INTRODUCTION

The environmental requirements and consciousness of the environment global issue

stimulate researchers to develop new composite materials stemming from renewable and
biodegradable resources [1], these new materials are one of the most promising alternatives
to replace the composites with the synthetic fibers especially for industrial applications
such as automotive and construction [2-5]. Currently, the polymer matrix composites
reinforced with natural fibers such as kenaf, hemp, flax, coir, cotton, jute, sisal, luffa,
etc...are studied by many researchers[6-9]. These composites offer a lot of advantages
compared to those based on synthetic fibers [10], these new materials have good properties
including low density, good mechanical properties, non-toxic, biodegradable, non-abrasive,
sound insulation and have moderate costs[11-14].

The mechanical behavior of cellulosic fibers in terms of specific tensile strength,

flexibility and specific stiffness are greater than that of the glass fiber [15]. All these
aspects make their use very attractive to the manufacture of polymer matrix composites,
However, some limitations such as low moisture resistance and hydrophilic nature that
leads to high moisture absorption resulting in dimensional changes in the fibers which
involves a decreased ability to transfer constraints between matrix and fibers[16]make these
natural fibers based composites not able to compete with those based on synthetic fibers in
some areas [17]. Furthermore, the addition of glass fibers contributes to a remarkable
improvement of the resistance to moisture, thermal properties[18]and increases engineering
applications. For example some studies [19] showed that the alkali treatment with sodium
hydroxide influences the mechanical properties of sisal fibers, the experimental results
obtained from treatment with 5% NaOH over 30 min, showed a 36% increase in resistance
tensile strength and a 53% improvement in the Young's modulus. Other results lead to the
conclusion that a reinforced composite 0.4Vf fiber mat Luffa treated with NaOH gained
13.7%, 6%, 72.43% and 163.6% of the resistance tensile, compression, flexural, and impact
strength, respectively, relative to composites reinforced by the untreated fiber[20].

The development of biodegradable materials that combine the properties of both

synthetic fibers and innovative and ecological properties of natural fibers could contribute
to the carbon cycle management in a sustainable way in reducing the use of synthetic
products. Many studies are dedicated to develop new composite containing both natural and
synthetic fibers, and these hybrid composites showed better impact strength and other
mechanical properties [21-25]

In the present work, we have developed hybrid composite materials based on

untreated Luffa and glass fibers added to a polyester matrix in form of laminates containing
four alternating layers LF sheet and GF sheets fabricated by the resin transfer molding
(RTM) method. The effect of LF volume fraction and the order of LF and GF sheets
superposition in the composite on the mechanical properties and water absorption behavior

1
were studied and discussed. The mechanical characterization tests such as tensile and three
points bend testing were carried out on samples for the determination of constants
characterizing our laminates. A modeling of the mechanical properties using various
analytic models has been also presented. At the best of our knowledge no study on the
effect of organization of the sheets of LF and GF on the mechanical properties has been
published in the literature.

MATERIALS AND METHODS

Materials

The materials used in this study are the unsaturated polyester resin (PU), Luffa fibers (LF)
and glass fibers (GF). Luffa fibers were collected from a rural area of morocco then cut in
two half to remove pips and the inner rough part of the dry fruit. Luffa fibers were then cut
in the RTM mold dimension and pressed with a hydraulic carver press. To prepare
composites, glass fibers mat and luffa fibers sheet with a surface mass of 0.0939 g/cm2
(Figure 1) were arranged sheet by sheet to reach the 20 vol.% and the required thickness of
the RTM mold.
The composite composition and the superposition of fibers sheets are described in Table 1.

Composites preparation

The implementation process used for manufacturing the composites is injection RTM (resin
transfer molding) in which a liquid pre-catalyzed resin is injected under pressure (2.5 bars,
at room temperature) through a fibrous reinforcement positioned in a closed homemade
mold. The polyester mixtures were cross linked using a 1.5% of a catalyst type Methyl
Ethyl Ketone Peroxide (MEKP) also commercially named AKPEROX A50. The used
reinforcement is the mats of glass fibers and luffa fibers. Prepared plates are dimensioned
as: (200mmx200mmx 8mm).

Scanning electron microscopy (SEM)

Microscopic observation of composites surfaces was carried out by (XL30ESEM), and it is

used to identify the fibrillose morphology of the luffa fibers also to evaluate surface
interaction between fibers and the polymer. The composites were fractured after having
been chilled in nitrogen liquid. Fractured surfaces were sputter-coated with gold prior to SEM
observation.

Mechanical tests

For each composite, tensile tests were performed using four specimens. The prepared plates
were cut to obtain tensile samples sized according to the norm DIN 50125[27] (Figure 2).

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Tensile tests were performed on a universal testing machine WP300 with a maximum load
capacity of 20kN, equipped with data acquisition software for the storage and processing of
data (load, strain, time…). The flexure tests were performed using rectangular specimens
sizing 70mm x 8mm x 8mm (length x width x thickness). For each composite an average of
four measurements has been performed to determine the flexural parameters.
Hardness test was carried out using the same universal machine WP300 as both previous
tests. The load was normally applied to the surface of the prepared samples (dimension:
303010mm3) According to the ISO 6506 [28]. A total of four specimens were tested for
each composite`s combination.
The Brinell hardness is calculated by dividing the load applied by the surface area of the
indentation.

2x0.102x
=
( − ( − )

Where D is the ball diameter (mm), F is the test load (N) and d is the mean diameter of the
imprint (mm).

Water uptake Tests

Water uptake tests were conducted by submerging the composite specimens in a water bath
at room temperature. The specimens were taken out from water, wiped with filter paper to
eliminate surface water, weighted in a high precision balance and then immersed again in
water, this process was repeated every two hours until reaching saturation plateau.
Measurement of the specimen`s weights was done as quick as possible to avoid evaporation
of water effects. The percentage of the water content (Mt) was determined using the
following equation [29]:

−
=

Where Wtis the weight of the sample at time t and Wois the initialweight of the sample.

RESULTS AND DISCUSSION

Morphological characterization
The SEM micrographs of composites fracture surfaces are shown in Figure 3-a and 3-b. It
can clearly be seen that the sheet of LF and GF are well filled by the resin. No voids were
detected. This means that RTM process is appropriate to prepare compact composites
owing to the high pressure used to fill the mold. On the other hand, the interfacial adhesion
isn`t good neither between the polymer and the luffa fibers nor between the polymer and
the glass fibers. In fact, at the fracture surface many fibers (LF and GF) are pulled out

3
letting clear holes at the opposite surface (see especially figure 3-c and 3-d). Some specific
treatment is needed to improve the adhesion at the interface.

Tensile testing

The results of tensile testing (Figure 4) showed that all the composites are brittle. The
mechanical characteristics vary depending on the rate of natural fibers and the position of
plies (table 2). Thus, when the LF plies and GF plies are alternating better mechanical
properties are obtained from tensile tests.
The load vs deformation derived from tensile test experiments is presented in figures 4. The
mechanical properties (Modulus and strength) derived from these results are presented in
table 2. It can be clearly seen that all the composites are brittle. The tensile modulus slightly
increased after introduction of 20 vol.% of Luffa but the strength decreases significantly.
This decrease can be attributed to the weak interfacial adhesion between the polymer and
Luffa fibers as has been shown by SEM analyses. However, it can be noted from table 2
that the mechanical properties of the laminates can be improved by the incorporation of
glass fiber sheets. The initial Young's modulus increased from 2.8 GPa for the polyester
matrix loaded with 20 vol.% of Luffa fibers to 9GPa for the alternate hybrid composite
(LF/GF/LF/GF). On the other hand, it can be clearly observed that manner of fibers sheets
organization in the composite has significant influence on the mechanical properties. In fact,
the tensile modulus is significantly higher for the composite (LF/GF/LF/GF) compared to
the composites ((GF/LF/LF/GF) and (LF/GF/GF/LF)). Similarly the strength is also
significantly higher for the first composite. This result is very interesting and could be
attributed to the change in stress repartition as function of the sheets organization in the
composite but also the interface could have an influence. We didn’t have clear explanation
to this phenomenon but this open a new field of investigation from experimental and
theoretical point of view.

Three points flexural test

The fiber content and fiber strength are influencing parameters for the strength of the
composite [30]. Figure 5 illustrates the three-point bending tests for laminate composite
structures consisting of different combination of plies (sheets). The effect of fiber content
and layers organization on the Flexural modulus of composites is shown in table 2. The
Flexural modulus increases with increase in glass fiber content up to 20vol.%. On the other
hand, the flexural modulus values of (GF/LF/LF/GF), (LF/GF/LF/GF) and (LF/GF/GF/LF)
composites differ even they have the same natural fiber content, however, composites with
GF layer in the bottom (GF/LF/LF/GF, LF/GF /LF/GF) have the higher flexural modulus
which is due the glass fibers tensile modulus. This bottom GF sheet undergoes a tensile like
deformation is more resistant to deformation in these composites.
A similarity between the flexural strength results and tensile strength can be observed in
table 2, where composite LF/GF/LF/GF showed the best flexural and tensile strength
properties (140.80MPa, 49.40MPa resp.) compared to GF/LF/LF/GF (139.96MPa,

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41.38MPa resp.) and LF/GF/GF/LF (92.43MPa, 33.08MPa resp.). Thus, composites with
GF layer in their bottom exhibit better flexural response.

Hardness tesing

The variation of the Brinell hardness value (BH) for laminate compositeis are shown in
table 2. The hardness of composite materials increases with increase in glass fiber content
up to 20 vol.%. The Brinell hardness value of (GF/LF/LF/GF),(LF/GF/LF/GF) and
(LF/GF/GF/LF) composites differ even they have the same natural fiber content, it is
clearly evident that the composites were GF layer is contact area with metal ball have the
higher hardness. The results showed that GF had a good ability to endure plastic
deformation.

Water uptake test

The results obtained from this experimental study are presented in figure 6. It can be seen
that all samples absorbed water very rapidly during the first hours, reaching a saturation
point and the water uptake of the composites increases with increasing the Luffa fiber
content up to 20 wt.%.

Free water molecules diffuse through the micro-cracking and pores into polymer matrix.
This further reduces interfacial adhesion of fiber with the matrix, causes swelling of the
luffa fibers, contributes to the formation micro-cracks in the matrix and may eventually
lead to debonding between the fiber and the matrix [31]. The glass fibers absorb less water
than luffa fibers and then contribute to a remarkable improvement of the resistance to
moisture [18].

The percentage of water uptake in the composites depends on two major factors, the first is
the LF and GF proportions and the second is the organization of the sheets in the laminate.
When the composite contains 20 vol.% (LF) layers (figure 7a), water absorption was in all
directions (lateral and transversal directions).However, when Luffa fiber layers are covered
between two glass fibers layers (figure 7b)it absorbs water principally from the lateral
directions. In case when glass fiber layers are covered between two Luffa fiber layers
(figure 7c), it was found that the absorption of water occurs laterally and transversely, and
is then higher the previous case. The composite with 20 vol.% (GF) showed higher
absorption in comparison to the neat polymer. This which is probably due to hydrophilic
character of glass fibers but could also due to the weak surface interaction between (GF)
and the polymer as shown by SEM analyses (figure 3).

Modeling

Experimental results of tensile tests were compared with the most commonly analytical
models. Voigt and Reuss models, Hirsh models, and hirsh-dougill equation have been used
to evaluate the modulus of composites.

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Voigt and Reuss models
Voigt assumes that the phases are arranged in parallel and the representative elementary
volume (REV) is solicited in the direction of the fibers.

E = υ E + (1 − υ )E (1)

Reuss supposesthat the REV is solicited in the direction perpendicular to the fiber, which
means that the phases are arranged in series.

E = (2)
υ ( υ)

Hirsch model

The Hirsch model is a combination of the two previous models of Voigt and Reuss, by
introducing an x parameter which depends mainly on the fiber orientation, it also takes into
account the transfer of stresses between the fiber and the matrix and the stress concentration
at the ends of the fibers. According to this model, the Young's modulus is calculated using
the following equations.

E = x (E (1 − υ ) + E υ )) + (1 − x ) (3)
( )

Were x is an adjustable parameter and its value is somewhere between 0 and 1. The
adjusting factor expresses the contribution of parallel and series type distribution of the
polymer matrix. For x = 0, the Hirsch model is reduced to Reuss model, and for x = 1, it is
reduced to Voigt model. The Figure 8 shows the orientation of Luffa’s fiber, it can be seen
that this orientation properly described withHirsch model.

In our case we have a mixture of different volume fractions of Luffa and Glass
fibers. For each composition we calculated an average modulus ‘’Ef’’ of the fibers
according to the following equation:

Ef = Xvol(Luffa). Eluffa + Xvol(Glass). EGlass (4)

We calculated the value of the modulus for the luffa according to the empirical formula
proposed by some researchers for natural fibers [26], we found:

Eluffa = 2.04 GPa

EGlass= 75 GPa

Thus for each fibers composition we have a different Ef. Table 3presents the values of the
modulus calculated according to the different models. It can be clearly seen that the
mechanical behavior of the composites is between the bounds of Voigt and Reuss models.

6
However, we note better correlation between the experimental results and those of the
Hirsch model with an adjustable parameter between 0.37 and 0.55, especially for the
composites filled with 20 vol.% LF and 20 vol.% of GF.

CONCLUSION

This study aims to prepare and judiciously characterize layered hybrid composite based on
polyester thermoset resin and the combination of Luffa and glass sheets of fibers. RTM
technique has been used for composites processing. The idea behind is to replace part of
glass fibers by natural fibers in order to reduce the cost and develop partially eco-friendly
composites.

The SEM characterization showed that the RTM process enable to prepare
composites free of voids. However the interface between the fibers (Luffa or glass) and the
polymer needs to be improved. The characterization of the mechanical properties has been
performed using tensile, three point flexural and hardness tests. The results show that the
mechanical properties of the laminates can be improved by the incorporation of the sheets
of glass fibers. While replacing 50% of glass fibers by Luffa fibers, good mechanical
properties are still maintained. Luffa fibres are hydrophilic in nature and hence have a poor
resistance to water uptake, the water absorption patterns of these composites at room
temperature was found to increase with increasing fibre content. On the other hand the
deposition of the two different fibers sheets has great influence on the mechanical
properties and water absorption.
The modeling of the mechanical properties showed that the mechanical properties are well
described by Hirsch model with an adjustable value between 0.37 and 0.55.

These results are very promising. Improvement could be performed in term of

interfacial adhesion promotion and sheets deposition. This work opens very good
perspective for Luffa fibers.

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List of figures caption:

Figure 1. (a) Glass fiber mat GF. (b) Luffa fiber LF.
Figure 2. Tensile test Specimens.
Figure 3. SEM analyses of the fractured surface of the composites reinforced with LF and
GF. (a) GF/GF/GF/GF, (b) and (c) LF/GF/LF/LF, (d) LF/GF/LF/GF.
Figure 4. Load vs deformation curves derived from tensile tests.
Figure 5. Load vs deformation curves derived from flexural tests.
Figure 6. Examples of the organization of LF and GF sheets in the composites: (a)
LF/LF/LF/LF composite, (b) LF/GF/GF/LF composite, (c) GF/LF/LF/GF composite and (d)
GF/GF/GF/GF composite
Figure 7. Water uptake curves for composite at different percent of natural fibers.
Figure 8. Luffa’sfiber arrangement. (a) lowerLuffa layer, (b) top Luffa layer

List of table caption

Table 1. Sample`s composition and their designations.

Table 2.Composite mechanical properties
Table 3.Values of the modulus calculated according to the different models.

11
 Designation Polyester (vol. %) Luffa fibers (vol. %) Glass fibers (vol. %)
Neat polyester 100 - -
LF/LF/LF/LF 80 20 -
LF/GF/LF/LF 80 15 5
LF/GF/LF/GF 80 10 10
GF/LF/LF/GF 80 10 10
GF/LF/GF/GF 80 5 15
GF/GF/GF/GF 80 - 20
 Designation Tensile Young's Flexural Flexural Brinell
stress modulus stress modulus hardness
(MPa) (GPa) (MPa) (GPa)
Neat Polyester 9.48 2.57 - - -
LF/LF/LF/LF 7.96 2.82 43.75 0.66 11
LF/GF/LF/LF 35.95 4.61 42.09 0.72 8
GF/LF/LF/GF 41.38 5.66 139.96 3.95 14
LF/GF/LF/GF* 49.40 9.00 140.80 3.82 17
LF/GF/GF/LF 33.08 5.36 92.43 2.17 15
GF/LF/GF/GF 59.95 9.03 161.1 5.32 16
GF/GF/GF/GF 72.74 8.9 172.9 5.67 30
*: GF has been the bottom in three point test but in the top for hardness test.
 LF/LF/LF/LF LF/GF/LF/LF LF/GF/GF/LF GF/LF/LF/GF LF/GF/LF/GF GF/LF/GF/GF GF/GF/GF/GF

Voigt 2.86 6.31 9.76 9.76 9.76 13.2 16.65

Reuss 2.77 3.11 3.15 3,15 3.15 3.17 3.18

Voigt/Reuss 3.74 4.84 5.18 5.18 5.18 5.36 5.46

Reuss/Voigt 2.40 3.95 3.61 3.61 3.61 3.44 3.31

Hirsch (x=0.37) 2,8 4.31 5.62 5.62 5.62 8.12 8.23

Hirsch (x=0.55) 2.82 4.87 6.78 6.78 6.78 8.68 10.58

Hirsch-Dougill 2.814 4.166 4.763 4.763 4.763 5.11 5.34

experimental
2.82 4.61 5.36 5.66 8.05 9.03 8.90
Results