Responsive Interfacial Assemblies Based on Charge-Transfer Interactions

Charge transfer (CT) interactions have been widely used to construct supramolecular systems, such as functional nanostructures and gels. However, to date, there is no report on the generation of CT complexes at the liquid-liquid interface. Here, by using an electron-deficient acceptor dissolved in water and an electron-rich donor dissolved in oil, we present the in situ formation and assembly of CT complex surfactants (CTCSs) at the oil-water interface. With time, CTCSs can assemble into higher-order nanofilms with exceptional mechanical properties, allowing the stabilization of liquids and offering the possibility to structure liquids into nonequilibrium shapes. Moreover, due to the redox-responsiveness of the electron-deficient acceptor, the association and dissociation of CTCSs can be reversibly manipulated in a redox process, leading to the switchable assembly and disassembly of the resultant constructs.

Automated summary

Charge transfer interactions are commonly used in constructing supramolecular systems, but the formation of CT complexes at the liquid-liquid interface has not been reported until now. By utilizing electron-deficient acceptors in water and electron-rich donors in oil, CT complex surfactants can be formed and assembled at the oil-water interface, ultimately leading to the creation of higher-order nanofilms with exceptional mechanical properties. The redox-responsiveness of the electron-deficient acceptor allows for reversible manipulation of the assembly and disassembly of CTCSs, offering the potential for switchable structures in liquids.