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    Low-Valent Metal Ions as MOF Pillars: A New Route Toward Stable and Multifunctional MOFs
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    • R. Eric Sikma
      R. Eric Sikma
      Department of Chemistry, University of Texas at Austin, 4.428 Welch Hall, 105 E. 24th Street Stop A5300, Austin, Texas 78712-0165, United States
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    • Naman Katyal
      Naman Katyal
      Department of Chemistry, University of Texas at Austin, 4.428 Welch Hall, 105 E. 24th Street Stop A5300, Austin, Texas 78712-0165, United States
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    • Su-Kyung Lee
      Su-Kyung Lee
      Research Center for Nanocatalysis, Korea Research Institute of Chemical Technology (KRICT), P.O. Box 107, Yusung, Daejeon 305-600, Korea
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    • Joseph W. Fryer
      Joseph W. Fryer
      Austin-International Framework Undergraduate Exchange Program, College of Natural Sciences, University of Texas at Austin, 120 Inner Campus Drive Stop G2500, Austin, Texas 78712, United States
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    • Catherine G. Romero
      Catherine G. Romero
      Austin-International Framework Undergraduate Exchange Program, College of Natural Sciences, University of Texas at Austin, 120 Inner Campus Drive Stop G2500, Austin, Texas 78712, United States
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    • Samuel K. Emslie
      Samuel K. Emslie
      Department of Chemistry, University of Texas at Austin, 4.428 Welch Hall, 105 E. 24th Street Stop A5300, Austin, Texas 78712-0165, United States
      Austin-International Framework Undergraduate Exchange Program, College of Natural Sciences, University of Texas at Austin, 120 Inner Campus Drive Stop G2500, Austin, Texas 78712, United States
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    • Elinor L. Taylor
      Elinor L. Taylor
      Austin-International Framework Undergraduate Exchange Program, College of Natural Sciences, University of Texas at Austin, 120 Inner Campus Drive Stop G2500, Austin, Texas 78712, United States
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    • Vincent M. Lynch
      Vincent M. Lynch
      Department of Chemistry, University of Texas at Austin, 4.428 Welch Hall, 105 E. 24th Street Stop A5300, Austin, Texas 78712-0165, United States
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    • Jong-San Chang*
      Jong-San Chang
      Research Center for Nanocatalysis, Korea Research Institute of Chemical Technology (KRICT), P.O. Box 107, Yusung, Daejeon 305-600, Korea
      *[email protected]
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      Orcidhttps://orcid.org/0000-0003-3640-8190
    • Graeme Henkelman*
      Graeme Henkelman
      Department of Chemistry, University of Texas at Austin, 4.428 Welch Hall, 105 E. 24th Street Stop A5300, Austin, Texas 78712-0165, United States
      *[email protected]
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      Orcidhttps://orcid.org/0000-0002-0336-7153
    • Simon M. Humphrey*
      Simon M. Humphrey
      Department of Chemistry, University of Texas at Austin, 4.428 Welch Hall, 105 E. 24th Street Stop A5300, Austin, Texas 78712-0165, United States
      *[email protected]
      More by Simon M. Humphrey
      Orcidhttps://orcid.org/0000-0001-5379-4623
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 34, 13710–13720
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    https://doi.org/10.1021/jacs.1c05564
    Published August 19, 2021
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    Abstract

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    PCM-102 is a new organophosphine metal–organic framework (MOF) featuring diphosphine pockets that consist of pairs of offset trans-oriented P(III) donors. Postsynthetic addition of M(I) salts (M = Cu, Ag, Au) to PCM-102 induces single-crystal to single-crystal transformations and the formation of trans-[P2M]+ solid-state complexes (where P = framework-based triarylphosphines). While the unmetalated PCM-102 has low porosity, the addition of secondary Lewis acids to install rigid P–M–P pillars is shown to dramatically increase both stability and selective gas uptake properties, with N2 Brunauer–Emmett–Teller surface areas >1500 m2 g–1. The Ag(I) analogue can also be obtained via a simple, one-pot peri-synthetic route and is an ideal sacrificial precursor for materials with mixed bimetallic MA/MB pillars via postsynthetic, solvent-assisted metal exchange. Notably, the M-PCM-102 family of MOFs contain periodic trans-[P2M]+ sites that are free of counter anions, unlike traditional analogous molecular complexes, since the precursor PCM-102 MOF is monoanionic, enabling access to charge-neutral metal-pillared materials. Four M-PCM-102 materials were evaluated for the separation of C2 hydrocarbons. The separation performance was found to be tunable based on the metal(s) incorporated, and density functional theory was employed to elucidate the nature of the unusual observed sorption preference, C2H2 > C2H6 > C2H4.

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    CCDC 2081306–2081311 contain 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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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 34, 13710–13720
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c05564
    Published August 19, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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