The development of sustainable and innovative products through solving the constantly raising demands of end users is one of the significant parts of research and development. Herein, the development of a green composite is reported with the reinforcement of naturally originated flax and artificial glass woven fabrics through incorporating with the methylene diphenyl diisocyanate (MDI) resin. The glass fabrics were treated with silane and flax fabrics by using NaOH before the composite production to increase the affinity of fibers toward the resin. Composite panels were developed with four different ratios of glass and flax woven fabric reinforcement (100/0, 83.33/16.67, 50/50, and 0/100) to investigate their performance with the MDI resin. The composites were characterized by tensile and flexural analysis to investigate the mechanical performances. The thermogravimetric characteristics of the composites were examined for checking the thermal stability of the produced composites. The surface morphology was investigated for observing the surfaces of the composites before and after applying tensile loads. Scanning electron microscopy (SEM) deployed EDX linear scanning was used for ensuring about the signals of different chemical constituents into the matrix. Fourier transform infrared spectroscopy (FTIR) was conducted for finding out the fingerprint of the chemical elements of the produced composites. Besides, the water absorption and moisture content tests were also conducted to examine the moisture absorption by the pure glass, flax, and hybrid composites. Further, statistical analysis of variances was performed to test the significance of the differences in the mechanical properties of the individual types of the composites developed. For investigating the relationship between the proportion of woven glass fabric in the reinforcement and the mechanical properties, regression analysis was used. The ANOVA test was also examined for checking the significance of the mechanical properties of the composites.
The development of sustainable and innovative products through solving the constantly raising demands of end users is one of the significant parts of research and development. Herein, the development of a green composite is reported with the reinforcement of naturally originated flax and artificial glass woven fabrics through incorporating with the methylene diphenyl diisocyanate (MDI) resin. The glass fabrics were treated with silane and flax fabrics by using NaOH before the composite production to increase the affinity of fibers toward the resin. Composite panels were developed with four different ratios of glass and flax woven fabric reinforcement (100/0, 83.33/16.67, 50/50, and 0/100) to investigate their performance with the MDI resin. The composites were characterized by tensile and flexural analysis to investigate the mechanical performances. The thermogravimetric characteristics of the composites were examined for checking the thermal stability of the produced composites. The surface morphology was investigated for observing the surfaces of the composites before and after applying tensile loads. Scanning electron microscopy (SEM) deployed EDX linear scanning was used for ensuring about the signals of different chemical constituents into the matrix. Fourier transform infrared spectroscopy (FTIR) was conducted for finding out the fingerprint of the chemical elements of the produced composites. Besides, the water absorption and moisture content tests were also conducted to examine the moisture absorption by the pure glass, flax, and hybrid composites. Further, statistical analysis of variances was performed to test the significance of the differences in the mechanical properties of the individual types of the composites developed. For investigating the relationship between the proportion of woven glass fabric in the reinforcement and the mechanical properties, regression analysis was used. The ANOVA test was also examined for checking the significance of the mechanical properties of the composites.
Naturally originated fiber reinforced
composite materials have
drawn significant attention since the last few decades for commercial
applications in the field of automobiles, construction, biomedicine,
packaging, and aerospace.[1] Natural fibers
are showing greater potentiality to reduce the dependency on artificial
fiber-based composites/products in terms of sustainable features.
The composite materials developed from renewable and green natural
fibers are termed as biocomposite, which is also getting more popularity
among the researchers and industrialists nowadays. There are several
plant-based fibers such as flax,[2] hemp,[3] coir,[4] ramie,[5] jute,[6] kenaf,[7] and so forth drawing attention to be potential
raw materials for biocomposite manufacturing. The outstanding features
of natural fibers such as biodegradability, renewability, and recyclability
have made them prominent raw materials in the emerging composite world.[8]Polyurethane (PU)-based resins are derived
from vegetable-/petroleum-based
oils[9] having widespread applications such
as coating materials, adhesives, automotive parts, and different infrastructures.
However, they are more popular for producing durable, lightweight,
and cost-effective composite products.[10] PU is highly compatible with plant-based fibers as the isocyanate
group present in PU interacts with the −OH (hydroxyl group)
of natural fibers.[9,11] Besides, PU also exhibits some
outstanding properties such as zero volatile organic compound emission,
comparatively cheaper price, feasible processing technology, higher
reactivity, and so on.[12] In this regard,
MDI is widely used for particle board productions by manufacturers.
However, it is not yet getting attention for laminated multilayered
hybrid composite productions. Therefore, research studies are needed
to find out novel routes of producing economical and feasible laminated
composite panel manufacturing.Although there are enormous advantages
of using plant fibers, still
there are some limitations for the inherent structural properties.
The polymeric resins are hydrophobic and nonpolar while the natural
fibers contain −OH groups, so they are hydrophilic and polar
in nature.[13] The compatibility problem
hampers the bonding when these two different properties of materials
are mixed together in the polymeric matrix. The mechanical properties
of biocomposites are affected by this kind of incompatibility because
the affinity toward the water is enhanced. The incorporation of synthetic
fibers such as glass or carbon with the natural fibers (such as flax,
hemp, kenaf, coir, jute, and so on) could overcome this challenge.
Kumar et al.[17] have reported that when
the hybrid composites are developed through reinforcing glass with
flax, the tensile strength was increased from 85.6 to 143.21 MPa.
The same study[17] also found a significant
improvement in impact strength and flexural properties of the hybrid
composites. Bajpai et al.[14] described in
another study that the reinforcement of three-layered jute and single-layer
glass with epoxy resin provided the highest flexural strength (107.78
MPa) and impact strength (72.24 J/m), making it useful for safety
helmets in industrial applications.Besides, composites made
from woven fabrics are also getting importance
to the researchers and industrialists for better comfort, dimensional
stability, strength, stiffness, lower fabrication cost, and so on.[15] Glass and flax woven fabrics were selected for
this research. Some studies also revealed that pretreatment of both
the flax and glass fibers could improve the interfacial bonding in
the polymeric composite;[1a,16] so both the flax and
glass woven fabrics were treated with NaOH and silane, respectively,
before producing the hybrid composite. Different percentages of flax
and glass woven fabrics were used as a reinforcement to fabricate
the composites through reinforcing with the MDI matrix. According
to our knowledge, no research studies have been conducted yet on pretreated
flax and glass woven fabric-based laminated composites reinforced
with the MDI polymeric resin. As MDI is used widely in industrial
particle board manufacturing process, we hope our current research
could facilitate the bulk productions of glass/flax reinforced MDI
composites. The mechanical, physical, morphological, thermal, and
statistical analyses have provided significant information on the
produced hybrid composites.
Materials and Methods
Materials
The
flax woven fabrics (article number: LV06506,
density: 230 g/m2, composition: 100% flax, Twill structure)
were purchased from Málitext (Pecs, Hungary). The glass woven
fabric [with a measured density of 255 g/m2, 100% glass,
and plain weave structure (grid size 4.4 × 4.2 mm2)] was procured from Tolnatext located in Tolna, Hungary. The alkaline
NaOH was bought from VWR International Kft. (Debrecen, Hungary) and
vinyltrimethoxysilane, C5H12O3Si
(L#MKBZ5796V, 98%, molecular weight 148.23 g/mol), from Sigma-Aldrich
Co. (St. Luis, MO, USA). The MDI (Ongronat XP-1161) was collected
from Borsodchem Zrt. (Kazincbarcika, Hungary). The hardener (H-240)
was collected from SC Kronospan Sebes SA, Hungary. The hardener (10%)
and MDI (90%) were mixed together to make the adhesive paste for applying
onto the stacked fabric layers into the composite panels. The Formula
Five mold release wax was procured from Novia (Hungary) to use as
a coating material between the composites and Teflon paper to avoid
stickiness of resin with the Teflon.
Methods
Initially,
the flax woven fabrics were pretreated
with 0.5% NaOH solution (the material liquor ratio was 1/20) for 30
min at a temperature of 100 °C to enhance the interaction of
fibers with polymeric resin. The reaction mechanism is shown in equation . The glass fabrics
were treated by vinyltrimethoxysilane at room temperature for 30 min
(the material liquor ratio was 1/10). After the pretreatment, the
fabrics were rinsed and washed three times to remove the alkaline
mucus, vinyltrimethoxysilane solutions, and other impurities from
the surface. The fabric samples were then dried in an oven dryer at
60 °C for 6 min. After that, six layers (Table ) of glass/flax woven fabrics (G1, GF2, GF3,
and F4) coated with MDI resin were stacked up by hand-layup method.
The ratio of MD resin and hardener was 10:1. The sequence of layers
in the laminates were (G,G,G,G,G,G/G,G,F,G,G,G/G,F,G,F,G,F/F,F,F,F,F,F)
with thicknesses of 1.56, 1.9, 2.58, and 3.6 mm for G1, GF2, GF3,
and F4 composites, respectively. The produced laminates were pressed
(3.5 MPa pressure) by a pressing machine for 15 min at room temperature.
Later on, the composites were then cured for 24 h at ambient conditions.
Table 1
Stacking Sequence,
Thickness, and
Density of Developed Hybrid Composites (G1, GF2, GF3, and F4)a
laminates
sequence of
stacking
thickness (mm)
ultimate thickness (mm)
density (kg/m3)
G1 (100% glass)
G,G,G,G,G,G
1.56 (0.012)
1.06 (0.004)
1727.62
(29.01)
GF2 (83.33% glass/16.67% flax)
G,G,F,G,G,G
1.9
(0.005)
1.52 (0.014)
1401.32 (60.28)
GF3 (50% glass/50% flax)
G,F,G,F,G,F
2.58 (0.007)
2.23 (0.007)
1091.53 (146.7)
F4 (100% flax)
F,F,F,F,F,F
3.6 (0.19)
2.51 (0.005)
1195.02 (32.10)
Composites were developed with different
densities and thickness. (Mean values with standard deviations in
parentheses.) G—glass, F—flax.
Composites were developed with different
densities and thickness. (Mean values with standard deviations in
parentheses.) G—glass, F—flax.
Characterization of the Composites
The tensile and
flexural properties of the produced composites were measured by using
the universal testing equipment Instron 4208 (Instron corporation,
USA). The tensile test was conducted as per the EN 310 procedures,
whereas flexural properties were also adopted by the EN 310 standard.
Six samples from each composite were selected for conducting the test.
The FTIR characterization of the composites was performed using a
FTIR-6300 (Jasco, Japan) spectrometer at 4000–500 cm–1. The morphological investigation was performed by using an SEM equipment
(SEM, S 3400N, Hitachi, Japan) at a 15.0 kV voltage within the magnifications
of 2000 times and 1000 times. Thermogravimetric analysis (TGA) and
derivative TG (DTG) analysis were conducted using a Themys thermal
analyzer (Setaram Instrumentation, France) within 25 to 850 °C
at a 10 °C/min temperature gradient under nitrogen (N2) conditioning. The water absorbency was tested at 2, 24, and 240
h time intervals as per the MSZ 13336-4:13379 method, which is a Hungarian
national standard. Samples of 50 mm by 50 mm dimensions were prepared
to execute this test. The composite samples were emerged into 30 mm
depth of water. The moisture content of the composite boards was investigated
in line with the EN 322 methods. The dimensions of the samples were
kept the same (50 mm by 50 mm).
Results and Discussion
Mechanical
Properties of Composites
The tensile properties
of composites are highly influential to assess the strength of the
produced materials. The tensile features of the manufactured composites
(Figure ) are given
in Table . The tensile
strengths of pure glass (G1), glass/flax (GF2 and GF3), and pure flax
(F4) reinforced MDI composites take the values of 78.61 (8.2), 69.63
(2.77), 49.44 (2.05), and 21.19 (1.59) MPa, respectively. While GF2
(hybrid composite) exhibited the highest tensile modulus [7.59 (0.58)
GPa], pure flax reinforced composite exhibited the lowest modulus
and tensile strength too. It is found from Table that synthetic glass reinforced composites
are stronger than naturally originated flax reinforced composites.
However, the laminated composites of glass/flax composites provided
more strength than flax itself. Besides, it is also observed that
the more loading of glass with flax enhances the composite strength.
A similar phenomenon was also described by other researchers for different
designs of fabric stackings (glass/flax)[17] with vinyl ester used as the polymeric resin.
Figure 1
Representation of hybrid
biocomposites: G1 (pure glass composite),
GF2 (hybrid composite from glass/flax), GF3 hybrid composite from
glass/flax, and F4 (pure flax composite).
Table 2
Tensile and Flexural Properties of
Produced Composites (G1, GF2, GF3, and F4)a
laminated composites
tensile
strength (MPa)
Youngs modulus,
E (GPa)
flexural strength
(MPa)
bending modulus, MOE
(GPa)
G1 (100% glass)
78.61 (8.2)
6.82 (0.15)
211.9 (17.9)
54.4 (1.8)
GF2 (75% glass/25% flax)
69.63 (2.77)
7.59 (0.58)
147.7 (18.5)
40.4 (7.8)
GF3 (50% glass/50% flax)
49.44 (2.05)
6.73 (0.52)
58.9 (9.5)
39.9 (4)
F4 (100%
flax)
21.19 (1.59)
2.54 (0.15)
43.9 (3.5)
3.9 (0.8)
coefficient of determinations (R2)
0.66
0.57
0.41
0.89
Pure glass and hybrid composites
exhibited better mechanical performances in contrast to natural flax.
(Means with standard deviations in parentheses.)
Representation of hybrid
biocomposites: G1 (pure glass composite),
GF2 (hybrid composite from glass/flax), GF3 hybrid composite from
glass/flax, and F4 (pure flax composite).Pure glass and hybrid composites
exhibited better mechanical performances in contrast to natural flax.
(Means with standard deviations in parentheses.)The flexural strengths followed
the same trend as the tensile characteristics.
The perceived flexural strengths were 211.9 (17.9), 147.7 (18.5),
58.9 (9.5), and 43.9 (3.5) MPa (Table ), respectively, for G1, GF2, GF3, and F4 composites.
Besides, Youngs modulus followed a similar pattern of flexural strengths
(54.4 (1.8), 40.4 (7.8), 39.9 (4.4), and 3.9 (0.8) MPa). As expected,
naturally originated flax reinforced composites provided the lowest
strengths while those with pure glass reinforcement produced the highest
values. However, the strength values started to increase with the
incorporation of more glass fiber loading into the hybrid composites.[17] Likewise, glass reinforced MDI composites provided
higher bending modulus, with higher tendency to bend without breaking
in contrast to flax reinforced composites.The load versus displacement
behavior of the test pieces is illustrated
in Figure a,b both
for tensile and flexural tests. In the case of tensile displacements,
all the curves showed a linear region initially; a nonlinear region
appeared whenever the cracking happened. Composite G1 attained a load
of approximately 2000 N in the linear range in tension. After exhibiting
a maximum load of around 2650 N at extended delamination, the load
started to decline with the increase of displacement until failure.
The decline of highest load depends on the onset of delamination and
development of cracking in the laminates. In the case of composites
GF2 and GF3, the highest observed loads in the linear range were 1500
and 750 N, respectively. Linearity for F4 ended at 50 N, although
load continued to increase with the increased delamination up to 500
N, then started to drop. In the course of flexural tests, the highest
load attained in the linear range by the composites G1, GF2, GF3,
and F4 was 26, 21, 14, and 7 N, respectively. Similar trends for load
and displacement patterns were also discussed in some other studies.
Figure 2
Load versus
displacement graphs for G1, GF2, GF3, and F4 composites:
(a) tensile test and (b) flexural test.
Load versus
displacement graphs for G1, GF2, GF3, and F4 composites:
(a) tensile test and (b) flexural test.
Statistical Analysis for Mechanical Performances
Regression
analyses of all the composites’ mechanical performances were
conducted in terms of glass fiber proportion in the composites. The R2 values (Table ) for all the composites are higher than 0.57, except
for flexural strength with R2 = 0.41.
It seems that the presence of glass fiber results in higher mechanical
performances of all the composites. The p values for tensile strength
and tensile modulus (Tables –6) stand far less than 0.05 except for flexural strength and
modulus, where the intercept parameter of the regression equation
did not prove to be significant; see the corresponding p values shown
in bold in Tables and 6. These results support the existence
of significant effects of glass fiber proportion on composite properties
with slopes higher for strength than for modulus of elasticity.
Table 3
Regression Analysis for Tensile Strength
in Terms of Glass Fiber Compositions on Different Composites
effects
tensile strength parameter
tensile strength standard error
tensile strength t
tensile strength p
intercept
27.95864
6.970652
4.010908
0.002474
composition
0.43630
0.100053
4.360751
0.001419
Table 6
Regression
Analysis for Flexural Modulus
in Terms of Glass Fiber Compositions on Different Composites
effects
flexural modulus parameter
flexural modulus standard error
flexural modulus t
flexural modulus p
intercept
7.653454
3.642373
2.101228
0.061949
composition
0.470820
0.052280
9.005672
0.000004
Table 5
Regression Analysis for Flexural Strength
in Terms of Glass Fiber Compositions on Different Composites
effects
flexural strength parameter
flexural strength standard error
flexural strength t
flexural strength p
intercept
44.25353
30.57797
1.447236
0.178442
composition
1.16265
0.43890
2.649016
0.024354
The mechanical features of the produced composites
were further
analyzed conducting one-way ANOVA with the type of composites as a
categorical factor. Overall F-tests of significance
for all the four mechanical properties provided evidence of effect
of all the composite types. For pairwise comparisons of the four types,
Newman–Keuls tests (Tables –10) were used because the statistical assumptions
of ANOVA were not always met. These tests showed that the strength
properties of the different composites are significantly different
as the p values are less than the assumed level of significance of
0.05. However, the modulus of elasticity values in two cases shown
in bold in the Tables and 6 do not exhibit the significant difference;
these are tensile modulus values for composites G1 and GF2 as well
as flexural modulus for GF2 and GF3.
Table 7
Newman–Keuls
Test Results for
Tensile Strength in Terms of Different Composites (G1, GF2, GF3, and
F4)
composites
{1}
{2}
{3}
{4}
G1
0.000201
0.003495
0.000231
GF2
0.000201
0.000223
0.000223
GF3
0.003495
0.000223
0.000201
F4
0.000231
0.000223
0.000201
Table 10
Newman–Keuls Test Results
for Flexural Modulus in Terms of Different Composites (G1, GF2, GF3,
and F4)
composites
{1}
{2}
{3}
{4}
G1
0.015094
0.011749
0.000233
GF2
0.015094
0.454250
0.000245
GF3
0.011749
0.454250
0.000250
F4
0.000233
0.000245
0.000250
Morphological Studies of Composites
The SEM photographs clearly exhibit
the uniform
MDI polymer distributions on the respective glass and flax woven fabric
reinforced composites. Although the stacked fibers cannot be observed
in Figure (a2,a3,c2,c3,e2,e3,g2,g3) for strong polymeric overlapping/coating
on the surface but could be clearly seen on the fractured surfaces
of the composites, see Figure (b2,b3,d2,d3,f2,f3,h2,h3). The surfaces
of the composites are flat, smooth, and uniform, which indicates the
perfect bonding of MDI resin with the glass and flax woven fabrics.
However, few holes could also be observed, which is indicating the
weaker adhesion[18] between the fabric and
resin into the matrix system. Such kind of holes were appeared only
for Figure (e2,e3) showing test pieces of 50% flax and 50% glass
with MDI. The surfaces of 100% glass, 100% flax, or 83.33% glass/16.87%
flax reinforced composites did not display any weak adhesion/interactions.
However in the case of Figure ( b2,b3,d2,d3,f2,f3,h2,h3), there are explicit breakage and presence
of fibers (flax and glass marked through red and yellow color, respectively).
Besides, as the glass fabrics were treated with silane, it helped
to form an interpenetrated network between the silane-treated glass
woven fabric and the MDI resin.[19]
Figure 3
Morphological
characterization of hybrid composites (a1,c1,e1,g1) for flexural test samples.
Morphological characterization of fractured hybrid composites (b1,d1,f1,h1) for tensile test
samples. Flat and uniform distribution of MDI resin on composites
with reinforcement of pure glass (a2,a3), hybrid
flax/glass (c2,c3,e2,e3), and pure flax (g2,g3) composites at different
magnifications. Holes appeared for incompatibility between the MDI
resin and woven fabrics (e2,e3). Fractured composites
after applying tensile load on composites with reinforcement of pure
glass (b2,b3), hybrid flax/glass (d2,d3,f2,f3), and pure flax (h2,h3) composites at different magnifications. Holes
for incompatibility between the MDI resin and woven fabrics are presented
through (e2,e3). SEM analysis of composites.
Figure 4
EDX spectrum of the composites (a) G1, (b) GF2, (c) GF3,
and (d)
F4. The presence of glass fiber is observed through the presence of
Si (a–c), while the presence of flax is confirmed by the presence
of C and O (b–d).
Morphological
characterization of hybrid composites (a1,c1,e1,g1) for flexural test samples.
Morphological characterization of fractured hybrid composites (b1,d1,f1,h1) for tensile test
samples. Flat and uniform distribution of MDI resin on composites
with reinforcement of pure glass (a2,a3), hybrid
flax/glass (c2,c3,e2,e3), and pure flax (g2,g3) composites at different
magnifications. Holes appeared for incompatibility between the MDI
resin and woven fabrics (e2,e3). Fractured composites
after applying tensile load on composites with reinforcement of pure
glass (b2,b3), hybrid flax/glass (d2,d3,f2,f3), and pure flax (h2,h3) composites at different magnifications. Holes
for incompatibility between the MDI resin and woven fabrics are presented
through (e2,e3). SEM analysis of composites.EDX spectrum of the composites (a) G1, (b) GF2, (c) GF3,
and (d)
F4. The presence of glass fiber is observed through the presence of
Si (a–c), while the presence of flax is confirmed by the presence
of C and O (b–d).
EDX Analysis of Composites
The energy-dispersive X-ray
(EDX) spectra provide the nature of glass, flax, and polymers embedded
into the matrix. It is clearly observed from Figure that silicon (Si) is one of the most significant
chemical compound indicating the presence of glass into the composite
(Figure a). Besides,
the detection of calcium (Ca), magnesium (Mg), and aluminum (Al) also
confirm the presence of different oxides into the glass woven fabrics
of the composites (Figure a–c). At the same time, the broad peak of C and oxygen
(O) denotes the good bonding of MDI. In the case of pure flax reinforced
composite (Figure d), there is no peak observed for silicon (Si) but there are peaks
for C and O (strong peaks for natural fibers) and chlorine (Cl). On
the contrary, Cl did not show any peaks for G1 composites, while they
are present in the spectra of GF2, GF3, and F4 composites. Presumably,
this difference can be attributed to the presence of flax. The presence
of C and O is detected for all the four composites, which may be an
indication of the bond developed between the woven fabric and the
MDI polymeric resin. Thus, the EDX spectrum confirms the successful
reinforcement of flax and glass with MDI.
FTIR Analysis of Composites
The chemical structures
of MDI-based glass/flax reinforced composites were investigated by
FTIR analysis. The broad absorption bands (Figure d) at 3331 cm–1 indicate
the presence of cellulosic structure (−OH unit) for flax fiber
reinforced MDI composites. Besides, the peaks at 2851 and 2920 cm–1 are related to the existence of CH2 groups
in the fiber. The presence of cellulosic structure in the composite
could be further confirmed by the peaks at 1654 and 1054 cm–1. A similar phenomenon was described by another study.[20] The broad bands ranging from 1017 to 3340 cm–1 (Figure a) represent the glassy material-based composites.[21] Specifically, the peak at 1017 cm–1 is responsible for the Si–O–Si group and 1409
cm–1 for other types of oxides (boron oxide,
aluminum oxide, calcium oxide, and so on), which are the specific
chemical compositions of the glass fiber.[22] There are also a few weaker bonds found at 1654 and 1409
cm–1, which are related to water adsorptions occurring
during the composite manufacturing process.[21] In Figure b,c, the
peaks around 3340 cm–1 may be attributed to the
bonding between the external hydrogen in glassy structures and cellulosic
structures (flax) −OH groups.[23] Besides,
the peaks around 2850 cm–1 (Figure a–c) may be related
to the treatment of glass surface with the silane. Further, the bonding of
MDI with the cellulosic structure is also further confirmed by
the peaks at 1508 cm–1 (CN–H, urethane holding
secondary amide), 1698 cm–1 (carbonyl urethane,
−C=O), and 1228 cm–1 (−C–O–C,
ether urethane) as can be seen in Figure b–d.[24]
Figure 5
FTIR analysis
of composites (G1, GF2, GF3, and F4). (a) Pure glass
composite, (b,c) hybrid composites, and (d) pure flax.
FTIR analysis
of composites (G1, GF2, GF3, and F4). (a) Pure glass
composite, (b,c) hybrid composites, and (d) pure flax.
Thermogravimetric Analysis
The thermal properties of
glass/flax reinforced MDI composites are shown in Figure . Initially, all the composites
except G1 displayed significant weight loss due to moisture evaporation
probably because of the presence of MDI polymer or flax and glass
fibrous material, as shown in Figure a. Weight loss is gradually increasing with the increase
of flax fiber content in the composites. Temperatures belonging to
5% weight loss of the composites are provided in Table . As illustrated in Figure , the maximum weight
losses (10–60%) occurred at temperatures ranging from 315 to
450 °C. Besides, the residues of the composites G1, GF2, GF3,
and F4 were amounted to 87.99, 36.01, 58.78, and 30.82%, respectively.
In summary, it could be stated that the combustion in the case of
glass reinforcement is of lower level than in the case of reinforcements
containing flax. Also, more residues are found for glass as compared
to flax. A similar phenomenon was also described by other studies
on glass with natural fiber-based laminated hybrid composites.[25]
Figure 6
Thermal behavior of composites (G1, GF2, GF3, and F4):
(a) TGA
and (b) DTG. Pure glass and hybrid glass composites are more stable
than natural flax reinforced composite (b–d).
Table 11
Onset and Maximum Temperature of
Hybrid Composites (G1, GF2, GF3, and F4)a
laminated hybrid composites
Tonset (°C)
Tmax (°C)
residues at 650 °C (weight %)
G1
359
650
87.99
GF2
310
650
36.01
GF3
197
650
58.78
F4
162
650
30.82
Glass reinforced composites exhibit
more residues compared to flax and hybrid composites.
Thermal behavior of composites (G1, GF2, GF3, and F4):
(a) TGA
and (b) DTG. Pure glass and hybrid glass composites are more stable
than natural flax reinforced composite (b–d).Glass reinforced composites exhibit
more residues compared to flax and hybrid composites.DTG curves in Figure b, showing some small peaks ranging from
250 to 340 °C, which
are related to the decomposition of organic components of hybrid composites.
The second stage degradation (367–372 °C) is associated
with the hemicellulose decompositions from flax constituents. Cellulose
degradation is indicated by the peaks within the range of 490–582
°C. The variation in temperatures is caused by the different
proportions of glass fiber present in the composite stackings (GF2
and GF3). A similar study was conducted by Atiqah et al.[25c] for thermoplastic polymer-based sugar palm/glass
composites. The DTG curves have clearly displayed the decomposition
pattern of glass/flax reinforced MDI polymeric composites.
Physical
Properties of Composites
The water absorption
by composition of pure flax, glass, and hybrid reinforcement is demonstrated
in Figure a. As expected,
the naturally originated flax reinforced composites exhibited higher
water absorption than reinforced with pure glass. This is because
the natural fibers contain hydrophilic groups (−OH, −COOH,
−CO, and −NH2),[25a] whereas the synthetic glass fibers do not. As a natural fiber, flax
contains enormous amounts of −OH groups (also found by FTIR
analysis). Therefore, the saturation point is higher for flax-based
composites than glass. The saturation point of flax decreases with
the loading of more glass woven fabrics into the hybrid composites.
The sequence is G1 < GF2 < GF3 < F4. The water absorption
was observed from 2, 24, and 240 h as illustrated in Figure a.
Figure 7
Water absorption (a)
and moisture content (b) of composites (G1,
GF2, GF3, and F4) within 2, 24, and 240 h time intervals. Natural
flax reinforced composites absorb more water and exhibit higher moisture
uptake compared to glass reinforced composites.
Water absorption (a)
and moisture content (b) of composites (G1,
GF2, GF3, and F4) within 2, 24, and 240 h time intervals. Natural
flax reinforced composites absorb more water and exhibit higher moisture
uptake compared to glass reinforced composites.The moisture content of pure glass, flax, and hybrid composites
also exhibited the same trend. The G1 (pure glass) sample absorbed
the lowest moisture, whereas F4 (pure flax) attained the highest moisture
content. The hybrid composites (GF2) attained a moisture content of
1.34 (0.32), 1.88 (0.29), and 2.15 (0.09)% after 2, 24, and 240 h,
whereas GF3 showed 3.76 (0.08), 3.84 (0.33), and 3.97 (0.04)% moisture
content within the same time period. Again, standard deviations are
shown in parentheses. It is noticed that the moisture content of flax
reinforced composites starts to decline with the increased loading
of glass woven fabrics.
Conclusions
The fabrication of composites
reinforced by laminated flax and
glass woven fabric with the use of MDI polymeric resin was performed
successfully. The glass woven fabric reinforcement with MDI resin
provided highest flexural and tensile strengths, whereas the flax
reinforced composites showed the lowest performance. However, when
the loading of glass was increased into flax/glass reinforced hybrid
composites, the strengths started to increase. The GF2 sample as a
hybrid composites developed through reinforcing by natural and synthetic
fibers together (83.33% glass and 16.87% flax) provided satisfactory
mechanical performance [tensile strength 69.63 (2.77) MPa and flexural
strength 147.7 (18.5) MPa]. The SEM micrographs also showed flat and
uniform surfaces of the produced composites with homogeneous distribution
of MDI resin into the woven fabric reinforced matrix. The EDX characterization
of the composites confirmed the successful reinforcement of glass
and flax woven fabrics with MDI resin through testifying their footprint
of elemental compositions. The thermogram studies of the produced
composites have proved the satisfactory thermal stability. The addition
of glass on flax/glass hybrid composites also enhanced the thermal
stability. The FTIR analysis provides the fingerprint of glass and
flax fiber presence on the hybrid composites. The water absorption
and moisture content investigation has shown that the natural flax
reinforced composite contains higher moisture than that of pure glass.
However, with the increased incorporation of synthetic glass, both
the water absorption and moisture content started to decline. However,
the incorporation of glass into the composites has significant influence
on tensile strength, tensile modulus, and flexural modulus (regression
analysis). The ANOVA test has further confirmed about the significance
of mechanical properties with the produced composites. The incorporation
of glass into the composites has significant influence on tensile
strength, tensile modulus, flexural strength, and flexural modulus
quantified by regression analysis. The ANOVA test has further confirmed
about the significance of the improvement of mechanical properties
with the produced composites. As MDI is popularly used by particle
board manufacturing companies, this report could be a benchmark for
hybrid composite manufacturing to the industries.
Table 4
Regression Analysis for Tensile Modulus
in Terms of Glass Fiber Compositions on Different Composites
effects
tensile modulus parameter
tensile modulus standard error
tensile modulus t
tensile modulus p
intercept
3.607239
0.771544
4.675349
0.000874
composition
0.040050
0.011074
3.616449
0.004717
Table 8
Newman–Keuls Test Results for
Tensile Modulus in Terms of Different Composites (G1, GF2, GF3, and
F4)
composites
{1}
{2}
{3}
{4}
G1
0.500496
0.000352
0.000201
GF2
0.500496
0.000367
0.000223
GF3
0.000352
0.000367
0.000231
F4
0.000201
0.000223
0.000231
Table 9
Newman–Keuls Test Results for
Flexural Strength in Terms of Different Composites (G1, GF2, GF3,
and F4)