Chemical Fuel-Driven Dissipative Supramolecular Polymerization at a Liquid-Liquid Interface

Dissipative supramolecular materials play a key role in life and biological systems, such as microtubules and actin filaments. During the process of supramolecular polymerization, the assembly is often controlled by the kinetics of system, leading to a kinetically trapped out-of-equilibrium state. Formation of dissipative supramolecular polymers (DSPs), are good candidates to construct man-made living materials. However, these DSPs are usually prepared in solution, which require similar solubility of monomers, and severely limit the development of DSPs. Here, by integrating orthogonal dynamic interactions, we develop a strategy to generate DSPs at a liquid-liquid interface with chemical fuels. When the fuel is consumed, the supramolecular polymer chains disassociate gradually, leading to the destruction of the nonequilibrium state. Using interfacial tensiometry, the assembly mechanism, lifetime and responsiveness of DSPs is studied. Additionally, the binding energy of DSPs is sufficient to jam at the liquid-liquid interface, offering ability to generate transient all liquid constructs with reconfigurability and responsiveness. This work opens new opportunities to fabricate soft materials with controlled lifetime, responsiveness, reconfigurable and adaptive properties.