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Quantitative pyrolysis-gas chromatography has been performed on 96 kerogen samples isolated from 17 wells on the Norwegian Continental shelf. Petrographic and bulk geochemical measurements were also performed on the samples, and a combined data set of 117 variables for each sample was analysed using principal components analysis (PCA). This approach provides an objective and reproducible means of kerogen characterisation, which can be easily automated. In addition to objective kerogen characterisation and facile visualisation of facies and maturity related chemical trends, the method has the potential to allow objective prediction of key geochemical parameters such as maturity level from pyrogram data. 相似文献
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Steve Larter 《International Journal of Earth Sciences》1989,78(1):349-359
A global kinetic model of vitrinite reflectance evolution is developed to illustrate a new approach to vitrinite reflectance modelling. The method utilizes quantitative pyrolysisgas Chromatographic data from isolated vitrinite kerogens to derive the concentrations of structurally specific moieties (alkylphenol precursors) in vitrinite kerogens as a function of rank. This data set is used to calibrate a gaussian distributed activation energy model for phenol-precursor loss from vitrinites using published burial histories. Phenol yield is then correlated with vitrinite reflectance. The predictive vitrinite reflectance model based on this phenol system is tested against a well from the US Gulf Coast area, the results being compared with a Lopatin model of the same well. This type of vitrinite reflectance model is numerically compatible with current generation kinetic models of hydrocarbon production from source rock kerogens, and has a better heating rate independence than Lopatin's method.
Zusammenfassung Um eine neue Annäherung an das Modellieren der Vitrinit-Reflexion zu demonstrieren, wurde ein global-kinetisches Modell der Entwicklung der Vitrinit-Reflexion erstellt. Die Methode verwendet Daten von quantitativer Pyrolyse-Gas Chromatographie isolierten Vitrinitkerogens, um die Konzentration von strukturspezifischen Moieten (Alkylophenol-Vorläufer) in Vitrinitkerogen als Funktion der Reihenfolge zu erhalten. Verwendet werden diese Daten, um ein nach Gauss verteiltes Aktivierungsenergiemodell zu kalibrieren, das mit Hilfe von veröffentlichten Ablagerungsgeschichten den Phenol-Vorläuferverlust von Vitriniten beschreibt. Die Phenol-Ausbeute wird dann mit der Vitrinit-Reflexion korreliert. Das auf dem Phenolsystem basierende Vitrinit-Reflexionsmodell wird in einem Test einem Bohrloch an der amerikanischen Golfküste gegenübergestellt. Die Ergebnisse werden mit dem Lopatinmodell des selben Bohrlochs verglichen. Diese Art eines Vitrinit-Reflexionsmodells ist numerisch wettbewerbsfähig mit der heutigen Generation kinetischer Modelle der Kohlenwasserstofferzeugung aus Trägergesteinskerogenen. Außerdem ist seine Unabhängigkeit von der Erhitzungsrate größer als mit der Lopatin-Methode.
Résumé L'auteur présente un modèle cinétique global de l'évaluation du pouvoir réflecteur de la vitrinite, afin d'illuster une approche nouvelle dans la modélisation de ce pourvoir réflecteur. Cette méthode utilise des données quantitatives fournies par la pyrolyse combinée à la Chromatographie en phase gazeuse et relatives à des kérogènes de vitrinite. A partir de ces données, on exprime les concentrations des fractions à structure spécifique dans les kérogènes vitrinitiques en fonction du degré d'évolution. A partir de cet ensemble de données, on établit un modèle de l'énergie d'activation selon une distribution gaussienne, applicable à la perte de phénol-précurseur dans les vitrinites, en se référant à cet effet aux déroulements historiques de l'enfouissement fournis par la littérature. La production de phénol est alors mise en relation avec le pourvoir réflecteur de la vitrinite. Le modèle du pouvoir réflecteur prévisible, basé sur ce système des phénols a été contrôlé dans un forage de la côte du golfe du Mexique (USA), et les résultats comparés à ceux du modèle de Lopatin appliqué au même forage. Le modèle présenté est numériquement compatible avec les modèles cinétiques habituels qui rendent compte de la production d'hydrocarbure à partir des kérogènes des roches-mères; il présente une meilleure indépendance que la méthode de Lopatin par rapport au taux d'échauffement.
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A series of hand-picked vitrinite samples from the Lower Kittanning Seam, Pennsylvania have been examined using quantitative pyrolysis-gas chromatography. These vitrinites ranged in rank from 0.59 to 1.71% reflectance, a rank range from high volatile C bituminous to low volatile bituminous. High molecular weight pyrolysis products included alkyl aromatic and phenolic compounds. Attempts have been made to correlate the pyrolysis product composition to rank parameters including vitrinite reflectance, volatile matter yield, carbon content, atomic H/C ratio and Rock-Eval determined Tmax. Total yield of phenols was found to be strongly and inversely rank related. A clear relationship between C8 alkyl-benzene yield and rank was not found for the sample set. 相似文献
4.
Sunil Bharati Richard L. Patience Steve R. Larter Guy Standen Iain J. F. Poplett 《Organic Geochemistry》1995,23(11-12)
The significance and validity of integrating data obtained from a variety of analytical techniques to understand, elucidate and model kerogen's complex chemical structure is reported here using degradative (open and closed system pyrolysis, chemical oxidation), non-degradative (13C CP/MAS NMR) and optical (incident white light and blue light) methods. Seven Cambrian Alum Shale samples, ranging in maturity from immature to post-mature with respect to petroleum generation, were studied and were chosen for their simple geological history, uniform organic matter type and high organic carbon content. The Alum Shale kerogens, which primarily consist of algal organic matter, liberate low molecular weight gaseous and aromatic compounds on pyrolysis and give mostly branched dicarboxylic acids on chemical oxidation. 13C NMR spectroscopy shows that the Alum Shale kerogens are anomalously rich in oxygen-bearing functional groups (such as C = O, ArCO, CHO, CHxO), most of which apparently remain intact within the kerogen macro-molecule (KMM) through the diagenetic and catagenetic stages. Fragments released by different degradative techniques are quantified and the aromaticity (fa), O/C and relative proportions of various carbon types estimated by 13C NMR. A synthesis of these data has allowed us to better understand the chemistry of the Alum Shale kerogen. 相似文献
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Melanoidins, acidic polymeric products of amino acid/sugar condensation reactions, are shown to be capable of reacting with and binding functionalized lipid molecules. Pyrolysis gas chromatography is used to monitor the inclusion of lipids (alcohols and acids) into, and to monitor the changes in composition caused by artificial diagenesis of, the melanoidins. Artificial diagenesis of the lipidcontaining melanoidins produces a material resembling kerogen. The possible role of melanoidins in the formation of kerogens is discussed as are internal transformations within kerogens during diagenesis. 相似文献
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A geochemical investigation of oils in sandstone core plugs and drill stem test oils was carried out on samples from a North Sea reservoir. A sample of diesel used as a constituent of the drilling fluids was also analysed. The aliphatic and aromatic hydrocarbons and polar non-hydrocarbons were isolated using solid phase extraction methods. GC analysis of the hydrocarbon fraction of the core extract indicated that contamination may be diesel derived. From analysis of diesel some compound classes are less likely to be affected by contamination from diesel itself including: steranes, hopanes, aromatic steroid hydrocarbons, benzocarbazoles and C0–C3-alkylphenols. 相似文献
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Barry Bennett Arnaud Lager Christopher A. Russell Gordon D. Love Stephen R. Larter 《Organic Geochemistry》2004,35(11-12):1427
Nitrogen compounds are ubiquitous in fossil fuels and yet our understanding of their origins in the geosphere is limited. In this study, high hydrogen pressure pyrolysis was performed on sample material representing potential contributors to sedimentary organic matter (algae, bacteria and archaea) and sediments representing early diagenetic accumulations from Lake Pollen (Norway) and Priest Pot (UK). Previous workers demonstrated the structurally conservative nature of high hydrogen pressure pyrolysis in that the technique maximizes the yields of covalently bound hydrocarbon biomarkers from organic matter without adversely affecting their stereochemistry (Love et al., 1995). Release of covalently bound biomarkers in high yields from kerogen via catalytic hydropyrolysis. In this study, the types and distributions of organic nitrogen compounds in the hydropyrolysates were characterised under similar conditions to such experiments where biomarker hydrocarbons undergo minimal rearrangement. Compounds identified by gas chromatography–mass spectrometry included alkyl-substituted indoles, carbazoles, benzocarbazoles, quinolines and benzoquinolines.Indoles are present in all hydropyrolysates, suggesting a common origin. A potential source of indoles is represented by tryptophan which was shown to degrade through a series of alkylated intermediates to indole. Carbazole, quinoline and benzoquinoline were also found in the hydropyrolysates of algae, bacteria and archaea. The presence of these petroleum-related nitrogen compounds in hydropyrolysates generated from biomass suggests an early origin for petroleum nitrogen compounds. A potential source of naturally occurring nitrogen compounds such as that in the alkaloids has yet to be realised.Benzocarbazoles were absent from hydropyrolysates of algae, bacteria and archeae, but present in those from recent sediments, suggesting their presence may be related to processes occurring during early diagenesis at, or immediately below, the sediment–water interface. In sediments from Lake Pollen, changes in the benzocarbazole ratio [a]/([a] + [c]) ratio coincides with the interval described as a transition from fjord to lake environment, suggesting that benzocarbazoles are sensitive to changes in depositional environment and may have potential to act as a marker for environmental conditions. 相似文献
10.
Roy Livermore Alex Cunningham Lieve Vanneste Robert Larter 《Earth and Planetary Science Letters》1997,150(3-4):261-275
Despite a spreading rate of 65–70 km Ma−1, the East Scotia Ridge has, along most of its length, a form typically associated with slower rates of sea floor spreading. This may be a consequence of cooler than normal mantle upwelling, which could be a feature of back-arc spreading. At the northern end of the ridge, recently acquired sonar data show a complex, rapidly evolving pattern of extension within 100 km of the South Sandwich Trench. New ridge segments appear to be nucleating at or near the boundary between the South American and Scotia Sea plates and propagating southwards, supplanting older segments. The most prominent of these, north of 56°30′S, has been propagating at a rate of approximately 60 km Ma−1 for at least 1 Ma, and displays a morphology unique on this plate boundary. A 40 km long axial high exists at the centre of this segment, forming one of the shallowest sections of the East Scotia Ridge. Beneath it, seismic reflection profiles reveal an axial magma chamber, or AMC, reflector, similar to those observed beneath the East Pacific Rise and Valu Fa Ridge. Simple calculations indicate the existence here of a narrow (<1 km wide) body of melt at a depth of approximately 3 km beneath the sea floor. From the topographic and seismic data, we deduce that a localised mantle melting anomaly lies beneath this segment. Rates of spreading in the east Scotia Sea show little variation along axis. Hence, the changes in melt supply are related to the unique tectonic setting, in which the South American plate is tearing to the east, perhaps allowing mantle flow around the end of the subducting slab. Volatiles released from the torn plate edge and entrained in the flow are a potential cause of the anomalous melting observed. A southward mantle flow may have existed beneath the axis of the East Scotia Ridge throughout its history. 相似文献