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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, 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   

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, 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   

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.
In July 2002, a combination of underway mapping and discrete profiles revealed significant along-shore variability in the concentrations of manganese and iron in the vicinity of Monterey Bay, California. Both metals had lower concentrations in surface waters south of Monterey Bay, where the shelf is about 2.5 km wide, than north of Monterey Bay, where the shelf is about 10 km wide. During non-upwelling conditions over the northern broad shelf, dissolvable iron concentrations measured underway in surface waters reached 3.5 nmol L−1 and dissolved manganese reached 25 nmol L−1. In contrast, during non-upwelling conditions over the southern narrow shelf, dissolvable iron concentrations in surface waters were less than 1 nmol L−1 and dissolved manganese concentrations were less than 5 nmol L−1. A pair of vertical profiles at 1000 m water depth collected during an upwelling event showed dissolved manganese concentrations of 10 decreasing to 2 nmol L−1, and dissolvable iron concentrations of 12–20 nmol L−1 in the upper 100 m in the north, compared to 3.5–2 nmol L−1 Mn and 0.6 nmol L−1 Fe in the upper 100 m in the south, suggesting the effect of shelf width influences the chemistry of waters beyond the shelf.These observations are consistent with current understanding of the mechanism of iron supply to coastal upwelling systems: Iron from shelf sediments, predominantly associated with particles greater than 20 μm, is brought to the surface during upwelling conditions. We hypothesize that manganese oxides are brought to the surface with upwelling and are then reduced to dissolved manganese, perhaps by photoreduction, following a lag after upwelling.Greater phytoplankton biomass, primary productivity, and nutrient drawdown were observed over the broad shelf, consistent with the greater supply of iron. Incubation experiments conducted 20 km offshore in both regions, during a period of wind relaxation, confirm the potential of these sites to become limited by iron. There was no additional growth response when copper, manganese or cobalt was added in addition to iron. The growth response of surface water incubated with bottom sediment (4 nmol L−1 dissolvable Fe) was slightly greater than in control incubations, but less than in the presence of 4 nmol L−1 dissolved iron. This may indicate that dissolvable iron is not as bioavailable as dissolved iron, although the influence of additional inhibitory elements in the sediment cannot be ruled out.  相似文献   

10.
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   

11.
U–Th decay series isotopes, δ18O and Si measurements in the river estuarine waters and sediments of the polluted Hooghly estuary as well as the surface waters of the Bay of Bengal, its high salinity end member, are reported. Dissolved Si indicates that there are probably two mixing regimes, dissolved U behaviour is nonconservative and δ18O behaves conservatively in the overall estuarine region. Isotopes of reactive elements, viz. 234Th and 210Po, are removed from the estuarine waters in <2 days and <1 month, respectively, which is due to high suspended matter (30–301 mg l−1). 228Ra and 226Ra are profusely released into the estuarine waters in the low to mid-salinity regions.As expected, the opposite trend is observed in the case of estuarine sediments and suspended matter. Reactive isotopes of Th, 210Pb and 210Po are enriched, whereas Ra isotopes are depleted with respect to their parent nuclides in the estuarine sediments and suspended matter. 232Th/Al ratio appears well suited to study the distribution and mixing of the bed load sediments of the Ganga–Brahmaputra (G–B) and the Hooghly rivers with those from other rivers on the Bay of Bengal floor.  相似文献   

12.
Nitrification rates, as oxidation of 15N-labelled ammonium and loss of nitrite from N-Serve treated samples, were measured in Kochi backwaters during three seasons. Nitrification rates ranged from undetectable to 166 nmol N L−1 h−1 in the water column and up to 17 nmol N (g wet wt)−1 h−1 in sediments. Nitrification rates were higher in intermediate salinities than in either freshwater or seawater end. Within this salinity range, nitrification rates could be related to ammonium concentrations. As shown by the relation between ammonification and nitrification rates, it is also likely that nitrification is more regulated by renewal rates, rather than by in situ concentrations, of substrate. Among other environmental parameters, temperature and pH may have an influence on nitrification. Potential nitrification rates calculated from loss of nitrite from N-Serve treated, nitrite-enriched samples were about 800 nmol N L−1 h−1 in the water column and 40 nmol N (g wet wt)−1 h−1 in sediments. While these rates are in balance with those of biological ammonium production they may be inadequate to mitigate ammonium pollution in this estuary.  相似文献   

13.
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   

14.
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   

15.
We have elucidated the seasonal and spatial variation in the potential denitrifying activity in estuarine and coastal lagoonal sediments in Lakes Shinji and Nakaumi, Japan. The denitrifying activity increased from summer through autumn and was positively correlated with the temperature of the overlying water at all sites except one, where the bottom was always more reductive than at the other sites and there was no NO3 − as a substrate for denitrification from spring to autumn. Moreover, the relationship between the denitrifying activity and the distance from the sea showed different trends in estuarine and lagoonal sediments. These spatial differences indicate that different factors regulate the denitrification in estuarine and lagoonal sediments. Denitrifying activity in estuarine sediment was regulated by the discharge of freshwater containing NO3 − or organic matter, while in the lagoonal sediments the occurrence of nitrification via the intrusion of oxic seawater into the reductive sediment appears to be a key requirement for the process of denitrification. Therefore, the denitrifying activity in the lagoonal sediment appears to be greater near the sea. Water intrusion is one of the key factors controlling denitrification in coastal marine ecosystems by affecting the supply of substrate available for denitrification.  相似文献   

16.
Water samples from the Tamar Estuary oxidized manganese when supplemented with Mn2+ (2 mgl−1). The rates of oxidation were depressed in the presence of various metabolic inhibitors. The effect of Mn2+ and temperature on the rate of manganese oxidation suggested that a biological process was largely responsible for converting Mn2+ to Mn4+. Rates of manganese oxidation were much higher in freshwater (3·32 μgl−1 h−1 in water containing 30 mgl−1 of suspended matter) than in saline water (0·7 μgl−1 h−1 in water of salinity 32‰) containing the same amount of particulate matter. The rate of manganese oxidation was proportional to the particulate load (up to 100 mgl−1 particulates).  相似文献   

17.
Iron-rich concretions are frequently found around plant roots in Tagus estuary (Portugal) where radial delivery of O2 takes place. Salt marsh sediments exhibit cracks that are an additional feature to introduce O2 and other solutes in the upper sediments. Metal concentrations in salt marsh sediments are clearly above the background levels reflecting the anthropogenic sources from a large city with 2.5 million inhabitants, and several industrial centres. In order to evaluate how both oxidised structures influences the redistribution of redox sensitive elements in salt marsh sediments, concretions were collected from roots of Halimione portucaloides below the oxygenated zone. These tubular cylindrical structures were analysed for Fe, Al, Mn, As, and P along 1-cm radial transect in a millimetre scale from the inner part to the adjacent anoxic sediment. In addition, oxidised cracks were analysed for the same spatial resolution, from the sediment–water interface to anoxic layers (2-cm transept). The parallelism between Fe, As, and P concentrations at this microscale is the most noticeable aspect. Iron and As presented very high concentrations in the 4-mm concretions (3.4 mmol g−1 and 3.1 μmol g−1, respectively) and decreased sharply to the host sediment. Oxygen released from roots oxidise the solid sulphides, and the reduced Fe and As are transported towards the root by both diffusion and pore water flow associated with the root water uptake. Subsequently, Fe(III) precipitates and As is retained by sorption and/or coprecipitation. These elements are also enriched in the first 2-mm of oxidised cracks, but in lower concentrations (50% and 30%, respectively). Manganese concentrations in concretions were low (11.8 μmol g−1), indicating that Fe dominates the sediment chemistry. Phosphorus and iron concentrations in the ascorbate fraction were higher in the oxidising surfaces of concretions (10.7 μmol g−1 and 1.6 mmol g−1, respectively) and of cracks (5.1 μmol g−1 and 0.47 mmol g−1). The parallelism of Fe and As distributions includes not only their similar redox chemistries, but also that to phosphate, including control by coprecipitation of the host iron phases. The mechanisms involved in the mobilisation of As and P are however different, whereas As comes from the oxidation of iron sulphides; dissolved P derives from reduction of ferri-hydroxide phases.  相似文献   

18.
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   

19.
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   

20.
《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   

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