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ACS Publications. Most Trusted. Most Cited. Most Read
Linker Exchange via Migration along the Backbone in Metal–Organic Frameworks

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Download Hi-Res ImageDownload to MS-PowerPointCite This:J. Am. Chem. Soc. 2021, 143, 28, 10541-10546
    Communication

    Linker Exchange via Migration along the Backbone in Metal–Organic Frameworks
    Click to copy article linkArticle link copied!

    • Nader Al Danaf
      Nader Al Danaf
      Department of Chemistry and Center for NanoScience, University of Munich, Butenandtstraße 5-13, 81377 Munich, Germany
      More by Nader Al Danaf
    • Waldemar Schrimpf
      Waldemar Schrimpf
      Department of Chemistry and Center for NanoScience, University of Munich, Butenandtstraße 5-13, 81377 Munich, Germany
      More by Waldemar Schrimpf
    • Patrick Hirschle
      Patrick Hirschle
      Department of Chemistry and Center for NanoScience, University of Munich, Butenandtstraße 5-13, 81377 Munich, Germany
      More by Patrick Hirschle
    • Don C. Lamb
      Don C. Lamb
      Department of Chemistry and Center for NanoScience, University of Munich, Butenandtstraße 5-13, 81377 Munich, Germany
      More by Don C. Lamb
      Orcidhttps://orcid.org/0000-0002-0232-1903
    • Zhe Ji*
      Zhe Ji
      Department of Chemistry, University of California-Berkeley, Berkeley, California 94720, United States
      *[email protected]
      More by Zhe Ji
      Orcidhttps://orcid.org/0000-0002-8532-333X
    • Stefan Wuttke*
      Stefan Wuttke
      Department of Chemistry and Center for NanoScience, University of Munich, Butenandtstraße 5-13, 81377 Munich, Germany
      BCMaterials (Basque Center for Materials, Applications & Nanostructures), Building Martina Casiano, 3rd Floor, Barrio Sarriena s/n, 48940 Leioa, Spain
      IKERBASQUE, Basque Foundation for Science, 48009 Bilbao, Spain
      *[email protected]
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      Orcidhttps://orcid.org/0000-0002-6344-5782
    Other Access OptionsSupporting Information (1)

    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 28, 10541–10546
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c04804
    Published July 6, 2021
    Copyright © 2021 American Chemical Society
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    Abstract

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    In metal–organic frameworks (MOFs), organic linkers are subject to postsynthetic exchange (PSE) when new linkers reach sites of PSE by diffusion. Here, we show that during PSE, a bulky organic linker is able to penetrate narrow-window MOF crystals. The bulky linker migrates by continuously replacing the linkers gating the otherwise impassable windows and serially occupying an array of backbone sites, a mechanism we term through-backbone diffusion. A necessary consequence of this process is the accumulation of missing-linker defects along the diffusion trajectories. Using fluorescence intensity and lifetime imaging microscopy, we found a gradient of missing-linker defects from the crystal surface to the interior, consistent with the spatial progression of PSE. Our success in incorporating bulky functional groups via PSE extends the scope of MOFs that can be used to host sizable, sophisticated guest species, including large catalysts or biomolecules, which were previously deemed only incorporable into MOFs of very large windows.

    Copyright © 2021 American Chemical Society

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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/jacs.1c04804.

    • Experimental, crystallographic, photophysical, and microscopy data including PXRD, SEM, fluorescence spectroscopy, and FLIM results (PDF)

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    Cited By

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    This article is cited by 11 publications.

    1. Adrian Hannebauer, Yaşar Krysiak, Andreas Schaate. A Method for Determining Incorporation Depth in Core–Shell UiO-66 Nanoparticles Synthesized Via Postsynthetic Exchange. Inorganic Chemistry 2024, 63 (25) , 11897-11906. https://doi.org/10.1021/acs.inorgchem.4c01787
    2. Junchang Chen, Mingxing Zhang, Jie Shu, Shengtang Liu, Xiao Dong, Chunyang Li, Linwei He, Mengjia Yuan, Yutian Wu, Jiahui Xu, Duo Zhang, Fuyin Ma, Guozhong Wu, Zhifang Chai, Shuao Wang. Radiation-Induced De Novo Defects in Metal–Organic Frameworks Boost CO2 Sorption. Journal of the American Chemical Society 2023, 145 (43) , 23651-23658. https://doi.org/10.1021/jacs.3c07778
    3. Feng-Zao Chen, Xiao-Xue Fu, Xiao-Jie Yu, Yu-Hang Qiu, Shi-Bin Ren, Yi-Chao Wang, De-Man Han, Wei-Wei Zhao. Biological Transformation of AgI on MOF-on-MOF-Derived Heterostructures: Toward Polarity-Switchable Photoelectrochemical Biosensors for Neuron-Specific Enolase. Analytical Chemistry 2023, 95 (23) , 9052-9059. https://doi.org/10.1021/acs.analchem.3c01401
    4. Ainara Valverde, Gabriel I. Tovar, Natalia A. Rio-López, Dimas Torres, Maibelin Rosales, Stefan Wuttke, Arkaitz Fidalgo-Marijuan, José María Porro, Mónica Jiménez-Ruiz, Victoria García Sakai, Andreina García, José Manuel Laza, José Luis Vilas-Vilela, Luis Lezama, María I. Arriortua, Guillermo J. Copello, Roberto Fernández de Luis. Designing Metal-Chelator-like Traps by Encoding Amino Acids in Zirconium-Based Metal–Organic Frameworks. Chemistry of Materials 2022, 34 (21) , 9666-9684. https://doi.org/10.1021/acs.chemmater.2c02431
    5. Yuan Gao, Meijin Li, Yongyi Zeng, Xiaolong Liu, Dianping Tang. Tunable Competitive Absorption-Induced Signal-On Photoelectrochemical Immunoassay for Cardiac Troponin I Based on Z-Scheme Metal–Organic Framework Heterojunctions. Analytical Chemistry 2022, 94 (39) , 13582-13589. https://doi.org/10.1021/acs.analchem.2c03263
    6. Jacopo Andreo, Romy Ettlinger, Orysia Zaremba, Quim Peña, Ulrich Lächelt, Roberto Fernández de Luis, Ralph Freund, Stefano Canossa, Evelyn Ploetz, Wei Zhu, Christian S. Diercks, Harald Gröger, Stefan Wuttke. Reticular Nanoscience: Bottom-Up Assembly Nanotechnology. Journal of the American Chemical Society 2022, 144 (17) , 7531-7550. https://doi.org/10.1021/jacs.1c11507
    7. Xiaofeng Chen, Pradeepkumar Jagadesan, Silvano Valandro, Joseph T. Hupp, Kirk S. Schanze, Subhadip Goswami. Identifying the Polymorphs of Zr-Based Metal–Organic Frameworks via Time-Resolved Fluorescence Imaging. ACS Materials Letters 2022, 4 (2) , 370-377. https://doi.org/10.1021/acsmaterialslett.1c00754
    8. Yang Shan, Guangxun Zhang, Yuxin Shi, Huan Pang. Synthesis and catalytic application of defective MOF materials. Cell Reports Physical Science 2023, 4 (3) , 101301. https://doi.org/10.1016/j.xcrp.2023.101301
    9. Andreina García, Bárbara Rodríguez, Maibelin Rosales, Yurieth M. Quintero, Paula G. Saiz, Ander Reizabal, Stefan Wuttke, Leire Celaya-Azcoaga, Ainara Valverde, Roberto Fernández de Luis. A State-of-the-Art of Metal-Organic Frameworks for Chromium Photoreduction vs. Photocatalytic Water Remediation. Nanomaterials 2022, 12 (23) , 4263. https://doi.org/10.3390/nano12234263
    10. Adrian Fuchs, Petra Mannhardt, Patrick Hirschle, Haoze Wang, Irina Zaytseva, Zhe Ji, Omar Yaghi, Stefan Wuttke, Evelyn Ploetz. Single Crystals Heterogeneity Impacts the Intrinsic and Extrinsic Properties of Metal–Organic Frameworks. Advanced Materials 2022, 34 (3) , 2104530. https://doi.org/10.1002/adma.202104530
    11. Christin Kirst, Nader A. Danaf, Fabian Knechtel, Tim Arczynski, Peter Mayer, Don C. Lamb, Konstantin L. Karaghiosoff. Methods for elucidating the structural–property relationship in luminescent materials. Journal of Materials Chemistry C 2021, 9 (38) , 13366-13375. https://doi.org/10.1039/D1TC02634H
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2021, 143, 28, 10541–10546
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.1c04804
    Published July 6, 2021
    Copyright © 2021 American Chemical Society
    Request reuse permissions

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