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

doi:10.7503/cjcu20140802

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

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. 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 Gang^3,^*, LIU Dahuan¹, YANG Qingyuan^1,^*(), ZHONG Chongli¹

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/Abstract

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

中图分类号:

O641
O634

TrendMD:

王佳晨, 童敏曼, 单超, 肖刚, 刘大欢, 阳庆元, 仲崇立. 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. 高等学校化学学报, 2015, 36(2): 316.

WANG Jiachen, TONG Minman, SHAN Chao, XIAO Gang, LIU Dahuan, YANG Qingyuan, ZHONG Chongli. Molecular Simulation of Effects of Impurities on Flue Gas Separation in Metal-Organic Frameworks^†. Chem. J. Chinese Universities, 2015, 36(2): 316.

图/表 8

Fig.1 Simulated selectivity of CO2 over N2 in the CO2/N2 binary mixture at 303 K a. ZIF-8; b. NOTT-300; c. UiO-66(Zr); d. UiO-66-NH2; e. UiO-66-2COOH.

Table 1 Isosteric heat of adsorption of CO2, N2, H2O, O2 and SO2 at infinite dilution in ZIF-8,NOTT-300, UiO-66(Zr), UiO-66-NH2 and UiO-66-2COOH at 303 K

Material	$Q st 0$ /(kJ·mol^-1)
Material	CO₂	N₂	H₂O	O₂	SO₂
ZIF-8	-19.04	-11.10	-11.47	-12.98	-25.91
NOTT-300	-24.43	-14.50	-27.90	-14.84	-34.66
UiO-66(Zr)	-25.93	-14.95	-42.15	-16.03	-34.21
UiO-66-NH₂	-28.86	-15.77	-46.05	-16.72	-37.13
UiO-66-2COOH	-37.95	-19.97	-57.80	-19.80	-50.62

Table 1 Isosteric heat of adsorption of CO2, N2, H2O, O2 and SO2 at infinite dilution in ZIF-8,NOTT-300, UiO-66(Zr), UiO-66-NH2 and UiO-66-2COOH at 303 K

Material	$Q st 0$ /(kJ·mol^-1)
Material	CO₂	N₂	H₂O	O₂	SO₂
ZIF-8	-19.04	-11.10	-11.47	-12.98	-25.91
NOTT-300	-24.43	-14.50	-27.90	-14.84	-34.66
UiO-66(Zr)	-25.93	-14.95	-42.15	-16.03	-34.21
UiO-66-NH₂	-28.86	-15.77	-46.05	-16.72	-37.13
UiO-66-2COOH	-37.95	-19.97	-57.80	-19.80	-50.62

Fig.2 Contour plots of the COM probability density distribution of CO2 in their mixture adsorbed in three MOFs at 0.1 MPa (A) UiO-66(Zr); (B) UiO-66-NH2; (C) UiO-66-2COOH. The bulk composition is V(CO2)∶V(N2)=15∶85. The framework of the material is represented by a ball-stick style(Zr, dark cyan; C, gray; O, red; N, blue; H, white).

Fig.3 Simulated selectivity for CO2 over N2(A) and calculated adsorption enthalpies of CO2(B) in the CO2/N2/H2O mixture at 303 K and 0.1 MPa as a function of the relative humidity a. ZIF-8; b. NOTT-300; c. UiO-66(Zr); d. UiO-66-NH2; e. UiO-66-2COOH.

Fig.4 Contour plots of the COM probability density distribution of H2O in their mixture adsorbed in three MOFs at 0.1 MPa (A) UiO-66(Zr); (B) UiO-66-NH2; (C) UiO-66-2COOH. The bulk composition n(CO2)∶n(N2)∶n(H2O)=15∶81∶4. The framework of the material is represented by a ball-stick style(Zr, dark cyan; C, gray; O, red; N, blue; H, white).

Fig.5 Radial distribution functions of CO2 and H2O molecules around the functionalized groups in two materials UiO-66-NH2(A, B) and UiO-66-2COOH(C, D) at 303 K n(CO2)∶n(N2)∶n(H2O)=15∶81∶4. (A) —OH; (B) —NH2; (C) —OH; (D) —COOH.

Fig.6 Simulated selectivity for CO2 over N2 in the different mixture at 0.1 MPa and 303 K in five MOFs (A) Effect of O2 concentration; (B) effect of SO2 concentration. a. ZIF-8; b. NOTT-300; c. UiO-66(Zr); d. UiO-66-NH2; e. UiO-66-2COOH.

Fig.7 Simulated selectivity of CO2 over N2 in the different mixture at 303 K and 0.1 MPa in five frameworks

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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

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

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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

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

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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

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