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The mechanical properties of natural rubber (NR) vulcanizate depend strongly on several factors, i.e., vulcanization systems and crosslink density. These two parameters are originally from the formulation design of the vulcanizate. To focus more on such details, influences of three different vulcanization systems (sulfur, peroxide, and phenolic resin) with variations in their crosslink densities were studied by focusing on the change of curing properties, crosslink densities, mechanical properties and network structures of the NR vulcanizates. The crosslink density of various vulcanization systems increased with increasing curing promotors, as revealed by temperature scanning stress relaxation measurement. The tensile modulus at 100% strain increased with increasing crosslink density in all systems but the tensile strength varied with the vulcanization systems and degree of crosslink density. At the same crosslink level, the greatest tensile strength was obtained when the sulfur was used as a crosslinker, which was 100% greater than those obtained from peroxide and 200% over phenolic systems. In comparison to the phenolic resin system, sulfur and peroxide crosslink systems had a more uniform distribution of the crosslink network structure. The size of the network structure was found to be independent of the tensile strength. The peroxide system had the most uniform distribution of the crosslink network structure.

In this study, the relationships between the structure of unvulcanized rubber and vulcanizate properties were investigated for the three natural rubber clones: RRIT251, PB235, and RRIM600. The highest tensile properties of rubber vulcanizates were achieved from the PB235 clone whereas the RRIM600 showed the lowest. The PB235 contained the largest average molecular weight (Mw) with the narrowest molecular mass distribution (MWD), whereas the least Mw was for RRIM600 with the broadest MWD. The highest protein contents were noticed in RRIM600 where the highest gel formation was found. In contrast, the PB235 showed the smallest amount of proteins and gel contents. Based on this finding, the results clearly suggested that the Mw represented as a key factor controlling the mechanical properties of vulcanizates. This was because the higher average Mw provide the greater active sites available for crosslinking reaction, while the protein content governed the gel formation in the unvulcanized rubber.

We investigated the reinforcement behavior of small amounts of chemically unmodified cellulose nanofiber (CNF) in eco-friendly natural rubber (NR) nanocomposites. For this purpose, NR nanocomposites filled with 1, 3, and 5 parts per hundred rubber (phr) of cellulose nanofiber (CNF) were prepared by a latex mixing method. By using TEM, a tensile test, DMA, WAXD, a bound rubber test, and gel content measurements, the effect of CNF concentration on the structure–property relationship and reinforcing mechanism of the CNF/NR nanocomposite was revealed. Increasing the content of CNF resulted in decreased dispersibility of the nanofiber in the NR matrix. It was found that the stress upturn in the stress–strain curves was remarkably enhanced when the NR was combined with 1–3 phr CNF, and a noticeable increase in tensile strength (an approximately 122% increase in tensile strength over that of NR) was observed without sacrificing the flexibility of the NR in the NR filled with 1 phr CNF, though no acceleration in their strain-induced crystallization was observed. Since the NR chains were not inserted in the uniformly dispersed CNF bundles, the reinforcement behavior by the small content of CNF might be attributed to the shear stress transfer at the CNF/NR interface through the interfacial interaction (i.e., physical entanglement) between the nano-dispersed CNFs and the NR chains. However, at a higher CNF filling content (5 phr), the CNFs formed micron-sized aggregates in the NR matrix, which significantly induced the local stress concentration and promoted strain-induced crystallization, causing a substantially increased modulus but reduced the strain at the rupture of the NR.

As most plastic materials disintegrate without being properly reused after they are discarded, this present study developed a novel thermoplastic elastomer (TPE) using recycled high-density polyethylene (rHDPE) and natural rubber (NR) with kenaf fibre as a sustainable filler. Apart from being used as filler, this present study aimed to examine the use of kenaf fibre as a natural anti-degradant as well. The results indicated that the tensile strength of the samples was found to have significantly decreased after 6 months of natural weathering and had decreased by a further 30% after 12 months due to the chain scission of the polymeric backbones and the degradation of the kenaf fibre. However, the composites that contained kenaf fibre significantly retained their properties post-natural weathering. In terms of tensile strength and elongation at the break, the addition of only 10 phr of kenaf increased the retention properties by 25% and 5%, respectively. This is noteworthy as kenaf fibre also contains a certain amount of natural anti-degradants. Therefore, as the kenaf fibre improves the weather resistance of composites, plastic manufacturers could use it as either a filler or a natural anti-degradant.

Natural rubber (NR) is incompatible with hydrophilic additives like halloysite nanotubes (HNT) due to their different polarity. The silane coupling agent is the ideal component to include in such a compound to solve this problem. Many types of silane are available for polymer composites depending on their functionalities. This work aimed to tune it to the composite based on NR and HNT. Four different silanes, namely Bis[3- (Triethoxysilyl)Propyl]Tetrasulfide (TESPT), 3-Aminopropyl triethoxysilane (APTES), N-[3-(Trimethoxysilyl)Propyl] Ethylenediamine (AEAPTMS), and Vinyltrimethoxysilane (VTMS) were used. Here, the mechanical properties were used to assess the properties, paying close attention to how their reinforcement influenced their crystallization behavior after stretching. It was revealed that adding silane coupling agents greatly improved the composites’ modulus, tensile strength, and tear strength. From the overall findings, AEAPTMS was viable for NR/HNT composites. This was in direct agreement with the interactions between NR and HNT that silanes had encouraged. The findings from stress-strain curves describing the crystallization of the composites are in good agreement with the findings from synchrotron wide-angle X-ray scattering (WAXS). The corresponding silanes have substantially aided the strain-induced crystallization (SIC) of composites.

Chemical treatment is one of the recognized methods that can be implemented to improve the overall performances of biocomposite materials. Unfortunately, trial and error methods were used to determine the optimal ratio between percentage of treatment agent and composite’s properties in the past. Hence, this research focuses on the optimization and validation of coupling agent percentage with properties of novel Polylactic Acid (PLA) / Nypa Fruticans Husks (NFH) biocomposite films via Central Composite Design (CCD) Method. Nypa Fruticans husks was grounded to obtain particulate form and mixed with Polylactic acid (PLA) using solvent casting method. Due to the different polarity between Nypa Fruticans Husks and Polylactic Acid, 3-Aminopropyltriethoxysilane was used to enhance the properties of the composite films. Central composite design (CCD) method was used to determine the optimized percentage of 3- Aminopropyltriethoxysilane and analysis of variance various (ANOVA) was performed to develop mathematical model to predict the tensile strength value in the range of factors in this research. Apart from that, the enzymatic biodegradation was also performed to investigate the composite’s degradation rate. It was found that, the incorporation of Nypa Fruticans Husks decreased the tensile strength and elongation at break, whereas the modulus of elasticity and degradation rate increased. However, composite films treated with 3% of 3-APE showed increment pattern in tensile strength and modulus of elasticity but decreased in elongation at break and degradation rate, respectively. The enhancement of the mechanical properties after treated with 3-Aminopropyltriethoxysilane was supported by the SEM micro-graphs and FTIR analysis.

A massive demand for rubber-based goods, particularly gloves, was sparked by the emergence of the COVID-19 epidemic worldwide. This resulted in thousands of tons of gloves being scrapped due to the constant demand for the items, endangering our environment in a grave way. In this work, we aimed to focus on the utilization of waste nitrile gloves (r-NBR) as a component blended with natural rubber (NR). The life span and other related properties of the blend can be improved by proper control of the chemical recipe. This study assessed three types of crosslinking systems, namely sulfur (S), peroxide (DCP), and mixed sulfur/peroxide (S/DCP) systems. The results indicate that choosing S/DCP strongly affected the tensile strength of the blend, especially at relatively high contents of r-NBR, improving the strength by 40–60% for cases with 25–35 phr of r-NBR. The improvement depended on the crosslink types induced in the blends. It is interesting to highlight that the thermal resistance of the blends was significantly improved by using the S/DCP system. This indicates that the life span of this blend can be prolonged by using a proper curing system. Overall, the S/DCP showed the best results, superior to those with S and DCP crosslinking systems.

Natural rubber (NR) nanocomposites reinforced with five parts per hundred rubber (phr) of two different nano-fillers, i.e., nanoclay (abbrev. NC) and cellulose nanofiber (abbrev. CNF), were prepared by using latex mixing approach, followed by mill-compounding and molding. The morphology, stress–strain behavior, strain-induced crystallization, and bound rubber of the NR nanocomposites were systematically compared through TEM, tensile test, WAXS, DMA, and bound rubber measurement. The aggregated CNFs were observed in the NR matrix, while the dispersed nanosized clay tactoids were detected across the NR phase. The reinforcement effects of NC and CNF were clearly distinct in the NR nanocomposites. At the same nano-filler content, the addition of NC and CNF effectively accelerated strain-induced crystallization of NR. The high tensile strength obtained in the NC-filled NR nanocomposite was attributed to strain-induced crystallization of NR accelerated by well-dispersed NC. However, the larger tensile modulus and low strain for the CNF-filled NR were related to the formation of immobilized NR at the interface between CNF aggregate and NR. The immobilization effect of NR at the CNF surface offered by a mutual entanglement of CNF aggregate and NR chain led to local stress concentration and accelerated strain-induced crystallization of CNF/NR nanocomposite. From the present study, the NR nanocomposites combined with 5 phr CNF shows high-tensile modulus and acceptable breaking tensile stress and strain, suggesting the application of CNF/NR based nanocomposite in automotive and stretchable sensors for next-generation electronic devices.

The performance of natural rubber (NR) relies heavily on the microstructural changes during deformation. This has brought to significant change in the stress response of NR. Besides, the stretching rate may also affect the stress response of NR. In this study, effects of stretching rate on tensile deformation and strain-induced crystallization of crosslinked NR were investigated. Results indicated that increasing the strain rate has increased the stress at given strain where the onset of strain-induced crystallization was shifted to a lower strain. The crystallinity of the crosslinked NR was shown to be higher at a high stretching rate and it corresponded well with the tensile response. The results clearly confirm that chain orientation and crystallization became stronger with increasing deformation rate. The study also suggests that the deformation could improve distribution of crosslinked network structures.

The effect of mastication time in an internal mixer on the physical properties and microstructure of natural rubber (NR) was studied. The Mooney viscosity, plasticity, and complex viscosity reduced with increases in the mastication time due to the molecular breakdown of the rubber. The microstructural changes in the NR were studied using small-angle X-ray scattering. The results revealed that a reduction in the physical properties correlated with the structural changes, which occurred due to mastication. Increases in mastication time affected the distribution and size of the nonrubber component aggregations and the uniformity of the molecular structure of the NR.

Properties of cyclized natural rubbers (NR) with various degrees of cyclization (∼4-22%) were investigated in this study. Prior to compounding with rubber additives, the cyclized rubbers were initially prepared by dropping various concentrations of acid (5-30 wt%) to the NR latex, followed by coagulation and drying. The results revealed that the degree of cyclization increased with acid concentration. Increased ring structure formation in the modified NR tended to increase the torque difference during crosslinking, as the cyclic ring structures acted as steric hindrances. The crosslink density was found to decrease with increasing cyclization level due to the loss of active sites for crosslink formation, increasing swelling capability of the cyclized rubbers. The 100% and 300% moduli, tensile strength and extensibility of the NR reduced with increasing degree of cyclization due to a reduction of crosslink density. As a result of cyclic structure formation and a reduction of unsaturated double bonds in the NR, the stability of cyclized NR at elevated temperatures was improved over the pure NR, in a manner dependent on the level of cyclization. Single glass transition temperature was seen in the NR while two glass transition temperatures were noticed in the cyclized NR. The thermal stability of 22% cyclized NR was 50°C higher than that of the pure NR and the aging properties of the cyclized NRs were also greater mainly due to a reduction of unsaturated double bonds. This suggests that cyclized NR may find applications in products requiring thermal resistance.

Natural rubber (NR) latex foam is one of the rubber products that are increasingly in demand in the market. This is simply because of its lightweight, good thermal insulation, and resilience. The applications of NR latex foam are mostly for pillows and mattresses. This has resulted in these products requiring antibacterial performance which is very important for the safety of the end-users. In this study, the antibacterial NR latex foam was prepared by incorporating the silver-doped zinc oxide (Ag-doped ZnO) into the NR latex foam. Ag-doped ZnO was prepared by microwave-assisted method and then characterized through morphological characteristics and X-ray diffraction (XRD). The content of Ag doped onto ZnO was designed by varying the AgNO3 content at 15 wt%, 50 wt%, and 100 wt% of ZnO. The results confirmed that the Ag was successfully doped onto ZnO. The silver particles were found to be in the 40–50 nm range, where the size of ZnO ranges between 300 and 400 nm, and the Ag attached to the ZnO particles. The XRD patterns of Ag-doped ZnO correspond to planes of hexagonal wurtzite ZnO structure and cubic metallic Ag. This Ag-doped ZnO was further added to NR latex foam. It was observed that Ag-doped ZnO did not affect the physical properties of the NR latex foam. However, it is clear that both the inhibition zone and percent reduction of bacteria (e.g., E. coli and S. aureus) were enhanced by the addition of Ag-doped ZnO. It showed a decrease in the amount of cell growth over contact time. The content of 100 wt% AgNO3 could reduce E. coli and S. aureus up to 64.72% and 58.90%, respectively, when samples were maintained for 24 h. This study provides a scientific understanding of how Ag-doped ZnO could facilitate the development of eventual rubber foam products based on the respective results.

Natural rubber (NR) and halloysite nanotube (HNT) composites are known to perform poorly due to polarity differences between the two components. As such, many extant studies have attempted to increase their compatibility. Therefore, this study introduced epoxidized natural rubber (ENR) together with silane coupling agents into the composite to ensure rubber-filler interactions. Four different silanes namely bis-[(triethoxysilyl)propyl] disulphide (TESPD), bis[(triethoxysilyl)propyl] tetrasulfide (TESPT), triethoxyvinylsilane (VTEO), and 3-mercaptopropyl-di(tridecan-1-oxy-13-penta(ethyleneoxide)) ethoxysilane (VPSi-363) were used. Fourier-transform infrared (FTIR) spectroscopy of the composite confirmed the formation of hydrogen bonds between the silane as the peak of Si-O shifted to higher wavenumbers; i.e., 1080 cm-1 to 1042 cm-1. Silane was also found to improve the tensile strength, modulus and tear strength regardless of functionality. This was further supported by the findings of the Payne effect. As for strain-induced crystallisation (SIC), the stress-strain curves agreed well with the development of crystallinity observed during synchrotron wide-angle X-ray scattering analysis.

Natural rubber latex (NRL) is a polymer (blend) extracted from the milky sap of para rubber trees. Due to being a natural biopolymer, NRL contains various proteins that may be allergenic to humans when in skin contact. Attempts have been made to use deproteinized natural rubber (DPNR) instead of impure NRL, and the final properties of these two types of rubber tend to differ. Thus, the correlations between their chemistry and properties are of focal interest in this work. DPNR was prepared by incubating NRL with urea, followed by aqueous washing/centrifugation. The physical, mechanical, and dynamic properties of incubated NRL before and after washing/centrifugation were examined to distinguish its influences from those of incubation with urea. According to the findings, the proteins, phospholipids, and chain entanglements were responsible for natural polymer networks formed in the NR. Although the proteins were largely removed from the latex by incubation, the properties of high ammonia natural rubber (HANR) were still maintained in its DPNR form, showing that other network linkages dominated over those contributed by the proteins. In the incubated latex, the naturally occurring linkages were consistently reduced with the number of wash cycles.

Carbonized natural filler can offer the production of low cost composites with an eco-friendliness value. The evolving field of electronics encourages the exploration of more functions and potential for carbonized natural filler, such as by modifying its surface chemistry. In this work, we have performed surface modification on carbonized wood fiber (CWF) prior to it being used as filler in the ethylene vinyl acetate (EVA) composite system. Zinc chloride (ZnCl2) with various contents (2 to 8 wt%) was used to surface modify the CWF and the effects of ZnCl2 composition on the surface morphology and chemistry of the CWF filler were investigated. Furthermore, the absorptive, mechanical, thermal, and electrical properties of the EVA composites containing CWF-ZnCl2 were also analyzed. SEM images indicated changes in the morphology of the CWF while FTIR analysis proved the presence of ZnCl2 functional groups in the CWF. EVA composites incorporating the CWF-ZnCl2 showed superior mechanical, thermal and electrical properties compared to the ones containing the CWF. The optimum content of ZnCl2 was found to be 6 wt%. Surface modification raised the electrical conductivity of the EVA/CWF composite through the development of conductive deposits in the porous structure of the CWF as a channel for ionic and electronic transfer between the CWF and EVA matrix.

The use of mineral fillers in rubber industry has been increasingly focused. Sepiolite is considered as one of the mineral fillers that exploits unique characteristics. This is due to its unique needle-like fibrous and a tunnel-like micro-pore channel structures. Therefore, adding this filler in natural rubber (NR) matrix would bring tremendous advantage. The study was carried out in the form of curing characteristics, tensile properties and morphology together with the dynamic properties. Filling sepiolite to NR has brought to a noticeable enhancement of curing characteristics, tensile properties and morphology. This is contributed to the distinctive structure of sepiolite itself, it provides a better dispersion to the NR. Surface roughness of the composites is visibly found which is responsible for the mechanical properties. Further verification was also monitored through the dynamic properties of the composites. The obtained profiles are in good agreement to the tensile properties and morphological characteristics observed.

Elastomeric foams based on 60/40 EVA/NR blend nanocomposite were prepared by melt mixing EVA, NR and clay (5 phr) in an internal mixer, and later foamed with azodicarbonamide through compression molding. Epoxidized natural rubber (ENR) with epoxide content of 25 mole% was used as a compatibilizer to improve interfacial adhesion between EVA and NR. The addition effect of ENR concentration on the blending and properties of EVA/NR blend nanocomposite foams was studied. XRD and TEM results showed that the clay in the EVA/NR blends was intercalated and locally existed in the NR phase as well as at the interface between EVA and NR. The EVA/NR blend nanocomposites showed dispersed NR domains in continuous EVA phase. The addition of ENR into EVA/NR blend nanocomposites reduced the size of the dispersed NR phase, indicating that the blend miscibility was improved. Mechanistic model was proposed for the miscibility improvement of a two-phase structure of EVA/NR blend nanocomposite in the presence of ENR and clay dispersion. However, the improved blend morphology did not significantly affect the cell structure of EVA/NR blend nanocomposites. The observation of cell structure of EVA/NR blend nanocomposites suggested that the increased addition of ENR caused a little increase in cell density, and had no influence on cell size. Furthermore, with increasing addition level of ENR in the blend nanocomposite foams, the foam density slowly decreased, whereas the specific tensile strength slightly increased. The elastomeric recovery of blend nanocomposite foams decreased with increasing ENR content. The thermal conductivity of EVA/NR blend nanocomposite foams also decreased with more addition of ENR, which had beneficial result in improving thermal insulation property.

Natural rubber (NR) composites filled with various sepiolite loadings were prepared and optimized by two different mixing methods, namely, melt mixing and latex mixing methods. The properties were evaluated through viscosity, stress relaxation, curing behaviors and tensile properties of rubber composites. The viscosity was influenced by sepiolite content and mixing methods. The greater interaction between rubber and sepiolite was obtained from melt mixing method. This reflected to the greater tensile strength found in this method. Considering the content of sepiolite, similar trend was observed for the curing properties and elongation at break. The greatest tensile strength was observed when the sepiloite content was at 1 phr.

Halloysite Nanotubes (HNT) are chemically similar to clay, which makes them incompatible with non-polar rubbers such as natural rubber (NR). Modification of NR into a polar rubber is of interest. In this work, Epoxidized Natural Rubber (ENR) was prepared in order to obtain a composite that could assure filler–matrix compatibility. However, the performance of this composite was still not satisfactory, so an alternative to the basic HNT filler was pursued. The surface area of HNT was further increased by etching with acid, the specific surface increased with treatment time. The FTIR spectra confirmed selective etching on the Al–OH surface of HNT with reduction in peak intensity in the regions 3750–3600 cm−1 and 825–725 cm−1, indicating decrease in Al–OH structures. The use of acid-treated HNT improved modulus, tensile strength, and tear strength of the filled composites. This was attributed to the filler–matrix interactions of acid-treated HNT with ENR. Further evidence was found from the Payne effect being reduced to 44.2% through acid treatment of the filler. As for the strain-induced crystallization (SIC) in the composites, the stress–strain curves correlated well with the degree of crystallinity observed from synchrotron wide-angle X-ray scattering.

Halloysite nanotubes (HNT) filled natural rubber composites were prepared in this study. To enhance the properties of the composites, two different approaches were applied to both HNT and rubber. HNT was treated with sulfuric acid (H2SO4) while epoxidized natural rubber was also used as compatibilizer in the composite system. Effect of acid treatment of HNT on BET surface area, mechanical and morphological properties of the obtained composites were investigated. The surface area of acid-treated HNT was greater than that of untreated HNT and it increased over treating time. This has brought to an enhancement of stress at high strain especially when the strain over 500%. From the SEM images, the particle size of acid-treated HNT was seen to be finer and well-dispersed. This is attributed to the possibility of strong adhesion formation among NR, ENR and HNTs, obtaining from acid treatment.

Nanocomposite foams were fabricated from 60/40 wt% ethylene vinyl acetate (EVA)/natural rubber (NR) blends by using azodicarbonamide as a blowing agent. Two different nanofillers (sodium montmorillonite and organoclay) were employed to study their effects on foam properties. The results were also compared with conventional (china clay)-filled foams. Transmission electron microscopy, X-ray diffraction, scanning electron microscopy, and three-dimensional Microfocus X-ray computed tomography scanning analysis were performed to characterize the EVA/NR blend morphology and foam structures. The results revealed that the nanofiller acted as a blend compatibilizer. Sodium montmorillonite was more effective in compatibilization, generating better phase-separated EVA/NR blend morphology and improving foam structure. Higher filler loading increased the specific tensile strength of rubber foams. The rubber nanocomposite foam showed superior specific tensile strength to the conventional rubber composite foam. The elastic recovery and compressive strength of the nanocomposite foams decreased with increasing filler content, whereas the opposite trend was observed for the conventional composite foams with china clay. The thermal conductivity measurement indicated that the nanofiller had better beneficial effect on thermal insulation over china clay filler. From the present study, the nanofillers played an important role in obtaining better blend morphology as compatibilizer, rather than the nucleating agent and the nanofiller content of 5 phr (parts by weight per hundred parts of rubber) was recommended for the production of EVA/NR nanocomposite foams. J. VINYL ADDIT. TECHNOL., 21:134–146, 2015. © 2014 Society of Plastics Engineers

Nanocomposites of natural rubber (NR)/polypropylene (PP) (80/20 wt %) blends filled with 5 phr pristine clay were prepared by melt-mixing process. Effects of clay incorporation technique via conventional melt-mixing (CV) and masterbatch mixing (MB) methods on nanostructure and properties of the blend nanocomposites were investigated. The XRD, SAXS, WAXD, and TEM results showed that the clays in the NR/PP blend nanocomposites were presented in different states of dispersion and were locally existed at the interface between NR and PP as well as dispersed in the NR matrix. The presence of clay caused unique morphological evolution such as fine fibrillar PP domains. The tensile strength was improved over the unfilled NR/PP blends by 53% and 224%, and the storage modulus at 25 °C was increased by 78% and 120% for the NR/PP/clay nanocomposites prepared by CV and MB methods, respectively. Significant improvement in both properties was particularly obtained from the MB method due to finer dispersion fibrillar PP phase in the NR matrix and stronger interfacial adhesion between NR and PP fibers, as suggested from DMA. The oil resistance of blend nanocomposites was also improved over that of the unfilled NR/PP blend, and this property was further progressed by the masterbatch mixing method. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 44574.

Nanocomposites of natural rubber (NR) and pristine clay (clay) were prepared by latex mixing, then crosslinked with phenolic resin (PhOH). For comparative study, the PhOH-crosslinked neat NR was also prepared. Influence of clay loading (i.e., 1, 3, 5, and 10 phr) on mechanical properties and structural change of PhOH-crosslinked NR/clay nanocomposites was studied through X-ray diffraction (XRD), transmission electron microscopic (TEM), wide-angle X-ray diffraction (WAXD), tensile property measurement, and Fourier transform infrared spectroscopy (FTIR). XRD and TEM showed that the clay was partly intercalated and aggregated, and that the dispersion state of clay was non-uniform at higher clay loading (>5 phr). From tensile test measurement, it was found that the pronounced upturn of tensile stress was observed when the clay loading was increased and a maximum tensile strength of the PhOH-crosslinked NR/clay nanocomposites was obtained at 5 phr clay. WAXD observations showed that an increased addition of clay induced more orientation and alignment of NR chains, thereby lowering onset strain of strain-induced crystallization and promoting crystallinity of the NR matrix during tensile deformation. FTIR investigation indicated a strong interfacial adhesion between NR matrix and clay filler through a phenolic resin bridge. This suggested that the PhOH did not only act as curative agent for crosslinking of NR, but it also worked as coupling agent for promoting interfacial reaction between NR and clay. The presence of strong interfacial adhesion was found to play an important role in the crystallization process, leading to promotion of mechanical properties of the PhOH-crosslinked NR/clay nanocomposites. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016, 133, 43214.

Nanocomposites of natural rubber (NR) and unmodified clay were prepared by latex compounding method. Phenolic resin (PhOH) was used to crosslink NR. Crosslinked neat NR was also prepared for comparison. The structure–property relationship of uncrosslinked and crosslinked NR/clay nanocomposites was examined to verify the reinforcement mechanism. Microstructure of NR/clay nanocomposites was studied by using transmission electron microscopic (TEM), X-ray diffraction (XRD), wide angle X-ray diffraction (WAXD), and small angle X-ray scattering (SAXS) analyses. The results showed the evidence of intercalated clay together with clay tactoids for the nanocomposite samples. The highest tensile strength was achieved for the crosslinked NR/clay nanocomposite. The onset strain of deformation induced the crystallization of NR for nanocomposites was found at almost the same strain, and furthermore their crystallization was developed at lower strain than that of the crosslinked neat NR because of the clay orientation and alignment. However, at high strain region, the collaborative crystallization process related to the clay dispersion and conventional crosslink points in the NR was responsible to considerably high tensile strength of the crosslinked NR/clay nanocomposite. Based on these analyses, a mechanistic model for the strain-induced crystallization and orientational evolution of a network structure of PhOH-crosslinked NR/clay nanocomposite was proposed. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015, 132, 42580.