Empty Fruit Bunches as a Reinforcement

in Laminated Bio-composites

H. P. S. ABDUL KHALIL,* M. R. NURUL FAZITA, M. JAWAID, A. H. BHAT

AND C. K. ABDULLAH
Division of Bioresource Technology, School of Industrial Technology, Universiti Sains
Malaysia, 11800 Penang, Malaysia

ABSTRACT: In this article, we study laminated bio-composites that were reinforced

with empty fruit bunches. Five-ply veneer laminated bio-composites were prepared
by alternately arranging oil palm trunk veneer and empty fruit bunch mat.
Composites were made with a gluing layer of 250 or 450 g/m2 of phenol formalde-
hyde. The mechanical, physical, and thermal (TGA) properties of the composite were
studied. Results indicated an improvement in mechanical, physical, and thermal
properties of the laminated bio-composites with the use of empty fruit bunches as
reinforcement. The water absorption and thickness swelling of laminated bio-com-
posites that were reinforced with empty fruit bunches were better than bio-compo-
sites not reinforced with empty fruit bunches. Laminated bio-composites with the use
of empty fruit bunch as reinforcement showed better bending strength, bending
modulus, and screw withdrawal. Thermal stability for laminated bio-composites
with empty fruit bunch also improved. Images taken with a scanning electron micro-
graph indicated an improvement in the fiber—matrix bonding for the laminated panel
glued with 450 g/m2 of phenol formaldehyde.

KEY WORDS: laminated bio-composites, oil palm trunk veneer, empty fruit
bunch.

INTRODUCTION

HE OIL PALM (Elaeis guineensis Jacq.) tree cultivation in Malaysia originated from
T West Africa where it was growing wild and later developed into an agricultural crop.
The oil palm is a tropical palm tree therefore it can be cultivated easily in Malaysia. The
first commercial oil palm estate in Malaysia was set up in 1917 at Tennamaran Estate,
Selangor [1]. Oil palm industries in Malaysia generate about 90 million tonnes of renew-
able biomass (trunks, fronds, shells, palm press fiber and empty fruit bunches) per year,
including about 8.2 million tonnes of oil palm trunks, 12.9 million tonnes of pruned and
felled fronds, and 15.8 millions tonnes of oil palm empty fruit bunches (EFB) [1,2]. The oil

*Author to whom correspondence should be addressed. E-mail: akhalilhps@gmail.com

Journal of COMPOSITE MATERIALS, Vol. 45, No. 2/2011 219

0021-9983/11/02 0219—18 $10.00/0 DOI: 10.1177/0021998310373520
ß The Author(s), 2011. Reprints and permissions:
http://www.sagepub.co.uk/journalsPermissions.nav
Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
220 H. P. S. ABDUL KHALIL ET AL.

palm biomass (OPB) is classified a lignocellulosic residues that typically contain 50%
cellulose, 25% hemicellulose, and 25% lignin in their cell wall [2]. These excess materials
have the potential to be used as raw materials in wood-based industries. As such, the oil
palm industry must be prepared to take advantage of the situation and utilize the available
biomass in the best possible manner [3].
A lot of construction material consists of engineered wood products. As such, the
intrinsic variability is stabilized, precise specifications are met, and by-products of wood
manufacturing can be processed. An important representative of this group of materials is
plywood showing excellent physical and mechanical properties [4]. Conventional plywood
consists of a flat panel built from sheets of veneer referred to as plies. Multiple plies are
placed under pressure with a bonding agent, producing a panel with an adhesive bond
between plies as strong as, or stronger, than wood. Plywood is assembled from an
odd number of layers, with the grains of adjacent layers arranged in a perpendicular
fashion [5]. More recently, new innovative bio-composite products based on natural
fibers, such as agricultural fibers or residues, or wood with natural fiber laminates, have
been introduced in the market and directly compete with traditional wood composites [6].
The first wood adhesive matrix material used in the mass production of plywood panels
was phenol formaldehyde (PF). Phenol formaldehyde is widely used in applications that
require stability in severe weather conditions, such as plywood for exterior construction [7].
Despite the emergence of several new classes of thermosets, high-performance polymers
and several other new generation materials that are superior in some respects, phenolic
resins retain industrial and commercial interest a century after their introduction. This
recognition emerges from the fact that these resins have several desirable characteristics,
such as superior mechanical strength, heat resistance and dimensional stability as well as
high resistance against various solvents, acids, and water. They are inherently flame resis-
tant, and evolve low smoke upon incineration [8]. PF type adhesives are environmentally
acceptable because of the negligible formaldehyde emission. They are structurally durable,
provide high quality wood bonding, and are suitable for use under all climatic conditions.
However, conventional PF adhesives are slow curing, require higher curing temperature,
and are less tolerant to variations in anatomical features and wood substrate [9].
Phenol—formaldehyde adhesives are used to glue the veneer plies of exterior-grade ply-
wood panels, the flakes of oriented strandboard (OSB) panels and particleboards panels.
PF resins provide high strength and are extremely resistant to moisture, which prevents
delamination and gives excellent temperature stability and low initial viscosity. This is in
part due to the more flexible nature of phenolic resins [10].
There is currently considerable research concerning the use of oil palm biomass as the
structural component in various products, with results showing that these materials have
the potential to replace traditional wood and fiber derived from forests. Previous work
using laminated bio-composites made from only oil palm trunk veneer did not achieve
satisfactory properties. Therefore, we investigate the properties of experimental low matrix
bio-composites using oil palm trunk veneer reinforced with oil palm empty fruit bunches in
a phenol—formaldehyde matrix in this study. Among the other oil palm fiber residues,
OPEFB offers the best prospect for commercial exploitation since it is readily available at
the palm oil mill which can minimize transportation and procurement costs. In Malaysia,
OPEFB is one of the biomass materials, which is a by-product from the palm oil industry.
This OPEFB has high cellulose content and has potential as natural fiber resources, but
their applications account for a small percentage of the total biomass productions. Several
studies showed that OPEFB of oil palm with the average of cellulose content of 49—65%

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 221

has the potential to be an effective reinforcement in thermoplastics and thermosetting

materials [11,12]. In this study, the physical, mechanical, and thermal properties of this
laminated bio-composite were evaluated.

EXPERIMENTAL

Materials

Phenol formaldehyde was supplied by Hexion Specialty Chemicals Sdn. Bhd. Oil palm
empty fruit bunch fiber (OPEFB) mats were obtained from Ecofuture Berhad. Oil palm
trunk (OPT) veneer was supplied by Kin Heng Timbers Industries Sdn. Bhd., Perak,
Malaysia.

Preparation of Laminated Bio-composites

The OPT veneers were cut to 600  300  4.0 mm3 samples and dried to approximately
10—12% moisture content. The determination of moisture content was carried out in
accordance with BS EN 322 : 1993. The moisture content of the samples measured by
placing the samples in a drying oven at a temperature of 103  2 C until a constant
mass was reached. The reinforcing empty fruit bunches was cut into mats
600  300  6 mm3. The OPT veneer and EFB fiber mat were then impregnated with PF
resin. The samples were then arranged into 5-ply laminated bio-composites, consisting of
alternating OPT veneers and EFB fiber mats with the veneer was arranged in different
direction for EFB-reinforced laminated bio-composites and for the OPT laminated bio-
composites, each veneer was arranged also in different direction as shown in Figure 1.
Four types of bio-composite samples, which are OPT composite and hybrid composite
(OPT þ EFB) with glue spread level (250 g/m2) and glue spread level (500 g/m2) were pre-
pared by mixing two type of materials, OPT veneer and EFB fiber mat impregnated with

Oil palm trunk laminated EFB-reinforced laminated

bio-composites bio-composites

Parallel veneer

Perpendicular veneer

Nonwoven EFB mat

Figure 1. Arrangement of OPT and EFB-reinforced laminated bio-composites.

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
222 H. P. S. ABDUL KHALIL ET AL.

PF resin. Composite was then cold pressed for 10 min and then it was placed in hot
pressing machine with processing temperature of 150 C for 25 min under pressure of
200 bars (3000 psi).

Mechanical Testing

Three types of mechanical testing were conducted: flexural, shear, and screw with-
drawal. A minimum of 10 samples were tested in each case.

FLEXURAL TEST
The flexural tests were performed according to BS EN 310 : 1993, using an Instron
Testing Machine Model 4204. Samples for flexural testing were cut into rectangular
strips with dimensions of approximately 240  50  12 mm3. The exact lengths, widths,
and thicknesses of the samples were measured and recorded. Samples were tested at a
crosshead speed of 10 mm/min over a span of 240 mm. All the specimens were conditioned
at ambient temperature (25  3 C) and at relative humidity of 30% ( 2%) before testing.

SCREW WITHDRAWAL TEST

The screw withdrawal tests were performed using an Instron Testing Machine Model
4204. The length, width, and thickness were measured and recorded. The tests were carried
out in accordance to BS EN 320 : 1993. The screw withdrawal tests were carried out on
samples with dimensions of 75  75  12 mm3. The test pieces were conditioned to constant
mass in an atmosphere with a mean relative humidity of 65  5% and a temperature of
20  2 C. For this test, a steel screw, nominal size 4.2  38 mm2 was used. The screw was
inserted into the hole to the full thickness of the board. The testing machine was set to a
crosshead speed of approximately (10  1) mm/min and until maximum load is achieved.

SHEAR TEST
Shear tests were performed according to BS EN 314-1 : 2004, using an Instron Testing
Machine Model 4204. The shear tests were performed on rectangular strips with dimen-
sions of approximately 135  25  12 mm3. The length, width, and thickness of each
sample was measured and recorded. Samples were tested at a crosshead speed of
1.5 mm/min. All of the specimens were conditioned at ambient temperature (25  3 C)
and a relative humidity of 30% (2%) before testing.
Prior to shear tests, phenol formaldehyde laminated bio-composites were subjected to a
water boil proof treatment (WBP). Samples were immersed for 4 h in boiling water, dried
in a ventilated drying oven for 16—20 h at 60  3 C, immersed for a second time in boiling
water for 4 h, and finally cooled in water at a temperature of 20  3 C for at least 1 h.
Before the water treatment, the length and width of the shear area were measured with
accuracy to within 0.1 mm. The shear tests were carried out on wet test pieces, allowing
for the use of a wiping based process. The shear test pieces were arranged in the center of
the clamping devices in such a way to allow the load to be transmitted from the testing
machine, through the ends of the test pieces and to the shear area without any transverse
loads. Slipping is only allowed in the initial stage of the loading. The clamp is positioned
on the sample faces. The load was applied at a constant moving rate, designed to induce
rupture within 30  10 s. Samples were tested at a crosshead speed of 1.5 mm/min.

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 223

Physical Testing

Four different physical tests were conducted in this study to test the following proper-
ties: density, water absorption, thickness swelling, and delamination.

DENSITY
The densities of the bio-composites were determined by measuring the mass and volume
of each sample. Each test sample was weighed with an accuracy of 0.01 g. The mass of each
sample was obtained by calculating the arithmetic mean of the mass of all of the test
samples taken from the same board. Accurate determination of test sample dimensions
was made using a sliding calliper, in accordance with BS EN 325 : 1993. The volumes of the
samples were obtained using the measured dimensions. The density, D was then calculated
using the formula in Equation (1):
m g 
D¼ , ð1Þ
v cm3
where m is the mass and v is the volume of the bio-composite sample.

WATER ABSORPTION AND THICKNESS SWELLING

To test water absorption and thickness swelling, samples were soaked in water for seven
days. The rate of water absorption initially increased with immersion time, until eventual
stabilization. The absorbed water in the samples (A) and the thickness swelling of the
samples (G) was calculated as a percentage according to the procedure given in BS EN
317 : 1993. The amount of absorbed water was calculated using Equation (2):
 
M1  M2
Að%Þ ¼  100, ð2Þ
M2
where M2 is the weight before the test and M1 is the measured weight (g).
The thickness swelling was calculated using Equation (3):
 
A1  A2
Gð%Þ ¼  100, ð3Þ
A2
where A2 is the thickness before the test and A1 is the thickness (mm) after the test.

DELAMINATION TEST
The delamination test was done following the standard BS EN 391 : 2002. It measured
the perimeter of failed glue line over the total perimeter of glue line available. The delam-
ination results are evaluated using Equation (4):
PglF
D¼  100, ð4Þ
Pgl  N
where D is delamination; PglF is the perimeter of failed glue line and Pgl the perimeter of
glue line, and N the number of gluelines.
Ten replications of bio-composite panels were constructed with OPT veneers and oil
palm EFB layers, using phenol formaldehyde resin. Samples were made in dimensions of
50  150 mm2 and were pre-treated. Test pieces were impregnated with water (vacuum at

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
224 H. P. S. ABDUL KHALIL ET AL.

70—85 kPa for 5 min, pressure at 500—600 kPa for 1 h, vacuum at 70—85 kPa for 5 min,
pressure at 500—600 kPa for 1 h), drying at 60—70 C for 21—22 h.

Thermogravimetric Analysis

Thermal stability of the bio-composites panels was investigated using thermogravimetric

analysis (TGA). Thermograms were obtained with a Perkin Elmer (TGA-6) instrument
with a heating rate of 20 C/min, over a temperature range of 25—900 C. All TGA runs
were performed under a nitrogen atmosphere.

Scanning Electron Microscopy

A scanning electron microscope (SEM; Leo Supra, 50 VP, Carl Ziess, SMT, Germany)
was used to analyze the morphology of the bio-composites materials. A thin section of the
sample was mounted on an aluminum stub using conductive silver paint and the sample
was sputter-coated with gold. The SEM micrographs were obtained under conventional
secondary electron imaging conditions using an acceleration voltage of 15 kV.

RESULTS AND DISCUSSION

Mechanical Properties

FLEXURAL PROPERTIES
Flexural test results were obtained for OPT laminated bio-composites and EFB-rein-
forced laminated bio-composites using phenol formaldehyde. Tests were performed to
investigate the effects of reinforcing oil palm trunk veneer with EFB on the mechanical
properties of the laminated bio-composites. Figure 2 shows the flexural strength and
flexural modulus of EFB-reinforced laminated bio-composites compared to OPT lami-
nated bio-composites.
Clearly, the flexural strength of the EFB-reinforced laminated bio-composite panels is
higher than that of OPT laminated bio-composites. This can be attributed to the higher
density of the EFB-reinforced laminated bio-composites, compared to OPT laminated bio-
composites (Table 1). Overall, the results showed that laminated bio-composites using
phenol formaldehyde exhibited high flexural strength. Interaction between cellulose fiber
with PF resin is excellent due to the hydrophilic nature of cellulosic fiber and PF resin.
Cellulosic hydroxyl groups (—OH) and lignin hydroxyl groups are the major component of
the fibers. These can easily form hydrogen bonds with the methylol and phenolic hydroxyl
groups of the resin and at 100 C these group can undergo condensation reaction leading to
three-dimensional network between fiber and matrix [13].
The flexural strengths of the laminated bio-composites and EFB-reinforced laminated
bio-composites that used a higher glue spread level (450 g/m2), were found to be higher
than the flexural strengths of the laminated bio-composites that used a lower adhesive
spread level (250 g/m2). The higher spread level allowed adhesive that was spread on the
surface of the OPT and EFB to enter the pores, where it solidified and anchored. This
implies that the lower glue spread amount of 250 g/m2 is inadequate to form full adhesion
between laminated bio-composite layers (both reinforced and not).

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 225

40 4

30 3

Flexural modulus (GPa)

Flexural strength (MPa)

20 2

10 1

0 0
OPT 250 OPT 450 OPT+EFB 250 OPT+EFB 450 OPT 250 OPT 250 OPT+EFB 250 OPT+EFB 450
g/m2 g/m2 g/m2 g/m2 g/m2 g/m2 g/m2 g/m2

Samples

Figure 2. Flexural strength and flexural modulus for OPT and EFB-reinforced laminated bio-composites with
different glue spread level using phenol formaldehyde (PF).

Table 1. Physical properties of OPT laminated bio-composites and EFB-reinforced

laminated bio-composites.

Adhesive Sample Physical properties

Water absorption Thickness swelling (%)

Density (g/cm3) (%) (After 7 days) (After 7 days)

PF OPT 250 0.6616 (0.05) 58.2614 (4.4) 12.8360 (1.2)

OPT 450 0.6410 (0.02) 56.6674 (3.9) 11.1814 (1.2)
OPT þ EFB 250 0.7261 (0.04) 50.4972 (3.2) 9.8509 (1.2)
OPT þ EFB 450 0.7414 (0.08) 43.6164 (4.2) 7.4136 (1.4)

As shown in Figure 2, EFB-reinforced laminated bio-composites using phenol formal-

dehyde possesses a higher flexural modulus than OPT laminated bio-composites. The
elastic properties were enhanced when the laminated bio-composites were reinforced
with EFBs, which increased the total fiber content and allowed the panels to withstand
a higher load. Among the different natural fibers, OPTs appear to be a promising material
because of their higher toughness [14,15].
High values of flexural modulus were obtained for panels made using phenol formal-
dehyde. When properly cured, phenol formaldehyde resin can be tougher than wood itself,
resulting in an impressively high flexural modulus [16]. The results showed that, as
expected, the flexural modulus was generally higher for the laminated bio-composites

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
226 H. P. S. ABDUL KHALIL ET AL.

that were made from a higher glue spread level, regardless of the adhesive used.
This is again attributed to the improved fiber-adhesive contact when a higher glue
spread level is used.

SCREW WITHDRAWAL PROPERTIES

Screw withdrawal strength varies with the type of tree from which the materials were
produced, the moisture content, the orientations of grains within a section, the duration of
extraction, the method of screwing, the panel dimensions, and the surface roughness [17].
The resistance of a screw shank against the direct withdrawal from a piece of wood depends
on the density of the laminated bio-composite material, the diameter of the screw, and the
depth of penetration. The surface condition of the screw at the time of driving and the glue
thickness also serve to influence the initial withdrawal resistance. The screw will fail in
tension when its strength is less than the withdrawal strength of the bio-composite.
Resistances of laminated bio-composite specimens to screw withdrawal were compared,
with constant screw diameters and screw types. Screw withdrawal strength properties are
showed in Figure 3. The results show that the screw withdrawal strength of EFB-rein-
forced laminated bio-composites is higher than OPT laminated bio-composites. From
Figure 4, we see a strong correlation between the screw withdrawal strength and the
specimen density. The limiting length for tension failure decreases as the density of the
laminated bio-composites increases, since the withdrawal strength of the laminated bio-
composites increases with density.
From the results, it can also be seen that laminated bio-composites with the higher
adhesive spread level (450 g/m2) show higher screw withdrawal values compared to lam-
inated bio-composites with lower adhesive spread level (250 g/m2). More glue will increase
the thickness of the layer, which influences the withdrawal strength of the nail and screw.

1000

800
Screw withdrawal (N)

600

400

200

0
OPT 250 g/m2 OPT 450 g/m2 OPT + EFB 250 g/m2 OPT + EFB 450 g/m2
Samples

Figure 3. Screw withdrawals of OPT and EFB-reinforced laminated bio-composites with different glue spread
level using phenol formaldehyde (PF).

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 227

SHEAR PROPERTIES
The shear properties of OPT laminated bio-composites and EFB-reinforced laminated
bio-composites were also studied. Figure 5 shows the shear properties for samples using
phenol formaldehyde, with different glue spread levels. From Figure 5, it can be clearly
seen that bond strength of laminated bio-composite panels was less for the samples using a
glue spread level of 250 g/m2.
Poor wettability is considered an indicator of poor bond durability. Wettability is rec-
ognized as an important criterion in evaluating the bonding ability of wood. The contact
angle that a drop of adhesive makes on a surface reflects the physical and chemical affinity
between the surface and the adhesive. In addition to chemical affinity, the rough surface of
the EFBs was a factor affecting adhesion because it was an obstruction to intimate contact
between veneer surfaces and adhesive molecules. Phenol formaldehyde adhesive showed
poor wettability and a hydrophobic surface; hence, the wettability and adhesion properties
of the surface were influenced negatively [18].
As expected, the shear strength was higher for the samples without pretreatment, com-
pared to samples that underwent pretreatment for WBP tests. Samples that underwent the
pretreatment experienced a drastic change in condition, which probably caused more
moisture to penetrate into the laminated bio-composites and those areas that were heavily
exposed to moisture, the strength weaken particularly during the WBP pretreatment,
because the bond type will affect the adhesive bonding and consequently reduce the
shear strength.
Figure 6 shows the shear strength for laminated bio-composites of WBP test, using
phenol formaldehyde as the adhesive resin. This test is designed to simulate exposure to
weather over sustained periods. From Figure 6, it can be seen that the shear strength
decreases after the WBP test. This may be due to swelling of the fibers during the treat-
ment, which will eventually lead to a reduction of the mechanical properties and shear
strength of the laminated bio-composites.

1000

800
Screw withdrawal (N)

600

400
PF

200

0
0.62 0.64 0.66 0.68 0.7 0.72 0.74 0.76
Density (g/cm3)

Figure 4. Relationship between screw withdrawal strength and density for phenol formaldehyde (PF)
laminated bio-composites.

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
228 H. P. S. ABDUL KHALIL ET AL.

2.0

1.5
Shear strength (MPa)

1.0

0.5

0.0
OPT 250 g/m2 OPT 450 g/m2 OPT + EFB 250 g/m2 OPT + EFB 450 g/m2
Samples

Figure 5. Shear strength of OPT and EFB-reinforced laminated bio-composites with different glue spread
level using phenol formaldehyde (PF).

2.0

DRY WBP

1.5
Shear strength (MPa)

1.0

0.5

0.0
OPT 250 g/m2 OPT 450 g/m2 OPT+EFB 250 g/m2 OPT+EFB 450 g/m2
Samples

Figure 6. Comparison of shear strength between dry and WBP treatment test of OPT and EFB-reinforced
laminated bio-composites with different glue spread level using phenol formaldehyde (PF).

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 229

Physical Properties

DENSITY
Table 1 shows the density of OPT laminated bio-composites and EFB-reinforced lam-
inated bio-composites with different glue spread levels of 250 and 450 g/m2 using phenol
formaldehyde. During the experiment, it was observed that the amount of glue resin and
the extent of compression of the veneer during hot pressing affect the density of the
laminated bio-composites, as seen in Table 1.
The characteristic property of laminated bio-composites strength is density. A higher
density corresponds to a higher laminated bio-composite strength, as seen in Table 1 and
Figures 2—6. Results showed that reinforcing laminated bio-composites of OPT with oil
palm EFBs using resin as an adhesive have higher densities than the laminated bio-com-
posites made from OPT using the same resin. This may be due to the difference in the
density of the raw materials that ultimately affects the laminated bio-composite density.
The density of OPT veneer is 0.15—0.4 g/cm3 and that of EFBs is 0.7—1.15 g/cm3. It is
obvious that the laminated bio-composite manufactured from layers of OPT will have a
lower density than the EFB-reinforced laminated bio-composites.
In addition to the raw materials density, the adhesive properties of the resin also con-
tribute to the density of the laminated bio-composites. The sample using phenol formal-
dehyde with a spread level of 450 g/m2 showed higher density compared to the samples
with different glue spread levels. This is due to the enhanced interfacial adhesion between
the phenol formaldehyde and the laminated bio-composites, attributed to the cross linking
reaction between the hydroxyl groups of the laminated bio-composites and the formalde-
hyde moiety of the resin [19].

WATER ABSORPTION
Table 1 shows the percentage of water absorption of OPT laminated bio-composites and
EFB-reinforced laminated bio-composites with different glue spread levels. Results indi-
cate that OPT laminated bio-composites have higher water absorption capacity compared
to the EFB-reinforced laminated bio-composites.
The higher uptake of water in OPT bio-composites may be due to the development of
both external and internal micro cracks in the material and/or the natural fiber swelling
due to moisture. This phenomenon maybe due to the theory that moisture absorption into
the composite materials is based on three major mechanisms, which are diffusion of water
molecules inside the microscopy between polymer chains; capillary transport of water
molecules into the gaps; and flaws at the interface between fibers and the polymer due
to the incomplete wettability; and also transport of water molecules by micro cracks in the
matrix formed during the compounding process. Fiber swelling will result in the fiber
debonding from the matrix due to the moist, high temperature environment [20].
Besides, this is also because OPT contains higher parenchyma which leads to the higher
water absorption. This can be explained by the greater affinity of the parenchyma to
absorb water as compared to the fiber bundles [21].
The percentage of moisture uptake decreased as reinforcement of OPT with EFBs. This
was expected due to the hydrophilic nature of the lignocellulosic fiber. The polar hydroxyl
groups in their molecular structures are able to form hydrogen bonds with water mole-
cules. The possibility of water being absorbed through the formation of hydrogen bonds
increases with fiber content. This phenomenon suggested that the OPT contains the max-
imum number of free hydroxyl group, OH while the minimum number of free OH group

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
230 H. P. S. ABDUL KHALIL ET AL.

are present in EFBs. This is due to the presence of OH group that enhances the water
absorption by forming the hydrogen bonding with water molecules [22].
The panels using a higher adhesive spread level (450 g/m2) have lower water absorption
compared to panels using a lower adhesive spread level (250 g/m2). This may be due to the
higher compatibility between the hydrophilic fiber and adhesive in the panels that use
higher adhesive spread level. The weak compatibility between the fiber surface and adhe-
sive could lead to the formation of void structures within the composites, which facilitates
water absorption [23].

THICKNESS SWELLING
Many physical properties of laminated bio-composites are affected by the amount of
moisture present in the laminated bio-composite. Laminated bio-composites exhibit
greater dimensional stability compared to most other wood-based building products.
Thickness swelling is independent of panel size and veneer thickness [24].
Table 1 shows that the OPT laminated bio-composites made with phenol formaldehyde
adhesives exhibited a higher degree of thickness swelling than EFB-reinforced laminated
bio-composites. This may be due to the structure of oil palm EFB mats, which have higher
densities, leading to a decrease in thickness swelling.
This test also showed that the thickness swelling of the composites increases with an
increase in the period of water exposure. The increase in water exposure time allows a
significant amount of water to be absorbed, resulting in fiber swelling. The EFB-reinforced
laminated bio-composites using phenol formaldehyde, a resin with an aromatic backbone,
showed a decrease in thickness swelling. The hydrophilic nature of the fibers that arises
from an abundance of hydroxyl groups makes them incompatible with the hydrophobic
matrices of phenol formaldehyde, resulting in lesser water absorption [19].

DELAMINATION TEST
The performance of laminated bio-composite panels depends a great deal on the bond-
ing strength between the resin and the substrate. Any failure in the glue bond weakens the
mechanical strength. Furthermore, good durability is associated with the absence of
delamination of laminated bio-composites samples [25]. Typically, in such an outdoor
out of ground application, plywood is not continuously wet but can be subjected to fre-
quent wetting and drying subsequently. It is generally known that moisture has a signif-
icant influence on the mechanical and physical properties of wood, plywood, and other
wood-based materials. As wood-based panels are hygroscopic and since their surface to
volume ratio is very high, physical deformations and cracks are possible. In the case of
plywood the strength properties of the glue lines are affected by changing moisture, result-
ing in a risk of delamination and panel failure [4].
Delamination assessment on 10 specimens from each OPT laminated bio-composites
and EFB-reinforced laminated bio-composites with different glue spread level revealed
that all of the laminated bio-composite panels presented almost no delamination.
It was observed that the laminated bio-composite specimens delaminated at the glue line
and cracks occurred on the edge of the sample. One in 10 samples of OPT laminated bio-
composites with glue spread level 250 g/m2 presented 0.6% delamination; and three in 10
samples of EFB-reinforced laminated bio-composites with glue spread 250 g/m2 presented
1.9% delamination as shown in Table 2. The samples of EFB-reinforced laminated bio-
composites with glue spread 250 g/m2 presented the highest delamination. No delamina-
tion was observed in the OPT laminated bio-composites with glue spread level 450 g/m2

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 231

and EFB-reinforced laminated bio-composites with glue spread 450 g/m2. The proportion
of samples (each combination was done with 10 replications) affected by the delamination
also is presented in Table 2. This result indicated that the laminated bio-composites with
higher glue spread (450 g/m2) exhibited better bonding strength between resin and the
substrate with no delamination compared to laminated bio-composites with lower glue
spread (250 g/m2).

Thermogravimetric Analysis

Thermogravimetric is a method to investigate the thermal stability of materials used for

various applications. In this work, TGA was used to investigate the thermal degradation
properties of laminated bio-composite panels.
From Figure 7, it is clear that all of the samples, regardless of the panel type, initially
undergo a loss of moisture at a temperature near 100 C. For the EFB-reinforced laminated

Table 2. Delamination and proportion of samples affected by

delamination test for OPT laminated bio-composites and EFB-reinforced
laminated bio-composites.

Proportion of samples affected by

Sample delamination test Delamination (%)

OPT 450 0/10 0

OPT 250 1/10 0.6
OPT þ EFB 450 0/10 0
OPT þ EFB 250 3/10 1.9

110
OPT+EFB 450
100
OPT+EFB 250
90

80
Intensity (a.u)

70

60

50

40

30
OPT 250
OPT 450
20

0 200 400 600 800 1000

Temperature (°C)

Figure 7. Thermograms of laminated bio-composites panels glued with phenol formaldehyde (PF).

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
232 H. P. S. ABDUL KHALIL ET AL.

Table 3. The degradation temperature and ash content from

thermograms of laminated bio-composite panels glued with
phenol formaldehyde.

Sample Ti ( C) Tf ( C) Ash (%)

OPT 450 220 340 23

OPT 250 213 335 22
OPT þ EFB 450 245 350 32
OPT þ EFB 250 225 343 30

bio-composites, the initial degradation temperature occurs at a higher temperature com-

pared to the OPT laminated bio-composite materials. The EFB-reinforced laminated panel
with a phenol formaldehyde glue spread of 450 g/m2 did not show signs of initial degra-
dation until approximately 245 C, indicating good thermal stability. The EFB-reinforced
laminated bio-composites with 450 g/m2 of phenol formaldehyde had a final degradation
temperature of 350  C and an ash content of 32%. Both the degradation temperature and
the ash content were higher for the EFB-reinforced laminated sample, compared to the
OPT panels (Table 3). For the EFB-reinforced laminated samples, the thermograms show
degradation upto a temperature of around 370 C, after which the thermogram plateaus, as
only ash is remaining.
Overall, panels glued with phenol formaldehyde with a spread level of 450 g/m2 had the
best thermal stability.

Scanning Electron Microscopy

SEM was used to conduct morphological analysis of the bio- composite panels. The
interaction of the adhesive in OPT laminated bio-composites and EFB-reinforced lami-
nated bio-composites, as observed from the FESEM, are shown in Figures 8(a) and (b)
and 9(a) and (b).
Views of EFB-reinforced laminated bio-composites using adhesive spread level of
250 g/m2 is shown in Figure 8(a). The adhesive can be seen filling up the available space
in the glue line, with some glue penetrating through the vessel lumen as mentioned by
Sulaiman et al. For the samples with the lower glue spread level, there are some spaces that
are not filled with adhesive and the presence of these voids can lead to poor adhesion. The
EFB-reinforced laminated bio-composite panels using phenol formaldehyde with a spread
level of 450 g/m2 showed a well-dispersed glue line (Figure 8(b)). The adhesive can be seen
filling up the available space in the glue line, with some glue able to penetrate through the
vessel lumen adjacent to the glue line. This spreading probably occurred during the glue
application. For samples with the higher glue spread level, there was enough adhesive to
fill up the lumen void, which probably improves the adhesion. The adhesive also pene-
trates between the OPT and the oil palm EFB fibers.
Figure 9(a) shows that less adhesive fills the spaces and parenchyma cells in the porous
surface of the OPT veneer. The SEM image revealed voids between OPT veneer and EFB
mat layers (Figure 9(a)). These voids may arise due to the inadequate amount of adhesive
in the 250 g/m2 glue spread level. For the samples with a glue spread level of 450 g/m2, it
was observed that the adhesive filled the lumen in the OPT laminated bio-composite panels

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 233

(a)

Spaces between
OPT veneer and
EFB mat layers

(b)

No spaces between
OPT veneer and EFB
mat layers

Figure 8. Scanning electron micrograph of EFB-reinforced laminated bio-composites with (a) 250 g/m2 and
(b) 450 g/m2 spread level (50  magnifications).

and filled the parenchyma of the OPT veneer (Figure 9(b)). The fact that the adhesive
fills the small cavities probably serves to improve the adhesion between the surfaces
of the OPT.

CONCLUSIONS

In this article, we report on the use of EFBs as a reinforcement in OPT bio-composites

and the potential of EFBs to be high performing raw materials for bio-composites using
phenol formaldehyde resin. The aim of this study was to characterize the mechanical,
thermal, and physical properties of EFB-reinforced laminated bio-composites. From
our results, we conclude that laminating EFB with OPT improves some properties of

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
234 H. P. S. ABDUL KHALIL ET AL.

(a)

Spaces which did not filled

up with the adhesives

(b)

Resin filled up the available

spaces of the surface

Figure 9. Scanning electron micrograph of OPT laminated bio-composites with (a) 250 g/m2 and
(b) 450 g/m2 spread level (50  magnifications).

bio-composites, such as bending strength and modulus, screw withdrawal. EFB-reinforced

laminated bio-composites also showed better physical properties than OPT laminated bio-
composites. It is obvious that the laminated bio-composite manufactured from layers of
OPT have a lower density than the EFB-reinforced laminated bio-composites. The thick-
ness swelling and water absorption of OPT laminated bio-composites was higher than the
thickness swelling determined in EFB-reinforced laminated bio-composites. The bio-com-
posites constructed with OPT and laminating EFB with OPT presented almost no delam-
ination. After the testing according to BS EN 391, the laminating EFB with OPT seemed
to have no negative effect on the quality of the glue line. In addition, laminated bio-
composites made using a glue spread level of 450 g/m2 have better mechanical and physical
properties than laminated bio-composites using a glue spread level of 250 g/m2. Besides,
the higher adhesives spread level (450 g/m2) samples showed lower water absorption and

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
Laminated Bio-composites Reinforced with Empty Fruit Bunches 235

thickness swelling from the samples with lower glue spread level (250 g/m2). The thermal
and morphological analysis of the EFB-reinforced laminated bio-composites glued with
phenol formaldehyde confirmed that the panels have good thermal resistance and good
adhesion, with a well-dispersed glue line. In conclusion, EFBs can be used to substitute
raw materials to produce laminated bio-composites.

ACKNOWLEDGMENTS

The researchers would like to thank the Ministry of Science, Technology and
Innovation (MOSTI) and the Universiti Sains Malaysia, Penang for providing the research
grant EScience Fund (RM-9) 03-01-05-SF0334 and 305/PTEKIND/613323 that made this
work possible.

REFERENCES

1. Sumathi, S., Chai, S.P. and Mohamed, A.R. (2008). Utilization of Oil Palm as a Source of
Renewable Energy in Malaysia, Renewable and Sustainable Energy Reviews, 12(9): 2404—2421.
2. Alam, M.Z., Mamun, A.A., Qudsieh, I.Y., Muyibi, S.A., Salleh, H.M. and Omar, N.M. (2009).
Solid State Bioconversion of Oil Palm Empty Fruit Bunches for Cellulase Enzyme Production
Using a Rotary Drum Bioreactor, Biochemical Engineering Journal, 46: 61—64.
3. Yusof, B. (2007). The Oil Palm Production Through Sustainable Plantations, European Journal
of Lipid Science and Technology, 109: 289—295.
4. Van den Bulcke, J., Van Acker, J. and De Smet, J. (2009). An Experimental Set-up for Real-time
Continuous Moisture Measurements of Plywood Exposed to Outdoor Climate, Building and
Environment, 44: 2368—2377.
5. Ronald, H.B. (1996). Construction and Industrial Plywood, National Institute of Standards and
Technology, Tacoma, Washington.
6. Jerrold, E.W. (2006). Advanced Wood- and Bio-composites: Enhanced Performance and
Sustainability, In: The 4th International Conference on Advanced Materials and Processes,
p. 27, University of Waikato, Hamilton, New Zealand, 10—13 December.
7. Kelvin, M.C. (2006). Wood-based Panels: Particleboard, Fibreboards and Oriented Strand
Board, In: Walker, J.C.F. (ed.), Primary Wood Processing Principles and Practice, 2nd edn,
p. 427, Springer, England.
8. Raquez, J.-M., Deléglise, M., Lacrampe, M.-F. and Krawczak, P. (2010). Thermosetting
(Bio)Materials Derived from Renewable Resources: A Critical Review, Progress in Polymer
Science, 35: 487—509.
9. Tonge, L.Y., Hodgkin, J., Blicblau, A.S. and Collins, P.J. (2001). Effects of Initial Phenol-
Formaldehyde (PF) Reaction Products on the Curing Properties of PF Resin, Journal of
Thermal Analysis and Calorimetr, 64: 721—730.
10. Moubarik, A., Pizzi, A., Allal, A., Charrier, F. and Charrier, B. (2009). Cornstarch and Tannin
in Phenol—Formaldehyde Resins for Plywood Production, Industrial Crops and Products, 30:
188—193.
11. Sreekala, M.S., Jayamol, G. and Sabu, T. (2001). Water-sorption Kinetics in Oil Palm Fibers,
Journal of Polymer Science. Part B. Polymer physics, 39: 1215—1223.
12. Myrtha, K., Holia, O., Dawam, Abdullah, A.H. and Anung, S. (2008). Effect of Oil Palm Empty
Fruit Bunch Fiber on the Physical and Mechanical Properties of Fiber Glass Reinforced
Polyester Resin, Journal of Biological Sciences, 8(1): 101—106.
13. Sreekala, M.S., Kumaran, M.G., Joseph, S., Jacob, M. and Thomas, S. (2000). Oil Palm Fibre
Reinforced Phenol Formaldehyde Composites: Influence of Fibre Surface Modifications on the
Mechanical Performance, Applied Composite Materials, 7: 295—329.

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015
236 H. P. S. ABDUL KHALIL ET AL.

14. Abdul Khalil, H.P.S., Hanida, S., Kang, C.W. and Nik Fuaad, N.A. (2007). Agro-Hybrid
Composite: The Effects on Mechanical and Physical Properties of Oil Palm Fiber (EFB)/
Glass Hybrid Reinforced Polyester Composites, Journal of Reinforced Plastics and
Composites, 26: 203—218.
15. Jacob, M., Thomas, S. and Varughese, K.T. (2004). Mechanical Properties of Sisal/Oil Palm
Hybrid Fiber Reinforced Natural Rubber Composites, Composites Science and Technology, 64:
955—965.
16. Richard, F.B. (1995). Adhesives and Bonding Techniques, In: Plywood and Veneer-Based
Products Manufacturing Practices, p. 256, Miller Freeman Inc, California, USA.
17. Celebi, G. and Kilic, M. (2007). Nail and Screw Withdrawal Strength of Laminated Veneer
Lumber Made Up Hardwood and Softwood Layers, Construction and Building Materials, 21:
894—900.
18. Ismail, A. and Gursel, C. (2007). Variation in Surface Roughness, Wettability and Some
Plywood Properties After Preservative Treatment with Boron Compounds, Building and
Environment, 42: 3837—3840.
19. Abdul, Khalil, H.P.S., Issam, A.M., Ahmad, Shakri, M., Suriani, R. and Awang, A.Y. (2007).
Conventional Agro-composites from Chemically Modified Fibres, Industrial Crops and
Products, 26: 315—323.
20. Suhara, P. and Mohini, S. (2007). Studies on the Water Absorption Properties of Short
Hemp—Glass Fiber Hybrid Polypropylene Composites, Journal of Composite Materials, 41:
1871—1883.
21. Siti Norralakmam, Y. (2007). Particleboards, In: Turning Oil Palm Residues into Products,
Research Pamphlets No.127, p. 27, Forest Research Institute Malaysia (FRIM) Kepong,
Malaysia.
22. Lai, J.C. (2007). Mechanical and Water Absorption Properties of Lignocellulosic Phenolic
Composites, MSc Thesis, UTM, Skudai, Johor, Malaysia.
23. Sreekala, M.S., Kumaran, M.G. and Thomas, S. (2002). Water Sorption in Oil Palm Fiber
Reinforced Phenol Formaldehyde Composite, Composites Part A: Applied science and
manufacturing, 33: 763—777.
24. Kelly, A. (1994). Plywood, In: Concise Encyclopedia of Composite Materials, revised edn, p. 240,
Pergamon, England.
25. Sellers, T. (1985). Plywood and Adhesives Technology, p. 535, Marcel Dekker, New York.

Downloaded from jcm.sagepub.com at East Tennessee State University on June 19, 2015