珠江口盆地恩平组泥页岩全岩及干酪根生烃动力学实验及初步应用研究
Kinetic pyrolysis simulation of hydrocarbon generation in shale system: A case study on Pearl River Mouth Basin, China
查看参考文献24篇
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文摘
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在限定体系(密封金管-高压釜体系)下, 采用珠江口盆地下渐新统恩平组低成熟度碳质泥页岩全岩及分离干酪根样品进行了生烃热模拟实验。在24.1MPa 压力条件下, 以20 ℃/h (373.5~525.0 ℃)和2℃/h(343.0~489.2℃)升温速率实验测定了气态烃类的生成量和化学组成。实验结果采用Kinetics 05生烃动力学软件模拟获得了有机质裂解生成甲烷及同系物等气态烃形成的动力学参数。结果表明, 泥页岩不同升温速率(2℃/h 和20 ℃/h)有机质热裂解过程中, 相同温度下, 全岩样品的气态烃产量和C_2–C_4等重烃气体的转化率明显低于干酪根样品, 但两者的甲烷转化率相近。全岩及干酪根具有相似的甲烷、乙烷、丙烷及丁烷的活化能分布(52×4.1840~64×4.1840 kJ/mol)。干酪根的分离对动力学参数几乎没有影响。对比表明, 干酪根热解生气的两个温度段为: 135.0 ~165.0 ℃和165.0 ~190.0 ℃, 液态烃二次裂解生气的两个温度段为: 190.0 ~225.0 ℃和225.0 ~260.0 ℃。热模拟晚期阶段重烃产量降低和甲烷产量的持续增加与早期形成的高碳数烃类分解有关。应用动力学方法外推到珠江口盆地的地质条件, 表明珠江口盆地在约19.6Ma 干酪根开始裂解生气, 目前仍处于干酪根裂解生气阶段。 |
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其他语种文摘
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Pyrolysis experiments were performed in a closed system of sealed gold tube using both whole rock and its kerogen separated from the low maturity carboniferous shale of the Lower Oligocene Enping Formation in the Pearl River Mouth Basin, China. The pyrolysis temperatures range from 373.5 to 525.0 ℃ and from 343.0 to 489.2 ℃ with heating rate of 20 ℃/h and 2 ℃/h, respectively. The pyrolysis pressure keeps constant at 24.1 MPa. The gaseous hydrocarbons released in pyrolysis have been analyzed for their yields and chemical compositions. The simulation data were used to calculate kinetic parameters (activation energy distribution and pre-exponential factor) in the generation of gaseous hydrocarbons by software Kinetics 05. The results showed that the yields of CH_4 from whole rock and its kerogen continually increase with increasing heating temperatures. Whereas, the yields of C_2H_6, C_3H_8 and C_4H_(10) firstly increased at the early stage of kerogen cracking but decreased thereafter. The whole rock shows significantly lower yields of gaseous hydrocarbons and lower conversion rate of C_2–C_4 than its kerogen at the same temperature. But whole rock showed conversion rate of CH_4 similar to its kerogen. At the same temperatures, the yields and conversion rate of gaseous hydrocarbons at the heating rate of 2 ℃/h are higher than those at the heating rate of 20 ℃/h. Whole rock and its kerogen show similar distributions of activation energies in the generation of CH_4, C_2H_6, C_3H_8 and C_4H_(10), ranging from 52×4.1840 kJ/mol to 64×4.1840 kJ/mol. Hydrocarbon generation kinetics of shale and its kerogen show that gaseous hydrocarbon is formed by kerogen cracking at two temperature intervals of 135.0–165.0 ℃ and 165.0–190.0 ℃, respectively. Similarly, gaseous hydrocarbon is formed by cracking of liquid hydrocarbon at two temperature intervals of 190.0–225.0 ℃ and 225.0–260.0 ℃. The continuous increase of the yield of methane is accompanied by the decrease of heavy hydrocarbons at the late stage of pyrolysis. It could be related to the decomposition of high carbon number hydrocarbons that are generated at the early stage of hydrocarbon generation. The kinetic parameters of gaseous hydrocarbon generation had been extrapolated to the geological conditions of the Pearl River Mouth Basin. It suggests that the Pearl River Mouth Basin started to generate gaseous hydrocarbon by kerogen cracking at ca. 19.6 Ma, and it is currently at the stage of kerogen cracking. |
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来源
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地球化学
,2014,43(5):518-528 【核心库】
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关键词
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烃源岩
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干酪根
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生烃动力学
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模拟实验
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珠江口盆地
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地址
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1.
兰州大学地质科学与矿产资源学院, 甘肃省西部矿产资源重点实验室, 甘肃, 兰州, 730000
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中国科学院广州地球化学研究所, 有机地球化学国家重点实验室, 广东, 广州, 510640
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语种
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中文 |
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文献类型
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研究性论文 |
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ISSN
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0379-1726 |
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学科
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地质学 |
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基金
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国家973计划
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教育部科学技术研究重大项目
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国家自然科学基金
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中国科学院广州地球化学研究所有机地球化学国家重点实验室基金
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兰州大学博士研究生学术新人奖基金
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文献收藏号
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CSCD:5268926
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