JOURNAL OF APPLIED POLYMER SCIENCE VOL. 17, PP.

1203-1225 (1973)

Stratified Two-Phase Flow of Molten Polymers

THOMAS C. YU and CHANG DAE HAN, Department of Chemical

Engineering, Polytechnic Institute of Brooklyn., Brooklyn, New York 11201

Synopsis
A study has been made of stratified two-phase flow of molten polymers in a slit diel.
For the experimental study, measurements were taken of wall normal stresses along the
longitudinal axis of a rectangular duct which had an aspect ratio of 10. Three pressuiie
transducers were flush-mounted on each of the rectangle’s long sides, directly opposite
from each other. The measurements permitted one t o determine the pressure gradients
of each component (their viscous properties) and the exit pressures of each component
(their elastic properties). For the theoretical study, the fully developed velocity dis-
tributions of two-phase flow were determined by solving the equations of motion by use
of a power law model. The volumetric flow rates, calculated theoretically by use of a
power law model, are compared with experimentally observed ones. Experimental
evidence is presented which clearly shows that polystyrene and polypropylene form two
incompatible phases in the molten state.

INTRODUCTION
Two-phase flow has been a subject of considerable interest to many
researchers during the past few decades. However, most studies were
concerned with gas-liquid systems, and only a small fraction of them dealt
with liquid-liquid systems. Among the studies made of liquid-liquid
systems, many have dealt with Newtonian fluids, but very few with non-
Newtonian viscoelastic fluids.
Two types of two-phase flow may be considered from the point of view
of the manner in which phase separation occurs. One type is the dis-
persed two-phase system in which one Component exists as a discrete phase
(droplets) dispersed in the other which forms a continuous phase. The
other is the stratified two-phase system in which both components form
continuous phases separated from each other by a continuous boundary.
Mixtures of heavy crudc oil and water flowing through long horizontal
pipelines havc been reported t o form stratified two-phase system. I n that
instance, stratification occurs owing to the large differences in densities and
viscosities between the heavy crudc oil and water. It was reported that
a n addition of a small amount of water to crudc oil flowing through thc
pipeline has considerably reduced the pressure gradient of the crude oil-
water mixture, resulting in a rcduction of pumping cost. This fact has
apparently stimulated many theoretical and experimcntal studies by
several investigator^^-^ who investigated stratified laminar flow of oil-
water mixtures in long, horizontal tubes or rectangular ducts.
1203
0 1973 by John Wiley & Sons, Inc.
1204 YU AND HAN

The recent development in formulating various polymer blends and

composite polymeric materials has prompted many researchers to investi-
gate the various flow problems involved with incompatible polymer systems
in the molten state. It is a fact ~vellknown t o the polymer processing
industry that both dispersed and stratified two-phase flow occur in several
important polymer processings. Two industrially important polymer
systems which form dispersed two-phase flow in the molten state are
rubber-reinforced polystyrene and acrylonitrilc-butadiene-styrene (ABS)
plastics. I n both, a rubbery component is dispersed in a glassy matrix of
the resin phase. Very recently, Han and Yu5s6demonstrated that blends
of polystyrene with polypropylene and blends of polystyrene with poly-
ethylene form two phases in the molten state when melted and extruded
through capillary dies.
Typical industrial processes which make use of stratified flow of molten
polymers are the production of composite materials such as conjugate
(bicomponent) fibers and multilayered films. I n making composite
materials, separate feed streams of molten polymers meet each other a t the
die inlet and then flow through circular or rectangular ducts. As molten
polymers possess both viscous and elastic properties, an analysis of the
stratified flow of molten polymers is much more complex than that of
Newtonian fluids. It is also to be noted that in general two chemically
dissimilar polymers are incompatible in the molten state.
At this point it is worth mentioning that earlier there has been some
important development reported on the production of conjugate fibers,
which met some commercial success due t o several industrial research
groups, namely, Sisson and h/lorehead7 and Hicks et al.*-1° The moti-
vation of their study was to produce crimped fibers very similar to natural
wool fibers. For this purpose, Sisson and RIorehead7 spun two viscose
solutions side by side through circular spinnerette holes and successfully
produced crimped fibers which possess a certain degree of bilateral structure
in a rayon. Similarly, Hicks et a1.8 developed the bicomponent acrylic
fiber (Orlon 21) which also produced crimps due to bilateral structure in an
acrylic fiber.
More recently, a few studies have been reported"-13 which were con-
cerned with the somewhat fundamental nature of the bicomponent stratified
flow of viscoclastic fluids. Southern and Ballman" investigated the
interfacial shape when two commercial polystyrenes were extruded side by
side, whereas White e t a1.12 investigated the flow patterns when two in-
compatible molten polymers (low-density polyethylene and polystyrene)
flow side by side. Slattery13 pressented an analysis on laminar two-phase
concentric flow of the simple fluid advanced by No11i4 and Coleman and
Noili5 in a circular tube. Slattery's analysis gives an analytical expression
for relating the total volumetric flow rate to two material functions, one
for each phase, which are unknown functions of the shear rate.
Unfortunately, there is scarcely any fundamental work published dealing
with the stratified two-phase flow of polymer melts as applied to industrially
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1205

important polymer processing methods. It is the purpose of this paper to

present the authors’ recent work on this topic. The paper discusses both
a theoretical and an experimental investigation made on the stratified
flow of polystyrene and polypropylene melts in a slit die.

ANALYSIS
One can conceive of a variety of different types of stratified flow. For
instance, such geometries as sketched in Figures la and l b have been
widely used in bilayered and multilayercd film extrusions. Similarly,
geometries such as sketched in Figurc l c and I d have been used in manu-
facturing bicomponent fibers. I n the following analysis, we shall consider
only the geometry of Figure la, in order t o simulate the actual experimental
system choscn for study.
Figure 2 depicts the flow geometry and the coordinate system of stratified
two-phase flow through a thin slit die (i.e., two parallel plates with infinite

[C) (d)
Fig. 1. Different geometries of stratified flow, which are of interest to polymer process-
ing.

Velocity
Distribution
+Flow Direction
X

Fig. 2. Plane slit geometry.

1206 YU AND HAN

width). For fully developed flow, the x-component of the equation of

motion is given by

Integrating eq. (1) gives

For phase 1,
r y z= -P’(y - C,) for 0 5y <a (2)
For phase 2,
fffZ= -P’(y - C,) fora<y<B (3)
where CI and Cz are integration constants and P‘ is the pressure gradient
dcfincd by P‘ = -dp/bx. Note that throughout this paper, variables
without the ovcrbar dcnotc phase 1, and variables with the overbar denote
phase 2. Note further in cqs. 2 and 3 that the pressure gradients in both
phases are assumed to bc the same. This assumption will be shown to be
corrcct, both theorctically and cxpcrimentally, in a latcr section.
For the flow geometry undcr consideration (see Fig. 2), the steady-state
velocity field is given by

Now, boundary conditions may be written as follows:

(i) At y = 0,
v=o (5)
(ii) At y = B,

(iii) AtJy = a,
v=P (7)
(iv) At y = a,

Tyr = Tyz. (8)

Use of boundary condition 8 in eqs. (2) and (3) yields
ryl = -P’(y - C ) for 0 5 y < m (9)
fffZ= -P’(y - C ) for a < ZJ I B (10)
whcre C = C1 = C2.
I n order to obtain the velocity profile and then to calculate the volu-
metric flow rate, one needs t o choose a constitutivc equation to solve cqs.
(9) and (10). I n thc past, a number of constitutive equations have been
suggestcd in the literature. I n fact, choice of a constitutive equation is
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1207

somewhat arbitrary. For our purpose here, we choose a power law fluid
because of its simplicity in subsequent mathematical manipulations.
For the velocity field given by cq. (4), a power law fluid may be written as
For phase 1,
rYZ= Ky" (11)
where
dV
y = - forO<y<C
dY
dV
y = --
dY
for C < y 5 a. (13)

For phase 2,
fYZ = Byi"
where

Note in eq. (11) that the shcar ratc y changes its sign a t thc position of
y = C , where a maximum velocity (hence zero velocity gradient, dV/cly
= 0) occurs, as shown schcmatically in Figure 2.
Now, equating the right-hand sides of eqs. (9) and (11) gives
y = [P'(C - y)/K]'I" (16)
or
y = C - (K/P')y".
Differentiating eq. (17) with respect t o y yields
dy = -(K/P')ny"-'dy.
Integrating eq. (12) with the aid of eq. (18), one obtains

where
yo = (y)@ = (P'C/K)'I".
It can be easily shown that eq. (19) is valid for thc cntirc distancc in phase
1 if y is defined as
y = (P'IC - yl/K)'I" for 0 Iy Ia. (21)
I n a similar manncr, onc can derive the velocity profile in phase 2 as
follows :

p(y) =
R12 (yB"+l - ?"+')
P n + l
1208 YU AND HAN

where
5 = [P'(y - C)/K]"" for a 2 y 5B (23)
YB = (T),=B = [P'(B - C)/R]"". (24)
It should be notcd that cqs. (19) and (22) contain a constant C, yet arc to
bc determined with thc aid of boundary condition 7. That is, the equation

should be solved for C , in which y p and 1, are to be evaluated from eqs.

(21) and (23), rcspcctivcly, by setting y = a. As may be supposed,
solution of eq. (25) for C requires a trial-and-error procedure using some
kind of successive iteration schcmc.
Once a correct value of C is found which satisfies eq. (25), one can calcu-
late the volumetric flow rate from
For phase 1,

(26)
For phase 2,

EXPERIMENTAL
Materials
Materials chosen for the experimental study were : general-purpose
polystyrene (DOW Styron 686) and polypropylene (Enjay Chemical Resin
E115). The main reason for choosing these materials is that previous
studies by the authors5s6have demonstrated that blends of these two poly-
mcrs form two phases when melted and extruded through a capillary.
Apparatus and Experimental Procedure
The apparatus consists of a 1-in. Killion extruder, a Zenith gear pump
driven by a variable-speed motor, a reservoir section which includes a
sharp-edged flow divider, and a slit die section. Figure 3 is a photograph
of the apparatus.
Two molten polymers were separately fed to the reservoir section :
polypropylene from the extruder, and polystyrene from the hydraulic
holding-tank (by means of a gear pump). Figure 4 shows detailed sketches
of both the feed and die sections, and Figure 5 is a detailed sketch of the die,
showing how the pressure transducers were mounted on the die. The
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1209

Fig. 3. Photograph of the apparatus.

hydraulic holding-tank was used t o supply one of the polymers because

there was only extruder available to us. This holding-tank was constructed
earlier for a melt-spinning experiment, and the details of the operating
procedures of the hydraulic system are given in a recent paper by Han and
Lamonte.16
The experimental procedure was straightforward. Two polymers were
fed separately t o the slit die, and measurements of wall normal stress were
made by means of melt pressure transducers (Dynisco Model PT 422),
which were flush-mounted on each of the rectangle's long sides, directly
opposite each other. When the flow was equilibrated after a new setting
of flow rate, mcasurements werc taken of wall pressures and flow rates of
each polymer. The outputs of the transducers were read in millivolts by a
potentiometer and null detector. The pressure transducers were cali-
bratcd against a dead weight tester. Measurements were repeatable
within 1% at pressures of 25 psig and above.
I n this experiment, good temperature control was crucial. The whole
system was heated by Calrod tubular heaters and was heavily insulated
with asbestos. Temperature was controlled within f1°F by Thermistor-
operated thermal regulators.

RESULTS AND DISCUSSION

Wall Pressure Measurements
Table I shows measurements of wall normal stresses along the longi-
tudinal axis of a thin slit die, through which polystyrene and polypropylenc
1210 YU AND HAN

#
FEED I 9

FEED SECTION
GELOK FITTING

HEATING ELEMENT

FLOW DIVIDER

DIE SECTION' ALUMINUM JACKET

THERMISTER
PROBE WELL

STEEL PLATE
BOTTOM HEATER

U U
Fig. 4. Detailed layout of the die assembly.

melts flow parallel to each other. It may be seen from Table I that,
within measurement error, the two pressure readings opposite each other
are essentially the same over the range of the variables investigated.
I n fact, one can show from the y-component of the equation of motion,

_ -bP + -bTuu
=o,
by dY
that the wall normal stresses must be the same for both phases. Using the
definition

'UY(YJZ) = -P(YJz> + TYY(Y) (29)

 TWO-PHASE FLOW OF MOLTEN POLYMERS 1211

I I I
(0) TOP VIEW (b) SDE VIEW

Fig. 5. Details of the slit die design.

one can rewrite eq. (28) as

For phase 1,

For phase 2,

bsy, = 0.
dY
Therefore we have from eqs. (30) and (31),
S, = S,, = constant.
This implies that, a t a fixed axial position z, the normal stresses, S, in
phase 1 and S,, in phase 2, are constant throughout their respective phases.
It is clear from eq. (32) that the pressures measured at the walls of the
long side of the rectangle can be expected to be the same for the two
phases (see Table I) because the wall pressures measured by means of
transducers are nothing but the negative wall normal stresses. Since for
fully developed flow the deviatoric component of normal stresses, T ~ , ( Y ) , is
independent of z, as may be seen from eq. (29), eq. (32) suggests further that

or
1212 YU AND HAN

TABLE I
Wall Pressure Measurements in the Stratified Two-Phase Flow of Polymer Melts
Flow Wall pressure,b psig Pressure
Run rate, gradient - d p / b ,
no. Materials cc/min PI p2 P3 psijin.
1 PS 6.80 210.0 118.4 28.6 90.80
PP 13.00 209.2 124.6 27.4
2 PS 9.20 217.6 123.4 29.9 94.07
PP 12.75 218.0 126.5 29.4
3 PS 10.60 222.5 128.1 31.1 97.07
PP 12.61 226.5 132.0 29.6
4 PS 11.94 226.0 129.5 32.0 98.67
PP 12.92 231 .'5 139.2 30.8
5 PS 9.28 206.8 115.7 30.6 88.45
PP 9.65 205.1 117.0 27.5
6 PS 10.61 211.0 118.8 31.5 91.07
PP 9.43 213.0 121.0 28.2
7 PS 12.36 215.0 122.5 32.0 92.22
PP 9.15 215.5 123.5 29.6
8 PS 13.41 219.0 125.5 33.0 95.00
PP 9.53 224.0 128.0 30.0
9 PS 6.93 234.7 134.4 33.6 100.48
PP 18.25 232.7 132.7 31.9
10 PS 9.28 243.6 139.6 35.5 104.40
PP 17.80 243.0 140.0 33.5
11 PS 10.60 245.9 140.6 36.6 105.40 .
PP 18.55 250.0 142.7 33.7
12 PS 11.95 247.5 145.0 37.1 107.65
PP 18.04 254.2 144.4 34.0
13 PS 6.85 235.0 134.5 34.5 101.12
PP 21.40 237.0 134.6 33.0
14 PS 9.26 235.0 134.4 34.5 101,oo
PP 17.70 236.0 134.5 32.5
15 PS 10.50 226.5 127.3 33.0 96.43
PP 13.75 223.2 126.5 31.0
a PS: Polystyrene (Dow Styron 686); PP: polypropylene (Enjay Chemical Resin
E115).
b Refer to Fig. 5 for the locations of pressure measurements.

That is, the pressure gradients are also expected to be the same in both
phases. This has been used already in the derivation of eqs. (2) and (3),
and finally in eqs. (26) and (27).
It should be noted that White et a1.12 also predicted that the t.wo pres-
sure readings opposite each ot,her in a slit die should be the same.
Figure 6 shows some representative plots of the axial distribution of wall
normal stresses with total volumetric flow rate as a parameter. Note that
in these plots the average values of the pressures of polystyrene and poly-
propylene melts were used. Two things are worth noting from the plots of
Figure 6. First, the axial pressure distribution is a straight line over the
distance where measurements were taken. Therefore, the slope of this
straight line permits us to determine the effective wall shear stress of the
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1213

220 -

200 -

180 -

160 -
-P
-2 140-

k3!
8
W
120-
E
g3 loo-
Q(cc/rnin)
RunNo. -
-
80 - 0 I 19.80
A 13 28.25

60 -

40 -

20 -

I 1 1 I I I 1

AXIAL DISTANCE (Inches)

Fig. 6. Plots of the axial pressure distribution.

two-phase system investigated. Second, the extrapolation of the measure-

ments taken nearest to the die exit gives rise to a nonzero exit pressure.
This has been referred to as “exit pressure” by Han and his co-workers,
who have made an extensive investigation of it during the past four
years. 17--21 Because of the experimental evidence that wall pressures are
the same in both phases (see Table I), the exit pressures also should be
the same in both phases. More will be said later about the exit pressure.
Viscous and Elastic Effects
For comparison purposes, measurements of the wall normal stresses
of individual components in single-phase flow are shown in Table 11. It is
clearly seen that, at comparable flow rates, wall pressures of polystyrene
melts are much higher than those of polypropylene melts, and hence higher
pressure gradients exist in polystyrene than in polypropylene.
 TABLE I1
Experimental Data of the Slit Flow of Pure Components

Wall pressure, psig Exit

Flow rate, - 3P/% 7W Yw, pressure,
Material cc/min p1 PZ pa psi/in. psi sec-1 wig 7 , poise
~~~ 4
Polystyrene 19.6 305.3 180.9 48.6 128.3 6.416 11.95 13.89 0.370 X 105
37.0 385.4 225.7 61.5 161.9 8.095 22.58 16.78 0.247 X lo6 5
48.8 412.1 241.7 65.6 173.3 8.664 29.77 17.83 0.201 x 106 a
55.7 426.9 250.9 67.9 179.5 8.974 33.95 18.66 0.183 X 106
70.1 446.1 259.7 72.1 187.0 9.351 42.74 19.78 0.151 X lo6
Polypropylene 26.6 176.0 105.8 29.3 73.4 3.67 16.2 9.69 0.156 X 105
48.9 233.7 139.8 38.2 97.8 4.88 29.8 11.98 0.113 X 105
57.6 254.2 150.3 41.3 106.4 5.32 35.1 12.28 0.104 x 106
72.3 278.8 163.9 44.8 116.9 5.85 44.1 12.63 0.915 X lo4
89.0 298.9 176.1 48.0 125.5 6.27 54.3 13.63 0.796 X lo'
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1215

200 -
150 -

100 -
90 -
80 -
70 -
60-
50-
I I I 1 I I I L
20 30 40 50 70 9(
0 (cc/rnin)
Fig. 7. Pressure gradients vs. volumetric flow rate for single- and two-phase systems.

Figure 7 shows plots of the pressure gradient versus volumetric flow

rate for both single- and two-phase flow. It is seen that the pressure
gradients of two-phase flow lie between those of two single-phase flows.
This indicates that the presence of polypropylene, which is less viscous,
brings a reduction in the pressure gradients of polystyrene, which is more
viscous. Figure 8 shows cross plots of Figure 7, indicating that the pres-
sure gradients of polystyrene melts are reduced by about 30%. This
appears to be independent of the amount of polypropylene present in the
two-phase system, say 3(t70%. I n Figure 8, the pressure gradient re-
duction factor (P.G.R.F.) is defined as the ratio of the pressure gradient
of the two-phase system to that of the more viscous phase alone (in this
case polystyrene), the flow rate being the same in each case:

for constant QT.

At this point, it is appropriate to point out the earlier studies by Charles
and Lilleleht3 and Gemmel and Epsteiq2 who reported that a drastic
reduction of power requirement was observed in the transportation of
heavy, viscous crude oil through a pipeline when a relatively small amount
of water was injected into the pipeline. These authors contended that the
observed reduction in power consumption was due to the reduction in
pressure gradient caused by the preferential wetting of the pipe wall by the
lesR viscous water. A similar situation has been known to the polymer
processing industry which processes polymer blends containing low molec-
ular weight materials as either lubricants or plasticizers. A prevailing
theory for the observed reduction in pressure drops across the die is that
low molecular weight materials tend to migrate toward the die wall, hence
giving rise to much lower shear stresses at the wall.
Table I11 shows the observed effects of the component ratios on pressure
gradients and exit pressures. It is seen that the pressure gradient (hence
wall shear stress) is not sensitive to change in the polystyrene/polypropyl-
1216 YU AND HAN

VOLUME FRACTION OF POLYPROPYLENE

Fig. 8. Pressure gradient reduction factor vs. volume fraction of polypropylene.

ene ratio, and that the exit pressure increases as the amount of poly-
styrene is increased while keeping the total flow rate constant. This in-
crease in exit pressure is as expected because Table I1 shows that at com-
parable flow rates, polystyrene gives higher exit pressures than polypropyl-
ene. According to Han and his ~ o - w o r k e r s , ~the
~ - ~existence
~ of the exit
pressure is a manifestation of the elastic properties of the materials in-
vestigated. Hence, one can conclude from Table I1 that wall pressure
measurements in stratified two-phase flow may be used to follow the changes
in the elastic properties of mixtures due to changes in the component ratio,
but not to follow the changes in the viscous properties.

TABLE I11
Effect of the Component Ratio on Exit Pressure
-a p / a z , Pexiti
Run no. Qt, cc/min QpJQ t psi/in. psi
T ~ , Psig
1 19.80 0.345 90.80 4.54 3.385
6 20.04 0.529 91.07 4.55 3.917
2 21.95 0.419 94.07 4.704 3.624
7 21.51 0.575 92.22 4.611 4.876
3 23.21 0.456 97.07 4.854 3.947
8 22.94 0.585 95.00 4.750 4.888

The present study shows further that the pressure gradient (a viscous
property) is quite sensitive to changes in the total volumetric flow rate,
as shown in Table IV. It is seen there that, for a fixed component ratio,
both wall shear stress and exit pressure increase with total volumetric
flow rate. Again, this is to be expected in view of the results shown in
Table I1 for single-phrtse flow.
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1217

TABLE IV
Effect of the Total Flow Rate on Exit Pressure
- hP/% Pexit,
Run no. Qt, cc/min Q d Q t psi/in. rm,psi PSk
1 19.80 0.345 90.80 4.540 3.385
14 26.96 0.343 101.00 5.050 5.102
10 27.08 0.346 104.40 5.220 5.463

Comparison of Experimental with Theoretically Predicted

Volumetric Flow Rate
The usefulness of the theoretical development given above may be
evaluated by comparing the calculated volumetric flow rates with the
experimentally observed ones. A comparison is given in Table V, in
which the calculated 00w rates are based on the power law model, that is,
by use of eqs. (26) and (27).
TABLE V
Comparison of the Calculated with Experimentally Observed Volumetric Flow Rate
Experimentally observed Calculated flow
Run no. Material flow rate, cc/min rate, cc/min
1 PS 6.80 4.01
PP 13.00 13.23
2 PS 9.20 6.32
PP 12.75 11.74
3 PS 10.60 8.00
PP 12.61 11.51
4 PS 11.94 9.15
PP 12.92 11.21
5 PS 9.28 6.82
PP 9.65 8.11
6 PS 10.61 8.32
PP 9.43 7.87
7 PS 12.36 9.63
PP 9.15 7.15
8 PS 13.41 10.74
PP 9.53 7.50
9 PS 6.93 3.55
PP 18.25 21.22
10 PS 9.28 6.05
PP 17.80 19.20
11 PS 10.60 6.97
PP 18.55 18.51
12 PS 11.95 8.71
PP 18.04 17.78
13 PS 6.85 2.82
PP 21.40 23.93
14 PS 9.26 5.52
PP 17.70 17.51
15 PS 10.50 12.00
PP 13.75 7.25
1218 YU AND HAN

I
10 15 20 25 30 40 50 60 70809oKx)
7, (sec-1)
Fig. 9. Flow curves for polystyrene and polypropylene melts.

For computation, two material constants, K and n, in the power law

model were determined for the individual components, polystyrene and
polypropylene, respectively. This was dyne by preparing plots of the wall
shear rate as shown in Figure 9, where rwand yw are defined by

Tw = (2) B
2
(35)

respectively. Having established the fact that both polystyrene and poly-
propylene melts follow a power law, we obtained the two material con-
stants K and n from
rw = Ky" (37)
where y is the true shear rate after the Rabinowitch-Mooney correction is
properly made :

Y = (
2n +1
7 ) Y w

in which n = d In r w / d In yw. Table VI shows the numerical values of K

and n for polystyrene and polypropylene melts, respectively, at 200°C.
It is seen from Table V that the calculated flow rates are consistently
lower than the experimentally observed ones by about 10% in polypropylene
and about 30% in polystyrene, on the average. However, they may be
considered to be acceptable, considering the first three assumptions made
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1219

TABLE VI
Material Constants in Power Law Model
Material Temp., "C K, lb/in.%ec-n n (dimensionless)

Polystyrene 200 2.598 0.301

Polypropylene 200 0.902 0.451

in the theoretical development. The first is that the flow through a thin
slit die (aspect ratio of 10 in the present study) is assumed to be one-
dimensional, not two-dimensional. The second is that the phase interface
is assumed to be a flat surface. The third is that the power law constants,
K and n, of the individual components are assumed to hold in stratified
two-phase flow. All of these assumptions have considerably simplified the
mathematical manipulations for deriving the expressions for the volumetric
flow rate. However, it is quite conceivable that any of these assumptions
could have contributed to the difference between the calculated and
measured flow rates. In particular, the latter two assumptions could play
an important role in accurately determining the volumetric flow rate.
At present, an experimental investigation is under way to help better
understand the interfacial phenomenon in the two-phase flow of molten
polymers.

Calculation of Velocity Distributions

The power law model was used further to calculate the velocity dis-
tributions in the stratified two-phase flow of polystyrene and polypropylene
melts under the experimental conditions. Some representative results are
shown in Figures 10 and 11.
Figure 10 shows the velocity distributions of two phases for different
pressure gradients, keeping the polystyrene/polypropylene ratio the same.
It is seen that, as expected, the larger the pressure gradients, the higher the
local velocities are, while still maintaining the same shape of velocity
profiles.
However, Figure 11 shows that a change in polystyrene/polypropylene
ratio, keeping total volumetric flow rates constant, brings a change in shape
of the velocity profiles. It should be noted, however, that the effective
pressure gradients in the two cases are the same, although with different
exit pressures (see Table 111). This raises an interesting and important
question. Is it valid to use two material constants, K and n, determined
from wall shear stress measurements of the individual components, in
order to predict the volumetric flow rate in stratified two-phase flow? After
all, wall shear stresses determined by the use of wall pressure measurements
are not sensitive to changes in the ratio of the two components.
It is expected, however, that a change of velocity profiles due to changes
of polystyrene/polypropylenc ratio may be attributable to changes in
both viscous and elastic properties of the two materials flowing together,
parallel to each other. At present, we are pursuing a study of how the
1220 YU AND HAN

0.9~

DISTANCE, cm
Fig. 10. Velocity distributions for different pressure gradients, keeping the polystyrene/
polypropylene ratio constant.

interactions of two materials might be taken into account in order to

correctly describe the flow behavior of two incompatible viscoelastic fluids.

Evidence of Incompatibilityin the Polystyrene/Polypropylene System

I n previous work, the authors5s6have shown that blends of polystyrene
and polypropylene, when melted and extruded through a capillary die,
exhibit complete incompatibility. For the sake of completeness, we
present the pictures in Figure 12, which show the microstructure of ex-
trudate samples obtained from a blend. Note that these pictures were
taken as part of an earlier study which was concerned with the rheological
properties of blend systems. I n the blend, polystyrene forms the discrete
phase (black portions of the picture), and polypropylene, the continuous
phase (white portions). The fact that these two materials form two phases,
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1221

0.8

0.7

0.6

0
I
\ 0.5
5
>
t
8 0.4
J
W
>

0.3
I

I
'
1
1
\\\\

0.2

0.1
POLYPROPYLENE POLYSTYRENE

0 LI1I 1 1 1 1 I l I I I I I I 1 I l 1 1 1 I I I

0 0.05 0.0 0.15 0.20 0.25

DISTANCE, cm
Fig. 11. Velocity distributions for different polystyrene/polypropyleneratios, keeping
the total volumetric flow rate constant.

at least under the extrusion conditions, may be expected on the following

two accounts: First, polystyrene belongs to the aromatic group (containing
benzene rings) , while polypropylene belongs to the aliphatic group (con-
taining straight carbon chains) ; second, the residence time involved in the
extrusion operation is considered to be too short to allow any sort of
molecular diff usion. These macromolecules have extremely large values
of viscosity (2000-4000 poises at 200°C) over the range of shear rates
investigated.
Based on the pictures shown in Figure 12, one would then expect to
have a completely stratified flow when polystyrene and polypropylene melts
are fed separately to a die inlet and flow through the die. The authors
have found that this was indeed thc case when extrudate samples were
collected and cross-sectioned. In fact, polystyrene and polypropylenc
initially forming .a single piece of extrudate have split apart into two
Eeparate pieces when completely frozen. Figure 13 shows a picture of the
cross section of separated extrudates of polystyrene and polypropylene.
1222 YU AND HAN

(b1
Fig. 12. Pictures (200X) showing the microstructure of an extrudate sample of 50
wt-% polystyrene/50 wt-% polypropylene blends, extruded in a circular tube of LID =
20 ( D = 0.125 in.) at 200°C: (a) middle portion of extrudate cross section; (b) middle
portion of extrudate in the longitudinal direction.

It may be worth making a few observations on the picture in Figure 13.

First, the interface is not really a well-defined flat surface; rather, it has a
curvature. Second, the interface appears to have a mild corrugation.
Interestingly enough, Yu and Sparrow4 have observed a similar interface
when they studied thc stratified flow of two Newtonian fluids flowing
through a rectangular duct. It should be noted, however, that the interface
shown in Figure f3 might not be the one actually exiting in the die. While
 TWO-PHASE FLOW OF MOLTEN POLYMERS 1223

Fig. 13. Picture of extrudate cross section showing the phase interface in stratified
flow of polystyrene and and polypropylene melts in a slit die a t 200°C.

being cooled, the polypropylene, which is a crystalline polymer, would be-

have (i.e., shrink) differently from the polystyrene, which is an amorphous
polymer. In other words, the rate of crystallization of polypropylene
during cooling could alter the shape of the interface between two molten
polymers, conceivably giving rise to corrugated, deformed interfaces in the
frozen state.
At present, an experimental study is under way for making visual
observations of the interface in fully developed, stratified two-phase flow of
molten polymers, using a thin slit die made of a special quality of quartz.

CONCLUSIONS
An experimental and theoretical study has been carried out to investi-
gate the stratified two-phase flow of molten polymers in a slit die. From
the study, the following conclusions may be drawn:
1. Measurements of wall normal stresses in the two phases give the
theoretically expected result, namely, the same wall pressures in both
phases and consequently the same pressure gradients in both.
2. The effective wall pressure gradient of polystyrene, which is the more
viscous, is reduced by about 30% in the presence of polypropylene over
the range of component ratios investigated.
3. At a fixed volumetric flow rate of the combined stream, wall pressure
measurements are insensitive to changes in the component ratio, but very
sensitive to changes in the total volumetric flow rate. Wall pressures
increase with flow rate.
4. Exit pressure is found to be sensitive to changes in both the total
volumetric flow rate and component ratio.
5 . Although the power law model cannot describe the elastic effects of
molten polymers, which are viscoelastic in the present case, it enables US
to calculate the volumetric flow and velocity profiles by solving the equa-
tions of motion. The volumetric flow rates, calculated theoretically by
use of a power law model, are somewhat low compared to the experimen-
1224 YU AND HAN

tally observed values. Reasons are given which might explain the dis-
crepancy.
6. Further experimental evidence is presented which clearly shows that
polystyrene and polypropylene form two incompatible phascs in the molten
atate.
This work was supported in part by the National Science Foundation under Grant
GK-23623, for which the authors are grateful.

Notation
thickness of the slot in a slit die
a position a t which maximum velocity is attained
material consistency of phases 1 and 2, respectively, in the power
law fluid
power law constant of phases 1 and 2, respectively
isotropic pressure
pressure gradient defined by - bp/bx
volumetric flow rate of polystyrene
volumetric flow rate of polypropylene
total volumetric flow rate
volumetric flow rate of phases 1 and 2, respectively
total normal stress in the y-direction of phases 1 and 2, respectively
velocity profiles of phases 1 and 2, respectively
width of the slot in a lit die
wall shear stress
apparent shear rate
true shear rate
fluid density
a location of phase interface

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 TWO-PHASE FLOW OF MOLTEN POLYMERS 1225

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Received August 4, 1972