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This work is concerned with determining empirical parameters in stress and fiber orientation models required to accurately simulate the fiber orientation in injection molded composites. An independent approach aims to obtain the material parameters using a sliding plate rheometer to measure the rheology of fiber suspensions at increased fiber lengths subjected to transient shear flow. Fiber orientation was measured in conjunction with shear stress to determine the relationship between stress and fiber orientation. Using a compression molding sample preparation procedure, the transient shear stress response was measured for glass and carbon fiber suspensions up to a number average fiber aspect ratio (length/diameter) of 100. Increases in concentration or fiber aspect ratio caused the magnitude of the stress response to increase by as much as an order of magnitude when compared to the suspending matrix. The degree of shear thinning at low shear rates also increased with increases in aspect ratio and concentration. The compression molding sample preparation procedure provided poor control of the initial fiber orientation which led to the investigation of samples subjected to flow reversal and samples generated through injection molding. The samples prepared through injection molding provided improved repeatability in the measured shear stress response and fiber orientation evolution during the startup of flow compared to compression molded samples and samples subjected to flow reversal. From repeatable stress and orientation evolution data, models for stress and fiber orientation were assessed independently. Current theories for stress were unable to reflect the overshoot in the measured stress response and could at best capture the steady state. The transient behavior of the fiber orientation models were found to be highly dependent on the initial fiber orientation. The repeatable orientation data obtained from the injection molding sample preparation procedure provided material parameters in the strain reduction factor and reduced strain closure models. The injection molded samples provided evolution data from different initial fiber orientations to provide further scrutiny or validation of the material parameters. Orientation model parameters that provided reasonable agreement to multiple sets of fiber evolution data in simple shear flow should allow for a better assessment of the orientation models in complex flow simulations. / Ph. D.

The dynamics of fiber orientation is of great interest for efforts to predict the microstructure and material properties of a suspension flow system. In this research a fiber-level, hybrid simulation method, LBM‒EBF (coupled lattice‒Boltzmann method with the external boundary force method) is undertaken to advance the current understanding of the hydrodynamic interaction induced rotational diffusion mechanism for rigid fibers in semidilute suspension of low Reynolds number flow. The LBM‒EBF simulations correctly predict the orbit constant distribution of fibers in a sheared semidilute suspension flow. It is demonstrated that an anisotropic, weak rotary diffusion model can fit the orbit constant distribution very well, but it can not describe the asymmetry in Stokes flow observed in semidilute suspension. The rotational diffusion process is then characterized with a three dimensional spatial tensor representation of the rotational diffusivity. A scalar measure of the rotational diffusion‒'scalar Folgar‒Tucker constant', C[subscript I], is extracted from this tensor. The study provides substantial numerical evidence that the range of C[subscript I] (0.0038 to 0.0165) obtained by Folgar&Tucker (J. reinf. plast. and comp, v.3, 1984) in a semidilute regime is overly diffusive, and that the correct magnitude is of O(10⁻⁴). The study reveals that the interactions among fibers become more frequent with either the decrease of fiber aspect-ratio, r[subscript p] (keeping nL³ constant, where n is the fiber number density, and L is the fiber length) or with the increase of nL³ (keeping r[subscript p] constant) in the semidilute regime, which in consequence causes an increase in C[subscript I]. The rheological properties of sheared semidilute suspension are also computed with direct LBM‒EBF simulations. The LBM‒EBF investigation is extended to characterize the fiber orientation in a linearly contracting channel similar to a paper machine 'headbox'. It is found that the rotational diffusion is the predominant term over the strain rate in the semidilute regime for a low Reynolds number flow, and it results in a decreasing trend of rotational Peclet number, Pe, along the contraction centerline. Lastly, in order to improve the numerical consistency of the existing LBM‒EBF approach, a modification to the body force term in the LB equation is suggested, which can recover the exact macroscopic hydrodynamics from the mesoscale.

Rheological properties of idealised models which exhibit all the non-Newtonian flow phenomenology commonly seen in dense suspensions are investigated by particulate-dynamics computer-simulations. The objectives of these investigations are: (i) to establish the origins of various aspects of dense suspension rheology such as shear-thinning, shear thickening and dilatancy; (ii) to elucidate the different regions of a typical dense suspension rheogram by examining underlying structures and shear induced anisotropies in kinetic energy, diffusivity and pressure; (iii) to investigate the scaling of the simplest idealised model suspension; i.e. the hard-sphere model in Newtonian media and its relationship to the isokinetic flow curves obtained through non-equilibrium molecular dynamics (NEMD) simulations; (iv) to preliminarily determine the effect of perturbations present in all real colloidal suspensions, namely particle size polydispersity and a slight 'softness' of the interparticle potential. Non-equilibrium isokinetic simulations have been performed upon ;systems of particles interacting through the classical hard-sphere potential and a perturbation thereof, in which the hard-core is surrounded by a 'slightly soft' repulsive skin. The decision to base the present work upon isokinetic studies was made in order to obtain a better under- standing of suspension rheology by making a direct connection with previous NEMD studies of thermal systemst(93). These studies have shown that the non-linear behaviour exhibited by these systems under shear is atttributable to a shear-induced perturbation of the equilibrium phase behaviour. The present study shows this behaviour to correspond to the high shear region of the generalised suspension flow curve.

A suspension is a fully saturated mixture of discrete solid particles and interstitial liquid. Examples of suspensions include pastes, slurries, cement, food-spreads, drilling fluids and some geophysical flows. The present work focusses on granular (as opposed to colloidal) suspensions, which we define as those for which the thermal motion of the solid particles is negligible. Despite such ubiquity in industry and nature, our understanding of the mechanical properties of suspensions lags behind that of their constituent solid and liquids. In this thesis, the discrete element method is used to simulate suspension flow in shear, capillary and constriction geometries, mapping and characterising the fundamental flow, or rheological, regimes. As a starting point (Chapter 2), we consider an established regime map for dry granular materials, appropriate for flows of sand, grains and dry debris. Taking guidance from shear flow simulations that consider the lubricating effect of an interstitial liquid, we recast the regime map for a general suspension, elucidating flows comparable to the dry material or to a viscous liquid, dependent on the shear rate, liquid viscosity and particle stiffness. We give an account of the microstructural traits associated with each regime. Motivated by recent groundbreaking theoretical, computational and experimental work, we incorporate the emerging picture of frictional shear thickening into our regime map (Chapter 3). Our shear flow simulations capture the shear thickening behaviour and demonstrate that it may, in principle, occur in any of the identified flow regimes. Our simulations of time-dependent shear flows (Chapter 4), specifically flow reversal, provide a detailed micro-mechanical explanation of a longstanding and previously unexplained experimental finding, guiding future experimentalists in decomposing the particle and liquid contributions to the viscosity of any suspension. Indeed, the findings have already been exploited in the devising of an experimental protocol that has successfully proven the dominance of particle contacts in driving shear thickening. We next consider suspension flow in a microchannel (Chapter 5), finding that the identified shear flow regimes are locally applicable to flows in complex geometries under inhomogeneous stress conditions only when the local mean shear rate exceeds temporal velocity fluctuations. A more comprehensive description is therefore required to fully characterise the flow behaviour in this geometry. Finally (Chapter 6), we simulate pressure driven suspension flow through a constriction geometry, observing highly inhomogeneous stress distributions and velocity profiles. The roles of particle and fluid properties are considered in the context of an industrial paste extrusion process.

Three-dimensional printing is renowned for its ability to produce complex geometries. By utilizing a pressure-driven additive manufacturing (AM) process called direct ink write (DIW) with polymer composite ink, it is possible to create parts with tailored internal microstructures that enhance surface area and particle-particle adsorption kinetics for water remediation applications. However, DIW of particle-filled systems faces challenges, particularly nozzle clogging. This paper explores the relationship between dispersion of aggregate size, torsional rheology, and the capacity to print relatively highly particle-filled systems. Various characterization methods, including torsional rheology, dynamic light scattering (DLS), and field emission scanning electron microscopy (FESEM) were employed utilizing a chitosan-graphene-titanium dioxide (CS-G-TiO2) polymer composite ink composed of TiO2 nanoparticles (1 wt.% to 25 wt.%), graphene (1 wt.%), and chitosan (5 wt.% to 9 wt.%) to evaluate the effect of ultrasonication techniques (bath vs. probe) on aggregate size. Probe-sonicated dispersions showed a more narrow monodispersed and unimodal aggregate size distribution with a primary average aggregate size of 255 nm. In contrast, bath-sonicated dispersions exhibited a moderately polydispersed, trimodal distribution with modes centered at 90 nm, 295 nm, and 5.6 μm. Non-Newtonian rheological parameters such as yield stress, complex viscosity, storage, and loss moduli were higher for the probe-sonicated CS-G-TiO2 composite ink than for the bath-sonicated CS-G-TiO2 composite ink. This increase is likely attributed to enhanced particle interactions, which allow for greater CS adsorption. These findings offer valuable insights into optimizing formulations for desired rheological properties in DIW printing. The results enable the direct ink writing of intricate geometries with high surface areas and less shape distortion, providing significant insights into processing similar multi-component slurry-based composite inks for DIW. / Master of Science / Researchers are exploring new ways to remove harmful toxins from waterbodies using 3D printing technology. By employing a specialized additive manufacturing (AM) printing process called direct ink write (DIW) and a composite ink (CS-G-TiO2) composed of chitosan (CS), graphene (G), and titanium dioxide (TiO2), it is possible to create parts with a tailored internal microstructure that allows for greater surface area and enhanced particle-particle adsorption kinetics. However, challenges remain with DIW of particle-filled systems, particularly regarding nozzle clogging. This assessment focuses on how the size of aggregates in G-TiO2 dispersions affects printability and the rheological behavior of the CS-G-TiO2 composite inks. To address these issues, different ultrasonication techniques and their effects on aggregate size were investigated, as well as the shear-thinning and yield stress behavior of the inks. These findings could be further analyzed to understand the underlying mechanism in particle aggregation and optimize the formulation for desired rheological properties for direct ink write (DIW) printing.

The objective of the research was to develop fundamental understanding of the process of deposition of complex mixtures by the inkjet method. The rheological properties and DOD drop formation dynamics of carbon black pigmented inkjet inks were investigated. It was found that the suspension microstructure responses to bulk motions, leading to shear rate and time dependent shear viscosity. However, DOD drop formation dynamics of highly pigmented inkjet ink and pure Newtonian fluid is similar even though shear rate up to 105 s-1 exists during inkjet jetting process. A proposed explanation for these observations is that the shearing time during DOD drop ejection is insufficient for changing and stabilizing the microstructure of the suspension. The effects of signal amplitude and jetting frequency on DOD drop formation dynamics of pure Newtonian fluids were investigated. A transition of DOD drop formation dynamics when the inkjet nozzle is switched from idle to jetting was identified. A qualitative investigation of DOD drop impaction and post-impaction behavior on inkjet paper and textiles was carried out. Dynamics of DOD drop accumulation and spreading on the substrates and final ink distribution show drastic differences between these two substrates.

High surface area of used nanoparticles and their comparable size with polymer chains, are the most important characteristics of fillers in the preparation of non-Newtonian suspensions. Such structures at different concentrations have major influence on the rheological behavior of polymer solution in solvent. With increasing volume fraction of nanofiller, there is pseudoplastic or dilatant behavior present in the dissolved elastomers. Diploma thesis studies the influence of the concentration of different elastomers (SBR and SEBS copolymers) and nanofiller (hydrophobic nanosilica) in suspension, of rheological properties.

Determination of the relation between the bulk or rheological properties of a particle suspension and its microscopic structure is an old and important problem in physical science. In general, the rheology of particle suspension is quite complex, and the problem becomes even more complicated if the suspending particle is deformable. Despite these difficulties, a large number of theoretical and experimental investigations have been devoted to the analysis and prediction of the rheological behavior of particle suspensions. However, among these studies there are very few investigations that focus on the role of particle deformability. A novel method for full coupling of the fluid-solid phases with sub-grid accuracy for the solid phase is developed. In this method, the flow is computed on a fixed regular 'lattice' using the lattice Boltzmann method (LBM), where each solid particle, or fiber, is mapped onto a Lagrangian frame moving continuously through the domain. The motion and orientation of the particle are obtained from Newtonian dynamics equations. The deformable particle is modeled by the lattice-spring model (LSM).The fiber deformation is calculated by an efficient flexible fiber model. The no-slip boundary condition at the fluid-solid interface is based on the external boundary force (EBF) method. This method is validated by comparing with known experimental and theoretical results. The fiber simulation results show that the rheological properties of flexible fiber suspension are highly dependent on the microstructural characteristics of the suspension. It is shown that fiber stiffness (bending ratio BR) has strong impact on the suspension rheology in the range BR < 3. The relative viscosity of the fiber suspension under shear increases significantly as BR decreases. Direct numerical simulation of flexible fiber suspension allows computation of the primary normal stress difference as a function of BR. These results show that the primary normal stress difference has a minimum value at BR ∼ 1. The primary normal stress differences for slightly deformable fibers reaches a minimum and increases significantly as BR decreases below 1. The results are explained based on the Batchelor's relation for non-Brownian suspensions. The influence of fiber stiffness on the fiber orientation distribution and orbit constant is the major contributor to the variation in rheological properties. A least-squares curve-fitting relation for the relative viscosity is obtained for flexible fiber suspension. This relation can be used to predict the relative viscosity of flexible fiber suspension based on the result of rigid fiber suspension. The unique capability of the LBM-EBF method for sub-grid resolution and multiscale analysis of particle suspension is applied to the challenging problem of platelet motion in blood flow. By computing the stress distribution over the platelet, the "blood damage index" is computed and compared with experiments in channels with various geometries [43]. In platelet simulation, the effect of 3D channel geometry on the platelet activation and aggregation is modeled by using LBM-EBF method. Comparison of our simulations with Fallon's experiments [43] shows a similar pattern, and shows that Dumont's BDI model [40] is more appropriate for blood damage investigation. It has been shown that channels with sharp transition geometry will have larger recirculation areas with high BDI values. By investigating the effect of hinge area geometry on BDI value, we intend to use this multiscale computational method to optimize the design of Bileaflet mechanical heart valves. Both fiber simulations and platelet simulations have shown that the novel LBM-EBF method is more efficient and stable compare to the conventional numerical methods. The new EBF method is a two-Cway coupling method with sub-grid accuracy which makes the platelet simulations possible. The LBM-EBF is the only method to date, to the best of author's knowledge, that can simulate suspensions with large number of deformable particles under complex flow conditions. It is hoped that future researchers may benefit from this new method and the algorithms developed here.

Lecithin wird unter anderem zur Steuerung der rheologischen Eigenschaften von Lebensmittelsuspensionen wie zum Beispiel Schokolade eingesetzt. In erster Linie findet dabei Sojalecithin Verwendung, wogegen die Wirkungen von Lecithinen aus Sonnenblumen oder Raps unzureichend dokumentiert sind. Anhand von Untersuchungen an Modellsuspensionen werden Wirkungsbeziehungen von Lecithin auf mikrostruktureller Ebene beleuchtet, um Ursachen für dessen Funktionalität in ölbasierten Suspensionen abzuleiten. Darüber hinaus erfolgt ein Vergleich der Wirkung von Soja-, Raps- und Sonnenblumenlecithin auf rheologische, sensorische und morphologische Eigenschaften von Schokolade. Rheologische Untersuchungen an Zucker/Öl- und Glaskugel/Öl-Suspensionen verdeutlichen den Einfluss der Suspensionsbestandteile auf die Wirkung von Lecithin in ölbasierten Suspensionen. Sedimentationsanalysen an Zucker/Öl-Suspensionen zeigen, dass die Reduktion der rheologischen Parameter mit der Senkung des Sedimentvolumens und einer verstärkt polydispersen Sedimentation einhergeht. Glaskugel/Öl-Suspensionen bilden im Vergleich zu Zucker/Öl-Suspensionen ein deutlich kompakteres Sediment, was auf geringer ausgeprägte Interaktionen zwischen den Glaspartikeln hindeutet und durch Untersuchungen mittels Rasterkraftmikroskop bestätigt wird. Die Anreicherung des Dispersionsmediums mit Lecithin führt zur Adsorption von grenzflächenaktiven Molekülen an der fest/flüssig-Grenzfläche und reduziert die adhäsiven Kräfte zwischen Zuckeroberflächen. In Zucker/Sojaöl-Suspensionen zeigen die Phospholipide Phosphatidsäure, Phosphatidylcholin und Phosphatidylethanolamin im Vergleich zu Sojalecithin eine geringer ausgeprägte Funktionalität bei kleinen Phospholipidkonzentrationen. Soja-, Raps- und Sonnenblumenlecithine besitzen in dunkler und in milchhaltiger Schokoladenmasse lediglich hinsichtlich ihrer Wirkung auf die Fließgrenze leichte Unterschiede. Die Präparate zeigen keine verallgemeinerbaren Wirkunterschiede auf die Fettkristallmorphologie und die Textur von gelagerter dunkler und milchhaltiger Schokolade. Des Weiteren lassen sensorische Untersuchungen keine signifikant ausgeprägte Präferenz für dunkle oder milchhaltige Schokolade erkennen, wenn die Probe mit Soja-, Raps- oder Sonnenblumenlecithin versetzt wird. Die Ergebnisse zeigen, dass die Reduktion der adhäsiven Kräfte zwischen Zuckerpartikeln eine Ursache für die Senkung der rheologischen Parameter und des Sedimentvolumens von Zucker/Öl-Suspensionen darstellt. Außerdem ist zu erkennen, dass bei geringen Phospholipidkonzentrationen synergetische Effekte zwischen unterschiedlichen grenzflächenaktiven Substanzen zu einem Anstieg der Funktionalität des eingesetzten Präparates führen können. Darüber hinaus ist festzustellen, dass Soja-, Raps- und Sonnenblumenlecithin die rheologischen, sensorischen und morphologischen Eigenschaften von Schokolade in gleichem Maß beeinflussen. / Lecithin is used in the food industry, for example to control the rheological properties of oil-based suspensions, such as chocolate. First and foremost, soybean lecithin is used, whereas the effects of possible alternatives, such as lecithin from sunflower or canola, are still insufficient documented. On the basis of model suspensions the effect of lecithin on the microstructural level will be investigated to derive causes of the functionality of the surfactant in oil-based suspensions. Additionally, a comparison is made regarding the effects of soybean lecithin, canola lecithin and sunflower lecithin on the rheological and morphological properties as well as on sensory characteristics of chocolate. Rheological studies illustrate the influence of the suspension components to the action of lecithin in oil-based suspensions. While, in sugar/oil-suspensions, lecithin reduces apparent viscosity and yield stress, the effect of the surfactant in glass sphere/oil-suspensions depends on the dispersion medium. Sedimentation analyses of sugar/oil-suspensions show that the reduction of the rheological parameters coincides with the reduction of the sediment volume and an increased polydisperse sedimentation. The sediment of glass sphere/oil-suspensions is more compact in comparison to sugar/oil-suspensions, indicating less pronounced interactions between glass spheres. Investigations using atomic force microscopy show the less pronounced interactions between glass spheres. While interactions (adhesive forces) are detectable between sugar surfaces dispersed in oil, no interactions can be determined between glass surfaces. The enrichment of the dispersion medium with lecithin results in the adsorption of the surfactants at the sugar surface and reduces the adhesive forces. In sugar/soybean oil suspensions and at low phospholipid concentrations the results indicate a less pronounced functionality of the individual phospholipids, phosphatidylcholine, phosphatidylethanolamine and phosphatidic acid in comparison to soybean lecithin. In dark chocolate and milk chocolate soybean lecithin, canola lecithin and sunflower lecithin reduces apparent viscosity at low to medium shear rate in the same way. In contrast, small differences in terms of their effect on the yield stress are observed. The lecithins do not show differences regarding their impact on fat crystal morphology and texture of stored dark chocolate and milk chocolate. Furthermore, in sensory studies, no significant preference differences were detectable in case of dark chocolate or milk chocolate containing soybean lecithin, canola lecithin or sunflower lecithin. The results show that the reduction of the adhesive forces between sugar particles causes the reduction of rheological parameters and the sediment volume of sugar/oil-suspensions. Furthermore, at low phospholipid concentrations possible synergistic effects between different surfactants can lead to an increase of the functionality of suractants. Additionally it can be concluded that soybean lecithin, canola lecithin and sunflower lecithin affect the rheological and morphological properties as well as the sensory characteristics of chocolate in equal measure.