Liquid–Liquid Encapsulation: Penetration vs. Trapping at a Liquid Interfacial Layer

Encapsulation protects vulnerable cores in an aggressive environment and imparts desirable functionalities to the overall encapsulated cargo, including control of mechanical properties, release kinetics, and targeted delivery. Liquid-liquid encapsulation to create such capsules, where a liquid layer (shell) is used to wrap another liquid (core), is an attractive value proposition for ultrafast encapsulation (∼100 ms). Here, we demonstrate a robust framework for stable liquid-liquid encapsulation. Wrapping is achieved by simple impingement of a target core (in liquid form) on top of an interfacial layer of another shell-forming liquid floating on a host liquid bath. Poly(dimethylsiloxane) (PDMS) is chosen as the shell-forming liquid due to its biocompatibility, physicochemical stability, heat curability, and acceptability as both a drug excipient and food additive. Depending on the kinetic energy of the impinging core droplet, encapsulation is accomplished by either of the two pathways─necking-driven complete interfacial penetration and subsequent generation of encapsulated droplets inside the host bath or trapping inside the interfacial layer. Combining thermodynamic argument with experimental demonstration, we show that the interfacially trapped state, which results in a low kinetic energy of impact, is also an encapsulated state where the core droplet is wholly enclosed inside the floating interfacial layer. Therefore, despite being impact-driven, our method remains kinetic energy independent and minimally restrictive. We describe the underlying interfacial evolution behind encapsulation and experimentally identify a nondimensional regime of occurrence for the two pathways mentioned above. Successful encapsulation by either path offers efficient long-term protection of the encased cores in aggressive surroundings (e.g., protection of honey/maple syrup inside a water bath despite their miscibility). We enable the generation of multifunctional compound droplets via interfacial trapping, where multiple core droplets with different compositions are encapsulated within the same wrapping shell. Further, we demonstrate the practical utility of the interfacially trapped state by showing successful heat-curing of the shell and subsequent extraction of the capsule. The cured capsules are sufficiently robust and remain stable under normal handling.