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1.
The molecular and carbon isotopic compositions of polar isopranyl glycerol ether lipids, which are direct indicators of viable archaea, and neutral isopranyl glycerol ether lipids, which are derived from polar lipids via hydrolysis, in near-surface sediments from a methane seep in the Nankai Trough (off central Japan) were investigated. Procedures for extracting, separating and derivatizing polar and neutral ether lipids for detection using gas chromatography were first examined with one sediment sample and a cultivated methanogen. For all sediment samples, archaeol and hydroxyarchaeol were detected in both the polar and neutral ether lipid fractions. Acyclic and cyclic biphytanes were also detected in both types of lipid fractions after treatment with HI/LiAlH4 for ether cleavage and alkylation. The δ13C values of archaeol, sn-2-hydroxyarchaeol, and sn-3-hydroxyarchaeol in the sample from 0.82 m below the seafloor were lower than −100‰ relative to PDB, indicating that diverse living methanotrophic archaea are present in the seep sediments. Biphytanes released from polar ether lipids in the same sample were less depleted in δ13C (−71‰ to −36‰). The wide range of δ13C values suggests that the biphytanes were derived not only from methanotrophic but also from non-methanotrophic archaea, and that the relative contributions of the methanotrophic and non-methanotrophic archaea differed, depending on the biphytane compound. The vertical profiles and δ13C values of the neutral ether lipids were similar to those of the intact polar ether lipids, suggesting that neutral ether lipids derived from fossil archaea in the samples had mainly been lost by the time of sampling.  相似文献   

2.
We report the presence of coenzyme factor 430 (F430), a prosthetic group of methyl coenzyme M reductase for archaeal methanogenesis, in the deep sub-seafloor biosphere. At 106.7 m depth in sediment collected off Shimokita Peninsula, northwestern Pacific, its concentration was estimated to be at least 40 fmol g sediment−1 (i.e. 36 pg g−1 wet sediment). This is about three orders of magnitude lower than typical concentrations of archaeal intact polar lipids in similar sub-seafloor sediments. On the basis of the concentration of F430 in methanogens and conversion to biomass composed of typical sub-seafloor microbial cells, we estimated that ca. 2 × 106 cells g−1 could be methanogens in the deeply buried marine sediment.  相似文献   

3.
In order to develop new tools in the reconstruction of microbiological processes in ancient continental settings, we determined the concentration of archaeol and sn-2-hydroxyarchaeol in four Holocene ombrotrophic peatlands, spanning a range of European climate zones. Neither ether lipid was present in the aerobic acrotelm peat, consistent with an origin from anaerobic archaea, presumably methanogens. At the depth of the maximum seasonal water table, archaeol and sn-2-hydroxyarchaeol concentration markedly increased at all four sites, again consistent with an anaerobic source, but differed strongly among sites. The differences apparently reflect a combination of vegetation - ericaceous and graminoid plants as opposed to Sphagnum spp. and other mosses lacking root systems - and temperature influence on methanogenesis. In particular, low ether lipid concentrations in Finland probably reflect the lack of vascular vegetation possessing well-developed root systems, together with low mean annual temperature. Similarly low concentrations of archaeol and sn-2-hydroxyarchaeol in a German bog likely result from winter temperatures below 0 °C and a relatively shorter growing season. The occurrence of sn-2-hydroxyarchaeol is limited to a narrow and shallow depth range, indicating that it is poorly preserved, but archaeol persists throughout the cores. Decoupling the concentration of archaeol and the more labile sn-2-hydroxyarchaeol below ca. 50 cm suggests that the former records fossil biomass rather than living biomass. If so, then downcore variation in archaeol concentration likely reflects past changes in methane cycling, and archaeol, pending further developmental research, could serve as a new tool for reconstruction of past peatland biogeochemistry.  相似文献   

4.
Convergent lines of molecular, carbon-isotopic, and phylogenetic evidence have previously indicated (Hinrichs, K.-U., Hayes, J.M., Sylva, S.P., Brewer, P.G., DeLong, E.F., 1999. Methane-consuming archaebacteria in marine sediments. Nature 398, 802–805.) that archaea are involved in the anaerobic oxidation of methane in sediments from the Eel River Basin, offshore northern California. Now, further studies of those same sediments and of sediments from a methane seep in the Santa Barbara Basin have confirmed and extended those results. Mass spectrometric and chromatographic analyses of an authentic standard of sn-2-hydroxyarchaeol (hydroxylated at C-3 in the sn-2 phytanyl moiety) have confirmed our previous, tentative identification of this compound but shown that the previously examined product was the mono-TMS, rather than di-TMS, derivative. Further analyses of 13C-depleted lipids, appreciably more abundant in samples from the Santa Barbara Basin, have shown that the archaeal lipids are accompanied by two sets of products that are only slightly less depleted in 13C. These are additional glycerol ethers and fatty acids. The alkyl substituents in the ethers (mostly monoethers, with some diethers) are non-isoprenoidal. The carbon-number distributions and isotopic compositions of the alkyl substituents and of the fatty acids are similar, suggesting strongly that they are produced by the same organisms. Their structures, n-alkyl and methyl-branched n-alkyl, require a bacterial rather than archaeal source. The non-isoprenoidal glycerol ethers are novel constituents in marine sediments but have been previously reported in thermophilic, sulfate- and nitrate-reducing organisms which lie near the base of the rRNA-based phylogenetic tree. Based on previous observations that the anaerobic oxidation of methane involves a net transfer of electrons from methane to sulfate, it appears likely that the non-archaeal, 13C-depleted lipids are products of one or more previously unknown sulfate-reducing bacteria which grow syntrophically with the methane-utilizing archaea. Their products account for 50% of the fatty acids in the sample from the Santa Barbara Basin. At all methane-seep sites examined, the preservation of aquatic products is apparently enhanced because the methane-oxidizing consortium utilizes much of the sulfate that would otherwise be available for remineralization of materials from the water column.  相似文献   

5.
At the Chapopote Knoll in the Southern Gulf of Mexico, deposits of asphalt provide the substrate for a prolific cold seep ecosystem extensively colonized by chemosynthetic communities. This study investigates microbial life and associated biological processes within the asphalts and surrounding oil-impregnated sediments by analysis of intact polar membrane lipids (IPLs), petroleum hydrocarbons and stable carbon isotopic compositions (δ13C) of hydrocarbon gases. Asphalt samples are lightly to heavily biodegraded suggesting that petroleum-derived hydrocarbons serve as substrates for the chemosynthetic communities. Accordingly, detection of bacterial diester and diether phospholipids in asphalt samples containing finely dispersed gas hydrate suggests the presence of hydrocarbon-degrading bacteria. Biological methanogenesis contributes a substantial fraction to the methane captured as hydrate in the shallow asphalt deposits evidenced by significant depletion in 13C relative to background thermogenic methane. In sediments, petroleum migrating from the subsurface stimulates both methanogenesis and methanotrophy at a sulfate-methane transition zone 6-7 m below the seafloor. In this zone, microbial IPLs are dominated by archaeal phosphohydroxyarchaeols and archaeal diglycosidic diethers and tetraethers. Bacterial IPLs dominate surface sediments that are impregnated by severely biodegraded oil. In the sulfate-reduction zone, diagnostic IPLs indicate that sulfate-reducing bacteria (SRB) play an important role in petroleum degradation. A diverse mixture of phosphohydroxyarchaeols and mixed phospho- and diglycosidic archaeal tetraethers in shallow oil-impregnated sediments point to the presence of anaerobic methane-oxidizing ANME-2 and ANME-1 archaea, respectively, or methanogens. Archaeal IPLs increase in relative abundance with increasing sediment depth and decreasing sulfate concentrations, accompanied by a shift of archaeol-based to tetraether-based archaeal IPLs. The latter shift is suggested to be indicative of a community shift from ANME-2 and/or methanogenic archaea in shallower sediments to ANME-1/methanogenic archaea and possibly benthic archaea in deeper sediments.  相似文献   

6.
Detailed knowledge of the extent of post-genetic modifications affecting shallow submarine hydrocarbons fueled from the deep subsurface is fundamental for evaluating source and reservoir properties. We investigated gases from a submarine high-flux seepage site in the anoxic Eastern Black Sea in order to elucidate molecular and isotopic alterations of low-molecular-weight hydrocarbons (LMWHC) associated with upward migration through the sediment and precipitation of shallow gas hydrates. For this, near-surface sediment pressure cores and free gas venting from the seafloor were collected using autoclave technology at the Batumi seep area at 845 m water depth within the gas hydrate stability zone.Vent gas, gas from pressure core degassing, and from hydrate dissociation were strongly dominated by methane (> 99.85 mol.% of ∑[C1–C4, CO2]). Molecular ratios of LMWHC (C1/[C2 + C3] > 1000) and stable isotopic compositions of methane (δ13C = ? 53.5‰ V-PDB; D/H around ? 175‰ SMOW) indicated predominant microbial methane formation. C1/C2+ ratios and stable isotopic compositions of LMWHC distinguished three gas types prevailing in the seepage area. Vent gas discharged into bottom waters was depleted in methane by > 0.03 mol.% (∑[C1–C4, CO2]) relative to the other gas types and the virtual lack of 14C–CH4 indicated a negligible input of methane from degradation of fresh organic matter. Of all gas types analyzed, vent gas was least affected by molecular fractionation, thus, its origin from the deep subsurface rather than from decomposing hydrates in near-surface sediments is likely.As a result of the anaerobic oxidation of methane, LMWHC in pressure cores in top sediments included smaller methane fractions [0.03 mol.% ∑(C1–C4, CO2)] than gas released from pressure cores of more deeply buried sediments, where the fraction of methane was maximal due to its preferential incorporation in hydrate lattices. No indications for stable carbon isotopic fractionations of methane during hydrate crystallization from vent gas were found. Enrichments of 14C–CH4 (1.4 pMC) in short cores relative to lower abundances (max. 0.6 pMC) in gas from long cores and gas hydrates substantiates recent methanogenesis utilizing modern organic matter deposited in top sediments of this high-flux hydrocarbon seep area.  相似文献   

7.
This study focuses on the morphometry and taxonomy of the Late Cretaceous coccolith genus Arkhangelskiella. Sixty samples from the Campanian–Maastrichtian interval of DSDP Hole 390A (Blake Nose) were investigated for their contents of Arkhangelskiella spp. In each sample one hundred specimens of Arkhangelskiella spp. were examined by measuring the coccolith length and width, as well as the length and width of the central area. In the samples investigated the Arkhangelskiella group exhibits a large size variation, specimens length varies from 4.95 μm to 14.52 μm. Former taxonomic concepts, based on morphometry, subdivided the Arkhangelskiella group into three species: Arkhangelskiella maastrichtiana, Arkhangelskiella confusa and Arkhangelskiella cymbiformis. Our data show a large variability of the morphometric data (coccolith length, width of the outer rim). There is no indication for three independant species; two of the quoted taxa (1. thick outer rim = Arkhangelskiella maastrichtiana; 2. very thin outer rim = Arkkhangelskiella cymbiformis) seem to be extreme forms of a continuous morphometric lineage. The lower part of the investigated succession (139.92–133.42 mbsf) is dominated by small specimens with an average length of 6.8 μm whereas the upper part (132.86–126.15 mbsf) is characterized by larger specimens (mean 8.7 μm). In DSDP Hole 390A the size increase appears to be very abrupt, within two samples (samples 133.42 mbsf, 132.86 mbsf) the mean size increases by 1.51 μm. Previous morphometric studies of Arkhangelskiella indicate a more continuous size increase throughout the late Campanian–Maastrichtian. The abrupt size increase observed here hints toward a minor hiatus in DSDP Hole 390A separating upper Campanian from lower Maastrichtian sediments. It seems likely that the size increase of Arkhangelskiella reflects changes of various environmental factors like nutrient supply and sea water chemistry (Mg/Ca ratio; Ca concentration). A comparison of morphometric results with previous palaeoecological studies documents a nutrient control for the growth of Arkhangelskiella. Small specimens can be related to more mesotrophic conditions whereas large specimens are linked to oligotrophic surface waters.  相似文献   

8.
Authigenesis of iron-rich phosphate nodules occurs in iron-rich cold-seep sediments (MD052911 core) at Yung-An Ridge offshore southwestern Taiwan. Raman, FTIR, and quantitative X-ray energy-dispersive spectroscopic analyses indicate that the phosphate mineral is vivianite (or barićite) and shows Fe/Mg molar ratios spanning from ca. 0.6 to 4.0 and a general down core trend of increasing Fe/Mg ratios. The formation of vivianite is limited to a depth interval of 13–17 mbsf (meters below seafloor) and is most prominent at ∼16 mbsf in association with high dissolved iron concentrations and depleted dissolved sulfide below a peak sulfidization zone (enriched in mackinawite and greigite). Alternate growths of vivianite and iron monosulfides and compositional zoning with Mg enriched towards the peripheries of individual nodules occur in the transition from the zone of vivianite mineralization to the sulfidization zone. The crystallization of vivianite below the sulfidization front could have been favored by scavenging of downward diffusive dissolved sulfide from pore waters in the sulfidization zone. Alternate growths and overlapping of the zones of iron monosulfides and vivianite can be attributed to fluctuations of the sulfidization front and methane flux. The discovery of vivianite in the Yung-An Ridge sediments implies that authigenic vivianite can be an important sink for phosphorus burial in cold-seep sediments that have high reactive-iron contents and high sedimentation rates.  相似文献   

9.
The saturated and unsaturated hydrocarbons of two samples (HD-19 and HD-21) from the same section of the Middle Eocene lacustrine Huadian oil shale in NE China were identified and shown to be mainly from algal and bacterial sources. Comparison of the two samples provided an opportunity to explore the contribution from telalginite to the hydrocarbon profiles. Cells identified from microscopy as Botryococcus in the telalginite of HD-21 were confirmed as belonging to the L race of B. braunii from the presence of monoaromatic lycopane derivatives and small amounts of several lycopadienes. Lycopane was abundant and was probably derived from biohydrogenation of lycopadienes and related lipids on the basis of δ13C values. Hopane distributions showed a dominance of those with the biological 17β,21β-stereochemistry, as expected for an immature shale, with low amounts of 17β,21α-hopanes (moretanes) and 17α,21β-hopanes. Two hopenes were also abundant and assigned as C29 and C30 neohop-13(18)-enes, which occurred together with the C29 and C30 hop-17(21)-enes. These had depleted carbon isotope values (−43.7‰ to −50.8‰), indicative of production by methane oxidizing bacteria (methanotrophs). The high proportion of hopanoids with carbon numbers < C32 indicates extensive post-depositional diagenetic alteration of bacteriohopanepolyols as well as a direct input of C30 hopanoids. The data clearly indicate that there was active utilization of methane in this lacustrine depositional setting, but isoprenoid hydrocarbon biomarkers for methanogens, such as pentamethylicosane (PMI) and squalane, were in surprisingly low abundance. It is possible that these bacterial contributions were present as polar lipids. The origins of an unusual C38 isoprenoid alkane assigned as bipristane are uncertain, but may be from methanogens. Steranes and sterenes were relatively minor components, but abundant diasterenes and 4-methyldiasterenes were present, reflecting significant conversion of the original lipid composition by way of clay-catalysed diagenesis. The biomarker data suggest that the bottom waters in the original depositional environment had low O2 content, but the sediments were probably neither sulfidic nor strongly reducing. The high content of organic matter in the shale likely reflects both high (but fluctuating) productivity due to eutrophic conditions in the overlying water and good preservation in the sediments.  相似文献   

10.
Structural diversity and fate of intact polar lipids in marine sediments   总被引：1，自引：0，他引：1  
Marine sediments harbor an enormous quantity of microorganisms, including a multitude of novel species. The habitable zone of the marine sediment column begins at the sediment-water interface and probably extends to depths of several thousands of meters. Studies of the microbial diversity in this ecosystem have mostly relied on molecular biological techniques. We used a complementary method - analysis of intact polar membrane lipids - to characterize the in-situ microbial community in sediments covering a wide range of environmental conditions from Peru Margin, Equatorial Pacific, Hydrate Ridge, and Juan de Fuca Ridge. Bacterial and eukaryotic phospholipids were only detected in surface sediments from the Peru Margin. In contrast, deeply buried sediments, independent of their geographic location, were dominated by archaeal diether and tetraether lipids with various polar head groups and core lipids. We compared ring distributions of archaeal tetraether lipids derived from polar glycosidic precursors with those that are present as core lipids. The distributions of these related compound pools were distinct, suggestive of different archaeal sources, i.e., the polar compounds derive from sedimentary communities and the core lipids are fossil remnants from planktonic communities with possible admixtures of decayed sedimentary archaea. This in-situ production of distinct archaeal lipid populations potentially affects applications of the TEX86 paleotemperature proxy as demonstrated by offsets in reconstructed temperatures between both pools. We evaluated how varying cell and lipid stabilities will influence the sedimentary pool by using a box-model. The results are consistent with (i) a requirement of continuous inputs of freshly synthesized lipids in subsurface sediments for explaining the observed distribution of intact polar lipids, and (ii) decreasing lipid inputs with increasing burial depth.  相似文献   

11.
Glycerol ether lipid distributions have been developed as proxies for reconstructing past environmental change or, in their intact polar form, for fingerprinting the viable microbial community composition. However, due to their structural complexity, full characterization of glycerol ether lipids requires separate protocols for the analysis of the polar head groups and the alkyl chain moieties in core ether lipids. As a consequence, the valuable relationship between core ether lipid composition and specific polar head groups is often lost; this limits understanding of the diversity of ether lipids and their utility as biogeochemical proxies. Here, we report a novel reversed phase liquid chromatography–electrospray ionization-mass spectrometry (RP-ESI-MS) protocol that enables the simultaneous analysis of polar head groups (e.g. phosphocholine, phosphoglycerol, phosphoinositol, hexose and dihexose) and alkyl moieties (e.g. alkyl moieties modified with different numbers of cycloalkyl moieties, hydroxyl and alkyl groups and double bonds) in crude lipid extracts without further preparation. The protocol greatly enhances detection of archaeal intact polar lipids (IPLs) and core lipids (CLs) with double bond- and hydroxyl group-bearing alkyl moieties. With these improvements, widely used ratios that describe relative distributions of the core lipids, such as TEX86 and ring index, can now be directly determined in specific intact polar lipids (IPL-specific TEX86 and ring index). Since IPLs are the putative precursors of the environmentally persistent core lipids, their detailed examination using this protocol can potentially provide new insights into diagenetic and biological mechanisms inherent to these proxies. In a series of 12 samples from diverse settings, core and IPL-specific TEX86 values followed the order: 2G-GDGTs > core GDGTs > 1G-GDGTs > 1G-GDGT-PI and the ring indices followed: 1G-GDGTs ≈ core GDGTs > 2G-GDGTs > 1G-GDGT-P1G > 2G-OH-GDGTs ≈ 1G-OH-GDGTs (1G, monoglycosyl; 2G, diglycosyl; P1G, phosphomonoglycosyl; GDGT, glycerol dialkyl glycerol tetraether).  相似文献   

12.
Porewater advection stimulates nutrient exchange and microbial activity in shallow marine sediments, whereas element cycling in deeper diffusion-dominated sediments is comparatively slow due to limited nutrient supply. We studied the vertical distribution of microbial communities and organic matter (OM) cycling in these contrasting porewater regimes down to 5 m depth at an intertidal flat of the southern North Sea. Archaea, Bacteria and Eukarya were targeted, combining intact polar lipid (IPL) analysis with qualitative and quantitative molecular biological techniques. The largely sandy section 1 of the core (<75 cm) is characterized by rapid burial of fresh marine OM and intense porewater advection. This supply fuels heterotrophic microbes, as evident from the 13C isotopic composition of total organic carbon and IPL derivatives. Major sources of OM are algae and cyanobacteria, as suggested by the elevated amount of eukaryotic 18S rRNA gene copies and phosphate-free IPLs. The relative abundance of most phospholipids remained largely constant over the entire core, except for diphosphatidylglycerol, which represented about half of total IPL abundance in the lower part of section 1 (>50 cm) and the diffusion-dominated section 2 (75–490 cm). This suggests bacteria adapting their membranes in response to increasing physicochemical stress and starvation in the nutrient limited, fine grained sediments of section 2 with less bioavailable, predominantly terrestrial, OM. Relative amounts of bacterial acyl ether and diether phospholipids increased in this lower section and were assigned to sulfate reducers and yet uncultured myxobacteria. Archaea were an order of magnitude less abundant than Bacteria, and were affiliated mainly with Methanosarcinales and Methanomicrobiales. Accordingly, the archaeal IPL composition was typical for a methanogenic community. IPLs not exclusively derived from in situ microbial production emphasize that these biomarkers have to be interpreted with caution in sediments with complex hydrogeology. Our results demonstrate that contrasting subsurface flow regimes significantly impact on the vertical zonation of biogeochemical properties and microorganisms in marine sediments.  相似文献   

13.
We investigated the distribution of lipids in Lower Triassic sedimentary rocks (252–247 myr) from South China, including a shallow water microbialite in the uppermost section of the outcrop. Archaeal derived hydrocarbons were the major constituents of the microbialite from the latest Early Triassic. Among these, we detected (i) abundant C40 acyclic and monocyclic biphytanes (possibly derived from glycerol dialkyl glycerol tetraether lipids) and their degradation products, C30–39 pseudohomologues and (ii) a C25 head-to-tail linked (regular) isoprenoid hydrocarbon [possibly derived from dialkyl glycerol diether lipids (DGDs)] and its degradation products, C21–24 pseudohomologues and abundant pristane and phytane. Through combination of compound-specific stable carbon isotope analysis of isoprenoid hydrocarbons, which had average δ13C values of −35‰ to −30‰, and their molecular distribution, it was not possible to unambiguously define the archaeal source for the biphytanes in the microbialite. The δ13C values for pristane and phytane were similar to those for head-to-tail linked C21–25 isoprenoids; potential source organisms for these compounds were halophilic archaea. Except for methane seep microbialites, no other ancient or recent phototrophic microbialites have been reported to contain predominantly archaeal isoprenoid hydrocarbons. Our findings suggest the presence of a new type of microbialite.  相似文献   

14.
We studied the distribution of glycerol dialkyl glycerol tetraethers (GDGTs) in suspended particulate matter from the water column of Lake Tanganyika (East Africa), where sediment studies had shown the applicability of the TEX86 proxy for reconstructing surface lake water temperature. GDGTs, in particular crenarchaeol, showed maximum abundance within the suboxic zone (100–180 m), suggesting that this is the preferred niche of ammonia-oxidizing Thaumarchaeota. Despite evidence for anaerobic methane oxidation in deep anoxic water (300–1200 m) no unambiguous evidence for an imprint of methanotrophic archaea on GDGT distribution was found. Comparison of TEX86 and BIT indices with those of surface sediments suggests that the sedimentary GDGTs are derived predominantly from the oxic zone and suboxic zone of the lake.  相似文献   

15.
《Chemical Geology》2007,236(3-4):350-366
A gas hydrate field with highly active venting of methane was recently found near Sado Island in the eastern Japan Sea. Piston cores were collected from active venting sites and nearby locations in the Umitaka Spur–Joetsu Knoll area during two cruises in 2004 (UT04) and 2005 (KY05-08). We report here halogen concentrations and 129I/I ratios in pore waters associated with gas hydrates from these expeditions. The strongly biophilic behavior of I and, to a lesser degree, of Br together with the presence of the long-lived iodine radioisotope (129I) allow evaluation of potential source materials for methane in gas hydrate systems. Depth profiles of all three halogens, particularly the very rapid downward increases of Br and I concentrations, strongly suggest input of deep fluids enriched in Br and I, but the profiles also display the effects of gas hydrate formation and dissociation. Although the 129I/I ratios are modified by 129I from seawater and sediments at shallow depth, likely ratios of the deep fluids are estimated to be between 400 × 10− 15 and 600 × 10− 15, equivalent to a Late Oligocene to Early Miocene age. Ages in the active methane venting sites typically are closer to the old end of this range than those in the reference sites. This age range suggests that the methane associated with venting and gas hydrate formation in this area is derived from organic materials accumulated during the initial opening of the Japan Sea. The Umitaka Spur–Joetsu Knoll gas hydrate field demonstrates the movement of deep fluids associated with the release of significant amounts of methane from the seafloor, processes which might be important components of mass transfer and carbon cycle in the shallow geosphere.  相似文献   

16.
Ether lipids such as non-isoprenoid mono and dialkyl glycerol ethers (MAGEs and DAGEs) and archaeol have been found in carbonate rocks and mud rocks deposited during the Early and Middle Triassic (250–240 Ma). The oldest previous discovery of ether lipids is from Cretaceous black shale deposited during the Albian (112 Ma). Paleoenvironmental reconstruction using ether lipids has therefore not been conducted on pre-Cretaceous sediments. Archaeol derives from archaea (e.g. methanogenic, methanotrophic, halophilic and thermophilic archaea). The non-isoprenoid DAGEs and MAGEs likely derive from sulfate-reducing bacteria (SRB), which are restricted to anaerobic environments. The presence of ether lipids thus indicates that anoxic conditions expanded in the depositional and/or water column environment in the Qingyan area during the Early–Middle Triassic. These ether lipids may be useful for the reconstruction of paleoredox conditions and paleoecosystems in the area. Furthermore, their occurrence suggests that paleoenvironmental reconstruction using ether lipids may be possible throughout the Mesozoic and Cenozoic.  相似文献   

17.
Although rates and mechanisms of early diagenesis have been well studied, the effects of microbial metabolism on the molecular composition of the sedimentary organic matter (SOM) over long periods of time need more investigation. In this study, we characterize the early diagenesis of marine SOM from organic rich sediments of the Ocean Drilling Program site 1082 located off Namibia, in the vicinity of the Benguela coastal upwelling system. We used both Fourier transform infrared spectroscopy (FTIR) and nuclear magnetic resonance spectroscopy (13C NMR) to assess the quantitative partitioning of the organic carbon into major compound classes (aliphatic, aromatic, ester, carboxylic, amide and carbons from carbohydrates). Then, we calculate the SOM composition in the main biomolecules (proteins, carbohydrates, lipids and lignin) on the basis of previous 13C NMR based estimates of the molecular composition of the organic mixtures. Results show that the SOM is still labile at 7 m below the seafloor (mbsf) and composed of about 25% proteins and 15% carbohydrates. With increasing depth, the protein content exponentially decreases to 13% at 367 mbsf, whereas the carbohydrate content decreases linearly to 11%. The lignin and lipid content consistently represent around 10% and 40% of the SOM, respectively, and show an increase with depth, due mostly to selective enrichment as the more labile components are lost by degradation. Thus, these components of the SOM are considered refractory at the depth scale considered. The calculated remineralization rates are extremely slow ranging from 5.6 mol C m−3 ky−1 at the top of the core to 0.2 mol C m−3 ky−1 according to the organic carbon flux to the seafloor. Knowing the labile carbon losses, we propose a method to calculate the initial TOC before the diagenesis took place.  相似文献   

18.
Seepage of asphalt forms the basis of a cold seep system at 3000 m water depth at the Chapopote Knoll in the southern Gulf of Mexico. Anaerobic microbial communities are stimulated in the oil-impregnated sediments as evidenced by the presence of intact polar membrane lipids (IPLs) derived from archaea and Bacteria at depths up to 7 m below the seafloor. Detailed investigation of stable carbon isotope composition (δ13C) of alkyl and acyl moieties derived from a range of IPL precursors with distinct polar head groups resolved the complexity of carbon metabolisms and utilization of diverse carbon sources by uncultured microbial communities. In surface sediments most of the polar lipid-derived fatty acids with phosphatidylethanolamine (PE), phosphatidylglycerol (PG) and diphosphatidylglycerol (DPG) head groups could be tentatively assigned to autotrophic sulfate-reducing bacteria, with a relatively small proportion involved in the anaerobic oxidation of methane. Derivatives of phosphatidyl-(N)-methylethanolamine (PME) were abundant and could be predominantly assigned to heterotrophic oil-degrading bacteria. Archaeal IPLs with phosphate-based hydroxyarchaeols and diglycosidic glyceroldibiphytanylglyceroltetraethers (GDGTs) were assigned to methanotrophic archaea of the ANME-2 and ANME-1 cluster, respectively, whereas δ13C values of phosphate-based archaeols and mixed phosphate-based and diglycosidic GDGTs point to methanogenic archaea. At a 7 m deep sulfate-methane transition zone that is linked to the upward movement of gas-laden petroleum, a distinct increase in abundance of archaeal IPLs such as phosphate-based hydroxyarchaeols and diglycosidic archaeol and GDGTs is observed; their δ13C values are consistent with their origin from both methanotrophic and methanogenic archaea. This study reveals previously hidden, highly complex patterns in the carbon-flow of versatile microbial communities involved in the degradation of heavy oil including hydrocarbon gases that would not have been evident from classical compound-specific isotope analyses of either bulk IPL or apolar lipid derivatives.  相似文献   

19.
This study presents isotope geochemical analyses conducted on water column samples and core sediments collected from the Swan Lake Basin. Water analyses include the dissolved methane (CH4) content and the ratio of carbon-13 to carbon-12 (δ13C) in dissolved inorganic carbon (DIC). The core sediments – sandy muds containing inorganic calcite, organic matter, and opal phases ± ostracods – were examined by X-ray diffraction, dated by radiocarbon (14C), analyzed for wt% organic carbon, wt% organic nitrogen, wt% organic matter, wt% calcite, δ13C of bulk-sediment insoluble organic matter (kerogen), 18O:16O ratio (δ18O) and δ13C of bulk and ostracod calcite. Of particular significance is the large enrichment in carbon-13 (δ13C = +4.5 to +20.4‰ V-PDB) in the calcite of these sediments. The 13C-enriched calcite is primarily formed from DIC in the water column of the lake as a result of the following combined processes: (i) the incorporation of 13C enriched residual carbon dioxide (CO2) after partial reduction to CH4 in the sediments and its migration into the water column-DIC pool; (ii) the preferential assimilation of 12C by phytoplankton during photosynthesis; (iii) the removal of 13C-depleted CH4 by ebullition and of organic matter by sedimentation and burial. The 13C enrichment was low between 3624 and 2470 yr BP; high between 2470 and 1299 yr BP; and moderate since 1299 yr BP. Low 13C enrichment was formed under low water-column carbon levels while higher ones were formed under elevated rates of biomass and calcite deposition. These associations seem to imply that biological productivity is the main reason for carbon-13 enrichments.  相似文献   

20.
Ethane and propane are low molecular weight hydrocarbons observed widely at trace levels in cold marine sediments where thermogenic sources are considered insignificant, but their biological sources remain poorly constrained. In this study, several C2 and C3 compounds including alkenes, alcohols, thiols and carboxylic acids with a C2 or C3 skeleton were tested for their relative alkane-producing potential in an anoxic estuary sediment. Maximum conversion efficiency of substrates to ethane or propane was observed in the sediment supplemented with ethylene (up to 38%), followed by additions with ethanethiol (0.01%) and propanethiol (0.003%). Experiments with sterilized sediment, 2-bromoethanesulfonic acid or NaNO3 were negative for alkane production, suggesting that methanogens were involved in alkane generation. Detailed investigation on ethanogenesis from ethylene showed that this reaction required H2 but at reasonably low concentration (< 120 nmol dissolved H2 l−1 slurry) and caused a slight stable carbon isotope effect (εethane/ethylene = −8.6 ± 2.4‰). The high ethane-producing potential, reasonable H2 requirement and extensive occurrence of ethylene make ethylene reduction a plausible explanation for ethane in cold marine sediment. Phylogenetic analysis was first carried out with an ethane-producing enrichment with ethylene as the substrate and showed a dominance of homoacetogenic bacteria and the methanogenic genus Methanocalculus. Although we cannot rule out the possibility that other methanogens in the gene libraries are responsible for ethanogenesis from ethylene, the dominance of Methanocalculus, with its hydrogenotrophic cultured representatives, is in accord with our biogeochemical observation that H2 is required for this reaction.  相似文献   

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