咸化环境盐类物质与有机质相互作用研究
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摘要
我国东部咸化湖盆油气资源丰富,其中烃源岩与不同盐类物质共存。盐类物质是否影响有机质生烃过程,生成油气又有什么特征。研究咸化环境油气成因不仅可以深化油气地质及地球化学领域基础问题,而且有助于油气勘探,因此,该选题具有重要的科学和实际意义。
本论文通过文献调研,针对有机质与盐类物质相互作用问题,提出了一整套理论研究方法,即低熟气成因利用等温热模拟手段、高熟气成因开展程序升温热模拟实验,查明碳酸盐、硫酸盐和氯化盐等对有机质的催化生烃过程;阐明了民丰等地区的天然气成因机制;最后利用化学动力学方法查明了盐类物质作用下油气成因模式,完善了咸化湖盆油气成因理论。
在调研咸化湖盆烃源岩组合及其油气藏富集关系基础上,对东营凹陷沙四段盐湖相有机质及产出油气的地质地球化学研究发现,该区深层油型气高环烷烃(甲基环己烷指数38%)、高芳烃(苯指数26%)轻碳同位素(δ~(13)C_1为-48.95~-44.66‰)特征与有机质类型(I型II1型)及热演化史(Ro约1.1-1.6%)并不完全匹配,天然气成因问题存在争议。
通过热模拟盐类物质作用下低熟气的生成过程发现,不同蒸发盐、热解温度和恒温时间影响源岩降解生油气数量,其中,温度对油气生成起控制作用。碳酸盐和硫酸盐对低熟气的生成有较强催化作用(产率分别提高34%和28%),氯化盐催化生气能力较弱(提高15%)。盐湖相低熟气具有烃类组分偏湿,苯含量高的特征(提高近3倍)。
盐湖相高成熟天然气生成的热模拟结果表明,石膏对烃源岩热解成气的催化作用最强(提高77%),石盐对原油裂解的催化最显著(提高43%)。在16种单体烃及三类轻烃参数热演化规律中发现,蒸发盐的催化作用表现为加快有机质降解生油气过程,使生烃反应提前向下一个温阶即更高成熟度条件下进行,故所生烃类气体的成熟度更高。
高成熟阶段盐类物质作用下的源岩热解和原油裂解成因天然气都以烃类组分偏干、环烷烃和芳烃含量增高为特征。其中,盐湖相高成熟源岩热解气的C_5环烷烃/C_5链烷烃>1.6,而原油裂解气C_5环烷烃/C_5链烷烃<1.3,相反盐湖相原油早期裂解的C_5环烷烃/C_5链烷烃值较高,均大于1。
高成熟阶段热模拟气与民丰天然气比较发现,较源岩、原油自身降解,膏盐作用下热模拟气iC_4/nC_4、烷芳指数、环烷指数等更接近天然气。相似系数数理分析得出,民丰天然气主要是烃源岩与石膏相互作用热解形成,其次是原油与石盐裂解成因。只有膏盐与有机质相互作用才能解释民丰天然气组成与热演化史并不匹配的问题。
利用平行一级动力学模型计算发现,平均活化能降低是气态烃产率增加的重要机制,蒸发盐改变重要单体烃的活化能分布。将生烃动力学模型应用于埋藏热演化史,建立膏盐作用下天然气生成模式,定量计算出石膏和石盐对生烃门限和热演化史的影响。
A large number of natural gas and oil are discovered in saline-lake facies. The deposition of organic matter in saline is different from that in freshwater lake. In the oil-gas generation, there may be the interaction of source rock and oil with evaporates in saline-lakes. Natural gases from saline maybe have sepecial geochemical characteristics. These are related to oil-gas genese in saline lake. Furthermore, oil-gas generation has affected the direction of oil field exploration and resources evaluation in saline-lake.
Basing on the identification of relationship against oil-gas reservoirs and source rocks in saline, this paper conducts a series of thermal simulations about organic matter with /without evaporates in low and high evolution phase. The simulation results show that carbonate, gypsum, and sodium chlorite intensive catalysize on organic matter degradation and gases product has certain geochemical characteristics. Furthermore, combinating with the organic matter evolution in Minfeng sag, gas generation modle is established in saline-lakes facies.
It is worth noting that the natural gas in Minfeng area is of special geochemical characteristics such as the index of methylcyclohexane is about 38%, the index of benzene is about 26%,the methane carbon isotope composition is from -48.95 to -44.66‰. These characteristics don’t match with the maturity of orgain matter(Ro=1.1-1.6%). Hence, the gas generation causes controversy.
For the low evolution kerogen-degraded gas, different salts、pyrolysis temperature and thermostatic time affect the yield of gas generation in varying degrees. Simulated temperature plays an important role in the gas generation. Adding carbonate or gypsum to the source rock sample, the number of catalysizing hydrocarbon would raise 34% and 28% spectively. It is found that generating gas is with some geochemical characteristics such as relative wet hydrocarbon composition and high benzene content.
It is discovered that source rock-gupsum and oil-sodium chlorate has the largest gas production compared with other salts in high evolution. On the analysis of each C_(5-8) hydrocarbon and light hydrocarbon parameters evolutation, it is found that gypsum and sodium chlorite could accelerate the process of hydrocarbon generation from organic matter. The catalysizing essence is that the degraduation reaction of is advanced to the following higher evolution phase (thermal temperature).
The hydrocarbon composition of kerogen-generated gas and oil-cracked one are of relative drying gases, high content of cycloalkane and aromatic in high evolution phase. The gas index of C_5 cyclane/C_5 paraffin from kerogen with evaporates is more than 1.6 and the parameter ration of oil-cracked gas is lower than 1.3. Otherwise, this ration is more than 1 in the the low evolution phase of oil cracking.
Generating gas from source rock or oil sample with evaporates is more light carbon isotope composition compared with those from the simulated samples without evaporites. The carbon isotope of kerogen-degraded gas with/without evaporates is from -33.9‰to -34.8‰, the one of oil-cracked gas with/without evaporates ranges from -42.4‰to -44.4‰. In addition, analogying with the the carbon isotope of gas product from thermaled samples of organic matter single degraded or degraded with other salts, the one of organic matter with sodium is more light 1-2‰.
The paper selects parameters such as iC4/nC4、the index of alkand-aromatic、the index of cycloalkaneⅠandⅢ. Comparing with the above index, it is found that gas product from organic matter degraded with gypsum or sodium chlorite is more similar to natural gase from Minfeng sag. The similarity coefficient of source rock samples with evaporates and natural gases is much close than the one of oil samples with evaporates. Comprehensive the analysis of the gas product, carbonate isotope compostion and geological setting, it is believed that natural gas found in Minfeng sag is generated from the interaction of source rocks-gypsum, followed from oil-halitethe cracking. Furthermore, only the interaction of organic matter and gypsum-halitethe could explain the problem why the gases geochemical characteristics don’t match with the evolution of organic matter in Minfeng area.
Based on the parallel first order reaction kinetics model, it is found that the decreasement of the activation energy is the mechanism to increase the hydrocarbon number from orgaic matter pyrolysised. Evaporates influence gas generation and change the activation energy distribution of hydrocarbon. In addition, the dynamic model of hydrocarbon generation could make applicaton with this area evolution and establish gas generation model of organic with gypsum or halitethe in saline basin. After doing quantitative calculation, it is obtained that gypsum or halitethe could effect the hydrocarbon generation threshold and evolution history of organic matter(source rocks and ancient reservoir).
本论文通过文献调研,针对有机质与盐类物质相互作用问题,提出了一整套理论研究方法,即低熟气成因利用等温热模拟手段、高熟气成因开展程序升温热模拟实验,查明碳酸盐、硫酸盐和氯化盐等对有机质的催化生烃过程;阐明了民丰等地区的天然气成因机制;最后利用化学动力学方法查明了盐类物质作用下油气成因模式,完善了咸化湖盆油气成因理论。
在调研咸化湖盆烃源岩组合及其油气藏富集关系基础上,对东营凹陷沙四段盐湖相有机质及产出油气的地质地球化学研究发现,该区深层油型气高环烷烃(甲基环己烷指数38%)、高芳烃(苯指数26%)轻碳同位素(δ~(13)C_1为-48.95~-44.66‰)特征与有机质类型(I型II1型)及热演化史(Ro约1.1-1.6%)并不完全匹配,天然气成因问题存在争议。
通过热模拟盐类物质作用下低熟气的生成过程发现,不同蒸发盐、热解温度和恒温时间影响源岩降解生油气数量,其中,温度对油气生成起控制作用。碳酸盐和硫酸盐对低熟气的生成有较强催化作用(产率分别提高34%和28%),氯化盐催化生气能力较弱(提高15%)。盐湖相低熟气具有烃类组分偏湿,苯含量高的特征(提高近3倍)。
盐湖相高成熟天然气生成的热模拟结果表明,石膏对烃源岩热解成气的催化作用最强(提高77%),石盐对原油裂解的催化最显著(提高43%)。在16种单体烃及三类轻烃参数热演化规律中发现,蒸发盐的催化作用表现为加快有机质降解生油气过程,使生烃反应提前向下一个温阶即更高成熟度条件下进行,故所生烃类气体的成熟度更高。
高成熟阶段盐类物质作用下的源岩热解和原油裂解成因天然气都以烃类组分偏干、环烷烃和芳烃含量增高为特征。其中,盐湖相高成熟源岩热解气的C_5环烷烃/C_5链烷烃>1.6,而原油裂解气C_5环烷烃/C_5链烷烃<1.3,相反盐湖相原油早期裂解的C_5环烷烃/C_5链烷烃值较高,均大于1。
高成熟阶段热模拟气与民丰天然气比较发现,较源岩、原油自身降解,膏盐作用下热模拟气iC_4/nC_4、烷芳指数、环烷指数等更接近天然气。相似系数数理分析得出,民丰天然气主要是烃源岩与石膏相互作用热解形成,其次是原油与石盐裂解成因。只有膏盐与有机质相互作用才能解释民丰天然气组成与热演化史并不匹配的问题。
利用平行一级动力学模型计算发现,平均活化能降低是气态烃产率增加的重要机制,蒸发盐改变重要单体烃的活化能分布。将生烃动力学模型应用于埋藏热演化史,建立膏盐作用下天然气生成模式,定量计算出石膏和石盐对生烃门限和热演化史的影响。
A large number of natural gas and oil are discovered in saline-lake facies. The deposition of organic matter in saline is different from that in freshwater lake. In the oil-gas generation, there may be the interaction of source rock and oil with evaporates in saline-lakes. Natural gases from saline maybe have sepecial geochemical characteristics. These are related to oil-gas genese in saline lake. Furthermore, oil-gas generation has affected the direction of oil field exploration and resources evaluation in saline-lake.
Basing on the identification of relationship against oil-gas reservoirs and source rocks in saline, this paper conducts a series of thermal simulations about organic matter with /without evaporates in low and high evolution phase. The simulation results show that carbonate, gypsum, and sodium chlorite intensive catalysize on organic matter degradation and gases product has certain geochemical characteristics. Furthermore, combinating with the organic matter evolution in Minfeng sag, gas generation modle is established in saline-lakes facies.
It is worth noting that the natural gas in Minfeng area is of special geochemical characteristics such as the index of methylcyclohexane is about 38%, the index of benzene is about 26%,the methane carbon isotope composition is from -48.95 to -44.66‰. These characteristics don’t match with the maturity of orgain matter(Ro=1.1-1.6%). Hence, the gas generation causes controversy.
For the low evolution kerogen-degraded gas, different salts、pyrolysis temperature and thermostatic time affect the yield of gas generation in varying degrees. Simulated temperature plays an important role in the gas generation. Adding carbonate or gypsum to the source rock sample, the number of catalysizing hydrocarbon would raise 34% and 28% spectively. It is found that generating gas is with some geochemical characteristics such as relative wet hydrocarbon composition and high benzene content.
It is discovered that source rock-gupsum and oil-sodium chlorate has the largest gas production compared with other salts in high evolution. On the analysis of each C_(5-8) hydrocarbon and light hydrocarbon parameters evolutation, it is found that gypsum and sodium chlorite could accelerate the process of hydrocarbon generation from organic matter. The catalysizing essence is that the degraduation reaction of is advanced to the following higher evolution phase (thermal temperature).
The hydrocarbon composition of kerogen-generated gas and oil-cracked one are of relative drying gases, high content of cycloalkane and aromatic in high evolution phase. The gas index of C_5 cyclane/C_5 paraffin from kerogen with evaporates is more than 1.6 and the parameter ration of oil-cracked gas is lower than 1.3. Otherwise, this ration is more than 1 in the the low evolution phase of oil cracking.
Generating gas from source rock or oil sample with evaporates is more light carbon isotope composition compared with those from the simulated samples without evaporites. The carbon isotope of kerogen-degraded gas with/without evaporates is from -33.9‰to -34.8‰, the one of oil-cracked gas with/without evaporates ranges from -42.4‰to -44.4‰. In addition, analogying with the the carbon isotope of gas product from thermaled samples of organic matter single degraded or degraded with other salts, the one of organic matter with sodium is more light 1-2‰.
The paper selects parameters such as iC4/nC4、the index of alkand-aromatic、the index of cycloalkaneⅠandⅢ. Comparing with the above index, it is found that gas product from organic matter degraded with gypsum or sodium chlorite is more similar to natural gase from Minfeng sag. The similarity coefficient of source rock samples with evaporates and natural gases is much close than the one of oil samples with evaporates. Comprehensive the analysis of the gas product, carbonate isotope compostion and geological setting, it is believed that natural gas found in Minfeng sag is generated from the interaction of source rocks-gypsum, followed from oil-halitethe cracking. Furthermore, only the interaction of organic matter and gypsum-halitethe could explain the problem why the gases geochemical characteristics don’t match with the evolution of organic matter in Minfeng area.
Based on the parallel first order reaction kinetics model, it is found that the decreasement of the activation energy is the mechanism to increase the hydrocarbon number from orgaic matter pyrolysised. Evaporates influence gas generation and change the activation energy distribution of hydrocarbon. In addition, the dynamic model of hydrocarbon generation could make applicaton with this area evolution and establish gas generation model of organic with gypsum or halitethe in saline basin. After doing quantitative calculation, it is obtained that gypsum or halitethe could effect the hydrocarbon generation threshold and evolution history of organic matter(source rocks and ancient reservoir).
引文
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