PEG-in-PDMS drops stabilised by soft silicone skins as a model system for elastocapillary emulsions with explicit morphology control.

Hypothesis: The morphology of ordinary macro-emulsions is controlled by their high interfacial energies, i.e., by capillarity, leading to well-known structural features which can be tuned only over a narrow range. We claim here that a more explicit control over a much wider range of morphologies can be obtained by producing "elastocapillary emulsions" in which interfacial elasticity acts simultaneously with interfacial tension.

Experiments: We develop a model-system composed of PEG-in-PDMS emulsions, in which a catalyst diffuses from the PEG drops into the silicone matrix containing two reactive silicone polymers, which are cross-linked in a non-reactive silicone matrix to form a silicone gel of controlled thickness and mechanical properties on the drop surface. We characterise the cross-linking process of the gel in bulk and at the interface, and we analyse the skin growth kinetics. We then use the obtained understanding to produce emulsions with controlled elastocapillary interfaces using in-flow-chemistry in a purpose-designed millifluidic circuit.

Findings: We show that this approach allows to create interfaces over the full range of elastocapillary properties, and that very different emulsion morphologies can be generated depending on whether capillarity or elasticity dominates. These findings advance our fundamental understanding of the morphology of emulsions with complex interfaces, and they are of importance for the design of polymerised High Internal Phase Emulsions (polyHIPEs) with original structure/property relations. They will also be useful for the design of silicone capsules with fine-tuned mechanical properties.