Delivery Systems for Low Molecular Weight Payloads: Core/Shell Capsules with Composite Coacervate/Polyurea Membranes

Composite polyurea/coacervate core/shell capsules are formed by coupling associative biopolymer phase separation with interfacial polymerization. They combine the excellent chemical stability of synthetic polymer barriers with the strong adhesive properties of protein‐based complex coacervates, inspired by biological underwater glues. To encapsulate volatile oil droplets, a primary coacervate hydrogel capsule is formed by a protein and weak polyanion and is reinforced with a polyurea membrane synthesized in situ at the interface between the coacervate and the oil core. The polyurea layer provides an excellent permeability barrier against diffusion of small volatile molecules while the coacervate portion of the shell enhances adhesion on the targeted substrate.