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Multi-Stimuli-Responsive Interconversion between Bowl- and Capsule-Shaped Self-Assembled Zinc(II) Complexes

Cite this: J. Am. Chem. Soc. 2020, 142, 1, 407–416
Publication Date (Web):December 5, 2019
https://doi.org/10.1021/jacs.9b11099
Copyright © 2019 American Chemical Society

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    Abstract

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    Self-assembled metal–organic architectures have great potential to undergo major structural changes into different architectures. Such molecular transformation is widely applicable to responsive systems like drug delivery and allosteric catalysis. A great number of metal–organic architectures responsive to a specific stimulus have been reported so far. However, interconversion between a pair of distinct metal–organic structures in response to multiple stimuli is rarely reported despite its high versatility. Herein we report multi-stimuli-responsive interconversion between a bowl-shaped and a capsule-shaped self-assembled ZnII complexes, [ZnII4L3X6] and [ZnII4L4], respectively, which were found to form in equilibrium from porphyrin-based ligand L and ZnII ions with different stoichiometry. Specifically, this interconversion was induced by four distinct external stimuli: exogenous ligands, Brønsted base/acid, solvents, and guest molecules. The mechanisms of the interconversion system are discussed in detail focusing on the species included in the equilibria. Thus, these findings would provide a helpful clue to design principles for multi-stimuli-responsive systems with functional versatility.

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.9b11099. Crystallographic files are also deposited with the Cambridge Crystallographic Data Center as CCDC 1936146 and 1936147.

    • Experimental procedures, characterization of compounds, NMR spectra, ESI-MS spectra, UV–vis absorption spectra, crystallographic data, details of the structural refinement, and structure comparison (PDF)

    • Single-crystal X-ray diffraction data for 1′ (CIF)

    • Single-crystal X-ray diffraction data for 2 (CIF)

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