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A Preliminary Study

on Bladder-Assisted
Rotomolding of Thermoplastic
Polymer Composites
A. SALOMI, A. GRECO
Department of Engineering for Innovation, Università del Salento, via per Monteroni 73100 Lecce, Italy

F. FELLINE, O. MANNI
Consorzio CETMA, Department of Materials and Structural Engineering,
Cittadella della Ricerca SS Appia km 7+300, 72100 Brindisi, Italy

A. MAFFEZZOLI
Department of Engineering for Innovation, Università del Salento, via per Monteroni 73100 Lecce, Italy
Received: December 13, 2006
Revised: April 23, 2007

ABSTRACT: In this preliminary work, a new process is examined for


manufacturing hollow parts from continuous fiber-reinforced thermoplastic
polymer. The new process combines the basic idea of bag forming (or
bladder-assisted forming) with the rotation of the mold for the processing of
thermoplastic matrix composites. A pressurized membrane is used to compact
the composite on the inner wall of a mold, which is placed inside a forced
convection oven. The mold is removed from the oven for the cooling stage. The
process was initially developed by using a thermoplastic pre-preg obtained using
yarns of commingled E-glass fibers with isotactic polypropylene (iPP). A
preliminary characterization of the thermoplastic composite showed that the
material can be consolidated with pressures as low as 0.01 MPa, which is readily

Correspondence to: A. Maffezzoli; e-mail: alfonso.maffezzoli@


unile.it

Advances in Polymer Technology, Vol. 26, No. 1, 21–32 (2007)



C 2007 Wiley Periodicals, Inc.
ROTOMOLDING OF THERMOPLASTIC POLYMER COMPOSITES

achievable with the process of this study. The design of the mold and membrane
was carried out on the basis of both structural analysis of the aluminum shell and
thermal analysis of the mold. The mold thickness is of great importance with
respect to both the maximum pressure allowed in the process and the overall
cycle time. Molding was performed on stacks of three and six layers of yarn,
varying the applied pressure between 0.01 and 0.05 MPa and maximum
temperature of the internal air between 185◦ C and 215◦ C. The composite shells
obtained under different processing conditions were characterized in terms of
physical and mechanical properties. Mechanical properties comparable with
those obtained by compression molding and vacuum bagging were obtained. The
maximum values obtained are 12.1 GPa and 290 MPa for the flexural modulus
and the flexural strength, respectively. Furthermore, the results obtained show
that mechanical properties improve with increasing the pressure during the cycle
and with the maximum temperature used in the process.  C 2007 Wiley

Periodicals, Inc. Adv Polym Techn 26: 21–32, 2007; Published online in Wiley
InterScience (www.interscience.wiley.com). DOI 10.1002/adv.20085

KEY WORDS: Composites, Mechanical properties, Processing, Rotomolding,


Woven fabric

fiber-reinforced polymers are very difficult to be pro-


Introduction cessed to produce complex shapes.
Processing of thermoplastic-based composites re-

C ontainers with capacity as large as 5 m3 can be


produced by rotational molding starting from
commodity polymer powders such as polyethylene
quires high pressures and temperatures to achieve
complete dispersion of the fibers into the polymer
matrix and removal of entrapped air.6,7 At high tem-
peratures, the lower viscosity of the polymer and the
and polypropylene.1 Rotational molding is an at-
applied pressure cause an out-of-plane flow of the
tractive and economic technique for the production
molten phase, which impregnates the fibers8−10 and
of hollow parts by using thermoplastic polymers.1
expels the air.
However, shape stability and strength are limited
The flow of the molten material is governed by
by the properties of these polymers. To improve the
Darcy’s law,11,12 which implies that low viscosities
mechanical properties of rotomolded articles, par-
and low migration distance of the polymer matrix
ticulate filler or very short fibers can be incorpo-
are required for complete consolidation. For this rea-
rated into the polymer matrix.2,3 Continuous fibers
son, commingled yarn pre-pregs, or semi-pregs, are
have not, hitherto, been used in rotational molding
used for this purpose, allowing composites to be
of polymer composites, despite the attractions de-
processed at low pressures.
rived from the huge improvements expected in the
Processing techniques for these materials fall
properties of the products, which can be obtained
into two categories: (a) pressing between matched
only with filament winding methods. Thermoplastic
dies (matched die forming, hydro forming, rubber
matrix composites, based on commodity polymers,
block forming, and shaped rubber tool forming) and
are also very attractive, owing to their processabil-
(b) other methods in which the consolidation force
ity, high-impact strength, good chemical resistance,
is provided by means of a diaphragm or film (dou-
low moisture absorption, unlimited shelf life of raw
ble diaphragm forming, vacuum bag consolidation,
materials, and low cost. The ability of thermoplastic
and autoclave processing).13−15 None of these tech-
matrix composites to be recycled is a major advan-
niques, however, is suitable for the production of
tage over thermosetting matrix composites4,5 partic-
hollow components, which severely limits the range
ularly for automotive applications. Moreover, iso-
of applications of thermoplastic-based composites.
tactic polypropylene (iPP) is considered one of the
In this work, a new process for manufactur-
most suitable polymers for many industrial appli-
ing hollow components with continuous fibers-
cations. Despite the many advantages, continuous
reinforced thermoplastic polymer was developed.

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ROTOMOLDING OF THERMOPLASTIC POLYMER COMPOSITES

The material used is a commingled woven fabric The consolidation characteristics of the commin-
made of iPP and glass fibers.16 The developed pro- gled fabric were assessed on a Lloyd Instruments
cess has the following features: LR 5K universal testing machine, equipped with a
forced convection oven, using 20-cm diameter steel
a. hollow parts can be produced from plates for compression tests. Three Twintex layers
continuous-fiber thermoplastic matrix com- were placed between compression plates with fibers
posite; of each layer aligned in the same direction. Three
b. heat transfer is one dimensional and takes pressure values were chosen, 1 × 10−2 , 4 × 10−2 ,
place directly from the oven to the mold and to and 5 × 10−2 MPa, which are in the range of the
the material; air pressures that can be conveniently applied to the
bladder during the process. In the compression tests,
c. thin wall products can be obtained, since heat-
the force on the material was held constant, while
ing of the material takes place slowly;
the temperature was raised at a controlled rate and
d. parts of large dimensions can be produced, measured by a thermocouple system. The resulting
provided that the low pressures can be used. displacement of the loading plate was recorded dur-
ing the test. The observed displacement is the sum
The process developed combines the advantages of two contributions, the first resulting from com-
of rotational molding for the production of hollow posite consolidation and the second from expansion
thin walled parts of large dimensions, with the capa- of the steel plates and tools. A calibration run was
bility of molding thermoplastic matrix composites. performed in the absence of the composite sample
The present study was carried out to assess the to measure the effect of the thermal expansion of the
possibility of achieving an efficient compaction at tools, and to obtain a baseline for the compaction of
low applied pressures. A small prototype tank was the composite.
manufactured to demonstrate the feasibility of the Tensile tests were performed on the silicone used
developed process for the production of hollow to build membrane. Tensile specimens with a waste
parts, using continuous fiber-reinforced thermoplas- line 3-mm thick were cut from a silicone sheet. The
tic composites. Molded parts were characterized in material was tested at three different temperatures
terms of physical and mechanical properties to ex- (30◦ C, 100◦ C, and 200◦ C) using a crosshead speed of
amine the effect of processing conditions on the qual- 50 mm/min.
ity of composites. Flexural tests were performed on molded compo-
nents, with the longitudinal axis of the samples par-
allel to the fiber direction. Tests were performed us-
ing the same Lloyd Instrument, following the ASTM
D-790 standard for flexural tests, using a span-to-
Experimental thickness ratio 20:1.
Density measurements were made on small sam-
The material used in this work is a plain weave ple cut from the molded products, using a Sartorius
commingled woven fabric (TWINTEX® PP60), GP 3202 balance, modified for weighing in water,
based on E-glass fibers and iPP fibers, supplied by following the ASTM D 792 standard.
Saint-Gobain Vetrotex. The material tested is a bal- The fiber content of the molded components was
anced woven fabric (i.e., the fiber fraction is the determined following the ASTM D3171 standard.
same in the weave and in the weft directions) with The theoretical density of the composite is es-
60% by weight of E-glass and 40% by weight of timated from the contributions of polymer matrix
iPP and a specific weight of 1485 g/m2 . The aver- and E-glass fiber density. Furthermore, the matrix
age diameters of E-glass and iPP fibers are 17.5 and density is the sum of the contributions from the
30 µm, respectively.17 TWINTEX plies can be formed amorphous and the crystalline phase, whose frac-
into rigid laminates under the simultaneous appli- tions depend on the cooling rate stage.19,20 Then, the
cation of heat and pressure. According to technical theoretical density of composite ρct can be estimated
datasheets from Vetrotex, the compacted material from the rule of mixtures:
has an average tensile modulus of 13.8 GPa and a
tensile strength of 280 MPa. The corresponding val-
ues measured on samples obtained by vacuum bag- 1 Wm Wf
= + (1)
ging are 11.6 GPa and 273 MPa.18 ρct ρm ρf

Advances in Polymer Technology DOI 10.1002/adv 23


ROTOMOLDING OF THERMOPLASTIC POLYMER COMPOSITES

where Wm and Wf are, respectively, the weight frac- with a hole, necessary to remove the membrane at
tions of matrix and fibers in the composite and ρm the end of each cycle. If necessary, the mold can be
and ρf their respective density. The density of the pressurized at room temperature, and a nonreturn
glass fibers was taken as 2540 kg/m3 , and that of the valve can be connected to the top of the mold. This
polypropylene matrix as 890 kg/m3 . The measured ensures the possibility of rotating the mold. The pres-
density was used to calculate the void fraction Vv as sure profile during the cycle can be easily predicted
applying the law for ideal gases, to take into account
ρce the effects of heating on the air or gases used for the
Vv = 1 − (2)
ρct bag inflation.
An aluminum mold, characterized by higher heat
where ρce is the measured composite density. transfer coefficient and lower weight than steel, was
A scanning electron microscope (SEM) Zeiss EVO used. The mold has a very simple shape, a box
40 equipped with a tungsten filament was used to ev- (250 × 250 × 200 mm) with round corners 30 mm
idence the presence of void in the molded samples. in radius. To ensure the planarity of the flat com-
A Perkin Elmer DSC-7 was used to determine the posite surfaces, the deformation of the walls of the
matrix melting temperature range, and to calculate mold must be limited. The maximum deformation of
the degree of melting, α, a dimensionless parameter, the mold wall was calculated considering the static
which represents the fraction of material molten at scheme of a simply supported plate 250 × 250 mm
each time or temperature: in size. The maximum acceptable deflection at the
center of the plate was taken as 3 mm, assuming a
t   maximum consolidation pressure of 4 MPa accord-
1 dH
α(t) = − BL dt (3) ing with the typical values reached in compression
Htot dt
00 molding. The actual constraint behaves as an elastic
fixed end, thus ensuring a deformation lower than
Htot in Eq. 3 represents the total heat of melting and the calculated one. Using the Galerkin approximated
BL a baseline. method and allowing for marginal errors, the calcu-
lated wall thickness was 13 mm.
The membrane was fabricated by AEROVAC
Europe (UK). It is a silicone membrane that is able
Design of the Mold and to withstand high stresses at high temperatures. Its
Accessories size and shape were designed to fit into the cavity of
the mold with a gap between the membrane and the
inner mold surface of 3 mm. Tensile tests, carried out
A scheme of the mold system with the lay-up of at different temperatures up to 200◦ C, the maximum
the commingled preform and membrane is shown in temperature used during the process, indicated that
Figure 1. The mold is composed of two halves with the elastic modulus is weakly affected by tempera-
flanges for mold closure. The upper part is provided ture. The small reduction in tensile strength is not a
problem, since the membrane experiences very low
deformations. The results of tensile test on the mem-
brane material are reported in Table I.

Composite Molding

The molding process involves lay-up of the com-


mingled pre-form on the inner surface of the hollow
mold. The pre-form shown in Figure 2 was wrapped
on the outer surface of the membrane. Commin-
gled yarn-based pre-forms retain very high pliabil-
ity, and can be easily conformed to meet the shape of
FIGURE 1. Molding equipment setup. the membrane. The pre-form comprises two squares

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ROTOMOLDING OF THERMOPLASTIC POLYMER COMPOSITES

TABLE I
Tensile Strength, Strain to Failure and Tensile Modulus of the Silicone Rubber Sheet at Different Temperatures
Temperature (◦ C) Tensile Strength (MPa) Strain to Failure (mm/mm) Elastic Modulus (MPa)

30 3.89 ± 12 × 10−3 5.44 ± 11 × 10−3 685 10−3 ± 6.1 × 10−3


100 3.08 ± 20 × 10−3 3.88 ± 16 × 10−3 680 10−3 ± 6.2 × 10−3
200 2.29 ± 40 × 10−3 2.85 ± 35 × 10−3 676 10−3 ± 4.8 × 10−3

250 × 250 mm and four rectangles 250 × 200 mm. rial takes place by conduction from the mold sur-
One of the 250 × 250 mm squares has a hole, nec- face. When the matrix melts, flow takes place as a
essary to extract the membrane after molding. Di- consequence of the applied pressure, and air is re-
mensional stability of the pre-forms was improved moved from the composite through the mold part-
by heating the pre-form with a thermal gun at the ing line. After reaching full consolidation, the mold
box edges. The fiber orientation was the same for is removed from the oven and the cooling phase
each layer, i.e., parallel to mold edges; however, the takes place, while the composite is still under pres-
lay-up was such that the folded edges appeared sure, in order to prevent warpage associated with
on different sides of the mold in building up the anisotropic shrinkage and temperature gradients in
lamination. the material.
Consolidation of the composite was obtained by Laminates about 1.5 and 3 mm thick were molded,
the simultaneous effect of pressure and tempera- corresponding to stacking of 3 and 6 Twintex layers.
ture. The preform and the membrane are placed In this work, molding was carried out in a static
inside the mold, which is set to a temperature of mode, where the mold is not rotating. This may in-
300◦ C. The maximum temperature during the cycle volve a nonuniform heating of the mold, particularly
was measured on the air inside the membrane. In for large dimensions of the mold, which can be pre-
different experiments, the mold was extracted from vented by using a rotating mold, as in conventional
the oven when the temperature reached a value of rotational molding.
185◦ C, 190◦ C, 200◦ C, and 215◦ C. The membrane is
connected to an external pressurization system. Dur-
ing tests, the pressure inside the membrane is held
constant. Three pressure levels were chosen, namely Results and Discussion
1 × 10−2 , 3 × 10−2 , and 5 × 10−2 MPa. During the pro-
cess, the pressurized membrane forces the compos-
ite on the inner wall surface. Heating of the mate- COMPRESSION TESTS
Compression tests were performed on three lay-
ers of Twintex, holding a constant pressure on the
material and varying its temperature. The temper-
ature recorded for the tests at three different pres-
sures, in correspondence of the inner layer, as re-
ported in Figure 3, is not influenced by the applied
pressure. The laminate thickness as a function of
temperature is reported in Figure 4 for the three
compaction pressures. In Figure 4, for comparison
purposes, also the degree of melting of the iPP ma-
trix as a function of the temperature is reported.
Before compaction, each ply of Twintex is about
1.5 mm thick. As a consequence, for a stack of 3
layer, an initial thickness about 4.5 mm should be
observed. As shown in Figure 4, the thickness of
samples significantly decreases even if only a mod-
erate pressure is applied on the material. As pres-
FIGURE 2. Schematic drawing of the preform used. sure increases, the initially high void fraction of the

Advances in Polymer Technology DOI 10.1002/adv 25


ROTOMOLDING OF THERMOPLASTIC POLYMER COMPOSITES

matrix, and sufficient time for the flux to take place.


The three curves show a very similar behavior, but
the rapid thickness reduction takes place at lower
temperatures as the pressure increases, in accor-
dance with the relationship between flow rate and
pressure. Above 175◦ C, a further thickness decrease
can be observed, indicating that the compaction pro-
cess can be regarded as a two-stage process, the
first relating to fiber impregnation, and the second
to void reduction and expulsion from the laminate
boundaries.23,24 The results reported in Figure 4 indi-
cate that the material can be successfully processed
at very low pressures (down to 1 × 10−2 MPa).
FIGURE 3. Laminate temperatures measured during
consolidation test with isothermal oven temperature (—), ANALYSIS OF THERMAL CYCLE
at 1 × 10−2 (), 4 × 10−2 (), and 5 × 10−2 (◦) MPa.
The knowledge of the thermal events in the heat-
ing and cooling stage of the process is very important
to determine the most appropriate processing condi-
composite decreases owing to the compressibility of tions. The basic equation used to model heat transfer
the commingled woven plies. The compressibility of during process is the Fourier equation:
the dry composites is attributed to bending, sliding,
and rearranging of fibers.21,22 At low temperatures, • dT
the thickness of the material increases with temper- ∇(ki ∇ • T) ± q = c Pi ρi (4)
dt
ature, as a consequence of thermal expansion. Up to
the melting point of PP the matrix is a solid semi- the subscript i refers to the mold, composite, or sili-
crystalline polymer, and matrix flow and fiber im- cone bag properties, T is the temperature, t the time,
pregnation cannot take place. k the thermal conductivity,

c p the specific heat, ρ
For each of the three curves reported, a significant the density, and q a heat source term, accounting
thickness reduction takes place at higher tempera- for polymer phase transition. The sign is positive
tures (above 150◦ C) when the polymer starts melt- in endothermic processes (melting) or negative in
ing. From comparison of melting and compaction exothermic processes (crystallization). Equation (4)
curves, it is noted that compaction takes place at is quite complex and is better solved by numerical
higher temperatures. This is to be expected, since methods. The main approximation that can be ap-
fiber impregnation requires a fully liquid polymer plied is the assumption of unidirectional heat trans-
fer, which is typical of problems where one dimen-
sion is much lower than the others, as is the case
of the process developed. With this assumption,
only the thermal gradients through the thickness of
the mold/preform/membrane system are taken into
account.
A second simplification that can be applied is the
assumption of negligible thermal gradients through
mold thickness. This can be better understood by
writing the heat flux continuity equation at the
mold/oven air interface S:

∂ T 
−k S = h est (Test − T|z=S ) (5)
∂z z=S

FIGURE 4. Comparison of the thickness variation, at where Test is the oven temperature, TS is the tem-
 ),4 × 10−2 (—),
1 × 10−2 (— ◦ ) MPa, with
 and 5 × 10−2 (— perature at the interface between the mold and the
the degree of melting, α (—). oven, h est is the convective heat transfer in forced

26 Advances in Polymer Technology DOI 10.1002/adv


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convection, and ks is the mold thermal conductiv-


ity. Introducing then the following dimensionless
variables:

T| S − Test 
T∗ =
Tref − Test ⇒ dTs = (Tref − Test )dT

∗ (5)
z dz = δdz
z∗ =
δ

where Tref is a reference temperature, and δ the mold


thickness, and substituting Eq. (5) into Eq. (4) yields

dT∗ h est δ ∗
= T (6)
dz∗ ks FIGURE 5. Temperature profile of the mold during
 lower
heating without composite. Internal air (—),
the dimensionless number h estks
δ
is the Biot number. ◦ ), and lateral surfaces (—
surfaces (—  ).
dT ∗ ∗
When Bi  1, d x∗  T , and thermal gradients in the
solid mold walls can be neglected. In our study, as-
suming h est = 10 (W/m2 K),25 and ks = 168 (W/m K), The temperatures were also measured during
and being δ = 13 mm yields Bi = 7.7 × 10−4  1 indi- processing of composite laminates with different
cating a uniform temperature across the mold thick- thickness and pressures. In every test, the tempera-
ness. An improved estimation of the convective heat ture of the oven was set at 300◦ C. Three thermocou-
transfer coefficient can be obtained using a global ples were placed at three different positions, respec-
heat balance for the mold, when no composite ma- tively, the interfaces between mold and composite
terial is present: (T1 ), between composite and membrane (T2 ), and in
  contact with the internal air (T3 ).
dT The typical evolution of T1 , T2 , and T3 during the
ρc p V = h est A(Test − T) (7)
dt process is reported in Figure 6 for a 3-layer configu-
ration and a pressure of 5 × 10−2 MPa. The profiles
where V is the mold volume, A the convective heat shown in Figure 6 are very similar to those exper-
transfer surface. Assuming V/A= δ, Eq. (7) can be imentally observed1,26 and numerically predicted27
written as for conventional rotational molding of plastics. The
temperature profile as a function of time shows six
dT h est different stages. The first one is heating with the
= (Test − T) (8)
dt ρc p δ

By integration of Eq. 8, the mold temperature can


be calculated as a function of the time:
 
Test − T0 h est
ln = t (9)
Test − T ρc p δ

The temperature measured at different positions


on the mold surface, during heating without the
composite material, is reported in Figure 5. From
nonlinear curve fitting according to Eq. (9) of the
experimental results, assuming ρ = 2750 kg/m3 ,
c p = 890 J/(kg × K), a convective heat transfer coef-
ficient of 20 W/(m2 K) was obtained. This is a value
higher than the first approximation used, and con- FIGURE 6. Temperature profiles for T1 (—),  T2 (—◦ ), and
firms the negligible temperature gradients obtained  ) during a molding cycle with an isothermal oven
T3 (—
by Biot number analysis. temperature of 300◦ C.

Advances in Polymer Technology DOI 10.1002/adv 27


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material in solid form. In conventional rotomolding,


when the polymer begins to melt, a plateau is ob-
served, due to energy adsorption necessary to pro-
mote melting. In this work, a thickness lower than
those typically used in rotational molding and a low
amount of polymer matrix in the composite are re-
sponsible for negligible energy adsorption during
melting. Melting of the material involves the de-
crease of thermal gradient across composite thick-
ness. The temperature continuously increases up to
a maximum value occurring immediately before the
mold is extracted from the oven for cooling. The
maximum temperature is very important to deter-
mine the processing times and product quality, as FIGURE 7. Temperature gradient through the
will be discussed later. After extraction of the mold composite thickness for six layers of Twintex during
from the oven, the temperature decreases at a rate de- ◦ ) and 3 × 10−2 (—)
molding cycle at 1 × 10−2 (—  MPa.
pending on the cooling medium. In this work, cool-
ing is performed in quiescent air and consequently
is quite slow. When crystallization of the polymer
matrix takes place, a second plateau should be ob- cesses, for which the heat transfer conditions are
served. Nevertheless, for the same reasons explained very similar to those of rotational molding, major
before, the energy release during crystallization is issues are the prediction of the overall cycle time,
very low. The last stage is cooling of the solid ma- which depends on mold and sample thickness and
terial, which takes place until the material has ade- thermal properties, and the possibility of material
quate mechanical properties for extraction from the degradation, which is related to the internal peak
mold. temperature and wall thickness of the product.28 De-
The temperature T1 is the highest one and the dif- tails about the prediction of the evolution of temper-
ference between T1 and T2 is related to the low ther- ature during the molding cycle for rotomolding can
mal conductivity of the polymer composite, and to be found in reference 27.
the thickness of Twintex preform. The temperature
of the air, T3 , is the lowest one, since air is heated
CHARACTERIZATION OF MOLDED
by natural convection from the inner surface of the
SAMPLES
membrane, which also acts as an additional ther-
mal insulation. The temperature T3 is used for pro- Samples were obtained by stacking three or six
cess control. As shown in Figure 6, the temperature layers of Twintex with fibers of each layer aligned in
gradient through the composite thickness decreases the same direction, to obtain a [0/90] lay-up. The lay-
when the polymer matrix melts. This is attributed to up of the laminate is such that, according to laminate
the compaction of the composite, which involves an theory, the expected properties of the laminate, in the
increase of its thermal conductivity, and a decrease direction of the fibers, are the same as the properties
in thickness as air is expelled. of the lamina.
The effect of pressure on the temperature gra- A typical prototype built according to the pro-
dients in the composite was also analyzed. This posed processing method is shown in Figure 8. To
is shown in Figure 7, showing the difference be- study the homogeneity of the material eventually re-
tween T1 and T2 for a 6-layer laminate at pressures lated to in-plane polymer flux, the fiber content of the
of 1 × 10−2 and 3 × 10−2 MPa. At the higher pres- composite was measured at different distances from
sure, the lower thickness of the material at the initial the center of the laminate. The results reported in
stage of heating is responsible for lower thermal gra- Table II show a homogeneous fiber weight fraction.
dient. After polymer melting and compaction of the A first indication about the efficiency of the con-
composite, the thermal gradients are no longer de- solidation of the material was obtained by measur-
pendent on pressure. The analysis reported in this ing the thickness, the density, and the void content of
section is aimed to compare the thermal resistances the molded laminates. The results obtained for sam-
of mold, bladder, and composite. In this type of pro- ples molded at different temperatures are reported

28 Advances in Polymer Technology DOI 10.1002/adv


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FIGURE 8. Picture of a molded part.

in Table III. Each value of thickness, density, and tained assuming a weight fraction of fibers of 0.6, is
void fraction is obtained as the average of 15 val- also reported in Table III, and is not dependent on
ues, obtained on samples extracted at 15 different the processing conditions. On the other hand, as re-
positions on the composite. Results reported in Ta- ported in Table III, density increases with maximum
ble III show that the laminate thickness decreases temperature during cycle. The increase of density
with temperature. The theoretical density values, ob- was attributed to a reduction of void fraction. SEM
micrographs were taken on the fracture surface of
samples broken in liquid nitrogen. Results obtained
TABLE II with a 2000× magnification are reported in Figure 9
Fiber Weight Fraction for a Molded Sample at Different for the sample molded at 185◦ C and in Figure 10 for
Distances from the Center of the Panel the sample molded at 200◦ C. In Figure 9, the SEM
Distance from the Fiber micrograph on the sample molded at low tempera-
Panel Center (mm) Weight Fraction ture shows limited impregnation and the presence
of voids close to glass fibers. The SEM micrograph
0–16 0.603 obtained on the sample molded at 200◦ C, reported
16–32 0.613 in Figure 10, on the other hand, shows a reduced
32–48 0.602 amount of voids associated with increased molding
48–64 0.613
temperature and consequent lower viscosity of the
64–80 0.614
matrix.

TABLE III
Physical Properties of Parts Obtained with the New Method at Different Molding Temperatures
Maximum Number of Thickness Density Theoretical Density Void Content
Pressure (MPa) Temperature (◦ C) Layers (mm) (kg/m3 ) (kg/m3 ) (%)

3 × 10−2 185 3 1.624 ± 0.01 1404 ± 6 4.16 ± 0.41


3 × 10−2 190 3 1.593 ± 0.02 1417 ± 19 1460 3.27 ± 1.3
3 × 10−2 200 3 1.578 ± 0.02 1428 ± 11 2.52 ± 0.75

Advances in Polymer Technology DOI 10.1002/adv 29


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FIGURE 9. Scanning electron microscope micrograph obtained at 2000 × magnification on the sample molded at
185◦ C.

The effect of pressure on the samples molded with crease, and is indicative of a higher efficiency of the
six layers of Twintex was also analyzed. The results impregnation.
reported in Table IV show that the thickness of the The data reported in Table III and IV confirm
composite is reduced by increasing the pressure. The the results obtained in compression tests, indicating
density increase is associated to a void content de- that an improved impregnation and consolidation

FIGURE 10. Scanning electron microscope micrograph obtained at 2000× magnification on the sample molded at
200◦ C.

30 Advances in Polymer Technology DOI 10.1002/adv


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TABLE IV
Physical Properties of Parts Obtained with the New Method at Different Pressures
Maximum Number of Thickness Density Theoretical Density Void Content
Pressure (MPa) Temperature (◦ C) Layers (mm) (kg/m3 ) (kg/m3 ) (%)

1 × 10−2 215 6 3.21 ± 0.02 1423 ± 10 2.87 ± 0.68


3 × 10−2 215 6 3.18 ± 0.004 1433 ± 9 1460 2.18 ± 0.61
5 × 10−2 215 6 3.09 ± 0.005 1436 ± 7 1.97 ± 0.47

can be achieved by increasing either the pressure or turn, increase mold-manufacturing costs and results
the maximum temperature of the mold. However, in longer cycle times.
it must be borne in mind that increasing the max- The flexural strength of 3 ply composites ob-
imum temperature can promote polymer degrada- tained at different temperatures and a pressure of
tion and increase cycle times. On the other hand, 3 × 10−2 MPa are reported in Figure 11 (A). The flex-
a higher pressure requires heavier molds that, in ural strength of the laminates obtained using the de-
scribed processing method are higher than those ob-
tained using conventional vacuum molding,18 and
comparable with the reference value of the technical
data sheet of Twintex (280 MPa). In agreement with
the physical characterizations, the flexural strength
of composite increases with increasing molding tem-
perature. The flexural modulus shown in Figure 11
(A) indicates that the laminates obtained by the new
method display a stiffness comparable to that of lam-
inates obtained by vacuum molding,18 but lower
than the reference values from the technical data
sheet (13.8 GPa).
The effect of pressure on flexural strength and
modulus of samples molded at a maximum tem-
perature of 215◦ C is reported in Figure 11 (B). The
flexural strength of the laminates obtained by the
new method are comparable with the values ob-
tained on laminates molded by vacuum bagging,18
and with reference values, even though the lami-
nates obtained by the new method are processed
at lower pressures. The modulus is comparable with
that of laminates obtained by vacuum bagging,18 but
lower than the value reported by the technical data
sheet.

Concluding Remarks

In this work, a new method for the produc-


tion of hollow components with continuous fiber-
FIGURE 11. (A) Effect of molding temperature on the
flexural strength and modulus of 3 layers of Twintex reinforced thermoplastic materials was evaluated.
molded at 3 × 10−2 MPa. (B) Effect of molding pressure The method represents an adaptation of bag form-
on the flexural strength and modulus of 6 layers of ing to thermoplastic pre-pregs, and is particularly
Twintex molded at 215◦ C. suitable for the production of hollow parts, with thin

Advances in Polymer Technology DOI 10.1002/adv 31


ROTOMOLDING OF THERMOPLASTIC POLYMER COMPOSITES

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typically used in the composite industry can be
1995, 54, 349–358.
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to be accounted for are cycle time and mold costs. 1150–1173.
Potential applications of the new process are struc- 13. Bernet, N.; Michaud, V.; Bourban, P.-E.; Manson, J.-A. E.
Compos Pt A 2001, 32, 1613–1626.
tural components for lightweight, fuel efficient, and
14. Bernet, N.; Wakeman, M. D.; Bourban, P.-E.; Manson, J.-A. E.
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The work has been partially financed by MIUR
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32 Advances in Polymer Technology DOI 10.1002/adv

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