Vertical Assembly of Giant Double- and Triple-Decker Spoked Wheel Supramolecular Structures

Die Liu; Mingzhao Chen; Yiming Li; Yixian Shen; Jian Huang; Xiaoyu Yang; Zhilong Jiang; Xiaopeng Li; George R Newkome; Pingshan Wang

doi:10.1002/anie.201809819

Vertical Assembly of Giant Double- and Triple-Decker Spoked Wheel Supramolecular Structures

Angew Chem Int Ed Engl. 2018 Oct 22;57(43):14116-14120. doi: 10.1002/anie.201809819. Epub 2018 Oct 4.

Authors

Die Liu¹, Mingzhao Chen², Yiming Li³, Yixian Shen², Jian Huang², Xiaoyu Yang², Zhilong Jiang^{1

2}, Xiaopeng Li³, George R Newkome^{4

5}, Pingshan Wang^{1

2}

Affiliations

¹ Key Laboratory for Water Quality and Conservation, of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou, 510006, China.
² College of Chemistry and Chemical Engineering, Central South University, Changsha, 410083, China.
³ Department of Chemistry, University of South Florida, Tampa, FL, 33640, USA.
⁴ Departments of Polymer Science and Chemistry, University of Akron, Akron, OH, 44325-4717, USA.
⁵ Center for Molecular Biology and Biotechnology, Florida Atlantic University, 5353 Parkside Dr., Jupiter, FL, 33458, USA.

Abstract

The double- or triple-decker 3D metallo-hexagons were obtained by self-assembly of multitopic tris-terpyridines with Cd²⁺ ions in near-quantitative yield. Comprising up to 72 ionic pairs, the multiple spoked wheels display characteristic reversible gelation properties under thermodynamic conditions. The supramolecular metallo-nanoarchitectures were characterized by ¹ H NMR, 2D NMR (COSY and NOESY), and diffusion-ordered spectroscopy (DOSY) and HR-ESI-MS, traveling-wave ion mobility mass spectrometry (TWIM-MS), TEM, and AFM. For the first time, the self-assembly of 45 units at once was demonstrated to yield exceptional giant triple-decker hexagons of up to circa 42 000 Da.

Keywords: coordination; gelation; molecular spoked wheels; self-assembly; terpyridine.

Grants and funding

R01 GM128037/GM/NIGMS NIH HHS/United States