页岩CO2封存中的矿物溶蚀/沉淀特征及作用规律

doi:10.7623/syxb202412009

石油学报 ›› 2024, Vol. 45 ›› Issue (12): 1833-1850.DOI: 10.7623/syxb202412009

页岩CO₂封存中的矿物溶蚀/沉淀特征及作用规律

代旭光^1,2, 桑树勋^1,2, 王猛^1,2, 刘世奇^1,2, 郑司建^1,2, 宋新贺³, 师轩⁴, 宋昱⁵, 冯光俊⁵, 全方凯⁶

1. 中国矿业大学江苏省煤基温室气体减排与资源化利用重点实验室江苏徐州 221008;
2. 中国矿业大学碳中和研究院江苏徐州 221008;
3. 鸿灌环境技术有限公司江苏苏州 215200;
4. 南京晨光集团有限责任公司江苏南京 210006;
5. 中国矿业大学煤层气资源与成藏过程教育部重点实验室江苏徐州 221008;
6. 安徽理工大学安全科学与工程学院安徽淮南 232001

收稿日期:2024-04-25 修回日期:2024-08-12 出版日期:2024-11-25 发布日期:2025-01-03
通讯作者: 桑树勋,男,1967年11月生,1994年获中国矿业大学博士学位,现为中国矿业大学碳中和研究院院长、教授、博士生导师,主要从事碳中和地质技术(CO₂地质封存等)、煤系非常规油气勘探开发相关研究。Email:shxsang@cumt.edu.cn
作者简介:代旭光,男,1991年8月生,2023年获中国矿业大学地质资源与地质工程专业博士学位,现为中国矿业大学碳中和研究院博士后,主要从事CO₂地质封存、煤系非常规天然气地质相关研究。Email:18252430765@163.com
基金资助:
国家重点研发计划项目(2023YFE0120500)、国家自然科学基金青年科学基金项目(No.42402177,No.42302194,No.42202190)、国家资助博士后研究人员计划项目(GZC20233002)和中央高校基本科研业务费专项资金项目(2023KYJD1001,2024QN11069)资助。

Mineral corrosion/precipitation characteristics and regularities during CO₂ sequestration in shale

Dai Xuguang^1,2, Sang Shuxun^1,2, Wang Meng^1,2, Liu Shiqi^1,2, Zheng Sijian^1,2, Song Xinhe³, Shi Xuan⁴, Song Yu⁵, Feng Guangjun⁵, Quan Fangkai⁶

1. Jiangsu Key Laboratory of Coal-based Greenhouse Gas Control and Utilization, China University of Mining and Technology, Jiangsu Xuzhou 221008, China;
2. Carbon Neutrality Institute, China University of Mining and Technology, Jiangsu Xuzhou 221008, China;
3. Hongguan Environmental Technology Company Limited, Jiangsu Suzhou 215200, China;
4. China Aerospace Science and Industry Nanjing Chenguang Group, Jiangsu Nanjing 210006, China;
5. MOE Key Laboratory of Coalbed Methane Resource & Reservoir Formation Process, China University of Mining & Technology, Jiangsu Xuzhou 221008, China;
6. School of Safety Science and Engineering, Anhui University of Science and Technology, Anhui Huainan 232001, China

Received:2024-04-25 Revised:2024-08-12 Online:2024-11-25 Published:2025-01-03

摘要/Abstract

摘要： 超临界CO₂(scCO₂)反应会引起页岩的物质成分和储渗条件发生动态变化,但目前对于以溶蚀/沉淀等为特征的水-岩反应及其作用规律研究鲜有报道。基于高压水热反应实验装置和系列表征测试,分析了scCO₂-水-页岩反应过程中页岩在化学组分、矿物成分、表面形貌和孔隙结构方面的变化特征,揭示了在CO₂封存条件下页岩产生矿物溶蚀、离子溶出和沉淀作用的规律。研究结果表明:在短期反应过程中,页岩主要表现出溶蚀特征,其内方解石形貌发生改变,次生溶蚀孔发育;在长期反应过程,页岩仍以溶蚀作用为主,并在局部伴有碳酸盐沉淀现象。溶蚀过程主要受方解石的发育条件控制,方解石溶蚀导致页岩的孔体积和比表面积增大;沉淀过程受以伊利石和伊/蒙混层为代表的黏土矿物的影响,二者含量的增加会导致更多碳酸盐沉淀产生。scCO₂-水-页岩反应总体上表现为一种以溶蚀作用为主、沉淀作用为辅的地球化学行为。在溶蚀/沉淀作用下,页岩的封存空间呈正向递增演化;方解石的溶蚀有利于提高页岩的封存能力;而黏土矿物可为CO₂的矿化封存提供必要的阳离子。研究页岩在CO₂封存中的溶蚀/沉淀特征有助于了解在CO₂封存条件下的矿物-流体地球化学作用规律,对于揭示页岩的CO₂地质封存机理和发展页岩气强化开采技术有重要的参考价值。

关键词: 页岩气储层, CO₂地质封存, 超临界CO₂-水-页岩反应, 矿物成分, 溶蚀/沉淀特征

Abstract: Supercritical CO₂ (scCO₂) reaction may lead to dynamic changes in the material composition, accumulation and seepage conditions of shale. However, there are few reports on the water-rock reaction characterized by corrosion/precipitation and its influence regularities. Based on the use of high-pressure hydrothermal reaction experimental device and a series of characterization tests, the paper analyzes the changes of shale in chemical composition, mineral composition, surface morphology and pore structure during scCO₂-water-shale reaction, revealing the regularities of mineral corrosion, ion dissolution and precipitation in shale under CO₂ sequestration conditions. The results show that in the short-term reaction process, shale primarily exhibits corrosion characteristics, with changes in the internal calcite morphology and the development of secondary corrosion pores. In the long-term reaction process, corrosion is still dominant in shale, accompanied with occasional carbonate precipitation in partial areas. The corrosion process is mainly controlled by the development conditions of calcite, and calcite corrosion leads to an increase in the pore volume and specific surface area of shale. The precipitation process is affected by clay minerals represented by illite and illite/smectite mixed layers, and an increase in both contents can lead to the formation of more carbonate precipitates. In general, scCO₂-water-shale reaction exhibits a geochemical behavior that predominated by corrosion and supplemented by precipitation. Under the effect of corrosion or precipitation, the sequestration space in shale presents a positive incremental evolution. The calcite corrosion helps improve hydrocarbon sequestration capability in shale. Clay minerals can provide essential cations for CO₂ mineralization. The investigation on the corrosion/precipitation characteristics of shale during CO₂ sequestration can help understand the geochemical regularities of minerals and fluids under CO₂ sequestration conditions, which is of great reference value for revealing the CO₂ geo-sequestration mechanism of shale and developing the enhanced shale gas recovery techniques.

Key words: shale gas reservoir, CO₂ geo-sequestration, scCO₂-water-shale reaction, mineral composition, corrosion/precipitation characteristics

中图分类号:

TE122.3

代旭光, 桑树勋, 王猛, 刘世奇, 郑司建, 宋新贺, 师轩, 宋昱, 冯光俊, 全方凯. 页岩CO₂封存中的矿物溶蚀/沉淀特征及作用规律[J]. 石油学报, 2024, 45(12): 1833-1850.

Dai Xuguang, Sang Shuxun, Wang Meng, Liu Shiqi, Zheng Sijian, Song Xinhe, Shi Xuan, Song Yu, Feng Guangjun, Quan Fangkai. Mineral corrosion/precipitation characteristics and regularities during CO₂ sequestration in shale[J]. Acta Petrolei Sinica, 2024, 45(12): 1833-1850.

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页岩CO₂封存中的矿物溶蚀/沉淀特征及作用规律

Mineral corrosion/precipitation characteristics and regularities during CO₂ sequestration in shale

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