The design of supramolecular nanostructures is of great importance, as self-assembly allows the production of a variety of structures for applications, such as carrier systems, sensors, or transducers. In particular, potential lies in assemblies that can respond to external triggers. Recently we have introduced an approach to electrostatic self-assembly for the formation of supramolecular particles in solution: polyelectrolytes and multivalent stiff organic counterions build well-defined and stable nano-objects. In addition to electrostatics, secondary interactions between counterions such as π-π-stacking directs the association. Aggregates with narrow size distribution and varying shape such as spheres, cylinders, vesicles and networks result. pH-responsive assemblies can be repeatedly switched “on” and “off” because either macroion or counterion respond to pH with a change in charge status.
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