Chapter 1 INTRODUCTION

Laminar liquid jets possess several attractive advantages over other types of apparatus for fundamental studies of the mechanism of gas absorption. To obtain a valid experimental test of unsteady state diusion theory in a ow system, it is imperative that the uid dynamics of the system be known accurately. L. E. Scriven & R. L. Pigford (1959) Liquid-liquid systems are important to workers in many areas of engineering, physics, and chemistry. A few examples of current interest are liquid-liquid extraction equipment (Treybal, 1963, 1980; Jereys, 1987; Rousseau, 1987, Tsouris and Tavlarides, 1990), liquid-liquid jets (Richards et al., 1993, 1994a, 1994b), space applications in propulsion systems, life support, and storage (Kim et al., 1994), coating ows (Ruschak, 1985; Christodoulou and Scriven, 1989), oil-water mixtures in pipeline ow (Joseph et al., 1984), extrusion of polymers (Mavridis et al., 1987), secondary oil recovery (Weidner and Schwartz, 1991), interfacial tension measurements (Li and Fu, 1992), liquid bridges (Russo and Steen, 1989; Slobozhanin and Perales, 1993), static menisci (Finn, 1986; Cuvelier and Schulkes, 1990), and interfacial rheology (Edwards et al., 1991). In this dissertation we seek an improved understanding of the uid mechanics underlying liquid-liquid extraction, a widely used unit operation in which solutes dissolved in a liquid solution are separated by contact with another, generally immiscible, liquid. If dierent solutes in the original solution distribute themselves dierently between the two phases, a certain degree of separation will develop, and this may be enhanced by multiple contacts in staged operation. If 1

2 the liquids are left in contact long enough, mass transfer between the two phases causes the solute distribution to approach an equilibrium condition. Extractors can be constructed in many forms, which can be run batch or continuous, e.g., mixer-settlers, plate columns, packed columns, as well as more exotic designs. Many articles and books have been written on the subject, and the details of current design techniques are well documented in, for example, Treybal (1963, 1980), Jereys (1987), and Rousseau (1987). The eciency and stability of the separation depend on the underlying processes taking place in the stage. These are the uid ow eld, the thermodynamic equilibria, and the mass transfer within and between phases. The research proposed here focuses on the uid mechanics alone, as once the ow eld is known, the mass transfer and thermodynamic eects can, in principle, be added to complete the analysis. The uid mechanics of the extractor are dependent on the type of device considered. If it is a sieve-tray extractor, the light uid rises through the continuous phase in trains of drops. If the extractor is a mixer-settler, the dispersed phase is broken into drops by the energy of an impeller, with turbulent ow commonly found in practice. 1.1 Four Distinct Levels of Analysis Various levels of analysis can be applied to liquid-liquid extractors, depending on the information sought, and can be classied as corresponding to the discrete macroscopic (phenomenological), pseudo-continuum, continuum, or the molecular level. Each level of analysis can be used to answer dierent questions to dierent degrees of accuracy. Most plant design work is typically performed at the macroscopic level, where little information is required on the internal details of the system. Equipment design is at the pseudo-continuum level where empirical information is needed to determine appropriate values of model parameters. This dissertation is not concerned with questions at the macroscopic level such as the ones related to the overall performance of the extractor, where most of the

3 design work has occurred in the past. On the opposite end of the scales of length, questions addressed at the molecular level are mostly concerned with the physical properties of the components of the system and the boundary conditions, which again are fairly well characterized. It remains to examine the extractor at the two remaining levels. A more detailed level of analysis than the macroscopic level, sometimes referred to as the pseudo-continuum level, provides a more elaborate description of the internal structure of the system and the transport within it. For example, mass transfer coecients are often used in equipment design (Treybal, 1980). However, such descriptions still involve spatial averaging (e.g., over a swarm of droplets or over random column packing) or temporal averaging (in turbulent ow), so that quantities such as velocities and concentrations do not represent the true values at a given point in the system. Further, the transport properties (e.g., turbulent viscosities) are not true state properties, and their process dependence again makes empirical information necessary. These limitations are obviated at the continuum level, where velocities and concentrations are local quantities and transport properties such as viscosities, densities, surface tensions, and diusivities, are true state variables. The obvious problem is that most actual liquid-liquid contactors are much too complex in their geometry and operation to permit a full continuum description, even with the computational capabilities available today. In this dissertation, therefore, we seek a middle ground, by analyzing at the continuum level idealized liquid-liquid systems pertinent to actual extractors. We expect these analyses to enhance our understanding of more realistic systems in two ways: i. Among the systems we examine are ones that represent key elements of one or more types of actual contactors; for example, a liquid-liquid jet is representative of the situation above an orice on a sieve tray. ii. The parametric dependence of the behavior seen in the ideal model systems is expected to be related to that in more complex systems; dimensionless

4 parameters that determine the size and the specic surface area of liquid-liquid jets and drops are investigated. The object is to model the velocity and pressure elds as well as the interface shape and location in a two-phase system that has one or more free surfaces. Various simplied situations can be envisioned. The ones chosen for this work are the liquid-liquid jet, and the drops formed before and during jetting. Two regions are considered for the liquid-liquid jets: the steady region near the nozzle, and the entire region from the nozzle to the breakup of the jet into drops. 1.2 Background As noted above, most previous analysis and design work on liquid-liquid contactors has been performed at the macroscopic or the pseudo-continuum level. Results of such studies, and procedures based on them, may be found in, for instance, Treybal (1963, 1980), Perry and Green (1984), Jereys (1987), and Rousseau (1987). More detailed analyses at the pseudo-continuum level have been undertaken using other approaches. For example, Guimaraes et al. (1988, 1990) used the population balance approach to model the eects of drop breakage and coalescence on the hydrodynamics and mass transfer eciency of liquidliquid continuous-ow stirred tanks at steady-state. However, even in these more elaborate models it is necessary to estimate parameter values based on empirical data. It is only at the continuum level, where transport properties are true state variables, that this problem can be overcome. However, as noted earlier, the analysis of only relatively idealized systems is possible at the continuum level, even with the computational capabilities available today. A variety of such systems have been studied in the past: Isolated drops. Analytical models of single drops in idealized situations have a long history. For example, the oscillation of a stationary drop can be described exactly in the inviscid case (Lamb, 1932), and it has been studied more recently for small Reynolds numbers by Lundgren and Mansour (1988). More complex

5 systems have been examined either numerically or experimentally or both. Oliver and Chung (1987) investigated the ow of a uid sphere translating in another uid by solving numerically the steady-state Navier-Stokes equations inside and outside the sphere using a streamfunction formulation. They obtained numerically the velocity and pressure distributions inside and outside the sphere. Surface tension acts to keep the drop spherical, but at high shear rates the drop will deform, and eventually break. Isolated drops have been experimentally investigated during breakup and coalescence (Clift et al., 1978; Ashgriz and Poo, 1990). The slender body theory of Acrivos and Lo (1978) can be used for breakup at non-zero Reynolds numbers, but requires that the drop or bubble that is breaking up must be elongated. Stone and Leal (1989) have numerically investigated the dynamics of drop deformation and breakup at low Reynolds numbers; Bentley and Leal (1986) studied these eects experimentally. Basaran et al. (1989) studied small amplitude drop oscillations in liquid-liquid systems both experimentally and theoretically and Jeelani and Hartland (1991) investigated the collision of two oscillating liquid drops. Liquid-liquid jet. When one liquid is injected into another, a jet may be formed. That this occurs in sieve plate columns has motivated its study in apparatuses specically designed for mass transfer and surface tension experiments with a single jet (Skelland and Huang, 1977, 1979; Skelland and Walker, 1989). Meister and Scheele (Meister, 1966; Meister and Scheele, 1967, 1969a, 1969b; Scheele and Meister, 1968) worked to develop an understanding of the jet and drop formation based on experiments obtained with 15 liquid-liquid systems. They reported theoretical results based on linear stability analysis for jet breakup and drop formation, and overall force balances for drop formation below jetting. It was noted by Meister (1966) that mass transfer coecients in extraction columns are generally reported as overall coecients on a volumetric basis Ky Ss because of the diculty of separating the mass transfer coecient Ky from the specic surface Ss . To obtain better predictions of the volumetric mass transfer coecient, and

6 hence of the mass transfer rate, better predictions of the specic surface formed in the injection process are required. More accurate estimates of the mass transfer coecients can be obtained once the velocity and concentration elds in the two phases are known. For an example of mass transfer coecients calculated using the concentration and velocity proles in a liquid jet falling in (and absorbing) carbon dioxide, see Scriven and Pigford (1959). Richards and Scheele (1985) measured velocity proles in liquid jets of xylene injected upwards into water and found good agreement of the boundary layer theory (Yu and Scheele, 1975; Gospodinov et al., 1979) with jet radius measurements, but poor agreement with velocity measurements. Even today, the liquid-liquid jet and drop system is still not completely understood. Liquid jets into air have been studied extensively (Scriven and Pigford, 1959; Vrentas and Vrentas, 1982), with current research focusing on jet breakup (Mansour and Lundgren, 1990). Current limitations of jet breakup calculations, such as those of Mansour and Lundgren (1990), who used a boundary element method (BEM), are that they are generally inviscid and can only be carried out only as far as the pinch point, at which time the Lagrangian mesh is highly distorted. The Eulerian volume of uid (VOF) technique discussed in section 1.3 can overcome both of these limitations; an example of a simple free liquid cylinder capillary breakup modeled by this method is given by Kothe et al. (1991). Rayleigh-Taylor problem. An even simpler situation is the case of a heavier uid above a lighter uid in a gravitational eld. It was rst investigated in the linear stability analysis limit by Rayleigh (1883) and by Taylor (1950) and has since then been the subject of numerous studies. Linear stability analysis can be used to show when this situation is unstable (Harlow and Welch, 1966; Drazin and Reid, 1987), but this solution holds only for small interface deformations. The subsequent evolution of the interface and the ow eld is more interesting for our purposes. This has been examined in both two and three dimensions. The problem was studied numerically by Daly (1967, 1969a) using a Marker

7 and Cell (MAC) type method. Tan (1986) reexamined this unstable situation assuming incompressible, inviscid and irrotational uid ow in a bounded threedimensional domain. Steady solutions to this problem exist and were derived in approximate form by using bifurcation theory. It was shown that the surface develops into a bubbles-and-spikes conguration that can be stable to innitesimal disturbances. Tryggvason and Arefs (1983, 1985) numerical investigation of the Rayleigh-Taylor ow (renamed Taylor-Saman for Hele-Shaw-cell ow) found that the evolution of the resulting ngers was aected only by the viscosity ratio. More recently, Tryggvason and Unverdi (1990) have performed numerical studies in three dimensions using a front-tracking technique. Both theory and experiment for the three-dimensional Rayleigh-Taylor instability were studied by Jacobs and Catton (1988). Kelvin-Helmholtz problem. This problem is a generalization of the previous one in that the uids are moving relative to each other. Even when the heavy uid is below the light uid, instability can occur due to shear, as can be shown by a linear stability analysis (Drazin and Reid, 1987). Surface tension and viscosity tend to stabilize the ow. Linear stability analyses have also been applied to more complex situations, e.g., to the Couette ow of two uids between rotating concentric cylinders (Renardy and Joseph, 1985a, 1985b), to two-uid pipe ow (Joseph et al., 1984), and more recently to air-water ow (Bontozoglou and Hanratty, 1990). For larger interface deformations, few (numerical) results appear to have been reported. An example is the Kelvin-Helmholtz analog of the HeleShaw cell studied by Pozrikidis and Higdon (1985), who found dierent initial perturbations to result in dierent nal rollups of the nite vortex sheet. However, many of these and other analyses of the Kelvin-Helmholtz problem are limited to inviscid, linear regimes, or to the Hele-Shaw approximation (see also Weidner and Schwartz, 1991). The Kelvin-Helmholtz problem for two uids has also been studied experimentally by Thorpe (1968, 1969), using a long rectangular tube containing two

8 immiscible uids. When the tube was tilted away from the horizontal, a uniformly accelerating ow was produced, with shear at the interface leading to instability characterized by growing waves. Although these phenomena had already attracted considerable attention by the end of the last century, a comprehensive parametric investigation of the eects of dierent parameters (Reynolds number, Weber number, etc.) on the development of the mixing of the two phases is still lacking. This particular example is an inherently unsteady one that is pertinent to the startup of stirred tank contactors, and may help to shed light on the phenomenon of phase inversion (Quinn and Sigloh, 1963; Selker and Sleicher, 1965). Despite the fact that these problems are ones that have been extensively studied, a signicant part of the eort has been devoted to developing solution methods, and not much attention has been paid to examining parametric dependence of the solutions. This is a key aspect aecting the relevance of the idealized continuum problems to more complex systems, as similarities can be expected at least in the qualitative eects of dierent dimensionless parameters. Several dierent kinds of parameters are important in a real contactor: (i) physical property parameters, e.g., density ratio, viscosity ratio; (ii) geometric parameters, e.g., aspect ratio; (iii) hydrodynamic parameters, e.g., Reynolds numbers, Weber numbers. Each of the idealized problems outlined above is characterized by a smaller number of parameters, e.g., the classic Rayleigh-Taylor problem contains only physical property parameters, but by imposing a nite vertical or lateral size, geometric parameters are added. Similarly, the transition from the Rayleigh-Taylor to the Kelvin-Helmholtz problem introduces one or two hydrodynamic parameters. The liquid-liquid jet and drop formation problem includes all of the kinds of parameters seen in the simpler systems already noted. Thus it is particularly relevant to liquid-liquid contactors. Also, since it is not completely understood at the present time, it has been chosen as a model problem for this dissertation. The systematic study of parametric dependence of solutions to idealized problems is what we expect to shed light on the behavior of more complex systems.

9 1.3 Numerical Methods for Multiphase Flow The simulation of the dynamics of isolated drops, liquid-liquid jets, and Rayleigh-Taylor and Kelvin-Helmholtz involve the solution of the continuity and momentum equations for the two uids with specied boundary conditions. The description of the free surface oers a particular challenge, which can be dealt with numerically from either the Eulerian or Lagrangian view. The Eulerian mesh remains xed in space with the ow moving through it, while the Lagrangian mesh is convected with the ow. The major drawback of the Lagrangian approach, e.g., Ramaswamys (1990) study of free surface liquid sloshing in a container, is that only simple nonintersecting interfaces can be represented due to a limitation on the amount of mesh distortion allowed. The nite element method (FEM) has been used successfully in calculating steady free jet ows (Reddy and Tanner, 1978; Omodei, 1980; Georgiou et al., 1988; Cuvelier and Schulkes, 1990). Kheshgi and Scriven (1984) have reviewed the nite element analysis of unsteady free surface ows, while the works by Baker (1983) and Zienkiewicz (1988) provide a general reference for the FEM method. As can be seen by examining these studies, it may be possible to use the Lagrangian FEM to solve the specic steady liquid-liquid jet problem considered in this dissertation. However, we are further interested in predicting jet breakup and subsequent drop formation, past the point of necking and through pinch-o of drops (with possible subsequent drop coalescence), which precludes the FEM since it cannot, at the present time, be used to model such complex breaking and reforming of interfaces. Two basic Eulerian approaches have been formulated to track the interface and have been reviewed by Hyman (1984) and Unverdi (1990), namely front tracking and volume tracking. Front tracking uses the technique of characterizing the interface by computational elements, such as a string of particles, which are convected with the ow (Daly 1967, 1969a, 1969b). Tryggvason and Unverdi (1990) used an additional grid with nite thickness that was convected with the ow. Volume tracking involves using markers (MAC (marker and cell) method,

10 Harlow and Welch, 1966) or a marker function convected by the ow (VOF (volume of uid) method, Hirt and Nichols, 1981). Yeung (1982) has presented a general review of the numerical methods used in free-surface ows, while general references for computational uid dynamics (CFD) are Peyret and Taylor (1983) and Anderson et al. (1984). A completely dierent approach is the use of lattice-gas automata (Stockman et al., 1990), which are collections of discrete particles constrained to move on xed geometric lattices. This approach allows complex interface shapes to evolve in time, and can be implemented on special parallel architectures. Initially only uids with the same density could be accommodated with this method, and an extremely large number of cells had to be used to obtain accurate results comparable to the explicit dierential equation methods. More recently, formulation of lattice-Boltzmann techniques has circumvented most of these deciencies (Succi et al. 1991). Volume of uid method. The major incentive for using the VOF method is that the types of problems that can be solved involve highly complex free surface ows. Reasonable accuracy is attainable and yet the method is relatively simply implemented. The basic algorithm is available in a two-uid code called SOLAVOF (Nichols et al., 1980; Hirt and Nichols, 1981), and part of our work has been devoted to modifying this algorithm to adapt it to the problems of interest, which involve transient free surface ows with two immiscible uids. More recently, Kothe et al. (1991) introduced a one-uid code, RIPPLE, which incorporates various improvements to the one-uid VOF algorithm. The VOF formulation assumes that the ow in each phase is unsteady, viscous, and incompressible. The equations of motion and continuity are solved in a manner similar to that used by Nichols et al. (1980) with appropriate boundary conditions for no-slip, free-slip, continuative, periodic, and contact angle, in twodimensional Cartesian or axisymmetric coordinates. The interface surface forces are incorporated as accelerations in the momentum equations rather than as

11 boundary conditions using a marker function eld, dened as F = 1 for uid 2 and F = 0 for uid 1. This VOF function F is obtained by solving a kinematic relation. The discontinuous density and viscosity elds are obtained from linear interpolations using the F function. In our work, we have also included in the algorithm the calculation of the streamfunction, which can be obtained from a Poisson equation. The SOLA-VOF code is well suited for high Reynolds number ows, including those involving free surfaces. Among the latter, however, it is better suited for gas-liquid than for liquid-liquid systems, and relaxing this limitation has been an important part of our eorts. A one-uid program, RIPPLE, which implements the Continuum Surface Force (CSF) algorithm and incorporates various improvements in the SOLA-VOF algorithm, has been introduced by Kothe et al. (1991) and Brackbill, et al. (1992). 1.4 Dissertation Objectives The goal of this dissertation is to model aspects of complex liquid-liquid ow behavior, implemented within a robust and ecient code to simulate steady-state and transient liquid-liquid ows, including high Reynolds number ones. This code is applied to the realistic simulation of aspects of the complex uid mechanical behavior in order to develop quantitative insight into the underlying processes involved, such as drop and jet formation, size, shape, and breakup. Of course, it is unavoidable that a limited range of the parameters has been investigated, dictated primarily by the availability of reliable experimental data. The two principal barriers to further progress in the area of liquid-liquid separations are perceived to be the lack of a fundamental understanding of the uid mechanical phenomena associated with the development and destruction of free surfaces separating two immiscible liquid phases, and the lack of a robust and ecient numerical code that would enable the reliable simulation of key test ow cases. This dissertation aims to contribute towards the resolution of both the

12 above issues, physical and computational. First, we have focused our research eorts towards the improvement of the VOF numerical technique that we consider to be the best approach to the numerical solution of free surface problems that involve two immiscible liquid phases, high Reynolds number laminar ows and complex, time-dependent interfaces. Considerable progress has recently been made in developing VOF codes for 2-D and 3-D free surface ows involving liquid-air or liquid-vacuum interfaces (RIPPLE and FLOW-3D (developed by Flow Science, Los Alamos, NM, Hirt, 1988) are two examples), and although these indicate the appropriateness of the technique for complex free surface problems, no commercially available code exists for liquidliquid high Reynolds numbers free surface problems beyond the original SOLAVOF (Hirt and Nichols, 1981). POLYFLOW (Crochet, 1987), one of the best commercial codes based on FEM that can perform multiple phase calculations, is best suited for low Reynolds number ows as, for example, the low Reynolds number free jet die swell problem (Hill and Chenier, 1984). This code, as do other codes, uses the method of spines for representation of the free surface, so it can only represent simple, nonintersecting, single valued interfaces. A spine is a line segment connecting two interface nodes and each interior node must belong to a single spine. Thus, there is a constraint on the type of meshes that can be formed with the use of spines. The SOLA-VOF code represented the starting point for our computational code development. However, due to the age of the original code (it was written before 1980), substantial further improvement was necessary in order to transform it to a versatile (robust) and ecient research tool for complex high Reynolds number free surface ows. Second, we have contributed to the knowledge base on liquid-liquid interface issues by investigating a few selected test cases, using the code developed as discussed above. Specically, we have examined a liquid jet injected into another immiscible liquid. As explained in section 1.2, this is a critical problem for the understanding of liquid-liquid separations. However, and in contrast to the much

13 more widely studied liquid-air jet problem, little information is available on the ow characteristics associated with the jet and the corresponding jet breakup problem. Most of the available information comes from the previous experimental work of Meister and Scheele (Meister, 1966; Meister and Scheele, 1967, 1969a, 1969b; Scheele and Meister, 1968) and Richards and Scheele (1985), whereas the theoretical work, limited to boundary-layer solutions of the problem, seems to be in considerable disagreement with the experimental data for the established velocity proles, despite correctly capturing the jet shape. We have used our simulations to predict the velocity proles in an eort to validate the approach and simultaneously to enable us to do a systematic parametric search. We also evaluated numerically the breakup conditions as well as the subsequent non-linear evolution of the drops, as a function of time. Thus, this research is expected to have a signicant impact on the way complex liquid-liquid contactors are designed in the future, not to mention a plethora of other important technological applications (such as, for example, ink jet printing studied by Croucher and Hair, 1989 or low-gravity ows in space vehicles, Ostrach, 1982), where the understanding of interface development is of paramount importance. 1.5 Dissertation Outline The chapters of this dissertation are organized in the following manner. In chapter 2 the governing equations that are used throughout this work are derived from a fundamental viewpoint both to serve as a rigorous basis for the dissertation and to indicate where future extensions may evolve. Here the Volume of Fluid (VOF) function is introduced in conjunction with the novel use of the Heaviside step function, which is an invaluable analytical tool to describe the interface. The solutions to these problems involve the solution of the equations of motion and continuity for two uids with specied boundary conditions. The free surface oers a particular challenge. During the course of this work we have found diculty in producing numerically stable free surface results with the SOLA-VOF

14 surface tension algorithm. In chapter 3 we have combined the two-uid capability of the SOLA-VOF algorithm with the free surface implementation of the CSF algorithm to investigate problems that involve transient 2-D free surface ows with two immiscible uids with possibly high Reynolds numbers, and found the results to be much more numerically stable. The numerical method used to solve the nite dierence equations for the velocity and pressure and the advection of the free surface is described. The surface force calculation is detailed as well as the boundary conditions used in the free surface problems. Numerical stability issues are also discussed. Several test problems that have known analytical or numerical solutions were used to test the accuracy and validate the modied algorithm and are detailed in section 3.8. The results of these problems indicate reasonable accuracy, with some diculty encountered in the capillary tube at small contact angles and very low Reynolds numbers (Re < 1). It was also found that the viscosity could not be considered spatially constant across the free surface as it was in the original SOLA-VOF code, since it was found that the normal stresses were not equal at the free surface in the problem of two-phase cocurrent ow between parallel plates. Thus, the code was rewritten in terms of a variable viscosity. In chapter 4 an ecient and robust method is presented for solving the Young-Laplace equation that describes the shape of the meniscus in a vertical cylinder for a constrained liquid volume. This serves as a test problem for future work and as an introduction to the static free-surface equation. An overview of this eld is covered by Finn (1986). The method of solution proposed here explicitly incorporates the constraint in the equation, transforming the two-point boundary value problem into an initial value one with the constraint determining the unknown centerline height. This allows rapid determination of the solution families, which are characterized by only centerline height and meniscus arclength. The method can be generalized to other axisymmetric systems such as spheres, cones, and ellipsoids with or without axial rotation. In chapter 5 we investigate the steady liquid-liquid jet. When a liquid

15 is injected into another liquid a jet may be formed. This occurs in liquid-

liquid extraction plate columns as well as apparatus specically designed for mass transfer experiments with a single jet. The axisymmetric steady-state laminar ow of a Newtonian liquid jet injected vertically into another immiscible Newtonian liquid is investigated for various Reynolds numbers. The steady-state solution was calculated by solving the axisymmetric transient equations of motion and continuity using a numerical scheme based on the Volume of Fluid (VOF) method combined with the new Continuum Surface Force (CSF) algorithm. The analysis takes into account pressure, viscous, inertial, gravitational, and surface tension forces. The liquid-liquid jets eventually break up due to the increasing amplitude of disturbance waves on their surface. In chapter 6 we investigate the length of the resulting jets, which is dependent on many factors. Meister and Scheele (1969a) have so far provided the most complete picture of liquid-liquid jet breakup. The axisymmetric, dynamic breakup of a Newtonian liquid jet injected vertically into another immiscible Newtonian liquid at various Reynolds numbers is investigated in chapter 6. The full transient from jet startup to breakup into drops was simulated numerically by solving the time-dependent axisymmetric equations of motion and continuity using the code developed in this dissertation. The algorithm has been further rened here based on its performance on transient problems such as the solution of the free liquid-liquid capillary jet breakup problem. The simulation results are compared with previous experimental measurements of jet length under conditions where all forces, i.e., viscous, inertial, buoyancy, and surface tension, are important. The size of the drops produced before and during jetting is important from an industrial standpoint due to the creation of large, new surface area. In chapter 7 the formation of drops by the vertical injection of a Newtonian liquid into another stationary immiscible Newtonian liquid, at low to high Reynolds numbers, before and after jet formation, is investigated. The full transient from before startup

16 to breakup into drops was simulated numerically by solving the time-dependent axisymmetric equations of motion and continuity. The numerical simulations are compared with experiments and previous simplied analyses of Meister and Scheele (1968, 1969b) based on drop formation before and after jetting. Prediction of the sizes of these drops over wide ranges of Reynolds numbers is another important result from this work, where only approximate theories have existed up until this time. Solutions to these dicult problems shed light on the distortion of interfaces into various shapes and the physical variables that are important in extractors from a hydrodynamic viewpoint.