高稳定铪金属-有机骨架材料的合成及二氧化碳捕获性能

doi:10.3969/j.issn.0438-1157.2014.05.021

化工学报

高稳定铪金属-有机骨架材料的合成及二氧化碳捕获性能

李亮莎¹, 王可可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:2014-01-20 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）。

Synthesis of exceptional stable Hf-based metal-organic frameworks：characterization, stability and CO₂ adsorption performance

LI Liangsha¹, WANG Keke¹, 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:2014-01-20 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： 采用高温高浓度的溶剂热方法，合成了具有高结晶度的一种金属-有机骨架（metal-organic framework，MOF）材料UiO-66（Hf），并发现该材料在沸水、酸碱等苛刻条件下具有非常好的化学稳定性。为了提高其对气体的吸附分离性能，进一步采用具有不同官能团的有机配体——氨基对苯二甲酸（H₂BDC-NH₂）、硝基对苯二甲酸（H₂BDC-NO₂）、溴对苯二甲酸（H₂BDC-Br），设计合成了孔道表面具有不同化学性质的三种新型铪MOF材料，且这些材料与UiO-66（Hf）具有相同的拓扑结构。同时，气体吸附实验结果表明，极性基团的引入，尤其是氨基的引入，能极大提高材料对CO₂/N₂以及CO₂/CH₄体系的分离性能。这为以后应用于化工体系分离的新型多孔材料合成提供了理论指导。

关键词: 金属-有机骨架材料, 铪, 稳定性, 功能化修饰, 吸附, 二氧化碳捕集

Abstract: By a high temperature and high concentration method, a metal-organic framework (MOF), UiO-66(Hf), was synthesized in a high degree of crystalline, and its thermal and chemical stability were examined in various environments including boiling water as well as strong acidic and basic solutions. In order to enhance its performance for gas separation, three new Hf-based MOFs with the pore surfaces having different chemical properties were further synthesized, using three organic ligands with different functional groups, aminoterephthalic acid (H₂BDC-NH₂), nitroterephthalic acid (H₂BDC-NO₂) and bromoterephthalic acid (H₂BDC-Br). The synthesized materials were characterized using PXRD, TG, and N₂ adsorption measurements, and the separation performance of these MOFs towards CO₂/N₂ and CO₂/CH₄ systems were also explored on the basis of adsorption isotherms for CO₂, N₂ and CH₄. It is shown that the material presents exceptionally high stability under these conditions. The materials modified with functional groups have the same topology to the parent UiO-66(Hf). In addition, the introduction of polar functional groups, especially the amino (-NH₂) group, can greatly improve the separation performance of materials for the removal of CO₂ from these two systems. The knowledge obtained may provide theoretical guidance for the synthesis of novel nanoporous materials towards practical applications in the separation of chemical systems of interest.

Key words: metal-organic frameworks, hafnium, stability, functional modification, adsorption, CO₂ capture

中图分类号:

TQ028.1

李亮莎, 王可可, 黄宏亮, 阳庆元, 张轶, 王少华, 吴平易, 兰玲, 刘大欢, 仲崇立. 高稳定铪金属-有机骨架材料的合成及二氧化碳捕获性能[J]. 化工学报, DOI: 10.3969/j.issn.0438-1157.2014.05.021.

LI Liangsha, WANG Keke, HUANG Hongliang, YANG Qingyuan, ZHANG Yi, WANG Shaohua, WU Pingyi, LAN Ling, LIU Dahuan, ZHONG Chongli. Synthesis of exceptional stable Hf-based metal-organic frameworks：characterization, stability and CO₂ adsorption performance[J]. CIESC Journal, DOI: 10.3969/j.issn.0438-1157.2014.05.021.

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高稳定铪金属-有机骨架材料的合成及二氧化碳捕获性能

Synthesis of exceptional stable Hf-based metal-organic frameworks：characterization, stability and CO₂ adsorption performance

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高稳定铪金属-有机骨架材料的合成及二氧化碳捕获性能

Synthesis of exceptional stable Hf-based metal-organic frameworks：characterization, stability and CO2 adsorption performance

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Synthesis of exceptional stable Hf-based metal-organic frameworks：characterization, stability and CO₂ adsorption performance