Dissipative Interfacial Supramolecular Polymerization

Dissipative supramolecular assemblies are ubiquitous in natural biological systems, such as actin filaments and microtubules. Fully artificial dissipative supramolecular polymer (DSP) assemblies at interfaces having spatiotemporal control would provide an opportunity to mimic biological materials with unique, life-like properties. Producing DSPs at liquid–liquid interfaces, rather than in a bulk phase, remains a significant challenge. Here, we report the development of a DSP at the water–oil interface by coupling a chemical reaction network with orthogonal self-assembly based on host–guest interactions and metal–ligand coordination. The resulting interfacial DSP shows a controllable lifetime and can undergo depolymerization in response to redox or guest-competitive stimuli. Using interfacial tensiometry, the assembly mechanism, lifetime and responsiveness of DSPs was investigated. The binding energy of DSPs is sufficient to induce jamming at the liquid-liquid interface, enabling the formation of transient all-liquid constructs with reconfigurable and responsive properties. This work opens new opportunities to fabricate soft materials with programmable lifetime, responsiveness, reconfigurable and adaptive properties.