China Particuology 5 (2007) 50–60

Ferrofluid magnetoviscous control of wall flow

channeling in porous media
Faı̈çal Larachi ∗ , Damien Desvigne
Department of Chemical Engineering, Laval University, Que. G1K 7P4, Canada
Received 18 April 2006; accepted 5 December 2006

Abstract
We analyzed the phenomenon of ferrofluid magnetoviscosity in high-permeability wall-region non-magnetic porous media of the Müller kind.
After upscaling the pore-level ferrohydrodynamic model, we obtained a simplified volume-average zero-order axisymmetric model for non-Darcy
non-turbulent flow of steady-state isothermal incompressible Newtonian ferrofluids through a porous medium experiencing external constant
bulk-flow oriented gradient magnetic field, ferrofluid self-consistent demagnetizing field and induced magnetic field in the solid. The model was
explored in contexts plagued by wall flow maldistribution due to low column-to-particle diameter ratios. It was shown that for proper magnetic field
arrangement, wall channeling can be reduced by inflating wall flow resistance through magnetovisco-thickening and Kelvin body force density
which reroute a fraction of wall flow towards bed core.
© 2007 Chinese Society of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V.
All rights reserved.

Keywords: Ferrofluid; Magnetosviscosity; Porous medium; Volume-average ferrohydrodynamic model; Kelvin body force; Spin-vorticity coupling

1. Introduction
Ferrofluids are non-naturally occurring magnetic liquid sus-
pensions obtained by seeding surfactant-wrapped single-domain
superparamagnetic nanoparticles in appropriate organic or aque-
ous carrier matrices (Odenbach, 2003; Rinaldi & Zahn, 2002;
Rosensweig, 1997). Such stabilized ferrocolloidal suspensions
exhibit a number of intriguing behaviors when subjected to
external – uniform, spatially inhomogeneous or oscillating –
magnetic fields. Owing to a giant single-domain magnetic
moment, ca. 104 Bohr magnetons, each nanoparticle stands as a
small permanent magnetic dipole. Collective response of these
nanoparticles to magnetic field stimulation gives rise to strong
and coherent magnetization which, for motionless ferrofluids,
aligns along the direction of the total magnetic field, and which
obeys the equilibrium Langevin magnetic-field-locked magne-
tization law. In this study, we will make the assumptions that
the Brownian relaxation outweighs the Néelian relaxation (i.e.,
magnetic moment spatially locked to nanoparticle) and that the
magnetic dipole interaction energy is unable to oppose neither
∗ Corresponding author. Tel.: +1 418 656 3566; fax: +1 418 656 5993.
E-mail address: faical.larachi@gch.ulaval.ca (F. Larachi).
the deconstructing thermal agitation nor shear flow, thus main-
taining the nanoparticles afloat and unassociated. In addition,
should the ferrofluid motionless state be restored, the non-
zero magnetization relaxation time will impede instantaneous
directional readjustment of magnetization vector towards equi-
librium.
When ferrofluids are brought to motion in shear flows,
misalignment between “dynamic” magnetization M and total
magnetic field H vectors arises due to an asynchrony between
the nanoparticle spin ␻ and the ferrofluid vorticity, ½ × v
(Rosensweig, 1997). For illustration purposes, the total magnetic
field vector and the fluid vorticity vector are assumed orthogonal
as depicted in Fig. 1, and in first approximation, both angu-
lar acceleration and diffusive couple dyadic contributions are
ignored. Hence, this spin-vorticity asynchrony gives rise to a
mechanical torque that will tend to pull the dynamic magnetiza-
tion vector out from the direction of equilibrium (or equivalently,
the direction of the local total magnetic field at motionless state).
Non-collinearity between dynamic magnetization and magnetic
field in return results in a counteracting magnetic torque, which
will try to pull in the magnetization vector back to its equilib-
rium position. The mechanical torque is proportional to a vortex
viscosity, which proportionates the magnetic torque response.
Two magnetoviscous behaviors, as a consequence, could arise

1672-2515/$ – see front matter © 2007 Chinese Society of Particuology and Institute of Process Engineering, Chinese Academy of Sciences. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.cpart.2006.12.001
 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60 51

Nomenclature V bounded open set representing the averaging

region
a coefficient in the Müller porosity model |V| volume of the averaging region V (m3 )
b coefficient in the Müller porosity model
V␥ open set region within V occupied by the fer-
B magnetic flux density (T)
rofluid
BPw wall by-pass fraction |V␥ | volume of V␥ (m3 )
C symmetric couple stress dyadic (kg/s2 )
V␬ union of a finite number of open sets within V
d grain diameter (m) occupied by porous media (granular)
D column diameter (m) x position vector locating in the macroscale frame,
dh hydrodynamic diameter of coated nanoparticle the centroid of the averaging volume region V (M)
(m) y relative position vector in the microscale frame of
dm nanoparticle diameter of magnetic core (m) a point in V (M)
eθ unit vector in tangential direction z axial coordinate in the column (m)
E-- antisymmetric triadic
f0 Larmor frequency (Hz) Greek letters
G body couple density vector (Pa) Γ ␥␬ Ferrofluid-solid interface inside V
g gravity vector (m/s2 ) Ξ demagnetization LMM Correction
h self-consistent demagnetizing field vector α gradient programming of the applied magnetic
induced inside the magnetized ferrofluid mat- field (A/m2 )
ter and the induced magnetic field in the β offset constant of the applied magnetic field (A/m)
non-magnetic granular phase (A/m) χ0 initial magnetic susceptibility
he equilibrium demagnetizing field vector prevail- χ␣ magnetic susceptibility of ␣-phase
ing in the ferrofluid phase at magnetohydrostatic χ␬ magnetic susceptibility of non-magnetic material
conditions (A/m) making up the granular phase
H dynamic total magnetic field vector (A/m) εb coefficient in the Müller porosity model
He magnetohydrostatic total magnetic field vector ε␥ porous medium porosity
(A/m) φh hydrodynamic volume fraction of the surfactant-
H0 externally applied magnetic field vector (A/m) dressed nanoparticles
I moment of inertia density of the magnetic φm suspension volume fraction of magnetic material
nanoparticles (m2 ) embedded in the nanoparticles
I idemfactor dyadic γ␣ gravitational amplification factor of ␣-phase
k Boltzmann constant (J/K) η dynamic viscosity (Pa s)
K anisotropy constant of the single-domain uniaxial η0 dynamic viscosity of the liquid carrier (Pa s)
ferromagnetic nanoparticle (J/m3 ) η shear spin viscosity (kg m/s/rad)
L column length (m) ␸␥ ␥-phase-side values of the variable ␸ on Γ ␥␬
m̄ magnetic dipole moment of an individual ␸␬ ␬-phase-side values of the variable ␸ on Γ ␥␬
nanoparticle (A/m) ϕ̃ spatial fluctuation of the bounded piecewise con-
M ferrofluid dynamic magnetization vector (A/m) tinuous scalar field ϕ around the intrinsic average
My magnetic stress tensor in ␥-phase in Vγ ∪ Γγκ
n␥␬ normal canonical unit vector associated with con- ϕ̃ spatial fluctuation of the bounded piecewise con-
tour (␥␬ ) tinuous vector field ϕ around the intrinsic average
P pressure (Pa) in Vγ ∪ Γγκ
r radial coordinate in the column (axisymmetry) λ second coefficient of viscosity (Pa s)
(m) λ bulk spin viscosity (kg m/s/rad)
R column radius (m) μ0 absolute magnetic permeability of vacuum,
R position vector locating a point in V (m) 4␲ × 10−7 (N/A2 )
t time (s) ρ density (kg/m3 )
T absolute temperature (K) ρs dressing surfactant density (kg/m3 )
T pressure-viscous-spin/vorticity stress tensor (Pa) ρP magnetic core density (kg/m3 )
U0 ferrofluid superficial velocity (inlet) (m/s) υ␣ kinematic viscosity of ␣-phase (m2 /s)
v ferrofluid local instantaneous velocity vector τ effective relaxation time of magnetization (s)
(m/s) τB Brownian relaxation time (s)
∂V V associated entrance/exit contours τN Néelian relaxation time (s)
∂V␥e ␥-phase associated entrance/exit contours ␻ spin density vector (rad/s)
∂V␬e ␬-phase associated entrance/exit contours ζ vortex viscosity (Pa s)
52 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60
Subscripts
l Langevin
r radial projection of variable
z axial projection of variable
␥ phase related to ferrofluid
␬ phase related to granular porous media
θ azimuthal projection of variable
Tensor operations
t transpose

|| || Euclidian norm (for vectors): ϕ||ϕ|| = ϕ• ϕ
⊗ Tensor product
: double contracted product
• dot product or contracted product
× curl product
 gradient
• divergence
× curl
 Laplacian
depending on magnetic field and ferrofluid vorticity magnitudes
and mutual orientations with respect to wall.
Magnetoviscothickening, a magnetically driven apparent
inflation in local ferrofluid suspension viscosity, occurs when
the fluid vorticity and the magnetized nanoparticle spin are in
contrarotation or are in corotation with fluid vorticity faster than
the nanoparticle spin velocity (Fig. 1a). The retarding effect by
the nanoparticle spin velocity results locally in an increased dis-
sipation in the flow and, eventually, a slow down in fluid linear
velocity. Magnetoviscothickening has been reported for Hagen-
Poiseuille and turbulent pipe flows with steady and oscillating
spatially homogeneous magnetic fields (Schumacher, Sellien,
Knoke, Cader, & Finlayson, 2003). Similarly, Magnetoviscoth-
inning, tantamount to an apparent drop off in local ferrofluid
suspension viscosity, occurs when fluid vorticity and magne-
tized nanoparticle spin are in corotation with the nanoparticle
spin velocity faster than the fluid vorticity (Fig. 1b). Part of the
nanoparticle internal angular momentum is transmitted to the
fluid deflating fluid dissipation as in drag reduction reminiscent
of polymeric behaviors. This phenomenon has been observed in
laminar pipe flow with high-frequency oscillating linearly polar-
ized magnetic fields (Bacri, Perzynski, Shliomis, & Burde, 1995;
Zeuner, Richter, & Rehberg, 1998). An intermediate case, corre-
sponding to classical fluid mechanics situation, also exists when
no spin lag between fluid element and magnetized nanoparticle
yields null magnetic and hydrodynamic torques. This cancels
the internal angular momentum equation and eliminates spin
coupling with linear momentum balance.
We propose to explore in this paper potential applications
of magnetoviscosity in chemical engineering. The demonstra-
tion example will highlight the control of wall channeling
in porous media exhibiting low column-to-particle diameter
ratio. It is well known that such low-ratio columns may occa-
sion severe maldistribution due to large radial permeability
contrast with preferential flow short-circuiting alongside the
high-permeability wall area. The challenge will be to identify
which configurations are propitious to creating sufficient mag-
netoviscosity near the vessel wall to hammer the bypass and to
reroute maximum fraction of fluid flow towards bed core.
High fluid vorticity is encountered near the vessel wall where
an unobstructed gross wall flow develops. Conversely, bed core
vorticity is the lowest due to porosity distribution damping,
which implies weaker local velocity variations. It is anticipated
that application of magnetic fields to ferrofluids would yield skin
magnetoviscothickening mainly located in the wall region. It is
hoped that nanoparticle spin retardation would therefore arti-
ficially increase resistance to flow in this region thus yielding
lower wall bypass fraction. One simple arrangement to induce
magnetoviscosity corresponds to axisymmetric magnetic field
and geometry to have magnetic torque, vorticity and spin veloc-
ity orthoradial (Fig. 1). To sharpen the contrasts in the velocity
profiles owing to the Kelvin body force, a divergenceless exter-
nal magnetic field with positive and negative constant-gradient
streamwise component is chosen.
Magnetoviscosity is analyzed by formulating the general
local ferrohydrodynamic model, the general upscaled volume-
average model in porous media with the closure problem, and
solution and discussion of a simplified zero-order steady-state
isothermal incompressible axisymmetric model for non-Darcy
flow of a Newtonian ferrofluid in a Müller porous medium sub-
ject to a total magnetic field accounting for bulk-flow oriented
external field H0 , ferrofluid self-consistent demagnetizing field
h and induced magnetic field h in the non-magnetic granu-
lar phase. Shliomis (1972) magnetization relaxation equation
has been written in the fluid compressible form according to
Felderhof (2001). Both external and total magnetic fields are
taken to be irrotational (zero free-current density in packed bed,
i.e., non-conducting ferrofluid and porous medium).
2. Problem statement
2.1. Local description
Isothermal and incompressible single-phase Newtonian fer-
rofluid (␥-phase) upflow in a non-magnetic (␬-phase) rigid
Müller porous medium (Fig. 2c) is assumed. Also, a pseudo-
Coulombic approach of the coupled magnetostatic problem is
used. The Cauchy (or boundary-value) problem describing flow
in the macroscopic region V, needed for spatial averaging, is
stated in Table 1. The (macroscopic region) open set V, bounded
by the ∂V␥e and ∂V␬e phase-associated entrance/exit contours
on V faces, is composed of the ferrofluid part, V␥ , the porous
medium part, V␬ , and the fluid-solid interface, Γ ␥␬ , inside V
(Fig. 2b): V = V␥ + V␬ + Γ ␥␬ . For the sake of brevity, the bound-
ary conditions on ∂V = ∂V␥e + ∂V␬e of the velocity (v␥ ), spin
(␻␥ ), magnetization (M␥ ), induced magnetic fields (h␥ , h␬ )
and the initial conditions are omitted, even though these are
usually not known a priori. We will postulate, without proof,
that there exists for our model porous medium, a spatially peri-
odic representative elementary volume REV of the order of the
macroscopic volume, such that ignorance of these boundary
 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60 53

Fig. 1. Illustration of the magnetoviscosity effect: (a) magnetoviscothickening and (b) magnetoviscothinning.

conditions does not harm the closure problem of the volume-
averaged equations (Whitaker, 1999). Table 1 summarizes the
continuity, linear momentum, internal angular momentum, mag-
netization relaxation, Maxwell-flux law and Ampère-Maxwell
law local equations in V, along with Γ ␥␬ boundary conditions
and constitutive tensor and vector equations. Table 2 gathers the
auxiliary equations for the relaxation time, τ, ferrofluid dynamic
and vortex viscosities, η and ζ, suspension volume fraction, φh ,
scalar moment of inertia density, I, fluid initial magnetic suscep-
tibility, χ0 , linear magnetic material (LMM) approximation for
demagnetizing and induced fields, Ξ, porosity model, ε, external
magnetic field, H0 , volume-average Langevin magnetization,
m , under resultant external and equilibrium demagnetizing
fields, and wall bypass fraction, BPw .

Table 1
Local ferrohydrodynamic model
Continuity ∇ • v␥ = 0 in V␥ (1)
∂
Linear momentum ρv + ∇ • ρv␥ ⊗ v␥ = ∇ • T + ∇ • M + ρg in V␥ (2)
∂t ␥ ␥ ␥
∂
Internal angular momentum ρI␻␥ + ∇ • ρI␻␥ ⊗ v␥ = ∇ • C − E : T + G␥ in V␥ (3)
∂t ␥ ␥
∂
Magnetization relaxation M␥ + ∇ · M␥ ⊗ v␥ = ␻␥ × M␥ − τ −1 (M␥ − Ml ) in V␥ (4)
∂t
Maxwell-flux law ∇ • μ0 (H0 + h␥ + M␥ ) = 0 in Vτ (5)
∇ • μ0 (1 + χ␬ )(H0 + h␬ ) = 0 in V␥ (6)
∇ • μ0 H 0 = 0 in V (7)
Ampère-Maxwell law ∇ × (H0 + h␥ ) = 0 in V␥ (8)
∇ × (H0 + h␬ ) = 0 in V␬ (9)
∇ × H0 = 0 in V (10)
Boundary conditions on fluid-solid interface v␥ = 0 on Γ␥␬ (11)
Γ ␥␬ inside macroscopic region V
(h␬ − h␥ ) × n␥␬ = 0 on Γ␥␬ (12)
(h␬ − h␥ ) • n␥␬ = M␥ • n␥␬ on Γ␥␬ (13)
μ0
Constitutive relations ω␥ = M × (H0 + h␥ )on Γ␥␬ (14)
4ζ ␥
␻␥ × M␥ = τ −1 (M␥ − Ml )on Γ␥␬ (15)
Pressure-viscous stress tensor T = −p␥ I + η(∇v␥ + t ∇v␥ ) + λ∇ • vγ I + ζE · (∇ × vγ − 2ωγ ) (16)
␥
μ0
Magnetic stress tensor M = − ||H0 + h␥ ||2 I + μ0 (H0 + h␥ + M␥ ) ⊗ (H0 + h␥ ) (17)
␥ 2
Couple stress dyadic C = η (∇␻␥ +t ∇␻␥ ) + λ ∇ • ␻␥ I (18)
␥
External–internal exchange angular momentum −E : T = 2ζ(∇ × v␥ − 2␻␥ ) (19)
␥
Body couple density G␥ = μ0 M␥ × (H0 + h␥ ) (20)
  π μ m̄  6 kT
 H + he
3 0 e −1 0 ␥
Langevin equilibrium (e) magnetization Ml = φm m̄ coth dm ||H0 + he␥ || − ||H + h␥ || (21)
6 kT 3 μ m̄
πdm 0
0
||H0 + he␥ ||
54 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60
Fig. 2. Porous medium details.
2.2. Upscaling
Upscaling is an inescapable prerequisite step allowing the
passage from complex and still out-of-reach pore level solutions
of the above physical phenomena. Upscaling consists in formu-
lating an equivalent set of volume-average equations describing
the ferrofluid macroscopic behavior at the porous medium level
Table 2
Auxiliary equations used in ferrohydrodynamic model
1 1
Relaxation time
τ τB
from a description using the local ferrohydrodynamic equations.
We have used the spatial averaging theorem and its corollaries,
the theorem of derivative-integral interchange, a spatial decom-
position around the intrinsic averages and truncation at the
zeroth order of the Taylor expansion around the macroscopic
volume centroid (Fig. 2b) of the non-localized intrinsic aver-
ages to build the volume-average ferrohydrodynamic model.
Without going into the details of the procedure, the resulting
volume-average equations contain several integrals of the spa-
tially fluctuating microscale terms that need to be approximated
regarding velocity, spin density, magnetization, external mag-
netic field, ferrofluid demagnetizing field and induced magnetic
field in granular phase. The macroscopic ferrohydrodynamic
model with the unknown closure terms is summarized in Table 3.
Note that this model applies to the points belonging to the packed
bed interior domain excluding the vessel peripheral boundaries,
which need appropriate boundary conditions. Formulation of the
15 model closure terms is a task of formidable complexity, and
to the authors’ best knowledge, such closures have not been yet
formulated for porous media flows.
2.3. Closure problem
Assuming as in Schumacher et al. (2003) that spin viscosity
shear and bulk coefficients are zero relaxes four closure terms
1 2kT 3
= + = + f0 e−K/kTπdm /6 (22)
τN πdh3 η0
 
−1
η 5 dn − dm 3 dn − dm 6
Ferrofluid suspension viscosity = 1 − φm 1+ − 1.552φm 1 + (23)
η0 2 dm dm
Hydrodynamic-to-magnetic volume fraction φh dm = φm dh
3 3
(24)
5 + ρ (d 5 − d 5 )
1 ρp dm s h m
Scalar moment of inertia density I= (25)
3
10 ρp dm + ρs (dh3 − dm
3
)
Vortex viscosity ζ = 1.5ηφh (26)
π φm μ0 m̄2 dm3
Initial magnetic susceptibility χ0 = (27)
18 kT
LMM approximation correction Ξ = χ0 (3 + 2χ0 )−1 (28)
a(D − 2r)

Bed porosity radial distribution (Müller model) ε(r) = εb + (1 − εb )J0 e−b(D−2r)/2d (29.1)
2d
(−1)i r2i
∞

J0 (r) = (29.2)
22i (i!)2
i=0
d
εb = 0.365 + 0.22 (29.3)
⎧ D
⎨ 7.45 − 3.15 d D ∈ [2.02 − 13.0]
a= D d (29.4)
⎩ 7.45 − 11.25 d D ≥ 13.0
D d
d
b = 0.315 − 0.725 (29.5)
r D

External magnetic field H 0= − αt

0 αz + β (30)
2  π μ m̄  
6 kT
Volume-average Langevin magnetization ||ml || = φm m̄ coth 3 0
dm ||H0 + he || − ||H0 + he ||−1 (31.1)
 6 kT  πdm μ0 m̄
3

H0r + her H0z + hez

ml = t
||ml ||0 ||ml || (31.2)
||H0 + he || ||H0 + he ||
 D/2  D/2 −1

Wall bypass fraction BPw = rε(r)vz (r) dr( rU0 dr) (32)
D/2−d/2 D/2−d/2
 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60 55

Table 3
Complete volume-average ferrohydrodynamic model
Volume conservation ε␥ + ε␬ = 1 (33)
 
Continuity ∇ · ε␥ v␥ =0 (34)
␥

∂        
Linear momentum ρ ε␥ v␥ + ρε␥ ∇ v␥ • v␥ + ρ∇ • ṽ␥ ⊗ ṽ␥ =
∂t ␥ ␥ ␥  
    ε␥     ∇ε␥   1
−ε␥ ∇ p␥ + ε␥ ρg + (η + ζ)ε␥ Δ v␥ + v␥ + ∇ v␥ • + 2ζε␥ ∇ × ␻␥ + 2ζ n ×
␥ ␥ ε␥ ␥ ␥ ε␥ ␥ |V | Γ ␥␬
   γκ

     
1
␻
˜ ␥ dσ + μ0 ∇ H̃ 0 + h̃␥ • M̃ ␥ + μ0 ε␥ ∇ H 0 + h␥ + (H̃ 0 + h̃␥ ⊗ n␥␬ dσ) •
␥ |V |
 Γγκ
  1
M␥ (−p̃␥ I + (η + ζ)∇ ṽ␥ ) • n␥␬ dσ (35)
␥ |V |
Γγκ
∂        
Internal angular momentum ρI ε␥ ␻␥ + ρI∇ ␻␥ • ε␥ v␥ + ρI∇ • ␻ ˜ ␥ ⊗ ṽ␥ =
∂t  ␥ ␥ ␥ 
  ∇ε␥           
+2ζε␥ ∇ × v␥ + × v␥ − 2 ␻␥ + ε␥ μ0 M ␥ × (H 0 + h␥ ) + μ0 M̃ ␥ × H̃ 0 + h̃␥ +
␥ ε␥ ␥ ␥ ␥ ␥
   

   
    1   
 1
η ε␥ Δ ω␥ + (η + λ )ε␥ ∇∇ • ␻␥ + (η + λ )∇ ˜ ␥ • n␥␬ dσ
␻ + η +λ ˜ ␥ n␥␬ dσ + η ∇ •
∇ •␻
␥ ␥ |V | |V |
   
Γγκ Γγκ

1 1
˜ ␥ ⊗ n␥␬ dσ
␻ + η ∇␻
˜ ␥ • n␥␬ dσ (36)
|V | Γγκ
|V | Γγκ
∂            
Magnetization relaxation ε␥ M ␥ + ∇ε␥ M ␥ • v␥ + ε␥ M ␥ ∇ • v␥ + ∇ • M̃ ␥ ⊗ ṽ␥ =
∂t   ␥ ␥ ␥ ␥ ␥
    ε␥    
+ε␥ ␻␥ × M ␥ + ω̃␥ × M̃ ␥ − ( M ␥ − M l ) (37)
␥ ␥ τ ␥ ␥

     
Maxwell-flux law ∇ • (ε␥ h␥ + ε␥ M ␥ + ε␬ h␬ )=0 (38)
␥ ␥ ␬

  1
ε␬ ∇ • h␬ − h̃␬ • n␥␬ dσ = 0 (39)
␬ |V | Γ␥␬
∇ • H0 = 0 (40)

   
Ampère-Maxwell law ∇ × (ε␥ h␥ + ε␬ h␬ )=0 (41)
␥ ␬

  1
ε␬ ∇ × h␬ − n␥␬ × h̃␬ dσ = 0 (42)
␬ |V | Γ␥␬
∇ × H0 = 0 (43)

   
LMM approximation h␬ = (1 + Ξ) h␥ (44)
␬ ␥

in (36). In addition, the integrand of the last closure term in virtually opens onto a deadlock when attempting to infer a
the linear momentum balance equation (35) contains the sum mean-field effective magnetic permeability of the composite
of the ferrofluid dynamic and vortex viscosities multiplied by ferrofluid-granular system. When fluid and solid magnetic per-
the gradient of the fluctuating velocity on Γ ␥␬ . This suggests meabilities do not differ much and a linear magnetic materials
that unlike classical drag formulation, the drag function here (LMM) behavior is valid (case of low magnetic field linear-
must account for the occurrence in the laminar Darcy or Ergun Langevin limit), the effect of contacts between non-magnetic
equation term of the total viscosity rather than only the dynamic grains is not very important and the Maxwell-Garnett theory
viscosity. can be used (Khuzir, Bossis, Bashtovoi, & Volkova, 2003).
The closures (39) and (42) hide in the granular induced mag- This theory assumes random distribution of grains in a car-
netic field vector a monumental complexity associated with rier medium subject to a local Lorentz field. For spheres in
the hydrodynamic perturbation of the ferrofluid dynamic mag- densely packed beds with LMMs, the previous closures can
netization vector as well as the non-linear Langevin equation be replaced by (44) which relate the ferrofluid demagnetiz-
between equilibrium magnetization, external and equilibrium ing field and the induced magnetic field in the granular phase.
demagnetizing fields ((31.1)–(31.2)). In the general case, this Due to lack of better alternatives, we extend in this work the
56 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60

LMM approximation even to the non-linear region. This arti- ing the modified Ergun drag function in (45) and (46). Solution
fice allows ignoring the closures associated with (39) and (42). of the coupled partial differential and integral equations is per-
In addition, the solid magnetic susceptibility, χ␬ , is neglected formed using a finite difference scheme on an Aspen Custom
with respect to the initial ferrofluid magnetic susceptibility, Modeler platform. Discretization meshes along r and z direc-
χ0 , yielding the LMM approximation correction (28). In addi- tions are, respectively, 0.2 and 4 mm. To ensure convergence of
tion, since ferrofluid magnetization is the chief determinant the numerical scheme, both fast-Newton method for non-linear
of both solid induced magnetic and ferrofluid demagnetizing solver with convergence criterion on residuals, and a MA48 lin-
fields, these should remain small with respect to the external ear solver are used. Typical simulation duration is 30 min on a
field to attempt further simplifications to be discussed next. 3 GHz CPU and 1.5 Giga octet RAM computer with a 10−5 for
Closure of the eight remaining terms entails mathematical com- the absolute equation tolerance.
plications and physical efforts beyond the scope of this study. It is noteworthy that the ferrofluid velocity and nanopar-
Rather, we will restrict to solve the zero-order formulation and ticle spin density fields are invariant to switching H0 into
leave the complete formulation as an open problem for future −H0 because the induced magnetic field in the solid and the
research. demagnetizing field in the ferrofluid have been neglected in the
ferrohydrodynamic bloc of equations. For consistency purposes,
the H0 z-projection is always positive. Furthermore, parameter
2.4. Zero-order axisymmetric volume-average model
β of the magnetic field (30) is chosen such that H0z = 0 at the
entrance (positive gradient) or at the exit (negative gradient).
Assuming that all the variables in the physical problem are
Fig. 3 illustrates the evolution of the fractional bypass nor-
independent of the azimuthal coordinate (axisymmetry), the pro-
malized with respect to the bypass when H0 = 0 as a function of
jections of Table 3 model equations along the three (r, θ, z)
the z-component external magnetic field positive and negative
coordinate axes are given in Table 4 together with the boundary
gradients. By convention, the external magnetic field is always
conditions chosen at the four peripheral boundaries of the porous
bulk-flow oriented. The volume-average asynchrony, defined
medium: z = 0, z = L, r = 0, r = R. We will assume without proof,
earlier, corresponds, regardless of magnetic gradient sign, to
uniqueness of solution for the system of equations describing
Fig. 1a case. Therefore, there is confirmation of a magnetovis-
this ferrohydrodynamic model.
cothickening effect, which tends to reduce the preferential flow
The pressure field is assumed to depend only on the axial
alongside the wall. The maximum reduction could be as low as
coordinate. The external magnetic field is purposely chosen to
18% at the highest negative gradient. The non-symmetry of the
exhibit only radial and axial dependences while fulfilling the
bypass with respect to the vertical axis, which is more severe for
divergenceless condition, thus H0θ = 0 ((40), (57.1)). This entails
negative gradient than for positive gradient, is due to a global
that azimuthal component of the equilibrium magnetization vec-
outcome of magnetoviscosity and Kelvin body force density.
tor is zero. In addition, the boundary conditions ((69)–(80),
Because of the gross approximations made in Section 2.4 regard-
(93)–(96)) as well as ((48)–(50), (54)) are verified by the trivial
ing the demagnetizing field and its gradient with respect to the
set ωr = ωz = 0, mθ = 0 and vθ = 0. These are taken as solutions for
external magnetic field and its gradient, the curve in the vicinity
our model. As for the equilibrium magnetization on eθ direction,
of dH0z /dz = 0 has to be considered with caution because of the
the last equality mθ = 0 is also coherent with H0θ = 0. Therefore,
approximation of the neglect of the demagnetizing field under
according to ((31.1)–(31.2)), it is not unrealistic to assume also
low external magnetic fields.
that hθ = 0 (57.2).
Preliminary simulations reveal that typically
||h|| < 10%||H0 || suggesting a further simplifica-
tion of the model towards decoupling magnetostatics
((55)–((58.1)–(58.3))) from the ferrohydrodynamic equa-
tions (45)–(54). Strictly speaking, this requires that the norm
1/2 1/2
condition (t ∇ h- : ∇ h- ) << (t ∇ H : ∇ H ) , due to the
- - - -0 - -0
Kelvin force terms in (46), (47) must also be verified; which
is always the case except near the wall, the entrance (positive
gradient) and the exit (negative gradient) regions at low
magnetic fields.

3. Implementation and discussion

Table 5 contains the simulation parameters of the simplified

zero-order axisymmetric volume-average ferrohydrodynamic
model of Table 4. Note that a fluid superficial velocity of 0.2 m/s
is chosen such that ferrofluid inertia cannot be ignored (non-
Darcy flow). The consensual values for the laminar and inertial Fig. 3. Normalized bypass fraction for various z-component external magnetic
Ergun constants are used, i.e., respectively, 150 and 1.75; yield- field gradients.
 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60 57

Table 4
Simplified zero-order axisymmetric volume-average ferrohydrodynamic model
 D/2
U0 D2
Continuity ε vz r dr =
8

0
 (45)
∂vr v2 ∂vr
Linear momentum (radial) ρ vr − θ + vz =
∂r r ∂z
   
∂2 vr 1 ∂vr vr ∂2 vr vr d2 ε 1 dε 1 dε ∂vr ∂ωθ
(η + ζ) + − 2 + 2 + + + − 2ζ +
∂r2 r ∂r r ∂z ε dr2 r dr ε dr ∂r ∂z
μ0
dH ∂hr

∂hr

0r
mr + + mz
ε
vr 1 − ε
dr ∂r
η+ζ 1−ε
∂z
ρ 2

− 150 2 + 1.75 vr + v2z + v2θ

d ε d ε d
∂v
    (46)
z ∂vz ∂2 vz 1 ∂vz ∂2 vz vz d2 ε 1 dε 1 dε ∂vz
Linear momentum (axial) ρ vr + vz = (η + ζ) + + + + + +
∂r ∂z ∂r2 r ∂r ∂z2 ε dr2 r dr ε dr ∂r
∂ω ωθ

μ0
dH0z ∂hz

∂hz

θ
2ζ + + mz + + mr −
∂r r ε dz ∂z
∂r dp
vz 1 − ε η+ζ 1−ε ρ 2
150 2 + 1.75 vr + v2z + v2θ − − ρg
d ε d ε d dz
∂v vθ

∂vθ

(47)
θ
Linear momentum (azimuthal) ρ vr + + vz = (η +
 ∂r r ∂z    ∂ω

2
∂ vθ 1 ∂vθ vθ 2
∂ vθ vθ d2 ε 1 dε 1 dε ∂vθ r ∂ωz
ζ) + − + + + + + 2ζ − +
∂r2 r ∂r r2 ∂z2 ε dr2 r dr ε dr ∂r ∂z ∂r
μ0
H0r hr

vθ 1 − ε
η+ζ 1−ε ρ 

mθ + − 150 2 + 1.75 v2r + v2z + v2θ

ε r r d ε d ε d
∂ω ωθ ∂ωr

∂vθ

μ0
(48)
r
Internal angular momentum (radial) ρI vr − vθ + vz = −2ζ + 2ωr + mθ (H0z + hz )
∂r r ∂z ∂z ε
∂ω ∂ωz

vθ ∂vθ vθ dε

μ0
(49)
z
Internal angular momentum (axial) ρI vr + vz = 2ζ + + − 2ωz − mθ (H0r + hr )
∂r ∂z ε dr
∂ω ωr ∂ωθ

r ∂r ε (50)
θ
Internal angular momentum (azimuthal) ρI vr + vθ + vz =
∂v ∂r ∂v r v dε ∂z
μ
r z z 0
2ζ − − − 2ωθ + (mz (H0r + hr ) − mr (H0z + hz ))
∂z ∂r ε dr ε
∂mr mθ ∂mr
vr ∂vr ∂vz

(51)
Magnetization relaxation (radial) vr − vθ + vz + mr + + = ωθ mz − ωz mθ − τ −1 (mr − εmr ) (52)
∂r
∂mz
r
∂mz
v
∂z
∂vr
r
∂vz
∂r
∂z
= −ωθ mr + ωr mθ − τ −1 (mz − εmlz )
r
Magnetization relaxation (axial) vr + vz + mz + + (53)
∂r
∂m m∂zr ∂mθ r
v ∂z∂v
∂r ∂vz

= ωz mr − ωr mz − τ −1 mθ
θ r r
Magnetization relaxation (azimuthal) vr + vθ + vz + mθ + +
∂r r ∂z r ∂r
mr ∂mr ∂mz
h ∂hr ∂hz

∂z dε
(54)
r
Maxwell-flux law (demagnetizing field) + + = −ε + + + Ξ(H0r + hr ) − (1 −
r ∂r ∂z r
∂r ∂z

dr
H0r ∂H0r ∂H0z hr ∂hr ∂hz
ε) Ξ + + + (Ξ + 1) + +
r ∂r ∂z r ∂r ∂z
∂h ∂hz

dε
(55)
r
Ampère-Maxwell law (azimuthal) (1 + Ξ(1 − ε)) − + Ξ(H0z + hz ) =0
∂z ∂r dr (56)
Azimuthal external magnetic field H0θ = 0 (57.1)

Azimuthal demagnetizing field hθ = 0 (57.2)

Induced magnetic field in granular phase hr = (1 + Ξ)hr (58.1)

hz = (1 + Ξ)hz (58.2)

hθ = 0 (58.3)

d2 dp
Boundary conditions on packed bed (0) = 0
dz2 dz
domain peripheral boundaries (59)
d dp
(L) = 0
dz dz
  (60)
vr (r, 0) = 0 r ∈ 0; D/2
(61)
∂vr
(r, L) = 0 r ∈ [0; D/2]
∂z (62)
58 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60

Table 4 (Continued )
vr (0, z) = 0 z ∈ ]0; L[ (63)
vr (D/2, z) = 0 z ∈ ]0; L[ (64)
vz (r, 0) = Uo r ∈ [0; D/2] (65)
∂vz
(r, L) = 0 r ∈ [0; D/2] (66)
∂z
∂vz
(0, z) = 0 z ∈ ]0; L[ (67)
∂r
vz (D/2, z) = 0 z ∈ ]0; L[ (68)
vθ (r, 0) = 0 r ∈ [0; D/2] (69)
∂vθ
(r, L) = 0 r ∈ [0; D/2] (70)
∂z
vθ (0, z) = 0 z ∈ ]0; L[ (71)
vθ (D/2, z) = 0 z ∈ ]0; L[ (72)
ωr (r, 0) = 0 r ∈ [0; D/2] (73)
ωr (r, L) : Extension by continuity (49) r ∈ [0; D/2] (74)
ωr (0, z) = 0 z ∈ ]0; L[ (75)
ωr (D/2, z) = 0 z ∈ ]0; L[ (76)
ωz (r, 0) = 0 r ∈ [0; D/2] (77)
ωz (r, L) : Extension by continuity (50) r ∈ [0; D/2] (78)
∂ωz
(0, z) = 0 z ∈ ]0; L[ (79)
∂r
ωz (D/2, z) = 0 z ∈ ]0; L[ (80)
ωθ (r, 0) = 0 r ∈ [0; D/2] (81)
∂2 ωθ
(r, L) = 0 r ∈ [0; D/2] (82)
∂z2
ωθ (0, z) = 0 z ∈ ]0; L[ (83)
ωθ (D/2, z) : Extension by continuity (51) z ∈ ]0; L[ (84)
mr (r, 0) = 0 r ∈ [0; D/2] (85)
mr (r, L) : Extension by continuity (52) r ∈ ]0; D/2] (86)
mr (0, z) = 0 z ∈ ]0; L[ (87)
mr (D/2, z) : Extension by continuity (52) z ∈ ]0; L[ (88)
mz (r, 0) = 0 r ∈ [0; D/2] (89)
mz (r, L) = Extension by continuity (53) z ∈ ]0; D12] (90)
∂mz
(0, z) = 0 z ∈ ]0; L[ (91)
∂r
mz (D/2, z) : Extension by continuity (53) z ∈ ]0; L[ (92)
mθ (r, 0) = 0 r ∈ [0; D/2] (93)
mθ (r, L) : Extension by continuity (54) r ∈ ]0; D/2] (94)
mθ (0, z) = 0 z ∈ ]0; L] (95)
mθ (D/2, z) : Extension by continuity (54) z ∈ ]0; L] (96)
hr (r, 0) = 0 r ∈ [0; D/2] (97)
hr (r, L) : Extension by continuity (55) r ∈ ]0; D/2] (98)
hr (0, z) = 0 z ∈ ]0; L] (99)
hr (D/2, z) : Extension by continuity (55) z ∈ ]0; L[ (100)
hz (r, 0) = 0 r ∈ [0; D/2] (101)
hz (r, L) : Extension by continuity (56) r ∈ ]0; D/2] (102)
∂hz
(0, z) = 0 z ∈ ]0; L] (103)
∂r
hz (D/2, z) : Extension by continuity (56) z ∈ ]0; L[ (104)
 F. Larachi, D. Desvigne / China Particuology 5 (2007) 50–60 59

Table 5
Selected numerical property values used in ferrohydrodynamic model
Anisotropy constant K (kJ/m3 ): 23
Bed height L (cm): 10
Boltzmann constant k (yJ/K): 13.8
Demagnetization LMM correction Ξ: 0.23
Diameter of column D (cm): 2
Diameter, hydrodynamic coated dh (nm): 28
Diameter, magnetic (uncoated) dm (nm): 15
Diameter of packing d (mm): 2
Ferrofluid density ρ (kg/m3 ): 1056
Ferrofluid viscosity η (mPa s): 0.2
Ferrofluid vortex viscosity ζ (mPa s): 0.07
Initial magnetic susceptibility χ0 : 1.28
Larmor frequency f0 (GHz): 1
Magnetic particle density ρp (kg/m3 ): 5300
Liquid carrier viscosity η0 (mPa s): 0.1
Magnetic dipole moment m̄ (MA/m): 0.45
Moment of inertia density I (am2 ): 45
Relaxation, Brownian τ B (␮s): 0.83
Relaxation, Néelian τ N (␮s): 18.4
Second coefficient of viscosity λ (Pa s): 0
Shear/bulk spin viscosities η , λ (kg m/s/rad): 0
Superficial ferrofluid velocity U0 (m/s): 0.2
Surfactant density ρS (kg/m3 ): 500
Temperature T (K): 300
Volume fraction, hydrodynamic φh (%): 23.4
Volume fraction, magnetic φm (%): 3.6
Vacuum permeability μ0 (␮N/A2 ): 26

Fig. 4 shows the outlet pressure gradient normalized with

respect to the pressure gradient at H0 = 0 for the conditions sim-
ulated for Fig. 3. Although the negative gradient region coincides
with the expected magneto-viscothickening, the positive gradi-
ent region seems to contradict Fig. 3 findings since pressure
drops in the positive gradient branch are predicted to be lower
than when H0 = 0. This result is easily explained by the fact that
spatially inhomogeneous magnetic fields give rise to a Kelvin
body force, which produces work. In the positive gradient case,
the Kelvin body force z-component is oriented streamwise thus
creating conditions of hypogravity with a tendency to chase the
ferrofluid more quickly out of the bed. As a result of this mag-
netic levitation, pressure gradient diminishes. On the contrary,
when the magnetic field gradient is negative, the Kelvin body
force acts counterstreamwise to the flow like gravitation and
opposes to the ferrofluid from exiting the bed. This artificial
hypergravity state gives rise to a resistive work the ferrofluid
must fight against to be able to get out of the bed. As a follow
Fig. 5. Typical (r,z) contour plot of radial magnetization component for a neg-
up to this study, additional work on the topic could focus on rig- ative z-component external magnetic field gradient.
orous calculations of the demagnetizing field effects at very low
external magnetic fields as well as on the proper formulation
of the closure terms involving the fluctuations of spin den-

sity, magnetization and demagnetizing and induced magnetic

fields.
Fig. 5 exhibits a typical contour plot of the radial compo-
nent of dynamic magnetization for a negative gradient external
magnetic field of −2000 Oe/m.

Acknowledgements

The authors gratefully acknowledge Laval University and

Total S.A. for their fellowship supports.

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