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1.
How dissolved organic matter (DOM) undergoes chemical changes during its transit from river to ocean remains a challenge due to its complex structure. In this study, DOM along a river transect from black waters to marine waters is characterized using an offline combination of reversed-phase high performance liquid chromatography (RP-HPLC) coupled to electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (ESI-FTICR-MS), as well as tandem ESI-FTICR-MS. In addition, a water extract from degraded wood that mainly consists of lignins is used for comparison to the DOM from this transect. The HPLC chromatograms of all DOM samples and the wood extract show two major well-separated components; one is hydrophilic and the other is hydrophobic, based on their elution order from the C18 column. From the FTICR-MS analysis of the HPLC fractions, the hydrophilic components mainly contain low molecular weight compounds (less than 400 Da), while the hydrophobic fractions contain the vast majority of compounds of the bulk C18 extracted DOM. The wood extract and the DOM samples from the transect of black waters to coastal marine waters show strikingly similar HPLC chromatograms, and the FTICR-MS analysis further indicates that a large fraction of molecular formulas from these samples are the same, existing as lignin-like compounds. Tandem mass spectrometry experiments show that several representative molecules from the lignin-like compounds have similar functional group losses and fragmentation patterns, consistent with modified lignin structural entities in the wood extract and these DOM samples. Taken together, these data suggest that lignin-derived compounds may survive the transit from the river to the coastal ocean and can accumulate there because of their refractory nature.  相似文献   

2.
Reversed-phase liquid chromatography/mass spectrometry (LC/MS) is introduced as a new molecular fingerprinting technique for tracing terrigenous dissolved organic matter (DOM) and its photochemical decay in the ocean. DOM along a transect from the mangrove-fringed coast in Northern Brazil to the shelf edge was compared with mangrove-derived porewater DOM exposed to natural sunlight for 2–10 days in a photodegradation experiment. DOM was isolated from all samples via solid-phase extraction (C18) for LC/MS analysis. DOM in the estuary and ocean showed a bimodal mass distribution with two distinct maxima in the lower m/z range from 400 to 1000 Da (intensity-weighted average of 895 Da). Terrigenous porewater DOM from the mangroves was characterized by a broad molecular mass distribution over the detected range from 150 to 2000 Da (intensity-weighted average of 1130 Da). Polar compounds, i.e., those that eluted early in the reversed-phase chromatography, absorbed more UV light and had on average smaller molecular masses than the more apolar compounds.  相似文献   

3.
Dissolved organic matter (DOM) and dissolved copper-organic complexes were isolated from the estuarine waters of Narragansett Bay, RI, using reverse-phase liquid chromatography (RPLC). Different types of reverse-phase BOND ELUT columns (Analytichem International), including C2, C18 and phenyl-bonded phases, were studied to determine their adsorption efficiency for extracting DOM. Extraction efficiencies followed the order phenyl > C18 > C2, and phenyl − C18 > C2 for DOM and organic copper, respectively. However, comparisons of BOND ELUT and C18 SEP-PAK (Waters Associates) columns indicated that SEP-PAK columns were the most efficient when both DOM and organic copper were considered. Chromatographic profiles of the isolated DOM obtained using high-performance liquid chromatography were similar in elution characteristics and resembled chromatograms typical of fulvic acid. The UV-absorption characteristics of the DOM showed small differences and suggested that the different reverse-phase columns isolated material that was qualitatively similar.Copper-organic complexes isolated using C18 RPLC were studied to examine the dissociation of organically bound copper in seawater as the pH is lowered. Only a small amount of the complexed copper was displaced by the H+ with about 40% of the copper remaining bound at pH 3. However, the chromatographic elution behavior of the DOM and organic copper was significantly altered under acidic conditions as a result of protonation of acidic functional sites on the organic matter.  相似文献   

4.
Dissolved organic matter (DOM) was investigated along a gradient across the Subtropical Convergence (STC) off the South Island, New Zealand. Ultrahigh resolution electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR-MS), excitation emission matrix fluorescence (EEM) spectroscopy, and molecular lignin analysis techniques were used to study this DOM. The analysis revealed a group of compounds found only in the coastal DOM samples, which were also characterized by an elevated terrestrial DOM fluorescence pattern and elevated lignin content if compared to the offshore samples. This group exhibited a high degree of carbon unsaturation, as evident from high double bond equivalence minus oxygen values (DBE-O > 9) and maximum fluorescence intensity. Sulfur-containing molecular formulae for summer DOM samples were much more abundant across the entire transect of the STC compared to winter and exhibited distinctly different hydrogen:carbon and oxygen:carbon elemental ratios, suggesting a possible correlation between biological activity and sulfur compounds. The molecular formulae common to all STC samples were compared with those calculated for DOM extracted from freshwater collected from a stream discharging into Doubtful Sound (West Coast, New Zealand). ESI-FT-ICR-MS measurements undertaken in negative electrospray ionization (ESI?) mode indicated that 30% of the molecular formulae were present in both types of DOM, while in positive ESI mode (ESI+) over 90% of the formulae were present in all samples. Hence, a significant portion of the molecular formulae assigned to the solid-phase extractable DOM pool (SPE-DOM) appear to be identical in oceanic and freshwater samples.  相似文献   

5.
Results are presented from an investigation of the relationship between molecular mass distribution and optical properties for colored dissolved organic matter (CDOM); a complex assembly of organic macromolecules of marine and freshwater origin found throughout the surface ocean. Unique data are derived from the application of a new technique, a combination of a hydrophilic–lipophilic copolymer-based solid phase extraction (SPE) with electrospray ionization (ESI) continuous flowing ion trap mass spectrometry (cf-MS), for the direct determination of CDOM mass distribution. An evaluation of this copolymer-based extraction technique for the analysis of Suwannee River Natural Organic Matter (SRNOM) reference material revealed that the current method compares favorably with C18 modified silica or XAD resin-based extraction methods reported in the literature when considering extraction efficiency or low extraction bias for CDOM. The mass distribution of CDOM in several freshwater to marine transition zones along coastal southwestern Florida has been determined with this technique. All rivers in the study region had a bimodal distribution of masses. A case study of the Caloosahatchee River outflow CDOM mass distribution data are presented as an example of the modification in mass distributions. The lower mass mode of the bimodal distribution was observed to have a relatively stable mean throughout the study region at 406±9 Da, while decreasing in concentration in a non-conservative manner with salinity. In contrast, the upper mass mode of the bimodal distribution was observed to have a variable mean, reaching 1408 Da in the least saline waters and decreasing by 174 Da through the transect toward higher salinity coastal waters. Coinciding with this reduction in mean mass for the upper distribution is a non-conservative reduction in concentration when compared with salinity. We define apparent organic carbon (AOC) as a function of the cf-MS determined total integrated area and use this value to determine concentration of the total extracted CDOM. Unique correlations between the CDOM fluorescence (350-nm excitation/450-nm emission) and the AOC for these coastal samples have been observed for each of three rivers in the study region. The steepest slope and highest correlation between optical and mass spectral properties are observed in rivers with strongly absorbing waters originating in the Florida Everglades and lowest in rivers draining clearer waters from widely variable and anthropogenic influenced regions. The trends in molecular mass distribution and corresponding optical properties support the theory that CDOM in coastal zones is environmentally processed material from terrestrial sources. Probable cause of the reduction in mean mass and suggestions for further investigation of sources and transformations of CDOM are discussed.  相似文献   

6.
北极孔斯峡湾表层沉积物中溶解有机质的来源与转化历史   总被引：7，自引：0，他引：7  
在北极地区孔斯峡湾采集28个表层沉积物样品,测定了其中水溶性有机质(也称溶解有机质,DOM)的分子量分布、紫外/可见吸收光谱和三维荧光光谱特征,并利用平行因子分析(PARAFAC)模型对DOM的荧光组分和来源进行了解析。结果表明:孔斯峡湾表层沉积物中有色溶解有机质(CDOM)及其中的荧光溶解有机质(FDOM)含量均从内湾向外湾方向呈逐渐累积的趋势,但CDOM中的FDOM所占比例逐渐减小,与DOM趋于老龄化密切相关。沉积作用减弱以及长期的光化学降解和微生物降解作用对此起主要贡献,并导致腐殖质和小分子组分在沉积物DOM中所占的比例呈逐渐递增的趋势。沉积物DOM包含陆源类腐殖质、自生源类腐殖质和类蛋白等三个荧光组分,但是其组成比例空间差异很大。吸收光谱斜率比(SR)随自生源所占百分比增加而减小,随DOM腐殖质组分中陆源与自生源的比值增加而增加;腐殖化指数(HIX)随类腐殖质与类蛋白质比值和水深的增加而增加,生物源指数(BIX)随自生源比例增加而增加。峡湾沉积物DOM的组成和来源存在着高度的空间差异,在冰川湾区由水体颗粒有机质(POM)的近期转化和迁移而来,而在峡湾中央及口门附近以较老的腐殖质为优势,主要源于水体DOM长期迁移和转化。研究表明,FDOM/CDOM,SR,HIX和BIX等构成的CDOM光谱指纹信息可以作为揭露沉积物溶解有机质来源及迁移转化历史的工具,对探索海洋与冰川相互作用影响下的峡湾环境演变有着重要意义。  相似文献   

7.
Particulate matter from the atmosphere over the Atlantic Ocean along the South American and African Continents has been analyzed for organic tracers from natural and biomass burning emissions. The major biomarker compounds characterized are natural products from continental vegetation consisting primarily of epicuticular wax components. For example, n-alkanes ranged from C25 to C35, with an odd carbon number predominance and carbon maxima (Cmax) at 29 or 31. Concentrations of n-alkanes varied from 0.3 to 680 ng/m3. Nevertheless, n-alkanols are the dominant terrestrial tracers in almost all samples (concentrations from 0.1 to 780 ng/m3) and ranged from C22 to C34 with an even carbon number predominance. Despite the major presence of the natural tracers, organic components from biomass burning emissions are also present in the particulate matter. The major tracers from this source are thermal degradation products from the biopolymer cellulose, namely the dianhydromonosaccharide derivatives levoglucosan, galactosan, and mannosan. In general, the concentrations of levoglucosan, the major derivative from this source in all samples, varied from 0.0008 to 0.15 ng/m3 in atmospheric samples collected over the ocean and from 0.04 to 4860 ng/m3 in terrestrial particulate matter, used as reference in this study. Dehydroabietic acid, another marker compound emitted from burning of Gymnosperm fuel, is also detectable in most oceanic samples at concentrations ranging from 0.0001 to 0.4 ng/m3, whereas in terrestrial aerosol particulate matter, this component is present at much higher concentrations (0.23–440 ng/m3). The presence of these tracers in atmospheric particulate matter over the ocean confirms the long-range transport of smoke from biomass burning off the continents.  相似文献   

8.
Concurrent distributions of dissolved and suspended particulate organic carbon (DOC and POCsusp), nitrogen (DON and PONsusp) and phosphorus (DOP and POPsusp), and of suspended particulate inorganic phosphorus (PIPsusp), are presented for the open ocean water column. Samples were collected along a three-station transect from the upper continental slope to the abyssal plain in the eastern North Pacific and from a single station in the Southern Ocean. The elemental composition of surface sedimentary organic matter (SOM) was also measured at each location, and sinking particulate organic matter (POMsink) was measured with moored sediment traps over a 110-d period at the abyssal site in the eastern North Pacific only. In addition to elemental compositions, C : N, C : P and N : P ratios were also calculated. Surface and deep ocean concentrations of dissolved organic matter (DOM) and inorganic nutrients between the two sites displayed distinct differences, although suspended POM (POMsusp) concentrations were similar. Concentrations of DOM and POMsusp displayed unique C, N and P distributions, with POMsusp concentrations generally about 1–2 orders of magnitude less than the corresponding DOM concentrations. These differences were likely influenced by different biogeochemical factors: whereas the dissolved constituents may have been influenced more by the physical regime of the study site, suspended particulate matter may have been controlled to a greater extent by biological and chemical alteration. Up to 80% of total particulate P in POMsusp, POMsink and SOM consisted of PIP. For all organic matter pools measured, elemental ratios reveal that organic P is preferentially remineralized over organic C and organic N at both sites. Increases in C : P and N : P ratios with depth were also observed for DOM at both sites, suggesting that DOP is also preferentially degraded over C and N as a function of depth. A simple one-dimensional vertical eddy diffusion model was applied to estimate the contributions of dissolved and suspended particulate organic C, N and P fluxes from the upper mixed layer into the permanent thermocline. Estimated vertical DOM fluxes were 28–63% of the total organic matter fluxes; POMsusp and POMsink fluxes were 8–20 and 28–52% of the total.  相似文献   

9.
Temporal and spatial variations in the composition of particulate organic matter (POM) from Florida Bay, USA were examined. The predominance of short-chain homologues for n-alkanes, n-alcohols and n-fatty acids as well as relatively high abundance of C27 and C28 sterols suggested that an autochthonous/marine source of OM was dominant bay-wide. Several biomarker proxies such as Paq [(C23 + C25)/(C23 + C25 + C29 + C31) n-alkanes], short/long chain n-alkanes, (C29 + C31) n-alkanes and taraxerol indicated a spatial shift in OM sources, where terrestrial OM rapidly decreased while seagrass and microbial OM markedly increased along a northeastern to southwestern transect. Regarding seasonal variations, POM collected during the dry season was enriched in terrestrial constituents relative to the wet season, likely as a result of reduced primary productivity of planktonic species and seagrasses during the dry season. Principal component analysis (PCA) classified the sample set into sub-groups based on PC1 which seemed to be spatially controlled by OM origin (terrestrial-mangrove vs. marine-planktonic/seagrass). The PC2 seemed to be more seasonally controlled suggesting that hydrological fluctuations and seasonal primary productivity are the drivers controlling the POM composition in Florida Bay.  相似文献   

10.
Carbon overconsumption, i.e. the consumption of inorganic carbon relative to inorganic nitrogen in excess of the Redfield ratio at the sea surface, was examined in relation to the dynamics of dissolved organic carbon and nitrogen (DOC and DON) in the northeast Atlantic. We observed the presence of N-poor dissolved organic matter (DOM) in surface water during summer, requiring the consumption of inorganic carbon and nitrogen in a ratio exceeding the Redfield ratio. The C : N ratio of bulk DOM is not only different from the Redfield ratio but also variable, i.e. no fixed conversion factor of C and N exists where DOM is important in C and N transformations. The existence of N-poor DOM is recognized as a feature typical of oligotrophic systems. At the same time, the C : N ratios of particles conform to Redfield stoichiometry as does deep-ocean chemistry. The implications of this finding are discussed, the conclusion being that, while DOM buildup contributes to CO2 drawdown seasonally, its impact on long-term carbon and nitrogen balance of the ocean is small.  相似文献   

11.
《Marine Chemistry》2001,73(3-4):253-271
The influence of mangrove-fringed tropical estuaries on coastal carbon budgets has been widely recognised. However, a quantitative differentiation between riverine and mangrove-derived inputs to the dissolved (DOM) and microparticulate organic matter (POM) pool of these environments has been hitherto not possible. Based on lignin-derived phenols and stable carbon isotopes a chemical signature for mangrove, terrestrial and marine-derived organic matter was established for a mangrove estuary in North Brazil. A mixing model was applied to calculate the contribution of each of the three sources to the DOM and POM pool in the estuary throughout 18 tidal cycles in the course of one year. Best source assignment for POM was reached with the yield of lignin phenols and δ13C as paired indicators, while the origin of DOM was best identified by the yield of lignin phenols and the acid to aldehyde ratio of vanillyl phenols. Although only about 6% of the fluvial catchment area is covered by mangroves, their contribution to the estuarine DOM and POM pool generally exceeded several times the terrigenic input from the hinterland. This outwelling of mangrove-derived organic matter was enhanced during the rainy season. DOM and POM were exported from the mangrove to the estuary in similar proportions. Most mangrove-POM was rapidly removed from the water column, while mangrove-DOM behaved conservatively. In contrast, terrestrial DOM was almost entirely removed in the outer part of the estuary, which was accompanied by a concomitant increase in terrestrial POM. This seems to be the result of a geochemical barrier zone for this type of DOM in the estuary. Generally, a high proportion of mangrove-DOM was present in the outer part of the estuary, even at high tide. This indicates DOM outwelling from mangroves in adjacent bays or estuaries and points to similar driving forces controlling this process on a regional scale. Mangroves probably play a more important role than rivers for marine carbon budgets along the North Brazilian coast south of the Amazon estuary.  相似文献   

12.
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   

13.
Chromophoric dissolved organic matter (CDOM), as the light absorbing fraction of bulk dissolved organic matter (DOM), plays a number of important roles in the global and local biogeochemical cycling of dissolved organic carbon (DOC) and in controlling the optical properties of estuarine and coastal waters. Intertidal areas such as salt marshes can contribute significant amounts of the CDOM that is exported to the ocean, but the processes controlling this CDOM source are not well understood. In this study, we investigate the production of DOM and CDOM from the decomposition of two salt marsh cordgrasses, Spartina patens, a C4 grass, and Typha latifolia, a C3 grass, in well-controlled laboratory experiments. During the seven-week incubation period of the salt marsh grasses in oxic and anoxic seawater, changes in dissolved organic carbon (DOC) concentrations, dissolved nitrogen (DN) concentrations, stable carbon isotopic composition of DOC (DOC-δ13C), and CDOM fluorescence demonstrate a significant contribution of DOC and CDOM to estuarine waters from salt marsh plants, such as Spartina and Typha species. In the natural environment, however, the release processes of CDOM from different cordgrass species could be controlled largely by the in situ oxic and anoxic conditions present during degradation which affects both the production and decomposition of DOC and CDOM, as well as the optical properties of CDOM in estuarine and coastal waters.  相似文献   

14.
We investigated the composition, recycling, and mass accumulation rates of sediments along a transect in the Southern Ocean located from 66°S to 57°S at 170°W. This transect also corresponds to the location of a sediment trap mooring line. The sediments at the seven sites studied range from largely terrigenous material to nearly pure (>90%) biogenic silica. CaCO3 is a minor but persistent component at most sites. Mass accumulation rates have been determined on the basis of excess 230Th in the sediments, i.e., 230Th-normalized accumulation rates. The influence of redistribution of sediments on the sea floor has been estimated from 14C analyses. The recycling of material delivered to the sediments has been characterized on the basis of pore water studies that make extensive use of both in situ sampling and shipboard extractions. The influence of the highly variable rates of input of particulate matter that characterize much of the Southern Ocean upon pore water gradients and fluxes across the sediment water interface has been considered.We find only poor correspondence between BSiO2 burial fraction (=burial/particulate flux), a quantifiable measure of preservation efficiency, and BSiO2 particulate rain along the transect. However, preservation does appear to be closely linked to a combination of sedimentation rate and particulate rain.The burial fraction of BSiO2 is small relative to benthic rain (5–19%). Despite the small fraction buried, burial flux normalized to (sedimentation rate)1/2 appears to provide a very consistent means of predicting benthic particulate rain over a large range of rain rates, including data from a number of different studies and environments. At sites with BSiO2 rain 250 mmol m−2 yr−1 the average difference between predicted and observed rain is 25–30%. Such rain rates occur in many marine areas, particularly the Southern Ocean, with the result that this relationship potentially provides a means of estimating BSiO2 benthic rain over prolonged periods in the past on the basis of readily measured sediment parameters.At the southern-most deep ocean station, the particulate flux was characterized by an extremely high Corg/CaCO3 ratio (>10), but this high ratio does not appear to have a substantial influence on CaCO3 burial. CaCO3 is preserved in the sediments at this site despite a particulate flux with a 10-fold excess of Corg above that required for complete dissolution in the sediments. The unexpectedly high preservation of CaCO3 is due largely to the very steep Corg oxidation rate profile at this site. As a result, a large fraction of the organic matter oxidized in the sediments does so in close proximity to the sediment–water interface where most of the metabolic CO2 is neutralized by CO32− from the overlying water, rather than by the dissolution of sedimentary CaCO3.Diagenetic modeling indicates that at several of the stations, the remineralization fluxes of carbonate species across the sediment–water interface may not have been at steady state as a result of the highly pulsed nature of particulate rain in this environment. We estimate that at the time of our sampling it is possible that near-interface fluxes could have been a factor of 1.6–2 times the annual average.At every site on the transect, the burial fluxes of detrital material are substantially greater than the detrital particulate rain measured in the sediment traps, by as much as a factor of 40. Detrital burial is bimodal, being greatest at the southern and northern extremes of the transect. We postulate that the excess of burial over particulate rain in the south reflects the contribution of ice rafted debris at these high latitudes. Increases in the supply at the northern stations must have a different source. We believe that the excess at these stations is material eroded from the sea floor to the west, possibly on the Campbell Plateau, and advected by currents to the northern portion of the transect at depths below the shallow traps.  相似文献   

15.
The direct injection of CO2 in the deep ocean is a promising way to mitigate global warming. One of the uncertainties in this method, however, is its impact on marine organisms in the near field before CO2 is diluted widely in the ocean. Since field experiments cost enormously, computational simulations are expected to show detailed information on the dilution process near injection points and its impact on marine organisms. In general, the LC50 concept is widely applied for testing the acute impact of a toxic agent on organisms. As a biological impact model we therefore consider mortality, which reflects recent laboratory experiments on zooplankton at various concentrations of CO2. Here we regard the sigmoid-transformed mortality as a linear function of time in the logarithmic scale, and not just of the concentration of CO2 in the logarithmic scale. This model was installed in a computational simulation code for the reconstruction of small-scale ocean turbulence. The results suggest that the biological effect is not significant when the ship speed is 4 knots and CO2 is injected at 0.1 ton/sec in the form of a spray through 100 nozzles provided vertically on a pipe at 10 m intervals. It is therefore considered that the moving-ship method is effective for direct CO2 injection. This revised version was published online in July 2006 with corrections to the Cover Date.  相似文献   

16.
The stable carbon isotopic composition of particulate organic matter in the ocean, δ13CPOC, shows characteristic spatial variations with high values in low latitudes and low values in high latitudes. The lowest δ13CPOC values (−32‰ to −35‰) have been reported in the Southern Ocean, whereas in arctic and subarctic regions δ13CPOC values do not drop below −27‰. This interhemispheric asymmetry is still unexplained. Global gradients in δ13CPOC are much greater than in δ13CDIC, suggesting that variations in isotopic fractionation during organic matter production are primarily responsible for the observed range in δ13CPOC. Understanding the factors that control isotope variability is a prerequisite when applying δ13CPOC to the study of marine carbon biogeochemistry. The present model study attempts to reproduce the δ13CPOC distribution pattern in the ocean. The three-dimensional (3D) Hamburg Model of the Oceanic Carbon Cycle version 3.1 (HAMOCC3.1) was combined with two different parametrizations of the biological fractionation of stable carbon isotopes. In the first parametrization, it is assumed that the isotopic fractionation between CO2 in seawater and the organic material produced by algae, P, is a function of the ambient CO2 concentration. The two parameters of this function are derived from observations and are not based on an assumption of any specific mechanism. Thus, this parametrization is purely empirical. The second parametrization is based on fractionation models for microalgae. It is supported by several laboratory experiments. Here the fractionation, P, depends on the CO2 concentration in seawater and on the (instantaneous) growth rates, μi, of the phytoplankton. In the Atlantic Ocean, where most field data are available, both parametrizations reproduce the latitudinal variability of the mean δ13CPOC distribution. The interhemispheric asymmetry of δ13CPOC can mostly be attributed to the interhemispheric asymmetry of CO2 concentration in the water. However, the strong seasonal variations of δ13CPOC as reported by several authors, can only be explained by a growth rate-dependent fractionation, which reflects variations in the cellular carbon demand.  相似文献   

17.
由于海水盐度大、有机质含量低,从海水中提取和纯化克级溶解性有机质(dissolved organic matter,DOM)一直十分困难。基于Bond Elut PPL固相萃取小柱法进行海水DOM固体样品提取的放大试验,建立DOM自动化调酸、PPL树脂吸附技术,最后形成提纯、冷冻干燥PPL-DOM(通过PPL树脂提取的DOM)完整工艺。采用元素分析、三维荧光光谱、红外光谱和固态13C核磁共振(NMR)波谱法进行样品表征。结果表明:(1)该方法对近海表层海水DOM回收率稳定在50%以上,搭建的提取装置DOM日吸附量可达230mg;(2)鳌山湾四个季节批次PPL-DOM整体分析结果表明,样品的元素组成和光谱特征相似,表明方法适用性和稳定性较好;(3)三种水生态环境的PPL-DOM13C NMR谱图显示样品的基本特征相似,以烷基碳、碳水化合物碳、芳香碳和羧基碳/酰胺碳为主,其中偶极去相(dipolar dephasing)谱显示了DOM前体化合物来源的差异。多种结果表明放大后的PPL固相萃取法可稳定提取克级DOM样品。  相似文献   

18.
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   

19.
Fluorescent dissolved organic matter (DOM), a fraction of chromophoric DOM, is known to be produced in the deep ocean and is considered to be bio-refractory. However, the factors controlling fluorescence properties of DOM in the deep ocean are still not well understood. In this study, we determined the fluorescence properties of DOM in the deep waters of the Okhotsk Sea and the northwestern North Pacific Ocean using excitation-emission matrix (EEM) fluorescence and parallel factor analysis (PARAFAC). One protein-like, two humic-like components, and one uncertain component, which might be derived from a fluorometer artifact, were identified by EEM-PARAFAC. Fluorescence intensity levels of the protein-like component were highest in the surface waters, decreased with depth, but did not change systematically in the bathypelagic layer (1000 m - bottom). Fluorescence characteristics of the two humic-like components were similar to those traditionally defined as marine and terrestrial humic-like fluorophores. The fluorescence intensity levels of the two humic-like components were lowest in the surface waters, increased with depth in the mesopelagic layer (200 - 1000 m), and then slightly decreased with depth in the bathypelagic layer. The ratio of the two humic-like components remained in a relatively narrow range in the bathypelagic layer compared to that in the surface layer, suggesting a similar composition of humic-like fluorophores in the bathypelagic layer. In addition, the fluorescence intensities of the two humic-like components were linearly correlated to apparent oxygen utilization (AOU) in the bathypelagic layer, suggesting that both humic-like components are produced in situ as organic matter is oxidized biologically. These findings imply that optical characteristics of humic-like fluorophores once formed might not be altered further biologically or geochemically in the deep ocean. On the other hand, relationships of fluorescence intensities with AOU and Fe(III) solubility were different between the two humic-like components in the mesopelagic layer, suggesting different environmental dynamics and biogeochemical roles for the two humic-like components.  相似文献   

20.
Wax esters (ranging from C32 to C44), very long mid-chain ketones (ranging from C31 to C43) and sterol ethers were isolated from Walvis Bay diatomaceous ooze and identified by glass capillary gas chromatography/mass spectrometry and direct probe high-resolution mass spectrometry.The wax ester compositions of co-eluting wax esters with the same molecular weight were determined from fragment ions characteristic for the alcohol and fatty acid moieties. Dominant wax esters are the C3(16F-20A), C36(18F-18A), C38(16F-22A), C38(18F-20A), C40(18F-22A), C40(20F-20A) and C40(24F-16A).The presence of isoprenoid wax esters and the chain length distributions of alcohol and fatty acid moieties point to an origin from zooplankton. The position of the ketogroup in the mid-chain ketones is determined from characteristic fragment ions. Major ketones are the C38(C18H37-CO-C19H39) and C40(C18H37-CO-C21H43).The sterol ethers have C8 and C9 ether moieties and C27, C28, and C29 steroid moieties. The origin and significance of the ketones and the sterol ethers is obscure.  相似文献   

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