TY - JOUR
T1 - Effects of Activation Temperature and Densification on Adsorption Performance of MOF MIL-100(Cr)
AU - Yang, Jiangfeng
AU - Bai, Honghao
AU - Zhang, Feifei
AU - Liu, Jiaqi
AU - Winarta, Joseph
AU - Wang, Yong
AU - Mu, Bin
N1 - Funding Information:
B.M. acknowledges financial support from the National Science Foundation (Grant Nos. CBET-1748641 and CMMI-1825594). J.Y. is grateful to the funding from the National Natural Science Foundation of China (Nos. 21676175 and 51672186).
Funding Information:
B.M. acknowledges financial support from the National Science Foundation (Grant Nos. CBET-1748641 and CMMI-1825594). J.Y. is grateful to the funding from the National Natural Science Foundation of China (Nos. 21676175 and 51672186).
Publisher Copyright:
Copyright © 2019 American Chemical Society.
PY - 2019/12/12
Y1 - 2019/12/12
N2 - Metal-organic frameworks (MOFs) with open metal sites have attracted lots of attention because of their high binding energy for adsorbates. MIL-100(Cr) is one of the potential MOFs for challenging separations. Multicomponent breakthrough studies on MOF pellets are critically needed because only pelletized adsorbents can be used in pressure or temperature swing adsorption processes. Thus, in this study, we compared the adsorption equilibrium of MIL-100(Cr) powder and pellets and carried out a breakthrough study of multicomponent gas mixtures on pelletized MIL-100(Cr), which revealed interesting effects of activation conditions on its performance. The experimental results show that the CO2 adsorption capacity of MIL-100(Cr) powder activated at 523 K and high vacuum (10-10 bar) was about 2.5 times higher than that of MIL-100(Cr) treated under mild activation conditions (423 K). The highest 5.8 mol/g CO2 capacity at 298 K and 1 bar is consistent with the high CO2-Cr3+ binding energy of 63 kJ/mol, determined using density functional theory calculations. However, the number drops to 4.05 mol/g for pelletized samples. The negative impact of densification on the adsorption capacity follows the order of CO2 N2 CH4 for MIL-100(Cr)250 and CH4 N2 CO2 for MIL-100(Cr)150, which also suggests that the effects of open Cr sites on the adsorption capacity follows the order of CO2 N2 CH4 on MIL-100(Cr). The selectivity of MIL-100(Cr) pellets based on breakthrough measurements for CO2/N2 (20/80) and CO2/CH4 (40/60) mixtures was 4.3 and 10.7, respectively.
AB - Metal-organic frameworks (MOFs) with open metal sites have attracted lots of attention because of their high binding energy for adsorbates. MIL-100(Cr) is one of the potential MOFs for challenging separations. Multicomponent breakthrough studies on MOF pellets are critically needed because only pelletized adsorbents can be used in pressure or temperature swing adsorption processes. Thus, in this study, we compared the adsorption equilibrium of MIL-100(Cr) powder and pellets and carried out a breakthrough study of multicomponent gas mixtures on pelletized MIL-100(Cr), which revealed interesting effects of activation conditions on its performance. The experimental results show that the CO2 adsorption capacity of MIL-100(Cr) powder activated at 523 K and high vacuum (10-10 bar) was about 2.5 times higher than that of MIL-100(Cr) treated under mild activation conditions (423 K). The highest 5.8 mol/g CO2 capacity at 298 K and 1 bar is consistent with the high CO2-Cr3+ binding energy of 63 kJ/mol, determined using density functional theory calculations. However, the number drops to 4.05 mol/g for pelletized samples. The negative impact of densification on the adsorption capacity follows the order of CO2 N2 CH4 for MIL-100(Cr)250 and CH4 N2 CO2 for MIL-100(Cr)150, which also suggests that the effects of open Cr sites on the adsorption capacity follows the order of CO2 N2 CH4 on MIL-100(Cr). The selectivity of MIL-100(Cr) pellets based on breakthrough measurements for CO2/N2 (20/80) and CO2/CH4 (40/60) mixtures was 4.3 and 10.7, respectively.
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U2 - 10.1021/acs.jced.9b00770
DO - 10.1021/acs.jced.9b00770
M3 - Article
AN - SCOPUS:85074237634
SN - 0021-9568
VL - 64
SP - 5814
EP - 5823
JO - Journal of Chemical and Engineering Data
JF - Journal of Chemical and Engineering Data
IS - 12
ER -