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1.
New insights into the origin of perylene in geological samples   总被引：1，自引：0，他引：1  
The origin of the polycyclic aromatic hydrocarbon (PAH) perylene in sediments and petroleum has been a matter of continued debate. Reported to occur in Phanerozoic organic matter (OM), fossil crinoids and tropical termite mounds, its mechanism of formation remains unclear. While a combustion source can be excluded, structural similarities to perylene quinone-like components present in e.g. fungi, plants, crinoids and insects, potentially suggest a product-precursor relationship. Here, we report perylene concentrations, 13C/12C, and D/H ratios from a Holocene sediment profile from the Qingpu trench, Yangtze Delta region, China. Perylene concentrations differ from those of pyrogenic PAHs, and rise to prominence in a stratigraphic interval that was dominated by woody vegetation as determined by palynology including fungal spores. In this zone, perylene concentrations exhibit an inverse relationship to the lignin marker guaiacol, D/H ratios between −284‰ and −317‰, similar to the methoxy groups in lignin, as well as co-variation with spores from wood-degrading fungi. 13C/12C of perylene differs from that of land plant wax alkanes and falls in the fractionation range expected for saprophytic fungi that utilise lignin, which is isotopically lighter than cellulose and whole wood. During progressive lignin degradation, the relative carbon isotopic ratio of the perylene decreases. We therefore hypothesise a relationship of perylene to the activity of wood-degrading fungi. To support our hypothesis, we analysed a wide range of Phanerozoic sediments and oils, and found perylene to generally be present in subordinate amounts before the evolutionary rise of vascular plants, and to be generally absent from marine-sourced oils, few exceptions being attributed perhaps to a contribution of marine and/or terrestrial-derived fungi, anoxia (especially under marine conditions) and/or contamination of core material by fungi. A series of low-molecular-weight aromatic quinones bearing the perylene-backbone were detected in Devonian and Cretaceous sediments, potentially representing precursor components to perylene.  相似文献   

2.
Perylene was found in a variety of marine sediments, in a shale and in peat. It is suggested that its precursors arise predominantly from land organisms and are carried into oceanic traps along with detrital minerals. When rates of deposition are fast, and reducing conditions are established within the sediment, biogenic pigment precursors of perylene are converted to the polycyclic aromatic hydrocarbon, which is then stabilized by π-bonding with metals and protected from degradation.  相似文献   

3.
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4.
Suspended sediments (SS) from the Atchafalaya River (AR) and the Mississippi River and surficial sediment samples from seven shallow cross-shelf transects west of the AR in the northern Gulf of Mexico were examined using elemental (%OC, C/N), isotopic (δ13C, Δ14C), and terrigenous biomarker analyses. The organic matter (OM) delivered by the AR is isotopically enriched (∼−24.5‰) and relatively degraded, suggesting that soil-derived OM with a C4 signature is the predominant OM source for these SS. The shelf sediments display OC values that generally decrease seaward within each transect and westward, parallel to the coastline. A strong terrigenous C/N (29) signal is observed in sediments deposited close to the mouth of the river, but values along the remainder of the shelf fall within a narrow range (8-13), with no apparent offshore trends. Depleted stable carbon isotope (δ13C) values typical of C3 plant debris (−27‰) are found near the river mouth and become more enriched (−22 to −21‰) offshore. The spatial distribution of lignin in shelf sediments mirrors that of OC, with high lignin yields found inshore relative to that found offshore (water depth > 10 m).The isotopic and biomarker data indicate that at least two types of terrigenous OM are deposited within the study area. Relatively undegraded, C3 plant debris is deposited close to the mouth of the AR, whereas more degraded, isotopically enriched, soil-derived OM appears to be deposited along the remainder of the shelf. An important input from marine carbon is found at the stations offshore from the 10-m isobath. Quantification of the terrigenous component of sedimentary OM is complicated by the heterogeneous composition of the terrigenous end-member. A three-end-member mixing model is therefore required to more accurately evaluate the sources of OM deposited in the study area. The results of the mixing calculation indicate that terrigenous OM (soil-derived OM and vascular plant debris) accounts for ∼79% of the OM deposited as inshore sediments and 66% of OM deposited as offshore sediments. Importantly, the abundance of terrigenous OM is 40% higher in inshore sediments and nearly 85% higher in offshore sediments than indicated by a two-end-member mixing model. Such a result highlights the need to reevaluate the inputs and cycling of soil-derived OM in the coastal ocean.  相似文献   

5.
Surface sediments from the Outer Continental Shelf of Alaska were analyzed for hydrocarbons as part of an environmental survey sponsored by NOAA/BLM. Sediments were collected from the proposed oil lease areas of Beaufort Sea, southeastern Bering Sea, Norton Sound, Navarin Basin, Gulf of Alaska, Kodiak Shelf and lower Cook Inlet. Data on normal and branched alkanes and di- and triterpenoids from capillary gas chromatography (GC) and gas chromatography-mass spectrometry (GC/ MS) indicate that the area displays little evidence of petroleum hydrocarbons (i.e., seeps) except at a few isolated stations. Beaufort Sea sediments have the highest hydrocarbon budget, whereas Kodiak Shelf sediments have the lowest. The molecular markers of the hydrocarbons are of a mixed marine autochthonous and terrestrial allochthonous origin. Norton Sound and Cook Inlet sediments contain the highest levels of terrigenous lipids and Kodiak Shelf the lowest. The abundance of alkenes implies that relatively low oxidizing conditions exist in some of the depositional areas studied, suggesting that extraneous petroleum hydrocarbons introduced into these sediments would be expected to have a relatively long residence time. The distribution of polynuclear aromatic hydrocarbons (PAH) is complex and shows a pyrolytic origin. The data on perylene strongly favor the hypothesis that it is “performed” from terrigenous precursors and transported into the marine environment with no apparent in situ generation. Polynuclear aromatic hydrocarbons of diagenetic origin are probably dominant in Gulf of Alaska and Kodiak Shelf sediments.Two stations, north of Kalgin Island, in lower Cook Inlet and one in southeastern Bering Sea show typical weathered petroleum distribution of n-alkanes and triterpenoids. Probable pathways of transport and fate of petroleum hydrocarbons in case of an oil spill are also briefly discussed.  相似文献   

6.
Sediment cores from Sagamore Lake and Woods Lake in New York State's Adirondack Park, an area remote from industrial activities, were analyzed for polynuclear aromatic hydrocarbons (PAH) by high resolution gas chromatography/mass spectrometry (GC/MS). Their composition and distribution with depth in the sediment indicate that the parental PAH in the surface sediments are primarily produced by anthropogenic combustion of fossil fuels. Perylene in deep sediments is apparently transformed from natural precursors in the reducing environment, however, the exact precursors remain unknown. The rather even sediment distributions of the non-parental PAH differ from the parental, suggesting biogenic origins. Based on their chemical structures, retene and alkylated and partially hydrogenated phenanthrenes are believed to be biogenically converted from abietic acid; hydrochrysenes and hydropicenes, from pentacyclic triterpenes.  相似文献   

7.
Oil shales were deposited in the Songliao Basin (NE China) during the Upper Cretaceous period, representing excellent hydrocarbon source rocks. High organic matter (OM) contents, a predominance of type-I kerogen, and a low maturity of OM in the oil shales are indicated by bulk geochemical parameters and biomarker data. A major contribution of aquatic organisms and minor inputs from terrigenous land plants to OM input are indicated by n-alkane distribution patterns, composition of steroids, and organic macerals. Strongly reducing bottom water conditions during the deposition of the oil shale sequences are indicated by low pristane/phytane ratios, high C14-aryl-isoprenoid contents, homohopane distribution patterns, and high V/Ni ratios. Enhanced salinity stratification with mesosaline and alkaline bottom waters during deposition of the oil shales are indicated by high gammacerane index values, low MTTC ratios, high β-carotene contents, low TOC/S ratios, and high Sr/Ba ratios. The stratified water column with anoxic conditions in the bottom water enhanced preservation of OM. Moderate input of detrital minerals during the deposition of the oil shale sequences is reflected by titanium concentrations. In this study, environmental conditions in the paleo-lake leading to OM accumulation in the sediments are related to sequence stratigraphy governed by climate and tectonics. The first Member of the Qingshankou Formation (K2qn1) in the Songliao Basin, containing the oil shale sequence, encompasses a third-order sequence that can be divided into three system tracts (transgressive system tract—TST, highstand system tract—HST, and regressive system tract—RST). Enrichment of OM changed from low values during TST-I to high-moderate values during TST-II/III and HST-I/II. Low OM enrichment occurs during RST-I and RST-II. Therefore, the highest enrichment of OM in the sediments is related to stages of mid-late TST and early HST.  相似文献   

8.
Fifteen sediment samples were studied from five drill sites recovered by the ‘Glomar Challenger’ on Legs I and IV in the Gulf of Mexico and western Atlantic. This study concentrated on compounds derived from biogenic precursors, namely: (1) hydrocarbons, (2) fatty acids, (3) pigments and (4) amino acids.Carbon isotope (δC13) data (values < ? 26%, relative to PDB), long-chain n-alkyl hydrocarbons ( ?C277) with odd carbon numbered molecules dominating even carbon numbered species, and presence of perylene proved useful as possible indicators for terrigenous contributions to the organic matter in some samples. Apparently land-derived organic matter can be transported for distances over 1000 km into the ocean and their source still recognized.The study was primarily designed to investigate: (i) the sources of the organic matter present in the sediment, (ii) their stability with time of accumulation and (iii) the conditions necessary for in situ formation of new compounds.  相似文献   

9.
The composition of sand-silt and pelite fractions of deep-sea sediments deposited under different hydrodynamic conditions was studied. Assemblages of clastic, clayey, biogenic, and authigenic minerals formed under the influence of surface and bottom currents were traced. It is shown that biogenic opal, fine-dispersed celestobarite, and authigenic protosyngenetic ferromanganese micronodules, which are composed of only manganese phases, represent indicators of cyclonic gyres characterized by enhanced bioproductivity. Collophane (bone detritus), phillipsite, palagonite, and large celestobarite crystals prevail in mineral assemblages below the anticyclonic gyres, whereas ore micronodules are depleted in manganese. Surface and bottom currents control the distribution of clastic (terrigenous edaphogenic, terrestrial-volcanogenic) and clay minerals, as well as biogenic opal in the form of Ethmodiscus frustules in sediments. Edaphogenic mineral assemblages represent the reliable indicators of bottom currents.  相似文献   

10.
The prerequisite for obtaining variations of terrigenous grain-size of marine sediments is how to effectively remove non-terrigenous matters and preserve terrigenous particles synchronously. Combined with observations under biological microscope and scanning electron microscope, a comparative study of biogenic debris removal effect and terrigenous grain-size analysis under different pretreatment condition was performed on core sediments, which were retrieved in the South China Sea during the MD190 cruise. Our new results showed that the main three biogenic particles, namely, organic matter, carbonate, and opal in marine sediments could be removed effectively by 30% H2O2 in a stirring water bath at 60 ℃ for 3 h, 0.5% HCl for 1 h, and 2 mol/L Na2CO3 in a stirring water bath at 85 ℃ for 5 h, in turn. Such pretreatments achieved the goals of biogenic debris removal efficiency and relatively well-preserved terrigenous particles. Prior to selecting an appropriate pretreatment method, this study suggested that the actual effects of biogenic detritus on grain-size results of diverse marine sediment samples should be taken into account. If the laboratory data are ensured to be closer to the natural grain-size distribution of terrigenous particles, the removals of all biogenic debris are not always needed, and the less pretreatment processes the better. For example, opal particles have little effect on terrigenous grain-size distribution when their percentage is lower than 2%. Thus, there is no use to remove them from marine sediments before laboratory grain-size analysis of terrigenous particles. Additionally, ultrasonic is not suggested through the whole process of terrigenous grain-size analysis because the strong energy of ultrasonic can lead to the fragmentation of some fragile terrigenous particles.  相似文献   

11.
The concentration and structural diversity of a suite of bacteriohopanepolyols (BHPs) was measured in suspended particulate matter (SPM) from six stations along a river-ocean transect off the Pacific coast of Panama. Riverine SPM contained BHPs diagnostic of soil input consistent with a terrigenous source. The concentration of BHPs was 10 times greater in riverine SPM than marine SPM demonstrating that terrigenous OM exported to marine sediments could provide a significant contribution to the marine sedimentary hopanoid inventory. Given the rich structural diversity of BHPs in terrigenous SPM, interpretations of the sedimentary record of hopanoids in coastal marine settings must resolve inputs from marine pelagic and terrigenous sources.  相似文献   

12.
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13.
The molecular composition and distribution of the concentration of n-alkanes are considered for sediments of boreholes drilled in the shallow part of the Laptev Sea, in the area of Buor Khaya Gulf. The diverse molecular composition of n-alkanes is dominated by long-chain odd homologs, which indicate terrigenous organic matter (OM). Heterogeneous distribution and burial of OM are shown under conditions of pulsating contribution of river and thermoabrasive material and multiple changes in them up to hiatuses in sedimentation.  相似文献   

14.
The chemical composition of organic matter (Corg, Norg, δ13C, δ15N, and n-alkanes) was studied in the top layer of bottom sediments of the East Siberian Sea. Possible ways were proposed to estimate the amount of the terrigenous component in their organic matter (OM). The fraction of terrigenous OM estimated by the combined use of genetic indicators varied from 15% in the eastern part of the sea, near the Long Strait, to 95% in the estuaries of the Indigirka and Kolyma rivers, averaging 62% over the sea area.  相似文献   

15.
Available data on synthesis, input, and decomposition of organic matter (OM) in the water column and recent bottom sediments of the World Ocean are generalized. The most reliable values of OM production and masses in the ocean, the total supply of organic carbon, and the input of terrigenous OM with coastal erosion, river runoff, and eolian matter are estimated. Maps of fossilization coefficients, distribution, and accumulation of OM in recent bottom sediments of the World Ocean are presented. A numerical expression is proposed for the main circumcontinental pattern of OM accumulation in the ocean. The group and elemental compositions of living matter of the ocean, land, and the Earth as a whole and the organic composition of bottom sediments are briefly considered.  相似文献   

16.
Late Jurassic-early Cretaceous black shales and an overlying sequence of Albian-Campanian zeolitic claystones from the Falkland Plateau (DSDP/IPOD Leg 71, Site 511) were analyzed for tetrapyrrole pigment type and abundance. The “black shale” sequence was found to be rich in DPEP-series dominated free-base, nickel (Ni) and, to a lesser extent, vanadyl (V = 0) porphyrins. A low level of organic maturity (i.e. precatagenesis) is indicated for these strata as nickel chelation by free-base porphyrins is only 50–75% complete, proceeding down-hole to 627 meters sub-bottom. Electronic and mass spectral data reveal that the proposed benzo-DPEP (BD) and tetrahydrobenzo-DPEP (THBD) series are present in the free-base and Ni species, as well as the more usual occurrence in V = 0 porphyrin arrays. Highly reducing conditions are suggested by an abundance of the PAH perylene, substantial amounts of the THBD/BD series and a redox equilibrium between free-base DPEP and 7,8-dihydro-DPEP series, which exist in a 7:1 molar ratio. The Albian-Campanian claystone strata were found to be tetrapyrrolepoor, and those pigments present were typed as Cu/Ni highly dealkylated (C26 max.) etioporphyrins, thought to be derived via redeposition and oxidation of terrestrial organic matter (OM). Results from the present study are correlated to our past analyses of Jurassic-Cretaceous sediments from Atlantic margins in an effort to relate tetrapyrrole quality and quantity to basin evolution and OM sources in the proto-Atlantic.  相似文献   

17.
Perylene and penta-aromatic hydrocarbons were determined in sediments as part of a study that was dedicated to the aquatic ecosystem of Elelenwo Creek (Southern Nigeria) in order to carry out a critical corroboration of occurrence and diagenetic evolution of perylene in the sediments of the creek. The results show that the annual mean levels of Benzo [g, h, i] Perylene ranged from 209.00–245.28 ?g/kg dry weight at the various stations sampled. Meanwhile, Station 3 recorded the highest mean level of 245.28 ?g/kg dry weight. The observed values for total penta-aromatic hydrocarbons were high (787.00–1154.36?g/kg dry weight) in all the stations sampled. In addition, the highest mean value of 1154.36?g/kg dry weight was again recorded at station 3 for the penta-aromatic hydrocarbons. One origin index or concentration ratio of Ip/Ip+BghiP was also used to evaluate the suitability of the penta-aromatic hydrocarbons as a tracer to distinguish between contaminations arising from different sources. The values for the sampling stations therefore ranged from 0.41 to 0.43. A critical appraisal of the PAH index, consequently, suggested that petroleum combustion is the major penta-aromatic hydrocarbon source in sediments of the creek. The PAH group profile shows that perylene was high in the sediments and would pose apparent effects in fauna. The high concentration of perylene in the sediments was also indicative of an in situ biogenic derivation. Furthermore, a concentration of perylene > 10 % of total penta-aromatic hydrocarbons established a credible diagenetic origin.  相似文献   

18.
The results of the thorough study of organic matter (OM) in the Oligocene-Miocene Maikop sequence of the North Caucasus are considered. It is shown that its distribution within the Maikop sequence is characterized by irregular patterns. Despite that these rocks show the elevated TOC content, their hydrocarbon-generating potential is, as a rule, low. The low quality of OM is partly related to its intense anaerobic decomposition in anoxic environments with terrigenous sedimentation. The elevation of OM concentrations and hydrocarbon-generating potential could be connected with the reinforced phytoplankton influx into sediments. Sediments deposited in the second half of the Early Oligocene were synchronously enriched in OM. This enrichment chronologically corresponded to the restoration of connection with the World Ocean of the formerly partly isolated and freshened basin. Most probably, this event resulted from the sharp increase in biological productivity.  相似文献   

19.
Origin of perylene in ancient sediments and its geological significance   总被引：2，自引：0，他引：2  
The distributions of polycyclic aromatic hydrocarbons (PAHs) in sediments of three Upper Triassic to Middle Jurassic sedimentary sequences from the Northern Carnarvon Basin, Australia have been investigated. Perylene was found to be a major PAH component in the top Lower to base Middle Jurassic sediments that are immature or at low maturity. Its depth/age profiles are not related to the combustion-derived PAHs that have been believed to be produced during ancient vegetation fires before deposition. This suggests a diagenetic origin for perylene. The concentration of perylene in the sediments is proportional to the amount of terrestrial input, decreasing with distance from the source of land sediments. Its carbon isotope composition is slightly heavier than higher-plant derived PAHs, but still in the range of the terrestrially sourced PAHs including higher-plant PAHs and combustion-derived PAHs as suggested previously. Fungi are proposed to be the major precursor carriers for perylene in sediments based on the facts that (1) perylenequinone structures have been previously suggested to be the natural precursors for perylene; (2) perylenequinone pigments exist in many fungal bodies; (3) fungi have played an important role during geological processes.  相似文献   

20.
Evidence of environmental and vegetation changes in the catchment area of a small pond created artificially during the Middle Ages from a swampy area was provided by coupling palynology data and a detailed study of macromolecular organic matter (OM). Tetramethylammonium hydroxide (TMAH) thermochemolysis after solvent extraction was used to characterize macromolecular OM and particularly lignin and fatty acids (FAs). Molecular ratios such as TAR(FA), C16:1/C16:0 and C18:1/C18:0 were calculated to characterize the FAs incorporated into the macromolecular OM. Moreover, syringyl vs. vanillyl phenols (S/V) and cinnamyl vs. vanillyl phenols (C/V) molecular ratios were investigated to fingerprint the lignin sources. These different markers suggested that the swampy area was dominated by a non-woody angiosperm input and gave rise to pond status over a period of several centuries. Indeed, TAR(FA) correlated with the aquatic contribution, which became predominant after creation of the pond. The use of ratios of total acid phenols to the total aldehyde phenols of syringyl or vanillyl units (Ad/Al(s), Ad/Al(v)), which are related to the degree of oxidation of lignin, revealed the irregular operation of oxidative conditions.  相似文献   

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