Progress and prospects in the research on pore structures of organic-rich mud shales
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摘要:
探究富有机质泥页岩孔隙结构的划分方案、前沿表征方法、演化及发育影响因素，对页岩油储量评价及商业开发具有指导意义。通过调研富有机质泥页岩孔隙结构研究进展，归纳孔隙的划分方案，对比不同现代测试手段在泥页岩孔隙结构表征过程中的优劣性，探讨海、陆相泥页岩孔隙结构的演化模式和有机、无机孔隙发育的主控因素，展望富有机质泥页岩孔隙研究未来的发展趋势。结果表明：（1）泥页岩储层表征的手段主要可以划分为成像法、流体侵入法、吸附法、散射法四类。（2）红外连用的原子力显微镜（AFM-IR）能够揭示泥页岩中显微组分的化学和岩石力学非均质性，小角中子散射（SANS）、核磁共振（NMR）和纳米CT技术是揭示孔隙连通性的重要途径。（3）沉积环境控制着泥页岩岩相和有机质母质来源，成岩和生烃作用及其相互间影响是泥页岩孔隙演化的主控因素，海、陆相泥页岩孔隙演化随时间和深度总体上均有“减孔→增孔→减孔→增孔→减孔”的规律，但陆相泥页岩在未熟-成熟阶段孔隙变化得更频繁。（4）Ⅰ型干酪根的有机质孔发育潜力远高于Ⅲ型干酪根，强生烃能力的腐泥组显微组分可发育丰富的有机孔隙，液态烃运移之后经二次裂解形成的焦沥青能提供更有效的连续性渗透路径。（5）成岩过程中无机矿物间的相互转化，长石、碳酸盐岩等矿物差异性溶蚀，压实、压溶和胶结作用等均会复杂化无机孔隙网络，有机-无机相互作用及矿物自身的岩石力学性质也是无机孔隙发育的重要影响因素。岩心在地表和地下所处环境差异巨大，未来的研究需要建立一个页岩孔隙在地面与地层条件下的反馈机制和矫正机制，进一步还原页岩油气在地下孔隙结构中真实的赋存状态。
Abstract:Exploring the division scheme, frontier characterization method, evolution and influence factors of pore structures of organic-rich shales is important for the evaluation and development strategy of shale oil reserves. The classification scheme of the pore structure and the advantages of different modern testing tools in characterizing the pore structure of mud shale were summarized by investigating the research progress on the pore structures of organic-rich shales. The evolutionary patterns of pore structures and the main controlling factors of organic pores and inorganic pores in marine shales and continental shales were discussed. The future development trend of pore research in organic-rich shales was foreseen. Our results indicate that the means of shale reservoir characterization can be divided into four main categories: imaging method, fluid intrusion method, adsorption method, and scattering method. Infrared-linked atomic force microscopy (AFM-IR) can reveal non-homogeneity in the chemical and rock mechanics of microscopic components in mud shales. The application of small-angle neutron scattering (SANS), nuclear magnetic resonance (NMR), and nano-CT is an important way to reveal pore connectivity. The sedimentary environment controls the lithofacies of shale and the source of organic matter. Diagenesis, hydrocarbon generation and their interaction are the main controlling factors for pore evolution of shale. The porosity of marine and terrestrial mud shale exhibits a pattern of decreasing, subsequently increasing, once again decreasing, then increasing again, and finally decreasing, with time and depth. However, in the immature to mature stage of continental shale, the porosity changes occur more frequently compared with marine shale. The development potential of organic pores of type Ⅰ kerogen is much higher than that of type Ⅲ kerogen, and abundant organic pores can develop in sapropelic macerals with strong hydrocarbon generation capacity. Pyrobitumen, formed by secondary cracking of migratory liquid hydrocarbon, can provide a more efficient and continuous infiltration path. The interconversion between different inorganic minerals during diagenetic processes, the differential dissolution of feldspar, carbonate rock and other minerals, as well as the compaction, pressolution, and cementation of minerals, all complicate the inorganic pore network. Organic-inorganic interactions and the rock mechanical properties of minerals are also important influences on the development of inorganic pores. The environments in which cores are located at the surface and in the subsurface vary greatly, and future research needs to establish a feedback mechanism and correction mechanism for pore structure between surface and subsurface realities of the core, in order to further restore the real state of shale oil and gas in the pore structures of the subsurface.
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Key words:
- organic-rich shale /
- pore structure /
- maturity /
- pore evolution
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图 1 泥页岩孔隙大小分类（改自Loucks et al., 2012）
Figure 1.
图 2 页岩含油气系统成像、孔隙表征和物理化学测量的技术（改自Hackley et al., 2021）
Figure 2.
图 3 高压压汞与小角中子散射孔隙/孔喉分布对比（张林浩等, 2021）
Figure 3.
图 4 松辽盆地青一段页岩样品萃取前后1H化合物2D NMR检测谱图（白龙辉等, 2021）
Figure 4.
图 5 页岩内组分物质的三维分布（苟启洋等, 2018）
Figure 5.
图 6 FIB-HIM 镜下龙马溪组页岩焦沥青及有机质孔隙发育特征（王朋飞等, 2020）
Figure 6.
图 7 泥页岩样品三维形貌（改自Liu et al., 2019）
Figure 7.
图 8 俄亥俄州泥盆系页岩样品海洋藻类的CLSM图像（Hackley et al., 2020）
Figure 8.
图 10 海陆相富有机质泥页岩孔隙结构演化模型（改自Wang Y et al., 2019；黄振凯等, 2020）
Figure 10.
图 11 泥页岩生、排、滞留烃模式（基于Tissot and Welte, 1978修改）
Figure 11.
图 12 固体沥青在反射光和油浸下形态的显微照片（Mastalerz et al., 2018）
Figure 12.
图 13 固体沥青和焦性沥青源岩的生成过程、温度和成熟度示意图（改自Mastalerz at al., 2018）
Figure 13.
图 14 泥页岩埋藏成岩作用主要阶段与孔隙类型/丰度演变之间的关系图（改自Loucks et al., 2012）
Figure 14.
图 15 矿物组成对泥页岩孔隙发育和保存的影响三角图（改自Loucks et al., 2012）
Figure 15.
表 1 不同沉积背景下页岩岩相及孔隙特征
Table 1. Lithofacies and pore features of shales under different sedimentary backgrounds
沉积背景 研究对象 优势岩相 孔隙特征 海相 四川盆地龙马溪页岩 富有机质硅质页岩（中粗纹层组合段岩性为砂质、粉砂质、碳酸盐岩） 高孔体积及比表面积 海陆过渡相 鄂尔多斯盆地临兴
地区太原组富有机质黏土类页岩 有机质孔较为发育，微孔发育较好，孔隙体积和比表面积较大，生烃潜力明显 陆相 川东北陆相页岩 富有机质（高腐泥质）泥质页岩和富有机质（高腐泥质）混合质页岩（硅泥比2/3） 发育大量黏土矿物孔隙和有机质孔隙 吉木萨尔凹陷芦草沟组 富有机质长英质岩屑粉细砂岩和云质粉砂岩 孔隙度高，多发育大孔径的粒间（溶）孔、粒内溶孔 玛湖凹陷风城组 粉细砂岩、泥质粉砂岩及白云岩 孔隙度高，多发育大孔径的粒间（溶）孔、粒内溶孔 古龙凹陷青山口组 富有机质硅质页岩 孔隙度高，孔径分布呈介孔-宏孔“双峰”分布，粒间孔隙发育 
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