铪金属-有机骨架材料的孔尺寸调控及其吸附性能

doi:10.3969/j.issn.0438-1157.2014.05.020

化工学报

铪金属-有机骨架材料的孔尺寸调控及其吸附性能

王可可¹, 李亮莎¹, 黄宏亮¹, 阳庆元¹, 张轶², 王少华², 吴平易³, 兰玲³, 刘大欢¹, 仲崇立¹

1 北京化工大学有机无机复合材料国家重点实验室, 北京 100029;
2 中国昆仑工程公司辽宁分公司, 辽宁辽阳 111003;
3 中国石油化工研究院, 北京 100195

收稿日期:2013-12-26 修回日期:2014-01-27 出版日期:2014-05-05 发布日期:2014-05-05
通讯作者: 王少华,兰玲
基金资助:
国家重点基础研究发展计划项目（2013CB733503）；国家自然科学基金项目（21136001，21322603）；教育部新世纪优秀人才项目（NCET-12-0755）。

Control of pore size in Hf-based metal-organic frameworks and exploration of their adsorption properties

WANG Keke¹, LI Liangsha¹, HUANG Hongliang¹, YANG Qingyuan¹, ZHANG Yi², WANG Shaohua², WU Pingyi³, LAN Ling³, LIU Dahuan¹, ZHONG Chongli¹

1 State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology, Beijing 100029, China;
2 China Kunlun Contracting Engineering Corporation Liaoning Company, Liaoyang 111003, Liaoning, China;
3 Petrochemical Research Institute, PetroChina, Beijing 100195, China

Received:2013-12-26 Revised:2014-01-27 Online:2014-05-05 Published:2014-05-05
Supported by:
supported by the National Basic Research Program of China (2013CB733503), the National Natural Science Foundation of China (21136001,21322603) and the Program for New Century Excellent Talents in University (NCET-12-0755).

摘要/Abstract

摘要： 利用三种不同长度的有机配体——反丁烯二酸（H₂FUM）、对苯二甲酸（H₂BDC）和联苯二甲酸（H₂BPDC），合成了一系列具有不同孔尺寸的新型铪（Hf）金属-有机骨架（MOF）材料（Hf-FUM、Hf-BDC和Hf-BPDC），并考察了CO₂、N₂和CH₄三种气体在这些材料中吸附分离行为。研究结果表明，这三种材料具有和UiO-66（Zr）相同的拓扑结构，且具有很好的热稳定性。Hf-FUM和Hf-BDC的结构在水中能够保持稳定，而Hf-BPDC在水中会发生降解。同时，具有最小孔尺寸的Hf-FUM材料对CO₂/N₂以及CO₂/CH₄体系具有最好的分离性能。这为以后设计用于CO₂分离的新型纳微结构材料提供了参考依据。

关键词: 金属-有机骨架材料, 铪, 孔尺寸调控, 稳定性, 吸附, 二氧化碳捕集

Abstract: By incorporating three organic carboxylic acids with different lengths, fumaric (FUM), 1,4-benzene- dicarboxylate (BDC) and 4,4'-biphenyl-dicarboxylate (BPDC) acids, three novel Hf-based metal-organic frameworks (MOFs), Hf-FUM, Hf-BDC and Hf-BPDC, were synthesized using a solvothermal method combined with conventional electric heating. These MOFs were characterized by various experimental techniques including PXRD, N₂ adsorption, TG and SEM. Moreover, the stabilities of these materials were examined by soaking the samples in water. The PXRD results reveal that all of these Hf-based MOFs have a topology similar to that of UiO-66(Zr), and Hf-FUM is stable up to 400 ℃ while Hf-BDC and Hf-BPDC remain stable at 500 ℃. The structures of Hf-FUM and Hf-BDC are water-resistant, while that of Hf-BPDC will decompose after water treatment. On the basis of the adsorption isotherms of CO₂, N₂ and CH₄ at 298 K, the effect of pore size on the separation of CO₂/N₂and CO₂/CH₄ systems were also investigated. It is found that Hf-FUM with the smallest pore size possesses the highest adsorption selectivity for CO₂ over N₂and CH₄. This is the first study on the performance of Hf-based MOFs for gas separation, and the knowledge obtained in this work provides a foundation for the design of new nanoporous materials towards CO₂ capture from various gas mixtures.

Key words: metal-organic frameworks, hafnium, pore-size regulation, stability, adsorption, CO₂ capture

中图分类号:

TQ028.1

王可可, 李亮莎, 黄宏亮, 阳庆元, 张轶, 王少华, 吴平易, 兰玲, 刘大欢, 仲崇立. 铪金属-有机骨架材料的孔尺寸调控及其吸附性能[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.020.

WANG Keke, LI Liangsha, HUANG Hongliang, YANG Qingyuan, ZHANG Yi, WANG Shaohua, WU Pingyi, LAN Ling, LIU Dahuan, ZHONG Chongli. Control of pore size in Hf-based metal-organic frameworks and exploration of their adsorption properties[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.020.

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铪金属-有机骨架材料的孔尺寸调控及其吸附性能

Control of pore size in Hf-based metal-organic frameworks and exploration of their adsorption properties

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