蓟县剖面元古宙沉积物（1.8-0.85Ga）的分子有机地球化学研究
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摘要
迄今为止，地球科学家的注意力仍主要集中于显生宙地球的研究，而对早期地球与早期生命的演化段却知之甚少。本研究以我国著名的中晚元古代地层剖面天津蓟县剖面(1.8-0.85Ga)中保存的沉积有机质为研究对象，运用分子有机地球化学的方法和理论系统研究了该剖面元古宙沉积物中的可溶有机分子特征、干酪根化学与热降解产物分子特征以及各种有机质类型(包括可溶单体烃类、干酪根等)和共生碳酸盐的碳同位素特征。在研究和讨论中还重点结合了蓟县剖面丰富的古环境和古生物的资料，从分子和同位素的角度对燕山盆地及其生命在全球演化大背景下的早期演化进行了深入探讨。
剖面生物标志化合物特征的调查显示整个剖面具有基本相似的分子组成。值得一提的是在剖面串岭沟组约1.8Ga的页岩中发现了指示真核生物存在的古老甾烷和指示原生动物存在的目前所知的最古老的伽马蜡烷。通过对剖面分子特征与独立的古环境和古生物资料的对比研究发现蓟县剖面中的有机分子很好地记录了燕山盆地元古宙各阶段的生物和古环境演化的信息。
干酪根和共生碳酸盐的碳同位素组成(δ~(13)C_k和δ~(13)C_(carb))以及二者的差值(Δ_C)反映了在全球大环境演化下的燕山盆地小生境的演化特征。δ~(13)C_k和δ~(13)C_(carb)的剖面特征表明，大约1.55Ga前，全球CO_2浓度曾持续快速下降，而之后趋于稳定。Δ_C被证明能有效反映局部环境中不同生物群落在利用CO_2过程中的碳同位素分异程度的差异。Δ_C在剖面上的规律性变化显示了燕山盆地生物整体同位素分异程度在元古宙演化过程中出现旋回式波动。这一波动能很好地被解释为燕山盆地周期性海进与海退所导致的不同生物群落的更迭。
单体烃碳同位素组成与共生干酪根碳同位素组成之间的关系提供了燕山盆地演化中更为深层次的有关生物地球化学循环方面的信息。剖面中具有较重同位素组成的类异戊二烯化合物和早于高于庄期(＞1.4Ga)的样品中的正构烷烃可能较多地来源于生存在燕山古海中的喜盐等古细菌类脂，而高于庄期后样品中的正构烷烃可能较多地起源于具有相对较轻同位素组成的原始藻类有机质。正构烷烃与共生干酪根碳同位素关系在高于庄末期(1.4Ga)的明显倒转可能表明在高于庄末期以后原始有机质的异养生物降解程度明显降低。这一降低可能与燕山盆地进入稳定的浅水陆表海沉积环境有关。蓟县剖面元古宙沉积有机质中独特的单体烃与共生干酪根的碳同位素关系特征地反映了具有明显局限特征
中科院广州地球化学研究所博士学位论文
的元古宙燕山盆地所特有的生物地球化学循环过程。
Rock－Eval等数据以及初步的干酪根化学和热降解的研究表明剖面中大部
分干酪根样品己对应成熟至油窗结束阶段，且只有来自剖面洪水庄组干酪根具
有开展全面有机地球化学研究的价值。多种有机地球化学方法对剖面洪水庄组
干酪根的综合研究不仅获得了洪水庄组干酪根重要的分子结构特征和有机质生
物起源的信息，而且还从干酪根的角度证实了洪水庄组可溶有机质原生性的本
质。
通过对剖面洪水庄组与北美老页岩组分子特征及其他地球化学特征的对比
表明华北地块很可能在1112亿年以前与劳伦大陆是紧紧挨在一起的。
此项研究具有以下特色和创新之处：（）研究对象连续时间跨度最长；门）
研究内容涉及面较全面；（3）较早详细探讨了前寒武纪沉积有机质的分子特征
与古环境和生物群落的演化关系；N）独立推导和论证了吵C＿和5’3C。的差
值（八C）的生物和环境的重要意义：6）在前寒武纪有机质研究中区分了局部
封闭环境下的生物地球化学循环过程与广域海环境下的生物地球化学过程的差
异：（6）开展了前寒武纪干酪根化学和热降解研究；（）开创性地将分子有机
地球化学的数据应用于元古宙Rodinia超大陆的重建中。
The Precambrian, one of the most important stages in the history of the Earth, so far, is still less known to us mostly because of the absence of intact morphological fossils in the Precambrian strata. This study systemically investigated the molecular (including soluble saturates and hydrocarbon products of keogen degradation) and carbon isotopic (including soluble hydrocarbons, kerogens and coexisted carbonates etc.) characteristics of Paleo- to Neoproterozoic (1.8-0.85Ga) sediments from the famous Jixian strata section, North China. The environmental and biological evolutions of Proterozoic Yanshan Basin companied by the global evolution were also discussed in detail with these molecular and isotopic data combined with independent palaeoenvironmental and palaeontologic information as acquired from these strata.
Analogous hydrocarbon types were detected in almost all samples from Jixian strata section. It is worth noting that the old steranes and the so far oldest gammacerane was detected in the l.SGa shales from Chuanlinggou Formation, which denote the presences of eucaryotes and protozoans respectively. The agreement of molecular characteristics with palaeoenvironmental and fossils data as derived from these strata suggests that the biomarkers preserved in these Proterozoic sediments are good indicators for the evolution of the palaeoenvironment and the early life in Yanshan basin.
The stable carbon isotopic characteristics of kerogen (813Ct) and coexisting carbonate (Sl3Ccait>) derived from the strata show a rapid decline of atmospheric CO2 concentration before 1.55Ga, and a stable concentration after 1.55Ga. It is confirmed that the difference (Ac) between the isotopic compositions of carbonate and associated kerogen can reflect the extent of carbon isotope fractionations accompanying biological usage of COa- The cyclic variations along the strata sequence exhibited by AC record may reflect the periodical marine transgression and regression that occurred in Yanshan basin during the Proterozoic age, and in turn, the changes of biocommumties adaptable to the changed environments.
The carbon isotopic relationships among kerqgens and n-alkanes and isoprenoids from these strata are consistent with the hypothesis that before 1.4Ga both n-alkanes and isoprenoids were mainly derived from heterotrophic halophiles and other possible archaebacteria, but after 1.4Ga only isoprenoids were still mainly originated from the archaebacteria while n-alkanes were significantly derived from primitive organic matter of photosynthetic organisms such as cyanobacteria. The change of biological origins of n-alkanes around 1.4Ga may suggest a marked decline of heterotrophic reworking to primitive lipids after 1.4Ga. This decline might be related to the formation of stable epicontinental sea characterized by shallow water environment. The isotopic relationship between individual hydrocarbons and associated kerogens derived from Jixian strata section may suggest special biogeochemical processes existed in closed Proterozoic Yanshan Basin compared to those of open sea system.
Rock-Eval analysis and kerogen degradations show that most of the kerogens from the strata section are over mature. Only the kerogen acquired from Hongshuizhuang Formation can meet the chemolysis and thermolysis of kerogen. Abundant structural and biological original information was obtained from this kerogen based on the integrated applications of multiple organic geochemical methods significantly including RTCO and Py-GC-MS. Moreover, the indigenous natures of soluble hydrocarbons derived from Hongshuizhuang Fm. are also suggested by these integrated applications.
The molecular and other geochcmicaf correlations between ttongshuizhuang i^m. and Nonesuch Fm. from Central North American Rift System show the possible linkage between North China Block and Laurentia Block before 1.1-1.2Ga.
Features and innovations in this study: (1) Longest successive time scale of Precambrian samples is studied; (2) The environmental and biological significances of the d
剖面生物标志化合物特征的调查显示整个剖面具有基本相似的分子组成。值得一提的是在剖面串岭沟组约1.8Ga的页岩中发现了指示真核生物存在的古老甾烷和指示原生动物存在的目前所知的最古老的伽马蜡烷。通过对剖面分子特征与独立的古环境和古生物资料的对比研究发现蓟县剖面中的有机分子很好地记录了燕山盆地元古宙各阶段的生物和古环境演化的信息。
干酪根和共生碳酸盐的碳同位素组成(δ~(13)C_k和δ~(13)C_(carb))以及二者的差值(Δ_C)反映了在全球大环境演化下的燕山盆地小生境的演化特征。δ~(13)C_k和δ~(13)C_(carb)的剖面特征表明，大约1.55Ga前，全球CO_2浓度曾持续快速下降，而之后趋于稳定。Δ_C被证明能有效反映局部环境中不同生物群落在利用CO_2过程中的碳同位素分异程度的差异。Δ_C在剖面上的规律性变化显示了燕山盆地生物整体同位素分异程度在元古宙演化过程中出现旋回式波动。这一波动能很好地被解释为燕山盆地周期性海进与海退所导致的不同生物群落的更迭。
单体烃碳同位素组成与共生干酪根碳同位素组成之间的关系提供了燕山盆地演化中更为深层次的有关生物地球化学循环方面的信息。剖面中具有较重同位素组成的类异戊二烯化合物和早于高于庄期(＞1.4Ga)的样品中的正构烷烃可能较多地来源于生存在燕山古海中的喜盐等古细菌类脂，而高于庄期后样品中的正构烷烃可能较多地起源于具有相对较轻同位素组成的原始藻类有机质。正构烷烃与共生干酪根碳同位素关系在高于庄末期(1.4Ga)的明显倒转可能表明在高于庄末期以后原始有机质的异养生物降解程度明显降低。这一降低可能与燕山盆地进入稳定的浅水陆表海沉积环境有关。蓟县剖面元古宙沉积有机质中独特的单体烃与共生干酪根的碳同位素关系特征地反映了具有明显局限特征
中科院广州地球化学研究所博士学位论文
的元古宙燕山盆地所特有的生物地球化学循环过程。
Rock－Eval等数据以及初步的干酪根化学和热降解的研究表明剖面中大部
分干酪根样品己对应成熟至油窗结束阶段，且只有来自剖面洪水庄组干酪根具
有开展全面有机地球化学研究的价值。多种有机地球化学方法对剖面洪水庄组
干酪根的综合研究不仅获得了洪水庄组干酪根重要的分子结构特征和有机质生
物起源的信息，而且还从干酪根的角度证实了洪水庄组可溶有机质原生性的本
质。
通过对剖面洪水庄组与北美老页岩组分子特征及其他地球化学特征的对比
表明华北地块很可能在1112亿年以前与劳伦大陆是紧紧挨在一起的。
此项研究具有以下特色和创新之处：（）研究对象连续时间跨度最长；门）
研究内容涉及面较全面；（3）较早详细探讨了前寒武纪沉积有机质的分子特征
与古环境和生物群落的演化关系；N）独立推导和论证了吵C＿和5’3C。的差
值（八C）的生物和环境的重要意义：6）在前寒武纪有机质研究中区分了局部
封闭环境下的生物地球化学循环过程与广域海环境下的生物地球化学过程的差
异：（6）开展了前寒武纪干酪根化学和热降解研究；（）开创性地将分子有机
地球化学的数据应用于元古宙Rodinia超大陆的重建中。
The Precambrian, one of the most important stages in the history of the Earth, so far, is still less known to us mostly because of the absence of intact morphological fossils in the Precambrian strata. This study systemically investigated the molecular (including soluble saturates and hydrocarbon products of keogen degradation) and carbon isotopic (including soluble hydrocarbons, kerogens and coexisted carbonates etc.) characteristics of Paleo- to Neoproterozoic (1.8-0.85Ga) sediments from the famous Jixian strata section, North China. The environmental and biological evolutions of Proterozoic Yanshan Basin companied by the global evolution were also discussed in detail with these molecular and isotopic data combined with independent palaeoenvironmental and palaeontologic information as acquired from these strata.
Analogous hydrocarbon types were detected in almost all samples from Jixian strata section. It is worth noting that the old steranes and the so far oldest gammacerane was detected in the l.SGa shales from Chuanlinggou Formation, which denote the presences of eucaryotes and protozoans respectively. The agreement of molecular characteristics with palaeoenvironmental and fossils data as derived from these strata suggests that the biomarkers preserved in these Proterozoic sediments are good indicators for the evolution of the palaeoenvironment and the early life in Yanshan basin.
The stable carbon isotopic characteristics of kerogen (813Ct) and coexisting carbonate (Sl3Ccait>) derived from the strata show a rapid decline of atmospheric CO2 concentration before 1.55Ga, and a stable concentration after 1.55Ga. It is confirmed that the difference (Ac) between the isotopic compositions of carbonate and associated kerogen can reflect the extent of carbon isotope fractionations accompanying biological usage of COa- The cyclic variations along the strata sequence exhibited by AC record may reflect the periodical marine transgression and regression that occurred in Yanshan basin during the Proterozoic age, and in turn, the changes of biocommumties adaptable to the changed environments.
The carbon isotopic relationships among kerqgens and n-alkanes and isoprenoids from these strata are consistent with the hypothesis that before 1.4Ga both n-alkanes and isoprenoids were mainly derived from heterotrophic halophiles and other possible archaebacteria, but after 1.4Ga only isoprenoids were still mainly originated from the archaebacteria while n-alkanes were significantly derived from primitive organic matter of photosynthetic organisms such as cyanobacteria. The change of biological origins of n-alkanes around 1.4Ga may suggest a marked decline of heterotrophic reworking to primitive lipids after 1.4Ga. This decline might be related to the formation of stable epicontinental sea characterized by shallow water environment. The isotopic relationship between individual hydrocarbons and associated kerogens derived from Jixian strata section may suggest special biogeochemical processes existed in closed Proterozoic Yanshan Basin compared to those of open sea system.
Rock-Eval analysis and kerogen degradations show that most of the kerogens from the strata section are over mature. Only the kerogen acquired from Hongshuizhuang Formation can meet the chemolysis and thermolysis of kerogen. Abundant structural and biological original information was obtained from this kerogen based on the integrated applications of multiple organic geochemical methods significantly including RTCO and Py-GC-MS. Moreover, the indigenous natures of soluble hydrocarbons derived from Hongshuizhuang Fm. are also suggested by these integrated applications.
The molecular and other geochcmicaf correlations between ttongshuizhuang i^m. and Nonesuch Fm. from Central North American Rift System show the possible linkage between North China Block and Laurentia Block before 1.1-1.2Ga.
Features and innovations in this study: (1) Longest successive time scale of Precambrian samples is studied; (2) The environmental and biological significances of the d
引文
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