Poly(vinyl alcohol)–lignin blended resin for cellulose‐based composites

Wood has limitations in strength because of its biostructural defects, including vessels. To overcome this limitation, composite materials can be innovated by breaking wood down into cellulose and lignin and reassembling them for bio‐originating strong structural materials. In this study, an ecofriendly resin was developed that was suitable for cellulose‐based composites. To overcome the low dimensional stability of lignin and to increase its interactions with cellulose, it was blended with poly(vinyl alcohol) (PVA). The PVA–lignin resin was characterized with scanning electron microscopy, Fourier transform infrared spectroscopy, thermal analysis, mechanical tensile testing, and lap‐shear joint testing. The adhesion properties of the PVA–lignin resin increased with increasing PVA content. PVA played the role of synthetic polymer and that of linker between the cellulose and lignin, like hemicellulose does in wood. The PVA–lignin resin exhibited a high miscibility, mechanical toughness, and good adhesion properties for nanocellulose composites. © 2018 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 46655.     

Study on flax fiber toughened poly (lactic acid) composites

Poly (lactic acid) (PLA) is a renewable and biodegradable polymer with high modulus, high strength but low toughness. Blending PLA with plant fiber has been believed an available strategy to improve the toughness of PLA. PLA/Flax composites were fabricated by extrusion and injection molding processes. The flax fiber surfaces were modified before blending to improve the compatibility, and the chemical structures of both untreated and treated fiber were characterized by Fourier transform infrared spectroscopy. Results of mechanical test showed that the impact strength and elongation at break of PLA/Flax composites were remarkably higher than PLA. The impact fractures of PLA/Flax composites were also observed by scanning electron microscope. The results showed uniform dispersion of fibers in PLA matrix and good compatibility between treated fibers and PLA matrix. Moreover, it can be observed that crazing propagation was hindered by fibers and transcrystalline developed along fibers by polarized optical microscope. Differential scanning calorimetry analysis was carried out to study the crystallinity of PLA and it was found that incorporation of fiber improved the crystallinity of PLA. The toughening mechanism of PLA/Flax composites was discussed according to the results. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 42573.     

Polypropylene composites obtained from self‐reinforced hybrid fiber system

The purpose of the study was to obtain a composite material with the self‐reinforced structure, which processing provide increased mechanical properties. The composites used in presented work were prepared from the two types of fiber mixtures, both were based on polypropylene fibers, the difference was in used cellulose or wood flour filler. Composites were prepared using the hot compaction method. The presented research describes the effect of the composite composition and processing conditions. The results include the static tension measurements, tensile impact tests and thermal analysis, including: DSC and DMTA. The structure has been studies using the SEM observations. Results of presented studies confirm the self‐reinforcing effect in obtained hybrid composites. It provides in the comparison to the standard wood polymer composites to the higher level of material reinforcement with lower amount of natural filler. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43283.     

Development and characterization of flax fiber reinforced biocomposite using flaxseed oil‐based bio‐resin

In this study, acrylated epoxidized flaxseed oil (AEFO) resin is synthesized from flaxseed oil, and flax fiber reinforced AEFO biocomposites is produced via a vacuum‐assisted resin transfer molding technique. Different amounts of flax fiber and styrene are added to the resin to improve its mechanical and physical properties. Both flax fiber and styrene improve the mechanical properties of these biocomposites, but the flexural strength decreases with an increase in styrene content. The mass increase during water absorption testing is less than 1.5% (w/w) for all of the AEFO‐based biocomposites. The density of the AEFO resin is 1.166 g/cm³, which increases to 1.191 g/cm³ when reinforced with 10% (w/w) flax fiber. The flax fiber reinforced AEFO‐based biocomposites have a maximum tensile strength of 31.4 ± 1.2 MPa and Young's modulus of 520 ± 31 MPa. These biocomposites also have a maximum flexural strength of 64.5 ± 2.3 MPa and a flexural modulus of 2.98 ± 0.12 GPa. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41807.     

Poly(lactic acid)/pulp fiber composites: The effect of fiber surface modification and hydrothermal aging on viscoelastic and strength properties

Poly(lactic acid) (PLA)/kraft pulp fiber (30 wt%) composites were prepared with and without a coupling agent (epoxidized linseed oil, ELO, 1.5 wt%) by injection molding. The non-annealed composite samples, along with lean PLA, were exposed to two hydro-thermal conditions: cyclic 50% RH/90% RH at 23 and 50°C, both up to 42 days. The aging effects were observed by size exclusion chromatography, differential scanning calorimetry, dynamic and tensile mechanical analysis, and fracture surface imaging. ELO temporarily accelerated the material's internal transition from viscous to an increasingly elastic response during the aging at 50°C. ELO also slowed down the tensile strength reduction of the composites at 50°C. These observations were explained with the hydrophobic ELO molecules' coupling and plasticizing effects at fiber/matrix interfaces. No effects were observed at 23°C.     

Modification of wood flour/PLA composites by reactive extrusion with maleic anhydride

MA modified wood flour/PLA composites were prepared by one‐step reactive extrusion, in which wood flour and poly(lactic acid) (PLA) were used as raw material, maleic anhydride (MA) was used as modifier, and dicumyl peroxide (DCP) was used as initiator. The influences of MA concentration on the morphology, thermal stability, rheological, and mechanical properties of the composites were studied. The addition of MA improved the compatibility of the composites significantly. The thermal and rheological results showed that with the increase of the concentration of MA, the thermal stability of the composites decreased, the storage modulus and complex viscosity of the composites also decreased. The MA modified composites had an enhanced mechanical strength compared to the unmodified one. As the concentration of the MA increased, the tensile and flexural strength of the composites first increased and then decreased, and reached a maximum when the concentration of MA was 1 wt %. The MA modified composites showed a better water resistance than the unmodified ones. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43295.     

Bio‐composites for structural applications: Poly‐l‐lactide reinforced with long sisal fiber bundles

Fully bio‐based and biodegradable composites were compression molded from unidirectionally aligned sisal fiber bundles and a polylactide polymer matrix (PLLA). Caustic soda treatment was employed to modify the strength of sisal fibers and to improve fiber to matrix adhesion. Mechanical properties of PLLA/sisal fiber composites improved with caustic soda treatment: the mean flexural strength and modulus increased from 279 MPa and 19.4 GPa respectively to 286 MPa and 22 GPa at a fiber volume fraction of V_f = 0.6. The glass transition temperature decreased with increasing fiber content in composites reinforced with untreated sisal fibers due to interfacial friction. The damping at the caustic soda‐treated fibers‐PLLA interface was reduced due to the presence of transcrystalline morphology at the fiber to matrix interface. It was demonstrated that high strength, high modulus sisal‐PLLA composites can be produced with effective stress transfer at well‐bonded fiber to matrix interfaces. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40999.     

Halloysite nanotubes immobilized by chitosan/tannic acid complex as a green flame retardant for bamboo fiber/poly(lactic acid) composites

In order to develop an environmentally benign flame retardant for bamboo/PLA composites (BPC), chitosan (CS) and tannic acid (TA) were used as cationic and anionic polyelectrolyte respectively to stabilize halloysite nanotubes (HNT) on the surface of bamboo fiber (BF) and poly(lactic acid) (PLA). Mechanical performance tests showed that the flexural properties of BPC were moderately enhanced with the addition of HNT, while the incorporation of CS/TA complex (FR) exhibited a slight increase. The results of thermogravimetric analysis demonstrated that CS/TA complex and HNT improved the thermal stability of the BPC synergistically, which increased the char residue. Limiting oxygen index and cone calorimetry tests were used to study the flammability of BPC and the results showed that the addition of CS/TA complex and HNT had a synergistic effect on the flame retardant performance of BPC materials. The macroscopic and microscopic morphological studies confirmed the formation of HNT layer in the matrix of BPC/5FR@5HNT samples, which facilitated more stabile char residue with the best flame retardant performance.     

Preparation and analysis of poly(l-lactic acid) composites with oligo(d-lactic acid)-grafted cellulose

α-Cellulose extracted from jute fiber was grafted with oligo( d -lactic acid) (ODLA) via a graft polycondensation reaction in the presence of para-toluene sulfonic acid and potassium persulfate in toluene at 130 °C for 9 h under 380 mmHg. ODLA was synthesized by the ring-opening polymerization of d -lactides in the presence of stannous octoate (0.03 wt % lactide) and d -lactic acid at 140 °C for 10 h. Composites of poly( l -lactic acid) (PLLA) with the ODLA-grafted α-cellulose were prepared by the solution-mixing and film-casting methods. The grafting of ODLA onto α-cellulose was confirmed by Fourier transform infrared (FTIR) spectroscopy and scanning electron microscopy (SEM). The analysis of the composites was performed with FTIR spectroscopy, SEM, wide-angle X-ray diffraction, and thermogravimetric analysis. The distribution of the grafted α-cellulose in the composites was uniform and showed better compatibility with PLLA through intermolecular hydrogen bonding. Only homocrystalline structures of PLLA were present in the composites, and the thermal stability increased with increasing percentage of grafted α-cellulose. © 2019 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2019 , 136, 47424.     

Asolectin from soybeans as a natural compatibilizer for cellulose‐reinforced biocomposites from tung oil

The free radical copolymerization of tung oil, divinylbenzene, and n‐butyl methacrylate results in bio‐based thermosetting polymers with tunable properties. Biocomposites have been obtained by the reinforcement of such bio‐based resins with α‐cellulose. Asolectin from soybeans consists of a mixture of natural, polyunsaturated phospholipids. Because of its long, unsaturated fatty acid chains, and the presence of phosphate and ammonium groups, asolectin from soybeans is a good candidate for acting as a natural compatibilizer between the hydrophobic matrix and the hydrophilic reinforcement. In the current work, we investigate the changes in properties resulting from the addition of asolectin to a tung oil‐based polymer reinforced with α‐cellulose. An evaluation of the cure‐kinetics of the tung oil‐based resin has been conducted by dielectric analysis (DEA), and the final biocomposites have been thoroughly characterized by differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), dynamic mechanical analysis (DMA), Soxhlet extraction, and scanning electron microscopy (SEM). © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41833.     

Ultrathin and nanofibers via room temperature electrospinning from trifluoroacetic acid solutions of untreated lignocellulosic sisal fiber or sisal pulp

Lignocellulosic sisal fiber (LSF) and sisal pulp (SP) were electrospun at room temperature from solutions in trifluoroacetic acid (TFA) prepared at concentrations of 2 × 10⁻² g mL⁻¹ and 3 × 10⁻² g mL⁻¹, respectively. Scanning electron microscopy images of the electrospun LSF showed fibers with diameters ranging from 120 to 510 nm. The presence of defects decreased along with increasing the flow rate of the SP solution, which generated nanofibers and ultrathin fibers with diameters in the range of 40–60 (at 5.5 µL min⁻¹) up to 90–200 nm (at 65.5 µL min⁻¹). Despite the known ability of TFA to esterify the hydroxyl groups present in the starting materials, the Fourier transform infrared spectra indicated the absence of trifluoroacetyl groups in the electrospun samples. The thermal stability of the final materials proved suitable for many applications even though some differences were observed relative to the starting materials. This study demonstrated a feasible novel approach for producing nano/ultrathin fibers from lignocellulosic biomass or its main component, which allows for a wide range of applications for these materials. © 2015 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41826.     

Improvement in impact strength of modified cardanol‐bonded cellulose thermoplastic resin by adding modified silicones

The impact strength of cellulose diacetate (CDA) bonded with a modified cardanol (3‐pentadecylphenoxy acetic acid: PAA) was greatly improved up to 9 kJ/m² by adding a relatively small amount of modified silicones while suppressing a decrease in bending strength. In our recent research, this thermoplastic resin (PAA‐bonded CDA) exhibited high rigidity, glass transition temperature, and water resistance. However, its impact strength was insufficient for use in durable products. Therefore, silicones modified with polyether, amino, and epoxy groups were investigated as possible ways to improve the impact strength. The results show that adding polyether‐modified silicone (polyether silicone) with moderate polarity relative to PAA‐bonded CDA resulted in shearing deformation greatly enhances its impact strength while maintaining other properties, including glass transition temperature (T_g), water resistance, and thermoplasticity. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40366.     

Processing and thermal properties of composites based on recycled PET,sisal fibers,and renewable plasticizers

This investigation focuses on the preparation of bio‐based composites from recycled poly (ethylene terephthalate) (PET) and sisal fibers (3 cm, 15 wt %), via thermopressing process. Plasticizers derived from renewable raw materials are used, namely, glycerol, tributyl citrate (TBC) and castor oil (CO), to decrease the melting point of the recycled PET (T_m ∼ 265°C), which is sufficiently high to initiate the thermal decomposition of the lignocellulosic fiber. All used materials are characterized by thermogravimetric analysis and differential scanning calorimetry, and the composites are also characterized via dynamic mechanical thermal analysis. The storage modulus (30°C) and the tan δ peak values of CT [PET/sisal/TBC] indicate that TBC also acts as a compatibilizing agent at the interface fiber/PET, as well as a plasticizer. To compare different processing methods, rheometry/thermopressing and compression molding are used to prepare the recycled PET/sisal/glycerol/CO composites. These two different methods of processing show no significant influence on the thermal properties of these composites. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 40386.     

Composites based on renewable materials: Polyurethane‐type matrices from forest byproduct/vegetable oil and reinforced with lignocellulosic fibers

The use of products and byproducts from the agro‐industry and forest biorefinery is essential for the development of value‐added and low environmental‐impact materials. In this study, polyurethanes were prepared using sodium lignosulfonate (NaLS) and castor oil (CO) as reagents and were used to prepare composites reinforced with lignocellulosic fibers, namely, curaua and coir fibers (30 wt %, 3 cm length, and randomly oriented). The SEM images of fractured surfaces of the composites revealed excellent adhesion at the fiber/matrix interface of both coir and curaua composites, which probably resulted from the favorable interactions between polar groups, as well as amid low polarity domains that are present in both the matrix and the reinforcements. The composites exhibited different impact/flexural and strength/flexural moduli (NaLS/CO/Curaua = 465 Jm^?1/44 MPa/2 GPa; NaLS/CO/Coir = 180 Jm^?1/25 MPa/1 GPa). The higher tensile strength/aspect ratio of the curaua fibers (485 MPa/259) compared with that of the coir fibers (120 MPa/130) most likely contributes to the enhanced performance of its composite. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci., 2013     

Improvement in impact strength of modified cardanol‐bonded cellulose thermoplastic resin by using olefin resins

Impact strength of a modified cardanol‐bonded cellulose thermoplastic resin was greatly improved by using a small amount of olefin resins. As we showed, this thermoplastic resin (3‐pentadecylphenoxy acetic acid (PAA)‐bonded cellulose diacetate (CDA): PAA‐bonded CDA) exhibited high practical properties such as bending strength, heat resistance, and water resistance. However, its impact strength was insufficient for use in durable products. We improved the impact strength of PAA‐bonded CDA by adding hydrophobic olefin resins, such as polyethylene or polypropylene, while maintaining good bending strength and breaking strain. Furthermore, the application of olefin resins also increased water resistance and fluidity. © 2013 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2014 , 131, 39829.     

Building and origin of bio‐based bismaleimide resins with good processability,high thermal,and mechanical properties

Bio‐based high performance thermosetting resins have been urgently required by cutting‐edge fields for meeting sustainable development. A new kind of high performance thermosetting resins (BA‐n) with good processability, high thermal resistance, and mechanical properties was developed based on 4,4′‐bismaleimidodiphenylmethane (BDM) and renewable bis(5‐allyloxy)‐4‐methoxy‐2‐methylphenyl)methane (ABE) from bio‐based lignin derivative. The effect of the molar ratio of allyl to imide (n) on structures and properties of BA resins were systematically researched. BA‐n resins have much better processability, thermal, and mechanical properties than their petroleum‐based counterparts, 2,2′‐diallylbisphenol A‐modified BDM (BD‐n) resins. Compared with BD‐0.86, the best available bismaleimide (BMI) resin, BA‐0.86 not only has 6 h longer process window and 13.7 °C higher glass transition temperature, but also owns the highest flexural strength and modulus among all bio‐based allyl compound‐modified BMI resins reported. The origin behind these attractive performances of BA resins is revealed by discussing the unique crosslinked structure. © 2017 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2018 , 135, 45947.     

Recycling of wood fiber‐reinforced HDPE by multiple reprocessing

The mechanical recycling of high‐density polyethylene (HDPE) reinforced with wood fiber was studied by means of repeated injection moulding. The change in properties during the recycling was monitored by tensile and flexural tests, Charpy impact tests, differential scanning calorimetry (DSC), thermogravimetric analysis (TGA), FTIR spectroscopy, and by measuring the fiber lengths. Tests were also done where injection moulding was combined with subsequent accelerated thermo‐oxidative ageing and thereafter repeated numerous times. The results showed that the HDPE composites were relatively stable toward both the ageing conditions and the repeated injection moulding. The change of the mechanical properties was mainly observed as an increased elongation at max. © 2016 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2016 , 133, 43877.     

Nanomechanical properties and thermal stability of recycled cellulose reinforced starch–gelatin polymer composite

Samples of starch?gelatin polymer reinforced with 5% of recycled cellulose were prepared using an extrusion‐compression molding process. Nanoindentation and atomic force acoustic microscopy (AFAM) techniques were used to study the effect of reinforcement at nanoscale level. Nanoindentation tests show a 163% increase in hardness and 123% of elastic modulus enhancement after recycled cellulose inclusion. AFAM shows that distribution of recycled cellulose into the polymer matrix is rather homogeneous at nanoscale which improves load transfer. Thermogravimetric analysis indicates an increase in thermal stability of the cellulose reinforced polymer matrix samples. © 2014 Wiley Periodicals, Inc. J. Appl. Polym. Sci. 2015 , 132, 41787.     

Fire retardant cellulose aerogel with improved strength and hydrophobic surface by one-pot method

Bio-based materials with multifunctional performance are getting immense attention nowadays for their environment friendly and renewable character. Inspired by toughening effect of graphene nanosheets and borate chemistry, a simple in-situ borate crosslinking in water and freeze-drying method was employed to fabricate a fire retarded bio-based aerogel. The structure of the material was evaluated and analysis by SEM, XRD, FTIR, Raman and XPS. Importantly, the bio-based aerogel has improved strength and adsorption properties due to unique structure. The compressive strength of rGO(reduced graphene oxide) + CMC (carboxymethyl cellulose) aerogel could reach 128 ± 2.1 kPa which is five times that of neat CMC aerogel. The bio-based aerogel can load more than 2500 times of self-weight. The adsorption capacity for organic solvents and oil of rGO+CMC aerogel is also greatly improved by a little rGO (1%) introducing due to its unique porous structure and hydrophobic nature of rGO. Additionally, rGO+CMC aerogel is also found fire resistant with relatively low thermal conductivity due to the borate and GO introduction.     

Enhanced biodegradation and processability of biodegradable package from poly(lactic acid)/poly(butylene succinate)/rice-husk green composites

This work aims to study the possibility to process PLA/PBS/RH green composites into hexagonal plant-pots employing a large-scale industrial operation using injection molding. Green composites based on poly(lactic acid) (PLA), poly(butylene succinate) (PBS), and rice husk (RH) with various RH contents (10–30%wt.) were produced successfully using a twin-screw extruder. The compatibility of RH-matrix was improved by chemical surface modifications using a coupling agent. RH was analyzed as an effective filler for PLA to develop green composites with low cost, high biodegradability, improved processability, and comparable mechanical properties as unfilled PLA. With increasing RH content, tensile modulus of the composites increased gradually. The addition of PBS, at PLA/PBS ratio of 60/40, improved the elongation at break and impact strength of PLARH30 by 55% and 7.1%, respectively. The suitable processing temperatures for PLA decreased from 220–230°C to 170–180°C when 30%wt. RH was composited into PLA matrix and were further reduced when PBS was applied. After biodegradation via either enzymatic degradation or hydrolysis, surface erosion with a large number of voids, mass loss, and the substantial decrease in tensile strength of all the composites were observed. In addition, the biodegradation of the composites has been improved by the addition of either RH or PBS.