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A non-dimensional parameter (ζ) for prediction of double emulsion formation mode as a function of the capillary numbers of all fluids and device geometry was developed and its critical values were determined using simulation and experimental data. At logζ>5.7, drops were formed in dripping mode; the widening jetting occurred at 5

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A novel microfluidic mixing strategy was developed and used to prepare polyvinylpyrrolidone (PVP) capped gold nanoparticles (AuNPs). In this process, 1 mM tetrachloroauric acid (HAuCl4) stream containing 1% (w/v) PVP was injected through the inner capillary tube and mixed with 20 mM L-ascorbic acid solution delivered co-currently through the outer coaxial capillary. The reaction mixture was hydrodynamically flow focused by the environmentally friendly oil Miglyol 840 delivered from the opposite side of the outer capillary, which resulted in the generation of reaction droplets in a tapered collection tube. The reactants were rapidly mixed within droplets by internal circulating flows induced by hydrodynamic interactions of fluids inside the droplets with the carrier oil. The size of the prepared AuNPs was measured by both dynamic light scattering and transmission electron microscopy and was found to decrease with decreasing the droplet size and increasing the difference in velocity between the two reactant streams, which improved mixing efficiency within droplets. The smallest nanoparticles were obtained when the outlet section of the injection tube was positioned at the entry section of the collection tube due to the highest shear at the liquid interface. The carrier oil formed a hydrophobic barrier between the droplets and the reactor walls preventing deposition of the synthesised particles. As a result, the size of the AuNPs was smaller than in the co-flow mixer operated with two continuous reactant streams.

Emulsions formed by mixing reactant streams inside microdroplets are efficient microscale reactors for the synthesis of nano/microparticles/crystals due to small quantities of reagents confined within each droplet and the separation of droplet contents from the reactor walls. In this work, the synthesis of size-tunable gold nanoparticles (AuNPs) within emulsion droplets generated in a three-phase glass capillary microfluidic device was investigated experimentally and numerically using computational fluid dynamics (CFD). AuNPs were produced by micromixing two aqueous streams, 1.15 mM HAuCl 4 containing the 1% poly(vinylpyrrolidone) capping agent and 20 mM ascorbic acid solutions, inside monodispersed droplets created by three-dimensional (3D) counter-current flow focusing in a medium-chain triglyceride. The mean particle size of AuNPs was tunable in the range between 26 and 56 nm and depended on the degree of premixing of the reactant streams shortly before droplet generation, and the mixing efficiency within droplets, which was controlled by hydrodynamic conditions within the microfluidic device. The CFD results were compared and validated against experimental observations and revealed the presence of a recirculation zone near the outer wall of the injection capillary tip. The mixing efficiency was higher at smaller droplet size causing a reduction in the particle size of the AuNPs.

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