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Composites: Part A 38 (2007) 14551461

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Mechanical behavior and microstructural analysis of sugarcane


bagasse bers reinforced polypropylene composites
S.M. Luz a, A.R. Goncalves
b

a,*

, A.P. DelArco Jr.

a
Escola de Engenharia de Lorena, Universidade de Sao Paulo, P.O. Box 116, CEP 12602-810 Lorena/SP, Brazil
Divisao de Materiais, Instituto de Aeronautica e Espaco, Comando Tecnico Aeroespacial, Pc Mal do Ar Eduardo Gomes,
50, Vila das Acacias, 12228-904, Sao Jose dos Campos, SP, Brazil

Received 28 December 2004; received in revised form 23 November 2006; accepted 14 January 2007

Abstract
The compression and injection molding processes were performed in order to evaluate the better mixer method for ber (sugarcane
bagasse, bagasse cellulose and benzylated bagasse) and matrix (polypropylene). The samples (composites and polypropylene plates) were
cut and submitted to mechanical tests in order to measure exural and tensile properties. The morphological and microstructural analyses of fracture surface and specimens from composites can be easily evaluated by microscopic techniques. The fracture surface was evaluated by SEM and selected specimens from composites were analyzed by reected light in OM. The better tested method for composites
obtainment was the injection molding under vacuum process, by which composites were obtained with homogeneous distribution of
bers and without blisters. The mechanical properties show that the composites did not have good adhesion between ber and matrix;
on the other hand, the ber insertion improved the exural modulus and the material rigidity.
 2007 Elsevier Ltd. All rights reserved.
Keywords: A. Polymermatrix composite (PMCs); B. Microstructure; D. Mechanical testing; E. Injection molding

1. Introduction
Polymeric composites may be understood as the combination of two or more materials, for example, reinforcement elements or ller involved by a polymeric matrix
[1]. The introduction of bers (treated or in natura) into a
polymer is known to cause substantial changes in the
resulting composites [2,3], which may result, dierently
from the original materials, in good mechanical properties
and rigidity [4].
In recent years, studies about the utilization of lignocellulosic materials as reinforcement in polymeric composites
are increasing due to the improvements that natural bers
can provide to the product, such as low density and biodegradability, besides the fact that these materials are from
*

Corresponding author. Tel.: +55 012 31595033; fax: +55 012


31533165.
E-mail address: adilson@debiq.faenquil.br (A.R. Goncalves).
1359-835X/$ - see front matter  2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compositesa.2007.01.014

renewable and less expensive sources [5]. Many natural


bers have been used in automobiles, trucks, and railway
cars [4,6]. The sugarcane bagasse is a residue widely generated in high proportions in the agro-industry [7]. A Fibrous
residue of cane stalks is left over after the crushing and
extraction of juice from the sugarcane. It is a lignocellulosic
by-product of the sugar and alcohol industries and is
almost completely used by the sugarcane factories as fuel
for the boilers [8]. Dimensions of bagasse are of 1.2 mm
length and 15 lm width with 80 L/D [9]. The bagasse is a
vegetable ber mainly constituted by cellulose, that is a glucosepolymer with relatively high modulus, often found as
brillar component of many naturally occurring composites (wood, sugarcane straw and bagasse) in association
with lignin [10]. Many naturally occurring bers are used
in composites, but mostly in applications involving not
very high stresses [4].
Fibers and thermoplastic matrix can be placed together
in contact in the forms of polymer solution, polymeric

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lms, polymer in powder or granules, utilizing the mechanisms of compression molding by heating and injection
molding [1,11,12]. In these two mechanisms, the bers are
placed in intimate contact with the matrix.
Thermoplastic polymers are materials thoroughly used
in emergent technologies having low processing cost and
density, among other properties, such as transparency
and possibility of recycling [13]. Polypropylene (PP) was
the thermoplastic polymer used in this work, being a
semi-crystalline polymer and an important engineering
thermoplastic with various industrial applications [14],
but it is also a commodity polymer by the low cost, low
level of mechanical resistance, processing facility and larger
production [15]. Therefore, the combination of lignocellulosic material with thermoplastic matrix can present a considerable problem: incompatibility between the polar and
hygroscopic ber and the non-polar and hydrophobic
matrix. The possible solution for this problem has been
studied through the chemical modication of bers due
to the presence of hydroxyl groups, very reactive and susceptible to chemical reactions. Non-polar groups can be
inserted in the bers, resulting in hydrophobic characteristics compatibles with thermoplastic matrices [1,16,17].
Other alternative to improve the compatibility between
ber and matrix is to modify the matrix, for example, with
maleic anhydride [18].
Recent studies in respect to mechanical behavior of reinforcement bers in composites show that these materials
can present structural and non-structural applications.
The synergetic characteristics of composite materials
depend on the initial characteristics of the reinforcement
or the matrix [2]. Damage in the composites is associated
to matrix crack, failed interfacial bond between ber and
matrix, ber break and delamination. Composites fracture
surfaces have been studied by scanning electron microscopy (SEM), due to the great depth of focus exhibited by
this technique. Specimens are fractured by normal physical
testing procedures and SEM is used to evaluate size, distribution and adhesion of the ller bers or particles. The nature of adhesion between the matrix and the reinforcement
and information relating the structure of mechanical properties can be obtained by SEM assessment of the composite
fracture surface [19].
Reected light microscopy is a typical optical microscopy (OM), which provides an overview of composite
microstructure. Specimens are polished and examined in
reected light, generally at magnications about 30500
[19]. The strength of ber-reinforced composite depends
on the ber length and orientation, on the proportion of
bers in the matrix and on interfacial bond between the
ber and matrix [19].
This work aimed to evaluate the mechanical characteristics of PP-composites obtained by compression and
injection molding processes utilizing the bagasse, benzylated bagasse and bagasse cellulose as reinforcement. Some
composites were analyzed by SEM and OM techniques in
order to evaluate the morphological characteristics of

composites fracture surfaces, ber distribution and


microstructure.
2. Experimental
2.1. Materials description
Depithed sugarcane bagasse was kindly furnished by
Usina Sao Jose ZL (Brazil); the bagasse was washed, dried
and milled at particles <1 mm. Cellulose from sugarcane
bagasse was obtained by pulping with soda/anthraquinone
as described by Luz and Goncalves [20]. Benzylated
bagasse was obtained from sugarcane bagasse reacted with
benzyl chloride during 4 h, as described by Luz and
Goncalves [21]. Sawdust/PP composites, material utilized
as intern coating in cars, with 20 wt% sawdust were furnished by Simoldes Plasticos Ltda. Pinus elliottii is the
wood species of sawdust inserted inside PP. Polypropylene
(PP), material presented in granules (H 503), was kindly
furnished by OPP (Brazil).
2.2. Compression molding
In an uniaxial press, containing heating elements (inferior and superior), a molding tool was placed, containing
the materials for compression [bagasse (5 wt%)/polypropylene, and polypropylene]. The temperature, heating rate
and platform time were determinated utilizing the polypropylene. The adjusted parameters were: 205 C, 2 C min1
heating rate and 3 h platform time. Both composites and
polypropylene plates were obtained with these parameters.
The bagasse/polypropylene composite and polypropylene plate were cut using a dual-tape saw (Mecanica Europa
equipment with 1/400 sheet) in the necessary dimensions for
the mechanical tests (exural and tensile) and the material
polishing was made with sandpaper A80 (Acerbi
equipment).
2.3. Injection molding
Samples of 8.710 wt% bagasse, 6.7 wt% cellulose from
bagasse and 10 wt% benzylated bagasse were initially
mixed with polypropylene. The mixture was placed in an
injector camera at 200 C and 2 C min1 heating rate.
Starting from this temperature, the platform time was
3 h. The melted material was injected with or without vacuum in a pre-warm mold (200 C) with 3.2 220 230 mm
dimensions. Cutting and polishing were performed as
described in the compression molding.
2.4. Tensile tests
Composites were analyzed in an Instron universaltesting machine (model 4301), equipped with pneumatic
claws at a cross-head speed of 2 mm min1. Five specimens
of composites were analyzed, with dimensions in agreement
with the ASTM D 638 standard [22]: 19 mm width,

S.M. Luz et al. / Composites: Part A 38 (2007) 14551461

165 mm length and 3.2 mm thickness. The standard


demands specimens with dogbone or tie format, however, the specimens were cut in rectangular form; hence, the
results of the tests will be analyzed only comparatively.
2.5. Flexural tests
For these tests, the Instron universal-testing machine
(model 4301) equipment was also used, where a load was
applied on the specimen with crosshead motion rate of
1.3 mm.min1. The 5 specimens were analyzed with dimensions in agreement with the ASTM D 790 standard [23]:
25 mm width, 76 mm length and 3.2 mm thickness. The
adopted exural analysis was four-point at 1/4 points
method.
2.6. Scanning electron microscopy
The samples submitted to tensile tests were cut and the
composite intact fracture surface was analyzed in a LEO
1450 V scanning electron microscopy with tungsten lament operating at 20 kV, utilizing low vacuum technique
and work distance of 12 mm. Magnications of 60 and
4000 were made and a secondary electron detector was
utilized.
2.7. Optical microscopy
The selected region of the sample was cut and placed in
molds. Polyester resin and hardeners were mixed, poured
into the mold and cured to provide support. The samples
grinding was made with sandpaper ranging from 120 to
1000 grit. The specimens were polished using graded alumina suspensions in water. After the polishment, the specimens were observed by reected light in a LEICA optical
microscopy.
3. Results and discussion
The materials obtained by dierent methods (compression and injection molding) were analyzed separately.
3.1. Compression molding
The uniaxial press has two heating elements (inferior
and superior). The composites obtained by compression

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molding showed a homogeneous distribution of the bers


in the matrix. However, the distribution in the plate was
not uniform. Larger and shorter bers were found in the
superior and inferior parts of the plate, respectively. The
press action is from up to down and the shorter bers easily
penetrated into the melted polymer. Other problem found
in the composite was the presence of many blisters also
present in the polypropylene plate.
The amount of added reinforcement did not contribute to
the variation of the tensile and exural moduli (Table 1).
The bers insertion can contribute to the modulus increase,
because the Youngs modulus of the bers is higher than the
thermoplastic modulus. However, to obtain a signicant
increase, a good interfacial bond between ber and matrix
is necessary [24]. The exural and tensile strengths exhibited
a poor interaction between ber and matrix, with decreases
of 24.1% and 31.8%, respectively, in relation to the polypropylene.
The elongation decrease at break value (tensile test) for
the composite in comparison to the polypropylene, is
probably due to the defects generated in the material after
the bers insertion, which were not well aggregated to the
polypropylene. The rupture of the specimen was probably
originated by the presence of blisters. The blisters are
empty spaces, caused probably by air entrance in the
mold. This showed that the compression molding is not
the adequate method for thermoplastic composites
preparation.
3.2. Injection molding
In injection molding, after the optimization of temperature, platform time and heating rate conditions, various
composites from variable reinforcements were obtained:
bagasse, cellulose from bagasse and benzylated bagasse.
Sawdust/PP composite, material industrially obtained
was used for comparison.
The injected polypropylene did not present blisters
(Fig. 2a and b). In bagasse (8.7 wt%)/PP composite, the
bers distribution was homogeneous and random.
The composites presented few blisters in the interior of
the plate.
The composite with 10 wt% bagasse, utilizing polypropylene as matrix, did not present visible blisters, because
the injection was made under vacuum. The bers distribution was also homogeneous and random.

Table 1
Properties of the materials obtained by compression molding
Samples

Elongation at break (tensile) (mm)

Tensile strength (MPa)

Tensile modulus (MPa)

Polypropylene (PP)
Bagasse (5.0%)/PP composite

7.2 1.2
3.0 0.3

27.4 1.6
18.7 2.2

991.6 57.8
1001.9 95.7

Elongation at break (exural) (mm)

Flexural strength (MPa)

Flexural modulus (MPa)

7.9 0.4
6.9 0.5

25.3 1.0
19.2 3.1

Polypropylene (PP)
Bagasse (5.0%)/PP composite
Reinforcement in wt%.

241.9 18.4
223.8 21.4

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The cellulose from sugarcane bagasse and benzylated


bagasse was not adequate as reinforcement, since they left
several ber agglomerations in the matrix. The agglomeration is due to inecient bers dispersion inside matrix.
Hydrophilic bers are strongly attracted by themselves,
resulting in clusters.
The materials obtained by injection molding were jointly
analyzed in respect to the mechanical characteristics supplied by the tensile and exural properties.
Fig. 1 shows that the samples elongated before the rupture. In respect to the elongation (tensile tests), the
obtained composites presented shorter elongation compared to the polypropylene. Two hypothesis can be considered: (A) bers are failed points that can generate a crack,
and (B) there is a sliding of the bers in relation to the
matrix. The elongation at break of the composites in the
exural tests is smaller than that in the tensile tests, because
in this method the force application is dierent.
According to Sawer [19], the elongated materials present
ductile fracture and the failed points in composites exhibit
the brittle fracture (Figs. 3ad and 5ad). The Fig. 2a and b
show the SEM of polypropylene fracture surface and present a brittle fracture in lateral region and ductile fracture in
the border of the sample.
The strength properties in Fig. 1 show that the tensile
strength of the composites decreased in relation to the
polypropylene. The bers distribution of the bagasse
(10 wt%)/polypropylene composite was homogeneous
and without presence of blisters and the tensile strength
decreased only 33%, dierently of the composite with
8.7 wt% of bagasse, which value decreased 38% in relation to the polypropylene. This is probably due to the
interference of other defects, generated by the presence
of blisters. Fig. 3a shows a bagasse/polypropylene composite region that presents bers clumps and the bers
preservation can be observed by the morphological characteristic of lignocellulosics. The polypropylene (matrix)
presented a brittle fracture around the bers. Fig. 3b
shows the bagasse/matrix interface and that the failed
propagation goes into ber direction. The Fig. 3c and d
show the higher magnied micrograph of ber and
matrix interface and that the bers were pulled out of

Tensile

Sawdust (20%)/PP

Flexural

Cellulose bagasse (6.7%)/PP


Benzylated bagasse (10%)/PP
Bagasse (10%)/PP
Bagasse (8.7%)/PP
Polypropylene (PP)

10

11

12

13

Elongation at break (mm)

Tensile

Sawdust (20%)/PP

Flexural

Cellulose bagasse (6.7%)/PP


Benzylated bagasse (10%)/PP
Bagasse (10%)/PP
Bagasse (8.7%)/PP
Polypropylene (PP)
0

12

16

20

24

28

32

Strength (MPa)

Sawdust (20%)/PP
Cellulose bagasse (6.7%)/PP
Benzylated bagasse (10%)/PP
Bagasse (10%)/PP
Bagasse (8.7%)/PP

Tensile

Polypropylene (PP)
0

Flexural
200

400

600

800

1000

1200

1400

Modulus (MPa)

Fig. 1. Mechanical properties of composites materials obtained by


injection molding. The amount of reinforcement is expressed in weight
percentage.

the polymer and the adhesion between ber and matrix


failed.
The optical micrograph (Fig. 4a) exhibits the shape of
bagasse within matrix and a random distribution can be
observed. The higher magnied micrograph of bagasse
and polypropylene interface (Fig. 4b) shows a wetting or
major penetration of polypropylene into the ber, resulting
in better adhesion between ber and matrix.
Due to the agglomeration of reinforcement in some
points, the tensile strength, respectively for the composites
of cellulose from bagasse and benzylated bagasse,

Fig. 2. SEM of fracture surfaces of injected polypropylene: (a) lateral detail exhibits classical brittle fracture, and (b) detail of extremity of specimens
fracture exhibits a ductile fracture.

S.M. Luz et al. / Composites: Part A 38 (2007) 14551461

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Fig. 3. SEM of fracture surfaces of bagasse/polypropylene composite injected under vacuum. (a) Morphology of composite fracture surfaces towards the
bagasse the presence exhibits of brittle fracture. (b) Morphology of composite fracture surfaces exhibits the limit region between ber and matrix (brittle
fracture). (c and d) Higher magnication of limit region between ber and matrix.

Fig. 4. Optical micrograph with reected light of composite polished surface (bagasse/polypropylene). (a) 50 Magnied micrograph exhibits the bagasse
forms and distribution within the matrix. (b) 100 Magnied micrograph shows the detail of limit region between ber and matrix.

decreased 50% and 42%, when compared to the polypropylene. In the composite with sawdust/polypropylene
industrially produced, the tensile strength decreased 62.3%.
The modied ber (benzylated bagasse)/matrix interface
is shown in Fig. 5a. The bers presented circular cross-section shapes. In a recent work [20], in the chemical modication process, the lignin (natural ber component) was
partially removed by NaOH addition and the morphology
of benzylated bagasse was dierent in respect to in natura
bagasse as shown in Fig. 5b. In Fig. 5a, the bers are transversally aligned to the fracture. The higher magnied
micrograph of ber and matrix interface (Fig. 5c) exhibits
the pulled-out bers of the matrix by tensile stress. The

ber clumps were observed within matrix, resulting in areas


concentrated with bers and areas with excessive thermoplastic, which ultimately decreases mechanical properties.
The bagasse cellulose/matrix interface is shown in
Fig. 5d. Fibers exhibited poor ber wetting, as shown by
the clumps of bers with no polypropylene. The bers presented circular cross-section shapes.
The formation of clumps in the material is disadvantageous, due to the decrease of tensile strength (reinforcement:
cellulose from bagasse and benzylated bagasse). However,
in exural strength, these materials act dierently, resulting
in a smaller decrease of these values. For the composite with
sawdust, as the particles are very small (about 20 mesh), the

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Fig. 5. SEM composite fracture surface injected under vacuum: (a) benzylated bagasse/polypropylene interface showing the clumping and morphological
bers; (b) the micrograph shows the shapes of benzylated bagasse; (c) higher magnied micrograph shows the detail of region interface between ber and
matrix; and (d) bagasse cellulose and matrix interface showing the morphology of their composites.

exural strength decreased about 54% in respect to the polypropylene, due to larger amount of failed points.
The tensile and exural moduli are related to the material rigidity, and as previously mentioned, the Youngs
modulus was higher for the bers than for thermoplastics.
If the bers are distributed and aggregated to the matrix, a
higher exural modulus for the material can be resulted.
Comparing the values of tensile modulus between the
composites (Fig. 1), bagasse (10 wt%)/PP and sawdust
(20 wt%)/PP, the composites presented values very similar
to the neat polypropylene. The tensile modulus values for
the bagasse (8.7 wt%)/PP, benzylated bagasse (10 wt%)/
PP and cellulose from bagasse composites are smaller due
to the disadvantageous presence of defects.
For the composites, the exural modulus increased in
relation to that of the neat polypropylene (Fig. 1; except
for the composite with benzylated bagasse). As the exural
tests were made by the four-points method, the composite
with random distribution of the bers had a better performance. Better performance of composites with random distribution into the matrix is attained due to homogeneous
distribution of bers. The stress transference between ber
and matrix is more eective, aecting positively the
performance.
4. Conclusions
The best molding process is the injection under vacuum,
which leads to materials with homogeneous distribution of

bers and free of blisters. The exural and tensile tests show
that the obtained composites did not present good exural
and tensile strengths. The blisters and/or the non-homogeneity of the bers are defects in the material that directly
interfere in the mechanical properties, harming the obtainment of a material with high resistance. The composites did
not present, in general, a good interfacial contact between
ber and matrix. However, the bers insertion caused an
increase in the exural modulus, turning the materials more
rigid. The mechanical properties of the obtained composites
are comparable to the commercial material with 20 wt%
sawdust and PP. The composites utilizing bagasse (treated
or in natura) can be investigated, seeking a similar application, for example, in coatings of pieces of automobiles. The
SEM and OM techniques permit the study of the morphology and microstructure of composites.
Acknowledgements
The authors acknowledge FAPESP, Capes and CNPq
for fellowships and nancial support.
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