Flax fibers can be used as environmentally friendly alternatives to conventional reinforcing fibers (e.g., glass) in composites. The interest in natural fiber-reinforced polymer composites is growing rapidly due to its high performance in terms of mechanical properties, significant processing advantages, excellent chemical resistance, low cost and low density. These advantages place natural fiber composites among the high performance composites having economic and environmental advantages. In the field of technical utilization of plant fibers, flax fiber-reinforced composites represent one of the most important areas. On the other hand, lack of good interfacial adhesion and poor resistance to moisture absorption make the use of natural fiber-reinforced composites less attractive. In order to improve their interfacial properties, fibers were subjected to chemical treatments, namely, mercerization, silane treatment, benzoylation, and peroxide treatment. Selective removal of non-cellulosic compounds constitutes the main objective of the chemical treatments of flax fibers to improve the performance of fiber-reinforced composites. The objective of this study was to determine the effects of pre-treated flax fibers on the performance of the fiber-reinforced composites. Short flax fibers were derived from Saskatchewan-grown flax straws, for use in fiber-reinforced composites. Composites consisting of high-density polyethylene (HDPE) or linear low-density polyethylene (LLDPE) or HDPE/LLDPE mix, chemically treated fibers and additives were prepared by the extrusion process. Extrusion is expected to improve the interfacial adhesion significantly as opposed to simple mixing of the two components. The extruded strands were then pelletized and ground. The test samples were prepared by rotational molding. The fiber surface topology and the tensile fracture surfaces of the composites were characterized by scanning electron microscopy to determine whether the modified fiber-matrix interface had improved interfacial bonding. Mechanical and physical properties of the composites were evaluated. The differential scanning calorimetry technique was also used to measure the melting point of flax fiber and composite. Overall, the scanning electron microscopy photographs of fiber surface characteristics and fracture surfaces of composites clearly indicated the extent of fiber-matrix interface adhesion. Chemically treated fiber-reinforced composites showed better fiber-matrix interaction as observed from the good dispersion of fibers in the matrix system. Compared to untreated fiber-reinforced composites, all the treated fiber-reinforced composites had the same tendency to slightly increase the tensile strength at yield of composites. Silane, benzoylation, and peroxide treated fiber-reinforced composites offered superior physical and mechanical properties. Strong intermolecular fiber-matrix bonding decreased the high rate of water absorption in biocomposites. The incorporation of 10% untreated or chemically treated flax fibers also increased the melting point of composites. Further investigation is required to address the effect of increase in fiber content on the performance of composites.

Flax fibers can be used as environmentally friendly alternatives to conventional reinforcing fibers (e.g., glass) in composites. The interest in natural fiber-reinforced polymer composites is growing rapidly due to its high performance in terms of mechanical properties, significant processing advantages, excellent chemical resistance, low cost and low density. These advantages place natural fiber composites among the high performance composites having economic and environmental advantages. In the field of technical utilization of plant fibers, flax fiber-reinforced composites represent one of the most important areas. On the other hand, lack of good interfacial adhesion and poor resistance to moisture absorption make the use of natural fiber-reinforced composites less attractive. In order to improve their interfacial properties, fibers were subjected to chemical treatments, namely, mercerization, silane treatment, benzoylation, and peroxide treatment. Selective removal of non-cellulosic compounds constitutes the main objective of the chemical treatments of flax fibers to improve the performance of fiber-reinforced composites. The objective of this study was to determine the effects of pre-treated flax fibers on the performance of the fiber-reinforced composites. Short flax fibers were derived from Saskatchewan-grown flax straws, for use in fiber-reinforced composites. Composites consisting of high-density polyethylene (HDPE) or linear low-density polyethylene (LLDPE) or HDPE/LLDPE mix, chemically treated fibers and additives were prepared by the extrusion process. Extrusion is expected to improve the interfacial adhesion significantly as opposed to simple mixing of the two components. The extruded strands were then pelletized and ground. The test samples were prepared by rotational molding. The fiber surface topology and the tensile fracture surfaces of the composites were characterized by scanning electron microscopy to determine whether the modified fiber-matrix interface had improved interfacial bonding. Mechanical and physical properties of the composites were evaluated. The differential scanning calorimetry technique was also used to measure the melting point of flax fiber and composite. Overall, the scanning electron microscopy photographs of fiber surface characteristics and fracture surfaces of composites clearly indicated the extent of fiber-matrix interface adhesion. Chemically treated fiber-reinforced composites showed better fiber-matrix interaction as observed from the good dispersion of fibers in the matrix system. Compared to untreated fiber-reinforced composites, all the treated fiber-reinforced composites had the same tendency to slightly increase the tensile strength at yield of composites. Silane, benzoylation, and peroxide treated fiber-reinforced composites offered superior physical and mechanical properties. Strong intermolecular fiber-matrix bonding decreased the high rate of water absorption in biocomposites. The incorporation of 10% untreated or chemically treated flax fibers also increased the melting point of composites. Further investigation is required to address the effect of increase in fiber content on the performance of composites.

Flax fiber-reinforced plastic composites have attracted increasing interest because of the advantages of flax fibers, such as low density, relatively high toughness, high strength and stiffness, and biodegradability. Thus, oilseed flax fiber derived from flax straw, a renewable resource available in Western Canada, is recognized as a potential replacement for glass fiber in composites. Among plastics, polyethylene is a suitable material for use as a matrix in composites. However, there are not many studies in this area. Therefore, the main goal of this research was to develop flax fiber-polyethylene (PE) biocomposites via injection molding and investigate the effect of material properties and processing parameters on their properties. <p>Alkali, silane, potassium permanganate, sodium chlorite, and acrylic acid treatments were employed to flax fiber to decrease the hydrophilic of fiber and improve the adhesion between the fiber and the matrix. All chemically treated fiber-HDPE biocomposites had higher tensile strength and lower water absorption compared with non-chemically treated ones. Acrylic acid treatment of the fiber resulted in slight increase in its degradation temperature; using this treated fiber resulted in biocomposites with the best performance. Therefore, the morphological, chemical, and thermal properties of acrylic acid treated fiber were also studied. <p>Linear Low Density Polyethylene (LLDPE) and High Density Polyethylene (HDPE) were the main matrices investigated in this research. Showing a high tensile strength and similar water absorption, HDPE was used as the matrix in further research. Flax fiber with 98-99% purity was chosen as reinforcement since the flax shive mixed with the fiber decreased the tensile and flexural properties but increased the water absorption of the biocomposite. <p>Acrylic acid-treated fiber-HDPE biocomposites had been developed through injection molding under different processing conditions. Increasing the fiber content of biocomposite increased its tensile and flexural strengths, especially flexural modulus, but its water absorption capacity also increased. It was possible to improve the mechanical properties of biocomposites and decrease the water absorption by adjusting injection temperature and pressure. Injection temperature had more influence on the quality of the biocomposite than injection pressure. Injection temperature lower than 195°C was recommended to achieve good composite quality. <p>Melts of HDPE and flax fiber-HDPE biocomposites were categorized as power-law fluids. Apparent viscosity, consistency coefficient, and flow behavior index of biocomposites were determined to study their flow behavior. The statistical relationship of these parameters with temperature and fiber content were modeled using the SAS and SPSS softwares. The injection filling time was related to the material rheological properties: biocomposites required longer filling time than pure HDPE. Low injection temperature also resulted in long filling time.<p>The thermal conductivity, thermal diffusivity, and specific heat of biocomposites containing 10, 20, and 30% fiber by mass were determined in the processing temperature range of 170 to 200°C. Fiber content showed a significant influence on the thermal properties of the biocomposites. The predicted minimum cooling time increased with the thickness of the molded material, mold temperature, and injection temperature, but it decreased with the ejection temperature.

The environmental menace associated with the existing eco-unfriendly conventional plastics prompted the exploration of natural polymers such as starch for the development of biodegradable plastics. These efforts have seen starch used in various ways, one of which is in the processing of thermoplastic starch (TPS). Thermoplastic starch (also known as plasticized starch) is the product of the interaction between starch and a plasticizer in the presence of thermomechanical energy. While starch blends with conventional plastics only yield products that biofragment, thermoplastic starch (TPS) offers a completely biodegradable option. However, it is limited in application due to its weak mechanical strength and poor moisture resistance. To this end, the objective of this study was to determine the effects of incorporating polycaprolactone (PCL) and flax fiber into glycerol-plasticized pea starch. The effects of processing moisture content on the physical properties of glycerol-plasticized pea starch were also evaluated. The physical properties investigated included morphology, tensile properties, moisture absorption, and thermal properties.<p> Accordingly, two thermoplastic pea starch mixtures containing 9.3 and 20% processing moisture contents were prepared while maintaining starch (pea starch) and glycerol in ratio 7:3 by weight (dry basis). Polycaprolactone was then compounded at 0, 10, 20, 30, and 40% by weight in the solid phase with the TPS mixtures to determine the effects of processing moisture content and PCL incorporation on the physical properties of glycerol-plasticized pea starch. This experiment was structured as a 2 x 5 factorial completely randomized design at 5% level of significance. Subsequently, PCL and flax fiber were compounded with the TPS mixture containing 20% processing moisture to determine the effects of PCL (0, 20, and 40% wt) and flax fiber (0, 5, 10, and 15% wt) incorporation on the physical properties of glycerol-plasticized pea starch. This was structured as a 3 x 4 factorial completely randomized design at 5% level of significance. All the samples were compressed at 140°C for 45 min under 25000-kg load. The compression-molded samples were characterized using scanning electron microscopy (SEM), tensile test, moisture absorption test, and differential scanning calorimetry (DSC) techniques.<p> The tensile fracture surfaces showed a moisture-induced fundamental morphological difference between the two TPSs. The TPS prepared at 20% processing moisture content revealed complete starch gelatinization, thus, exhibiting a rather continuous phase whereas the TPS prepared at 9.3% processing moisture content revealed instances of ungelatinized and partly gelatinized pea starch granules. Consequently, the tensile strength, yield strength, Youngs modulus, and elongation at break increased by 208.6, 602.6, 208.5, and 292.0%, respectively at 20% processing moisture content. The incorporation of PCL reduced the degree of starch gelatinization by interfering with moisture migration during compression molding due to its (PCL) hydrophobicity. At both processing moisture levels of 9.3 and 20%, PCL incorporation had significant impacts on the tensile properties of the plasticized pea starch. Flax fiber incorporation also increased the tensile strength, yield strength, and Youngs modulus while concomitantly reducing the elongation at break of the plasticized pea starch. In the TPS/PCL/flax fiber ternary composites, both PCL and flax fiber improved the tensile strength by acting as independent reinforcing materials as no PCL-fiber interfacial bonding was observed. Maximum tensile strength of 11.55 MPa was reached at 10% flax fiber and 40% PCL reinforcement. While the PCL-TPS interfacial interaction was poor, some degree of TPS-flax fiber interfacial bonding was noticed due to their chemical similarity.<p> TPS prepared at 20% moisture showed more moisture affinity than that prepared at 9.3% moisture. The moisture absorption of TPS dropped progressively with the addition of hydrophobic PCL. Fiber incorporation also reduced moisture absorption by the plasticized pea starch. PCL-fiber incorporation also yielded improved moisture resistance vis-à-vis pure TPS. Finally, the TPS processed at 9.3% moisture exhibited higher thermal stability than that processed at 20%. Individual components of the composites retained their respective thermal properties, thus, implying thermodynamic immiscibility.

The environmental menace associated with the existing eco-unfriendly conventional plastics prompted the exploration of natural polymers such as starch for the development of biodegradable plastics. These efforts have seen starch used in various ways, one of which is in the processing of thermoplastic starch (TPS). Thermoplastic starch (also known as plasticized starch) is the product of the interaction between starch and a plasticizer in the presence of thermomechanical energy. While starch blends with conventional plastics only yield products that biofragment, thermoplastic starch (TPS) offers a completely biodegradable option. However, it is limited in application due to its weak mechanical strength and poor moisture resistance. To this end, the objective of this study was to determine the effects of incorporating polycaprolactone (PCL) and flax fiber into glycerol-plasticized pea starch. The effects of processing moisture content on the physical properties of glycerol-plasticized pea starch were also evaluated. The physical properties investigated included morphology, tensile properties, moisture absorption, and thermal properties.<p> Accordingly, two thermoplastic pea starch mixtures containing 9.3 and 20% processing moisture contents were prepared while maintaining starch (pea starch) and glycerol in ratio 7:3 by weight (dry basis). Polycaprolactone was then compounded at 0, 10, 20, 30, and 40% by weight in the solid phase with the TPS mixtures to determine the effects of processing moisture content and PCL incorporation on the physical properties of glycerol-plasticized pea starch. This experiment was structured as a 2 x 5 factorial completely randomized design at 5% level of significance. Subsequently, PCL and flax fiber were compounded with the TPS mixture containing 20% processing moisture to determine the effects of PCL (0, 20, and 40% wt) and flax fiber (0, 5, 10, and 15% wt) incorporation on the physical properties of glycerol-plasticized pea starch. This was structured as a 3 x 4 factorial completely randomized design at 5% level of significance. All the samples were compressed at 140°C for 45 min under 25000-kg load. The compression-molded samples were characterized using scanning electron microscopy (SEM), tensile test, moisture absorption test, and differential scanning calorimetry (DSC) techniques.<p> The tensile fracture surfaces showed a moisture-induced fundamental morphological difference between the two TPSs. The TPS prepared at 20% processing moisture content revealed complete starch gelatinization, thus, exhibiting a rather continuous phase whereas the TPS prepared at 9.3% processing moisture content revealed instances of ungelatinized and partly gelatinized pea starch granules. Consequently, the tensile strength, yield strength, Youngs modulus, and elongation at break increased by 208.6, 602.6, 208.5, and 292.0%, respectively at 20% processing moisture content. The incorporation of PCL reduced the degree of starch gelatinization by interfering with moisture migration during compression molding due to its (PCL) hydrophobicity. At both processing moisture levels of 9.3 and 20%, PCL incorporation had significant impacts on the tensile properties of the plasticized pea starch. Flax fiber incorporation also increased the tensile strength, yield strength, and Youngs modulus while concomitantly reducing the elongation at break of the plasticized pea starch. In the TPS/PCL/flax fiber ternary composites, both PCL and flax fiber improved the tensile strength by acting as independent reinforcing materials as no PCL-fiber interfacial bonding was observed. Maximum tensile strength of 11.55 MPa was reached at 10% flax fiber and 40% PCL reinforcement. While the PCL-TPS interfacial interaction was poor, some degree of TPS-flax fiber interfacial bonding was noticed due to their chemical similarity.<p> TPS prepared at 20% moisture showed more moisture affinity than that prepared at 9.3% moisture. The moisture absorption of TPS dropped progressively with the addition of hydrophobic PCL. Fiber incorporation also reduced moisture absorption by the plasticized pea starch. PCL-fiber incorporation also yielded improved moisture resistance vis-à-vis pure TPS. Finally, the TPS processed at 9.3% moisture exhibited higher thermal stability than that processed at 20%. Individual components of the composites retained their respective thermal properties, thus, implying thermodynamic immiscibility.

Flax fiber-reinforced plastic composites have attracted increasing interest because of the advantages of flax fibers, such as low density, relatively high toughness, high strength and stiffness, and biodegradability. Thus, oilseed flax fiber derived from flax straw, a renewable resource available in Western Canada, is recognized as a potential replacement for glass fiber in composites. Among plastics, polyethylene is a suitable material for use as a matrix in composites. However, there are not many studies in this area. Therefore, the main goal of this research was to develop flax fiber-polyethylene (PE) biocomposites via injection molding and investigate the effect of material properties and processing parameters on their properties. <p>Alkali, silane, potassium permanganate, sodium chlorite, and acrylic acid treatments were employed to flax fiber to decrease the hydrophilic of fiber and improve the adhesion between the fiber and the matrix. All chemically treated fiber-HDPE biocomposites had higher tensile strength and lower water absorption compared with non-chemically treated ones. Acrylic acid treatment of the fiber resulted in slight increase in its degradation temperature; using this treated fiber resulted in biocomposites with the best performance. Therefore, the morphological, chemical, and thermal properties of acrylic acid treated fiber were also studied. <p>Linear Low Density Polyethylene (LLDPE) and High Density Polyethylene (HDPE) were the main matrices investigated in this research. Showing a high tensile strength and similar water absorption, HDPE was used as the matrix in further research. Flax fiber with 98-99% purity was chosen as reinforcement since the flax shive mixed with the fiber decreased the tensile and flexural properties but increased the water absorption of the biocomposite. <p>Acrylic acid-treated fiber-HDPE biocomposites had been developed through injection molding under different processing conditions. Increasing the fiber content of biocomposite increased its tensile and flexural strengths, especially flexural modulus, but its water absorption capacity also increased. It was possible to improve the mechanical properties of biocomposites and decrease the water absorption by adjusting injection temperature and pressure. Injection temperature had more influence on the quality of the biocomposite than injection pressure. Injection temperature lower than 195°C was recommended to achieve good composite quality. <p>Melts of HDPE and flax fiber-HDPE biocomposites were categorized as power-law fluids. Apparent viscosity, consistency coefficient, and flow behavior index of biocomposites were determined to study their flow behavior. The statistical relationship of these parameters with temperature and fiber content were modeled using the SAS and SPSS softwares. The injection filling time was related to the material rheological properties: biocomposites required longer filling time than pure HDPE. Low injection temperature also resulted in long filling time.<p>The thermal conductivity, thermal diffusivity, and specific heat of biocomposites containing 10, 20, and 30% fiber by mass were determined in the processing temperature range of 170 to 200°C. Fiber content showed a significant influence on the thermal properties of the biocomposites. The predicted minimum cooling time increased with the thickness of the molded material, mold temperature, and injection temperature, but it decreased with the ejection temperature.

Cette thèse de doctorat a été réalisée dans le cadre du projet Fiabilin, qui regroupe 15 partenaires industriels et académiques, et vise à structurer une filière industrielle de production de biocomposites polyamide-11/fibres de lin. Ces travaux ont pour objectif de déterminer des performances multi-échelles de ce composite 100% biosourcé, afin d’envisager son usage en substitution de composites pétrosourcés. Nous avons tout d’abord mis en évidence la sensibilité des fibres de lin aux cycles temps-température des procédés de mise en œuvre, tant du point de vue de leurs propriétés mécaniques que de leur structure biochimique. Ensuite, nous avons montré les capacités du système PA11-lin à produire des performances mécaniques en traction compétitives vis-à-vis d’autres composites pétrosourcés. La qualité de l’interface fibre/matrice du biocomposite a également été étudiée à différentes échelles, montrant une compatibilité supérieure à celles de systèmes lin-résines thermodurcissables. La fin de vie du composite PA11-lin a été envisagée à travers le recyclage par broyages et injections successives. Les propriétés mécaniques du biocomposite à fibres courtes ainsi obtenu sont semblables au composite PPgMA-lin, avec une déformation à rupture accrue et qui augmente significativement avec le nombre de recyclages. Une analyse des cycles de production de plusieurs composites révèle les plus faibles impacts environnementaux du PA11-lin lors d’un dimensionnement des pièces en rigidité équivalentes. / This thesis has been carried out as part of the project Fiabilin, which includes 15 different academic and industrial partners, with an aim to develop industrial production of polyamide-11/flax biocomposite. The purpose of this work is to determine multi-scale performances of 100% biosourced composite, in order to substitute composite materials containing glass fibers and/or matrix derived from petroleum. First, we highlighted the flax fiber sensibility toward processing cycles (time and temperature), from mechanical and biochemical structure aspects. Then, we revealed the capacity of PA11-flax association to produce competitive mechanical properties compared to others usual composites. Fiber-matrix interface of the biocomposite was studied at micro and macro scales, showing a higher compatibility than some flax-thermoset resin systems. The end-of-life of the biocomposite was considered by recycling with successive grinding and injections. Then stiffness and strength at break of short fiber biocomposites thus obtained are similar to PPgMA-flax composites, whereas a strong increase of the strain at break according to the number of injection cycles was observed. A life cycle analysis of some composites production steps shows lower environmental impacts of PA11-flax when sizing was made through equivalent material stiffness.

This thesis provides an approach to incorporate natural composites like Flax Fiber using a resin with 30% bio-content to enhance the packaging boxes made of corrugated cardboard. The objective of introducing natural composite skins is to reduce/eliminate the compressive loading subjected to the boxes while stacking in warehouses.

Indiana University-Purdue University Indianapolis (IUPUI) / This thesis provides an approach to incorporate natural composites like Flax Fiber using a resin with 30% bio-content to enhance the packaging boxes made of corrugated cardboard. The objective of introducing natural composite skins is to reduce/eliminate the compressive loading subjected to the boxes while stacking in warehouses.

Extrusion compounding addresses such problems as the non-homogeneity of the mixture and separation of fiber from the polymer during rotational molding, which consequently affect the mechanical and physical properties of the resulting composites. <p>Using triethoxyvinylsilane as chemical pre-treatment on flax fibers and linear low density polyethylene (LLDPE) and high density polyethylene (HDPE) as polymer matrices, this study focused on the effects of flax fiber content (0%, 12.5% or 25%) and extrusion parameters such as barrel zone temperatures (75-110-120-130-140°C or 75-120-130-140-150°C) and screw speed (110 or 150 rpm) on the extrudate and composite properties (extrudate color, extrudate density, extrudate melt flow index, extrudate morphology, composite color, composite density, composite morphology, composite tensile strength and composite water absorption). <p>A mixture of chemically pre-treated flax fibers and powdered polyethylene matrices underwent extrusion compounding using a twin-screw extruder. The extrudates were then pelletized, ground, rotationally molded and cut into test specimens (composites). The mechanical and physical properties of both the extrudates and the composites from different treatments were then measured and compared. <p>Using multiple linear regression, models were generated to show quantitatively the significant effects of the process variables on the response variables. Finally, using response surface methodology and superposition surface methodology on the preceding data, the following optimum values for fiber content and extrusion parameters were determined: for LLDPE composites, fiber content = 6.25%, temperatures = 75-117.3-127.3-137.3-147.3°C, screw speed = 117.5 rpm; for HDPE composites, fiber content = 5.02%, temperatures = 75-118.1-128.1-138.1-148.1°C, screw speed = 125.56 rpm.