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Transient Catenation in a Zirconium-Based Metal–Organic Framework and Its Effect on Mechanical Stability and Sorption Properties

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    Transient Catenation in a Zirconium-Based Metal–Organic Framework and Its Effect on Mechanical Stability and Sorption Properties
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    • Lee Robison
      Lee Robison
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      International Institute of Nanotechnology, Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-7419-4499
    • Xinyi Gong
      Xinyi Gong
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      International Institute of Nanotechnology, Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0003-0295-3959
    • Austin M. Evans
      Austin M. Evans
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-3597-2454
    • Florencia A. Son
      Florencia A. Son
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-7524-3774
    • Xingjie Wang
      Xingjie Wang
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-5802-9944
    • Louis R. Redfern
      Louis R. Redfern
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-0209-064X
    • Megan C. Wasson
      Megan C. Wasson
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-9384-2033
    • Zoha H. Syed
      Zoha H. Syed
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
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      Orcidhttp://orcid.org/0000-0002-0074-2253
    • Zhijie Chen
      Zhijie Chen
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0001-9232-7382
    • Karam B. Idrees
      Karam B. Idrees
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-9603-3952
    • Timur Islamoglu
      Timur Islamoglu
      International Institute of Nanotechnology, Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0003-3688-9158
    • Massimiliano Delferro
      Massimiliano Delferro
      Chemical Sciences and Engineering Division, Argonne National Laboratory, Lemont, Illinois 60439, United States
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      Orcidhttp://orcid.org/0000-0002-4443-165X
    • William R. Dichtel
      William R. Dichtel
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
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      Orcidhttp://orcid.org/0000-0002-3635-6119
    • François-Xavier Coudert
      François-Xavier Coudert
      Chimie ParisTech, PSL University, CNRS, Institut de Recherche de Chimie Paris, 75005 Paris, France
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      Orcidhttp://orcid.org/0000-0001-5318-3910
    • Nathan C. Gianneschi*
      Nathan C. Gianneschi
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      International Institute of Nanotechnology, Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
      Department of Biomedical Engineering, Department of Materials Science & Engineering, Department of Pharmacology, Simpson-Querrey Institute, Chemistry of Life Processes Institute, Lurie Cancer Center, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      *[email protected]
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      Orcidhttp://orcid.org/0000-0001-9945-5475
    • Omar K. Farha*
      Omar K. Farha
      Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      International Institute of Nanotechnology, Department of Chemistry, Northwestern University, Evanston, Illinois 60208, United States
      Department of Chemical and Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, United States
      *[email protected]
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      Orcidhttp://orcid.org/0000-0002-9904-9845
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 3, 1503–1512
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    https://doi.org/10.1021/jacs.0c11266
    Published January 12, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    Interpenetration of two or more sublattices is common among many metal–organic frameworks (MOFs). Herein, we study the evolution of one zirconium cluster-based, 3,8-connected MOF from its non-interpenetrated (NU-1200) to interpenetrated (STA-26) isomer. We observe this transient catenation process indirectly using ensemble methods, such as nitrogen porosimetry and X-ray diffraction, and directly, using high-resolution transmission electron microscopy. The approach detailed here will serve as a template for other researchers to monitor the interpenetration of their MOF samples at the bulk and single-particle limits. We investigate the mechanical stability of both lattices experimentally by pressurized in situ X-ray diffraction and nanoindentation as well as computationally with density functional theory calculations. Both lines of study reveal that STA-26 is considerably more mechanically stable than NU-1200. We conclude this study by demonstrating the potential of these MOFs and their mixed phases for the capture of gaseous n-hexane, used as a structural mimic for the chemical warfare agent sulfur mustard gas.

    Copyright © 2021 American Chemical Society

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.0c11266.

    • Physical methods and instrumentation, syntheses of TMTB linker and Zr-MOFs, PXRD data, NMR data, SEM and TEM images, mapping script, computational methods, and mechanical properties measurements (PDF)

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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 3, 1503–1512
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.0c11266
    Published January 12, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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