Giant, Hollow 2D Metalloarchitecture: Stepwise Self-Assembly of a Hexagonal Supramolecular Nut

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• 作者：Yiming Li ; Zhilong Jiang ; Ming Wang ; Jie Yuan ; Die Liu ; Xiaoyu Yang ; Mingzhao Chen ; Jun Yan ; Xiaopeng Li ; Pingshan Wang
• 刊名：Journal of the American Chemical Society
• 出版年：2016
• 出版时间：August 10, 2016
• 年：2016
• 卷：138
• 期：31
• 页码：10041-10046
• 全文大小：603K
• 年卷期：0
• ISSN：1520-5126

文摘

A polyterpyridinyl building block-based nutlike hexagonal bismetallo architecture with a central hollow Star of David was assembled by a stepwise strategy. This nanoarchitecture can be viewed as a recursive mathematical form that possesses a supramolecular corner-connected cyclic structure, i.e., a triangle or rhombus at various levels of scale or detail. The key metallo-organic ligand (MOL) with four uncomplexed free terpyridines was obtained by a final Suzuki cross-coupling reaction with a tetrabromoterpyridine Ru dimer. The molecular metallorhombus was prepared by reacting the MOL with a 60° bis-terpyridine and Fe²⁺. The giant hollow hexagonal nut with a diameter of more than 11 nm and a molecular weight of ca. 33 kDa was obtained in near-quantitative yield by mixing the two types of multi-terpyridine ligands with Fe²⁺. The supramolecular architecture was characterized by NMR (¹H and ¹³C), 2D NMR (COSY and ROESY), and DOSY spectroscopies, high-resolution electrospray ionization mass spectrometry, traveling-wave ion mobility mass spectrometry, and transmission electron microscopy.