The objective of this study is to process and characterize the compatibilized blends of acrylonitrile-butadiene-styrene (ABS) and polyamide-6 (PA6) using olefin based reactive copolymers and subsequently to utilize this blend as a matrix material in short glass fiber (SGF) reinforced composites and organoclay based nanocomposites by applying melt processing technique. In this context, commercially available epoxydized and maleated olefinic copolymers, ethylene-methyl acrylate-glycidyl methacrylate (EMA-GMA) and ethylene-n butyl acrylate-carbon monoxide-maleic anhydride (EnBACO-MAH) were used as compatibilizers at different ratios. Compatibilizing performance of these two olefinic polymers was investigated through blend morphologies, thermal and mechanical properties as a function of blend composition and compatibilizer loading level. Incorporation of compatibilizer resulted in a fine morphology with reduced dispersed particle size. At 5 % EnBACO-MAH, the toughness was observed to be the highest among the blends produced. SGF reinforced ABS and ABS/PA6 blends were prepared with twin screw extrusion. The effects of SGF concentration and extrusion process conditions on the fiber length distribution, mechanical properties and morphologies of the composites were examined. The most compatible organosilane type was designated from interfacial tension and short beam flexural tests, to promote adhesion of SGF to both ABS and PA6. Increasing amount of PA6 in the polymer matrix improved the strength, stiffness and also toughness of the composites. Effects of compatibilizer content and ABS/PA6 ratio on the morphology and mechanical properties of 30% SGF reinforced ABS/PA6 blends were investigated. The most striking result of the study was the improvement in the impact strength of the SGF/ABS/PA6 composite with the additions of compatibilizer. Melt intercalation method was applied to produce ABS/PA6 blends based organoclay nanocomposites. The effects of process conditions and material parameters on the morphology of blends, dispersibility of nanoparticles and mechanical properties were investigated. To improve mixing, the screws of the extruder were modified. Processing with co-rotation yielded finer blend morphology than processing with counter-rotation. Clays were selectively exfoliated in PA6 phase and agglomerated at the interface of ABS/PA6. High level of exfoliation was obtained with increasing PA6 content and with screw speed in co-rotation mode. Screw modification improved the dispersion of clay platelets in the matrix.

With this research, we work towards the overall objective of being able to accurately simulate fiber orientation in complex flow geometries of composite fluids of industrial significance. The focus of this work is to understand the rheological behavior of these materials and its connection to fiber orientation as determined in simple shear flow. The work includes the development of a novel approach to characterizing the transient rheology; an experimental study of the relationship between the stress growth functions in startup of flow and the fiber orientation; a critical assessment of the limitations of current fiber suspension theory; and an approach to determining unambiguous model parameters by fitting. A key difference between the rheological studies performed in this work and others is the use of a cone-and-plate device combined with "donut" shaped samples (CP-D) to prevent boundary effects on the measurement. The conventional method for obtaining transient rheological data is to use parallel disk (PP) geometry set at a gap where the measurements are independent of disk spacing. However, this work suggests that the inhomogeneous velocity gradient imposed by the PP geometry induces excessive fiber-fiber contact contributing to exaggerated measurements of the stress growth functions. An experimental study of the transient rheological behavior of a 30 wt% short glass fiber-filled polybutylene terephthalate was performed using the CP-D. Stress growth measurements during startup of flow were performed in combination with direct measurement of the fiber orientation to determine the relationship between the transient rheology and the fiber microstructure. The well defined fiber orientation and rheological experiments allowed for a quantitative assessment of current fiber suspension theory. Comparison between the experimental fiber orientation and predictions based on Jeffery's equation and the Folgar-Tucker model show that the fiber orientation evolves much slower than predicted. In addition, the addition of a "slip" term improved the agreement between the predictions and experimental results. Predictions using the Lipscomb model coupled with the Folgar-Tucker model, with slip, were fit to the transient stresses to determine the feasibility of fitting unambiguous model parameters for a specific composite fluid. Model parameters determined by fitting at a shear rate of 6 s-1 allowed for reasonable predictions of the transient stresses in flow reversal experiments at all the shear rates tested. / Ph. D.

Injection molded short fiber reinforced composites have generated commercial interest in the manufacturing of lightweight parts used in semi-structural applications. Predicting these materials’ fiber orientation with quantitative accuracy is crucial for technological advancement, but the task is difficult because of the effect of inter-particle interactions at high concentrations of fiber found in parts of commercial interest. A complete sample preparation procedure was developed to obtain optical micrographs with optimal definition of elliptical and non-elliptical footprint borders. Two novel aspects in this procedure were the use of tridimensional markers to identify specific locations for analysis and the use of controlled-etching to produce small shadows where fibers recede into the matrix. These images were used to measure fiber orientation with a customized image analysis tool. This tool contains several modifications that we introduced in the method of ellipses which allow us to determine tridimensional fiber orientation and to obtain measurements in regions with fast changes in orientation. The tool uses the location of the shadow to eliminate the ambiguity problem in orientation and characterizes non-elliptical footprints to obtain the orientation in small sampling areas. Cavitywise measurements in two thin center-gated disks showed the existence of an asymmetric profile of orientation at the gate and an orientation profile that washed out gradually at the entry region until disappearing at about 32 gap widths. This data was used to assess the prediction of cavitywise orientation using a delay model for fiber orientation with model parameters obtained from rheometrical experiments. Model predictions combining slip correction and experimentally determined orientation at the gate are in agreement with experimental data for the core layers near the end-of-fill region. Radialwise measurements of orientation at the shell, transition and core layer, and microtextural description of the advancing front are included in this dissertation. The analysis and assessment of the radial evolution of fiber orientation and advancing front based on comparing the experimental data with simulation results are under ongoing investigation. / Ph. D.

Le présent travail de thèse se consacre au développement d'un nouveau modèle micromécanique pour les composites en thermoplastique renforcé par des fibres de verre courtes. L'objectif est notamment la modélisation du comportement visco-endommageable en fatigue du PA66-GF30. Ce matériau, particulièrement utilisé dans l'industrie automobile, est sujet à une microstructure spécifique issue du procédé de moulage par injection. L'approche multi-échelles développée consiste en une méthode de Mori-Tanaka modifiée, appliquée à des renforts avec enrobage et prenant en compte l'évolution de l'endommagement à l'échelle microscopique. La description des mécanismes d'endommagement se base sur une investigation expérimentale poussée préalablement menée au sein de l'équipe. Des scénarios d'endommagement ont été proposés et incluent trois processus locaux différents : la décohésion de l'interface, la microfissuration de la matrice et les ruptures de fibres. Ceux-ci sont spécialement affectés par la microstructure. L'approche développée intègre ces cinétiques d'endommagement ainsi que la viscoélasticité non-linéaire de la matrice et la distribution d'orientation des inclusions due au procédé de fabrication. Chaque mécanisme d'endommagement est modélisé par une loi d'évolution basée sur les contraintes locales calculées à l'échelle microscopique. La loi constitutive finale, à l'échelle du volume élémentaire représentatif, est implémentée dans une bibliothèque scientifique en C++, SMART+, et est conçue pour être compatible avec une analyse de structures par éléments finis. L'identification du modèle est réalisée par rétro-ingénierie, en tirant profit de résultats expérimentaux multi-échelles, dont notamment des tests in-situ au MEB ainsi qu'une analyse qualitative et quantitative par μCT. / The current work focuses on a new micromechanical high cycle fatigue visco-damage model for short glass fiber reinforced thermoplastic composites, namely: PA66/GF30. This material, extensively used for automotive applications, has a specific microstructure which is induced by the injection process. The multi-scale developed approach is a modified Mori-Tanaka method that includes coated reinforcements and the evolution of micro-scale damage processes. Their description is based on the experimental investigations of damage mechanisms previously performed by the team. Damage chronologies have been proposed involving three different local degradation processes: fiber-matrix interface debonding/coating degradation, matrix microcracking and fiber breakage. Their occurrence strongly depends on the microstructure. The developed model integrates these damage kinetics and accounts for the complex matrix viscoelasticity and the reinforcement orientation distributions induced by the process. Each damage mechanism is introduced through an evolution law involving local stress fields computed at the microscale. The developed constitutive law at the representative volume element scale is implemented into a C++ scientific library, SMART+, and is designed to work with Finite Element Methods. The model identification is performed via reverse engineering, taking advantage of the multiscale experimental results: in-situ SEM tests as well as quantitative and qualitative μCT investigations.

Dans ce travail, l’effet du vieillissement thermique sur le comportement en fatigue ducomposite de poly (sulfure de phénylène) renforcé par fibres de verre (PPS/FV) a été étudié. Ce matériau est d’abord étudié par différentes méthodes d’analyse afin de déterminer ses caractéristiques physicochimiqueset mécaniques. Ensuite, le matériau subit un vieillissement thermo-oxydatif accéléré à différentes températures comprises entre 100 °C et 200 °C. Certaines caractéristiques du matériau sont d’ailleurs suivies au cours du vieillissement. A partir des résultats obtenus, un mécanisme d’oxydation estproposé et un modèle cinétique est développé. La validité de ce modèle est vérifiée par les résultats expérimentaux, essentiellement obtenus par la spectrométrie infrarouge. L’effet du vieillissement sur lecomportement mécanique est étudié par les deux axes suivants : D’abord d’une manière indirecte en étudiant l’évolution de la morphologie de la phase cristalline au cours du temps et ensuite par la méthode directe. Dans cette méthode directe, premièrement, le comportement en fatigue et en traction-traction duPPS/FV a été étudié en faisant varier la fréquence et l’amplitude de la sollicitation. La courbe de Wöhler est tracée en fonction du nombre de cycles à la rupture. Il a été constaté que le vieillissement modifie lepositionnement et l’allure de la courbe de Wöhler. Ensuite les éprouvettes vieillies à différentes températures sont testées en fatigue (traction-traction) avec une amplitude maximale (σmax=40 MPa) et un rapport de chargement (R=0,1) afin de suivre l’influence de la dégradation thermo-oxydative au cours du vieillissement. Il a été constaté que l’oxydation a un effet néfaste sur le comportement en fatigue du PPS/FV. Ce matériau perd significativement de ses performances même au début du vieillissement etsurtout à haute température de vieillissement. La perte de la performance en fatigue du matériau s’accentue au fur et à mesure que le processus d’oxydation se poursuit. / In this work, the effect of thermal aging on the fatigue behavior of a glass fiber reinforced poly (phenylene sulfide) composite (PPS/GF) was studied. This material is first characterized by differentmethods of analysis to determine its physicochemical and mechanical characteristics. Subsequently, thematerial undergoes accelerated thermo-oxidative aging at different temperatures between 100 °C and 200 °C. Some characteristics of this material are followed during thermal aging. From the results obtained, an oxidation mechanism is proposed and a kinetic model is developed. The validity of this model is verifiedby the experimental results, essentially obtained by infrared spectrometry. The effect of thermal aging on mechanical behavior is studied in two ways: Firstly, indirect manner by studying the evolution of the morphology of the crystalline phase over time and subsequently by the direct method. In this directmethod, firstly the tension-tension fatigue behavior of PPS/GF was studied by varying the frequency and amplitude of stress. The Wöhler curve is plotted on the basis of the number of cycles at break. Thermalaging has been found to alter the position and shape of the Wöhler curve. Then the samples aged at different temperatures were tested by tension-tension fatigue with a maximum amplitude (σmax = 40 MPa)and a loading ratio (R = 0.1) to follow the influence of thermo-oxidative degradation during aging. It has been found that thermal aging has a detrimental effect on the fatigue behavior of PPS/GF. This material loses its performance significantly even at the beginning of aging, especially in high aging temperature.The loss of fatigue performance grows in the oven as the oxidation process continues.