天然气生成过程中氢同位素分馏动力学研究及应用
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摘要
借助无水条件下实际源岩、原油样品和不同类型官能团模型化合物热解成气实验与不同水介质条件下十八烷热解成气的模拟实验,对天然气生成过程中氢同位素分馏的机理和影响因素进行了探讨,重点研究了有机质生气过程中水介质参与作用的机理和体现。建立并标定了天然气生成过程中氢同位素分馏的化学动力学模型,进而进行了初步的地质应用。
研究发现,与碳同位素分馏类似,天然气生成过程中组分氢同位素组成具有总体变重,低/高温阶段变轻的特点,并以正序列分布为主,与地质条件下普遍存在的天然气组分氢同位素组成序列相符。低/高温阶段的变轻主要由有机质的非均质性和成气机理的复杂性造成,可造成一定程度的氢同位素序列倒转,高温阶段早期所生重烃气的裂解使重烃气同位素组成的变轻趋势更加明显。
十八烷加不同水量裂解实验暗示,在有机质漫长的地质演化过程中,广泛存在的地层水会增加天然气(烃气、H_2、CO_2)的生成量,且这一作用将在有机质的晚期热演化阶段表现突出。地层水作为外来氢、氧源会在有机质晚期热演化阶段,为残余有机质提供氢、氧(自由基),使其可以更多地参与热解生气反应,同时,氢自由基的相互结合还会造成大量H_2的生成。伴随生气量的增大地层水的存在还会延长有机质的成气过程。与无水实验相比,加水实验所生烃气氢同位素组成明显较轻,并以乙烷最为显著。与产率曲线相比,不同加水量条件下烃气氢同位素组成曲线间的差别更为明显,反映了天然气氢同位素指标的敏感性,暗示了水源氢对有机质成气的影响更多地体现在天然气的氢同位素组成上。与加水量相比水介质性质对有机质成气产率、组分组成和氢同位素组成的影响较小。
除生气先质的氢同位素组成和有机质的热成熟作用外,有机质的沉积演化环境(水介质环境)会对天然气的氢同位素组成产生重要影响。由于地质条件下地层水是广泛存在的,鉴于水对有机质成气组分氢同位素组成的影响,在利用有机质成气过程中的氢同位素分馏规律对天然气的运聚成藏史进行研究时我们必须要考虑地层水的影响。
有机质生烃以自由基反应机制为主。有机质演化过程中地层水的参与是通过有机质的水解歧化反应进行的。一方面水中的氢可以自由基的形式与有机质裂解过程中产生的烃类(烯烃、烷烃)自由基结合生烃,另一方面水可以将有机质按照烯烃→醇→酮→羧酸→脱羧生成CO_2的顺序逐步氧化。
分馏机理的一致性决定了碳同位素分馏模型可以成功地引入到氢同位素分馏研究中。地质应用表明,在进行天然气资源评价时考虑地层水的影响将得出更加准确、乐观的评价结果,碳、氢同位素指标的结合应用可以反映更为详实、准确的地质信息。
Two kinds of simulation experiments were designed, one is gas generation experiment with samples of source rock, crude oil and model compounds with different functional groups under anhydrous condition, the other is gas generation from n-C_918)H_(38) cracking under different aqueous medium conditions. Based on the two kinds of experiments, the mechanism and influential factors of hydrogen isotopic fractionation during the generation of natural gas were investigated, and the participation mechanism and behaviors of aqueous medium were especially investigated. Hydrogen isotopic fractionation model based on chemical kinetics was established, calibrated and then extrapolated to geological settings.
During the generation of natural gas, the hydrogen isotopic composition has a tendence of becoming heavier in general, and becoming lighter in the low or high temperature periods, it aslo has a normal sequence distribution in accordance with geological settings. These features are similar to those of carbon isotopic fractionation. The fact that hydrogen isotopic composition becoming lighter in the low or high temperature periods is mainly caused by the heterogeneity of the parent material and the complexity of gas generation mechanism, which can lead to a reverse of the hydrogen isotopic sequence to some extent. During the high temperature period, the cracking of heavy hydrocarbon gas (C_(2-5)) has an obvious effect on the becoming lighter of its hydrogen isotopic composition.
The n-C_(18)H_(38) cracking experiments with different aqueous amounts suggest that, the plentiful formation water can increase the generation quantity of natural gas (hydrocarbon gas, H_2 and CO_2), especially during the high maturity stage. As the hydrogen and oxygen sources, the formation water can provide hydrogen and oxygen free radicals which have contribution to the pyrolysis reaction, at the same time more H_2 will be produced through the combination of hydrogen free radical. With the gas quantity increasing, the formation water will prolong the mature process of organic matter. In addition, the hydrogen isotopic composition of the hydrocarbon gas generated during hydrous experiment is obvious lighter, especially for that of ethane, compared with that of anhydrous experiment. The difference of hydrogen isotopic composition curves is more obvious than that of yield curves under different aqueous amounts, which indicates as an geological index the hydrogen isotopic index of natural gas is sensitive, and also suggests that the impact of hydrogen from formation water during the gas generation process will be more reflected through the hydrogen isotope composition of natural gas. Compared with water amount, the quality of aqueous medium has less effect on the yields, components and hydrogen isotopic composition.
Besides the effects of the hydrogen isotopic composition and thermal maturation of parent matter, the sediment enviroment (aqueous mediums enviroment) has an important influence on the hydrogen isotopic composition of natural gas. As the formation water widely exists in geological situation, the effect of the formation wate must be taken into account when the hydrogen isotopic fractionation during the gas generation process is used to investigate the gas migration and accumualtion history.
The free radical reaction is the main mechanism of hydrocarbon generation from organic matter. The participation of the formation water goes on through the hydrolysis disproportionation of organic matter during the evolvement process of organic matter. On the one hand, the water-derived hydrogen (hydrogen free radical) can be combinated with the hydrocarbon (alkene and alkane) free radical generated during the thermal maturation process of organic matter. On the other hand, organic matter can be oxidated by formation water following the hydrocarbon-alcohol-ketone-carboxylic acid-CO_2 sequence.
The consistency of carbon and hydrogen isotopic fractionation mechanisms determines that hydrogen isotopic fractionation can be described by using the carbon isotopic fractionation model. The geological extrapolation results show that a more exact and optimistic conclusion of natural gas resource assessment can be drawn if we consider the effect of formation water, and more abundant and reliable geological information can be obtained through the combination applications of carbon and hydrogen isotopic indexes.
研究发现,与碳同位素分馏类似,天然气生成过程中组分氢同位素组成具有总体变重,低/高温阶段变轻的特点,并以正序列分布为主,与地质条件下普遍存在的天然气组分氢同位素组成序列相符。低/高温阶段的变轻主要由有机质的非均质性和成气机理的复杂性造成,可造成一定程度的氢同位素序列倒转,高温阶段早期所生重烃气的裂解使重烃气同位素组成的变轻趋势更加明显。
十八烷加不同水量裂解实验暗示,在有机质漫长的地质演化过程中,广泛存在的地层水会增加天然气(烃气、H_2、CO_2)的生成量,且这一作用将在有机质的晚期热演化阶段表现突出。地层水作为外来氢、氧源会在有机质晚期热演化阶段,为残余有机质提供氢、氧(自由基),使其可以更多地参与热解生气反应,同时,氢自由基的相互结合还会造成大量H_2的生成。伴随生气量的增大地层水的存在还会延长有机质的成气过程。与无水实验相比,加水实验所生烃气氢同位素组成明显较轻,并以乙烷最为显著。与产率曲线相比,不同加水量条件下烃气氢同位素组成曲线间的差别更为明显,反映了天然气氢同位素指标的敏感性,暗示了水源氢对有机质成气的影响更多地体现在天然气的氢同位素组成上。与加水量相比水介质性质对有机质成气产率、组分组成和氢同位素组成的影响较小。
除生气先质的氢同位素组成和有机质的热成熟作用外,有机质的沉积演化环境(水介质环境)会对天然气的氢同位素组成产生重要影响。由于地质条件下地层水是广泛存在的,鉴于水对有机质成气组分氢同位素组成的影响,在利用有机质成气过程中的氢同位素分馏规律对天然气的运聚成藏史进行研究时我们必须要考虑地层水的影响。
有机质生烃以自由基反应机制为主。有机质演化过程中地层水的参与是通过有机质的水解歧化反应进行的。一方面水中的氢可以自由基的形式与有机质裂解过程中产生的烃类(烯烃、烷烃)自由基结合生烃,另一方面水可以将有机质按照烯烃→醇→酮→羧酸→脱羧生成CO_2的顺序逐步氧化。
分馏机理的一致性决定了碳同位素分馏模型可以成功地引入到氢同位素分馏研究中。地质应用表明,在进行天然气资源评价时考虑地层水的影响将得出更加准确、乐观的评价结果,碳、氢同位素指标的结合应用可以反映更为详实、准确的地质信息。
Two kinds of simulation experiments were designed, one is gas generation experiment with samples of source rock, crude oil and model compounds with different functional groups under anhydrous condition, the other is gas generation from n-C_918)H_(38) cracking under different aqueous medium conditions. Based on the two kinds of experiments, the mechanism and influential factors of hydrogen isotopic fractionation during the generation of natural gas were investigated, and the participation mechanism and behaviors of aqueous medium were especially investigated. Hydrogen isotopic fractionation model based on chemical kinetics was established, calibrated and then extrapolated to geological settings.
During the generation of natural gas, the hydrogen isotopic composition has a tendence of becoming heavier in general, and becoming lighter in the low or high temperature periods, it aslo has a normal sequence distribution in accordance with geological settings. These features are similar to those of carbon isotopic fractionation. The fact that hydrogen isotopic composition becoming lighter in the low or high temperature periods is mainly caused by the heterogeneity of the parent material and the complexity of gas generation mechanism, which can lead to a reverse of the hydrogen isotopic sequence to some extent. During the high temperature period, the cracking of heavy hydrocarbon gas (C_(2-5)) has an obvious effect on the becoming lighter of its hydrogen isotopic composition.
The n-C_(18)H_(38) cracking experiments with different aqueous amounts suggest that, the plentiful formation water can increase the generation quantity of natural gas (hydrocarbon gas, H_2 and CO_2), especially during the high maturity stage. As the hydrogen and oxygen sources, the formation water can provide hydrogen and oxygen free radicals which have contribution to the pyrolysis reaction, at the same time more H_2 will be produced through the combination of hydrogen free radical. With the gas quantity increasing, the formation water will prolong the mature process of organic matter. In addition, the hydrogen isotopic composition of the hydrocarbon gas generated during hydrous experiment is obvious lighter, especially for that of ethane, compared with that of anhydrous experiment. The difference of hydrogen isotopic composition curves is more obvious than that of yield curves under different aqueous amounts, which indicates as an geological index the hydrogen isotopic index of natural gas is sensitive, and also suggests that the impact of hydrogen from formation water during the gas generation process will be more reflected through the hydrogen isotope composition of natural gas. Compared with water amount, the quality of aqueous medium has less effect on the yields, components and hydrogen isotopic composition.
Besides the effects of the hydrogen isotopic composition and thermal maturation of parent matter, the sediment enviroment (aqueous mediums enviroment) has an important influence on the hydrogen isotopic composition of natural gas. As the formation water widely exists in geological situation, the effect of the formation wate must be taken into account when the hydrogen isotopic fractionation during the gas generation process is used to investigate the gas migration and accumualtion history.
The free radical reaction is the main mechanism of hydrocarbon generation from organic matter. The participation of the formation water goes on through the hydrolysis disproportionation of organic matter during the evolvement process of organic matter. On the one hand, the water-derived hydrogen (hydrogen free radical) can be combinated with the hydrocarbon (alkene and alkane) free radical generated during the thermal maturation process of organic matter. On the other hand, organic matter can be oxidated by formation water following the hydrocarbon-alcohol-ketone-carboxylic acid-CO_2 sequence.
The consistency of carbon and hydrogen isotopic fractionation mechanisms determines that hydrogen isotopic fractionation can be described by using the carbon isotopic fractionation model. The geological extrapolation results show that a more exact and optimistic conclusion of natural gas resource assessment can be drawn if we consider the effect of formation water, and more abundant and reliable geological information can be obtained through the combination applications of carbon and hydrogen isotopic indexes.
引文
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