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Supersnowflakes: Stepwise Self-Assembly and Dynamic Exchange of Rhombus Star-Shaped Supramolecules

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† Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, School of Chemistry, Central China Normal University, Wuhan, Hubei 430079, China
‡ Department of Chemistry, University of South Florida, Tampa, Florida 33620, United States
§ Department of Chemistry, Texas State University, San Marcos, Texas 78666, United States
∥ Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University, Shanghai 200062, China
⊥ State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University, Changchun, Jilin 130012, China
# Single Molecule Study Laboratory, College of Engineering and Nanoscale Science and Engineering Center, University of Georgia, Athens, Georgia 30602, United States
*[email protected]
*[email protected]
*[email protected]
Cite this: J. Am. Chem. Soc. 2017, 139, 24, 8174–8185
Publication Date (Web):May 30, 2017
https://doi.org/10.1021/jacs.7b01326
Copyright © 2017 American Chemical Society
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    Abstract

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    With the goal of increasing the complexity of metallo-supramolecules, two rhombus star-shaped supramolecular architectures, namely, supersnowflakes, were designed and assembled using multiple 2,2′:6′,2″-terpyridine (tpy) ligands in a stepwise manner. In the design of multicomponent self-assembly, ditopic and tritopic ligands were bridged through Ru(II) with strong coordination to form metal–organic ligands for the subsequent self-assembly with a hexatopic ligand and Zn(II). The combination of Ru(II)–organic ligands with high stability and Zn(II) ions with weak coordination played a key role in the self-assembly of giant heteroleptic supersnowflakes, which encompassed three types of tpy-based organic ligands and two metal ions. With such a stepwise strategy, the self-sorting of individual building blocks was prevented from forming the undesired assemblies, e.g., small macrocycles and coordination polymers. Furthermore, the intra- and intermolecular dynamic exchange study of two supersnowflakes by NMR and mass spectrometry revealed the remarkable stability of these giant supramolecular complexes.

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    • Synthetic details, molecular modeling, and ligand and complex characterization, including 1H NMR, 13C NMR, 2D COSY, 2D NOESY, 2D ROESY, ESI-MS, TWIM-MS, and MALDI-TOF (PDF)

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