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Polyolefin composites with curaua fibres: Effect of the processing conditions

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Article  in  Composites Science and Technology · January 2010

DOI: 10.1016/j.compscitech.2009.09.002

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 Composites Science and Technology 70 (2010) 29–35

Contents lists available at ScienceDirect

Composites Science and Technology

journal homepage: www.elsevier.com/locate/compscitech

Polyolefin composites with curaua fibres: Effect of the processing conditions

on mechanical properties, morphology and fibres dimensions
B. Mano, J.R. Araújo, M.A.S. Spinacé, M.-A. De Paoli *
Instituto de Química, Unicamp, CP 6451, 13083-970 Campinas, SP, Brazil

a r t i c l e i n f o a b s t r a c t

Article history: Composites of polypropylene (PP) and high density polyethylene (HDPE) reinforced with 20 wt.% of cur-
Received 14 April 2009 aua fibres were prepared using a twin-screw extruder and the effect of screw rotation speed (SRS) was
Received in revised form 19 June 2009 evaluated by measuring the output, the mechanical properties of the composites, the morphology and
Accepted 10 September 2009
the fibre dimensions. Increase in SRS causes a decrease in length, diameter and aspect ratio of the fibres
Available online 13 September 2009
in both composites, due to the high shear forces acting in the molten polymer and transferred to the
fibres. Consequently, the reinforcement effect of the fibres decreased, as evidenced by the flexural and
Keywords:
tensile mechanical properties of the composites. Additionally, polymeric matrices undergoes thermo-
A. Short-fibre composites
B. Mechanical properties
mechanical degradation during processing, this also contributed to the changes in the mechanical prop-
D. Scanning electron microscopy (SEM) erties. Comparison between the matrices showed that PP composites are less affected by changes in SRS,
E. Extrusion suffering fewer changes in fibre dimensional parameters and in the mechanical properties than HDPE
E. Injection moulding composites.
Ó 2009 Elsevier Ltd. All rights reserved.

1. Introduction region of Brazil. The fibres are extracted by decortication and dried.
The dry fibres are light, resistant and present numerous applica-
Reinforcing agents, such as short fibres, synthetic and vegetal, tions in the industry [6]. Presently, the curaua fibres are considered
are widely used by industry to obtain materials with improved as an alternative for glass fibres in the reinforcement of thermo-
mechanical properties. The synthetic fibres present some disad- plastics, especially in automotive devices, due to its excellent spe-
vantages in relation to vegetal fibres, such as: their production con- cific mechanical properties [7].
sumes energy, have a high cost in relation to others fillers, are Short vegetal fibres can be used in large scale processing equip-
abrasive to the processing equipment, are not degradable and are ments, like extruders and injection moulding machines. Thus,
generated from non-renewable sources. The use of vegetal fibres polymeric composites reinforced with short vegetal fibres become
as reinforcement agents in polymeric matrices is not a new prac- interesting because they can be continuously produced by rapid,
tice, but due to economical and environmental concern, there is a low cost and environmentally friendly processes, in contrast to
renewed interest in developing these composites materials [1]. composites with long fibres that are processed by thermoforming.
Vegetal fibres are produced from renewable sources, present low The mechanical properties of polymeric composites reinforced
density, competitive specific mechanical properties, are not abra- with short fibres depend on several factors which determine the
sive to the processing equipments and are biodegradable [2]. Now- surface area available for transmission of stresses from the matrix
adays, different car makers are using thermoformed composites to the fibres [8]. These include the geometric parameters of the
with vegetal fibres in panels. The most used vegetal fibres are: fibres (length, diameter and aspect ratio) and orientation and dis-
wood chips, jute, henequen, coir, sugar cane bagasse, flax, hemp tribution of the fibres in the matrix. All these factors depend on the
and sisal [2–4]. However, most of them are used as filler and not processing conditions [9]. Additionally, the adhesion of the fibres
as reinforcing agent. to the matrix is responsible for the efficiency of load transfer caus-
Curaua fibres have attracted much attention of the polymer ing the reinforcement [10]. The effect of the processing conditions
industry, due to the interest of the Brazilian automotive industries on the mechanical performance of composites with short fibres
[5]. These fibres are extracted from the 1.60 m long leaves of the was studied by several authors [8,9,11].
Curaua plant (Ananas erectifolius, gender L.B. Smith) from the Bro- Baiardo et al. observed that increasing the mixing rate caused
meliaceae family, which is cultivated in large scale in the Amazon fibre shortening and length distribution narrowing in composites
of Bionolle and flax fibres prepared in a mixing chamber. The de-
* Corresponding author. Tel.: +55 1935213075; fax: +55 1935213023. crease in fibre length affected the tensile modulus of the compos-
E-mail address: [email protected] (M.-A. De Paoli). ite, producing a 32% decrease, when the average fibre length was

0266-3538/$ - see front matter Ó 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compscitech.2009.09.002
30 B. Mano et al. / Composites Science and Technology 70 (2010) 29–35

50% shorter [10]. fibre shortening was also observed in composites D638-02 and ASTM D790-02 for tensile and flexural tests, respec-
reinforced with sisal fibres, processed by extrusion and increasing tively. For PP composites the temperature profile used in the injec-
screw rotation speed (SRS) from 25 to 80 rpm. Alvarez et al. re- tion moulding machine (Arburg, All-rounder M250) from hopper to
ported for sisal composites that, additionally to fibre shortening, nozzle was 180, 185, 190, 200 and 205 °C, 1200 MPa of injection
the fibre diameter also decreased, but the aspect ratio increased pressure, 800 MPa of hold pressure, hold time of 5 s, injection
with SRS. In spite of the higher aspect ratio of the fibres the velocity of 20 cm3 sÿ1, mould temperature of 20 °C and 10 s of
mechanical properties decreased, this was attributed to thermo- cooling time. For HDPE composites the temperature profile used
mechanical degradation of the matrix [11]. in the injection moulding machine was 150, 160, 165, 170, and
The final mechanical properties of the composites are also af- 165 °C, 1200 MPa of injection pressure, 800 MPa of hold pressure,
fected by the shear and heat induced degradation of the polymer hold time of 5 s, injection velocity of 25 cm3 sÿ1, mould tempera-
matrix during processing. Canevarolo et al. studied the mechanical ture of 20 °C and 10 s of cooling time.The specific mechanical en-
and thermo-oxidative degradation of high density polyethylene ergy (SME) of the extruder was calculated using Eq. (1) [14],
(HDPE) and polypropylene (PP) after multiple extrusions [12]. For where -T and PT are, respectively the maximum screw rotation
the HDPE samples, infrared analyses showed an increase in car- speed in RPM and power of the extruder motor in kW, %T is the
bonyl index (CI) and in the concentration of trans-vinylene groups percent torque and Q is the feed rate in kg hÿ1. The maximum
during extrusion, while the concentration of vinyl groups de- screw speed is 1200 rpm and the power of the motor is 27 kW.
creased after multiple extrusions. The authors concluded that the
thermo-mechanical degradation mechanism of HDPE occurs by ÿ1 - %T PT
SME ðkW h kg Þ ¼   ð1Þ
two competitive processes: chain scission and cross-linking [12]. -T 100 Q
Canevarolo et al. also studied the degradation of polypropylene, Milled fibres were examined by optical microscopy to deter-
PP, after multiple extrusions in a twin-screw extruder using differ- mine their dimensions. In the case of the composites, fibres were
ent screw profiles with an increasing shear [13]. The molecular isolated from the matrices by extraction in boiling xylene for 1 h
weight distribution curves after five extrusions exhibited a nar- and the solvent was evaporated at 100 °C. An optical microscope
rower profile than the curves for the virgin polymer, indicating (Nikon E-800) connected to a digital camera was used to collect
preferential chain scission of the longer chains and a reduction of the fibre images. The software Image Pro PlusÒ was used to mea-
the polydispersity. sure the length, diameter and aspect ratio of each of the extracted
The aim of this work is to evaluate the effect of screw rotation fibres. Dimensions of 100 fibres were measured for each sample
speed, in a co-rotating intermeshing twin-screw extruder, on the and data were statistically analyzed to obtain the cumulative dis-
fibre dimensional parameters in the composites of HDPE and PP tribution function (normalized frequency), where P(x) is the num-
with curaua fibres after injection moulding. We also correlate ber of fibres with dimension shorter or equal to x and Ni is the
these dimensional parameters change with the mechanical proper- number of fibres with dimension I, Eq. (1).
ties and morphology of the composites. The change of aspect ratio Px
of the fibres after the processing is analyzed, because it is an Ni
PðxÞ ¼ Pi¼0
1 ð2Þ
important factor connected with the mechanical properties of the i¼0 N i
composites.
Before mechanical tests, the specimens were conditioned for
48 h at 23 (±5) °C and 50 (±5)% room humidity. Tensile and flexural
tests were carried out in a universal testing machine (EMIC,
2. Experimental
DL2000), with cross head speed of 5 mm minÿ1, according to ASTM
standards D638-02 and D790-02, respectively. An extensometer
Commercially available grades of isotactic polypropylene (Bras-
with gauge length of 50 mm was used in the tensile tests.
kem, H301, melt flow index of 10 g/10 min at 230 °C and 2.16 kg,
Scanning electron microscopy (SEM) was used to monitor the
density q = 0.905 g cmÿ3) and high density polyethylene (Braskem,
cryogenic fracture surface of the fibres and injection moulded com-
JV060U, melt flow index of 6.8 g/10 min at 190 °C and 2.16 kg,
posites. The samples were maintained for 30 min in liquid N2 be-
q = 0.957 g cmÿ3) were used as matrices. Curaua fibres, supplied
fore fracturing and were coated with Pt/Au (80:20) by sputtering.
by Embrapa-PA (Belém, Brazil), were milled in a three knives rota-
Composites samples were prepared with the specimens with
tory mill (Rone, model NFA 1533) with a 7 mm mesh sieve to a
mechanical properties closer to the average values of the mechan-
length of 7–3 mm and a number-average diameter of 140 lm
ical tests. SEM analyses (Jeol, JSM–6360LV) were performed at an
(measured by optical microscopy, see below for details).
accelerating voltage of 25 kV.
Composites were processed in a co-rotating intermeshing twin-
screw extruder (ZSK 26 Mc, Coperion Werner & Pfleiderer, Ger-
many) with an L/D ratio of 44. fibres were fed through a side-feeder 3. Results and discussion
and degassing was also employed. The temperature profile used
(from feed to die) was 160, 160, 165, 165, 170, 170, 170, 170, 3.1. Effect of screw rotation speed in fibre dimensions
180, 175, 170 °C for PP and 120, 120, 125, 125, 130, 130, 135,
135, 140, 135, 130 °C for HDPE and the composites were cooled Several studies [8–10] have shown that during extrusion and
in water. To evaluate the effect of the screw rotation, the compos- injection molding processes, fibre geometrical parameters change,
ites containing 20 wt.% of fibres were prepared at different screw due to fibre breakage and disaggregation. To study this effect, com-
rotations, 250, 300, 350, 400 and 500 rpm. The SRS of the side-fee- posites containing 20 wt.% of curaua fibres were prepared at differ-
der was maintained 50 rpm below the SRS of the main screw for ent screw rotations, ranging from 250 to 500 rpm, for both
HDPE and 35 rpm for PP. All materials were processed with the thermoplastic matrices used. Fig. 1 shows the variation of the
same screw profile. The extruder was manually fed and the dosage cumulative distribution function of fibre length, diameter and as-
of the material was controlled by the torque percentage (ca. 30%). pect ratio for both composites processed at different screw rota-
Percentage of the fibre in the processed composites was evaluated tions. As shown in Fig. 1, fibre length shortening was observed
by measuring the density in a helium picnometer. The granulated after processing for all composites with PP and HDPE. Table 1
composites were dried in a conventional oven at 100 °C for 1 h shows the number-average fibre length for fibres before and after
and injection moulded into test specimens according to ASTM processing. Shear during processing causes a fibre length decrease
 B. Mano et al. / Composites Science and Technology 70 (2010) 29–35 31

a 1.0 b 1.0

0.8 PP matrix 0.8 HDPE matrix

0.6 0.6

CDF
CDF

0.4 0.4

0.2 0.2

0.0 0.0
0 2 4 6 8 10 12 14 16 18 0 2 4 6 8 10 12 14 16 18
Length (mm) Length (mm)
c 1.0 d 1.0

0.8 0.8
PP matrix HDPE matrix
0.6
CDF

0.6
CDF
0.4 0.4

0.2 0.2

0.0 0.0
0.00 0.04 0.08 0.12 0.16 0.20 0.24 0.28 0.32 0.00 0.04 0.08 0.12 0.16 0.20 0.24 0.28 0.32
Diameter (mm) Diameter (mm)

e 1.0 f 1.0

0.8
PP matrix 0.8 HDPE matrix
0.6 0.6
CDF

CFD

0.4 0.4

0.2 0.2

0.0
0 20 40 60 80 100 120 0 20 40 60 80 100 120
Aspect ratio Aspect Ratio

Fig. 1. Cumulative distribution function (CDF) of fibre length, diameter and aspect ratio for pristine fibre ( ) and composites of PP (a, c, e) and HDPE (b, d, f), respectively,
extruded at (e) 250, (s) 300, (4) 350 (h), 400 and ( ) 500 rpm.

from 5 mm to, at least, 0.90 mm for PP and 0.29 mm for HDPE

Table 1 matrix.
Effect of screw rotation speed (SRS) on number-average fibre length, diameter and
Increasing the extruder screws rotation cause a decrease in fibre
aspect ratio. Polydispersity of the data is given in parentheses.
length for both matrices, in agreement with results obtained by
SRS (rpm) Length (mm) Diameter (lm) Aspect ratio other authors [17,11]. An important factor that can be considered
Pristine fibre is the specific mechanical energy (SME) transferred to the material
– 4.7 (1.71) 139 (1.19) 36 (1.90) during compounding in relation to different SRS [15]. The SME is a
HDPE matrix function of screw rotation and may contribute to fibre breakage
250 0.29 (1.67) 26 (2.27) 18 (1.97) [15]. In this case, there was no significant increase in the SME for
300 0.26 (2.30) 24 (1.60) 16 (2.18) both matrices studied, Table 2, because the feeding in the extruder
350 0.20 (2.25) 20 (1.56) 15 (1.91)
400 0.19 (1.68) 19 (1.42) 12 (1.65)
was done maintaining the torque approximately constant at 35%.
500 0.10 (1.35) 17 (1.25) 7 (1.43) Thus, the effect of SME is not considered in this work.
PP matrix
It is possible to observe that for the same screw rotation, the fi-
250 0.90 (1.52) 73 (1.33) 15 (1.76) bres suffer more breakage in length when processed with the HDPE
300 0.70 (1.93) 60 (1.20) 15 (1.32) matrix than in PP matrix, this is possibly related to their intrinsic
350 0.54 (2.88) 46 (1.57) 13 (2.50) rheological properties [11]. In this study, the differences in the
400 0.50 (2.25) 47 (1.65) 11 (2.50)
MFI of the matrices may also contribute to the phenomena. The
500 0.28 (2.80) 40 (1.66) 9 (2.55)
MFI of HDPE (7 g/10 min) is lower than for PP (10 g/10 min), what
32 B. Mano et al. / Composites Science and Technology 70 (2010) 29–35

Table 2
Parameters registered during processing for the composites with PP and HDPE matrices.

SRS (rpm) Mass temperature (°C) Pressure (bar) Torque (%) Output (kg/h) SME (W h/kg)
HDPE matrix
250/200 136–160 4–19 33–40 1.9 1.1
300/250 143–164 4–22 34–38 2.2 1.1
350/300 140–168 6–16 30–42 2.4 1.2
400/350 151–172 5–23 28–41 3.1 1.0
500/450 145–178 9–14 32–37 3.5 1.1
PP matrix
250/215 171–195 7–16 31–41 2.5 0.8
300/265 177–195 8–16 30–37 2.6 0.9
350/315 177–199 7–16 29–34 2.6 1.0
400/365 175–204 10–16 27–34 2.9 1.0
500/465 178–202 10–12 29–37 3.6 1.0

implies in a higher viscosity for the polyethylene matrix. Shear erties of the composites. The efficiency of the reinforcement in-
stresses increase due to increase in viscosity [11] and, in this case, creases with aspect ratio until a maximum in continuous fibre
fibres may be subjected to stronger shear stresses in HDPE than in composites [19]. The aspect ratio can change, depending on the var-
PP, resulting in shorter fibres in the HDPE composites, Table 1. iation of fibre geometry: larger variation in length than in diameter
According to Von Turcovich and Erwin [16], in their study of the result in smaller aspect ratio after processing; on the other hand,
behaviour of glass fibres under shear flow, three principle mecha- larger variation in diameter than in length result in higher aspect
nisms explain the phenomena of fibre length decrease: fibre–fibre ratio. As can be seen in Fig. 1d and e, fibre aspect ratio decreases
interactions, fibre–equipment surfaces interactions and fibre inter- after processing, showing that fibre breakage is more intensive than
action with the polymer. The first two mechanisms are considered fibrillation. The reinforcement effect is a strong function of the fibre
as minor contributors to the phenomena. The main factor is fibre– aspect ratio and length distribution. The optimum aspect ratio, L/D,
polymer interaction, which is related to the melt rheology [8]. Dur- is around 100 and aspect ratio below 10 results in a decrease of the
ing the processing, shear forces generated within the extruder and reinforcement effect, due to stress concentrations that reduce the
acting in the molten polymer are transferred to the fibres and overall strength of the matrix [23]. According to Table 1, the aspect
breakage occurs when the shear stresses overcome the fibre tensile ratio decreases with SRS increase, for both matrices, being more
strength [17]. This model can be also applied to the present study. pronounced for PP above 300 rpm. For both matrices an aspect ratio
In contrast to synthetic fibres, changes in diameter occur with of 15–16 is achieved at 300 rpm, which is reasonable for a short fi-
vegetal fibres during processing, as a result of fibrillation. The tech- bre reinforcement agent.
nical fibre, shown in Fig. 2, is a fibre bundle composed of several
connected individual fibres [18]. Under shear, the individual 3.2. Mechanical properties
microfibres may disconnect from the bundle and, as a result, com-
posites have fibre bundles with shorter diameter and individual During the extrusion process, shear and heat are applied to the
microfibres dispersed in the matrix, as shown in Fig. 4. In Fig. 1c material at the same time. In this case, the mechanical effect asso-
and d and in Table 1, it can be seen that the fibre diameter distri- ciated with the temperature induces the thermo-mechanical deg-
bution in the composites is shifted to smaller values indicating that radation of the matrix. It is expected that the energy supplied by
fibrillation occurs in the processing. The diameter decreases three the extruder and by the heat induces the formation of macro-rad-
times, depending on the matrix and screw rotation speed, as icals from scissions of the polymer chains. The result of this effect
shown in Table 1. For both matrices, fibre diameter does not have depends on the chemical structure of the polymer, molecular inter-
any significant change at screw rotations up to 300 rpm. fibre actions, time of application of shear and temperature [20]. Similar
diameter variation is different in both matrices, indicating that to this, in the case of composites, the fibres also suffer the effects of
fibrillation also depends on the polymer matrix. However, higher shear and heat, however, curaua fibres thermal degradation starts
shear also induces a stronger fibre breakage; thus, for each SRS at 220 °C [21]. Both effects lead to consequences in the mechanical
the aspect ratio in both cases is the same, within the experimental properties of the composites [22,23]. In Fig. 3 we compare the
error. results of yield stress, r, modulus, E, and elongation at break, ?,
Aspect ratio is the ratio between the length and diameter of obtained from the tensile and flexural tests of the composites
fibres and is an important parameter affecting the mechanical prop- prepared at different screw rotations.

Fig. 2. SEM of technical curaua fibre before extrusion and injection molding: (a) side view and (b) top view of a cryogenic fracture.
 B. Mano et al. / Composites Science and Technology 70 (2010) 29–35 33

a 55 b 55
HDPE matrix PP matrix
50 50
σmáx. / MPa 45 45

40

σ máx. / MPa
40

35 35

30 30

25 25

250/200 300/250 350/300 400/350 500/450 250/215 300/265 350/315 400/365 500/465
screw rotation / side-feeder screw rotation / side-feeder

c 4.0
HDPE matrix d 4.0
PP matrix
3.5 3.5

3.0 3.0
2.5 2.5

E / GPa
E / GPa

2.0 2.0
1.5 1.5
1.0 1.0
0.5 0.5

250/200 300/250 350/300 400/350 500/450 250/215 300/265 350/315 400/365 500/465
screw rotation/side-feeder screw rotation / side-feeder

e 6
HDPE matrix
f 6
PP matrix
5 5

4 4
ε /%

3
ε /%

2 2

1 1

250/200 300/250 350/300 400/350 500/450 250/215 300/265 350/315 400/365 500/465
screw rotation / side-feeder screw rotation / side-feeder

Fig. 3. Yield stress, modulus and elongation at break in strain (j) and flexural (h) tests for HDPE (a, c, d) and PP (b, d, f), respectively.

The yield stress in tensile and flexural tests for the composites parameters, such as feed rate, screw rotation speed, temperature
with PP and HDPE matrix, Fig. 3a and b, decrease with the increase profile and residence time. Thus, in addition to the fibre geometri-
in SRS. For HDPE the decrease rate is higher. This is in agreement cal parameters, the loss in mechanical properties for the compos-
with the previous observation of decrease of aspect ratio with ites that occurs when changing the screw rotation from 250 to
SRS increase. Tensile modulus for HDPE, Fig. 3c, presents also a de- 500 rpm may also have contribution from the thermo-mechanical
crease with SRS increase; however, the flexural modulus is not af- degradation of the polymer matrix.
fected by the SRS. For PP composites, tensile and flexural moduli At the temperatures above the polymer melting temperature,
are not affected by SRS, within the experimental error, Fig. 3d. flow occurs with an alignment of the polymeric chains and the
The elongation at break presents a different behaviour; it increases shear stresses promote breakage of chemical bonds. In this case,
for HDPE at screw rotations above 300 rpm, Fig. 3e, and slightly in- part of the energy is supplied by heating and the scission of the
creases for PP composites above 350 rpm, Fig. 3f. chemical bonds is more favoured than at room temperature. Chain
These variations of mechanical properties can be correlated to scission depends on the elastic energy stored in the macromolecule
the variations in fibre aspect ratio shown in Table 1. A lower aspect and on the time that the molecule stays in the excited state. Chain
ratio will cause a lower reinforcement effect, as reflected by the de- scission will occur when the energy supplied (mechanical + ther-
crease in yield stress and tensile and flexural moduli with the in- mal) is higher than the energy of the chemical bond.
crease in SRS. Thus a higher SRS may lead to a higher output, but For HDPE, the thermo-mechanical degradation in an interme-
will compromise the mechanical properties of the composites. shing co-rotating extruder is caused by two competing processes:
Additionally, the polymeric matrices are also subjected to ther- chain-scission and chain branching, followed by cross-linking [12].
mo-mechanical degradation. From these results, we may conclude The origin of the chain-scission mechanism in HDPE is due to oxy-
that 300 rpm is the best processing condition for both matrices, gen attack to free radicals in the polymeric chain, yielding alkoxy
maintaining the temperature profile and screw design. and peroxy radicals. These radicals abstract hydrogen atoms from
In a processing technique, like extrusion, the thermo-mechani- the chain, giving rise to b-scission, leading to a decrease in molar
cal degradation strongly depends on screw design and processing mass and formation of carbonyl end groups. The chain branching
34 B. Mano et al. / Composites Science and Technology 70 (2010) 29–35

Fig. 4. Morphology of the fracture surface of injection molded HDPE composites with 20 wt.% of curaua fibres processed at: (a) 250 and (b) 500 rpm.

Fig. 5. Morphology of the fracture surface of injection molded PP composites with 20 wt.% of curaua fibres processed at: (a) 250 and (b) 500 rpm.

occurs when alkyl macro-radicals add to vinyl groups, yielding at The SEM images of the cryogenic fracture of the injection moul-
final stages crosslinked molecules [12]. ded composites of HDPE and PP, processed at 250 and 500 rpm, are
For PP, the mechanism of thermo-mechanical degradation oc- shown in Figs. 4 and 5, respectively. In all composites, there are fi-
curs by chain scission promoting a reduction in the molar mass bre bundles of different diameters and individual microfibres dis-
of the polymer. Polypropylene degrades preferentially by chain persed in the matrix. Better fibres dispersion and higher
scission due to the presence of hydrogen atoms bonded to tertiary fibrillation was observed in composites processed at higher screw
carbons in the backbone [12]. rotation, in agreement with the fibre diameter distribution shown
The parameters registered during the processing of the compos- in Fig. 1. It can be also observed that fibre pullout occurs during the
ites of PP and HDPE are shown in the Table 2. The mass tempera- cryogenic fracture [25]. No coupling agent was added to the com-
ture, i.e., the temperature registered at the die of the extruder, is posites; therefore the fibre–matrix interfacial adhesion probably
higher than programmed for this zone. For HDPE, the temperature should be limited, contributing to the occurrence of the fibre pull-
programmed at the die was 130 °C while for PP this temperature out [25].
was 170 °C. For both, the mass temperature increased with the
SRS due to high shear forces, causing degradation which may con-
tribute to changes in mechanical properties, as reported by Vas- 4. Conclusions
quez et al. [24]. The extruder output for both composites
increases with SRS, Table 2. The output depends not only on the The final properties of the composites reinforced with curaua
SRS, but also on the rheology of the material and the thermo- vegetal fibres processed by extrusion depend on several factors:
mechanical degradation of the matrix. the polymer matrix used for the preparation of the composites,
To access the effect of the thermo-mechanical degradation of the processing conditions and the geometrical parameters of the fi-
the polymer matrices the melt flow index of samples submitted bres after the manufacturing process.
to the same processing conditions was measured. In the case of The fibre dimensions decrease with the increase in SRS because
HDPE there is no detectable change in this parameter indicating higher shear forces cause fibre breakage and fibrillation. fibre
that chain-scission and cross-linking is occurring simultaneously, breakage occurred to a higher extension than fibrillation, decreas-
as reported by Canevarolo et al. [12]. For PP an increase of MFI, ing the aspect ratio of the fibres. In addition to the decline in the
from 10 to 12 g/10 min, is observed confirming the predominance aspect ratio, the increase in SRS promotes thermo-mechanical deg-
of the chain-scission mechanism. radation of both matrices (PP and HDPE), contributing to losses in
the yield resistance. The elongation at break increases due to the
chain scission processes that occur in both matrices at higher
3.3. Morphology SRS. The morphology showed that the dispersion of the fibres
was higher for composites processed at 500 rpm, due to increased
The morphology of the fibre before processing is shown in fibrillation, however, at 300 rpm the aspect ratio of the fibres is
Fig. 2. It can be seen that before extrusion and injection moulding, higher and the final mechanical properties are better.
the fibre is a bundle composed of several connected ultimate This work shows that a careful study of the processing condi-
microfibres, which give rise to the technical fibre. During the pro- tions is necessary to produce composites of polyolefins reinforced
cessing, the ultimate fibres can disconnect from the bundle, with vegetal fibres with adequate mechanical properties, in order
decreasing the fibre diameter distribution [11]. to compete with the traditional synthetic reinforcement agents.
 B. Mano et al. / Composites Science and Technology 70 (2010) 29–35 35

Acknowledgements [11] Alvarez V, Iannoni A, Kenny JM, Vazquez A. Influence of twin-screw processing
conditions on the mechanical properties of biocomposites. J Compos Mater
2005;39:2023–38.
Authors thank EMBRAPA-PA for the fibres, Braskem for the [12] Pinheiro LA, Chinelatto MA, Canevarolo SV. The role of chain scission and chain
polymer samples, FAPESP for financial support (2004/15084-6) branching in high density polyethylene during thermo-mechanical
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