This paper presents a method to form micron-sized droplets in an aqueous two-phase system (ATPS) and to subsequently polymerize the droplets to produce hydrogel beads. Owing to the low interfacial tension in ATPS, droplets do not easily form spontaneously. We enforce the formation of drops by perturbing an otherwise stable jet that forms at the junction where the two aqueous streams meet. This is done by actuating a piezo-electric bending disc integrated in our device. The influence of forcing amplitude and frequency on jet breakup is described and related to the size of monodisperse droplets with a diameter in the range between 30 and 60 μm. Rapid on-chip polymerization of derivatized dextran inside the droplets created monodisperse hydrogel particles. This work shows how droplet-based microfluidics can be used in all-aqueous, surfactant-free, organic-solvent-free biocompatible two-phase environment.

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This paper studies the Rayleigh-Plateau instability for co-flowing immiscible aqueous polymer solutions in a microfluidic channel. Careful vibration-free experiments with controlled actuation of the flow allowed direct measurement of the growth rate of this instability. Experiments for the well-known aqueous two phase system (ATPS, or aqueous biphasic systems) of dextran and polyethylene glycol solutions exhibited a growth rate of 1 s(-1), which was more than an order of magnitude slower than an analogous experiment with two immiscible Newtonian fluids with viscosities and interfacial tension that closely matched the ATPS experiment. Viscoelastic effects and adhesion to the walls were ruled out as explanations for the observed behavior. The results are remarkable because all current theory suggests that such dilute polymer solutions should break up faster, not slower, than the analogous Newtonian case. Microfluidic uses of aqueous two phase systems include separation of labile biomolecules but have hitherto be limited because of the difficulty in making droplets. The results of this work teach how to design devices for biological microfluidic ATPS platforms.

Catalyst-assisted self-assembly is widespread in nature to achieve spatial control over structure formation. Reported herein is the formation of hydrogel micropatterns on catalytic surfaces. Gelator precursors react on catalytic sites to form building blocks which can self-assemble into nanofibers. The resulting structures preferentially grow where the catalyst is present. Not only is a first level of organization, allowing the construction of hydrogel micropatterns, achieved but a second level of organization is observed among fibers. Indeed, fibers grow with their main axis perpendicular to the substrate. This feature is directly linked to a unique mechanism of fiber formation for a synthetic system. Building blocks are added to fibers in a confined space at the solid-liquid interface.