Elongational and shear rheology of carbon nanotube suspensions

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.     

Scaling behavior of the elastic properties of non-dilute MWCNT�Cepoxy suspensions

In this paper, the network structure of multiwalled carbon nanotube (MWCNT)?Cepoxy suspensions was investigated under the influence of flow history and temperature using the scaling behavior of the linear viscoelastic properties of the concentrated suspensions above their gel point. It is shown that the suspensions have a self-similar fractal structure with the dimension of about 2.15, characteristic of weakly flocculating suspensions and their elasticity originates from inter- and intra-floc links of nanotubes. From the scaling behavior of the flow-induced storage modulus and the critical strain for the limit of linearity, it is shown that the fractal dimension and so the superstructure of the network did not change significantly under the influence of the flow history due to the initial compact structure of the network before pre-shearing. The time?Ctemperature superposition principle was verified for the CNT suspensions and the shift factor was accounted for by an Arrhenius equation. The reduced storage and loss moduli of the suspensions using the complex modulus of the neat epoxy were shown to increase with temperature revealing more inter-particle interactions as the temperature was raised. However, it was impossible to conclude on the changes of the fractal dimensions with temperature.     

In situ flow visualization of capillary flow of concentrated alumina suspensions

A new approach was taken to understand the flow behavior of concentrated particle suspensions in pressure-driven capillary flow. The flow of concentrated alumina suspensions in a slit channel was visualized and quantitatively analyzed with modified capillary rheometer. The suspensions showed complex flow behaviors; unique solid–liquid transition and shear banding. At low flow rates, 55 vol% alumina suspension showed a unique transient flow behavior; there was no flow at first and continuous change of flow profile was observed with time. At low shear rates in particular, the suspensions exhibited shear-banded flow profile which could be divided into three regions: the region with low flow rate near the wall, the region with rapid increase of flow velocity to maximum, and the region of velocity plateau. Based on both flow visualization and measurement of shear stress, it was found that the shear-banded flow profile in pressure-driven slit channel flow was strongly correlated with shear stress. The banding in pressure-driven flow was different from that in Couette flow. The banding of concentrated alumina suspensions was unique in that sluggish velocity profile was pronounced and two inflection points in velocity profile was exhibited. In this study, shear banding of concentrated alumina suspensions in slit channel flow was visualized and quantitatively analyzed. We expect that this approach can be an effective method to understand the flow behavior of particulate suspensions in the pressure-driven flow which is typical in industrial processing.     

Sliding plate rheometry of planar oriented concentrated fiber suspension

The rheology of concentrated planar fiber suspensions is investigated. A new experimental technique for fiber suspensions based on a sliding plate rheometer incorporating a shear stress transducer is developed. It is shown that this instrument works well for the tested material systems. The rheological behavior in steady shear is subsequently investigated. The results can be largely explained by a combination of frictional and hydrodynamic interaction. Despite this evidence of friction no yield stress could be detected for the investigated shear rates. It was also found that the fiber aspect ratio did not influence the steady shear viscosity.     

A self-similar behavior for the relative viscosity of concentrated suspensions of rigid spheroids

A viscosity model for suspensions of rigid particles with predictive capability over a wide range of particle volume fraction and shear conditions is of interest to quantify the transport of suspensions in fluid flow models. We study the shear viscosity of suspensions and focus on the effect of particle aspect ratio and shear conditions on the rheological behavior of suspensions of rigid bi-axially symmetric ellipsoids (spheroids). We propose a framework that forms the basis to microscopically parameterize the evolution of the suspension microstructures and its effect on the shear viscosity of suspensions. We find that two state variables, the intrinsic viscosity in concentrated limit and the self-crowding factor, control the state of dispersion of the suspension. A combination of these two variables is shown to be invariant with the imposed shear stress (or shear rate) and depends only on the particle aspect ratio. This self-similar behavior, tested against available experimental and numerical data, allows us to derive a predictive model for the relative viscosity of concentrated suspensions of spheroids subjected to low (near zero) strain rates. At higher imposed strain rates, one needs to constrain one of the state variables independently to constrain the state of dispersion of the suspension and its shear dynamic viscosity. Alternatively, the obtained self-similar behavior provides the means to estimate the state variables from the viscosity measurements made in the laboratory, and to relate them to microstructure rearrangements and evolution occurring during deformation.     

Direct simulation for concentrated fibre suspensions in transient and steady state shear flows

A numerical method to simulate fibre suspensions in transient and steady state shear flows for concentrated solutions is reported, which takes into account short-range hydrodynamic interaction via lubrication forces, contact forces and hydrodynamic forces. Fibres are assumed to have varying lengths as observed in industrial composites and this can be described with a fibre distribution length function. Stresses in the composite have been calculated from a constitutive equation or from an approximate expression for the effective stress of fibre suspensions. This simulation will assist in modelling of short fibre filled industrial composites. Our first results shown here qualitatively agree with experiments.     

Harmonic analysis in rheological property measurement

 Sudden change in the linear stress-strain relationship has long been known to produce interesting discontinuities in the flow properties of polymer melts, concentrated particle suspensions, and gels as the shear rate amplitude is increased. The non-linear effect produces stress harmonics, which contain information about the material properties that is otherwise difficult to obtain. This note describes a generalized procedure for extracting yield stress material functions from the discrete Fourier transform of the stress signal. Received: 23 April 2001 Accepted: 27 July 2001     

Bulk stress of a periodic suspension of solid particles of arbitrary shape

An analytical study is made of the bulk stress of a periodic array of solid identical and force-free particles of arbitrary shape in an incompressible Newtonian fluid. Asymptotic expressions are derived for the bulk stress of dilute periodic suspensions. Asymptotic expressions are also derived for a concentrated suspension of almost-touching ellipsoids at an instant when the suspension has orthotropic symmetry.     

Size segregation and particle velocity fluctuations in settling concentrated suspensions

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.     

Rheological properties of concentrated latex suspensions of poly(styrene-butadiene)

Concentrated suspensions of charged latex particles of poly(styrene-butadiene) have been used as model systems to investigate the influence of surface charges on the rheology of colloidal suspensions. The suspensions were found to behave as elastic solids at small strains and to require a finite stress to flow. This was related to an ordered structure of the suspensions at rest, resulting from electrostatic and van der Waals forces. Important shear-thinning effects were observed as a consequence of structure rearrangements under shear. At a fixed shear rate, the steady-shear viscosity as a function of the ionic strength exhibits a minimum. Under oscillatory shear flow, the behavior of the concentrated suspensions was found to be non-linear above a very small strain amplitude. The non-linear output signal from dynamic experiments was analyzed using a fast Fourier transform algorithm. A maximum in the third harmonic intensity as a function of the strain amplitude was observed and the intensity of higher harmonics decreased with increasing ionic strength. The behavior of the suspensions could be adequately described using the structural model of Yziquel et al. (Yziquel F, Carreau PJ, Moan M, Tanguy PA (1999) Rheological modeling of concentrated colloidal suspensions. J Non-Newtonian Fluid Mech 86:133–155).     

Yield stress and maximum packing fraction of concentrated suspensions

The yield stress and features of the structure of concentrated suspensions based on silica flour, with particles of average diameter around 4 m, were investigated in terms of a phenomenological model. The yield stress of a concentrated suspension of known solid volume concentration is estimated by employing a shear-dependent maximum packing fraction _m which is obtained by model fitting equilibrium viscosity data, and by incorporating a first-order kinetic equation. The model proposed was examined by using several mineral suspensions in which silica flour was mixed with metal oxide particles so that microstructural features of the suspensions could be adjusted. A cocoa fat suspension was also used as a test sample having radically different chemistry. The agreement between the model prediction and independently obtained experimental evidence is acceptable. Furthermore, a qualitative explanation is obtained by a scaling analysis in an effort to relate the model parameters with the suspension structure that stems from interactions among the suspension constituents.     

Peculiar features in the rheological behavior of electrorheological suspensions

Studies have been made of concentrated (up to 60%) diatomite suspensions in transformer oil, the structure and theological properties of which depend on an applied electric field. Studies have been conducted of steady-state and transient regimes of straining involving continuous and periodic shear. The structure in such suspensions is formed in the presence of an electric field of 10^–3 –10² duration. The suspensions under continuous stationary strain behave as non-Newtonian fluids with a yield stress dependent on electric intensity. Under periodic deformation conditions the test suspensions exhibit elasticity which abruptly diminishes with increasing deformation amplitude.     

The flow of fiber suspensions in complex geometries

A continuum theory for dilute suspensions of large-aspect-ratio particles is applied to the flow of fiber suspensions through contractions. The theory, which incorporates the statistical orientation distribution function into the stress equation, predicts that the flow of dilute suspensions will differ qualitatively from the flow of the suspending fluid. The theory is in excellent agreement with experiments on the flow of suspensions of chopped-glass fibers through axisymmetric contractions, where substantial enlargement of the recirculating corner vortex is observed at volume fractions of 0.1% and less.     

Rheology of concentrated suspensions containing mixtures of spheres and fibres

Optimising flow properties of concentrated suspensions is an important issue common for many industries. The rheology of concentrated suspensions has therefore been studied intensively both experimentally and theoretically. Most studies have focused on monodisperse and polydisperse suspensions of either spheres or fibres. In practice, most suspensions contain particles that are polydisperse both in size and shape. A mixing rule for such systems is expected to be a powerful tool for engineers and product designers. Therefore in this work, suspensions of spheres, fibres and mixtures thereof were characterised using rotational shear rheometry and in-line image analyses. Thereby, total solids volume concentration and fibre fraction was varied. Results from transient and steady-state shear rheometry are discussed with respect to concentration, fibre fraction, and shear induced microstructure. Experimentally obtained viscosity data were accurately fitted using the model proposed by Farris (T Soc Rheol 12:281, 1968) for mixtures of monodisperse non-interacting spheres of different sizes.Originally presented at the Annual European Rheology Conference 2003, AERC 2003     

Thixotropy, yielding and ultrasonic Doppler velocimetry in pulp fibre suspensions

This paper reports thixotropy in concentrated pulp fibre suspensions and studies their transient flow behaviour using conventional rheometry coupled with a velocimetry technique. Specifically, an ultrasonic Doppler velocimeter is used in conjunction with a rate-controlled rheometer to deduce the local velocity profiles of pulp fibre suspensions. Pulp suspensions are found to exhibit a plateau in their flow curves where a slight increase in the shear stress generates a jump in the corresponding shear rate, implying the occurrence of shear banding. The velocity profiles were found to be discontinuous in the vicinity of the yielding radius where the Herschel–Bulkley model failed to predict the flow. Shear history and the time of rest prior to the measurement were found to play a significant role on the rheology and the local velocity profiles of pulp suspensions.     

A review of microstructure in concentrated suspensions and its implications for rheology and bulk flow

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.     

Transient phenomena in thixotropic systems

A nonlinear rheological model which accounts for the time-dependent elastic, viscous and yielding phenomena is developed in order to describe the flow behavior of thixotropic materials which exhibit yield stress. A key feature of the formulation is a smooth transition from an ‘elastically’ dominated response to a ‘viscous’ response without a discontinuity in the stress–strain curve. The model is phenomenological and is based on the kinetic processes responsible for structural changes within the thixotropic material. As such, it can predict thixotropic effects, such as stress overshoot during start-up of a steady shear flow and stress relaxation after cessation of flow. Thus this model extends a previously proposed viscoplastic model [J. Rheol. 34 (1991) 647] to include thixotropy.An analysis and comparison to experimental data involving oscillatory shear flow are provided to evaluate the accuracy of the model and to estimate the model parameters in a prototype concentrated suspension. The experiments were conducted using a series of concentrated suspensions of silicon particles and silicon carbide whiskers in polyethylene. The data obtained with this experimental system indicated much better agreement between the theory and experiments that obtained in earlier work.     

Forced convective flow drag and heat transfer characteristics of carbon nanotube suspensions in a horizontal small tube

This study paid attention to the effect of fluid temperatures on the forced convective flow drag and heat transfer characteristics of multi-wall carbon nanotube (MWNTs)-water suspensions without any surfactants. The experiments were carried out under the two fixed average fluid temperatures of 29 and 58°C. A horizontal small stainless steel tube with an inner diameter of 1.02 mm was used as the test section. The experiment results show that the flow drag characteristics of suspensions are almost the same as those of water. While the heat transfer of MWNTs suspensions with high mass concentration or high fluid temperature is significantly enhanced. The fluid temperature does not affect flow drag characteristics but has great effect on the heat transfer characteristics. Nanometer characteristics are presented by suspensions with high MWNT mass concentration or high temperature on convective heat transfer.     

Refractive-index and density matching in concentrated particle suspensions: a review

Optical measurement techniques such as particle image velocimetry (PIV) and laser Doppler velocimetry (LDV) are now routinely used in experimental fluid mechanics to investigate pure fluids or dilute suspensions. For highly concentrated particle suspensions, material turbidity has long been a substantial impediment to these techniques, which explains why they have been scarcely used so far. A renewed interest has emerged with the development of specific methods combining the use of iso-index suspensions and imaging techniques. This review paper gives a broad overview of recent advances in visualization techniques suited to concentrated particle suspensions. In particular, we show how classic methods such as PIV, LDV, particle tracking velocimetry, and laser induced fluorescence can be adapted to deal with concentrated particle suspensions.     

Collective Behaviour of Swimming Micro-organisms

The occurrence and mechanism of bioconvection patterns in suspensions of upswimming micro-organisms are described, and the linear stability theory for bioconvection in an otherwise uniform dilute suspension is outlined for the case of algae which swim upwards because they are bottom-heavy. Particular attention is paid to the effect of the stress generated in the suspension by the force-dipole exerted by each swimming cell. Coherent structures are also observed in concentrated suspensions, of bacteria in particular, and it is postulated that these come about solely through the hydrodynamic interactions between cells. We examine the deterministic swimming of model organisms which interact hydrodynamically but do not exhibit intrinsic randomness except in their initial positions and orientations. A micro-organism is modelled as a squirming, inertia-free sphere with prescribed tangential surface velocity. Pairwise interactions have been computed using the boundary element method, and the results stored in a database. The movement of a number of identical squirmers is computed by the Stokesian Dynamics method, with the help of the database of interactions. It is found that the spreading in three dimensions is correctly described as a diffusive process after a sufficiently long time. Scaling arguments are used to estimate this time-scale and the diffusitivities. These depend strongly on volume fraction and mode of squirming. However, in two dimensions the squirmers show a definite tendency to aggregation.