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在开放、变温热解实验中,对三个碳酸盐岩样品进行了在线特定化合物C/~(12) 稳定同位素分析,其中三个样品分别取自德国西北(石炭系Westphalian煤岩,I_H=286 mgHC/gTOC,R_o=0.72％)、西西伯利亚(白垩系Cenomanian页岩,I_H=192mgHC/gTOC,R_o=0.36％)和马来西亚(三叠系Miocene煤岩,I_H=190mgHC/gTOC,R_o=0.36％)。主要研究对象为甲烷、乙烷和丙烷+丙烯,测得的热解产物碳同位素值分布在热成因天然气范围内(—20‰～—40‰)。热解产物表现出随着热模拟温度升高,一般富集~(13)C,然而,甲烷碳同位素在某些温度段表现出倒转现象。在实验数据分析基础上,利用平行一级反应和Arrhenius温度方程得出反应动力学参数,将Westphalian煤岩得到的动力学参数应用到地热演化史中建立德国西北盆地气藏中天然气生成与聚集过程中组份和同位素组成变化模型。热模拟甲烷计算获得的碳同位素值表现出与德国西北天然气田的碳同位素特征一致。同位素反应动力学结合区域热演化史能有效地解释在天然气聚集过程中同位素组成变化特征。研究结果表明,虽然热解实验与地质条件有着本质区别,但开放、变温热解实验能提供一些有意义的同位素反应动力学参数,这些参数能满意地描述在地质系统中天然气生成过程中的同位素效应。在盆地建模中,应用这些?
In open and variable temperature pyrolysis experiments, three carbonate samples were subjected to an online C / ~ (12) stable isotope analysis, of which three samples were taken from northwestern Germany (Carboniferous Westphalian coal, I_H = 286 mg HC / g TOC, R_o = 0.72%), western Siberia (Cretaceous Cenomanian shale, I_H = 192mgHC / gTOC, R_o = 0.36%) and Malaysia (Triassic Miocene coal, I_H = 190mgHC / gTOC, R_o = 0.36%). The main research objects are methane, ethane and propane + propylene. The measured carbon isotopic values of pyrolysis products are distributed in the range of (-20 ‰ ~ -40 ‰) of natural gas. The pyrolyzed products generally show the enrichment of ~ (13) C with increasing temperature of the thermal simulation. However, the carbon isotope of methane shows a reversal at some temperature. Based on the experimental data analysis, the kinetic parameters were obtained by using the parallel first-order reaction and the Arrhenius temperature equation, and the kinetic parameters obtained from the Westphalian coal and rock were applied to the geothermal evolution history to establish the process of gas generation and accumulation in the gas pools in Northwest Germany. Component and isotopic composition change model. Carbon isotope values obtained from thermal simulation of methane show a consistent carbon isotope pattern with gas fields in Northwest Germany. Isotopic reaction kinetics combined with regional thermal evolution history can effectively explain the characteristics of isotopic composition during natural gas accumulation. The results show that although pyrolysis experiments are fundamentally different from geological conditions, the open and variable temperature pyrolysis experiments can provide some meaningful kinetic parameters of isotope reaction. These parameters can satisfactorily describe the natural gas production processes in geological systems Isotope effect. In basin modeling, apply these?