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Keywords: Effective and rapid mixing is crucial for chemical and biological processes. The purpose of the current study is to
Micromixing investigate the effect of steady and varying magnetic field on the mixing of a water-based ferrofluid and two
Microfluidics streams of deionized water inside a microchannel for Lab-on-Chip applications. To this end, the nonlinear
Ferrofluid governing equations, the momentum equation, the continuity equation, the mass transport equation and the
Magnetism
Maxwell-Ampere equations are numerically solved. A commercial code based on the finite-element method is
Lab-on-chip
used and the numerical simulations are validated by the experimental results in the literature. To augment the
mixing performance, the effects of influencing parameters such as the magnetic field strength and frequency,
inlet velocity, relative inlet velocity, and duty cycle (the ratio of signal activation on the total signal length) are
investigated. A mixing efficiency as high as 94.4% only after 13 s is achieved with a peak current of 1 A, a
frequency of 5 Hz, 100 μm/s of inlet velocity, a relative inlet velocity between the ferrofluid and water streams of
0.8 and a duty cycle of 0.2. This proposed model provides a versatile and low-cost solution to intensify mi-
crofluidic mixing performance and develop efficient Lab-on-Chip platforms.
1. Introduction velocity also has limitations, especially when dealing with cells and
bioparticles sensitive to high shear rates. Therefore, designing rapid and
The development and implementation of microfluidic devices are efficient micromixers should be done thoroughly in order to achieve
gaining attention in fields ranging from academia to industry due to adequate mixing.
their small sample volume, low cost and high efficiency [1]. These The diffusion time constant, D , is expressed as
systems are being frequently exploited in biology, pharmacy, bio-
L2
chemistry and other fields [2]. By their versatile characteristics, mi- D =
(1)
D
crofluidic systems can be used for applications varying from detecting
minute amounts of chemical samples [3] to DNA sequencing [4]. To where D is the molecular diffusion coefficient, D = kB T /3 dp , where is
name only a few components of microfluidic systems, valves, pumps, the Boltzmann constant (1.381 × 10 23m2kg/(s2K) ), T is the absolute
detectors, sensors, microreactors and micromixers can be enumerated temperature, and dp is the diameter of magnetic nanoparticles (MNPs),
[5]. respectively. The molecular diffusion and thus the diffusion time con-
Among these elements, micromixers (miniaturized mixing devices stant are based on Brownian motion [8]. The typical value of the mo-
for at least two different phases [6]) are of especial interest. Due to lecular diffusion coefficient for water-soluble molecules is around
miniaturization effects, micromixers typically have low Reynolds 10 9 m2 / s . The diffusion time constant for a system with L = 60 µm ,
numbers (Re = vL/ , where , v , L and are the density of the fluid, dp = 10nm and = 2.5mPa.s at T= 298K is 206.1 s, which is quite long
velocity of the stream, characteristic length of the system and dynamic especially for biomolecules. Therefore, reducing the required time for
viscosity of the fluid, respectively) and the flows are essentially within microfluidic mixing is crucial for designing micromixers.
the laminar region [7]. This size reduction emerges challenges due to Micromixers generally can be categorized into passive and active
the dominance of surface effects over volume effects [6]. The inlet micromixers depending on their operation mechanism [9]. Passive
E-mail addresses: saadat.ac@outlook.com (M. Saadat), behshad@sharif.edu (M.B. Shafii), ghasemi@kntu.ac.ir (M. Ghassemi).
https://doi.org/10.1016/j.cep.2019.107727
Received 24 July 2019; Received in revised form 8 October 2019; Accepted 5 November 2019
Available online 13 November 2019
0255-2701/ © 2019 Elsevier B.V. All rights reserved.
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
micromixers do not have any moving part or energy source other than Nguyen numerically and experimentally investigated the mixing in a
the instruments pumping the fluids. Several strategies are present for circular chamber with a ferrofluid under a uniform external magnetic
passive micromixers such as splitting and injecting of flows [10], dis- field. They achieved a maximum mixing efficiency of 90% at a rela-
turbance generation by using microchannel bas-relief structures [11], tively low magnetic flux density less than 10 mT [1]. Owen et al. pre-
multi-lamination [12], geometry modification [13–16], strips on mi- sented a novel method for mixing using an array of rotating magnetic
cromixer walls [17], or constraining the flow to generate droplets microbeads. They reported a rapid mixing in short channel lengths
[18,19]. However, the usage of passive micromixers faces difficulties [37]. Hejazian et al. reported that a non-uniform magnetic field by
due to their complicated design. On the other hand, active micromixers permanent magnets can help mass transport in a microfluidic device
employ disturbance to enhance the mixing [7]. Active micromixers [38]. Azimi et al. studied the liquid-liquid mass transfer enhancement
typically exploit mechanical disturbance [20], electrical actuation in a Y-type micomixer using ferrofluids [39]. Maleki et al. numerically
[21,22], magnetohydrodynamics [23,24], acoustic streaming [25], investigated the mixing of ferrofluid with a neutral fluid within a dro-
thermal agitation [26], and ultrasonic waves [27] as their actuating plet under a magnetic field. They reported a significant improvement in
energy [4]. Among these strategies, magnetohydrodynamics provides a the mixing efficiency for a specific ratio between the magnetic force and
wireless, low cost and versatile solution for a wide range of applica- the shear force [40]. In another study, Cao et al. proposed a novel
tions, e.g. biomolecular tagging, separation, drug delivery [1,28], par- design by combing a static gradient magnetic field generated by two
ticle fabrication for cell targeting [29], and cell sorting [30]. Ferrofluids microcoils and an alternating magnetic field generated by two coaxial
(stable colloidal suspensions of single-domain MNPs in a carrier liquid Helmholtz coils. They reported a high mixing efficiency of two fluids
[31]) have the fluidity advantages of liquids and the magnetic prop- within 6 s.
erties of solids [32]. Therefore, they are suitable choices for micro- As discussed,micromixers exploiting DC magnetic fields and mag-
mixers exploiting magnetohydrodynamics. netic fields generated by permanent magnets are extensively in-
To fully understand the effect of magnetism on the behavior of ac- vestigated. However, studies concerning the mixing under low-strength
tive micromixing, several studies have been conducted. Bau et al. the- and low-frequency magnetic field and its interactions with the velocity
oretically and experimentally studied the effect of the coupling between and concentration fields are relatively narrow. Also, to the knowledge
the magnetic and electric fields which induced Lorentz body force and of the authors, studies investigating flow-focusing micromixing in
therefore improved mixing [23]. Lu et al. proposed a mixer with ro- straight microchannels and the effect of duty cycle on the mixing be-
tating magnetic field which forces a single magnetic bar, or an array of havior of ferrofluids have not been conducted so far. Therefore, the
them, to rotate rapidly [20]. Suzuki et al. proposed a time-varying purpose of the current study is to numerically investigate the mixing of
magnetic-force-based micromixer consisting of two embedded micro- ferrofluid with two streams of deionized (DI) water under varying
coils. They numerically and experimentally showed that these micro- magnetic field generated by two embedded microcoils. The effects of
coils can generate a magnetic field strong enough to deflect and attract magnetic field strength, current switching frequency ( f ), inlet velocity
nearby magnetic microbeads [30]. Mao and Koser experimentally in- (u 0 ), relative inlet velocity between the ferrofluid and DI waters, and
vestigated the effect of an alternating magnetic field generated by duty cycle of the microcoils are explored in order to reach an optimum
embedded copper coils on the mixing of water-based ferrofluid and a micromixer capable of generating enough disturbance to mix the
fluorescein buffer solution. They reported a micromixer able to rapidly streams efficiently.
mix ferrofluid with the fluorescein buffer solution in a microchannel
forming a 45° angle with respect to embedded coils [33]. Tsai et al.
2. Mathematical modeling and implementation
experimentally investigated the effect of a permanent magnet on the
mixing between ferrofluid and water. They reported a rapid mixing
In the following two sections, the governing equations and the nu-
immediately downstream of the permanent magnet [34]. Wen et al.
merical procedure are explained, respectively.
experimentally investigated the effect of an AC electromagnetic field on
the mixing of ferrofluid and another stream containing fluorescence dye
A Governing Equations and Boundary Conditions
(Rhodamine B) within a microchannel. They reported a high mixing
efficiency at the AC frequency range (45 Hz < f < 300 Hz) within 2 s of
The schematic of the current design is depicted in Fig. 1. The depth
electromagnet actuation [35]. In another study, Wen et al. studied the
of the microchannel inside the paper is assumed to be large enough for
effects of DC and AC electromagnetic fields on the mixing efficiency.
the variations in the depth to be negligible in comparison with the
They achieved a high mixing efficiency at the peak magnetic strength of
changes in the x-y plane. Also, the surface effects far from the walls
approximately 4770 A/m [7]. In another study, Munir et al. proposed a
become small and the 2-D results can qualitatively represent three-di-
finite-element mathematical model to illustrate the mixing behavior of
mensional simulations [41]. Therefore, the domain is assumed to be
the MNPs under different magnetic field frequencies and different flow
two-dimensional (2-D). The computational geometry consists of 3 main
velocities. They found that in order to reach an effective mixing, an
domains: The microchannel, the microcoils generating magnetic field
optimum frequency is needed, which depends on the applied magnetic
and air; see Fig. 1.
field, inlet velocity, channel geometry, and MNP size [36]. Zhu and
The governing equations, i.e. the continuity equation, the
Fig. 1. Geometry of the model. Grey region represents the initial concentration of the ferrofluid inside the microchannel.
2
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
momentum equation, and the mass transport equation for a time- oxide nanoparticles [7]. It is assumed that the magnetic susceptibility
varying system are listed as follows, respectively: varies linearly with the concentration, i.e. = init C where init is the
initial susceptibility of the ferrofluid. This assumption is valid for fer-
. v =0 (2)
rofluids below saturation magnetization, which is the case for our
v model. In Eq. (11), (H ) H using vector analysis can be rewritten as
+ (v . )v = p+ 2v + Fvol
t (3) 2
1/2 H for an electrically-nonconductive fluid [44].
C 2C For the momentum equation, velocity inlet boundary condition is
+ (v )C = D
t (4)
set. At the outlet, the zero-pressure boundary condition is used. At the
where v is the velocity vector, and are the density and dynamic walls, the no-slip boundary condition is applied. For the mass transport
viscosity of the mixture, respectively, p is the pressure and Fvol is the equation, a step function for initial value and inflow concentration
magnetic body force (in ) acting against the fluid. C in Eq. (4) is the (Dirichlet boundary condition) with smoothing around the jump points
dimensionless volume concentration. is used. At the outlet, the no-flux boundary condition is selected. For the
In Eq. (3), gravity is omitted due to miniaturization effects. In Eqs. magnetic field module, coil node is chosen in order to generate a high
(2) and (3), fluids are assumed to be essentially incompressible due to gradient magnetic field with relatively low peak magnetic flux density
the very low velocities. In Eq. (4) it is assumed that the ferrofluid (around 90 G for 1 A current.) The magnetic insulation boundary
particles flow with the velocity field [36], i.e. the convective velocity of condition is applied for the surrounding air.
the MNPs is equal to fluid flow velocity. It is also assumed that the In order to quantify the mixing behavior inside the microchannel, a
MNPs do not agglomerate and thus are monodispersed. The MNPs are parameter has been introduced as a measure to evaluate the mixing
also assumed to be spherical. efficiency:
The Maxwell-Ampere equation reads: h
0
|C C | dy
ME = × 100(%)
×H = J (5) h
| C0 C | dy
0 (12)
where H and J are the magnetic field strength and current density
where ME is the mixing efficiency parameter, C is the concentration
vector, respectively. J is nonzero only for the microcoils and has a for a complete mixing, which is 1/3 for our model and C0 is the inlet
nonzero magnitude only in z-direction. The magnetic flux density, B concentration, which is 0 for DI water streams and 1 for the ferrofluid.
follows the Gauss law: This definition has been checked and a mixing efficiency equal to unity
is achieved with C = 1/3 assuming a steady-state condition with a
B =0 (6)
trivial inlet velocity and a high diffusion constant. In Eq. (12), h is the
The relation between B and H is described by a constitutive relation: height of the microchannel, which is 60µm for our model. Eq. (12) can
be further simplified as:
B = µ 0 (M + H ) (7) h
3 0
|C 1/3| dy
where µ 0 and M are the permeability of the vacuum (=4 × 10 ) 7N/A2 ME = × 100(%)
80
and the magnetization vector, respectively. Introducing a magnetic (13)
vector potential, A , the magnetic flux density takes the form: Eq. (13) and the normalized concentration at the outlet of the micro-
channel are the two factors explaining the quantity and quality of
B = ×A, A =0 (8)
mixing. The higher the mixing efficiency and the uniformity of the
By inserting Eq. (8) into Eqs. (5–7), the magnetic vector potential fi- normalized concentration at the outlet cross section, the better the
nally becomes: mixing performance.
During the mixing process, variations of density and viscosity are
A ×
×A
M =J taken into account using the concept of dimensionless volume con-
µ 0 µr (9) centration [1]:
3
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
Fig. 2. Excitation signal for DC = 0.2 , I0 = 1A and f = 5Hz . When the left coil is
active for 0.2 of the total signal length, the right coil is consequently active for
0.8 of the signal length.
4
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
Fig. 5. Normalized ferrofluid concentration field for different peak currents and excitation frequencies after 15 s. u0 = 200 µm/ s . Two squares for each concentration
distribution represent the microcoils. Complete mixing corresponds to a concentration index equal to 1/3.
1.2 µm (the median of 1 µm and 1.4 µm , which was used by them), iron phenomenon relies heavily on Brownian motion. However, for I0 = 1A ,
oxide content of 12% and relative permeability of 11.3 are used to the magnetic force generates enough lateral disturbance even at higher
replicate their work, as shown in Fig. 4. Also, a constant current of 1 A frequencies and the fingering structures (similar to that reported by
is applied to the microcoils in order to simulate the induced horizontal Wen et al. [7]) emerge, as can be identified in Fig. 5. In addition, Fig. 5
force on the line starting from the centerline of two microcoils to 100 indicates that the complete mixing occurs for concentration index equal
µm towards the right, as shown in Fig. 1. Inlet velocity is set to zero in to 1/3.
order to simulate the induced magnetic velocity. A magnetic flux den- The normalized concentration and mixing efficiencies for different
sity around 44 G is calculated in our work for I0 = 0.5A which agrees magnetic frequencies and currents are shown in Figs. 6 and 7, respec-
with the data reported by Suzuki et al. It is also seen that the trend and tively. As shown, it is seen that the median of the concentration value
range of the horizontal induced force (Fm _ x ) on each microparticle
agree well with that ( 0.18 pN 0.3 pN ) reported by them [30].
5
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
falls far below the ideal concentration value (1/3) with a high standard eventually overtake the higher velocity cases. For shorter intervals, the
deviation as well. The value of mixing efficiency without magnetic MNPs are dominated by the magnetic field and more volume of MNPs
actuation is only 69.5% which is obtained with the steady-state con- would accumulate around the microcoils. After reaching the so-called
dition without any magnetic body force. This clearly indicates that the steady state, i.e. approximately 12 s, the fluid inertia forces the MNPs to
mixing due to molecular diffusion suffers severely from inhomogeneous move away from the microcoils and the MNPs are able to disperse in the
concentration profile. As can be seen in Fig. 7, fluctuations in the lateral direction. Therefore, the mixing efficiency experiences a steep
mixing efficiency directly corresponds to the signal frequency, i.e. the increase for u 0 = 100µm/s . Moreover, from Fig. 8b it is seen that this
mixing efficiency oscillates approximately in one second for f = 1Hz inlet velocity can provide a more uniform concentration at the outlet.
and so on. By analyzing the data of the normalized concentration and Thus, inlet velocity equal to 100µm/s is selected as the best value for our
the mixing efficiency, it is concluded that two probable cases are able to model.
provide highest mixing performance: I0 = 0.5A, f = 1Hz, and
I0 = 1A, f = 5Hz . From Fig. 7a, a mixing efficiency within the range D Velocity ratio
83%–94% is seen for the former case, while this range is around
u
88%∼90% for the latter case, as can be seen from Fig. 7b. Thus, the The effect of relative inlet velocity, i.e. ff where uff and u w are the
uw
latter case, i.e. I0 = 1A, f = 5Hz , is chosen as the suitable condition for inlet velocities of the ferrofluid and DI waters, respectively, is shown in
the magnetic field due to its smaller fluctuation band. These values of Fig. 9. Higher ferrofluid inlet velocity strongly weakens the mixing
peak current and frequency are kept constant to investigate the effect of performance of the system to the extent that the mixing efficiency falls
inlet velocity in the next section. less than that without any magnetic field. This observation can be ex-
plained by the MNPs residence time. At higher velocity ratios, the
C Inlet velocity ferrofluid nanoparticles do not have enough residence time to properly
absorb the magnetic field and thus provide agitation. In other words,
The effect of inlet velocity on the mixing efficiency is depicted in the inertia of the ferrofluid stream drives the MNPs to flow and this
Fig. 8a. As was expected, the MNPs at higher inlet velocities are not prevents the ferrofluid to move in lateral direction and thus improve the
able to properly absorb the magnetic force even at a relatively high mixing efficiency. Therefore, the normalized concentration remains
switching frequency, i.e. 5 Hz. For higher inlet velocities, the fluid in- parabolic and the streams remain unmixed, as can be concluded from
ertia dominates the magnetic field induction and compromises the Fig. 9b. However, it is seen that the mixing efficiency is higher for
mixing performance of the design. It is seen that the more the flow rate
uff uff
uw
= 0.8 rather than u = 0.5, which is expected to have higher mixing
and the inlet velocity are, the less the mixing efficiency becomes, as was
w
efficiency due to the extended residence time of the ferrofluid stream.
reported by Zhu et al. [1]. For u 0 = 100µm/s , the mixing efficiency is This observation can be justified by the amount of ferrofluid that is
less for approximately 10 s, while in the long run, this value will always near the microcoils and the net amount of ferrofluid that is
6
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
uff
the averaged normalized ferrofluid concentration for uw
= 0.8 is 0.346
uff uff
while this value is 0.301 for u = 0.5. Therefore, u = 0.8 is selected as
w w
the preferred value for the velocity ratio, which provides 94% of mixing
efficiency.
E Duty cycle
4. Conclusion
7
M. Saadat, et al. Chemical Engineering & Processing: Process Intensification 147 (2020) 107727
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