J. Non-Newtonian Fluid Mech.

102 (2002) 19–36

Influence of filters in the die entrance region on gross

melt fracture: extrudate and flow visualization
Yannick Goutille, Jacques Guillet∗
Laboratoire de Rhéologie des Matiéres Plastiques, FRE 2396 CNRS, Faculté de Sciences et Techniques, Université Jean
Monnet (UJM), 23 Rue du Docteur Paul Michelon, 42023 Saint-Etienne Cedex 2, France
Received 15 December 2000; received in revised form 29 April 2001

Abstract
The purpose of the present work is to analyze the influence of filters in the die entrance region on gross melt
fracture. Various experimental techniques will enable gross melt fracture to be identified and characterized. First,
capillary rheometer experiments have been performed with two natural linear and star-branched styrene butadiene
rubber copolymers (SBR). The succession and evolution of the different flow defects have been clearly identified.
Whatever the microstructure of the polymer melts is, it was found that filtering significantly reduces the severity of the
gross melt fracture defect. To explain the possible mechanism for the effect of the filters, rheological measurements
using a parallel-plate rheometer have been carried out. Then, we have reported flow visualization experiments on
the linear SBR copolymer through a transparent slit die attached to a capillary rheometer. Instabilities are generated
in the upstream region for the flow regimes at which melt fracture appears. By stacking filters at the die entrance,
the stream lines have been partially stabilized and the extrudate samples less distorted. Consequently, these results
emphasize that gross melt fracture is attributed to instabilities developing in the elongational flow field upstream
the die entrance. © 2002 Elsevier Science B.V. All rights reserved.
Keywords: Gross melt fracture; Filters; Extrusion defects; Flow instabilities; Polymer melts

1. Introduction

Over the past half century, many progresses have been realized in new materials, and in particular
in synthetic polymers. However, many processing operations including film blowing, melt spinning, or
cast film extrusion are still limited by the onset of flow instabilities. Extrusion defects which impose a
serious limitation in plastics processing rates have been extensively studied by many researchers [1–9].
All these experimental works have allowed to clarify many problems. However, there are still a lot
of unexplained points on the subject as the physical origin, the triggering criteria, and the physical
mechanisms.
∗
Corresponding author. Tel.: +33-477-481-550; fax: +33-477-485-126.
E-mail address: guillet j@univ-st-etienne.fr (J. Guillet).

0377-0257/02/$ – see front matter © 2002 Elsevier Science B.V. All rights reserved.
PII: S 0 3 7 7 - 0 2 5 7 ( 0 1 ) 0 0 1 2 5 - 2
20 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

The polymer can exhibit various extrusion defects depending on its nature [10] which can be classified
as a function of flow rate. The different types of instabilities, previously assigned to melt fracture were
clearly identified in a comprehensive review by Petrie and Denn [4]. At low flow rates, the first visually
detectable defect appears in the form of cracks on the surface of the extrudate. It is usually called surface
melt fracture or sharkskin. This phenomenon is often described as a high-frequency and small-amplitude
defect, although more severe distortions may be observed for very high molecular weight materials [7,11].
Now, it is well established that sharkskin is a surface instability which is initiated in the die exit region. At
higher throughput, the extrudate samples consist of a periodic alternation of smooth and sharkskin-like
sections. This surface defect is named the stick–slip or oscillating melt fracture. This leads to pressure
oscillations for controlled flow conditions or to sudden fluctuations in the flow rate for controlled pressure
conditions. It is now clear that the cyclic melt fracture is accompanied by slip at the wall. Once a certain
flow rate is reached, the extrudate becomes smooth and transparent as for the lower regimes [1]. It was
found that low concentrations of fluoropolymers added to the base polymer [12–14] or low surface energy
at the wall [15–17] can eliminate surface and stick–slip melt fracture. At the same time, these processing
aids increase the extruder performance and reduce energy cost.
At higher flow regime, gross melt fracture is characterized by larger irregular distortions in the extrudate
rod. At these high flow rates, it is no longer surface instabilities which rule the appearance of this
phenomena, but instabilities in the entry flow. So, most of the authors agree to consider gross melt
fracture as a volume instability.
Some authors [18,19] have emphasized that a slip between the polymer and the wall could be at the
origin of gross melt fracture. However, the extrudate samples can exhibit gross melt fracture before
the appearance of a macroscopic slip at the wall [10,17,20]. To eliminate or delay extrusion defects to
higher shear rates and thus increase the flow rate, processing aids are used. The effect of polymer/wall
interactions during gross melt fracture has been studied by analyzing the flow through dies made of
different materials or by adding additives to the polymer. However, they do not appear to have an effect
on gross melt fracture. In recent works, Hong et al. [21] and Rosenbaum et al. [22] have, respectively,
reported solutions to eliminate not only surface irregularities but also the gross melt fracture defect. Hong
et al. [21] have studied the use of hyperbranched polymers (HBPs) for linear low density polyethylene.
They have claimed that melt fracture and sharkskin were successfully eliminated. However, they have
only shown HBPs’ effect on surface defects like sharkskin. Rosenbaum et al. [22] have investigated the
influence of fines particles of boron nitride (BN) on the processability of polyolefins and fluoropolymers
in extrusion. The additive was reported to eliminate surface melt fracture and to delay the onset of gross
melt fracture. Actually, the addition of BN is not efficient to reduce the gross melt fracture defect in the
case of capillary dies. Boron nitride seems to delay gross melt fracture to higher flow rates with a special
annular die. However, the extrudate samples seem to exhibit surface melt fracture and not gross melt
fracture. Indeed, El Kissi and Piau [11] have shown that the magnitude of the cracks in the sharkskin
defect could be of the order of magnitude of the capillary diameter. Furthermore, the flow curves do not
depict the succession of the different extrusion defects. As a matter of fact, it is difficult to validate the
results obtained by Rosenbaum and co-workers.
Actually, the literature suggests that the region upstream the contraction is the site of initiation of
gross melt fracture [2–4,7,10,20,23]. The visualization of the stream lines with tracers, and birefringence
patterns have showed that upstream instabilities occur with gross melt fracture appearance. However, the
accurate mechanism governing these instabilities is not yet completely clear, and many researchers agree
that gross melt fracture may involve the interaction of several independent processes.
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 21

An examination of the published works on extrusion defects reveals that a decrease of the die entrance
angle allow to reduce the severity of the gross melt fracture defect [24–26]. This paper focuses attention
on the role of shear stresses and deformations in the die entrance region on flow instabilities. In particular,
we were interested in the effect of filters stacked in the die entrance region on the appearance and the
development of gross melt fracture. Similar studies have been driven by Done et al. [27] and Piau et al.
[28] to examine the effect of porous media of different filtering rates on the processability of polymer
melts. Done et al. [27] have first underlined the influence of porous media on the flow of polymer melts
in capillaries. The addition of porous media in the entry region was found to obviously increase the total
pressure drop. However, the porous media placed in the entrance of a capillary were found to decrease the
pressure drop across the capillary for a polystyrene with a long relaxation time. They have also shown that
the effective pressure drop across the capillary die depends on the distance between the porous media and
the die entrance. For a polyethylene terephthalate with a short relaxation time, no significant reduction
in the pressure drop across the capillary was found. Finally, porous media in the entrance of the die
allow to delay the onset of gross melt fracture to higher shear rates. Done et al. [27] have attributed these
results to chain disentanglement of the polymer through the porous medium which temporarily changes
the rheological properties of the polymer melt. Piau et al. [28] have investigated porous media during
the extrusion of a high-density polyethylene and a polydimethylsiloxane oil. Porous media have been
found to affect the oscillation regimes which appear when a simple die was used. Thus, the flow curves
do not show anymore discontinuity or hysteresis. Photographs of the extrudate rod taken right at the die
exit show that this gross melt fracture defect is mitigated, since its frequency is higher and its amplitude
smaller than without porous medium. Furthermore, porous medium with a high filtering rate allows to
delay the occurrence of gross melt fracture. Piau and co-workers considered that the introduction of a
porous medium in the die entrance region modifies the flow geometry, combining thus elongational strains
with pre-shearing that leads to mitigation of gross melt fracture.
Series of extrusion experiments have been achieved in a capillary rheometer with two well-defined
styrene butadiene rubber copolymers. It was shown that setting filters in the die entrance region leads to
reduction of gross melt fracture. Another purpose of the study is to get a better insight in the physical
origin of this defect. By setting filters in the die entrance region, we have also tried to show the importance
of this region on the appearance of gross melt fracture. In order to visualize the polymer flow at the die
entrance, a two-dimensional die with lateral windows have been specifically designed. Lastly, rheological
measurements were performed to study the effect induced by the filters on the processability of the SBR
copolymers.

2. Experimental set-up

2.1. Fluids used

Two styrene butadiene statistic copolymers (SBRs) with linear and star-branched microstructure were
supplied by MICHELIN. Their chemical formula is given as follows:
22 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Table 1
Main characteristics of the two SBR copolymers studied
Microstructure Tg (◦ C) Density Styrene (%) M w (g mol−1 ) Ip

Linear −53 0.936 26 140 × 103 1.08

Star-branched −53 0.933 25 91.2 × 103 1.29

Conversely to rubber compounds, they contain no fillers (carbon black or silica) and no additives
(plasticisers, lubricants, or processing aids) which lead to complex heterogeneous materials with spe-
cific rheological properties. Their chemical characteristics are given in Table 1. The samples are suf-
ficiently fluid at room temperature to allow experiments at 30◦ C. Moreover, these are transparent and
birefringent.

2.2. Rheological characterization equipment

2.2.1. Capillary die apparatus

Most experiments were carried out with a capillary rheometer at 30◦ C. Both SBR copolymers have
been extruded through tungsten carbide axisymetrical dies. The rheometer is a SWO (Rheo) piston-driven
constant speed capillary unit with a standard barrel of 9.5 mm diameter. The abrupt circular dies used have
different capillary diameters (1 or 2 mm) and different L/D ratios (5, 10, or 30). Prior to each experiment,
the polymers have been degassed under vacuum for 3 days at 90◦ C.
The total pressure drop was measured by a transducer placed at the bottom of the reservoir. For each
flow rate, enough time was allowed to ensure that a steady regime has been reached and to check the
pressure loss and the photos of the extrudate samples. The photographs were extracted from a video
recording film of the extrudate samples just downstream of the die exit. The lighting used was a 10 W
lamp focused by a convex lens.

2.2.2. Slit die apparatus

A transparent slit die was specially designed to visualize the polymer flow at the die entrance. The
die was attached to the SWO capillary rheometer. The sample is driven through the two-dimensional slit
die by the piston movement in the barrel of the capillary rheometer. When the piston travels down at
a given speed, it generates an apparent shear rate at the slit die wall that can be deduced from the die
dimensions:
6Q
γ̇app = ,
H 2W
where W and H are, respectively, the width and the height of the slit die, and Q the volumetric flow
rate.
The dimensions of the two-dimensional die are given in Fig. 1. The contraction ratio between the
reservoir and the die is 8:1. The die wall has a high surface energy (stainless steel). The front side of
the reservoir and the die is covered by a 25 mm thick glass windows. In order to visualize the upstream
and downstream flow, silicium carbide particles (13 ␮m in diameter) were introduced in the material as a
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 23

Fig. 1. Schematic diagram showing dimensions of the transparent slit die.

tracer. Such low level of silicium carbide loading does not affect the rheological behavior of both polymer
melts. These particles are illuminated using a lamp focused by a convex lens. The slit die was also designed
to allow the visualization of the extrudate samples at the die exit region. All the experiments were carried
out at 30◦ C.

2.2.3. Parallel-plate apparatus

A dynamic stress rheometer (SR-5000, Rheometric Scientific) was used for rheological measurements.
The stainless steel parallel plates of the rheometer were 25 mm in diameter, while the gap between the
two plates was in the range of 1–1.05 mm. Stress tests were carried out on all samples prior to frequency
tests in order to ensure the measurements to be recorded within the linear viscoelastic domain. The
stress applied during the frequency sweeps was 1000 Pa. All runs were performed at 30◦ C, within a
frequency range of 100–10−4 rad s−1 . The samples used in these experiments were obtained from the
extrudate rods after extrusion through different filter stacks in a capillary die (L/D = 10 and D = 1 mm)
at 30◦ C.

2.3. Filters

The filters were constituted by cylindrical stainless steel wires whose characteristics are given in
Table 2. They are generally used for filtering of polymer melt during processing operations. Indeed,
industrial products often contain solid particles which damage the quality of the final parts. This filter-
ing operation eliminates undesirable particles and ensures homogenization of the product. So, one can
reduce the breaks of production and the scraps. These wires form a square mesh which is defined by
its nominal opening, NO, and its step, P (Fig. 2a). The nominal opening is the distance between two
24 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Table 2
Geometrical characteristics of the filters used
References NO (␮m) φ wire (␮m) P (␮m) T (%)

MN 446 100 71 171 36

IAN 1110 250 160 410 42

consecutive wire of the mesh. The step is obtained by adding the nominal opening to the wire diam-
eter. As illustrated in Fig. 2b, every wire passes successively above and below the crosswire with an
unwed of one wire for every cycle to form the gauze. For a square mesh, the transparency percentage is
given by

NO2
T (%) = × 100.
P2

For each experiment, the wire gauze was placed in the reservoir, right at the flat die entrance of the
capillary dies.

Fig. 2. (a) Dimensions of the square mesh; (b) representation of the wire gauze.
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 25

3. Results and discussion

3.1. Capillary rheometer experiments

3.1.1. Linear SBR copolymer

Fig. 3 illustrates the different aspects of the linear SBR copolymer obtained from the SWO capil-
lary rheometer (D = 2 mm, L/D = 10). Initially, surface melt fracture invaded the entire surface
of the extrudate. For an apparent shear rate of 0.2 s−1 , the extrudate alternatively exhibits smooth and
sharkskin-like sections. This defect leads to oscillations in the instantaneous pressure between two val-
ues. A super-extrusion region exists just before the gross melt fracture regime; here the extrudate appears
smooth and transparent. This region begins at the apparent shear rate of 0.4 s−1 and ends at 1 s−1 . As the
throughput increases, the extrudate instability becomes more and more severe.
The flows curves and the extrusion defects of the linear SBR copolymer obtained with different capillary
dies (D = 2 mm, L/D = 10 or 30), with or without filters at the die entrance, are given in Fig. 4. When
considering the flow curves obtained with two filters stacked at the die entrance (D = 2 mm, L/D = 10),
some differences appear. First, at the apparent shear rate corresponding to the occurence of the oscillating
defect, the surface of the extrudate rods exhibits cracks and local slip. As already observed by Piau et al.
[28], the transition from stable regimes to flow regime with slip takes place progressively. Note that the
critical apparent shear rate corresponding to the triggering of gross melt fracture was slightly delayed to
higher shear rate. It was also found that the apparent shear rate at the onset of gross melt fracture was

Fig. 3. Extrudate samples of the linear SBR copolymer extruded through a capillary die (D = 2 mm, L/D = 10, T = 30◦ C):
(a) γ̇app = 0.1 s−1 ; (b) γ̇app = 0.2 s−1 ; (c) γ̇app = 0.4 s−1 ; (d) γ̇app = 8 s−1 .
26 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Fig. 4. Flow curves and extrusion defects of the linear SBR copolymer through capillary dies having D = 2 mm, L/D = 10
and 30 at T = 30◦ C, with and without filter stacks at the die entrance.

higher for the die with L/D = 30 than for the die with L/D = 10. It must also be underlined that the total
pressure drop in the L/D = 30 die is more important than that of the L/D = 10 die with the different
filters stacked at the entrance.
Photographs of the corresponding extrudate samples of the linear SBR copolymer are given in Fig. 5.
The extrudate rod visualization have been realized just at the die exit to avoid any perturbation due to
relaxation processes. It is important to note on the flow curves (Fig. 4) that for an apparent shear rate
of 6 s−1 , the extrusion conditions correspond to gross melt fracture regimes. Fig. 5a and b show the
effect of the length-to-diameter ratio on the processability of the linear SBR copolymer (D = 2 mm,
α = 180◦ C, L/D = 10 and 30). It can be seen that the rise in length-to-diameter ratio slightly reduces
the gross melt fracture severity and oscillations of the extrudate rod. It must be pointed out that the
polymer melt has more time to relax in the long die. These could explain why gross melt fracture
arises at higher shear rates in the L/D = 30 die. Indeed, by increasing the capillary length, part of the
flow instabilities have been damped out. The stream lines have more time to be stabilized through the
longer die and thus the cross-sectional variations are less noticeable at the die exit. However, this length
increase results in a pressure loss increase in the die entrance region from 16 × 106 to 43 × 106 Pa.
To study the effect of the stainless steel filters on gross melt fracture, the linear SBR copolymer was
first extruded with three filters with NO = 250 ␮m. It can be seen in Fig. 5c that with three filters,
the diameter of the rod is almost constant at shear rate, where the extrudate (extrusion without filter)
would normally exhibit gross melt fracture in the L/D = 10 and 30 die without filter. It seems that the
volume flow defect has been removed but surface defect, whose origin is quite different, still remains.
Moreover, the pressure loss is only of 25 × 106 Pa. When reducing the nominal opening of the filters from
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 27

Fig. 5. Effect of the filters at the die entrance on the processability of the linear SBR copolymer obtained in capillary dies with
D = 2 mm at γ̇app = 6 s−1 and T = 30◦ C: (a) without filter and L/D = 10; (b) without filter and L/D = 30; (c) with three
filters (NO = 250 ␮m, φ = 160 ␮m) and L/D = 10; (d) with three filters (NO = 100 ␮m, φ = 71 ␮m) and L/D = 10.

250 to 100 ␮m (Fig. 5d) to enhance the shear deformations at the die entrance, we do not observe any
improvement, although the overall stack height is shortened for the same number of filters. In the best case,
the pressure drop is equal to about 30 × 106 Pa. Despite these problems, it was found that there exists an
optimal composition for the stacks, which permits to eliminate gross melt fracture for reasonable pressure
losses.

3.1.2. Star-branched SBR copolymer

Fig. 6 describes the influence of the die length on the processability at 30◦ C of the star-branched SBR
copolymer, with dies of dimensions, D = 1 mm, L/D = 10 or 30, with or without filters. The succession
of the different extrusion defects is depicted. Here again, the onset of surface melt fracture (sharkskin) is
found to be independent of the die length. Just before the gross melt fracture region, a narrow zone exists
where the extrudate rods appear almost smooth and transparent. The triggering of gross melt fracture was
indicated by a slope change on the flow curve. Fig. 6 shows that increase in die length slightly shifts the
apparent shear rate corresponding to the onset of gross melt fracture from 50 to 60 s−1 .
The photographs of the star-branched SBR copolymer depict the effect of the filtration in comparison to
the die length on gross melt fracture (Fig. 7). First, increasing the length improves the processability of the
polymer by erasing part of the cross-section distortions even if the extrudate rod is still rough. However,
best results were obtained with filters having NO = 250 ␮m and φ = 160 ␮m. Fig. 7c and d shows that
increasing the number of filters from three to five reduces the magnitude of the residual distortions for the
star-branched SBR copolymer samples. Here again, it must be underlined that the pressure loss is more
28 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Fig. 6. Flow curves and extrusion defects of the star-branched SBR copolymer through capillary dies having D = 1 mm,
L/D = 10 and 30 at T = 30◦ C, with and without filter stacks at the die entrance.

Fig. 7. Effect of the filters at the die entrance on the processability of the star-branched SBR copolymer obtained in capillary dies
with D = 1 mm at γ̇app = 100 s−1 and T = 30◦ C: (a) without filter and L/D = 10; (b) without filter and L/D = 30; (c) with
three filters (NO = 250 ␮m, φ = 160 ␮m) and L/D = 10; (d) with five filters (NO = 250 ␮m, φ = 160 ␮m) and L/D = 10.
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 29

important with L/D = 30 die (p = 69 × 106 Pa) than with the L/D = 10 die with five filters stacked
(p = 45 × 106 Pa). For an apparent shear rate of 100 s−1 , the total pressure loss is about 80% higher
than the L/D = 10 capillary die without filtration when considering the flow through five filters and
L/D = 10 die. However, the pressure increase is much more important when the L/D = 30 capillary
die is considered in comparison to the L/D = 10 die. In this case, the total pressure drop is about 180%
higher. So, the small differences obtained are still interesting, and the influence of the filters on the gross
melt fracture defect cannot be assimilated to an artificial increase of the die length.

3.2. Rheological properties

In our point of view, the increase of the shear strain and of the total pressure loss induced by the filter
stacks in the die entrance region could have modified the rheological properties of the SBR copolymers.
These effects have first been studied on the linear SBR copolymer in steady-state shear flow experiments
with the SWO rheometer. The number of filters and the apparent shear rate have been determined to
work at higher pressure than that encountered in the previous experiments. The samples used in these
experiments were obtained after extrusion with different filter stacks in a capillary die whose dimensions
are L/D = 10 and D = 1 mm at 30◦ C and for an apparent shear rate of 25 s−1 . For this given apparent
shear rate, the total pressure losses were, respectively, 19×106 , 32×106 , and 41×106 Pa when considering
the flow through the capillary die without filter, with five filters having NO = 250 ␮m and with three
filters having NO = 100 ␮m. These results imply that the total pressure drop was about 1.5 times higher
with five filters having NO = 250 ␮m, and two times higher with three filters having NO = 100 ␮m than
that obtained for flow through the capillary die without any filter. Fig. 8a represents a superposition of
the flow curves of the samples submitted to different extrusion conditions. It is clear that the rheological
properties of the linear SBR copolymer are not modified by extrusion through the filter stacks. The same
extrudate samples were also studied with a dynamic stress rheometer. Fig. 8b represents the variations of
the dynamic moduli and of the complex viscosities, and it can be seen that all the curves are superposed.
This is true even at very low frequencies, so that it is possible to claim that the samples did not undergo
structure modification during the extrusion process.
Similar results, not presented in this paper, were obtained with the star-branched SBR copolymer.
As a conclusion, whatever the material considered, the effect of filters on gross melt fracture cannot
be explained by a permanent change in rheology. These results are in agreement with the literature
[28].

3.3. Two-dimensional flow experiments

3.3.1. Flow curve and extrudate visualization

The flow curve of the linear SBR copolymer obtained from the stainless steel slit die (W = 25 mm,
H = 1 mm, L = 10 mm) at 30◦ C is given in Fig. 9a. The succession and evolution of the different
extrusion defects have been clearly identified. Fig. 9b shows photographs of the extrudate samples for the
different extrusion regimes just at the die exit. One can see in Fig. 9b(i) that superficial scratches appear
on the surface of the extrudate. They are localized on bands parallel to the flow direction. These scratches
gradually invade the surface of the extrudate as the shear rate increases. The sample becomes progressively
dull and opaque. However, we have never seen lines of cracks rectilinear and perpendicular to the flow
direction. For an apparent shear rate of 0.7 s−1 , the extrudate appears almost smooth and transparent
30 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Fig. 8. Effect of high pressure on rheological properties of the linear SBR copolymer: (a) flow curves obtained in a capillary
rheometer having D = 1 mm, L/D = 10 at T = 30◦ C; (b) dynamic moduli, G and G , and complex viscosity, η∗ , obtained in
a dynamic stress rheometer at T = 30◦ C.

(Fig. 9b(ii)). In Fig. 9b(iii), the extrudate leaving the die begins to exhibit the gross melt fracture defect.
As the flow rate increases, the extrudate distortion becomes gradually more pronounced (Fig. 9b(ii–vi)).
In particular, Fig. 9b(v and vi) illustrates the chaotic aspect of the extrudate for an apparent shear rate of
5 s−1 with two different shoots.
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 31

3.3.2. Flow visualization

Upstream flow visualization of the linear SBR copolymer was examined for regimes covering the
portion of gross melt fracture. Fig. 10 represents the polymer flowing through the transparent slit die at an
apparent shear rate of 15 s−1 . These photographs have been chosen to depict the flow instabilities in the
die entrance region. Time scale between two pulsations on the same side (Fig. 10b–d) is about 3 s. The
visualization of the particle tracers in the polymer melt shows that the flow is unstable and asymmetric
in the die entrance region. Moreover, the flow is nonlaminar in the slit die. In order to illustrate our
observations, the different parts of the flow are underlined with black lines. The arrows indicate the
direction of the polymer melt flowing. Note that vortices are not observed in the die entrance corners
when the extrudate exhibits gross melt fracture at the die exit. One can see in Fig. 10a that the linear
SBR copolymer enters in the die by the right area of the reservoir. On the other hand, the left part is
clearly held up and the polymer flows back (little black arrow). This sequence was chosen because of
the black trail formed by silicium carbide particles in the left area of the photographs. In the photograph
shown in Fig. 10b, the left part can flow in the die, while the right area flows back in the reservoir. This
phenomenon is illustrated by the lengthening of the black trail which is submitted to high extensional
strains. So, the area which has been flowing through the die retracts, and the polymer melt from the
other area of the upstream flow field can enter in the die. The same mechanism is observed in the other
photographs. Fig. 10c clearly shows the back flow of the carbide particle trail which was fractured when
the other part of the upstream flow field entered in the die. In the photograph depicted in Fig. 10d, the
black trail is again submitted to high elongational stresses like in Fig. 10b.
In a second step, flow visualization was carried out to study the flow behavior of the linear SBR
copolymer, as it is processed through the abrupt slit die with and without filters (Fig. 11). For regime

Fig. 9. (a) Flow curve and (b) extrudate samples of the linear SBR copolymer extruded through the slit die (W = 25 mm,
H = 1 mm, L/H = 10, T = 30◦ C): (i) γ̇app = 0.1 s−1 ; (ii) γ̇app = 0.7 s−1 ; (iii) γ̇app = 1.5 s−1 ; (iv) γ̇app = 3 s−1 ; (v) and (vi)
γ̇app = 5 s−1 .
32 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Fig. 9. (Continued).

corresponding to the formation of gross melt fracture, the flow upstream the die entrance is completely
asymmetric. Fig. 11a and b shows photographs of the upstream flow conditions taken at two different
times for a shear rate of 10 s−1 . The photos clearly exhibit the disturbance of the polymer at the die
entrance and the nonlaminarity of the flow through the slit die. The polymer flows into the die through
an asymmetric and unstable cone. One can see that the polymer enters alternatively in the slit die by
two different parts of the reservoir. These pulsations occur at regular intervals. Time scale between two
pulsations that occur on the same area is about 4 s. It is confirmed that the gross melt fracture defect
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 33

Fig. 10. Stream lines visualization of the linear SBR copolymer flowing through the transparent slit die at γ̇app = 15 s−1
(W = 25 mm, H = 1 mm, L/H = 10, T = 30◦ C).

and the flow instabilities occuring upstream of the die entrance are completely dependent on each other
[7,9]. The path of the encircled carbide particle also illustrates these flow instabilities. Indeed, the carbide
particle passes from one side in the die entrance region to the opposite side in the slit die.
Fig. 11c and d shows photographs of the flow in the same extrusion conditions when adding one filter
having NO = 250 ␮m at the die entrance. The flow is now symetric and one can see in the photographs
34 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36

Fig. 11. Stream lines visualization of the linear SBR copolymer flowing through the transparent slit die at γ̇app = 10 s−1
(W = 25 mm, H = 1 mm, L/H = 10, T = 30◦ C): (a) and (b) without filter; (c) and (d) with one filter (NO = 250 ␮m,
φ = 160 ␮m).
 Y. Goutille, J. Guillet / J. Non-Newtonian Fluid Mech. 102 (2002) 19–36 35

that the filter stabilizes the stream lines that reduces the magnitude of gross melt fracture. This result
is in agreement with the capillary rheometer experiments previously described. We must underline that
small pulsations in the die entrance region still remain, whose time scale is 3.5 s. These small pulsations
cannot be compared to the previous ones, when no filtration was considered and when the entire flow was
perturbed by their occurrence (Fig. 11a and b). As we still observe small velocity fluctuations, we cannot
claim that the flow is fully stable. Indeed, we expect that a subsequent stack of filters should remove
these small velocity fluctuations. Unfortunately, pictures of the upstream flow obtained with three filters
are not available because of problem arising from high pressure which provokes window breaks. In this
case, the path of the carbide particle (black circle) is much more stable than when considering the flow
without filtration (Fig. 11a and b). Done et al. [27] have suggested a mechanism of chains disentanglement
through the porous medium to explain the observed effects. In our paper, flow visualization experiments
have clearly shown that filters do not only influence the flow in the die land but also mitigate upstream flow
instabilities, mainly because of a new balance between shear and extensional strains at the die entrance.

4. Conclusions

The flow of two SBR copolymers through various dies was observed in order to study extrusion detects.
Capillary rheometer and two-dimensional flow experiments enabled gross melt fracture to be studied and
characterized. It must be underlined that it is possible to significantly reduce the severity of gross melt
fracture by setting filters in the die entrance region. Steady-state shear flow experiments and oscillatory
shear experiments have shown that the effect of filters on gross melt fracture cannot be explained by
modification in the equilibrium rheological behavior. Flow visualization has been used to study the flow
behavior of the linear SBR copolymer, as it is processed through a transparent slit die with and without
filters. The filters allow to stabilize the stream lines and to reduce the amplitude of gross melt fracture. So,
by enhancing the shear deformations with respect to elongational deformations, it is possible to reduce
the severity of gross melt fracture.
To summarize, the importance of the die entrance region on the apparition and the development of gross
melt fracture have been outlined. Their occurrence and evolution are influenced by the modification of the
stress fields provoked by the filter stacks in the entry zone. Whatever the polymer melts microstructure
were, filters were found to minimize the magnitude of the gross melt fracture defect. This method could
be used to improve the processability of polymer melts in terms of quality and productivity. To go further
in the understanding of the physical origin of the gross melt fracture defect, the quantification of the
elongational stresses in the die entrance region should be realized.

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