Supramolecular\nComplex Surfactants and Structured\nLiquids Enabled by Cation‑π and Charge-Transfer Interactions

Cation-π and charge-transfer (CT) interactions\nare pervasive\nwith significant implications in the fields of chemistry, materials\nscience, and biology. However, much less is known about the construction\nof interfacial assemblies based on the two interactions. Here, by\ncombining cation-π and CT interactions between an acceptor molecule,\ndicationic naphthalenediimide, and an aromatic donor, pyrene-terminated\npoly-l-lactic acid, we report the generation of supramolecular\ncomplex surfactants (SCSs) in situ at the toluene–water interface.\nThe utilization of SCSs as building blocks enables the fabrication\nof interfacial assemblies including 2D films, emulsions, and structured\nliquids. By modification of the redox state of the acceptor molecules\nunder chemical stimulus, the association/assembly and dissociation/disassembly\nof SCSs can be precisely regulated, imparting intriguing redox-responsive\nproperties to the resulting assemblies.