The widespread use of titanium and its alloys in structural applications has been limited to few highend applications. The dominant reason for this being cost implications. These high costs arise from extracting titanium from its mineral form as well as that of the manufacturing processes to develop a final product. Since producing titanium products includes expensive starting stock, high machinability costs and high wastage, a need for a process that may minimize one or more of these factors is necessary. One such technology that exists is a branch of powder metallurgy (PM), direct powder rolling (DPR) which allows for a continuous approach to produce strip or sheet metal. Products developed by this process are however known to possess inferior properties to its wrought counterpart. The present study comprises of a parametric study observing how two different blends of powder differ in the development of Ti-6Al-4V strip by employing the blended elemental (BE) approach to direct powder rolling. The objectives of this work include predicting the compaction behavior of the two respective blends during powder rolling to inform the production of high density green strip and to compare the outcomes of the prediction method to experimentally determined results using a gravity-fed laboratory-scale rolling mill with roll diameter of 265 mm and roll width of 150 mm. Johanson’s rolling theory was applied to predict rolling outcomes and a fixed set of rolling parameters were implemented for the simulation and experimental segment of this dissertation. The two blends being investigated include blending titanium powder with an elemental blend consisting of aluminium and vanadium powders (B1) and a master alloy blend of a 60Al-40V master alloy (B2). These two blends were used to validate the Johanson simulated rolling data. Fixed parameters applied to the rolling mill included using a roll speed of 14 rpm, roll face width of 65 mm and gravity-fed hopper outlet diameter of 25 mm. Variable roll gaps of 0.5, 1 and 1.5 mm were studied. Average relative green densities of B1 and B2 strips achieved at a roll gap of 1 mm were 77% and 73% respectively. Rolling performance of the B1 powder blend were higher than that of B2, reaching higher green densities and showing superior formability, as rolling at smaller roll gaps was achievable for B1 and not B2. Green strength of B1 and B2 strips at a roll gap of 1 mm reflected similar outcomes where B1 strips required a greater breaking load to fracture samples when compared to B2 indicating a stronger self-supporting compact. Furthermore, the Johanson rolling model proved to overestimate reasonable roll pressure values, although, the general trend of compactibility between B1 and B2 powder blends was reasonably predicted showing B1 to be more compressible than B2 during powder rolling. iv Subsequent sintering at 1200 °C for 3 hours in a vacuum environment was applied to green strips to further densify and homogenize strips. Average relative sintered densities achieved for B1 and B2 strips rolled at a roll gap of 1 mm were 78% and 87% respectively. While green densities of B1 strips were higher than that of B2 strips, it was evident that the addition of the 60Al-40V master alloy to blend B2 resulted in superior sinterability as final sintered densities surpassed that of B1, even when starting at a lower green density after rolling. SEM/EDX was used to evaluate what effect sintering had on homogenization. A standard wrought Ti-6Al-4V specimen was used as the benchmark to compare homogenization results. B2 strips homogenized more than B1 strips when comparing to the baseline wrought sample. It was concluded that both B1 and B2 powders used to create Ti-6Al-4V strip by direct powder rolling (DPR) exhibited high levels of porosity and a subsequent step is necessary to fully densify the material. While B1 strips exhibit superior rollability with higher green densities and green strength; after applying a sintering practice to both B1 and B2 strips, B2 sintered densities surpassed those of B1 and prove to homogenize to a greater degree than B1 strips. The superior roll compaction ability and inferior sinterability for B1 powders was attributed to the elemental powder, aluminium. While the addition of ductile aluminium to B1 aids roll compaction, its low melting point results in large pores evolving at sintering temperatures almost twice its melting point.

Les solides divisés telles que les poudres pharmaceutiques nécessitent souvent des processus d'agrandissement de taille par agglomération pour améliorer leur comportement mécanique, notamment la coulabilité. Pour cette raison, le procédé de "granulation en voie sèche" est utilisé dans l'industrie pharmaceutique. Le procédé consiste à comprimer la poudre en la faisant passer entre deux rouleaux séparés par un entrefer, pour produire des plaquettes qui sont ensuite broyées en granulés et comprimés en compacts. Dans ce procédé, l'existence de différents modèles de compacteurs à rouleaux et de systèmes de broyage d’une part, et l'interaction entre les paramètres des procédés et des propriétés des produits (plaquettes, granulés et comprimés) d’autre part, rendent difficile la compréhension des phénomènes et des mécanismes sous-jacents. En particulier, le procédé entraîne une perte de résistance mécanique des comprimés formés à partir de granulés (comparativement à celles des comprimés de poudres non-granulés) et ce phénomène est encore mal compris. Ces aspects sont étudiés dans ce travail de thèse en menant des caractérisations expérimentales et des modélisations numériques permettant de mieux comprendre les modifications micro et macro structurales des poudres mises en forme par granulation sèche. Le but ultime est de progresser dans la compréhension des relations "propriétés des poudres - paramètres des procédés". Enfin, la compréhension des différences de comportement en compression de poudres granulées et non-granulées est menée à l’aide d’une modélisation du comportement dans le cadre de la mécanique des milieux continus poreux. / Particulate solids such as pharmaceutical powders often require size enlargement processes to improve the manufacturing properties like flowability. For that reason, dry granulation by roll compaction has been widely used in the pharmaceutical industry. The process consists of compressing powders between two counter-rotating rolls to produce ribbons that will be subsequently milled into granules. The obtained granules are tableted for oral dosage. In this process there are two main limitations: the existence of different designs of the roll compactors, milling systems and the interaction between process parameters and raw material properties are still a challenge and the roll-compaction process leads to an inferior tensile strength of tablets compared with direct compression. These aspects are investigated in this work. In the first part of this thesis, an analysis on the effect of different roll-compaction conditions and milling process parameters on ribbons, granules and tablet properties was performed, highlighting the role of the sealing system and the ribbon density distribution characteristics. In the second part, die compaction of roll-compacted powders, as the last stage of the process, is further investigated in terms of experimental analysis (effect of the granule size and composition and stress transmission measurements) and modelling the compaction behavior of granules.

Roll compaction is a continuous process commonly used in the pharmaceutical industry for dry granulation of moisture and heat sensitive powder blends. It is intended to increase bulk density and improve flowability. Roll compaction is a complex process that depends on many factors, such as feed powder properties, processing conditions and system layout. Some of the variability in the process remains unexplained. Accordingly, modeling tools are needed to understand the properties and the interrelations between raw materials, process parameters and the quality of the product. It is important to look at the whole manufacturing chain from raw materials to tablet properties. The main objective of this thesis was to investigate the impact of raw materials, process parameters and system design variations on the quality of intermediate and final roll compaction products, as well as their interrelations. In order to do so, we have conducted a series of systematic experimental studies and utilized chemometric tools, such as design of experiments, latent variable models (i.e. PCA, OPLS and O2PLS) as well as mechanistic models based on the rolling theory of granular solids developed by Johanson (1965). More specifically, we have developed a modeling approach to elucidate the influence of different brittle filler qualities of mannitol and dicalcium phosphate and their physical properties (i.e. flowability, particle size and compactability) on intermediate and final product quality. This approach allows the possibility of introducing new fillers without additional experiments, provided that they are within the previously mapped design space. Additionally, this approach is generic and could be extended beyond fillers. Furthermore, in contrast to many other materials, the results revealed that some qualities of the investigated fillers demonstrated improved compactability following roll compaction. In one study, we identified the design space for a roll compaction process using a risk-based approach. The influence of process parameters (i.e. roll force, roll speed, roll gap and milling screen size) on different ribbon, granule and tablet properties was evaluated. In another study, we demonstrated the significant added value of the combination of near-infrared chemical imaging, texture analysis and multivariate methods in the quality assessment of the intermediate and final roll compaction products. Finally, we have also studied the roll compaction of an intermediate drug load formulation at different scales and using roll compactors with different feed screw mechanisms (i.e. horizontal and vertical). The horizontal feed screw roll compactor was also equipped with an instrumented roll technology allowing the measurement of normal stress on ribbon. Ribbon porosity was primarily found to be a function of normal stress, exhibiting a quadratic relationship. A similar quadratic relationship was also observed between roll force and ribbon porosity of the vertically fed roll compactor. A combination of design of experiments, latent variable and mechanistic models led to a better understanding of the critical process parameters and showed that scale up/transfer between equipment is feasible.

Dans l’industrie pharmaceutique, la granulation sèche par compactage à rouleaux est un procédé d’agglomération de poudres en granulés pour améliorer les propriétés d’écoulement nécessaire pour le procédé de compression en matrice. Comprendre le procédé de compactage à rouleaux et optimiser l’efficacité de production est limitée par l’utilisation de l’approche expérimentale à cause du coût élevé des poudres, le temps des essais et la complexité du procédé. Dans ce travail, une méthode d’éléments finis en 3D, est développée dans le but d’identifier les paramètres critiques du matériau et du procédé pour le contrôle de la qualité de la production. Le modèle de comportement de Drucker-Prager Cap est utilisé pour décrire le comportement en compression de poudres et sa calibration est déterminée à partir des essais standard. Pour surmonter la complexité liée à l’existence de deux mécanismes différents, l’alimentation en poudre par une vis sans fin et le compactage entre les rouleaux, une nouvelle méthode d’interfaçage entre la méthode des éléments discrets (DEM) employée pour décrire l’écoulement dans l’alimentation et la méthode des éléments finis (FEM) utilisée pour le compactage entre les rouleaux est développée. Enfin, pour une modélisation de compactage de rouleaux plus réaliste, prenant en compte la variation de l’entrefer entre les rouleaux, une nouvelle approche de couplage Euler-Lagrange est proposée. Les résultats de simulations par éléments finis montrent clairement l’effet des différents paramètres du procédé sur les distributions de pression et de densité dans la zone de compactage. En outre, les résultats montrent que l'utilisation de plaques de confinement de la poudre entre les rouleaux, développe une distribution de pression et de densité non homogène dans le compact, avec une densité plus élevée au centre et plus faible aux bords. D'autre part, l’utilisation de rouleaux dont l’un est surmonté d’une jante de confinement, a montré une distribution de propriétés globalement plus uniforme sur la largeur du compact avec des valeurs légèrement plus élevées aux bords qu’au centre. La méthodologie combinant les méthodes DEM & FEM montre clairement une corrélation directe entre la vitesse des particules entraînées par la vis dans la zone d’alimentation et la pression du rouleau. Tous les deux oscillent avec la même période. Cela se traduit par un compact anisotrope avec un profile de densité variant de manière sinusoïdale le long de sa largeur. Afin d'étudier la capacité du modèle à prédire les propriétés des compacts produits par compactage à rouleaux, les prédictions par simulations numériques sont comparées aux données de la littérature et validées par des mesures spécifiques. / In the pharmaceutical industry, dry granulation by roll compaction is a process of size enlargement of powder into granules with good flowability for subsequent die compaction process. Understanding the roll compaction process and optimizing manufacturing efficiency is limited using the experimental approach due to the high cost of powder, time-consuming and the complexity of the process. In this work, a 3D Finite Element Method (FEM) model was developed to identify the critical material properties, roll press designs and process parameters controlling the quality of the product. The Drucker-Prager Cap (DPC) model was used to describe the powder compaction behavior and was determined based on standard calibration method. To overcome the complexity involving two different mechanisms of powder feeding by the screw and powder compaction between rolls, a novel combined approach of Discrete Element Method (DEM), used to predict the granular material flow in the feed zone and the Finite Elements Method (FEM) employed for roll compaction, was developed. Lastly, for a more realistic roll compaction modelling, allowing the fluctuation of the gap between rolls, a Coupled-Eulerian Lagrangian (CEL) approach was developed. FEM simulation results clearly show the effect of different process parameters on roll pressure and density distribution in the compaction zone of powder between the rolls. Moreover, results show that using a cheek-plates sealing system causes a nonuniform roll pressure and density distribution with the highest values in the middle and the lowest at the edges. On the other hand, the resultant pressure and density distributions with the rimmed-roll obtained higher values in the edges than in the middle and overall a more uniform distribution. The combined DEM-FEM methodology clearly shows a direct correlation between the particle velocity driven by the screw conveyor to the feed zone and the roll pressure, both oscillating in the same period. This translates into an anisotropic ribbon with a density profile varying sinusoidally along its length. To validate the results, the simulations are compared with literature and experimentally measured values in order to assess the ability of the model to predict the properties of the produced ribbons.