Dual-Redox Responsive Interfaces Based on Donor–Acceptor Interactions

Nanoparticle surfactant (NPS) is a highly competitive means for stabilizing liquid-liquid interfaces, endowing interfacial assemblies with functionalities, and enabling the construction of all-liquid devices. Integrating different types of supramolecular interactions into NPSs would open possibilities to generate interfaces that are responsive to multiple stimuli. Here, by using donor-acceptor interactions between polydopamine nanoparticles (PDA NPs) and methyl viologen (MV²⁺) terminated polystyrene, the formation, assembly, and jamming of a supramolecular NPS at the water-toluene interface is demonstrated. Harnessing the redox properties of both catechol and MV²⁺, the dual-redox responsiveness can be achieved, allowing the reconfiguration of NPS-based structured liquids. Using NPS as an emulsifier, oil-in-water (O/W), water-in-oil (W/O), and oil-in-water-in-oil (O/W/O) Pickering emulsions can be obtained in one step, which exhibit smart responsiveness to redox reagents. Taking advantage of the adsorption capacity of PDA NPs, the purification of dye-polluted water can be achieved through O/W Pickering emulsions. We envision that this unique dual-redox responsive biphasic system would hold great potential for developing sophisticated controlled-release systems as well as other intelligent, functional materials.