo, Sb and U exhibited a general decrease in concentration with the increase of the [DOC]. The lowest concentration of these elements was observed in DOC-rich humic, acidic (4.9 ≤ pH ≤ 6.1) upland lakes fed by surrounding bogs. These elements marked the influence of underground feeding in July during summer baseflow, which was most visible in flood lakes in the Ob riparian zone and the Ob River itself. In May, the flood lakes were statistically similar to the Ob River. The elevated concentration of DOC (up to 60 mg/L) in the upland lakes was not correlated with groundwater-related elements, suggesting a lack of significant groundwater feeding in these lakes. In contrast, insoluble, usually low mobile elements (Al, Fe, other trivalent hydrolysates, Ti, Zr, Hf) and some metals (Cr, Zn, Ni, Pb) demonstrated a steady increase in concentration with increasing DOC, with the lowest values observed in the Ob River and the highest values observed in small tributaries and organic-rich upland lakes in July. It follows that these elements are limited by their main carriers – organic and organo-ferric colloids, rather than by the availability of the source, peat and mineral soil or plant litter. While for the majority of non-colloidal, groundwater-fed elements with high mobility (DIC, Na, Mg, Ca, K, Sr…) the small tributaries can be used as representatives of the Ob main stream, this is not the case for low mobility “insoluble” elements, such as Fe, Al, trivalent and tetravalent hydrolysates, and metal micronutrients (Cu, Zn, and Mn). The low soluble elements and divalent metals exhibited a much lower concentration in the river mainstream compared to that in the flood lakes, upland lakes and small rivers. This difference is significantly more pronounced in the baseflow in July compared to the spring flood in May. Presumably, autochthonous processes, such as the photo-oxidation and bio-oxidation of organo-ferric colloids and phytoplankton uptake are capable decreasing the concentration of these elements in the river mainstream. 相似文献
14.
Flocculation of colloidal size fraction for Cu, Zn, Pb, Ni and Mn was investigated on a series of mixtures with water salinities
ranging from 1.5 to 9.5‰ during mixing of Haraz River with the Caspian Sea water. The flocculation trend of Zn (85.5%) > Mn
(55.2%) > Cu (39.6%) > Pb (33.7%) > Ni (11.3%) indicates that Cu, Zn, Pb and Mn have non-conservative behavior and Ni has
relatively conservative behavior during estuarine mixing. Highest flocculation of heavy metals occurs between salinities of
1.5 and 4.5‰. Statistical analysis indicates that the flocculation of Cu, Zn and Ni is governed by pH and total nitrogen. 相似文献
15.
Wan Ying Lim Ahmad Zaharin Aris Tengku Hanidza Tengku Ismail Mohamad Pauzi Zakaria 《Environmental Earth Sciences》2013,70(3):993-1004
This paper discusses the hydrochemistry variation and its quality status in Langat River, based on the chemistry of major ions, metal concentrations and suitability for drinking purposes. Water samples were collected from 30 different stations to assess their hydrochemical characteristics. The physico-chemical parameters selected were temperature, electrical conductivity, total dissolved solids (TDS), salinity, dissolved oxygen , pH, redox potential, HCO3, Cl, SO4, NO3, Ca, Na, K, Mg, 27Al, 138Ba, 9Be, 111Cd, 59Co, 63Cu, 52Cr, 57Fe, 55Mn, 60Ni, 208Pb, 80Se and 66Zn to investigate the variation of the constituents in the river water. Most of the parameters comply with the Drinking Water Quality Standard of the World Health Organization and the Malaysian National Standard for Drinking Water Quality by the Malaysia Ministry of Health except for EC, TDS, Cl, HCO3, SO4, Na, Mg, Al, Fe and Se. The results show that the Langat River is unsuitable for drinking purposes directly without treatment. 相似文献
16.
《Applied Geochemistry》2005,20(7):1391-1408
Surface water samples from the St. Lawrence River were collected in order to study the processes controlling minor and trace elements concentrations (Al, Fe, Mn, Cd, Co, Cu, Ni and Zn), and to construct mass balances allowing estimates of the relative importance of their natural and anthropogenic sources. The two major water inputs, the upper St. Lawrence River, which drains waters originating from the Lake Ontario, and the Ottawa River were collected fortnightly over 18 months. In addition, other tributaries were sampled during the spring floods. The output was monitored near Quebec City at the river mouth weekly between 1995 and 1999. Dissolved metal concentrations in the upper St. Lawrence River carbonated waters were lower than in the acidic waters of the tributaries draining the crystalline rocks of the Canadian shield and the forest cover. Biogeochemical and hydrodynamic processes occurring in Lake Ontario drive the seasonal variations observed in the upper St. Lawrence River. Biogeochemical processes relate to biological uptake, regeneration of organic matter (for Cd and Zn) and oxyhydroxide formation (for Mn and Fe), while hydrodynamic processes mainly concern the seasonal change in vertical stratification (for Cd, Mn, and Zn). In the Ottawa River, the main tributary, oxyhydroxide formation in summer governs seasonal patterns of Al, Fe, Mn, Cd, Co and Zn. The downstream section of the St. Lawrence River is a transit zone in which seasonal variations are mainly driven by the mixing of the different water masses and the large input of suspended particulate matter from erosion. The budget of all dissolved elements, except Fe and Zn, was balanced, as the budget of particulate elements (except Cd and Zn). The main sources of metals to the St. Lawrence River are erosion and inputs from tributaries and Lake Ontario. Direct anthropogenic discharges into the river accounted for less than 5% of the load, except for Cd (10%) and Zn (21%). The fluxes in transfer of dissolved Cd, Co, Cu and Zn species from the river to the lower St. Lawrence estuary were equal to corresponding fluxes calculated for Quebec City since the distributions of dissolved concentrations of these metals versus salinity were conservative. For Fe, the curvature of the dilution line obtained suggests that dissolved species were removed during early mixing. 相似文献
17.
Urbanisation and industrial development lead to contamination of estuaries and streams with dispersed loadings of heavy metals and metalloids. Contributions of these elements also occur from natural sources. This study provides baseline geochemical data on the respective natural and anthropogenic inputs of Cu, Pb, Zn, Cd, As, Sb, Cr, Ni, Mn and S to estuarine, fluvial and wetland sediments, and adjacent soils, in the Kooloonbung Creek catchment that drains the Port Macquarie urban area in north coastal New South Wales. There have been anthropogenic additions of Cu, Pb, Zn and As from dispersed urban sources at Port Macquarie, but they are restricted to the local catchment and do not impact on the adjacent Hastings River estuary. The most contaminated sediments display enrichment factors up to 20 × for Cu and Pb, 9 × for Zn and 5 × for As relative to local background values. However, only one value (for Pb) exceeds National Water Quality Management Strategy interim sediment quality guideline (high) values. On the other hand, sediments and local soils are commonly strongly enriched in Cr, Ni and Mn, reflecting adjacent ultramafic and mafic rock substrate and lateritic regolith. Concentrations of Cr and Ni are commonly well above interim sediment quality guideline (high) values for sediments, but are in mineralogical forms that are not readily bioavailable. Sediment and soil quality guideline values consequently need to recognise natural enrichments and the mineralogical siting of heavy metals. Although dissolved concentrations of heavy metals in stream waters are commonly low, there is evidence for mobility of Cu, Zn, Fe and Al. Parts of the Kooloonbung Creek wetland area lie on sulfidic estuarine sediments (potential acid sulfate soils). Experimental oxidation of uncontaminated and contaminated sulfidic sediments leads to substantial dissolution of heavy metals under acid conditions, with subsequent aquatic mobility. The results warn about disturbance and oxidation of potential acid sulfate soils that have been contaminated by urban and natural heavy-metal sources. 相似文献
18.
Keith A. Hunter 《Geochimica et cosmochimica acta》1983,47(3):467-473
The estuarine mixing of dissolved Fe, Cu, Ni, Si and surface-active organic matter has been investigated in the Taieri Estuary, New Zealand, simultaneously with measurements of the electrokinetic charge on colloidal particles. Dissolved Fe showed almost quantitative removal from solution characteristic of the coagulation of iron-containing colloids by seawater electrolytes. Surface active organic matter behaved conservatively, indicating that a relatively constant fraction of estuarine organic matter is surface active, but that organic species associated with iron during removal are a minor fraction. Results for Cu, Ni and Si were scattered but offered no evidence for gross removal during estuarine mixing. The negative charge on suspended colloids was not reversed by adsorption of seawater cations, but remained uniformly negative throughout the salinity range, decreasing sharply in magnitude during the first few %. salinity. 相似文献
19.
Corinne Casiot Marion Egal Françoise Elbaz-Poulichet Odile Bruneel Chrystelle Bancon-Montigny Marie-Ange Cordier Elena Gomez Catherine Aliaume 《Applied Geochemistry》2009
Dissolved and particulate concentrations of metals (Fe, Al, Mn, Co, Ni, Cu, Zn, Cd, Tl, Pb) and As were monitored over a 5 year period in the Amous River downstream of its confluence with a creek severely affected by acid mine drainage (AMD) originating from a former Pb–Zn mine. Water pH ranged from 6.5 to 8.8. Metals were predominantly in dissolved form, except Fe and Pb, which were in particulate form. In the particulate phase, metals were generally associated with Al oxides, whereas As was linked to Fe oxides. Metal concentrations in the dissolved and/or particulate phase were generally higher during the wet season due to higher generation of AMD. Average dissolved (size < 0.22 μm) metal concentrations (μg/L) were 1 ± 4 (Fe), 69 ± 49 (Al), 140 ± 118 (Mn), 4 ± 3 Co, 6 ± 4 (Ni), 1.3 ± 0.8 (Cu), 126 ± 81 (Zn), 1.1 ± 0.7 (Cd), 0.9 ± 0.5 (Tl), 2 ± 3 (Pb). Dissolved As concentrations ranged from 5 to 134 μg/L (30 ± 23 μg/L). During the survey, the concentration of colloidal metals (5 kDa < size < 0.22 μm) was less than 25% of dissolved concentrations. Dissolved metal concentrations were generally higher than the maximum concentrations allowed in European surface waters for priority substances (Ni, Cd and Pb) and higher than the environmental quality standards for other compounds. Using Diffusion Gradient in Thin Film (DGT) probes, metals were shown to be in potentially bioavailable form. The concentrations in Leuciscus cephalus were below the maximum Pb and Cd concentrations allowed in fish muscle for human consumption by the European Water Directive. Amongst the elements studied, only As, Pb and Tl were shown to bioaccumulate in liver tissue (As, Pb) or otoliths (Tl). Bioaccumulation of metals or As was not detected in muscle. 相似文献
20.
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