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

doi:10.7503/cjcu20140802

Abstract

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

CLC Number:

O641
O634

TrendMD:

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^†[J]. Chem. J. Chinese Universities, 2015, 36(2): 316.

Figures/Tables 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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