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Creating Order in Ultrastable Phosphonate Metal–Organic Frameworks via Isolable Hydrogen-Bonded Intermediates

Cite this: J. Am. Chem. Soc. 2023, 145, 39, 21263–21272
Publication Date (Web):September 22, 2023
https://doi.org/10.1021/jacs.3c05279
Copyright © 2023 American Chemical Society

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    Abstract

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    The stability presented by trivalent metal–organic frameworks (MOFs) makes them an attractive class of materials. With phosphonate-based ligands, crystallization is a challenge, as there are significantly more binding motifs that can be adopted due to the extra oxygen tether compared to carboxylate counterparts and the self-assembly processes are less reversible. Despite this, we have reported charge-assisted hydrogen-bonded metal–organic frameworks (HMOFs) consisting of [Cr(H2O)6]3+ and phosphonate ligands, which were crystallographically characterized. We sought to use these HMOFs as a crystalline intermediate to synthesize ordered Cr(III)-phosphonate MOFs. This can be done by dehydrating the HMOF to remove the aquo ligands around the Cr(III) center, forcing metal–phosphonate coordination. Herein, a new porous HMOF, H-CALF-50, is synthesized and then dehydrated to yield the MOF CALF-50. CALF-50 is ordered, although it is not single crystalline. It does, however, have exceptional stability, maintaining crystallinity and surface area after boiling in water for 3 weeks and soaking in 14.5 M H3PO4 for 24 h and 9 M HCl for 72 h. Computational methods are used to study the HMOF to MOF transformation and give insight into the nature of the structure and the degree of heterogeneity.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.3c05279.

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    CCDC 2264317 contains 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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    Cited By

    This article is cited by 1 publications.

    1. Chen Jia, Shuai Liang, Yu-Xuan Wen, Zhen-Zhen Xue, Jie Pan, Ji-Xiang Hu, Guo-Ming Wang. Photochromic Ln-Phosphonates Assembled by an Imidazole Derivative: Construction, Crystal Structures, and Light-Enhanced Proton Conductivity. Crystal Growth & Design 2024, 24 (5) , 2202-2209. https://doi.org/10.1021/acs.cgd.3c01515