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Abstract
In this research, a complete systematic technique for fabricating and characterising the various properties of
Cochlospermum Gossypium (CG) and oil palm mesocarp fibre (OPMF) reinforced composites are reported.
Following the hand lay-up method for manufacturing composites with varying OPMF weight percentages (5, 10, and
15), the composites were subjected to a variety of characterisation tests. To improve the interfacial bonding, capabilities
of OPM fibre surfaces were treated with sodium hydroxide (NaOH). Microstructural studies, such as scanning electron
microscopy, were performed on the produced samples, followed by mechanical characteristics like tensile, flexural, and
impact tests. Furthermore, the TGA (thermogravimetric analysis) test was performed as part of the thermal tests. The
treated composites were found to be increased by 69.64% in tensile strength and 38.37% in flexural strength when com-
pared with untreated composites and neat matrix in the tensile test. Thermal study revealed that 15% of fibre content
outperforms the other weight fractions of the composites under investigation, as evidenced by TGA, microstructural, and
mechanical testing.
Keywords
Oil palm mesocarp fibre, Cochlospermum Gossypium, mechanical and thermal behaviour, composites, and natural resin
as their volume content, are directly related to the strength glycerol and 20% glutaraldehyde shows better mechanical
and stiffness of composites. The resin helps to keep the and thermal characteristics of the composites. Jagadeesh
fibres in a relative position within the composite and, et al.38 propylene glycol plasticised wheat protein isolate
more significantly, distributes the load between broken new green films: production and attributes. The results dem-
and unbroken fibres. As a result, the resin/fibre interaction onstrate that when plasticiser content increases, tensile
process is most crucial in composite preparation otherwise strength increases, young’s modulus decreases, and the
they can cause a big impact on composite parameters like percent of elongation increases. In FTIR amide groups
toughness and transverse fracture stress. To summarise, in were increased and thermal stability also improved.
order to fabricate high-strength composites, it is essential Vinayagamoorthy and Venkatakoteswararao22 development
to consider all three composite elements, namely fibre and characterization of bio-composites using senegalia
characteristics, resin characteristics, and fibre/resin inter- catechu resin. They reported a positive sign in bio resin-based
face characteristics. composites to have superior mechanical and thermal charac-
The mechanical characteristics of the composites were teristics as compared to synthetic composites. Coppen39
studied by using natural plant resins or biodegradable studied gums, resins, and latexes of plant origin. In this
resins. Park et al.,30 studied the tensile characteristics and paper, a variety of gums’ uses are detailed in the relevant
solubility parameters of biopolymers made from soy areas. These applications include those in food, medicine,
protein isolate (SPI) after they were crosslinked with glutaral- and other technological fields. Janaki and Sashidhar40 iden-
dehyde (GA). They reported that the tensile properties of tify the kondagogu gum physicochemical properties and
crosslinked SPI were higher than unmodified SPI. Joel compared them to other established tree gums such as gum
Grevellec et al.,31 created biodegradable products out of cot- Arabic, gum tragacanth, and gum karaya. Later, Vinod
tonseed protein that has been plasticised with glycerol and et al.,25 discussed on morphological, physicochemical, and
investigated the effect of glycerol content on characteristics. structural properties of this novelty gum. The literature men-
They concluded that cotton seed proteins were acted like tioned above looked into the usage of various natural resins
thermoplastic macromolecules and hence susceptible to low- and fibres in reinforced composites. Over the past few
moisture processing. Jean-Luc Audic et al.,32 with the devel- years, natural plant resins are gained more attraction, and
opment of eco-friendly materials for use in packaging appli- there placed synthetic resins for fabricating biocomposite
cations, by using the casting procedure, a water solution of materials.41 This paper discusses the new gum, Kondagogu
sodium caseinate and plasticisers was used to generate plasti- gum which is obtained from the Kondagogu tree.
cised protein films. They reported improved tensile character- The world’s forests are a key source of a variety of forest
istics by using a suitable plasticiser such as triethanolamine products other than timber. In such a way that this substance
(TEA) or glycerol. It was proven in detail how sensitive the is a member of the bixaceae family and is known locally as
film is to changes in relative humidity as well as how plasti- Kondagogu gum (Cochlospermum Gossypium).42 Almost
ciser and relative humidity interact to affect the mechanical the gums are natural exudates process and it is extracted
properties of the film. Jayasekara et al.33 prepared several from stripping the bark of a tree. In first 24 h of blazing,
starch/PVA/glycerol polymer blends that were solution cast the maximum amount of gum is produced and solidified in
and composted for 45 days to test for biodegradation. The form of tears. It continued for several days. Before the
starch and glycerol components were destroyed during this rainy season, the top quality gum is collected in the month
timeframe, leaving the PVA component virtually intact, of April to June, then the gum collection process is continued
they reported. Lodha et al.34 produced environmentally up to a month of September, in this period gum is produced
friendly fibre reinforced composites with soy protein isolate dark and less viscous. After collection of this entire gum is
(SPI) and evaluated the mechanical and interfacial character- cleaned and sorted manually or mechanically. The commer-
istics of these materials. They reported that they were able to cial kondagogu gum in india is available in three different
significantly increase the tensile capabilities of both the grades: Grade-I, Grade-II, and Grade-III. Grade-1 represents
SPI-polymer and composites using natural fibres. Lodha light yellowish colour, grade−2 is orange and grade−3 is a
et al.,35 Using ramie fibre and soy protein isolate (SPI) reddish colour. Generally, gums are hydrophilic in nature;
resin, entirely biodegradable and environmentally friendly it is composed of glycerol and glutaraldehyde and was
composites were made and their mechanical properties used as reactive sites to prepare a new composite matrix.
were investigated. They stated that their ramie/modified SPI Natural fibres have various benefits over synthetic fibres
composites outperformed ramie/SPI composites in terms of in the preparation of composites, including renewability,
mechanical properties and that this composite could be reasonable cost, low density, and biodegradability.43,44
used as a green composite in certain applications. Chabba Plant fibres such as kenaf,5 jute,7 coir,11 cotton,9 bamboo,10
et al.36 developed green composites made of plant fibres and oil palm mesocarp fibre45 have all been thoroughly
and resins that are environmentally benign and entirely bio- researched for polymer/fibre composite construction. With
degradable and examined their qualities. These qualities increasing fibre content, Rozman et al.,11 OPEFBF was
appear to be sufficient for evaluating these green composites found to improve tensile modulus but reduce tensile strength,
for interior structural applications, according to them. percentage of elongation at break, and impact strength when
Jagadeesh et al.,37 biodegradable films made from wheat incorporated into the polypropylene matrix.
protein isolate synthesis and characteristics. They discussed The lignocellulosic material created in the oil palm plan-
on optimum condition of wheat protein isolate with 10% of tation during the extraction of oil process is known as the
Srikanth and Reddy 3
biomass of oil palm mesocarp fibre (OPM fibre). OPM fibre and Kondagogu gum matrix material are presented in Table 1.
is a by-product obtained during oil extraction from oil palm The fibre was further chemically treated with NaOH solution
fruits.46 The oil palm plantation either discards them or to remove the non-cellulose material from the fibre surface
uses them as fuel for boilers to produce steam and and improve the surface roughness.53 Glutaraldehyde and
power.47,48 However, the present use of such fibres has ser- Glycerol, two additional basic compounds, were employed to
iously harmed the ecosystem. As a result, this study was con- increase the cross-linking and flexibility of the composite mater-
ducted in order to better utilise them as fillers in the creation of ial.37 To neutralize the composite mixture HCl was added.27
biocomposites. Future oil palm biomass will benefit from the Ammonia solution was utilized to boost the adhesion properties
usage of these fibres in the production of biocomposites. of resin material by raising the pH.25 Distilled water was pur-
Other scientists have described combining OPM fibre chased from Narmada (India) and employed for the preparation
with high-density polyethylene,49 and polypropylene50 to of resin and composite material.
produce polymer/fibre composites in the past,51,52 but there
is no literature on reinforcing natural gums to date.
The researcher was created untreated and surface- Alkali treatment
treated OPM fibre composites with varied weight ratios,
OPM fibres were dried under sunlight for a week and
such as 100:0, 95:05, 90:10, and 85:15, in this research.
washed with water to remove pulp, dirt, and mud. To
The physical and mechanical characteristics of composites
remove hemicelluloses, lignin, and wax of non-cellulose
are heavily influenced by the interface. Fibre-surface treat-
material from the fibre surface, alkali treatment adopted
ment is required to get a better interface between hydro-
with NaOH solution. Such chemical treatment on natural
philic OPM fibre and the hydrophobic matrix when using
fibre helps to improve the surface roughness of the fibre
OPM fibre reinforcement in composites. Natural and artifi-
and contributes to enhancing the interfacial bond between
cial impurities can be removed by alkali treatment, which
the OPM fibre and CG matrix through mechanical inter-
results in uneven topography on the surface. Chemical
locking.45,53,54 For alkaline treatment, oil palm mesocarp
treatment also results in fibre/fibre disintegration, which
fibres were soaked in the 2 wt.% NaOH solution for
is the fragmentation of the fibre bundle into thinner
almost 24 hrs to eliminate the hemicellulose and other
fibres. It increases the actual surface area that the matrix
greasy materials. The removal of these materials is consid-
resin can wet. Therefore, increasing the fibre aspect ratio
ered necessary to increase the hydrophobicity of natural
via reducing the fibre size and generating a rough surface
fibres. The hydrophobic nature was generated by replacing
topography enhances the mechanical and adhesive capabil-
the fibre surface water-sensitive OH groups with fibre
ities of the fibre/matrix interface. The composites were
surface cell-O-Na groups.54 Such treated fibre surface
made using Kondagogu gum resin as a matrix. Tensile,
reduces the swelling of fibre as well as the void formation
flexural, impact, thermal gravimetric analysis, and SEM
and debonding in CG composites. The fibres were then con-
tests were used to characterise the final products.
tinuously rinsed with water to neutralise any NaOH present
in the fibre. Finally, the treated fibres were allowed to dry in
the oven for 24 h at 70°C, then placed into zip covers & kept
Materials and methods in a desiccator until they were needed.
Materials
In this investigation, Cochlospermum Gossypium (CG) in the Composites fabrication
native language (Telugu) called Kondagogu gum (KGG) was
procured from Nutriroma Pvt. Ltd, India, which is a light To meet the objective of this research work, OPM fibre/
yellowish colour and available in the open market. Similarly, CG composite material was prepared by hand layup tech-
the Oil palm mesocarp fibres were collected from 3F Oil nique as shown in Figure 1. Cochlospermum Gossypium
Palm Pvt. Ltd and used as a reinforcing phase in natural compos- (CG) resin was prepared by weighing the required amount
ite material. The physical and chemical properties of OPM fibre of Cochlospermum Gossypium (CG) powder separately
and mixing 20 times (by wt. CG powder) of glycerol
with distilled water in a glass beaker for 20 to 30 min to
Table 1. OPM fiber and Kondagogu gum properties. get the desired solution. After stirring, a solution was
added to NaOH and HCl to neutralise the homogenous
Parameters OPM Fibre45 Kondagogu Gum42
suspension. After 20 min of continuous incubation, glu-
Density (g/cc) 0.246 1.28 taraldehyde and ammonia solutions 25–30 times (by
Moisture (g %) 8.6 15.2 + 1.18 weight of CG powder) are weighed separately and com-
Ash (g %) 5.8 7.3 + 0.3 bined with the initial gum. This solution was added to
pH — 4.9–5.0 the pure Cochlospermum Gossypium suspension to
Intrinsic viscosity, dL/g — 32.68 ± 0.22 achieve a pH of 7–8. As a cross-linking agent to increase
Nature of Structure Amorphous Amorphous the tensile properties and thermal stability of the resin, dif-
Cellulose (%) 23.7 — ferent quantities of glutaraldehyde were applied. To min-
Hemicellulose (%) 30.5 —
imise the brittleness of the resin, varying amounts of
Lignin (%) 27.3 —
glycerol were added.
4 Proc IMechE Part E: J Process Mechanical Engineering 0(0)
Figure 1. A schematic presentation of OPM fiber/CG composite material preparation by hand layup technique and as prepared
composite laminates.
Figure 2. (a) Tensile testing samples according to ASTM D 638, (b) three-point bending test/flexural strength testing samples as per
the ASTM D 790, and (c) Izod impact testing samples following ASTM D 256.
machine (UTM Zwick/Roell Z010) with a capacity of 10 kN holes on the fibre’s surface.53 The cross-section of the fibre
and cross-head speed of 5 mm/min, measure 165 × 19 × exposes a lacuna-like region in the centre. This type of
3 mm, as illustrated in Figure 2(a). Figure 2(b) depicts three- porous fibres for composite manufacturing does not
point flexural strength testing samples that were prepared in exhibit superior mechanical characteristics than the
accordance with ASTM D 790 standards and measured 127 matrix.55 Figure 4(b) presents the treated fibre surface.
× 12.70 × 3 mm. The specimens were tested in tensile and The pores grew more apparent after being treated with
three-point bending using a universal testing machine alkali. Figure 4(a) and (b) depict the oil palm mesocarp
(UTM Zwick/Roell Z010) with a capacity of 10 kN and fibre prior to and after alkali treatment, respectively.
cross-head speeds of 1 and 2 mm/min, respectively. The Figure 4(b) shows micrographs of the treated fibre surface
mechanical responses of the samples were recorded during procedure that will remove the waxy cuticle layer from the
the testing. The load on the specimen was applied until it surface. This may be seen in the micrographs. Figure 4(b)
was fractured, and the breaking load was computed. illustrates the surface properties of untreated oil palm meso-
Moreover, to evaluate the impact strength, 64 × 12.7 × carp fibre. The surface of the fibre is rough, with projecting
3 mm specimens were made according to ASTM D 256, parts and groove-like patterns. The morphological altera-
and the supplier is Deepak Poly Plastic Pvt. Ltd, Gujarat. tions of fibre induced by alkali treatment are obvious in
An impact tester (IZOD/Charpy Impact Tester) was used the corresponding SEM images presented in Figure 4(b).
for impact testing samples, as shown in Figure 2(c). Figure 4(c) and (d) depict untreated fibre composites with
resin cracked surface of CG resin at 5% OPM fibre. In both
Figures, there are numerous cavities, gaps, and fibre breaks
Scanning electron microscopy (SEM) due to improper bonding. In this composite, the load was
Using a TESCAN VEGA 3 LMU scanning electron micro- not successfully transmitted from the resin to the fibre.
scope with a 20 kV accelerating voltage, the morphology Figure 4(c) depicts the fractured surface of untreated compo-
of the fractured samples was examined. Prior to capturing sites containing 5% OPM fibre, revealing that the failure was
the micrographs, the fractured surfaces were electrodepos- caused by resin cracking, followed by crack propagation by
ited with gold to increase electrical conductivity. fibre. When the fibre weight percentage in the resin is low, the
resin bears the largest load rather than the fibre, which is sup-
posed to carry the bulk of the stress; hence, the matrix frac-
Thermal analysis tures rapidly. Due to the relatively high fibre wt.%, the
interface between matrix and fibre was ineffective; thus,
Thermogravimetric analyses (TGA) were performed as
none of the fibres were able to bond with the matrix;
per ASTM E1131--20 mg samples utilising NETZSCH,
instead, they formed clusters, lowering their strength.
STA 2500 Regulus (Figure 3) by heating from 25°C to
Figure 4(f) is an illustration of interfacial bonding between
600°C at a heating rate of 10°C/min at a continuous
the CG matrix and 10% OPM fibre. The presence of matrix
flow rate of 20 mL/min of nitrogen to produce an inert
on fibre surfaces shows that these two components are in
environment to inhibit oxidation. The TGA control and
close touch at their interfaces. As a result of the SEM find-
biocomposite were investigated.
ings, composites containing 10 wt.% OPM fibres exhibited
maximal tensile strength and a strong connection between
Results and discussion the CG matrix and OPM fibres.
Figure 3. (a) TGA sample and (b) thermogravimetric analyses testing machine.
6 Proc IMechE Part E: J Process Mechanical Engineering 0(0)
Figure 4. (a) SEM showing before alkali treatment of the fiber; (b) SEM for showing after alkali treatment of the fiber; (c) and (d) SEM
for untreated OPMF/CG composites (5 wt.% of OPM fiber); (e) SEM for OPMF/CG composites (15 wt.% of OPM fiber); (f) SEM for
treated OPMF/CG composites (10 wt.% OPM fiber).
displayed in Figure 5. Furthermore, tensile properties were cellulosic chemically untreated OPM fibres produced coarse,
evaluated from the noted readings. Figure 6 illustrates the low-quality fibres. The elevated concentrations of OH and C
influence of treatment development and fibre weight circum- = O suggest the existence of non-cellulosic compounds.45 As
stances on the TS (Tensile Strength) of OPM fibre-reinforced a result, the interfacial adhesion with the matrix was weak,
CG composites. In all loading circumstances, it was shown which led to a poor load distribution between the fibres and
that treated fibre-reinforced composites consistently had a the matrix, resulting in the failure of the composites.54
higher value than the neat matrix and untreated OPM fibre Figure 6 further demonstrates that the TS of both
composites. It is obvious from the data that treated fibres treated and untreated CG composites increases with
interacted more effectively with the CG matrix than untreated increasing fibre wt.%. This result was consistent with
fibre composites. Strong interaction between the fibre and the the common observation that the strength of mechanical
matrix would increase the transfer of load between constitu- composites increased up to a particular loading level
ents, resulting in a better outcome for the treated fibre.54 This before diminishing. The tensile strength of the composite
is due to the removal of unwanted substances such as wax and material increases dramatically when 10 wt.% of OPM
pectin from the surface of the natural fibre, which leads to fibres were introduced to composites. From the perspec-
improved surface roughness and creates more adherents tive of composite morphology, there appears to be good
and a strong bond with the matrix.53 On the other hand, non- mechanical interlocking between the fibre and matrix
Srikanth and Reddy 7
Figure 5. (a) A universal testing machine with a capacity of 10 kN (UTM Zwick/Roell Z010) and (b) optical images of fracture tensile
samples under tensile strain. All tensile samples ruptured within the gauge length and the crack propagated normally to the tensile load
axis.
Figure 8. (a) A three-point bending test set up on a universal testing machine with a capacity of 10 kN (UTM Zwick/Roell Z010) and
(b) optical images of 3P bending tested samples. It seems the tested samples subjected to bending force and plastic deformation were
exhibited but physical fracture has not occurred during the test The OPM fiber/CG composite samples shown high ductile nature.
Figure 10. (a) Izod testing machine with sample loading and pendulum arrangements and (b) optical images of fractured impact
samples.
Thermogravimetric analysis
The thermal behaviour of the composites was charac-
terised by thermogravimetric analysis (TGA). Mass deg-
radation temperature is an important parameter that
decides the performance of the composites in high-
temperature applications. Figure 12 depicts the TGA
curve at a heating rate of 10°C/min. Treated oil palm
mesocarp reinforced composites exhibit better thermal
conductivity than neat CG and raw composites based on
the TGA plot. From Figure 12(a), for the thermograms
of the Neat CG resin and varying fibre percentages of com-
posites, it can be seen that the composites are degraded in
Figure 11. Impact strength of randomly oriented oil palm multiple steps. In the initial stage, the neat CG matrix
mesocarp/CG composites.
moisture content is evaporated at 100°C by losing 10%
of its original mass. In the second stage, hemicellulose
that the fibres can function as a stress transfer agent for the and lignin heat degradation is indicated, which occurs in
CG matrix, particularly at 5 wt.% and below. the ranges (200°C–600°C), the wt. loss was found at
Figure 11 compares the impact strength of randomly 91% of its original mass. In untreated composites, a 5%
oriented treated/untreated composites with varying fibre content composite maintains its stability up to 100°
weight percent loadings and matrix. At a 5% treated C while losing just 9% of its initial amount, and it loses
fibre weight, the impact strength of a variety of compo- 88% of its mass between 200°C and 600°C; Only 8% of
sites was investigated. The following parameters its original weight. is lost by a 10% fibre content composite
observed: It was about 1.95 times that of CG matrix com- up to 100°C, and 84.21% of its mass is lost between 200°C
posites in untreated composites; 2.27 times that of 5%; and 600°C.; Composite materials with a 15% fibre content
3.33 times that of 10%; and 4.82 times that of 15%; and maintain their stability at temperatures up to 100°C while
1.20 times that of 10% and 2.44 times that of 15% in losing only 8% of their initial mass, and between 200°C
treated composites. Suresh et al.66 reviewed the weight and 600°C, they lose 81.74% of their mass; The treated
percentage of reinforcing particles in the range of com- composites of thermal stability are 5% fibre content,
posite materials (5, 10, 15, 20, and 25 wt.%) and their which is stable up to 100°C while losing just 8% of its ori-
influence on mechanical characteristics. Compared to ginal mass and loses 78.79% of its mass between 200°C
hybrid composites, this natural fibre composite yields and 600°C; At temperatures between 100°C and 600°C,
the same results. a composite with 10% fibre content maintains its stability
Comprehensive comparison of mechanical properties while losing only 7% of its initial mass; When exposed to
and production cost of composite material is presented temperatures between 100°C and 600°C, a composite
in Table 2. Fabrication of the 250 × 250 × 3 mm size material with 15% fibre content maintains its stability
OPM fibre/CG composite mat cost is around Rs. 1500/-. while losing only 6% of its initial mass. Surface treatment
the cost of preparation may bring down further during increases the cellulose degradation temperature and the
mass production. It is found that the present OPM fibre/ thermal stability of the fibre, according to the thermogram
10 Proc IMechE Part E: J Process Mechanical Engineering 0(0)
Table 2. Comprehensive comparison of mechanical properties and production cost of composite material.
Mechanical Properties
Figure 12. TGA (a) and DTG (b) curves of the oil palm mesocarp/CG composites.
data, which is attributed to the loss of lignin and hemicel- which is attributed to hydrogen bonding among the hydroxyl
lulose, as well as the enhancement of crystalline order. groups of the cellulose component. The thermal stability of
Finally, the thermal stability of the treated 15% fibre composites was investigated with comparable results to
content is determined to be up to 232°C, indicating that Joseph et al.,70 who examined the thermal behaviour of
it can be employed in reinforced composites with process- sisal fibre/polypropylene composites that were randomly
ing temperatures below 232°C. oriented, and Mofokeng et al.,71 who investigated the
The DTG curves showed a modest peak decrease, indicat- thermal properties of composites made of random-oriented
ing that the degradation rate slowed slightly and that the com- sisal fibre and polypropylene and PLA, respectively,
pressed oil palm mesocarp/CG interfacial combination increased fibre content improves thermal stability, with poly-
influenced their thermal stability. Highest wt. loss occurs propylene showing a more significant improvement.
during the primary degradation period, which ranges from
255°C to 400°C. Figure 12(b) indicates the DTG peak
(Tmax) better thermal stability is observed: Treated composite
Conclusion
reinforced with 15% fibre content (Tmax = 269°C), untreated In this study, the CG matrix from CG powder successfully
15% fibre content (Tmax = 258°C) then compared to the synthesised and biodegradable composite materials devel-
matrix (Tmax = 245°C). The matrix has the biggest derivative oped using the hand layup approach. Short OPM fibres, at
wt. loss, which may be explained by the fact that the addition different fibre loadings (5, 10, 15 wt.%), were included in
of fibres stabilised the composite’s thermal deterioration, the CG matrix as a reinforcement phase. To improve the
Srikanth and Reddy 11
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