Characterization and Properties of Treated Oil Palm Empty Fruit Bunch Regenerated Cellulose Biocomposite Films with Butyl Methacrylate Using Ionic Liquid

Regenerated cellulose biocomposite films from oil palm empty fruit bunch and microcrystalline cellulose were prepared using N,N-dimethylacetamide and lithium chloride. The effects of oil palm empty fruit bunch contents and butyl methacrylate on properties of regenerated cellulose biocomposite films were investigated. At 2?wt% of untreated oil palm empty fruit bunch content showed highest crystallinity index, tensile strength, modulus of elasticity, and thermal stability but lower elongation at break than other oil palm empty fruit bunch content. The treated regenerated cellulose biocomposite films with butyl methacrylate showed better tensile strength, modulus of elasticity, thermal stability, and crystallinity index while Fourier transform infrared spectroscopy study showed interaction between cellulose and butyl methacrylate.     

Preparation of acylated microcrystalline cellulose using olive oil and its reinforcing effect on poly(lactic acid) films for packaging application

A novel poly(lactic acid) (PLA) based composite, reinforced by microcrystalline cellulose (MCC) was prepared. MCC was modified by esterification reaction using olive oil for improving the compatibility with PLA matrix. The acylated microcrystalline cellulose (AMCC) exhibited reduced polarity in comparison to unmodified MCC. AMCC/ PLA composite films were prepared using solvent casting technique. The effects of the MCC surface modification on morphological, mechanical, physical, thermal, biodegradability and barrier properties of the PLA based MCC composites were studied. FTIR analysis confirmed acylation reaction of MCC. Scanning electron microscopy analysis exhibited a uniform distribution of AMCC in PLA matrix. Barrier properties of AMCC based composites were improved as compared to MCC based composites. The tensile strength and tensile modulus of composite films (at 2 wt.% AMCC) were improved about 13% and 35% as much as those of the pure PLA films, respectively. These biodegradable composite films can be a sustainable utilization of olive oil and microcrystalline cellulose in the food packaging application.     

Study of nanoreinforced shape memory polymers processed by casting and extrusion

Multi‐walled carbon nanotubes (CNTs) and cellulose nanofibers (CNFs) reinforced shape memory polyurethane (PU) composite fibers and films have been fabricated via extrusion and casting methods. Cellulose nanofibers were obtained through acid hydrolysis of microcrystalline cellulose. This treatment aided in achieving stable suspensions of cellulose crystals in dimethylformamide (DMF), for subsequent incorporation into the shape memory matrix. CNTs were covalent functionalized with carboxyl groups (CNT‐COOH) and 4,4′‐methylenebis (phenylisocyanate) (MDI) (CNT‐MDI) to improve the dispersion efficiency between the CNT and the polyurethane. Significant improvement in tensile modulus and strength were achieved by incorporating both fillers up to 1 wt% without sacrificing the elongation at break. Electron microscopy was used to investigate the degree of dispersion and fracture surfaces of the composite fibers and films. The effects of the filler (type and concentration) on the degree of crystallinity and thermal properties of the hard and soft segments that form the PU sample were studied by calorimetry. Overall, results indicated that the homogeneous dispersion of nanotubes and cellulose throughout the PU matrix and the strong interfacial adhesion between nanotubes and/or cellulose and the matrix are responsible for the enhancement of mechanical and shape memory properties of the composites. POLYM. COMPOS., 2011. © 2011 Society of Plastics Engineers     

All-cellulose nanocomposite

Cellulose-based nanocomposite films with different ratio of cellulose I and II were produced by means of partial dissolution of microcrystalline cellulose powder in lithium chloride/N,N-dimethylacetamide and subsequent film casting. The mechanical and structural properties of the films were characterised using tensile tests and X-ray diffraction. The films are isotropic, transparent to visible light, highly crystalline, and contain different amounts of undissolved cellulose I crystallites in a matrix of regenerated cellulose. The results show that, by varying the cellulose I and II ratio, the mechanical performance of the nanocomposites can be tuned. Depending on the composition, a tensile strength up to 240 MPa, an elastic modulus of 13.1 GPa, and a failure strain of 8.6% were observed. Moreover, the nanocomposites clearly surpass the mechanical properties of most comparable cellulosic materials, their greatest advantage being the fact that they are fully biobased and biodegradable, but also of relatively high strength.     

The effects on mechanical properties and crystallization of poly (l‐lactic acid) reinforced by cellulosic fibers with different scales

Bacterial cellulose (BC), microcrystalline cellulose (MCC), and bamboo cellulosic fibers (BCFs) were used to reinforce poly(l ‐lactic acid) (PLLA) based bio‐composites. The mechanical properties and crystallization of the composites were studied through mechanical testing, differential scanning calorimetry, X‐ray diffraction, scanning electron microscopy, and polarizing microscope. The incorporation of all three kinds of cellulose increased the stiffness of the composites compared to pure PLLA. The reinforcing effect of the MCC in the composites is most significant. The Young's modulus and impact toughness of the MCC/PLLA composites were increased by 44.4% and 58.8%, respectively. The tensile strength of the MCC/PLLA composites was increased to 71 MPa from 61 MPa of PLLA. However, the tensile strength of the composites reinforced with BCF or BC was lower than PLLA. The three kinds of cellulosic fibers improved the crystallization of PLLA. The BC with smallest size provided the composites with smallest grain and highest crystallinity. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 41077.     

Preparation of cellulose nanofibrils by high-pressure homogenizer and cellulose-based composite films

Cellulose nanofibrils were prepared from starting material microcrystalline cellulose (MCC) by an application of a high-pressure homogenizer at 20,000 psi and treatment consisting of 0, 1, 2, 5, 10, 15 and 20 passes. Hydroxypropyl cellulose (HPC) films reinforced with those cellulose nanofibrils were prepared at different filler loading levels. According to the morphology study by scanning electron microscope (SEM), the complete filbrillation of the bulk cellulose fibrils to nanoscale and high aspect ratio was accomplished by the homogenization process. The HPC film reinforced with cellulose fibrils after the 5–10 passes through the homogenizer improved significantly the tensile modulus and strength values for the HPC films. The thermal stability of HPC films is not affected by the addition of the cellulose nanofibrils, although MCC has the lower thermal stability than neat HPC. The development of novel cellulose nanofibrils and composites with high strength can be achieved by an application of the homogenization process.     

Ionic Liquid Approach Toward Manufacture and Full Recycling of All‐Cellulose Composites

All‐cellulose composites (ACCs) are prepared from high‐strength rayon fibers and cellulose pulp. The procedure comprises the use of a pulp cellulose solution in the ionic liquid (IL) 1‐ethyl‐3‐methyl imidazolium acetate ([EMIM][OAc]) as a precursor for the matrix component. High‐strength rayon fibers/fabrics are embedded in this solution of cellulose in the IL followed by removal of the IL. Different concentrations of cellulose in the IL are investigated and the mechanical properties of the final ACCs are determined via tensile, bending, and impact testing. ACCs prepared in this study show mechanical properties comparable to thermoplastic glass fiber‐reinforced plastics. Apart from being bio‐based, they possess several advantages such as biodegradability and full recyclability. The recycling of ACCs is successfully demonstrated in several cycles by using the recycled cellulose for subsequent matrix preparation.     

Synthesis and characterization of short Grewia optiva fiber‐based polymer composites

Natural fibers, such as Flax, Sisal, Hibiscus Sabdariffa, and Grewia optiva (GO) possess good reinforcing capability when properly compounded with polymers. These fibers are relatively inexpensive, easily available from renewable resources, and possess favorable values of specific strength and specific modulus. The mechanical performance of natural fiber‐reinforced polymers (FRPs) is often limited owing to a weak fiber‐ matrix interface. In contrast, urea–formaldehyde (UF) resins are well known to have a strong adhesion to most cellulose‐containing materials. This article deals with the synthesis of short G. optiva fiber‐reinforced UF polymer matrix‐based composites. G. optiva fiber‐reinforced UF composites processed by compression molding have been studied by evaluating their mechanical, physical, and chemical properties. This work reveals that mechanical properties such as: tensile strength, compressive strength, flexural strength, and wear resistance of the UF matrix increase up to 30% fiber loading and then decreases for higher loading when fibers are incorporated into the polymer matrix. Morphological and thermal studies of the matrix, fiber, and short FRP composites have also been carried out. The swelling, moisture absorbance, chemical resistance, and water uptake behavior of these composites have also been carried out at different intervals. The results obtained lay emphasis on the utilization of these fibers, as potential reinforcing materials in bio‐based polymer composites. POLYM. COMPOS., 2010. © 2009 Society of Plastics Engineers     

Morphological,barrier, and mechanical properties of cassava starch films reinforced with cellulose and starch nanoparticles

A comparative performance study of cellulose and starch nanoparticles on plasticized starch reinforcement has been presented. Starch nanoparticles were obtained by ultrasound and acid hydrolysis, and cellulose nanoparticles were extracted by acid hydrolysis from microcrystalline cellulose and sisal fibers. The nanoparticles were characterized according to the zeta potential, the particle-size distribution, transmission electron microscopy, X-ray diffraction, and thermogravimetric analysis. The influence of the addition of these nanoparticles to starch films on the morphology, water vapor permeability (WVP), and mechanical properties of the nanocomposites films were investigated. The cellulose nanoparticles exhibited higher electrical stability than those originating from starch. Acid hydrolysis produced starch nanoparticles with higher crystallinity than ultrasound. All the nanoparticles significantly reduced the WVP. The cellulose nanoparticles significantly increased the tensile strength of the starch films; however, they reduced the flexibility of the nanocomposites. The results of this work support the application of starch and cellulose nanostructures for the development of reinforced biodegradable materials. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47001.     

Mechanical behavior,structure, and reinforcement processes of TEMPO‐oxidized cellulose reinforced poly(lactic) acid

Poly(lactic) acid (PLA) was reinforced with acetylated TEMPO‐oxidized fibrillated cellulose (TOFC) prepared from birch pulp. Composite films were studied using dynamic mechanical thermal analysis, differential scanning calorimetry (DSC), as well as static mechanical testing. The storage modulus as well as tensile strength of PLA was improved on the addition of 30 wt% of TOFC by approximately 50% and 40%, respectively. Thermal stability as well as strength properties in moist environments (up to 90% relative humidity) was significantly improved at 15, 20, 25, and 30 wt% of TOFC. DSC showed that crystallization from solution took place during preparation of the composite films and was much greater than melt crystallization. POLYM. COMPOS., 2012. © 2013 Society of Plastics Engineers     

Transparent,flexible, and high‐strength regenerated cellulose/saponite nanocomposite films with high gas barrier properties

Regenerated cellulose‐saponite nanocomposite films were prepared from LiOH/urea solutions, and exhibited high optical transparency and flexibility. The saponite platelets formed intercalated nanolayered structures in the composites. The longitudinal directions of both the cellulose II crystallites and the saponite platelets were preferentially oriented parallel to the film surface in the composites. The good nanodispersibility and high orientation of the saponite platelets in the composite films resulted in high mechanical strength, high Young's modulus, and good thermal dimensional stabilities, and gas barrier properties in the composites, compared with a reference cellulose film. Moreover, the tensile strength and Young's modulus of the composite film reached 241 MPa and 7.7 GPa, respectively, when a simple drawing process was applied to the wet composite film; this is probably owing to the improvement in the orientation of the cellulose II crystallites and saponite platelets in the composites. The composite films also showed high toughness and ductility. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 130: 3168–3174, 2013     

Starch‐based biocomposite films reinforced with cellulose nanocrystals from garlic stalks

The study was conducted to reinforce starch‐based biocomposite films using cellulose nanocrystals (CNCs) from garlic stalks. An average yield of 4.6% by mass based from air‐dried garlic stalks was obtained through alkali delignification, acid hydrolysis and sonication. The isolated CNCs are spherical and have an average diameter of 35 nm and crystallinity of 62%. Fourier transform infrared spectra correspond to the structure of cellulose, but some absorption bands corresponding to hemicelluloses were also noticed. Starch‐based biocomposite films with varying amount of the isolated CNCs as reinforcing filler were prepared by solution casting and evaporation method. Scanning electron micrographs of the films showed homogeneous dispersion of CNC in the starch matrix. Improvement in tensile strength and modulus was at maximum when the starch to CNC ratio is 100:5. The thermal stability of the films, on the other hand, decreased with the addition of CNC. Finally, CNC‐reinforced films had lower moisture uptake than nonreinforced films. POLYM. COMPOS. 34:1325–1332, 2013. © 2013 Society of Plastics Engineers     

Numerical simulation of the effect of nanotube orientation on tensile modulus of carbon‐nanotube‐reinforced polymer composites

By correlating the curvature of carbon nanotubes to the orientation of fibers in a polymer, the effect of the curvature of nanotubes on the tensile modulus of carbon‐nanotube‐reinforced polymer composites was investigated with a numerical simulation method. The simulation results showed that the tensile modulus of a nanotube‐reinforced composite drops sharply when the nanotubes diverge from their orientation in the axial direction, and the presence of curved nanotubes in the polymer matrix significantly decreases the modulus of the composite. This finding could explain, partly, why in most cases, the predicted tensile modulus of a carbon‐nanotube‐reinforced composite, based on the assumption that the nanotubes are fully isolated and aligned in the polymer matrix, is much higher than the value obtained from experiments. Copyright © 2004 Society of Chemical Industry     

Plasticization effects of dihydroxyl soybean oil improve flexibilities of epoxy‐based films for coating applications

Novel bio‐based coating materials were developed through cationic ring‐opening photopolymerization of dihydroxyl soybean oil (DSO) with commercial epoxy monomers [i.e., epoxidized soybean oil (ESO) and 3,4‐epoxycyclohexylmethyl‐3,4‐epoxycyclohexanecarboxylate (ECHM). The ether cross‐linking and post‐polymerization of the polymeric network were observed using Fourier transform infrared spectroscopy. Thermal properties of the bio‐based coating materials and their copolymerization behaviors were examined using differential scanning calorimetry and a thermogravimetric analyzer. Cross‐link density and molecular weight between cross‐link were obtained from dynamic mechanical analysis. ECHM/DSO (1 : 1.43 weight ratio) films showed the highest elongation at break (49.2%) with a tensile strength of 13.7 MPa. After 2 months of storage, the elongation at break and tensile strength of films were 32% and 15.1 MPa, respectively. ESO/DSO films (w/w ratios of 1 : 0.1, 1 : 0.15, and 1 : 0.2) exhibited stable flexibility of 11–13% of elongation at break without significant reductions in tensile strength (2.5–4.4 MPa) during a 2‐month shelf life. Optical transparencies of the films were comparable to commercial glass and polymers, and water uptake properties (0.72% and 2.83%) were significantly low. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41773.     

Mechanical properties of silk fibroin–microcrystalline cellulose composite films

Silk fibroin–microcrystalline cellulose (cellulose whisker) composite films with varied compositions were prepared by casting mixed aqueous solution/suspensions of the two components. Silk fibroin was dissolved in 10M LiSCN followed by dialysis; a cellulose whisker suspension was prepared by sulfuric acid hydrolysis of tunicate cellulose. Macroscopically homogeneous films were obtained at all mixing ratios. While the Young's modulus of the composite films showed a linear, additive dependence on the mixing ratio, the tensile strength and ultimate strain showed a maximum at a 70–80% cellulose content, reaching five times those of fibroin‐alone or cellulose‐alone films. At the same mixing ratio, infrared spectra of the composite films showed a shift of the amide I peak from 1654 to 1625 cm^?1, indicating the conformational change of fibroin from a random coil to a β structure (silk II) at the whisker–matrix interface. This change seems to be induced by contact of fibroin molecules with a highly ordered surface of cellulose whisker. © 2002 Wiley Periodicals, Inc. J Appl Polym Sci 86: 3425–3429, 2002     

Preparation and mechanical characterization of chicken feather/PLA composites

Green composites, a bio‐based polymer matrix is reinforced by natural fibers, are special class of bio‐composites. Interest about green composites is continuously growing because they are environment‐friendly. This study describes the preparation and mechanical characterization of green composites using polylactic acid (PLA) matrix including chicken feather fiber (CFF) as reinforcement. Extrusion and an injection molding process were used to prepare CFF/PLA composites at a controlled temperature range. CFF/PLA composites with fiber mass content of 2%, 5%, and 10% were manufactured. The effects of fiber concentration and fiber length on mechanical properties of CFF/PLA composites have been studied. Mechanical properties of composites were investigated by tensile, compression, bending, hardness, and Izod impact testing. The results of experiments indicated that Young's modulus, compressive strength, flexural modulus, and hardness of the PLA reinforced CFF composites are higher but tensile strength, elongation at break, bending strength and impact strength of them are lower than pure PLA. The results indicate that these types of composites can be used for various applications. POLYM. COMPOS., 38:837–845, 2017. © 2015 Society of Plastics Engineers     

Influence of fillers on the mechanical response of an amorphous liquid‐crystalline polymer

A semirigid and amorphous commercial liquid‐crystalline copolyester (Rodrun) was filled with mica and calcium carbonate (up to 25 wt %) by direct injection molding. The fillers led to decreases in the processability, as observed by torque increases, but maintained the thermal resistance of Rodrun. The effects of the two fillers on the modulus of elasticity, ductility, and tensile strength were the same or very similar. The decrease in the tensile strength (20% for a 10% filler content) was compensated by a generally slight increase in the modulus of elasticity, whatever the filler content was. This balance of properties found in these new liquid‐crystalline‐polymer‐based materials and the important savings that the fillers bring may spread the applications of these materials' matrices. © 2003 Wley Periodicals, Inc. J Appl Polym Sci 88: 998–1003, 2003     

Hybridized reinforcement of natural rubber with silane‐modified short cellulose fibers and silica

Natural‐rubber‐based hybrid composites were prepared by the mixture of short cellulose fibers and silica of different relative contents with a 20‐phr filler loading with a laboratory two‐roll mill. The processability and tensile properties of the hybrid composites were analyzed. The tensile modulus improved, but the tensile strength and elongation at break decreased with increasing cellulose fiber content. The scorch safety improved with the addition of 5‐phr cellulose fiber in the composites. The Mooney viscosity significantly decreased with increasing cellulose fiber content. To modify the surface properties of the cellulose fiber and silica fillers, a silane coupling agent [bis(triethoxysilylpropyl)tetrasulfide, or Si69] was used. The effects of Si69 treatment on the processing and tensile properties of the hybrid composites were assessed. We found that the silane treatment of both fillers had significant benefits on the processability but little benefit on the rubber reinforcement. The strength of the treated hybrid composite was comparable to that of silica‐reinforced natural rubber. Furthermore, to investigate the filler surface modification and to determine the mixing effects, infrared spectroscopic and various microscopic techniques, respectively, were used. From these results, we concluded that the fillers were better dispersed in the composites, and the compatibility of the fillers and natural rubber increased with silane treatment. In conclusion, the hybridized use of short cellulose fibers from a renewable resource and silica with Si69 presented in this article offers practical benefits for the production of rubber‐based composites having greater processability and more environmental compatibility than conventional silica‐filler‐reinforced rubber. © 2011 Wiley Periodicals, Inc. J Appl Polym Sci, 2011     

Development of renewable resource–based cellulose acetate bioplastic: Effect of process engineering on the performance of cellulosic plastics

This paper deals with the development of a cellulose acetate biopolymer. Plasticization of this biopolymer under varying processing conditions to make it a suitable matrix polymer for bio‐composite applications was studied. In particular, cellulose acetate was plasticized with varying concentrations of an eco‐friendly triethyl citrate (TEC) plasticizer, unlike a conventional, petroleum‐derived phthalate plasticizer. Three types of processing were used to fabricate plasticized cellulose acetate parts: compression molding, extrusion followed by compression molding, and extrusion followed by injection molding. The processing mode affected the physicomechanical and thermal properties of the cellulosic plastic. Compression molded samples exhibited the highest impact strength, tending towards the impact strength of a thermoplastic olefin (TPO), while samples that were extruded and then injection molded exhibited the highest tensile strength and modulus values. Increasing the plasticizer content in the cellulosic plastic formulation improved the impact strength and strain to failure while decreasing the tensile strength and modulus values. The coefficient of thermal expansion (CTE) of the cellulose acetate increased with increasing amounts of plasticizer. Plasticized cellulose acetate was found to be processable at 170–180°C, approximately 50°C below the melting point of neat cellulose acetate.     

Bio‐nanocomposite films based on cellulose nanocrystals filled polyvinyl alcohol/chitosan polymer blend

Bio‐nanocomposite films based on polyvinyl alcohol/chitosan (PVA/CS) polymeric blend and cellulose nanocrystals (CNC) were prepared by casting a homogenous and stable aqueous mixture of the three components. CNC used as nanoreinforcing agents were extracted at the nanometric scale from sugarcane bagasse via sulfuric acid hydrolysis; then they were characterized and successfully dispersed into a PVA/CS (50/50, w/w) blend to produce PVA/CS–CNC bio‐nanocomposite films at different CNC contents (0.5, 2.5, 5 wt %). Viscosity measurement of the film‐forming solutions and structural and morphological characterizations of the solid films showed that the CNC are well dispersed into PVA/CS blend forming strong interfacial interactions that provide an enhanced load transfer between polymer chains and CNC, thus improving their properties. The obtained bio‐nanocomposite films are mechanically strong and exhibit improved thermal properties. The addition of 5 wt % CNC within a PVA/CS blend increased the Young's modulus by 105%, the tensile strength by 77%, and the toughness by 68%. Herein, the utilization of Moroccan sugarcane bagasse as raw material to produce high quality CNC has been explored. Additionally, the ability of the as‐isolated CNC to reinforce polymer blends was studied, resulting in the production of the aforementioned bio‐nanocomposite films with improved properties. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42004.