MOF-5上甲醇、乙醛和丙酮吸附机理的密度泛函理论研究

doi:10.3969/j.issn.0438-1157.2013.08.027

化工学报 ›› 2013, Vol. 64 ›› Issue (8): 2891-2897.DOI: 10.3969/j.issn.0438-1157.2013.08.027

MOF-5上甲醇、乙醛和丙酮吸附机理的密度泛函理论研究

吴永标, 刘德飞, 吴颖, 奚红霞

华南理工大学化学与化工学院, 广东广州 510641

收稿日期:2012-12-08 修回日期:2013-04-11 出版日期:2013-08-05 发布日期:2013-08-05
通讯作者: 奚红霞
作者简介:吴永标(1987- ),男,硕士研究生。
基金资助:
国家自然科学基金项目(20936001,21176084);广东省自然科学基金团队项目(S2011 030001366);国家高技术研究发展计划项目(2013AA065005)。

Adsorption mechanism of methanol,acetaldehyde and acetone on MOF-5 with density functional theory

WU Yongbiao, LIU Defei, WU Ying, XI Hongxia

College of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510641, Guangdong, China

Received:2012-12-08 Revised:2013-04-11 Online:2013-08-05 Published:2013-08-05
Supported by:
supported by the National Natural Science Foundation of China(20936001,21176084),the Natural Science Foundation of Guangdong Province (S2011 030001366)and the High-tech Research and Development Program of China(2013AA065005).

摘要/Abstract

摘要： 采用密度泛函理论对甲醇、乙醛和丙酮3种VOCs气体在MOF-5中的吸附机理进行了系统的理论研究,结果表明:3种气体分子在MOF-5中的吸附位置主要有4种,分别为大胞腔中的金属簇Zn₄O、苯环BDC位置和小胞腔中的金属簇Zn₄O、苯环BDC位置,其中在金属簇Zn₄O位置吸附能皆为最大。对比甲醇、乙醛和丙酮的结构特性和在MOF-5中的吸附能,结果预测:在有机配体苯环中引入吸电子基团有利于甲醇这类含有羟基基团的有机分子在MOF-5上的吸附,而引入给电子基团或更多含氧官能团,则有利于增强乙醛和丙酮这类含有羰基基团的有机分子与MOF-5的吸附作用。

关键词: 金属-有机骨架材料, 密度泛函理论, 甲醇, 乙醛, 丙酮, 吸附, VOCs

Abstract: The density functional theory is used to study the adsorption mechanism of volatile organic compounds(VOCs)on MOF-5,including methanol,acetaldehyde and acetone.The results show that these VOC molecules are adsorbed in four adsorption sites of MOF-5 and Zn₄O clusters are the most favorable adsorption sites.Comparison and analysis on the structural properties and adsorption energy of VOC molecules adsorbed on MOF-5 indicate that the functional groups play the key role.The introduction of electron-withdrawing functional groups to the aromatic rings of MOF-5 increases the interaction between organic molecules containing hydroxyl(such as methanol)and MOF-5 frameworks.The introduction of electron-donating functional groups and oxygen containing groups to the organic linkers increases the adsorption capacity of organic molecules containing carbonyl(such as acetaldehyde and acetone)in MOF-5.

Key words: metal-organic framework, density functional theory, methanol, acetaldehyde, acetone, adsorption, volatile organic compounds

中图分类号:

TQ021.9

吴永标, 刘德飞, 吴颖, 奚红霞. MOF-5上甲醇、乙醛和丙酮吸附机理的密度泛函理论研究[J]. 化工学报, 2013, 64(8): 2891-2897.

WU Yongbiao, LIU Defei, WU Ying, XI Hongxia. Adsorption mechanism of methanol,acetaldehyde and acetone on MOF-5 with density functional theory[J]. CIESC Journal, 2013, 64(8): 2891-2897.

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MOF-5上甲醇、乙醛和丙酮吸附机理的密度泛函理论研究

Adsorption mechanism of methanol,acetaldehyde and acetone on MOF-5 with density functional theory

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