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Potential of a pH-Stable Microporous MOF for C2H2/C2H4 and C2H2/CO2 Gas Separations under Ambient Conditions

Cite this: Inorg. Chem. 2022, 61, 45, 18293–18302
Publication Date (Web):November 1, 2022
https://doi.org/10.1021/acs.inorgchem.2c03275
Copyright © 2022 American Chemical Society

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    Abstract

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    Cost-effective adsorption-based C2H2/C2H4 and C2H2/CO2 gas separations are extremely important in the industry. Herein, a pH-stable three-dimensional (3D) metal–organic framework (MOF), IITKGP-25, possessing exposed functional sites is presented, which facilitates such separations with excellent ideal adsorbed solution theory (IAST) selectivity (4.61 for C2H2/C2H4 and 3.93 for C2H2/CO2) under ambient conditions (295 K, 100 kPa, 50:50 gas mixtures) and a moderate affinity toward C2H2 (26.6 kJ mol–1). Interestingly, IITKGP-25 can maintain structural integrity in water and in aqueous acidic/alkaline (pH = 2–10) medium because of the higher coordination numbers around the metal center and the hydrophobicity of the ligand. The adsorption capacity for C2H2 remains unchanged for a minimum of up to five consecutive cycles and 15 days of exposure to 97% relative humidity, which are the prerequisites of an adsorbent for practical gas separation application. Density functional theory (DFT) calculations reveal that the open Cd(II) sites and carboxylate oxygen-coordinated Cd(II) corner of the triangle-shaped one-dimensional (1D) channel are the enthalpically more preferred binding sites for C2H2, which stabilize the adsorbed C2H2 through nonlocal stronger H-bonding and also pπ–dπ and CH−π interactions.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acs.inorgchem.2c03275.

    • Instrument details, synthesis of the ligand and MOF, basic characterization data, including PXRD, TGA, and NMR data; X-ray crystallographic parameters, virial fitting plots, IAST calculations, fitting plots, table of fitting parameters, and DFT computational details (PDF)

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    CCDC 2207356 contains the supplementary crystallographic data for this paper. These data can be obtained free of charge via www.ccdc.cam.ac.uk/data_request/cif, or by emailing [email protected], or by contacting The Cambridge Crystallographic Data Centre, 12 Union Road, Cambridge CB2 1EZ, UK; fax: +44 1223 336033.

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    Cited By

    This article is cited by 8 publications.

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    2. Yufeng Chen, Shixiong Li, Yubing Liu, Ping Shi, Shihua Xu, Yuejing Bin. A Bifunctional Three-Dimensional Zn(II) Metal–Organic Framework with Strong Luminescence and Adsorption Cr(VI) Properties. ACS Omega 2024, 9 (16) , 18429-18437. https://doi.org/10.1021/acsomega.4c00431
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    7. Nilanjan Seal, Athulya S. Palakkal, Renjith S. Pillai, Subhadip Neogi. Coordination Unsaturation and Basic Site-Immobilized Nanochannel in a Chemorobust MOF for 3-Fold-Increased High-Temperature Selectivity and Fixation of CO2 under Mild Conditions with Nanomolar Recognition of Roxarsone. Inorganic Chemistry 2023, 62 (29) , 11528-11540. https://doi.org/10.1021/acs.inorgchem.3c01160
    8. Shyam Chand Pal, Rajamani Krishna, Madhab C. Das. Highly scalable acid-base resistant Cu-Prussian blue metal-organic framework for C2H2/C2H4, biogas, and flue gas separations. Chemical Engineering Journal 2023, 460 , 141795. https://doi.org/10.1016/j.cej.2023.141795

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