Research Progress of Burial Dissolution and Modification of Carbonate Reservoirs and Fluid⁃Rock Simulation Experiments
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摘要: 深层-超深层碳酸盐岩是当前全球油气勘探的焦点，也是未来我国有望实现油气商业发现的热点领域. 对于深埋藏环境下优质碳酸盐岩储层形成而言，目前研究普遍强调了早期表生溶蚀作用和晚期埋藏溶蚀改造作用的重要性. 作为表征储层溶蚀作用机理的有效手段，水岩溶蚀模拟实验能够再现实际地质条件下碳酸盐岩和地层流体之间的相互作用过程，为碳酸盐岩储层溶蚀改造研究提供了新视角.为此，系统回顾了近年来碳酸盐岩溶蚀模拟实验的研究进展，并尝试从实验模拟的角度讨论溶蚀作用对深层-超深层碳酸盐岩成储过程的控制作用.首先回顾了碳酸盐岩储层的溶蚀改造作用，同时总结了碳酸盐岩水岩溶蚀模拟实验的技术与方法，其次梳理了基于溶蚀模拟实验取得的碳酸盐岩储层溶蚀改造规律与认识，最后展望了现有研究对深层-超深层油气勘探以及碳封存与再利用中的应用前景.不难看出，开展碳酸盐岩溶蚀模拟实验有望为寻找埋藏成岩过程中的次生孔隙发育带、阐释规模性溶蚀作用发生的有利条件提供依据，同时也可为未来碳酸盐岩成储机制和实验模拟研究提供一定的借鉴意义.Abstract: Deep to ultra⁃deep carbonate reservoirs have always been the focus of global oil and gas exploration at present, which are also the future fields of commercial hydrocarbon discovery in China. The importance of early epigenetic dissolution and/or late burial dissolution modification has been generally emphasized for the formation of high⁃quality carbonate reservoirs in deep burial environments. As an effective way to characterize the mechanism of reservoir dissolution, the fluid⁃rock dissolution simulation experiment can reproduce the interaction process between carbonate rocks and diagenetic fluids under actual geological conditions, thus providing a new perspective for determining the dissolution and modification of carbonate reservoirs. In this paper, the research progress of carbonate dissolution simulation experiments in recent years is systematically reviewed. In addition, the controlling factors of dissolution on the formation of deep to ultra⁃deep carbonate rocks are discussed from the perspective of experimental simulation. Firstly, the dissolution and modification of carbonate reservoirs are reviewed, and the techniques and methods of carbonate fluid⁃rock dissolution simulation experiments are summarized. Secondly, the law and understanding of carbonate reservoir dissolution and modification based on simulation experiments are sorted out. Finally, the application prospect of current research on deep to ultra⁃deep hydrocarbon exploration and carbon sequestration and recycling is prospected. Generally, the simulation experiment of carbonate dissolution is expected to provide a basis for discovering the secondary pore development zones during burial diagenesis and clarifying the favorable conditions for the occurrence of large⁃scale dissolution. Furthermore, this work can provide certain reference significance for future research on the formation mechanism and experimental simulation of carbonate reservoirs.
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图 1 四川盆地三叠系飞仙关组鲕滩储层中的铸模孔形成模式图
修改自冯林杰等(2021)
Fig. 1. Schematic diagram showing formation of moldic pore system in the Triassic Feixianguan oolitic shoal reservoir
图 2 不同深度范围碳酸盐岩孔隙度分布特征统计图
修改自马永生等(2019)
Fig. 2. Statistical chart of porosity distribution characteristics of carbonate rocks in different depth ranges
图 4 (a) 半开放体系中碳酸盐岩的溶蚀质量损失率与温度的关系(数据引自He et al., 2017)；(b)含不同有机酸浓度的地层水中碳酸盐岩饱和溶蚀量与温度的关系(数据佘敏等，2020)
Fig. 4. (a)Relationship between carbonate dissolution weight loss and temperature in the semi⁃open system(modified after He et al., 2017); (b)Relationship between saturated dissolution and temperature of carbonate rocks in formation water with different organic acid concentrations(modified after She et al., 2020)
图 5 基于“反应-传输模型”的水岩界面反应示意图(修改自Shabani and Zivar, 2020)
Fig. 5. A geochemical⁃transport model⁃based schematic of the brine⁃rock reaction on the interface(modified after Shabani and Zivar, 2020)
图 6 溶蚀改造后的白云石晶体表面微观形态特征
修改自Jones(2013)；a. 白云石内部沿裂隙优先发生溶蚀；b. 溶蚀作用形成残余“蜂窝状”或“网格状”空间；c. 菱形溶坑扩溶、合并形成“蜂窝状”结构；d，e. 晶体内部的差异性溶蚀作用，CB. 晶体核心与边缘分界，GSB. 晶体生长分区边界
Fig. 6. Microarchitecture of dolomite crystals after dissolution
图 7 不同岩性的碳酸盐岩样品溶蚀改造后孔隙结构和表面溶蚀深度对比
修改自Jora et al.(2021); a, b. 为Mg含量较高的样品1的核磁T2图谱和CT扫描获得的表面酸蚀深度分布与热图成像; c, d. 为Mg含量较低的样品2的核磁T2图谱和CT扫描获得的表面酸蚀深度分布与热图成像
Fig. 7. Pore structure and surface dissolution distance of carbonate rock samples
图 8 溶蚀过程中岩样的渗透率演化规律
Fig. 8. Figure showing the evolution of rock permeability during dissolution
表 1 不同水岩溶蚀模拟实验技术与方法对比
Table 1. Comparison of experimental techniques and methods of different water rock dissolution simulations
研究方法 模拟条件 主要研究内容 样品要求 方法评述 反应前后的溶蚀效果对比 参考文献 旋转岩盘 温度：0~200 ℃
压力：0~50 MPa(1)溶蚀反应速率
(2)宏/微观岩石表面形貌演化
(3)水-岩反应体系成分变化柱塞样(直径3.8 cm，长度2.0 cm) 优势：操作步骤简单，实验流程便捷易行
局限：反应体系封闭，适用条件受限
范明等(2009)；黄康俊等(2011)；Yoo et al.(2018) 高温高压釜 温度：0~600 ℃
压力：0~120 MPa(1)溶蚀反应速率
(2)岩石饱和溶蚀量
(3)宏/微观岩石微观形貌演化
(4)水-岩反应组分原位分析
(5)渗透率在线检测柱塞样(直径2.5 cm，长度3.8 cm)；颗粒样(粒径 > 0.85 mm) 优势：可实时检测柱塞样渗透率变化
局限：无法开展致密岩性的内部溶蚀改造实验
寿建峰等(2016)；彭军等(2018)；佘敏等(2020) 金刚石压腔 温度：0~600 ℃
压力：0~120 MPa(1)微观溶蚀反应能力
(2)微观矿物溶蚀-沉淀行为
(3)水-岩反应组分原位分析颗粒样(150目，100 μm) 优势：可开展微观矿物尺度研究，与配套方法结合可实现反应过程原位观测
局限：样品制备与实验流程复杂
杨云坤等(2014)；张单明等(2015)；刘诗琦等(2021) 人工合成包裹体 温度：0~200℃
压力：0~0.06 MPa(1)微观溶蚀反应能力
(2)微观矿物溶蚀-沉淀行为
(3)水-岩反应组分原位分析颗粒样(粒径 < 0.3 mm) 优势：可与配套方法结合实现反应过程原位观测，开展矿物与富硅流体水岩反应时无需额外引入SiO2
局限：熔融硅管胶囊制备复杂
Chou et al.(2008)；王小林等(2017) 注：*表 1所列不同类型实验适用的模拟温压条件来自本文引用的文献中的实际实验条件(统计时间截至2022年8月)，并不代表该方法所能达到的极限温压条件. 
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