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Enhanced Physico-Mechanical Properties of LDPE Reinforced Using
Agro-Wastes as Hybrid Fillers
*Emehige, K. P., Chris-Okafor, P. U., and Anarado, C.E
Department of Pure and Industrial Chemistry, Faculty of Physical Sciences, Nnamdi Azikiwe
University, Awka, Anambra State, Nigeria. P.M.B. 5025, Nigeria
*Corresponding Author
DOI: https://doi.org/10.51584/IJRIAS.2025.1010000045
Received: 26 Sep 2025; Accepted: 03 Oct 2025; Published: 03 November 2025
ABSTRACT
The environmental persistence of petroleum-based plastics such as low-density polyethylene (LDPE) has
necessitated research into eco-friendly alternatives. This study investigates the incorporation of mixed agro-
waste fillers; coconut husk, breadfruit hull, and periwinkle shell into LDPE matrices to assess their
mechanical, thermal, morphological, solvent imbibitions, and biodegradation properties. The composites were
fabricated using injection moulding at filler loadings of 10-40wt% and evaluated according to ASTM
standards. Results revealed significant improvements in tensile, compressive, shear, impact, and hardness
strengths at 20-30wt% loadings, after which agglomeration reduced performance. Differential Scanning
Calorimetry (DSC) indicated melting transitions between 120-170ºC and oxidation stability above 200ºC.
Scanning Electron Microscopy (SEM) confirmed uniform filler dispersion at lower loadings and voids at
higher concentrations. Solvent imbibitions tests showed negligible water absorption but significant uptake in
benzene and toluene, while soil burial tests revealed limited biodegradation, with composites showing
moderate weight loss compared to neat LDPE. These findings suggest that agro-waste reinforced LDPE
composites can serve as cost-effective, sustainable materials for packaging, household, and light construction
applications.
Keywords: LDPE composites, agro-waste fillers, mechanical properties, thermal stability, morphology,
solvent imbibition, biodegradation
INTRODUCTION
Low –density polyethylene (LDPE) is a versatile thermoplastic widely employed in packaging, films,
containers, and insulation due to its toughness, flexibility, and chemical resistance (Ragaert et al., 2017; Khare
and Baruah, 2021). However, its non-biodegradability contributes significantly to global plastic pollution
(Geyer et al., 2017). Research has shown that agro-waste fillers, particularly lignocellulosic residues, can
improve mechanical performance while promoting partial degradability (Ogudo et al., 2021). Previous studies
on LDPE composites reinforced with rice husk (Daramola et al., 2022), snail powder (Chris-Okafor et al.,
2018), and corn cob (Zhu et al., 2018) demonstrated that filler incorporation improves stiffness, tensile
strength, and hardness but reduces elongation at break. The synergistic use of multiple fillers, however,
remains underexplored. This study evaluates the effect of mixed agro-wastes (coconut husk, breadfruit hull,
and periwinkle shell) on the performance of LDPE composites, emphasizing their mechanical, thermal, solvent
resistance, and biodegradation behaviors.
MATERIALS AND METHODS
Sample collection and preparation
LDPE (Indorama Eleme Petrochemicals, grade NGL105FS) was used as matrix. Agro-waste fillers; coconut
husk, breadfruit hull, and periwinkle shell were processed to fine powders (<75µm). Composites were
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prepared at 10-40wt% filler loadings by injection moulding. Mechanical, thermal, morphological, solvent
uptake and biodegradation tests followed ASTM protocols.
Preparation of composites
The fillers were blended in a 1:1:1 ratio and incorporated into LDPE at 10, 20, 30, and 40 wt%. Injection
moulding (200 g capacity) produced test specimens, with an average cycle time of 33secs.
Mechanical properties analysis of the composites
The mechanical properties of the composites considered in this work include; tensile strength, compressive
strength, shear strength, impact strength, and hardness, which were measured using the American Standard
Testing and Measurement method.
Tensile strength
The tensile strength of the composites was measured according to the ASTM standards-ASTM D-638-14,
using the universal testing machine Hounsfield tensometer 8889 made in England. The test piece was
measured to 160mm x 19mm x 3.2mm dimension.
Compressive strength
The compressive strength is the capacity of the composites to withstand loads tending to reduce its size. The
compressive strength of the composites was measured according to the American Standard Testing Method D-
695, using the Hounsfield Monsanto Tensometer 8889. The test piece was measured to 40x40mm dimension
square shape.
Shear strength
The shear strength of the composites was measured according to the American Standard Testing Method D-
732, using the Hounsfield Monsanto Tensometer 8889. The test piece was measured to 20 mm x 20 mm. The
readings were automatically recorded and the values computed.
Impact strength
Testing material impact typically refers to evaluating how a material behaves when subjected to a sudden force
or shock, commonly known as an impact test. The test piece was measured to 100mm x 19mm x 3.2mm.
Hardness strength
The hardness strength of the composite was measured according to the ASTM D2240, using shore scale
Durometer hardness tester, made in England. The values were automatically measured and read. The test was
measured to (100 x 19 x 3.2) mm dimension.
Thermal Analysis
The thermal properties of the composites were studied using Modulated Differential Scanning Calorimeter
MDSC 2920 CE USA. Aluminum pans and lids were used for samples and reference and heating rate of 10ºC
per minute to determine the glass transition temperature (Tg), crystallization temperature (Tc), fusion
temperature (Tm), enthalpy variation and heat capacity.
Surface Morphological study
The microstructural arrangements of the composites were conducted using Scanning Electron Microscope
(SEM) model: JEOL-JSM 7600F.
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Solvent imbibition Analysis
The solvent absorption of the composites was determined using Standard ASTM D-570-98. The composites
cut into 50x50mm dimension were immersed in water, benzene, and toluene respectively for a period of 3days.
The moisture absorption by the composite was measured by the weight gain of the material at daily intervals.
The percentage moisture absorption capacity was expressed as the ratio of increase in mass of the composite to
the initial mass.
Degradation study
This test is done to determine the extent the composites will degrade in the environment. This was determined
using soil burial degradation test. Composites were buried in a soil obtained from an automobile mechanic
workshop for degradation. Composites were cut into 50x50mm dimension, weighed and buried into the soil at
12cm depth for a three-month period. The composites were weighed at interval of 30 days during the test
period to determine the extent of degradation. The degradation rate was calculated using the formula;
Percentage degradation = Wf – Wi x 100
Wi
Wf=Final weight, Wi= Initial weight
RESULTS AND DISCUSSION
The results of the mechanical properties of the low density polyethylene with coconut husk, breadfruit hull and
periwinkle shell composites are shown in the figures below.
Mechanical properties
Tensile strength
Tensile strength measures the resistance of a material to breaking under tension. The result of the tensile
strength of the composites is shown in Fig. 1.
Fig. 1. Effect of filler loading on the Tensile strength of LDPE composites
The tensile strength of LDPE composites increased with filler loading up to an optimum point before
declining, as shown in Figure 1. With increasing filler load (10-30wt%), tensile strength improved
significantly, reaching a peak of 115N/mm
2
at 30wt% loading, attributed to effective stress transfer, restricted
polymer chain mobility, and strong filler-matrix adhesion (George et al., 2016; Essabir et al., 2013). Beyond
this level (40 wt%), tensile strength decreased sharply (<30N/mm
2
), likely due to filler agglomeration, poor
0
20
40
60
80
100
120
140
0 10 20 30 40
TENSILE TEST (N/mm
2
)
FILLER LOAD (%)
LDPE TENSILE TEST (N/mm
2
)
LDPE TENSILE
TEST (N/mm2)
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dispersion, and stress concentration effects, which created weak zones and reduced mechanical integrity
(Jawaid and Khalil, 2011).
Compressive strength
Fig. 2. Effect of filler loading on the Compressive strength of LDPE composites
The compressive strength increases steadily as filler loading rises to 10 wt% and reaches a peak at 20 wt%
filler content (5.0 N/mm
2
). This enhancement can be attributed to improved stress transfer between the matrix
and the filler, good interfacial adhesion, and effective dispersion of the filler particles within the LDPE matrix,
which restricts polymer chain mobility and enhances load-bearing capacity (Rahman et al., 2019). Beyond 20
wt% filler loading, the compressive strength decreased gradually, dropping about 4.0 N/mm
2
at 30 wt% and
further to 3.0 N/mm
2
at 40 wt%. This decline is often linked to agglomeration of filler particles at higher
concentrations, which introduces voids, micro-cracks, and weak filler-matrix bonding, thereby reducing stress
transfer efficiency (Azeez et al., 2020). Such behavior is consistent with the findings of Sanyang et al. (2015)
that polymer composite where optimum mechanical strength is studied, is typically observed at moderate
loadings due to poor dispersion and stress concentration effects.
Shear strength
Fig. 3. Effect of filler loading on the Shear strength of LDPE composites
The LDPE shear strength test shows that shear strength increased from about 7 N/mm
2
at 0% filler to 13
N/mm
2
at 20 wt% filler, dropped slightly to 10 N/mm
2
at 30 wt%, and then rose sharply to 15 N/mm
2
at
40wt% filler load. The initial increase is attributed to good filler dispersion and enhanced interfacial bonding,
which improve stress transfer and restrict polymer chain mobility (Callister and Rethwisch, 2020). The decline
0
2
4
6
0 10 20 30 40
COMPRESSIVE TEST (N/mm
2
)
FILLER LOAD (%)
LDPE COMPRESSIVE TEST
(N/mm
2
)
LDPE
COMPRESSIVE TEST
(N/mm2)
0
2
4
6
8
10
12
14
16
0 10 20 30 40
SHEAR TEST (N/mm
2
)
FILLER LOAD (%)
LDPE SHEAR TEST (N/mm
2
)
LDPE SHEAR TEST
(N/mm2)
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at 30 wt% filler suggests possible filler agglomeration and weak adhesion that create stress concentration
points. However, the sharp improvement at 40 wt% indicates that higher filler content promoted denser
packing and better reinforcement within the matrix, thereby enhancing resistance to shear forces (Ahmed et al.,
2012).
Impact strength
Fig. 4. Effect of filler loading on the Impact strength of LDPE composites
A significant decline was observed at 10wt% filler loading, where the impact toughness dropped drastically to
around 25 J/m
2
. This reduction can be attributed to poor interfacial adhesion between the filler and the polymer
matrix, which promotes stress concentration and reduces energy absorption capacity (Idris et al., 2020). An
improvement in impact toughness was recorded at 20 wt% filler loading, suggesting better filler dispersion and
interfacial bonding at this concentration, which could enhance energy dissipation during impact. Beyond 20
wt%, a gradual decline in impact strength was observed up to 40 wt%, likely due to filler agglomeration and
matrix embrittlement, which hinder stress transfer efficiency and create microvoids that act as crack initiation
sites (Owonubi et al., 2020). Overall, the result indicates that moderate filler loading (around 20 wt%)
enhances impact performance, while excessive filler addition deteriorates the toughness of LDPE composites.
This is in line with the observations of Raj et al. (2023) that optimal filler concentration enhances polymer
toughness through improved filler-matrix compatibility, while higher loadings lead to brittleness and reduced
ductility.
Hardness strength
Fig. 5. Effect of filler loading on the Hardness strength of LDPE composites
0
20
40
60
80
100
0 10 20 30 40
IMPACT TOUGHNESS (J/m
2
)
FILLER LOAD (%)
LDPE IMPACT TOUGHNESS (J/m
2
)
LDPE IMPACT
TOUGHNESS (J/m2)
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As observed, the hardness strength initially increased sharply from the neat LDPE value ( 0% filler) to its peak
at 10 wt% filler loading, after which it gradually declined with further increases in filler content up to 40 wt%.
The initial increase in hardness strength can be attributed to the efficient dispersion of filler particles within the
LDPE matrix, which enhances rigidity and resistance to deformation (Abdul Khalil et al., 2012). At this stage,
good interfacial adhesion between the filler and polymer matrix likely restricted the movement of polymer
chains, leading to improved surface hardness (Nwabanne et al., 2017). However, beyond 10 wt% filler loading,
the hardness strength decreased progressively, indicating that excess filler led to particle agglomeration and
poor stress transfer efficiency within the matrix (Osei et al., 2020). Such agglomeration creates weak points
that act as stress concentrators, thereby reducing the overall resistance of the composite to indentation. This is
in line with the works of Eze et al. (2019), who reported that excessive filler content often results in poor
matrix-filler interfacial bonding and increased void formation, thereby lowering hardness.
Thermal analysis
Fig. 6a: DSC thermogram of 10wt% LDPE composite
Fig. 6b: DSC thermogram of 20wt% LDPE composite
0
50
100
150
200
250
Enthalpy (J/g) Peak melting
temperature
(˚C)
Oxidation
temperature
(˚C)
Onset melting
temperature
(˚C)
Values
Thermal Analysis of 20% LDPE composite
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Fig. 6c: DSC thermogram of 30wt% LDPE composite
Fig. 6d: DSC thermogram of 40wt% LDPE composite
From Figures 6a-d, the DSC results showed that the LDPE composites generally exhibited melting transitions
within 120-170ºC and oxidation stability in the range of 200-237ºC. This is in agreement with the works of
Zhang et al., (2018) that LDPE composites typically display melting peaks around 120-135ºC and oxidation
temperatures above 200ºC depending on filler interaction. The observed enthalpy values reflect variations in
crystallinity, which is consistent with findings that filler loading can either promote or restrict chain packing
(Joseph et al., 2020). At low filler loading (10wt%), higher melting (169.53ºC) and oxidation temperature
(236.95ºC) suggest enhanced stability and this is in agreement with Essabir et al., (2013), that reported
improved thermal resistance at low filler levels. However, the sharp reduction in melting temperatures at 20-
30wt% contrast with George et al. (2016), who found more gradual changes with increasing filler. The decline
in enthalpy at 30-40wt% indicates imperfect crystallization, aligning with Singh et al. (2017), who observed
reduced crystallinity in overloaded composites.
Surface morphology study
Fig. 7a LDPE 10% LDPE 20% LDPE 30% LDPE 40%
0
50
100
150
200
250
Enthalpy (J/g) Peak melting
temperature
(˚C)
Oxidation
temperature
(˚C)
Onset melting
temperature
(˚C)
Values
Thermal Analysis of 30% LDPE composite
0
50
100
150
200
250
Enthalpy (J/g) Peak melting
temperature
(˚C)
Oxidation
temperature
(˚C)
Onset melting
temperature
(˚C)
Values
Thermal Analysis of 40% LDPE composite
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From Figure 7a, 10-20wt% showed visible voids, micro cracks distributed across the matrix. Such features can
be due to inadequate filler-matrix adhesion and phase separation at lower filler loadings (AlMaadeed et al.,
2012). The elongated streaks and uneven dispersion suggest partial agglomeration of fillers, which may hinder
uniform stress transfer during mechanical loading. The moderate roughness observed in these micrographs is
advantageous for biodegradation. Surface irregularities and voids increase the accessible surface area for
microbial attack and enzymatic penetration, facilitating gradual breakdown of the polymer composite (Ojijo
and Ray, 2013). This aligns with the work of Chiellini et al. (2003) that composites with discontinuous
morphologies tend to degrade faster due to increased hydrophilicity and moisture uptake pathways created by
interfacial defects. The higher filler loadings (30-40 wt%) showed good dispersion and this can be due to
matrix-filler compatibility which improved the interfacial adhesion and minimized agglomeration.
Solvent imbibtion study
Fig. 8: Effect of filler loading on the solvent imbibition properties of LDPE composites.
The solvent imbibition behavior of low density polyethylene composites varied with solvent type, filler
loading, and immersion time. Low density polyethylene showed very low affinity for water at room
temperature for seventy-two hours. This is in line with the works of Ogudo et al., (2021); Nwokoye et al.,
(2024) that observed no water adsorption by the hybrid filler. Thus, the non-absorption of water by the
composites could be due to its hydrophobic nature, with only slight weight change attributed to surface
adsorption. In contrast, higher absorption was observed in toluene and benzene, consistent with their non-polar
character and closer solubility parameters to low density polyethylene (Sivakumar and Rajini, 2016). Benzene
exhibited the highest uptake, indicating stronger polymer-solvent interaction. On the other hand, filler content
also influenced solvent uptake. At lower loading (0-10 wt%), absorption was relatively low due to reduced free
volume and better polymer-filler adhesion. Intermediate loadings (20-30wt%) showed higher uptake, likely
from microvoids and weak interfacial bonding that facilitated solvent diffusion (Thakur et al., 2014). At higher
filler content (40 wt%), solvent absorption stabilized, suggesting restricted chain mobility and limited
penetration. Moreover, weight gain increased with immersion time and tended towards equilibrium after 48-72
hours, characteristic of fickian-type diffusion (Sreekumar et al., 2007). Overall, low density polyethylene
composites demonstrated good resistance to water but significant swelling in organic solvents, implying
suitability for wet environments but reduced stability in hydrocarbon-rich conditions.
0
2
4
6
8
10
12
0 24 48 72
Weight (g)
TIME (Hr)
LDPE0% water
LDPE 0% toluene
LDPE0% benzene
LDPE10% water
LDPE10% toluene
LDPE 10% benzene
LDPE 20% water
LDPE 20% toluene
LDPE 20% benzene
LDPE 30% water
LDPE30% toluene
LDPE30% benzene
LDPE 40% water
LDPE 40% toluene
LDPE40% benzene
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Biodegradation test
Fig. 9: Effect of filler loading on the degradation of LDPE composites
From Figure 9, there was no reduction in weight for 0% LDPE during the 90 days test periods. For 30wt%
composites, minimal weight loss was noticed indicating limited microbial attack and surface oxidation. This is
in line with the works of Arutchelvi et al., (2008) that pure polypropylene undergoes very slow biodegradation
due to its hydrophobic backbone and high crystallinity. This observation corroborates the research findings of
Narancic et al., (2018) that incorporating LDPE into biodegradable matrices slows the overall degradation. The
minimal degradation exhibited as the filler loading increased could be attributed to the organic nature of the
fillers, which attracted the presence of micro organisms. These microbes will usually attack the sites of fillers
interaction thereby creating voids in the composites framework, hence a collapse of the framework after
sometime.
CONCLUSION
Mixed agro-waste fillers effectively reinforced LDPE composites, improving mechanical and thermal
properties at moderate loadings (20-30 wt%). However, high filler loadings compromised performance due to
agglomeration. Limited solvent resistance and biodegradation highlight the need for compatibilizers and
further modification.
RECOMMENDATIONS
1. Employ coupling agents (e.g., maleic anhydride grafted polyethylene) to enhance interfacial adhesion.
2. Long-term biodegradation under real environmental conditions should be evaluated.
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