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J Am Chem Soc. 2017 Jun 21;139(24):8174-8185. doi: 10.1021/jacs.7b01326. Epub 2017 Jun 8.

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

Author information

1
Key Laboratory of Pesticide & Chemical Biology, Ministry of Education, School of Chemistry, Central China Normal University , Wuhan, Hubei 430079, China.
2
Department of Chemistry, University of South Florida , Tampa, Florida 33620, United States.
3
Department of Chemistry, Texas State University , San Marcos, Texas 78666, United States.
4
Single Molecule Study Laboratory, College of Engineering and Nanoscale Science and Engineering Center, University of Georgia , Athens, Georgia 30602, United States.
5
Shanghai Key Laboratory of Green Chemistry and Chemical Processes, Department of Chemistry, East China Normal University , Shanghai 200062, China.
6
State Key Laboratory of Supramolecular Structure and Materials, College of Chemistry, Jilin University , Changchun, Jilin 130012, China.

Abstract

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.

PMID:
28558196
DOI:
10.1021/jacs.7b01326

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