Chemically Fueled Interfacial Supramolecular Polymerization

Systems capable of dissipative self-assembly emulate the dynamic, adaptive behavior of biological systems, yet spatial control over this behavior remains a challenge. Here, we show how to generate chemically fueled supramolecular polymers at liquid-liquid interfaces by coupling a chemical reaction network with an orthogonal self-assembly based on host-guest interactions and metal-ligand coordination. Confinement to the interface yields readily tunable lifetimes for the polymers as well as an ability to undergo controlled depolymerization in response to stimuli, including redox cues or competitive guests. These polymers can jam at the interface enabling the generation of all-liquid constructs that are time-programmable and multistimuli responsive, providing a versatile platform for designing adaptive, out-of-equilibrium soft materials.