Parallelised production of fine and calibrated emulsions by coupling flow-focusing technique and partial wetting phenomenon

The capacity of microfluidic technology to fabricate monodisperse emulsion droplets is well established. Parallelisation of droplet production is a prerequisite for using such an approach for making high-quality materials for either fundamental or industrial applications where product quantity matters. Here, we investigate the emulsification efficiency of parallelised drop generators based on a flow-focusing geometry when incorporating the role of partial wetting in order to make emulsion droplets with a diameter below 10 μm. Confinement intrinsically encountered in microsystems intensifies the role played by interfaces between liquids and solids. We thus take advantage of partial wetting to enhance the maximum confinement accessible due to liquid flow focusing. We compare the performances brought by partial wetting to more established routes such as step emulsification. We show that the step configuration and the partial wetting regime are both well suited for being parallelised and thus open the way to the production of fine and calibrated emulsions for further applications. Finally, this new route of emulsification that exploits partial wetting between the fluids and the channel walls opens possibilities to the formation of substantially smaller droplets, as required in many fields of application.     

Formation of Microdroplets in Liquids Utilizing Active Pneumatic Choppers on a Microfluidic Chip

Monodispersed emulsions are of great significance for a variety of applications. The current study reports a new microfluidic system capable of formation of microdroplets in liquids for emulsification applications. This new emulsion chip can precisely generate uniform droplets using a novel combination of hydrodynamic-focusing and liquid-chopping techniques. Experimental data show that microdroplets with diameters ranging from 6 to 100 mum with a variation less than 3% can be precisely generated. The size of the droplets is tunable using three approaches including adjusting the relative sheath/sample flow velocity ratios, the applied air pressure and the applied chopping frequency. Moreover, focusing and chopping of multiple flows has been demonstrated to increase the emulsion process throughput     

On-demand double emulsification utilizing pneumatically actuated,selectively surface-modified PDMS micro-devices

This article presents an active, two-step emulsification scheme that is capable of producing double emulsions with desired geometries and compositions on demand. Three-layer PDMS micro-devices with pneumatically actuated membrane-valves constructed on top of specially designed fluidic-channels are utilized to meter and shape immiscible fluids into double emulsions. By intermittently squeezing a fluid into another one, controlled emulsification is realized, and successive emulsification steps result in the formation of multiple emulsions. In the prototype demonstration, a three-layer PDMS molding and bonding process was employed to fabricate the proposed microfluidic devices, whose channel surfaces were selectively modified into hydrophilic by a photo-grafting process. A governing computer program cooperating with a set of control hardware was employed to coordinate the actuation of the prototype system. It has been demonstrated that: (1) both water-in-oil-in-oil and water-in-oil-in-water double emulsions can be produced; (2) the sizes of inner aqueous droplets and outer oil drops can be controlled independently; and (3) adjacent oil drops with varying overall sizes, and both diameters and numbers of inner aqueous droplets can be produced on demand. As such, the demonstrated emulsification scheme could potentially fulfill the real-time controllability on emulsion formation, which is desired for a variety of chemical and biological applications.     

Y- and T-junction microfluidic devices: effect of fluids and interface properties and operating conditions

Water-in-oil emulsions were produced in microchannels with Y- and T-junction geometries by individual droplet generation. For each microchannel configuration, the effect of the fluids and interface properties as well as of the process conditions was evaluated. The size of the droplets depended mainly on the relative velocity between continuous and dispersed phases and the relative fluid viscosity between phases. Those variables were related to the shear stress between the phases, which caused the droplet detachment. In addition, the interfacial forces played a minor role in Y-junction, and they had no effect in the droplets formation in T-junction microchannels. In Y-junction, a large variation in the droplet size was observed, depending on the system composition and the operating conditions. At low relative velocity and fluid viscosity, no droplets were generated. In contrast, the process in T-junction resulted in a lower variation of droplets size and the droplets were formed even at less favorable conditions. Such results indicate that the knowledge of the mechanism of droplets generation in each microchannel geometry makes it possible to choose the appropriate configuration according to the type of fluid, and the operating conditions can be adjusted to obtain the desired final emulsion.     

Micro-droplet formation in non-Newtonian fluid in a microchannel

Micro-droplet formation from an aperture with a diameter of micrometers is numerically investigated under the cross-flow conditions of an experimental microchannel emulsification process. The process involves dispersing an oil phase into continuous phase fluid through a microchannel wall made of apertured substrate. Cross-flow in the microchannel is of non-Newtonian nature, which is included in the simulations. Micro-droplets of diameter 0.76–30 μm are obtained from the simulations for the apertures of diameter 0.1–10.0 μm. The simulation results show that rheology of the bulk liquid flow greatly affects the formation and size of droplets and that dispersed micro-droplets are formed by two different breakup mechanisms: in dripping regime and in jetting regime characterized by capillary number Ca. Relations between droplet size, aperture opening size, interfacial tension, bulk flow rheology, and disperse phase flow rate are discussed based on the simulation and the experimental results. Data and models from literature on membrane emulsification and T-junction droplet formation processes are discussed and compared with the present results. Detailed force balance models are discussed. Scaling factor for predicting droplet size is suggested.     

Microchannel emulsification for mass production of uniform fine droplets: integration of microchannel arrays on a chip

We present a novel microchannel emulsification (MCE) system for mass-producing uniform fine droplets. A 60 × 60-mm MCE chip made of single-crystal silicon has 14 microchannel (MC) arrays and 1.2 × 10⁴ MCs, and each MC array consists of many parallel MCs and a terrace. A holder with two inlet through-holes and one outlet through-hole was also developed for simply infusing each liquid and collecting emulsion products. The MCE chip was sealed well by physically attaching it to a flat glass plate in the holder during emulsification. Uniform fine droplets of soybean oil with an average diameter of 10 μm were reliably generated from all the MC arrays. The size of the resultant fine droplets was almost independent of the dispersed-phase flow rate below a critical value. The continuous-phase flow rate was unimportant for both the droplet generation and the droplet size. The MCE chip enabled mass-producing uniform fine droplets at 1.5 ml h⁻¹ and 1.9 × 10⁹ h⁻¹, which could be further increased using a dispersed phase of low viscosity.     

Formation of satellite droplets in flow-focusing junctions: volume and neck rupture

This work focuses on the rupture of the neck of a main droplet, leading to the formation of satellite droplets in a flow-focusing junction. The size of these satellites is determined by image analysis. Emphasis is given to the influence of viscosity and rheological behaviour of the fluids, using both Newtonian and non-Newtonian fluids as continuous phases. The scaling of the size of the satellite droplet with the capillary number of the continuous phase shows two different areas separated by a critical capillary number of 10^?2. Below this critical capillary number, the size of satellites hardly changes. Above this critical value, the size of the droplet increases almost linearly with the capillary number. This critical value appears also as a difference in shape of the rupture of the neck of the droplet for Newtonian continuous fluids: symmetrical for low capillary numbers and asymmetrical rupture of the neck of the droplet for higher capillary numbers. The higher the viscosity ratio (viscosity of dispersed phase/viscosity of continuous phase), the bigger is the main satellite droplet. For more viscous dispersed phases, numerous satellite droplets can be formed. When the continuous phase is non-Newtonian (polyacrylamide solutions) the number of satellites droplets is even higher and their sizes are found interdependent according to a cascade scenario.     

Scale-up and control of droplet production in coupled microfluidic flow-focusing geometries

A single microfluidic chip consisting of six microfluidic flow-focusing devices operating in parallel was developed to investigate the feasibility of scaling microfluidic droplet generation up to production rates of hundreds of milliliters per hour. The design utilizes a single inlet channel for both the dispersed aqueous phase and the continuous oil phase from which the fluids were distributed to all six flow-focusing devices. The exit tubing for each of the six flow-focusing devices is separate and individually plumbed to each device. Within each flow-focusing device, the droplet size was monodisperse, but some droplet size variations were observed across devices. We show that by modifying the flow resistance in the outlet channel of an individual flow-focusing device it is possible to control both the droplet size and frequency of droplet production. This can be achieved through the use of valves or, as is done in this study, by changing the length of the exit tubing plumbed to the outlet of the each device. Longer exit tubing and larger flow resistance is found to lead to larger droplets and higher production frequencies. The devices can thus be individually tuned to create a monodisperse emulsion or an emulsion with a specific drop size distribution.     

Multi-helical micro-channels for rapid generation of drops of water in oil

High throughput generation of microscopic mono-dispersed droplets of one liquid into the continuous flow of another is important for large number of engineering and biomedical applications. However, meeting conflicting demands of both uniformity of size and high rate of droplet generation have been a difficult task to be accomplished in conventional systems. We have attempted to address this problem by designing a novel multi-helical micro-channel which we have used to generate water droplets in a continuous flow of oil. The channel consists of three or more helical flow paths joined along their contour length forming a single channel with inherently asymmetric geometry. Helix angle and radius are found to be two additional geometric parameters which influence different drop break-up regimes. We have shown that both time period of generation of drops and the droplet size can be minimized by suitably altering the helix angle. A scaling law has been derived to rationalize these results.     

Preparation of monodispersed oil-in-water emulsions through semi-metal microfluidic EDGE systems

EDGE (Edge-based Droplet GEneration) emulsification systems with the ability to produce multiple droplets simultaneously from a single nozzle, were used for the preparation of monodispersed oil-in-water emulsions. The devices (with plateau height of 1 µm) were coated with metals (Cu, CuNi and CuNi/Cu) and had different surface roughness and wettability properties. This influenced the emulsification behavior significantly. The large surface roughness of the CuNi/Cu coated system resulted in stronger non-uniform filling of the plateau as compared to the smoother surfaces of Cu and less rough CuNi, and less droplet formation points in the CuNi/Cu coated system relative to the Cu and CuNi systems. The less hydrophilic CuNi surface, however, provided wider pressure stability than the more hydrophilic Cu and CuNi/Cu surface. A narrower pressure stability (Cu surface) and lower number of droplet formation points (CuNi/Cu surface) resulted in lower overall droplet formation frequency when compared with CuNi system. All metal coated EDGE systems reliably produced monodispersed droplets (with sizes being 6 times the plateau height), similar to the silicon-based EDGE systems having much smoother surfaces. The pressure stability for CuNi coated surfaces was wider, while the droplet formation frequency was comparable to that with the silicon system. This indicated that the use of metal is not a limitation in these systems as initially expected, but may be used for more robust and productive emulsification systems, which lend themselves well for scale-out to practical productivity rates.     

Capillary and electrostatic limitations to the contact angle in electrowetting-on-dielectric

The shape of a conducting liquid droplet placed on a hydrophobic dielectric surface is simulated numerically by solving the Laplace–Young capillary equation. The electric force, acting on the conducting surface, distorts the droplet shape leading to a change in the apparent contact angle; its variation is compared with a theoretical Young–Lippman prediction. At sufficiently large values of voltage, applied to the droplet, the numerical algorithm fails to converge, which is interpreted as the break-up of the droplet surface with small droplets being ejected from the surface. These highly charged droplets, as well as any other electric charges near the triple contact line, generated for example by the electric corona discharge, cause a change of the distribution of the electric forces. This effect can be helpful in explaining saturation of the apparent contact angle: an appropriately selected surface charge near the contact line can completely stop droplet distortion, and the contact angle variation, despite the increased droplet voltage. Furthermore, the simulation results show the effect of the permittivity of the medium surrounding the droplet, on the contact angle variation.     

Investigation of viscosity effect on droplet formation in T-shaped microchannels by numerical and analytical methods

Both numerical and analytical models have been developed to explore the viscosity effect of the continuous phase on drop formation at a T-shaped junction in immiscible liquids. The effects of the generalized power law coefficient, the power law exponent and the yield stress on the mechanism of drop breakup, final drop size and frequency of drop formation are studied by using the numerical three-dimensional volume of fluid model. Droplets coalescence in Bingham fluids is observed in the beginning transient period. The effect of yield stress on drop extension is also discussed. Predictions of drop size by using an analytical force balance show satisfactory agreement with simulation results for Newtonian and power law fluids with different viscosity ratios. The approximation error associated with the analytical model for Bingham fluids is also acceptable. This analytical model can greatly shorten the prediction time as compared with the numerical model, which is helpful for on-line control.     

Effect of geometry on droplet formation in the squeezing regime in a microfluidic T-junction

In the surface tension-dominated microchannel T-junction, droplets can be formed as a result of the mixing of two dissimilar, immiscible fluids. This article presents results for very low Capillary numbers and different flow rates of the continuous and dispersed phases. Through three-dimensional lattice Boltzmann-based simulations, the mechanism of the formation of “plugs” in the squeezing regime has been examined and the size of the droplets quantified. Results for Re_\textc << 1 Re_{\text{c}} \ll 1 show the dependence of flow rates of the two fluids on the length of the droplets formed, which is compared with existing experimental data. It is shown that the size of plugs formed decreases as the Capillary number increases in the squeezing regime. This article clearly shows that the geometry effect, i.e., the widths of the two channels and the depth of the assembly, plays an important role in the determination of the length of the plugs, a fact that was ignored in earlier experimental correlations.     

Monodisperse droplets by impinging flow-focusing

We proposed a new flow-focusing technique for generation of monodisperse femtoliter droplets, based on the capillary micro-cross. A funnel-shaped interface of two phase system is observed in a capillary cross for mass production of uniform drops, where a tapered exit orifice is extruded into the dispersed feeding capillary. The droplets, down to 2 μm in size at frequency of 20 kHz, are controllable in size when choosing orifice and capillary sizes, as well as flow rates of inner and outer fluids. For a specific diameter of exit orifice, there is a maximal flow rate of outer fluid, beyond which the interface will be penetrated. Until then, the interface is in steady state and all droplets are highly uniform (<3%), implicating an absolute instability in the whole process.     

Formation of fully closed microcapsules as microsensors by microfluidic double emulsion

Microcapsules templated from microfluidic double emulsions attract a great attention due to their broad new potential applications. We present a method to form transparent polymer microcapsules in small sizes of ~30 μm with aqueous cores and fully closed shells. We controlled the size ratio of the aqueous core to the polymer shell not only by flow rates of the double emulsions, but also by synergetic interaction between surfactants at the interface of immiscible fluids. We also found that fully closed shells can be formed by generating the double emulsion droplets in a jetting regime, in which the aqueous cores are confined centrally in the double emulsion droplets. We demonstrated the formation of barcodes in these microcapsules for multiplexed bioassays. These transparent microcapsules also have wide and high potentials for the development of various microsensors by functionalizing the liquid-state cores with compounds sensitive and responsive to temperature, light or electromagnetic field.     

Monodispersed water-in-oil emulsions prepared with semi-metal microfluidic EDGE systems

Monodispersed water-in-oil emulsions were prepared with EDGE (Edge based Droplet GEneration) systems, which generate many droplets simultaneously from one junction. The devices (with plateau height of 1.0 μm) were coated with Cu and CuNi having the same hydrophobicity but different surface roughness. Emulsification was performed by using water as dispersed phase and oils with different viscosities (hexadecane, decane, hexane and sunflower oil) as continuous phases; lecithin, polyglycerol polyricinoleate (PGPR) and span80 were used as emulsifiers. The roughness affected the emulsification behaviour significantly. The smoother Cu surface exhibited droplet formation over the entire length of the droplet formation unit, while the rougher CuNi surface showed non-uniform filling of the plateau and much lower droplet formation frequency. In spite of this different behaviour, monodispersed droplets (CV <10 %) were produced by both systems (with span80 and PGPR), with a size six times the plateau height (d _avg ≈ 6.0 μm). The droplet size decreased with increasing viscosity ratio and remained constant above some critical value. The emulsification process was stable over a wider range of pressures as previously found for silicon-based systems. The amount of PGPR influenced the pressure stability, but the system could be used effectively, while with lecithin and span80 the stable pressure range was very small. The pressure and viscosity stability of these semi-metal systems with rough surfaces show that the EDGE system has potential for practical applications, especially since overall productivity is not affected.     

Guiding of emulsion droplets in microfluidic chips along shallow tracks defined by laser ablation

We demonstrate controlled guiding of nanoliter emulsion droplets of polar liquids suspended in oil along shallow hydrophilic tracks fabricated at the base of microchannels located within microfluidic chips. The tracks for droplet guiding are generated by exposing the glass surface of polydimethylsiloxane (PDMS)-coated microscope slides via femtosecond laser ablation. The difference in wettability of glass and PDMS surfaces together with the shallow step-like transverse topographical profile of the ablated tracks allows polar droplets wetting preferentially the glass surface to follow the track. In this study, we investigate guiding of droplets of two different polar liquids (water/ethylene glycol) with and without surfactant suspended in an oil medium along surface tracks of different depths of 1, 1.5, and 2 \(\upmu\)m. The results of experiments are also verified with computational fluid dynamics simulations. Guiding of droplets along the tracks as a function of the droplet composition and size and the surface profile depth is evaluated by analyzing the trajectories of moving droplets with respect to the track central axis, and conditions for stable guiding are identified. The experiments and numerical simulations indicate that while the track topography plays a role in droplet guiding using 1.5- and 2-\(\upmu\)m deep tracks, for the case of the smallest track depth of 1 \(\upmu\)m, droplet guiding is mainly caused by surface energy modification along the track rather than the presence of a topographical step on the surface. Our results can be exploited to sort passively different microdroplets mixed in the same microfluidic chip, based on their inherent wetting properties, and they can also pave the way for guiding of droplets along reconfigurable tracks defined by surface energy modifications obtained using other external control mechanisms such as electric field or light.     

Continuous generation of hydrogel beads and encapsulation of biological materials using a microfluidic droplet-merging channel

In this paper, we describe a method for encapsulation of biomaterials in hydrogel beads using a microfluidic droplet-merging channel. We devised a double T-junction in a microfluidic channel for alternate injection of aqueous fluids inside a droplet unit carried within immiscible oil. With this device, hydrogel beads with diameter <100 μm are produced, and various solutions containing cells, proteins and reagents for gelation could merge with the gel droplets with high efficiency in the broad range of flow rates. Mixing of reagents and reactions inside the hydrogel beads are continuously observed in a microchannel through a microscope. By enabling serial injection of each liquid with the dispersed gel droplets after they are produced from the oil-focusing channel, the device simplifies the sample preparation process, and gel-bead fabrication can be coupled with further assay continuously in a single channel. Instantaneous reactions of enzyme inside hydrogel and in-situ formation of cell-containing beads with high viability are demonstrated in this report.     

Droplet Formation Utilizing Controllable Moving-Wall Structures for Double-Emulsion Applications

The formation of microscale single- and double-emulsion droplets with various sizes is crucial for a variety of industrial applications. In this paper, we report a new microfluidic device which can actively fine-tune the size of single- and double-emulsion droplets in liquids by utilizing controllable moving-wall structures. Moreover, various sizes of external and internal droplets for double emulsions are also successfully formed by using this device. Three pneumatic side chambers are placed at a T-junction and flow-focusing channels to construct the controllable moving-wall structures. When compressed air is applied to the pneumatic side chambers, the controllable moving-wall structures are activated, thus physically changing the width of the microchannels. The size of the internal droplets at the intersection of the T-junction channel is then fine-tuned due to the increase in the shear force. Then, the internal droplets are focused into a narrow stream hydrodynamically and finally chopped into double-emulsion droplets using another pair of moving-wall structures downstream. For single emulsions, oil-in-water droplets can be actively fine-tuned from 50.07 to 21.80 under applied air pressures from 10 to 25 psi with a variation of less than 3.53%. For a water-in-oil single emulsion, droplets range from 50.32 to 14.76 with a variation of less than 4.62% under the same applied air pressures. For double emulsions, the sizes of the external and internal droplets can be fine-tuned with external/internal droplet diameter ratios ranging from 1.69 to 2.75. The development of this microfluidic device is promising for a variety of applications in the pharmaceutical, cosmetics, and food industries.     

An investigation on the mechanism of droplet formation in a microfluidic T-junction

This paper reports the findings of a numerical investigation on the droplet break-up in a microfluidic T-junction. The numerical flow visualization of the droplet formation process is validated with the experimental flow visualization. From the computational results, we show that the pressure profile of the dispersed phase and the continuous phase in the squeezing regime changes as the droplet break-up process proceeds. The assumption taken by other researchers that the dispersed phase pressure profile, during the droplet formation process at a T-junction, remains constant and only the continuous phase pressure changes according to the blockage of the channel is proved to be invalid. We provide new insights on the pressure difference between the dispersed phase and the continuous phase during the droplet break-up process and show that the minimum pressure difference happens at the last moment of the droplet break-up and not during the second and third stage of the droplet formation mechanism in the squeezing regime as suggested by other researchers.