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Time-dependent tube flow of compressible suspensions
subject to pressure dependent wall slip: Ramifications
on development of flow instabilities
H. S. Tang a) and Dilhan M. Kalyon b)
Stevens Institute of Technology, Castle Point St., Hoboken, New Jersey 07030
(Received 1 August 2007; final revision received 19 May 2008
Synopsis
A mathematical model developed earlier for the time-dependent circular tube flow of compressible
polymer melts subject to pressure-dependent wall slip
Tang and Kalyon, J. Rheol 52 , 507–525
was applied to the tube flow of polymeric suspensions with rigid particles. The model
relies on the apparent slip mechanism for suspension flow with the additional caveat that the
polymeric binder slips at the wall according to a pressure-dependent wall slip condition. The
numerical simulations of the tube flow of concentrated suspensions suggest that steady flow is
generated when the flow boundary condition at the wall is a contiguous strong slip condition along
the entire length of the tube wall. The findings of the simulations are consistent with the
experimental flow curves and flow instability data collected on suspensions of a poly dimethyl
siloxane , which itself exhibits wall slip, compounded with rigid and hollow spherical particles in
the 10–40% by volume range. Increasing the concentration of rigid particles gives rise to the
expansion of the range of flow rates over which the flow remains stable, as consistent with the
experimental observations. © 2008 The Society of Rheology.
2008
DOI: 10.1122/1.2955508
I. INTRODUCTION
The development of flow instabilities during the flow of concentrated suspensions of
rigid particles incorporated into polymeric binders in simple capillary dies
cylindrical
reservoir connected to a converging entry region into a straight circular tube
can involve
time-dependent changes in the concentration of particles or changes in the shape of the
extrudates emerging from tube flow. Time-dependent changes in the concentration of
particles generally occur on the basis of time-periodic oscillations in extrusion pressure,
upon the formation and break-up of mats of solids at the capillary entrance and the
filtration of the binder phase
. The time-
dependent changes in the concentration of rigid particles of extrudates of concentrated
suspensions become especially significant with decreasing binder shear viscosity
Yaras et al.
1994
; Rough et al.
2000
filtra-
tion based flow instabilities are especially prevalent with Newtonian binders
, increasing
particle size, increasing capillary convergence ratio
reservoir diameter over the tube
diameter
. On the other hand, with
increasing shear viscosity of the binder phase, concentrated suspensions exhibit time and
apparent shear rate-dependent changes in the shape of extrudates emerging from tube
, and decreasing flow rate
Yilmazer et al.
1989
a
Currently with City College, City University of New York.
b
Author to whom correspondence should be addressed; electronic mail: dkalyon@stevens.edu
© 2008 by The Society of Rheology, Inc.
J. Rheol. 52 5 , 1069-1090 September/October
2008
0148-6055/2008/52 5 /1069/22/$27.00
1069
1070
H. S. TANG AND D. M. KALYON
flow
akin to flow instabilities associated with various types
of extrudate shape distortions observed in the tube flow of polymeric melts
Birinci and Kalyon
2006
Benbow and
Lamb
1963
; Kalika and Denn
1987
; Denn
2001
; Robert et al.
2004
; Hatzikiriakos
and Migler
.
The effects of the presence and the concentration of rigid particles on the development
of shape distortions of the extrudates of suspensions are pronounced and contradictory.
For an elastomer that does not exhibit flow instabilities over a wide range of shear rates
in capillary or rectangular slit flows, the incorporation of particles induced extrudate
shape distortions over the same apparent shear rate range
2005
.On
the other hand, for other polymer melts that exhibit instabilities upon flow through cy-
lindrical dies, the incorporation of particles reduces the range of apparent shear rates over
which flow instabilities are observed at relatively low particle concentrations
Tang and Kalyon
2004a
Rosen-
baum et al.
2000
; Birinci and Kalyon
2006
and eliminates them altogether at rela-
tively high particle concentrations
. Currently, there is no
explanation for this type of contradictory behavior involving the induction or elimination
of flow instabilities upon the incorporation of particles into polymeric melts.
The slip-based theoretical treatment of the development of flow instabilities of poly-
mer melts in simple channels has generally relied on the considerations of the compress-
ibility and various empirical nonmonotonic wall slip velocity versus wall shear stress
expressions
Birinci and Kalyon
2006
Hatzikiriakos and Dealy
1992a
; Den Doelder et al.
1998
; Georgiou
. For polymeric liquids the pressure dependence of the wall slip velocity can be
significant
2003
Vinogradov and Ivanova
1967
; Hatzikiriakos and Dealy
1992b
; Person
and Denn
with the slip velocity decreasing with in-
creasing pressure. Since the flow curves characterized over relatively high apparent shear
rates are subject to wall slip, and since such slip is a function of wall shear stress, as well
as pressure, new methodologies, including the use of inverse problem solutions and
squeeze flow, are necessary for the characterization of the parameters of pressure-
dependent wall slip and shear viscosity material functions
1997
; Tang and Kalyon
2008
.
With suspensions the primary cause of wall slip is the apparent slip mechanism asso-
ciated with the formation of a pure binder or binder-rich apparent slip layer at the wall
Tang and Kalyon
2008
. In the following, first the analysis of the apparent slip mechanism of
concentrated suspensions is expanded to include the hitherto-neglected slip of the poly-
meric binder at the wall. Second, a mathematical model and corresponding numerical
simulation results of the time-dependent isothermal tube flow of compressible suspen-
sions with rigid spherical particles, subject to pressure-dependent wall slip, are provided
and applied to a model suspension at differing concentrations of rigid particles. Third,
procedures for the experimental determination of the parameters of pressure-dependent
wall slip and shear viscosity material function for suspensions
Reiner
1960
based principally on the
inverse-problem solution methodologies
are presented. Finally, the capillary flow data of
suspensions of a poly
, PDMS, incorporated with rigid spherical glass
particles, collected with relatively long capillary dies, are compared directly with the
time-dependent numerical simulation results of tube flow to elucidate the underlying
mechanisms for the development of flow instabilities for concentrated suspensions.
dimethyl siloxane
II. APPARENT WALL SLIP BEHAVIOR OF CONCENTRATED SUSPENSIONS
WITH RIGID PARTICLES
The wall slip behavior of the concentrated suspensions of rigid particles with rela-
tively low aspect ratios, incorporated into a non-Newtonian binder, is considered to occur
on the basis of the apparent slip mechanism subject to the wall slip of the polymeric
TIME-DEPENDENT TUBE FLOW OF SUSPENSIONS
1071
FIG. 1. Schematics of the apparent slip mechanism of suspensions with the binder liquid exhibiting slip at the
wall with slip velocity u sb .
binder
Fig. 1
. The apparent slip layer
Vand layer, i.e., a zone which is free of particles
and thus consists solely of the binder
has a thickness,
, at the wall. Since the thickness
of the slip layer,
, would be significantly smaller than the channel gap, the formation of
the slip layer gives the appearance of wall slip; hence the “apparent slip” at the wall
Reiner
1960
; Cohen and Metzner
1985
; Yilmazer and Kalyon
1989
; Kok Hartman
et al.
. This mechanism is depicted in an
exaggerated manner in Fig. 1 , which shows the apparent slip layer formed next to the
wall of the tubular die. Such apparent wall slip may or may not be significant in com-
parison to the mean velocity in the channel, i.e., constituting the weak versus strong wall
slip of the suspension. The rigidity of the particles can alter the dynamics of the forma-
tion of the apparent slip layer
2002
; Tabuteau et al.
2004
; Kalyon
2005
.
Unlike the earlier analyses in the treatment of apparent slip, here the binder itself is
also considered to be subject to a slip condition with the wall slip velocity of the poly-
meric binder, u sb , following a hyperbolic tangent-type dependence on the wall shear
stress,
Meeker et al.
2004
; Adams et al.
2004
w
Tang and Kalyon
2004a
; Tang and Kalyon
2008
:
b s 1
u sb =
0.5 + 0.5 tanh
w
c
,
1
where
b and s 1 are the slip coefficient
referred to as Navier’s slip coefficient for s 1
=1
and slip exponent of the polymeric binder, respectively, and
is a positive constant
describing the sharpness of the weak-to-strong slip transition in the slip
velocity of the polymeric binder at the critical wall shear stress,
typically 1–20
c .
, for viscoelastic polymer melts the slip
velocity should be a function of the pressure and the first and second normal stress
differences at the wall. For polymeric suspensions with rigid particles the development of
normal stress differences would also be affected by the formation of anisotropic particle
clusters
As noted by Hatzikiriakos and Dealy
1992b
. For the materials considered in
our experimental study the normal stress effects were determined to be small and only the
pressure effect is considered in our analysis. The slip coefficient for the binder,
Nott and Brady
1994
; Zarraga et al.
2000
b ,is
assumed to vary inversely with pressure, akin to the slip of compressible gases during
flow through simple conduits
Knudsen
1950
:
997727302.010.png
1072
H. S. TANG AND D. M. KALYON
,
p a
p
b =
0
2
where p is pressure at any location in the die, p a is the atmospheric pressure,
0 is the slip
coefficient of the binder at atmospheric pressure. The exponent
becomes equal to one
for Knudsen flow but needs to be determined experimentally for a polymeric melt
Tang
and Kalyon
2008
and its suspensions with rigid particles with
dependent on the
concentration of particles, i.e.,
. The available experimental data for polymer melts
Vinogradov and Ivanova
1967
; Hatzikiriakos and Dealy
1992b
indicate that the slip
coefficient decreases with increasing pressure
. The principal under-
lying mechanisms for pressure dependence of wall slip are considered to be the entrain-
ment of air into the binder phase of the suspension and the residence time dependence of
the establishment of the apparent slip condition as discussed later.
It is assumed that the Ostwald-de Waele or “power law” behavior represents the
behavior of
thus
is positive
the shear viscosity of
the binder phase in tube flow,
i.e.,
rz =
n b −1
m b
is the axial z velocity and m b and n b are the con-
sistency index and the power law index parameters of the Ostwald-de-Waele “power-
law” equation for the pure binder, respectively. The slip velocity, u s , for the apparent slip
mechanism
du
/
dr
du
/
dr
, where u
r
consists of the contributions of the slip of the binder, u sb , and the contribution of the
apparent slip mechanism, u sa :
Kalyon,
2005
subject to the slip of the binder at the tube wall
Fig. 1
u s = u sa + u sb = s b
s b +1
R
1− R
1−
+ u sb .
3
m s b
s b +1
Considering that the reciprocal power-law index of the binder, i.e., s b =1
n b , is positive
and assuming an integer value—the use of Binomial Theorem provides
/
s b +1
1−
/
R
R , the slip velocity at the interface between the apparent slip layer and the
bulk of the suspension, u s , i.e., at r = R
1−
s b +1
/
, becomes:
u s = u sa + u sb = s b
a s b + u sb ,
m s b
+ u sb =
4
where
a is the Navier’s slip coefficient resulting from the apparent slip mechanism, i.e.,
m s b
a =
/
Kalyon
2005
. A correlation for the apparent slip layer thickness,
, and the
m sb
Navier’s slip coefficient
a =
D p /
1−
/ m
can be used
Kalyon
2005
, where D p
is the particle diameter,
m is the maxi-
mum packing fraction of solids. This correlation for the mean value of the slip layer
thickness
is the volume percent of rigid particles, and
over the length of the die
applies for concentrated suspensions with rigid
particles exhibiting low aspect ratios at
m and suggests that the flow of the concen-
trated suspension approaches plug flow as
m . This is seen below from the simplified
analysis of the apparent wall slip of a Newtonian suspension with viscosity,
s and with
a Newtonian binder with viscosity
b and on the basis of a no-slip condition at the wall
for the Newtonian binder, which constitutes the apparent slip layer. The total flow rate, Q ,
versus the wall shear stress,
w , relationship for the apparent slip flow of a Newtonian
suspension in a tube with radius, R , becomes:
997727302.011.png 997727302.012.png
 
TIME-DEPENDENT TUBE FLOW OF SUSPENSIONS
1073
R 3
R 3
R 3
Q = Q s +
w
R 2 u s +
w
R 2
b w +
w
=
=
,
5
4
s
4
s
4
s
R 2
where Q s =
/ b w . The ratio of the flow rate due to slip Q s over the total flow rate,
Q , i.e., Q s /
Q , indicates the relative importance of wall slip at any wall shear stress,
w ,
and is given by:
b
R
Q s
Q =
=
.
6
b
R
4
R +
1
4
+
s
r
Upon replacing the relative viscosity of
the suspension,
r =
s / b , with
r =
1
−2.0
/ m
Krieger and Dougherty
1959
and the apparent slip layer thickness,
,
with
/
D p
=1−
/ m
Kalyon
2005
, Q s /
Q becomes
Q s
Q =
1
.
7
1+ R
4 D p
1−
m
Therefore, the application of the apparent slip mechanism to a Newtonian suspension
suggests that as
m , Q s /
1, i.e., the flow approaches plug flow with increasing
concentration of the rigid particles and that apparent slip has a negligible effect for
relatively small concentration of rigid particles, i.e.,
Q
D p . Such
plug flow behavior is indeed observed during the Poiseuille flow of Newtonian suspen-
sions with increasing
0, Q s /
Q
0 since R
.
Thus, with the contributions of the slip of the binder and the apparent slip mechanism
the apparent wall slip velocity, u s , of the suspension becomes:
, irrespective of the flow rate
Karnis and Mason
1967
s b .
p a
p
+ D p
m s b
1−
m
s 1
u s =
0
0.5 + 0.5 tanh
w
c
8
The rheological characterization of the polymeric binder provides
c .
Upon the characterization of the shear viscosity and the wall slip behavior of the binder
of the suspension and the physical properties of the rigid phase
0 , s 1 , s b , m b , and
the harmonic mean
particle diameter, D p , volume fraction,
, and maximum packing fraction of the particles,
m
the only unknown in Eq.
8
that describes the wall slip behavior of the suspensions
with the same binder is,
.
The typical slip velocity, u s , versus the wall shear stress and pressure behavior gener-
ated by Eq.
=0.2 is shown in Fig. 2 . Various properties
of this model suspension are listed in Table I . The wall slip velocity is affected by both
the pressure and the wall shear stress and undergoes significant changes at various critical
wall shear stress and pressure combinations representing the weak to strong slip transition
that Eq.
8
for a model suspension with
represents. Figure 2 suggests that if the critical pressure and the wall shear
stress conditions
8
were
to be encountered at any location along the length of the flow channel, significant
changes in the flow boundary condition at the wall will develop.
at which the slip behavior is converted from weak to strong slip
997727302.001.png 997727302.002.png 997727302.003.png 997727302.004.png 997727302.005.png 997727302.006.png 997727302.007.png 997727302.008.png 997727302.009.png
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