On the influence of the hydrodynamic interactions on the aggregation rate of magnetic spheres in a dilute suspension

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Abstract

Magnetostatic attraction may lead to formation of aggregates in stable colloidal magnetic suspensions and magneto-rheological suspensions. The aggregation problem of magnetic composites under differential sedimentation is a key problem in the control of the instability of non-Brownian suspensions. Against these attractive forces are the electrostatic repulsion and the hydrodynamic interactions acting as stabilizing effects to the suspension. This work concerns an investigation of the pairwise interaction of magnetic particles in a dilute sedimenting suspension. We focus attention on suspensions where the Péclet number is large (negligible Brownian motion) and where the Reynolds number (negligible inertia) is small. The suspension is composed of magnetic micro-spheres of different radius and density immersed in a Newtonian fluid moving under the action of gravity. The theoretical calculations are based on direct computations of the hydrodynamic and the magnetic interactions among the rigid spheres in the regime of low particle Reynolds number. From the limiting trajectory in which aggregation occurs, we calculate the collision efficiency, representing the dimensionless rate at which aggregates are formed. The numerical results show clear evidence that the hydrodynamic interactions are of fundamental relevance in the process of magnetic particle aggregation. We compare the stabilizing effects between electrostatic repulsion and hydrodynamic interactions.

Introduction

Technological control of the stability against aggregate formation in colloidal magnetic suspensions and rheological magnetic suspensions (MRS) is important in a number of industrial processes. Aggregation may be induced to increase the settling rate, modifying the rheological properties of suspensions. In the treatment of waste water, suspended material must be separated so that the water can be recycled or so that the pollution of streams and rivers is reduced [1]. The phenomena examined for a gravitationally driven motion of magnetic particles made of homogeneous suspensions, a complex shape evolution, including aggregates formation, are fundamental to the mechanics of multiphase flows, and have direct and indirect applications in many chemical process such as instability of MRS. For colloidal suspensions, particles must first be brought close together by Brownian motion. They then experience an attractive force which may be sufficiently strong to overcome any repulsive forces and the fluid—mechanical lubrication to relative motion. At a critical size, however, their sedimentation speed becomes significant and thereafter the aggregates grow by the larger and faster aggregates sweeping up the smaller ones. So, even in an unstable colloidal magnetic suspension, after a critical size of the micro-aggregates, differential sedimentation becomes the key mechanism to the particle aggregate rather than Brownian motion. Fig. 1 shows clearly the aggregates formation in a suspension of micro-spherical magnetic composites of about 100μm. Owing to particle polydispersity differential sedimentation might bring (in the absence of Brownian motion) particles close together and attractive magnetic force between the particles lead to particle aggregate. The near field hydrodynamic interactions (lubrication regime between the composites) on the other hand appear to decrease the flocculation efficiency. This new effect is explored in this paper. The motivation is to understand how can a MRS become unstable. Aggregates form and they precipitate as shown in the experiments carried out in this work about sedimentation of magnetic composites, see Fig. 1, in which we can see typical aggregates that form in a dilute suspension of magnetic non-Brownian particles, initially statistically homogeneous.

The central issue in these systems is to understand and to predict the macroscopic behavior of such suspension from their microstructure. When particle aggregation occurs in a dilute suspension, the quantity of interest is the rate of doublet formation. The pioneer studies to estimate the rate of aggregation [2] considered that the particles are submitted only to a sticking force on contact, i.e. without any hydrodynamic interaction (HI) or interparticle forces. After this, the effects of hydrodynamic interaction and interparticle force were included [3] to compute the rate of aggregation of a dispersion of equal spheres subject to simple shear and to uniaxial extensional flow. For gravity-induced aggregation of rigid spheres, Davis [4] developed a theoretical model to investigate the influence of van der Waals and Maxwell slip on the collision efficiency for rapid aggregation regimes. Moreover, the collision rates of spherical and deformable drops in a shear flow were calculated [5], [6], [7]. While the subject of particle aggregation is generally well known, it must be appreciated that the present study is the first one based on a hydrodynamically interacting magnetic suspensions of non-Brownian particles. Several works have examined by numerical simulations the aggregation process of magnetic spheres in suspensions studying the formation of clusters and chain-like structures in the suspension [8], [9], [10]. Surprisingly, they have neglected the influence of the hydrodynamic interactions in their simulations considering free-energy models and Monte Carlo simulations only. In a study related to the present one [11], [12] included the effects of hydrodynamic interaction and interparticle force, and computed the relative trajectories and the hydrodynamic diffusivities for two spherical particles interacting in a simple shearing flow and in sedimentation, respectively.

The interest here is to examine the influence of the hydrodynamic interaction on the dynamics of aggregate formation in a dilute magnetic suspension of non-Brownian micro-particles. From the computation of the relative trajectories of pairwise interactions between magnetic spherical composites at low particle Reynolds number we investigate the influence of particle magnetization on the rate of particle aggregation for different conditions of the physical parameter which considers the relative importance between interparticle and gravity forces. We calculate theoretically the rate at which aggregates are formed (collision efficiency) in a dilute suspension of magnetic composites.

Section snippets

Formulation of the problem

Consider a dilute suspension composed of two species of rigid smooth magnetic spheres of radius a1 and a2, densities ρ1 and ρ2 and magnetizations M1=M1d^1 and M2=M2d^2 suspended in a Newtonian fluid of density ρ and viscosity μ. Here, the inertial effects are neglected, as we have small particle Reynolds numbers, so that the creeping flow equations can be applied in the scale of the particle motion. The suspension is submitted to a settling motion so that the uniform gravitational force per

Trajectory equations

Making the balance between the hydrodynamic force and the applied force Fi, one obtains the governing equation for the relative motion, i.e. the vector s time evolution, given by the differential equation ds/dt=U12U2U1. By substituting the expression for Fi (11) into (3) the mobility relations in Section 2.1, one obtains an expression for the relative velocity U12 in terms of dimensionless quantities, namelyU12=e2·Mg(QMφMd+QEφEd)·Mi,withMg=sss2L(s)+Isss2M(s)andMi=sss2G(s)+Isss2H(s),where

Numerical results

In order to perform the integration of the system of differential equations that govern the relative motion of the particles, Eq. (14), a fourth-order Runge–Kutta scheme is used, i.e. a predictor–corrector method with four steps of evaluations of the velocity function U12 at each time-step. The asymptotic forms of the mobility functions for widely separated spheres (7), (8), (9), (10) were used for s>2.3. Otherwise, the near field mobilities given by (5), (6) are considered. Furthermore, in

Acknowledgements

The authors are grateful to the Brazilian research funding agencies CNPq and CAPES for their generous support of this work. We thank Prof. Yuri Dumaresq Sobral (MAT-UnB) for helpful comments on this work.

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