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1.
原油金属卟啉化合物对于揭示古环境变化过程中有机—无机相互作用及海洋缺氧事件具有重要意义。目前关于金属含量低于10 mg/kg的高成熟原油金属卟啉的分子组成研究鲜见报导。针对基质辅助激光解吸电离源（MALDI）,合成了比金属卟啉电离能高出1.3 eV的新型电离基质,用于促进金属卟啉电离。通过液液萃取富集了塔里木盆地高成熟原油（等效Ro为1.79～2.42%）中的金属卟啉。利用MALDI结合傅里叶变换离子回旋共振质谱（FT-ICR MS）实现了金属含量小于4.0 mg/kg的高成熟原油中痕量金属卟啉的分子组成分析。新发现并鉴定了10个含有1个氧原子的钒卟啉,7个含有2个氧原子的钒卟啉和1个同时含有1个氧原子和1个硫原子的钒卟啉,实现了在痕量钒卟啉和镍卟啉的同步分析,证实了在高成熟原油中存在金属卟啉化合物。并对新发现的金属卟啉的形成机理进行了讨论。 相似文献
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我国有机地球化学的发展与瞻望 总被引：4，自引：0，他引：4
我国有机地球化学的发展与瞻望郝石生①（石油大学，北京１０００８３）有机地球化学自１９３４～１９３６年ＡｌｆｒｅｄＴｔｅｉｂｓ首次鉴定和研究石油沉积物中的金属卟啉色素开始已经历了６０年的历史，现已发展为一门新兴的、成熟的、边缘交叉学科，并且拥有众多分支。 相似文献
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海洋沉积物中现存微生物化学标志物完整极性膜脂研究进展 总被引：3，自引：0，他引：3
完整极性膜脂作为活的微生物细胞的化学标志物,能够反映海洋沉积物中现存微生物群落结构和生物量等信息.与生物学方法相比,完整极性膜脂分析技术具有无需培养、快速和普适性等特点.综述了海洋沉积物中细菌和古菌的细胞膜完整极性膜脂的组成特点及其在生物地球化学和微生物生态学等研究中的应用,重点评述了在生物地球化学循环中有特殊作用的微生物,如厌氧氨氧化细菌、甲烷氧化古菌、氨氧化古菌、具有四醚膜脂结构的海洋泉古菌等,或者是一些特殊生态系统,如冷泉、海底深部生物圈等研究中完整极性膜脂应用的进展.还简要介绍了完整极性膜脂的分析方法,并对其应用前景进行了展望. 相似文献
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湖相沉积物有机地球化学在古环境研究中的应用 总被引：2，自引：0，他引：2
湖相沉积物中的有机质蕴含着丰富的地球化学信息,是古环境研究中必要的基础资料之一。文章综述了近年来湖相沉积物有机地球化学在古环境研究中的应用,结果表明:1在应用有机地球化学信息探讨古环境时,首先要根据有机质组成特征区分其来源,不同来源的有机质,其地球化学特征存在差异;2有机质碳同位素(δ13Corg)是研究古气候变化的常用指标,在区分暖湿、暖干、冷湿、冷干气候类型时需结合沉积物中总有机质丰度(TOC)、总有机氮丰度(TN)、自生碳酸盐氧同位素(δ18O)等资料;3脂肪酸不饱和度可作为恢复古环境温度的定性指标,UK37和UK37'在定量恢复古湖水表层温度中有较好的应用效果,TEX86有望应用在古湖水表层温度的重建;4生物标志化合物可较好地区分沉积物中有机质的来源、沉积水体的盐度及氧化还原性。可见,有机地球化学是研究古环境常用且有效的技术手段,多项有机地球化学参数相互验证能够更精确地重建古环境并预测其演化趋势。 相似文献
5.
地质体物质中卟啉的检出以及由叶绿素到石油卟啉演化模式的提出，增加了研究这些化石色素作为生物标志化合物的兴趣。研究表明，从原油、页岩、煤和沥青中分离的石油卟啉，主要是由脱氧叶红初卟啉(DPEP)和初卟啉(Aetio)的镍、钒络合物组成，次 相似文献
6.
量子地球化学的研究进展和发展展望 总被引：4，自引：0，他引：4
量子地球化学是应用量子力学理论研究地球物质的结构物理与结构化学的一个新理论。综述了量子地球化学理论建立以来,在矿物的结构、地球化学特征,乃至地球科学中的研究方面的最新进展,揭示了矿物中的元素分配与晶体结构等量子地球化学的研究核心,以及矿物的表面和内部电子结构、元素的分配及其动力学机制,显示量子地球化学在地球科学理论和应用领域有极广阔的前景。 相似文献
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生物标志化合物及其在石油勘探中的应用生物标志化合物(或地化化石)是在沉积物堆积时来自活生物体的分子,它们被保存下来,没有发生次生变化,或者只有很小的变化。这样就保留了其化学结构的主要持征。近年来在该领域中有很多进展。事实上,确定现代或古代沉积物中化石分子的进展与天然产物的化学研究及其在活生物体中分布的研究是平行发展,相互关联的,在一些实例中,如三萜的藿烷类,是在认识到它们广泛存在于现今活的原核生物以前,就已经在所有类型沉积物中鉴定出来。 相似文献
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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
12.
S.E. Palmer E.W. Baker L.S. Charney J.W. Louda 《Geochimica et cosmochimica acta》1982,46(7):1233-1241
Analyses of forty-two United States humic coals have revealed a striking divergence between chlorophyll diagenesis in coals when compared to the more widely studied marine sediments, shales, asphalts and petroleums. Porphyrins of humic coals have been found to be dominated by the ETIO-series, to lack members above C-32, and, in lower ranked samples (e.g. Sub-bituminous-B, high volatile C) to exhibit mass spectral envelopes with unique even-carbon number predominances. The weighted average mass, as well as the carbon number maximum (viz. mode), of these coal porphyrin homologies has been found to decrease as rank increases. The generation of porphyrins of the ETIO-series is suggested as occurring both during early coal formation, including oxidative scission of the isocyclic ring at the phorbide stage, and later during the catagenic alteration of surviving DPEP-series porphyrins. A preliminary study of chlorophyll diagenesis in a South Florida peat partially substantiates this suggestion and has further shown that the coal porphyrins can be derived from bacterial, as well as higher plant, chlorophylls. 相似文献
13.
Abelsonite has been obtained from five widely separated cores in the Green River Formation of Utah. Each occurrence was in fractures or bedding plane partings of lean oil shales. High resolution mass spectra show that the abelsonite samples are vitually identical from core to core and consist largely of the nickel complex of a C-31 porphyrin of DPEP type. 1H-NMR spectra of some of the samples have been recorded and are compared with spectra of several model nickel porphyrin complexes. From these spectra it is deduced that abelsonite is largely the nickel complex of a nor-DPEP. Abelsonite is believed to differ from nickel DPEP in having a methyl substituent in place of an ethyl substituent at either carbon 3 or 8. Abelsonite is shown not to have a hydrogen substituent on any pyrrolic carbon. A chlorophyll origin of abelsonite is thus indicated. Abelsonite appears to have been introduced into the fractures and bedding planes of the rocks in which it is found subsequent to their lithification, as porphyrins different from abelsonite were extracted from shales associated with abelsonite. 相似文献
14.
Christian B. Eckardt Lynne Dyas Peter W. Yendle Geoffrey Eglinton 《Organic Geochemistry》1988,13(4-6)
A novel method for handling and presenting multimolecular abundance data, derived from gas chromatographic-mass spectrometric analyses (GC-MS), is introduced. The method facilitates carbon number labeling of compounds, specifically in the case of porphyrins, by means of a porphyrin-index, which is part of a novel identification code for porphyrins. Identification code, relative abundance and structure information of each compound recognised are stored in a database, which affords a variety of characteristic displays and tables upon manipulation. The combined facilities allow the direct comparison of samples of different origin, maturity and/or palaeoenvironment. Correlation studies, such as oil/oil or oil/source rock, are also facilitated by comparison of characteristic “fingerprint” histogram patterns. The ability of the method is exemplified through analysis of the porphyrin distributions of Boscan oil, La Luna shale, Gilsonite bitumen and Serpiano shale. 相似文献
15.
R. Bonnett 《International Journal of Coal Geology》1996,32(1-4)
The background to recent developments in investigations on coal porphyrins is reviewed. Essentially all the work of the past ten years has been with lignites and coals of the humic series. The concentrations of porphyrins and metalloporphyrins are low (0-ca. 10 μg g−1), which makes for difficulties in isolation and analysis.The preferred methods of isolation and analysis are summarised. The coal porphyrins differ from the porphyrins from crude oil, oil shale and related deposits in a variety of ways which are discussed. The major differences are the predominance of the etio series over the cycloetio series (DPEP series), the presence of Fe and Ga porphyrins (rather than Ni and VO porphyrins), and the presence of mesoporphyrin IX in lignite.Recent results tend to support Treibs' original idea (1935) that, for the coal porphyrins, both chlorophyll and iron porphyrin (haem) sources are important. The application of a weighted mean molecular mass of the porphyrins present as a biological marker in determining coal rank (Porphyrin Index of Coalification) is illustrated. Current activity is directed to the isolation and identification of individual iron complexes, and here a combination of thin layer chromatography and paramagnetically shifted 1H-NMR spectroscopy (of dicyanoferrihaems), together with direct comparison with authentic haems especially synthesised for the purpose, has been rewarding. 相似文献
16.
焉耆盆地侏罗纪煤系源岩显微组分组合与生油潜力 总被引：3，自引：1，他引：2
焉耆盆地为我国西部含煤、含油气盆地, 侏罗系含煤地层是最重要的潜在源岩.对侏罗纪煤系中的暗色泥岩、碳质泥岩和煤层分别进行了有机岩石学、Rock-Eval热解分析和核磁共振分析.泥岩、碳质泥岩和煤层具有不同的有机岩石学和有机地球化学特征, 其中煤层具有3种有机显微组分组合类型, 不同显微组分组合类型的煤层具有不同的生油、生气潜力或倾油、倾气性.基质镜质体、角质体、孢子体等显微组分是煤中的主要生烃组分.侏罗系泥岩、碳质泥岩和煤层具有不同的生物标志物分布特征, 生物标志物组合分析表明焉耆盆地已发现原油是泥岩、碳质泥岩和煤层生成原油的混合产物.含煤地层的地球化学生烃潜力分析和已发现原油的油源对比均表明, 含煤地层不仅是重要的气源岩, 而且可成为有效的油源岩. 相似文献
17.
Sensitivity of biomarker properties to depositional environment and/or source input in the Lower Toarcian of SW-Germany 总被引：1，自引：0，他引：1
A sequence of Lower Toarcian sediments which are highly contrasting in their depositional environment over a 5 m depth interval has been investigated in detail for the variability of geochemical properties which are used for source characterization and oil-to-source correlation. Lower Liassic marls are representative of a well-aerated shallow-water environment in contrast to the immediately overlying bituminous shales which are deposited under extremely reducing conditions. Various properties have been found to vary considerably within these two units. Amongst the most important are carbon isotopic composition of the kerogen, the pristane/phytane ratios, nickel as opposed to vanadyl porphyrins, and the C27 dia-/regular steranes. Although maturation within the profile does not change, some of the maturation-dependent biomarker properties such as the monoaromatic steroid side-chain cracking and the Tm/Ts ratio exhibit large changes which can be assigned to diagenetic processes. Another maturation-dependent property, the 20S/20R epimerization of C29 steranes, exhibits smaller changes which could also be due to early diagenetic processes. The study suggests that reducing and oxidizing conditions, i.e. Eh and pH in the sediment, exert an influence on several biomarker precursor-product pathways. In maturation studies initial variations due to depositional conditions have therefore to be taken into account. 相似文献
18.
The development of three Tertiary deltaic complexes has resulted in the deposition of up to 10 km of sandstones and shales comprising the sources and reservoirs for crude oils that occur onshore, near-offshore and, with future exploration efforts, those likely to be encountered in deepwater reservoirs north of the Brunei coastline. We examined a series of offshore oils and onshore rock samples in Brunei Darussalam (a) to delineate oil family groups and their source rock characteristics, and (b) to assess the source potential of the sedimentary sequence with respect to lithology and depositional setting. Twelve offshore oils and 53 shales, coaly shales and coals were examined. The oils contain indicators of allochthonous (e.g. bicadinanes, oleananes) and autochthonous (e.g. cholestanes and methylcholestanes) components in the source organic matter. Predictable geographic variations of this mixed input are clearly evident in the sample set (e.g. allochthonous input appears to increase in offshore Brunei to the northeast). Although this molecular source signature is relatively clear, migration of these oils from deep (and unidentified) source rocks has resulted in extensive migration-contamination with respect to the tetracyclic and pentacyclic hydrocarbons. This contamination has resulted in strong correlations between certain molecular maturity indicators and the present-day temperature of the reservoirs. Liquid hydrocarbon source rock potential is present in the tidal and coastal embayment facies, and is greatest in the Miocene coals. Neither the shales nor coaly shales contain significant oil generative potential. The thermal immaturity of the sample set precludes valid oil–source rock correlations without conducting artificial maturation experiments on the coals. 相似文献
19.
Immature samples of the Permian Kupferschiefer from the Lower Rhine Basin in N.W. Germany were analysed for tetrapyrrole pigment type and abundance. The sediment, thought to have been deposited in a marine regime with enhanced salinity, was found to contain high concentrations of metalloporphyrins. The porphyrins are complexed to nickel (Ni) and oxovanadium (V=0), but high abundances of iron (Fe) porphyrins were also detected using UV/visible spectroscopy and mass spectrometry. The presence in the latter of series of aetioporphyrins, cycloalkanoporphyrins, di-cycloalkanoporphyrins and benz-cycloalkanoporphyrins was confirmed by accurate mass measurements; HPLC co-injection of deoxophylloerythroetioporphyrin (C32 DPEP) with the demetallated iron porphyrins indicated its presence in the sediment as an iron complex. The study provides the first evidence for the occurrence of Fe porphyrins in geological samples other than coals and lignites, and reports the highest concentrations in sedimentary organic matter to date. 相似文献
20.
Manzur Ahmed Herbert Volk Simon C. George Mohinudeen Faiz Linda Stalker 《Organic Geochemistry》2009,40(7):810-831
Organic geochemical and petrological assessment of coals/coaly shales and fine grained sediments, coupled with organic geochemical analyses of oil samples, all from Permo–Triassic sections of the Southern Sydney Basin (Australia), have enabled identification of the source for the widely distributed oil shows and oil seeps in this region. The Permian coals have higher hydrogen indices, higher liptinite contents, and much higher total organic matter extract yields than the fine grained sediments. A variety of source specific parameters obtained from n-alkanes, regular isoprenoids, terpanes, steranes and diasteranes indicate that the oil shows and seeps were generated and expelled predominantly from higher plant derived organic matter deposited in oxic environments. The source and maturity related biomarkers and aromatic hydrocarbon distributions of the oils are similar to those of the coals. The oil-coal relationship also is demonstrated by similarities in the carbon isotopic composition of the total oils, coal extracts, and their individual n-alkanes. Extracts from the Permo–Triassic fine grained sediments, on the other hand, have organic geochemical signatures indicative of mixed terrestrial and prokaryotic organic matter deposited in suboxic environments, which are significantly different from both the oils and coal extracts. The molecular signatures indicating the presence of prokaryotic organic matter in some of the coal extracts and oils may be due to thin sections of possibly calcareous lithologies interbedded within the coal measures. The genetic relationship between the oils and coals provides new evidence for the generation and expulsion of oils from the Permian coals and raises the possibility for commercial oil accumulations in the Permian and Early Triassic sandstones, potentially in the deeper offshore part of the Sydney Basin. 相似文献