生物成因煤层气定量判识及其成藏效应研究
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摘要
混合成因煤层气（热成因与生物成因气）在世界各含煤盆地广泛地被发现和报道，定量查明煤层气内生物成因气的相对含量及其成藏演化过程是一个重要的问题。为此，本文以柳林地区和芦岭地区为对象，采用物理实验与数值模拟方法，重点探讨生物成因煤层气定量研究方法及其成藏演化特征，取得如下主要成果。
首先，基于高压釜封闭体系生烃热模拟实验，提出热成因气成熟演化阶段判识模型，揭示气体碳氢同位素组成与样品演化阶段对应关系及演化特征。认为随有机质演化程度升高，甲烷、乙烷和丙烷碳同位素组成具有先变轻后变重，而甲烷氢同位素组成及二氧化碳碳同位素组成具有逐渐变重的特征。
其次，采用数理统计方法，系统分析不同成因类型煤型气分布特征，提出多个判识煤型气成因类型图版。认为生物成因气δ~(13)C_1<-60‰，热成因气δ~(13)C_1>-30‰，混合成因气介于二者之间。随有机质演化程度增强，从生物成因气至热成因气，δ~(13)C_1、δ~(13)C_(CO_2)-CH_4、δ~(13)C_(2-1)及CH_4/(C_2H_6+C_3H_8)具有变重趋势且相关性明显， δ~(13)C_1与δ~(13)C_(CO_2)-CH_4、δ~(13)C_1与δ~(13)C_(2-1)及δ~(13)C_1与CH_4/(C_2H_6+C_3H_8)是划分煤型气成因类型的图版。
再次，基于次生生物成因气模拟产出实验，结合生物成因气甲烷累积产率分析，完善生物成因气生烃地质模型与数学模型。运用红外光谱分析，从分子学角度分析热解和微生物降解前后样品分子结构变化特征。认为样品经微生物降解后分子间作用力变弱，含硫化合物对微生物降解具抑制作用。借助甲烷碳同位素组成地化测试手段，提出一个定量计算生物成因气相对含量新方法，定量考察同位素分馏作用对甲烷碳同位素组成的影响，二者结果偏差较小。
最后，运用数值模拟方法，探讨生物成因煤层气成藏演化特征及其与热成因气成藏效应，定量查明生物成因气对现今煤层含气量贡献。认为生物成因气对煤层累积生气量和含气量贡献显著，其演化过程具明显的阶段性，在不同地质演化阶段，生物成因煤层气发生运移的方式不同，主要以扩散、渗流和盖层突破为主。原生生物成因气对现今煤层含气量贡献较小，次生生物成因气贡献相对较大。
Coal bed methane (CBM) mixed by thermogenic and biogenic gases has beensubsequently discovered and reported in many coal basins all over the word. It is importantto quantitatively investigate the relative amount of biogenic gas in CBM reservoir and theprocess of reservoiring. To understand thses, the Liulin and Luling CBM exploitation sitesare taken as the study areas. Quantitative method and reservoiring characteristic ofbiogenic CBM are emphatically discussed by using laboratory experiments and numericalsimulation technology. Major innovations are as follows.
Firstly, based on hydrocarbon thermal simulation experiments in an autoclave closedsystem, the model for identifing the evolution stage of thermogenic gas generated byorganic matter is proposed. The evolutionary characteristics and ralationships betweencarbon and hydrogen isotopic compositions of gas with the evolution stage of samples arereviewed. The carbon isotopic compositions of methane, ethane, and propane changedfrom heavy to light, then back to heavy, whereas the hydrogen isotopic composition ofmethane and the carbon isotopic composition of carbon dioxide become increasinglyheavier with increasing evolution of organic matters (Rovalues).
Secondly, following mathematical statistics method, the distribution characteristics ofdifferent genetic types of coal type gas are systematically analyzed, and several charts foridentifying the genetic types of coal type gas are also raised. Results show that the δ~(13)C_1value of biogenic gas, thermogenic gas, and a mixture of both types are less than-60‰,more than-30‰, and occur in between, respectively. From biogenic gas to thermogenicgas, the δ~(13)C_1, δ~(13)C_(CO_2)-CH_4, δ~(13)C_(2-1), and CH_4/(C_2H_6+C_3H_8) values gradually become heavierwith the increase of Rovalues, and an obvious positive correlation exists among theaforementioned parameters. The charts of δ~(13)C_1-δ~(13)C_(CO_2)-CH_4, δ~(13)C_1-δ~(13)C_(2-1), andδ~(13)C_1-CH_4/(C_2H_6+C_3H_8) can be used to divide the genetic types of coal type gas.
Thirdly, by conducting secondary biogenic gas simulation experiments and combiningthe analysis of biogenic gas cumulative yields, hydrocarbon geologic and mathematicalmodels of biogenic gas are perfected. From the perspective of molecular structure, thechangements of samples from before and after during pyrolysis and microbial degradationare studied by using infrared spectrum analysis. The intermolecular forces of samples areweakening during the microbial degradation. Sulfocompound possibly has an inhibitoryaction on microbial degradation. By geochemical testing of methane carbon isotopiccomposition, a new method for quantitatively calculating the relative content of biogenicgas is presented. And the fractionation effect on methane carbon isotopic composition is also quantitatively inverstigated. By comparing these results, it is found that there is asmall deviation.
Fourthly, using numerical simulation technology, the reservoiring characteristics ofbiogenic gas and the reservoiring affect of biogenic and thermogenic gases are discussed.Biogenic gas contributed to the methane content of coal seam presently is alsoquantitatively studied. Biogenic gas has obviously contribution on cumulative gasproduction and gas content in coalbed. An obvious periodicity exists in the process ofCBM reservoiring. CBM containing biogenic gas migrate in different way at differentevolution stage, mainly in the way of diffusion, percolation, and cap outburst dissipation.Primary biogenic gas has relatively small contribution on the gas content of coal seampresently, whereas secondary biogenic gas has much.
首先，基于高压釜封闭体系生烃热模拟实验，提出热成因气成熟演化阶段判识模型，揭示气体碳氢同位素组成与样品演化阶段对应关系及演化特征。认为随有机质演化程度升高，甲烷、乙烷和丙烷碳同位素组成具有先变轻后变重，而甲烷氢同位素组成及二氧化碳碳同位素组成具有逐渐变重的特征。
其次，采用数理统计方法，系统分析不同成因类型煤型气分布特征，提出多个判识煤型气成因类型图版。认为生物成因气δ~(13)C_1<-60‰，热成因气δ~(13)C_1>-30‰，混合成因气介于二者之间。随有机质演化程度增强，从生物成因气至热成因气，δ~(13)C_1、δ~(13)C_(CO_2)-CH_4、δ~(13)C_(2-1)及CH_4/(C_2H_6+C_3H_8)具有变重趋势且相关性明显， δ~(13)C_1与δ~(13)C_(CO_2)-CH_4、δ~(13)C_1与δ~(13)C_(2-1)及δ~(13)C_1与CH_4/(C_2H_6+C_3H_8)是划分煤型气成因类型的图版。
再次，基于次生生物成因气模拟产出实验，结合生物成因气甲烷累积产率分析，完善生物成因气生烃地质模型与数学模型。运用红外光谱分析，从分子学角度分析热解和微生物降解前后样品分子结构变化特征。认为样品经微生物降解后分子间作用力变弱，含硫化合物对微生物降解具抑制作用。借助甲烷碳同位素组成地化测试手段，提出一个定量计算生物成因气相对含量新方法，定量考察同位素分馏作用对甲烷碳同位素组成的影响，二者结果偏差较小。
最后，运用数值模拟方法，探讨生物成因煤层气成藏演化特征及其与热成因气成藏效应，定量查明生物成因气对现今煤层含气量贡献。认为生物成因气对煤层累积生气量和含气量贡献显著，其演化过程具明显的阶段性，在不同地质演化阶段，生物成因煤层气发生运移的方式不同，主要以扩散、渗流和盖层突破为主。原生生物成因气对现今煤层含气量贡献较小，次生生物成因气贡献相对较大。
Coal bed methane (CBM) mixed by thermogenic and biogenic gases has beensubsequently discovered and reported in many coal basins all over the word. It is importantto quantitatively investigate the relative amount of biogenic gas in CBM reservoir and theprocess of reservoiring. To understand thses, the Liulin and Luling CBM exploitation sitesare taken as the study areas. Quantitative method and reservoiring characteristic ofbiogenic CBM are emphatically discussed by using laboratory experiments and numericalsimulation technology. Major innovations are as follows.
Firstly, based on hydrocarbon thermal simulation experiments in an autoclave closedsystem, the model for identifing the evolution stage of thermogenic gas generated byorganic matter is proposed. The evolutionary characteristics and ralationships betweencarbon and hydrogen isotopic compositions of gas with the evolution stage of samples arereviewed. The carbon isotopic compositions of methane, ethane, and propane changedfrom heavy to light, then back to heavy, whereas the hydrogen isotopic composition ofmethane and the carbon isotopic composition of carbon dioxide become increasinglyheavier with increasing evolution of organic matters (Rovalues).
Secondly, following mathematical statistics method, the distribution characteristics ofdifferent genetic types of coal type gas are systematically analyzed, and several charts foridentifying the genetic types of coal type gas are also raised. Results show that the δ~(13)C_1value of biogenic gas, thermogenic gas, and a mixture of both types are less than-60‰,more than-30‰, and occur in between, respectively. From biogenic gas to thermogenicgas, the δ~(13)C_1, δ~(13)C_(CO_2)-CH_4, δ~(13)C_(2-1), and CH_4/(C_2H_6+C_3H_8) values gradually become heavierwith the increase of Rovalues, and an obvious positive correlation exists among theaforementioned parameters. The charts of δ~(13)C_1-δ~(13)C_(CO_2)-CH_4, δ~(13)C_1-δ~(13)C_(2-1), andδ~(13)C_1-CH_4/(C_2H_6+C_3H_8) can be used to divide the genetic types of coal type gas.
Thirdly, by conducting secondary biogenic gas simulation experiments and combiningthe analysis of biogenic gas cumulative yields, hydrocarbon geologic and mathematicalmodels of biogenic gas are perfected. From the perspective of molecular structure, thechangements of samples from before and after during pyrolysis and microbial degradationare studied by using infrared spectrum analysis. The intermolecular forces of samples areweakening during the microbial degradation. Sulfocompound possibly has an inhibitoryaction on microbial degradation. By geochemical testing of methane carbon isotopiccomposition, a new method for quantitatively calculating the relative content of biogenicgas is presented. And the fractionation effect on methane carbon isotopic composition is also quantitatively inverstigated. By comparing these results, it is found that there is asmall deviation.
Fourthly, using numerical simulation technology, the reservoiring characteristics ofbiogenic gas and the reservoiring affect of biogenic and thermogenic gases are discussed.Biogenic gas contributed to the methane content of coal seam presently is alsoquantitatively studied. Biogenic gas has obviously contribution on cumulative gasproduction and gas content in coalbed. An obvious periodicity exists in the process ofCBM reservoiring. CBM containing biogenic gas migrate in different way at differentevolution stage, mainly in the way of diffusion, percolation, and cap outburst dissipation.Primary biogenic gas has relatively small contribution on the gas content of coal seampresently, whereas secondary biogenic gas has much.
引文
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