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1.
Thermogenic organic matter dissolved in the abyssal ocean   总被引：1，自引：2，他引：1  
Formation and decay of thermogenic organic matter are important processes in the geological carbon cycle, but little is known about the fate of combustion-derived and petrogenic compounds in the ocean. We explored the molecular structure of marine dissolved organic matter (DOM) for thermogenic signatures in different water masses of the Southern Ocean. Ultrahigh-resolution mass spectrometry via the Fourier transform-ion cyclotron resonance technique (FT-ICR-MS) revealed the presence of polyaromatic hydrocarbons (PAHs) dissolved in the abyssal ocean. More than 200 different PAHs were discerned, most of them consisting of seven condensed rings with varying numbers of carboxyl, hydroxyl, and aliphatic functional groups. These unambiguously thermogenic compounds were homogenously distributed in the deep sea, but depleted at the sea surface. Based on the structural information alone, petrogenic and pyrogenic compounds cannot be distinguished. Surface depletion of the PAHs and first estimates for their turnover rate (> 1.2 · 1012 mol C per year) point toward a primarily petrogenic source, possibly deep-sea hydrothermal vents, which is thus far speculative because the fluxes of combustion-derived and petrogenic matter to the ocean are not well constrained. We estimate that > 2.4% of DOM are thermogenic compounds, and their global inventory in the oceans is > 1.4 · 1015 mol C, significantly impacting global biogeochemical cycles.  相似文献   

2.
C. Arnosti   《Marine Chemistry》2004,92(1-4):263
The observation that a fraction of organic matter produced in marine systems evades the concerted efforts of microbial communities and is buried in sediments suggests that there are ‘speed bumps’ in carbon degradation pathways that impede microbially driven remineralization processes. The initial step in degradation of macromolecules, extracellular enzymatic hydrolysis, is often stated to be ‘the’ rate-limiting step in carbon remineralization. Experimental investigations described here, however, demonstrate that at least in certain cases, microbes produce extracellular enzymes on time scales of hours to tens of hours in response to substrate addition, and hydrolysis is extremely rapid. If enzymatic hydrolysis can be rapid, what factors slow or stop organic matter degradation? A lack of the correct inducer to initiate enzyme production, and/or a lack of the correct organism to produce the required enzyme, may result in a complete lack of hydrolysis in certain environments—a barricade, rather than a speed bump. Preliminary evidence supporting this hypothesis includes a comparison of polysaccharide hydrolysis in seawater and sediments, which demonstrates that the spectrum of enzymes active in seawater and sediments are fundamentally different. Furthermore, a survey of enzyme activities in surface waters from a range of locations suggests that pelagic microbial communities also differ widely in their abilities to express specific extracellular enzymes. Trans-membrane transport through porins is yet another potential location of structure-related selectivity.Our efforts to identify speed bumps and barricades are hampered by our inability to structurally characterize in sufficient detail the macromolecular structures present in marine systems. Furthermore, assessments of organic matter ‘quality’ from a chemical perspective do not necessarily accurately reflect the availability of organic carbon to microbial communities. For these communities, in fact, ‘quality’ may be a variable, which depends on the enzymatic and uptake capabilities of community members. To begin to assess substrate structure and quality from a microbial perspective, we will have to combine specific knowledge of macromolecular structures with detailed investigations of the enzymatic and transport capabilities of heterotrophic marine microbes.  相似文献   

3.
The vertical and horizontal distribution of fluorescent dissolved organic matter (FDOM), determined by fluorescence intensity at 320 nm excitation and 420 nm emission, were clarified in nine stations on two transects at the Southern Ocean, including a subtropical, subantarctic, polar frontal and Antarctic zone. All vertical profiles of fluorescence intensity showed that levels were lowest in the surface waters, increased with increasing the depth in mid-depth waters ( 2000 m), and then stayed within a relatively narrow range from there to the bottom. Such vertical profiles of FDOM were similar to those of nutrients, but were adverse to dissolved oxygen. In water columns below the temperature-minimum subsurface water (dichothermal waters) in the Antarctic zone and below the winter mixed layer in the other zones, we determined the relationships of fluorescence intensity to concentrations of nutrients and apparent oxygen utilization (AOU) over the entire area of the present study, and found significant linear correlations between the levels of fluorescence intensity and nutrient concentrations (r =  0.70 and 0.71 for phosphate and nitrate + nitrite, respectively) and AOU (r = 0.91). From the strong correlation coefficient between fluorescence intensity and AOU, we concluded that FDOM in the Southern Ocean is formed in situ via the biological oxidation of organic matter. The regeneration of the nutrients/consumption of the oxygen/formation of FDOM was active in mid-depth waters. However, the correlations between fluorescence intensities and nutrients and AOU were different in the mid-depth water masses, Subantarctic Mode Water (SAMW), and Antarctic Intermediate Water (AAIW), indicating that the sources of organic matter responsible for FDOM formation were different. A considerable amount of FDOM in the SAMW is thought to be produced by the remineralization of DOM in addition to sinking particulate organic matter, while DOM is less responsible for FDOM formation in the AAIW.  相似文献   

4.
The bioavailability and bacterial degradation rates of dissolved organic matter (DOM) were determined over a seasonal cycle in Loch Creran (Scotland) by measuring the decrease in dissolved organic carbon (DOC), nitrogen (DON) and phosphorous (DOP) concentrations during long-term laboratory incubations (150 days) at a constant temperature of 14 °C. The experiments showed that bioavailable DOC (BDOC) accounted for 29 ± 11% of DOC (average ± SD), bioavailable DON (BDON) for 52 ± 11% of DON and bioavailable DOP (BDOP) for 88 ± 8% of DOP. The seasonal variations in DOM concentrations were mainly due to the bioavailable fraction. BDOP was degraded at a rate of 12 ± 4% d– 1 (average ± SD) while the degradation rates of BDOC and BDON were 7 ± 2% d– 1 and 9 ± 2% d– 1 respectively, indicating a preferential mineralization of DOP relative to DON and of DON relative to DOC. Positive correlations between concentration and degradation rate of DOM suggested that the higher the concentration the faster DOM would be degraded. On average, 77 ± 9% of BDOP, 62 ± 14% of BDON and 49 ± 19% of BDOC were mineralized during the residence time of water in Loch Creran, showing that this coastal area exported C-rich DOM to the adjacent Firth of Lorne. Four additional degradation experiments testing the effect of varying temperature on bioavailability and degradation rates of DOM were also conducted throughout the seasonal cycle (summer, autumn, winter and spring). Apart from the standard incubations at 14 °C, additional studies at 8 °C and 18 °C were also conducted. Bioavailability did not change with temperature, but degradation rates were stimulated by increased temperature, with a Q10 of 2.6 ± 1.1 for DOC and 2.5 ± 0.7 for DON (average ± SD).  相似文献   

5.
An interaction of dissolved natural organic matter (DNOM) with copper ions in the water column of the stratified Krka River estuary (Croatia) was studied. The experimental methodology was based on the differential pulse anodic stripping voltammetric (DPASV) determination of labile copper species by titrating the sample using increments of copper additions uniformly distributed on the logarithmic scale. A classical at-equilibrium approach (determination of copper complexing capacity, CuCC) and a kinetic approach (tracing of equilibrium reconstitution) of copper complexation were considered and compared. A model of discrete distribution of organic ligands forming inert copper complexes was applied. For both approaches, a home-written fitting program was used for the determination of apparent stability constants (Kiequ), total ligands concentration (LiT) and association/dissociation rate constants (ki1,ki- 1).A non-conservative behaviour of dissolved organic matter (DOC) and total copper concentration in a water column was registered. An enhanced biological activity at the freshwater–seawater interface (FSI) triggered an increase of total copper concentration and total ligand concentration in this water layer. The copper complexation in fresh water of Krka River was characterised by one type of binding ligands, while in most of the estuarine and marine samples two classes of ligands were identified. The distribution of apparent stability constants (log K1equ: 11.2–13.0, log K2equ:8.8–10.0) showed increasing trend towards higher salinities, indicating stronger copper complexation by autochthonous seawater organic matter.Copper complexation parameters (ligand concentrations and apparent stability constants) obtained by at-equilibrium model are in very good accordance with those of kinetic model. Calculated association rate constants (k11:6.1–20 × 103 (M s)− 1, k21: 1.3–6.3 × 103 (M s)− 1) indicate that copper complexation by DNOM takes place relatively slowly. The time needed to achieve a new pseudo-equilibrium induced by an increase of copper concentration (which is common for Krka River estuary during summer period due to the nautical traffic), is estimated to be from 2 to 4 h.It is found that in such oligotrophic environment (dissolved organic carbon content under 83 µMC, i.e. 1 mgCL− 1) an increase of the total copper concentration above 12 nM could enhance a free copper concentration exceeding the level considered as potentially toxic for microorganisms (10 pM).  相似文献   

6.
The dynamics of high molecular weight organic matter in marine systems are influenced by molecular conformation, interactions with surfaces and susceptibility to enzymatic hydrolysis, parameters that are difficult to observe experimentally. Here we use electron paramagnetic resonance spectroscopy (EPR) and spin-labeled (SL-) polysaccharides to monitor the sorption of SL-polysaccharides to natural sediment surfaces and to montmorillonite and to observe decreases in polysaccharide size due to enzymatic hydrolysis. SL-pullulan, SL-xylan and SL-maltoheptaose all sorbed rapidly to muddy sediments but not to sandy sediments. SL-pullulan and SL-maltoheptaose also both sorbed to montmorillonite; however, SL-pullulan reached substantially greater final surface loadings than did SL-maltoheptaose. Using EPR has the advantages of being rapid (spectra can be acquired in 100 seconds), non-destructive and functional in complex media, including sediment slurries, muddy water or other optically opaque samples, permitting investigation of the interactions between biomacromolecules, extracellular enzymes and mineral surfaces in aquatic environments.  相似文献   

7.
To increase our understanding of the roles of black carbon (BC), a highly sorptive and recalcitrant material, we measured BC concentrations and fluxes in marine particulate organic carbon (POC) out of the water column in the Gulf of Maine (GoM), a representative coastal area downwind of important BC sources of the Northeastern United States. Concentrations ranged from < 0.1 to 16 μg/L in the spring and late summer, typically contributing between 1 and 20% of the POC. Water-column export fluxes were near 10 gBC/m2∙yr. These observations suggest that (a) up to 50% of the “molecularly uncharacterized” POC in this region's seawater is combustion-derived BC, and (b) the “bioavailabilities” of hydrophobic pollutants like polycyclic aromatic hydrocarbons (PAHs) would be influenced substantially by sorption to BC. The observed BC spatial distributions imply that a large part of the BC was carried offshore by wind and that much of it is accumulated in the coastal sediments. On a global scale, these results suggest the GoM and other coastal areas with similar BC loadings accumulate significant amounts of highly recalcitrant organic carbon that remineralizes on geological time scales in the world's oceans.  相似文献   

8.
The release of ammonium from the photochemical degradation of dissolved organic matter (DOM) has been proposed by earlier studies as a potentially important remineralisation pathway for refractory organic nitrogen. In this study the photochemical production of ammonium from Baltic Sea DOM was assessed in the laboratory. Filtered samples from the Bothnian Bay, the Gulf of Finland and the Arkona Sea were exposed to UVA light at environmentally relevant levels, and the developments in ammonium concentrations, light absorption, fluorescence and molecular size distribution were followed. The exposures resulted in a decrease in DOM absorption and loss of the larger sized fraction of DOM. Analysis of the fluorescence properties of DOM using parallel factor analysis (PARAFAC) identified 6 independent components. Five components decreased in intensity as a result of the UVA exposures. One component was produced as a result of the exposures and represents labile photoproducts derived from terrestrial DOM. The characteristics of DOM in samples from the Bothnian Bay and Gulf of Finland were similar and dominated by terrestrially derived material. The DOM from the Arkona Sea was more autochthonous in character. Photoammonification differed depending on the composition of DOM. Calculated photoammonification rates in surface waters varied between 121 and 382 μmol NH4+ L− 1 d− 1. Estimated areal daily production rates ranged between 37 and 237 μmol NH4+ m− 2 d− 1, which are comparable to atmospheric deposition rates and suggest that photochemical remineralisation of organic nitrogen may be a significant source of bioavailable nitrogen to surface waters during summer months with high irradiance and low inorganic nitrogen concentrations.  相似文献   

9.
The Banc d'Arguin, a non-estuarine area of shallows and intertidal flats off the tropical Saharan coast of Mauritania, is characterised by extensive intertidal and subtidal seagrass beds. We examined the characteristics of intertidal seagrass (Zostera noltii) meadows and bare areas in terms of the presence and abundance of molluscs (gastropods and bivalves). To explain observed differences between molluscan assemblages in seagrass and bare patches, some aspects of the feeding habitat (top-5 mm of the sediment) and of food (organic materials) of molluscs were examined. The novelty of this study is that phytopigments were measured and identified to assess source and level of decay (freshness) of organic material in the sediment and to study their importance as an explanatory variable for the distribution of molluscs. Over an area of 36 km2 of intertidal flats, at 12 sites, paired comparisons were made between seagrass-covered and nearby bare patches. Within seagrass meadows, dry mass of living seagrass was large and amounted to 180 ±10 g AFDM m− 2 (range 75–240). Containing twice the amount of silt per unit dry sediment mass, seagrass sediments were muddier than bare areas; the relative amount of organic material was also larger. The total number of species of bivalves and gastropods amounted to 27, 14 of which were found only in seagrass areas, 4 only in bare and 9 in both types of habitat. Among the three numerically most abundant species, the bivalves Anadara senilis, Dosinia hepatica and Loripes lacteus, the first was numerically most abundant in bare and the other two in seagrass-covered areas. Bare intertidal areas had greater mean total biomass of molluscs (80.5 g AFDM m− 2) than seagrass meadows (30.0 g AFDM m− 2). In both habitats, the bulk of the biomass was made up by A. senilis. Excluding this species, bare mudflats contained on average only 3.1 g AFDM m− 2 and seagrass meadows 6.9 g AFDM m− 2. As compared to previous surveys in 1980–1986, the biomass of A. senilis had increased almost 10-fold and D. hepatica, previously found in very small numbers, had become the most numerous species. However, the total biomass excluding that of A. senilis was similar. Concentrations of phytopigments were similar to those observed at temperate mudflats, indicating that the Banc d'Arguin might not be as oligotrophic as previously thought. Per unit of dry sediment mass, smaller amounts of phytopigments were found in bare than in seagrass areas. Per unit of dry organic material, bare sediments contained most (fresh) phytopigments. This suggests that in seagrass-covered meadows the organic material is more degraded than in bare sediments. Overall, the composition of phytopigments, quite surprisingly, indicated a benthic-diatom-dominated trophic system. Multivariate statistics revealed that patterns of zoobenthic assemblages were correlated with patterns of a combination of four environmental parameters: grain size of the sediment, amount of fresh phytopigments and amounts of leaves and roots of seagrass.  相似文献   

10.
The activities of extracellular enzymes that initiate the microbial remineralization of high molecular weight organic matter were investigated in the water column and sandy surface sediments at two sites in the northeastern Gulf of Mexico. Six fluorescently labeled polysaccharides were hydrolyzed rapidly in the water column as well as in permeable sediments. This result contrasts with previous studies carried out in environments dominated by fine-grained muds, in which the spectrum of enzymes active in the water column is quite limited compared to that of the underlying sediments. Extracts of Spirulina, Isochrysis, and Thalassiosira were also used to measure hydrolysis rates in water from one of the sites. Rates of hydrolysis of the three plankton extracts were comparable to those of the purified polysaccharides. The broad spectrum and rapid rates of hydrolysis observed in the water column at both sites in the northeastern Gulf of Mexico may be due to the permeable nature of the sediments. Fluid flux through the sediments is sufficiently high that the entire 1.5 m deep water column could filter though the sediments on timescales of a few days to two weeks. Movement of water through sediments may also transport dissolved enzymes from the sediment into the water column, enhancing the spectrum as well as the rate of water column enzymatic activities. Such interaction between the sediments and water column would permit water column microbial communities to access high molecular weight substrates that might otherwise remain unavailable as substrates.  相似文献   

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