Abstract

AbstractThe interfacial jamming of nanoparticle surfactants offers the possibility of structuring liquids and fabricating all‐liquid constructs with advanced functionality. However, less attention has been given to structured liquids with multiple responsiveness. Here, we show a novel, yet highly simplified nanoparticle surfactant model, pillar[6]arene (PA[6]) surfactant, by taking advantage of the host–guest interactions between a water‐soluble PA[6] and an oil‐soluble ligand, ferrocenium terminated polystyrene. PA[6] surfactants form rapidly at the oil–water interface, assemble into an elastic film with excellent mechanical strength, and when jammed, offer a “solid‐like” assembly to lock‐in highly nonequilibrium shapes of the liquids. The interfacial assembly/jamming and disassembly/unjamming of PA[6] surfactants can be controlled by chemical redox or competitive guest reagents, endowing the structured liquids with redox or guest‐competitive responsiveness.

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