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Register a new userPopulation-balance description of shear-induced clustering, gelation and suspension viscosity in sheared DLVO colloids
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Application of shear flow to charge-stabilized aqueous colloidal suspensions is ubiquitous in industrial applications and as a means to achieve controlled field-induced assembly of nanoparticles. Yet, applying shear flow to a charge-stabilized colloidal suspension, which is initially monodisperse and in quasi-equilibrium leads to non-trivial clustering phenomena (and sometimes to a gelation transition), dominated by the complex interplay between DLVO interactions and shear flow. The quantitative understanding of these strongly nonequilibrium phenomena is still far from being complete. By taking advantage of a recent shear-induced aggregation rate theory developed in our group, we present here a systematic numerical study, based on the governing master kinetic equation (population-balance) for the shear-induced clustering and breakup of colloids exposed to shear flow. In the presence of sufficiently stable particles, the clustering kinetics is characterized by an initial very slow growth, controlled by repulsion. During this regime, particles are slowly aggregating to form clusters, the reactivity of which increases along with their size growth. When their size reaches a critical threshold, a very rapid, explosive-like growth follows, where shear forces are able to overcome the energy barrier between particles. This stage terminates when a dynamic balance between shear-induced aggregation and cluster breakage is reached. It is also observed that these systems are characterized by a cluster mass distribution that for a long time presents a well-defined bimodality. The model predictions are quantitatively in excellent agreement with available experimental data, showing how the theoretical picture is able to quantitatively account for the underlying nonequilibrum physics.
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Colloidal suspensions that are out of thermodynamic equilibrium undergo physical aging wherein their structure evolves to lower the free energy. In aqueous suspension of Laponite, physical aging accompanies increases of elastic and viscous moduli as a function of time. In this work we study temporal evolution of elastic and viscous moduli at different frequencies and observe that freshly prepared aqueous suspension of Laponite demonstrates identical rheological behavior reported for the crosslinking polymeric materials undergoing chemical gelation. Consequently at a certain time tan{delta} is observed to be independent of frequency. However, for samples preserved under rest condition for longer duration before applying the shear melting, the liquid to solid transition subsequent to shear melting shows greater deviation from classical gelation. We also obtain continuous relaxation time spectra from the frequency dependence of viscous modulus. We observe that, with increase in the rest time, continuous relaxation time spectrum shows gradual variation from negative slope, describing dominance of fast relaxation modes to positive slope representing dominance of slow relaxation modes. We propose that the deviation from gelation behavior for the shear melted suspensions originates from inability of shear melting to completely break the percolated structure thereby creating unbroken aggregates. The volume fraction of such unbroken aggregates increases with the rest time. For small rest times presence of fewer number of unbroken aggregates cause deviation from the classical gelation. On the other hand, at high rest times presence of greater fraction of unbroken aggregates subsequent to shear melting demonstrate dynamic arrest leading to inversion of relaxation time spectra.
Transport properties of dense fluids are fundamentally challenging, because the powerful approaches of equilibrium statistical physics cannot be applied. Polar fluids compound this problem, because the long-range interactions preclude the use of a simple effect-diameter approach based solely on hard spheres. Here, we develop a kinetic theory for dipolar hard-sphere fluids that is valid up to high density. We derive a mathematical approximation for the radial distribution function at contact directly from the equation of state, and use it to obtain the shear viscosity. We also perform molecular-dynamics simulations of this system and extract the shear viscosity numerically. The theoretical results compare favorably to the simulations.
We study a novel phase of active polar fluids, which is characterized by the continuous creation and destruction of dense clusters due to self-sustained turbulence. This state arises due to the interplay of the self-advection of the aligned swimmers and their defect topology. The typical cluster size is determined by the characteristic vortex size. Our results are obtained by investigating a continuum model of compressible polar active fluids, which incorporates typical experimental observations in bacterial suspensions by assuming a non-monotone dependence of speed on density.
The velocity fluctuations present in macroscopically homogeneous suspensions of neutrally buoyant, non-Brownian spheres undergoing simple shear flow, and their dependence on the microstructure developed by the suspensions, are investigated in the limit of vanishingly small Reynolds numbers using Stokesian dynamics simulations. We show that, in the dilute limit, the standard deviation of the velocity fluctuations is proportional to the volume fraction, in both the transverse and the flow directions, and that a theoretical prediction, which considers only for the hydrodynamic interactions between isolated pairs of spheres, is in good agreement with the numerical results at low concentrations. We also simulate the velocity fluctuations that would result from a random hard-sphere distribution of spheres in simple shear flow, and thereby investigate the effects of the microstructure on the velocity fluctuations. Analogous results are discussed for the fluctuations in the angular velocity of the suspended spheres. In addition, we present the probability density functions for all the linear and angular velocity components, and for three different concentrations, showing a transition from a Gaussian to an Exponential and finally to a Stretched Exponential functional form as the volume fraction is decreased. We also show that, although the pair distribution function recovers its fore-aft symmetry in dilute suspensions, it remains anisotropic and that this anisotropy can be accurately described by assuming the complete absence of any permanent doublets of spheres. We finally present a simple correction to the analysis of laser-Doppler velocimetry measurements.
The permeability anisotropy that results from a shear displacement u between the complementary self-affine walls of a rough fracture is investigated. Experiments in which a dyed fluid displaces a transparent one as it is radially injected into a transparent fracture exhibit a clear anisotropy in the presence of shear displacements, and allow us to estimate the ratio of the permeabilities for flows parallel and perpendicular to u. A simple model which accounts for the development of channels perpendicular to u qualitatively explains these results, and predicts a permeability decreasing (increasing) linearly with the variance of the aperture field for flow parallel (perpendicular) to the shear displacement. These predictions are then compared to the results of numerical simulations performed using a lattice-Boltzmann technique and to the anisotropies measured in displacement experiments.
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