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Showing papers in "Rheologica Acta in 2009"


Journal ArticleDOI
TL;DR: An overview of present understanding of microstructure in flowing suspensions is provided in this paper, where an emphasis is placed on how the micro-structure leads to observable bulk flow phenomena unique to mixtures.
Abstract: An overview of present understanding of microstructure in flowing suspensions is provided. An emphasis is placed on how the microstructure leads to observable bulk flow phenomena unique to mixtures. The bridge between the particle and bulk scales is provided by the mixture rheology; one focus of the review is on work that addresses the connection between microstructure and rheology. The non-Newtonian rheology of suspensions includes the well-known rate dependences of shear thinning and thickening, which have influence on bulk processing of suspensions. Shear-induced normal stresses are also measured in concentrated suspensions and include normal stress differences, and the isotropic particle pressure. Normal stresses have been associated with shear-induced migration, and thus have influence on the ultimate spatial distribution of solids, as well as the flow rate during processing; a second focus is on these uniquely two-phase behaviors and how they can be described in terms of the bulk rheology. An important bulk fluid mechanical consequence of normal stresses is their role in driving secondary flows.

240 citations


Journal ArticleDOI
TL;DR: In this article, the phenomenological aspects and physical origin of shear localization and shear banding in various material types, namely emulsions, suspensions, colloids, granular materials, and micellar systems, are reviewed and compared.
Abstract: We review and compare the phenomenological aspects and physical origin of shear localization and shear banding in various material types, namely emulsions, suspensions, colloids, granular materials, and micellar systems. It appears that shear banding, which must be distinguished from the simple effect of coexisting static-flowing regions in yield stress fluids, occurs in the form of a progressive evolution of the local viscosity toward two significantly different values in two adjoining regions of the fluids in which the stress takes slightly different values. This suggests that from a global point of view, shear banding in these systems has a common physical origin: Two physical phenomena (for example, in colloids, destructuration due to flow and restructuration due to aging) are in competition, and depending on the flow conditions, one of them becomes dominant and makes the system evolve in a specific direction.

198 citations


Journal ArticleDOI
TL;DR: In this article, a set of rheological, electrical, and thermal conductivity measurements of polycarbonate/multiwalled carbon nanotube nanocomposites were analyzed using TEM, SEM, and AFM techniques.
Abstract: This paper is concerned with several issues related to the rheological behavior of polycarbonate/multiwalled carbon nanotube nanocomposites. The composites were prepared by diluting a masterbatch of 15 wt.% nanotubes using melt-mixing method, and the dispersion was analyzed by SEM, TEM, and AFM techniques. To understand the percolated structure, the nanocomposites were characterized via a set of rheological, electrical, and thermal conductivity measurements. The rheological measurements revealed that the structure and properties were temperature dependent; the percolation threshold was significantly lower at higher temperature suggesting stronger nanotube interactions. The nanotube networks were also sensitive to the steady shear deformation particularly at high temperature. Following preshearing, the elastic modulus decreased markedly suggesting that the nanotubes became more rigid. These results were analyzed using simple models for suspensions of rod-like particles. Finally, the rheological, electrical, and thermal conductivity percolation thresholds were compared. As expected, the rheological threshold was smaller than the thermal and electrical threshold.

160 citations


Journal ArticleDOI
TL;DR: In this article, a collaborative effort to measure the rheology of a biomass slurry at four separate laboratories has been undertaken, and a comprehensive set of rheological properties were measured using several different rheometers, flow geometries, and experimental methods.
Abstract: The conversion of biomass, specifically lignocellulosic biomass, into fuels and chemicals has recently gained national attention as an alternative to the use of fossil fuels. Increasing the concentration of the biomass solids during biochemical conversion has a large potential to reduce production costs. These concentrated biomass slurries have highly viscous, non-Newtonian behavior that poses several technical challenges to the conversion process. A collaborative effort to measure the rheology of a biomass slurry at four separate laboratories has been undertaken. A comprehensive set of rheological properties were measured using several different rheometers, flow geometries, and experimental methods. The tendency for settling, water evaporation, and wall slip required special care when performing the experiments. The rheological properties were measured at different concentrations up to 30% insoluble solids by mass. The slurry was found to be strongly shear-thinning, to be viscoelastic, and to have a significant concentration-dependent yield stress. The elastic modulus was found to be almost an order of magnitude larger than the loss modulus and weakly dependent on frequency. The techniques and results of this work will be useful to characterize other biomass slurries and in the design of biochemical conversion processing steps that operate at high solids concentrations.

159 citations


Journal ArticleDOI
TL;DR: In this article, an investigation related to the rheological behavior of alkali-activated fly-ash pastes (AAFA) is described, and it is shown that the most efficient admixtures for these new cementitious pastes are those based in polycarboxylates.
Abstract: In this paper, an investigation related to the rheological behaviour of alkali-activated fly-ash pastes (AAFA) is described. Those pastes were prepared by mixing the fly ash with an alkaline dissolution containing 85% of a 12.5 M NaOH solution and 15% of waterglass and adding some commercial chemical admixtures usually used in the Portland cement concrete fabrication, like lignosulphonates, melamines (first and second generation products) and polycarboxylates (latest generation). The fly ash rheological data were determined by rotational viscometry measurements as well as by the use of the flow table test. Results indicate that chemicals admixtures used do not work the same in the Portland cement systems than in alkali-activated fly ash systems. As a general rule, it seems that the most efficient admixtures for these new cementitious pastes (AAFA) are those based in polycarboxylates.

141 citations


Journal ArticleDOI
TL;DR: In this paper, a method of flow-ultra small angle neutron scattering was used to probe the colloidal microstructure under steady flow conditions on length scales suitable to characterize the formation of hydroclusters.
Abstract: Reversible shear thickening in colloidal suspensions is a consequence of the formation of hydroclusters due to the dominance of short-ranged lubrication hydrodynamic interactions at relatively high shear rates. Here, we develop and demonstrate a new method of flow-ultra small angle neutron scattering to probe the colloidal microstructure under steady flow conditions on length scales suitable to characterize the formation of hydroclusters. Results are presented for a model near hard-sphere colloidal suspension of 260 nm radius (10% polydisperse) sterically stabilized silica particles in poly(ethylene glycol) at shear rates in the shear thinning and shear thickening regime for dilute, moderately concentrated, and concentrated (ordered) suspensions. Hydrocluster formation is observed as correlated, broadly distributed density fluctuations in the suspension with a characteristic length scale of a few particle diameters. An order–disorder transition is observed to be coincident with shear thickening for the most concentrated sample, but the shear-thickened state shows hydrocluster formation. These structural observations are correlated to the behavior of the shear viscosity and discussed within the framework of theory, simulation, and prior experiments.

112 citations


Journal ArticleDOI
TL;DR: In this article, an experimental investigation of the solid-fluid transition in a yield stress shear thinning physical gel (Carbopol® 940) under shear is presented, where the deformation power corresponding to the hysteresis region scales linearly with the rate at which the material is being forced.
Abstract: We present an experimental investigation of the solid–fluid transition in a yield stress shear thinning physical gel (Carbopol® 940) under shear. Upon a gradual increase of the external forcing, we observe three distinct deformation regimes: an elastic solid-like regime (characterized by a linear stress–strain dependence), a solid–fluid phase coexistence regime (characterized by a competition between destruction and reformation of the gel), and a purely viscous regime (characterized by a power law stress-rate of strain dependence). The competition between destruction and reformation of the gel is investigated via both systematic measurements of the dynamic elastic moduli (as a function of stress, the amplitude, and temperature) and unsteady flow ramps. The transition from solid behavior to fluid behavior displays a clear hysteresis upon increasing and decreasing values of the external forcing. We find that the deformation power corresponding to the hysteresis region scales linearly with the rate at which the material is being forced (the degree of flow unsteadiness). In the asymptotic limit of small forcing rates, our results agree well with previous steady state investigations of the yielding transition. Based on these experimental findings, we suggest an analogy between the solid–fluid transition and a first-order phase transition, e.g., the magnetization of a ferro-magnet where irreversibility and hysteresis emerge as a consequence of a phase coexistence regime. In order to get further insight into the solid–fluid transition, our experimental findings are complemented by a simple kinetic model that qualitatively describes the structural hysteresis observed in our rheological experiments. The model is fairly well validated against oscillatory flow data by a partial reconstruction of the Pipkin space of the material’s response and its nonlinear spectral behavior.

109 citations


Journal ArticleDOI
TL;DR: In this article, a method for the determination of highly precise continuous relaxation spectra is presented, based on the use of piecewise cubic Hermite splines, which are fairly easy to tabulate by using their knots.
Abstract: We present a new method for the determination of highly precise continuous relaxation spectra. The method is based on the use of piecewise cubic Hermite splines, which are fairly easy to tabulate by using their knots. The Hermite splines method allows a continuous description of the spectrum by a series of polynomial functions. The numerical instabilities of the spectrum calculation are minimized by limiting the slope of the spectrum to physically meaningful values. The reproducibility of the spectrum calculation is within an error margin of about ±10% in the physically relevant relaxation time range. This method is able to retrieve the spectrum based on data calculated from a benchmark with high accuracy and precision.

98 citations


Journal ArticleDOI
TL;DR: The damping function has been a concept introduced in rheology since more than 30 years ago, and although a similar concept was already earlier implemented in studying rubber materials, its implementation in the modeling of polymer melts was an essential step forward in the classification and understanding of nonlinear viscoelasticity phenomena as discussed by the authors.
Abstract: The damping function has been a concept introduced in rheology since more than 30 years ago, and although a similar concept was already earlier implemented in studying rubber materials, its implementation in the modeling of polymer melts was an essential step forward in the classification and understanding of nonlinear viscoelasticity phenomena. It is the objective of this contribution to give an overview on the theoretical background and physical interpretation of the concept of the damping function for different types of deformation, as well as a review on the experimental results including the experimental artefacts to be considered. Besides homopolymers, a summary is given on different investigations of other types of systems, where the concept of the damping function has also been applied, for example, rubbers, rubber-like materials, block copolymers, polymer composites, liquid crystals, polymer blends, suspensions, emulsions, micellar systems, and in food rheology.

95 citations


Journal ArticleDOI
TL;DR: In this article, the authors investigate the rheology of dilute dispersions of fumed colloidal particles with attractive interactions in hydrocarbon liquids and show that these systems display shear thickening due to the breakdown of densified flocs and a concomitant increase in the effective volume fraction of fractal particles in the fluid.
Abstract: We investigate the rheology of dilute dispersions of fumed colloidal particles with attractive interactions in hydrocarbon liquids. Surprisingly, these systems display shear thickening due to the breakdown of densified flocs and a concomitant increase in the effective volume fraction of the fractal particles in the fluid. We show that this shear thickening is controlled by a critical stress and accompanied by a positive increase in the first normal stress difference, N 1, at the shear thickening transition. This is in contrast to the well-known hydrocluster mechanism of shear thickening in concentrated hard-sphere and repulsive systems. Gel elasticity depends strongly on the stress applied to suspensions in preshear, scaling roughly as $G'\sim\sigma_{\text{preshear}}^{2}$ . We propose a simple model to account for these results in terms of the cluster number density determined by the preshear stress. At low shear rates, vorticity-aligned aggregates are present at $\dot\gamma\approx 10^0 {\rm{s}}^{-1}$ . In this regime, the system displays a small but noticeable increase in viscosity on increasing shear rate. We investigate the effect of tool roughness and find that wall slip is not responsible for the observed phenomena. Instead, the increase in the apparent viscosity results from increased flow resistance due to the presence of gap-spanning log-like flocs in rolling flow.

88 citations


Journal ArticleDOI
TL;DR: In this article, a rearrangement of the classical Cox and Merz rule suggests that the shear stress value of steady shear flow, τ, and complex modulus value of small amplitude oscillatory shear, G∗∗(ω) = (G′2 + G″2)1/2, are equivalent in many respects.
Abstract: A slight rearrangement of the classical Cox and Merz rule suggests that the shear stress value of steady shear flow, $\tau (\mathop \gamma \limits^. )$ , and complex modulus value of small amplitude oscillatory shear, G ∗ (ω) = (G′2 + G″2)1/2, are equivalent in many respects. Small changes of material structure, which express themselves most sensitively in the steady shear stress, τ, show equally pronounced in linear viscoelastic data when plotting these with G ∗ as one of the variables. An example is given to demonstrate this phenomenon: viscosity data that cover about three decades in frequency get stretched out over about nine decades in G ∗ while maintaining steep gradients in a transition region. This suggests a more effective way of exploiting the Cox–Merz rule when it is valid and exploring reasons for lack of validity when it is not. The τ −G ∗ equivalence could also further the understanding of the steady shear normal stress function as proposed by Laun.

Journal ArticleDOI
TL;DR: In this article, a series of experiments in which the step-stretch parameters of final length, and the extension rate of the stretch were varied and their effects on the measured extensional viscosity and extensional relaxation time were recorded.
Abstract: Extensional rheometry has only recently been developed into a commercially available tool with the introduction of the capillary breakup extensional rheometer (CaBER). CaBER is currently being used to measure the transient extensional viscosity evolution of mid to low-viscosity viscoelastic fluids. The elegance of capillary breakup extensional experiments lies in the simplicity of the procedure. An initial step-stretch is applied to generate a fluid filament. What follows is a self-driven uniaxial extensional flow in which surface tension is balanced by the extensional stresses resulting from the capillary thinning of the liquid bridge. In this paper, we describe the results from a series of experiments in which the step-stretch parameters of final length, and the extension rate of the stretch were varied and their effects on the measured extensional viscosity and extensional relaxation time were recorded. To focus on the parameter effects, well-characterized surfactant wormlike micelle solutions, polymer solutions, and immiscible polymer blends were used to include a range of characteristic relaxation times and morphologies. Our experimental results demonstrate a strong dependence of extensional rheology on step-stretch conditions for both wormlike micelle solutions and immiscible polymer blends. Both the extensional viscosity and extensional relaxation time of the wormlike micelle solutions were found to decrease with increasing extension rate and strain of the step-stretch. For the case of the immiscible polymer blends, fast step-stretches were found to result in droplet deformation and an overshoot in the extensional viscosity which increased with increasing strain rates. Conversely, the polymer solutions tested were found to be insensitive to step-stretch parameters. In addition, numerical simulations were performed using the appropriate constitutive models to assist in both the interpretation of the CaBER results and the optimization of the experimental protocol. From our results, it is clear that any rheological results obtained using the CaBER technique must be properly considered in the context of the stretch parameters and the effects that preconditioning has on viscoelastic fluids.

Journal ArticleDOI
TL;DR: In this article, low-density polyethylenes (LDPE) were synthesized in a laboratory-scale autoclave under high pressure, and they were found to possess a high molar mass tail, resulting in a distinctly bimodal distribution and a lower concentration of long-chain branching than typical of commercial LDPEs.
Abstract: Low-density polyethylenes (LDPE) were synthesized in a laboratory-scale autoclave under high pressure These samples were found to possess a high molar mass tail, resulting in a distinctly bimodal molar mass distribution and a lower concentration of long-chain branching than typical of commercial LDPEs Rheological experiments in elongation showed that these samples exhibit a very pronounced strain hardening, which could be favorable for distinct processing operations Although the samples have a rather high molar mass (\(M_{\rm w} = 2{\ldots}4 \times 10^{6}\) g/mol), their zero shear-rate viscosities η0 and their shear thinning behavior are still in a range, where thermoplastic processing is possible A qualitative understanding of the experimental results is tried by the model of the Cayley tree

Journal ArticleDOI
TL;DR: In this paper, the authors used steady and dynamic rheometry to detect non-flocculated suspensions in polypropylene glycol, in which hydroxyl groups have been mostly substituted by alkyls groups.
Abstract: We have found in this study, by means of steady and dynamic rheometry, that Aerosil® R816 particles, in which hydroxyl groups have been mostly substituted by alkyls groups, form nonflocculated suspensions in polypropylene glycol, in comparison to what was expected from previous studies. Steady flow curve shows shear-thickening behavior between two shear-thinning regions. The transient rheological response has been analyzed using a protocol proposed a long time ago by Cheng (Rheol Acta 25:542–554, 1986). It has been found that, within the reversible shear-thickening region, all the constant structure curves overlap, which suggests that the response at a certain shear rate does not depend significantly on the previous state. As a consequence, this protocol is proposed as an alternative technique for distinction between flocculated and nonflocculated suspensions.

Journal ArticleDOI
TL;DR: In this article, a review of recent results on dense, non-Brownian suspensions is presented, and simple invariance arguments permit to clarify the conditions of occurrence of viscous and inertial scaling in suspensions, and show in particular that both may occur in dense flows even in the presence of significant contact forces.
Abstract: Recent years have seen significant progress in our understanding of the rheology of dry granular materials. A scale invariance of equations of motion in the rigid grain limit has helped identifying dimensionless quantities which govern flow. After a review of recent results on dry granular materials, we show how this same dimensional analysis carries over to the case of dense, non-Brownian suspensions. Our review is based on compiled data from various sets of numerical simulations, using both molecular and contact dynamics. It covers the breakdown of kinetic theory, which arises when contact forces dominate collisional forces in inertial flows, and the approach to dense flows up to the quasi-static limit. We show that simple invariance arguments permit to clarify the conditions of occurrence of viscous and inertial scaling in suspensions, and show in particular that both may occur in dense flows even in the presence of significant contact forces, up to the jamming limit. Some implications of the properties of steady uniform quasistatic granular flow under constant pressure for very dense suspensions near the maximum concentration are also discussed.

Journal ArticleDOI
TL;DR: In this paper, the authors investigated the yield stress of ferrofluid-based magnetorheological fluids (F-MRF) and proposed a scaling relation for yield stress modeling.
Abstract: In this work, the yield stress of ferrofluid-based magnetorheological fluids (F-MRF) was investigated. The fluids are composed of a ferrofluid as the liquid carrier and micro-sized iron particles as magnetic particles. The physical and magnetorheological properties of the F-MRF have been investigated and compared with a commercial mineral oil-based MR fluid. With the addition of a ferrofluid, the anti-sedimentation property of the commercial MR fluids could be significantly improved. The static yield stress of the F-MRF samples with four different weight fractions (ϕ) of micro-sized iron particles were measured using three different testing modes under various magnetic fields. The effects of weight fraction, magnetic strength, and test mode on the yielding stress have been systematically studied. Finally, a scaling relation, $\tau _{\rm ys} = {\rm a}B^{\rm b}$ , was proposed for the yield stress modeling of the F-MRF system.

Journal ArticleDOI
TL;DR: Three-dimensional holographic particle tracking is used to perform microrheological measurements of model gelled media, including the polysaccharide pellicle of dental biofilms created by the common cariogenic oral pathogen Streptococcus mutans.
Abstract: We use three-dimensional holographic particle tracking to perform microrheological measurements of model gelled media, including the polysaccharide pellicle of dental biofilms created by the common cariogenic oral pathogen Streptococcus mutans. Nanometer-resolution video-rate holographic tracking of embedded colloidal spheres provides accurate measurements of the gels’ complex viscoelastic moduli, including insights into these properties’ heterogeneity. When applied to polysaccharides of S. mutans biofilms, these techniques promise quantitative microscopic assays for candidate therapeutic agents against cariogenic dental biofilms.

Journal ArticleDOI
TL;DR: In this article, a quasi-one-dimensional model is used to describe the self-thinning process of carbon nanotubes in uniaxial elongation and simple shear.
Abstract: Rheological behavior of concentrated suspensions of chemical vapor deposition carbon nanotubes in uniaxial elongation and simple shear is studied experimentally and theoretically. Nanotubes are suspended in viscous host liquids—castor oil or its blends with n-decane. The elongational measurements are performed by analyzing self-thinning (due to surface tension effect) liquid threads of nanotube suspensions. A quasi-one-dimensional model is used to describe the self-thinning process, whereas corrections accounting for thread nonuniformity and necking are introduced a posteriori. The effects of nanotube concentration and aspect ratio, viscosity of the suspending liquid, and initial diameter of the self-thinning thread in uniaxial elongation are elucidated. The results for uniaxial elongation are compared with those for simple shear. The correspondence in the results of the shear and elongational measurements is addressed and interpreted. The results conform to the Herschel–Bulkley rheological constitutive equation (i.e., power law fluids with yield stress). However, the yield stress in elongation is about 40% higher than in simple shear flow, which suggests that the original Herschel–Bulkley model need modification with the yield stress being a function of the second invariant of the deviatoric stress tensor. The present effort is the first to study capillary self-thinning of Herschel–Bulkley liquids, which are exemplified here by suspensions of carbon nanotubes.

Journal ArticleDOI
TL;DR: In this article, the leveling, thixotropic, and screenprinting characteristics of concentrated zirconia inks were investigated by a variety of rheological and imaging methods.
Abstract: Screen-printing is a cost-effective method for the mass manufacture of zirconia-based solid oxide fuel cells (SOFCs) and oxygen separation membranes. The present work outlines an investigation into the leveling, thixotropic, and screen-printing characteristics of concentrated zirconia inks by a variety of rheological and imaging methods. A combination of viscosity, shear rate jump experiments, creep and recovery analysis, and yield stress measurements were used to assess ink thixotropy. Oscillatory rheometry and scanning electron microscopy/optical microscopy revealed a consistent effect of ethyl cellulose (binder) content upon the thixotropic and leveling characteristics of zirconia inks. While the yield stress (τ0), extent of recovery R(%), and rate of recovery (K) increase with increasing binder content, so did the surface roughness and thickness of the screen-printed films. Increasing the binder content not only increases the network strength of the thick films but also leads to increased leveling time. As a result, rheological modifiers are proposed to be necessary to improve the leveling characteristics of zirconia inks without losing the green strength of the thick films.

Journal ArticleDOI
TL;DR: In this paper, a ball measuring system was used to measure the rheology of large particles up to grain sizes of 10mm, and the results showed that the results were similar to the results obtained using a standard rheometer.
Abstract: For large-particulated fluids encountered in natural debris flow, building materials, and sewage treatment, only a few rheometers exist that allow the determination of yield stress and viscosity. In the present investigation, we focus on the rheometrical analysis of the ball measuring system as a suitable tool to measure the rheology of particulated fluids up to grain sizes of 10 mm. The ball measuring system consists of a sphere that is dragged through a sample volume of approximately 0.5 l. Implemented in a standard rheometer, torques exerted on the sphere and the corresponding rotational speeds are recorded within a wide measuring range. In the second part of this investigation, six rheometric devices to determine flow curve and yield stress of fluids containing large particles with maximum grain sizes of 1 to 25 mm are compared, considering both rheological data and application in practical use. The large-scale rheometer of Coussot and Piau, the building material learning viscometer of Wallevik and Gjorv, and the ball measuring system were used for the flow curve determination and a capillary rheometer, the inclined plane test, and the slump test were used for the yield stress determination. For different coarse and concentrated sediment–water mixtures, the flow curves and the yield stresses agree well, except for the capillary rheometer, which exhibits much larger yield stress values. Differences are also noted in the measuring range of the different devices, as well as for the required sample volume that is crucial for application.

Journal ArticleDOI
TL;DR: In this article, particle level simulations were used to investigate the effects of size bidispersity and particle size ratios on the static and yielding behaviour of magnetorheological fluids (MRF).
Abstract: Particle level simulations were used to investigate the effects of size bidispersity and particle size ratios on the static and yielding behaviour of magnetorheological fluids (MRF). The MRF were treated as linearly magnetisable, neutrally buoyant particles dispersed in a viscous carrier liquid. In the quiescent mode (static structures), the bidisperse suspensions were found to have a higher tendency to form straight chains than the monodisperse suspensions; this is consistent with previous findings. Under steady shearing, the bidisperse suspensions exhibited higher stress enhancement than the monodisperse systems. The stress enhancement in bidisperse suspensions is likely to be due to the population and orientation of interacting large particles in the bidisperse suspensions.

Journal ArticleDOI
TL;DR: In this article, the effect of pressure on viscosity of polymeric materials was investigated and the Simha-Somcynsky equation of state was applied to the pressure-volume-temperature experimental data of both materials to obtain the dependence of free volume on temperature and pressure.
Abstract: The effect of pressure on viscosity is an important but often overlooked aspect of the flow properties of polymeric materials. In this work, two polymers (an atactic and a syndiotactic Polystyrene) were characterized to determine the effect of pressure on viscosity. In particular, a device was adopted to increase the exit pressure of a standard capillary rheometer, thus obtaining data of viscosity under high pressure and high shear rates. The Simha-Somcynsky equation of state was applied to the pressure–volume–temperature experimental data of both materials to obtain the dependence of free volume on temperature and pressure. The Doolittle equation was eventually employed to verify the dependence of viscosity on free volume. It was found that, for both materials, a linear relationship holds between the logarithm of zero-shear-rate viscosity (at several temperatures and pressures) and the inverse of free volume.

Journal ArticleDOI
TL;DR: In this paper, Pivokonsky et al. used the molecular stress function model for broadly distributed, randomly branched molecular structures for quantitative modeling of melt rheology in both shear flow and elongational flow.
Abstract: Experimental data of two low-density polyethylene (LDPE) melts at 200°C for both shear flow (transient and steady shear viscosity as well as transient and steady first normal stress coefficient) and elongational flow (transient and steady-state elongational viscosity) as published by Pivokonsky et al. (J Non-Newtonian Fluid Mech 135:58–67, 2006) were analysed using the molecular stress function model for broadly distributed, randomly branched molecular structures. For quantitative modelling of melt rheology in both types of flow and in a very wide range of deformation rates, only three nonlinear viscoelastic material parameters are needed: Whilst the rotational parameter, a 2, and the structural parameter, β, are found to be equal for the two melts considered, the melts differ in the parameter $f_{\rm max}^2 $ describing maximum stretch of the polymer chains.

Journal ArticleDOI
TL;DR: In this paper, the authors investigate the sedimentation of concentrated suspensions at low Reynolds numbers to study collective particle effects on local particle velocity fluctuations and size segregation effects and report measurements of the interstitial fluid pressure during settling.
Abstract: We investigate the sedimentation of concentrated suspensions at low Reynolds numbers to study collective particle effects on local particle velocity fluctuations and size segregation effects. Experiments are carried out with polymethylmetacrylate (PMMA) spheres of two different mean diameters (190 and 25 μm) suspended in a hydrophobic index-matched fluid. Spatial repartitions of both small and large spheres and velocity fluctuations of particles are measured using fluorescently labelled PMMA spheres and a particle image velocimetry method. We also report measurements of the interstitial fluid pressure during settling. Experiments show that size segregation effects can occur during the sedimentation of concentrated suspensions of either quasi-monodisperse or bidisperse spheres. Size segregation is correlated to the organisation of the sedimentation velocity field into vortex-like structures of finite size. A loss of size segregation together with a significant decrease of the fluid pressure gradient in the bulk suspension is observed when the size of vortex-like structures gets on the order of the container size. However, the emergence of channels through the settling zone prevents a complete loss of size segregation in very concentrated suspensions.

Journal ArticleDOI
TL;DR: In this article, the authors studied the effect of polyhedral oligomeric silsesquioxane (POSS) particles on zero-shear rate viscosity of polymeric components and their blends.
Abstract: Polyhedral oligomeric silsesquioxane (POSS) are hybrid nanostructures of about 1.5 nm in size. These silicon (Si)-based polyhedral nanostructures are attached to a polystyrene (PS) backbone to produce a polymer nanocomposite (POSS–styrene). We have solution blended POSS–styrene of $\overline{M}_w =14.5\times 10^3\;\rm{g/mol}$ with commercial polystyrene (PS), $\overline{M}_w =2.8\times 10^5\;\rm{g/mol}$ , and studied the rheological behavior and thermal properties of the neat polymeric components and their blends. The concentration of POSS–styrene was varied from 3 up to 20 wt.%. Thermal analysis studies suggest phase miscibility between POSS–styrene and the PS matrix. The blends displayed linear viscoelastic regime and the time–temperature superposition principle applied to all blends. The flow activation energy of the blends decreased gradually with respect to the matrix as the POSS–styrene concentration increased. Strikingly, it was found that POSS–styrene promoted a monotonic decrease of zero-shear rate viscosity, η 0, as the concentration increased. Rheological data analyses showed that the POSS–styrene increased the fractional free volume and decreased the entanglement molecular weight in the blends. In contrast, blending the commercial PS with a PS of $\overline{M}_w =5\times 10^3\;\rm{g/mol}$ did not show the same lubrication effect as POSS–styrene. Therefore, it is suggested that POSS particles are responsible for the monotonic reduction of zero-shear rate viscosity in the blends.

Journal ArticleDOI
TL;DR: In this paper, the effect of crosslink density on shear and elongational flow properties of alkali-swellable acrylic thickener solutions using a mixing series of the two commercial thickeners Sterocoll FD (Sterocoll D) as model system was investigated.
Abstract: We have investigated the effect of crosslink density on shear and elongational flow properties of alkali-swellable acrylic thickener solutions using a mixing series of the two commercial thickeners Sterocoll FD and Sterocoll D as model system. Linear viscoelastic moduli show a smooth transition from weakly elastic to gel-like behavior. Steady shear data are very well described by a single mode Giesekus model at all mixing ratios. Extensional flow behavior has been characterized using the CaBER technique. Corresponding decay of filament diameter is also well fitted by the Giesekus model, except for the highest crosslink densities, when filament deformation is highly non-uniform, but the non-linearity parameter α, which is independent of the mixing ratio, is two orders of magnitude higher in shear compared to elongational flow. Shear relaxation times increase by orders of magnitude, but the characteristic elongational relaxation time decreases weakly, as gel content increases. Accordingly, variation of gel content is a valuable tool to adjust the low shear viscosity in a wide range while keeping extensional flow resistance essentially constant.

Journal ArticleDOI
TL;DR: In this article, the authors made measurements on concrete and mortars to characterize the shear-thickening behavior of certain concrete mix designs and found that the reduction of friction between polymer-coated materials appears to be a key phenomenon to delay onset shear thickening in industrial processes.
Abstract: Rheological measurements were made on concrete and mortars to characterize the shear thickening behavior of certain concrete mix designs. Shear thickening reduction levers were found by selecting and designing admixtures. Since the shear-thickening phenomena occur at the scale of the finest particles, industrial limestone fillers were studied that behave like cementitious materials. Theories based on previous academic works were relevant. The shear stress-dependent effects of shear thickening and size scaling were very helpful to distinguish between surface interactions, such as lubrication and volumetric contributions and also including the packing effects. The suspension viscosity curves vary accordingly to the Newtonian viscosity of the solvent medium. In both the shear thinning and shear thickening regimes, viscosity is controlled by adjusting the amount of two specific admixtures. The reduction of friction between polymer-coated materials appears to be a key phenomenon to delay onset shear thickening in industrial processes.

Journal ArticleDOI
TL;DR: In this paper, a magneto-slit die of 0.34 mm height and 4.25 mm width was attached to a commercial piston capillary rheometer, enabling the measurement of apparent flow curves of a magnetorheological fluid (MRF) in the high shear rate regime.
Abstract: We describe a magneto-slit die of 0.34 mm height and 4.25 mm width attached to a commercial piston capillary rheometer, enabling the measurement of apparent flow curves of a magnetorheological fluid (MRF) in the high shear rate regime (apparent shear rates 276 up to 20,700 s − 1, magnetic flux density up to 300 mT). The pressure gradient in the magnetized slit is measured via two pressure holes. While the flux density versus coil current without MRF could directly be measured by means of a Hall probe, the flux density with MRF was investigated by finite element simulations using Maxwell® 2D. The true shear stress versus shear rate is obtained by means of the Weissenberg–Rabinowitsch correction. The slit die results are compared to plate–plate measurements performed in a shear rate regime of 0.46 up to 210 s − 1. It is shown that the Casson model yields a pertinent fit of the true shear stress versus shear rate data from plate–plate geometry. Finally, a joint fit of the slit and plate–plate data covering a shear rate range of 1 up to 50,000 s − 1 is presented, again using the Casson model. The parameterization of the MRF behavior over the full shear rate regime investigated is of relevance for the design of MR devices, like, e.g., automotive dampers. In the Appendix, we demonstrate the drawbacks of the Bingham model in describing the same data. We also show the parameterization of the flow curves by applying the Herschel–Bulkley model.

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TL;DR: In this paper, the rheological behavior of high molecular mass polyamide 6 (PA6)/organo-montmorillonite nano-composites, obtained via melt blending, was investigated under shear and extensional flow.
Abstract: In this work, the rheological behaviour of high molecular mass polyamide 6 (PA6)/organo-montmorillonite nano-composites, obtained via melt blending, was investigated under shear and extensional flow. Capillary rheometry was used for the measurement of high shear rate steady state shear viscosity and die entrance pressure losses; further, by the application of a converging flow method (Cogswell model) to these experimental results, elongational viscosity data were indirectly calculated. The extensional behaviour was directly investigated by means of melt spinning experiments, and data of apparent elongational viscosity were determined. The results evidenced that the presence of the organo-clay in filled PA6 melts modifies the rheological behaviour of the material, with respect to the unfilled polymer, in dependence on the type of flow experienced by the fluid. In shear flow, the nano-composites showed a slightly lower viscosity than neat PA6, whereas in elongation, they appeared much more viscous, in dependence on the organo-clay content.

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TL;DR: In this article, the behavior of short glass fiber-polypropylene suspensions in extensional flow was investigated using three different commercial instruments: the SER wind-up drums geometry (Extensional Rheology System) with a strain-controlled rotational rheometer, a Meissner-type Rheometer (RME), and the Rheotens.
Abstract: The behavior of short glass fiber–polypropylene suspensions in extensional flow was investigated using three different commercial instruments: the SER wind-up drums geometry (Extensional Rheology System) with a strain-controlled rotational rheometer, a Meissner-type rheometer (RME), and the Rheotens. Results from uniaxial tensile testing have been compared with data previously obtained using a planar slit die with a hyperbolic entrance. The effect of three initial fiber orientations was investigated: planar random, fully aligned in the stretching flow direction and perpendicular to it. The elongational viscosity increased with fiber content and was larger for fibers initially oriented in the stretching direction. The behavior at low elongational rates showed differences among the various experimental setups, which are partly explained by preshearing history and nonhomogenous strain rates. However, at moderate and high rates, the results are comparable, and the behavior is strain thinning. Finally, a new constitutive equation for fibers suspended into a fluid obeying the Carreau model is used to predict the elongational viscosity, and the predictions are in good agreement with the experimental data.