孙路长;连少翰;王凯亮;王争荣;张士明;韩文荃;宋春风;
SUN Luchang;LIAN Shaohan;WANG Kailiang;WANG Zhengrong;ZHANG Shiming;HAN Wenquan;SONG Chunfeng;China Huadian Engineering Co.,Ltd.;School of Environmental Science and Technology,Tianjin University;Jiangsu Huadian Jurong Power Generation Co.,Ltd.;

• 1:中国华电科工集团有限公司
• 2:天津大学环境科学与工程学院
• 3:江苏华电句容发电有限公司

摘要(Abstract)：

化学吸收法吸收CO_2作为CCUS过程的主要技术之一,已经广泛应用于混合气源中CO_2的捕集与纯化。传统的单一MEA水溶液作为吸收剂吸收CO_2过程中存在解吸能耗高、腐蚀性强和易降解等缺点。因此,开发新一代混合胺吸收液成为当前研究的重点。以空间位阻胺2-氨基-2-甲基-1-丙醇(AMP)为基础,合成了一系列TETA/AMP复合水基吸收液用于烟气中CO_2捕集。通过对不同配比的吸收液进行吸收-解吸性能对比测试,综合考察吸收量、吸收速率、再生速率等因素,优选出最佳配比。结果表明,质量比为1∶1的TETA/AMP复合吸收液具有最佳的吸收与解吸表现,饱和吸收量相比纯AMP提升近1倍,再生速率最高可达0.03 g/min。在复合吸收液吸收CO_2过程中,具有较快吸收速率的空间位阻胺AMP能快速捕集CO_2分子,并将其活化,之后传递给具有多反应位点的烯基胺TETA进行储存。而在解吸过程中,由于AMP的空间位阻效应,与CO_2分子间的连接更易断开,从而提升了再生速率。同时采用量子化学计算方式对AMP、TETA单体以及复配单元进行模拟计算,从而对复配体系的形成过程进行推导。发现分子表面静电势分布与形成复配体系的单体间的比例关系,分析了不同官能团在复配体系形成过程的作用,提出了羟基基团在复配体系形成中的必要性。
As one of the main technologies in CCUs process,chemical absorption technologies have been widely used in CO_2 capture and purification process. However,traditional industrial MEA solution as absorbent has many disadvantages,such as high energy consumption,strong corrosion and degeneration. Therefore,the development of a new generation of composite amine absorbent has become the focus of current research. In this study,based on the sterically hindered amine 2-amino-2-methyl-1-propanol( AMP),a series of TETA/AMP composite water-based absorbents were synthesized for CO_2 capture in flue gas. Through the comparison test of absorption-desorption performance of solutions with different ratios,the absorption capacity,absorption rate,regeneration rate and other factors were comprehensively investigated,and finally the best ratio was obtained. And it is found that the TETA/AMP composite absorption liquid with a mass ratio of 1: 1 has the best absorption and desorption performance. Compared with pure AMP,its saturated absorption capacity is nearly doubled,and the maximum regeneration rate can reach 0.03 g/min. In the process of CO_2 absorption by the composite absorbent,the sterically hindered amine AMP with a faster absorption rate can quickly capture and activate CO_2 molecules,and then it is transfered to the alkenylamine TETA with multiple reaction sites for storage. In the desorption process,due to the steric hindrance effect of AMP,the connection with CO_2 molecules is easier to be broken,thereby increasing the regeneration rate. At the same time,quantum chemical calculations are used to simulate the monomers and compound unit,so as to deduce the formation process of the compound system. In this work,the relationship between the distribution of the electrostatic potential on the molecular surface and the monomers forming the compound system was discovered,the role of different functional groups in the formation of the compound system was analyzed,and the necessity of the hydroxyl group in the formation of the compound system was proposed.

关键词(KeyWords)： 二氧化碳;复合胺;三乙烯四胺;2-氨基-2-甲基-1-丙醇;密度泛函理论
CO_2;complex amine;triethylenetetramine;2-amino-2-methyl-1-propanol;density functional theory

Abstract:

Keywords:

基金项目(Foundation): 国家自然科学基金资助项目(21878228);; 国家重点研发计划“政府间国际科技创新合作/港澳台科技创新合作”重点专项资助项目(2017YFE0127200);; 中国华电科工集团有限公司二氧化碳吸收液开发合作项目

作者(Author): 孙路长;连少翰;王凯亮;王争荣;张士明;韩文荃;宋春风;
SUN Luchang;LIAN Shaohan;WANG Kailiang;WANG Zhengrong;ZHANG Shiming;HAN Wenquan;SONG Chunfeng;China Huadian Engineering Co.,Ltd.;School of Environmental Science and Technology,Tianjin University;Jiangsu Huadian Jurong Power Generation Co.,Ltd.;

Email:

DOI: 10.13226/j.issn.1006-6772.EP20092801

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