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https://doi.org/10.1007/s10404-019-2306-y
RESEARCH PAPER
Received: 1 August 2019 / Accepted: 12 November 2019 / Published online: 21 November 2019
© Springer-Verlag GmbH Germany, part of Springer Nature 2019
Abstract
We present a flexible and noninvasive approach for efficient continuous micromixing and microreaction based on direct
current-induced thermal buoyancy convection in a single microfluidic unit. Theoretically, microfluids in this microsystem are
unevenly heated by powering the asymmetrically arranged microheater. The thermal buoyancy convection is then formed to
induce microvortices that cause effective fluidic interface disturbance, thereby promoting the diffusion and convective mass
transfer. The temperature distribution and the convection flow in the microchip are first characterized and studied, which can
be flexibly adjusted by changing the DC voltage. Then the mixing performance of the presented method is validated by joint
numerical and experimental analyses. Specifically, at U = 7 V, the mixing efficiencies are higher than 90% as the flow rate
is lower than Qv= 600 nL/s. So high-quality chemical or biochemical reactions needing both suitable heating and efficient
mixing can be achieved using this method. Finally, as one example, we use this method to synthesize nano-sized cuprous
oxide (Cu2O) particles by effectively mixing the Benedict’s solution and glucose buffer. Remarkably, the particle size can
be tuned by changing the voltage and the concentration of Benedict’s solution. Therefore, this micromixer can be attractive
for diverse applications needing homogeneous sample mixtures.
Keywords Continuous microfluid mixing · Thermal buoyancy convection · Cuprous oxide particles · Particle synthesis
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2 Theoretical background The heat transfer in fluids meets the liquid heat transfer
equation,
The fluids in microchannel will be unevenly heated when ( )
𝜕T
the asymmetical microheater is powered. Since the physi- 𝜌0 cp + u ⋅ ∇T − ∇ ⋅ (kf ∇T) = 0 (6)
𝜕t
cal parameters of fluids (e.g., density and viscosity) are all
temperature-dependent, there will be a density difference where, 𝜌0 is the density, cp the heat capacity, kf the thermal
in the unevenly heated microfluids. Then the fluids will conductivity.
be driven by the density difference-induced force (buoy- At the interfaces of different materials, the temperature
ancy force). Finally a three-dimensional convection flow and the normal heat flux are continuous.
is formed in the fluids of interest. The convection flow- Since the microdevice is exposed to the air, the surface-
induced microvortices on cross-sections help to disturb the air satisfies,
fluidic interface and improve the convective mass transfer. ( )
𝜕T
The basic theories describing the heat and mass transfer in −k = h(Ts − Tr ) (7)
𝜕n s
this microdevice are as follows.
where, k is the thermal conductivity, h the convective heat
transfer coefficient, n the external normal line of the outer
2.1 Heat transfer surface of the microchip, Ts the temperature of the chip’s
surface, Tr the temperature of the surrounding air.
The heat in this microdevice comes from the Joule heat-
ing effect of the ITO-made microheater. The temperature
distribution of the microheater meets the heat-conduction 2.2 Mass transfer
differential equation with internal heat source,
The thermal buoyancy convection is governed by the
𝜕T
𝜌I cI = ∇ ⋅ (kI ∇T) + q (1) Navier–Stokes and the continuity equations
𝜕t
where, 𝜌I is the density of ITO film, cI the heat capacity, kI 𝜌0 (u ⋅ ∇)u = 𝜇(T)∇2 u − ∇p + F (8a)
the thermal conductivity, q the Joule heating source.
The Joule heating flux density q is related to the electric ∇⋅u=0 (8b)
current density and electric field intensity,
where, 𝜌0 is the fluid density at room temperature T0 , 𝜇(T)
q = J⋅ E = 𝜎 ⋅ |∇𝜙| 2
(2) the dynamic viscosity at temperature T, p the pressure, F the
buoyancy force, F = −g[𝜌0 − 𝜌(T)] ≈ −g𝜌0 𝛽T (T − T0 )(𝜌(T)
where, q is the Joule heat flux density, J the electric current the fluid density at temperature T, 𝛽T the thermal expansion
density, E the electric field intensity, σ the conductivity of coefficient).
ITO film. 𝜙 the electric potential. At fluid–wall interfaces, the flow field meets the no-slip
The electric potential distribution of the microheater boundary condition: uwall = 0.
meets the Laplace’s equation. The concentration of samples meets the convective-dif-
fusion equation,
∇ ⋅ (𝜎E) = −𝜎∇2 𝜙 = 0 (3)
𝜕c
At the microheater’s surface, the electric current density + (u ⋅ ∇)c = ∇ ⋅ [D(T)∇c] (9)
𝜕t
J meets the following equation,
where, c is the concentration of species, D(T) the diffusion
J⋅n=0 (4) coefficient at the temperature T.
where, n is the unit normal vector. The dimensionless convective-diffusion equation can be
As for the glass substrate and PDMS channel, their tem- given by
perature distributions satisfy the unsteady-state heat-con- 𝜕c∗ 1 2 ∗
duction differential equation without internal heat source, + (u∗ ⋅ ∇)c∗ = ∇c (10)
𝜕t∗ Pe
𝜌gp cgp
𝜕T
= ∇ ⋅ (kgp ∇T) (5) where Pe(T) = UL
D(T)
is the Peclet number, which represents
𝜕t the ratio of convection effect-to-molecular diffusion. U is the
where, 𝜌gp is the density, cgp the heat capacity, kgp the thermal characteristic convection rate, L the characteristic size of
conductivity. microchannel, D(T) the diffusion coefficient at temperature
T.
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At the surfaces, inlets and outlet of the microchannel, the also be prepared by the following process. First, 85 grams of
concentration field meets the following boundary conditions, sodium citrate and 50 grams of anhydrous sodium carbonate
are dissolved in 400 mL of deionized water. Then 8.5 grams
⎧ 0 Inlet1 of anhydrous copper sulfate is added to 50 mL of hot water.
⎪
⎨ 1 Inlet2 (11) Finally, the Benedict’s solution is obtained by mixing the
⎪ n ⋅ ∇c = 0 Wall,Outlet solutions prepared in the first two steps. The concentration
⎩
of glucose buffer used in experiments is 0.2 M. The syn-
where, n is the unit normal vector of channel walls and thesized particles are visualized using a scanning electron
outlet. microscope (SU-8010, Hitachi, Japan).
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Fig. 2 a–bTemperature distributions on the xy-plane (z = 0 μm) (a) e The temperature difference (Th(x)− Tc(x)) (marked in Fig. 2a) along
and the I–I, II–II, and III–III cross-sections (marked in Fig. 2a) b at the channel length under different voltages when the flow rate Qv
U = 6 V and Qv = 300 nL/s. c Flow fields on the I–I, II–II, and III–III is 300 nL/s. f The average transverse convection velocity along the
cross sections at U = 6 V and Qv = 300 nL/s. (d) The current–voltage channel length under different voltages when the flow rate Qv is 300
and the maximum temperature Tm-voltage curves of the microheater. nL/s
Figure 2e shows the plots of temperature difference strongly temperature-dependent, so the temperature of fluid
Th(x)− Tc(x) (Th(x) and Tc(x) are marked in Fig. 2a) versus chan- can be determined according to the relationship between
nel length L at different DC voltages. It is observed that the local temperature and florescent intensity of the 0.1 mM
Th(x)− Tc(x) decreases along the channel length, whereas, it Rhodamine B solution (Zhao et al. 2013).
can be treated as a constant when L is smaller than 6 mm.
Moreover, Th(x)− Tc(x) increases as the voltage rises, and it T(K) = [A0 + A1 S(T) + A2 S2 (T) + A3 S3 (T)](K) (12)
can reach 11 K at U = 8 V. Figure 2f depicts the relation-
where S(T) = I(T)/IRT is the dimensionless fluorescent inten-
ships between the average transverse convection velocity
sity, I(T) the fluorescent intensity at temperature T, IRT the
(average|uy|) and the channel length under different voltages
fluorescent intensity at room temperature (293.15 K). The
and the fixed flow rate of 300 nL/s. Although the average|uy|
fitting parameters in Eq. (12) are determined by measuring
varies with the channel length, the difference is very small
the fluorescent intensities of 0.1 mM Rhodamine B solution
and can be neglected. And also, the average|uy| is positively
at various temperatures (Fig. 3a). Specifically, A0 = 387.81,
affected by the increased DC voltage. Specifically, the
A1 = −246.58, A2 = 264.17, A3 = −112.25.
average transverse convection velocity increases from 0 to
0.1 mM Rhodamine B solutions are simultaneously
480 μm/s as the DC voltage rise from 0 to 8 V. This can be
injected into the main channel of the micromixers through
explained that the temperature difference positively depends
two separate inlets. The distributions of fluorescent intensity
on the DC voltage (Fig. 2e), and the increased temperature
under different DC voltages are obtained through a fluores-
induces more intensive buoyancy flow (Eq. 8a). Therefore,
cence microscope (IX73, Olympus, Japan) with a CMOS
the buoyancy-flow-induced micromixing process can be con-
camera (Prime 95B) and an image J software. Finally,
trolled by the DC voltage.
the average (Th− Tc) and Tm (Th, Tc, and Tm are marked
To experimentally determine the temperature distribution
in Fig. 2a) can be calculated using Eq. (12). As shown in
of the fluid–substrate interface and validate the accuracy of
Fig. 3b, the experimental temperatures and temperature dif-
numerical analyses, a kind of thermometry based on tem-
ferences match well with the numerical results, proving the
perature-dependent fluorescent intensity is used in this work.
accuracy of above numerical analyses.
That is, the fluorescent intensity of Rhodamine B solution is
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Fig. 4 a Simulated concentration distribution when power is off at centration distribution at U = 6 V and Qv= 900 nL/s. b1 exhibits the
Qv= 900 nL/s. a1 exhibits the concentration distribution on xy-plane. concentration distribution on xy-plane. b2–b4 show the concentration
a2–a4 show the concentration distributions on the I–I, II–II, and III– distributions on the I–I, II–II, and III–III section, respectively. b5–b7
III section, respectively. a5–a7 display the concentration gradient display the concentration gradient on I–I, II–II, and III–III section,
on the I–I, II–II, and III–III section, respectively. b Simulated con- respectively
Then we adjust the electrode displacement w5 (marked shown in Fig. 5b, when the DC voltage and flow rate are
in Fig. 1b), the distance between the upper edge of the fixed at 6 V and 300 nL/s, respectively, the mixing efficiency
electrode and the upper side of main channel, to study the decreases from 98.4 to 86.0% as the electrode displacement
influence of electrode position on mixing performance. As w5 increases from 0 to 1 mm. This negative relationship
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Fig. 5 a Mixing efficiencies and average transverse convection veloc- ing efficiencies of the final design under different voltages at Qv= 300
ities under different electrode widths at P = 0.72 W and Qv= 300 nL/s. nL/s. e Mixing efficiencies of the final design under different flow
b Mixing efficiencies and average transverse convection velocities rates at U = 6 V. Velocity ratio refers to the ratio of average transverse
under different electrode displacements at U = 6 V and Qv= 300 nL/s. velocity to the average axial velocity. f Mixing efficiencies under dif-
c Mixing efficiencies and average transverse convection velocities ferent viscosities at U = 6 V and Qv= 300 nL/s
under different channel heights at U = 6 V and Qv= 900 nL/s. d Mix-
is due to the fact that the temperature difference decreases on the mixing performance are studied. Figure 5d shows the
and the vortex changes from a vortex crossing the whole mixing efficiencies of the chip under different DC voltages
section to a counter-rotating vortex pair as the electrode dis- at Qv = 300 nL/s. It can be seen that the mixing efficiency
placement rises. Similar to above analyses, the decreased has a positive relationship with the applied voltage. And the
temperature difference and the changed vortex pattern both mixing efficiency can reach as high as 99.1% at U = 8 V and
negatively influence the mixing efficiency. Therefore, the Qv = 300 nL/s. Since the increased flow rate will decrease
final electrode displacement is set as 0 mm based on this the working time and the relative intensity of transverse con-
numerical result. vection flow, the mixing efficiency decreases as the flow rate
The effect of channel height on the mixing efficiency is rises (Fig. 5e). And compared with the mixing efficiency
further analyzed. As shown in Fig. 5c, the mixing efficiency at Qv = 300 nL/s, the result at Qv = 900 nL/s decreases by
is positively influenced by the channel height. Specifically, 12.6%. Finally, we analyze the effect of fluid viscosity on
at the fixed voltage of 6 V and the constant flow rate of mixing performance. As shown in Fig. 5f, the mixing per-
900 nL/s, the mixing efficiency increases by 163.5% (from formance is negatively affected by the fluid viscosity. The
37.3 to 98.3%) as the channel height rises from 0.5 to 3 mm. mixing efficiency decreases from 98.4 to 52.2% when the
This result can be explained that the magnitude of buoy- fluid viscosity rises from 1 to 8 mPa s. This phenomenon
ancy force acting on whole fluid is proportional the cube of is due to the fact that the fluid viscosity will decrease the
the characteristic size of microchannel. And the buoyancy intensity of convection flow. So the convective mass transfer
force positively affects the intensity of thermal buoyancy process can be weakened by the increased fluid viscosity.
convection (Zhang et al. 2019). In previous micromixing
studies, the homogeneous concentration distribution pro- 4.2 Experimental validation
files obtained from the top view of the chip can be used
to represent the excellent mixing state of the whole fluid Besides the numerical analyses, we also perform system-
only when the aspect ratio of microchannel is no less than atic micromixing experiments by injecting deionized (DI)
3 (Chen and Yang 2007; Loucaides et al. 2012; Ng et al. water and fluorescent buffer (fluorescence dissolved in DI
2009). Therefore, the channel width and height are set as water) into the main channel through two separate inlets.
3 mm and 1 mm, respectively. Figure 6a–c shows the concentration distribution profiles
When the dimension parameters of the chip are deter- under different voltages. Specifically, an unmixed laminar
mined, the influences of DC voltage and fluid parameters flow state at Qv = 300 nL/s is observed when power is off
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Fig. 6 a–c Concentration distribution profiles under different voltages at Qv= 300 nL/s. d Normalized fluorescent intensities across the channel
width at L(x) = 6 mm
(Fig. 6a). Whereas, the homogeneous mixing of DI water shows the concentration distribution profiles at three flow
and fluorescein is achieved when the microheater is pow- rates and the fixed DC voltage of 6 V. The mixing length
ered. Importantly, compared with the result at U = 4 V used for thorough fluid mixing increases with the rising flow
(shown in Fig. 6b), a shorter mixing length is needed at rates. Figure 7b indicates the plots of mixing efficiency ver-
a higher voltage (Fig. 6c). To quantify the mixing perfor- sus channel length under three flow rates and the fixed volt-
mance, the cross-sectional dye concentration profiles (the age of 6 V. It can be seen that the mixing efficiency increases
dashed lines in Fig. 6) are plotted by measuring the gray with the channel length. This phenomenon can be explained
value of the experimental images. As shown in Fig. 6d, the that the working time of transverse convection flow improves
normalized intensities of the unmixed fluids are 0 for deion- as the channel length rises. Importantly, the mixing perfor-
ized water and 1 for the dyed solution. When the microheater mance can reach 93.4%, a highly efficient mixing state, at
is powered by a 6-V DC voltage, the normalized fluorescent Qv = 300 nL/s and L = 6 mm. Figure 7c exhibits the varia-
intensity is uniform across the microchannel width. tions of mixing efficiency with DC voltage under three flow
According to the quantitative index of mixing efficiency rates and the fixed channel length of 6 mm (See Movie S1
(Eq. 13), we first study the effects of the DC voltage and flow in the Supporting Information). Since the intensity of ther-
rate on the mixing performance of water solution. Figure 7a mal buoyancy convection increases with the rising voltage,
Fig. 7 a Concentration distribution profiles under different flow rates d Mixing efficiencies under different flow rates at U = 6 V and
at U = 6 V. b Mixing efficiencies under different channel lengths at L(x) = 6 mm. e Mixing performances of absolute ethanol under differ-
U = 6 V. c Mixing efficiencies under different voltages at L(x) = 6 mm. ent DC voltages at L(x) = 6 mm
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the DC voltage has a positive influence on the mixing effi- During the experimental process, the standard Benedict’s
ciency. Concretely, at a fixed flow rate of 300 nL/s, the mix- solution and glucose buffer with a concentration of 0.2 M are
ing efficiency improves from 13.5 to 97.3% as the voltage simultaneously injected into the main channel. And the volume
ranges from 0 to 8 V. Figure 7 d shows the experimental and flow rate in the main channel is 300 nL/s. Then these two fluids
numerical mixing efficiencies at different flow rates and a are effectively mixed by the transverse convection flow. Mean-
fixed DC voltage of 6 V. The flow rate negatively affects the time, the reaction between the Benedict’s solution and glucose
mixing of water solution and fluorescent dye. Specifically, buffer is triggered by the elevated fluid temperature. Figure 8
the mixing performance decreases from 93.4 to 74.4% as b–c exhibit the SEM images of synthesized C u2O particles
the flow rate rises from 300 to 900 nL/s. This is owing to at U = 5 V (Fig. 8b) and 8 V (Fig. 8c), respectively. It can be
the fact that the working time and the relative intensity of seen that the synthesized Cu2O particles are all cubic. The
transverse convection flow decrease with the increased flow particle size distributions at these two different voltages are
rate. Additionally, the experimental and numerical results given in Fig. 8d. Specifically, the average size and the stand-
have a good agreement with each other, demonstrating the ard deviation of particle size at U = 5 V are 0.967 μm and
accuracy of our numerical analyses. 0.12 μm, respectively. However, the synthesized particles are
Besides the mixing of water solution, we further use the much smaller and more uniform at U = 8 V since the average
insulating absolute ethanol as an experimental sample to size and the standard deviation of particle size, respectively,
study the applicability of designed chip on the mixing of decrease to 0.680 μm and 0.09 μm. The influence of DC volt-
insulating fluids. During the experimental process, one solu- age on particle size is further exhibited in Fig. 8e. It is shown
tion is absolute ethanol, the other is fluorescently labeled that the particle size is negatively affected by DC voltage. The
absolute ethanol. Figure 7e shows the variations of mix- particle size decreases by 29.7% as the DC voltage rises from
ing efficiency of absolute ethanol with DC voltage at three 5 to 8 V.
flow rates. It can be seen that the DC voltage also positively Furthermore, we investigate the effect of the concentration
affects the mixing states of ethanol. And the absolute ethanol of Benedict’s solution on particle size. During the experimen-
can reach a highly effective mixing state (Me = 90.8%) at tal process, the DC voltage and the concentration of glucose
U = 6 V and Qv = 300 nL/s. This experiment demonstrates buffer are fixed at 7 V and 0.2 M, respectively. As for the
that the presented design can be used for the mixing of both Benedict’s solution, it is diluted using deionized water, and the
conducting and insulating buffers. Therefore, compared with dilution ratio ranges from 1 to 8. The particle images under dif-
the commonly used electrokinetic micromixing devices rely- ferent dilution ratios are exhibited in Fig. 9a–c. It is observed
ing on the conductivity of buffer solution (Cao et al. 2007; that the dilution ratio negatively affects the particle size.
Jain et al. 2009; Sugioka 2010), the presented method can be According to the statistical result given in Fig. 9d, the particle
used in a broader range of on-chip applications. size declines from 0.793 to 0.477 μm when the dilution ratio
changes from 1 to 8. On the basis of above analyses, the par-
5 Nano‑sized Cu2O particle synthesis ticle size can be flexibly tuned by changing the DC voltage
and the concentration of Benedict’s solution. And this particle
Cu2O is a kind of semiconductor material, which has a good synthesis experiment successfully proves the feasibility of the
absorption characteristic to visible light, and the theoretical presented approach in efficient micromixing and simultane-
energy conversion rate can be as high as 14– 20% (Akimoto ous microreaction. Moreover, compared with the synthesis
et al. 2006; Nian et al. 2008). So the Cu2O has been widely experiments of C u2O in traditional labs (Dong et al. 2001;
used in solar cells, photo-catalytic degradation of organic pol- Huang et al. 2009), our microfluidic platform is simple and
lutants, photohydrolysis of water for hydrogen, and gas sen- flexible, and the synthesis period is shortened a lot. Therefore,
sors (Kim et al. 2013; Kwon et al. 2015; Lee et al. 2011). this fluid mixing and particle synthesis method is attractive in
To demonstrate the applicability of this thermal microreactor diverse applications including biochemical analysis, material
on material synthesis, Cu2O particles are tried to synthesize synthesis, and so on.
by rapidly and efficiently mixing the Benedict’s solution and
glucose buffer. The synthesis mechanism of C u2O particles is
shown in Fig. 8a and Eqs. (14) and (15). 6 Conclusion
Cu2+ + 2OH− → Cu(OH)2 (14) In this paper, we present a novel method for efficient con-
tinuous microfluid mixing and microreaction based on direct
CH2 OH(CHOH)4 CHO + 2Cu(OH)2 current-induced thermal buoyancy convection in a single
microfluidic unit. The fluids of interest are unevenly heated
⟶ ΔCH2 OH(CHOH)4 COOH + 2H2 O + Cu2 O ↓ (15) using an asymmetrically arranged ITO-made microheater,
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Microfluidics and Nanofluidics (2020) 24:1 Page 11 of 14 1
leading to the formation of thermal buoyancy convection. this design’s capability for simultaneously conducting reac-
Microfluids then can be effectively mixed by the convection tions, nano-sized C u2O microparticles are synthesized by
flow-induced microvortices. The temperature distribution effectively mixing the Benedict’s solution and glucose buffer
and the natural convection flow in the microchip are first in this microdevice. Remarkably, the particle size can be
studied and characterized, which can be flexibly adjusted by tuned by changing the DC voltage and the concentration of
changing the DC voltage. Then the mixing performance of Benedict’s solution. The particle size decreases from 0.967
the presented micromixer is investigated by joint numerical to 0.680 μm as the DC voltage rises from 5 to 8 V. When the
and experimental analyses. The DC voltage positively affects DC voltage and the concentration of glucose buffer are fixed
the mixing performance. However, the flow rate has a nega- at 7 V and 0.2 M, respectively, the particle size declines
tive effect on mixing efficiency. Specifically, at a fixed flow from 0.793 to 0.477 μm as the dilution ratio of Benedict’s
rate of 300 nL/s, the mixing efficiency improves from 13.5 solution improves from 1 to 8. Therefore, this thermal-based
to 97.3% as the voltage ranges from 0 to 8 V. And the mixing micromixer can be attractive for diverse applications because
performance decreases from 93.4 to 74.4% as the flow rate of its simplicity, high throughput and flexibility.
rises from 300 to 900 nL/s at U = 6 V. Finally, to demonstrate
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Acknowledgements This work is financially supported by the National Cui W et al (2016) Localized ultrahigh frequency acoustic fields
Natural Science Foundation of China (No.11672095, No.11872165, induced micro-vortices for submilliseconds microfluidic mixing.
No. 11702075, No. 11702035). Self-Planned Task (SKLRS201803B) Appl Phys Lett 109:253503. https://doi.org/10.1063/1.4972484
of State Key Laboratory of Robotics and System (HIT). Deng Y, Zhou T, Liu Z, Wu Y, Qian S, Korvink JG (2018) Topology
optimization of electrode patterns for electroosmotic micromixer.
Int J Heat Mass Transf 126:1299–1315. https://doi.org/10.1016/j.
ijheatmasstransfer.2018.06.065
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