Quantifying the Limits of CH4–CO2 Hydrate Replacement: Impact of Critical Replacement Thickness, Particle Size, and Flow Rate on Recovery Efficiency

IF 5.3 3区 工程技术 Q2 ENERGY & FUELS Energy & Fuels Pub Date : 2025-03-18 DOI:10.1021/acs.energyfuels.5c00371
Jin-Rong Zhong, Kai-Bo Huang, Shan Yang, Zuo-Zhi Luo, Ya-Xuan Zhu, Li Wan, Yi-Fei Sun, Chang-Yu Sun, Guang-Jin Chen and Yue-Fei Zhang*, 
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Abstract

The CH4–CO2 hydrate replacement exploitation method has gained high attention, but its low recovery efficiency hampers its application, and the reported limits of CH4–CO2 replacement vary greatly among different studies. This study introduces the concept of critical replacement thickness to quantify the exploitation limits of CH4–CO2 hydrate replacement, based on a series of CH4–CO2 replacement experiments conducted in a one-dimensional high-pressure reactor with well-defined hydrate-bearing sediments. Real-time hydrate composition analysis was employed to calculate the CH4–CO2 replacement limitation and critical replacement thickness at various stages of CO2 flooding. The results show that during the initial stage, the replacement thickness is approximately 2–4 μm, while it decreases to 0.1–0.3 μm in the final stage. Additionally, the study systematically examines the impact of the hydrate particle size and fluid flow rate on CH4 recovery and CO2 sequestration. It is found that smaller particle sizes and higher flow rates significantly improve recovery efficiency, with CH4 recovery increasing from 39.1 to 63.4% through optimization of these factors. Moreover, the mass transfer resistance created by the reformed CH4–CO2 hydrate film restricts the critical replacement thickness to no more than 7 μm for a particle size distribution of 0–250 μm without additional stimulation. The findings provide a clearer understanding of the factors influencing CH4 recovery and offer insights into optimizing the replacement method for improved efficiency. These results contribute to the development of more effective strategies for the CH4–CO2 replacement exploitation in hydrate reservoirs.

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量化CH4-CO2水合物置换极限:临界置换厚度、粒径和流量对采收率的影响
CH4-CO2水合物替代开采方法备受关注,但采收率低阻碍了其应用,且不同研究对CH4-CO2替代极限的报道差异较大。本研究通过在具有明确含水沉积物的一维高压反应器中进行一系列CH4-CO2置换实验,引入临界置换厚度概念,量化CH4-CO2水合物置换开采极限。通过实时水合物组成分析,计算CO2驱各阶段CH4-CO2替代极限和临界替代厚度。结果表明:在初始阶段,置换厚度约为2 ~ 4 μm,在后期阶段,置换厚度逐渐减小至0.1 ~ 0.3 μm;此外,本研究系统考察了水合物粒径和流体流速对CH4回收和CO2封存的影响。研究发现,粒径越小、流量越大,采收率越高,CH4回收率由39.1%提高到63.4%。此外,重整后的CH4-CO2水合物膜产生的传质阻力限制了在无额外刺激的情况下,粒径分布在0-250 μm的临界置换厚度不超过7 μm。研究结果对影响CH4采收率的因素有了更清晰的认识,并为优化替代方法以提高效率提供了见解。这些结果有助于制定更有效的水合物储层CH4-CO2替代开发策略。
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来源期刊
Energy & Fuels
Energy & Fuels 工程技术-工程:化工
CiteScore
9.20
自引率
13.20%
发文量
1101
审稿时长
2.1 months
期刊介绍: Energy & Fuels publishes reports of research in the technical area defined by the intersection of the disciplines of chemistry and chemical engineering and the application domain of non-nuclear energy and fuels. This includes research directed at the formation of, exploration for, and production of fossil fuels and biomass; the properties and structure or molecular composition of both raw fuels and refined products; the chemistry involved in the processing and utilization of fuels; fuel cells and their applications; and the analytical and instrumental techniques used in investigations of the foregoing areas.
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