Journal
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
Volume 139, Issue 25, Pages 8639-8645Publisher
AMER CHEMICAL SOC
DOI: 10.1021/jacs.7b03635
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Funding
- URC
- University Grants Committee Areas of Excellence (AoE) [AoE/P-03/08]
- General Research Fund (GRF) grant from Research Grants Council of the Hong Kong Special Administrative Region, People's Republic of China [HKU 17334216]
- National Basic Research Program of China (973 Program) [2013CB834701]
- University Postdoctoral Fellowship
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Dinuclear alkynylplatinum(II) metallofoldamers with an oligomeric m-phenyleneethynylene backbone have been designed with the incorporation of a sterically undemanding, p-conjugated, and hydrophobic 2,6-bis(N-dodecylbenzimidazol-2'-yl)pyridine pincer ligand. The complex with the optimal chain length has been found to exhibit gelation behavior via stabilization by noncovalent Pt center dot center dot center dot Pt and pi-pi stacking interactions in the hierarchical architecture constructed from the single-turn helix. The chain lengths of the complexes have been found to be a critical determinant for their gelation behavior, conformations, and morphologies. Such a gelation process has been found to undergo a cooperative assembly mechanism according to the nucleation-elongation model. Their self-assembly via the Pt center dot center dot center dot Pt and pi-pi stacking interactions has been studied by H-1 NMR, 2D ROESY NMR (ROESY = rotating-frame Overhauser spectroscopy), electronic absorption, and emission spectroscopy, and density functional theory calculations have provided further insights into the folded state geometry of this class of metallofoldamers.
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