Chemically Triggered Coalescence and Reactivity of Droplet Fibers.

We describe the role of functional polymer surfactants in the construction and triggered collapse of droplet-based fibers and the use of these macroscopic supracolloidal structures for reagent compartmentalization. Copolymer surfactants containing both zwitterionic and tertiary amine pendent groups were synthesized for stabilization of oil-in-water droplets, in which the self-adherent properties of the selected zwitterions impart interdroplet adherence, while the amine groups provide access to pH-triggered coalescence. Macroscopic fibers, obtained by droplet extrusion, were prepared with reagents embedded in spatially distinct components of the fibers. Upon acidification of the continuous aqueous phase, protonation of the polymer surfactants increases their hydrophilicity and causes rapid fiber disruption and collapse. Cross-linked versions of these supracolloidal fibers were stable upon acidification and appeared to direct interdroplet passage of encapsulants along the fiber length. Overall, these functional, responsive emulsions provide a strategy to impart on-demand chemical reactivity to soft materials structures that benefits from the interfacial chemistry of the system.