Microchannel Emulsification Using Stainless‐Steel Chips: Oil Droplet Generation Characteristics

The first stainless‐steel microchannel (MC) emulsification chips with grooved MC arrays, each consisting of uniform‐sized parallel channels and a terrace, were developed. These chips enabled successful spontaneous‐transformation‐based generation of uniformly sized droplets of soybean oil and silicone oil. As for the influence of the dispersed‐phase velocity in a channel, the critical velocity below which uniform‐sized droplets were obtained from the channels depended on the interfacial tension between two phases. The maximum productivity of uniform‐sized oil droplets for the stainless‐steel MC emulsification chips was estimated to be several milliliters per hour. An adapted capillary number that considers the wettability of the dispersed phase of two different oils could be useful for understanding the flow state of the dispersed phase during droplet generation.     

Preparation of monodispersed emulsion with large droplets using microchannel emulsification

Microchannel (MC) emulsification is a novel technique for producing monodispersed emulsions with coefficients of variation of less than 5%. To produce emulsions with large droplets, we designed three MC with large dimensions. The MC structure consists of two parts: a channel and a terrace. Terrace length was defined as the length from the exit of the MC to the end of the terrace. The MC plates used in this study have deeper channels and longer terraces. The size limit of droplets prepared by MC emulsification was studied. Monodispersed emulsions with droplets as large as 100 μm were prepared using an MC with a depth of 16 μm and a terrace length of 240 μm. The average diameter (coefficient of variation) of the emulsion droplets was 98.1 μm (2.5%). Emulsions with larger-diameter droplets were prepared using an MC with a longer terrace. The effect of the applied pressure on emulsification behavior was studied and discussed from the viewpoint of the droplet formation mechanism. At low applied pressures, droplet diameters were independent of the applied pressure, and monodispersed emulsions were produced. The pressure ranges of constant droplet diameter for large-droplet emulsions were narrower than those for the 5 to 30 μm droplet size emulsions because interfacial tension is more significant on a smaller scale compared with the other forces.     

Effect of emulsifiers on the preparation of food‐grade oil‐in‐water emulsions using a straight‐through extrusion filter

This paper describes the preparation characteristics of food‐grade soybean oil‐in‐water (O/W) emulsions using a novel straight‐through extrusion filter, named a silicon straight‐through microchannel (MC). Polyglycerol fatty acid ester (PGFE), polyoxyethelene sorbitan monolaurate (Tween 20), and sucrose fatty acid ester were tested as emulsifiers. Optical observations of the emulsification process exhibited that monodisperse oil droplets were stably formed from an oblong straight‐through MC for PGFE and Tween 20. The effect of the emulsifier on the straight‐through MC emulsification behavior is discussed. The selected PGFE‐ and Tween 20‐containing systems enabled us to prepare monodisperse O/W emulsions with droplet diameters of 38—39 μm and coefficients of variation below 3% using an oblong straight‐through MC with a 16 μm‐equivalent channel diameter.     

正弦型微通道内液-液两相流型及流动特性实验研究

采用实验的方法对不混溶的液液两相流体在不同入口结构下的正弦微通道(直通道正弦、波峰正弦和波中正弦)内液滴的流动特性进行了分析。硅油作为离散相,含有0.5% SDS的蒸馏水作为连续相,观测到弹状流、滴状流和射状流。分析了两相流动参数及不同的微通道入口结构对流型和液滴长度的影响。流型受微通道入口结构影响较大,波峰正弦微通道能够生成最大范围的稳定的流型。液滴长度随离散相体积流量和离散相与连续相体积流量之比的增大而增大,随连续相的体积流量和毛细数的增大而降低。微通道入口结构对液滴长度有影响,直通道的正弦微通道内液滴长度最短,更有利于液滴的形成。三种通道生成的液滴中,最大的液滴尺寸是最小的液滴尺寸的1.15~1.39倍,但正弦流动段对液滴速度几乎没有影响。     

Production of quasi-monodisperse emulsions with large droplets using a micromachined device

The development and operation of a modified method for the preparation of quasi-monodisperse (CV<16%) emulsions are reported. The device uses a microfabricated-nozzle (MN) array, produced by micromachining technology, to achieve a higher rate of emulsification [76.8 m³/(m²·h)] than previously reported for microchannel (MC) emulsification methods. The dispersed phase is extruded into a continuous phase through the MN, and the emulsions droplets are formed by viscous drag force of the continuous phase. The droplet diameter decreased with an increase in the flow velocity and viscosity in the continuous phase, which was explained by the theoretical model. The range of droplet diameters produced (130 to 370 μm) was larger than in previously reported MC emulsification, membrane emulsification, and shear-rupturing methods.     

Optimal design of drainage channel geometry parameters in vane demister liquid–gas separators

Vane liquid–gas demisters are widely used as one of the most efficient separators. To achieve higher liquid disposal and to avoid flooding, vanes are enhanced with drainage channels. In this research, the effects of drainage channel geometry parameters on the droplet removal efficiency have been investigated applying CFD techniques. The observed parameters are channel angle, channel height and channel length. The gas phase flow field was determined by the Eulerian method and the droplet flow field and trajectories were computed applying the Lagrangian method. The turbulent dispersion of the droplets was modeled using the discrete random walk (DRW) approach. The CFD simulation results indicate that by applying DRW model, the droplet separation efficiency predictions for small droplets are closer to the corresponding experimental data. The CFD simulation results showed that in the vane, enhanced with drainage channels, fewer low velocity sectors were observed in the gas flow field due to more turbulence. Consequently, the droplets had a higher chance of hitting the vane walls leading to higher separation efficiency. On the other hand, the parameters affect the liquid droplet trajectory leading to the changes in separation efficiency and hydrodynamic characteristic of the vane. To attain the overall optimum geometry of the drainage channel, all three geometry parameters were simultaneously studied employing 27 CFD simulation cases. To interpolate the overall optimal geometry a surface methodology method was used to fit the achieved CFD simulation data and finally a polynomial equation was proposed.     

CHARACTERISTICS OF MICROMETER AND SUBMICROMETER SIZE O/W EMULSIONS PRODUCED BY RAMOND SUPERMIXER®

A novel motionless mixer named the Ramond Supermixer® (RSM®) was employed to produce O/W emulsions composed of micrometer and submicrometer-size droplets. Liquid paraffin as dispersed phase, aqueous sucrose solution as continuous phase, and anionic sodium dodecyl sulfate as emulsifying agent were used as the model emulsification system. Pressure drop, droplet size distribution, Sauter mean diameter (d₃₂), and geometric standard deviation of the droplet size distribution (σ_g) were investigated under the various combinations of process variables; superficial liquid velocity, number of mixing units, number of passages through RSM®, dispersed phase viscosity (η_d), continuous phase viscosity (η_c), and dispersed phase volume fraction. Different modes of droplet size variations with process variables were obtained, with respect to micrometer- and submicrometer-size ranges, and theoretical explanations are forwarded. For the micrometer-size range, maximum droplet diameter (d_max) was proportional to d₃₂. For the submicrometer-size range, d_max varied with d₃₂ in the range of 1.53-2.19-fold, and a correlation is proposed with K (=η_d/η_c); d₃₂ and σ_g were well correlated with the process variables. Furthermore, a semi-empirical mechanistic model was developed for the formation of droplets obtained under inertial sub-range to interpret the effect of process variables.     

Morphology development during blending of immiscible polymers in screw extruders

The present work reports evolution of morphology from initial (presence of striation) to final (droplet formation) stages in a single‐screw extruder. Morphology development during the blending process controls the final size of the dispersed phase, which in turn significantly affects the properties of the blends. The experiments were carried out using a 70/30 wt% polypropylene/ethylene vinyl acetate (PP/EVA) blend; samples were collected along the length of the screw, by screw pullout experiment, to analyze the size and size distribution of the dispersed phase present both as striated layers and subsequently as droplets. Average size of the dispersed phase and standard deviation were taken into account to monitor the morphology evolution along the length of the screw. Pre‐breakup morphology development was studied by analyzing the sample collected from the feed zone of the extruder in terms of upper and lower layers along the cross section of screw channel. Examination of micrographs revealed the existence of pattern of ordered striations along the length of the melting zone containing striations from average size of 1000 μm down to 50 μm decreasing rapidly along the length of the screw. The breakup process was captured at the start of compression zone where step‐up in the shear as well as elongational flow was applied due to decrease in the channel depth along the compression zone. The observed droplet size formed by the breakup of filaments is found to be in accordance with theory. The final droplet size is found to be governed by the emulsification process occurring as a result of stretching, breakup and coalescence in the metering section of the screw and is in the order of 2 μm.     

Computational fluid dynamics model of viscous droplet breakup

A computational fluid dynamics (CFD) model is being developed to help guide the design of equipment to enhance viscous droplet breakup. The first generation model was able to show qualitative agreement with experimental results. This 2D model follows a single droplet (with a specified initial diameter) flowing past a series of cylinders using a volume of fluid (VOF) method to track the interface. The model is able to predict droplet breakup and provide insights into the physics of the breakup process. Three different breakup mechanisms are hypothesized that help explain experimental observations, including a minimum in breakup efficacy (ability to create smaller droplets) versus velocity data. Important parameters include the system rheology, velocity, cylinder size versus droplet size, and cylinder layout.     

CHARACTERISTICS OF MICROMETER AND SUBMICROMETER SIZE O/W EMULSIONS PRODUCED BY RAMOND SUPERMIXER®

A novel motionless mixer named the Ramond Supermixer® (RSM®) was employed to produce O/W emulsions composed of micrometer and submicrometer-size droplets. Liquid paraffin as dispersed phase, aqueous sucrose solution as continuous phase, and anionic sodium dodecyl sulfate as emulsifying agent were used as the model emulsification system. Pressure drop, droplet size distribution, Sauter mean diameter (d ₃₂), and geometric standard deviation of the droplet size distribution (σ_g) were investigated under the various combinations of process variables; superficial liquid velocity, number of mixing units, number of passages through RSM®, dispersed phase viscosity (η_d), continuous phase viscosity (η_c), and dispersed phase volume fraction. Different modes of droplet size variations with process variables were obtained, with respect to micrometer- and submicrometer-size ranges, and theoretical explanations are forwarded. For the micrometer-size range, maximum droplet diameter (d _max) was proportional to d ₃₂. For the submicrometer-size range, d _max varied with d ₃₂ in the range of 1.53–2.19-fold, and a correlation is proposed with K (=η_d/η_c); d ₃₂ and σ_g were well correlated with the process variables. Furthermore, a semi-empirical mechanistic model was developed for the formation of droplets obtained under inertial sub-range to interpret the effect of process variables.     

New cellular ceramics from high alkane phase emulsified suspensions (HAPES)

Open porous mechanically stable ceramic foams are developed by a simple direct foaming process. The new processing route is based on the transition of a surfactant stabilized highly concentrated alkane phase homogeneously distributed in a stabilized aqueous ceramic powder suspension into high performance ceramic foams with porosities up to 90% and cell sizes ranging from 3 to 200 μm. The droplet size distribution of the high alkane phase emulsified suspensions (HAPES) is efficiently controlled by the stirring velocity during emulsification experimentally investigated for varying powder particle contents. Stable foams with tailored structural features can be prepared by adjusting the rheological characteristics of HAPES being dependent on the system and process parameters. The influence of the emulsification stirring velocity on the resulting HAPES droplet size is analysed on the basis of the Taylor model of mechanical shearing describing the stresses responsible for the fragmentation of the droplets.     

Robust generation of monodisperse droplets using a microfluidic step emulsification device with triangular nozzle

In this work, the droplet generation process in the microfluidic step emulsification chip with a triangular nozzle (SE-T) was investigated in the combination of visualization experiment and numerical simulation, through a comparison with a rectangular nozzle (SE-R). The flow regimes, including dripping, dripping-jetting transition, and jetting, were observed in the SE-T, among which the dripping is the preferred flow regime to generate monodispersed droplet with corresponding C.V. (coefficient of variation) of the droplet size smaller than 1.9%. Compared with the SE-R, the larger space and expanding structure of the triangular nozzle in the SE-T enhance the wall wetting effects, which induces earlier appearance and accelerates shrinking of the neck. As a result, the SE-T exhibits more robust droplet performance under the dripping regime, which produces the droplets with nearly unchanged size and higher monodispersity, especially little related to the variations of surfactant concentrations and dispersed phase flow rates.     

Droplet break-up by in-line Silverson rotor–stator mixer

Silverson high shear in-line rotor–stator mixers are widely applied in industry for the manufacture of emulsion-based products but the current understanding of droplet breakage and coalescence in these devices is limited. The aim of this paper is to increase the understanding of droplet break-up mechanisms and to identify appropriate literature correlations for in-line rotor–stator mixers. Silicone oils with viscosities ranging from 9.4 to 969 mPa s were emulsified with surfactant in an in-line Silverson at rotor speeds up to 11,000 rpm and flow rates up to 5 tonnes/h. The effect of rotor speed, flow rate, dispersed phase fraction up to 50 wt%, inlet drop size and viscosity ratio on droplet size was investigated. It was found that rotor speed and dispersed phase viscosity have a significant effect on the droplet size, while flow rate, inlet droplet size, viscosity ratio and dispersed phase volume have a lesser effect. The results indicate that low viscosity droplets are broken by turbulent inertial stresses, while droplets smaller than the Kolmogorov length scale are broken by a combination of inertial and viscous stresses. It also appears that the weak dependence of drop size on flow rate enables the energy efficiency of an in-line high shear Silverson to be significantly improved by operating at as high a flow rate as possible.     

Parametric study of droplet size in an axisymmetric flow-focusing capillary device

A conventional technique for microfluidic droplet generation is Co-axial Flow Focusing(CFF) in which a contraction zone is placed downstream of the dispersed phase nozzle. In this contraction zone, the dispersed-phase(dphase) fluid is pinched off by continuous-phase(c-phase) fluid to generate micro-droplets. Studying the influence of multiple parameters such as the fluids velocities and viscosities, the interfacial tension, and nozzle and orifice diameters on the droplet size is of great importance for the design and application of CFF devices. Thus,development of more complete numerical models is required. In this paper, we show our model is compatible with experimental data and then numerically investigate the effects of aforementioned parameters on the droplet generation in a CFF microfluidic device. Simulation results showed that the c–phase flow rate, viscosity and the interfacial tension had great impacts on the droplet size. The effect of the nozzle diameter on the generated droplet size was small compared to that of the orifice in a CFF device. Using the simulation results, a correlation was also developed and suggested which predicts the droplet size with less than 15% error in a wide range of the introduced dimensionless parameters.     

Kenics型静态混合器内分散相液滴破碎和聚结过程的CFD-PBM数值模拟

采用CFD-PBM耦合方法对Kenics型静态混合器内分散相油滴破碎及聚并行为进行数值模拟研究,分析了雷诺数、混合元件数、元件长径比等参数对分散相液滴粒径的影响,揭示了分散相在Kenics静态混合器内流动过程中液滴粒径的演化规律.结果表明,随雷诺数增大,分散相液滴出口粒径不断减小,并出现临界趋势;静态混合器的前几个元件...     

Piezoelectric Droplet Generator for the Calibration of Particle‐Sizing Instruments

Using a piezoceramic tube and a continuous glass capillary, droplets in a diameter range between 10 μm and 100 μm can be generated. This corresponds to a volume of up to 0.6 pl. The velocity of the generated droplets depends on droplet size but is constant for each diameter. The liquid can be dosed as single droplet, as an accumulation of droplets or as a chain of droplets in a frequency range between 1 Hz up to 3 kHz. The lifetime of the droplets depends on droplet size and the chemical and physical properties of the dispersed liquid. In addition, for water droplets the humidity of the air near the droplet trajectory influences the lifetime of the droplets.     

Deformation of an oil droplet on a solid substrate in simple shear flow

Displacement of immiscible fluids is important in sub-surface processes such as enhanced oil recovery, oil sand processing and detergency. In this study, simulation of an oil droplet deformation on a solid substrate in simple shear flow has been carried out using computational fluid dynamics tool (Fluent 6.3) and the shape of the oil droplet is compared with that of the experimental observation. The dynamic behavior of a two-dimensional oil droplet subject to shear flow in a closed channel is considered under the condition of negligible inertial and gravitational forces. The volume of fluid method is used in Fluent to determine the dynamics of free surface of the oil droplet during the fluid flow. The oil droplet deformation increases with the increase in capillary number, Reynolds number and size of the oil droplet. The deformation of an oil droplet attached to channel surface in simple shear flow is studied experimentally in laminar flow through visual observation using microscope (Ziess, SV11 APO) with high speed camera (PCO). Aniline and isoquinoline was used to form oil droplet and distilled water was used as shearing fluid. The deformation of aniline and isoquinoline droplets was recorded using a high speed camera connected to a PC. The recorded image was replayed and the deformation of aniline and isoquinoline droplets was analyzed using Axio Vision software and compared with the results obtained from CFD simulation. The deformation of different sizes of aniline and isoquinoline droplets at different flow rates of shearing fluid and with time are well predicted by the CFD simulation.     

高压静电破乳中离散液滴的动力学分析

考虑乳化液离散液滴的直径分布,对高压直流静电破乳过程中离散液滴的运动进行了理论模拟。模拟及实验结果表明,在高压静电作用下,离散滴液从一侧电极向另一侧电极运动。沿液滴运动方向,液滴浓度逐渐增大,并在电极附近达到最大。随着静电作用时间的延长,电极附近液滴浓度近似呈线性规律增大。在相同的作用时间内,高电压液滴浓度的增长幅度要更大。因此,尽可能提高施加电压要比单纯延长静电作用时间的破乳效果更好。此外,大的液滴运动速度更快,故对于离散相滴径较大的乳化液,破乳效率会更高。     

Numerical simulation and experimental study of emulsification in a narrow-gap homogenizer

The present experimental and theoretical study investigates the fragmentation of the oil phase in an emulsion on its passage through a high-pressure, axial-flow homogenizer. The considered homogenizer contains narrow annular gap(s), whereupon the initially coarse oil drops break into fine droplets. The experiments were carried out using either a facility with one or two successive gaps, varying the flow rate and the material properties of the dispersed phase. The measured drop size distributions in the final emulsion clearly illustrated that the flow rate, as well as the dispersed-phase viscosity, and the interfacial tension can significantly affect the drop size after emulsification. The larger mean and maximum drop diameters obtained for the homogenizer with one gap in comparison to those obtained with two gaps (at the same Reynolds number and material parameters of the emulsion phases), highlighted the strong relevance of the flow geometry to the emulsification process. The numerical simulation of the carrier phase flow fields evolving in the investigated homogenizer was proven to be a very reliable method for providing appropriate input to theoretical models for the maximum drop size. The predictions of the applied droplet breakup model using input values from the numerical simulations showed very good agreement with the experimental data. In particular, the effect of the flow geometry—one-gap versus two-gaps design—was captured very well. This effect associated with the geometry is missed completely when using instead the frequently adopted concept of estimating input values from very gross correlations. It was shown that applying such a mainly bulk flow dependent estimate correlation makes the drop size predictions insensitive to the observed difference between the one-gap and the two-gaps cases. This obvious deficit, as well the higher accuracy, strongly favors the present method relying on the numerical simulation of the carrier phase flow.     

Preparation of monodisperse water-in-oil-in-water emulsions using microfluidization and straight-through microchannel emulsification

Water-in-soybean oil-in-water (W/O/W) emulsions with an internal water phase content of 10–30% (vol/vol) were prepared by a two-step emulsification method using microfluidization and straight-through microchannel (MC) emulsification. A straight-through MC is a silicon array of micrometer-sized through-holes running through the plate. Microfluidization produced water-in-oil (W/O) emulsions with submicron water droplets of 0.15–0.26 μm in average diameter (d _av,w/o) and 42–53% in CV (CV_w/o) using tetraglycerin monolaurate condensed ricinoleic acid esters (TGCR) and polyglycerin polycondensed ricinoleic acid esters (PGPR) as surfactants dissolved in the oil phase. The d _av,w/o and viscosity of the W/O emulsions increased with an increase in internal water phase content. Straight-through MC emulsification was performed using the W/O emulsions as the to-be-dispersed phase and polyoxyethylene (20) sorbitan monooleate (Tween^® 80) as a surfactant dissolved in the external water phase. Monodisperse W/O/W emulsions with d _av,w/o/w of 39.0–41.0 μm and CV_w/o/w below 5% were successfully formed from a straight-through MC with an oblong section (42.8×13.3 μm), using the TGCR-containing systems. The d _av,w/o/w of the monodisperse W/O/W emulsions decreased as the internal water phase content increased because of the increase in viscosity of the to-be-dispersed phase. Little leakage of the internal water droplets and no droplet coalescence or droplet break-down were observed during straight-through MC emulsification.