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为研究实际地质体或地质剖面中的C31到C3517α(H), 21β(H)升藿烷生物标志物构型转化参数22S/(22S+22R)及升藿烷指数C35/∑（C31—C35)等的分布、演化特征,对东营凹陷主要烃源岩层系古近系沙河街组三段（淡水—微咸水层系）和沙河街组四段（咸水层系）的系列样品进行了研究,分析样品来源于1 300~4 000的暗色泥岩,其中2 800~4 000 m的样品对应于东营凹陷古近系烃源岩的生油初期到生油晚期。研究结果表明,C31、C32、C33、C34、C35升藿烷（17α(H), 21β(H)）构型转化参数的分布除与异构体之间的手性碳立体构型转化作用有关外,不同异构体之间降解或裂解速率和新生成速率的差异也是其主要控制因素,沉积环境（如高盐环境）也在一定程度上影响了其分布;从未熟—低熟状态到成熟状态,相关升藿烷构型转化参数22S/(22S+22R)总体均表现出随埋藏深度增大而加大的特点,并从离散状态聚集到热演化的平衡状态附近;在到达成熟状态后,相关升藿烷的构型转化参数22S/(22S+22R)从缓慢增大过渡到一个持续的热演化平衡状态,并且该构型转化参数的热演化平衡状态对应于生油门限附近;在高盐环境中除C33升藿烷保持不变的热演化平衡状态外,其它升藿烷均呈现不同幅度的逆转特征,表明高含量的盐类矿物对升藿烷成熟度参数亦具有抑制作用或迟缓效应;C31、C32、C33、C34、C3517α升藿烷之间的22S/(22S+22R)分布型式复杂多变,其中对于成熟源岩样品,C35升藿烷22S/(22S+22R)值变化强烈,表现出“翘尾”状的上升型特征和“坠尾”状的下降型特征,而对于低熟—未熟样品, C32升藿烷的22S/(22S+22R)显示相对高值,并且多数样品显示为C31C33C35的偶数碳优势的特征;研究显示C31到C33升藿烷的构型转化参数S/(S+R)热演化平衡值均为0.6,而C34 S/(S+R)及C35S/(S+R)热演化平衡值相对较高,沙三段、沙四段的C34 S/(S+R)及沙四段的C35S/(S+R)分别达到0.63、0.62、0.65;升藿烷指数C35/∑（C31—C35)受热演化影响也比较明显,在生油期间随着埋藏深度增加而减小,在高盐环境中表现出相对高值,研究表明该指数的变化与其22R异构体演化有关,并且参数C31/∑（C31—C35）、C32/∑（C31—C35）、C33/∑（C31—C35）、C34/∑（C31—C35）、C35/∑（C31—C35)演化特征截然不同。 相似文献
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The reactions of alkoxy radicals determine to a large extent the products formed during the atmospheric degradations of emitted organic compounds. Experimental data concerning the decompositions, 1,5-H shift isomerizations and reactions with O2 of several classes of alkoxy radicals are inconsistent with literature estimations of their absolute or relative rate constants. An alternative, although empirical, method for assessing the relative importance under atmospheric conditions of the reactions of alkoxy radicals with O2 versus decomposition was derived. This estimation method utilizes the differences in the heats of reaction, (H)=(Hdecomposition–HO
2
reaction), between these two reactions pathways. For (H)[22–0.5(HO
2
reaction)], alkoxy radical decomposition dominates over the reaction with O2 at room temperature and atmospheric pressure of air, while for (H)[25-0.5(HO
2
reaction)], the O2 reaction dominates over decomposition (where the units of H are in kcal mol–1). The utility and shortcomings of this approach are discussed. It is concluded that further studies concerning the reactions of alkoxy radicals are needed. 相似文献
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LI Sumei 《中国地质大学学报(英文版)》2002,13(4)
31 samples of shales and mudstones developed in reducing hypersaline and freshwater setting and 20 oil samples of Bamianhe oilfield, Bohai Bay basin were collected for a detailed study of petroleum system. Composition and distribution, especially significance of steroids, are discussed as a part of those. Abundant steroidal biomarkers, including C27-29 regular steranes, C28-30 4-methyl steranes, dinosteranes and aromatic steranes, were detected. Results show that the composition and distribution of the steroids in samples studied are functions of thermal maturity, organic source, paleoenvironment and lithology of potential source rocks. Alga-rich Es4 shales (brackish water) developed in the south slope of depocenter (Niuzhuang sag) were found particularly rich in steroidal biomarkers including C30 4-methyl steranes and dinosteranes. Es3 mudstones (fresh water) were found devoid of dinosteranes. Distribution patterns of regular steranes are completely different from methyl steranes indicating different origins of the specific compounds of the fraction. Diagnostic distribution of steranes in rock extracts of diverse intervals makes the compounds to be essential indictors of source-rock tracing. Methyl steranes prove to be much more useful in oil-source rock correlation than regular steranes. Results also show that alga-rich Es4 shales located in the south slope are not likely the primary source rock responsible for the oils discovered based on the composition and distribution of steroids. 相似文献
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异构比φiC4 /φnC4 和φiC5 /φnC5 的石油地质意义 总被引：6，自引：1，他引：6
同分子量的正构烷烃和异构烷烃存在着物理化学性质差异,在运移过程中受围岩的物理化学性质及其它外部因素的影响必然产生分异效应,从而使二者在空间分布上具有一定的特征和规律,异构比指标可以在一定程度上反映出这种特征和规律性。用异构比φiC4 /φnC4 和φiC5 /φnC5 指标可以判断有机质的成熟度,研究轻烃运移的途径、方向、生成环境及轻烃的生物降解。 相似文献
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The study of geochemical transformations undergone by ‘biological markers’ after their incorporation into sediments is an important field of organic geochemistry. Combined with laboratory simulation experiments, molecular mechanics calculations have been shown to be very useful to establish the reaction pathways, and to predict intermediate components and stable reaction end products, especially in the case of the acid-catalyzed isomerization reactions of steroid and terpenoid hydrocarbons. Many commercially available softwares are able to optimize (minimize) the geometries of molecules and compute some of their thermodynamical data with either molecular mechanics (MM) or semi-empirical methods of quantum chemistry. In order to verify the reliability of these methods, we have computed the relative thermodynamic stabilities of a large number of steradiene isomers with MM3 (Tripos Inc.), MM+ (HYPERCHEMTM) and MM2 (Chem3D, CambridgeSoft Corp.) empirical force fields, and with AM1 and PM3 (HYPERCHEMTM) semi-empirical methods. The calculation results of thermodynamic stabilities of steradiene isomers are used to explain the compounds produced by the rearrangement of cholesta-3,5-diene when treated with p-toluenesulfonic acid in acetic acid at 70°C. The end products, namely the spirosteradienes 7–8, obtained by this treatment are the most stable steradiene isomers according to all computational methods. The relative thermodynamic stabilities of cholestadienes are also consistent with the mechanism postulated for the spirosteradiene formation proceeding through a pathway including cholestadienes 2–6 as intermediates. 相似文献
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