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题名	二氧化碳的电石渣捕集与深部煤层封存
作者	张登峰
学位类别	博士
答辩日期	2011-11-29
授予单位	中国科学院研究生院
导师	林伟刚
关键词	二氧化碳 电石渣 捕集 煤 封存
其他题名	Carbon Dioxide Capture by Carbide Slag and Sequestration in Deep Coal Seams
学位专业	环境工程
中文摘要	温室气体排放导致全球变暖问题对地球生态系统和人类社会构成主要威胁。二氧化碳（CO2）是最重要的一类人为温室气体。新兴的CO2捕集与封存（CCS）技术极具缓解气候变化的潜力。为此，本文开展了相关CCS技术的研究。研究包括利用工业废弃物电石渣进行CO2循环捕集和强化煤层气-甲烷（CH4）开采的CO2封存（CO2 Sequestration in Coal Seams with Enhanced Coal-bed Methane (CH4) Recovery，CO2-ECBM）两方面内容。 本文主要研究结论包括： 论文第一部分主要基于煅烧/碳酸化反应循环捕集CO2工艺，研究了电石渣和广泛使用的天然CaO基吸收剂的CO2吸收性能。系统研究了温度、粒径和反应时间等重要参数对循环过程中电石渣的CO2吸收性能和反应动力学的影响。结果表明碳酸化循环捕集CO2过程中，电石渣的性能优于天然CaO基吸收剂。X射线衍射（XRD）分析表明电石渣在煅烧过程中生成钙铝石（Ca12Al14O33），该物质能够减小碳酸化循环过程中电石渣颗粒的烧结程度。过程分析表明在碳酸化循环捕集CO2工艺中，电石渣相对石灰石表现出更为优越的CO2捕集性能。 论文第二部分针对CO2煤层封存进行研究，考察了中国的四种煤阶煤的单组分CH4和CO2的超临界吸附行为。探明了温度和煤阶对吸附容量及有效扩散系数的作用规律。验证了利用Ono-Kondo格子模型描述煤的CH4和CO2吉布斯吸附等温线的有效性。 为了更真实地模拟CO2-ECBM工艺过程，本文通过建立新颖的实验方法和数据处理方法获得了向饱和CH4煤样注入CO2的相关信息。结果证实了CO2-ECBM技术的可行性。建立了CO2注入致使CH4解吸过程的概念模型。对于实施CO2-ECBM技术，建议采取先减压解吸CH4再注入CO2的方法以改善CO2封存效果。 本文还探讨了封存过程中煤和CO2之间的固-气作用关系。结果发现超临界CO2能够将煤基质中溶解的小分子烃类物质萃取出来。这些烃类物质具有向含水层运移的能力，因而需要评估CO2-ECBM技术对生态环境造成的负面影响。 最后建立了煤层封存CO2的方法体系，并以鄂尔多斯盆地为例，初步评价了位于该盆地深部不可采煤层的CO2封存潜力。初步评价结果表明鄂尔多斯盆地最适于CO2封存的两大区块的煤层气资源量和最大CO2封存量分别为2.11×108 m3和0.73×106 t。
英文摘要	Global warming caused by greenhouse gas (GHG) emissions is recognized as the major threat to the terrestrial ecosystem and human society. Carbon dioxide (CO2) is one of the most important anthropogenic greenhouse gases. CO2 Capture & Sequestration (CCS) is emerging as a promising mitigation option of climate change. This work is performed in related to part of CCS technologies, which consists of two parts: one is to study the cyclic capture of CO2 by using an industrial waste, carbide slag and the other is to investigate the CO2 sequestration in coal seams with enhanced coal-bed methane (CH4) recovery (CO2-ECBM). The main conclusions from this work are summarized as follows: In the first part of the thesis, the performance of cyclic CO2 capture by carbide slag is studied in contrast to widely used natural CaO based sorbent in CO2 capture by calcination/carbonation looping. The influence of important parameters, such as temperature, particle size and reaction time on the CO2 capture capacity and kinetics of carbide slag in looping cycles were systematically investigated. The results indicate that the CO2 capture in carbonate looping process is somewhat better than that of natural CaO based sorbent. X ray diffraction (XRD) analysis shows that mayenite (Ca12Al14O33) is formed during the calcination, which reduces the tendency of sintering of carbide slag particles in the carbonate looping process. Process analysis indicates that the CO2 capture performance of carbide slag in the carbonate looping process is better than that of limestone. In the second part of the thesis, supercritical pure CH4 and CO2 adsorption behaviors of four different ranks of coal in China have been studied with consideration of CO2 sequestration in coal seams. Temperature and coal rank dependence of adsorption capacity and effective diffusivity is established and applicability of Ono-Kondo lattice model for simulation of Gibbs adsorption isotherms of CH4 and CO2 on coal is confirmed. In order to relevantly simulate CO2-ECBM process, novel experimental method and data processing method are established to obtain the information of the displacement behavior of CH4 adsorbed on coals by CO2 injection. The results demonstrate that CO2-ECBM process is feasible. A conceptual model is proposed to elucidate the process of CH4 desorption due to CO2 injection. It is indicated that for implement of CO2-ECBM, it would be better to inject CO2 after partial desorption of CH4 by depressurizing in order to improve CO2 sequestration. Interaction between coal and CO2 during sequestration process is discussed in the thesis, as well. It is found that low molecular weight hydrocarbons dissolved in coal matrix can be extracted by supercritical CO2. The extracted hydrocarbons are able to move to aquifer. Thus, negative effect of CO2-ECBM on the ecosystem should be considered. Finally, methodology of CO2 sequestration in coal seams is established and a preliminary evaluation of the CO2 sequestration potential in unminable coal seams of Erdos basin is carried out. The preliminary evaluation results show that the coalbed methane recovery and the maximum CO2 sequestration potential of the two blocks suitable to sequestrate CO2 are 2.11×108 m3 and 0.73×106 t, respectively.
语种	中文
公开日期	2013-09-24
内容类型	学位论文
源URL	[http://ir.ipe.ac.cn/handle/122111/1752]
专题	过程工程研究所_研究所（批量导入）
推荐引用方式 GB/T 7714	张登峰. 二氧化碳的电石渣捕集与深部煤层封存[D]. 中国科学院研究生院. 2011.

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