文献类型：期刊文献

中文题名：氨基修饰微孔/介孔复合材料AM-5A-MCM-41对CO_(2)吸附分离的分子模拟

英文题名：Molecular simulation of CO_(2)adsorption on amine modified micro/mesoporous composite of AM-5A-MCM-41

作者：周建海[1];赵会玲[1];胡军[1];刘洪来[1];胡英[1]

机构：[1]华东理工大学化学工程联合国家重点实验室,化学与分子工程学院,上海200237

年份：2014

卷号：65

期号：5

起止页码：1680

中文期刊名：化工学报

外文期刊名：CIESC Journal

收录：CSTPCD;;EI(收录号：20142317795632);Scopus;北大核心:【北大核心2011】；CSCD:【CSCD2013_2014】；

基金：国家重点基础研究发展计划项目(2013CB733501);国家自然科学基金项目(21176066,91334203);中央高校基本科研业务费专项资金

语种：中文

中文关键词：分子模拟;二氧化碳吸附;氨基修饰;微孔;介孔材料;选择性

外文关键词：molecular simulation;CO_(2)adsorption;amine modification;micro/mesoporous;selectivity

摘要：构建了氨基修饰微孔/介孔复合材料AM-5A-MCM-41的全原子模型,采用巨正则Monte Carlo(GCMC)方法研究了它的CO_(2)吸附分离性能,采用加权混合规则来描述氨基和CO_(2)分子的弱化学作用。模拟结果表明,CO_(2)分子优先吸附在复合材料介孔表面的氨基附近,CO_(2)纯气体的吸附量和吸附热有了显著提高,而N_(2)的吸附量和吸附热则基本不受影响。对于CO_(2)和N_(2)的混合气分离,由于复合材料对CO_(2)的弱化学吸附作用,显著提高了CO_(2)吸附量和吸附选择性,在573 K和100 kPa时CO_(2)/N_(2)的选择性达到了87.0。通过分子模拟研究可以从微观角度了解CO_(2)在氨基修饰的微孔/介孔复合材料中的吸附分离的细节和机理,为实验设计和合成高效CO_(2)吸附剂提供指导。
Combining the advantages of high selectivity of amine groups,high capacity of microporous zeolite,and high transportation of mesoporous structures,amine modified micro/mesoporous composites may exhibit promising CO_(2)adsorption capability.In this study,a full-atomic mimetic amine modified micro/mesoporous composite of AM-5A-MCM-41 was constructed.CO_(2)adsorption and separation performance on AM-5A-MCM-41 composite were investigated by the grand canonical Monte Carlo(GCMC),in which a specific combining rule was used to describe the weak chemical interaction between CO_(2)molecule and amine group.The simulation results demonstrate that CO_(2)is preferentially adsorbed around amine groups,which is grafted at the surface of mesoporous channels;and the CO_(2)adsorption capacity and its isosteric heat are greatly improved on AM-5A-MCM-41,whereas those of N_(2)are almost kept unchanged.For the separation of mixed gas of CO_(2)and N_(2),both CO_(2)adsorption capacity and CO_(2)/N_(2)selectivity are greatly improved,due to the enhanced interaction between CO_(2)molecules and amine groups.The chemisorption plays a significant role in the capture of CO_(2)at low pressures and high temperature,giving a selectivity as high as 87.0 at 573 K and 100 kPa.The overall results show that molecular simulations serve as a powerful implement to assist the design and development of new promising CO_(2)adsorbents,highlighting the importance of this approach.