鄂尔多斯盆地上古生界煤的生烃动力学及其分子特征研究
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摘要
鄂尔多斯盆地是我国重要的含油气沉积盆地之一，上古生界煤是盆地内上古生界天然气藏的主要的气源岩。过去的大量研究工作主要集中在气源岩的评价上，并取得了一系列的成果，基于生烃动力学实验的煤成气的生成和运移历史的研究较少。开展这方面的研究对于鄂尔多斯盆地上古生界煤成气的勘探开发具有重要的意义。
本论文以鄂尔多斯盆地上古生界太原组和山西组的煤为研究对象，采用目前最接近地质生烃过程的有压力存在的黄金管限定体系系统地进行了生烃动力学模拟，结合盆地实际对盆地上古生界生烃史和天然气的运移史进行了恢复。同时，采用Py-GC-MS和钌离子催化氧化(RICO)手段，系统地研究了这两组原煤、其中的非共价键物理缔合结构的组分以及共价键骨架结构的组分的分子特征，这些对于进一步了解煤的生烃机理可以提供有意义的信息。
热解动力学实验结果表明，两组原煤的生烃动力学参数和镜质体反射率(Ro)动力学参数均存在差异。通过生烃动力学恢复的煤成烃的生烃史说明，鄂尔多斯盆地上古生界烃源岩在盆地后期的抬升降温过程中不会发生大规模的二次生烃。由Ro动力学计算的最大古地温和砂岩气液包裹体的均一温度的对比结果显示，盆地中部和东部上古生界地层内的气水界面已经发生迁移，而盆地北部上古生界地层中的气水界面未完全迁移。这表明，盆地中部和东部具有良好的天然气勘探前景。
Py-GC-MS和RICO结果显示，两组原煤及其CS_2-NMP混合溶剂的抽提物和抽余物的分子特征都存在差别，正是这种差别内在地引起了两组原煤的生烃行为的差异。进一步的研究显示，原煤的CS_2-NMP混合溶剂的抽余物由大量复杂的稠合芳香组分以及连接在其上的少量的烷基构成，结构相对稳定，仅在芳香族内部的组成上存在差别。另一方面，CS_2-NMP的抽提物的组成复杂多变，与常见的认识不同，其中同样有复杂的稠合芳香组分以及连接在芳香结构上的烷基。
论文最后讨论了抑制和破坏煤及干酪根中的非共价键缔合作用生烃的可能性，认为物理缔合结构对于生烃具有十分重要的意义，并以此解释了许多地质和实验的事实。
It is reported that the Upper Paleozoic coals are the major gas-source rocks in Ordos
basin, one of the most important oil-gas sedimentary basin in our country. Remarkably
successes have achieved in the evaluation on hydrocarbons potentials of the source rocks. However, the researches about the generation and transformation evolution of coal-derived hydrocarbons based on the new technique-kinetic of the hydrocarbon generation are limited. However, it is important for the natural gas exploration and recovery.
Regarding the Upper Paleozoic coals (Taiyuan coal and Shanxi coal) in Ordos Basin, the present paper aims to discuss the geological and geochemical problems related with these coals, such as the generation and transformation evolution of coal-derived hydrocarbons by pyrolysis kinetic under constant high pressures, and these coals molecular properties by Py-GC-MS and Ruthenium-Ion-Catalyzed-Oxidation (RICO) reaction, including those of the raw coals, their covalent bond networks and non-covalent
bond associated fractions. These results may supply helpful information to the mechanism
on the hydrocarbons generation.
The results of pyrolysis kinetic indicate that there are differences between these two coal's kinetic parameters of the hydrocarbon generation and of vitrinite reflectance. The coal-derived hydrocarbons' generation and transformation evolutions reconstructed by the kinetic of the hydrocarbon generation suggest that, large-scale secondary hydrocarbon generation is not likely during the uplifting and cooling process of Ordos basin. Compared the homogenization temperature of fluid inclusion with the maximum palaeotemperarure from the Ro kinetic, it infer that, the water-gas interfaces have migrated out of the strata driven by the natural gas in the middle and the east of Ordos basin, and the natural gas formed have not driven the water out in the north of Ordos basin. These results imply the good natural gas exploration foreground in the middle and the east of Ordos basin.
The results from Py-GC-MS and RICO indicate that, there are differences in the
molecular characterization between these two raw coals, their extracts and residues of
CS2-NMP mixed solvents, which is the key lead to the differences in their hydrocarbons generation behaviors. Further researches suggest the molecular structures, which are composing with abundant complex condensed aromatic fractions and a few alkyl groups attached to aromatic nuclei, are relatively constant of the residues of CS2-NMP mixture,
and the differences are only in the composition of aromatic fractions. On the other hand, the molecular structure of the CS2-NMP mixture extracts, which are relatively variable, unexpectedly, have some complex condensed aromatic fractions and alkyl groups attached to aromatic nuclei.
The paper discusses the possibility of hydrocarbons generation by the destroying and restraint of the associated structure and think that associated structure is important to hydrocarbons generation. A great deal of the geological and experimental facts can satisfactory explain with the existence of associated structure in coal and source rocks.
本论文以鄂尔多斯盆地上古生界太原组和山西组的煤为研究对象，采用目前最接近地质生烃过程的有压力存在的黄金管限定体系系统地进行了生烃动力学模拟，结合盆地实际对盆地上古生界生烃史和天然气的运移史进行了恢复。同时，采用Py-GC-MS和钌离子催化氧化(RICO)手段，系统地研究了这两组原煤、其中的非共价键物理缔合结构的组分以及共价键骨架结构的组分的分子特征，这些对于进一步了解煤的生烃机理可以提供有意义的信息。
热解动力学实验结果表明，两组原煤的生烃动力学参数和镜质体反射率(Ro)动力学参数均存在差异。通过生烃动力学恢复的煤成烃的生烃史说明，鄂尔多斯盆地上古生界烃源岩在盆地后期的抬升降温过程中不会发生大规模的二次生烃。由Ro动力学计算的最大古地温和砂岩气液包裹体的均一温度的对比结果显示，盆地中部和东部上古生界地层内的气水界面已经发生迁移，而盆地北部上古生界地层中的气水界面未完全迁移。这表明，盆地中部和东部具有良好的天然气勘探前景。
Py-GC-MS和RICO结果显示，两组原煤及其CS_2-NMP混合溶剂的抽提物和抽余物的分子特征都存在差别，正是这种差别内在地引起了两组原煤的生烃行为的差异。进一步的研究显示，原煤的CS_2-NMP混合溶剂的抽余物由大量复杂的稠合芳香组分以及连接在其上的少量的烷基构成，结构相对稳定，仅在芳香族内部的组成上存在差别。另一方面，CS_2-NMP的抽提物的组成复杂多变，与常见的认识不同，其中同样有复杂的稠合芳香组分以及连接在芳香结构上的烷基。
论文最后讨论了抑制和破坏煤及干酪根中的非共价键缔合作用生烃的可能性，认为物理缔合结构对于生烃具有十分重要的意义，并以此解释了许多地质和实验的事实。
It is reported that the Upper Paleozoic coals are the major gas-source rocks in Ordos
basin, one of the most important oil-gas sedimentary basin in our country. Remarkably
successes have achieved in the evaluation on hydrocarbons potentials of the source rocks. However, the researches about the generation and transformation evolution of coal-derived hydrocarbons based on the new technique-kinetic of the hydrocarbon generation are limited. However, it is important for the natural gas exploration and recovery.
Regarding the Upper Paleozoic coals (Taiyuan coal and Shanxi coal) in Ordos Basin, the present paper aims to discuss the geological and geochemical problems related with these coals, such as the generation and transformation evolution of coal-derived hydrocarbons by pyrolysis kinetic under constant high pressures, and these coals molecular properties by Py-GC-MS and Ruthenium-Ion-Catalyzed-Oxidation (RICO) reaction, including those of the raw coals, their covalent bond networks and non-covalent
bond associated fractions. These results may supply helpful information to the mechanism
on the hydrocarbons generation.
The results of pyrolysis kinetic indicate that there are differences between these two coal's kinetic parameters of the hydrocarbon generation and of vitrinite reflectance. The coal-derived hydrocarbons' generation and transformation evolutions reconstructed by the kinetic of the hydrocarbon generation suggest that, large-scale secondary hydrocarbon generation is not likely during the uplifting and cooling process of Ordos basin. Compared the homogenization temperature of fluid inclusion with the maximum palaeotemperarure from the Ro kinetic, it infer that, the water-gas interfaces have migrated out of the strata driven by the natural gas in the middle and the east of Ordos basin, and the natural gas formed have not driven the water out in the north of Ordos basin. These results imply the good natural gas exploration foreground in the middle and the east of Ordos basin.
The results from Py-GC-MS and RICO indicate that, there are differences in the
molecular characterization between these two raw coals, their extracts and residues of
CS2-NMP mixed solvents, which is the key lead to the differences in their hydrocarbons generation behaviors. Further researches suggest the molecular structures, which are composing with abundant complex condensed aromatic fractions and a few alkyl groups attached to aromatic nuclei, are relatively constant of the residues of CS2-NMP mixture,
and the differences are only in the composition of aromatic fractions. On the other hand, the molecular structure of the CS2-NMP mixture extracts, which are relatively variable, unexpectedly, have some complex condensed aromatic fractions and alkyl groups attached to aromatic nuclei.
The paper discusses the possibility of hydrocarbons generation by the destroying and restraint of the associated structure and think that associated structure is important to hydrocarbons generation. A great deal of the geological and experimental facts can satisfactory explain with the existence of associated structure in coal and source rocks.
引文
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