TETA/AMP复合水基CO_2吸收液研究Research on aqueous TETA/AMP solution for CO_2 capture
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.;
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
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
参考文献(References):
- [1]郭晖.有机胺/醇醚非水混合体系吸收CO2过程特性研究[D].石家庄:河北科技大学,2019.GUO Hui.Research on CO2absorption process using originic amine/glycerol ether non-aqueous blends[D].Shijiazhuang:Hebei University of Science and Technology,2019.
- [2]陆诗建,高丽娟,李欣泽,等.有机胺吸收CO2反应热实验[J].中国石油大学学报(自然科学版),2018,42(4):164-173.LU Shijian,GAO Lijuan,LI Xinze,et al.Experimental study on reaction heat of carbon dioxide absorption with organic amines[J].Journal of China University of Petroleum (Edition of Natural Science),2018,42(4):164-173.
- [3]朱立宾,陆诗建,张慧.MEA-PEHA复配溶液吸收二氧化碳实验研究[J].山东化工,2018,47(14):1-4.ZHU Libin,LU Shijian,ZHANG Hui.Experimentalstudy on carbon dioxide absorption of MEA-PEHA compound solution[J].Shandong Chemical Industry,2018,42(04):1-4.
- [4]杨钧晗.醇胺水溶液吸收CO2过程的腐蚀特性研究[D].北京:华北电力大学,2018.YANG Junhan.Study on corrsion characteristics of CO2absorption of amine aqueous solution[D].Beijing:North China Electric Power University,2018.
- [5]林海周,裴爱国,方梦祥.燃煤电厂烟气二氧化碳胺法捕集工艺改进研究进展[J].化工进展,2018,37(12):4874-4886.LIN Haizhou,PEI Aiguo,FANG Mengxiang.Progress of research on process modifications for amine solvent-based post combustion CO2capture from coal-fired power plant[J].Chemical Industry and Engineering Progress,2018,37(12):4874-4886.
- [6]REN H,LIAN S,WANG X,et al.Exploiting the hydrophilic role of natural deep eutectic solvents for greening CO2capture[J].Journal of Cleaner Production,2018,193:802-810.
- [7]赵毅,王永斌,王添颢.有机胺法吸收二氧化碳的研究进展[J].再生资源与循环经济,2020,13(7):26-29.ZHAO Yi,WANG Yongbin,WANG Tianhao.Research progress on the absorption of carbon dioxide by organic amine method[J].Recyclable Resources and Circular Economy,2020,13(7):26-29.
- [8]陆诗建,耿春香,赵东亚,等.基于AEEA的二元复合胺试剂吸收CO2降解性能研究[J].高校化学工程学报,2017,31(6):1442-1451.LU Shijian,GENG Chunxiang,ZHAO Dongya,et al.Study on the degradation of AEEA based mixed amines in CO2absorption[J].Journal of Chemical Engineering of Chinese Universities,2017,31(6):1442-1451.
- [9]康顺吉,沈喜洲,向丽.MDEA及其复合胺溶液对CO2吸收与解吸研究进展[J].天然气化工(C1化学与化工),2019,44(4):124-130.KANG Shunji,SHEN Xizhou,XIANG Li,Research progresses in carbon dioxide absorption and desorption from MDEA and its activated amine[J].Natural Gas Chemical Industry,2019,44 (4):124-130.
- [10]陆诗建,李欣泽,赵东亚,等.TETA-MDEA复合溶液吸收与解吸CO2实验研究[J].山东化工,2019,48(7):192-198.LU Shijian,LI Xinze,ZHAO Dongya,et al.Experimental analysis on absorption and desorption of CO2by TETA-MDEA complex Solution[J].Shandong Chemical Industry,2019,48 (7):192-198.
- [11]朱立宾,陆诗建.DETA-PZ复合溶液吸收与解吸CO2实验研究[J].山东化工,2019,48(16):29-32,35.ZHU Libin,LU Shijian.Experimentalstudy on absorption and desorption of CO2by DETA-PZ complex solution[J].Shandong Chemical Industry,2019,48(16):29-32,35.
- [12]程毅.基于BZA-DEEA/DMEA/1DMA2P/AMP二元混合胺的CO2捕获性能研究[D].湘潭:湘潭大学,2019.CHENG Yi.CO2absorption and desorption performance of BZA-DEEA/DMEA/1DMA2P/AMP binary blended amines[D].Xiangtan:Xiangtan University,2019.
- [13]王中红,陆诗建.DETA-MDEA复合溶液吸收与解吸CO2实验研究[J].当代化工,2019,48(5):1004-1008,1012WANG Zhonghong,LU Shijian.Experimentalanalysis on absorption and desorption of CO2by DETA-MDEA complex solution[J].Contemporary Chemical Industry,2019,48 (5):1004-1008,1012.
- [14]连少翰.氨基酸类低共熔溶剂的合成及捕集CO2性能研究[D].石家庄:河北科技大学,2019.LIAN Shaohan.Synthesis of amino acids-based deep eutectic solvent and its performance for CO2capture[D].Shijiazhuang:Hebei university of Science and Technology,2019.
- [15]SHAMAIR Z,HABIB N,GILANI M A,et al.Theoretical and experimental investigation of CO2separation from CH4and N2through supported ionic liquid membranes[J].Applied Energy,2020,268:115016.
文章评论(Comment):
|
||||||||||||||||||
|
- 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
- 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.
- 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.