Single-crystal-to-single-crystal metalation of a metal-organic framework: A route toward structurally well-defined catalysts

Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A.; Teat, Simon J.; Long, Jeffrey R.

doi:10.1021/acs.inorgchem.5b00096

Title: Single-crystal-to-single-crystal metalation of a metal-organic framework: A route toward structurally well-defined catalysts

Journal Article · Mon Jul 20 00:00:00 EDT 2015 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.5b00096· OSTI ID:1176798

Gonzalez, Miguel I. ^[1]; Bloch, Eric D. ^[1]; Mason, Jarad A. ^[1]; Teat, Simon J. ^[2]; Long, Jeffrey R. ^[3]

Univ. of California, Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Metal–organic frameworks featuring ligands with open chelating groups are versatile platforms for the preparation of a diverse set of heterogeneous catalysts through postsynthetic metalation. The crystalline nature of these materials allows them to be characterized via X-ray diffraction, which provides valuable insight into the structure of the metal sites that facilitate catalysis. A highly porous and thermally robust zirconium-based metal–organic framework, Zr₆O₄(OH)₄(bpydc)₆ (bpydc^2– = 2,2'-bipyridne-5,5'-dicarboxylate), bears open bipyridine sites that readily react with a variety of solution- and gas-phase metal sources to form the corresponding metalated frameworks. Remarkably, Zr₆O₄(OH)₄(bpydc)₆ undergoes a single-crystal-to-single-crystal transformation upon metalation that involves a change in space group from $$Fm\bar{3}m$$ to $$Pa\bar{3}m$$. This structural transformation leads to an ordering of the metalated linkers within the framework, allowing structural characterization of the resulting metal complexes. Furthermore, Zr₆O₄(OH)₄(bpydc)₆ yields an active heterogeneous catalyst for arene C–H borylation when metalated with [Ir(COD)₂]BF₄ (COD = 1,5-cyclooctadiene). These results highlight the unique potential of metal–organic frameworks as a class of heterogeneous catalysts that allow unparalleled structural characterization and control over their active sites.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI ID:: 1176798

Journal Information:: Inorganic Chemistry, Vol. 54, Issue 6; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: ENGLISH

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Cited by: 138 works

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Acidic ionic liquid based UiO-67 type MOFs: a stable and efficient heterogeneous catalyst for esterification Xu, Zichen; Zhao, Guoying; Ullah, Latif RSC Advances, Vol. 8, Issue 18 https://doi.org/10.1039/c8ra01119b	journal	January 2018
Solvent-free heterogeneous catalysis for cyanosilylation in a dynamic cobalt-MOF Cui, Xin; Xu, Mei-Chen; Zhang, Ling-Juan Dalton Transactions, Vol. 44, Issue 28 https://doi.org/10.1039/c5dt01456e	journal	January 2015
Catalytic chemoselective functionalization of methane in a metal−organic framework Zhang, Xuan; Huang, Zhiyuan; Ferrandon, Magali Nature Catalysis, Vol. 1, Issue 5 https://doi.org/10.1038/s41929-018-0069-6	journal	May 2018
Chelation of transition metals into MOFs as a promising method for enhancing CO ₂ capture: A computational study Hu, Jianbo; Liu, Yang; Liu, Jing AIChE Journal, Vol. 66, Issue 2 https://doi.org/10.1002/aic.16835	journal	October 2019
Postsynthetic Modification of Zirconium Metal-Organic Frameworks: Postsynthetic Modification of Zirconium Metal-Organic Frameworks Marshall, Ross J.; Forgan, Ross S. European Journal of Inorganic Chemistry, Vol. 2016, Issue 27 https://doi.org/10.1002/ejic.201600394	journal	July 2016
Encapsulation of an organometallic cationic catalyst by direct exchange into an anionic MOF Grigoropoulos, Alexios; Whitehead, George F. S.; Perret, Noémie Chemical Science, Vol. 7, Issue 3 https://doi.org/10.1039/c5sc03494a	journal	January 2016
Controlling interpenetration through linker conformation in the modulated synthesis of Sc metal-organic frameworks Marshall, Rj; Lennon, Ct; Tao, A. Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.20975	text	January 2018
Organometallic chemistry using partially fluorinated benzenes Pike, Sebastian; Crimmin, Mr; Chaplin, Ab Apollo - University of Cambridge Repository https://doi.org/10.17863/cam.8845	text	January 2017
Non-Porous Iron(II)-Based Sensor: Crystallographic Insights into a Cycle of Colorful Guest-Induced Topotactic Transformations Rodríguez-Jiménez, Santiago; Feltham, Humphrey L. C.; Brooker, Sally Angewandte Chemie International Edition, Vol. 55, Issue 48 https://doi.org/10.1002/anie.201608813	journal	October 2016
Mapping-Out Catalytic Processes in a Metal-Organic Framework with Single-Crystal X-ray Crystallography Burgun, Alexandre; Coghlan, Campbell J.; Huang, David M. Angewandte Chemie International Edition, Vol. 56, Issue 29 https://doi.org/10.1002/anie.201611254	journal	February 2017

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CCDC 1042960: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc1408w9 The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042961: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc1408xb The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042964: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc14090g The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042868: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc1405x7 The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042996: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc140b1j The current record is supplemented by this dataset	dataset	January 2015
CCDC 1434430: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc1k4my8 The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042962: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc1408yc The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042965: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc14091h The current record is supplemented by this dataset	dataset	January 2015
CCDC 1042867: Experimental Crystal Structure Determination Gonzalez, Miguel I.; Bloch, Eric D.; Mason, Jarad A. https://doi.org/10.5517/cc1405w6 The current record is supplemented by this dataset	dataset	January 2015