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1.
《Applied Geochemistry》1999,14(3):395-407
An ultrafiltration procedure has been developed to study the interaction between organic C and Hg species in natural waters, and a pilot study was conducted in the surface waters of the Florida Everglades. Compared to total Hg, CH3Hg shows different distribution patterns in the suspended particulate, colloidal, and truly dissolved phases. Colloidal forms (0.22 μm, 3 kDa) contain the majority of the total dissolved Hg, while the amount found in the truly dissolved fraction (<3 kDa) is small (about 10%). However, CH3Hg, which shows strong binding capability with low molecular-weight dissolved organic C, is present almost entirely in the lower molecular-weight fraction of the colloids and in the truly dissolved fraction. Quantitative CH3Hg data correlate well with those for dissolved organic C, an indication that the organic matter present in the system plays an important role in the fate and transport of organomercury. Distribution coefficients between water and the different-sized fractions of the dissolved organic C were determined for both total Hg and CH3Hg. Results for total Hg were in general agreement with other reports resulting from studies of molecular size distributions of total Hg in freshwater systems. This is, to the best of our knowledge, the first report of such distribution profiles for CH3Hg between different-sized fractions of dissolved organic C in natural waters.  相似文献   

2.
The localized impact of blooms of the mixotrophic ciliate Myrionecta rubra in the Columbia River estuary during 2007–2010 was evaluated with biogeochemical, light microscopy, physiological, and molecular data. M. rubra affected surrounding estuarine nutrient cycles, as indicated by high and low concentrations of organic nutrients and inorganic nitrogen, respectively, associated with red waters. M. rubra blooms also altered the energy transfer pattern in patches of the estuarine water that contain the ciliate by creating areas characterized by high primary production and elevated levels of fresh autochthonous particulate organic matter, therefore shifting the trophic status in emergent red water areas of the estuary from net heterotrophy towards autotrophy. The pelagic estuarine bacterial community structure was unaffected by M. rubra abundance, but red waters of the ciliate do offer a possible link between autotrophic and heterotrophic processes since they were associated with elevated dissolved organic matter and showed a tendency for enhanced microbial secondary production. Taken together, these findings suggest that M. rubra red waters are biogeochemical hotspots of the Columbia River estuary.  相似文献   

3.
The speciation and partition of mercury in a macrotidal estuary (Seine estuary, France) was studied in order to explore the role of the high turbidity zone (HTZ) in mercury transfer to the adjacent coastal waters. Water and particles were analyzed to determine the concentrations of various mercury species, including monomethylmercury and the inorganic fraction. The exchangeable particulate mercury, which varies with salinity, and the mercury fraction associated with the amorphous oxyhydroxides were evaluated. The distribution of dissolved mercury species during early mixing suggests non-conservative behavior of organically bound mercury at the head of the estuary. Mercury in the particles covaried positively with suspended particulate matter concentrations up to a threshold, which constitutes the typical mercury load of particles and deposited sediments of the HTZ. This distribution pattern is well explained by a dilution model: a slowly settling, low metal population of particle, characterized by relatively invariant turbidity, becomes admixed with a variable amount of higher metal content particles derived from the resuspension in the HTZ. In addition, in the HTZ, which acts as a degradation reactor for particulate organic matter, particulate mercury concentrations increase with increasing C:N ratios and amorphous oxyhydroxides particles. Mercury reaches the estuarine HTZ mainly associated with the riverine and marine particles, including organic matter and oxyhydroxides, which are temporarily trapped in the HTZ and mixed with autochthonous HTZ particles. The largest particles periodically settle and undergo diagenetic reactions and resuspensions, which lead to their mercury enrichment. Depending upon hydrodynamic conditions, mercury escapes seaward as fine particulate within the plume, partially associated with the oxyhydroxides. A surface complexation model reproduces most of the partitioning observed. In the dissolved phase the model simulation suggests that a very strong ligand must be present to explain the field observations.  相似文献   

4.
Pristine water bodies in the Negro River basin, Brazilian Amazon, show relatively high concentrations of mercury. These waters are characterized by acidic pH, low concentrations of suspended solids, and high amounts of dissolved organic matter and are exposed to intense solar radiation throughout the year. This unique environment creates a very dynamic redox chemistry affecting the mobility of mercury due to the formation of the dissolved elemental species (Hg0). It has been shown that in this so-called black water, labile organic matter from flooded forest is the major scavenger of photogenerated H2O2. In the absence of hydrogen peroxide, these black waters lose their ability to oxidize Hg0 to Hg2+, thus increasing Hg0 evasion across the water/atmosphere interface, with average night time values of 3.80 pmol m?2 h?1. When the dry period starts, labile organic matter inputs gradually diminish, allowing the increasing concentration of H2O2 to re-establish oxidative water conditions, inhibiting the metal flux across the water/atmosphere interface and contributing to mercury accumulation in the water column.  相似文献   

5.
Marine chemistry of the coastal environment starts with principles of rock weathering that use carbonic acid to mobilize elements, only some of which comprise the majority of sea salt. The principle reason is reverse weathering, extensively represented in coastal waters, and returns most elements to newly formed colloids or minerals while recycling carbon dioxide to the atmosphere. This includes the deeper ocean expanse of sediment diagenesis, plus hydrothermal plumes and attendant low-temperature basalt alteration. Within the estuarine and extended shelf regimes, both conservative and non-conservative processes can be distinguished and modeled to determine proportions of weathered elements transmitted to the sea or consumed by reverse weathering. Conceptually, the steady-state processes that lead to the composition of seawater can be viewed as heterogeneous equilibria between dissolved constituents and solid mineral products taking hundreds of millennia. However, initial processes in the estuarine and coastal environment are characterized by shorter term scavenging associated with inorganic and organic colloids. These recycle both carbon and trace elements on timescales commensurate with estuarine flushing and coastal exchange with the ocean. The natural uranium and thorium decay series provide powerful tools for quantifying the rates of estuarine processes, including those within groundwater and the subterranean estuary. In the future, new mass spectrometric and nuclear magnetic resonance techniques will help to define the molecular nature of newly formed estuarine colloids as has been done for dissolved organic matter. As the coastal environment undergoes the forces of climate change in the form of warming and sea level rise, future research should address how these will impact chemistry of the coastal environment as a net source or sink of carbon dioxide and associated organic material.  相似文献   

6.
Many developing countries have regions of high demographic density, where untreated residuary waters from different sources are often discharged into rivers, streams and other water bodies. This paper discusses the reducing action of organic matter of anthropic origin on the mercury redox cycle in the Jundiaí River impacted by discharged wastes, and on the Piraí River, a non-impacted water body. The total mercury concentrations in these locations vary from 1.7 to 32?ng?L?1 in the former and from 0.6 to 10.6?ng?L?1 in the latter. Dissolved organic carbon concentrations of up to 68.3 and 6.5?mg?L?1 were observed, confirming the higher impact on the Jundiaí River. It was found that an inverse correlation between the concentration of dissolved organic carbon and total mercury was stronger in the Jundiaí River, given that it receives higher organic loads, suggesting that organic matter exerts a reducing action on mercury, which is released as gas into the atmosphere. This correlation was not observed in the Piraí River, where the organic matter of natural origin is probably not sufficiently labile to act intensely upon the Hg redox cycle, favoring the metal transport.  相似文献   

7.
We used high-resolution in situ measurements of turbidity and fluorescent dissolved organic matter (FDOM) to quantitatively estimate the tidally driven exchange of mercury (Hg) between the waters of the San Francisco estuary and Browns Island, a tidal wetland. Turbidity and FDOM??representative of particle-associated and filter-passing Hg, respectively??together predicted 94?% of the observed variability in measured total mercury concentration in unfiltered water samples (UTHg) collected during a single tidal cycle in spring, fall, and winter, 2005?C2006. Continuous in situ turbidity and FDOM data spanning at least a full spring-neap period were used to generate UTHg concentration time series using this relationship, and then combined with water discharge measurements to calculate Hg fluxes in each season. Wetlands are generally considered to be sinks for sediment and associated mercury. However, during the three periods of monitoring, Browns Island wetland did not appreciably accumulate Hg. Instead, gradual tidally driven export of UTHg from the wetland offset the large episodic on-island fluxes associated with high wind events. Exports were highest during large spring tides, when ebbing waters relatively enriched in FDOM, dissolved organic carbon (DOC), and filter-passing mercury drained from the marsh into the open waters of the estuary. On-island flux of UTHg, which was largely particle-associated, was highest during strong winds coincident with flood tides. Our results demonstrate that processes driving UTHg fluxes in tidal wetlands encompass both the dissolved and particulate phases and multiple timescales, necessitating longer term monitoring to adequately quantify fluxes.  相似文献   

8.
This study examined freshwater discharge of dissolved organic matter (DOM) to the shallow Lavaca–Matagorda (LM) Bay estuarine system along the central Texas coast and investigated whether chromophoric DOM (CDOM) photochemical reactions have the potential to stimulate microbial activity within LM estuarine waters. Dissolved organic carbon (DOC) concentrations ranged from 3 to 10 mg C l−1 and CDOM levels (reported as a 305) ranged from 8 to 77 m−1 during April and July, 2007, when the LM system was experiencing very high freshwater inputs. DOC and CDOM levels were well-correlated with salinities > 3, but exhibited considerable variability at salinities < 3. CDOM photobleaching rates (i.e., decrease in a 305 resulting from exposure to solar radiation) for estuarine samples ranged from 0.014 to 0.021 h−1, corresponding to photobleaching half-lives of 33–50 h. Our data indicate when Matagorda Bay waters photobleach; dissolved organic carbon utilization is enhanced perhaps due to enhanced microbial respiration of biologically labile photoproducts (BLPs). Net ecosystem metabolism calculations indicate that most of the LM system was net heterotrophic during our study. We estimate that BLP formation could support up to 20% of the daily microbial respiratory C demand in LM surface waters and combined with direct photochemical oxygen consumption could have an important influence on O2 cycles in the LM system.  相似文献   

9.
The ability of organic matter as well as carbonate ions to extract rare earth elements (REEs) from sandy sediments of a Coastal Plain aquifer was investigated for unpurified organic matter from different sources (i.e., Mississippi River natural organic matter, Aldrich humic acid, Nordic aquatic fulvic acid, Suwannee River fulvic acid, and Suwannee River natural organic matter) and for extraction solutions containing weak (i.e., CH3COO−) or strong (i.e., ) ligands. The experimental results indicate that, in the absence of strong REE complexing ligands in solution, the amount of REEs released from the sand is small and the fractionation pattern of the released REEs appears to be controlled by the surface stability constants for REE sorption with Fe(III) oxides/oxyhydroxides. In the presence of strong solution complexing ligands, however, the amount and the fractionation pattern of the released REEs reflect the strength and variation of the stability constants of the dominant aqueous REE species across the REE series. The varying amount of REEs extracted by the different organic matter employed in the experiments indicates that organic matter from different sources has different complexing capacity for REEs. However, the fractionation pattern of REEs extracted by the various organic matter used in our experiments is remarkable consistent, being independent of the source and the concentration of organic matter used, as well as solution pH. Because natural aquifer sand and unpurified organic matter were used in our experiments, our experimental conditions are more broadly similar to natural systems than many previous laboratory experiments of REE-humic complexation that employed purified humic substances. Our results suggest that the REE loading effect on REE-humic complexation is negligible in natural waters as more abundant metal cations (e.g., Fe, Al) out-compete REEs for strong binding sites on organic matter. More specifically, our results indicate that REE complexation with organic matter in natural waters is dominated by REE binding to weak sites on dissolved organic matter, which subsequently leads to a middle REE (MREE: Sm-Ho)-enriched fractionation pattern. The experiments also indicate that carbonate ions may effectively compete with fulvic acid in binding with dissolved REEs, but cannot out compete humic acids for REEs. Therefore, in natural waters where low molecular weight (LMW) dissolved organic carbon (DOC) is the predominant form of DOC (e.g., lower Mississippi River water), REEs occur as “truly” dissolved species by complexing with carbonate ions as well as FA, resulting in heavy REE (HREE: Er-Lu)-enriched shale-normalized fractionation patterns. Whereas, in natural terrestrial waters where REE speciation is dominated by organic complexes with high molecular weight DOC (e.g., “colloidal” HA), only MREE-enriched fractionation patterns will be observed because the more abundant, weak sites preferentially complex MREEs relative to HREEs and light REEs (LREEs: La-Nd).  相似文献   

10.
Using stable isotope tracer techniques in 4-h bottle incubations, the importance of organic matter transfer from phytoplankton to heterotrophic bacteria (bacteria) has been re-evaluated in the Delaware Estuary, considering carbon (C) and nitrogen (N) cycles separately. The hypothesis is that the transfer of C and N from phytoplankton to bacteria varies both temporally and spatially along estuarine gradients in response to variation in factors such as terrestrial organic C supply, inorganic N speciation and concentrations, and extracellular release of dissolved organic matter by phytoplankton. The percentage of autochthonous dissolved organic C being assimilated by bacteria varied between 3% and 10% of primary production and was not related to the rate of primary production. The transfer of N was considerably more variable when compared to C transfer, averaging ca. 20% of phytoplankton N assimilation; individual experiments yielded rates as high as 50%. Unlike C, autochthonous dissolved organic N transfer appears to vary with the magnitude of primary production, and its assimilation by bacteria accounted for 0–56% of the total measured bacterial N uptake. The results highlight the importance of separate consideration of C and N elemental cycles in evaluating sources of organic matter to the estuarine microbial loop.  相似文献   

11.
A 1-D biogeochemical reactive transport model with a full set of equilibrium and kinetic biogeochemical reactions was developed to simulate the fate and transport of arsenic and mercury in subaqueous sediment caps. Model simulations (50?years) were performed for freshwater and estuarine scenarios with an anaerobic porewater and either a diffusion-only or a diffusion plus 0.1-m/year upward advective flux through the cap. A biological habitat layer in the top 0.15?m of the cap was simulated with the addition of organic carbon. For arsenic, the generation of sulfate-reducing conditions limits the formation of iron oxide phases available for adsorption. As a result, subaqueous sediment caps may be relatively ineffective for mitigating contaminant arsenic migration when influent concentrations are high and sorption capacity is insufficient. For mercury, sulfate reduction promotes the precipitation of metacinnabar (HgS) below the habitat layer, and associated fluxes across the sediment–water interface are low. As such, cap thickness is a key design parameter that can be adjusted to control the depth below the sediment–water interface at which mercury sulfide precipitates. The highest dissolved methylmercury concentrations occur in the habitat layer in estuarine environments under conditions of advecting porewater, but the highest sediment concentrations are predicted to occur in freshwater environments due to sorption on sediment organic matter. Site-specific reactive transport simulations are a powerful tool for identifying the major controls on sediment- and porewater-contaminant arsenic and mercury concentrations that result from coupling between physical conditions and biologically mediated chemical reactions.  相似文献   

12.
The estuarine mixing of dissolved Fe, Cu, Ni, Si and surface-active organic matter has been investigated in the Taieri Estuary, New Zealand, simultaneously with measurements of the electrokinetic charge on colloidal particles. Dissolved Fe showed almost quantitative removal from solution characteristic of the coagulation of iron-containing colloids by seawater electrolytes. Surface active organic matter behaved conservatively, indicating that a relatively constant fraction of estuarine organic matter is surface active, but that organic species associated with iron during removal are a minor fraction. Results for Cu, Ni and Si were scattered but offered no evidence for gross removal during estuarine mixing. The negative charge on suspended colloids was not reversed by adsorption of seawater cations, but remained uniformly negative throughout the salinity range, decreasing sharply in magnitude during the first few %. salinity.  相似文献   

13.
The sandy beachface at Cape Henlopen, Delaware, receives dissolved nutrient inputs from fresh upland groundwater and estuarine seawater and exports nutrients through intertidal and submarine groundwater discharge. The discharge of brackish beachface waters indicates that there must be additional diagenetic nutrient sources and sinks within the porous beachface aquifer. At some times of the year, diagenetic processes within the beachface remove nitrate from waters draining the beachface consistent with the stoichiometry of either denitrification or dissimilatory nitrate reduction to ammonium. Up to 50–100% of the nitrate load from the upland groundwaters is apparently reduced to N2O/N2 gas or ammonium during these periods. At other times, ammonium and nitrate are added to beachface waters consistent with the stoichiometry of organic matter remineralization and nitrification. Dissolved reactive phosphorus and silica are similarly consumed and produced by beachface processes at different times of the year, presumably by adsorption or desorption. Infiltration of reactive estuarine particles may be an additional source of nutrients and carbon that supports the diagenetic activity in the beachface aquifer. These observations suggest that sandy beachfaces are biogeochemically reactive systems that can serve as sources, sinks, and temporary reservoirs of nutrients to support the primary and secondary production of the adjacent intertidal zone.  相似文献   

14.
Stable carbon isotope (δ13C) analysis was used in the Peridido Estuary, Florida U.S. to determine the predominant carbon source that supports the bacterial assemblage. Stable carbon isotope values were measured in the suspended particulate matter (SPM), dissolved organic and inorganic matter, and bacteria. Stable nitrogen isotope (δ15N) ratios were measured in SPM and nitrate to assist in understanding carbon cycling through the estuary. Analyses were conducted on samples from riverine, coastal, and anthropogenic sources and compared with samples from the bay. Stable isotope ratio analysis was coupled with estimates of mixing of riverine and coastal waters into the bay. Preliminary observation of the °13C data indicates that terrestrial organic matter is the primary carbon source that is assimilated by bacteria in the ecosystem. Stable isotope data from carbon and nitrogen pools in combination with analysis of estuarine current velocities indicates that primary production is an important factor in the carbon cycle. This study demonstrates the importance of stable isotope analysis of multiple carbon and nitrogen pols to assess sources and cycling of organic matter.  相似文献   

15.
Two organic rich sediments, an oxic muddy sand and a silty mud containing sulphate reducing and methane producing metabolic zones, were sampled from Loch Duich, a fjord type estuary in the N.W. coast of Scotland. Dissolved organic carbon (DOC), as measured by dry combustion and UV absorption, remained constant (8.3–15.8 mg C/l) with depth in the oxic pore waters at a concentration at least twice that of the overlying seawater. DOC in the anoxic pore waters increased linearly with depth from 13.6 at the surface to 55.9–70.5 mg C/l at 80cm. Most of the DOC was present in the high molecular weight (HMW) fraction as separated by ultrafiltration; the low molecular weight (LMW) fraction remained constant (10.0 mg C/l) in both oxic and anoxic pore waters. Spectroscopic data showed the ‘humic’ fraction of the HMW dissolved organic matter was mainly fulvic acid, a small proportion (approx 1%) of humic acid, and a third fraction, possibly melanoidins, which increased relative to fulvic acid with depth. These data confirm the pathway of humification (NissenBaum et al, 1971; nissenbaum and Kaplan, 1972) where HMW organic matter accumulates in pore waters as condensation products of LMW organic substances.  相似文献   

16.
The sedimentary geochemistry of dissolved Al is complicated by a number of different reactions. In this study we show that complexation by organic matter, adsorption to Fe-oxyhydroxides, and reaction with Si in solution have important effects on the distribution of dissolved Al in sediments. In the absence of physical resuspension of sediment into overlying waters, dissolved Al is rapidly consumed at the sediment-water interface and is subsequently released upon reduction of Fe-oxyhydroxides. This release does not cause noticeable perturbations in dissolved Al concentrations in sediments because of rapid consumption reactions which mask the true mobility of Al. Results suggest that one of the consumption reactions may be due to formation of an Fe-Al-silicate. The amount of authigenic aluminosilicate formed in estuarine sediments must be very small relative to the detrital component. In the deep-sea, however, the long residence time of Fe-oxyhydroxides at the sediment-water interface, with resulting greater accumulation of adsorbed Al may explain the abundance of Al in Fe-smectites reported from many different areas.  相似文献   

17.
Seasonal succession and composition of both attached and free-living bacterial communities were studied in subtropical estuarine and coastal waters with contrasting hydrographic conditions. A higher abundance of attached bacteria was recovered in the estuarine waters containing high concentrations of dissolved organic carbon (DOC) resulting from the freshwater discharge in the adjacent Pearl River, and Proteobacteria, including ??-, ??-, and ??-groups, predominated the attached community at both stations. Free-living bacterial communities at both stations showed higher diversity and lower seasonality than their attached counterparts, and ??-Proteobacteria accounted for the highest proportion at both stations. Redundancy analysis (RDA) demonstrated that, in addition to the obvious temperature effects, DOC and microphytoplankton (>20???m Chl a) drive the temporal variation of attached bacteria at the estuarine and coastal stations, respectively. On the other hand, picophytoplankton (<2???m Chl a) and dissolved oxygen concentration explained most of the free-living bacterial community succession at the estuarine station, while those at the coastal station were associated with micro- and picoplankton (Chl a fractions of <2 and >20???m). These findings suggest that temperature and bottom?Cup effects play a more important role for the spatial?Ctemporal variations of both attached and free-living bacterial communities in the subtropical estuarine and coastal waters.  相似文献   

18.
This project examined concentrations, composition and turnover neutral sugars in the Delaware estuary to gain insights into dissolved inorganic nitrogen (DIN) use by heterotrophic bacteria and into the lability and diagenetic state of dissolved organic material (DOM) during passage through the estuary. Dissolved free monosaccharides were not measurable (<5 nM) in the estuary whereas concentrations of dissolved combined neutral sugars (DCNS) were high, much higher than observed in oceanic waters. DCNS made up a similar fraction of dissolved organic carbon (DOC) as in the oceanic waters examined to date, and the monosaccharide composition of the DCNS pool was similar to that of oceanic waters. The composition did not vary substantially within the estuary or seasonally, but it did vary among three size fractions of the organic matter pool. Glucose was enriched in the low molecular weight fraction of DOC and in particulate material, whereas the high molecular weight DOC fraction was slightly depleted in glucose. Depletion experiments indicated that DCNS is not used extensively on the day time scale in the Delaware estuary, although freshly-produced polysaccharides may still be important carbon sources for heterotrophic bacteria. The very low concentrations of free monosaccharides in the Delaware estuary help to explain why DIN use by heterotrophic bacteria is relatively low in this estuary. Although DOC-DIN interactions in the Delaware apparently differ from oceanic waters, the portion of DOM traced by DCNS, which is thought to be the labile fraction, appears to be similar to that of oceanic DOM, suggesting that organic material in the estuary is degraded extensively before being exported to the coastal ocean.  相似文献   

19.
Using high-resolution measures of aquatic ecosystem metabolism and water quality, we investigated the importance of hydrological inputs of phosphorus (P) on ecosystem dynamics in the oligotrophic, P-limited coastal Everglades. Due to low nutrient status and relatively large inputs of terrestrial organic matter, we hypothesized that the ponds in this region would be strongly net heterotrophic and that pond gross primary production (GPP) and respiration (R) would be the greatest during the “dry,” euhaline estuarine season that coincides with increased P availability. Results indicated that metabolism rates were consistently associated with elevated upstream total phosphorus and salinity concentrations. Pulses in aquatic metabolism rates were coupled to the timing of P supply from groundwater upwelling as well as a potential suite of hydrobiogeochemical interactions. We provide evidence that freshwater discharge has observable impacts on aquatic ecosystem function in the oligotrophic estuaries of the Florida Everglades by controlling the availability of P to the ecosystem. Future water management decisions in South Florida must include the impact of changes in water delivery on downstream estuaries.  相似文献   

20.
The influence of Zn speciation on Zn transport by drainage from different soils to surface water is examined in a stream catchment in an agricultural area. Drainage waters were collected from two types of soils, a mineral soil (MS) and a soil rich in organic matter (OS) by means of artificial drainage pipes. The speciation of dissolved Zn in the stream and the drainage waters was determined using ligand-exchange and voltammetry. About 50–95% of dissolved Zn is bound in strong complexes, and the free Zn2+ ion concentration is in the range of 1–16% of dissolved Zn. A substantial part of Zn is present in weaker organic or inorganic complexes. The simulated Zn speciation using the WHAM VI model is compared to the determined speciation. Free Zn2+ concentrations predicted by the WHAM VI model are generally higher than the analytically determined free Zn2+, but are mostly within the same order of magnitude. Effects of different soil organic matter content on Zn speciation and transport are discussed. Zn speciation in the drainage at the OS site is influenced by the distribution of organic matter between the solid and solution phase. The abundant organic Zn complexes in solution contribute to facilitate Zn transport from soil into surface waters, through the drainage at the OS site. Drainage from the OS site contributes about twice as much Zn input to the receiving water as the MS soil, as related to specific area. The mineral soil contains much lower organic matter, and a part of Zn bound with inorganic phases can hardly be released by dissolved organic ligands, leading to much higher Zn retention at the MS site.  相似文献   

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