Chapter 8

CONCLUSIONS AND RECOMMENDATIONS

In the mathematical investigations I have usually employed such
methods as present themselves naturally to a physicist. The pure
mathematician will complain, and (it must be confessed) sometimes
with justice, of deficient rigour. But to this question there are two
sides. For, however important it may be to maintain a uniformly
high standard in pure mathematics, the physicist may occasionally
do well to rest content with arguments which are fairly satisfactory
and conclusive from his point of view. To his mind, exercised in
a different order of ideas, the more severe procedure of the pure
mathematician may appear not more but less demonstrative.
Lord Rayleigh, Theory of sound (1894)
8.1

Conclusions
The overall goal in this dissertation has been to understand certain aspects

of complex liquid-liquid flow behavior. Towards that goal, we developed a numerical code for the solution of axisymmetric liquid-liquid flow problems, including
high, but still corresponding to laminar flow, Reynolds number ones. We have
applied this code to the realistic simulation of aspects of the complex fluid mechanical behavior, and developed quantitative insight into the underlying processes
involved, such as drop and jet formation, size, shape, and breakup. The problem
was numerically and physically complex in that buoyancy, surface tension, viscous,
and inertial forces were all important in the experimental systems studied.
In this work we have first developed a robust and flexible numerical methodology to solve a fairly general class of axisymmetric free surface liquid-liquid flow
problems of relevance to, for example liquid-liquid extraction. We have used this
numerical technique to investigate the steady-state and transient liquid-liquid jet
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formation and breakup as well as drop formation. The numerical code can already
be used to help design liquid-liquid extraction systems, by obtaining for example,
the specific surface area of drops forming from a specific nozzle under pre-specified
conditions. The same approach can be used, in principle, for 3-dimensional investigation, although some code efficiency issues still remain, as discussed below.
Kothe (1993) has indicated that the CSF algorithm has been extended and is capable of solving 3-D problems. The simulation results developed here encompasses
and generalizes the results of many workers in the past who used limiting forms
of the equations or other significant approximations. Our simulation predictions
compare favorably to available experimental results and defined the domain of
applicability of the simplified models of previous investigators.
Our research philosophy in this dissertation has been to approach these
complex issues in a very basic, generic way. We have taken a numerical approach
since the more complex problems defy closed-form or analytical solutions. The
emphasis has been on validation of the numerical method with numerous test
problems that exercise the various parts of the algorithm as well as obtaining favorable comparisons with available experimental data on liquid-liquid jet and drop
systems. From these studies we have located deficiencies in the original SOLAVOF algorithm and improved it where necessary. We have used the simulations to
help interpret the data and prevailing mechanisms as well as explore the regions
of validity of the best existing simplified analytical and numerical models of other
workers. We believe this approach has enabled us to lay a firm foundation for
future investigations in other liquid-liquid applications as will be discussed further
in this chapter.
As discussed in chapter 1, the efficiency and stability of the separation
depend on the fluid flow field, the thermodynamic equilibria, and the mass transfer
within and between phases. We have focused on the fluid mechanics alone which
are dependent on the type of contactor considered. The work here has been
concentrated on the continuum level, where velocities and concentrations are local

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quantities and transport properties such as viscosities, densities, surface tensions,
and diffusivities, are true state variables. Since actual contactors are too complex
for a complete simulation at the present time, we have analyzed idealized liquidliquid systems that possess key aspects of actual extractors. The parametric
dependence of the behavior seen in the model systems is expected to be related to
that in these more complex systems. The information developed thus far will be
needed in the next stage of sophistication, i.e., that of adding solutes and possibly
surfactants to solve more general problems of interest.
Thus, in this dissertation, we have learned about, and accomplished, two
major goals set forth in our original objectives: that of significant contributions
to the numerical methodology and the application of this method to solve a few
simplified problems of important practical interest in a more detailed fashion than
was possible previously. To accomplish these goals the following procedure was
taken (details can be found in the individual conclusion sections at the end of
chapters 37):
First, we have discussed in chapter 3 the combination of the Volume of
Fluid (VOF) method with the Continuous Surface Force (CSF) algorithm for the
calculation of possibly high Reynolds numbers free surface flows. In chapter 2, we
developed the field equations that are used in this dissertation from a fundamental
point of view so that the assumptions involved, and the proofs of the validity of the
equations, are evident using framework developed by Scriven (1960) and Edwards
et al. (1991). Also, future workers should be able to relax the assumptions in
the program quite readily to include, for example, the effects of surfactant on the
free surface dynamics. Numerous test problems were used to explore the limits
and improve the algorithms, including the new solution of the Young-Laplace
equation with constraint discussed in chapter 4. The numerical solution algorithm
developed in this dissertation turned out to be intimately linked with the specific
problems of interest, so that it proved impossible to solve these problems with any
existing CFD code.

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Second, with this methodology we examined the liquid-liquid jet formation
and breakup and drop formation before and after jetting in great detail. This work
is covered in chapters 57. We have successfully simulated low to high Reynolds
number, high buoyancy number, and low Weber number flows, up to the limit
of physical instability. The use of this direct numerical simulation allowed us to
ascertain the validity of the other approximate steady-state numerical schemes,
encompassing all of the physics of the previous models. We have also introduced a
new macroscopic momentum balance (5.9) predicting interface position that shows
qualitative agreement with the experiments and reduces to the result of Slattery
and Schowalter (1964) when Nj = 0. We have compared the predicted interface
and drop shapes and average jet lengths with experimental data and numerical results of previous workers (Addison and Elliott, 1950; Meister and Scheele,
1966, 1967, 1969a, 1969b; Duda and Vrentas, 1967; Scheele and Meister, 1968; Yu
and Scheele, 1975; Gospodinov et al., 1979; Richards, 1978; Anwar et al., 1982;
Richards and Scheele, 1985; Bright, 1985). We conclude that the present simulation agrees satisfactorily with the data, within experimental error. The use of this
direct numerical simulation allowed us to ascertain the accuracy of the approximate numerical models and to examine the validity of their approximations. With
our method, there is no need to switch between various mechanisms depending
on the flow regime, as is done in the simplified models, as the correct physics is
embedded in the full equations of motion and continuity.
8.2

Recommendations for Future Work

8.2.1 Physical System Issues

The experimental system used in this work displays many aspects of an
actual liquid-liquid contactor but it is especially difficult to simulate. Unknown
disturbances as well as the nonlinearity of the governing equations lead to further
difficulties when comparing with actual experiments. Additional issues include
such aspects as impure materials, resulting in the possible need to include dynamic

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surface tension, which has an influence on the predicted jet lengths. Predominant
among the issues that the present study revealed is the sensitivity to the external
disturbances. An experimental study to characterize these ambiguities further
could be undertaken with pure materials and forced amplitude and frequency
perturbations for liquid-liquid jets, analogous to the experiments of Donnelly and
Glaberson (1966), who investigated liquid jets in air. The jets in this study were
simulated only in the region where axisymmetric disturbances were dominant.
To examine stability in the presence of non-axisymmetric disturbances, full 3-D
calculations will be required.
Also a very wide variety of other liquid-liquid flows mentioned in chapter 1 could be investigated. A key objective would be detailed simulation, then
development of more compact approximate representations of pseudo-continuum
events. For example, further elucidation of drop breakage and coalescence frequency expressions useful in pseudo-continuum population balance formulations
used by Guimaraes et al. (1988, 1990) who studied the hydrodynamics and mass
transfer efficiency of liquid-liquid continuous-flow stirred tanks. Another example
that is an inherently unsteady one and is pertinent to the startup of stirred tank
contactors is the phenomenon of phase inversion (Quinn and Sigloh, 1963; Selker
and Sleicher, 1965). Here, as discussed in chapter 1 simplified flows such as the
Kelvin-Helmholtz problem may be used as a starting point to generate insight into
these more complex behaviors.
Addition of the convective-diffusion equation to the existing model would
allow the calculation of concentration profiles. A general reference discussing the
use and solution of this equation in various applications once the flow field is known
is Cussler (1984). For example, Coyle et al. (1981) performed a linear stability
analysis for liquid-liquid viscous jets assuming dilute solute mass transfer, with
the undisturbed solute concentration linear within the jet and uniform outside,
while the undisturbed velocity profile corresponded to plug flow in the jet. The
difficulty with this solution is that the base state plug flow profile is inconsistent

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with the actual profile in viscous liquid-liquid jets (as was the case with Bright,
1985) and the local nature of the analysis. The present model, augmented with the
convective-diffusion equation, would enable calculation of mass transfer coefficients
without these difficulties. Mass transfer coefficients in other liquid-liquid systems,
such as a swarm of drops in a given shear field, could, in principle, be evaluated
with this extension to the present numerical algorithm. This would be useful
in predicting mass transfer rates in staged column extractors such as the ones
described by Tsouris and Tavlarides (1990) and other types of equipment discussed
by Jeffreys (1987).
Turbulent systems are also important in liquid-liquid systems and this
would mean solving the time-averaged equations of motion and continuity (Bird,
1960) along with the convective-diffusion equation. If this were possible, extending
the present method, turbulent agitated liquid-liquid extractors could be simulated.
For example, Skelland and Moeti (1990) used semi-empirical expressions on the
basis of local isotropic turbulence theory, for mass transfer coefficients in nine
turbine-agitated liquid-liquid systems, in baffled vessels. That this may be possible
is the fact that the one-phase commercial predecessor to SOLA-VOF, namely
FLOW-3D (Hirt, 1988), can perform turbulent simulations at the present time
using the k  model (Harlow and Nakayama, 1967) of turbulence.
The case of the effect of a surface tension gradient due to a temperature
gradient has recently been investigated by Sasmal and Hochstein (1993) in the
context of the VOF method. Surfactant concentration variations at the interface
also produce surface tension gradients. The consideration of these effects couples
the surfactant species balances with the momentum equations. Additions to the
model to understand this behavior would involve equations of state for surface
tension and, perhaps, the addition of surface shear and dilatational viscosities
to the present model.

These are concepts that have already been discussed

briefly in chapter 2 and are discussed more thoroughly in Edwards et al. (1991).
Appropriate modifications would be made to the surface boundary condition

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(2.50) and momentum equations (2.51). The more general interfacial boundary
condition, first derived by Scriven (1960), can be found in chapter 4 and the surface
equations of state and the species convective-diffusion equations can be found in
chapter 5 of Edwards et al. (1991). A recent example of the FEM calculation of a
coating flow using surface viscosities can be found in Giavedoni and Saita (1992).
An example of surfactant effects on the motion of drops at low Reynolds number
using an Oseen-type solution has been performed by O
guz and Sadhal (1988).
8.2.2 Numerical Method Issues
The main drawback of the current numerical method is the work required
to carry out a full realistic free surface calculation. This will become particularly
critical if 3-D calculations are desired. A stringent numerical stability criterion
(Hirt and Nichols, 1981) is used to adjust the time step automatically to a small
value (typically 1 105 s), and combined with the large number of mesh cells,
this results in about 10 teraflop (101012 flop) of work for a typical full jet breakup
calculation reported in this work. However, massively parallel teraflop machines
involving hundreds or thousands of processors will become reality in the next few
years (Orszag et al., 1993). Parallel machines have been exploited to solve, for
example, 3-D time-dependent incompressible flows using the FEM (Salinger et al.,
1993); parallelization of the code is one possibility, but, it is not known at this
time if this will be possible.
Most of the work in the present code is being performed in the SOR
iteration to satisfy continuity. The RIPPLE program (Kothe et al., 1991) uses
a pre-conditioned conjugate gradient method to solve a Poisson equation for
pressure pi,j , designed to cut down on the number of iterations during a time step.
However, if the Poisson equation for pi,j is used instead of the iterative method
for pi,j described in chapter 3, pressure boundary conditions on p are required
to be supplied, and for flexibility, we have chosen not to implement this method.
Moreover, RIPPLE can not be used directly since it has a serious limitation in that

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it has only been implemented to incorporate free-slip boundary conditions on the
pressure p. A new method designed to solve the Poisson-like equation (3.38) for
pi,j along with equations (3.45)(3.49) for ui,j , vi,j could be implemented with
the conjugate-gradient method, while still retaining simple boundary conditions
on pi,j . An example of this type of approach has been implemented by Wilkes
et al. (1985) and Kightley (1985) with the SIMPLE algorithm of Patankar (1980).
An alternative is to use the Alternating Direction Implicit (ADI) method as does
FLOW-3D (Hirt, 1988).
Another way to address this issue is to decrease the number of variables
that need to be solved for during the pressure iteration by reducing the mesh
size. Adaptive multigrid methods have been used by Thompson and Ferziger
(1989) to solve steady-state incompressible Navier-Stokes equations and may be
one possibility. It has been suggested to us by Eggermont (1993) that the VOF
advection equation (3.8) could be solved on a finer grid using the velocity fields
interpolated from a coarser grid. Another, perhaps more promising, method is
local refinement of the mesh, particularly at the interface. Locally refined grids
have been developed, for example, by Young et al. (1991) and Chen et al. (1990) to
simulate geometrically complex aircraft designs, by solving the velocity potential
equation using the FEM method. Here local refinement is implemented by dividing
a Cartesian grid cell into a number of smaller cells.
Several possibilities exist for accuracy improvement beyond simple mesh
refinement. First, the current Hirt-Nichols VOF function advection algorithm
advects the free surface assuming it to be either near-horizontal or near-vertical.
This advection algorithm can be replaced with the more accurate Youngs (1982)
algorithm where the interface is approximated by a straight line cutting through
the cell (Kothe, 1993). A related algorithm is FLAIR (flux line-segment model for
advection and interface reconstruction) by Ashgriz and Poo (1991). Second, the
advection terms in the momentum equations use a linear combination of centraldifference and upwinding by making use of upstream velocities for stability. Kothe

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et al. (1991) have implemented in RIPPLE an accuracy improvement on the
upwinding procedure by retaining second-order terms in the Taylor expansion
for the upwind velocities, as originally developed by van Leer (1979). Third, as
suggested by Kothe et al. (1991), implicit treatment of the surface tension terms
(e.g., as is the pressure in the current algorithm) it is possible to eliminate the
sometimes restrictive surface tension stability criterion. Fourth, again as suggested
by Kothe et al. (1991), a fully second-order solution procedure may be implemented
in time as well as space as proposed by Dukowicz and Dvinsky (1992).
In summary, the program and numerical techniques developed in this dissertation have been used to solve free surface problems involving two immiscible
liquid phases, high Reynolds number laminar flows and complex, time-dependent
interfaces, which is still a topic of much current research. We have contributed to
the understanding of liquid-liquid interface issues by investigating the liquid-liquid
jet and drop system. We expect this research to influence the way complex liquidliquid contactors are designed in the future, with extensions to other technologies
such as ink jet printing and low-gravity flows in space vehicles where complex
interface formation must be addressed.