Gemini supra-amphiphiles with finely-controlled self-assemblies

Novel gemini supra-amphiphiles, [Mim-4-Mim][DBS]2 and [Mim-4-Mim][DS]2, were facilely constructed. A slight variation of building blocks can effectively modulate the driving forces for the fabrication of gemini supra-amphiphiles, thus leading to the fine control of subsequent self-assemblies. [Mim-4-Mim][DS]2, constructed via electrostatic attraction, tends to form micelles and hexagonal liquid crystals. Rich lamellar structures, including unilamellar and multilamellar vesicles, planar bilayers, and lamellar liquid crystals can be formed by [Mim-4-Mim][DBS]2, which is constructed through electrostatic and π–π stacking interactions. With increasing temperatures, [Mim-4-Mim][DBS]2 exhibits interesting phase separation in the La phase, behaving like common nonionic surfactants. The cross-linking between vesicles, where the “bola-type” [Mim-4-Mim]2+ cations act as the bridges, was found to promote the elongation of aggregates until the occurrence of phase separation.