Materials Research.

2022; 25:e20220406
DOI: [Link]

Investigation of TiO2 Nano Filler in Mechanical, Thermal Behaviour of Sisal/Jute Fiber

Reinforced Interpenetrating Polymer Network (IPN) Composites

Kumar Vijayendra Gopala, Kuttynadar Rajammal Vijaya Kumara,

Gopi Sureshb* , Vezhavendhan Rajasekharanc, Prasumanna Krishnamurthy Nagarajanb,

Chinathambi Muthukaruppan Meenakshid

Dr. M. G. R. Educational and Research Institute, Department of Mechanical Engineering, Chennai, India.
a

b
Rajalakshmi Institute of Technology, Department of Mechanical Engineering, Kuthambakkam, Chennai, India.
c
School of Mechanical Engineering, Department of Manufacturing Engineering, VIT, Vellore, India.
d
Bharath Institute of Higher Education and Research, Department of Mechanical Engineering, Chennai, India.

Received: September 11, 2022; Accepted: October 01, 2022

In this work, various proportionate (0%, 1%, 3% 5% & 7%) of titanium di-oxide nano-filler was
utilized as particulate matter along with the sisal/jute fiber reinforcement, in the view to increase the
physical properties of the composite materials. Beside, as matrix material the mixture of Epoxy (E) and
Polyurethane (PE) was chosen with the proportionate of 70 and 30 wt.% respectively, in order to extract
the specific qualities of both the matrices to achieve the interpenetrating polymer networks (IPNs).
Moreover, to exactly find out the thermo-mechanical characteristics of the sisal/jute fiber reinforced
IPN composites, tests like thermo-gravimetric analysis (TGA), tensile, flexural, Impact, short beam
strength and water absorption tests were carried out as per standards. It was found that, incorporation
of 5% of TiO2, increases the mechanical properties such as tensile, flexural, impact and short beam
strength. Similarly, incorporation of TiO2 into IPN matrix enhances the thermal stability and water
absorption resistance. All the obtained values of various filler weight % of TiO2 were compared with
each other against with and without particulate incorporated IPN laminate in the purpose of using the
same in construction industries.

Keywords: Epoxy, polyurethane, TiO2, thermo-gravimetric analysis, mechanical properties.

1. Introduction
Nowadays, natural fiber reinforced composites are thermosetting polymers. Mostly the thermoplastic networks
currently becoming one of the focal topic due to their wide include polypropylene and polyethylene resins, while the
range of applications like low-cost, non-toxic, biodegradable, thermosetting matrices are epoxy, vinyl ester, polyester,
and easily recyclable. Because of its unique nature and and polyurethane8,9.
good biocompatibility, it could be employed to substitute Among all sets of natural fibers available in the market,
commonly used chemical fibers such as carbon and glass sisal and jute play the major role and are extensively employed
fibers1-3. Natural fiber reinforced with different matrices have in most of the industrial and commercial applications.
been explored in recent studies moderately, in that about In fact, the main reasons behind those fibers in the field of
15–20 percent is being employed in the vehicle industry natural fiber reinforced composites are their cheapness and
and even more exclusively used in construction industries easy availability and processing10. Sisal is a fiber extracted
due to all applications4-6. In the researcher’s point of view, from the Agave plant that is native to Tropical america. It is
natural fibers are generally divided into two categories: a tough shrub that thrives in hot conditions. Furthermore,
plant-based and animal-based. In the first category of plant it is capable of growing in dry places that are typically
fiber base, sisal, hemp, cotton, coir, pineapple, and kenaf inappropriate for plants11-13. Similarly, Jute fibers are made
are holding the main role in developing the natural fiber from the plant called genus Corchorus of the Malvaceae
(plant fiber based) based composites7. Though animal fibers family. Jute fibers are renewable and biodegradable and
not having that much significant importance due to their reusable, making them environmentally sustainable distinct
unavailability as well as scarcity, still it passively holds as processing methods are employed indeed. Likewise, Jute
the second position in developing animal based fibers which fibers have excellent insulation and strength properties, with
includes silk, feathers, and wool etc., as the base material. moderate water absorption regain and no skin problems while
Moreover, depending on the various applications, the having contact with the humans. On the other hand, the recent
fibers can be combined with thermoplastic elastomers and annual global production of jute fibers is estimated to be
around 3 million tonnes as well which is used for a variety
*e-mail: saisuresh1979@[Link] of applications all around the world14. Jute backpacks have
2 Gopal et al. Materials Research

gained in popularity as an eco-friendly alternative to both of epoxy and polyurethane (IPNs) has been taken as the matrix
non - compostable poly bags derived from oil and garbage material. Besides, various proportions of TiO2 (0%, 1%, 3%
bags that require a significant amount of wood. Normally 5% & 7%) is taken as the particulate matter along with the
all kinds of natural fibers are extracted from the plants IPN (epoxy and polyurethane) mix. All through this study,
through the method called decortication, in which plant the chosen reinforcement fibers are sisal and jute, singly each
leaves or roots are crushed, brushed, beaten either manually fibers (sisal and jute) have been selected as the reinforcing
or mechanically, and finally sent through rotating wheels in agent, also along with that combination of sisal/jute fibers
the intention to avail lengthy fibers15,16. separate laminate have been be prepared in the intention to
In the due course, various abstraction methods and fabricate the hybrid composite with various proportionate
procedures are employed to extract the natural fibers to of particulate matter. As well, to test the formed laminate,
compete with the artificial fibers. Even though it become as the tests like TGA, tensile, flexural, impact, short beam shear
moderate substitute of synthetic fibers, still it is not completely strength and water absorption tests are conducted on the
believed as the suitable replacement of the synthetic fibers. fabricated laminate. The obtained results were compared
Hence to improve the strength of the fibers various techniques to each other to evaluate the influence of particulate matter
were used to get the superior final product, in that sequence, in the IPN matrix24,25.
techniques like utilizing the different sizes of the natural fibers
as reinforcements as well properly choosing the appropriate 2. Materials and Method
alkali treatment methods, are nowadays widely used to get
the required strength and compatibility, especially in the area 2.1. Preparation of titanium dioxide nano powder
of fiber strengthening aspects, dramatic research activity
During the preparation of titanium dioxide, Nano
is happening in the past few decades. In line of the above,
powder as such received from the suppliers were used for
treatments like alkaline, acetylation, acrylation, bleaching,
the processing without any further purification. Likewise,
bezoylation, isocynate, silane are the universally and widely
titanium tetra iso-propoxide and heptane are also purchased
adopted methods to strengthen the fibers17,18. Additionally,
from Chin Chin Chemicals for the chemical processing. Along
matrix material also exclusively plays a wide spectrum of
with that, the required amount of heptane and propoxide was
role in increasing the strength of the composite laminate. taken with a percentage of 29.3 ml and 100 ml respectively.
In that sequence, thermoset matrices like epoxy, vinyl ester Additionally, these solutions were physically stirred for the
and polyurethane generally play a vital role in structuring the period of 2 hours. Above and beyond, the required amount
composite material based on the user preference19. Though of distilled water (8 ml) was slowly added to the mixture
each material has had some unique characteristics while and it was kept at ambient temperature for the period of
opting for fabrication purposes, manufacturers or users often 80 hours. Finally, the obtained mixture was filtered with
complain of some service/service defects. To overcome the normal filter paper following which the calcination process
issues encountered in each matrix, the concept of mixing was carried out for the period of 24 hours by maintaining the
the two different sets of monomers has been proposed by temperature of 80°C likewise again raising the temperature
chemists in the name of interpenetrating polymer networks of 220°C for the period of 2 hours26.
(IPNs). Numerous research activities are presently happening
in these particular IPNs, in order to exactly use the final 2.2. Preparation of ipns and titanium dioxide
matrix material to the various industrial applications20,21. blend
In addition to that, to further strengthen the laminates to
To get the exact proportionate of the IPNs, the required
the discrete level, at the present time, particulate fillers have
amount of epoxy and polyurethane (70:30) wt. ratio was
made remarkable contributions. Furthermore, numerous
mixed and their viscosity also maintained, by placing the
researchers have suggested and tried out different types of
blend at the temperature of 80°C, for the period of 20 minutes
nano fillers in their own accord. Mostly, fillers are broadly
as prescribed from the supplier data sheet as mentioned in
classified as organic and inorganic fillers, in the family of
the Table 1.
series of inorganic nano fillers, widely accepted nano fillers Following the mixing procedure, the various proportions
are aluminium trihydrate, ammonium polyphosphate and (0%, 1%, 3% 5% & 7%) of TiO2 was taken separately by
Titanium dioxide etc., Among all nano fillers, TiO2 have weighing with accuracy of ±0.1 mg. While preparing the
been considered as the special one as reinforcing agents TiO2 for the fabrication purpose, the particulate was dried
because of its unique characteristics like high refractive completely by maintaining it at the temperature of 100°C. Most
index, hydrophobicity and non-toxicity. Though the separate of the studies suggested that, it is the best method to disperse
mechanical analysis have been performed as substituting the particulate into the matrix was mechanical stirring, in this
the TiO2 as the particulate matter with the neat thermoset
resins, the concept of incorporating the TiO2 with IPNs along
with the natural fibers are not completely exploited. In the Table 1. Property of raw materials14.
view to meritoriously utilize the remarkable contributions
of the IPNs and filler particulate (TiO2) the concept of Properties Epoxy Polyurethane
particulate filled natural fiber reinforced IPN laminate has Density (g/cm3) 1.15 1.45
been conceptualized22,23. Tensile strength (MPa) 74 46.43
During the course of this study, sisal and jute fiber have Tensile modulus (GPa) 3.74 2.12
been taken as the reinforcement agent whereas the combination Poisson’s ratio 0.32 0.24
 Investigation of TiO2 Nano Filler in Mechanical, Thermal Behaviour of Sisal/Jute Fiber Reinforced Interpene-
trating Polymer Network (IPN) Composites 3

work also high speed magnetic stirring was adopted followed 2.4. Thermo-gravimetric (TGA)
by the sonication processes. The prime reason behind that of
TGA was performed on all fifteen sets of sisal/jute
stirring was that, magnetic stirring might decrease the bubble
fiber reinforced hybrid IPN laminates to determine their
formation and tend to reduce the void content significantly.
thermal stability and compare each other towards to predict
The matrixes with TiO2 of variant weight proportions were
the laminate behaviour. The testing was conducted on a
stirred for the period of one hour to completely disperse the
Shimadzu DTG-50 instrument in a nitrogen atmosphere
nano particles into the matrix to avoid the agglomeration issues. (40 ml/min). Hybrid IPN laminate specimens with a volume
Also, the required amount of hardeners like HY951 grade and of 7-8 mg each were heated from 30°C to 530°C at a steady
MOCA was added for epoxy and polyurethane respectively. rate of 10°C/min29.
The IPN blend with titanium dioxide mixture was used for
the final fabrication processes27. 2.5. Methodology
2.3. IPN laminate preparation The fabricated natural hybrid laminate with various
combinations of filler material was systematically investigated
Initially to do the fabrication process, exact proportionate through the different mechanical tests to thoroughly
of particulates were taken along with the premixed matrix understand the physical behaviourism of the IPN laminate.
IPN Blend. The exact schematic processes representing the Nevertheless, to carry over the above processes different tests
entire fabrication processes were represented in the Figure 128. were performed on the IPN composite as shown in Table 430.
From the fiber preparation perspective, the chosen sisal
and jute fiber was already dried at ambient temperature to 2.5.1. Tensile test
completely remove the water absorption content and their To do the tensile test analysis, specimen edges were
corresponding physical properties were mentioned in Table 2. firmly fixed on the universal testing machine chucks and the
Secondly the 60:40 wt.% ratio of (weighed) pre-cut sisal/ load was applied in longitudinal direction until the specimen
jute fiber and matrix was taken for the laminate preparation, fracture. Besides, during the testing procedure, cross head
following which through the hand-layup technique the speed of 2 mm/min was maintained.
laminate were prepared by placing the fiber mat and matrix
one over another. In the same way, the formed laminate was 2.5.2. Flexural test
placed in the compression mould which was having the The specimen was laid horizontally over the two contact
dimension of 300 x 300 x 3 mm, following this; required points and vertical load was applied on the top of the specimen
amount of pressure (12 MPa) was applied over the laminate, till the sample specimen fractures. All through the course
by maintaining the temperature of 100°C to form the hybrid of study, cross head speed of 5 mm/min was maintained.
IPN laminate. In fact, to thoroughly understand the various
combinations of fiber/matrix and filler materials, a different set 2.5.3. Impact
of combinations of natural fiber reinforced (particulate filled) The impact test specimen was initially placed in the
IPN composite was fabricated as mentioned in the Table 3. charpy test work piece holder and allowed the weight to fall

Table 2. Properties of sisal and jute fibers10-12.

Properties Units Sisal fiber Jute fiber
Density g/m3 1.5 1.3
Elongation at break % 2.2-2.7 1.4-1.9
Tensile strength MPa 514-720 382-774
Young’s modulus GPa 10.2-22.5 27.5
Cellulose % 66 62-72
Lignin % 10.2 12.5-13.5
Microfibrillar angle - 23 9
Wax % 2.2 0.6
Hemi-cellulose % 23 15-21
Pectin % 11 0.3
Ash % 0.6-1.1 0.6-2.1 Figure 1. Schematic view of fabrication of Sisal, Jute, Sisal/Jute
(TiO2 loaded) IPN composite.

Table 3. Combination of sisal/jute hybrid IPN composites.

TiO2
Fiber IPN – Combinations (Epoxy/Polyurethane)
0% 1% 3% 5% 7%
Sisal (S) SIP0 SIP1 SIP3 SIP5 SIP7
Jute (J) 70:30 (wt.%.) JIP0 JIP1 JIP3 JIP5 JIP7
Hybrid (SJIP) SJIP0 SJIP1 SJIP3 SJIP5 SJIP7
S – Sisal, J – Jute, E - Epoxy, PU – Polyurethane.
4 Gopal et al. Materials Research

over the specimen and their corresponding energy absorption

values were noted down. To do all sets of test procedures, ∆M ( t )
= ( ( m – m ) / m ) ×100
1 2 2 (2)
five specimens from each proportionate were identified and
their corresponding results were averaged. Where, ΔM (t) – Water uptake at time “t”, m1 – wet weight,
m2 – dry weight.
2.5.4. Short beam shear strength
To do shear beam shear test, the specimens were placed 2.6. Fractrography
on the horizontal shear test fixture by maintaining the fibers The JEOL JSM-6480LV instrument was often used to
were parallel to the loading edge. As well, the beam strength examine the Fractrographic characteristics of sisal/jute fiber
was calculated with help of the formula mentioned in the reinforced hybrid composites. Across most application fields,
Equation 1. samples are gathered over a specific area of the material’s
surface, and a two-dimensional image displaying spatial
Short beam shear strength = heterogeneity characteristics was generated. The morphological
(1) study can also be used to analyse specific locations on the
( 3 × Peak load ) / ( 4 × breadth × thickness ) sample; this method was particularly useful in evaluating the
surface chemistry, crystal structures, and crystallographic
Further to this, the entire procedure was done by keeping
structure in a descriptive or moderate manner. Specimens
the cross head speed of 2mm/min.
were also fixed with base coat before going through graded
2.5.5. Water absorption alcohol dehydration series to prepare them for the analysis.
To actually carry out the standard water absorption test The samples are fully prepared to be interpreted on the SEM
on composites, during this course of study, specimens were once the gold coating was already completed32.
thoroughly dried with (2 hours) help of the oven to make
sure that specimens were completely water absorption free. 3. Result and Discussion
After cleaning the specimens by manual process, their initial
weight was measured with an electronic weighing instrument 3.1. Thermo-gravimetric
to the level of ±0.1. After weighing was done, the specimens’ The thermo-gravimetric analysis of the sisal, jute, sisal/
edges (sides) were completely coated with epoxy resin to jute (hybrid) fiber reinforced (TiO2) particulate loaded IPN
avoid the water penetration through the fiber matrix bonding composite were shown in the Figure 2 (a) (b) (c). It was
areas. At last the specimens were placed in the deionized observed that, irrespective of fiber reinforcement, the significant
water for the specific duration. In this particular study, the weight loss was observed up to the level of 5%, during the
specimens were exposed to the humid environment for the initial time, this effect or weight loss was purely because of
period of 12 months. Moreover, to get to know the water the removal of moisture content from the IPN composite.
absorption in a specific interval of time, specimens were Subsequently major weight loss was witnessed from all the
taken from every interval and cleaned with linen free cloth graphs up to the level of 75%, at higher temperatures due
and weighed. As well, the percentage of water absorption was to the effect of matrix degradation as well volatilization of
calculated by the variation obtained from the initial weight IPNs. After the test specimens were subjected to higher
and final weight. The following Formula 2 was mostly used temperatures, residue formation had been visualized such
in calculating the water absorption ratio of all composites31. a way that maximum weight loss would be accomplished;
this was called the final weight loss. The initial and major
weight loss of the sisal, jute, sisal/jute fiber (particulate
Table 4. ASTM standards30,31 and dimensions of the specimen. loaded) reinforced composite temperatures were given in
the Table 5.
Size of the specimen It was clearly found that, irrespective of fiber reinforcement,
ASTM Standards (Length x breadth x
all kind fiber reinforced IPN composite specimens had shown
thickness in “mm”)
the same set of TG values. However, the particulate addition
ASTM D 3039 - Tensile 250 x 25 x 3.2
into the IPN composite significantly shows a higher TG
ASTM D 790- Flexural 127 x 12.7 x 3.2
value than the neat IPN resin (without particulate loading)
ASTM D 256 – Impact 63 x 12.8 x 3.2
composite. To prove this, a particulate (sisal fiber reinforced)
ASTM D 2344 – Short beam shear 18 × 6 × 3
loaded specimen gives the TG value as 310°C, 340°C,
ASTM D 570 – Water absorption ⌀50.4 x 3.2 380°C and 410°C for 1%, 3%, 5% and 7% respectively.

Table 5. TGA – analysis of sisal, jute and sisal/jute (particulate loaded) hybrid IPN composite.
0% 1% 3% 5% 7%
Fiber /Particulate
WL (°C) WL (°C) WL (°C) WL (°C) WL (°C)
SISAL 480 490 495 510 515
JUTE 445 485 490 512 513
SISAL/JUTE 465 492 492 514 516
WL – Weight Loss at 75%.
 Investigation of TiO2 Nano Filler in Mechanical, Thermal Behaviour of Sisal/Jute Fiber Reinforced Interpene-
trating Polymer Network (IPN) Composites 5

Figure 2. Thermogravimetric analysis of (a) sisal (b) jute (c) sisal/jute fiber reinforced (TiO2) particulate loaded IPN composite.

During the study, it was observed that, the 1% of loading of

particulates had substantially raised the TG value as 4.8%,
this uptrend was kept seen upon loading of particulates into
the IPN composite. Likewise, 3%, 5% and 7% addition of
particulates had shown the rise in value of nearly 9.5%,
11.5%, and 7.8% respectively. In the same way, jute fiber
reinforced particulate loaded composite as well shows the
same trend as such positive trend line shown in the sisal
fiber, even the hybrid fiber as well showed the same hike
in trend line as seen in the sisal and jute fibers. Mostly all
the fiber reinforced composites had shown the equal rise in
trend line upon loading of particulate matters. From the study,
it was clearly understood that, the fiber reinforcement had
Figure 3. Tensile strength analysis of (a) sisal (b) jute (c) sisal/jute
not shown any remarkable impact on the TG values, in-turn
fiber reinforced (TiO2) particulate loaded IPN composite.
particulate loading into the IPNs shown the significant rise
in the TG value. The additions of particulate matter into the
IPN composite greatly rise the TG value to distinguished
manners. Actually, the particulate fillers and IPN blend higher levels of stresses as compared with their counterpart
inevitably makes a better mutual entanglement mechanism jute fiber. As well, the common failure procedure starts
between them and vice versa enhances the improved heat from cracks on the matrix, follows with the detorting the
resistance upon the fiber and resins. Since particulate matter interfacial stresses between the fiber and matrix and at last
improvises adhesion property between the fiber and resin ends up with the fiber scissoring, pull out and fiber breaking.
amongst the IPN laminate, this effect directly enriches the All the above fiber breakages as well were observed on all
TG value to notable level. the specimens irrespective of the particulate loading and fiber
reinforcement. Whereas, particulate loading significantly
3.1. Tensile strength improves the laminate strength to a considerable level.
The tensile strength and modulus of various proportions This was evident on all the specimens upon loading of the
of particulate loading of TiO2 were shown in the Figure 3. particulate matter into the IPN laminate. Moreover to prove
During the initial investigation on the specimens with 0% this, the 1% particulate addition into the IPNs had shown
(pure resin loaded) particulate loading had shown the tensile the stress value as 41.53, 24.09 and 32.81 MPa for SIP, JIP
strength value of 38.46, 22.41, 30.53 MPa for SIP, JIP and and SJIP respectively. Yet evidence upon the particulate
SJIP respectively. However, it was found that the sisal fiber addition, IPN laminate shows the substantial level of strength
reinforced specimens had shown the higher strength value advancement in all levels of incorporation of titanium dioxide.
as compared with the jute fiber reinforced IPN composites. Upon loading the 1% of particulate, the difference of climb
This effect predominately shows that sisal fiber transfers was seen as 6.95%, 6.54% and 7.12% for corresponding
6 Gopal et al. Materials Research

SIP, JIP and SJIP. Similarly the 3% addition of particulate a higher level of flexural load bearing capacity as compared
into the IPNs showed the significant rise in stress value, the with the remaining all set of IPN composites such as JIP
observed values as 45.62, 26.46 and 36.04 MPa for SIP, JIP and SJIP. To evidence this, the neat IPN (without loading
and SJIP individually. In turn their respective level of climb of particulate) had shown the flexural strength value as
was observed as 8.96%, 9.12% and 9.01% for all SIP, JIP 42.64 MPa, whereas their counterpart JIP shows flexural
and SJIP. Again the same trend of increased strength value strength value as 31.94 MPa. Similarly their combination
was observed upon adding the 5% of titanium dioxide. (hybrid) had shown the flexural strength value as 37.29 MPa.
But the observed values were quite high in all levels of fiber Equally, upon loading of the particulate matter into the IPN
reinforcement; the obtained numerals were 52.72, 30.58 and matrix significantly increases their flexural strength value to
41.65 MPa for SIP, JIP and SJIP respectively. In this above marginal level. To mark this, IPN laminate’s with various
connection of increasing trend in all sets of strength values reinforcement shows the strength value as 44.52, 33.35 and
were shown that, the titanium dioxide extensively plays the 38.93 MPa for 1% TiO2 loading into the matrix for the fiber
major role in stiffening the laminate, the added particulate reinforcement of SIP, JIP and SJIP respectively. Nevertheless,
matter completely diffuses into the matrix material in the 3% particulate loading again shows the same trend
large, and evenly distributes into the IPN blend as much line of strength growth. The observed values were 49.12,
as possible. Besides, the incorporated particulates were 36.79 and 42.96 MPa SIP, JIP and SJIP respectively. Beside
filled deep into the voids present in the fibers and creates the 5% particulate addition also shows the hike in the flexural
the better interfacial adhesion between the fiber and matrix, strength value, the obtained value was 53.82, 40.31 and
due to this reason, the stress transfer was happening in the 47.07 MPa for SIP, JIP and SJIP respectively. All through
linear manner along the direction of fiber and laminate bears the investigation of the flexural analysis, it was observed
the higher strength value, all this effect were evident in the that the load was evenly distributed between fibers and the
graphs upon addition of particulate into the matrix material. IPN matrix when the specimen was subjected to gradual
As such, an increasing trend of values observed in the tensile loading before fracture occurs. As well, crack propagates
stress graphs, their corresponding modulus value also indeed longitudinally along the IPN laminate cross section and
shows the same level of increasing effect by loading the simultaneously disturbs the inter-laminar shear strength
particulate matter into the IPN matrix. To evidence this, the between the fiber and matrix. However, the loading of 7%
neat IPN laminate (without particulate loading) showed the particulate loading into the IPN matrix slightly shows the
modulus value as 2.51 GPa for SIP, whereas the increase decreasing scenario of flexural strength value, the obtained
upon loading the particulate matter, it shows the value of values were 47.14, 35.31 and 41.22 for SIP, JIP and SJIP
3.15 GPa as modulus value. However, this trend of increase respectively. The prime reason for absorbing the negative
in modulus value was continuously observed in all sets of trend was that, the particulate could not evenly distribute
IPN laminate’s with due respect of addition of particulate into the matrix and thus the problem of agglomeration
matter into the matrix. The actual reason behind that increase (clustering) happened in the laminate, hence it loses the
in modulus was directly correlated with the stiffening effect stress transfer mechanism between the fiber and matrix.
of IPN laminate. The addition of the particulate matter into Due to this concern, the energy transfer was not properly
the matrix inversely increases the modulus level and directly
initiated between the fiber and matrix instead it forms the
increases the tensile strength level irrespective of all fiber
localized zone of stress concentration along the line of fiber
reinforcement and matrix material33,34.
and initiates the premature crack following with the fiber
3.2. Flexural strength breakage and pull-out, the same was again leads to the earlier
failure due to the continuous prorogation of the cracks along
The flexural strength and modulus with various proportions direction of stress concentration zones. Flexural modulus also
of particulate loading of TiO2 were shown in the Figure 4. increased up to the level of 2.01, 1.62 and 1.82 GPa for SIP,
While doing the flexural strength analysis, as observed
JIP and SJIP respectively. As such interpretation observed in
from tensile strength results, the SIP specimens were shown
the tensile test analysis, in flexural modulus also the same
kind of stiffening of the laminate happens due to this stress
value increasing marginally, and directly proportional to the
modulus. Again, it was clearly understood that, as much as
addition of particulate matter into the matrix, it significantly
induces the stiffness factor and thus increases the modulus
with due respect to the loading of particulate matter35,36.

3.3. Impact strength

The impact strength analyses of various proportions of
particulate loading of TiO2 were shown in the Figure 5. Upon
loading the particulate matter into the IPN blend with the
reinforcement, the impact strength parameters of the IPN
laminate shows phenomenal growth like trend, up to the
level of 5% of addition of particulate matter.
Figure 4. Flexural strength analysis of (a) sisal (b) jute (c) sisal/jute To prove this, the neat IPN laminate shows the impact
fiber reinforced (TiO2) particulate loaded IPN composite. strength value as 27.13, 24.12 and 25.625 kJ/m2 for SIP,
 Investigation of TiO2 Nano Filler in Mechanical, Thermal Behaviour of Sisal/Jute Fiber Reinforced Interpene-
trating Polymer Network (IPN) Composites 7

Figure 5. Impact strength analysis of (a) sisal (b) jute (c) sisal/jute Figure 6. Inter-laminar shear strength analysis of (a) sisal (b) jute (c)
fiber reinforced (TiO2) particulate loaded IPN composite. sisal/jute fiber reinforced (TiO2) particulate loaded IPN composite.

JIP and SJIP respectively. The addition of 1% of particulate their corresponding obtained values were 43.92, 45.13,
into the matrix increases the impact strength value to the 48.11 and 46.52 MPa for 1%, 3%, 5% and 7% respectively.
level of 29.42, 25.91 and 27.665 kJ/m2 for SIP, JIP and SJIP All the specimens showed the gradual propagation of cracks
respectively. The value obtained by the addition of even 1% and delamination upon subjecting with vertical force, in the
of particulate into the matrix had significantly increased to end, losses its stiffness and structural strength before failure
8.44, 7.43 and 7.89% for SIP, JIP and SJIP respectively. occurs. As such value noted in all sets of previous analysis,
In this context, upon loading of particulate into the matrix the 7% particulate loading showed the early fracture as
massively increases the impact strength value with due respect compared with 5% addition of TiO2 addition. Likewise,
to particulate addition. All sets of IPN laminates had shown the JIP also showed the positive trend up to the level of 5%
the same kind of trend line throughout the entire study. In the and their subsequent 7% loading shows the negative trend
same way, the 3% addition of particulates into the matrix of energy absorption, as a proof for this, the obtained values
showed the values of 32.12, 26.99 and 29.55 kJ/m2 for SIP, were 28.42, 30.13, 32.62, 35.74 and 34.91 MPa for 0%, 1%,
JIP and SJIP respectively. Along the way, 5% particulate 3%, 5% and 7% separately. Whereas the SJIP showed the
loading as well showed the values of 34.32, 28.13 and mixture response of SIP and JIP, it shows that the sisal and
31.225 kJ/m2 for SIP, JIP and SJIP correspondingly. But it jute fibers evenly absorbs the stresses and impact energy,
was interesting to note that, to the contrary, the 7% loading depending on their individual strengths and contributes
of particulates showed the decrease in impact strength value. the same energy transfer when hybrid formation happens.
The obtained value of 7% of particulate loading was 32.91, Eventually, it was proved that the 5% of particulate loading
27.32 and 30.115 kJ/m2 SIP, JIP and SJIP respectively. Despite demonstrates the higher level of stress transfer and 7%
the TiO2 loading these specimens had shown the negative particulate addition shows the marginal level of negative
trend of impact strength values. The understandable reason trend due respect to their individual tests38.
was that, the same problem of agglomeration into the matrix,
the same kind of negative trend or fall of strength values were 3.5. Water absorption
also absorbed in tensile and flexural strength upon loading Water absorption behaviour of the sisal, Jute and sisal/
of 7% of particulate. The particulates were not properly jute (hybrid) fiber reinforced TiO2 particulate loaded IPN
distributed throughout the entire matrix due to which, the laminate were thoroughly investigated with respect to various
energy absorption of the laminate had fallen to a marginal intervals. The corresponding graphs were plotted against
level. From the study, again it was clearly understood that water absorption versus square root of no of days as shown
the 5% of particulate loading proves as the optimistic level in the Figures 7, 8, 9.
of incorporation into the matrix material beyond the limit During the initial days of study, from the Figure 7 it was
the laminates show the negative level of energy absorption seen that, the laminate absorbed the water absorption content
and stress transfer37. very rapidly. Moreover, it was clearly seen from the graph
that in between the days of √o to √4 days (during initial
3.4. Short beam shear strength days of immersion) the IPN laminate started to vigorously
The inter-laminar shear strength analyses of various absorb the water absorption content for all sets of particulate
proportions of particulate loading of TiO2 were shown in loaded IPN laminate irrespective of fiber reinforcement.
the Figure 6. The main objective of this study was that to However, it was realized that the 7% particulate loaded IPN
thoroughly analysis the composite resistance against the laminate had absorbed nearly 0.8% to 0.85% of total water
delamination damage. absorption of total weight, as compared with the remaining
During this entire course of study, the SIP specimens set of particulate loaded specimens during the early days.
always held and exhibited higher levels of short beam shear To evident this, From the Figure 8, it was noticed that,
strength as compared with other sets of laminate’s. The neat for the same period of immersion time, the 1%, 3%, 5%
SIP showed the value of 42.14 MPa, upon loading of various and 7% particulate loaded specimens had shown the water
proportionate of particulate into the matrix subsequently absorption rate as 1.3%, 1.25%, 1.1% and 0.9% respectively,
increases their shear strength value up to the level of 5%, whereas the 7% particulate loaded IPN laminate conversely
8 Gopal et al. Materials Research

the absorption rate was conversely negligible and reaches

to the level of almost saturation in √19 days.
From the Figure 9, it was seen that, as much as loading
of particulate matter into the IPN blend, the laminate’s level
of water absorption significantly decreases. This was evident
in all sets of IPN laminate; the 1% particulate into the IPN
laminate decreases its value to the level of 1.21%, 1.31% and
1.26% for SIP, JIP and SIP/JIP respectively. Similarly, the 3%
addition of particulate decreases the value of 1.29%, 1.45%
Figure 7. Water absorption absorption analysis of sisal fiber reinforced
and 1.37% for the corresponding SIP, JIP and SIP/JIP, this
(TiO2) particulate loaded IPN composite. trend has kept advances in all sets of particulate inclusion into
the matrix material. Eventually, the 7% predominantly takes
the minimum water uptake to the level of 1.45%, 1.71% and
1.58% for the same. Actually, the particulate arrests the partial
voids in between the fiber and matrix materials. Apart from
that, most of the natural fibers had the nature of hydrophilic
network, in that initially the water penetrates deep into the
cellulose network of the fibers and through the action of
capillary rise water absorption fills the space between the
fibrils. As well, the rigidity of the cellulose molecule and
structure was partially or completely plasticized because
of the water absorption uptake in turn induces the cellulose
molecules to freely move; due to this most of the cellulose
system was substantially softened and changes the structure
Figure 8. Water absorption analysis of jute fiber reinforced (TiO2) of the fiber easily. From the entire study, it was observed that
particulate loaded IPN composite. as much as addition of the particulate reduces the hydroxyl
group in turn reduces the water absorption uptake to the
notable level and saturates after some quiet interval of time,
irrespective of fiber reinforcement39.

3.6. Fractrography
The sisal, jute and sisal/jute fiber reinforced impact
fractured specimens were subjected to the scanning electron
microscope investigations in order to understand the various
micro and macro failure mechanisms that happened during
the fractured test. During the Fractrographic analysis, it was
clearly understood from the Figure 10 that 3% particulate
loaded specimens had shown better fiber matrix adhesion
Figure 9. Water absorption analysis of sisal/jute fiber reinforced also lessens the void presence on account of adding the
(TiO2) particulate loaded IPN composite. particulate into the matrix material. Common issue of matrix
cracking was observed on all sets of fractured specimens; this
effect predominantly shows the strengthening mechanism
shown the absorption rate as 0.8% which was very less of the matrix due to the addition of particulates into the
amongst all combinations of IPN laminate. Since the IPN IPN composite. Another breakage of fiber scissoring was
blend was incorporated with the combinations of VER and commonly noticed in all jute fiber reinforced particulate loaded
PU, the PU often shows good water resistance as compared specimens. Furthermore, shear cups were also noticed upon
with other types of resins (same class). Though PU resin was the addition of particulate into the IPN matrix, this shear
hydrophobic in nature, when it was mixed with other sets of cups normally enrichens the strengthening factor between
resin material their counterpart blend resins habitually showed the fiber and matrix in significant way and also it was the
smaller variation towards the hydrophobic nature, this was proof for better interfacial adhesion between the fiber and
the reason that the absorption rate of IPN polymer network matrix material40.
possibly changes the absorption rate. Along with that, as the The Figure 11 illustrates the fracture mechanism of the
IPN was blended with the PU, their soft segment presence jute fiber reinforced with various amounts of particulate
generally repels the nonpolar molecules and maintains the loaded fractured specimens. Common finding was that,
hydrophobic nature upon the blend. Another finding from irrespective of fiber reinforcement all sets of IPN laminates
all three sets (a), (b) and (c) laminate was that the absorption showed the fracture on account of fiber pull out. Actually,
rate was drastically slowed down after √4 days. In fact, the the particulate were better circulated over the void presence
sisal, a jute and sisal/jute fiber absorbs the water absorption of the fiber as well on the circumference of the fiber and
content very slowly once their initial rapid absorption creates the substantial adhesion between the fiber and matrix,
period is over. Almost, after remaining √4 days of study, thus the way, it correspondingly increases the better strength
 Investigation of TiO2 Nano Filler in Mechanical, Thermal Behaviour of Sisal/Jute Fiber Reinforced Interpene-
trating Polymer Network (IPN) Composites 9

Figure 10. SEM analysis of sisal fiber reinforced (a) 3% TiO2 (b) 5% TiO2 (c) 7% TiO2 (impact fractured) particulate IPN composite.

Figure 11. SEM analysis of jute fiber reinforced (a) 3% TiO2 (b) 5% TiO2 (c) 7% TiO2 (impact fractured) particulate IPN composite.

on the IPN composites. As much as addition of particulate The Figure 12 elucidates the fracture mechanism of the sisal/
loading increases the better interfacial adhesion among jute fiber reinforced with various amounts of particulate loaded
the IPN composites. Additionally, fiber delamination was fractured specimens. Irrespective of fiber reinforcement all impact
frequently noticed on all the specimens, initially matrices fractured specimens showed the same trend of matrix cracking,
tended to absorb all the forces and transmit the same to the delamination, fiber pull out and scissoring, this was generally
fibers. Once the threshold limit of the laminate exceeds, notified in all the specimens. Potholes were also notified in all
finally it leads to fiber delamination and fiber scissoring41. specimens due to stress concentration on void presence areas.
10 Gopal et al. Materials Research

Figure 12. SEM analysis of sisal/jute fiber reinforced (a) 3% TiO2 (b) 5% TiO2 (c) 7% TiO2 (impact fractured) particulate IPN composite.

The common findings from the fractrographics analysis beam shear strength analysis also showed the hike
were that, as much as addition of particulates into the matrix in strength value as 10.39%. On the contrary, in all
remarkably increases the better interfacial adhesion between the tests, the 5% particulate loaded specimens alone
the fiber and matrix, in turn strength of the composite showed higher strength as compared with all other
increases specifically42-44. specimens. Whereas the 7% addition particulate
shows the negative trend in all the physical tests,
4. Conclusions this was mainly due to the problem of agglomeration
effect in the blends. Particulates could not evenly
The influence of TiO2 nano filler loading on water
distribute into the blend beyond the limit of 5%.
absorption, mechanical, and thermal characteristics of sisal,
3. A water absorption characteristic shows the positive
jute, sisal/jute IPN composite was the prime focus of this
trend in value, as much as addition of particulate
study. The conclusions regarding the same were written
matter into the matrix, it keeps decreases the water
as follows.
1. The thermogravimetric analysis shows that, as much absorption value in agreed level. All the specimens
as addition of TiO2 enhances the glass transition irrespective of fiber reinforcement show the same
temperature of the composite in significant ways. hydrophobic nature upon particulate loading into
As the evidence to showcase this, the 1% particulate the matrix. The variation was observed as 0% - 1.01,
loaded specimen shows the TGA value as 310°C and 7% - 1.45 towards the filler material incorporation
the value progressively increases (5% loaded) up to into the IPNs.
the level of 410°C upon loading of the particulate 4. Nevertheless, fractrography images revealed that,
into the IPN matrix. as much as addition of particulates into the matrix,
2. Also, mechanical properties were shown the better increases the better interfacial adhesion between
enhancement towards loading the particulate matters the fiber and matrix, micro crack bridging through
into the composite. Upon loading the fillers (TiO2) particulates. However, the common mode of failure
into the composite, the tensile strength shows the mechanism like fiber pull-out, interface debonding,
growth level up to (variation from 0% to 7%) fiber breakage and matrix cracking was observed.
20.3%, progressively by adding particulates.
Correspondingly, flexural strength as well shows 5. References
the hike in value by adding particulate into the IPN
1. Eiras D, Pessan LA. Mechanical properties of polypropylene/
matrix, the increase in strength value was notified calcium carbonate nanocomposites. Mater Res. 2009;12(4):517-22.
as (variation from 0% to 7%) 10.6%. Additionally, 2. Eiras D, Pessan LA. Influence of calcium carbonate nanoparticules
impact strength also proves better shock absorption on the crystallization of olypropylene. Mater Res. 2009;12(4):523-7.
characteristics by showing the increase in trend value 3. Souza MA, Pessan LA. Poly(vinyl chloride) (PVC) nanocomposites/
as (variation from 0% to 7%) 50%. Finally the short organophilic clays. Polymers (Basel). 2006;16:257-62.
 Investigation of TiO2 Nano Filler in Mechanical, Thermal Behaviour of Sisal/Jute Fiber Reinforced Interpene-
trating Polymer Network (IPN) Composites 11

4. Oliveira VB, Beatrice CAG, Leal RM No, Silva WB, Pessan LA, Botta 23. Farooq U, Teuwen J, Dransfeld C. Toughening of epoxy
WJ, et al. Hydrogen absorption/desorption behavior of a cold-rolled systems with Interpenetrating Polymer Network (IPN): a review.
tife intermetallic compound. Mater Res. 2021;24(6):e20210204. Polymers (Basel). 2020;12(9):1908. [Link]
[Link] polym12091908.
5. Zepon G, Silva BH, Zlotea C, Botta WJ, Champion Y. 24. Feng Q, Shen M, Zhu J, Li J, Zhang J, Guo S. Realization of
Thermodynamic modelling of hydrogen-multicomponent polyurethane/epoxy interpenetrating polymer networks with a
alloy systems: calculating pressure-composition-temperature broad high-damping temperature range using β-cyclodextrins
diagrams. Acta Mater. 2021;215:117070. as chain extenders. Mater Des. 2021;212:110208. [Link]
6. Wolf W, Bolfarini C, Kiminami CS, Botta WJ. Fabrication of Al‐ org/10.1016/[Link].2021.110208.
matrix composites reinforced with quasicrystals: from metastable 25. Barbezat M, Brunner AJ, Necola A, Rees M, Gasser P, Terrasi
to conventional processing. Mater Res. 2021;36(1):281-97. G. Fracture behavior of GFRP laminates with nanocomposite
7. Karimah A, Ridho MR, Munawar SS, Adi DS, Ismadi, Damayanti epoxy resin matrix. J Compos Mater. 2009;43(9):959-76. http://
R, et al. A review on natural fibers for development of eco- [Link]/10.1177/0021998308100799.
friendly bio-composite: characteristics, and utilizations. J Mater 26. Oliveira FR, Galvão FMF, Nascimento JHO, Silva KKOS,
Res Technol. 2021;13:2442-58. Medeiros JI, Zille A. Photocatalytic properties of sisal fiber
8. Kandola BK, Mistik S, Pornwannachai W, Anand S. Natural coated with nano titanium dioxide. Mat Today: Proceedings.
fibre-reinforced thermoplastic composites from woven- 2015;2:41-8. [Link]
nonwoven textile preforms: mechanical and fire performance 27. Soundararajah QY, Karunaratne BSB, Rajapakse RMG.
study. Compos, Part B Eng. 2018;153:456-64. Mechanical properties of poly(vinyl alcohol) montmorillonite
9. Boopalan M, Niranjanaa M, Umapathy MJ. Study on the nanocomposites. J Compos Mater. 2009;44(3):303-11. http://
mechanical properties and thermal properties of jute and banana [Link]/10.1177/0021998309347040.
fiber reinforced epoxy hybrid composites. Compos, Part B Eng. 28. Mohanty AK, Misra M, Hinrichsen G. Biofibres, biodegradable
2013;51:54-7. polymers and biocomposites: an overview. Macromol Mater
10. Ramesh M, Palanikumar K, Reddy KH. Comparative evaluation Eng. 2000;276-277(1):1-24.
on properties of hybrid glass fiber- sisal/jute reinforced epoxy 29. Koohestani B, Darban AK, Mokhtari P, Yilmaz E, Darezereshki
composites. Procedia Eng. 2013;51:745-50. [Link] E. Comparison of different natural fiber treatments: a literature
org/10.1016/[Link].2013.01.106. review. Int J Environ Sci Technol. 2019;16(1):629-42. https://
11. Ramesh M, Palanikumar K, Reddy KH. Mechanical property [Link]/10.1007/s13762-018-1890-9.
evaluation of sisal–jute–glass fiber reinforced polyester 30. Mishra S, Mohanty AK, Drzal LT, Misra M, Parija S, Nayak
composites. Compos, Part B Eng. 2013;48:1-9. [Link] SK, et al. Studies on mechanical performance of biofiber/glass
org/10.1016/[Link].2012.12.004. reinforced polyester hybrid composites. Compos Sci Technol.
12. Gao C, Fu Q, Huang L, Yan L, Gu G. Jute fiber-reinforced 2003;63(10):1377-85.
polymer tube-confined sisal fiber-reinforced recycled aggregate 31. Nayak RK, Mahato KK, Ray BC. Water absorption behavior,
concrete waste. Polymers (Basel). 2022;14(6):1260. mechanical and thermal properties of nano tio2 enhanced glass
13. Jawaid M, Abdul Khalil HPS, Hassan A, Dungani R, Hadiyane fiber reinforced polymer composites. Compos, Part A Appl Sci
A. Effect of jute fibre loading on tensile and dynamic mechanical Manuf. 2016;90:736-47.
properties of oil palm epoxy composites. Compos, Part B Eng. 32. Sai Krishnan G, Jayakumari LS, Ganesh Babu L, Suresh G.
2013;45(1):619-24. Investigation on the physical, mechanical and tribological
14. Torres FG, Cubillas M. Study of the interfacial properties of natural properties of areca sheath fibers for brake pad applications.
fibre reinforced polyethylene. Polym Test. 2005;24(6):694-8. Mater Res Express. 2019;6(8):085109.
15. Herrera-Franco PJ, Valadez-Gonzalez A. Mechanical properties 33. Suresh G, Jayakumari LS. Analyzing the mechanical behavior
of continuous natural fibre-reinforced polymer composites. of E-glass fibre-reinforced interpenetrating polymer network
Compos, Part A Appl Sci Manuf. 2004;35(3):339-45. composite pipe. J Compos Mater. 2016;50(22):3053-61.
16. Alavudeen A, Rajini N, Karthikeyan S, Thiruchitrambalam 34. Nayak RK, Mahato KK, Routara BC, Ray BC. Evaluation of
M, Venkateshwaren N. Mechanical properties of banana/kenaf mechanical properties of Al2O3 and TiO2 nano filled enhanced
fiber-reinforced hybrid polyester composites: effect of woven glass fiber reinforced polymer composites. J Appl Polym Sci.
fabric and random orientation. Mater Des. 2015;66:246-57. 2016;133(47):497-501.
17. Sydenstricker TH, Mochnaz S, Amico SC. Pull-out and other 35. Suresh G. Analyzing the mechanical behaviour of carbon fiber
evaluations in sisal-reinforced polyester biocomposites. Polym reinforced spur gear with IPN as matrix material. USA: SSRN/
Test. 2003;22(4):375-80. Elsevier Publications; 2019.
18. Ganan P, Cruz J, Garbizu S, Arbelaiz A, Mondragon I. Stem 36. Nayak RK, Mahato KK, Ray BC. Water absorption behavior,
and bunch banana fibers from cultivation wastes: effect of mechanical and thermal properties of nano TiO2 enhanced glass
treatments on physico-chemical behaviour. J Appl Polym Sci. fiber reinforced polymer composites. Compos, Part A Appl Sci
2004;94(4):1489-95. Manuf. 2016;90:736-47.
19. Suresh G, Jayakumari LS. Evaluating the mechanical properties 37. Raghavendra S, Lingaraju, P Balachandra S, Mukunda PG.
of E-Glass fiber/carbon fiber reinforced interpenetrating polymer Mechanical properties of short banana fiber reinforced natural
networks. Polímeros. 2015;25(1):49-57. rubber composites. Int J Innov Res Technol Sci Eng Technol.
20. Gopi S, Loganathan GB, Sekar BK, Krishnamoorthy RK, Sekaran 2013;2(5):1652-55.
V, Mohan AR. Influence of water absorption on glass fibre 38. Venkateshwaran N, Elayaperumal A. Banana fiber reinforced
reinforced IPN composite pipes. Polímeros. 2019;29(3):e2019038. polymer composites a review. J Compos Mater. 2010;29(15):2387-
21. Rathore DK, Prusty RK, Kumar DS, Ray BC. Mechanical 96.
performance of CNTfilled glass fiber/epoxy composite in in- 39. Thipperudrappa S, Hiremath A, Nagaraj BK. Synergistic effect
situ elevated temperature environments emphasizing the role of of ZnO and TiO2 nanoparticles on the thermal stability and
CNT content. Compos Part Appl Sci Manuf. 2016;84:364-76. mechanical properties of glass fiber-reinforced LY556 epoxy
[Link] composites. Polym Compos. 2021;42(9):4831-44. [Link]
22. Chang LN, Chow WS. Accelerated weathering on glass fiber/ org/10.1002/pc.26193.
epoxy/organomontmorillonite nanocomposites. J Compos Mater. 40. Haneefa A, Bindu P, Aravind I, Thomas S. Studies on
2010;44(12):1421-34. [Link] tensile and flexural properties of short banana/glass hybrid
12 Gopal et al. Materials Research

fiber reinforced polystyrene composites. J Compos Mater. 43. Nayak RK, Mahato KK, Routara BC, Ray BC. Evaluation
2008;42(15):1471-89. of mechanical properties of Al2O3 and TiO2 nano filled
41. Suresh G, Vivek S, Ganesh Babu L, Stephen Bernard S, Akash enhanced glass fiber reinforced polymer composites. J Appl
RM, Rajesh Kanna SK, et al. Evaluation of mechanical behaviour Polym Sci. 2016;133(47):44274. [Link]
of carbon fiber reinforced nanoclay filled IPN matrix composite. app.44274.
Mater Res Express. 2019;6(12):125311. 44. Sumesh KR, Kanthavel K. Effect of TiO2 nanofiller in mechanical
42. Devireddy SBR, Biswas S. Physical and thermal properties and free vibration damping behavior of hybrid natural fiber
of unidirectional banana–jute hybrid fiber-reinforced epoxy composites. J Braz Soc Mech Sci Eng. 2020;42(4):211. https://
composites. J Reinf Plast Compos. 2016;35(15):1157-72. [Link]/10.1007/s40430-020-02308-3.