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Advances in Micro-Droplets Coalescence Using Microfluidics

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DOI: 10.1016/S1872-2040(15)60886-6

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CHINESE JOURNAL OF ANALYTICAL CHEMISTRY
Volume 43, Issue 12, December 2015
Online English edition of the Chinese language journal

Cite this article as: Chin J Anal Chem, 2015, 43(12), 1942–1954. REVIEW

Advances in Micro-Droplets Coalescence Using Microfluidics

SHEN Feng1,2, LI Yi1, LIU Zhao-Miao1,*, CAO Ren-Tuo1, WANG Gui-Ren2
1
College of Mechanical Engineering and Applied Electronics Technology, Beijing University of Technology, Beijing 100124, China
2
Department of Mechanical Engineering & Biomedical Engineering Program, University of South Carolina, Columbia, SC, 29208, USA

Abstract: Recently, with the development of lab-on-a-chip researches, the use of microfluidics to precisely control the droplet
behaviors in microchannel has received more and more research attention. This article firstly introduces the basic theory and mechanism
of the droplets coalescence. Then, it carefully reviews the passive methods of droplets coalescence used in current researches by
changing microchannel geometry and adding surfactants. The active methods to trigger droplet fusion such as applied electric field,
magnetic fields, temperature gradients, surface acoustic wave and focused lasers are also introduced briefly. We also introduce the fluid
dynamics of the droplets coalescence and forecast its progress at last to provide useful guidance for microfluidic devices design and
wide use of the drop-based microfluidics.

Key Words: Microfluidics; Droplets coalescence; Microchannel; Review

1 Introduction disease diagnosis, cell research, drug screening, environmental

Microfluidic chip also known as lab-on-a-chip developed
rapidly in last decade in the research field of
multi-disciplinary[1]. It can be characterized as the science and
technology of manipulating and controlling fluids in
micro-scale[2]. With silicon, glass or polymer materials as the
substrate, microfluidic chip involves many functional units
such as microchannel, micropump, microvalve, and
microreactor. By utilizing micro-electronic mechanical system
(MEMS) technology and driving force fields such as electric
or pressure field, microfluidic chip can realize accurate
manipulating, processing and controlling functions of micro
fluid or samples[3]. Besides, microfluidic chip can integrate a
variety of biological, chemical and other laboratories
operating functions such as sample preparation, reaction,
separation and detection, cell culture, separation and sorting,
into a piece of a few square centimeters (or less) chip[4].
Compared with the traditional method, microfluidic chip has
many advantages including low cost, less sample consumption,
easy automation, fast and flexible in operation, and easy to
miniaturization, showing broad prospects in the application of
________________________
Received 22 June 2015; accepted 16 August 2015
* Corresponding author. Email: lzm@bjut.edu.cn
This work was supported by the Beijing Natural Science Foundation of China (No. 7152012), the China Scholarship Council (No. 201406545031), and the Training
Plan of New Talent of Beijing University of Technology, China (No. 2015-RX-L02).
Copyright © 2015, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. Published by Elsevier Limited. All rights reserved.
DOI: 10.1016/S1872-2040(15)60886-6
monitoring, green energy, materials synthesis, ect[4]. Therefore,
the reviews reported in Nature considered the lab on a chip
may be “the century technology”[5‒7].
Droplet microfluidic chip is a new manipulation technology
of small volume liquid developed in recent years.
Microdroplet control technology generally refers to two
incompatible fluids, such as water and oil, among which one
is used as continuous phase, and the other as dispersed phase
(10‒15‒10‒9 L). It can realize the function of microdroplet
generation, transport, splitting, merging, sorting, positioning
and capture by using microfluidic technology and controlling
the behavior of two phase flow[2,4]. Droplet microfluidic chip
technology has become an important development direction in
the research of microfluidic chip[5‒8]. Owing to the feature of
high surface to volume ratio, high mass and heat transfer
efficient and short diffusion distance etc, the reaction in
microdroplets has shorter reaction time than the conventional
system. Therefore, microdroplet in the microfluidic chip has
the function of microreactor[9‒13]. In addition, due to its high
monodispersity, small volume and unlimited generating
number, microdroplets provide a unique miniaturization
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954
platform for the chemical and biological research, in which
the volume and flow behavior can be controlled accurately.
The internal of microdroplets can produce physical and
chemical reaction environment, which are different with the
outside continuous phase fluid due to the effect of the
interfacial tension. Meanwhile, to reduce the influence of
microchannel surface properties on the internal response, the
internal fluid in microdroplets can be isolated from the
microchannel wall[8]. On account of these unique advantages,
microdroplets were widely used in cellular and subcellular
structure analysis[14‒17], protein crystallization[18,19], synthesis
of nanoparticles[20,21], nanomolecular self-assembly[22,23] and
high flux injection[24,25], etc.
Microdroplets-based biochemical reactions, for example,
the process of micro and nano particle synthesis, need two
different droplets to be fused together to get good effect of
mixing. Therefore, controllable droplet coalescence becomes
an important microfluidic technology in multi-step reactions
in droplets[8‒13]. Microdroplet coalescence refers to that two or
more microdroplets contact and fuse together. Microdroplet
coalescence needs to overcome the surface tension of the
droplets and make droplet interface unstable. As the limitation
of the upper and the lower microchannel wall, continuous
phase fluid film needs to be discharged from a limited space,
increasing the difficulty of coalescence. Meanwhile, droplet
interface is no longer global, and the balance of capillary force,
viscous force and inertia force are different from macro scale
in fusion process. Thus the theory in macro scale is difficult to
describe coalescence in micro-scale quantitatively[2].
Moreover, the deformability of the droplet interface leads to a
series of new fluid mechanics problems such as non-uniform
change of interfacial tension and droplet nonlinear[8,26], for
example, small change of the inlet pressure will lead to the
flow transition from droplets to jet, generating nonlinear
unstable flow[2,8].
At present, microdroplet coalescences can be mainly
divided into passive and active methods[2,8,9]. Taking
advantage the flow characteristics of droplets and continuous
phase, passive methods make the velocity of front droplets
slow (or captures it in a particular location temporarily) by
changing microchannel structure, increasing special
microstructure, adjusting droplets generation rate or altering
channel surface wettability. So that the rear droplets could
catch up with the front one and merges with it in a specific
location. During the process of two droplets move close to
each other, the continuous phase fluid between them will be
drained empty gradually. While in contacting, the interfaces of
droplets become unstable and rupture due to stress or shear
force, inducing coalescence of droplets[2]. Compared with
active methods, passive methods are simpler and do not
require active control or electricity. However, it needs to
design the microchannel scientifically and get a better
understanding of the two-phase flow characteristics in
microchannel. One main advantage of passive methods is that
the possibility of inter-droplet contamination is lower than that
of active methods, so that the passive methods are feasible for
cell biochemical analysis. However, passive method has lower
efficiency than most active methods as it is limited by the rate
of natural phenomena, such as surface tension fluctuations[27].
Active method refers to using electric field[28], magnetic
field[29], temperature field[30], surface acoustic wave[31,32] and
laser focus[33] to induce droplets interface instability and
coalesce. This method is inherently more complex than
passive method, since it requires fabrication of electrodes and
precise timing of electrical signals. Moreover, the electrode
may cause contamination between droplets, for instance,
droplet contents may deposit on the electrode and electrical
signals may affect the biocompatibility of biological
molecules (DNA or proteins). Active method can hasten the
development of instabilities of the surface tension between
droplets using electrode and has higher efficiency[29].
In this review, we firstly expound the basic theory and
influence factors of droplet coalescence in microchannel.
Subsequently, we review the reported passive and active
methods of droplets coalescence that by controlling the
influence factors, including controlling channel structure,
surfactant and applying electric field, magnetic field,
temperature field, surface acoustic wave and laser focus.
Meanwhile, we elaborate the hydrodynamic characteristics of
droplets coalescence in microchannel. Finally, we forecast its
progress in various applications.
2 Microdroplet basic theory
From the view of microfluidics, a series of basic operations
for microdroplets, such as generation, transport, reaction and
synthesis, are performed in the form of multiphase flow[2]. The
fundamental characteristic of multiphase flow is that two or
more components obviously separated by phase interface exist
in the flow field at the same time. Therefore, nonlinear effects
will be introduced to the micro-scale flow as the existence of
the interface, and flow behavior becomes complicated[2,8,26].
Meanwhile, due to the limitation of the microchannel wall, the
surface to volume ratio is very high, and the boundary effects
caused by wall wetting play an important role in microdroplet
behaviors, causing the significant difference in evolution of
microdroplets compared with macro-scale flow[2]. Further
study of droplet flow behavior in microchannel will promote
the optimization of microfluidic chip structure design and
innovation of the microdroplet control technique, which have
significant value in theoretical guidance and practical
applications of microfluidic chip[2,3,8,26,34‒37].
2.1 Surface tension
Due to the effect of droplet interface, surface tension should
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954
be considered. Surface tension σ is caused by the imbalance of
molecular attraction along the liquid interface and can be
defined as force per unit length (N m‒1) or energy per unit area
(J m‒2)[2,8]. Imbalanced surface tension can trigger the flow
from the zone of low surface tension to zone of high surface
tension (Marangoni convection). Surface tension driven flows
caused by temperature gradient or change of surfactant
molecules are called thermal capillary convection or solute
capillary convection, respectively[8]. Meanwhile, due to the
effect of surface tension, droplet tends to minimize its
interface area to reduce the surface energy. When the surface
of isolated droplet or bubble is spherical, the surface area
reaches the minimum. However, due to the limit of the wall,
droplet interface presents a bent shape but not spherical shape
in microchannel. The curvature of the interface can lead to
pressure jump, named Laplace pressure, between the outside and
inside of the interface. The Laplace pressure is described below:
ΔP = σ (1 R1 +1 R2 ) (1)
where, R1 and R2 are curvature radii of droplet interface at
different locations. As it can be seen from Equation (1), ΔP is
increased with the decreasing radii. As the radii of curvature is
different at different spatial locations, the pressure distribution
inside droplet is different, which plays an important effect on the
evolution of internal and external flow fields of the droplet[2].
2.2 Dimensionless numbers
The behavior of microdroplets in multiphase flow depends
on various forces, including viscous force, inertia force,
gravity, surface tension, shear force, and separation pressure,
etc. The relative influence of them on flow can be described
with the following dimensionless parameter[2]:
(i) Reynolds number, Re
Re = ρUl/μ (2)
where, ρ, μ, U and l represent mass density, dynamic viscosity,
characteristic velocity and characteristic length, respectively.
Re is the ratio of inertial force (ρU2/l) to viscous force (ρU/l2).
Generally, flow is laminar at Re < 10. Inertia force can be
ignored in most cases, while it has certain effects on the
microdroplet with high speed or at the instant of rupture.
(ii) Weber number, We
We = ρU2l/σ (3)
where, We represents the ratio of inertial force to surface
tension. In microchannel, it is usually much smaller than in
macro scale, so the surface tension has a prominent effect on
the flow.
(iii) Bond, Bo
Bo = ∆ρgl2/σ (4)
where, g and ∆ρ represent gravity acceleration and the
difference in mass density between the two fluids, respectively.
Bo is the ratio of gravity effect to surface tension. In
micro-scales, generally Bo << 1, meaning that gravity effect
can be ignored.
(iv) Capillary number, Ca
Ca = μcU/σ (5)
where, μc is the viscosity of continuous phase, U is the
characteristic velocity in the location of droplet fusion, σ is the
surface tension at the interface of continuous phase and
dispersed phase. Ca is the ratio of viscous stress to surface
tension. At low Ca, surface tension becomes a key factor
which led to the droplet is more stable, and at the end of
droplets is spherical. On the contrary, viscous force plays an
important role, leading to large deformation of the droplets
and asymmetric geometry.
From the definition of the previous dimensionless
parameters, it can be found that Re, We and Bo are all small
for microdroplet flow, leading to the characteristics as viscous
laminar flow, where surface tension and viscous forces (Ca)
play leading roles in most cases. Furthermore, many influence
factors, including limitation of microchannel wall, wall
wetting, ratio of microchannel geometry size and the droplet
size, have important effects on microdroplet multiphase
flow[8,26]. Additional exerted force fields (such as electric field,
thermal, acoustic, etc.) require characterization of the relative
importance of applied forces and surface tension to descript
their effect mechanisms[26].
2.3 Surfactant effect
Surfactants are usually added into continuous phase to
reduce surface tension to favor microdroplets generation and
transport. Surfactant can make the droplet interface relatively
stable and thus make the coalescence difficult, so the
microdroplets are used as microreactors. However, as the
influence of the factors such as flow and molecular diffusion,
the distribution of surfactant concentration becomes uneven,
which leads to the changes of surface tension in space and
then affects the flow of interface. Surfactants can make
droplets in the metastable state[38], and there are two kinds of
mechanisms when two droplets close to each other, as shown
in Fig.1a. The first one is that the rejection force of the
surfactant molecules makes the two closed interface more
stable. The second one is that in the drainage process of
continuous phase, the external flow induces the change of
surfactant concentration, which leads the changes of surface
tension σ at each point. Then the Marangoni stress occurs[8,38]:
∂u ∂u
μ d ‖ = μ c ‖ + ∇ || σ
∂r in ∂r out (6)
where, μd and μc are viscosity of dispersed phase and
continuous phase, respectively. μ|| is tangential velocity, r is
radius direction, and ∇ || is surface tension derivative in the
direction of tangent in arbitrarily point of interface. Marangoni
convection along the border to center of the liquid film is
generated under the effect of Marangoni stress, as shown in
Fig.1b. It hinders the drainage of continuous phase and increases
the drainage time, making microdroplets more stable[38].
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954
Fig.1 Schematic representation of film drainage of continuous phase between drops. (a) Absence of surfactant; (b) Marangoni stress (red arrows)
induced by the gradient of surface density of the surfactant counteracts the film drainage[26,37]
2.4 Coalescence mechanism
Microdroplet coalescence includes four basic process: (1)
droplets capture or positioning, (2) two droplets close to each
other, collision and deformation, (3) drainage of continuous
phase liquid film between droplets, and (4) the interface film
of droplet rupture and fusion[39]. At present, most of the
researches focus on the generation of microdroplets.
Coalescence mechanism still needs further study. The factors
affecting droplets coalescence are complex, including channel
geometry, inlet velocity, surfactants, wall properties, and
external force fields, etc. Now, the effect of external force
fields cannot be measured quantitatively and it is unable to
characterize the relative importance of external fields and the
surface tension accurately. Furthermore, due to external force
fields effect, the deformation of droplet interface and the
problem of transient nonlinear vibration are the challenge of
the research. Until now, droplet coalescence under external
force fields is most relying on experimental experience, and
there is no accurate theoretical analysis yet to describe their
mechanism.
In the current, liquid film drainage model is used to
describe the process of passive fusion between two droplets[39].
Two droplets may be attached together after contacting, but
they may be not fused because of the liquid film between them.
After contacting, they also have tendency of mutual
compressing or relative sliding. Rotation may occur, which
results in that the center line of two droplets is no longer
parallel to the microchannel. Meanwhile, continuous phase
liquid membrane between two droplets begin to be drained,
and redundant capillary force between the films help
draining[40]. The rate for drainage is mainly determined by the
many factors, such as impact velocity and viscosity of liquid
membrane, namely the capillary number Ca. Critical capillary
Fig.2 Influence of capillary number (Ca) on drop coalescence. (a) Ca < Cac, coalescence; (b) Ca > Cac, slipping[3]
number (Cac) is a key parameter to determine whether fusion
occurs[3]. According to the research, fusion almost occurs at
collision with low speed (Cac ≈ 10−2). Fusionis more likely to
happen below the Cac[3], as shown in Fig.2a. When above the
Cac, droplets may slip over the previous one without
coalescence[3], as shown in Fig.2b.
Liquid film between two droplets will become thinner if
contact time is long enough. When the liquid film is thin
enough, van der Waals force and other molecular inter-atomic
forces begin to play a leading role, then membrane ruptures
and fusion occurs[3,41]. Generally, the efficiency of film
drainage increases with the increasing Ca. Furthermore, the
collision angle has an effect on drainage time as well[42].
Klaseboer et al[43] described the expression of liquid film
drainage time when collision in front:
t drain ≈ 40 r μ c σ U (7)
Moreover, Hu et al[44] found that Cac of two droplets
collision depends on the droplet radius r and the viscosity
ratio of two phase fluid λ = μd/μc. It can be represented by the
following formula:
Cac ∝ ( λ ) ( 2r )
−0.41± 0.06 −0.82 ± 0.03
(8)
Currently, many experiments and numerical simulations
showed that film drainage time, Cac andf usion angle were
also influenced by droplet size[45,46], viscosity ratio[45,47],
deformation of droplet[48,49] and migration of collision[42], etc.
Meanwhile, wall wetting also has important influence on film
drainage. Li et al[50] studied the fusion of droplets and fluid
column in hydrophilic microchannel, and found that better
hydrophilic surface, smaller channel size, shorter distance to
the entrance and larger droplet size could induce greater
capillary pressure. Other forms of coalescence, such as fusion
caused by simple shear flow[51,52] and a large number of
emulsion fusion in special structures induced by smooth
surface[53,54], also received research attention.
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954

3 Control method of microdroplet coalescence
3.1 Controlled microchannel geometry structure
3.1.1 Flow resistance structures
A common method to realize microdroplet coalescence is to
add flow resistance structures in microchannel by micro
machining. Xu et al[55] reported three different flow obstacle
structures, including wall protuberance, enlarged circular
cross section, and enlarged ellipse cross section. The
microdroplet coalescence process typically includes the
following steps: adding obstacle structure, droplet trapping,
collision, fusion and moving together.
To slow down the flow of the front droplet, Tan et al[56]
designed and investigated three different channel geometries,
including a rectangular expansion, a tapered expansion and a
flow rectify. As shown in Fig.3, the first design enabled the
deceleration of the droplet in the rectangular expansion, which
was helpful for the discharge of continuous phase liquid,
reduced the space between droplets, and led to coalesce. The
length and width of expansion area and speeds of two phase
flow have important effects on the droplet fusion. In the
tapered expansion, with the rapidly decreasing droplet speed
and the drainage of continuous phase, many subsequent
droplets fuse. The droplet number of fusion is uncontrollable.
Different with the former two structures, the cross-shaped
rectification design can control the drainage time by
controlling the flow rate in upper and lower microchannel to
control the fusion at the intersection[56].
Similar to the rectification design, Gunes et al[57] added
many vertical channels on both sides of the main channel to
control flow, as shown in Fig.4a. By controlling the flow in
vertical channels, the film drainage was accelerated for
controllable fusion and multiple droplets fusion was achieved.
The advantage of this structure was that collision and
separation could be controlled independently without obvious
flow interference. Tan et al[58] studied the influence of width
of the rectification channel on droplet fusion at the
intersection. Two to six droplets fusion was achieved by
increasing the width of the rectification channel, for example,
the two to three droplets fusions is shown in Fig.4b.
Niu et al[59] designed two rows of micro columns for droplet
trapping in an expanded channel (Fig.5). The droplets were
trapped in the micro column cavity due to the extrusion for
micro column to droplets, until extrusion coalescence
occurred with later droplet. The droplets after coalescence left
the micro column cavity when the pressure of continuous
phase liquid became greater than the surface tension of the
droplet.
Expanding channel became a general structure for droplet
coalescence[56,58,60]. As the width of channel was increased,
velocity of continuous phase was reduced, leading to a
deceleration of front droplet and then be closer to the later one
gradually until fusion. However, different from the phenomenon
generally accepted for extrusion coalescence, according to the
experiment made by Bremond et al[61], droplet coalescence did
not occur for the first time when they met in expanding
channel, but it took place in separation when the front one
came into the narrow channel and fused with the latter one
(Fig.6a). The separation caused instantaneous instability of
surface tension and nipple on the surface of the droplets
(Fig.6b), and then surface tension was broken and two droplets
fused rapidly. Later, Lai et al[62] studied the mechanisms of this

Fig. 3 Three different microchannels for droplet fusion[56]

Fig.4 Controlled droplet fusion using (a) list of small mediated flow channel[57] and (b) Widened mediated flow channel[58]

Fig.5 Droplet fusion using micro column structures in microchannel[59]

 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954

Fig.6 (a) Fusion process of droplet in separation caused by flow destabilization in extend channel and (b) fusion mechanism[61]

phenomenon and found that the nipple increased local
contacting area rapidly, leading to instability of droplet
surface in some location and then to coalesce.
3.1.2 Junction structures
Besides the flow resistance structure, junction structure is
also a common method to promote droplet coalescence
effectively. The basic principle for fusion is to ensure that two
microdroplets moving relatively meet at junction. As the
extrusion effect, they realize drainage and achieve coalescence
at the instant of liquid film rupture. Compared with droplets
movement in the same direction, relative collision droplets
have high efficiency of coalescence, meanwhile, multiple
coalescence does not occur and coalescence has high
controllability. However, in practice, it is difficult to control
the droplets arriving at the junction synchronously. To
overcome the problem, we should precisely control the
droplets movement in upstream.
There are mainly two kinds of junction structures, namely
T-type and Y-type. Liquid viscosity and flow rate of two
phases have important influence on the fusion. Generally, the
increasing liquid viscosity of continuous phase or flow rate of
two phases will make the fusion difficult. Meanwhile,
according to the theory of film drainage, surface contact time
and drainage time are also the key factors to determine
whether coalescence occurs. In addition, flow velocity, total
flow rate, droplet size, and aspect ratio of microchannel are
also important for drainage efficiency. Yang et al[63] observed
three kinds of phenomena about coalescence of micro bubble
T-junction microchannel, namely, absolute coalescence,
probabilistic coalescence and non-coalescence. They also
analyzed the influence factors for coalescence probability.
Christopher et al[41] studied the influence of droplet size and
flow rate on coalescence in T-junction microchannel. There
were six kinds of phenomena after collision, namely, except
for coalescence and sliding (Fig.2), splitting, multiple splitting,
later coalescence and later sliding (Fig.7). In their study[41], it
is found that droplet size and flow rate had important effects
on coalescence. Collision at low speed is easy to coalesce,
small droplets with high velocity are not easy to coalesce, and
large droplets with high velocity are not easy to be split into
multiple droplets when squeezed with each other. The
research results also show that the coalescence of droplets
may occur only by precisely controlling the arriving time of
droplets to junction to achieve synchronization, and to make
the arriving time of two droplets far less than the stop time in
the junction.
Liu et al[64] investigated the influence of different
Y-junction angles of 30°, 60°, 90°, 120°, 150° and 180° on
droplet coalescence in microchannel. They found that Cac
decreases with the increase of junction angle and film
drainage time was shortened by increasing the flow rate of
two phases and the junction angle. Wang et al[65] designed
three different kinds of Y-junctions with the angle of 60°,
120° and 180°, and observed the process of droplets
contacting, extrusion, coalescence and separation in the
junction, as shown in Fig.8. They also analyzed the influence
of droplet size, collision angle and fluid physical properties on
film drainage time, droplet contact time and Cac. The
experimental results showed that it was helpful for promoting
coalescence by reducing droplets collision angle. They also
proposed formula to forecast the Cac for coalescence.
The abovementioned two junction channels need to control
the arriving time for reaching the junction synchronously and
precisely, which increases the difficulty of the experiment.

Fig.7 Four different forms of droplet collision at microfluidic junctions[41]

(a) Splitting; (b) Multiple splitting; (c) Late coalescence; (d)Late splitting
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954

Fig.8 (a) Coalescence and (b) separation behaviors of microdroplets at different microchannel junctions[65]

Therefore, Wang et al[66] solved the synchronization issue of
droplets by designing a cross channel. Compared with T-type
and Y-type structures, the cross channel provided symmetrical
flow field that was relative stable. As shown in Fig.9, the first
arriving droplet was stayed in the junction until the next drop
moved to the junction and contacted with it, which allowed
certain deviation for arriving time.
Mazutis et al[67] changed the flow form of T-junction
microchannel and made two different droplets match in the
junction and move together in the widen channel downstream.
Then coalescence occurred, as shown in Fig.10a. Due to the
effect of surfactant, the droplet surfaces contacted but not
coalesced. In the process of coalescence, emulsion droplets with
small diameter rotated around the large one due to the effect of
flow field. After rotating to a certain angle, the small droplets
were stretched out of shape. Until the center distance between
two droplets increased to a critical value, the surface tension
became unbalanced and coalescence occurred (Fig.10b). As
shown in Fig.10c, this method realized coalescence after
rotating with emulsion number ratio of 1:1, 1:2 and 1:3.
3.1.3 Micro-lancet structure
Deng et al [68] reported an innovative and efficient
surgery-like strategy using micro-lancet for achieving
coalescence of droplets in the junction. The balance of liquid
membrane on droplet surface was destroyed by micro-lancet
when droplets flowed through it,and caused temporarily local
scattering of surfactants, thus induced their coalescence by
joining up their scratched wounds. They also analyze the
influence of hydrophobicity and hydrophilicity on micro-
lancet surface and the tip shape on fusion, as shown in Fig.11.

Fig.9 (a) Coalescence and (b) separation behaviors of microdroplets at the cross-shaped microchannel junctions[66]

Fig.10 (a) Schematic of microfluidic chip, (b) flow-induced droplet rotation and coalescence, and (c) process of 1:2 coalescence[67]
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954
Fig.11 Droplets fusion induced by micro-lancets[68]
The results showed that the micro-lancet with a hydrophilic
surface and sharp tip was more beneficial to destroy the
stability of droplet interface, inducing coalescence.
3.2 Adding surfactant for coalescence
Besides the above mentioned methods using geometry
structure and flow characteristics, adding surfactants in
continuous phase to reduce surface tension has become
another way to achieve droplet coalescence. Baret et al[37]
reviewed the important influence of surfactants on the control
of droplet in microfluidic chip and elaborated the mechanism
of interface stability damage for its compatibility in biological
system and the field of molecular exchange between droplets.
They also pointed out that the surfactant molecules could be
dissolved in oil and coalescence occurred due to the diffusion
of oil molecular. Mazutis et al[69] studied a simple and reliable
device, by which coalescence was achieved for one-to-one
under the frequency of kHz in microfluidic system. This
technique needed to add surfactants in stable droplet surface
and connect it to an appropriate geometry. Fryd et al[70]
investigated the emulsion of water-in-oil and used a kind of
ionic surfactant to keep droplet stable and another kind of
ionic surfactant with opposite electric charge to achieve
coalescence. However, there was a certain duality for using
surfactants. Liu et al[71] found that with the increase of
surfactant concentration, droplet size decreased gradually and
coalescence was uneasy to happen. Moreover, Shestopalov et
al[21] found that surfactant increased to 5% in weight led to
droplets separation and coalescence would not occur.
Tullis et al[72] proposed an effective method for coalescence
of specified droplet pairs in parallel arrays microchannel.
They achieved coalescence of droplets in pairs for removing
surfactants on droplet surface by reducing the surfactant of oil
phase in the external flow. They also found that coalescence
time was shortened if there were no surfactants on the surface
of oil phase. However, coalescence without using surfactant
also had its disadvantages, such as accidental coalescence and
further manipulation of droplets was restricted after
coalescence.
Also some scholars studied the passive fusion of droplets
with surfactants. Mazutis et al[69] invented a microchannel to
achieve coalescence with an obviously asymmetric channel
size under the action of surfactants, discovering that
coalescence of droplets was not carried out in accordance with
the scheduled way. Therefore, the best way for coalescence is
to make droplets stable using surfactants first and then
achieving coalescence by using external forces.
3.3 Active fusion using external field force
Because the microchannel dimension is very small, it is
difficult to control the motion droplets precisely. To achieve
droplet capture, coalescence and reaction, external field forces
may be needed. So far, electro-coalescence is the most
common way used in active fusion[73], and the principle of
which is to make the droplets have opposite charges by
electricity inducement and thus results in coalescence of
droplets. Under electrostatic forces, droplets can close to each
other and coalesce. In other case, the droplet interface would
deform and rupture under Maxwell stress produced by electric
field, leading to coalesce of droplets. The conditions for the
action of electric field are very broad. The coalescence can be
better controlled in the voltage range from 1 V to several kV
and the frequency range from DC to several kHz. In addition,
electrodes can be embed in microchannel or a few millimeters
away from channel when using electro-coalescence, and the
direction of electric field can be parallel or perpendicular to
droplet surface.
Wang et al[74] captured droplets by using applied electric
field to achieve coalescence of droplet pairs. The structure of
microfluidic chip is shown in Fig.12a. From the research, it
was found that the droplets flowed along the main channel and
could not come into the groove without electric field.
However, the droplets came into the micro groove and were
captured to wait for coalescence under applied electric field.
Besides, droplets would move along the main channel again if
the electric field was removed (Fig.12b).
Hao et al[75] designed a local embedded electric field to
manipulate droplet coalescence in microchannel with better
control. According to the principle of electro-wetting and fluid
dynamics control, the droplets size and generation frequency
can be changed separately. Hundreds of observations found
that the efficiency of on-demand coalescence reached 98%. In
this system, a cross field was used to promote droplet
coalescence. When the electric field was turned off, the
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954

Fig.12 Droplet trapping and fusing using electric field[74]

(a) Microfluidic platform diagram; (b) Droplet trapping and fusing process

surfactant was stable and the droplets would not coalesce
although the droplets squeezed with each other. But when
opening the electric switch for need, coalescence occurred due
to the unstable surface.
Schoeman et al[76] designed a microchannel to realize cell
droplets generation and coalescence. They used double T-type
channels to form droplets with single-cell encapsulation. By
adjusting flow parameters of two phases, two droplets with
single-cell encapsulation arrived Y-junction channel at the
same time to realize pairing, then electric field generated by
microelectrode was applied to make droplet coalesce (Fig.13).
In addition to coalescence by using applied electric field,
other methods were employed for active fusion, including
magnetic field[29], temperature field[30], surface acoustic
wave[31,32] and laser focus[33], etc. Among them, surface
acoustic wave method could realize not only microdroplet
manipulation[26,77], but also controllable coalescence. Fu et
al[78] installed an interactive sensor and a reflector in a
piezoelectric substrate using microelectronic technique.
Because of the surface acoustic wave interference between
them, the droplet coalescence was achieved in microchannel.
The results indicated that the size of droplets, the distance and
the signal strength affected droplet coalescence significantly.
Based on the theory that different propagation resistance of
acoustic wave could produce sound scattering forces in
two-phase fluid, Muhsincan et al[79] made a surface acoustic
wave device. As shown in Fig.14a, a droplet was captured into
a micro rectangle groove by surface acoustic wave to wait for
coalescence with the next one. The coalescence of two or
three droplets was achieved by this step. When droplet volume
exceeded a certain critical value after coalescence, droplets
would flow out of the groove under the force of the
continuous phase (Fig.14b).
Relative high voltage was generally required for electro-
coalescence, while thermal-coalescence was proposed to
overcome the disadvantages of passive fusion and electric
fusion. Luong[80] and Xu et al[81] studied the process of droplet
coalescence under heating condition in the fusion chamber in
experiment. The results showed that the flow rate had
significant influence on critical temperature. Peng et al[82]
studied the physical process of droplet coalescence induced by
the decreasing gap between the two adjacent droplets in a
heating chamber and analyzed the process through the
mathematical formula derivation and the solution of physical
equation. Droplet coalescence was realized by introducing a
laser beam as well. Some scholars achieved droplet coalescence

Fig.13 Process of single-cell encapsulation, droplet pairing and fusion[76]

Fig.14 Droplet merging using surface acoustic waves[79]

(a) Microfluidic chip design; (b) Droplet trapping and merging
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954

under the effect of light through capturing vortex and inducing
thermal gradient by laser[83,84]. They heated the location of the
contact area of two droplets using the heating effect of laser.
On one hand, the surfactant molecules on droplet surface was
discharged, on the other hand, it induced complex three-
dimensional flow. Both of them discharged the fluid film
between two droplets effectively, thus promoting droplet
coalescence. Jin et al[85] put forward an optical method of high
precision to induce droplet coalescence. They captured
droplets by using light dispersion and gradient force to squeeze
droplets before coalescence and used the analysis model for
experiment, finding that their influences were consistent.
3.4 Flow field characteristics in coalescence
At present, taking advantage of fluid mechanics experiment
method and micro particle image velocimetry(Micro-PIV), it
has become an important research content to study the flow
field characteristics of coalescence, aiming to reveal the
coalescence mechanism deeply. Jin et al86] studied
coalescence process of droplets in straight channel and
convergent channel. Their researches show that the process of
coalescence involved contact, drainage, surface fusion,
seepage or package and other steps, which were mainly
depend on channel geometry and effect of various forces. In
straight channel, back droplet infiltrated to the front one and
merged instantaneously (Fig.15a). However, a strong vortex
formed in convergent channel when back droplet surround the
front one (Fig.15b).
Wang et al[66] studied the internal velocity vector fields in
the state of droplet extruding and rotating in the cross channel
and analyzed the viscous shear stress (Fig.16). Figure 16a
shows that velocity vectors at the edge of the contacting area
are along the vertical direction. Meanwhile, squeezing
between two droplets caused by shear effect (Fig.16b) reduced
film drainage time obviously until coalescence. Compared
with Fig.16a, the velocity vector field in Fig.16c is completely
different and shear stresses are asymmetric. So the movement
of droplets was no helpful to drainage. Therefore, droplet
coalescence did not occur after rotation[66].
Liu et al[64] studied the velocity vector fields of collision
and separation induced coalescence in cross of Y-junction
microchannel with angle of 30°. They found that the
generation of internal vortex in droplets was caused by
relative shear movement at contact area in front of the droplet.
The smallest velocity occurred at the contact area between
droplets and microchannel wall. Due to the squeezing effect of
the rear droplet to the front one during coalescence, the
velocity in the contact area of front droplet was increased
significantly (Fig.17a). In separation induced coalescence, two
droplets moved relatively to each other, rapid coalescence
occurred due to surface nipple of droplets and the velocity
near the contact area of nipple was increased significantly, as
shown in Fig.17b.

Fig.15 Velocity vector and schematics of forces acting on the two droplets at the instant of coalescences in straight microchannel (a) and
convergent microchannel (b)[84]

Fig.16 Velocity fields of droplet under two different conditions[66]

(a) Droplets squeezing; (b) Schematic diagram of the viscous shearing force; (c) Droplets rotating; (d) Schematic diagram of droplet rotation driven by shearing forces
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954
Fig.17 Velocity fields in droplet fusion[64]
(a) Collision fusion; (b) Separating fusion at Y-shaped microchannel junctions
Yan et al[87] introduced surface tension to the Navier-Stokes
equation (N-S) and studied the flow characteristics of droplets
in convergence microchannel using numerical simulation. The
results showed that the flow behaviors depended on the initial
velocity of droplets. They also proposed a microchannel
parameter “Da” for the first time to describe the geometric
features in convergent channel:
Da = αβγ (9)
where, α is the width ratio on both ends of the channel, β is the
ratio of droplet diameter and spacing, γ is the ratio of channel
length and droplets interval. According to different “Da”
values and initial velocities, they summarized three kinds of
coalescence modes, namely absolute coalescence,
probabilistic coalescence and non-coalescence. The results
also showed that there was a nonlinear relationship between
the location of droplet coalescence and the ratio of channel
width, and it was conducive to promoting droplet coalescence
by increasing the droplet diameter, the entrance width and
length of the channel.
4 Conclusions and prospection
This paper reviews the basic microdroplet theory and
influence factors of droplets behaviors in microchannel. The
research progresses of both passive and active methods of
microdroplet coalescence are presented in detail[2,8,9].
Moreover, the flow dynamic characteristics of droplet
coalescence are elaborated. Now, the research of droplets
coalescence has made some progress, meanwhile, the
influence factors of droplet coalescence have also been
studied. However, there are still many challenges in
coalescence of microdroplets:
(1) The behaviors of microdroplet should be controlled
more precisely, especially for automation control of
coalescence of multiple droplets. At present, research mainly
focuses on coalescence of two droplets, while few focus on
coalescence of multiple droplets. Coalescence of multiple
droplets with precise control will become an important
direction for future research.
(2) At present, passive fusion method mainly depends on
the flow characteristics of droplets with low efficiency.
Coalescence in multi-parallel microchannel with high
throughput will become a key content for practical
applications in future.
(3) Active fusion method needs external fields, additional
equipment and microelectrode machining, which increases the
difficulty of integration of microfluidic chip system and
restricts the development of integration in large scale. In
addition, active fusion method needs to optimize the control
conditions for external field to achieve coalescence and reduce
the influence on biological cells. These issues will continue to
be an important content in the future study.
(4) Coalescence of microdroplets becomes a new platform
for biological cell analysis, and accurate control of multiple
emulsion, etc. Its application field is expanding constantly.
However, there are still many specific problems need to be
solved in practical applications, which will be an important
part in the future study.
(5) Moreover, the process of droplets control belongs to the
category of micro-scale two-phase flow. The influence factors
are complex and difficult to be measured and controlled
quantitatively, especially for the non-uniform change of
surface tension caused by droplet interface deformation and
hydromechanics problems induced by droplet nonlinear
problem. These issues need to be investigated in depth. In the
process of active fusion, the forces of external fields are more
complex. It is impossible to be studied quantitatively, and the
coalescence mechanism is still unclear now.
(6) For better understanding of flow mechanism in droplet
control, achieving high sensitivity and precise control
technology of microdroplets, and broadening the application
field of droplet based microfluidics, it still needs effort and
cooperation of relevant multi-disciplinary researchers.
In a word, droplet based microfluidics becomes an
important research direction in microfluidic chip[5‒8].
Coalescence of microdroplets becomes one of the most
important content[8−13]. Microdroplet reactor has the
advantages such as less sample consumption, high mixing
speed, high flux and stable reaction conditions, etc. Taking
advantages of multi-disciplinary research, microdroplet
coalescence will be applied in many fields. The application
fields are also expanding, including cellular and subcellular
structure analysis[14‒17], protein crystallization[18,19], synthesis
of nanoparticles[20,21] and nanometer molecular self-
assembly[22,23], as well as high throughput injection[24,25], etc.
Meanwhile, flow characteristics of microdroplet are studied,
 SHEN Feng et al. / Chinese Journal of Analytical Chemistry, 2015, 43(12): 1942–1954
and more work is needed to be done to further reveal the flow
dynamics of coalescence, especially the influence of external
field force in active fusion. The theory of microdroplet
coalescence will be further studied to provide theoretical
guidance for droplet control technology with high accuracy.
The development of this multi-disciplinary research area also
needs the effort and cooperation of microelectronics
mechanical scientist, chemist, biologist and physicist of
microfluidics.
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