高等学校化学学报 ›› 2015, Vol. 36 ›› Issue (2): 316-324.doi: 10.7503/cjcu20140802

• 物理化学 • 上一篇    下一篇

杂质对金属-有机骨架材料分离烟道气性能 影响的分子模拟研究

王佳晨1, 童敏曼1, 单超2, 肖刚3, 刘大欢1, 阳庆元1(), 仲崇立1   

  1. 1. 北京化工大学化学工程学院, 先进纳微结构材料实验室, 北京100029
    2. 北京石油化工工程有限公司, 北京100107
    3. 中国石油吉林石化公司, 吉林132022
  • 收稿日期:2014-09-04 出版日期:2015-02-10 发布日期:2015-01-20
  • 作者简介:联系人简介: 阳庆元, 男, 博士, 教授, 主要从事新型多孔杂化材料的分子设计与合成研究. E-mail: qyyang@mail.buct.edu.cn
  • 基金资助:
    国家“九七三”计划项目(批准号: 2013CB733503)和国家自然科学基金(批准号: 21136001, 21322603)资助

Molecular Simulation of Effects of Impurities on Flue Gas Separation in Metal-Organic Frameworks

WANG Jiachen1, TONG Minman1, SHAN Chao2, XIAO Gang3,*, LIU Dahuan1, YANG Qingyuan1,*(), ZHONG Chongli1   

  1. 1. Laboratory of Advanced Nano/Micro Materials, Department of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
    2. Beijing Petrochemical Engineering Ltd. Co., Beijing 100107, China
    3. PetroChina Jilin Petrochemical Company, Jilin 132022, China
  • Received:2014-09-04 Online:2015-02-10 Published:2015-01-20
  • Contact: XIAO Gang,YANG Qingyuan E-mail:qyyang@mail.buct.edu.cn
  • Supported by:
    Supported by the National Key Basic Research Program of China(No.2013CB733503) and the National Natural Science Foundation of China(Nos.21136001, 21322603)

摘要:

采用分子模拟方法系统研究了杂质(水、 O2和SO2)对5种金属-有机骨架材料(ZIF-8, NOTT-300, UiO-66(Zr), UiO-66-NH2和UiO-66-2COOH)的烟道气分离性能的影响, 并探讨了其微观机理. 结果表明, O2和SO2对这些材料的CO2/N2分离选择性影响不大; 水对ZIF-8和UiO-66(Zr)的分离选择性影响不大, 而对NOTT-300和UiO-66-NH2的分离选择性具有提升作用; UiO-66-2COOH对CO2的选择性有所降低. 在干燥的环境下, UiO-66-2COOH的选择性最高, 而在湿润的环境下, UiO-66-NH2的选择性最高. 为捕获CO2的新型材料设计提供理论指导.

关键词: 气体分离, 分子模拟, 烟道气, 选择性, 金属-有机骨架材料, 二氧化碳

Abstract:

The resulting excessive release of CO2 into the atmosphere has triggered great change in the climate which calls for urgent cuts in the emission of such primary anthropogenic greenhouse gas. In this regard, one significant challenging separation problem nowadays is associated with the selective CO2 capture from the flue gas emitted by large stationary point sources such as power plants. In this work, a computational study was performed to systematically investigate the effects of impurities(H2O, O2 and SO2) on the performance of five metal-organic frameworks(MOFs)[ZIF-8, NOTT-300, UiO-66(Zr), UiO-66-NH2 and UiO-66-2COOH] for the separation of flue gas under the industrial conditions, and the underlying microscopic mechanisms were also explored. The accuracy of the force fields adopted was verified by comparing the simulated adsorption isotherms with those experimental data. Then, molecular simulations were performed to investigate the separation behavior of flue gas consisting of CO2, N2, O2, SO2 and H2O in these materials. The results show that O2 and SO2 have a negligible influence on the CO2/N2 selectivity of the MOFs. Water has a negligible effect on the separation performance of ZIF-8 and UiO-66(Zr) and can enhance the CO2/N2 selectivity of NOTT-300 and UiO-66-NH2. However, the separation ability of UiO-66-2COOH is weakened in the presence of water. The current study demonstrates that the UiO-66-2COOH can be a promising candidate for selective CO2 separation from dried flue gas, while UiO-66-NH2 can be a good candidate for the separation of moist flue gas. The information obtained in current study could provide a theoretical guidance for the design of novel CO2 capture materials.

Key words: Gas separation, Molecular simulation, Flue gas, Selectivity, Metal-organic framework, CO2

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