Research progress of CO2 storage technology by mineralization of coal-based solid waste
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摘要:
“碳达峰、碳中和”目标是中国维护全球生态安全的大国责任担当，也是实现高质量发展和生态文明建设的重要途径，CO2减排势在必行。“相对富煤、贫油、少气”的能源资源禀赋格局导致中国主体能源仍以碳排放强度较高的煤炭为主，煤炭作为电力、钢铁、煤化工等高耗能行业的重要能源与原料，在“双碳”目标实现过程中占有重要地位，煤炭工业通过低碳转型实现碳达峰，既是煤炭工业高质量发展的内在要求，也是落实国家“双碳”战略目标的重要抓手。相对于传统天然矿化原料，煤基固废矿化封存CO2具有原料丰富、产物友好、能耗较低、反应迅速等优点，同时可以产出高附加值产物用于化工、建筑等领域，受到了广泛的关注。介绍了我国主要煤基固废煤矸石、粉煤灰、脱硫石膏、气化渣、炉底渣的特点，分析了我国主要CO2排放源及产生量；回顾了按照矿化封存位置不同的原位和非原位CO2矿化技术及按照矿化机理不同的直接碳酸化和间接碳酸化技术；综述了以煤基固废作为原料进行CO2矿化封存技术的研究进展，发现该技术反应条件苛刻，成本较高，处理规模小，研究尚停留在实验室阶段；简述了以煤基固废作为载体，利用采空区作为储源矿化封存CO2技术，主要包括构筑功能性充填体及制备负碳型充填材料2种技术；分析了煤基固废矿化封存CO2现存问题及未来研究方向。煤基固废为原料的CO2矿化技术，未来应优化工艺流程，降低反应成本，进一步加强工业化推广的研究；针对以煤基固废作为载体，利用采空区作为储源的CO2矿化封存技术，未来应加强对深度矿化机理、封存风险评价及长期稳定性的研究，提高CO2封存规模和长期稳定性。在此基础上，利用煤基固废制备浆体充填材料，以水为载体，以泵为动力，以管路为通道，将充填材料及CO2输送至采空区进行矿化反应，同时结合微生物诱导碳酸钙沉淀（MICP）技术，封闭岩体采动裂隙，实现CO2矿化封存。
Abstract:The goal of “carbon peak and carbon neutrality” is China’s responsibility as a major country to maintain global ecological security, and it is also an important way to achieve high-quality development and ecological civilization construction. CO2 emission reduction is imperative.As a result of the energy resource endowment pattern of “rich in coal, poor in oil and less gas”, the main energy in China is still coal with high carbon emission intensity. Coal is an important energy and raw material for high energy-consuming industries such as electric power, iron and steel and coal chemical industry. it plays an important role in the process of achieving the goal of “double carbon”. The coal industry achieves carbon peak through low-carbon transformation, which is the inherent requirement of the high-quality development of coal industry. It is also an important starting point for the implementation of the national “double carbon” strategic goal. Compared with the traditional natural mineralization raw materials, coal-based solid waste mineralization and storage CO2 has the advantages of rich raw materials, friendly products, low energy consumption and rapid reaction. At the same time, it can produce high value-added products for chemical industry, construction and other fields. The characteristics of main coal-based solid waste coal gangue, fly ash, desulphurization gypsum, gasification slag and furnace bottom slag in China are introduced, the main CO2 emission sources and production in China are analyzed, and the in-situ and ex-situ CO2 mineralization technologies according to different mineralization and storage locations and direct and indirect carbonation technologies according to mineralization mechanism are reviewed. The research progress of CO2 mineralization and storage technology using coal-based solid waste as raw material is reviewed, and it is found that this technology has harsh reaction conditions, high cost, small treatment scale, and the research is still in the laboratory stage. This paper briefly describes the mineralization and storage technology of CO2 with coal-based solid waste as carrier and goaf as storage source, which mainly includes two technologies: construction of functional filling body and preparation of negative carbon filling material. The existing problems and future research direction of coal-based solid waste mineralization and storage of CO2 are analyzed. For the CO2 mineralization technology with coal-based solid waste as raw material, the technological process should be optimized, the reaction cost should be reduced, and the research on industrialization promotion should be further strengthened. aiming at the CO2 mineralization and storage technology with coal-based solid waste as carrier and goaf as storage source, the research on deep mineralization mechanism, storage risk assessment and long-term stability should be strengthened in the future, so as to improve the storage scale and long-term stability of CO2. On this basis, the slurry filling material is prepared from coal-based solid waste, with water as carrier, pump as power and pipeline as channel, the filling material and CO2 are transported to the goaf for mineralization reaction, and combined with microbial induced calcium carbonate precipitation (MICP) technology, the mining fissures in rock mass are closed to realize CO2 mineralization and storage.
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图 1 宁东基地煤基固废产量和利用率
Figure 1. Production and utilization rate of coal-based solid waste from Ningdong Base
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图 3 2022年世界不同地区及主要国家二氧化碳排放量
Figure 3. Carbon dioxide emissions from different regions and major countries in world in 2022
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图 4 2000—2022年全球与能源有关的温室气体排放
Figure 4. Global energy-related greenhouse gas emissions, 2000—2022
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图 8 矿山功能性充填的CO2封存架构
Figure 8. CO2 storage architecture for functional filling in mines
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图 9 煤基固废充填井下碳封存工艺
Figure 9. Underground carbon storage technology for coal based solid waste filling
表 1 典型原位矿化试点项目
Table 1 Typical in-situ mineralization pilot project
地区 储源 盖层 储存潜力 美国纽约州 含钙斜长石和辉石的榴辉岩，
目标层孔隙度5%[28-29]纽瓦克盆地的湖相沉积，泥岩、长石、
碳酸盐结核、页岩和碎屑层序测试榴辉岩的CO2缓存潜力 美国华盛顿州、俄勒冈州
和爱达荷州哥伦比亚河玄武岩群目标层孔隙度
为15%～25%[30-31]渗透率极低的玄武岩层 10～50 Gt CO2 美国东海岸近海 桑迪胡克盆地玄武岩，孔隙度15%[32] 沉积盖层、泥岩、粉砂、黏土 900 Mt CO2 美国西海岸近海 胡安德富卡板块玄武岩，平均孔隙率为10%[33] 细粒浊积层序与黏土沉积 920 Gt CO2 冰岛 超基性至碱性（45%～49%SiO2）玄武岩流动和橄榄拉斑
玄武岩组成的透明碎屑岩[34-35]低孔玄武岩 12 Mt CO2 
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