A. A. ANBAN et al.: MECHANICAL BEHAVIOUR OF INFLORESCENCE/GLASS-FIBRE-REINFORCED HYBRID ... 637–643 MECHANICAL BEHAVIOUR OF INFLORESCENCE/GLASS-FIBRE-REINFORCED HYBRID EPOXY COMPOSITES MEHANSKO OBNA[ANJE HIBRIDNEGA EPOKSI KOMPOZITA OJA^ANEGA S KOMBINACIJO NARAVNIH IN STEKLENIH VLAKEN Athithanambi Anna Anban 1* , Manomani Krishnaswamy 2 , Rajesh Appasamy 3 1 Nehru Institute of Engineering and Technology, Coimbatore, Tamil Nadu 2 Government College of Engineering, Tirunelveli, Tamil Nadu 3 Sri Krishna College of Engineering and Technology, Coimbatore, Tamil Nadu Prejem rokopisa – received: 2022-08-03; sprejem za objavo – accepted for publication: 2022-10-07 doi:10.17222/mit.2022.588 The biodegradability and environmental friendliness of natural fibres makes them suitable for implementation in a circular econ- omy. As a result, several natural fibres and processing methods have evolved. The hydrophilic nature of ligno cellulose fibrils restricts the effective adhesion at the interface of fibre and matrix. The hybridization of natural fibres with synthetic fibres leads to promising characteristics of the resulting composite materials. This paper deals with the hybridization of conventional glass fibre and natural fibre extracted from coconut inflorescence. The effect of hybridization on the tensile and flexural strengths of surface-modified inflorescence fibre with glass fibres was investigated. The composites were fabricated using a hand-layup tech- nique by varying the inflorescence fibre and glass-fibre reinforcement composition by (5, 10, 15 and 20) %. A notable improve- ment in the tensile and flexural strengths of 193.65 MPa and 240.69 MPa was observed for 85 % of glass and 15 % of benzoyl-chloride-modified inflorescence-fibre-reinforced hybrid composites. The elimination of amorphous constituents in the inflorescence fibres was checked by XRD and FTIR analyses. A surface-morphology analysis of unmodified and benzoyl-chlo- ride-modified inflorescence fibres revealed pores and cavity formation on the fibril walls. These composites with superior me- chanical properties can be an alternative to synthetic fibre composites and ensure the implementation of a circular economy and sustainable manufacturing. Keywords: inflorescence fibres, hybridization, X-ray diffraction, Fourier-transform infrared, scanning electron microscope V novej{em ~asu je bilo razvitih in izdelanih ve~ vrst procesnih metod za izdelavo kompozitov z oja~itvijo iz naravnih vlaken z namenom ekonomi~nega in kro`nega gospodarjenja za ohranjanje okolja in zmanj{evanje njegove degradacije. Hidrofilna narava ligno-celuloznih vlaken omejuje u~inkovito adhezijo amidov na mejah med vlakni in matrico. Hibridizacija naravnih vlaken s sinteti~nimi vlakni vodi do obetavnih lastnosti izdelanih kompozitnih materialov. V tem ~lanku avtorji opisujejo hibridizacijo konvencionalnih steklenih vlaken z naravnimi vlakni, pridobljenimi iz kokosovih cvetov. Analizirali so u~inek hibridizacije na natezno in upogibno trdnost naravnih vlaken, ki so jih povr{insko modificirali s steklenimi vlakni. Kompozite so izdelali s preprosto ro~no tehniko ter pri tem spreminjali vsebnost naravnih in steklenih vlaken (5, 10, 15 in 20) %. Ugotovili so znatno izbolj{anje natezne in upogibne trdnosti epoksi kompozita (193,65 MPa in 240,69 MPa), ki je vseboval kombinacijo 85 % steklenih in 15 % z benzoil-kloridom modificiranih naravnih vlaken iz kokosovih cvetov. Odstranitev amorfnih sestavin v naravnih vlaknih so potrdili z XRD in FTIR analizami. Analize povr{inske morfologije nemodificiranih in z benzoil-kloridom modificiranih naravnih vlaken so odkrile porozno in jami~asto tvorbo na stenah vlakenc. Opisani kompoziti z odli~nimi mehanskimi lastnostmi so lahko alternativa kompozitom, ki vsebujejo samo sinteti~na vlakna pri zagotavljanju implementacije kro`nega gospodarjenja in trajnostno naravnane proizvodnje. Klju~ne besede: naravna vlakna, hibridizacija, rentgenska difrakcija, spektroskopija na osnovi fourierjeve transformacije infrarde~e svetlobe (FTIR), vrsti~ni elektronski mikroskop (SEM) 1 INTRODUCTION Composite materials are replacing conventional ma- terials owing to their higher specific strength, improved stiffness, decreased weight and better thermal properties. A composite material can be described as a material con- sisting of two or multiple distinct phases in which one is the reinforcement material (known as the load-carrying element) and other is a matrix material. For the past two decades composite materials have been emerging as dominant materials. The application of composite materials is increasing steadily in terms of volume and numbers, finding a prominent place in newer markets. Contemporary composite materials aggregate a momen- tous rate of the engineered materials starting from day-to-day products to highly complicated applications. Over the years, composite materials have been proven to be lower-weight materials, but the present goal is to make them economically viable. The possibility of man- ufacturing composite materials with low cost resulted in innovative fabrication techniques that are currently em- ployed in composite industries. To overcome the cost factors in the development of composite materials there Materiali in tehnologije / Materials and technology 56 (2022) 6, 637–643 637 UDK 620.168.3 ISSN 1580-2949 Original scientific article/Izvirni znanstveni ~lanek MTAEC9, 56(6)637(2022) *Corresponding author's e-mail: aathithanambi@live.com (Athithanambi Anna Anban) must be a unified effort on the design, processing, tool- ing and manufacturing for the composite material to be competitive enough with metals. The business scale of composite materials is found to be promising in all fields compared to aerospace applications. Polymer matrix ma- terials and reinforcement, such as synthetic/natural fibres, have shown a significant result in terms of use and quantity (volume). The behaviour of composite materials can be modified based on the control of design parame- ters. Proper selection of the reinforcement materials re- sults in developed composite materials’ properties that can be customized enough to fit any application. The ma- terials’selection relies on important factors such as prod- uct complexity, operating conditions of the product, and the fabrication skills of the person to achieve the optimal characteristics of the composites. For a better under- standing on the behaviour of the developed composites, it can be used in association with traditional materials. A recent literature survey showed that several works reported by researchers on different natural fibre-rein- forced polymer composites for wide assortment of uses. The survey also covers how natural fibres can be ex- tracted, different surface treatments made on the natural fibres, thereby the resulting natural-fibre-reinforced polymer composite exhibits better mechanical, tribolo- gical and other related properties in comparison to artifi- cial-fibre-fortified polymer composites. The outcome of soluble base execution on the mechanical and other re- lated characteristics of ensete stem fibre fortified with unsaturated polyester matrix showed improvement in the fibre properties. 1 They found that alkali-treated fibres contribute to an improvement in the composite properties in contrast to untreated fibre-reinforced composites. In addition, they found5%ofNaOH treatment resulted in better mechanical characteristics of the ensete stem fibres. The possibility of using Acacia planifrons fibres 2 as a possible reinforcement material with polymer matri- ces was tested. The fibres were extracted by the process of retting. The extracted fibres were subjected to alkali- zation with different percentages of sodium hydroxide. It was found that the alkalization leads to an improvement of the crystallinity index, thermal stability and removal of amorphous substances present in the fibres. The opti- mal alkali treatment was found to be 5 %. The outcome of fibre content over flexural behaviour of malva fibre 3 reinforced with an epoxy matrix was investigated. The composites are manufactured via the compression- moulding technique by assorting the fibre’s volume frac- tion. The flexural behaviour of the composites was found to be good for a 30 % volume fraction of continuous and well aligned malva fibres. The feasibility of using coffee hull 4 as a reinforcement member with high density poly- ethylene matrix revealed it could improve the impact strength of the composites. The mechanical, moisture characteristics of hydrophilic treated jute fibre fortified unsaturated polyester composites 5 revealed composites have a better role to play in different sectors. The silane coupling agent’s influence on the tribological behaviour of corn-stalk-fibre-fortified polymer composites 6 re- vealed an improvement in the hydrophilic tendency of fi- brils. Hybridization in which two or more fibres either syn- thetic/natural fibre or both combined together to improve the mechanical properties of the resulting composites. 7,8 Hybridization of natural fibres with glass fibres offers numerous advantages, like reduced moisture-absorption characteristics 9 of the resulting composites with im- proved tribological characteristics. 10 From the existing literature it is concluded that the hybridization of glass fibre with coconut inflorescence fibres is not yet ex- plored. This has been the motivation for this research work. Based on the extensive literature survey it was found that several natural fibres have been explored and used as an alternate to synthetic fibre that has a prominent role to play in fibre-reinforced polymer composites for a wide variety of application components, ranging from automo- biles to aerospace applications. The application of natu- ral fibrils as reinforcement materials results in compos- ites that are partially or fully degradable in nature. However, the natural fibre extracted from a coconut tree is limited by the application. Thus, there arises a situa- tion in which natural fibre with superior properties is to be identified and extracted from a coconut tree. Therefore, the present research work focusses on the hybridization of inflorescence fibre with glass fibre and epoxy resin as the matrix. Before the hybridization, the inflorescence fibre is to be surface treated with5%of NaOH, KOH, benzoyl chloride solution to remove the amorphous constituents present in the fibres. The un- treated and surface-modified fibres are taken for the manufacturing of hybrid composites. The hybrid com- posites are to be fabricated using the hand layup tech- nique and curing by compression moulding. 2 EXPERIMENTAL PART The coconut tree is a prominent source of natural fi- bre, from which the fibrils are weeded out from the vari- ous elements of the tree. In this investigation, one such part of the coconut tree is identified, which is named in- florescence, 11 shown in Figure 1, and the extracted fibre, as shown in Figure 2, and efforts were made to extract fibre from the inflorescence There are different methods to extract natural fibres from which a process called ret- ting a simple biodegradable treatment of subjecting the fibres by placing it in water for a specific time interval is adopted in this research work. As a result of retting, the outer layers of the coconut inflorescence are softened, and then the fibres can be extracted from coconut inflo- rescence by malleting. The presence of an amorphous substance in the coco- nut inflorescence fibre hinders effective adhesion be- tween the interface of the fibre and the matrix. There- A. A. ANBAN et al.: MECHANICAL BEHAVIOUR OF INFLORESCENCE/GLASS-FIBRE-REINFORCED HYBRID ... 638 Materiali in tehnologije / Materials and technology 56 (2022) 6, 637–643 fore, the inflorescence fibre after extraction is exposed to a surface treatment with 5 % w/v of NaOH, KOH and benzoyl chloride for one hour. Then the fibrils are washed completely with distilled water to separate the chemical contents from the coconut inflorescence fibre. The effect of surface treatment on the fibre’s properties improvement can be inferred from XRD and FTIR analy- ses. Commercially available glass fibre mats, epoxy resin LY556 and hardener HY951 were used for the hybridiza- tion of the glass fibre with coconut inflorescence fibre. Sixteen different composite samples were prepared by varying the coconut inflorescence fibre content of (5, 10, 15 and 20) % for untreated, NaOH-treated, KOH-treated and benzoyl-chloride-treated coconut inflorescence fibres. The fabricated samples were sized as per the ASTM D638 and ASTM D790 standards for tensile and flexural tests. Figure 3 shows the fabricated composite sample. 3 RESULTS AND DISCUSSIONS For the present research work, glass and inflores- cence fibres were reinforced with epoxy matrix for the development of composites. An increasing volume frac- tion of inflorescence fibres was used to analyse the influ- ence on the tensile and flexural strengths. The tensile and flexural strengths recorded for the composite samples are listed in Table 1. Table 1: Tensile and flexural strengths of glass/inflorescence fibre composites Sample No. Fibre type Glass fi- bre (%) Coconut inflores- cence fi- bre (%) Tensile strength (MPa) Flexural strength (MPa) 1 Untreated fibre 95 5 178.84 214.48 2 90 10 174.49 215.14 3 85 15 171.63 218.63 4 80 20 161.21 207.93 5 NaOH treated fibre 95 5 181.32 219.39 6 90 10 179.68 221.65 7 85 15 176.03 224.87 8 80 20 163.74 210.11 9 KOH treated fibre 95 5 183.65 225.97 10 90 10 182.96 228.32 11 85 15 179.68 233.06 12 80 20 169.82 212.86 13 Benzoyl treated fibre 95 5 189.35 231.67 14 90 10 191.64 233.00 15 85 15 193.65 240.69 16 80 20 176.21 219.38 A. A. ANBAN et al.: MECHANICAL BEHAVIOUR OF INFLORESCENCE/GLASS-FIBRE-REINFORCED HYBRID ... Materiali in tehnologije / Materials and technology 56 (2022) 6, 637–643 639 Figure 3: Fabricated glass/inflorescence hybrid composite sample Figure 1: Coconut inflorescence Figure 2: Extracted inflorescence fibre 3.1 FTIR characterization A KBr pellet technique was adopted to characterize the coconut inflorescence fibres subjected to different surface treatments. The wave numbers were varied from 500 cm –1 to 4000 cm –1 . The corresponding functional groups and their elimination can be seen in Figure 4. The wave number 3300 cm –1 corresponds to O–H stretching vibration of hemicellulose, 12 whereas the peak narrow down at 5 % benzoyl chloride which clarifies the elimination of hemicellulose, the peak at 2850 cm –1 cor- responds to C–H symmetrical stretching, 13 the peak dis- appeared in 5 % benzoyl-chloride-treated fibre, which concludes the elimination of lignin and wax constituents. The amorphous peak at 1750 cm –1 relates to carboxyl group stretching vibration 14 , the corresponding peak evaded at 5 % benzoyl-chloride-modified fibre, which concludes the elimination of hemicellulose and lignin. The peak at 1070 cm –1 belongs to the CO–O–CO stretching 15 whereas the disappearance of the peak at 5 % benzoyl chloride fibre confronts the elimination of wax and other oil-covering constituents. The peak at 750 cm –1 corresponds to the C=C bending of alkene, 16 which con- firms the elimination of hemicellulose in coconut inflo- rescence fibres. Finally, from the FTIR characterization studies it is concluded thata5%benzoyl chloride modi- fication has a major influence on the elimination of amorphous substances in the coconut inflorescence fibres. 3.2 XRD characterization X-ray characterization studies were performed on un- treated and alkali-treated inflorescence fibres and re- vealed an increase in the crystallinity size and the index of the fibres. Figure 5 shows the XRD peaks of the un- treated and surface-treated inflorescence fibres. The value of the 2 angle of amorphous and crystallin peaks are mentioned below. The crystalline and amorphous peaks of the untreated fibres were observed at 29.63° and 21.85°, whereas for 5 % benzoyl-chloride-treated fibres the crystalline and amorphous peaks observed at 27.32° and 19.81°. The percentage of crystallin index for the untreated and 5 % benzoyl chloride were found to be 35.6 % and 37.92 %. The cementing materials of inflo- rescence fibres had a greater interaction with the 5 % benzoyl chloride solution, which means the 5 % benzoyl chloride had a prominent effect on the elimination of amorphous constituents. This is the reason behind the in- crease in crystallinity and the swelling of fibres is visible from SEM morphology studies. The benzoylation of coconut inflorescence fibre re- sults in fibre cells rearrangement ahead the direction of A. A. ANBAN et al.: MECHANICAL BEHAVIOUR OF INFLORESCENCE/GLASS-FIBRE-REINFORCED HYBRID ... 640 Materiali in tehnologije / Materials and technology 56 (2022) 6, 637–643 Figure 5: XRD peaks of untreated and surface-treated inflorescence fibres Figure 4: FTIR spectra of untreated and surface-treated inflorescence fibre tensile deformation, which enhances better dispense of the load in the fibre as a result the stress concentration of the fibre reduces. Therefore, the tensile strength of the coconut inflorescence fibre increases. In addition, the di- ameter of the fibre is found to reduce because of the ax- ial splitting of the fibrils. The diameter of the fibre is de- termined using an image analysis technique. As a result of the benzoylation of the coconut inflorescence fibre, the hydroxyl groups present in the fibres are broken down, which further reacts with water molecules and be- comes eroded from the fibre surface. The elimination of hemicellulose, lignin and other functional groups’ exis- tence in the fibrils were tested by the FTIR analysis. The XRD analysis tested that the crystallinity size increases as a result of the orientation change of tightly packed crystalline cellulose structure. Finally, the surface of the fibres becomes cleaner as a result of micro voids’ elimi- nation and also the resistance to moisture and stress transfer among the coconut inflorescence fibre becomes improvised. 3.3 Tensile strength From the tensile-test experiment, it is evident that hy- bridization of inflorescence fibre with glass fibre attrib- uted to an increase in the tensile strength of the compos- ites. A gradual increase in the tensile strength was observed, as shown in Figure 6. The maximum tensile strength of 193.65 MPa was observed for 15 % benzoyl-chloride-treated inflorescence fibre hybridized with glass fibre. A sudden drop in the tensile strength was observed for a 20 % volume fraction of inflores- cence/glass fibre composites. This can be the result of a higher weight percentage of inflorescence fibre in the composites. From the tensile test results it can be con- cluded that 15 % of benzoyl chloride treated inflores- cence fibre contributed to the maximum tensile strength. This can be due to better interfacial adhesion between the glass/inflorescence fibre. The benzoyl-treated fibres enhance the better dispersion of load in the fibre as a re- sult the stress concentration of the fibre reduces, thereby hybridization with glass fibre contributed to the maxi- mum tensile strength. 3.4 Flexural strength Figure shows the flexural strength of glass/inflores- cence-fibre-reinforced hybrid epoxy composites. The flexural strength of the glass/inflorescence-fibre hybrid composites was found to be increasing with an increase in the volume fraction of inflorescence fibre, as shown in Figure 7. An increase in the flexural strength was ob- served for inflorescence fibre volume fractions of (5, 10 and 15) %. When the inflorescence fibre volume fraction is increased to 20 % a sudden drop in the flexural strength was observed, like with the tensile strength re- sults. The maximum flexural strength of 240.69 MPa was observed for 15 % reinforced inflorescence fibre hy- bridized with 85 % of glass fibre. The phenomenon can be governed by benzoylation of inflorescence fibre, which makes the surface of the fibres cleaner as a result of the micro voids’ elimination and also the resistance to A. A. ANBAN et al.: MECHANICAL BEHAVIOUR OF INFLORESCENCE/GLASS-FIBRE-REINFORCED HYBRID ... Materiali in tehnologije / Materials and technology 56 (2022) 6, 637–643 641 Figure 7: Flexural strength of hybrid glass/inflorescence-fibre-rein- forced epoxy composites Figure 6: Tensile strength of hybrid glass/inflorescence-fibre-rein- forced epoxy composites Figure 8: Untreated fibre moisture and the stress transfer among the coconut inflo- rescence fibre is improved. 3.5 SEM characterization The surface morphology of untreated and 5 % benzoyl-chloride-modified inflorescence fibres was ex- amined using scanning electron microscope, which is shown in Figures 8 and 9. The surface of the untreated inflorescence fibres was nonporous and the absence of any cavity were recorded. The 5 % benzoyl-chlo- ride-modified inflorescence fibres revealed the surfaces of the fibres were more porous and cavities were ob- served on the surface. Thereby during reinforcement with epoxy matrix contributed to maximum tensile strength for 15 % benzoyl chloride modified coconut in- florescence fibres. 4 CONCLUSIONS Coconut inflorescence fibres and glass-fibre-rein- forced hybrid composites were fabricated using a hand lay-up technique and cured by compression moulding. The inflorescence before reinforcement were surface treated with 5 % w/v of NaOH, KOH and benzoyl chlo- ride. The extensive experimentation draws the following conclusions: 1) Among the surface treatments, benzoyl chloride has a prominent effect on the removal of amorphous con- stituents existing in the inflorescence fibres. Benzoyl chloride modification contributes to a better load distri- bution along the tensile deformation direction, as a result the tensile strength of the inflorescence fibre increases. 2) X-ray diffraction of benzoyl-chloride-modified in- florescence fibres revealed an increase in the crystallinity size and index of the fibres. 3) Fourier-transform infrared spectroscopy analysis of the benzoyl-chloride-modified inflorescence fibres re- vealed the elimination of amorphous constituents present in the fibres. 4) A maximum tensile strength of 193.65 MPa was observed for a 15 % reinforced benzoyl-chloride-modi- fied inflorescence fibre hybridized with glass fibre. 5) A maximum flexural strength of 240.69 MPa was observed for a 15 % reinforced benzoyl-chloride-modi- fied inflorescence fibre hybridized with glass fibre. 6) A scanning electron microscope analysis of un- modified and benzoyl-chloride-modified inflorescence fibre revealed surface-modified fibres were porous, and cavities were observed, which contributed to better inter- facial bonding during reinforcement with glass and ep- oxy matrix. 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