氨基修饰微孔/介孔复合材料AM-5A-MCM-41对CO2吸附分离的分子模拟

doi:10.3969/j.issn.0438-1157.2014.05.018

化工学报

氨基修饰微孔/介孔复合材料AM-5A-MCM-41对CO₂吸附分离的分子模拟

周建海, 赵会玲, 胡军, 刘洪来, 胡英

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

收稿日期:2013-12-31 修回日期:2014-01-17 出版日期:2014-05-05 发布日期:2014-05-05
通讯作者: 胡军
基金资助:
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。

Molecular simulation of CO₂ adsorption on amine modified micro/mesoporous composite of AM-5A-MCM-41

ZHOU Jianhai, ZHAO Huiling, HU Jun, LIU Honglai, HU Ying

State Key Laboratory of Chemical Engineering, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, China

Received:2013-12-31 Revised:2014-01-17 Online:2014-05-05 Published:2014-05-05
Supported by:
supported by the National Basic Research Program of China (2013CB733501),the National Natural Science Foundation of China (21176066,91334203) and the Fundamental Research Funds for the Central Universities.

摘要/Abstract

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CO₂吸附分离性能，采用加权混合规则来描述氨基和CO₂分子的弱化学作用。模拟结果表明，CO₂分子优先吸附在复合材料介孔表面的氨基附近，CO₂纯气体的吸附量和吸附热有了显著提高，而N₂的吸附量和吸附热则基本不受影响。对于CO₂和N₂的混合气分离，由于复合材料对CO₂的弱化学吸附作用，显著提高了CO₂吸附量和吸附选择性，在573 K和100 kPa时CO₂/N₂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CO₂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CO₂吸附剂提供指导。

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

Abstract: 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 CO₂ adsorption capability. In this study, a full-atomic mimetic amine modified micro/mesoporous composite of AM-5A-MCM-41 was constructed. CO₂ 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 CO₂ molecule and amine group. The simulation results demonstrate that CO₂ is preferentially adsorbed around amine groups, which is grafted at the surface of mesoporous channels; and the CO₂ adsorption capacity and its isosteric heat are greatly improved on AM-5A-MCM-41, whereas those of N₂ are almost kept unchanged. For the separation of mixed gas of CO₂ and N₂, both CO₂ adsorption capacity and CO₂/N₂ selectivity are greatly improved, due to the enhanced interaction between CO₂ molecules and amine groups. The chemisorption plays a significant role in the capture of CO₂ 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 CO₂ adsorbents, highlighting the importance of this approach.

Key words: molecular simulation, CO₂ adsorption, amine modification, micro/mesoporous, selectivity

中图分类号:

TQ028.8

周建海, 赵会玲, 胡军, 刘洪来, 胡英. 氨基修饰微孔/介孔复合材料AM-5A-MCM-41对CO₂吸附分离的分子模拟[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.018.

ZHOU Jianhai, ZHAO Huiling, HU Jun, LIU Honglai, HU Ying. Molecular simulation of CO₂ adsorption on amine modified micro/mesoporous composite of AM-5A-MCM-41[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.018.

参考文献 24

[1]	Goeppert A, Czaun M, Surya Prakash G K, Olah G A. Air as the renewable carbon source of the future: an overview of CO2 capture from the atmosphere[J]. Energy & Environmental Science, 2012, 5 (7): 7833-7853
[2]	Liu Chang (刘畅), Lu Xiaohua (陆小华). Carbon reduction pattern in China:comparison of CCS and biomethane route[J]. CIESC Journal(化工学报), 2013, 64(1): 7-10
[3]	Liu Z, Grande C A, Li P, Yu J, Rodrigues A E. Adsorption and desorption of carbon dioxide and nitrogen on zeolite 5A[J]. Separation Science and Technology, 2011, 46(3): 434-451
[4]	Yang J, Li J, Wang W, Li L, Li J. Adsorption of CO2, CH4, and N2 on 8-, 10-, and 12-membered ring hydrophobic microporous high-silica zeolites: ddr, silicalite-1, and beta[J]. Industrial & Engineering Chemistry Research, 2013, 52(50): 17856-17864
[5]	Harlick P J E, Tezel F H. An experimental adsorbent screening study for CO2 removal from N2[J]. Microporous and Mesoporous Materials, 2004, 76(1/2/3): 71-79
[6]	Sayari A, Belmabkhout Y, Serna-Guerrero R. Flue gas treatment via CO2 adsorption[J]. Chemical Engineering Journal, 2011, 171(3): 760-774
[7]	Sanz R, Calleja G, Arencibia A, Sanz-Pérez E S. Amino functionalized mesostructured SBA-15 silica for CO2 capture: exploring the relation between the adsorption capacity and the distribution of amino groups by TEM[J]. Microporous and Mesoporous Materials, 2012, 158: 309-317
[8]	Yan W, Tang J, Bian Z, Hu J, Liu H. Carbon dioxide capture by amine-impregnated mesocellular-foam-containing template[J]. Industrial & Engineering Chemistry Research, 2012, 51 (9): 3653-3662
[9]	Liu J, Thallapally P K, McGrail B P, Brown D R, Liu J. Progress in adsorption-based CO2 capture by metal-organic frameworks[J]. Chemical Society Reviews, 2012, 41(6): 2308-2322
[10]	Ding S Y, Wang W. Covalent organic frameworks (COFs): from design to applications[J]. Chemical Society Reviews, 2013, 42(2): 548-568
[11]	Yue M B, Sun L B, Zhuang T T, Dong X, Chun Y, Zhu J H. Directly transforming as-synthesized MCM-41 to mesoporous MFI zeolite[J]. Journal of Materials Chemistry, 2008, 18(17): 2044-2050
[12]	Xu H, Guan J, Wu S, Kan Q. Synthesis of beta/MCM-41 composite molecular sieve with high hydrothermal stability in static and stirred condition[J]. Journal of Colloid and Interface Science, 2009, 329(2): 346-350
[13]	Chew T L, Ahmad A L, Bhatia S. Ordered mesoporous silica (OMS) as an adsorbent and membrane for separation of carbon dioxide (CO2) [J]. Advances in Colloid and Interface Science, 2010, 153(1/2): 43-57
[14]	Serna-Guerrero R, Belmabkhout Y, Sayari A. Modeling CO2 adsorption on amine-functionalized mesoporous silica(Ⅰ): A semi-empirical equilibrium model[J]. Chemical Engineering Journal, 2010, 161(1/2): 173-181
[15]	Bhagiyalakshmi M, Yun L, Anuradha R, Jang H. Synthesis of chloropropylamine grafted mesoporous MCM-41, MCM-48 and SBA-15 from rice husk ash: their application to CO2 chemisorption[J]. Journal of Porous Materials, 2010, 17(4): 475-484
[16]	Zhuo S, Huang Y, Hu J, Liu H, Hu Y, Jiang J. Computer simulation for adsorption of CO2, N2 and flue gas in a mimetic MCM-41[J]. The Journal of Physical Chemistry C, 2008, 112(30): 11295-11300
[17]	Jaramillo E, Chandross M. Adsorption of small molecules in LTA zeolites(Ⅰ): NH3, CO2, and H2O in zeolite 4A[J]. Journal of Physical Chemistry B, 2004, 108(52): 20155-20159
[18]	Plant D F, Maurin G, Jobic H, Llewellyn P L. Molecular dynamics simulation of the cation motion upon adsorption of CO2 in faujasite zeolite systems[J]. The Journal of Physical Chemistry B, 2006, 110(29): 14372-14378
[19]	Zhuo S, Huang Y, Hu J, Liu H. Atomistic simulations for adsorption and separation of flue gas in MFI zeolite and MFI/MCM-41 micro/mesoporous composite[J]. Frontiers of Chemical Science and Engineering, 2011, 5(2): 264-273
[20]	Builes S, Vega L F. Understanding CO2 capture in amine- functionalized MCM-41 by molecular simulation[J]. The Journal of Physical Chemistry C, 2012, 116(4): 3017-3024
[21]	Sonwane C G, Li Q. Molecular simulation of RMM: ordered mesoporous SBA-15 type material having microporous ZSM-5 walls[J]. The Journal of Physical Chemistry B, 2005, 109(38): 17993-17997
[22]	Williams J J, Wiersum A D, Seaton N A, Düren T. Effect of surface group functionalization on the CO2/N2 separation properties of MCM-41: a grand-canonical Monte Carlo simulation study[J]. The Journal of Physical Chemistry C, 2010, 114(43): 18538-18547
[23]	Zhou J, Zhao H, Li J, Zhu Y, Hu J, Liu H, Hu Y. CO2 capture on micro/mesoporous composites of (zeolite A)/(MCM-41) with Ca2+ located: computer simulation and experimental studies[J]. Solid State Sciences, 2013, 24: 107-114
[24]	Zhu Y, Zhou J, Hu J, Liu H. The effect of grafted amine group on the adsorption of CO2 in MCM-41: a molecular simulation[J]. Catalysis Today, 2012, 194(1): 53-59

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氨基修饰微孔/介孔复合材料AM-5A-MCM-41对CO₂吸附分离的分子模拟

Molecular simulation of CO₂ adsorption on amine modified micro/mesoporous composite of AM-5A-MCM-41

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