4.7 Article

A metal-organic framework for C2H2/CO2 separation under highly humid conditions: Balanced hydrophilicity/hydrophobicity

Journal

CHEMICAL ENGINEERING JOURNAL
Volume 427, Issue -, Pages -

Publisher

ELSEVIER SCIENCE SA
DOI: 10.1016/j.cej.2021.132033

Keywords

Metal-organic frameworks; Scalable synthesis; C2H2/CO2 separation; Llydrophilicity/hydrophobicity; Adsorption kinetics

Funding

  1. National Natural Science Foundation of China [21731002, 21975104]
  2. Guangdong Major Project of Basic and Applied Research [2019B030302009]
  3. Guangdong Basic and Applied Basic Research Foundation [2020A1515011005]

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JNU-2, a cage-interconnected microporous MOF, demonstrates high C2H2 capture capacity and selectivity, surpassing benchmark materials like UTSA-74a and FeNi-M'MOF. The surface interactions of JNU-2 enable preferential binding of C2H2 over CO2, contributing to its efficient C2H2/CO2 separation capability.
Metal-organic frameworks (MOFs) intended for C2H2/CO2 separation should possess high C2H2/CO2 adsorption selectivity and large C2H2 adsorption capacity. Here we report the scalable synthesis of a cage-interconnected microporous MOF (JNU-2). Dynamic column breakthrough experiments on JNU-2 manifest a C2H2-capture capacity of 3.08 mmol g(-1) for an equimolar C2H2/CO2 mixture at 298 K and 1 bar, exceeding the benchmark materials such as UTSA-74a and FeNi-M'MOF. Meanwhile, the selectivity factor was estimated to be ca. 1.5 for JNU-2 and consistent with the increasing flow rate. Theoretical calculations confirm that the surface of the JNU-2 framework enables preferential binding of C2H2 over CO2 via multiple C-H center dot center dot center dot O, C-H center dot center dot center dot N, and pi-complexation interactions. More importantly, JNU-2 retains its C2H2/CO2 separation capacity under highly humid conditions. Although the equilibrium adsorption of H2O is much higher than those of C2H2 and CO2, kinetic studies reveal that the diffusion of C2H2 and CO2 in JNU-2 is more than two orders of magnitude faster than that of H2O. A balanced hydrophobicity/hydmphilicity of the MOF framework surface might be the key to achieving large adsorption capacity for nonpolar gas molecule while minimizing the competition of water vapor adsorption.

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