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Nanoparticle‐shelled bubbles, prepared with glass capillary microfluidics, are functionalized to produce catalytic micromotors that exhibit novel assembly and disassembly behaviors. Stable microbubble rafts are assembled at an air–solvent interface of nonaqueous propylene carbonate (PC) solvent by creating a meniscus using a glass capillary. Upon the addition of hydrogen peroxide fuel, catalytic microbubbles quickly break free from the bubble raft by repelling from each other and self‐propelling at the air–fuel interface (a mixture of PC and aqueous hydrogen peroxide). While most of micromotors generate oxygen bubbles on the outer catalytic shell, some micromotors contain cracks and eject bubbles from the hollow shells containing air. Nanoparticle‐shelled bubbles with a high buoyancy force are particularly attractive for studying novel propulsion modes and interactions between catalytic bubble micromotors at air–fuel interfaces.

 

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.

 

Inhomogeneous microcapsules that can encapsulate various cargo for controlled release triggered by osmotic shock are designed and reported. The microcapsules are fabricated using a microfluidic approach and the inhomogeneity of shell thickness in the microcapsules can be controlled by tuning the flow rate ratio of the middle phase to the inner phase. This study demonstrates the swelling of these inhomogeneous microcapsules begins at the thinnest part of shell and eventually leads to rupture at the weak spot with a low osmotic pressure. Systematic studies indicate the rupture fraction of these microcapsules increases with increasing inhomogeneity, while the rupture osmotic pressure decreases linearly with increasing inhomogeneity. The inhomogeneous microcapsules are demonstrated to be impermeable to small probe molecules, which enables long‐term storage. Thus, these microcapsules can be used for long‐term storage of enzymes, which can be controllably released through osmotic shock without impairing their biological activity. The study provides a new approach to design effective carriers to encapsulate biomolecules and release them on‐demand upon applying osmotic shock.

 

The suppression of lithium dendrite is critical to the realization of lithium metal batteries. 3D conductive framework, among different approaches, has shown very promising results in dendrite suppression. A novel cost‐effective and versatile dip‐coating method is presented here to make 3D conductive framework. Various substrates with different geometries are coated successfully with copper, including electrically insulating glass fiber (GF) or rice paper and conducting Ni foam. In particular, the as‐prepared copper coated GF shows promising results to serve as the lithium metal substrate by the electrochemical battery tests. The method significantly broadens the candidate materials database for 3D conductive framework to include all kinds of intrinsically insulating 3D substrates.

 

Although the utilization of rigid particles can afford stable emulsions, some applications require eventual emulsion destabilization to release contents captured in the particle-covered droplet. This destabilizing effect is achieved when using stabilizers that respond to controlled changes in environment. Microgels can be synthesized as stimuli responsive polymeric gel networks that adsorb to oil/water interfaces and stabilize emulsions. These particles are commonly hydrogels that swell and collapse in water in response to environmental changes. However, amphiphilic functionality is desired to enhance the adsorption abilities of these hydrogels while maintaining their stimuli responsivity. Microfluidic techniques are used to synthesize Janus microgels with two opposing stimuli responsive hemispheres. The particles have a temperature responsive domain connected to a pH responsive network where each side changes its hydrophilicity in response to a change in temperature or pH, respectively. The Janus microgels are amphiphilic in acidic conditions at 19 °C and alkaline conditions at 40 °C, while the opposite conditions cause a reduction of the amphiphilicity. By stabilizing emulsions with these dual responsive microgels, “smart” droplets that respond to environmental cues are formed. Emulsion droplets remain stable with smaller diameters when aqueous solution conditions favor amphiphilic particles yet, coalesce to larger droplets upon changing pH or temperature. These responsive Janus microgels represent the advancing technology of responsive droplets and demonstrate the applicability of microgels as emulsion stabilizers. 

Quantification of cell-secreted molecules, e.g. , cytokines, is fundamental to the characterization of immune responses. Cytokine capture assays that use engineered antibodies to anchor the secreted molecules to the secreting cells are widely used to characterize immune responses because they allow both sensitive identification and recovery of viable responding cells. However, if the cytokines diffuse away from the secreting cells, non-secreting cells will also be identified as responding cells. Here we encapsulate immune cells in microfluidic droplets and perform in-droplet cytokine capture assays to limit the diffusion of the secreted cytokines. We use microfluidic devices to rapidly encapsulate single natural killer NK-92 MI cells and their target K562 cells into microfluidic droplets. We perform in-droplet IFN-γ capture assays and demonstrate that NK-92 MI cells recognize target cells within droplets and become activated to secrete IFN-γ. Droplet encapsulation prevents diffusion of secreted products to neighboring cells and dramatically reduces both false positives and false negatives, relative to assays performed without droplets. In a sample containing 1% true positives, encapsulation reduces, from 94% to 2%, the number of true-positive cells appearing as negatives; in a sample containing 50% true positives, the number of non-stimulated cells appearing as positives is reduced from 98% to 1%. After cells are released from the droplets, secreted cytokine remains captured onto secreting immune cells, enabling FACS-isolation of populations highly enriched for activated effector immune cells. Droplet encapsulation can be used to reduce background and improve detection of any single-cell secretion assay. 

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.