Highly productive droplet formation by anisotropic elongation of a thread flow in a microchannel

We developed a microfluidic device to form monodisperse droplets with high productivity by anisotropic elongation of a thread flow, defined as a threadlike flow of a dispersed liquid phase in a flow of an immiscible, continuous liquid phase. The thread flow was anisotropically elongated in the depth direction in a straight microchannel with a step, where the microchannel depth changed. Consequently, the elongated thread flow was given capillary instability (Rayleigh-Plateau instability) and was continuously transformed into monodisperse droplets at the downstream area of the step in the microchannel. We examined the effects of the flow rates of the dispersed phase and the continuous phase on the droplet formation behavior, including the droplet diameter and droplet formation frequency. The droplet diameter increased as the fraction of the dispersed-phase flow rate relative to the total flow rate increased and was independent of the total flow rate. The droplet formation frequency proportionally increased with the total flow rate at a constant dispersed-phase flow rate fraction. These results are explained in terms of a mechanism similar to that of droplet formation from a cylindrical liquid thread flow by Rayleigh-Plateau instability. The microfluidic device described was capable of forming monodisperse droplets with a 160-microm average diameter and 3-microm standard deviation at a droplet formation frequency of 350 droplets per second from a single thread flow. The highest total flow rate achieved was 6 mL/h using the present device composed of a straight microchannel with a step. We also demonstrated parallel droplet formation by anisotropic elongation of multiple thread flows; the process was applied to form W/O and O/W droplets. The highly productive droplet formation process presented in this study is expected to be useful for future industrial applications.     

Formation of droplets and bubbles in a microfluidic T-junction-scaling and mechanism of break-up

This article describes the process of formation of droplets and bubbles in microfluidic T-junction geometries. At low capillary numbers break-up is not dominated by shear stresses: experimental results support the assertion that the dominant contribution to the dynamics of break-up arises from the pressure drop across the emerging droplet or bubble. This pressure drop results from the high resistance to flow of the continuous (carrier) fluid in the thin films that separate the droplet from the walls of the microchannel when the droplet fills almost the entire cross-section of the channel. A simple scaling relation, based on this assertion, predicts the size of droplets and bubbles produced in the T-junctions over a range of rates of flow of the two immiscible phases, the viscosity of the continuous phase, the interfacial tension, and the geometrical dimensions of the device.     

Thixotropy in Native Petroleum Emulsions

Native water in crude oil emulsions, stabilized by indigenous surfactants, exhibit both positive thixotropy (PT) and negative thixotropy (NT) in Couette flow. PT is associated with microscopic processes, local break-up of droplet clusters in emulsions with low and moderate volume fractions of water φ, or fracturing of emulsion-gels with φ > 0.7. The latter process involves the coalescence of water droplets along a fracture plain, which results in vorticity banding of emulsion flow. NT reflects evolution of the macroscopic radial banding in flow of emulsions with 0.18 < φ < 0.58 and is dictated by the displacement of the interface between the sheared and unsheared regions.     

Prediction of emulsion particle sizes using a computational fluid dynamics approach

For many food products emulsification processes play an important role. Examples are ice cream, spreads, sauces, etc. As is well known, droplet break-up and coalescence phenomena are the local processes underlying the control of particle size in an emulsion process. Quite a number of studies have generated scaling laws which can be easily applied and which are useful in the design of a process. However, the prediction of particle sizes in an inhomogeneous flow, where the flow velocity is changing spatially in strength and direction and with time, is not yet well established. For one-phase flows computational fluid dynamics (CFD) methodologies are in use to predict details on the flow with quite some success. This methodology has been extended to capture the dispersed phase in an efficient way. The essence is that break-up and coalescence processes determine source terms in a transport equation for the moments of the particle size distribution, while velocity vectors as obtained in the one-phase CFD simulation determine the convective term. This method allows particle size prediction in any equipment. The approach is illustrated for the particle size evolution of an oil-in-water emulsion, for a phase-separated biopolymeric mixture (a so-called water-in-water emulsion) and for the escape of the included oil droplets from a double emulsion of the type oil-in-water-in-oil. In all cases experimental results are compared with simulation results, which match very well. This shows the strength of the method.     

The role of the surfactant head group in the emulsification process: binary (nonionic-ionic) surfactant mixtures

Dilute emulsions of dodecane in water were prepared under constant flow rate conditions with binary surfactant systems. The droplet size distribution was measured as a function of the mixed surfactant composition in solution. The systems studied were (a) the mixture of anionic sodium dodecyl sulfate (SDS) with nonionic hexa(ethyleneglycol) mono n-dodecylether (C12E6) and (b) the mixture of cationic dodecyl pyridinium chloride (DPC) with C12E6. At a constant concentration of SDS or DPC surfactant in solution (below the CMC) the mean emulsion droplet size decreases with the increase in the amount of C12E6 added to the solution. However, a sharp break of this droplet size occurs at a critical concentration and beyond this point the mean droplet size did not significantly change upon further increase of the C12E6. This point was found to corresponded to the CMC of the mixed surfactant systems (as previously determined from microcalorimetry measurements) and this result suggested the mixed adsorption layer on the emulsion droplet was similar to the surfactant composition on the mixed micelles. The emulsion droplet size as a function of composition at the interface was also studied. The mean emulsion droplet size in SDS-C12E6 solution was found to be lower than that in DPC-C12E6 system at the equivalent mole fraction of ionic surfactant at interface. This was explained by the stronger interactions between sulphate and polyoxyethylene head groups at the interface, which facilitate the droplet break-up. Counterion binding parameter (beta) was also determined from zeta-potential of dodecane droplets under the same conditions and it was found that (beta) was independent of the type of the head group and the mole fraction of ionic surfactant at interface.     

Shear mixing and phase diagram shift of polymer blends

For a low molecular weight polystyrene/polybutadiene blend, the effect of shear on the suppressing of critical fluctuations and the critical temperature has been studied and is in good agreement with the predictions of Onuki and Kawasaki. By assuming the symmetry of this critical scaling into the two phase region, together with the Taylor theory, the observed (phase separated) droplet break-up and the formation of string pattern can be explained. The exact shear dependence of T_c(γ) can be obtained by the use of the fluorescence microscope under steady shear.     

Efficient Generation of Microdroplets Using Tail Breakup Induced with Multi-Branch Channels

In recent years, research on the application of microdroplets in the fields of biotechnology and chemistry has made remarkable progress, but the technology for the stable generation of single-micrometer-scale microdroplets has not yet been established. In this paper, we developed an efficient and stable single-micrometer-scale droplet generation device based on the fragmentation of droplet tails, called “tail thread mode”, that appears under moderate flow conditions. This method can efficiently encapsulate microbeads that mimic cells and chemical products in passively generated single-micrometer-scale microdroplets. The device has a simple 2D structure; a T-junction is used for droplet generation; and in the downstream, multi-branch channels are designed for droplet deformation into the tail. Several 1–2 µm droplets were successfully produced by the tail’s fragmentation; this continuous splitting was induced by the branch channels. We examined a wide range of experimental conditions and found the optimal flow rate condition can be reduced to one-tenth compared to the conventional tip-streaming method. A mold was fabricated by simple soft lithography, and a polydimethylsiloxane (PDMS) device was fabricated using the mold. Based on the 15 patterns of experimental conditions and the results, the key factors for the generation of microdroplets in this device were examined. In the most efficient condition, 61.1% of the total droplets generated were smaller than 2 μm.     

Investigating the effects of precursor concentration and gelling parameters on droplet-based generation of Ca-Alginate microgels: identifying new stable modes of droplet formation

Droplet-based microfluidics is an attractive approach for producing microgels due to its high potential to control the size and shape of the particles and precisely entrap the substances within the hydrogel matrix. However, the microfluidic generation of monodisperse microgels with desired structures is still challenging. Indeed, the rheological and interfacial properties of the immiscible fluids, as well as the adopted gelling strategy, play important roles in microfluidic methods. Herein, sodium alginate droplets with different concentrations are generated via a microfluidic device with a flow-focusing unit. Besides, a combined in situ and ex situ strategy is optimized to crosslink sodium alginate droplets in the presence of calcium ions. The effects of alginate concentration and junction width in the flow focusing unit are investigated on droplet size and droplet formation regimes. It is observed that by increasing the alginate concentration, the dripping regime of droplet formation may be transformed to one of the binary dripping or quasijetting regimes. In the binary dripping regime, two successive different-sized droplets are generated in each period of droplet formation, which leads to low monodispersity in the collected droplets. However, the droplets produced in the quasijetting regime are interestingly monodisperse and also smaller than those of the dripping and binary dripping regimes. The breakup dynamics of the alginate thread is also analyzed with a computational fluid dynamics (CFD) code. This analysis discloses that the viscous stresses, as well as the viscous dissipation, have important roles in controlling the stable modes of droplet formation.     

Wire-Arc Spray Modeling

A model is presented describing the details of the wire-arc spray process. The model consists of several submodels each treating a different part of the process. A compressible flow model describes the supersonic nozzle flow upstream of the wire tips. The arc is described by a 3-D arc in cross-flow model using different boundary conditions for the cathode and the anode boundary. The resulting temperature and velocity contours serve as upstream boundary for a 2-D turbulent jet model. Particle generation and acceleration is described by treating the initial droplet formation for the anode and the cathode wire separately and then using the resulting particle size and velocity distributions in a secondary break-up model. Comparison with some experimental results show acceptable agreement. This modeling approach may be used for optimization of wire-arc spray equipment.     

Numerical simulation of deformation behavior of droplet in gas under the electric field and flow field coupling

The water droplets in the process of electrostatic coalescence are important when studying electrohydrodynamics. In the present study, the electric field and flow field are coupled through the phase field method based on the Cahn–Hilliard formulation. A numerical simulation model of single droplet deformation under the coupling field was established. It simulated the deformation behavior of the movement of a droplet in the continuous phase and took the impact of droplet deformation into consideration which is affected by two-phase flow velocity, electric field strength, the droplet diameter, and the interfacial tension. The results indicated that under the single action of the flow field, when the flow velocity was lower, the droplet diameter was greater as was the droplet deformation degree. When the flow velocity was increased, the droplet deformation degree of a small-diameter droplet was at its maximum size, the large-diameter droplet had a smaller deformation degree, and the middle-diameter droplet was at a minimum deformation degree. When the flow velocity was further increased, the droplet diameter was smaller, and the droplet deformation degree was greater. Under the coupled effect of the electric field and flow field, the two-phase flow velocity and the electric field strength were greater, and the degree of droplet deformation was greater. While the droplet diameter and interfacial tension were smaller, the degree of droplet deformation was greater. Droplet deformation degree increased along with the two-phase flow velocity. The research results provided a theoretical basis for gas–liquid separation with electrostatic coalescence technology.     

Field-induced textures of polymer-dispersed chiral liquid crystal microdroplets

We have microscopically observed the textures of very large droplets of cholesteric liquid crystal in a polymer matrix under the influence of an electric field E. When E = 0, the droplets exhibit rings and often a disclination line extends from the centre to the periphery of the droplet. As E increases, the droplet undergoes a progressive transition to a uniform-appearing texture. This uniform region first occurs near the centre of the droplet, then increases in radius as the field is increased. We propose that the field-off texture corresponds to the Frank-Pryce spherulite model while the uniform field-on texture is the planar texture.     

Dynamics of Splat Formation in Plasma Spray Coating Process

The paper describes recent developments in modeling formation of plasma spray coatings. Specific attention is paid to the three-dimensional simulation of droplet impact and solidification under plasma spraying conditions. It is shown that the extent of maximum spread is primarily determined by the Reynolds number and, to a lesser degree, by the Weber number. Splashing and break-up is shown to be the result of solidification; fluid instabilities do not play a significant role in this regard. Finally, the effect of solidification on droplet spreading is insignificant when the ratio of Stefan number to Prandtl number is much smaller than unity.     

Fast on-demand droplet fusion using transient cavitation bubbles

A method for on-demand droplet fusion in a microfluidic channel is presented using the flow created from a single explosively expanding cavitation bubble. We test the technique for water-in-oil droplets, which are produced using a T-junction design in a microfluidic chip. The cavitation bubble is created with a pulsed laser beam focused into one droplet. High-speed photography of the dynamics reveals that the droplet fusion can be induced within a few tens of microseconds and is caused by the rapid thinning of the continuous phase film separating the droplets. The cavitation bubble collapses and re-condenses into the droplet. Droplet fusion is demonstrated for static and moving droplets, and for droplets of equal and unequal sizes. Furthermore, we reveal the diffusion dominated mixing flow and the transport of a single encapsulated cell into a fused droplet. This laser-based droplet fusion technique may find applications in micro-droplet based chemical synthesis and bioassays.     

Microfluidic separation of satellite droplets as the basis of a monodispersed micron and submicron emulsification system

Emulsions are widely used to produce sol-gel, drugs, synthetic materials, and food products. Recent advancements in microfluidic droplet emulsion technology has enabled the precise sampling and processing of small volumes of fluids (picoliter to femtoliter) by the controlled viscous shearing in microchannels. However the generation of monodispersed droplets smaller than 1 microm without surfactants has been difficult to achieve. Normally, the generation of satellite droplets along with parent droplets is undesirable and makes it difficult to control volume and purity of samples in droplets. In this paper, however, several methods are presented to passively filter out satellite droplets from the generation of parent droplets and use these satellite droplets as the source for monodispersed production of submicron emulsions. A passive satellite droplet filtration system and a dynamic satellite droplet separation system are demonstrated. Satellite droplets are filtered from parent droplets with a two-layer channel geometry. This design allows the creation and collection of droplets that are less than 100 nm in diameter. In the dynamic separation system, satellite droplets of defined sizes can be selectively separated into different collecting zones. The separation of the satellite droplets into different collecting zones correlates with the cross channel position of the satellite droplets during the breakup of the liquid thread. The delay time for droplets to switch between the different alternating collecting zones is nominally 1 min and is proportional to the ratio of the oil shear flows. With our droplet generation system, monodispersed satellite droplets with an average radius of 2.23 +/- 0.11 microm, and bidispersed secondary and tertiary satellite droplets with radii of 1.55 +/- 0.07 microm and 372 +/- 46 nm respectively, have been dynamically separated and collected.     

Field-induced textures of polymer-dispersed chiral liquid crystal microdroplets

Abstract

We have microscopically observed the textures of very large droplets of cholesteric liquid crystal in a polymer matrix under the influence of an electric field E. When E = 0, the droplets exhibit rings and often a disclination line extends from the centre to the periphery of the droplet. As E increases, the droplet undergoes a progressive transition to a uniform-appearing texture. This uniform region first occurs near the centre of the droplet, then increases in radius as the field is increased. We propose that the field-off texture corresponds to the Frank-Pryce spherulite model while the uniform field-on texture is the planar texture.     

Plateau Rayleigh instability simulation

The well-known phenomena of Plateau-Rayleigh instability has been simulated using computational fluid dynamics (CFD). The breakup of a liquid film into an array of droplets on a cylindrical element was simulated using a volume-of-fluid (VOF) solver and compared to experimental observations and existing theory. It is demonstrated that the VOF method can correctly predict the breakup of thins films into an array of either axisymmetric droplets or clam-shell droplets, depending on the surface energy. The existence of unrealistically large films is precluded. Droplet spacing was found to show reasonable agreement with theory. Droplet motion and displacement under fluid flow was also examined and compared to that in previous studies. It was found that the presence of air flow around the droplet does not influence the stable film thickness; however, it reduces the time required for droplet formation. Novel relationships for droplet displacement were derived from the results.     

Formation and Release of Cobalt(II) Sorption and Precipitation Products in Aging Kaolinite-Water Slurries

A comprehensive simulation of the coarsening mechanism coalescence-induced coalescence (CIC) is developed to predictthe growth rate of inviscid droplets in a viscous matrix fluid. In CIC, the shape relaxations of coalescing droplets establish flow fields that drive other droplets into contact, thus creating a cascade of coalescence events. It is believed that CIC is responsible for droplet growth in some demixed polymer solutions, such as isotactic polypropylene (iPP) and diphenyl ether (DPE). A cascade of coalescence events is simulated using a three-dimensional molecular dynamics-like simulation of a dispersed two-phase isopycnic fluid system. The coalescence-induced flow is driven mostly by the strong gradients in curvature at the neck of a coalescing pair of droplets, and the flow is modeled analytically by approximating it as due to a ring of point forces. The resultant velocity of each droplet in the suspension is calculated by superimposing all of the coalescence-induced flow fields and applying Faxen's Law. The mean droplet size grows like t(xi), where t is the coarsening time and xi a growth exponent that increases with increasing minority phase volume fraction varphi. Good agreement with experimental values of xi (0.22/=0.23. It is also shown that the droplet size distribution broadens for semidilute suspensions (varphi/=0.54). A phenomenological kinetic theory of coalescence is proposed. It is believed that in nondilute emulsions, CIC can account for coarsening that has been attributed previously to more traditional coalescence mechanisms. Copyright 2000 Academic Press.     

Polymer particles with various shapes and morphologies produced in continuous microfluidic reactors

We report a novel approach to continuous and scalable production of core-shell droplets and polymer capsules in microfluidic devices. The described method is also useful in the synthesis of polymer particles with nonspherical shapes. We used capillary instability-driven break-up of a liquid jet formed by two immiscible fluids. Precise control of emulsification of each liquid allowed for the production of highly monodisperse core-shell droplets with a predetermined diameter of cores and thickness of shells. We also achieved control over the number of cores per droplet and the location of cores in the droplet. We carried out fast throughput photopolymerization of the monomeric shells and obtained polymer particles with various shapes and morphologies, including spheres, truncated spheres and, hemispheres, and single and multicore capsules.     

芳香共聚酯B-N多种向列织构的形态研究

从一种聚芳酯B-N得到了丝状(包括细丝和粗丝)、纹影状和大理石纹状等与小分子向列液晶相似的多种织构。由于样品淬火后晶片装饰在织构上而不影响分子取向矢的分布,因而可以用化学刻蚀和电镜技术揭示其向错和取向矢图。电镜和光学显微镜的结果相互补充,表明了细丝和粗丝状织构的分子取向矢分布很不相同,是两种不同的织构,而粗化始于第二熔融降温。在这些向列织构中分别发现了S=±(1/2)和s=+1的向错的例子和平面内微区转向壁的证据。     

Analysis of the microfluid flow in an evaporating sessile droplet

The axisymmetric time-dependent flow field in an evaporating sessile droplet whose contact line is pinned is studied numerically and using an analytical lubrication theory with a zero-shear-stress boundary condition on the free surface of the droplet at low capillary and Reynolds numbers. A finite element algorithm is developed to solve simultaneously the vapor concentration and flow field in the droplet under conditions of slow evaporation. The finite element solution confirms the accuracy of the lubrication solution, especially when terms of higher order in the droplet flatness ratio (the ratio of droplet height to radius, h/R) are included in the lubrication theory to account more accurately for the singular flow near the contact line.