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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  
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.
A one-dimensional, hydrodynamical model of the Tamar Estuary shows good agreement with measured tidal elevations and currents. Computed currents are used to drive a one-dimensional moving-element model of the salt balance. The moving-element model overcomes the numerical difficulties associated with strong tidal advection. Axial distributions of salinity at high water, computed using the moving-element model, compare well with measurements. The modelled and observed high water salinity distributions in this macrotidal estuary show little dependence on tidal range. The major variability in salinity is due to runoff. This strong and rapid dependence on runoff is a consequence of short residence (or flushing) times. Typically, residence times are less than one day throughout the year in the upper 10 km of estuary. The residence times maximize in summer, reaching 14 d for the whole estuary. During high runoff winter periods residence times are less than 5 d. Mixing coefficients for the moving-element salinity model are deduced from salinity measurements. Dispersion coefficients at fixed locations along the estuary are deduced from solutions of the salinity model. The spatially-averaged coefficients at mean spring and neap tides are 180 and 240 m2 s?1, respectively, for average runoff. Therefore, spring-neap variations in dispersion are fairly small and show a negative correlation with tidal range. The spatially-averaged dispersion coefficients at mean tides vary from 150 to 300 m2 s?1 for typical summer and winter runoff, respectively. The increase in dispersion with runoff and the decrease with tidal range implies that buoyancy-driven currents generate an important component of the shear dispersion in this estuary.  相似文献   

3.
From July to October 2004, five sites in the Hampton–Seabrook Estuary in New Hampshire were sampled with beam and otter trawls. The goals were to describe winter flounder (1) abundance in the estuary, (2) size class distributions, (3) spatial distribution by different size classes, and (4) distribution patterns. Of the 19 species caught, winter flounder was the most abundant and was dominated by young-of-the-year (YOY) fish. The five sites were fairly homogenous in depth, bottom type, salinity, and temperature. However, YOY abundance ranged from 2.1 to 32.1 fish 1,000 m?2 depending on the site. Benthic community was the best indicator of juvenile winter flounder abundance. Catch data of other organisms fluctuated, but no one species was a strong predictor of winter flounder abundance and distribution. During late summer and early fall, the estuary is used primarily by YOY winter flounder, indicating that this estuary functions as a nursery ground.  相似文献   

4.
The temporal and spatial distributions of salinity, dissolved oxygen, suspended particulate material (SPM), and dissolved nutrients were determined during 1983 in the Choptank River, an estuarine tributary of Chesapeake Bay. During winter and spring freshets, the middle estuary was strongly stratified with changes in salinity of up to 5‰ occurring over 1 m depth intervals. Periodically, the lower estuary was stratified due to the intrusion of higher salinity water from the main channel of Chesapeake Bay. During summer this intrusion caused minimum oxygen and maximum NH4 + concentrations at the mouth of the Choptank River estuary. Highest concentrations of SPM, particulate carbon (PC), particulate nitrogen (PN), total nitrogen (TN), total phosphorous (TP) and dissolved inorganic nitrogen (DIN) occurred in the upper estuary during the early spring freshet. In contrast, minimum soluble reactive phosphate (SRP) concentrations were highest in the upper estuary in summer when freshwater discharge was low. In spring, PC:PN ratios were >13, indicating a strong influence by allochthonous plant detritus on PC and PN concentrations. However, high concentrations of PC and PN in fall coincided with maximum chlorophyll a concentrations and PC:PN ratios were <8, indicating in situ productivity controlled PC and PN levels. During late spring and summer, DIN concentrations decreased from >100 to <10 μg-at l?1, resulting mainly from the nonconservative behavior of NO3 ?, which dominated the DIN pool. Atomic ratios of both the inorganic and total forms of N and P exceeded 100 in spring, but by summer, ratios decreased to <5 and <15, respectively. The seasonal and spatial changes in both absolute concentrations and ratios of N and P reflect the strong influence of allochthonous inputs on nutrient distributions in spring, followed by the effects of internal processes in summer and fall.  相似文献   

5.
The bioavailability of metals and their potential for environmental pollution depends not simply on total concentrations but on their chemical form. Consequently, knowledge of aqueous metal speciation is essential in investigating potential metal toxicity and mobility. Dissolved (<1 kDa), colloidal (1 kDa–0.45 μm) and particulate (>0.45 μm) size fractions of sulfate, organic C (OC) and 18 metals/metalloids were investigated in the extremely acidic Vörå River system in Western Finland, which is strongly affected by acid sulfate (AS) soils. In addition, geochemical modelling was used to predict the formation of free ions and complexes in these acidic waters. The most important finding of this study is that the very large amounts of elements known to be released from AS soils (including Al, Ca, Cd, Co, Cu, Mg, Mn, Na, Ni, Si and U) occur and can prevail mainly in toxic forms throughout acidic river systems; as free ions and/or sulfate-complexes. This has serious effects on the biota and particularly dissolved Al can be expected to have acute effects on fish and other organisms. In the study area, only the relatively forested upstream area (higher pH and contents of OC) had significant amounts of a few bioavailable elements (including Al, Cu, Ni and U) due to complexation with the more abundantly occurring colloidal OC in the upstream area. It is, however, notable that some of the colloidal/particulate metals were most likely associated with metal bearing phyllosilicates eroded from clay soils. Moreover, the mobilisation of Fe and As was small and As was predicted to be associated with Fe oxides, indicating a considerable influence of Fe oxides on the mobilisation/immobilisation processes of As. Elements will ultimately be precipitated in the recipient estuary, where the acidic metal-rich river water will gradually be diluted/neutralised with brackish seawater in the Gulf of Bothnia. According to speciation modelling, such a pH rise may first cause precipitation of Al, Cu and U together with organic matters closest to the river mouth, in line with previous sediment studies from the estuary.  相似文献   

6.
Concentrations of rare earth elements (REE) and yttrium (Y), and major metals (Al, Fe and Mn) were measured in suspended particulate matter (SPM) and bottom sediments of the Kali estuary, western India, for their distribution and fractionation. The contents of SPM and metals in it were more uniform along the longitudinal transect during the monsoon. During the post- and pre-monsoons, low SPM in the upper/middle estuary coincided with high Fe and Mn and total REE (∑REE). But in the lower estuary SPM and its ∑REE content increased seaward, while Fe and Mn decreased. The Y/Ho ratios decreased seaward during the monsoon but increased during the post-monsoon. Sm/Nd ratios were more uniform along the transect during monsoon but decreased marginally seaward in other seasons. The Post-Archean Average Australian Shale (PAAS)-normalized REE patterns exhibited middle REE and heavy REE enrichment with positive Ce (\({\text{Ce}}/{\text{Ce}}^{*}\)), Eu (\({\text{Eu}}/{\text{Eu}}^{*}\)) and Y anomalies. The \({\text{Ce}}/{\text{Ce}}^{*}\) increased but \({\text{Eu}}/{\text{Eu}}^{*}\) decreased marginally seaward. The fine-grained sediments showed higher ∑REE and lower Y/Ho ratios than in coarse-grained sediments. The PAAS-normalized REE patterns of sediment were similar to that of SPM. The results revealed two processes, colloidal flocculation and coagulation of metals in the low-salinity zone and an estuarine turbidity maximum in the high salinity zone. Rare earths and yttrium (REY) in SPM and sediments primarily reflected the source rock composition than that of chemical weathering. Apart from physico-chemical processes, the mineralogy and grain size of sediments controlled the distribution and fractionation of REY in the estuary.  相似文献   

7.
To evaluate biogeochemical characteristics, eco-environmental risks and sources of trace elements (TEs: As, Hg, Se, Sb, Te, Sn, Bi and Ge), their total concentrations and chemical speciation in surface sediments collected from the Changjiang Estuary were determined. Total concentrations for As, Hg, Se, Sb, Te, Sn, Bi and Ge were 4.57–30.20, 0.01–0.40, 0.04–0.38, 0.36–1.48, 0.02–0.10, 0.48–6.58, 0.13–0.64 and 0.83–2.43 μg/g, respectively, with higher values at the estuary. This distribution pattern was attributed to the riverine input and high clay and total organic carbon contents. The sequential extraction suggested that TEs mainly occurred in residual fractions. The risk assessment code suggested that As, Hg and Sn were at low risk, whereas Bi, Se, Sb, Te and Ge were at medium risk. The geoaccumulation index (I geo) and principal component analysis indicated that Se and Sn mainly came from the natural input (crustal and biological inputs), whereas As, Sb, Hg, Bi and Te came from both of the crustal and anthropogenic inputs via atmosphere and rivers. In addition, Ge possibly came from the natural (crustal and biological inputs) and anthropogenic inputs.  相似文献   

8.
The behaviour of dissolved Al in the Great Ouse estuary, in particular with respect to salinity, is complex. There is, however, evidence from field data as well as laboratory mixing experiments to suggest that flocculation and sorption mechanisms play important roles affecting the concentrations of dissolved Al during the early stages of estuarine mixing. In contrast, a near-buffering of dissolved Al occurs in the entire stretch of the estuary (salinity >0.2) with concentrations varying around 1.4 μg l−1. This distribution and lack of variation with salinity is attributable to sorption processes which might dominate over other processes in these turbid estuarine waters (suspended particulate load 48–888 mg l−1) impacting dissolved Al levels. Sorption models have been developed for both dissolved and leachable particulate Al concentrations in these waters. These observations provide compelling evidence of sorption processes that might be important in the geochemistry of Al in estuarine waters.  相似文献   

9.
The colloidal distribution and size fractionation of organic carbon and trace elements were studied in a seasonally stratified, organic-rich boreal lake, Lake Maselga, located in the European subarctic zone (NW Russia, Arkhangelsk region). This study took place over the course of 5?years in winter (glacial) and summer periods and during the spring and autumn overturn. A newly developed in situ dialysis technique (1, 10, and 50?kDa) and traditional frontal filtration and ultrafiltration (20, 10, 5, 0.22, and 0.025???m) were used to assess element concentrations at different depths. No significant changes in element concentrations occurred during filtration through sub-colloidal pore-size membranes (20?C0.22???m), suggesting a negligible amount of particulate Fe, OC, and associated trace metals. Large colloids (0.025?C0.22???m) were found to be the main carriers of poorly soluble elements (Fe, Al, Ti, Zr, REEs, Th, and U) during the summer and winter stratification. There was also a clear change in the vertical pattern of the percentage of colloidal Al, Ti, V, Cr, Fe, and Ni during different seasons, and the greatest proportion of colloidal forms was observed during the spring and autumn overturn. This pattern is most likely linked to the dominance of soil (allochthonous) organic carbon, which complexes with trace metals during these periods. During the summer seasons, autochthonous production of small exometabolites or photodegradation increases the concentration of the low-molecular weight fractions (<1?kDa) that dominate the speciation of divalent heavy metals in surface horizons. The colloidal status of As (30?C60%), which was documented in different seasons along the full depth of the water column, is most likely linked to the presence of organic complexes. The overall results of this study suggest that changes in the colloidal speciation of trace elements with depth in different seasons depend on changes in the redox conditions, the input of soil OM, the biodegradation of plankton biomass releasing dissolved organic matter in the bottom horizons, and in upward diffusion from the sediments.  相似文献   

10.
Four Chinese estuaries, the Jiaojiang, Luanhe, Shuangtaizihe, and Yalujiang were investigated to determine Al geochemistry and inter-relations between Al and nutrients. These estuaries are characterised by low particulate organic carbon and high turbidity, with various tidal regimes. Dissolved Al was determined by fluorescence method after liquid–liquid extraction into n-hexanol. Concentrations of Al in the Luanhe estuary are relatively high (1.5–2.0 μM) and approximately uniform over the salinity range sampled, suggesting the influence of in situ sources/processes. In the Shuangtaizihe estuary, riverine concentrations of Al (1.8–2.2 μM) decrease with higher chlorinity, indicating the predominance of simple dilution by seawater. The Jiaojiang and Yalujiang provide evidence that Al is removed from water column at early stages of estuarine mixing, owing to probably the particle–solution reactions (e.g. flocculation) in the estuary. The Al data are further compared with total suspended matter and nutrients in these estuaries. The data sets indicate that aluminum is not dominantly coupled to the cycle of nutrients.  相似文献   

11.
Florida Bay is a shallow carbonate estuary in South Florida. It receives fresh waters from the Everglades that contribute a number of metals to the Bay. The Bay is the largest estuary in Florida with nearly pristine conditions. In this paper we report the first extensive studies of trace metals in the Bay. The seasonal distributions of trace metals (Sc, V, Cr, Co, Cu, Fe, Pb, Mn, Ni and Al) were determined on surface waters in Florida Bay and adjacent waters. The measurements in the Bay were made from May 2000 to May 2001, and the adjacent waters were sampled in September 2000 and May 2002. Most of the dissolved trace metals exhibited their maximum concentrations in summer, except Al and Pb that did not show any seasonal variability. The seasonal variations of the metals are related to the influx of fresh water from rainfall. The lowest concentrations are found during the dry season in the winter and the highest during the wet season in the summer. Several metals (V, Mn, Al, Sc, Fe, Co, Ni and Cr) exhibited their highest concentrations in the western zone of the Bay. These waters from agricultural areas are influenced by Gulf of Mexico waters, which carry metals coming from Barron, Broad and Shark rivers into the Bay. The Shark River always exhibited high concentrations of V, Mn, Al, Sc, Co and Cr. Other possible influences in the western and north-central zone of the Bay are from Flamingo Center, the creeks of Taylor Slough and the mangrove fringe of the Everglades. High concentrations of Al, Co, Ni, Cr, Cu, Fe, and Pb were detected in the eastern zone. The high values found in the northeast are influenced by Taylor Slough runoff and in the southeast by Key Largo, Tavernier Marina and the drainage from the main highway (US1) on Tavernier Key. The minimum concentrations for most of the metals were found in areas near the Key channels that exchange waters between Florida Bay and the Atlantic Ocean (Gulf Stream). The adjacent waters in the Atlantic side including the Gulf Stream waters showed very low concentrations for all the metals studied except for V. In the Bay correlations of V were found: (1) V with salinity and Al and (2) Sc with Si. Most of the other metals did not show any strong correlations with nutrients or salinity. Florida Bay is thus not a typical estuary due to the unique structure of its mud banks and multiple inputs of metals from the mangrove fringe in the north.  相似文献   

12.
The natural isotopic composition of suspended particulate organic nitrogen was determined in the Southern Bight of the North Sea and in the Scheldt estuary. These data show that δ15N constitutes a convenient tracer of the origin of the suspended matter.In the winter, in the absence of intensive primary production, the suspended organic matter of the Scheldt estuary is a mixture of two components: a continental detrital component characterized by a low δ value of 1.5%. and a marine component with a mean δ value of 8%..During the phytoplankton flowering period, lasting from early May to October, intensive primary production occurs throughout the estuary giving rise to a third source of organic matter. This material is characterized by high δ values reflecting the isotopic composition of ammonia, the nitrogenous nutrient assimilated by phytoplankton in the estuary.The nitrification process occuring in the mixing area of the Scheldt estuary leads to higher downstream δ values of ammonia (>20%.) which permits the distinction between estuarine from fresh-water phytoplankton. Simple isotopic budget calculations show that, both in the upstream part and in the downstream part, autochthonous phytoplanktonic material contributes a major part of the total suspended matter in the Scheldt estuary during summer.  相似文献   

13.
Fourteen siderophile and other non-lithophile elements determined in 31 Semarkona (LL3.0) chondrules by neutron activation analysis are severely fractionated relative to lithophile elements. Their chondrule/whole-rock abundance ratios vary by factors of up to 1000; the mean ratio is ~0.2. Non-refractory siderophile abundance patterns in Ni-rich chondrules are smooth functions of volatility and in Ni-poor chondrules patterns are more irregular. Refractory siderophile elements are often fractionated from Ni; they covary, confirming the presence of a refractory metal component. The chalcophile element Se correlates with Br and siderophile elements. Zinc is uniformly low and uncorrelated with other elements.Most metal and sulfide in chondrules was probably present in the solar nebula before chondrule formation; most siderophile and chalcophile elements were in these materials. Some Fe was also in silicates, as were minor amounts of Ni, Co, Au, Ge and possibly Se. The amount of metal formed by reduction during chondrule melting was minor. The common metal component in chondrules is similar to, and may be the same as the common component involved in the metal/silicate fractionation of the ordinary chondrite groups.Chondrules are depleted in metal chiefly because they sampled metal-poor precursor assemblages. Metal segregation during the molten period and subsequent loss was a minor process that may be responsible for most surface craters on chondrules.  相似文献   

14.
Concentrations of total and dissolved elements were determined in 35 water samples collected from rivers in Sardinia, a Mediterranean island in Italy. The overall composition did not change for waters sampled in both winter and summer (i.e., January at high-flow condition and June at low-flow condition), but the salinity and concentrations of the major ions increased in summer. Concentrations of elements such as Li, B, Mn, Rb, Sr, Mo, Ba and U were higher in summer with only small differences between total and dissolved (i.e., in the fraction <0.4 μm) concentrations. The fact that these elements are mostly dissolved during low flow periods appears to be related to the intensity of water–rock interaction processes that are enhanced when the contribution of rainwater to the rivers is low, that is during low-flow conditions. In contrast, the concentrations of Al and Fe were higher in winter during high flow with total concentrations significantly higher than dissolved concentrations, indicating that the total amount depends on the amount of suspended matter. In waters filtered through 0.015 μm pore-size filters, the concentrations of Al and Fe were much lower than in waters filtered through 0.4 μm pore-size filters, indicating that the dissolved fraction comprises very fine particles or colloids. Also, Co, Ni, Cu, Zn, Cd and Pb were generally higher in waters collected during the high-flow condition, with much lower concentrations in 0.015 μm pore-size filtered waters; this suggests aqueous transport via adsorption onto very fine particles. The rare earth elements (REE) and Th dissolved in the river waters display a wide range in concentrations (∑REE: 0.1–23 μg/L; Th: <0.005–0.58 μg/L). Higher REE and Th concentrations occurred at high flow. The positive correlation between ∑REE and Fe suggests that the REE are associated with very fine particles (>0.015 and <0.4 μm); the abundance of these particles in the river controls the partitioning of REE between solution and solid phases.Twenty percent of the water samples had dissolved Pb and total Hg concentrations that exceeded the Italian guidelines for drinking water (>10 μg/L Pb and >1 μg/L Hg). The highest concentrations of these heavy metals were observed at high-flow conditions and they were likely due to the weathering of mine wastes and to uncontrolled urban wastes discharged into the rivers.  相似文献   

15.
This paper examines the issues related to salinization and water quality in the complex drainage system of the historical land reclamation of Lamone basin (Ravenna coastal plain, northern Italy), with the aim of guiding ongoing agricultural-related decisions. Major and trace element concentration and O–H–B–Sr isotope-ratios were measured on surface water from a network of canals and ditches. Sampling was carried out during the winter period and in summer, to assess the effects of agricultural water management on the aquatic system. Results show widespread salinization of waters over the entire crop, due to both the direct saltwater inland flushing through the canals in proximity of the mouths, and sea salt leaching from soils. During winter, salinization is partly mitigated by rainfalls, while in summer dilution processes are due to freshwater input from outside the watershed, planned to assist the agricultural water demand. In the winter season, the concentration of some elements such as Fe, Mn, Al, and Cu in waters exceeds the maximum permissible limits imposed by the Italian regulations, while during summer the concentration of these elements is significantly reduced. A seasonal cycling is established, where the bottom sediments of canals and ditches act as sinks of harmful elements, mostly through adsorption by Fe–Mn–Al oxy-hydroxide solid phases. The irrigation practice, although improving the water quality, increases water turbidity by re-mobilization of sediments which act as transport agents of contaminants, with detrimental effects that may become significant over the years.  相似文献   

16.
Gulf sturgeon,Acipenser oxyrinchus desotoi, forage extensively in the Suwannee River estuary following emigration out of the Suwannee River, Florida. While in the estuary, juvenile Gulf sturgeon primarily feed on benthic infauna. In June–July 2002 and February–April 2003, random sites within the estuary were sampled for benthic macrofauna (2002 n = 156; 2003 n = 103). A mean abundance of 2,562 ind m−2 (SE ± 204) was found in the summer, with significantly reduced macrofaunal abundance in the winter (mean density of 1,044 ind m−2, SE ± 117). Benthic biomass was significantly higher in the summer with an average summer sample dry weight of 5.92 g m−2 (SE ± 0.82) compared to 3.91 g m−2 (SE ± 0.67) in the winter. Amphipods and polychaetes were the dominant taxa collected during both sampling periods. Three different estimates of food availability were examined taking into account principal food item information and biomass estimates. All three estimates provided a slightly different view of potential resources but were consistent in indicating that food resource values for juvenile Gulf sturgeon are spatially heterogeneous within the Suwannee River estuary.  相似文献   

17.
Palaemon longirostris was sampled monthly at 12 sites in the Mira River estuary (southwest Portugal) from October 1990 to September 1991. Animals were counted, measured, and sexed. The estuarine distribution of prawns appeared to follow the salinity displacement, the animals being found at river stations during summer and autumn when saline encroachment up the estuary was greater. During winter and spring when freshwater input from the river was greatest, and thus moving the salinity gradient toward the mouth, the prawns migrated downstream to brackish areas. Ovigerous females were collected only from estuarine areas (January to August), suggesting that reproduction does not take place in freshwater habitats. Higher percentages of females than males were generally observed. Females, particularly ovigerous ones, were larger than males.  相似文献   

18.
Monthly growth of the fouling community at eight test panel sites in the Loxahatchee River Estuary was related to salinity and temperature. Growth was lowest in January 1981 (averaging 23 g per m2, dry weight), and increased during spring and early summer with increasing water temperature. Maximum growth occurred during early or midsummer at upstream locations, before river or canal discharge substantially reduced salinity, and in late summer at downstream locations. Growth was greatest at salinities slightly less than that of seawater and decreased at salinities less than about 10‰. Growth was suppressed throughout the estuary in August 1981, probably because of the sudden decrease in temperature and salinity, and perhaps the increase in physical scouring, caused by runoff from Tropical Storm Dennis. Large loads of nutrients transported to the estuary from storm runoff, however, may have subsequently stimulated growth, which increased in September 1981 to the maximum for the year (averaging 683 g per m2, dry weight).  相似文献   

19.
During weathering, elements enriched in black shale are dispersed in the environment by aqueous and mechanical transport. Here a unique evaluation of the differential release, transport, and fate of Fe and 15 trace elements during progressive weathering of the Devonian New Albany Shale in Kentucky is presented. Results of chemical analyses along a weathering profile (unweathered through progressively weathered shale to soil) describe the chemically distinct pathways of the trace elements and the rate that elements are transferred into the broader, local environment. Trace elements enriched in the unweathered shale are in massive or framboidal pyrite, minor sphalerite, CuS and NiS phases, organic matter and clay minerals. These phases are subject to varying degrees and rates of alteration along the profile. Cadmium, Co, Mn, Ni, and Zn are removed from weathered shale during sulfide-mineral oxidation and transported primarily in aqueous solution. The aqueous fluxes for these trace elements range from 0.1 g/ha/a (Cd) to 44 g/ha/a (Mn). When hydrologic and climatic conditions are favorable, solutions seep to surface exposures, evaporate, and form Fe-sulfate efflorescent salts rich in these elements. Elements that remain dissolved in the low pH (<4) streams and groundwater draining New Albany Shale watersheds become fixed by reactions that increase pH. Neutralization of the weathering solution in local streams results in elements being adsorbed and precipitated onto sediment surfaces, resulting in trace element anomalies.Other elements are strongly adsorbed or structurally bound to solid phases during weathering. Copper and U initially are concentrated in weathering solutions, but become fixed to modern plant litter in soil formed on New Albany Shale. Molybdenum, Pb, Sb, and Se are released from sulfide minerals and organic matter by oxidation and accumulate in Fe-oxyhydroxide clay coatings that concentrate in surface soil during illuviation. Chromium, Ti, and V are strongly correlated with clay abundance and considered to be in the structure of illitic clay. Illite undergoes minimal alteration during weathering and is concentrated during illuvial processes. Arsenic concentration increases across the weathering profile and is associated with the succession of secondary Fe(III) minerals that form with progressive weathering. Detrital fluxes of particle-bound trace elements range from 0.1 g/ha/a (Sb) to 8 g/ha/a (Mo). Although many of the elements are concentrated in the stream sediments, changes in pH and redox conditions along the sediment transport path could facilitate their release for aqueous transport.  相似文献   

20.
Elemental size distributions, from truly dissolved through colloidal to particulate, have been studied in a subarctic boreal river. The measurements, carried out during 2002, ranged from winter to summer conditions, including an intense spring flood event. Results are reported for a total of 42 elements. Size distributions were characterised using a combination of cross-flow (ultra)filtration (CFF), flow field-flow fractionation (FlFFF), and diffusive gradients in thin-films (DGT). The three techniques showed similar trends, but quantitative comparisons reveal some important differences that warrant further investigation.Previous work has identified two colloidal carrier phases in fresh waters, dominated by iron and carbon, respectively. The majority of the elements studied are associated with one or both of these colloidal carrier phases. The exceptions are the alkali metals and several anions that are only very weakly associated with colloidal material, and which therefore occur mainly as truly dissolved material (<1 kDa in molecular weight). We discuss the likely origin for the two colloidal carrier phases and consider how associated trace elements fit into the geochemical framework. The relative affinities of the elements for iron and carbon colloidal carrier phases are related to their chemistries, and are compared with earlier data from the Delsjö Creek in southern Sweden.Elemental colloidal concentrations show strong seasonal variations related to changes in the colloidal carrier phase(s) with which they associate. In particular, many elements show a strong spring maximum in colloidal concentrations associated with the strong maximum in colloidal carbon concentration during the spring flood.  相似文献   

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