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Microfluidic devices enable the production of uniform double emulsions with control over droplet size and shell thickness. However, the limited production rate of microfluidic devices precludes the use of monodisperse double emulsions for industrial-scale applications, which require large quantities of droplets. To increase throughput, devices can be parallelized to contain many dropmakers operating simultaneously in one chip, but this is challenging to do for double emulsion dropmakers. Production of double emulsions requires dropmakers to have both hydrophobic and hydrophilic channels, requiring spatially precise patterning of channel surface wettability. Precise wettability patterning is difficult for devices containing multiple dropmakers, posing a significant challenge for parallelization. In this paper, we present a multilayer dropmaker geometry that greatly simplifies the process of producing microfluidic devices with excellent spatial control over channel wettability. Wettability patterning is achieved through the independent functionalization of channels in each layer prior to device assembly, rendering the dropmaker with a precise step between hydrophobic and hydrophilic channels. This device geometry enables uniform wettability patterning of parallelized dropmakers, providing a scalable approach for the production of double emulsions. 

Droplet-based microfluidics is used to fabricate thin shell hydrogel microcapsules for the removal of methylene blue (MB) from aqueous solutions. The microcapsules composed of a poly(methacrylic acid) hydrogel shell exhibit unique properties, including permeation, separation, purification, and reaction of molecular species. Photocatalytic TiO 2 and ZnO nanoparticles encapsulated in the microcapsules, i.e. photocatalyst in capsule (PIC), are used to remove organic pollutants using an adsorption–oxidation mechanism. A prototype flow microreactor is assembled to demonstrate a controllable water purification approach in short time using photocatalysts. Our studies of aqueous and homogeneous hydrogel environments for the photocatalysts provide important insights into understanding the effectiveness of MB removal. Hydrogel capsules have MB removal rate comparable to homogeneous particles. Further reduction of both capsule and photocatalyst sizes can potentially aid in quicker water purification. 

Abstract Dynamic microcapsules are reported that exhibit shell membranes with fast and reversible changes in permeability in response to external stimuli. A hydrophobic anhydride monomer is employed in the thiol–ene polymerization as a disguised precursor for the acid‐containing shells; this enables the direct encapsulation of aqueous cargo in the liquid core using microfluidic fabrication of water‐in‐oil‐in‐water double emulsion drops. The poly(anhydride) shells hydrolyze in their aqueous environment without further chemical treatment, yielding cross‐linked poly(acid) microcapsules that exhibit trigger‐responsive and reversible property changes. The microcapsule shell can actively be switched numerous times between impermeable and permeable due to the exceptional mechanical properties of the thiol–ene network that prevent rupture or failure of the membrane, allowing it to withstand the mechanical stresses imposed on the capsule during the dynamic property changes. The permeability and molecular weight cutoff of the microcapsules can dynamically be controlled with triggers such as pH and ionic environment. The reversibly triggered changes in permeability of the shell exhibit a response time of seconds, enabling actively adjustable release profiles, as well as on‐demand capture, trapping, and release of cargo molecules with molecular selectivity and fast on‐off rates.