Continuous cellulose fiber-reinforced cellulose ester composites. II. Fiber surface modification and consolidation conditions

We prepared thermoplastic composite panels using solution impregnation of continuous lyocell (regenerated cellulose) fibers with a cellulose mixed-ester (cellulose acetate butyrate) matrix. We examined both fiber-matrix adhesion and melt consolidation in an effort to produce uniform panels having low void content and high mechanical strength. We characterized the effect of surface modification by acetylation on interfacial adhesion between the cellulose fiber and cellulose ester. Whereas wood fiber acetylation had previously been observed to result in significant strength gains in (discontinuous) wood fiber- reinforced composites (with the same matrix material), we did not observe a similar increase in strength in the continuous lyocell cellulose fiber system. This suggests that interfacial stress transfer is not a limitation in this system. This was confirmed by microscopic examination of the fracture surfaces, which indicated that fiber-matrix adhesion was considerable in the absence of fiber surface modification. We then systematically varied melt consolidation conditions (temperature, pressure and time) in an attempt to define optimum consolidation parameters by using design of experiments (DOE) methodology. We measured both interlaminar shear strength (ILSS) and composite void volume. We found that a minimal void content (ca. 2.83 vol. %) occurred at moderate temperatures (200°C), low consolidation pressures (81.4kPa) and long press times (13min). This was also where we maximized the interlaminar shear strength (ILSS) at a value of 16.3MPa. This agrees with the regression model predictions. We observed the highest tensile properties at the ILSS and void-volume optimal-consolidation condition: a tensile modulus of 22GPa and tensile strength of 246MPa were obtained.     

Effect of fiber length and composition on mechanical properties of carbon fiber‐reinforced polybenzoxazine

The mechanical strength and modulus of chopped carbon fiber (CF)‐reinforced polybenzoxazine composites were investigated by changing the length of CFs. Tensile, compressive, and flexural properties were investigated. The void content was found to be higher for the short fiber composites. With increase in fiber length, tensile strength increased and optimized at around 17 mm fiber length whereas compressive strength exhibited a continuous diminution. The flexural strength too increased with fiber length and optimized at around 17 mm fiber length. The increase in strength of composites with fiber length is attributed to the enhancement in effective contact area of fibers with the matrix. The experimental results showed that there was about 350% increase in flexural strength and 470% increase in tensile strength of the composites with respect to the neat polybenzoxazine, while, compressive properties were adversely affected. The composites exhibited an optimum increase of about 800% in flexural modulus and 200% in tensile modulus. Enhancing the fiber length, leads to fiber entanglement in the composites, resulted in increased plastic deformation at higher strain. Multiple branch matrix shear, debonded fibers and voids were the failures visualized in the microscopic analyses. Defibrillation has been exhibited by all composites irrespective of fiber length. Fiber debonding and breaking were associated with short fibers whereas clustering and defibrillation were the major failure modes in long fiber composites. Increasing fiber loading improved the tensile and flexural properties until 50–60 wt% of fiber whereas the compressive property consistently decreased on fiber loading. Copyright © 2008 John Wiley & Sons, Ltd.     

Morphology control of poly(lactic) acid/polypropylene blend composite by using silanized cellulose fibers extracted from coir fibers

The objective of this work is the use of cellulose fibers extracted from coir fibers as Janus nanocylinders to suppress the phase retraction and coalescence in poly(lactic) acid/polypropylene bio-blend polymers via prompting the selective localization of cellulose fibers at the interface using chemical modification. The untreated and modified cellulose fibers extracted from coir fibers using a silane molecule (tetraethoxysilane) were used as reinforcement and as Janus nanocylinder at two weight contents (2.5 wt% and 5 wt%) to manipulate the morphology of the bio-blends. Their bio-composites with PLA-PP matrix were prepared via melt compounding (at PLA/PP: 50/50). The treatment effect on component interaction and the bio-composites properties have been studied via Scanning electron microscopy, infrared spectroscopy, and differential calorimetry analysis. The mechanical and rheological properties of nanocomposites were similarly assessed. Young's modulus and tensile strength of PLA-PP nanocomposites reinforced by silanized cellulose fibers show a great enhancement as compared to a neat matrix. In particular, there was a gain of 18.5% in Young's modulus and 11.21% in tensile strength for silanized cellulose fiber-based bio-blend composites at 5 wt%. From the rheological point of view, it was found that the silanized cellulose fibers in PLA-PP at both fibers loading enhances the adhesion between both polymers leading to tuning their morphology from sea-island to the continuous structures with the appearance of PLA microfibrillar inside of bio-composites. This change was reflected in the relaxation of the chain mobility of the bio-blend composites.

     

Short Twaron aramid fiber reinforced thermoplastic polyurethane

Mechanical, dynamic mechanical, and rheological behaviors of a short p‐aramid fiber reinforced thermoplastic polyurethane (TPU) have been studied in the range of 0–30 wt% of fibers. The tensile strength of the composite is improved slightly at higher fiber content with a minimum at around 10 wt% of fibers. The addition of fibers markedly reduces elongation at break and entails a steady increase in the elastic modulus, but decreases the wear resistance of the matrix. Storage modulus (E′) is increased and the shapes of loss tangent (tan δ) peaks point to a possible fiber–matrix interaction. Rheological studies show a power law behavior for all composites and increased viscosity with fiber loading. Study of the tensile and cryogenic fracture surfaces by scanning electron microscopy (SEM) indicates good correlation between the modes of failure and strength of the composites. The micrographs reveal good interfacial adhesion and extensive peeling and fibrillation of the fibers in the compounded and fractured composites. Theoretical models have been used to fit the experimental modulus data. Copyright © 2008 John Wiley & Sons, Ltd.     

Continuous cellulose fiber-reinforced cellulose ester composites III. Commercial matrix and fiber options

Thermoplastic composites were prepared using two continuous regenerated cellulose fiber types, rayon and lyocell, and with several different commercially-available thermoplastic cellulose esters as matrix. Matrix options included cellulose acetate propionate (CAP), and several cellulose acetate butyrates (CAB) with different butyryl content, having different molecular weights and different methods of plasticization (adipates and very low molecular weight cellulose ester fractions). Choice of cellulose ester type was generally found to have little or no effect on mechanical properties. A significant effect, however, was revealed for fiber type. The lyocell-based composites thereby were reflective of the greater stiffness of a fiber produced from anisotropic solution state. Their modulus consistently exceeded 20GPa whereas the rayon fiber-based composites had moduli between 6 and 8GPa. The latter, however, possessed failure strains that were 3 to 4 times greater than their stiffer counterparts.     

Mechanical properties of phenol/formaldehyde resin composites reinforced by cellulose microcrystal with different aspect ratio extracted from sisal fiber

Sisal cellulose fiber (SCF) and sisal fiber cellulose microcrystal (SFCM), produced with sulfate pulping method and ball‐milling approach separately, were in‐situ polymerized and dispersed into phenol/formaldehyde (PF) resin, to manufacture SCF/PF and SFCM/PF composites via rolling and molding method and investigate the effect of SCF and SFCM on the impact, flexural, and dynamic mechanical properties of the SCF/PF and SFCM/PF composites. As a result, under the condition of same content, SFCM could preferably enhance these properties maybe resulting from the better dispersion in resin matrix than SCF. In particular, when SFCM content was 7%, the impact strength and equilibrium relaxation modulus of the SFCM/PF composite were increased by 26.5% and 37.7%, while the creep deformation was decreased by 26.5%. In addition, when SFCM content was 5%, the flexural strength, initial storage modulus and glass transition temperature of SFCM/PF composite were increased by 8.5%, 22.6%, and 13°C. Copyright © 2016 John Wiley & Sons, Ltd.     

Effects of cellulose whiskers on properties of soy protein thermoplastics

Environmentally-friendly SPI/cellulose whisker composites were successfully prepared using a colloidal suspension of cellulose whiskers, to reinforce soy protein isolate (SPI) plastics. The cellulose whiskers, having an average length of 1.2 microm and diameter of 90 nm, respectively, were prepared from cotton linter pulp by hydrolyzing with sulfuric acid aqueous solution. The effects of the whisker content on the morphology and properties of the glycerol-plasticized SPI composites were investigated by scanning electron microscopy, dynamic mechanical thermal analysis, differential scanning calorimetry, ultraviolet-visible spectroscopy, water-resistivity testing and tensile testing. The results indicated that, with the addition of 0 to 30 wt.-% of cellulose whiskers, strong interactions occurred both between the whiskers and between the filler and the SPI matrix, reinforcing the composites and preserving their biodegradability. Both the tensile strength and Young's modulus of the SPI/cellulose whisker composites increased from 5.8 to 8.1 MPa and from 44.7 to 133.2 MPa, respectively, at a relative humidity of 43%, following an increase of the whisker content from 0 to 30 wt.-%. Furthermore, the incorporation of the cellulose whiskers into the SPI matrix led to an improvement in the water resistance for the SPI-based composites.     

The effect of fiber content on the mechanical and thermal expansion properties of biocomposites based on microfibrillated cellulose

A new method to obtain composites of phenolic resin reinforced with microfibrillated cellulose with a wide fiber content was established and the mechanical properties were evaluated by tensile test. A linear increase in Young’s modulus was observed at fiber contents up to 40 wt%, with a stabilizing tendency for higher fiber percentages. These results were ratified by measurements of the coefficient of thermal expansion (CTE) relative to fiber content, which indicated a strong thermal expansion restriction rate below 60 wt% fiber content, indicating the effective reinforcement attained by the cellulose microfibrils. The low CTE achieved of 10 ppm/K is one of the important properties of cellulose composites.     

Reinforcement of aligned cellulose fibers by lignin-polyester copolymers

With an ever-increasing attention on the climate change and the growing amount of plastic wastes generated, the search for an alternative to the petroleum-based plastics has never been as imperative. Inspired by the structure of natural wood, we aim to reproduce artificial equivalent using modified lignin and cellulose acetate. As natural wood are made up of an aggregation of fibers, electrospinning was used to produce the fiber component. Besides exploring the influence of various polymers on the properties of the eventual fibers, its properties were also examined in terms of its orientation – random and aligned. The addition of lignin copolymers was shown to remarkably improve the tensile strength and the Young’s modulus of cellulose acetate fibers up to 500% and 7,000% respectively. In contrast to the random fibers, the aligned fibers demonstrated better tensile strength and Young’s modulus which could be attributed to the higher crystallinity. Among the fibers, the longitudinal aligned C.A. + Lig-PHB fibers exhibited the best tensile strength and Young’s modulus which could be explored for load bearing applications.     

Effect of surface treatment with potassium permanganate on ultra-high molecular weight polyethylene fiber reinforced natural rubber composites

The effects of surface treatment using potassium permanganate on ultra-high molecular weight polyethylene (UHMWPE) fibers reinforced natural rubber (NR) composites were investigated. The results showed the surface roughness and the oxygen-containing groups on the surface of the modified fibers were effectively increased. The NR matrix composites were prepared with as-received and modified UHMWPE fibers added 0–6 wt%. The treated fibers increased the modulus and tensile stress at a given elongation. The tear strength increased with increasing fiber mass fraction, attained maximum values at 4 wt%. The hardness of composites exhibited continuous increase with increasing the fiber content. The dynamic mechanical tests showed that the storage modulus and the tangent of the loss angle were decreased in the modified UHMWPE fibers/NR composites. Several micro-fibrillations between the treated fiber and NR matrix were observed, which meant the interfacial adhesion strength was improved.     

A study of PP/PET composites: Factorial design,mechanical and thermal properties

Due to the economic importance of polypropylene (PP) and polyethylene terephthalate (PET), and the large amount of composites made with PP matrix and recycled PET as reinforcing material; an investigation was performed regarding the mechanical and thermal behavior of PP composites containing recycled polyethylene terephthalate fibers (rPET). Interfacial adhesion between the two materials was achieved by adding a compatibilizer, maleic anhydride grafted polypropylene, PP-g-MA. Mechanical behavior was assessed by tensile, flexural, impact and fatigue tests, and thermal behavior by HDT (Heat Deflection Temperature). Fractured surfaces and fiber were investigated by scanning electron microscopy. Multiple regression statistical analysis was performed to interpret interaction effects of the variables. Tensile strength, tensile modulus, flexural strength, flexural modulus and HDT increased after rPET fiber incorporation while strain at break, impact strength and fatigue life decreased. Addition of compatibilizer increased tensile strength, flexural strength and flexural modulus, fatigue life and HDT while tensile modulus, strain at break and impact strength decreased. However, at low fiber content, the impact strength increased, probably due to nucleation effects on PP.     

Tensile Testing of Single Regenerated Cellulose Fibres

Summary: A tensile testing set-up was developed for the determination of the elastic modulus, tensile strength, and failure strain of single regenerated cellulose fibres. Since the accuracy of strain measurement is crucial for the measured elastic modulus and failure strain, strain measurements were performed mechanically and with a non-contacting optical method in parallel. The optical validation of mechanical strain measurement showed an agreement of measured strain >99%, confirming the accuracy and usefulness of the set-up and sample geometry developed for the test series.     

Biocomposites based on Alfa fibers and starch‐based biopolymer

Biocomposite materials based on Alfa cellulose fibers (esparto grass plant) as reinforcing element and starch‐based biopolymer matrix were prepared and characterized in terms of mechanical performance, thermal properties, and water absorbance behavior. The fibers and the matrix were first mixed in the melted state under mechanical shearing using a plastograph and the obtained composites were molded by injection process. The tensile mechanical analysis showed a linear increase of the composite flexural and tensile modulus upon increasing the fiber content, together with a sharp decrease of the elongation at break. The fibers′ incorporation into the biopolymer matrix brings about an enhancement in the mechanical strength and the impact strength of the composite. Dynamic mechanical thermal analysis (DMTA) investigation showed two relaxations occurring at about ?30 and 35°C. The addition of Alfa fibers enhanced the storage modulus E′ before and after T_α, which is consistent with the reinforcing effect of Alfa cellulose fibers. Copyright © 2008 John Wiley & Sons, Ltd.     

The transparency and mechanical properties of cellulose acetate nanocomposites using cellulose nanowhiskers as fillers

Cellulose nanowhiskers (CNWs) were chemically modified by acetylating to obtain acetylated cellulose nanowhiskers (ACNWs) which could be well dispersed in acetone. The chemical modification was limited only on the surface of CNWs which was confirmed by transmission electron microscopy (TEM) and X-ray diffraction (XRD). Surface substitution degree of ACNWs was evaluated to be 0.45 through X-ray photoelectron spectroscopy (XPS). Fully bioresource-based nanocomposite films were manufactured by incorporation of ACNWs into cellulose acetate (CA) using a casting/evaporation technique. Scanning electron microscope (SEM) demonstrated that ACNWs dispersed well in the CA matrix, which resulted in high transparency of all CA nanocomposites. The tensile strength, Young’s modulus and strain at break of all CA nanocomposites exhibited simultaneous increase in comparison with neat CA matrix. At the content of 4.5 wt% ACNWs, the tensile strength, Young’s modulus and strain at break of the CA nanocomposite film were increased by 9, 39, and 44 % respectively.     

Liquid ammonia treatment of (cationic) nanofibrillated cellulose/vermiculite composites

Liquid ammonia was used to treat films of nanofibrillated cellulose (NFC), trimethylammonium-modified NFC (TMA-NFC), and their composites with vermiculite. Crystal structure, mechanical properties, water vapor permeation and water vapor adsorption of the resulting materials were investigated. Upon treatment, the crystal structure of (TMA-)NFC both in presence and absence of vermiculite changed from cellulose I to III. With the exception of TMA-NFC/vermiculite composites, pronounced effects on the addressed mechanical properties arose after exposure of the materials to ammonia. Furthermore, treatment of composite films with ammonia led to a distinct decrease in water vapor permeation. Remarkably, TMA-NFC/vermiculite composites films show the best water vapor barrier properties, highest tensile strength and highest elastic modulus after treatment with liquid ammonia. This is regarded to be at least partially a consequence of electrostatic attraction between the positively charged ammonium groups in TMA-NFC and the anionic silicate layers of vermiculite. © 2013 Wiley Periodicals, Inc. J Polym Sci Part B: Polym Phys, 2013     

Tensile Properties and Morphology of Oil Palm Empty Fruit Bunch Regenerated Cellulose Biocomposite Films

The regenerated cellulose (RC)biocomposite films were prepared using casting method where oil palm empty fruit bunch (OPEFB) and microcrystalline cellulose (MCC) were dissolved in N-dimethylacetamide/lithium chloride (DMAc/LiCl)solution. The increasing of OPEFB contents up to 2 wt% increased the tensile strength and modulus of elasticity of RC biocomposite films while the elongation at break decreased. However, at 3 and 4 wt% of OPEFB content, the tensile strength and modulus of elasticity decreased with increases OPEFB content, but elongation at break increased. The increment of tensile strength and modulus of elasticity at 2 wt% is due to the OPEFB fiber that partially dissolved and dispersed with the OPEFB matrix. The morphology studies illustrate that at 2 wt% of OPEFB content of biocomposite films surface consists less voids and agglomerations than at 4 wt%. This can be considered the RC filler was partially dispersed with the RC matrix in the biocomposite films.     

Sugar beet cellulose nanofibril-reinforced composites

Cellulose was isolated from sugar beet chips, a by-product of sugar production, by wet chemistry. Further processing of the cellulose with a high-pressure homogeniser led to the disruption of cell walls into nanofibrils. Cellulose sheets obtained by casting and slow evaporation of water showed higher strength and stiffness when homogenised cellulose was used compared to unhomogenised cellulose. These cellulose sheets showed significantly better mechanical performance than Kraft paper tested for reference. The addition of cellulose nanofibrils to a polyvinyl alcohol and a phenol-formaldehyde matrix, respectively, demonstrated excellent reinforcement properties. The best mechanical performance was achieved for a composite with a phenol-formaldehyde resin content of 10%, which showed a tensile strength of 127 MPa, a modulus of elasticity of 9.5 GPa, and an elongation at break of 2.9%.     

Effect of Chemical Treatment and Fiber Loading on Mechanical Properties of Borassus (Toddy Palm) Fiber/Epoxy Composites

The aim of the present study was to investigate and compare the mechanical properties of untreated and chemically modified Borassus fiber–reinforced epoxy composites. Composites were prepared by the hand lay-up process by reinforcing Borassus fibers with epoxy matrix. To improve the fiber-matrix adhesion properties, alkali (NaOH) and alkali combined with silane (3-aminopropyltriethoxysilane) treatment of the fiber surface was carried out. Examinations through Fourier transform-infrared spectroscopy and scanning electron microscopy (SEM) were conducted to investigate the structural and physical properties of the Borassus fibers. Tensile properties such as modulus and strength of the composites made with chemically modified and untreated Borassus fibers were studied using a universal testing machine. Based on the experimental results, it was found that the tensile properties of the Borassus-reinforced epoxy composites were significantly improved as compared with the neat epoxy. It was also found that the fiber treated with a combination of alkali and silane exhibited superior mechanical properties to alkali-treated and untreated fiber composites. The nature of the fiber/matrix interface was examined through SEM of cryo-fractured samples. Chemical resistance of composites was also found to be improved with chemically modified fiber composites.     

Short cellulose nanofibrils as reinforcement in polyvinyl alcohol fiber

Short cellulose nanofibrils (SCNF) were investigated as reinforcement for polyvinyl alcohol (PVA) fibers. SCNF were mechanically isolated from hard wood pulp after enzymatic pretreatment. Various levels of SCNF were added to an aqueous PVA solution, which was gel-spun into continuous fibers. The molecular orientation of PVA was affected by a combination of wet drawing during gel spinning and post-hot-drawing at a high temperature after drying. A maximum total draw ratio of 27 was achieved with various SCNF contents investigated. The PVA crystal orientation increased when small amounts of SCNF were added, but decreased again as the SCNF content was increased above about 2 or 3 %, likely due to SCNF percolation resulting in network formation that inhibited alignment. SCNF fillers were effective in improving PVA fiber tensile properties (i.e., ultimate strength and elastic modulus). For example, the ultimate strength and modulus of PVA/SCNF composite fiber with a SCNF weight ratio of 6 were nearly 60 and 220 % higher than that of neat PVA. Shifts in the Raman peak at ~1,095 cm^?1, which were associated with the C–O–C glycosidic bond of SCNF, indicated good stress-transfer between the SCNF and the PVA matrix due to strong interfacial hydrogen bonding. Cryogenic fractured scanning electron microscopy images of filled and unfilled PVA fibers showed uniform SCNF dispersion.     

Polymer matrix influence on stability of wood polymer composites

The aim of the presented work is to show the influence of the various polymer matrices and the different amounts of the cellulose filler on the composites properties. Samples based on polypropylene, polystyrene, polyoxymethylene, acrylonitrile butadiene styrene, polyester resin, and polylactic acid with different contents of cellulose fibers were prepared by injection molding process. The mechanical and dielectric properties of these composites were studied in order to check whether investigated wood polymer composites fulfill requirements for their application in electrical devices. For all tested composites, a linear increase of modulus with cellulose content was observed. Addition of cellulose to the tested polymers significantly reduces strain at break. In the case of polypropylene and polyoxymethylene composites, the tensile strength increases with the content of the filler. For other materials, there is an inverse relationship, namely the addition of cellulose decreases the tensile strength. The electrical strength decrease was observed with increased cellulose content for the majority of the investigated composites. Polar groups incorporated by cellulose fibers have led to dielectric constant increase. Furthermore, aging of composites in mineral oil and evaluation of water uptake for wood–plastic samples were performed. Wood polymer composites have changed significantly after aging. The water diffusion coefficients were determined, and the significant influence of the amount of cellulose on the water absorption was shown. Copyright © 2015 John Wiley & Sons, Ltd.