RESEARCH PAPER
Experimental study of microbubble coalescence in a T-junctionmicrofluidic device
Lu Yang • Kai Wang • Jing Tan • Yangcheng Lu •
Guangsheng Luo
Received: 7 August 2011 / Accepted: 9 November 2011 / Published online: 29 November 2011
� Springer-Verlag 2011
Abstract This study presents the microbubble coalescence
process in a confined microchannel. Triple T-junction
microfluidic devices with different main channel size were
designed to generate monodispersed microbubble pairs with
air/n-butyl alcohol–glycerol solution as the working system.
The head-on collision of microbubble pair was realized in the
microfluidic devices. Three collision results including
absolute coalescence, probabilistic coalescence, and non-
coalescence were distinguished. The effects of liquid vis-
cosities and two-phase superficial velocities on the coales-
cence behavior were determined. The results showed that
microbubble coalescence process in the confined space was
slightly faster than in the free space. Increasing liquid vis-
cosity apparently prevents coalescence. In the probabilistic
coalescence region, higher two-phase superficial velocity
could reduce the percentage of coalescence events. Two
characteristic parameters representing the bubble contact
time and film drainage time have been introduced to analyze
the microbubble coalescence behaviors and a linear corre-
lation could clearly distinguish the coalescence and non-
coalescence region.
Keywords Microfluidic � Microbubble �Head-on collision � Coalescence
1 Introduction
Microfluidic technology has been widely applied in many
research areas, such as analysis, chemical synthesis,
separation, material preparation, and biological engineer-
ing (Huebner et al. 2008; Song et al. 2006). These appli-
cations are attributed to the advantages of microfluidic
devices, where monodispersed microdroplets or micro-
bubbles can be controllably prepared and manipulated,
with enhancement of mass and heat transfer due to the
large specific surface area (Baroud et al. 2010; Teh et al.
2008; Gordillo et al. 2004). Gas/liquid system is one of
most important systems in scientific and industrial appli-
cations including chemistry, food, environment, and phar-
maceutical process. Combining the advantages of
microfluidic technology, a number of gas/liquid processes
involving reaction and mass transfer have been realized in
microfluidic device and developed rapidly during recent
years (Leclerc et al. 2008; Su et al. 2010). However, bubble
coalescence is a common phenomenon in the above prac-
tical applications. For the controllable use of gas/liquid
microfluidic system, the gas phase is sometimes required to
be stably dispersed in the liquid phase to keep good mixing
condition (coalescence need to be prevented), and some-
times efficient coalescence is desirable to enhance the
phase separation (coalescence is favorable). It can be seen
that a lack of control over the bubble coalescence would
severely limit their usefulness. Therefore, it is essential to
understand the fundamental fluid dynamics of microbubble
coalescence and to further realize effective control of
coalescence process.
The investigation of bubble coalescence behavior under
the general conditions has a long history and many
experimental and theoretical analyses have been carried out
to study the coalescence mechanisms, effect factors, and
coalescence models (Liao and Lucas 2010; Lessard and
Zieminski 1971; Stover et al. 1997). Several experimental
studies have been conducted and various methods have
been designed to observe the coalescence process between
L. Yang � K. Wang � J. Tan � Y. Lu � G. Luo (&)
The State Key Laboratory of Chemical Engineering,
Department of Chemical Engineering,
Tsinghua University, Beijing 100084, China
e-mail: [email protected]
123
Microfluid Nanofluid (2012) 12:715–722
DOI 10.1007/s10404-011-0912-4
bubble pairs. For example, Tsang et al. (2004) studied the
effect of electrolyte concentration on the bubble coales-
cence with adjacent capillaries. A critical electrolyte con-
centration, whose value increased with decreasing bubble
diameter from 4.2 to 1.4 mm, was found in their work. Ata
et al. (2010) observed the pH-induced coalescence of 2 mm
contacted air bubbles with parallel capillaries. A pH sen-
sitive latex was introduced to control the coalescence by
adjusting the latex structure on bubble surface. Martin et al.
(2007) investigated the bubble coalescence on sieve plates
with pore diameters varying from 1.5 to 2.5 mm and the
distance between two neighboring holes was controlled.
Kazakis et al. (2008) focused on the effect of liquid
properties and operating conditions on the bubble interac-
tion by using two adjacent micro-tubes and a porous
sparger. Their experimental results enhanced the compre-
hension of coalescence mechanism in the bubble genera-
tion (bubble diameter *1 mm). Tse et al. (1998) observed
the stages of coalescence process between two bubbles
formed in a stirred tank, where the bubbles get close and
contact each other under the action of buoyancy. In addi-
tion, some researchers also focus on the interaction and
force between coalesced bubbles from microcosmic point
of view and determined the coalescence conditions and
mechanisms by using atomic force microscope (Vakarelski
et al. 2010). Besides experimental researches, theoretical
studies have also been developed to understand the coa-
lescence phenomenon. Liao and Lucas (2010) reviewed
several theoretical models for bubble and droplet coales-
cence process including collision frequency and coales-
cence efficiency. Among those models, the film drainage
model is the most widely used, which describes the coa-
lescence efficiency with two time scales, i.e. the contact
time and the drainage time (the time required for the liquid
film to thin down to a critical thickness). This model states
that coalescence occurs when the liquid film ruptures
before bubbles separate.
According to the previous studies on bubble coalescence
process, researchers paid more attention to the ideal,
stagnant, and millimeter-sized bubbles in free spaces. In
contrast, few studies focus on the coalescence process of
microbubbles which flow in confined microchannels.
Therefore, it is valuable to explore the microbubble coa-
lescence in microfluidic device. In our previous works, the
generation of microbubbles has been investigated in
T-junction microfluidic devices with cross-flow and per-
pendicular-flow shearing methods (Tan et al. 2009; Wang
et al. 2011; Xu et al. 2006a, b). In this work, we used the
T-junction microfluidic device to give an in-depth study on
the coalescence behavior of microbubbles. Based on the
fusion studies of microdroplets in microchannels (Chris-
topher et al. 2009; Zhao and Middelberg 2011), the head-
on collision of fluid particles is a simple method to realize
coalescence of microdroplets in solutions. This method was
introduced into our experiment and coalescence process of
flowing microbubbles in confined T-junction microchannel
devices was investigated. The effects of liquid viscosity
and two-phase superficial velocity were carefully examined
and the fluid dynamic conditions of bubble coalescence
were analyzed based on the experimental results. To our
knowledge, the microbubble coalescence behavior in con-
fined microchannel space has not been reported.
2 Experimental section
2.1 Microfluidic device
A schematic figure of the microfluidic chip is shown in
Fig. 1. Two perpendicular rupture generators are used in
this device with T-shaped structure, and their section
width and height are 0.4 and 0.36 mm, respectively. The
main channel has a square section whose height and
width equal to 0.6 mm. The narrower side T-junctions
were designed to use the sudden expansion structure to
generate microbubbles, and the produced bubbles can be
more stable and well monodispersed. The advantages of
this perpendicular flow shearing method have been proved
by our previous work (Tan et al. 2009). For comparison,
another microfluidic device with main channel dimension
of 0.8 mm 9 0.8 mm and narrower channel dimension of
0.5 mm 9 0.48 mm was also used to study the micro-
bubble coalescence process in microchannel with different
widths. Microbubbles were generated in these specially
designed microfluidic devices and head-on collision of
microbubbles was realized at the T-shaped meeting
junction, as shown in Fig. 1. The microfluidic device was
fabricated on a polymethyl methacrylate (PMMA) plate
by precision milling, and sealed with another PMMA
plate by use of a high-pressure thermal sealing machine
(A274, Techson) at 0.4 MPa, 70�C.
Fig. 1 Schematic figure of microdevice, microbubbles generated
with perpendicular rupture method and then collided at meeting
junction
716 Microfluid Nanofluid (2012) 12:715–722
123
2.2 Operation and observation
Figure 2 shows the experimental set up. Experiments were
carried out with a microscope, which equipped with a high-
speed CCD camera (DK-2740, Dantec Dynamics) and set
over the microchannel chip. The collision processes of
microbubbles at the meeting junction were recorded with a
frame frequency of 2,500 fps. An optical-fiber light source
was placed on the bottom of the chip to illuminate the
microchannel. Both gas and liquid phases were delivered
and controlled by syringe pumps (LSP01-1A, Longer) with
gastight syringes. In the experiments, the gas phase was
pumped into the microchannel firstly and then the liquid
phase followed. After changing any operating conditions,
at least 2 min was allowed for the flows to reach stable
state. The gas flow rates (QG) were controlled at 50, 80,
100, 150, 160 lL/min, and the liquid flow rates (QL) were
varied from 120 to 800 lL/min. The average diameters of
generated bubbles were in the range of 362–543 and
492–626 lm, when using the microchannel with main
channel width of 0.6 and 0.8 mm, respectively. The poly-
dispersity index of bubble diameters at every operating
condition, which is defined as the ratio of the relative
deviation of bubble size to the average bubble diameter,
was less than 3%, so it indicates the microbubbles are
highly uniform (Xu et al. 2006a). Flows of both phases
were consistent in the two generators for equal-sized
bubbles in collision. In order to eliminate timing difference
between the arrivals of two bubbles at the meeting junc-
tion, the synchronization of the generators were strictly
controlled and all the results in this paper were chosen from
the tests that the head-on collision were taken place at the
meeting junction. At least 15 tests were repeated for one
operating condition to give parallel experimental results.
2.3 Working systems
Air and n-butyl alcohol solutions were introduced to form
the working systems in this work. Different concentrations
of glycerol (0, 7, 10, 15 and 20 wt%) were added into butyl
alcohol for varying the liquid phase viscosities. Analyti-
cally pure n-butyl alcohol and glycerol (C99.0%) used in
the experiment were provided from Beijing Chemical
Plant. The viscosities of the liquid phases were measured
with an Ubbelohde viscometer and the surface tension of
the working systems was measured by a pendent drop
interfacial tension meter (OCAH200, DataPhysics Instru-
ments GmbH) at 25�C. The physical properties of the
working systems are listed in Table 1.
3 Results and discussion
3.1 Observation of microbubble coalescence processes
Figure 3 shows a typical microbubble coalescence process
in the microchannel. The result shows the coalescence
process proceeds quickly at millisecond time scale in the
meeting junction, which can be divided into three distinct
stages. In the first stage, the opposite flowing bubbles
approach and contact each other forming a thin liquid film
between bubble surfaces, which has a typical thickness of
several micrometers (Ata et al. 2010). The second stage is
film thinning or drainage. With the drainage of liquid film,
the film thickness is gradually reduced. Thinning of the
film is primarily driven by capillary force which is sig-
nificantly affected by the physical properties. When the
film thickness reduces to about 100 nm, Van der Waals
attraction will accelerate the drainage process (Almatrou-
shi and Borhan 2006). Once the liquid film is thinning less
than a critical thickness (a few tens of nanometers) (Horn
et al. 2011), film rupture occurs instantaneously leading to
the bubble coalescence as the third stage. Following bub-
ble fusion process, the surface of coalesced bubble shows
strong oscillations due to the release of surface energy. The
bubble expands in the horizontal and vertical orientations
alternately (Ata et al. 2010), and then contracts to sphere.
The stages of microbubble coalescence almost are the
same as previous studies from a microcosmic aspect, but
the time scales are different. Figure 3 shows the time scale
for the microbubble coalescence in the confined space is
only within 1.6 ms. Comparing with the bubble coales-
cence in free space, where time scale for coalescence is
usually longer than 10 ms (Ata et al. 2010; Tse et al.
1998), the coalescence process of microbubble in the
confined space is slightly faster. It can be attributed to the
effects of small bubble size and microchannel confinement.
Because the small bubbles will result in the small diameter
of liquid film between two bubbles and it can reduce the
coalescence time. In addition, the channel wall will play an
important role in this process due to the microbubbles are
confined in microchannel. Especially at the meeting junc-
tion microchannel wall can push bubbles together to
facilitate them coalescence. Of course, the role of the
channel wall should be studied in our further research.Fig. 2 Experimental set up
Microfluid Nanofluid (2012) 12:715–722 717
123
Moreover, the film-thinning step is generally believed to
be the rate-controlling step in the coalescence process
(Almatroushi and Borhan 2006), so here the film-thinning
stage might be accelerated.
In contrast, we also observed bubble collision process
without coalescing, as shown in Fig. 4. At the meeting
junction, deformed bubbles lost their kinetic energy to
increase the surface energy with collision. For these bubble
pairs, the thin liquid film formation and film drainage
stages are the same as coalesced bubble pair in Fig. 3.
However, without film rupture occurring, the microbubbles
eventually slip past one another near the junction with
recovery of surface energy and travel downstream in a pair.
This result is quite different from Fig. 3, since the film
drainage stage is not completed in this collision process.
From Figs. 3 and 4, it can be seen that the collision
results of microbubble between different working systems
or operation conditions are different indeed. For all the
experimental observations, it could be concluded that the
coalescence behaviors of microbubble pair can be classi-
fied into three primary categories: (1) absolute coalescence,
(2) probabilistic coalescence and (3) non-coalescence as
shown in Fig. 5. Absolute coalescence behavior is defined
as the coalescence being observed for all bubble pairs in
repeated tests for one operating condition. On the contrary,
non-coalescence behavior is defined as all bubble pairs
separating from each other in repeated tests. Between the
absolute coalescence and non-coalescence behaviors, a
transition region, where part of the repeated tests showed
coalescence behaviors, was observed with varying test
conditions. This behavior is named as probabilistic coa-
lescence since the occurrence of coalescence is random
with a certain coalescence probability.
3.2 Studies of influence factors on microbubble
coalescence process
3.2.1 Effect of liquid viscosities
The liquid viscosity (lc) plays an important role in the
microbubble coalescence process. In our experiments, five
continuous phases with different viscosities were used to
explore the effects of liquid viscosity on microbubble
coalescence. As shown in Table 1, the viscosities of the
liquid phases are ranged from 2.42 to 5.47 mPa s.
Although the viscosity variation is not in a very wide
range, the change of microbubble coalescence behavior is
obvious in the experiment. Figure 6 shows all the experi-
mental results of the five working systems at different flow
conditions. The horizontal axis is liquid phase viscosity,
and vertical axis is the two-phase superficial velocity uTP
which is defined as uTP = (QG ? QL)/a, where a is the
cross section area of the microchannel. It can be seen that
absolute coalescence behavior almost appears at liquid
viscosity less than 3.48 mPa s and non-coalescence
behavior of microbubbles at viscosity higher than
3.48 mPa s. The working system with lc = 3.48 mPa s
contains absolute coalescence and probabilistic coales-
cence behaviors for both microdevices, and the working
system with lc = 4.28 mPa s contains probabilistic coa-
lescence and non-coalescence behaviors only for mic-
rodevice with main channel width of 0.8 mm. Thus, a
transition region appeared in these working systems, and
microbubble becoming less likely to coalesce with
increasing liquid viscosity.
As mentioned before, the theoretical studies on coales-
cence process (Liao and Lucas 2010) pointed out that the
Table 1 Physical properties at
25�CDensity q (g/mL) Surface tension c (mN/m) Viscosity l (mPa s)
Air 1.185 9 10-3 1.83 9 10-2
1. n-butyl alcohol 0.8039 21.0 2.42
2. 7% glycerol solution 0.8241 22.1 3.05
3. 10% glycerol solution 0.8342 22.7 3.48
4. 15% glycerol solution 0.8504 23.1 4.28
5. 20% glycerol solution 0.8704 23.9 5.47
Fig. 3 The typical microbubble coalescence process in microfluidic
device (the main channel dimension is 0.6 mm 9 0.6 mm and the
working system is air/7 wt% glycerol–butyl alcohol solution with gas
flow rate at QG = 100 lL/min and liquid flow rate at QL = 250 lL/
min. The moment of bubble contact each other is identified as the zero
time and the numbers under the pictures give the proceeding time)
718 Microfluid Nanofluid (2012) 12:715–722
123
film drainage model is the most popular theoretical model.
It used the lubrication theory, which starts with the Navier
Stokes Equation and the continuity equation and derives a
thinning equation. The drainage time in the model can be
obtained by integrating the film thinning equation. This
model mainly concerned if the interface of bubbles is
deformable and mobile, and according to this, the detailed
forms of model are different. Even in confined space, the
bubble size is in microscales, which is much larger than
interfacial scale. Therefore, the film drainage model is a
fundamental theory and it can be thought to be still suitable
for confined space. According to the film drainage model,
the film drainage stage can be significantly affected by
liquid viscosity, so microbubble obeys a similar rule as the
bubble in millimeter scale. Due to the film drainage time
increase with the increase of liquid viscosity, and the
contact time is not enough for film drainage, therefore the
bubble coalescing become gradually difficult.
3.2.2 Effect of two-phase superficial velocities
The experimental results showed that the two-phase super-
ficial velocities could affect the coalescence behavior mostly
for the working system with lc = 3.48 mPa s and
lc = 4.28 mPa s at the transition region. Figure 6a and b
indicates that in the working system with lc = 3.48 mPa s
for both microdevices, the coalescence behavior transforms
from absolute coalescence to probabilistic coalescence with
the increase of the two phase superficial velocities up to 18.5
and 14.6 mm/s, respectively. These superficial velocities
Fig. 4 The typical process indicating microbubble pair collision without coalescing (the main channel dimension is 0.6 mm 9 0.6 mm and the
working system is air/20 wt% glycerol–butyl alcohol solution with gas flow rate at QG = 100 lL/min and liquid flow rate at QL = 250 lL/min)
Fig. 5 The primary categories
of microbubble coalescence
behaviors: 1 absolute
coalescence, 2 probabilistic
coalescence, and 3 non-
coalescence
Fig. 6 Effect of liquid viscosities on the coalescence behavior of
microbubbles in the T-junction microchannel. The symbol (opensquare) is representing absolute coalescence, open circle is
probabilistic coalescence, and open triangle is non-coalescence.
a The main channel dimension is 0.6 mm 9 0.6 mm; b The main
channel dimension is 0.8 mm 9 0.8 mm
Microfluid Nanofluid (2012) 12:715–722 719
123
correspond to the transition capillary numbers whose values
are Ca = 0.0028 and 0.0022 (Ca = lcuTP/c). From Fig. 6b,
it can be seen that especially in the working system with
lc = 4.28 mPa s for the microdevice with main channel
width w = 0.8 mm, the coalescence behavior transforms
from probabilistic coalescence to non-coalescence with the
increase of superficial velocity up to 10.4 mm/s, and it
corresponds to transition capillary number Ca = 0.0019.
These results mean that the higher superficial velocity does
not facilitate the microbubble coalescence.
It is notable that the transition region appeared when the
working system with lc = 3.48 mPa s was applied. The
results showed in this transition region the percentage of
coalescence events is influenced by two phase superficial
velocity seriously, as shown in Fig. 7a. The percentage of
coalescence events is defined as the ratio of the accumu-
lated coalescence events to the total head-on collision
events in more than 15 repeated tests for one operating
condition. It can be found the percentage of coalescence
decreases with the increase of the two phase superficial
velocity for all gas flow rate conditions in the experiments
for microdevice with main channel width w = 0.6 mm.
Namely the higher two phase superficial velocity would
hinder the coalescence process. According to film drainage
model, the effects of two-phase superficial velocities could
be explained by the contact time of bubble pairs decreasing
with the increase of superficial velocity. The condition with
higher superficial velocity cannot provide sufficient time
for liquid film drainage, and then the bubbles move apart
from each other without coalescing.
Moreover, Fig. 7a also shows that at the same two-phase
superficial velocity condition (especially, when
uTP C 16.2 mm/s) the higher gas flow rate can result in the
lower percentage of coalescence. The microbubble diame-
ters d under different superficial velocity conditions are
shown in Fig. 7b. It can be found that the higher gas flow
rate leads to the larger bubble size. Thus, this result also
indicated that under the same liquid viscosity and two-phase
superficial velocity conditions, the small microbubbles are
more likely to coalesce than big bubbles. Figure 7c and d
shows the same tendency by comparison of two micro-
channels with different dimensions. Due to the microbubble
size in w = 0.8 mm microchannel is larger than in
w = 0.6 mm microchannel, under the same superficial
velocity condition the smaller microbubbles more tend to
coalesce, and the transition superficial velocity and capil-
lary number value in w = 0.8 mm microchannel mentioned
above are lower than in w = 0.6 mm microchannel. The
reason can be explained that the small bubbles will result in
the smaller diameter of liquid film, so the small bubbles
tend to coalesce due to requiring shorter film drainage time.
It is generally thought that small bubbles are more difficult
to coalesce than big bubbles, often because of the lower
collision frequency of small bubbles. Tsang et al. (2004)
also found that the smaller bubbles tend to coalesce in
electrolyte solution with the same concentration.
Fig. 7 a Effect of two phase
superficial velocities on
percentage of microbubble
coalescence events (the main
channel dimension is
0.6 mm 9 0.6 mm and the
continuous phase is 10wt%
glycerol–butyl alcohol
solution); b Microbubble
diameters under different
superficial velocity conditions
in the microdevice with main
channel width w = 0.6 mm.
The symbol with dot center is
representing absolute
coalescence, open symbol is
probabilistic coalescence;
c Percentage of microbubble
coalescence events in different
microchannels; d Comparison
of microbubble diameters in
different microchannels
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123
3.3 Fluid dynamic rule for the microbubble
coalescence
As the film drainage model mentioned before, the contact
time and drainage time are the crucial parameters for
bubble coalescence process. This concept is introduced in
this work and two characteristic parameters representing
the bubble contact time and film drainage time are defined
to analyze the fluid dynamic conditions of microbubble
coalescence. According to the theoretical model (Liao and
Lucas 2010), we define the characteristic drainage time as
tdrainage * lcd/c, where lc is the continuous phase vis-
cosity, c is the surface tension, and d is the bubble diam-
eter. The characteristic contact time is in inverse proportion
to uTP which is the two-phase superficial velocity, and
characteristic contact time tcontact can be estimated as w3/
2(QG ? QL), where w is the microchannel width. It is
representing the residence time scale of external flow,
which is starting from the moment that bubbles contact
each other at meeting junction and until they separate.
Therefore, the area of microbubble coalescence behavior in
the experiment could be distinguished by comparing the
bubble contact time with the film drainage time, as shown
in Fig. 8a, b. It can be found that the probabilistic coa-
lescence area is between the absolute coalescence and non-
coalescence regions. The straight solid lines in Fig. 8a and
b are representing the relations as w3/2(QG ? QL) = 600lc
d/c-25 and w3/2(QG ? QL) = 900lcd/c-50, for each
microfluidic device respectively. The area on the left side
of the line, i.e. with longer contact time, is absolute coa-
lescence region. In contrast, the area on the right side of the
line is non-coalescence region. The relative deviation
between solid line and dash line is ±10%, and nearly all
the probabilistic coalescence points can fall into this band
region.
4 Conclusion
In this work, the coalescence process of flowing micro-
bubbles in confined microchannels with different channel
size was observed, and different influence factors on the
coalescence process were investigated. The results showed
that the microbubble coalescence process in confined space
was slightly faster than in free space. Three behaviors
including absolute coalescence, probabilistic coalescence,
and non-coalescence were observed. The coalescence
behavior was mainly influenced by the liquid viscosity and
two phase superficial velocity. Increasing liquid viscosity
could apparently prevent the coalescence process. In the
probabilistic coalescence region, the higher two-phase
superficial velocity could reduce the percentage of coa-
lescence events. The fluid dynamic conditions of micro-
bubble coalescence were analyzed by defining the
characteristic contact time and film drainage time, and a
linear relation was developed to distinguish the coales-
cence and non-coalescence region. To our knowledge, it is
a first quantitative study on the microbubble coalescence in
confined microchannels.
With the aid of microfluidic device, the controllable
coalescence process of microbubbles was realized. This
method could offer a good tool for investigation of
microbubble coalescence behavior. In order to provide a
general equation for predicting the microbubble coales-
cence process, further studies on the process with different
working systems and much wider range of microbubble
size will be carried on in our research.
Acknowledgments We would like to acknowledge the support of
the National Natural Science Foundation of China (21036002,
20876084) and SRFDP (20090002110070) for this work.
Fig. 8 Comparison of characteristic contact time and film drainage
time. The symbol (open square) is representing absolute coalescence,
open circle is probabilistic coalescence, and open triangle is non-
coalescence. a The main channel dimension is 0.6 mm 9 0.6 mm
and the straight solid line represent w3/2(QG ? QL) = 600lcd/c-25;
b The main channel dimension is 0.8 mm 9 0.8 mm and the straightsolid line represent w3/2(QG ? QL) = 900lcd/c-50
Microfluid Nanofluid (2012) 12:715–722 721
123
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