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1.
随着色谱-质谱联用技术的引用,对原油及岩石抽提有机质开展了生物标志物的研究,使我们对陆相沉积岩中有机质的认识,深入到单烃化合物及其分子结构中了。这将使我们准确地鉴别出陆相沉积中特征有机化合物,对探讨石油起源、演化、运移等较复杂的地球化学问题,提供了可靠的信息,更好的为石油地质勘探服务。 相似文献
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The kerogen of an organic-rich sample, termed f top, from the Gorodische section (Russian platform) was studied using a combination of microscopic, spectroscopic and pyrolytic methods so as to examine its chemical structure, source organisms and formation pathway(s). This kerogen, which is mainly composed of orange gel-like, nanoscopically amorphous organic matter, exhibits a relatively high aliphatic character; organic sulphur is mainly present as di(poly)sulphides and alkylsulphides. The f top kerogen was chiefly formed via intermolecular incorporation of sulphur in algal or cyanobacterial lipids and carbohydrates. However, its formation also involved oxidative condensation via ether linkages. Comparison of f top sample with other S-rich kerogens points to a closer similarity with Monterey kerogens rather than with a kerogen from the bituminous laminites of Orbagnoux. 相似文献
4.
Hartgers WA Sinninghe Damsté JS Requejo AG Allan J Hayes JM Ling Y Xie TM Primack J De Leeuw JW 《Organic Geochemistry》1994,22(3-5):703-725
Pyrolysates of high-molecular-weight sedimentary fractions of the Duvernay Formation (Western Canada Basin) are dominated by 1,2,3,4- and 1,2,3,5-tetramethylbenzene, which, generated via beta-cleavage, indicate the presence of diaromatic carotenoids in the macromolecular aggregates. This was substantiated by desulphurization of sulphur-rich aggregates of the polar fraction, which released (partly) hydrogenated carotenoids. Furthermore, these components were important constituents of the aromatic hydrocarbon fractions and related oils. Apart from renieratane and isorenieratane, 1H NMR analysis established the aromatic substitution pattern of the most abundant component present, which was identified as a diaromatic compound with an unprecedented 2,3,6-/3,4,5-trimethyl aromatic substitution pattern. Molecular and isotopic analyses of both soluble and insoluble fractions of organic matter revealed relationships between diagenetically-derived carotenoids found in bitumen and related oils and their precursors incorporated into high-molecular-weight fractions. Aryl isoprenoids, important components in extracts and oils, were apparently derived from thermal cracking of bound diaromatic carotenoids rather than cleavage of free carotenoids as previously suggested. Furthermore, products derived from diaromatic carotenoids were substantially enriched in 13C relative to n-alkanes of algal origin. Together with the characteristic carotenoids, this isotopic enrichment provides evidence of significant contributions from photosynthetic green sulphur bacteria (Chlorobiaceae), which fix carbon via the reversed tricarboxylic acid (TCA) cycle. In spite of the prominence of these molecular signals, the overall isotopic composition of the organic matter indicated that only a very small portion of the preserved organic carbon was derived from the biomass of photosynthetic green sulphur bacteria. 相似文献
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A saline circuit has been studied as a model of coastal evaporite system. The lipid composition of diverse salt ponds encompassing calcite, gypsum and halite domains has been determined. Most of the lipid materials has been found in the carbonate samples and is related to algal/cyanobacterial debris. Lipids in the gypsum domain are of heterotropic microbialorigin and extreme halophilic bacteria constitute the main lipid contribution in the halite samples. n-Alkane distributions with high predominance of n-docosane constitute a previously described feature of sedimentary evaporitic conditions that is charateristics of the intermediate calcite/gypsum samples. In the calcite domain, the presence of C20 highly branched isoprenid olephines, tetrahymanol and the large amounts of phytol constitute likely precursors of lipids usually found in evaporitic environments (i.e. C20 highly branched isoprenoid alkanes, gammacerane and high phytane/pristane ratios). Their occurence point to dehydration and hydrogenations as two main diagenetic processes leading to the formation of “evaporitic molecular markers”. 相似文献
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The extractable organic matter of 10 immature samples from a marl bed of one evaporitic cycle of the Vena del Gesso sediments (Gessoso-solfifera Fm., Messinian, Italy) was analyzed quantitatively for free hydrocarbons and organic sulphur compounds. Nickel boride was used as a desulphurizing agent to recover sulphur-bound lipids from the polar and asphaltene fractions. Carbon isotopic compositions (delta vs PDB) of free hydrocarbons and of S-bound hydrocarbons were also measured. Relationships between these carbon skeletons, precursor biolipids, and the organisms producing them could then be examined. Concentrations of S-bound lipids and free hydrocarbons and their delta values were plotted vs depth in the marl bed and the profiles were interpreted in terms of variations in source organisms, 13 C contents of the carbon source, and environmentally induced changes in isotopic fractionation. The overall range of delta values measured was 24.7%, from -11.6% for a component derived from green sulphur bacteria (Chlorobiaceae) to -36.3% for a lipid derived from purple sulphur bacteria (Chromatiaceae). Deconvolution of mixtures of components deriving from multiple sources (green and purple sulphur bacteria, coccolithophorids, microalgae and higher plants) was sometimes possible because both quantitative and isotopic data were available and because either the free or S-bound pool sometimes appeared to contain material from a single source. Several free n-alkanes and S-bound lipids appeared to be specific products of upper-water-column primary producers (i.e. algae and cyanobacteria). Others derived from anaerobic photoautotrophs and from heterotrophic protozoa (ciliates), which apparently fed partly on Chlorobiaceae. Four groups of n-alkanes produced by algae or cyanobacteria were also recognized based on systematic variations of abundance and isotopic composition with depth. For hydrocarbons probably derived from microalgae, isotopic variations are well correlated with those of total organic carbon. A resistant aliphatic biomacromolecule produced by microalgae is, therefore, probably an important component of the kerogen. These variations reflect changes in the depositional environment and early diagenetic transformations. Changes in the concentrations of S-bound lipids induced by variations in conditions favourable for sulphurization were discriminated from those related to variations in primary producer assemblages. The water column of the lagoonal basin was stratified and photic zone anoxia occurred during the early and middle stages of marl deposition. During the last stage of the marl deposition the stratification collapsed due to a significant shallowing of the water column. Contributions from anaerobic photoautotrophs were apparently associated with variations in depth of the chemocline. 相似文献
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Structural studies of a sulphur-rich kerogen and macromolecular oil fractions from the Monterey Formation were performed by selective sequential chemical degradation. The method provides low-molecular weight compounds as former building blocks of the network which allow detailed analyses on a molecular level. The degradation sequence is based on three subsequently performed reactions—a selective cleavage of sulphur bonds in the first step carried out with Ni(0)cene/LiAlD4, an ether and ester bond cleavage (BCl3), and an oxidation of aromatic entities by ruthenium tetroxide as a final step. Each step of this sequence afforded a considerable amount of low-molecular weight material which was separated chromatographically and studied by GC and GC/MS, while the high-molecular weight or insoluble fractions were subjected to the next reaction step.The chemical degradation products—hydrocarbons and carboxylic acids—are discussed in terms of incorporation into the macromolecular structure, distribution of heteroatomic bridges and the genetic relationships between the different macromolecular crude oil fractions and kerogen.Labelling experiments with deuterium provided evidence for a simultaneous linkage by oxygen and sulphur functionalities or by aromatic units and sulphur bonds of cross-linking macromolecular network constituents.The determination of sulphur positions in the macromolecule suggests early diagenetic sulphur incorporation into the biological precursor compounds and subsequent formation of a cross-linked network. 相似文献
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J. Alonso‐Azcrate M. Rodas L. Fernndez‐Díaz S.H. Bottrell J. R. Mas S. Lpez‐Andrs 《Geological Journal》2001,36(2):159-170
The low‐grade metasediments of the Cameros Basin, northern Spain, host a number of deposits of spectacular quality pyrite mineralization. These formed during regional metamorphism and the pyrite crystals exhibit a wide range of morphologies. On the basis of pyrite crystal habit, the deposits can be classified into two groups: Group I comprises deposits with cubic, elongated or platy crystals; Group II comprises deposits characterized by pyritohedra and cubo‐pyritohedra with striated faces, along with blocky crystals and fine‐grained aggregates. Group I deposits are formed in sequences dominated by meandriform fluviatile sediments, while Group II is hosted by deltaic plain and lacustrine metasediments. Temperature differences between deposits and As content are possible causes of the different pyrite morphologies in the deposits, but no significant variation exists between the two groups for either factor. Comparison with experimentally grown pyrite crystals suggests that Group I deposits have morphologies indicative of lower degrees of pyrite supersaturation than pyrite crystals in Group II deposits. The sedimentary facies hosting Group II deposits provides a greater availability of sedimentary sulphur (pyrite and sulphates). Moreover, reactions involving sulphate during metamorphism may have modified fluid chemistry, which would also act to produce higher degrees of pyrite saturation in fluids derived from the sulphate‐rich deltaic plain and lacustrine metasediments hosting the Group II deposits. This hypothesis is confirmed by sulphur isotope data on the pyrites, which show a larger component of34S‐enriched sulphate‐derived sulphur in these deposits. Copyright © 2001 John Wiley & Sons, Ltd. 相似文献
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Geochemistry and morphology of metalliferous sediments and oxyhydroxides from the Endeavour segment, Juan de Fuca Ridge 总被引：3，自引：0，他引：3
We present first data on the geochemistry, mineralogy and morphology of near-vent sediments (35 and 200 m from active vent) and ridge flank sediments (approximately 3 km from the vent field) as well as oxyhydroxide deposits from the Endeavour segment, Juan de Fuca Ridge. The purpose of the study was to understand better the origin and characteristic features of metalliferous sediments associated with base and precious metal massive sulfides in volcanic terrains. Hydrothermal components in sediments are Fe-Si ± S-rich and Mn-Fe-Si-rich phases, sulfides and barite, which were exclusively derived from plume fallout. Sulfides are only a minor constituent of near-vent sediments (2-4 wt%) and were not detected in ridge flank sediments. The study suggests that the distribution of hydrothermal phases and associated elements in near-vent and ridge flank sediments is affected mainly by processes of agglomeration, dissolution, absorption and settling that take place within a plume and to a lesser extent post-depositional processes. Rapid deposition of sulfides in the vicinity of the vents is reflected in a sharp drop of the Cu concentrations in sediments with increasing distance from the vents. Besides sulfides, important carriers of Pb, Cu, Zn and Co in near-vent sediments are Fe-Mn oxyhydroxides that occur together with silica as aggregates of gel-like material and flaky particles and as coatings on filaments. Away from the vents, trace metals are mostly in Fe-Mn oxyhydroxides and authigenic Fe-rich montmorillonite. Oxyhydroxides at the Main Endeavour field are interpreted to have originated from oxidation of mound sulfides accompanied by precipitation of primary Fe-oxyhydroxide + silica from low-temperature fluids. At the Mothra field, seafloor deposits and chimney crusts composed of Fe-oxyhydroxide ± Mn + silica are considered to be direct precipitates from hydrothermal fluids that have been less diluted with seawater. Oxyhydroxide deposits exhibit unique microtextures that resemble mineralized microorganisms and may indicate existence of diverse microbial communities. 相似文献
10.
Anke Putschew Christine Schaeffer-Reiss Philippe Schaeffer Martin P Koopmans Jan W de Leeuw Michael D Lewan Jaap S Sinninghe Damsté James R Maxwell 《Organic Geochemistry》1998,29(8):1875-1890
An immature sulfur-rich marl from the Gessosso-solfifera Formation of the Vena del Gesso Basin (Messinian, Italy) has been subjected to hydrous pyrolysis (160 to 330°C) to simulate maturation under natural conditions. The kerogen of the unheated and heated samples was isolated and the hydrocarbons released by selective chemical degradation (Li/EtNH2 and HI/LiAlH4) were analysed to allow a study of the fate of sulfur- and oxygen-bound species with increasing temperature. The residues from the chemical treatments were also subjected to pyrolysis–GC to follow structural changes in the kerogens. In general, with increasing hydrous pyrolysis temperature, the amounts of sulfide- and ether-bound components in the kerogen decreased significantly. At the temperature at which the generation of expelled oil began (260°C), almost all of the bound components initially present in the unheated sample were released from the kerogen. Comparison with an earlier study of the extractable organic matter using a similar approach and the same samples provides molecular evidence that, with increasing maturation, solvent-soluble macromolecular material was initially released from the kerogen, notably as a result of thermal cleavage of weak carbon–heteroatom bonds (sulfide, ester, ether) even at temperatures as low as 220°C. This solvent-soluble macromolecular material then underwent thermal cleavage to generate hydrocarbons at higher temperatures. This early generation of bitumen may explain the presence of unusually high amounts of extractable organic matter of macromolecular nature in very immature S-rich sediments. 相似文献
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松辽盆地白垩系青山口阶界线层型剖面研究 总被引：3，自引：0，他引：3
茂206井是中国白垩纪大陆科学钻探工程井,全井获取了青山口阶497.02m的岩芯资料。茂206井青山口阶为典型的湖相沉积,它具有相对高的有机碳、无机碳稳定同位素,表示当时古湖泊具有较高的生产力;同时在青山口阶下部具有高的规则甾烷/藿烷比值和伽马蜡烷/C30藿烷比值以及低的重排甾烷/常规甾烷比值,表示当时的古湖泊曾发生过藻类勃发事件、水体分层事件和缺氧事件,由此导致了青山口阶优质烃源岩的形成。青山口阶底部出现的一些具重要时代意义的被子植物花粉Cranwellia,Lythraites,Complexiopollis,Borealipollis等,显示青山口阶具有晚白垩世土仑期以后的被子植物花粉色彩,以及湖相沉积岩夹层中的火山灰(斑脱岩)锆石U-Pb年龄也证实了青山口阶底界已属土仑期,其顶界已进入康尼亚克期。 相似文献
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The basin-scale spatial variability in lipid biomarker proxies in lacustrine sediments, which are established tools for studying continental environmental change, has rarely been examined. It is often implicitly assumed that a lake sediment core provides an average integral of catchment sources. Here we evaluated the distribution of lipid biomarkers in a modern ecosystem and compared it with the sedimentary record. We analyzed lipid biomarkers in terrestrial and aquatic organisms and in lake surface sediments from 17 locations within the saline–alkaline Lonar crater lake in central India. Terrestrial vegetation and lake surface sediments were characterized by relatively high average chain length (ACL) index values (29.6–32.8) of leaf wax n-alkanes, consistent with suggestions that plants in drier and warmer climates produce longer chain alkyl lipids than plants in cooler and humid areas. A heterogeneous spatial distribution of ACL values in lake surface sediments was found: at locations away from the shore, the values were highest (31 or more), possibly indicating different sources and/or transport of terrestrial biomarkers. In floating, benthic microbial mats and surface sediment, n-heptadecane, carotenoids, diploptene, phytol and tetrahymanol occurred in large amounts. Interestingly, these biomarkers of a unique bacterial community were found in substantially higher concentrations in nearshore sediment samples. We suggest that human influence and subsequent nutrient supply resulted in increased primary productivity, leading to an unusually high concentration of tetrahymanol in the nearshore sediments.In summary, the data showed that substantial heterogeneity existed within the lake, but leaf wax n-alkanes in a core from the center of the lake represented an integral of catchment conditions. However, lake level fluctuation may potentially affect aquatic lipid biomarker distributions in lacustrine sediments, in addition to source changes. 相似文献
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The triterpenol geochemistry of the Santa Monica Basin from the Southern California Borderland, off the U.S.A., is described from the study of two sets of trap deployments, five box cores (≈30 cm) and a hydroplastic core (≈1 m). The biogenic sources and diagenetic stability of the triterpenols are discussed.The 17β(H), 21β(H)-hopanols (22R isomer) occur in the carbon number range from 30 to 32 and their abundance is nearly uniform in the shallow sediment sections. However, the three hopanols follow the order of abundance, C32 > C31 C30, in deeper sections. Their concentrations spans from trace levels to 156 μg/g organic carbon (<15 ng to 7 μg/g dry sediment). Tetrahymanol (gammaceran-3β-ol) has been identified in all the samples except in one set of trap particles collected at 100 m water depth, from trace level (<1 μg) to 215 μg/g organic carbon (<20 ng to 9 μg/g dry sediment). Diplopterol is also detected in trace amounts in some samples. The triterpenols in the trap material generally increase with the water column depth and decrease with the subbottom depth in the sediment cores.The extended hopanols are either degradation products of polyhydroxybacteriohopanes or are biosynthesized by bacteria. Tetrahymanol is probably the only suggested biological precursor of gammacerane (the reduced counterpart of tetrahymanol), which has been recognized in numerous crude oils and lithified sediments. Although it has been reported earlier from Green River Shale and from a residual Pleistocene lake sediment, tetrahymanol has so far been positively identified from recent marine sediments only in two recent studies. The decreasing content of tetrahymanol in sedimentary depth profiles in the Santa Monica Basin would favor an origin for this compound in the water column or at the sediment surface. The ubiquitous occurrence of this compound throughout the study area suggests that this triterpenol most probably originates from primitive organisms (protozoa, bacteria?), hitherto not identified or, more likely, not yet analyzed for their lipid composition. 相似文献
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Evidence for,and implications of,a primary FeS phase in the lead-zinc bearing sediments at Mount Isa
Quantitative mineral data from the lead-zinc bearing sediments at Mount Isa were studied using linear correlation analysis and R-mode cluster analysis. Pyrrhotite was found to be preferentially associated with galena and sphalerite. It is postulated that during sedimentation, formation of lead and zinc sulphides depleted an already limited sulphur supply to the point where the field of FeS stability was entered. The primary iron monosulphide formed was, or has since become, pyrrhotite. This hypothesis is in contrast to the widely held opinion that pyrrhotite in stratiform ores formed by metamorphic decomposition of pyrite. Empirical support for the sedimentary formation of pyrrhotite is provided by textural and qualitative mineralogical data from Mount Isa and other stratiform lead-zinc deposits. 相似文献
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四川盆地富硫天然气与盆地周缘铅锌铜矿的成因联系 总被引：1，自引：0，他引：1
金属元素的搬运和沉淀是热液矿床成矿机理研究的重要方面。目前人们普遍认为热液矿床中金属元素主要呈硫的络合物和卤素络合物形式搬运。MVT铅锌矿床等硫化物矿床盐度较高,包裹体成分中阳离子以Na+、K+、Ca2+、Mg2+为主,阴离子以Cl-、F-、CO2-3为主,很少有HS-、S2-,表明金属元素主要以氯的络合物形式搬运,外来硫的加入是导致铅锌成矿物质以硫化物形式沉淀成矿的关键。四川盆地天然气中富含H2S,其与周缘MVT铅锌矿床具有密切的时空关系,据此推测天然气中的H2S可能是导致铅锌硫化物沉淀形成MVT铅锌矿床的主要硫源,天然气中的H2S与铅锌成矿流体在古油藏中作用形成含沥青的铅锌矿床;当含硫化氢的天然气运移离开古油藏后与含矿流体混合时,形成不含沥青的铅锌矿床。另外,石油热裂解产生的不含H2S的天然气使得含铜热液中的铜还原,以自然铜形式沉淀形成含沥青的玄武岩铜矿;石油热化学硫酸盐还原(TSR)过程中,还会发生溶蚀作用,扩大碳酸盐岩孔隙,为成矿提供空间。 相似文献
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A series of novel long-chain 3,4-dialkylthiophenes (C36–C54) was identified in a number of sediments ranging from Pleistocene to Cretaceous. The identifications were based on mass spectral characterisation, desulphurisation and mass spectral data of synthesised model compounds. These organic sulphur compounds are probably formed by sulphur incorporation into mid-chain dimethylalkadienes with two methylenic double bonds. These putative precursor lipids are unprecedented and may be considered rather unusual. The distribution of 3,4-dialkylthiophenes in sediments varies considerably with the depositional palaeoenvironment, indicating that these compounds have a potential as molecular markers reflecting changes in palaeoenvironment. 相似文献
18.
Regional background
34S values of pyrite-(marcasite) nodules throughout the Zechstein basin in Poland have been measured to help estimate the proportion of externally derived sulphur in the Kupferschiefer Cu-Ag ores. The
34S values of the 17 FeS2 nodules measured range widely, from -25.2 to -51.9%., similar to the previously published -28 to -43%. range in disseminated pyrite in the Kupferschiefer. The wide variation cannot be attributed to pyrite versus marcasite mineralogy, amount of contained chalcopyrite or sphalerite, carbonate versus shale host rock, early versus late formation, percent of included calcite, or to size, shape, or texture. There is also no relation with proximity to the centres of copper mineralization in southwestern Poland where sulphides are typically isotopically heavier. The
34S values do, however, vary directly with percent of host-rock fragments included in the nodules. Repeat samples that were washed with acid or hot water show the same wide variation, indicating that contamination by sulphate sulphur in the host rock is not a factor. Neither is organic sulphur because of its small volume. Instead, the sulphur composition may be fundamentally controlled by the formation mechanism of the nodule, whereby 34S-rich sulphide is preferentially concentrated, possibly replacing anhydrite lenses. Alternatively, a network of host rock inclusions might act as a more accessible conduit for later, 34S-rich fluids to infiltrate the nodule and add to earlier, 34S-poor pyrite.In the ore deposits, higher
34S values of ore nodules suggest less indigenous sulphur in limestone than shale lithologies. An isotopic temperature of 61 °C from a chalcopyrite-galena pair agrees with other estimates of <105°C. Higher values in ore nodules/veinlets than in adjacent disseminations, and the calculated
34Spy value from a pyrite-bornite mixture support the idea that metal-bearing 34S-rich fluids penetrated the Kupfer-schiefer through a network of fractures.Contribution to IGCP Project 254 Metalliferous Black Shales 相似文献
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西藏驱龙巨型斑岩Cu Mo矿床的富S、高氧化性含矿岩浆——来自岩浆成因硬石膏的证据 总被引：7，自引：1，他引：6
西藏冈底斯成矿带上的驱龙巨型斑岩Cu-Mo矿床以发育大量的硬石膏为特征.详细的岩相学研究发现:驱龙矿床不仅发育热液脉状的硬石膏,含矿斑岩中还产出岩浆成因硬石膏,这在国内系首次报道.观察表明,在岩浆演化早期的花岗闪长岩、黑云母二长花岗岩中,岩浆硬石膏以矿物包体的形式产于斜长石、石英中;在主成矿期的二长花岗斑岩、花岗闪长斑岩中,岩浆硬石膏以矿物包体产于斜长石斑晶中,局部以斑晶形式产出,并伴有富S的磷灰石(SO_3含量为0.11%～0.44%)、磁铁矿发育.后期热液活动也形成了大量的硬石膏±石英+硫化物脉,是矿区主要的矿化类型之一.电子探针分析结果显示,后期的热液硬石膏与岩浆硬石膏相比,在微量成分上明显富集Sr(分别为0.24%和0.03%),可能是由于在岩浆-热液演化过程中,Sr的不相容性或者/以及粘土化蚀变造成的.岩浆硬石膏以及与之共生的富S磷灰石的出现,明确指示驱龙矿床成矿岩浆具有富S、高氧逸度的特征;同时也为研究S在斑岩型矿床岩浆演化过程中的状态、行为,提供了很好的研究对象. 相似文献
20.
浅成低温热液型金矿床研究的某些进展 总被引：1，自引：0，他引：1
浅成低温热液型金矿床成矿流体在较深处(3～4km)发生相分离的同时导致不同成矿元素和载矿元素进入不同的相态,从而形成不同性质流体,其中富挥发S的气水相在高压下有很强的载矿能力,对特定矿化类型形成具有决定性意义。流体在向浅成低温环境演化过程中,携带大量成矿物质的气水相必须转化成液相才可能导致浅成低温成矿(深度1～2km),这个过程与含水的岩浆房冷却密切相关。通过冷却加压,富挥发S的气体在水盐体系的两相界面以上可转变为液体,将成矿元素Au等运移至浅部。浅成低温热液矿床与卡林型矿床均可形成于大陆裂谷环境,前者的高硫化类型与后者在流体性质、蚀变特征、成矿特征等方面具有明显的相似性和可比性。富碲型矿床的Te很可能是在相分离过程中以Te2(g)和H2Te(g)的形式进入气相,并在浅部被地下水吸收,形成Ag(HTe)2-和Au(HTe)2-络合物,伴随着流体的冷却和环境变化,使得碲化物沉淀。少硫(碲)化物特富金的浅成低温热液型矿床金可能以金硅络合物或是金硅合金氢化物形式进行搬运,在浅部SiO2和Au沉淀形成特富金矿。 相似文献