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1.
From the distribution of dissolved and solid arsenic species in a contaminated estuarine sediment and measured rates of flux of the various arsenic species we propose an empirical model for the cycling of arsenic between sediments and water column. The chemical form of arsenic in the sediment was largely determined by the redox state of the sediment. Arsenite was the dominant dissolved and solid species in the deeper reduced sediment, and arsenate was dominant in the oxidized surface layer. Arsenite in the interstitial water diffused toward the surface layer, where it was mostly oxidized to arsenate prior to leaving the sediments. Some arsenate adsorbed to the surface sediments and produced a surface layer enriched in arsenic. Small concentrations of methyl and dimethyl arsenic were produced in the sediments, and these also diffused into the overlying water.Nereis succinea, a burrowing polychaete, affected distribution and flux of arsenic from the sediments by its production of irrigated burrows. These burrows increased both the effective surface area of the sediment and the diffusion of arsenic by a factor of five. When the relative effects of the activities of Nereis succinea and physical resuspension are compared, results indicate that although physical resuspension can produce large pulses of materials from contaminated sediments, continuous biological activity is likely to be more important in the mobilization of contaminants from sediments in many estuarine environments.  相似文献   

2.
黄、东海海域溶解无解机砷分布特征与化学形态   总被引：2，自引：1，他引：1  
Distribution and chemical speciation of dissolved inorganic arsenic were examined in Yellow Sea and East China Sea. Results demonstrated that: (1) both As(III) and As(V) were detected, with As(V) domin...  相似文献   

3.
In this study, 36 fish species were collected from three coastal cities in Korea to investigate levels and patterns of six arsenicals (arsenite: As (III), arsenate: As (V), arsenocholine: AsC, arsenobetaine: AsB, monomethylarsonic acid: MMA, and dimethylarsinic acid: DMA). The levels of ∑6 As in the different fish species varied substantially, ranging from 0.02 μg As/g ww (Islaeli carp) to 9.65 μg As/g ww (Skate ray) with a median of 0.40 μg As/g ww. All the arsenicals in marine fishes showed higher levels than those in freshwater fishes due to fish feed living in saline water. Overall, marine carnivorous fishes seem to be more contaminated with arsenic. For all the fish samples, AsB (mean fraction: 90.6%) was dominant among the six arsenicals, indicating biomethylation of inorganic arsenic and accumulation of AsB. Fish species with high water contents showed elevated levels of As (III), but there was no further significant correlations between arsenicals and water/lipid contents. Concentrations of As (V) were significantly lower than those of As (III), which implies that As (V) is reduced during biomethylation of inorganic arsenic. Consequently, we hypothesize that the toxicity of arsenic (mainly derived from As (III)) can be increased by the reduction of As (V), especially for the fish species with higher water contents.  相似文献   

4.
Measurements of total dissolved arsenic (As(III+V)) and antimony (Sb(III+V) and their simple methylated species are presented for samples collected from three vertical profiles and along three surface transects in the Chatham Rise region, east of New Zealand. As(III+V) concentrations showed a slight increase with depth (16–17 nM at 25 m to 20 nM at 100 m) whereas Sb(III+V) concentrations were conservative with depth (1.02–1.12 nM). Along the three surface water transects, As(III+V) and Sb(III+V) concentrations showed little variation, with average concentrations of 18±2 and 0.99±0.05 nM, respectively. Inorganic arsenic was not correlated with orthophosphate (r2=0.01). Monomethyl- and dimethyl-arsenic (MMAs, DMAs) concentrations (0.04–0.01 and 0.65–0.07 nM, respectively) decreased with depth, suggesting surface water production by biota and degradation at depth. Along the Chatham Rise transect, DMAs concentrations increased on the Rise (0.65 nM maximum) compared to waters north and south of the Rise (∼0.22 nM). Fluctuation in MMAs concentrations were also seen for water samples collected on the Chatham Rise. Monomethyl-, dimethyl- and trimethyl-antimony (MMSb, DMSb, TMSb) species were detected in water samples collected along all the three surface water transects suggesting surface water production by biota. Concentrations of MMSb, DMSb and TMSb in water samples were fairly constant along all the three surface transects (0.06–0.07, 0.015–0.025 and 0.005–0.015 nM, respectively), showing no significant enrichment on the Chatham Rise. These arsenic and antimony results support the current global view that inorganic As and Sb are conservative and the methyl species are of biological origin.  相似文献   

5.
In this study, organic carbon (OC), total nitrogen (TN), stable carbon isotopic (δ13COC) and CuO reaction product compositions were used to identify the sources of organic matter (OM) and to quantify the relative importance of allochthonous and autochthonous contributions to the western Adriatic Sea, Italy. Suspended particulate material (195 samples) and surficial sediments (0–1 cm, 70 samples) from shallow cross-shelf transects were collected in February and May 2003, respectively. Vertical water column profiles were acquired along the same transects. Data include depth, potential temperature, salinity, density and chlorophyll fluorimetry.Along the western Adriatic shelf in the near-shore region, the phytoplankton growth was influenced by dynamics of the buoyant plumes from the Po and Appennine rivers. A small amount of very fine terrigenous material remained suspended within the coastal current and was exported southward along the shelf to the slope. High variability in the bulk composition was detected in the Po prodelta surficial sediments, whereas the western Adriatic shelf, although a larger area, exhibited a narrower range of values.A significant decoupling was observed between suspended particles in the water column and surficial deposits. The organic material collected in the water column was compositionally heterogeneous, with contributions from marine phytoplankton, riverine–estuarine phytoplankton and soil-derived OM. Frequent physical reworking of surficial sediments likely leads to the efficient oxidation of marine OC, resulting in the observed accumulation and preservation of refractory soil-derived OC delivered by the Po and Appennine rivers.  相似文献   

6.
Total arsenic, arsenate and arsenite concentration profiles for the water column of Saanich Inlet, an intermittently anoxic fjord located on Vancouver Island, B.C., Canada, were measured using independent analytical techniques for total arsenic and arsenic speciation to evaluate the accuracy of the speciation technique in both oxic and anoxic marine environments. Total arsenic profiles indicate a mid-depth minimum of about 1.0 ppb above the oxic—anoxic interface and an enrichment in the anoxic zone to about 2.0 ppb. This minimum may be due to either advection of arsenic-poor water into Saanich Inlet at mid-depth or arsenic incorporation onto solid phases within a bacteria- and manganese-rich particulate layer located immediately above the oxic—anoxic interface and subsequent removal via sinking particulate material. Ratios of total arsenic to phosphorus in the deep, anoxic waters of the basin are similar to those reported for marine algae, suggesting that the enrichment of total arsenic within the anoxic bottom layer may be due to its release upon organic matter decomposition.Arsenate and arsenite concentration versus depth profiles indicate a rapid (but incomplete in a thermodynamic sense) response to the oxic—anoxic interface. The arsenate/ arsenite concentration ratio is 15/1 in the oxic region of the water column and 1/12 in the anoxic zone. Arsenate—arsenite interconversion occurs at a depth shallower than ferric-ferrous but deeper than MnO2 —Mn2+ interconversions.Measurements of arsenite oxidation rates at near-ambient arsenite concentrations and temperatures using an 74As3+ radioactive tracer technique indicate that arsenite oxidation is initially ten times faster in seawater taken from the manganese-rich particulate layer at 165 m depth than in seawater collected near the surface at 50 m depth. Addition of antibiotics to seawater from 165 m depth initially suppressed the rate of arsenite oxidation, indicating that it may be partially microbially mediated.  相似文献   

7.
沉积物中氧化还原敏感元素（Redox Sensitive Element,RSE）含量变化是上覆水体氧化还原环境良好的替代指标。本文通过冲绳海槽中南部两个柱状沉积物（深度:30 cm）粒度、总有机碳、总氮及其同位素含量和氧化还原敏感元素含量等指标,探究复杂环境背景下冲绳海槽柱状沉积物中RSE的赋存机理与环境指示意义。研究发现,柱状沉积物中除了Cr亏损,其他RSE均显示有不同程度的富集。“粒控效应”对冲绳海槽柱状沉积物的RSE含量影响较小;分析可知,海水表层生产力是影响沉积物氧化还原环境的主要因素,通过Mn（氢）氧化物的吸附或解吸附作用实现RSE的富集与亏损。δCe、V/Cr、Ni/Co和V/（V+Ni）等指标指示沉积物整体处于氧化?弱氧化环境。沉积物中Mn元素通过还原作用以Mn2+形式向上扩散,在25～30 cm处被含氧间隙水氧化富集形成锰峰,指示柱状沉积物0～25 cm处为氧化环境,25～30 cm处为弱氧化环境。  相似文献   

8.
Chemical extraction techniques show that the majority of the arsenic in North Atlantic deep-sea sediments is associated with an iron phase compositionally similar to that found in deep-sea ferromanganese nodules (As/Fe ～ 11 · 10?4) and is probably of seawater origin. Some sediments also contain As associated with Fe oxides produced by continental weathering. A minority (～8%) of the arsenic is of detrital origin but is not associated with Fe or Mn oxides; it has a content (1.7 ppm) similar to the average crustal abundance. In the Eastern Mediterranean Sea, near-shore sediments contain As associated with land-derived Fe oxides (As/Fe ～ 2 · 10?4), but As/Fe ratios increase to ～ 13 · 10?4 in deep-sea sediments as the contribution of seawater derived arsenic becomes dominant. Arsenic is enriched in metalliferous sediments (As/Fe ～ 20?50 · 10?4) but As/P ratios of metalliferous sediments, deep-sea ferromanganese nodules and deep-ocean water are all similar. Although a hydrothermal contribution cannot be discounted, it is likely that the arsenic is also of seawater origin, suggesting that hydrothermal iron oxyhydroxides remove As more efficiently from seawater than do iron phases (goethite) in deep-sea sediments and nodules. Arsenic accumulates in deep-sea sediments (～ 6 μg cm?2 10?3 yr?1) at sediments (～ 120 μg cm?2 10?3 yr?1) at rate sufficient to balance river input input (～3 · 1010 g yr?1). These estimates give an oceanic residence time for arsenic of 1–2 · 105 yr.  相似文献   

9.
河口砷(As)的地球化学行为的研究是近几年才开始的。Waslenchuk和Windon在研究美国东南部一些河口砷的行为时,认为砷在河口的行为是保守的。Howard在调查英格兰南部的Beaulieu河口砷的行为时,发现有转移的迹象。黄河口及其近岸海域溶解砷的调查目的是想了解砷在黄河口的行为及其分布特征。  相似文献   

10.
The concentrations of arsenic species in continental-shelf waters of the southeastern U.S. are controlled mainly by simple physical mixing of shelf waters and Gulf Stream intrusions. The biota mediate redox reactions which result in a disequilibrium of arsenic species; up to 20% of the total arsenic (averaging 1.1 μg/l) occurs as unstable arsenite [As (III)] and dimethylarsenic, the remainder consists of thermodynamically favored arsenate [As (V)]. Uptake of arsenic by the biota has a minor effect on arsenic distribution in offshore waters, producing a deep-water arsenate maximum, and minima for arsenite and dimethylarsenic. Riverine and atmospheric arsenic inputs to the shelf waters are relatively insignificant. Southeastern rivers contain only about 0.3 μg/l dissolved arsenic, and the atmosphere adjacent to continental shelf waters contains about 1.7 ng/m3 of As (V), exclusively associated with the particulate fraction.  相似文献   

11.
With the rising cost of oil the electric power generating companies are turning to coal as a fuel source. Large amounts of fly ash are produced as a by product of coal combustion. This fly ash must then be disposed of, with the oceans being considered an alternative to land fill disposal. This research investigated the sorptive behavior of the surface-associated arsenic and utilized the results to project arsenic's impact on the water column during the ocean disposal of fly ash.Several acid digests were investigated to determine an effective method of arsenic recovery from fly ash. Of these, the HCl digest was the most effective technique, yielding 100% arsenic recoveries from fly-ash particles. The arsenic content of the fly ashes studied varied from 69 ± 11 μg g−1 to 323 ± 24 μg g−1, reflecting differences in the arsenic content of the source coal. In both seawater and freshwater there is an increase in arsenic desorption with increasing pH. The greatest release of arsenic occurred at pH 12 with generally over 80% of the surface arsenic released.Fly ash in contact with seawater and freshwater can exhibit either acidic or alkaline tendencies depending upon the soluble elemental composition on the surface of the flyash particle. The acidic ashes were shown to leach a greater percentage of arsenic (16.9%) than the more alkaline ashes (8.2%). During these leaching studies in seawater, arsenic was found to leach in both the pentavalent and trivalent oxidation state. The pentavalent state was predominant, comprising 77% of the arsenic initially desorbed.The dissolution in seawater of arsenic was utilized to assess the possible impact of the ocean disposal of fly ash. Based upon these data it appears that the natural levels of arsenic in the water column would not be significantly increased. Further research is needed on the fate of fly-ash particles in marine sediments.  相似文献   

12.
The chemical forms and distribution of dissolved arsenic species in the estuary of the River Beaulieu (Hampshire, U.K.) are reported. ‘Inorganic arsenic (V)’ in both the marine and riverine estuary inputs are in true solution, passing through ultrafiltration membranes having a nominal molecular weight cut-off of 500 daltons. Extensive removal of dissolved ‘inorganic arsenic (V)’ is apparent from the distribution of arsenic in the estuary, with laboratory mixing experiments indicating that removal is favoured in the low salinity region. ‘Inorganic arsenic (III)’ and methylated arsenic species account for up to 41% and 70% of the dissolved arsenic, respectively, but are only found during the warmer months when water temperatures exceed ca. 12°C.  相似文献   

13.
Replicate portions of a Delaware salt marsh were enclosed in cylindrical microcosms and exposed to elevated levels of inorganic arsenic (arsenate). All biotic and abiotic components in dosed cylinders rapidly incorporated arsenic. Spartina blades showed the greatest arsenic enrichment, with dosed plants incorporating arsenic concentrations an order of magnitude higher than controls. Spartina detritus and sediments also exhibited greatly elevated arsenic concentrations. Virtually all of the arsenic was incorporated into plant tissue or strongly sorbed to cell surfaces. Thus, elevated arsenic concentrations in estuarine waters will be reflected in living and non-living components of a salt marsh ecosystem, implying that increased arsenic will be available to organisms within the marsh ecosystem.  相似文献   

14.
Surface sediments along the Rimouski section in the St. Lawrence estuary were sampled at the surface and at 10 cm depth. Fatty acids were extracted and analysed. Saturated and unsaturated fatty acid contents at the two depths vary with the nature of the sediments. The clay sediments rich in organic matter contain more fatty acids than the corresponding sand or gravel. Unsaturated fatty acids were more abundant in the surface sediments. Some iso- and anteiso-odd carbon fatty acids were detected in the sediments; these acids could indicate a microbial activity. Correlation is made with the fatty acid contents of the water column together with the surface microlayer of the estuarine water.  相似文献   

15.
《Marine Geology》1999,153(1-4):77-89
The sediments of the eastern Mediterranean basin contain Corg-enriched layers (sapropels) interbedded with the Corg-poor sediments which form by far the greater part of the record. While it is generally appreciated that different surface ocean productivity and bottom water conditions are necessary for the formation and preservation of these two sediment types, less attention has been paid to diagenetic effects which are an expected consequence of transitions between dramatically different bottom water oxygenation levels. A geochemical interpretation has emerged of post-depositional oxidation of the most recent sapropel (S1), initially based on the relationship of the Mn, Fe, Corg and S concentration/depth profiles observed around S1, and the characteristic shapes of these elemental profiles known from other situations. This indicates that post-depositional oxidation has removed approximately half of the visual evidence of the sapropel (∼6 cm from a total of ∼12 cm in the deep basin). The oxidation interpretation from redox-sensitive element redistribution profiles has subsequently been consolidated with evidence from pore water (O2, NO−3, Mn2+ and Fe2+) studies, from characteristic solid phase Ba profiles which yield palaeoproductivity records, and from oxidation-sensitive indicator trace elements (I and Se). So far, these geochemical observations have been concentrated in the deeper central parts of the basin, where sediment accumulation rates are lower than on the basin margins, and radiocarbon dating indicates that S1 formation occurred between 5.3 and 9.0 ky (uncorrected conventional radiocarbon time). It remains to be demonstrated whether or not these times are applicable to the entire E. Mediterranean basin. The implications of these findings to guide sampling in future work on the S1 productivity episode and on older sapropels for palaeoenvironmental investigations are discussed.  相似文献   

16.
Both water and suspended particulate matter in the deep water of the Gulf of St. Lawrence are greatly enriched in manganese. Maximum dissolved manganese concentrations are encountered close to the sediment-water interface whereas the particulate matter with highest manganese content occurs 30–100 m above the bottom. The elevated concentrations are attributed to the diagenetic release of dissolved manganese from the underlying fine-grained sediments and its subsequent precipitation in the water column. The rate of manganese precipitation is rapid compared to the rates of diffusion and mixing in the bottom water. Part of the manganese-enriched particulate matter becomes mixed throughout the water column by advection and diffusion. Thus, particles enriched in manganese can ultimately be carried into the open ocean by prevailing currents. This process, which appears to be widespread in eastern Canadian coastal waters, enables manganese originally associated with rapidly settling terrigenous particles to be transferred to slowly settling fine-grained suspended particles entering the ocean from coastal environments. In this way, riverborne manganese of terrigenous origin may well account for a major proportion of the excess manganese in pelagic sediments.  相似文献   

17.
Summer porewater and spring and summer surficial sediment samples were collected from 26 locations in the intertidal region of the Fraser River estuary. Porewaters were analysed for dissolved iron and manganese (as defined by species <0·2μm in diameter) to assess the contribution of diagenesis to concentrations of iron and manganese oxides at the sediment–water interface. Surficial sediment samples were geochemically characterized as: % organic matter (% LOI); reducible iron (RED Fe, iron oxides) and easily reducible manganese (ER Mn, manganese oxides). Grain size at each site was also determined. The sediment geochemical matrix, as defined by the above four parameters, was highly heterogeneous throughout the intertidal region (three-way ANOVA;P<0·0001). For RED Fe and ER Mn, this heterogeneity could be explained by either diagenetic processes (RED Fe) or by a combination of the proximity of the sample sites to the mouth of the Fraser River estuary plus diagenetic processes (ER Mn). Correlation (Spearman Rank Correlation Test (rs), of dissolved iron within the subsurface sediments with amounts of RED Fe recovered from the associated surface sediments was highly significant (rs=0·80, P<0·0001); high concentrations of RED Fe at the sediment–water interface co-occurred with high concentrations of dissolved iron, regardless of the proximity of the sample locations to riverine input. Compared with iron, the relationship between dissolved manganese and ER Mn from surface sediments was lower (rs=0·58;P<0·0008). Locations most strongly influenced by the Fraser River contained greater concentrations of ER Mn at the sediment–water interface than that which would be expected based on the contribution from diagenesis alone. Sediment grain size and organic matter were also influenced by the proximity to riverine input. Surficial sediment of sites close to the river mouth were comprised primarily of percent silt (2·0μm–50μm) whereas sites not influenced by riverine input were primarily percent sand (grain size >50μm). Concentrations of organic matter declined from the mouth to the foreslope of the estuary. With the exception of RED Fe, temporal variation (May vs July) was insignificant (P>0·05, three-way ANOVA). Concentrations of RED Fe recovered from the surficial sediments were in general greater in the summer vs spring months, although spring and summer values were highly correlated (Pearson Product Moment Correlation Coefficient; PPCC; R=0·89;P<0·0001). As the bioavailability of metals is dependent on sediment geochemistry, availability throughout the intertidal region will also be spatially dependent. This heterogeneity needs to be taken into account in studies addressing the impact of metals on estuarine systems.  相似文献   

18.
The presence of a strongly developed oxygen minimum zone (OMZ; [O2]<2 μM) in the northeastern Arabian Sea affords the opportunity to investigate whether oxygen deficiency in bottom waters enhances the preservation of organic matter in the underlying sediments. We explored if the observed patterns of organic matter accumulation could be explained by differences in productivity, sedimentation rate, water depth, and mineral texture. The differences in the burial rates of organic matter in sediments deposited within or below the OMZ could not be explained on the basis of these factors. All collected evidence points to a coupling of low oxygen concentrations and enhanced organic matter preservation. Under more oxygenated conditions bioturbation as well as the presence of labile manganese and iron oxides are probably important factors for a more efficient microbially mediated degradation of organic matter. Pore water profiles of dissolved Mn2+ and Fe2+ show that reduction of manganese and iron oxides plays a minor role in sediments lying within the OMZ and a larger role in sediments lying below the OMZ.  相似文献   

19.
A sulfur budget for the Black Sea anoxic zone   总被引：1，自引：0，他引：1  
A budget for the sulfur cycle in the Black Sea is proposed which incorporates specific biogeochemical process rates. The average sulfide production in the water column is estimated to be 30–50 Tg yr−1, occurring essentially in the layer between 500 and 2000 m. About 3.2–5.2 Tg sulfide yr−1 form during sulfate reduction in surface sediments of the anoxic zone. Total sulfur burial in anoxic sediments of 1 Tg yr−1 consists of 10–70% (ca. 40–50% is the average) water column formed (syngenetic) component, the rest being diagenetic pyrite. As a maximum, between 3 and 5 Tg yr−1 contribute sulfide to the bottom water or diffuse downward in the sediment. About 20–50 Tg yr−1 sulfide is oxidized mostly at the chemocline and about 10–20% of this amount (4.4–9.2 Tg yr−1) below the chemocline by the oxygen of the Lower Bosphorus Current. A model simulating the vertical distribution of sulfide in the Black Sea water column shows net consumption in the upper layers down to ca. 500 m, essentially due to oxidation at the chemocline, and net production down to the bottom. On the basis of the calculated budget anoxic conditions in the Black Sea are sustained by the balance between sulfide production in the anoxic water column and oxidation at the chemocline. On average the residence time of sulfide in the anoxic zone is about 90–150 yr, comparable to the water exchange time between oxic and anoxic zones. Hydrophysical control on the sulfur cycle appears to be the main factor regulating the extent of anoxic conditions in the Black Sea water column, rather than rates of biogeochemical processes.  相似文献   

20.
Dissolved and total dissolvable manganese concentrations have been measured at four stations in the western North Atlantic Ocean. Total dissolvable manganese concentrations are high in surface waters, decrease to uniformly low levels throughout the bulk of the water column, and increase in the bottom nepheloid layer. Dissolved Mn (Mnd) concentrations follow the total dissolvable concentrations throughout the surface and deep waters but do not increase in the near-bottom waters.Deep water concentrations of Mnd decrease from 30 ng l?1 in the Newfoundland Basin to 20 ng l?1 in the Sargasso Sea. This change and other features of the deep water distribution of dissolved manganese could be associated with the slow oxidation of Mn2+ to MnO2. There is also evidence at one station of scavenging of manganese from the dissolved phase in the near-bottom layer which may again be related to the kinetics of manganese oxidation.  相似文献   

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