Controlling Self-Assembly Mechanisms through Rational Molecular Design in Oligo(p-phenyleneethynylene)-Containing Alkynylplatinum(II) 2,6-Bis(N-alkylbenzimidazol-2′-yl)pyridine Amphiphiles

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Abstract
The systematic control over association mechanisms of self-assembled materials has been demonstrated through the rational design and synthesis of a series of amphiphilic dinuclear alkynylplatinum(II) bzimpy (bzimpy = 2,6-bis(N-alkylbenzimidazol-2′-yl)pyridine) complexes containing the shape-persistent oligo(p-phenyleneethynylene)s. Multistage morphological transformations from plates to fibers and to spherical nanostructures under different solvent compositions have been demonstrated. The subtle balances between multiple noncovalent interactions including Pt···Pt, hydrophobic, hydrophilic, and π–π stacking interactions are found to have profound impact on the supramolecular assembly of the system, in which a change in the association mechanism from isodesmic to cooperative and back to isodesmic growth has been observed upon increasing hydrophilicity of the complexes.
Funding Information
  • Research Grants Council, University Grants Committee (HKU 17334216)
  • University of Hong Kong
  • University Research Committee, University of Hong Kong
  • University Grants Committee (AoE/P-03/08)

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