Origin of grained dolomite from the Buqu Formation of Zaring area in southern Qiangtang depression
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摘要:
以青藏高原南羌塘坳陷扎仁地区中侏罗统布曲组晶粒白云岩为对象对其进行成因的研究。通过显微镜观察、流体包裹体数据以及碳氧同位素分析，认为研究区白云岩可分为细粉晶白云岩、中晶白云岩以及粗晶白云岩，在裂隙附近还广泛发育晶粒较粗大的鞍形白云石。白云石中流体包裹体均一温度在150.2~216.0℃，盐度均值达到了24.5% NaCl，远高于方解石包裹体均一温度与盐度，表明白云石的形成经历了高温高盐度的过程。白云石碳氧同位素分析显示其δ13CPDB值为-0.01‰~3.43‰，δ18OPDB值为-11.17‰~-7.68‰，通过白云石-水氧同位素分馏方程得到白云化流体的δ18OSMOW值为4.82‰~12.85‰，δ13CPDB对比认为白云石受寄主灰岩环境的影响。通过碳氧同位素数据对比以及前人的研究结果，认为研究区白云岩为相对封闭环境下受岩浆活动加热的高盐度流体对寄主灰岩交代的产物，高盐度流体由于镁离子的消耗导致流体对方解石过饱和，继而沉淀了高温的方解石。因此，热液活动对研究区中侏罗统布曲组白云岩的发育具有重要意义，值得加强对这一方向的探索研究。
Abstract:The genetic mechanism of dolomite of the Middle Jurassic Buqu Formation in the Qiangtang depression was studied by using microscopy, fluid Inclusion data, and carbon and oxygen isotope analysis. The results show that the dolomites in the study area can be divided into fine-powdery dolomite, medium dolomite and coarse dolomite according to grain size. Dolomite generally has a fogged center and clear margin structure, in the cracks near the extensive development of grained saddle dolomite. Fluid inclusions in the dolomite have homogenization temperature ranging between 150.2 and 216.0℃ and average salinity of 24.5%NaCl, much higher than the homogenization temperature and salinity of fluid inclusions in calcite, indicating a high temperature and high salinity diagenetic environment. The isotopic analysis shows that δ13CPDB values vary from-0.01‰ to 3.43‰, and δ18OPDB values vary from-11.17‰ to -7.68‰; according to the dolomite-fluid oxygen isotope fractionation equation, the δ18OSMOW values of dolomitization fluid are in the range of 4.82‰-12.85‰, It is believed that the matrix dolomite and the saddle dolomite that are filled in the pores in the study area are the products of host limestone altered by the high salinity fluid heated by the magma activity in a close environment, while the high salinity fluid due to the consumption of magnesium ions led to over-saturation of fluid calcite and then to the precipitation if high-temperature calcite. Therefore, hydrothermal activity was very significant for the development of dolomite of the Middle Jurassic Buqu Formation in the study area.
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Keywords:
- fluid inclusion /
- carbon and oxygen isotope /
- dolomite /
- Buqu Formation /
- Zaring area
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1. 研究目的(Objective)
中国从2009年开展页岩气实质勘探以来，已在四川盆地上奥陶统五峰组(O3w)—下志留统龙马溪组(S1l)海相页岩成功实现页岩气商业开发，成为世界上少数几个实现页岩气工业开采的国家之一，近年来掀起了页岩气研究的热潮。国内学者在页岩气的形成、演化、保存和成藏等方面取得诸多突破，同时也遇到诸多科学难题，如地质条件下页岩的成烃演化规律、页岩气乙烷碳同位素与干酪根碳同位素差异较大、页岩气烷烃气碳同位素倒转等，究其原因是页岩气组分单一，难以获取较多的地球化学信息。川南五峰组—龙马溪组海相页岩中含H2S天然气的发现(N201-H1井，H2S含量=0.42%)，激发了笔者探索海相页岩气中H2S成因的兴趣。本文力争从海相页岩中找出H2S形成的地质、地球化学证据，尤其成烃演化过程中伴随的TSR证据，并探讨TSR与页岩气地球化学异常的关系。
2. 研究方法(Methods)
通过野外地质调查，系统采集重庆高谷剖面五峰组—龙马溪组含黄铁矿富有机质页岩，开展TOC测定、全岩X衍射分析、岩石薄片鉴定、扫描电镜与能谱分析、次生方解石碳同位素分析、方解石中包裹体分析。利用有机无机相结合的研究手段，重点关注页岩中黄铁矿的赋存形态、与有机质和无机矿物的共生关系，进而明确黄铁矿可能的成因类型。所有分析测试和研究工作均在页岩油气富集机理与有效开发国家重点实验室完成。
3. 研究结果(Results)
五峰组—龙马溪组样品(15件)的TOC介于1.6%~4.5%，均值为2.8%，岩矿分析结果显示为硅质页岩，黄铁矿含量介于4.5%~7.3%。多数样品中可见草莓状黄铁矿集合体零星或呈层状分布，粒径主要介于5~10 μm(11件)，个别样品中可见笔石黄铁矿化现象，其中的黄铁矿多为草莓状黄铁矿(3件)。在五峰组的2件样品中发现黄铁矿-石膏-方解石的共生脉体顺层发育，肉眼和镜下可见矿铁矿晶体呈立方体(图 1a)，从矿物之间的接触关系看，石膏最先形成，边缘有明显的溶蚀迹象，其次是黄铁矿，再是方解石(图 1b)；脉体上下页岩层中方解石碳同位素介于-0.5‰~-2.4‰，均值为-1.6‰(4件)，脉体中挑选出来的方解石碳同位素介于-5.2‰~-9.6‰，均值为-7.5‰(6件)，明显轻于页岩中的方解石碳同位素；脉体方解石中赋存气-液包裹体均一温度介于103℃~148℃，集中在135℃附近(12个点)。
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图 1 黄铁矿的分布及形态特征(Adr—石膏；Py—黄铁矿；Cal—方解石)Figure 1. Distribution and morphological characteristics of pyrite(Adr-Gupusm; Py-Pyrite; Cal-Calcite)沉积岩中黄铁矿的硫源主要源自H2S，而H2S主要成因为细菌硫酸盐还原作用(BSR)、热化学硫酸盐还原作用(TSR)和含硫有机质裂解作用(TDR)。五峰组—龙马溪组页岩中受控于原始有机质分布的草莓状黄铁矿属于同生期的BSR成因，而五峰组中发现的脉体具备TSR发生的物质和能量条件，辅以混入有机碳源的次生方解石证据，可以推断该区富有机质页岩成烃演化过程中发生过TSR反应，但由于H2S形成后极易与页岩中的金属离子结合而以硫化物的形式沉淀下来，导致现今海相页岩气藏中普遍不含和微含硫化氢，但是其对页岩气地球化学特征的影响不容忽视。已有模拟实验证明，可溶有机质裂解过程中TSR会导致烷烃气碳同位素序列倒转，因此，五峰组—龙马溪组页岩气碳同位素倒转可能与TSR有关。
4. 结论(Conclusions)
(1) 四川盆地五峰组—龙马溪组富有机质页岩层段普遍发育黄铁矿，其中大部分为受控于原始有机质分布的草莓状黄铁矿，为BSR成因；特殊的矿物组合、次生方解石碳同位素偏轻和包裹体均一温度表明部分黄铁矿为有机质成烃演化过程中的TSR成因。
(2) 硫化氢遇到金属离子极易以硫化物的形式沉淀下来，所以同生期BSR形成的硫化氢很难保存至今，现今页岩气藏中的硫化氢最可能是TSR形成。TSR不仅可以改变页岩气化学组成，还可能是导致页岩气碳同位素倒转的重要因素，值得进一步深入研究。
5. 致谢(Acknowledgement)
本文为国家自然科学基金项目“页岩解析气碳同位素分馏特征及其指示意义研究”(41503033)、石油化工联合基金重点项目“古生界页岩含气性原生有机质控制作用研究”(U1663202)和“海相含膏盐岩层系烃源岩发育特征与生烃潜力评价”(U1663201)的资助成果。
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图 1 扎仁地区布曲组白云岩分布及采样位置图
Figure 1. Distribution and sampling location of dolostones of Buqu Formation in Zaring area
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图 2 扎仁地区布曲组白云岩野外露头及柱状图
a—白云岩宏观露头照片；b—具水平纹层的白云岩；c—介壳白云岩；d—地表被风化白云岩；e—柱状图
Figure 2. Dolostone outcrops and stratigraphic column of Buqu Formation in Zaring area
a-Macroscopic outcrop photo of dolomite; b-Dolomite with horizontal lamina; c-Shell dolomite; d-Weathered dolomite; e- Columnar section of Buqu Formation
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图 3 布曲组白云岩显微照片（单偏光）
a—细粉晶白云岩；b—中晶白云岩，白云石具雾心亮边结构；c—粗晶白云岩；d—粉晶白云岩与裂隙附近的鞍形白云石构成不等晶结构
Figure 3. Photomicrographs of dolostone from Buqu Formation
a-Powder-fine crystallographic dolostone; b-Medium crystallographic dolostone, dolomite having a bright edge structure with fog; c-Coarse crystallographic dolostone; d-Powder crystallographic dolomite combined with the void-filling saddle dolomite to form crystal structure
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图 4 白云石与方解石包裹体均一温度分布直方图
Figure 4. Homogenization temperature histogram of fluid inclusions from dolomites and calcite
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图 5 Land分馏方程计算的温度与白云石矿物以及流体δ18O关系图
Figure 5. Plots of equilibrium relationship between δ18O fluid and temperature for various δ18O dolomite from Land's fractionation equation
表 1 白云石与方解石流体包裹体均一温度与盐度分析结果
Table 1 Analytical data of homogenization temperature and salinity of fluid inclusions in dolomite and calcite
下载: 导出CSV
表 2 布曲组白云岩碳氧同位素分析结果
Table 2 Analytical data of oxygen and carbon stable isotopes from dolostones from Buqu Formation
下载: 导出CSV
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