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Steric and Electronic Effects on the Interaction of Xe and Kr with Functionalized Zirconia Metal–Organic Frameworks

Cite this: ACS Materials Lett. 2021, 3, 5, 504–510
Publication Date (Web):March 31, 2021
https://doi.org/10.1021/acsmaterialslett.1c00077
Copyright © 2021 American Chemical Society

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    Abstract

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    The separation of xenon and krypton from their mixtures has been an enduring and complex venture due to their similar sizes and unreactive nature. Metal–organic frameworks (MOFs) have shown the potential to complete these challenging separations by utilizing pressure-swing adsorption (PSA) as a sustainable alternative to current cryogenic distillation techniques. To rationally design materials to better realize this goal, two main approaches have emerged: pore-size optimized and polarizability-based separations. To ascertain the efficacy of these strategies, we designed a series of UiO-type MOFs with terphenyl linkers that systematically varied their steric and electronic properties, including −Me, −F, −TMS, and −I functionalities, to assess their interactions with xenon and krypton. The prepared MOFs are all isoreticular and have similar pore size distributions, allowing us to directly evaluate the effects imposed by the functional groups. We found that the xenon uptake could be increased with greater polarizability of the functional group (−F < −Me ≈ −TMS < −I), whereas the selectivities seem to follow a trend more related to pore-steric effects (−TMS < −I < −Me < −F).

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsmaterialslett.1c00077.

    • Crystallographic information for UiO-68-Me2 (CIF)

    • Crystallographic information for UiO-68-F4 (CIF)

    • Crystallographic information for UiO-68-TMS2 (CIF)

    • Crystallographic information for UiO-68-I2 (CIF)

    • Materials and methods, synthesis procedures, X-ray diffraction, SEM images, gas adsorption measurements, stability studies, thermogravimetric and spectroscopic analysis, and NMR spectra (PDF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

    This article is cited by 5 publications.

    1. Shanshan Liu, Xin Lian, Bin Yue, Shutao Xu, Guangjun Wu, Yuchao Chai, Yinghui Zhang, Landong Li. Control of Zeolite Local Polarity toward Efficient Xenon/Krypton Separation. Journal of the American Chemical Society 2024, 146 (12) , 8335-8342. https://doi.org/10.1021/jacs.3c13994
    2. David W. Fox, Dennis-Xavier Antony, Yuen Yee Li Sip, Joshua Fnu, Azina Rahmani, Titel Jurca, Lei Zhai. Electrospun hydrogel fibers guide HKUST-1 assembly. Materials Today Communications 2022, 33 , 104535. https://doi.org/10.1016/j.mtcomm.2022.104535
    3. Jia-Xin Wang, Cong-Cong Liang, Xiao-Wen Gu, Hui-Min Wen, Chenghao Jiang, Bin Li, Guodong Qian, Banglin Chen. Recent advances in microporous metal–organic frameworks as promising adsorbents for gas separation. Journal of Materials Chemistry A 2022, 10 (35) , 17878-17916. https://doi.org/10.1039/D2TA04835C
    4. Chenghui Zhang, Xinglong Dong, Yongwei Chen, Houxiao Wu, Liang Yu, Kang Zhou, Ying Wu, Qibin Xia, Hao Wang, Yu Han, Jing Li. Balancing uptake and selectivity in a copper-based metal–organic framework for xenon and krypton separation. Separation and Purification Technology 2022, 291 , 120932. https://doi.org/10.1016/j.seppur.2022.120932
    5. David Fox, Dennis-Xavier Antony, Yuen Yee Li Sip, Joshua Fnu, Azina Rahmani, Titel Jurca, Lei Zhai. Electrospun Hydrogel Fibers Guide Hkust-1 Assembly. SSRN Electronic Journal 2022, 120 https://doi.org/10.2139/ssrn.4153284