面向生物甲烷分离的不同金属配位金属-有机骨架材料的分子设计

doi:10.3969/j.issn.0438-1157.2014.05.024

化工学报

面向生物甲烷分离的不同金属配位金属-有机骨架材料的分子设计

乔智威¹, 杨仁党², 王海辉¹, 周健¹

1 华南理工大学化学与化工学院, 绿色化学产品技术广东省重点实验室, 广东广州 510640;
2 华南理工大学轻工与食品学院, 制浆造纸工程国家重点实验室, 广东广州 510640

收稿日期:2013-12-31 修回日期:2014-01-14 出版日期:2014-05-05 发布日期:2014-05-05
通讯作者: 周健
基金资助:
国家重点基础研究发展计划项目（2013CB733500）；中央高校基本科研业务费专项资金（2014ZB0012）。

Molecular design of metal-organic frameworks with different metal ligands for bio-methane separation

QIAO Zhiwei¹, YANG Rendang², WANG Haihui¹, ZHOU Jian¹

1 Guangdong Provincial Key Laboratory for Green Chemical Product Technology, School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, Guangdong, China;
2 State Key Laboratory of Pulp and Paper, School of Light Industry and Food Sciences, South China University of Technology, Guangzhou 510640, Guangdong, China

Received:2013-12-31 Revised:2014-01-14 Online:2014-05-05 Published:2014-05-05
Supported by:
supported by the National Basic Research Program of China (2013CB733500) and the Fundamental Research Funds for the Central Universities (2014ZB0012).

摘要/Abstract

摘要： 采用巨正则Monte Carlo法（GCMC），对CH₄ /CO₂混合气体体系基于金属-有机骨架材料（MOFs）的吸附分离进行了模拟研究。吸附分离材料涉及3个系列（M-MOF-74、M-MIL-53和[M（atz）（bdc）_0.5]）（M=Mg，Co，Ni，Zn，Al，Cr）不同金属配位的8种MOF材料。研究表明，Mg-MOF-74的CO₂吸附性能在高压下优于其他材料；在低压时，拥有大量氨基官能团的[Zn（atz）（bdc）_0.5]和[Co（atz）（bdc）_0.5]材料有更高效的CO₂分离性能。通过径向分布函数和CO₂吸附构型快照重叠图进一步分析发现，各个系列材料不同金属配位对CO₂吸附构型的影响造成了材料吸附分离性能有较大的不同。研究结果能够为实验上设计和开发新型高效CO₂和CH₄吸附分离MOFs材料提供启发。

关键词: 分子模拟, 金属-有机骨架材料, 吸附, 分离, 生物甲烷

Abstract: The adsorption and separation capabilities of metal-organic frameworks (MOFs) for CO₂ and CH₄ gas mixtures were studied by grand canonical Monte Carlo (GCMC) simulations. Three sub-families (M-MOF-74, M-MIL-53 and [M(atz)(bdc)_0.5]) (M=Mg, Co, Ni, Zn, Al, Cr) MOFs with different metal ligands were investigated. Simulation results showed that the CO₂ adsorption capability of Mg-MOF-74 exceeded the others at high pressures; both amine functionalized [Zn(atz)(bdc)_0.5] and [Co(atz)(bdc)_0.5] MOFs had superior CO₂ separation performance at low pressures. The radial distribution functions and the overlapping snapshots of CO₂ adsorption showed that in each sub-family of MOFs, different metal ligands affected their CO₂ adsorption configuration and resulted in their different adsorption and separation capabilities. This work could provide some guidance for the design and development of new high performance MOFs for CO₂ and CH₄ separation.

Key words: molecular simulation, metal-organic framework, adsorption, separation, bio-methanePPT

中图分类号:

TQ013
O647.3

乔智威, 杨仁党, 王海辉, 周健. 面向生物甲烷分离的不同金属配位金属-有机骨架材料的分子设计[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.024.

QIAO Zhiwei, YANG Rendang, WANG Haihui, ZHOU Jian. Molecular design of metal-organic frameworks with different metal ligands for bio-methane separation[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.024.

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面向生物甲烷分离的不同金属配位金属-有机骨架材料的分子设计

Molecular design of metal-organic frameworks with different metal ligands for bio-methane separation

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