Multiple-Responsive Hierarchical Self-Assemblies of a Smart Supramolecular Complex: Regulation of Noncovalent...

We herein report a smart amphiphilic supramolecular complex ([MimA-EDA-MimA]@[DBS]₂) with stimuli-responsive self-assembly, constructed by 3-(3-formyl-4-hydroxybenzyl)-1-methylimidazolium chloride (MimACl), sodium dodecyl benzene sulfonate (SDBS), and ethylenediamine (EDA). The self-assembly of [MimA-EDA-MimA]@[DBS]₂ shows triple-sensitivities in response to pH, concentration, and salt. At a low pH, only micelles are formed, which can transform into vesicles spontaneously when the pH increases to 11.8. Vesicles can gradually fuse into vesicle clusters and elongated assemblies with increasing concentration of [MimA-EDA-MimA]@[DBS]₂. Chainlike aggregates, ringlike aggregates, or giant vesicles can be formed by adding inorganic salts (i.e., NaCl and NaNO₃), which could be derived from the membrane fusion of vesicles. The noncovalent interactions, including π-π stacking, hydrogen bonding, and electrostatic interactions, were found to be responsible for the topology evolution of assemblies. Thus, it provides an opportunity to construct smart materials through the regulation of the role of noncovalent interactions in self-assembly.