# Multiresponse Optimization of Mechanical Behaviour of Calotropis gigantea/Nano-Silicon-Based Hybrid Nanocomposites under Cryogenic Environment

Authors: Muruganantham Ponnusamy; L. Natrayan; Pravin P. Patil; G. Velmurugan; Subash Thanappan
Journal: Adsorption Science & Technology
 (2022)

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## Abstract

The utilization of natural fibre-based biodegradable polymers has expanded in the present circumstances since natural fibres are relatively inexpensive, recyclable, lighter, nonflammable, and harmless. However, hydrophilic nature is the most serious issue. To address this issue, the current study was applied to enhance the material characteristics of hybrid composites strengthened by CGF and nanosilica powder. To accomplish the mentioned goal, RSM calculated and optimized the following processing parameters using the BBD arrangement at various CGF fibre thickness (gsm), weight percent of nanosilica powder (wt. percent), and cryogenic treatment period (min). To prevent hydrophilic nature, the fibres were pretreated for four hours with a 5% alkaline solution. Deterioration models were created to analyze the material characteristics, and the optimal progression variables were determined. Based on the multiresponse surface methodology, the governable process variables for nano-silica- and CGF-based hybrid nanocomposites should be set at 3% silica, 300 gsm of CGF, and 30 minutes of cryogenic treatment. The tension, bending, and impact property correlation coefficient values (R2) are 0.95, 0.94, and 0.95, respectively. The above-mentioned combinations provide better water absorption and mechanical strength.


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## Body

## 1. Introduction

Nowadays, natural fibre-based composite materials have increased attention. Because of their good mechanical properties, flexibility, and lightweight, lignocellulosic fibres such as wood fibres, nonwoody fibres, and agricultural waste are commonly employed to support various thermoplastics and thermoset polymers [1]. Unlike common engineering fibres like carbon fibres and mineral additions (fillers), lignocellulosic fibres can impart advantages to the composites, including no health concerns, reduced machinery wear throughout production, and a greater level of flexibility than mineral fillers. This is true since, unlike glass fibres, these fibres will flex rather than rupture in preparation. The world consumption of wood pulp is increasing, whereas the supply of this resource is decreasing [2]. As a result of this circumstance, alternative lignocellulosic materials are being developed. Nonwoods are a significant alternative supply of composite materials for the 21st decade. They are a major fibre material in areas with limited woodland possessions and will endure showing a significant part in such areas [3]. Several nonwood plant fibres can be employed; however, most renewable energy sources are underutilized. Calotropis gigantea, called mudar or milkweed, is a wilderness plant yet to be industrially utilized.Calotropis is a member of the Asclepiadaceae family, which has 270 genera and 2500 species with a worldwide spread that would be most numerous in the subtropics and tropical and uncommon in colder nations [4]. That shrub is a spongy, deciduous, herbaceous perennial with soft leaves. It contains a few stems, a few limbs, and a few leaves, which are largely focused on the developing point. Mudar is a medium-sized shrubbery that grows to a height of 2 to 3 m and has a stem diameter of 26 cm. The plant can grow in an arid environment (150–1000 mm rainfall) and occasionally in too drained sandy in places with up to 2000 mm of seasonal rainfall. Presented with a severe scarcity of forest products in Iranian, scientific research and industrial growth are looking for alternative resources of cellulosic fibres [5], although there could be some research on mudar as an underutilized cellulose fibres for fibre-reinforced composites in the past [6]. The important condition for the long-term use of cellulosic sources like mudar is a comprehensive description of their chemical components, fibre shape, and unique properties in comparison to other natural resources. The morphological characteristics and chemical characteristics have a significant impact on the use. As a result, those qualities are critical as in technical issues concerned. In this research, plant bast fibre derived from Calotropis gigantea is used as strengthener for composite materials. Bast fibre is a group of fibres generated from the external film lockups of different shrub shoots. Indeed, this was inspired by the study of Ganeshan et al. [7]. They investigated the appropriateness of CG stem fibres as prospective reinforcements for biocomposites using morphological analyses such as crystallinity, shape, and spectrophotometric characteristics. Several bast fibres, like flax, jute, and sisal, are used in advanced applications for manufacturing composites [8]. Ashori and Bahreini [9] assessed the chemical components of CG bark and seed fibre for usefulness as a natural resource in composites. Retrieved Calotropis gigantea bark fibres contain 24% alkaline compounds, 58% cellulosic components, 17% hemicelluloses, and 16% lignin. The alkaline treatment would have two significant effects on natural textiles. (1) It enhances the exterior quality of the fibre, improving structural adhesion between all fibres and matrix; and (2) it upsurges the quantity of roughage visible on the fibre’s exterior, thereby increasing the potential reactants.Fernandes et al. [10] handled coir fibres in various NaOH concentrations (5% and 10%) and found that when the fibres are treated in 5% sodium hydroxide solutions, considerable solubilization occurs. Joshi et al. [11] investigated the material characteristic of sisal-based composites with 1, 3, 5, and 7% NaOH accumulation, and the results reported that 5% NaOH-treated composite has the highest tensile strength. Prajapati and Gupta [12] investigated the effects of composites made from kenaf fibre treated with NaOH (5, 10, and 15%) and found that at 5% NaOH treatment, composite tensile strength, flexural strength, and impact strength all improved by 13%, 14%, and 30%, respectively. When the concentrations of NaOH rise, unfavourable outcomes occur. Due to crystalline formation, the fibres become stiff and brittle due to the high concentrations, resulting in high resistance and limited expandability. When stressed, these fabrics shrank further due to increased brittleness, and they could not properly transmit load at the interfaces, lowering the material’s characteristics. As a result, in the current study, NaOH concentrations of 5% were used.On the other hand, natural materials possess poor mechanical properties like compression and flexibility. By way of an outcome, employing usual fibre unaided in a polymeric matrix is inadequate to fulfil all of the practical necessities for biodegradable polymer reinforcements [13]. As a consequence, our present goal is to progress unique mixture composites. Various characteristics influence composite toughness, such as fibre orientation, fibre content ratio, and a direct connection between the fibre and the matrix [14]. Polymeric materials are more prone to failure when mechanical loads, including compression and bending stresses, are applied. Asadi et al. [15] conducted a mechanical and physical investigation of fibre glass incorporated silica filter-based epoxy materials. They observed that glass fibre with a 25% concentration and nanosilica with a 3% concentration had better mechanical qualities than other weight percentages. The addition of nanosilica to glass fibre increases its properties. Nanofiller inclusion into matrices is a vital phase in manufacturing nanocomposite; there are numerous techniques, including shear mixing, mechanical churning, and ultrasonicating. Shear mixing demands the employment of two or four mills when the resins and nanomaterials are exposed to significant shear pressures [16, 17]. However, that technology has the problem of having a limited resin supply in the mills. Cavity creation is also aided by mechanical churning. Before ultrasonically mixing the nanofillers, they must first be mechanically mixed. Compared to the separate data, the combined findings have good mechanical properties [18, 19]. The most widely used method, ultrasonication, has already demonstrated significant promise in disintegrating particulate groupings and increasing solution uniformity [20]. Ultrasonic dispensation is utilized for various applications, like nanoemulsion in ignoble fluids, particle deaggregation, particulate magnitude drop, particulate mix and residue, and superficial functionality [21]. Ultrasonic radiation disperses particles in polymer binders because high-frequency waves may be transported over small packages. As the sonication time grows, such little packages of nanofillers gradually exfoliate into smoothly decreasing bundles and finally become entirely distributed as single nanofillers in the polymers [22, 23]. Cryogenic properties can improve the mechanical possessions of fibre-based organic materials. For occurrence, sources utilized in aviation structure must tolerate high heating or cooling rate of up to 200°C. Cryogenically treated composites and polymers have great strength, are more robust, and have increased stiffness and wearing confrontation. Consequently, fluid N2 treatment of materials may be an essential part of current research and development to improve organic resource-based composite material properties [24]. The Box-Behnken design (BBD) is regarded as an investigational strategy by RSM. RSM was used to gather arithmetical and scientific methodologies for emerging, enlightening, and analysing the processing variables. It is a multilayered hypersurface method for defining and visualizing the impactness of variables and their relationship among outcomes and controlled input parameters that influence productivities. BBD has a substantial benefit since it does not comprise mixtures in which all rudiments are simultaneously at their uppermost or lowermost standards. Moreover, the BBD is frequently employed in manufacturing because it was a low-cost statistical method with lone three stages for every constituent [25, 26].There have been no studies highlighting the usage of RSM and performance criteria in the fabrication of composites using CGF and nanosilica under a cryogenic environment (77 K). The author claimed it is the first research to analyze natural materials using interlaced CGF as reinforcing materials and nanosilica as additive fillers in the epoxy matrix under liquid nitrogen, highlighting the current work’s new element. The findings of this study are likely to approach new uses for organic fibre composite at extremely low temperatures. For the primary goal, the impacts of low temperature on the composite and chemical modifications on mechanical characteristics of Calotropis gigantea fibre were examined. The BBD statistics with the RSM method were utilized to accomplish the mentioned objective. Table1 shows the mechanical possessions of CG fibres and resin.Table 1
Mechanical belongings of CGF and epoxy resin.
Sl. noPropertiesCGF fibreEpoxy resin1Cellulose (%)76-77.9—2Hemi cellulose (%)57-58.2—3Lignin (%)18-19.20—4Density (g/cm3)1.3601.155Tensile strength (MPa)460-89029.5-31.256Young’s modulus (GPa)53-613.17Elongation (%)1.5-1.91.6


## 2. Experimental

### 2.1. Resources

Calotropis gigantea (CGF) is a South Asian shrub in India, Thailand, and Malaysia. To remove fibres from the plant’s stem bark, retting is employed. It is first divided into little strands up to a meter long and then weaved into a mat. CGF fibres and other reinforcements were collected in the GVR fibre factory in Madurai, Tamil Nadu, India. Naga chemical factory, Chennai, Tamil Nadu, India, supplied nanosilica powders for conventional pallets. Figure1 shows the reinforcement, filler, and matrix materials used in this research.Figure 1
The photographic images of Calotropis gigantea fibre, nano-SiO2, and epoxy matrix.


### 2.2. NaOH Processing

To remove the undesirable interference, the CG fibres would be washed independently at 65 to 70°C for 60 minutes using 1.5 to 3% washing mixtures, and then, they would be cleaned using purified water and dried in a drying oven at 60°C for 90 minutes, according to the described procedure [27]. The cleansed fibres were again immersed in 5 percentage sodium hydroxide solutions for four hours at 35°C. To get alkali-treated fibres, the strands were thoroughly cleansed with purified water or dried in the atmosphere.


### 2.3. Fabrication of Composites

In the first step, nanosilica and epoxy were blended for 15 minutes utilizing a mechanical churning process to integrate matrices and fillers. The ultrasonicator is then used to disseminate the filler into the matrix using ultrasonic vibrations. Several weight proportions of nanosilica filler loading were used to make a nanocomposite, such as 1.5, 3, and 4.5 wt.%. The nanosized silica and epoxy mixture was placed in a glass pipette, physically agitated, and kept in an elevated ultrasonic bath on pulse mode for 45 minutes.After the procedure, compression moulding was employed to manufacture CGF-/nano-silica-based hybrid composites. The composite specimen was created following the levels and parameters specified. The previously made epoxy/nanosilica mixture was then placed in the mould. The basic exterior was glued until the leftover adhesive was absorbed. Then, using an additional resin/nanosilica combination, more layers were created till showery. The same method was repeated until the entire fold was finished. Using a mechanical rolling element, the specimen was violently crushed to a width of around 3 mm. According to the ASTM standard, the hybrid nanocomposite specimens were cured at atmospheric conditions for a whole day before being sliced into an adequate dimension for mechanical testing. The composite parameters and their stages are shown in Table2.Table 2
Constrains and their stages for nanocomposite.
Sl. noConstrainsSymbolsStagesS1S2S31CGF fibre thickness (gsm)A2002503002Nano silica (wt.%)B1.534.53Cryogenic treatment (min)C153045


### 2.4. Cryogenic Treatment

The cryogenic healing was conducted in a controlled heat-based liquid nitrogen compartment with programmed controls. A regulated cooling rate (3°C/min) was used to get the temperature down to 196°C. The produced specimens were subsequently flooded in liquid N2 at 77 K for cryogenic healing for 15 minutes, 30 minutes, and 40 minutes, respectively, as per the design plans. After the processing, the composites were reheated at a continuous rate of 45°C/h to return to room temperature.


### 2.5. Design of Experimentation

RSM is a method for assessing the links between a collection of controllable variables and the difference between their results. One must first know the mechanism before you can even construct a statistical method. The approach has been well discussed [28, 29]. Performing technically prepared experiments, anticipating the characteristics in a rational approach, projecting the answers, and validating the model’s suitability are also the three main aspects of this optimization problem. Important aspects like pressure, duration, and temperatures were identified as critical and assigned the numerals X1, X2, and X3. Table 2 shows every parameter’s low, medium, and high standards, denoted by the letters -, 0, and +, respectively. Multiregression examination with the least squares method was utilized for intention.
(1)i=yi−y0∆y,wherei=1,2,3.Yi is now a coding value of conscience components, yi is really the true value of a conscience integration on the median, and y is the conscience variable adjustment criteria in the preceding formulas. In the BBD, a cluster of dots exist at the median of each border as well as the replicated middle of the volumetric box. All experiments were run 3 times, and the mean of the operation condition yield was taken as the result. The quadratic equation (2) could be used to express the direct proportionality of the reaction on these variables in an organisation having three primary conscience components, X1, X2, and X3.
(2)X=∂0+∂1Z1+∂2Z2+∂3Z3+∂11Z12+∂22Z22+∂33Z32+∂12Z1Z2+∂13Z1Z3+∂23Z2Z3+∈.The correlation criterionR2 was being used to characterise the similarity of a quadratic operation strategy. The crystallisation of a polypropylene utilized in this study is being used to regulate the quantities of CGF thickness, nanosilica, and cryo treatment. Multiple linear regression yields the variables, and the result must be used to determine the results. The level of randomization for this study was chosen as Box-Behnken, a factorial arrangement with three elements [30].


### 2.6. Testing of Composite Specimen

The fabricated composite specimens were cut to the ASTM standard of D 638-03 replicas with a measurement of150×15×3 mm for tensile testing, ASTM D-790 (width 10 mm, length 125 mm, and thickness 3 mm) for flexural testing, and ASTM D-256 (width 12.7 mm, length 64 mm, and thickness 3 mm) for impact strength.


## 2.1. Resources

Calotropis gigantea (CGF) is a South Asian shrub in India, Thailand, and Malaysia. To remove fibres from the plant’s stem bark, retting is employed. It is first divided into little strands up to a meter long and then weaved into a mat. CGF fibres and other reinforcements were collected in the GVR fibre factory in Madurai, Tamil Nadu, India. Naga chemical factory, Chennai, Tamil Nadu, India, supplied nanosilica powders for conventional pallets. Figure1 shows the reinforcement, filler, and matrix materials used in this research.Figure 1
The photographic images of Calotropis gigantea fibre, nano-SiO2, and epoxy matrix.


## 2.2. NaOH Processing

To remove the undesirable interference, the CG fibres would be washed independently at 65 to 70°C for 60 minutes using 1.5 to 3% washing mixtures, and then, they would be cleaned using purified water and dried in a drying oven at 60°C for 90 minutes, according to the described procedure [27]. The cleansed fibres were again immersed in 5 percentage sodium hydroxide solutions for four hours at 35°C. To get alkali-treated fibres, the strands were thoroughly cleansed with purified water or dried in the atmosphere.


## 2.3. Fabrication of Composites

In the first step, nanosilica and epoxy were blended for 15 minutes utilizing a mechanical churning process to integrate matrices and fillers. The ultrasonicator is then used to disseminate the filler into the matrix using ultrasonic vibrations. Several weight proportions of nanosilica filler loading were used to make a nanocomposite, such as 1.5, 3, and 4.5 wt.%. The nanosized silica and epoxy mixture was placed in a glass pipette, physically agitated, and kept in an elevated ultrasonic bath on pulse mode for 45 minutes.After the procedure, compression moulding was employed to manufacture CGF-/nano-silica-based hybrid composites. The composite specimen was created following the levels and parameters specified. The previously made epoxy/nanosilica mixture was then placed in the mould. The basic exterior was glued until the leftover adhesive was absorbed. Then, using an additional resin/nanosilica combination, more layers were created till showery. The same method was repeated until the entire fold was finished. Using a mechanical rolling element, the specimen was violently crushed to a width of around 3 mm. According to the ASTM standard, the hybrid nanocomposite specimens were cured at atmospheric conditions for a whole day before being sliced into an adequate dimension for mechanical testing. The composite parameters and their stages are shown in Table2.Table 2
Constrains and their stages for nanocomposite.
Sl. noConstrainsSymbolsStagesS1S2S31CGF fibre thickness (gsm)A2002503002Nano silica (wt.%)B1.534.53Cryogenic treatment (min)C153045


## 2.4. Cryogenic Treatment

The cryogenic healing was conducted in a controlled heat-based liquid nitrogen compartment with programmed controls. A regulated cooling rate (3°C/min) was used to get the temperature down to 196°C. The produced specimens were subsequently flooded in liquid N2 at 77 K for cryogenic healing for 15 minutes, 30 minutes, and 40 minutes, respectively, as per the design plans. After the processing, the composites were reheated at a continuous rate of 45°C/h to return to room temperature.


## 2.5. Design of Experimentation

RSM is a method for assessing the links between a collection of controllable variables and the difference between their results. One must first know the mechanism before you can even construct a statistical method. The approach has been well discussed [28, 29]. Performing technically prepared experiments, anticipating the characteristics in a rational approach, projecting the answers, and validating the model’s suitability are also the three main aspects of this optimization problem. Important aspects like pressure, duration, and temperatures were identified as critical and assigned the numerals X1, X2, and X3. Table 2 shows every parameter’s low, medium, and high standards, denoted by the letters -, 0, and +, respectively. Multiregression examination with the least squares method was utilized for intention.
(1)i=yi−y0∆y,wherei=1,2,3.Yi is now a coding value of conscience components, yi is really the true value of a conscience integration on the median, and y is the conscience variable adjustment criteria in the preceding formulas. In the BBD, a cluster of dots exist at the median of each border as well as the replicated middle of the volumetric box. All experiments were run 3 times, and the mean of the operation condition yield was taken as the result. The quadratic equation (2) could be used to express the direct proportionality of the reaction on these variables in an organisation having three primary conscience components, X1, X2, and X3.
(2)X=∂0+∂1Z1+∂2Z2+∂3Z3+∂11Z12+∂22Z22+∂33Z32+∂12Z1Z2+∂13Z1Z3+∂23Z2Z3+∈.The correlation criterionR2 was being used to characterise the similarity of a quadratic operation strategy. The crystallisation of a polypropylene utilized in this study is being used to regulate the quantities of CGF thickness, nanosilica, and cryo treatment. Multiple linear regression yields the variables, and the result must be used to determine the results. The level of randomization for this study was chosen as Box-Behnken, a factorial arrangement with three elements [30].


## 2.6. Testing of Composite Specimen

The fabricated composite specimens were cut to the ASTM standard of D 638-03 replicas with a measurement of150×15×3 mm for tensile testing, ASTM D-790 (width 10 mm, length 125 mm, and thickness 3 mm) for flexural testing, and ASTM D-256 (width 12.7 mm, length 64 mm, and thickness 3 mm) for impact strength.


## 3. Result and Discussion

The next segment briefly discusses the mechanical characteristics of epoxy composite, such as bending, tension, and impacting properties, based on their process variables.


### 3.1. Effect of CGF Fibre

Figure2 shows the effect of fibre thickness (gsm) on mechanical possessions like tension, bending, and impact strength of CGF- and nano-silica-based hybrid epoxy composites. Figure 2 shows the greatest tensile of 43.65 MPa, flexural of 64.23 MPa, and impact strength of 35.65 kg/m2. Compared to 200 gsm and 250 gsm, CGF fibre with 300 gsm has the best mechanical characteristics. The poor transfer of load owing to the irregular distribution of fibres across the matrix is the cause of the low performance at the 200 gsm composite structure. As a result, a matrix-rich area emerged in the composite, with poor fibre-to-fibre coupling. The fibre reinforcement was easily pulled out of the matrix when loaded in this state. It demonstrates that the CGF fibre composite’s 200 gsm reinforcing effect is insufficient to bear the mechanical load. The mechanical characteristics of the composite progress when the fibre proportions are raised from 200 gsm to 300 gsm. This is mostly owing to the development of good bonding among matrix and their reinforcement, which resulted from the fibres’ creating no gaps in the composite by accommodating more short fibres and ensuring good load sharing between them [19]. As the fibre content grew, the interaction between the fibre and matrix improved. As a result, greater energy is required to interrupt the interwoven fibre bundles’ connection. Figure 3 shows the surface plot of hybrid composites concerning CGF fibre thickness.Figure 2
Mean values of tension, bending, and impact strength of hybrid composites based on CGF fibre thickness.Figure 3
Surface plot of different CGF nanocomposites. (a) Tension, (b) bending, and (c) impact properties.
(a)(b)(c)


### 3.2. Effect of Filler Additions

Figure4 shows nanosilica filler additions’ tensile, flexural, and impact properties. Compared to 1.5 wt.% and 3 wt.% of nanosilica, 4.5 wt.% of silica additions revealed better mechanical strength. The increased mechanical characteristics of nanosilica in resin at a concentration of 3 wt.% might be attributed to improved stress distribution and transmission. Adding more filled silica to the epoxy matrix increased the conveyance and size of holes, influencing the decohesion closeness among the reinforcement and the resin [31]. Consequently, the epoxy, woven CGF, and silica formulations offer sufficient adhesion binding among surface adhesions at a concentration of 3 wt.%. Adding 1.5 and 4.5 wt.% silica, on the other hand, produced a negative result, signifying a decrease in mechanical strength. Furthermore, heavier and lighter loadings of 1.5 wt.% and 4.5 wt.% have been shown to have poor boundary adherence of fibre and matrix in woven CGF and epoxy, resulting in aggregation due to poor adhesion and inferior composite strength qualities [6]. Figure 5 shows the surface plot of hybrid composites concerning SiO2 nanofiller.Figure 4
Mean values of tension, bending, and impact strength of hybrid composites based on nano-SiO2 filler.Figure 5
Surface plot of silica addition on the nanocomposites. (a) Tension, (b) bending, and (c) impact properties.
(a)(b)(c)


### 3.3. Impacts of Liquid Nitrogen Process

In cryogenic processing, the composite specimens were subjected to fluid nitrogen at -196°C. Cryogenic treatment of polymer-based composites is a novel method of improving mechanical characteristics. The consequence of cryogenic handling on mechanical characteristics of composite is depicted in Figure6. Figure 6 demonstrates that 30-minute treatments resulted in the extreme tensile strength of 43.65 MPa, bending of 64.23 MPa, and impact of 35.65 kg/m2. It could be due to latent stress produced by the compression contact as a consequence of composite materials’ cryo straining. At colder concentrations, internal forces are formed due to shifting matrices and fabric shrinking. The earlier interfacial tensions help sustain fibre and matrices in interaction and enhance adherence, leading to higher results [18, 24, 32]. Figure 7 shows the surface plot of hybrid composites concerning cryogenic treatment.Figure 6
Mean values of tension, bending, and impactness of hybrid composites based on cryogenic treatment.Figure 7
Surface plot of cryogenic treatment on the nanocomposites. (a) Tensile, (b) flexural, and (c) impact properties.
(a)(b)(c)The research results are compression in the fibres and tension in the matrices since the fibres seem to have a lower heat process of continuous than that of the matrix materials [33]. Such compression contact stress maintains fibres and matrices in connection and improves adhesion, leading to better results. Composites that have been cryogenically embrittled become stronger at colder concentrations. The elastic of a specimen diminishes as its stiffness reduces due to the small distortion. The improved delamination resistance of nanoparticles and CGF nanocomposite by cryo processing is attributed to the rise of compression shrinking stress at the border [34]. Their elastic modulus deteriorates whenever composites are handled for more than 45 minutes. Extended cryo condition durations may result in significant heat expansion because of the increasing quantity of fibre incompatibility [35]. Due to the obvious weak contact, delamination events are much more harmful to nanoscale fillers and the CGF combination structure. It could be attributable to the fact that this significantly reduces the time required to dry epoxy coating. Low-bonded materials have high interfacial delamination regions, which exacerbate various critical mechanisms that lead to failure. The mentioned facts are generated by physical phenomena like potholing, matrix/fibre interaction delamination, and propagation of cracks [36].


### 3.4. RSM Models

The segment that follows describes a RSM modeling for such mechanical features of CGF and nanoparticulate composite samples. Torsion, bending, and impacting force coefficient of correlation readings (R2) were determined to be 0.95, 0.94, and 0.95, respectively, in this study. It illustrates the algorithms’ suitability as well as the correctness of the resulting component. It is clear that the correlations among the tensile behaviour and their factor properly account for data erraticism.
(3)TensileStrength=25.7−2.01A+7.36B+1.67C−8.89AB−3.14AC−7.15BC+0.362A2+1.67B2−0.805C2,(4)FlexuralStrength=46.31−3.01A+7.36B+1.98C−9.79AB−4.64AC−9.36BC+0.7862A2+3.25B2−0.915C2,(5)ImpactStrength=17.07+0.0685A−0.1575B+0.0590C+0.0380AB−0.1765AC−0.1565BC−0.90A2−0.060B2−0.046C2.


### 3.5. ANOVA Predictions

The statistical significance (ANOVA) for the magnetic strength of composite samples is shown in Tables1–3. Typically, the factorial approach aids in regulating the adequacy and applicability of a model equation as well as its variables. The F test is used to evaluate the model’s suitability. Table 3 reveals that the multiple regression analysis, with a prototype F-statistic of 63.97, is acceptable for forecasting tensile. The cubic model’s “Prob > F” score is below 0.0001, suggesting that the model is adequate, as per Table 3. Moreover, the substantial effects of nanoparticles (B) are modelling factors.Table 3
ANOVA for tension behaviour.
FactorsSOSdfMSF-rangep rangeModel1061.639117.9617.430.0005A-CGF fibre32.28132.284.770.0653B-weight ratio of nanosilica432.921432.9263.97<0.0001C-cryogenic treatment22.31122.313.30.1123AB315.951315.9546.690.0002AC39.31139.315.810.0468BC204.21204.230.170.0009A20.552510.55250.08160.7834B211.77111.771.740.2287C22.7312.730.40340.5455Residual47.3776.77Fit27.2539.081.810.2858Error20.1345.03Total1109.0116Apart from the versions stated previously, a couple others were not immediately apparent. Table4 reveals that the R-square, with a prototype F-statistic of 69.79, is acceptable for forecasting modulus of elasticity. Table 4 shows that the cubic model’s “Prob > F” score is less than 0.0001, and its coefficient of determination is significant. The weight percentage of nanosilica (B) prototypes is also noteworthy. Table 5 reveals that the model adequately, with a model F-statistic of 63.97, is acceptable for forecasting strength properties. Table 5 shows that the cubic model’s “Prob>F” score is below 0.0001, which means that the model is significant. The weight percentage of micro (B) prototypes is also noteworthy. Apart from the versions stated below, a couple others are really not immediately apparent.Table 4
ANOVA for bending behaviour.
FactorsSOSdfMSF-rangep rangeModel1046.976174.528.13<0.0001A-CGF fibre32.28132.285.20.0457B-weight ratio of nanosilica432.921432.9269.79<0.0001C-cryogenic treatment22.31122.313.60.0871AB315.951315.9550.93<0.0001AC39.31139.316.340.0305BC204.21204.232.920.0002Residual62.03106.2Fit41.9166.981.390.3916Error20.1345.03Total1109.0116Table 5
ANOVA for impact behaviour.
FactorsSOSdfMSF-rangep rangeModel1061.639117.9617.430.0005A-CGF fibre32.28132.284.770.0653B-weight ratio of nanosilica432.921432.9263.97<0.0001C-cryogenic treatment22.31122.313.30.1123AB315.951315.9546.690.0002AC39.31139.315.810.0468BC204.21204.230.170.0009A20.552510.55250.08160.7834B211.77111.771.740.2287C22.7312.730.40340.5455Residual47.3776.77Fit27.2539.081.810.2858Error20.1345.03Total1109.0116Figures8(a)–8(c) illustrate the usual anticipated versus actual remainder charts for composite characteristics. The model’s suitability is evaluated using a standard probability conspiracy of intermediates that assesses the information utilized in the system for composite quality. Haphazard and usually dispersed residues show the absence of any analytical evidence of the mistake. The remaining coefficient of reaction is tiny as they are so close to the zigzag pattern. As a consequence, the predictable half of the theory accurately describes the elastic modulus, leaving only the inherent unpredictability in the erroneous section [37].Figure 8
Prophesied vs. definite value of (a) tension, (b) bending, and (c) impact behaviour of CGF- and nano-silica-based nanocomposites.
(a)(b)(c)


### 3.6. Microstructural Analysis

The shattered surface of a hybrid composite specimen after additional minutes of low-temperature processing is shown in Figures9(a)–9(d). It could be due to latent stress from compression contact due to the composite material’s cryo straining. At colder concentrations, internal forces are formed, adapting to shifting matrices and fabric shrinking. That type of interfacial strain helps maintain fibres and matrices in interaction and improves adhesion, which leads to positive outcomes. Composites that have been cryogenically embrittled become stronger at colder concentrations. The flexibility of the specimen diminishes as its rigidity reduces due to a smaller deformation [38]. The mechanical characteristics of hybrid samples declined when samples were treated for longer than 30 min. Extended cryo processing durations may result in greater thermal stress because of the increasing quantity of fabric misfits. Caused by lower interaction, delamination is a much more damaging composite structure. It might be since it significantly reduces the time required to dry the epoxy resins. Large delamination zones in low adhesive composites intensify several potential risks that might lead to fracture. Increased stress concentration in the nanocomposites treated after 30 min is caused by decreased thermal expansion among the samples. The above findings lead to the failure of the composite specimens [39].Figure 9
Microstructure images of (a) dispersion of nanosilica in epoxy, (b) 15 min cryogenic, (c) 30 min cryogenic, and (d) 45 min cryogenic treatments.
(a)(b)(c)(d)


### 3.7. Water Absorption Characteristics

The findings of moisture absorption experiments are represented in the following segment. Moisture absorption was shown to be higher with higher duration of cryogenic treatment and lower with the inclusion of nanosilica powder. Figure10 shows the moisture absorption values of the composite samples under cryogenic treatment for 15 min, 30 min, and 45 minutes. Compared to 15 min and 45 min, the 30 min cryogenic treatment provides the lowest moisture uptake values. Figure 7 shows the moisture absorption properties of different durations of cryogenic treatment. It could be due to latent stress produced by compression contact due to the composite material’s cryo straining. At colder concentrations, internal forces are formed, adapting to shifting matrices and fabric shrinking. That type of interfacial strain helps maintain fibres and matrices in interaction and improves adhesion, which leads to positive outcomes. Composites that have been cryogenically embrittled become stronger at colder concentrations. The flexibility of the specimen diminishes as its rigidity reduces due to a smaller deformation [40].Figure 10
Moisture absorption characteristics of nanocomposite based on cryogenic treatment.Generally, it was discovered that adding silica powder restored the drop in water absorption characteristics resulting from the addition of epoxy. The inclusion of cryogenic treatment improved the nanocomposite’s hydrophilic nature [5, 36]. Furthermore, the results show that the negative impacts of epoxy on porosity may be mitigated by silica augmentation. According to the water uptake data, the biobased nanocomposite materials retain less water than natural fibres alone. Silica additives create a convoluted channel for water flow, improving the matrix’s barrier characteristics and allowing the detrimental effects of bioresin to be recovered [37]. Figure 11 shows moisture absorption characteristics of nanocomposites based on the weight ratio of silica filler addition.Figure 11
Moisture absorption characteristics of nanocomposite based on nanosilica filler addition.


## 3.1. Effect of CGF Fibre

Figure2 shows the effect of fibre thickness (gsm) on mechanical possessions like tension, bending, and impact strength of CGF- and nano-silica-based hybrid epoxy composites. Figure 2 shows the greatest tensile of 43.65 MPa, flexural of 64.23 MPa, and impact strength of 35.65 kg/m2. Compared to 200 gsm and 250 gsm, CGF fibre with 300 gsm has the best mechanical characteristics. The poor transfer of load owing to the irregular distribution of fibres across the matrix is the cause of the low performance at the 200 gsm composite structure. As a result, a matrix-rich area emerged in the composite, with poor fibre-to-fibre coupling. The fibre reinforcement was easily pulled out of the matrix when loaded in this state. It demonstrates that the CGF fibre composite’s 200 gsm reinforcing effect is insufficient to bear the mechanical load. The mechanical characteristics of the composite progress when the fibre proportions are raised from 200 gsm to 300 gsm. This is mostly owing to the development of good bonding among matrix and their reinforcement, which resulted from the fibres’ creating no gaps in the composite by accommodating more short fibres and ensuring good load sharing between them [19]. As the fibre content grew, the interaction between the fibre and matrix improved. As a result, greater energy is required to interrupt the interwoven fibre bundles’ connection. Figure 3 shows the surface plot of hybrid composites concerning CGF fibre thickness.Figure 2
Mean values of tension, bending, and impact strength of hybrid composites based on CGF fibre thickness.Figure 3
Surface plot of different CGF nanocomposites. (a) Tension, (b) bending, and (c) impact properties.
(a)(b)(c)


## 3.2. Effect of Filler Additions

Figure4 shows nanosilica filler additions’ tensile, flexural, and impact properties. Compared to 1.5 wt.% and 3 wt.% of nanosilica, 4.5 wt.% of silica additions revealed better mechanical strength. The increased mechanical characteristics of nanosilica in resin at a concentration of 3 wt.% might be attributed to improved stress distribution and transmission. Adding more filled silica to the epoxy matrix increased the conveyance and size of holes, influencing the decohesion closeness among the reinforcement and the resin [31]. Consequently, the epoxy, woven CGF, and silica formulations offer sufficient adhesion binding among surface adhesions at a concentration of 3 wt.%. Adding 1.5 and 4.5 wt.% silica, on the other hand, produced a negative result, signifying a decrease in mechanical strength. Furthermore, heavier and lighter loadings of 1.5 wt.% and 4.5 wt.% have been shown to have poor boundary adherence of fibre and matrix in woven CGF and epoxy, resulting in aggregation due to poor adhesion and inferior composite strength qualities [6]. Figure 5 shows the surface plot of hybrid composites concerning SiO2 nanofiller.Figure 4
Mean values of tension, bending, and impact strength of hybrid composites based on nano-SiO2 filler.Figure 5
Surface plot of silica addition on the nanocomposites. (a) Tension, (b) bending, and (c) impact properties.
(a)(b)(c)


## 3.3. Impacts of Liquid Nitrogen Process

In cryogenic processing, the composite specimens were subjected to fluid nitrogen at -196°C. Cryogenic treatment of polymer-based composites is a novel method of improving mechanical characteristics. The consequence of cryogenic handling on mechanical characteristics of composite is depicted in Figure6. Figure 6 demonstrates that 30-minute treatments resulted in the extreme tensile strength of 43.65 MPa, bending of 64.23 MPa, and impact of 35.65 kg/m2. It could be due to latent stress produced by the compression contact as a consequence of composite materials’ cryo straining. At colder concentrations, internal forces are formed due to shifting matrices and fabric shrinking. The earlier interfacial tensions help sustain fibre and matrices in interaction and enhance adherence, leading to higher results [18, 24, 32]. Figure 7 shows the surface plot of hybrid composites concerning cryogenic treatment.Figure 6
Mean values of tension, bending, and impactness of hybrid composites based on cryogenic treatment.Figure 7
Surface plot of cryogenic treatment on the nanocomposites. (a) Tensile, (b) flexural, and (c) impact properties.
(a)(b)(c)The research results are compression in the fibres and tension in the matrices since the fibres seem to have a lower heat process of continuous than that of the matrix materials [33]. Such compression contact stress maintains fibres and matrices in connection and improves adhesion, leading to better results. Composites that have been cryogenically embrittled become stronger at colder concentrations. The elastic of a specimen diminishes as its stiffness reduces due to the small distortion. The improved delamination resistance of nanoparticles and CGF nanocomposite by cryo processing is attributed to the rise of compression shrinking stress at the border [34]. Their elastic modulus deteriorates whenever composites are handled for more than 45 minutes. Extended cryo condition durations may result in significant heat expansion because of the increasing quantity of fibre incompatibility [35]. Due to the obvious weak contact, delamination events are much more harmful to nanoscale fillers and the CGF combination structure. It could be attributable to the fact that this significantly reduces the time required to dry epoxy coating. Low-bonded materials have high interfacial delamination regions, which exacerbate various critical mechanisms that lead to failure. The mentioned facts are generated by physical phenomena like potholing, matrix/fibre interaction delamination, and propagation of cracks [36].


## 3.4. RSM Models

The segment that follows describes a RSM modeling for such mechanical features of CGF and nanoparticulate composite samples. Torsion, bending, and impacting force coefficient of correlation readings (R2) were determined to be 0.95, 0.94, and 0.95, respectively, in this study. It illustrates the algorithms’ suitability as well as the correctness of the resulting component. It is clear that the correlations among the tensile behaviour and their factor properly account for data erraticism.
(3)TensileStrength=25.7−2.01A+7.36B+1.67C−8.89AB−3.14AC−7.15BC+0.362A2+1.67B2−0.805C2,(4)FlexuralStrength=46.31−3.01A+7.36B+1.98C−9.79AB−4.64AC−9.36BC+0.7862A2+3.25B2−0.915C2,(5)ImpactStrength=17.07+0.0685A−0.1575B+0.0590C+0.0380AB−0.1765AC−0.1565BC−0.90A2−0.060B2−0.046C2.


## 3.5. ANOVA Predictions

The statistical significance (ANOVA) for the magnetic strength of composite samples is shown in Tables1–3. Typically, the factorial approach aids in regulating the adequacy and applicability of a model equation as well as its variables. The F test is used to evaluate the model’s suitability. Table 3 reveals that the multiple regression analysis, with a prototype F-statistic of 63.97, is acceptable for forecasting tensile. The cubic model’s “Prob > F” score is below 0.0001, suggesting that the model is adequate, as per Table 3. Moreover, the substantial effects of nanoparticles (B) are modelling factors.Table 3
ANOVA for tension behaviour.
FactorsSOSdfMSF-rangep rangeModel1061.639117.9617.430.0005A-CGF fibre32.28132.284.770.0653B-weight ratio of nanosilica432.921432.9263.97<0.0001C-cryogenic treatment22.31122.313.30.1123AB315.951315.9546.690.0002AC39.31139.315.810.0468BC204.21204.230.170.0009A20.552510.55250.08160.7834B211.77111.771.740.2287C22.7312.730.40340.5455Residual47.3776.77Fit27.2539.081.810.2858Error20.1345.03Total1109.0116Apart from the versions stated previously, a couple others were not immediately apparent. Table4 reveals that the R-square, with a prototype F-statistic of 69.79, is acceptable for forecasting modulus of elasticity. Table 4 shows that the cubic model’s “Prob > F” score is less than 0.0001, and its coefficient of determination is significant. The weight percentage of nanosilica (B) prototypes is also noteworthy. Table 5 reveals that the model adequately, with a model F-statistic of 63.97, is acceptable for forecasting strength properties. Table 5 shows that the cubic model’s “Prob>F” score is below 0.0001, which means that the model is significant. The weight percentage of micro (B) prototypes is also noteworthy. Apart from the versions stated below, a couple others are really not immediately apparent.Table 4
ANOVA for bending behaviour.
FactorsSOSdfMSF-rangep rangeModel1046.976174.528.13<0.0001A-CGF fibre32.28132.285.20.0457B-weight ratio of nanosilica432.921432.9269.79<0.0001C-cryogenic treatment22.31122.313.60.0871AB315.951315.9550.93<0.0001AC39.31139.316.340.0305BC204.21204.232.920.0002Residual62.03106.2Fit41.9166.981.390.3916Error20.1345.03Total1109.0116Table 5
ANOVA for impact behaviour.
FactorsSOSdfMSF-rangep rangeModel1061.639117.9617.430.0005A-CGF fibre32.28132.284.770.0653B-weight ratio of nanosilica432.921432.9263.97<0.0001C-cryogenic treatment22.31122.313.30.1123AB315.951315.9546.690.0002AC39.31139.315.810.0468BC204.21204.230.170.0009A20.552510.55250.08160.7834B211.77111.771.740.2287C22.7312.730.40340.5455Residual47.3776.77Fit27.2539.081.810.2858Error20.1345.03Total1109.0116Figures8(a)–8(c) illustrate the usual anticipated versus actual remainder charts for composite characteristics. The model’s suitability is evaluated using a standard probability conspiracy of intermediates that assesses the information utilized in the system for composite quality. Haphazard and usually dispersed residues show the absence of any analytical evidence of the mistake. The remaining coefficient of reaction is tiny as they are so close to the zigzag pattern. As a consequence, the predictable half of the theory accurately describes the elastic modulus, leaving only the inherent unpredictability in the erroneous section [37].Figure 8
Prophesied vs. definite value of (a) tension, (b) bending, and (c) impact behaviour of CGF- and nano-silica-based nanocomposites.
(a)(b)(c)


## 3.6. Microstructural Analysis

The shattered surface of a hybrid composite specimen after additional minutes of low-temperature processing is shown in Figures9(a)–9(d). It could be due to latent stress from compression contact due to the composite material’s cryo straining. At colder concentrations, internal forces are formed, adapting to shifting matrices and fabric shrinking. That type of interfacial strain helps maintain fibres and matrices in interaction and improves adhesion, which leads to positive outcomes. Composites that have been cryogenically embrittled become stronger at colder concentrations. The flexibility of the specimen diminishes as its rigidity reduces due to a smaller deformation [38]. The mechanical characteristics of hybrid samples declined when samples were treated for longer than 30 min. Extended cryo processing durations may result in greater thermal stress because of the increasing quantity of fabric misfits. Caused by lower interaction, delamination is a much more damaging composite structure. It might be since it significantly reduces the time required to dry the epoxy resins. Large delamination zones in low adhesive composites intensify several potential risks that might lead to fracture. Increased stress concentration in the nanocomposites treated after 30 min is caused by decreased thermal expansion among the samples. The above findings lead to the failure of the composite specimens [39].Figure 9
Microstructure images of (a) dispersion of nanosilica in epoxy, (b) 15 min cryogenic, (c) 30 min cryogenic, and (d) 45 min cryogenic treatments.
(a)(b)(c)(d)


## 3.7. Water Absorption Characteristics

The findings of moisture absorption experiments are represented in the following segment. Moisture absorption was shown to be higher with higher duration of cryogenic treatment and lower with the inclusion of nanosilica powder. Figure10 shows the moisture absorption values of the composite samples under cryogenic treatment for 15 min, 30 min, and 45 minutes. Compared to 15 min and 45 min, the 30 min cryogenic treatment provides the lowest moisture uptake values. Figure 7 shows the moisture absorption properties of different durations of cryogenic treatment. It could be due to latent stress produced by compression contact due to the composite material’s cryo straining. At colder concentrations, internal forces are formed, adapting to shifting matrices and fabric shrinking. That type of interfacial strain helps maintain fibres and matrices in interaction and improves adhesion, which leads to positive outcomes. Composites that have been cryogenically embrittled become stronger at colder concentrations. The flexibility of the specimen diminishes as its rigidity reduces due to a smaller deformation [40].Figure 10
Moisture absorption characteristics of nanocomposite based on cryogenic treatment.Generally, it was discovered that adding silica powder restored the drop in water absorption characteristics resulting from the addition of epoxy. The inclusion of cryogenic treatment improved the nanocomposite’s hydrophilic nature [5, 36]. Furthermore, the results show that the negative impacts of epoxy on porosity may be mitigated by silica augmentation. According to the water uptake data, the biobased nanocomposite materials retain less water than natural fibres alone. Silica additives create a convoluted channel for water flow, improving the matrix’s barrier characteristics and allowing the detrimental effects of bioresin to be recovered [37]. Figure 11 shows moisture absorption characteristics of nanocomposites based on the weight ratio of silica filler addition.Figure 11
Moisture absorption characteristics of nanocomposite based on nanosilica filler addition.


## 4. Conclusion

In this experimental study, the mechanical features of silica-filled woven CGF-/epoxy-based hybrid composites were manufactured and optimized using RSM. Based on the multioptimization, the controllable processing variables for nanosilica and CGF-based hybrid nanocomposites should be set at 3% silica, 300 gsm of CGF, and 30 minutes of cryogenic treatment. The tension, bending, and impactness of correlation coefficient values (R2) are 0.9528, 0.9421, and 0.9547, correspondingly. According to the RSM result, the weight ratio of silica filler addition is the most important parameter. Compared to 1.5 wt.% and 4.5 wt.%, the 3 wt.% of silica revealed improved mechanical strength because the incidence of controlled filler additions balances the effects of voids. The SEM image confirmed this. When the number of CGF gsm in the hybrid composites was increased, the results were positive. The interaction zone between the fibre and the matrix has enhanced as the fibre content has augmented. As a result, additional energy is required to break down the interweaved fibre packages’ connection. The residual stresses created at the interface at the cryogenic healing were compressive, assisting in greater matrix-reinforcement adhesion, but only for the first 30 minutes of treatment. For that reason, this composite specimen absorbs the lowest amount of moisture.The extensive empirical investigation presented on evaluating the characteristics of CGF/nano-SiO2 was considered in this study. Nevertheless, it is well established that fabricating organic nanocomposites in a cold condition has several obstacles and impacts the material’s structure and capabilities. For fabricating professionals, determining on a consistent production path for developing composites for cooling applications is still challenging. As a consequence, it is advised that control parameters be selected and optimised in order to get a high product with more distinct characteristics. As a result, we still need more research and development activities by using a few matrix composites derived from natural fibres, and cryo processing is required. The existence of porous in the composites after overdiagnosis is a problematic marvel that should be prevented by means of suitable procedures.



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*Source: 4138179-2022-08-04.xml*