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. 2023 Nov 14;39(45):16006-16022.
doi: 10.1021/acs.langmuir.3c02102. Epub 2023 Nov 6.

Sedimentation of a Charged Spherical Particle in a Viscoelastic Electrolyte Solution

Affiliations

Sedimentation of a Charged Spherical Particle in a Viscoelastic Electrolyte Solution

Eleni Kouni et al. Langmuir. .

Abstract

When a charged particle translates through an electrolyte solution, the electric double layer around it deforms in response to the fluid motion and creates an electric force opposite the direction of motion, decreasing the settling velocity. This is a multidisciplinary phenomenon that combines fluid mechanics and electrodynamics, differentiating it from the classical problem of an uncharged sedimenting particle. It has many applications varying from mechanical to biomedical, such as in drug delivery in blood through charged microparticles. Related studies so far have focused on Newtonian fluids, but recent studies have proven that many biofluids, such as human blood plasma, have elastic properties. To this end, we perform a computational study of the steady sedimentation of a spherical, charged particle in human blood plasma due to the centrifugal force. We used the Giesekus model to describe the rheological behavior of human blood plasma. Assuming axial symmetry, the governing equations include the momentum and mass balances, Poisson's equation for the electric field, and the species conservation. The finite size of the ions is considered through the local-density approximation approach of Carnahan-Starling. We perform a detailed parametric analysis, varying parameters such as the ζ potential, the size of the ions, and the centrifugal force exerted upon the particle. We observe that as the ζ potential increases, the settling velocity decreases due to a stronger electric force that slows the particle. We also conduct a parametric analysis of the relaxation time of the material to investigate what happens generally in viscoelastic electrolyte solutions and not only in human blood plasma. We conclude that elasticity plays a crucial role and should not be excluded from the study. Finally, we examine under which conditions the assumption of point-like ions gives different predictions from the Carnahan-Starling approach.

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Conflict of interest statement

The authors declare no competing financial interest.

Figures

Figure 1
Figure 1
Schematic of the spherical particle sedimenting through a viscoelastic fluid under the effect of body force, formula image, which in this study is a centrifugal force. Here, Ω represents the area that the viscoelastic material occupies. As and Souter denote the axis of symmetry and the far-field boundary, respectively.
Figure 2
Figure 2
Effect of the g-factor, formula image, on (a) the particle velocity and (b) the electric force for different values of ζ and ΦB = 0. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 3
Figure 3
Contours of Tzz for (a) formula image, (Wi = 0.58) and (b) formula image, (Wi = 23.232), when ζ = 3 and ΦB = 0. Τhe extent of the EDL is indicated by the white dashed lines. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 4
Figure 4
Distortion of the dimensionless counterion concentration profiles for different Weissenberg numbers: (a) formula image, (Wi = 2.56), (b) formula image, (Wi = 9.16), and (c) formula image, (Wi = 23.232) when ζ = 3 and ΦB = 0. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 5
Figure 5
Electric potential and the corresponding electric field lines around the particle for different Weissenberg numbers: (a) formula image, (Wi = 2.56), (b) formula image, (Wi = 9.16), and (c) formula image, (Wi = 23.232), when ζ = 3 and ΦB = 0. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 6
Figure 6
Effect of the Weissenberg number on the particle velocity for formula image for different values of ζ and ΦB = 0. The particle is sedimenting in a viscoelastic material that follows the Giesekus model using the parameters of Table 2. Only the relaxation time varies here.
Figure 7
Figure 7
Effect of the Zeta potential on the particle velocity for (a) formula image, (Wi = 0.528) and (b) formula image, (Wi = 5.28). The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 8
Figure 8
Effect of the zeta potential on the (a) electric force, (b) viscoelastic drag, and (c) form drag for formula image, (Wi = 5.28). The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 9
Figure 9
Steric effect on ionic concentration for formula image, (Wi = 5.28) when ζ = 3, (a) cations and (b) anions. The left-hand side of each panel corresponds to ΦB = 0.2, and the right-hand side corresponds to ΦB = 0. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 10
Figure 10
Contours of Trr for formula image, (Wi = 0.528) and for two different values of zeta potentials: (a) ζ = 2 and (b) ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 11
Figure 11
Contours of Trz for formula image, Wi = 0.528 and for two different values of zeta potential: (a) ζ = 2 and (b) ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 12
Figure 12
Contours of the trace of the conformation tensor for formula image, Wi = 0.528 and for two different values of zeta potential: (a) ζ = 2 and (b) ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 13
Figure 13
Effect of the ratio of the diameter to the Debye length at ζ = 4 for (a) formula image, (Wi = 0.528) and (b) formula image, (Wi = 5.28). The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 14
Figure 14
Effect of the ratio of the particle diameter to the Debye length on (a) the form drag (left) and on (b) the viscoelastic drag (right) for formula image, Wi = 0.528 with ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 15
Figure 15
Contours of the pressure field for (a) K = 0.09, (b) K = 2, and (c) K = 4. The values of the other dimensionless numbers correspond to formula image, (Wi = 0.528) with ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 16
Figure 16
Contours of Trz for (a) K = 0.5 and (b) K = 1. The values of the other dimensionless numbers correspond to formula image (Wi = 0.528) and ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure 17
Figure 17
Contours of Trz for (a) ΦB = 0 and (b) ΦB = 0.2. The values of the other dimensionless numbers correspond to K = 1 for formula image, (Wi = 0.528) with ζ = 4. The particle is sedimenting in blood plasma which follows the Giesekus model using the parameters of Table 2.
Figure A1
Figure A1
(a) Effect of the Reynolds number on the particle velocity for K = 2 and different values of zeta potential. The range of formula image and the other dimensionless numbers is summarized in Table A1. (b) Mesh convergence for the Newtonian material for ζ = 4 and for three different meshes (Table A2) and (c) mesh convergence validation for the viscoelastic material for ζ = 3 and for three different meshes (Table A2).

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