Comparison of Polylactic Acid/Kenaf and Polylactic Acid/Rise Husk Composites: The Influence of the Natural Fibers on the Mechanical, Thermal and Biodegradability Properties

This paper investigates and compares the performances of polylactic acid (PLA)/kenaf (PLA-K) and PLA/rice husk (PLA-RH) composites in terms of biodegradability, mechanical and thermal properties. Composites with natural fiber weight content of 20% with fiber sizes of less than 100 μm were produced for testing and characterization. A twin-screw extrusion was used to compound PLA and natural fibers, and extruded composites were injection molded to test samples. Flexural and Izod impact test, TGA, soil burial test and SEM were used to investigate properties. All results were compared to a pure PLA matrix sample. The flexural modulus of the PLA increased with the addition of natural fibers, while the flexural strength decreased. The highest impact strength (34 J m⁻¹), flexural modulus (4.5 GPa) and flexural strength (90 MPa) were obtained for the composite made of PLA/kenaf (PLA-K), which means kenaf natural fibers are potential to be used as an alternative filler to enhance mechanical properties. On the other hand PLA-RH composite exhibits lower mechanical properties. The impact strength of PLA has decreased when filled with natural fibers; this decrease is more pronounced in the PLA-RH composite. In terms of thermal stability it has been found that the addition of natural fibers decreased the thermal stability of virgin PLA and the decrement was more prominent in the PLA-RH composite. Biodegradability of the composites slightly increased and reached 1.2 and 0.8% for PLA-K and PLA-RH respectively for a period of 90 days. SEM micrographs showed poor interfacial between the polymer matrix and natural fibers.     

Sustainable Bio-Composites from Renewable Resources: Opportunities and Challenges in the Green Materials World

Sustainability, industrial ecology, eco-efficiency, and green chemistry are guiding the development of the next generation of materials, products, and processes. Biodegradable plastics and bio-based polymer products based on annually renewable agricultural and biomass feedstock can form the basis for a portfolio of sustainable, eco-efficient products that can compete and capture markets currently dominated by products based exclusively on petroleum feedstock. Natural/Biofiber composites (Bio-Composites) are emerging as a viable alternative to glass fiber reinforced composites especially in automotive and building product applications. The combination of biofibers such as kenaf, hemp, flax, jute, henequen, pineapple leaf fiber, and sisal with polymer matrices from both nonrenewable and renewable resources to produce composite materials that are competitive with synthetic composites requires special attention, i.e., biofiber–matrix interface and novel processing. Natural fiber–reinforced polypropylene composites have attained commercial attraction in automotive industries. Natural fiber—polypropylene or natural fiber—polyester composites are not sufficiently eco-friendly because of the petroleum-based source and the nonbiodegradable nature of the polymer matrix. Using natural fibers with polymers based on renewable resources will allow many environmental issues to be solved. By embedding biofibers with renewable resource–based biopolymers such as cellulosic plastics; polylactides; starch plastics; polyhydroxyalkanoates (bacterial polyesters); and soy-based plastics, the so-called green bio-composites are continuously being developed.     

Effect of Fiber Surface Treatments on Thermo-Mechanical Behavior of Poly(Lactic Acid)/Phormium Tenax Composites

In the present study, Phormium Tenax fiber reinforced PLA composites were processed by injection molding and twin screw compounding with a fiber content ranging from 10 to 30 wt%. Three surface treatment methods have been used to improve the Phormium Tenax fiber-matrix interfacial bonding that are as follows: (1) aqueous alkaline solution, (2) silane coupling agent, and (3) a combination of alkaline and silane treatment. The mechanical, thermal and morphological properties of the resulting composites were investigated. The results have shown that the moduli of surface treated fiber reinforced composites are lower than the ones obtained for untreated composites (as a consequence of the decrease in fiber modulus caused by the chemical treatments) and no significant increase in strength was observed for any of the composites compared to neat PLA. SEM micrographs of composite fractured surfaces confirmed an improvement in the interfacial strength, which was insufficient nonetheless to significantly enhance the mechanical behavior of the resulting composites. Results from thermogravimetric analysis and differential scanning calorimetry suggest that surface treatment of Phormium affects the ability of PLA to cold crystallize, and the thermal stability of the composites at the different fiber contents was reduced with introduction of alkali and silane treated Phormium fibers.     

Chemical Treatments of Natural Fiber for Use in Natural Fiber-Reinforced Composites: A Review

Studies on the use of natural fibers as replacement to man-made fiber in fiber-reinforced composites have increased and opened up further industrial possibilities. Natural fibers have the advantages of low density, low cost, and biodegradability. However, the main disadvantages of natural fibers in composites are the poor compatibility between fiber and matrix and the relative high moisture sorption. Therefore, chemical treatments are considered in modifying the fiber surface properties. In this paper, the different chemical modifications on natural fibers for use in natural fiber-reinforced composites are reviewed. Chemical treatments including alkali, silane, acetylation, benzoylation, acrylation, maleated coupling agents, isocyanates, permanganate and others are discussed. The chemical treatment of fiber aimed at improving the adhesion between the fiber surface and the polymer matrix may not only modify the fiber surface but also increase fiber strength. Water absorption of composites is reduced and their mechanical properties are improved.     

Reactively Compatibilized Cellulosic Polylactide Microcomposites

Poly(lactic acid) (PLA) possesses a suite of favorable material properties that are enabling its penetration into diverse markets (e.g., as packaging material or textile fibers). In order to increase the range of applications for this material, it is necessary to modify its properties and for certain applications, reduce its cost. The introduction of fibers into a polymeric matrix is an established route towards property enhancement provided good dispersion and intimate interfacial adhesion can be achieved. In addition, cellulosic microfibers are obtainable at low to moderate cost. In this study, reactive compatibilization of cellulosic fibers with PLA is pursued. Hydroxyl groups available on the surface of cellulosic fibers are used to initiate lactide polymerization. Various processing strategies are investigated: (1) blending preformed PLA with the fiber material, (2) through a one-step process in which lactide is polymerized in the presence of the fibers alone, or (3) reactive compatibilization in the presence of preformed high molecular weight polymer. The results show that materials prepared by simultaneous introduction of lactide and preformed high molecular PLA at the beginning of the reaction possess superior mechanical properties compared to composites made by either purely mechanical mixing or solely polymerization of lactide in the presence of fibers. The modulus of materials containing 25% fibers which are prepared by reactive compatibilization of 30% preformed PLA and 70% lactide (30/70 P/L) improves by 53% compared to the homopolymer, whereas 36% reinforcement can be achieved upon purely mechanical mixing. A further increase to 35% fiber loading leads to a reduction in modulus due to an excess in initiating groups. The same trend was observed in systems containing 65% preformed PLA and 35% lactide (65/35 P/L) with an overall achievable reinforcement that was slightly lower.     

Analysis of Flax and Cotton Fiber Fabric Blends and Recycled Polyethylene Composites

Manufacturing composites with polymers and natural fibers has traditionally been performed using chopped fibers or a non-woven mat for reinforcement. Fibers from flax (Linum usitatissimum L.) are stiff and strong and can be processed into a yarn and then manufactured into a fabric for composite formation. Fabric directly impacts the composite because it contains various fiber types via fiber or yarn blending, fiber length is often longer due to requirements in yarn formation, and it controls the fiber alignment via weaving. Composites created with cotton and flax-containing commercial fabrics and recycled high-density polyethylene (HDPE) were evaluated for physical and mechanical properties. Flax fiber/recycled HDPE composites were easily prepared through compression molding using a textile preform. This method takes advantage of maintaining cotton and flax fiber lengths that are formed into a yarn (a continuous package of short fibers) and oriented in a bidirectional woven fabric. Fabrics were treated with maleic anhydride, silane, enzyme, or adding maleic anhydride grafted polyethylene (MAA-PE; MDEX 102-1, Exxelor^® VA 1840) to promote interactions between polymer and fibers. Straight and strong flax fibers present problems because they are not bound as tightly within yarns producing weaker and less elastic yarns that contain larger diameter variations. As the blend percentage and mass of flax fibers increases the fabric strength, and elongation generally decrease in value. Compared to recycled HDPE, mechanical properties of composite materials (containing biodegradable and renewable resources) demonstrated significant increases in tensile strength (1.4–3.2 times stronger) and modulus of elasticity (1.4–2.3 times larger). Additional research is needed to improve composite binding characteristics by allowing the stronger flax fibers in fabric to carry the composites load.     

Potential of <Emphasis Type="Italic">pinhão</Emphasis> Coat as Constituents of Starch Based Films Using Modification Techniques

The potential of lignocellulosic fibers obtained by dry grinding of pinhão coat as fillers in starch filmogenic solutions for packaging applications was evaluated in this work. To improve the incorporation of this waste into the starch solutions different physical and chemical treatments were conducted. Thereafter, morphology, chemical structure, crystallinity and water absorption of the pinhão coat powders were determined. The composites were also characterized regarding their morphology, chemical structure, crystallinity, mechanical properties, water vapor permeability and hydrophilicity. Poor fiber/matrix adhesion and high water absorption of the fibers were evidenced. Consequently, water vapor permeability of composites was increased by incorporating the fibers. Moreover, mechanical properties were improved and the morphological results were used to support the water absorption differences among the powders. Regarding the food packaging applications, starch/pinhão coat composites appeared as promising materials to reach the requirements of respiring food products.     

Molding Method, Thermal and Mechanical Properties of Jute/PLA Injection Molding

Natural composites have been important materials system due to preservation of earth environments. Natural fibers such as jute, hemp, bagasse and so on are very good candidate of natural composites as reinforcements. On the other hand regarding matrix parts thermosetting polymer and thermoplastic polymer deriver form petrochemical products are not environmental friendly material, even if thermoplastic polymer can be recycled. In order to create fully environmental friendly material (FEFM) biodegradable polymer which can be deriver from natural resources is needed. Therefore poly(lactic acid) (PLA) polymer is very good material for the FEFM. In this paper jute fiber filled PLA resin (jute/PLA) composites was fabricated by injection moldings and mechanical properties were measured. It is believable that industries will have much attention to FEFM, so that injection molding was adopted to fabricate the composites. Long fiber pellet fabricated by pultrusion technique was adopted to prepare jute/PLA pellet. Because it is able to fabricate composite pellets with relative long length fibers for injection molding process, where, jute yarns were continuously pulled and coated with PLA resin. Here two kinds of PLA materials were used including the one with mold releasing agent and the other without it. After pass through a heated die whereby PLA resin impregnates into the jute yarns and sufficient cooling, the impregnated jute yarns were cut into pellets. Then jute/PLA pellets were fed into injection machine to make dumbbell shape specimens. In current study, the effects of temperature of PLA melting temperature i.e. impregnation temperature and the kinds of PLA were focused to get optimum molding condition. The volume fractions of jute fiber in pellet were measured by several measuring method including image analyzing, density measurement and dissolution methods. Additionally, thermal and mechanical properties were investigated. It is found that 250° is much suitable for jute/PLA long fiber pultrusion process because of its less heat degradation of jute, better impregnation, acceptable mechanical property and higher production efficiency. Additionally the jute fibers seem much effective to increase deflection temperature under load, tensile modulus and Izod strength.     

Effect of <Emphasis Type="Italic">Moringa oleifera</Emphasis> Pod Husk Fibers on the Properties of Gelatin-Based Biocomposite

The objective of this work is to study the feasibility of reinforcing polymer composites by utilizing the biofibers from the agricultural residue of Moringa oleifera pod husks (MOPH). The chemical and physical properties of the fibers were comprehensively investigated to evaluate their potential as a filler in gelatin-based films. The effect of MOPH fiber concentrations of 0, 5, 10, and 15 wt% on the water vapor permeability (WVP), and mechanical and thermal properties of the gelatin-based films was studied. By incorporation of 10 wt% of the MOPH fibers in gelatin, the highest tensile strength and Young’s modulus, and the lowest WVP properties were obtained. Scanning electron microscopy (SEM) photographs indicated good interfacial adhesion between the fibers and the gelatin matrix. TGA of the biocomposites revealed an improvement of thermal stability. Moreover, under accelerated weathering, the gelatin-MOPH-10% biocomposite degraded more slowly than the gelatin control. These results indicate that the MOPH fibers are a good reinforcing filler and may be useful for biocomposite applications.     

Interactive Influence of Biofiber Composition and Elastomer on Physico-Mechanical Properties of PLA Green Composites

The objective of this work was to improve the impact and thermal properties of polylactic acid (PLA)-based biocomposite by appropriate application of cellulosic fiber and a bioelastomer. Biocomposites formulations with fiber contents of up to 20% in combination with a bioelastomer were extrusion-compounded in a twin-screw extruder followed by molding in an injection molding system. Fibers used in the formulations included three types of cellulosic fiber; namely, raw fiber from oat hull biomass (RF), hydrolysis byproduct (ATF) which was the solid fraction obtained from an acid-catalyzed hydrolysis of RF, and delignified fibers (AD30, AD65, AD100) which were the products of delignification of ATF. Formulated biocomposites were characterized for thermal (glass transition and melting temperatures, and enthalpy of melting) and physico-mechanical (tensile and bending strengths, stiffness, impact energy, and water absorption) properties. Among all types of biofibers, RF resulted in poor properties in the biocomposites due to the high hemicellulose content in the structure. On the other hand, the ratio of lignin to cellulose (in the absence of hemicellulose) in the modified fibers did not significantly affect the physico-mechanical and thermal properties of the biocomposites. The elastomer applied in the formulations improved the impact energy, thermal properties, and elongation at break of the composites. However, it adversely affected the strength and water resistance of biocomposites, especially in the presence of hemicellulose. The results indicated that, depending on the application, a wide range of PLA green composites with different physico-mechanical properties can be achieved.     

Effect of Hydrothermal Aging on Injection Molded Short Jute Fiber Reinforced Poly(Lactic Acid) (PLA) Composites

This work focused on the durability of short jute fiber reinforced poly(lactic acid) (PLA) composites in distilled water at different temperatures (23, 37.8 and 60 °C). Morphological, thermal and mechanical properties (tensile, flexural, and impact) of jute/PLA composites were investigated before and after aging. Different from traditional synthetic fiber reinforced polymer composites, the stability of jute/PLA composites in water was significantly influenced by hydrothermal temperature. The mechanical properties of the composites and molecular weight of PLA matrix declined quickly at 60 °C, however, this process was quite slower at temperatures of 23 and 37.8 °C. Impact properties of the composites were hardly decreased, but the tensile and flexural properties suffered a drop though to various degrees with three degradation stages at 23 and 37.8 °C. The poor interface of composites and the degradation of PLA matrix were the main damage mechanism induced by hydrothermal aging. Furthermore, considering the hydrolysis of PLA matrix, the cleavage of PLA molecular chain in different aging time was quantitatively investigated for the first time to illustrate hydrolysis degree of PLA matrix at different aging time.     

Anaerobic Biodegradation of Polymer Composites Filled with Natural Fibers

Polymer composites with natural fibers prepared by melt blending were investigated. Synthetic and natural macromolecules were used, including poly(lactic acid), polyhydroxybutyrate-co-polyhydroxyvalerate and low density polyethylene. These polymers were filled with flax fibers. Mechanical properties of the composites, biogas production and mass loss under anaerobic digestion have been presented. It has been shown that the mechanical properties sustain after 28 days of biodegradation. Such materials can be found in applications as packaging, as well as in medicine as polymeric scaffolds, and drug delivery systems etc.     

Mechanical Properties of Poly (Lactic Acid)/Hemp Fiber Composites Prepared with a Novel Method

This research dealt with a novel method of fabricating green composites with biodegradable poly (lactic acid) (PLA) and natural hemp fiber. The new preparation method was that hemp fibers were firstly blending-spun with a small amount of PLA fibers to form compound fiber pellets, and then the traditional twin-screw extruding and injection-molding method were applied for preparing the composites containing 10–40 wt% hemp fibers with PLA pellets and compound fiber pellets. This method was very effective to control the feeding and dispersing of fibers uniformly in the matrix thus much powerful for improving the mechanical properties. The tensile strength and modulus were improved by 39 and 92 %, respectively without a significant decrease in elongation at break, and the corresponding flexural strength and modulus of composites were also improved by 62 and 90 %, respectively, when the hemp fiber content was 40 wt%. The impact strength of composite with 20 wt% hemp fiber was improved nearly 68 % compared with the neat PLA. The application of the silane coupling agent promoted further the mechanical properties of composites attributed to the improvement of interaction between fiber and resin matrix.     

Hybrid Composites from Waste Materials

Hybrid composites of thermoplastic biofiber reinforced with waste newspaper fiber (NF) and poplar wood flour (WF) were prepared. The weight ratio of the lignocellulosic materials to polymer was 30:70 (w:w). Polypropylene (PP) and maleic anhydride grafted polypropylene (MAPP) were also used as the polymer matrix and coupling agent, respectively. The mechanical properties, morphology and thermal properties were investigated. The obtained results showed that tensile and flexural modulus of the composites were significantly enhanced with addition of biofibers in both types (fiber and flour), as compared with pure PP. However, the increasing in WF content substantially reduced the tensile, flexural and impact modulus, but improved the thermal stability. This effect is explained by variations in fiber morphological properties and thermal degradation. Increasing fiber aspect ratio improved mechanical properties. The effect of fiber size on impact was minimal compared to the effects of fiber content. Scanning electron microscopy has shown that the composite, with coupling agent, promotes better fiber–matrix interaction. The largest improvement on the thermal stability of hybrid composites was achieved when WF was added more. In all cases, the degradation temperatures shifted to higher values after addition of MAPP. This work clearly showed that biofiber materials in both forms of fiber and flour could be effectively used as reinforcing elements in thermoplastic PP matrix.     

Lignocellulosic Fiber-Reinforced Keratin Polymer Composites

Short fiber reinforced polymer composites were prepared from lignocellulose fibers and feather keratin polymer (FKP). The FKP matrix was prepared from the reactive processing of poultry feather keratin, glycerol, water, and sodium sulfite. Lignocellulose fibers of varying source, length, and mass fraction were used and it was found that positive reinforcement of FKP was affected by all three. Positive reinforcement was defined as an increase in elastic modulus when normalized by FKP with the same amount of glycerol but no fibers. Positive reinforcement was only able to occur for modulus but not stress at break indicating that the composites were of high physical properties only under small deformations. At large deformations, fiber pull-out was observed in the composites using scanning electron microscopy. The most likely origin of this behavior appeared to be from weak fiber–polymer interactions dominated by friction and rationalized by a force balance across the fiber–polymer interface. High fiber loadings were shown to be reinforcing because of the formation of a network of lignocellulose fibers. The addition of lignocellulose fibers increased the thermal stability of the material.     

The Effect of Fiber Pretreatment and Compatibilizer on Mechanical and Physical Properties of Flax Fiber-Polypropylene Composites

Recently, investigations have been conducted on the use of natural fibers as reinforcement in low-melting point thermoplastics to improve mechanical properties of composites. However, due to some limitations of natural fibers, composite formulation and processing parameters must be controlled to produce a product with improved properties. This study was conducted to investigate the influence of flax fiber loading, use of compatibilizer and pretreatment on physical and mechanical properties of compression-molded composite. In this study, untreated and treated (sodium hydroxide-treated and mild-bleached flax fibers) fibers at 15% and 30% of the total product mass were used in formulations. To investigate the effect of compatibilizer on product properties, maleic anhydride grafted polypropylene (MAPP) was added at 5% by mass in the formulations. After extrusion of composites formulations, they were formed using compression molding. Results indicated that using flax fiber in composites without pretreatment and compatibilizer could result into products with inferior physical and mechanical properties; this could be compensated by the use of a compatibilizer. However, the use of compatibilizer had some negative effects on some other physical properties like color and melt flow index (MFI).     

Preparation and Properties of Green Composites Based on Tapioca Starch and Differently Recycled Paper Cellulose Fibers

Green composites obtained from biodegradable renewable resources have gained much attention due to environmental problems resulting from conventionally synthetic plastics and a global increasing demand for alternatives to fossil resources. In this work we used different cellulose fibers from used office paper and newspaper as reinforcement for thermoplastic starch (TPS) in order to improve their poor mechanical, thermal and water resistance properties. These composites were prepared by using tapioca starch plasticized by glycerol (30 % wt/wt of glycerol to starch) as matrix reinforced by the extracted cellulose fibers with the contents ranging from 0 to 8 % (wt/wt of fibers to matrix). Properties of composites were determined by mechanical tensile tests, differential scanning calorimetry, thermogravimetric analysis, water absorption measurements, scanning electron microscopy, and soil burial tests. The results showed that the introduction of either office paper or newspaper cellulose fibers caused the improvement of tensile strength and elastic modulus, thermal stability, and water resistance for composites when compared to the non-reinforced TPS. Scanning electron microscopy showed a good adhesion between matrix and fibers. Moreover, the composites biological degraded completely after 8 weeks but required a longer time compared to the non-reinforced TPS. The results indicated that these green composites could be utilized as commodity plastics being strong, inexpensive, plentiful and recyclable.     

Surface Modification of Sisal Fibers (Agave sisalana) Using Bacterial Cellulase and Methyl Methacrylate

The hydrophilic nature of cellulose fibers often results in poor compatibility with hydrophobic polymer matrices. Therefore, it becomes necessary to modify the surface of natural fiber for better binding between fiber and matrix. Chemicals are commonly used for the modification of cellulosic materials but large amount of solvents are usually involved. Microwave radiation induced grafting is one of the promising methods for the surface modification of natural fibers. In the present paper, we have reported the microwave radiations induced grafting onto sisal fibers (Agave sisalana) using methyl methacrylate monomer, which has been compared to the surface modification of sisal fibers using bacterial cellulase. The effects of these treatments on the properties of sisal fibers are discussed in the present paper. The modified fibers were characterized by scanning electron microscopy, X-ray diffraction, and thermogravimetric analysis/differential thermal analysis techniques to determine their morphology, crystallinity and thermal stability.     

Biodegradable Polyester-Based Blend Reinforced with Curauá Fiber: Thermal,Mechanical and Biodegradation Behaviour

Biodegradable composites can be produced by the combination of biodegradable polymers (BP) as matrix and vegetal fibers as reinforcement. Composites of a commercial biodegradable polymer blend and curauá fibers (loaded at 5, 15 and 20 wt%) were prepared by melt mixing in a twin-screw extruder. Chemical treatments such as alkali treatment of the fiber and addition of maleic anhydride grafted polypropylene (MA-g-PP) as coupling agent were performed to promote polymer/fiber interfacial adhesion so that mechanical performance can be improved. The resulting composites were evaluated through hardness, melt flow index and tensile, flexural and impact strengths as well as water absorption. Thermal analysis and Fourier transform infrared spectroscopy were also employed to characterize the composites. The polymer/fiber interface was investigated through scanning electron microscopy analysis. The biodegradability of composites was evaluated by compost-soil burial test. The addition of curauá fiber promoted an increase in the mechanical strengths and composites treated with 2 wt% MA-g-PP with 20 wt% curauá fiber showed an increase of nearly 75% in tensile and 56% in flexural strengths besides an improvement in impact strength with respect to neat polymer blend. Nevertheless, treated composites showed an increase in water absorption and biodegradation tests showed that the addition of fiber retards degradation time. The retained mass of BP/20 wt% fiber composite with MA-g-PP and neat BP was 68 and 26%, respectively, after 210 days of degradation test.     

Enzyme-Retted Flax Fiber and Recycled Polyethylene Composites

Municipal solid wastes generated each year contain potentially useful and recyclable materials for composites. Simultaneously, interest is high for the use of natural fibers, such as flax (Linum usitatissimum L.), in composites thus providing cost and environmental benefits. To investigate the utility of these materials, composites containing flax fibers with recycled high density polyethylene (HDPE) were created and compared with similar products made with wood pulp, glass, and carbon fibers. Flax was either enzyme- or dew-retted to observe composite property differences between diverse levels of enzyme formulations and retting techniques. Coupling agents would strengthen binding between fibers and HDPE but in this study fibers were not modified in anyway to observe mechanical property differences between natural fiber composites. Composites with flax fibers from various retting methods, i.e., dew- vs. enzyme-retting, behaved differently; dew-retted fiber composites resulted in both lower strength and percent elongation. The lowest level of enzyme-retting and the most economical process produces composites that do not appear to differ from the highest level of enzyme-retting. Flax fibers improved the modulus of elasticity over wood pulp and HDPE alone and were less dense than glass or carbon fiber composites. Likely, differences in surface properties of the various flax fibers, while poorly defined and requiring further research, caused various interactions with the resin that influenced composite properties.