Sugar and tannin contents create problems for better interactions between the lignocellulosic fibers and polymers, hence prior going to composites fabrication the sugar and tannin content test was carried out. Sugar content of the lignocellulosic fiber was 0.3% and tannin content 25%, which are within the range (0.4% tannin content and 0.5% for sugar content (K. Hasan et al., 2020; Tibor L. Alpar- Éva Selmeczi, 2012)). Density of the produced panels were found to have the values by 641.3 (42.59), 644.9 (20.1), 644.9 (20), 656.7 (20.9), and 739.8 (20.1) kg/m3, respectively for 100% lignocellulosic fiber, 5% carbon/ 95% lignocellulosic materials, 10% carbon/ 90% lignocellulosic materials, 15% carbon/ 85% lignocellulosic materials, 20% carbon/ 80% lignocellulosic materials whereas the nominal density was 730 kg/m3 (taken into considerations during recipe formulation). Thickness of the boards were also found for the panels by 9.8 (0.04), 0.1 (0.016), 0.11 (0.016), 0.135 (0.015), and 0.147 (0.005) mm, respectively for 100% lignocellulosic fiber, 5% carbon/ 95% lignocellulosic materials, 10% carbon/ 90% lignocellulosic materials, 15% carbon/ 85% lignocellulosic materials, 20% carbon/ 80% lignocellulosic materials reinforced epoxy composites, whereas the nominal thickness was 10 mm (Table 2). The variation in the thicknesses and densities happened maybe due to the manual operations starting from measurements of the materials as per recipe calculation to composites fabrications and samples preparation for testing of the products. However, the variation in density is found to have declining pattern with the increase in carbon fibers in the composite system. It maybe that lignocellulosic fibers are bulkier compared to carbon fibers; hence the process loss was higher.
Table 2
Mechanical properties of lignocellulosic fiber/carbon fiber reinforced epoxy composites
Panels
|
D
(kg/m3)
|
T
(mm)
|
IBS
(MPa)
|
MOR
(MPa)
|
MOE
(GPa)
|
LE1
|
641.3 (42.59)
|
9.8 (0.04)
|
0.073 (0.005)
|
6.99 (1.2)
|
3.37 (0.52)
|
LE2
|
644.9 (20.1)
|
10.2 (0.15)
|
0.1 (0.016)
|
7.63 (0.43)
|
3.95 (0.22)
|
LE3
|
644.9 (20)
|
10.0 (0.08)
|
0.11 (0.016)
|
7.377 (0.74)
|
4.19 (0.24)
|
LE4
|
656.7 (20.9)
|
9.7 (0.11)
|
0.135 (0.015)
|
7.4 (0.98)
|
4.2 (0.34)
|
LE5
|
739.8 (20.1)
|
9.79 (0.01)
|
0.147 (0.005)
|
7.92 (0.16)
|
4.45 (0.26)
|
*D-Density, T- Thickness, IBS- Internal bonding strength, MOR- Flexural strength, MOE- Modulus of elasticity, EBS- Elongation at break (%), R2- Coefficient of variation |
Mechanical properties of the composite products were investigated further in terms of flexural properties (MOR and MOE) and internal bonding strength. The load versus displacement curves of the internal bonding strength and flexural properties are displayed in Fig. 2 (a and b). The curves shown a linear behavior at initial stage, however, became non-linear behavior after reached to the maximum load. However, the loading conditions causes a crack in the composite test specimens, which is continued with the extended level of displacements. As expected, 100% lignocellulosic fiber reinforced composites needed the lowest load to initiate the crack propagations, whereas the highest loads required by 20% carbon/ 80% lignocellulosic fiber reinforced epoxy resin. The sequence of load needed for crack propagation is LE1< LE2 < LE3 < LE4 <LE5 for the composite samples especially in the case of internal bonding strength. However, the maximum load needed to break the sample 1 is 57.2 N for LE1, 126.3 N for LE2, 199.9 N for LE3, 304.7 N for LE4, and 348.1 N for LE5. The similar consequences also noticed for flexural properties too. Highest loads need to bend the LE1 sample is 84.3 N, LE2 106.4 N for LE3 121.9 N, LE4 123.6 N, and LE5 is 131.6 N. The similar types of load/displacement results were also found for different other lignocellulosic panel products too (K. F. Hasan, Horváth, Kóczán, & Alpár, 2021; K. F. Hasan, P. G. Horváth, Z. Kóczán, M. Bak, & T. Alpár, 2021).
Like load-displacement curves, similar trends also seen for the mechanical properties of the products. 100% lignocellulosic fiber reinforced composites shown the lowest internal bonding strengths by 0.073 (0.005) MPa than that of 20% carbon fiber loaded composites with 80% lignocellulosic fiber by (0.147 (0.005)) MPa in the composite system. The other panels like LE2, LE3, and LE4 shown the intermediate strengths by 0.1 (0.016), 0.11 (0.016), and 0.135 (0.015) MPa, respectively. Additionally, the flexural strengths and modulus also followed the similar pattern of mechanical properties which is increased by the increase in carbon fibers in the composite system. MOR values of the composites were found to have the values by 6.99 (0.2), 7.63 (0.43), 7.377 (0.74), 7.4 (0.98), and 7.92 (0.16) MPa, whereas the MOE values were 3.37 (0.52), 3.95 (0.22), 4.19 (0.24), 4.2 (0.34), and 4.45 (0.26) MPa, respectively for LE1, LE2, LE3, LE4, and LE5 panels. In case of flexural properties, strength and modulus values also increased with the increase in carbon fibers in the composite system whereas 100% lignocellulosic fiber reinforced composites shown the lowest values and 20% carbon fiber loaded composites with 80% lignocellulosic fiber shown the highest performances.
Morphological images of the developed composites are shown Fig. 3. The presence of fibers is observed as uniformly distributed throughout the composite system. The traces of matrix are seen into and around the fibers. A strong bonding among the fibers and epoxy resin is noticed, whereas the 100% lignocellulosic fiber reinforced composites are seeming to have weaker adhesions. Therefore, the fractured samples are easy to separate the fibers from matrix system without any major cracking. However, it was difficult to separate the fibers from matrix as there is a hole created in the composites (5% carbon/ 95% lignocellulosic materials, 10% carbon/ 90% lignocellulosic materials, 15% carbon/ 85% lignocellulosic materials, and 20% carbon/ 80% lignocellulosic materials) when the samples were pulled out during internal bonding strength tests. Therefore, the composites reinforced with carbon fibers showing better internal bonding strength and flexural properties too. Overall, SEM micrographs provided a strong evidence regarding the fiber materials adhesion with epoxy matrix in the composite system. The similar morphological analysis were also reported for flax/ carbon fiber loaded epoxy hybrid composites (Bagheri, El Sawi, Schemitsch, Zdero, & Bougherara, 2013; Dhakal & Sain, 2020).
Additionally, to investigate the chemical elements present in the control materials (both carbon and lignocellulosic fibers) and their associated composites, EDX test was carried out further. As expected, EDX analysis of control lignocellulosic fibers displayed a dominant presence of carbon and oxygen by 49.6 and 40.4%, respectively whereas carbon fibers shown 88.7% carbon, 6.2% oxygen, and 4.9% nitrogen. As carbon is the main chemical compound for both types of control materials, hence their reinforced composites also displayed the dominance in carbon materials compared to others like oxygen and nitrogen. Moreover, the weight% of carbon also starts to increase with the increased loading of carbon fiber in the composite system too. Therefore, the weight% of carbon for 100% lignocellulosic fiber/ epoxy composite was 53.1%, 95% lignocellulosic fiber + 5% carbon fiber/ epoxy composite was 66%, 90% lignocellulosic fiber + 10% carbon fiber/ epoxy composite was 67.4%, 85% lignocellulosic fiber + 15% carbon fiber/ epoxy composite was 68%, and 80% lignocellulosic fiber + 20% carbon fiber/ epoxy composite was 72.6% (Fig. 4).
The reinforcement effects of lignocellulosic and carbon fibers with epoxy resin are investigated further using FTIR analysis for both control and composited products. The broad absorption band between 3600 and 3200 cm− 1 is associated with the stretching vibrations of -OH groups of carbohydrates and lignin. However, there are no such peaks noticed for control carbon fibers within this range (Fig. 5). The peaks within 2880 to 2930 cm− 1 are demonstrating the presence of C-H present in the cellulose and hemicellulose polymers. Control lignocellulosic fiber shown the peak at 3333 cm− 1, whereas composite materials displayed the peak at 3334, 3336, 3334, 3333, and 3333cm− 1. Albeit the control carbon fiber did not show any peak like this at this wavelength like as the cellulosic materials. A shift/stable bands are observed maybe after reinforcement with epoxy resin and carbon fibers. However, these bands are associated with the absorption of water from the surrounding atmosphere, therefore maybe absent from carbon fibers (neat). The similar patterns of lignocellulosic material reinforced composites are also goes in line with previous researches (K. Hasan, P. G. Horváth, Z. Kóczán, M. Bak, & T. Alpár, 2021; K. F. Hasan, P. G. Horváth, Z. Kóczán, M. Bak, et al., 2021). Neat epoxy resin also gives peak at 3364 cm− 1 (Cecen, Seki, Sarikanat, & Tavman, 2008), which can be shifted a bit after the reinforcement with fibers. There is an interaction happens between the -OH groups of the resin and lignocellulosic and the carbon fiber in the composite system. The peaks of the control and composited products are summarized in Table 3. Additionally, -CH stretching vibrations (aliphatic) are noticed within 2800 to 3000 cm− 1 bands (Barbosa et al., 2017; Cecen et al., 2008). However, variations are very little/not significant in the composite products. Interestingly, the formation of bonds between carbon fiber and epoxy resin could be detected by the bonds around 2361 to 2362 cm− 1 wavenumbers (Cecen et al., 2008). Emerging peaks at 895 to 896 cm− 1 are responsible for the C-OH groups due to the β-glycosidic linkages present in the monosaccharides (Cai, Takagi, Nakagaito, Li, & Waterhouse, 2016). The peaks 1028 to 1247 cm-1 are denoted for C = C functional group present both in the control cellulosic fiber and composited products (Rizal, Gopakumar, Thalib, Huzni, & Abdul Khalil, 2018). The stretching vibrations related to carboxylic acid and vinyl esters could be demonstrated by the bands at 1733 to 1734 cm− 1 both for the cases of control cellulosic fiber and composited products (Rizal et al., 2018). Overall, the peaks within 3200 to 3600 cm− 1 and 2361 to 2362 cm− 1 confirms about the successful reinforcements of lignocellulosic/ carbon fibers with epoxy resin.
Table 3
Summarized peak information on FTIR analysis of lignocellulosic/ carbon fiber reinforced epoxy composites
|
Carbon fiber
|
Lignocellulosic fiber
|
LE1
|
LE2
|
LE3
|
LE4
|
LE5
|
-OH group
|
|
3333
|
3334
|
3336
|
3334
|
3333
|
3334
|
-CH stretching vibrations
|
2912
|
2919
|
2921 and 2851
|
2918 and 2851
|
2920 and 2851
|
2919 and 2851
|
2918 and 2851
|
Carbon/epoxy bonding (with/without)
|
2362
|
|
2359
|
2360
|
2361
|
2360
|
2361
|
C-O-C stretching
|
|
1028 and 1241
|
1028 and 1237
|
1029 and 1237
|
1028 and 1241
|
1031 and 1238
|
1029 and 1242
|
C-OH
|
|
896
|
895
|
896
|
895
|
895
|
895
|
C = C
|
1733
|
1734
|
1733
|
1733
|
1733
|
1733
|
1734
|
Compared to all the composites, carbon fiber loaded products displayed the better flame retardancy, whereas 20% carbon fiber incorporated products shown the best stability and 100% lignocellulosic materials displayed the lowest one. The control samples started to burn immediately when exposed to flame. However, the incorporation of carbon fiber in the composite system facilitate to gradually decline this burning tendency (Fig. 6). Generally, wood is prone to be burnt when exposed to flame but conversely carbon fibers exist superior resistance against the fire (Grange et al., 2019). Therefore, as indoor products like furniture items are at a big risk of fire-related burning, hence the use of carbon fiber along with lignocellulosic materials would not only enhance the increased sustainability but also improve the mechanical properties and fire resistance as well (Bartlett, Hadden, & Bisby, 2019). The overall trends of flame retardancy sequence of the composites is LE5 > LE4 > LE3 > LE2 > LE1.
The moisture susceptibility is considered as one of the critical challenges of natural fiber reinforced composites. The reason behind this is the presence of hydrogen bond in fiber cell walls molecules as the plant-based fibers are comprised of dominating cellulosic and hemicellulosic polymers. The cellulosic materials are also composed of -OH (hydroxyl) and C (carbon). However, although cellulose polymer is enriched with crystalline regions which could retard the moisture penetrations, albeit they also contain amorphous regions which facilitates the water molecules to be defused and to break the hydrogen bonds (Moudood, Rahman, Öchsner, Islam, & Francucci, 2019). Therefore, an intermolecular distance is created in the cellulose chains and consequently the fibers are swollen. On the other hand, carbon fiber does not absorb moisture from surrounding environment or absorb water when immersed under the water (Zhai, Feng, Liu, & Li, 2016). Therefore, when the carbon fiber is loaded in the composite system with lignocellulosic materials, the affinity to absorb moisture by the test specimens are decreased. It is seen that (Fig. 7) 100% lignocellulosic materials reinforced composites absorb highest moisture by 3.72 (0.12) % whereas the lowest moisture was absorbed by 20% carbon/ 80% lignocellulosic materials reinforced composites by 3.13 (0.11)% after 2 h of oven drying. The modest moisture was absorbed by 10% carbon/ 90% lignocellulosic materials by 3.38 (0.12)% after the same period of immersion. However, the similar trends of moisture content also noticed even after 24 h of immersion, albeit an increase is observed compared to 2 h for overall moisture absorptions. Interestingly, the similar phenomenon also followed by the composite samples for water absorbency and thickness swelling too. The highest water as absorbed by the 100% lignocellulosic materials reinforced composites too showing the value 14.89 (0.56)% and lowest by 20% carbon/ 80% lignocellulosic materials 12.22 (0.29)% after 2 h of immersion. Moreover, highest thickness swelling was found in case of 100% lignocellulosic materials reinforced composites providing the value 18.97 (0.55)% and lowest one is 14.99 (0.23%) by 20% carbon/ 80% lignocellulosic materials. This phenomenon also agrees with our previous study for glass/flax fiber reinforced with MDI composites (K. F. Hasan, Horváth, & Alpár, 2021b). It seems the physical properties are becoming more stable with the incorporations of carbon fiber in the composite system.