TY - JOUR
T1 - Engineering Pore Environments of Sulfate-Pillared Metal-Organic Framework for Efficient C2H2/CO2 Separation with Record Selectivity
AU - Liu, Xing
AU - Zhang, Peixin
AU - Xiong, Hanting
AU - Zhang, Yan
AU - Wu, Ke
AU - Liu, Junhui
AU - Krishna, Rajamani
AU - Chen, Jingwen
AU - Chen, Shixia
AU - Zeng, Zheling
AU - Deng, Shuguang
AU - Wang, Jun
N1 - Publisher Copyright:
© 2023 Wiley-VCH GmbH.
PY - 2023/5/18
Y1 - 2023/5/18
N2 - Engineering pore environments exhibit great potential in improving gas adsorption and separation performances but require specific means for acetylene/carbon dioxide (C2H2/CO2) separation due to their identical dynamic diameters and similar properties. Herein, a novel sulfate-pillared MOF adsorbent (SOFOUR-TEPE-Zn) using 1,1,2,2-tetra(pyridin-4-yl) ethene (TEPE) ligand with dense electronegative pore surfaces is reported. Compared to the prototype SOFOUR-1-Zn, SOFOUR-TEPE-Zn exhibits a higher C2H2 uptake (89.1 cm3 g−1), meanwhile the CO2 uptake reduces to 14.1 cm3 g−1, only 17.4% of that on SOFOUR-1-Zn (81.0 cm3 g−1). The high affinity toward C2H2 than CO2 is demonstrated by the benchmark C2H2/CO2 selectivity (16 833). Furthermore, dynamic breakthrough experiments confirm its application feasibility and good cyclability at various flow rates. During the desorption cycle, 60.1 cm3 g−1 C2H2 of 99.5% purity or 33.2 cm3 g−1 C2H2 of 99.99% purity can be recovered by stepped purging and mild heating. The simulated pressure swing adsorption processes reveal that 75.5 cm3 g−1 C2H2 of 99.5+% purity with a high gas recovery of 99.82% can be produced in a counter-current blowdown process. Modeling studies disclose four favorable adsorption sites and dense packing for C2H2.
AB - Engineering pore environments exhibit great potential in improving gas adsorption and separation performances but require specific means for acetylene/carbon dioxide (C2H2/CO2) separation due to their identical dynamic diameters and similar properties. Herein, a novel sulfate-pillared MOF adsorbent (SOFOUR-TEPE-Zn) using 1,1,2,2-tetra(pyridin-4-yl) ethene (TEPE) ligand with dense electronegative pore surfaces is reported. Compared to the prototype SOFOUR-1-Zn, SOFOUR-TEPE-Zn exhibits a higher C2H2 uptake (89.1 cm3 g−1), meanwhile the CO2 uptake reduces to 14.1 cm3 g−1, only 17.4% of that on SOFOUR-1-Zn (81.0 cm3 g−1). The high affinity toward C2H2 than CO2 is demonstrated by the benchmark C2H2/CO2 selectivity (16 833). Furthermore, dynamic breakthrough experiments confirm its application feasibility and good cyclability at various flow rates. During the desorption cycle, 60.1 cm3 g−1 C2H2 of 99.5% purity or 33.2 cm3 g−1 C2H2 of 99.99% purity can be recovered by stepped purging and mild heating. The simulated pressure swing adsorption processes reveal that 75.5 cm3 g−1 C2H2 of 99.5+% purity with a high gas recovery of 99.82% can be produced in a counter-current blowdown process. Modeling studies disclose four favorable adsorption sites and dense packing for C2H2.
KW - adsorptive separation
KW - electrostatic separation
KW - metal-organic frameworks
KW - pore environment modification
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U2 - 10.1002/adma.202210415
DO - 10.1002/adma.202210415
M3 - Article
C2 - 36856017
AN - SCOPUS:85152003339
SN - 0935-9648
VL - 35
JO - Advanced Materials
JF - Advanced Materials
IS - 20
M1 - 2210415
ER -