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2 0 1 8;7(4):528–534

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Original Article

Critical length and interfacial strength of PALF and

coir fiber incorporated in epoxy resin matrix夽

Fernanda Santos da Luz ∗ , Flávio James Humberto Tommasini Vieira Ramos,

Lucio Fabio Cassiano Nascimento, André Ben-Hur da Silva Figueiredo,
Sergio Neves Monteiro
Military Institute of Engineering – IME, Materials Science Department, Praça General Tibúrcio 80, Urca, 22290-270 Rio de Janeiro, RJ,
Brazil

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

Article history: The several advantages of natural lignocellulosic fibers (NLFs), such as, economical, techni-
Received 11 November 2017 cal, environmental and social, make these fibers an alternative to replace synthetic fibers in
Accepted 24 April 2018 composite materials. The application of NLF as reinforcements in polymeric composites has
Available online 24 August 2018 increased in many industrial sectors from civil construction to automobiles. This demands
the characterization of promising fibers, such as those extracted from leaves of pineapple
Keywords: (PALF) and the mesocarp of coconut fruit (coir fiber), for possible application in composites.
Pullout test In the present work, pullout tests were performed to compare the interfacial adhesion with
Natural lignocellulosic fibers epoxy resin of these two fibers that have greatly different characteristics. Results showed a
Critical length critical length 70% higher for the coir fiber in comparison to PALF and a interfacial strength
Interface adhesion 3.5 times smaller, which indicates stronger adhesion of PALF with epoxy resin. This may
be justified by the distinct morphological aspects, particularly the rougher surface of PALF.
Mechanical tests were also performed in both coir fiber and PALF composites. In these tests,
it was observed the superiority of mechanical properties for the composite reinforced with
30 vol% of PALF. Additionally, ballistic tests were carried out. In this evaluation, composites
were used in a MAS type III against the 7.62 mm ammunition. The results revealed a rela-
tively low depth of penetration (18.2 mm) for the MAS with PALF composite as well as a depth
of penetration (31.6 mm) for MAS with coir composite, both considered efficient according
to the personal body armor standard. Therefore, all these results highlight the potential of
these fibers as polymer composites reinforcement in ballistic armors.
© 2018 Brazilian Metallurgical, Materials and Mining Association. Published by Elsevier
Editora Ltda. This is an open access article under the CC BY-NC-ND license (http://
creativecommons.org/licenses/by-nc-nd/4.0/).

夽
Paper was part of technical contributions presented in the events part of the ABM Week 2017, October 2nd to 6th, 2017,
São Paulo, SP, Brazil.
∗
Corresponding author.
E-mail: fsl.santos@gmail.com (F.S. Luz).
https://doi.org/10.1016/j.jmrt.2018.04.025
2238-7854/© 2018 Brazilian Metallurgical, Materials and Mining Association. Published by Elsevier Editora Ltda. This is an open access
article under the CC BY-NC-ND license (http://creativecommons.org/licenses/by-nc-nd/4.0/).
 j m a t e r r e s t e c h n o l . 2 0 1 8;7(4):528–534
a b
Fig. 1 – Natural lignocellulosic fibers as received: (a) coir fiber; (b) PALF.
1. Introduction
Over the last couple of decades, natural lignocellulosic fibers
(NLFs) are increasing their market share in many sectors, such
as furniture, packaging, building and automotive industries
[1–5]. This growing trend is due to their low environmental
impact, low cost and technical advantages in comparison
to synthetic fibers [2]. However, NLFs have hydroxyl groups
in their composition which makes them hydrophilic [6,7].
Indeed, the existing moisture on the surface of the fiber
might reduce its interfacial adhesion inside the composite,
because polymers commonly used as composite matrix have
hydrophobic character. Hence, chemical surface modification
or other pretreatment could be applied in NLFs to improve the
interfacial adhesion [2,6,8].
Initially, Kelly and Tyson [9] proposed the pullout test
to evaluate the interfacial adhesion between the fiber and
matrix, and later adapted by Monteiro and D’Almeida [10] for
lignocellulosic fibers. In this test, it is possible to determine the
fiber critical length and the interfacial strength that are asso-
ciated with the bonding efficiency of the fiber/matrix interface
[10].
In the present work, the fibers extracted from the leaves
of pineapple (Ananas comosus) known as PALF and the coir
fibers extracted from the mesocarp of the green coconut (Cocos
nucifera L.) were evaluated without pretreatment in pullout
tests embedded in epoxy matrix. These fibers are byproducts
of their fruits and, consequently, are inexpensive and abun-
dantly available. The physical characteristics of these fibers
differ greatly. The PALF has a high content of ␣-cellulose (up to
82 wt%), lignin content less than 12 wt% and low microfibrillar
angle (14◦ ), whereas the coir fiber is lignin-rich (>41 wt%) and
has around 40 wt% of cellulose and microfibril angle greater
than 40◦ [8]. Moreover, the PALF has an equivalent diameter
less than 300 ␮m [11] and the coir fiber has a higher diameter
(up to 600 ␮m) [12]. As a consequence the mechanical prop-
erties of PALF are superior than coir fiber and its behavior is
quite different [2,13].
In order to compare the adhesion behavior of these two
distinct fibers, pullout tests were performed to determine
the critical length and interfacial adhesion of PALF and coir
fiber with respect to the epoxy matrix, varying the embedded
lengths of the fibers as proposed by Kelly and Tyson [9] and
adapted by Monteiro and D’Almeida [10].
529
In addition, mechanical and ballistic tests were carried out
to evaluate the influence of interfacial adhesion of PALF/epoxy
and coir fiber/epoxy on the properties of their composites.
2. Materials and methods
The coir fibers were supplied by the Brazilian firm “Coco
Verde Reciclado” and PALF was provided by Desigan Natu-
ral Fibers, Brazil. Fig. 1 shows these fibers as received. Both
fibers were dried at 60 ◦ C in an air-oven for 24 h. The epoxy
resin of diglycidyl ether bisphenol-A (DGEBA) and hardener
triethylenetetramine (TETA) were used as matrix. These two
components were mixed with a stoichiometric ratio of phr
13.
Fig. 2 illustrates a specimen used for pullout tests. Epoxy
cylindrical blocks with 8 mm diameter were prepared by vary-
ing the single fiber embedded length from 2 mm to 43 mm for
both the PALF and coir fibers. The length and diameter of the
fibers were measured with a Zeiss Stemi 2000C stereoscope.
The pullout tests were performed by means of an Instron
universal model 3365 machine with a speed of 0.75 mm/min.
Tensile tests were also carried out in 10 single fibers for both
PALF and coir fiber.
The correlation between the interfacial adhesion and
mechanical properties for both PALF and coir fiber in epoxy
matrix was investigated through Izod and tensile tests. Epoxy
composites with 30 vol% of PALF as well as 30 vol% coir fiber
were produced, both with continuous and aligned fibers.
Embedded length
L
Fiber
σ σ
Epoxy block simulating
the composite matrix
Fig. 2 – Specimen used for pullout test.
530 j m a t e r r e s t e c h n o l . 2 0 1 8;7(4):528–534

a b
500
Tensile stress range

200 Present Work

400
[2,11,16,17]
Pullout Stress (MPa)

Pullout Stress (MPa)

160

300
120

200
80

100
40

lc = 12,4 mm Lc = 28,8 mm lc = 7,3 mm

0 0
0 5 10 15 20 25 30 35 40 45 50 0 5 10 15 20 25 30 35 40 45 50

Embedded lenght (mm) Embedded lenght (mm)

Fig. 3 – Results of the pullout test for the different embedded lengths: (a) coir fiber with epoxy resin; (b) PALF/epoxy.

Izod impact tests were carried out according to the ASTM Fig. 3a presents the linear adjustments of the coir fibers
D256 standard using an instrumented XC-50 model Pantec pullout tensile stress vs. embedded length, which correspond
pendulum. Composites specimens were cut with standard to Eqs. (1)–(3):
dimensions of 62.5 × 12.7 × 10 mm and notched with a 45◦ of
angle, transversely to fibers and the direction of compression f = 8.05 + 8.39 · L (1)
molding. Tensile tests were conducted in a model 3365 Instron
machine, according to ASTM D638 standard, with a cell load
f = 84.38 + 2.25 · L (2)
of 25 kN. In order to evaluate the influence of interfacial adhe-
sion in the dynamic response, ballistic tests were performed to
f = 156.05 − 0.24 · L (3)
compare the absorption capacity of the impact energy caused
by a 7.62 mm caliber high velocity ammunition in both 30 vol%
PALF and 30 vol% coir fiber composites used as a second layer Eqs. (4) and (5) represent the linear adjustment for PALF
in a multilayered armor system (MAS). The manufacturing of (Fig. 3b):
MAS has been described elsewhere [14]. These tests were con-
ducted at the Brazilian Army Evaluation Center (CAEx), in Rio f = 41.40 · L (4)
de Janeiro, Brazil, and the ballistic performance was assessed
by the depth of penetration caused in the clay witness as per f = 297.05 + 0.53 · L (5)
NIJ 0101.06 standard [15].
Analysis by scanning electron microscopy (SEM) were The intersection of Eqs. (1) and (2) defines the critical length
obtained in a model Quanta FEG 250, Fei microscope operating (lc ) for coir fiber. The same calculation could be done for PALF
with secondary electrons at 5 kV. through Eqs. (4) and (5). The critical length is reached at L
equal 7.3 mm and 12.4 mm for PALF and coir fiber, respectively.
Since small values of lc indicate greater interfacial fiber/matrix
adhesion [10], these results of 70% higher lc for coir fibers
reveal better adhesion between PALF and epoxy in comparison
3. Results and discussion with that of coir fiber.
As proposed by Monteiro and D’Almeida [10] it is possible to
Fig. 3 shows the results of the pullout tests for the different define a second critical length, Lc, for which the fiber does not
embedded lengths (L) for both PALF and coir fibers with respect detach completely from the matrix. This could be observed for
to the epoxy matrix. In the first stage, the tensile strength coir fiber (Fig. 3a). The value of Lc is given by the intersection
increases linearly with the embedded length of the fiber in of Eqs. (2) and (3), resulting in a length equal 28.8 mm.
the matrix. When this tensile strength reaches the fiber limit It is important to note that the error bars of the ten-
stress, then rupture occurs. The embedded length for which sile strength associated with L > lc are in the range of tensile
the fiber fails is known as critical length (lc ) i.e. for lengths strength reported in literature [2,11,16,17] and in the tensile
below lc the complete interfacial debonding occurs while at strength of the present work. This behavior is expected and
higher L the fiber failure occurs without debonding of the therefore corroborates the experimental data obtained.
fiber/matrix interface. The interfacial shear strength directly The interfacial strength ( c ) of PALF and coir fiber with
influence the mechanical behavior of the composite [8]. The respect to the epoxy matrix were evaluated by the equation
value of critical length defines if the fiber is long enough to act of Kelly and Tyson [9]:
as reinforcement or it is only an incorporated load. In other
words, whether or not there is stress transfer from matrix to d · f
lc = (6)
the fiber [10]. 2 · c
 j m a t e r r e s t e c h n o l . 2 0 1 8;7(4):528–534
a b
Fig. 4 – SEM of the heterogeneities of the NLFs cross sections: (a) coir fiber; (b) PALF.
a b
Fig. 5 – NLFs surfaces: (a) coir fiber; (b) PALF.
where  f is the tensile strength of the fiber and d is the equiv-
alent diameter of the fiber.
For each tested fiber the equivalent diameter was measured
as described in the work of Luz et al. [12]. This can be a source
of dispersion for NLFs diameters because of heterogeneity in
their cross sections, as shown in Fig. 4. The averages of equiva-
lent diameters were 238 ␮m and 314 ␮m for PALF and coir fiber,
respectively. The values obtained for interfacial strength were
1.42 MPa (coir fiber) and 4.93 MPa (PALF).
Therefore, the PALF/epoxy interfacial adhesion was
stronger than coir fiber/epoxy and PALF could more efficiently
transfer the mechanical strength to the composite matrix.
This higher adhesion could be attributed to the naturally
rougher surface of PALF [16–20], as illustrated in Fig. 5. Indeed,
a rougher surface allows an efficient penetration and anchor-
ing of the epoxy matrix.
Furthermore, the coir fiber has a thin aliphatic surface
layer (wax layer) which consists of a long chain of fatty acids
that are incompatible with polar matrix composites, resulting
in a weak interfacial adhesion, as reported in some studies
[4,5,10,21,22]. As coir fibers were used in as-received condition,
the presence of some protrusions with silicon-rich particles
was observed on their surface (Fig. 6). This may has also con-
tributed to low interfacial epoxy/coir fiber adhesion as noticed
by Prasad et al. [21]. They found that the removal of these par-
ticles and the wax layer from the coir fiber surface through
the NaOH mercerization process promoted a more rugged sur-
face resulting in a 90% increase in interfacial strength over
untreated fiber in the matrix polyester [21]. Fig. 7 reveals the
531
better impregnation of the epoxy resin in PALF than coir fiber,
which may contribute to the higher interfacial adhesion of
PALF/epoxy. Moreover, higher tensile strengths obtained for
single PALF fibers corroborate the trend reported in several
studies indicating higher mechanical strength for NLFs with
smaller diameters that could be explained by the lower prob-
ability of internal defects [2].
Table 1 shows the mechanical properties obtained in ten-
sile tests and the impact energy absorbed in Izod tests for both
epoxy composites reinforced with 30 vol% PALF and 30 vol%
coir fiber, in the longitudinal direction. It is clear that the PALF
composite presented more than twice the value of both ten-
sile strength and elastic modulus when compared to the coir
fiber composite. This can be explained by the predominance
of the brittle fracture mechanism for coir fiber composites,
which is typical of the epoxy resin. It also indicates that coir
fibers acted only as composite load, and no effective reinforce-
ment occurred in relation to the tensile properties. By contrast,
a higher pullout incidence was observed in PALF composites
in comparison to coir fiber composite. In PALF composites, the
brittle fracture mechanisms of the epoxy matrix together with
the debonding and rupture of the fiber justify a significant
increase in tensile strength and stiffness.
Although the heaviest hammer available (22 J) was used in
the Izod impact test, samples of composites reinforced with
30 vol% PALF did not break completely. Therefore, the impact
energy value for the PALF composite could not be compared
with the result of coir fiber composite, in which a complete
rupture occurred. However, the fact that PALF composite sam-
532 j m a t e r r e s t e c h n o l . 2 0 1 8;7(4):528–534

a b
Debonding epoxy/coir fiber interface

Si-rich particles

Fig. 6 – SEM showing the presence of some protrusions with silicon-rich particles in the surface and the debonding
interface.

a b

Fiber
debonding

Fig. 7 – SEM of the interface of composites: (a) coir fiber/epoxy; (b) PALF/epoxy.

Table 1 – Mechanical properties of epoxy composites reinforced with 30 vol% PALF and 30 vol% coir fiber.
Properties Composites

Epoxy/30 vol% coir fiber Epoxy/30 vol% PALF

Tensile strength (MPa) 28.7 ± 11.0 86.4 ± 16.9

Elastic modulus (GPa) 3.18 ± 0.30 7.97 ± 1.40
Elongation (%) 1.1 ± 0.7 1.3 ± 0.4
Impact strength (J/m) 111.0 ± 6.8 946.0 ± 140.0a

a
Did not occur complete breakage.

Table 2 – Depth of penetration (DOP) for MAS with different composites as second layer.
MAS second layer Depth of penetration (mm) Armor test velocity (m/s) Impact energy (kJ)

30 vol% coir fiber/epoxy 31.6 ± 2.7 852 ± 8 3.52

30 vol% PALF/epoxy 18.2 ± 2.7 847 ± 7 3.48

ples did not break completely is an indicative of the high
toughness of this composite, provided by PALF reinforcement.
In fact, if there were total rupture of this composite, the energy
absorbed would be even higher. In addition, the early failure
and low values of impact strength of coir fiber composite can
be attributed to the weak interfacial interaction between coir
fiber and epoxy resin.
DMA results are presented elsewhere [23], and support the
mechanical testing results. The curves of storage modulus also
indicated a greater reinforcement of epoxy composite with
30 vol% PALF in comparison to 30 vol% coir fiber. This trend
is given by the raising of the thermal mechanical stability at
high temperature denoted by a higher rubbery plateau for
PALF composite. These results also revealed an increase of
loss modulus and glass transition temperature values, which
means an efficient stress transfer through PALF/epoxy inter-
face.
The depth of penetration (DOP) in ballistic tests, corre-
sponding to the residual impact energy dissipated by the MAS,
was measured by means of a laser sensor and is shown in
 j m a t e r r e s t e c h n o l . 2 0 1 8;7(4):528–534
BEFORE
Fig. 8 – MAS with different second layers, before and after ballistic impact: (a) coir fiber composite; (b) PALF composite.
Table 2. The DOP results revealed that all values for both MAS
with 30 vol% coir fiber reinforced epoxy composite and 30 vol%
PALF/epoxy composite as second layer met the NIJ standard,
i.e. both exhibited an indentation (DOP) less than 44 mm [15]
(Table 2).
Based on these results, one should notice a reduction of
more than 42% in the DOP for the MAS with PALF composite
in relation to the coir fiber composite. A possible explanation
for it is due to the stronger PALF/epoxy interfacial adhesion.
Even though some ballistic studies on epoxy composites rein-
forced with different synthetic fibers have shown that higher
energy absorption occurs for weaker interfacial interactions
[24], the adhesion between coir fiber and the epoxy resin may
have been excessively weak causing premature failure of the
composite tested in this work.
Fig. 8 shows the aspect of MAS, with both coir fiber and
PALF composite, before and after ballistic tests. In these tests
it was verified that the coir fiber composites have been almost
completely spalled, owing to the brittle fracture of the epoxy
matrix. Thus, the coir fiber composite could not be used, in this
configuration, as a ballistic vest against high impact ammuni-
tion as 7.62 mm caliber. On the other hand, the MAS with PALF
composite, as a second layer, remained whole in most of sam-
ples after ballistic impact, which indicates the great potential
for the application of this fiber in ballistic armor.
4. Conclusions
• The coir fiber presented in pullout tests a critical length 70%
higher than PALF, which indicates weaker interfacial adhe-
sion between this fiber and epoxy matrix. Also, the value
533
AFTER
of interfacial strength for the PALF was 3.5 times greater
than coir fiber. This result could be justified by the rougher
surface of PALF and the presence of wax layer in the coir
fiber;
• A second critical length was found for the coir fiber. In the
embedded length between 12.4 mm and 28.8 mm the coir
fiber did not detach completely from the epoxy matrix;
• It was observed that the statistic dispersion of the tensile
strength associated with higher length is in the range of
tensile strength for single fiber found in literature and in the
present work for both PALF and coir fiber. This high disper-
sion is a consequence of their cross section heterogeneities;
• Coir fiber presented an equivalent diameter 30% higher than
PALF, which explains the higher strength associated with
PALF and corroborate the trend reported in several related
works;
• Tensile tests showed superior mechanical properties of
PALF composites as well as higher capacity of PALF com-
posites to absorb energy in Izod test in comparison to coir
fiber composite. This trend is supported by results of DMA
tests already published;
• In ballistic tests, the PALF composite exhibited the lowest
depth of penetration (18.2 mm), which represents a higher
ballistic performance as compared to MAS with coir fiber
composite. Combined, all these results highlight the poten-
tial of the PALF composite in ballistic armors.
Conflicts of interest
The authors declare no conflicts of interest.
534 j m a t e r r e s t e c h n o l . 2 0 1 8;7(4):528–534
Acknowledgements
The authors of the present work wish to thank the Brazilian
supporting agencies CAPES, CNPq and FAPERJ for the funding.
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