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21.
《Chemie der Erde / Geochemistry》2014,74(4):681-690
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
22.
应用高压封闭体系,对海相碳酸盐岩干酪根进行了热裂解模拟实验,并从气态烃、非气态烃产率及碳同位素演化特征等方面,探讨了海相碳酸盐岩烃源岩干酪根作为气源的生气机理。在模拟实验基础上,结合专用Kinetics软件求取碳酸盐岩烃源岩干酪根裂解产气动力学参数(活化能和指前因子),并将模拟实验结果外推至地质条件下,探讨其动力学模型的实际应用。结果表明,在该地质条件下,甲烷在EasyRo为0.9%时进入主生气期(转化率为10%),2.9%时主生气期结束(转化率为90%)。乙烷至戊烷在EasyRo为1.1%时进入主生气期(转化率10%),2.7%时主生气期结束(转化率90%)。该研究成果为我国海相碳酸盐岩裂解气的判识、资源评价提供了可靠的实验依据。 相似文献
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24.
Kevin G. Knauss Sally A. Copenhaver Robert L. Braun Alan K. Burnham 《Organic Geochemistry》1997,27(7-8)
Hydrous pyrolysis in flexible gold-bag autoclaves was used to study the production of carboxylic acids and light hydrocarbons from two marine type IIb source rocks (New Albany and Phosphoria Shales). Kerogen pyrolysis produced significant amounts of the monocarboxylic acids (acetic > propionic > butyric). The gases were dominated by CO2 and methane, in that order, and progressively smaller amounts of the alkanes (ethane > propane > butane > pentane). Kinetic analyses of production rates for the New Albany Shale suggest mean activation energies (E) of 51-54 kcal/mol for both the light hydrocarbons and acids. Pressure had little effect on measured production rates for either shale over the pressure range investigated. Chemical thermodynamic speciation modeling suggests that in these experiments metal-organic acid anion complexation had little impact on aluminum speciation/solubility, but was important with respect to the alkaline earths. 相似文献
25.
The degradation and preservation affecting the biomarker record of ancient metazoa are not fully understood. We report on a five month experiment on the fate of fatty acids (FAs) during the degradation of recent whale vertebrae (Phocoena phocoena). Whale bones were analysed for extractable FAs and macromolecularly bound n-acyl compounds. Fresh bone showed extractable FAs dominated by 16:1ω7c, 16:0, 18:1ω9c and 18:0. Calculated degradation rate constant (k) values showed a rapid decrease in FA concentration, with k values higher for unsaturated than for saturated compounds (0.08/day for 18:1ω9c, 0.05/day for 16:0). The appearance or increased abundance of distinctive methyl branched (e.g. i/ai-15:0 and -17:0, 10Me-16:0) and hydroxy FAs (e.g. 10OH-16:0 and 10OH-18:0) were observed, providing clear evidence for the microbial degradation of bone organic matter and an input of lipids from specialised bacteria. Catalytic hydropyrolysis (HyPy) of demineralised extraction residues released up to 0.13% of the total n-C16 and n-C18 moieties in the degraded bones. This revealed that only a small, yet sizeable, portion of bone-derived fatty acyl units was sequestered into (proto)kerogen during the earliest stages of degradation. 相似文献
26.
The mechanical properties of organic matter strongly affect the way shales deform and fracture. However, the way organic matter responds to mechanical stresses is poorly understood, representing a critical obstacle to assessing oil and gas production in shale formations. Little is known about the mechanical properties of organic matter in fine grained rocks primarily because it often occupies tiny nanometer-scale voids between the mineral grains which cannot be accessed using standard mechanical testing techniques. Here, we use a new atomic force microscopy technique (PeakForce QNM™) to map the mechanical properties of organic and inorganic components at the nanometer scale. We find that the method is able to distinguish between different phases such as pyrite, quartz, clays, and organic matter. Moreover, within the organic component Young's modulus values ranged from 0 to 25 GPa; in 3 different samples – all of which come from thermally mature Type II/III source rocks in the dry gas window – a modal value of 15–16 GPa was measured, with additional peaks measured at ≤10 GPa. In addition, the maps suggest that some porous organic macerals possess a soft core surrounded by a harder outer shell 50–100 nm thick. Thus, our results demonstrate that the method represents a powerful new petrographic tool with which to characterize the mechanical properties of organic-rich sedimentary rocks. 相似文献
27.
Nikolaos Kontopoulos Teresa Fokianou Abraham Zelilidis Christos Alexiadis Nikolaos Rigakis 《Marine and Petroleum Geology》1999,16(8):223
Two depocentres, >4200 m and >3200 m thick, have been recognized in the Mesohellenic piggy-back basin of middle Eocene to middle Miocene age, where submarine fans have accumulated unconformably over an ophiolite complex. The hydrocarbon potential is indicated by the presence of kerogen types II/III with minor amounts of type I; the evidence is mostly for wet gas and gas, with minor oil. Source rocks are the middle Eocene to lower Oligocene Krania and Eptachori formations, of up to 2000 m total thickness, reaching maturation during the early Miocene. The source rocks consist of outer fan and basin plain deposits. They are conformably overlain by the lower member (late Oligocene) of the up to 2600 m thick Pentalophos Formation, which consists mostly of thick submarine sandstone lobes. Possible stratigraphically trapped reservoirs include the lower member of the Pentalophos Formation, which overlies source rocks, as well as limestones tectonically intercalated within the ophiolite complex, underlying the source rocks. Traps may have formed also on the western side of an internal thrust (Theotokos Thrust), which influenced the evolution of the depocentres. 相似文献
28.
The “free” or “natural” light hydrocarbon composition obtained by thermal extraction-GC of source rock samples is compared with the light fraction generated by pyrolysis products of the kerogens. Even though there are large differences between the composition of the “free” C4–C13 hydrocarbon fraction and the same fraction generated by pyrolysis, some characteristics have been detected which can be used interchangeably for both data types. Visual inspection of gas chromatograms from thermal extracts and pyrolysates indicates that in particular the relative content of m+p xylene corresponds well between these two analytical methods. The source rock samples used are Upper Jurassic marine shales and Middle and Lower Jurassic coals and coaly shales from offshore Mid-Norway and Denmark. More detailed analysis of the data shows that the most effective parameter which can distinguish between different source rock types in both thermal extracts and pyrolysates is the m+p xylene/nC8 ratio. This parameter has been used to derive classification diagrams for interpreting the source of light hydrocarbons of both natural petroleum fluids analysed by gas chromatography and the same fraction generated by pyrolysis of asphaltenes from the fluids.The model was first tested on 17 natural petroleum fluids from Mid-Norway since a comprehensive study of light hydrocarbon distributions already has been published. Further, the parameter was applied to correlate with asphaltene pyrolysates of the fluids from Mid-Norway and a total of 22 natural oils and condensates from the southernmost Norwegian and Danish sectors. 相似文献
29.
This article reviews the abnormal characteristics of shale gases (natural gases produced from organic-rich shales) and discusses the cause of the anomalies and mechanisms for gas enrichment and depletion in high-maturity organic-rich shales. The reported shale gas geochemical anomalies include rollover of iso-alkane/normal alkane ratios, rollover of ethane and propane isotopic compositions, abnormally light ethane and propane δ13C values as well as isotope reversals among methane, ethane and propane. These anomalies reflect the complex histories of gas generation and associated isotopic fractionation as well as in-situ “mixing and accumulation” of gases generated from different precursors at different thermal maturities. A model was proposed to explain the observed geochemical anomalies. Gas generation from kerogen cracking at relatively low thermal maturity accounted for the increase of iso-alkane/normal alkane ratios and ethane and propane δ13C values (normal trend). Simultaneous cracking of kerogen, retained oil and wet gas and associated isotopic fractionation at higher maturity caused decreasing iso-alkane/normal alkane ratios, lighter ethane and propane δ13C and corresponding conversion of carbon isotopic distribution patterns from normal through partial reversal to complete reversal. Relatively low oil expulsion efficiency at peak oil generation, low expulsion efficiency at peak gas generation and little gas loss during post-generation evolution are necessary for organic-rich shales to display the observed geochemical anomalies. High organic matter richness, high thermal maturity (high degrees of kerogen-gas and oil-gas conversions) and late-stage (the stage of peak gas generation and post-generation evolution) closed system accounted for gas enrichment in shales. Loss of free gases during post-generation evolution may result in gas depletion or even undersaturation (total gas content lower than the gas sorption capacity) in high-maturity organic-rich shales. 相似文献
30.
碳酸盐岩干酪根催化降解生烃过程及动力学研究 总被引：8，自引：0，他引：8
以甘肃平凉地区奥陶系碳酸盐岩干酪根为对象,利用热模拟实验方法和化工催化原理,从热解生烃组成特征、生烃量及生烃动力学等方面考察了不同介质对干酪根热解生烃过程的影响。结果表明,碳酸盐岩对干酪根生烃过程具有反催化作用,随着温度的增加,反催化作用越明显。膏岩CaSO4则表现出正催化作用,各种盐类对干酪根生烃过程影响较小。干酪根热解动力学研究表明,生烃动力学参数活化能E与视频率因子A之间不是独立变化的,它们之间存在一定的关系,即:E与lnA呈线形关系,这对于认识碳酸盐岩干酪根的化学结构及热解生烃机理具有一定的参考价值。 相似文献