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1.
Understanding the biogeochemical process of Hg is critical in the overall evaluation of the ecological impacts resulting from the reuse of Hg-contaminated dredged sediment. Sediment banks (V1 and V2) were constructed with freshly dredged sediments from a navigational channel in Venice Lagoon, Italy, with the goal of clarifying potential differences in the biogeochemistry of Hg between the reused dredged sediments and those from surrounding sites (SS1 and S2). Toward this purpose, Hg and monomethylmercury (MMHg) concentrations, and Hg methylation rates (MMRs) in the surface 2.5 cm sediments were monitored, along with ammonium, iron, sulfate and sulfide concentrations in the pore waters of banks and surrounding sites from November 2005 to February 2007. Pore water analyses indicate that the bank sediments are characterized by lower levels of sulfate and iron, and by higher levels of ammonium and sulfide compared to the surrounding sediments. With respect to Hg speciation, the fractions of MMHg in total Hg (%MMHg/Hg) and the MMRs were significantly lower in the bank V1 compared to those in the reference site SS1, whereas the %MMHg/Hg and the MMRs were similar between V2 and S2. A negative correlation is found between the logarithm of the particle-water partition coefficient of Hg and the MMR, indicating that the reduced MMRs in V1 are caused by the limited concentrations of dissolved Hg. Organic matter appears to play a key role in the control of MMR via the control of Hg solubility.  相似文献   

2.
以富营养化的胶州湾一个柱状沉积物为例,用细化的铁形态分析及量化的铁氧化物还原活性相结合的方法研究了沉积物中铁的成岩作用过程。结果表明,这两种方法相结合的结果能更详细示踪铁的转化并能从多视角提供铁成岩作用的细微差别。这一方法有望应用于其它研究中更好地揭示复杂的铁和硫的生物地球化学循环。铁微生物还原在上部沉积物铁的还原中起重要作用,但12 cm深度以下铁被硫化物的化学还原为主要过程。最具生物活性的无定形铁氧化物是铁微生物还原的主要参与者,然后依次为弱晶态铁氧化物和磁铁矿,晶态铁氧化物几乎不参与铁的成岩循环。沉积物上部铁微生物还原的重要作用主要是活性铁含量高而活性有机质含量低共同作用的结果,且后者也是沉积物中硫酸盐还原速率以及硫化物积累的最终制约因素。对比研究表明,通过还原性溶解动力学方法表征的微生物可还原的铁氧化物主要由无定形和弱晶态铁氧化物组成,其总体活性常数相当于老化的水铁矿,且随深度增加而减低。  相似文献   

3.
Mercury concentration and speciation were measured in surface and deep ocean waters of the South and equatorial Atlantic. In the surface waters, total Hg was 2.9±1.7 pM on average, with a significant fraction present as reactive Hg (1.7±1.2 pM). The reactive Hg fraction consisted of elemental Hg (Hg°) as the dominant species (1.2±0.8 pM). Measurements in surface waters also showed that Hg partitioned to the “colloidal” phase (0.33±0.28 pM) and was associated with particulate matter (0.1±0.05 pM). No dimethylmercury (DMHg;<0.01 pM) or monomethylmercury (MMHg; <0.05 pM) was detected in mixed layer samples. The highest DMHg concentrations were found in recently formed deep waters – Antarctic Intermediate Water and Antarctic Bottom Water and in the equatorial sub-thermocline region. Higher concentrations of DMHg coincided with higher values of apparent oxygen utilization, indicative of a link between microbial activity and methylated Hg production. The lowest-deep water DMHg concentrations were found in the core of the North Atlantic Deep Water. Incubation experiments on-board demonstrated that light enhanced the decomposition of DMHg, with MMHg as the major product. In deep waters, Hg° was still an important constituent and is likely formed as a decomposition product from MMHg. These results suggest that methylated Hg production occurs primarily in regions of high biological activity, and that ionic Hg is strongly complexed to organic matter (colloidal material) in open ocean surface waters.  相似文献   

4.
A sediment disk reactor was tested in once flow-through mode to retrieve kinetic parameters for the Monod rate law that describes sulfate reduction. The experimental method was compared with a previously described procedure by the authors where a sediment plug-flow reactor was operated in a recirculation mode. In recirculation mode, accumulation of metabolic byproducts in certain cases may result in negative feedback, thus preventing accurate determination of kinetic information. The method described in this article provides an alternative to the recirculation sediment plug-flow-through reactor technique for retrieving kinetic parameters of microbially mediated reactions in aquatic sediments.For sulfate reduction in a saltmarsh site, a maximum estimate of the half-saturation concentration, Ks, of 204±26 μM and a maximum reaction rate, Rm, of 2846±129 nmol cm(wetsediment)3 d−1 was determined. The Ks value obtained was consistent with the one estimated previously (Ks=240±20 μM) from a different site within the same saltmarsh mud flat using a recirculating reactor. From the Rm value and reduction rates determined using 35SO42− incubation experiments, we infer that sulfate reduction is limited in the field. Substrate availability is not the main contributor for the limitation, however. Competition from other microbes, such as iron reducers affects the activity of sulfate reducers in the suboxic to anoxic zones, whereas aerobes compete in the oxic zone. High sulfide concentration in the pore water may also have acted as a toxin to the sulfate reducers in the field.  相似文献   

5.
This work describes a laboratory experiment designed to unravel mercury species reactivity in superficial coastal sediments oscillating between oxic and anoxic conditions. The experimental set-up has been applied to a sediment slurry from the Arcachon Bay (France) to follow the evolution of both naturally occurring (i.e. endogenous) and isotopically enriched added mercury species (i.e. exogenous, 1??IHg and 2?1MMHg) at environmental levels. The transformation and partition between the different phases (aqueous, solid and gaseous) of the endogenous and exogenous mercury species (inorganic Hg (IHg), monomethyl Hg (MMHg), elemental Hg (Hg?) and dimethyl Hg (DMHg)) have been investigated by isotopic speciation methods throughout the experiment. The results demonstrate that the experimental approach is able to promote sediment redox oscillations and to simultaneously follow the biogeochemical fate of naturally occurring or added mercury species. Experimentally driven redox transition events were found to significantly enhance the aqueous Hg species concentrations, while the MMHg burden is not greatly affected. Indeed, during the anoxic-oxic transition, while aqueous endogenous IHg and MMHg exhibited a two-fold increase, aqueous exogenous IHg and MMHg increased 7 and 4 times, respectively. Transient increases of the net IHg methylation were recorded during the redox transitions with the largest increase of the MMHg contents (factor 1.8) observed during the oxic-anoxic transition. High resolution in situ redox experiments have not been performed up to now, therefore the developed experimental set-up provides novel insights in both the influence of redox conditions on Hg methylation/demethylation and adsorption/desorption processes and kinetics in superficial sediments.  相似文献   

6.
Dissolved Fe and ligand concentrations and the Fe-binding strength of the organic ligands were measured in samples from the upper water column (150 m) of the oligotrophic waters of the Canary Basin (eastern North Atlantic Ocean). Concentrations of major nutrients, phytoplankton abundance and photosynthetic characteristics were also measured in the same samples.The concentrations of dissolved Fe and dissolved organic ligands were low with mean values of 0.31 ± 0.18 nM Fe and 1.79 ± 0.73 nEq of M Fe(n = 47), respectively. The conditional binding constant varied between 1019.8–1022.7 (n = 47). The largest variation with depth in the ligand concentrations (between 4.78 and 1.1 nEq of M Fe) was observed in the upper layer, above the Deep Chlorophyll Maximum (DCM located between 80 and 100 m), with high surface values in stations at 18 and 34.At the DCM where Fe was depleted, the ligand concentrations were still relatively high showing the same trend with depth as the amount of phytoplankton cells. Here 62% of the vertical variation in ligand concentrations can be explained by parameters describing phytoplankton cell abundance or biomass and orthosilicic acid concentration, which could reflect diatom growth. Ligand concentrations below the maximum of the DCM (n = 4) showed good linear positive relationships with the total phytoplankton biomass as well as with 2 out of 4 distinguished groups of phytoplankton (Synechococcus and pico-eukaryote I).In the maximum of the DCM and below this maximum the phytoplankton origin of the dissolved organic ligands of Fe is very probable. Data suggest a release of ligands by cell lysis and not by an active production. However, the origin in the surface layer is more difficult to explain. Although the amount of phytoplankton cells in the surface layer is reduced, it is still  25% of the cell concentration observed in the DCM. High concentrations of organic ligands could then be a remnant of past blooms or present production under nutrient depleted conditions. Input of Sahara dust can be another source of ligands.  相似文献   

7.
The influence of bioturbation on certain aspects of the biogeochemistry of sulfur and iron was examined in shallow-water sediments of Great Bay Estuary, New Hampshire. A bioturbated (JEL) and non-bioturbated (SQUAM) site were compared. Annual sulfate reduction measured with 35S, was 4·5 times more rapid at JEL. A significant portion of this difference was attributed to rapid rates which occurred throughout the upper 12 cm of sediment at JEL due to infaunal reworking activities. Sulfate reduction decreased rapidly with depth at SQUAM. FeS in the upper 2 cm at JEL increased in concentration from 3 to 45 μmol ml−1 from early May to late July while only increasing from 3 to 8 μmol ml−1 at SQUAM. Infaunal irrigation and reworking activities caused rapid and continous subsurface cycling of iron and sulfur at JEL. This maintained dissolved iron concentrations at 160–170 μM throughout the summer despite rapid sulfide production. Therefore, dissolved sulfide never accumulated in JEL pore waters. Although dissolved organic carbon (DOC) was generated during sulfate reduction, bioturbation during summer caused a net removal of DOC from JEL pore waters. Sulfate reduction rates, decomposition stoichiometry and nutrient concentrations were used to calculate turnover times of nutrients in pore waters. Nutrient turnover varied temporally and increased three-to five-fold during bioturbation. A secondary maximum in the abundance of recoverable sulfate-reducing bacteria occurred at 10 cm in JEL sediments only during periods of active bioturbation, demonstrating the influence of macrofaunal activities on bacterial distributions.  相似文献   

8.
In this study we test the hypothesized negative relationship between seagrass status and porewater hydrogen sulfide (H2S) levels, through a comparative analysis within a range of seven Posidonia oceanica meadows growing over carbonate sediments in the NW Mediterranean Sea around Mallorca Island. The studied meadows range from meadows growing on sediments with very low sulfide porewater concentrations (4.6 μM) to those growing over higher sulfide conditions (33.5 μM). Organic matter content, sulfate reduction rates and sulfide porewater concentrations in the sediments were determined concurrently with the assessment of demographic plant dynamics (specific mortality and net population growth rates). Sulfide porewater concentration increased with increasing organic matter content in the sediment, while net population growth decreased significantly with low increases of sulfide concentrations. Our results confirm the previously suspected vulnerability of seagrass meadows growing on carbonate sediments to increased sulfide levels. An excess of 10 μmols H2S L−1 porewater is identified to already conduce P. oceanica meadows to decline, which this study identifies, particularly, as strongly sensitive to sulfides. The results reported here suggest that even moderate increases in organic carbon inputs may lead to enhancement of dissolved sulfides and may be an important factor for seagrass status in these iron-depleted carbonate sediments from the Mediterranean Sea.  相似文献   

9.
Discovery Bay, a carbonate-dominated embayment in north Jamaica, has been subject to inputs for 40 years of iron-rich bauxite sediment associated with the local mining and transport of processed bauxite. As such, this site is an ideal natural laboratory to study the records and impacts of iron oxide inputs upon geochemical, diagenetic, and microbial processes in tropical carbonate sediments.Total Fe contents in sites in the bay not receiving bauxite inputs are negligible and porewater Ca2+, SO42− and Cl− indicate that bacterial sulphate reduction is an important process. In contrast, surface sediments receiving bauxite inputs contain significant total Fe, from 44 μmol/g in shallow (5 m water depth) sites to 110 μmol/g in deeper (20 m water depth) sites. Up-core increases in total Fe record increased temporal inputs into the bay. Within these Fe-rich sediments porewater data shows the presence of FeII released by bacterial FeIII reduction. There is no direct evidence for significant bacterial sulphate reduction in these sediments. Iron oxides within all bauxite-impacted sediments display a high potential reducibility, from 40% to 80% of the total Fe present as dithionite-extractable FeIII. Experimental analysis of the potential susceptibility to, and rates of, bacterial FeIII reduction, utilising Discovery Bay sediment and Shewanella putrefaciens CN32 (a known FeIII-reducer) has confirmed the high bacterial reducibility of iron oxides within the sediment. Up to 75% of initial dithionite-extractable FeIII in the sediments was reduced over 15 days.The presence of iron oxides within the Discovery Bay shallow marine carbonate systems has markedly altered the chemical diagenetic processes taking place, with a shift from apparent dominance of bacterial sulphate reduction at non-impacted (Fe-poor) sites, to highly significant bacterial FeIII reduction in Fe-rich bauxite-impacted sediments. Given the perceived global increases in terrigenoclastic sediment inputs into tropical carbonate systems as a result of land-use and climate changes, coupled with the documented role that iron oxide reduction plays in nutrient and contaminant cycling in sediment systems, more research into the perturbation of early diagenesis by iron oxide inputs is required.  相似文献   

10.
Methylmercury (MeHg) concentration and production rates were studied in bottom sediments along the mainstem of Chesapeake Bay and on the adjoining continental shelf and slope. Our objectives were to 1) observe spatial and temporal changes in total mercury (HgT) and MeHg concentrations in the mid-Atlantic coastal region, 2) investigate biogeochemical factors that affect MeHg production, and 3) examine the potential of these sediments as sources of MeHg to coastal and open waters. Estuarine, shelf and slope sediments contained on average 0.5 to 1.5% Hg as MeHg (% MeHg), which increased significantly with salinity across our study site, with weak seasonal trends. Methylation rate constants (kmeth), estimated using enriched stable mercury isotope spikes to intact cores, showed a similar, but weaker, salinity trend, but strong seasonality, and was highly correlated with % MeHg. Together, these patterns suggest that some fraction of MeHg is preserved thru seasons, as found by others [Orihel, D.M., Paterson, M.J., Blanchfield, P.J., Bodaly, R.A., Gilmour, C.C., Hintelmann, H., 2008. Temporal changes in the distribution, methylation, and bioaccumulation of newly deposited mercury in an aquatic ecosystem. Environmental Pollution 154, 77] Similar to other ecosystems, methylation was most favored in sediment depth horizons where sulfate was available, but sulfide concentrations were low (between 0.1 and 10 μM). MeHg production was maximal at the sediment surface in the organic sediments of the upper and mid Bay where oxygen penetration was small, but was found at increasingly deeper depths, and across a wider vertical range, as salinity increased, where oxygen penetration was deeper. Vertical trends in MeHg production mirrored the deeper, vertically expanded redox boundary layers in these offshore sediments. The organic content of the sediments had a strong impact on the sediment:water partitioning of Hg, and therefore, on methylation rates. However, the HgT distribution coefficient (KD) normalized to organic matter varied by more than an order of magnitude across the study area, suggesting an important role of organic matter quality in Hg sequestration. We hypothesize that the lower sulfur content organic matter of shelf and slope sediments has a lower binding capacity for Hg resulting in higher MeHg production, relative to sediments in the estuary. Substantially higher MeHg concentrations in pore water relative to the water column indicate all sites are sources of MeHg to the water column throughout the seasons studied. Calculated diffusional fluxes for MeHg averaged  1 pmol m− 2 day− 1. It is likely that the total MeHg flux in sediments of the lower Bay and continental margin are significantly higher than their estimated diffusive fluxes due to enhanced MeHg mobilization by biological and/or physical processes. Our flux estimates across the full salinity gradient of Chesapeake Bay and its adjacent slope and shelf strongly suggest that the flux from coastal sediments is of the same order as other sources and contributes substantially to the coastal MeHg budget.  相似文献   

11.
We have investigated the chemical forms, reactivities and transformation kinetics of Fe(III) species present in coastal water with ion exchange and filtration methods. To simulate coastal water system, a mixture of ferric iron and fulvic acid was added to filtered seawater and incubated for a minute to a week. At each incubation time, the seawater sample was acidified with hydrochloric acid and then applied to anion exchange resin (AER) to separate negatively charged species (such as fulvic acid, its complexes with iron and iron oxyhydroxide coated with fulvic acid) from positively charged inorganic ferric iron (Fe(III)′). By monitoring the acid-induced Fe(III)′ over an hour, it was found that iron complexed by fulvic acid dissociated rapidly to a large extent (86–92% at pH 2), whereas amorphous ferric oxyhydroxide particles associated with fulvic acid (AFO-L) dissociated very slowly with the first-order dissociation rate constants ranging from 6.1 × 10− 5 for pH 3 to 2.7 × 10− 4 s− 1 for pH 2. Therefore, a brief acidification followed by the AER treatment (acidification/AER method) was likely to be able to determine fulvic acid complexes and thus differentiate the complexes from the AFO-L particles (the dissolution of AFO-L was insignificant during the brief acidification). The acidification/AER method coupled with a simple filtration technique suggested that the iron–fulvic acid complexes exist in both the < 0.02 μm and 0.02–0.45 μm size fractions in our coastal water system. The truly dissolved iron (< 0.02 μm) was relatively long-lived with a life-time of 14 days, probably due to the complexation by strong ligands. Such an acid-labile iron may be an important source of bioavailable iron in coastal environments, as a significant relationship between the chemical lability and bioavailability of iron has been well recognised.  相似文献   

12.
This paper reports the initial results of a study of groundwater and coastal waters of southern Brazil adjacent to a 240 km barrier spit separating the Patos Lagoon, the largest coastal lagoon in South America, from the South Atlantic Ocean. The objective of this research is to assess the chemical alteration of freshwater and freshwater–seawater mixtures advecting through coastal permeable sands, and the influence of the submarine discharge of these fluids (SGD) on the chemistry of coastal waters. Here we focus on dissolved iron in this system and use radium isotopic tracers to quantify SGD and cross-shelf fluxes. Iron concentrations in groundwaters vary between 0.6 and 180 μM. The influence of the submarine discharge of these fluids into the surf zone produces dissolved Fe concentrations as high as several micromolar in coastal surface waters. The offshore gradient of dissolved Fe, coupled with results for Ra isotopes, is used to quantify the SGD flux of dissolved Fe from this coastline. We estimate the SGD flux to be 2 × 106 mol day− 1 and the cross-shelf flux to be 3.2 × 105 mol day− 1. This latter flux is equal to about 10% of the soluble atmospheric Fe flux to the entire South Atlantic Ocean. We speculate on the importance of this previously unrecognized iron input to regional ocean production and on the potential significance of this source to understanding variations in glacial–interglacial ocean production.  相似文献   

13.
《Marine Chemistry》2001,75(3):229-248
Dissolved and particulate mercury and methylmercury concentrations were determined in the Southern Bight of the North Sea and the Scheldt estuary in the period 1991–1999. Mercury and methylmercury concentrations are higher before 1995 than after 1995, especially in the fluvial part.The North Sea: In the offshore stations, dissolved Hg concentrations are generally higher in winter than in summer while the reverse is true for particulate Hg KD values (KD=the concentration of particulate Hg (HgP in pmol kg−1) divided by the concentration of dissolved Hg (HgD in pmol l−1)) range from 100,000 to 1000,000 l kg−1. Dissolved methylmercury concentrations vary from 0.05 to 0.25 pmol l−1 in summer and from d.l. to 0.23 pmol l−1 in winter and particulate methylmercury concentrations from 1.8 to 36 pmol g−1 in summer and from 0.9 to 21 pmol g−1 in winter. The KD ranges from 9,000 to 219,000 l kg−1.The Scheldt estuary: In winter, dissolved Hg concentrations are elevated in the upper estuary, decrease exponentially in the low salinity range followed by a very slow decrease towards the mouth. In summer, they are low in the fluvial part, increase in the low salinity range or in the mid-estuary and sometimes show an increase in the lower estuary. Particulate Hg concentrations do not show any seasonal trend.Dissolved MMHg concentrations are much lower in winter, when maximum concentrations are found in the upper estuary, than in summer. In summer, the MMHg concentrations are low at low salinity, they show a first increase in the salinity range from 3 to 12, a decrease in the mid-estuary and a second increase in the lower estuary.The highest particulate MMHg concentrations are found in the upper estuary, while in the lower estuary generally lower and more constant values are observed. The ratio of dissolved MMHg to dissolved Hg (cruise averages between 1.3% and 20%), is higher than the ratio of particulate MMHg to particulate Hg (cruise averages of 0.27–0.90%). The KD values for MMHg are lower in the summer (30,000–65,000) than in autumn and winter (77,000–114,000).The Scheldt river: In the fluvial part of the Scheldt, dissolved increases in the most upstream stations, while particulate Hg shows no particular pattern. Dissolved MMHg ranges from 0.1 to 0.39 pmol l−1 and particulate MMHg from 3.1 to 43.5 pmol g−1. The MMHg concentrations are comparable to those found in the estuary and no seasonal variations could be observed.  相似文献   

14.
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   

15.
Jingfeng Wu   《Marine Chemistry》2007,103(3-4):370-381
A low-blank pre-concentration procedure is described for the analysis of picomolar iron (Fe) in seawater by isotope dilution high-resolution inductively coupled plasma mass-spectrometry (HR-ICPMS). The procedure uses a two-step Mg(OH)2 co-precipitation procedure to extract Fe from a 50 ml seawater sample into a 100 μl 4% nitric acid (HNO3) solution followed by HR-ICPMS measurement. The high pre-concentration ratio ( 500:1) achieved by the procedure minimizes the Fe blank due to ICPMS instrumental Fe background and results in a detection limit of  2 pM and a precision of  4% at the 50 pM Fe level. The measurement of a low-Fe seawater sample spiked with gravimetric Fe standard shows that the method can clearly distinguish 0.01 nM Fe from 0.02 nM Fe in seawater with high accuracy. The method is demonstrated by the analysis of dissolved Fe in the equatorial Pacific Ocean.  相似文献   

16.
The accretionary wedge of offshore southwestern Taiwan contains abundant deposits of gas hydrate beneath the sea floor. High concentrations of methane in pore waters are observed at several locations with little data concerning historical methane venting available. To understand temporal variation of methane venting in sediments over geologic time, a 23-m-long Calypso piston core (MD05-2911) was collected on the flank of the Yung-An Ridge. Pore water sulfate, dissolved sulfide, dissolved iron, methane, sedimentary pyrite, acid volatile sulfide, reactive iron, organic carbon and nitrogen as well as carbonate δ13C were analyzed.Three zones with markedly different pyrite concentration were found at the study site. Unit I sediments (>20 mbsf) were characterized with a high amount of pyrite (251–380 μmol/g) and a δ13C-depleted carbonate, Unit II sediments (15–20 mbsf) with a low pyrite (15–43 μmol/g) and a high content of iron oxide mineral and Unit III sediments (<10 mbsf) by a present-day sulfate–methane interface (SMI) at 5 m with a high amount of pyrite (84–221 μmol/g) and a high concentration of dissolved sulfide.The oscillation records of pyrite concentrations are controlled by temporal variations of methane flux. With an abundant supply of methane to Unit I and III, anaerobic methane oxidation and associated sulfate reduction favor diagenetic conditions conducive for significant pyrite formation. No AOM signal was found in Unit II, characterized by typical organically-limited normal marine sediments with little pyrite formation. The AOM induced pyrite formation near the SMI generates a marked pyrite signature, rendering such formation of pyrite as a useful proxy in identifying methane flux oscillation in a methane flux fluctuate environment.  相似文献   

17.
Natural iron fertilization processes are occurring around the Crozet Islands (46°26′S–52°18′E), thus relieving the water masses from the normally encountered High Nutrients Low Chlorophyll (HNLC) conditions of the Southern Ocean. During austral summers 2004/2005 and 2005/2006, iron and aluminium concentrations were investigated in large particles (> 53 µm) collected from just below the mixed layer at stations under the influence of island inputs, and also in adjacent HNLC waters. These large particles are anticipated to sink out of the mixed layer, and to reflect the net effects of input and cycling of these elements in the overlying mixed layer. Labile and refractory fractions were determined by a two-stage leaching technique. Data showed that water masses downstream of the islands were enriched in total iron and aluminium (0.25–2.68 nmol L− 1 and 0.34–3.28 nmol L− 1 respectively), relative to the southern HNLC control sites (0.15–0.29 nmol L− 1 for Fe and 0.12–0.29 nmol L− 1 for Al), with only a small fraction (typically < 1%) being acid leachable in both environments. Particulate iron predominantly derived from the island system represents a significant fraction of the total water column iron inventory and may complement dissolved Fe inputs that help support the high summer productivity around the Crozet islands.  相似文献   

18.
The distribution of dissolved (D) and acid-dissolvable (AD) Fe, Ni, Cu and Pb in the upper water column (0–300 m depth) was determined in the Australian sector of the Southern Ocean (140°E meridian) during three cruises conducted between November 2001 and March 2002. For Ni and Cu, there was no significant difference in concentration between dissolved and acid-dissolvable species. DNi and DCu showed significant (P = 0.01) positive correlations with silicate, phosphate and nitrate, reflecting their strong nutrient-type behaviour. For Fe and Pb, the acid-dissolvable concentration mostly exceeded the dissolved concentration, reflecting the importance of labile particulate species for these elements. DPb decreased between January and February in the Polar Frontal Zone and in Antarctic continental shelf water. ADPb maxima occurred in the Antarctic Zone, resulting in a maximum AD/D ratio of 7. The mean DFe concentration in the surface mixed layer was 0.3 nM in the sub-Antarctic zone, 0.4 nM in the Polar Frontal Zone, 0.5 nM in the Antarctic Zone and increased southward beyond the Antarctic Divergence and towards the continent. DFe did not show a clear temporal change in its horizontal distribution, which was in contrast to the other nutrients and trace metals. ADFe substantially increased in Antarctic continental shelf water where the AD/D ratio reached 11. The following conclusions can be drawn from these data. (1) Ni and Cu exist exclusively as dissolved species and their distributions are mainly controlled by their biogeochemical cycling, similar to those of the major nutrients. (2) Pb is dominated by particulate species. The distribution of DPb is temporally and spatially variable due to a sporadic source and strong scavenging. (3) DFe is rather a minor fraction of total Fe in Antarctic continental shelf water where shelf sediments and Antarctic sea-ice appear to be strong sources for Fe. There is substantial temporal variation in the supply of Fe to the upper water column. DFe in the mixed layer of the open Southern Ocean is maintained at low concentrations throughout summer due to uptake by phytoplankton and scavenging.  相似文献   

19.
Community metabolism and nutrient, iron (Fe) and manganese (Mn) cycling were examined in two intertidal, marine, microbial mat communities during short (4–5 days) incubations in closed, flow-through microcosms. Sediment microcosms were incubated under either light (light–dark cycles) or dark (continuous darkness) conditions to assess the effect(s) of photosynthetic oxygen production and microalgal activity on nutrient, Fe and Mn cycling. The effects of chemical redox reactions between reduced sulphur (S), Fe and Mn cycling were examined by blocking sulphate reduction, and reduced S production, with 25 mM molybdate while incubating under dark conditions.In light-incubated microcosms, negligible fluxes of nutrients (nitrogen and phosphorus) and trace metals were observed. A substantial sediment–water flux of reduced Fe (Fe2+) and Mn (Mn2+) was observed in microcosms incubated under continuous darkness; highest fluxes were observed in molybdate-amended microcosms. At both sites, biologically-mediated redox reactions accounted for a substantial (>50%) portion of the Fe2+and Mn2+flux. Both microbial mat communities exhibited similar rates of gross photosynthetic oxygen (O2) production, but dramatically different rates of net benthic O2flux. Distinct patterns of net O2production and trace metal cycling arose from differences in either trace metal oxide availability or reactivity (mineralogy), organic carbon mineralization rates, or sediment characteristics (porosity). Variations in the microbial community responsible for trace metal cycling could have also contributed to the pattern. The present data illustrate that chemically-mediated redox reactions between metal oxides and reduced S complicate interpretation of Fe and Mn fluxes, underscoring the need to separate chemical and biological reactions when attempting to determine the role of biological trace metal reduction in organic carbon oxidation.  相似文献   

20.
The bioaccessibility of metals (Al, Ca, Fe, Mn, Ag, Cd, Co, Cu, Ni, Pb, Sn, Zn) in oxic estuarine sediments has been evaluated using solutions of a commercially available protein (bovine serum albumin; BSA) that mimic the chemical conditions encountered in the gut environment of many deposit-feeding organisms. Over a 20 h incubation period with 5 g L− 1 BSA, metal mobilisation was generally biphasic in that a relatively short period of rapid release was succeeded by more gradual release or approach to equilibrium, although in some cases metal readsorption was evident during the time-courses. Availability to BSA, defined as metal released after 20 h relative to metal extracted by boiling aqua regia, was greatest for Cd, Ni, Ca and Zn and lowest for Fe and Mn, and correlated well with, but was an order of magnitude lower than, metal digested by acidified hydrogen peroxide. Time-courses conducted in the absence of the protein revealed that significant quantities of Ca and Mn were water-soluble, reflecting the partial dissolution of carbonates and hydrous Mn oxides, respectively. Additional experiments indicated a net increase in metal release with increasing BSA concentration and, with the exception of Ca and Mn, a substantial increase in metal mobilisation after sediment organic matter had been digested by peroxidation. These observations suggest that, apart from Ca and Mn, metal release proceeds via complexation with component amino acids of the protein, denudation of organic host phases, and exposure of inorganic, metal-bearing minerals. Accordingly, the bioaccessibility of a metal is predicted to be dependent on its (i) affinity for proteinaceous ligands, (ii) association with components of digestible sediment organic matter, and (iii) degree of binding at relatively weak sites on sediment phases that are exposed or modified by the action of proteins and other chemical constituents of the gut environment.  相似文献   

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