期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 136, 期 24, 页码 8577-8589出版社
AMER CHEMICAL SOC
DOI: 10.1021/ja413047r
关键词
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资金
- NSFC/China [21322206, 21132005, 91027005]
- Key Basic Research Project of Shanghai Science and Technology Commission [13JC1402200]
- Fok Ying Tung Education Foundation [131014]
- Program for Changjiang Scholars and Innovative Research Team in University
A new family of discrete hexakis-pillar[5]arene metallacycles with different sizes have been successfully prepared via coordination-driven self-assembly, which presented very few successful examples of preparation of discrete multiple pillar[n]arene derivatives. These newly designed hexakis-pillar[S]arene metallacycles were well characterized with one-dimensional (1-D) multinuclear NMR (H-1 and (31) P NMR), two-dimensional (2-D) H-1-H-1 COSY and NOESY, ESI-TOF-MS, elemental analysis, and PM6 semiempirical molecular orbital methods. Furthermore, the host-guest complexation of such hexakis-pillar[S]arene hosts with a series of different neutral ditopic guests G1-6 were well investigated. Through host-guest interactions of hexakis-pillar[5]arene metallacycles H2 or H3 with the neutral dinitrile guest G5, the cross-linked supramolecular polymers H2 superset of(G5)(3) or H3 superset of(G5)(3) were successfully constructed at the high-concentration region, respectively. Interestingly, these cross-linked supramolecular polymers transformed into the stable supramolecular gels upon increasing the concentrations to a relatively high level. More importantly, by taking advantage of the dynamic nature of metal ligand bonds and host-guest interactions, the reversible multiple stimuli-responsive gel-sol phase transitions of such polymer gels were successfully realized under different stimuli, such as temperature, halide, and competitive guest, etc. The mechanism of such multiple stimuli-responsive processes was well illustrated by in situ multinuclear NMR investigation. This research not only provides a highly efficient approach to the preparation of discrete multiple pillar[n]arene derivatives but also presents a new family of multiple stimuli-responsive smart soft matters.
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