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Book Cover Bi-Axially Oriented Blown Film Technology
Book Cover Bi-Axially Oriented Blown Film Technology
cess. Bubble stability and thickness uniformity were assumed tation speed of the nip rolls (axial direction) and air pressure in-
as the main requirements for processability. The former was side the bubble (transversal direction). Takashige et al. (2003,
estimated by monitoring the time required to stabilize the bub- 2004a, 2004b, 2005, 2011) cited a series of studies of the double
ble and examining any variation/oscillation in size/shape. Bub- bubble technology, as well as of the processability, properties
ble stability depends on the interaction between various pa- and morphology of various polymers to be used in this process.
rameters, the most relevant being those related with the film
IPP 2012.27:348-357.
348 Carl Hanser Verlag, Munich Intern. Polymer Processing XXVII (2012) 3
O. S. Carneiro et al.: Bi-axially Oriented Blown Film Technology
onments created by the two technologies. Therefore, this work stress was adjusted to ensure that the measurements were per-
has the following two objectives: i) to investigate whether the formed within the linear viscoelastic regime. The discs for the
feasibility of materials for bi-axial film blowing can be antici- experiments were prepared by compression moulding at
pated in the laboratory, namely via rheological measurements, 190 8C, under a pressure of 20 t.
and ii) to study the effect of operating and machine variables The uniaxial melt strength was determined with a Göttfert
on processability. This work will be developed for the process Rheotens 71.97 device kept at a vertical distance of 100 mm
variant involving the extrusion of a tube followed by its bi-axial from the die exit of a Göttfert Rheo-Tester 2000 capillary rhe-
stretching, as a prototype laboratory equipment is available and ometer. The melt was extruded downwards (either at 190 8C, or
was validated previously (Carneiro et al., 2008). at 30 8C above the polymer melting temperature) with a ram
speed of 32 mm/s through a circular die with a diameter of
2 mm and a length of 30 mm, and then drawn axially by the ac-
2 Experimental celerating pair of counter-rotating rollers (set to 120 mm/s2).
The tensile force applied was plotted against the rollers velocity.
2.1 Materials The maximum force reached during the experiment was taken
as the melt strength and the corresponding velocity as the melt
Six commercial polyethylenes, most of them suggested by an extensibility (Wagner and Bernnat, 1998).
industrial manufacturer of bi-axially oriented films, were se-
lected for this study. They are produced by Total Petrochem-
icals, Polimeri Europa, Dow Plastics and Ineos Polyolefins. 2.3 Bi-oriented Blown Film Production
As seen in Table 1 where their main characteristics are pre-
sented, three are low density polyethylenes (coded LDPE 1, 2 The experiments were conducted in a prototype line designed to
and 3) and the remaining three are linear low density polyethy- produce bi-oriented and conventional blown films. The compo-
nents used in this study are schematically represented in Fig. 1.
by Kungliga Tekniska on August 28, 2015. For personal use only.
lenes (coded LLDPE 1, 2 and 3). The melt flow rates are simi-
lar, ranging between 0.25 and 0.80 and 0.75 and 1.00 g/ The two single screw extruders have a screw diameter (D) of
10 min for the LDPE and LLDPE, respectively. Therefore,
comparable viscosities at shear rates of the order of 1 s–1 are
anticipated. In the case of LLDPE, the densities and MFI match
well those of the grades selected by other authors studying the
IPP 2012.27:348-357.
*Melt flow index (at 190 8C/2.16 kg). (1) Data from polymer datasheet. (2) Determined from DSC (heating rate of 10 8C/min)
Table 1. Main characteristics of the polymers used
tion between them (see pipe at the lower part of Fig. 2A). In
each experiment, the pipe was quickly raised and immobilized
in its position inside the bi-orientation oven (already kept at a
stabilized temperature), the temperature evolution of the
square elements being recorded during 20 s.
During film production the die was kept at 210 8C, the
throughput at 4 kg/h, and the distance between the die and the
water ring was maintained at 37 mm. The water flow rate in the
water ring and calibrator was regulated to 120 l/h and 100 l/h, re-
spectively. The following processing parameters were varied:
i) Temperatures of the re-heating ovens;
ii) The primary tube take-up ratio (TURP), given by:
TURP = velocity of the 1st pair of pulling rolls/extrudate
B)
velocity at die exit. (1)
Fig. 2. Re-heating ovens: A) pre-heating (HR1 and HR2) and bi-ori-
iii) The film blow up (BURF) and take-up (TURF) ratios, de- entation (HR3 to HR5) ovens, B) thermogram of the bi-orientation
fined as: oven (set to 200 8C)
BURF = bubble diameter/primary tube diameter. (2) The thickness distribution of the primary tube and films was
rd measured with a digital micrometer both along the lay-flat
TURF = velocity of the 3 pair of pulling rolls/velocity of
width (at 12 and 22 positions equally distanced, respectively)
the 2nd pair of pulling rolls. (3)
and at axial increments of 20 cm. A homogeneity index (in per-
Practice has shown (Carneiro et al., 2008) that BURF centage) was calculated from the relative standard deviation:
should be kept preferably between 3 and 5, as lower values Homogeneity index (%) =
would yield a too thick film, outside the range of practical (1 – standard deviation/mean thickness) · 100. (4)
interest, while higher values would imply a too wide film
(the useful length of the pulling rolls is 300 mm). TURF
should obviously stay within the same limits if balanced 3 Results and Discussion
orientation is required.
iv) The cooling conditions, including the vertical position of 3.1 Rheological Properties of the Melts
the upper air ring, air flow rate and air velocity (controlled The rheological ability of the candidate materials to the double
by the gap of the upper ring). bubble technology should be estimated from the characteristics
of their response to shear and extensional stresses, which are ethylenes studied in terms of complex viscosity and loss tan-
determinant for the extrusion and blowing stages, respectively. gent (tan d). As expected, the complex viscosity of all materials
Fig. 3 presents the linear viscoelastic response of all the poly- is comparable in the range 0.3 to 1 Hz, but the behaviour of the
LDPEs is quite distinct from that of the LLDPEs. LDPE1 and
LDPE 3 exhibit the highest viscosity values at low frequencies
and a pronounced shear thinning behaviour that should be fa-
vourable to the extrusion step, since the die gap is relatively
small and power consumption should be minimized (the valid-
ity of the Cox-Merz rule is assumed here). The relative degree
of shear thinning is presented in Table 2, defined as the ratio
of the viscosities at 0.01 (where a Newtonian plateau is ob-
served) and 100 Hz. As most conventional polymer melts, the
materials show an elastic dominated response (tan d < 1) at
the higher frequencies and a viscous dominated behaviour
(tan d > 1) at the lower frequencies. Fig. 4 plots the crossover
modulus (at tan d = 1) against the crossover frequency. Since
polymers showing low values of the cross-over frequency have
higher elasticity and higher characteristic relaxation times
(Larson, 1988), it is expected that they will induce higher bub-
ble stability (Fang et al., 2003; Leal et al., 2006) and improved
orientation levels (Johnson et al., 2000). As seen in Fig. 4, the
A) LDPE resins have considerably lower values of the crossover
modulus and crossover frequency than the LLDPE resins.
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IPP 2012.27:348-357.
B)
Fig. 3. Linear viscoelastic response of all materials at 190 8C, A) com- Fig. 4. Crossover modulus versus crossover frequency for all materi-
plex viscosity, B) loss tangent als (at 190 8C)
Degree of shear thinning (g100/g0.01) 28.7 18.4 25.7 2.7 6.3 1.3
Among the LDPEs, LDPE1 and LDPE3 are the most elastic, 3.2 Effect of Machine Performance
which could be attributed to their higher average molecular
weight (as inferred from their lower melt flow rates, see Ta- As discussed above, the two sets of data on the variation of the
ble 1). Table 2 compares the crossover frequency of all the ma- uni-axial forces with increasing pulling velocities represented
terials. in Fig. 5 were obtained at two temperatures nearly 50 8C apart
The uni-axial forces measured by the Rheotens and the cor- (explicitly, at 142 8C and 190 8C for the LDPE). For each poly-
responding pulling speeds are depicted in Fig. 5 for two testing mer, the maximum force decreases with increasing test tem-
temperatures (more precisely, set temperatures of the capillary perature, but the strain-hardening characteristics of the LDPEs
rheometer). For each polymer, these were 190 8C and a tem- and the maximum velocities attained remain similar. There-
perature 30 8C above its melting temperature, as measured by fore, one would expect that some materials could allow for cer-
Differential Scanning Calorimetry (see Table 1). Since the tain flexibility in terms of viable process operating conditions.
Rheotens requires testing a melt, the second temperature corre- However, practice (both at the laboratory and industrial scales)
sponds to the minimum feasible value. The corresponding melt has demonstrated otherwise, i. e., that the operating window of
strengths and melt extensibilities are identified in Table 2. Not the double bubble process is usually quite narrow, particularly
surprisingly, the LDPEs exhibit the highest force/melt strength concerning the bi-orientation stage. The scientific literature
and extensibility, LDPE1 and LDPE3 showing the highest melt supports these conclusions: for example, Uehara et al. (2004a)
strength. varied extensively the set temperature of the pre-heating oven,
Consequently, shear and extensional measurements seem to but were only able to produce stable LLDPE films within an in-
indicate that LDPE1 and LDPE3 appear as the best candidates terval of 15 8C, corresponding to differences in film tempera-
for bi-axial orientation blown film processing. ture of 8 8C after the pre-heater. Therefore, it seems important
to assess whether equipment design/operation/control limita-
tions may offset the eventual flexibility allowed by the materi-
als, thus creating the observed practical operating difficulties.
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B)
Fig. 5. Rheotens data (uniaxial force versus pulling rolls velocity) for Fig. 6. Temperature evolution with time at two surface locations of a
all materials, A) T = Tm + 30 8C, B) T = 190 8C ceramic heater set to 200 8C
rate, the localized film over-thickness in the region of 2558 laboratory extrusion line used in this work showed that bubble
causes a deterioration of 2.7 % in the homogeneity index). stability depends on the interaction between the re-heating
The value of 98.3 % for the homogeneity index of the primary temperature, the stretching ratios (TURP, BURF and TURF)
tube is quite good – it corresponds to 2.5 % if calculated using and the cooling conditions (vertical position of the air rings,
the definition adopted by Takashige et al. (2004b), who ob- air flow rate and air velocity), which is in agreement with the
tained a value of 4 %. Similarly, values of 88.7 and 93.1 % for observations of Takashige et al. (2004a), even if using another
the film correspond to 25 and 13 % using the other definition, variant of the double bubble technology.
which are well within the range obtained by the same authors. Air flow rate seems to have the highest effect. For example,
Nevertheless, the decrease from 98.3 to 88.7 and 93.1 corre- using higher air flow rates limits the maximum TURP to 4.5
sponds to an amplification factor of the non-uniformity of 5 – and BURF and TURF to 3.5, requires the re-heating ovens to
10 using again the alternative definition, which is much larger be set around 340 8C and 360 8C (pre-heating and bi-orienta-
than the above suggested value of 2. tion, respectively) and that the top air ring is at least 0.1 m
For LLDPE, Uehara et al (2004a) reported fluctuations of away from the re-heating oven. Conversely, if the air flow rate
the transversal bubble deformation of the order of 20 %, which is sufficiently low, the onset of bi-orientation shifts from the
should induce significant thickness variations in the stretched outlet of the bi-orientation oven to immediately below the air
film. Takashige et al (2004a) also found a linear relationship ring on top (see Fig. 11). This effect has been experimentally
between the local thicknesses of the non-stretched and observed and theoretically predicted by Zatloukal and co-
stretched films. Such a direct correlation is not apparent in workers (2004, 2006). A decrease in the heat transfer coeffi-
Fig. 9. cient causes an increase in neck height, i.e, a change in the cur-
vature of the bubble from a LDPE-type bubble to a high stalk
HDPE-type bubble. Using a low air flow rate, stable bubbles strain hardening behavior, resulting in a less uniform primary
can be obtained up to 4.8 · 4.8 stretching ratios (BURF · tube and in a more unstable bubble. High BUR · TUR will
TURF) and 10 8C lower set temperatures in the re-heating cause helical instability, as reported previously by White
ovens (330 and 350 8C, respectively). The effect of the air flow (Kang et al., 1990; Song and White, 2000).
rate on the range of stretching ratios where a continuous stable Given the above discussion, the operating condition pre-
bubble is obtained is represented in Fig. 12. In the interval sented in Fig. 13 was used as the initial set point to study the ef-
tested, a low air flow rate yields a wider operating window fect of TURP, BURF, re-heating temperature, position of top air
and brings about more uniform films (see Fig. 9). The effect ring and air velocity. The results obtained are summarized in
should be similar to that of cooling air velocity, to be discussed Table 3 in terms of the ease to obtain a stable bubble and homo-
below. In fact, at constant air ring gap, an increase in air flow geneity index. Decreasing TURP from 4.5 to 3.5 facilitates pro-
rate results in an increase of air velocity. Probably, a high cool-
ing rate makes the polymer too rigid to allow the highest
stretching ratios. This effect was also observed by other re-
searchers (DiMaio et al., 2002; Song and White, 2000). It has
been demonstrated that bubble breakage occurs over a limiting
stress and that bubble instabilities develop below that stress
(DiMaio et al., 2002; Rhee and White, 2001; Takashige et al.,
2004a, 2004b; Song and White, 2000). Too small stretching ra-
tios generate a thick film, lowering the stretching stress and the
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IPP 2012.27:348-357.
Fig. 13. Initial operating condition used to study the effect of process-
ing parameters on processability
A)
Bubble Homogeneity
stability index
%
Fig. 12. Stability window for two different cooling conditions Table 3. Effect of processing conditions on bubble stability and thick-
(LDPE3), A) low air flow rate, B) high air flow rate ness homogeneity
cessing and yields a more uniform film. Two opposing effects operating window that might not assure the best performance
develop: i) the increasing thickness slows down cooling, fa- of the films. Hence, identifying the correlations between feasi-
vouring crystallinity; ii) due to its lower velocity, the time the ble operating window, structure development and properties is
tube is subjected to forced cooling increases, hindering crystal- also mandatory and will be considered in a separate study.
linity. The lower the degree of crystallinity, the higher the flex- Among the processing parameters investigated in this work,
ibility and the ability of the primary to be bi-axially stretched the air flow rate from the air cooling rings, together with their
(Song and White, 2000). Apparently, here the two effects are axial position and air velocity showed to be the most influent
balanced as the degree of crystallinity of the two primaries on bubble stability and film thickness homogeneity. In general,
was found to be similar (circa 29.0 % and 30.8 % for a TURP any combination of processing conditions leading to fast bub-
of 3.5 and 4.5, respectively, as determined by DSC). Therefore, ble cooling affects negatively both film stability and thickness
the beneficial effect of reducing TURP must be credited to the homogeneity.
higher primary tube thickness upon bi-orientation, enabling
higher stretching ratios. As expected and reported by other
authors (Takashige et al., 2004a), the higher the bi-orientation References
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by Kungliga Tekniska on August 28, 2015. For personal use only.
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http://dx.doi.org/10.1016/0377-0257(86)80053-2 Acknowledgements
Muke, S., et al., “Extensional Rheology of Polypropylene Melts from
the Rheotens Test”, J. Non-Newtonian Fluid Mech., 101, 77 – 93
(2001), http://dx.doi.org/10.1016/S0377-0257(01)00142- 2 The authors gratefully acknowledge funding by FEDER via
Munstedt, H., et al., “Influence of Molecular Structure on Rheological FCT, Fundação para a Ciência e Tecnologia, under the project
Properties of Polyethylenes”, Rheol. Acta, 37, 21 – 29 (1998), PTDC/CTM/67025/2006 and Plurianual Programs. Thanks
http://dx.doi.org/10.1007/s003970050087 are also due to Fibope – Filmes Biorientados, S.A. for practical
Rhee, S., White, J. L., “PA612 Double Bubble Tubular Film Process –
advice and material donation.
Processability and Structure Development”, Int. Polym. Proc., 16,
272 – 284 (2001)
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sion of Polybutylene Terephthalate”, Int. Polym. Proc., 15, 157 – 165 Date accepted: December 8, 2011
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(2000)
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Polym. Proc., 19, 47 – 55 (2004a)
IPP 2012.27:348-357.