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Simple and double microemulsions via the capillary breakup of highly stretched liquid jets

Published online by Cambridge University Press:  09 September 2016

A. Evangelio
Affiliation:
Área de Mecánica de Fluidos, Departamento de Ingenería Aeroespacial y Mecánica de Fluidos, Universidad de Sevilla, Avenida de los Descubrimientos s/n, 41092 Sevilla, Spain
F. Campo-Cortés
Affiliation:
Área de Mecánica de Fluidos, Departamento de Ingenería Aeroespacial y Mecánica de Fluidos, Universidad de Sevilla, Avenida de los Descubrimientos s/n, 41092 Sevilla, Spain
J. M. Gordillo*
Affiliation:
Área de Mecánica de Fluidos, Departamento de Ingenería Aeroespacial y Mecánica de Fluidos, Universidad de Sevilla, Avenida de los Descubrimientos s/n, 41092 Sevilla, Spain
*
†Email address for correspondence: jgordill@us.es

Abstract

We present an exhaustive experimental and theoretical study of the shapes of simple and compound jets formed when one (simple) or two (compound) immiscible liquids are injected into another liquid. The viscosity of the co-flowing external liquid is chosen to vary the characteristic Reynolds number of the outer stream, $Re_{o}$ , over a wide range of values. Our slender-body theory in Gordillo et al. (J. Fluid Mech., vol. 738, 2014, pp. 335–357) is extended to predict the shapes of simple jets when $Re_{o}$ is such that $Re_{o}\gg 1$ and also to predict the shapes of compound jets in the case of $Re_{o}\lesssim O(1)$ . The validity of our theoretical results, applicable to describe the dynamics of simple or compound jets within an outer carrier fluid in a wide variety of practical situations, is tested using a set-up where the liquids flow from a pressurized chamber towards an extraction tube, finding a very good agreement between the predicted and the observed shapes. Moreover, when $Re_{o}\lesssim O(1)$ , and thanks to the fact that the liquid jets produced using our method are highly stretched in the downstream direction, we find that the values of the critical capillary number above which a steady stretched jet is produced, with the capillary number defined here using the outer stream velocity and viscosity, is well below the corresponding critical values characterizing other similar procedures, like flow focusing. This experimental result, which is supported by a spatio-temporal stability analysis in which the axial gradients of the unperturbed solution are retained in the dispersion relation, imply a substantial saving of energy and of the volume of outer liquid necessary to generate a steady capillary jet from which drops are regularly produced. Additionally, making use of continuity arguments and of the fact that drops are formed as a consequence of the growth of a capillary instability, we provide closed expressions for the drop diameters and their production frequencies when the capillary number is above the critical one, in very good agreement with experiments. The simple or double microemulsions generated by the capillary disintegration of the type of simple or compound highly stretched steady jets described here might find applications in biotechnology, pharmacy, cosmetics or materials science.

Information

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Papers
Copyright
© 2016 Cambridge University Press 
Figure 0

Figure 1.Sketch of the drop production device operating in the regime of interest for applications, in which drops with very similar diameters $D_{d}$ are produced. Drops are regularly emitted from the tip of a steady and highly stretched liquid ligament attached at the exit of the injection needle. The origin of the dimensionless coordinate $x=X/L$ is located at the entrance of the square duct. The imposed inner liquid flow rate is $Q_{i}$ and the outer liquid flow rate is $UL^{2}$.

Figure 1

Figure 2.(a) Sketch illustrating the generation of simple emulsions. (b) In the case of double emulsions, two liquids with respective flow rates $Q_{i}$ (inner liquid) and $Q_{m}$ (middle liquid) are injected into the pressurized reservoir from a coaxial injection tube.

Figure 2

Table 1.Physical properties of the different liquids used in the experiments. The interfacial tension coefficients for the different combinations of immiscible liquids used in the experimental study are as follows: water – silicone oil, $\unicode[STIX]{x1D70E}=0.04~\text{N}~\text{m}^{-1}$; propylene glycol – silicone oil, $\unicode[STIX]{x1D70E}=0.01~\text{N}~\text{m}^{-1}$; glycerine $+$ water – silicone oil, $\unicode[STIX]{x1D70E}=0.03~\text{N}~\text{m}^{-1}$. In rows (g)–(i) mass percentages are used. The material properties of the different liquids used in this study have been obtained from the literature.

Figure 3

Figure 3.The effect of varying the different parameters governing the generation of O/W simple emulsions ($\unicode[STIX]{x1D70E}=0.04~\text{N}~\text{m}^{-1}$). (a) The effect of varying the diameter $D_{i}$ of the injector and of the distance $H$ on the drop generation process. Here, $U=0.85~\text{m}~\text{s}^{-1}$, $Q_{i}=30~\text{ml}~\text{h}^{-1}$, $\unicode[STIX]{x1D707}_{i}=5~\text{cP}$, $\unicode[STIX]{x1D707}_{o}=1~\text{cP}$ ($\unicode[STIX]{x1D706}_{i}=\unicode[STIX]{x1D707}_{i}/\unicode[STIX]{x1D707}_{o}=5$) and $Re_{o}=\unicode[STIX]{x1D70C}_{o}UL/\unicode[STIX]{x1D707}_{o}=850$. (b) The effects of varying both $U$ and $Q_{i}$. Here, $\unicode[STIX]{x1D707}_{i}=5~\text{cP}$, $\unicode[STIX]{x1D707}_{o}=1~\text{cP}$ ($\unicode[STIX]{x1D706}_{i}=5$), $Re_{o}=750$ (left) and $Re_{o}=940$ (right). (c) For a fixed value of the flow-rate ratio, $q_{i}=Q_{i}/(UL^{2})=0.011$, the images show the effect of varying the inner fluid viscosity for a value of the outer Reynolds number $Re_{o}=940$. In all images, $D_{i}=0.45$  mm, except at the bottom of panel (a), where $D_{i}=1.38$  mm. In all images, $H=0.95$  mm, except in the top left image of panel (a), where $H=0.45$  mm, and in the bottom image of panel (a), where $H=1.1$  mm.

Figure 4

Figure 4.The effect of varying the different parameters governing the generation of W/O emulsions ($\unicode[STIX]{x1D70E}=0.04~\text{N}~\text{m}^{-1}$). (a) The effect of varying the diameter $D_{i}$ of the injector and the distance $H$ on the drop generation process. Here, $U=0.275~\text{m}~\text{s}^{-1}$, $Q_{i}=1~\text{ml}~\text{h}^{-1}$, $\unicode[STIX]{x1D707}_{i}=1~\text{cP}$, $\unicode[STIX]{x1D707}_{o}=100~\text{cP}$ ($\unicode[STIX]{x1D706}_{i}=\unicode[STIX]{x1D707}_{i}/\unicode[STIX]{x1D707}_{o}=0.01$) and $Re_{o}=2.65$. (b) The effects of varying both $U$ and $Q_{i}$. Here, $\unicode[STIX]{x1D707}_{i}=1~\text{cP}$, $\unicode[STIX]{x1D707}_{o}=1000~\text{cP}$ ($\unicode[STIX]{x1D706}_{i}=0.001$), $Re_{o}=0.045$ (left) and $Re_{o}=0.06$ (right). (c) For a fixed value of the flow-rate ratio, $q_{i}=Q_{i}/(UL^{2})=0.001$, the images show the effect of varying the viscosity of the outer fluid. Here, $Re_{o}=2.09$ (left) and $Re_{o}=0.05$ (right). In all images, $D_{i}=1.38$  mm, except in the top images of panel (a), where $D_{i}=0.45$  mm. In all images, $H=1.85$  mm, except in the top left image of panel (a), where $H=0.45$  mm, and in the top right and bottom left images of panel (a), where $H=0.95$  mm.

Figure 5

Figure 5.The effect of varying the different parameters governing the generation of double emulsions. (a) The effect of varying the distance of the injector to the extraction tube when the middle fluid is propylene glycol and both the inner liquid and the continuous phase are silicone oils. Therefore, $\unicode[STIX]{x1D70E}_{i,m}=0.01~\text{N}~\text{m}^{-1}$, with $\unicode[STIX]{x1D70E}_{i}$ the interfacial tension coefficient between the inner and middle fluids and $\unicode[STIX]{x1D70E}_{m}$ the interfacial tension coefficient between the middle fluid and the continuous phase. Here, $\unicode[STIX]{x1D707}_{i}=10~\text{cP}$, $\unicode[STIX]{x1D707}_{m}=42~\text{cP}$, $\unicode[STIX]{x1D707}_{o}=1000~\text{cP}$, $U=0.02~\text{m}~\text{s}^{-1}$, $Q_{i}=0.5~\text{ml}~\text{h}^{-1}$, $Q_{m}=0.5~\text{ml}~\text{h}^{-1}$ and, consequently, $q=(Q_{i}+Q_{m})/(UL^{2})=0.014$ and $Re_{o}=0.02$. (b) The effects of varying both the outer fluid velocity and the total flow rate $Q=Q_{i}+Q_{m}$ on the generation of compound drops. In this case, the middle liquid is propylene glycol and both the inner fluid and the continuous phase are different silicone oils: $\unicode[STIX]{x1D70E}_{i,m}=0.01~\text{N}~\text{m}^{-1}$, $\unicode[STIX]{x1D707}_{i}=5~\text{cP}$, $\unicode[STIX]{x1D707}_{m}=42~\text{cP}$, $\unicode[STIX]{x1D707}_{o}=1000~\text{cP}$, $Re_{o}=0.015$ (left) and $Re_{o}=0.02$ (right). (c) The effect of varying the middle liquid viscosity on the generation of compound drops. In this case, the middle liquid is a mixture of glycerine $+$ water in two different proportions, while the inner liquid as well as the continuous phase are silicone oils of viscosities $\unicode[STIX]{x1D707}_{i}=10~\text{cP}$ and $\unicode[STIX]{x1D707}_{o}=1000~\text{cP}$, respectively, and $\unicode[STIX]{x1D70E}_{i,m}=0.03~\text{N}~\text{m}^{-1}$. Left: $U=0.045~\text{m}~\text{s}^{-1}$, $Q_{i}=1~\text{ml}~\text{h}^{-1}$, $Q_{m}=2~\text{ml}~\text{h}^{-1}$, $\unicode[STIX]{x1D706}_{i}=0.01$, $\unicode[STIX]{x1D706}_{m}=\unicode[STIX]{x1D707}_{m}/\unicode[STIX]{x1D707}_{o}=0.1$ and $Re_{o}=0.043$. Right: $U=0.045~\text{m}~\text{s}^{-1}$, $Q_{i}=2~\text{ml}~\text{h}^{-1}$, $Q_{m}=1~\text{ml}~\text{h}^{-1}$, $\unicode[STIX]{x1D706}_{i}=0.01$, $\unicode[STIX]{x1D706}_{m}=0.4$ and $Re_{o}=0.043$. In these experiments, the ratio $q=(Q_{i}+Q_{m})/(UL^{2})$ is kept constant. (d) The effect of varying the inner fluid viscosity on the generation of compound drops. In this case, the middle liquid is propylene glycol, $\unicode[STIX]{x1D707}_{m}=42~\text{cP}$, and the inner fluid and the continuous phase are silicone oils. The outer fluid viscosity is kept constant at $\unicode[STIX]{x1D707}_{o}=1000~\text{cP}$; therefore, $\unicode[STIX]{x1D706}_{m}=0.042$ and $\unicode[STIX]{x1D70E}_{i,m}=0.01~\text{N}~\text{m}^{-1}$. Left: $U=0.014~\text{m}~\text{s}^{-1}$, $Q_{i}=0.3~\text{ml}~\text{h}^{-1}$, $Q_{m}=0.3~\text{ml}~\text{h}^{-1}$, $\unicode[STIX]{x1D707}_{i}=5~\text{cP}$, $\unicode[STIX]{x1D706}_{i}=5\times 10^{-3}$ and $Re_{o}=0.013$. Right: $U=0.025~\text{m}~\text{s}^{-1}$, $Q_{i}=0.5~\text{ml}~\text{h}^{-1}$, $Q_{m}=0.5~\text{ml}~\text{h}^{-1}$, $\unicode[STIX]{x1D707}_{i}=10~\text{cP}$, $\unicode[STIX]{x1D706}_{i}=10^{-2}$ and $Re_{o}=0.024$. In these experiments, the ratio $q=(Q_{i}+Q_{m})/(UL^{2})$ is kept constant. In all cases, $H=1.75$  mm, except in the left image in panel (a), where $H=0.9$  mm. In all cases, $D_{i}=1$  mm and $D_{m}=1.2$  mm.

Figure 6

Figure 6.Sketches showing that the outer flow field (a) can be decomposed as the addition of two fields: the unperturbed flow field (b), which is calculated numerically using ANSYS Fluent, and the perturbed flow field (c), associated with the presence of the jet. The perturbed velocity field can be quantified as a continuous line of sources of intensity $S(X)$ located at the axis of symmetry.

Figure 7

Figure 7.Numerically calculated functions $u_{x}$ and $f$ in the Stokes limit for the particular case $H/L=0.97$ and $D/L=0.45$.

Figure 8

Figure 8.Simple jets – comparison between the predicted and observed shapes in the case of $\unicode[STIX]{x1D706}_{i}=10^{-2}$ for different geometrical arrangements: (a) $Ca_{o}=1.04$, $Re_{o}=3.92$, $Q_{i}=0.5~\text{ml}~\text{h}^{-1}$, $U=0.206~\text{m}~\text{s}^{-1}$; (b) $Ca_{o}=1.04$, $Re_{o}=3.92$, $Q_{i}=0.5~\text{ml}~\text{h}^{-1}$, $U=0.21~\text{m}~\text{s}^{-1}$; (c) $Ca_{o}=1.04$, $Re_{o}=3.92$, $Q_{i}=0.5~\text{ml}~\text{h}^{-1}$, $U=0.21~\text{m}~\text{s}^{-1}$. Notice that the agreement is excellent in spite of the fact that $Re_{o}\sim O(1)$. The agreement is equally good for the cases in which $Re_{o}\ll 1$.

Figure 9

Figure 9.Compound jets – comparison between the predicted and observed shapes for different values of the control parameters when the middle fluid is propylene glycol and the outer fluid viscosity is $\unicode[STIX]{x1D707}_{o}=1000~\text{cP}$: (a) $\unicode[STIX]{x1D706}_{m}=0.042$, $\unicode[STIX]{x1D706}_{i}=0.005$, $Ca_{o}^{\prime }=\unicode[STIX]{x1D707}_{o}U/(\unicode[STIX]{x1D70E}_{i}+\unicode[STIX]{x1D70E}_{m})=0.7$, $Re_{o}=0.027$, $Q_{i}=0.1~\text{ml}~\text{h}^{-1}$, $Q_{m}=0.1~\text{ml}~\text{h}^{-1}$, $U=0.014~\text{m}~\text{s}^{-1}$; (b) $\unicode[STIX]{x1D706}_{m}=0.04$, $\unicode[STIX]{x1D706}_{i}=0.005$, $Ca_{o}^{\prime }=0.7$, $Re_{o}=0.027$, $Q_{i}=0.3~\text{ml}~\text{h}^{-1}$, $Q_{m}=0.3~\text{ml}~\text{h}^{-1}$, $U=0.014~\text{m}~\text{s}^{-1}$; (c) $\unicode[STIX]{x1D706}_{m}=0.04$, $\unicode[STIX]{x1D706}_{i}=0.01$, $Ca_{o}^{\prime }=1.79$, $Re_{o}=0.067$, $Q_{i}=1~\text{ml}~\text{h}^{-1}$, $Q_{m}=1~\text{ml}~\text{h}^{-1}$, $U=0.035~\text{m}~\text{s}^{-1}$.

Figure 10

Figure 10.Numerically calculated function $u_{x}$ in the high-Reynolds-number limit for the particular case $H/L=0.97$ and $D/L=0.45$.

Figure 11

Figure 11.Comparison between the predicted and observed shapes of steady liquid jets in the case of the generation of oil drops in water, for which $Re_{o}\gg 1$ and $\unicode[STIX]{x1D70E}=0.04~\text{N}~\text{m}^{-1}$: in all cases, $\unicode[STIX]{x1D706}_{i}=5$; (a) $Q_{i}=40~\text{ml}~\text{h}^{-1}$, $U=0.75~\text{m}~\text{s}^{-1}$, $Re_{o}=755$; (b) $Q_{i}=20~\text{ml}~\text{h}^{-1}$, $U=0.75~\text{m}~\text{s}^{-1}$, $Re_{o}=755$; (c) $Q_{i}=50~\text{ml}~\text{h}^{-1}$, $U=0.85~\text{m}~\text{s}^{-1}$, $Re_{o}=850$.

Figure 12

Figure 12.Plots showing that the diameters (a) and frequencies (b) of the oil drops formed in water ($Re_{o}\gg 1$) follow the expected scalings $D_{d}\propto Lq^{1/2}$ and $f\propto U/(Lq^{1/2})$, respectively. However, note that the experimental data are rather dispersed with respect to the predicted trends.

Figure 13

Figure 13.Case of simple emulsions: the diameters (a) and frequencies (b) of the simple emulsions generated when $Re_{o}\lesssim O(1)$ follow the expected scalings given in (4.3) and (4.1), respectively, with $\ell _{o}/L$ calculated by means of (4.6) and $k_{max}$ deduced using (4.4). Notice that, in contrast with the high-Reynolds-number case, the dispersion of the experimental data with respect to the expected scaling is small.

Figure 14

Figure 14.Case of double emulsions: the diameters (a) and frequencies (b) of the double emulsions generated when $Re_{o}\lesssim O(1)$ follow the expected scalings given in (4.3) and (4.1), respectively, with $\ell _{o}/L$ calculated by means of (4.6) and $k_{max}$ deduced using (4.4). Notice that, in contrast with the high-Reynolds-number case, the dispersion of the experimental data with respect to the expected scaling is small. In this case, the capillary number is defined using an ‘effective’ interfacial tension coefficient, $\unicode[STIX]{x1D70E}=\unicode[STIX]{x1D70E}_{i}+\unicode[STIX]{x1D70E}_{m}$.

Figure 15

Figure 15.(a,b) The experimental shapes of simple jets for two values of the viscosity ratio. (c) The experimental values of the capillary numbers for which simple or compound drops are generated as a consequence of the capillary breakup of highly stretched steady capillary jets. In the case of simple emulsions, $Ca_{o}=\unicode[STIX]{x1D707}_{o}U/\unicode[STIX]{x1D70E}$, and for double emulsions, $Ca_{o}^{\prime }=\unicode[STIX]{x1D707}_{o}U/(\unicode[STIX]{x1D70E}_{i}+\unicode[STIX]{x1D70E}_{m})$. Observe that, in our experiments, the minimum values of the capillary numbers above which steady jets and, therefore, droplets with a low size dispersion are produced is well below the critical capillary number $Ca^{\ast }$ calculated under the parallel flow assumption (dispersion relation (4.4), $Ca^{\ast }\simeq 0.139\unicode[STIX]{x1D706}_{i}^{-1/2}$). However, if the $x$-dependent terms expressing the fact that the unperturbed jet diameter decreases downstream are included in the analysis (dispersion relation (5.1)), the agreement between observations and the predictions improves notably as $x$ lies within the realistic values depicted in panels (a) and (b). Dashed lines represent the values of the critical capillary number calculated using the dispersion relation (5.1) for fixed values of $x$. All the results shown correspond to a value of the flow-rate ratio $q_{i}=10^{-3}$. The values of the critical capillary number, however, are insensitive to variations of $q_{i}$ for $q_{i}\ll 1$.