CHINESE JOURNAL OF ANALYTICAL CHEMISTRY

Volume 45, Issue 2, February 2017

Online English edition of the Chinese language journal

Cite this article as: Chin J Anal Chem, 2017, 45(2), 282-296. REVIEW

Advances in Droplet-Based Microfluidic Technology and Its

Applications
LIU Zhao-Miao*, YANG Yang, DU Yu, PANG Yan
College of Mechanical Engineering and Applied Electronics Technology, Beijing University of Technology, Beijing 100124, China

Abstract: Micro-droplets, with the properties of small size, large surface area, high speed, high throughout, uniform size, closed
system, internal stability and etc., are widely used in the fields like drug controlled release, virus detection, synthetic of particulate
materials, catalysts and so on. The emergence and development of microfluidic technology provide a new platform for the generation
and precise manipulation of size-controlled microdroplet with different structures and functional characteristics. The fundamental
principles, generation and manipulation of droplet-based microfluidic technology were introduced in this review. Similarities and
differences of droplets’ conventional preparation methods and droplet-based microfluidic technology were compared and analyzed.
Finally, the applications of droplet-based microfluidic for the synthesis of functional materials, bio-medicine and design of food
structure were reviewed. In addition, the potential value and development direction of drop-based microfluidic were discussed and
forecasted.

Key Words: Microfluidic technology; Microdroplet; Droplet manipulation; Microchannel; Review

1 Introduction in drug delivery, biotechnology, disease protection, chemical

Droplet microfluidic is a new technology developed in
recent years for dealing with the generation, manipulation, and
applications of droplets with the dimensions, typically, in the
range from several micrometers to hundreds of micrometers in
diameter[1–4]. Two incompatible liquids as a continuous phase
and discrete phase are driven into the respective microchannel
at a fixed volume flow rate in the droplets synthetic basic
process. When the two streams meet in the intersection point,
the discrete phase thins gradually and eventually break up into
droplets due to the shear and squeezing forces exerted by the
continuous phase[5,6]. Microdroplets are widely used as
microreactors, which aims at achieving an array of diverse
applications that varies from biochemical reactions, reagents
rapid mixing and microparticles synthesis and so on. This
method generally strengthens the advantages of low
consumption, automation and high-throughput on microfluidic
chip. With the development of micro-electro-mechanical
system (MEMS), droplet-based microfluidic are widely used
________________________
Received 30 June 2016; accepted 9 September 2016
*Corresponding author. Email: lzm@bjut.edu.cn
This work was supported by the National Natural Science Foundation of China (No. 11572013).
Copyright © 2017, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences. Published by Elsevier Limited. All rights reserved.
DOI: 10.1016/S1872-2040(17)60994-0
analysis, cell research and function materials synthesis and
other fields[7–13].
Conventional methods for making microemulsion droplets
involved manual or mechanical agitation of multiphase
fluids[14], layer by layer deposition method[15,16], membrane
emulsification[17–19] and interfacial polymerization[20–22], etc. In
general, multistage treatments and specific emulsion
formulation were required, however, the shell thickness or
chamber structures inside multiple emulsion droplets were
troublesome to be controlled precisely. Therefore, the stability
and mechanical properties of synthetic particles, as well as
permeability between different substances, were severely
limited. In addition, the synthesized microparticles had lower
uniform size/morphology and narrower size distributions
because the high shear forces were introduced by conventional
methods.
In contrast, microfluidic technique as a new, robust droplets
synthesis method, has the following significant advantages. (1)
Microchannel packaging closed system has higher heat
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
efficiency and mass transfer property, more stable reaction
conditions and less reagent consumption which efficiently
avoid cross-contamination and simplify the post-processing.
(2) Microfluidic devices show great flexibility in preparing
shape-controlled microdroplets having unique chemical
compositions thanks to the excellent handling performance,
special laminar flow and interfacial characteristics of
microfluidic, such as interfacial polymerization, interfacial
extraction, and fusion of droplets/ multi-emulsions, etc. (3)
Complex microfluidic system can be updated by the free
combination of several single-stage microchannels, which
achieves the well-defined microdroplets of narrow particle
size distribution without the introduction of external stimuli
and further purification operation. The advantages above not
only effectively overcome the shortcomings of the
conventional methods, but also ensure the efficient packaging
of active ingredient, therefore, this technique is widely used
for biomedical engineering, virus detection, chemical analysis
and food/cosmetics processing etc[23–25].
Droplet-based microfluidic shows that the distribution of
localized flow field influencing the interface deformation is
determined by the microchannel’s geometry configurations,
liquid flow rate and other physical parameters. Simultaneously,
the balance between viscosity force and interfacial tension is
correlated to droplets’ fracture mechanism in
microchannel[4,26–30]. However, to achieve the precise
regulation on size, shape, uniformity and other factors of
microdroplets, existing researches mainly concentrated on
how to skillfully adjust the parameters like channel geometry,
two-phase viscosity, flow rate, wettability and interfacial
tension, etc. In this review, the fundamentals, generation and
manipulation of droplet-based microfluidic technology are
introduced, with comprehensive presentation of the
applications of droplet-based microfluidic for the synthesis of
functional materials, bio-medicine and design of food
structure, and so on. In addition, the potential value and
development direction of drop-based microfluidic are also
discussed and forecasted.
2 Droplet-based microfluidic technology
2.1 Microdroplet generation
Currently, the most commonly used methods for
microdroplet generation based on microfluidic can be divided
into two main categories: active and passive[2,6]. In generally,
droplet generation can be driven using active methods such as
piezoelectric actuators, thermal systems, electric fields,
magnetic field and other external driving forces. Compared
with active methods, passive droplet generation methods
benefit from the ability to increase deformation and instability
of flow field interface for preparing monodisperse droplets
simply by adjusting microchannel dimensions and geometries
or controlling the flow rates of two immiscible liquids without
additional driving forces. Passive droplet generator technique
was designed not only to provide precise control over
parameters such as size, shape, monodispersity and
components inside the droplets, but also to protect synthesized
droplets from outside interference and cross-contamination.
Therefore, this method was widely used to generate
continuous droplet stream of uniform size distributions
(1%–3% dispersity). According to the difference of
microchannels’ materials and geometries, the passive droplet
generation methods are mainly divided into three categories as
shown in Table 1.
2.1.1 PDMS-based microfluidic devices[31–33]
The main characters of polydimethylsiloxane (PDMS)- based
microfluidic devices are low cost, reusable and straightforward
to fabricate. PDMS device has good transparency to UV light
and unique elastoplastic property that make it suitable for
conformal contact with glass slides and non-planar substrates.
The PDMS devices, which are relatively easy to fabricate and
also constructed into different forms, are generally used to make
spherical particles, multi-phase particles (Janus particles), and
two-dimensionally extruded non-spherical particles whose
cross-sectional shapes can be varied. However, the swelling of
PDMS in nonpolar solvents is the major drawback hindering its
generality of applications. As listed in Table 1 (a–h), according
to the differences of channel geometries and two-phase flow
direction, five specific types of microfluidic devices are
currently in use for PDMS, including two-dimensionally
extruded structure[34,35], T-junction[36,37], flow-focus[38–40],
Co-flow[41], and Y-junction[42].
2.1.2 Glass capillary microfluidic devices[43–45]
According to the diversity of nesting structure, capillary
devices can be divided into single and multiple emulsions
(Table 1 (i–k)). Two-phase interface behaves Plateau- Rayleigh
instability caused by surface tension under continuous phases’
shear force introduced, when the dispersed phase flows into the
main channel through a glass capillary. Once two-phase
interface lost stability, the monodisperse droplets are formed.
Glass capillary devices offer a straightforward method to
generate hollow and multi-phase particles. A drawback with the
glass-based devices is the high expertise required for their
fabrication as well as the lack of applicability to synthesize two
dimensional extruded particles.
2.1.3 Terrace-based microfluidic devices[46]
The specific process of terrace-based microfluidic devices
is as follows: the dispersed phase flows along the
microchannel to a terrace area filled with a continuous phase,
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296

and then quickly grows to be a disk-shaped droplet with a high
Laplace pressure, which is thermodynamically unstable. When
the droplet comes to the terrace edge, it moves spontaneously
to a deeper region (well) and assumes a thermodynamically
more favorable spherical shape (Table 1 (l)). This mechanism
results in less controllability and is not suitable for generating
microemulsion droplets with complex structure/function, so its
flexibility of application range is seriously limited.
Polymethyl methacrylate (PMMA) and glass slides can also
be used to fabricate microfluidic devices; however, their
applications are much less common than PDMS and capillary
glasses. The structure/function of microdroplets were shown
to be tuned by simply varying flow parameters and solvent
composition of the disperse and continuous phases,
furthermore, better stable flow pattern characteristics for
generating stable droplets at the optimum flow ratio were also
demonstrated by scholars[47–49].
Droplet-based microfluidic combined via specific curing
approaches[50,51] were used to form spherical/irregular or Janus
particles, core-shell microcapsules and various complex
particles with different morphology and functional features[1–6].
Base on their complex structures, special morphology and
functional diversity, these particles were widely used in an
range of diverse applications, including the synthesis of
functional materials, biological sciences (such as drug
delivery, cell encapsulation and micro poison filter), pharmacy,
electronics, environmental governance, renewable energy and
other areas[4,6,7]. Figure 1 demonstrates the schematic diagrams
of spherical particles and composite particles with different
structures using microfluidic.

Table 1 Schematics of representative microfluidic devices

Name Style No. Device schematic Technique

Single-inlet,
(a)
Stop-flow
Two-dimensional
extruded structure
Multi-inlet
(b)
Stop-flow

Cross contact
(c)
T-junction
T-junction

(d) Head contact T-junction

PDMS
microfluidicdevices
(e) Parallel contact

Flow focusing

(f) Cross contact

Co-flow (g) Co-flow

Cross contact
Y-junction (h)
Y-junction

(i) Co-flow

Single emulsion droplet

structure

Capillary devices (j) Flow focusing

Multi-emulsion droplet Combined co-flow and

(k)
structure flow focusing

Shear force and extruding

Others device Terrace-based structure (l)
force
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296

Fig.1 Schematic diagrams of spherical particles and composite particles with different structures

2.2 Microdroplet manipulation
With the development of droplet-based microfluidic, more
technologies are being developed to control, manipulate, and
functionalize droplets. Once microdroplets are generated, they
can be precisely controlled and adjusted in either an active or
passive way according to practical demands. For instance,
parallel reactions can be expanded by splitting droplets several
times in a splitting array; complex chemical reactions and
biological experiments can be completed in the droplet fusion
and mixing of the droplet contents with different agents; the
droplets are used as microreactors in droplet trapping and
sorting processes according to different attributes, etc., and
then the internal analysis of the specific droplets can be
realized.
Droplet manipulation inside microfluidic mainly involves
the following aspects[4–6,52–57] (Fig.2): (1) droplet fusion; (2)
droplet fission; (3) mixing of the droplet contents; and (4)
droplet trapping and containing arrays. In addition, the phase
of the droplets can be changed through evaporation or
polymerization during microdroplet manipulation. With the
development of microfluidic technology, droplet manipulation
not only provides technical support for realizing the
multiplexing techniques of numerous droplets and ensuring

Fig.2 Schematic diagrams of microfluidic droplet’s manipulations: (A) Droplet fusion[52,53]; (B) Droplet fission[54]; (C) Microfluidic systems for
rapid mixing[55]; (D) Droplet trapping and containing arrays[56,57]
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
droplets’ wide application in large-scale complex biochemical
system, but also shows great application potential in virus
detection, such as microparticles synthesis, high-throughput
drug screening and other areas.
3 Applications of droplet-based microfluidic
technology
3.1 Applications of droplet microfluidic in materials
synthesis
With the development of droplet-based microfluidic, this
technology is widely used in preparing micro-scale oil-water
(O/W) and water-in-oil (W/O) microemulsion droplets. By
substituting the type of chemical agent, plenty of shape-
controlled microparticles are prepared including inorganics,
hydrogels, Janus and so on. Moreover, these particles with
well-defined morphology and dimensions can be precisely
tuned by series and parallel microchannels, which pave a way
for synthesizing complex microparticles with multiphase and
multicomposition.
3.1.1 Inorganic/polymer microparticles
Wang et al[58] prepared Si/Al composite hollow spheres
which were widely used as catalyst carrier with the co-axial
microchannel in a one-step method, by which the size control
and continuous operation of hollow spheres were easily
realized. In the experiment, the continuous phase consisted of
68% (by mass) liquid paraffin, 2% (by mass) span-85, and
30% (by mass) of trioctylamine (TOA), and the dispersed
phase was Si/Al sol prepared as specific formula. The
synthesized particle size was 450–600 μm with 40–150 μm
holes on its surface, while particle’s size could be adjusted by
the flow rate of the oil phase. Ding et al[59] synthesized TiO2
nanoparticles using poly (acrylamide-co-acrylic acid) and
polyethylene glycol/polyacrylic acid as templates and acrylic
acid as an inhibitor with similar co-axial microchannel. The
results indicated that these as-prepared TiO2 microspheres had
a uniform size distribution and good sphericity, because
polyethylene glycol/polyacrylic acid had lower expansion rate
of water-absorption and higher stability of precursor solution
compared with poly (acrylamide-co-acrylic acid).
Wacker et al[60] formed fluorescent SiO2 nanoparticles
(50–350 nm) with a flow focusing microfluidic system, the
detailed procedures were as follows: fluorescein
isothiocyanate (FITC) was coupled to ammonia propyl
triethoxy silane (APTES) and mixed off-chip with
tetraethoxysilane (TEOS) to yield a fluorescent silicon
alkoxide solution (SA). A hydrolysing mixture (HM) and SA
were injected into the microfluidic chip, where they were
merged and converted into a stream of droplets in fluorinert
oil (FC-40) by a flow-focusing nozzle. After evaporation of
the reagents, the SiO2 nanoparticles were synthesized and then
were widely used to reduce dry leakage and increase dry
stability. This synthesis in droplets led to a faster reaction and
allowed drastically improved nanoparticle size uniformity
(down to 3% relative standard deviation for 350 nm size
particles) in comparison with conventional bulk synthesis
methods, thanks to the precise control of reagent concentrations
and reaction times offered by the microfluidic format.
Yang et al[61] prepared low-density foam poly(divinylbenzene)
(PDVB) shells with diameter of 3.3–3.7 mm through the
photopolymerization using a microfluidic device. Furthermore,
they showed the systematical investigation on the influences
of monomer concentrations and illumination times in the
photopolymerization on the structures and properties of PDVB
shells, and found that the pore volumes and the average pore
diameters of PDVB shells decreased with the increase of
monomer concentrations and illumination times. It was
believed that the systematical investigation of the
photopolymerization could be beneficial for the optimization
of millimeter-size PDVB shells, which raised attentions for
the special application in laser fusion experiments or mandrels
for ICF targets.
Teshima et al[62] demonstrated that by using a micro-flow-
focusing device, monodisperse spherical assemblies (SAs)
displaying various structural colors in air were prepared from
a suspension containing environmentally friendly white and
black colloidal particles: monodisperse submicron-sized SiO2
colloidal particles and black magnetite colloidal particles
(Fig.3). The average size and the hue of the monodisperse SAs
could be adjusted by respectively changing the concentration
and the size of SiO2 colloidal particles presented in the
aqueous phase. Moreover, the saturation of the colors
produced by the monodisperse spherical assemblies could be
altered by adding the amount of modified magnetite colloidal
particles. The results above provided an ideal candidate of
structurally colored materials for future application in
pigments and test agents.
3.1.2 Hydrogel microparticles
Zhao et al[63] developed a facile microfluidic approach using
the aqueous solution with 2.0% (wt) chitosan and 2.0% (wt)
acetic acid as the inner fluid, and the silica sol as the middle
fluid, n-octanol as the continuous flow to prepare chitosan-
silica core-shell hybrid microspheres with different pore
structures by dual-coaxial capillary device. The hybrid
microspheres not only showed high mechanical intensity but
also good adsorption properties of the heavy metal ion Cu2+
due to the silica shell providing effective protection for ‒NH2.
After Cu2+ was reduced to Cu+, the hybrid microspheres also
exhibited outstanding catalytic activity in azide-alkyne
cycloaddition reactions, on top of which the catalyst was easy
to be recovered just through sedimentation or filtration. Wang
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296

et al[64] reported the controllable generation of gas/water/oil
(G/W/O) double emulsions by making a little adjustment to
the dual-coaxial capillary device: injecting a smaller capillary
into another capillary and making the tapered orifices align
where the single emulsification carries on to reduce the
distance of the two dispersion stages to a degree that the
interference between their flowing conditions could be
eliminated. They promised that the structure of the double
emulsions would be tuned easily by the three phase flow rates
and the dimensional range of the encapsulated microbubbles
could be expanded by integrating CO2 adsorption.
As shown in Fig.4a and b, Liu et al[65] developed smart
core-shell microspheres for selective Pb2+ adsorption and
separation using a microfluidic approach. The magnetic
poly(N-isopropylacrylamide-co-benzo-18-crown-6-acrylamide)
(PNB) core-shell microspheres exhibited selective and rapid
Pb2+ adsorption through the formation of stable B18C6Am/
Pb2+ host-guest complexes. Owing to the inner magnetic core,
the Pb2+ adsorbed microspheres could be separated from the
treated solution through an external magnetic field. The
prepared magnetic PNB core-shell microspheres exhibited an
interesting temperature-dependent Pb2+ adsorption behavior,
and their Pb2+ adsorption capacities decreased with increasing
the temperature, which was caused by the decrease of
formation constant of B18C6Am/Pb2+ complexes. Owing to
the inner magnetic core, the Pb2+ adsorbed microspheres could
be separated from the treated solution through an external
magnetic field. Moreover, the Pb2+ adsorbed magnetic PNB
core-shell microspheres could be easily regenerated by simply
increasing the operation temperature and washing with
deionized water.
Seo et al[66] directly miscibilized lipophilic, as-synthesized,
hydrocarbonstabilized nanoparticles (NPs) into lipophobic
perfluorocarbons (PFCs), using a removable cosolvent, diethyl

Fig.3 Schematics of synthesis structurally colored, monodisperse spherical assemblies (SAs) using microfluidic technology[62]. (a) Diagram of
SA preparation process; (b) Micro-flow-focusing device (MFFD) for synthesis of SA; (c) A glossy SA composed of 250 and 310 nm SiO2
colloidal particles appeared to be blue-green and red, respectively

Fig.4 Synthesis of intelligent core-shell microspheres and monodisperse scalable PFC droplets. (a) Schematic illustration of the fabrication
process of magnetic PNB core-shell microspheres and-Pb2+ adsorption and regeneration processes[65]; (b) Schematic illustration of
intelligent core-shell microspheres[65]; (c) Generation of NP-incorporated, monodisperse PFC droplets by the microfluidic device[66]; (d)
Schematic illustration of NP-incorporated, monodisperse PFC droplets[66]
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
ether (DEE), which eliminated the need of the typical time-
consuming and expertise-specific NP surface modification steps
previously required for NP incorporation into PFCs. This
NP-DEE/PFC solution was then used to synthesize
monodisperse, micrometer-scale, DEE infused NP-PFC
precursor droplets in water using flow focusing microfluidic
device. After precursor microdroplet generation, the DEE
cosolvent was removed by dissolution and evaporation, resulting
in dramatically smaller, monodisperse, NP-labeled nanodroplets
(Fig.4c and Fig.4d), these final droplet sizes were far smaller
than the minimum droplet size limit of the microfluidic system.
The final droplet sizes scaled with the PFC concentrations in the
precursor microdroplets, and the quantum dots (QDs) remained
localized within the droplets after DEE was removed from the
system. This method was robust and versatile, and comprised a
platform technology for other unmodified lipophilic NPs and
molecules to be incorporated into different types of PFC
droplets for the production of new NP-PFC hybrid agents in
medical imaging and therapy applications.
3.1.3 Janus and shape controlled polymer microparticles
Janus particle was first coined by Yang et al[67], and quickly
grew as a new member in the colloidal family. Strictly
speaking, a Janus should have areas with different chemistry,
polarity, functionalization and/or other properties with roughly
equal surface area. Recently, the term was expanded to
encompass other multi-segment structures with regions of
different composition co-existing in asymmetric geometries[68]
(Fig.5a), whereafter the synthesis of Janus and hybrid Janus
particles in microfluidic technology were extensively studied
by many scholars[69–75].
Due to the unique sizes, shapes, and aspect ratios of
microparticles that are the key factors affecting their functions,
the droplet-based microfluidic technology offers many unique
advantages in the preparation of size, shape precisely
controllable microparticles that do not exist in conventional
methods. Dendukuri et al[76] demonstrated a representative
experiment, in which an acrylate oligomer stream (typically
poly (ethylene glycol) diacrylate) containing a photosensitive
initiator was passed through a rectangular all-PDMS
Fig.5 Synthesis of Janus and different particles using microfluidic technology: (a) Illustration of common Janus particles[68]; (b) SEM images of
particles with different structures[76]
microfluidic device. Simultaneously, the flowing oligomer
was exposed under the controlled pulses of ultraviolet (UV)
light and collected in the device reservoir. By designing masks
with varied features and selecting channels of differing
heights, they synthesized the particles with several distinctive
shapes, sizes and aspect ratios, as shown in Fig.5b. Other
scholars conducted in-depth researches on the synthesis of
microparticles with different structure and morphology, such
as globoids[68], rods[69], donuts[77], etc.
Yang et al[78] demonstrated a simple and easy approach for the
one-step synthesis of tail-shaped Fe3O4-chitosan composite
particles using a micro-flow-focusing device with a mixture of
chitosan solution and ferro/ferri solution (containing FeCl2
and FeCl3 in 1:2 molar ratios) as dispersed phase and
sunflower oil as a continuous phase. After a spontaneous
self-assembly water-in-oil (W/O) emulsion was obtained at
the cross-junction, ferro-chitosan droplets were dripped into a
sodium hydroxide solution for the solidification of chitosan
droplets and the co-precipitation of both ferrous cations and
ferric cations, then the particles were collected by
centrifugation, and washed with distilled deionized water to
remove alkali. The synthesized iron oxide-chitosan composite
particles had a faster release rate and better encapsulation rate
of the drug than the chitosan particles and were potentially
useful for biomedical applications, such as magnetic
responsive drug carriers, magnetic resonance imaging (MRI)
enhancers, etc. Lin et al[79] reported the synthesis of tail-
shaped alginate particles using the similar microfluidic platform
combined with a sedimentation strategy. In their experiment, a
spontaneous self-assembly water-in-oil (W/O) emulsion was
achieved at the cross-junction by using two continuous oil
streams (sunflower seed oil solution) to shear the alginate
solution (1% Na-alginate in water), and then were dripped into
the CaCl2 solution to undergo a progressive crosslinking
process. The results showed that the tail length and
microparticle size were larger when the CaCl2 concentration
was smaller. In addition, the release behaviors of ampicillin-
loaded tail-shaped and spherical alginate microparticles were
also compared, and it was found that the tail-shaped particle
had a higher drug release rate than the spherical particle, and
this effect was more pronounced with increasing time.
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
3.1.4 Core-shell particles and microcapsules
Goran et al[80] demonstrated a glassy microcapillay device
which combined with co-flow and flow-focusing geometries
to generate controllable multiple emulsions. In their
experiments, the size-controlled droplets formed using this
device had either core/shell morphology or contained multiple
internal droplets per each outer drop, and the dominant regime
was controlled by adjusting fluid flow rate. The microcapillay
device effectively overcame the defects of PDMS-based
microfluidic devices, such as lower chemical strength, easier
swelling effect and worse functional regulation of surface
properties etc. The resultant drops could subsequently be
polymerised to produce spherical or non-spherical polymer
shells or monodisperse polymer capsules with a single or
multiple inner compartments, as well as functional vesicles
containing dissolved amphiphilic molecules or particles which
underwent self-assembly upon solvent evaporation. This
technology played a significant role in the synthesis of
functional capsule materials. Polenz et al[81] continuously
produced monodisperse polyurea microcapsules (PUMCs)
having either aqueous or nonaqueous cores with the multiple
emulsion drops formed by the reaction between an oil phase
containing isocyanate and aqueous phase containing amine as
templates through the similar microfluidic. The thickness of
PUMC shell was strongly dependent on the solubility of the
amine in the oil phase, which provided a convenient and
efficient operation mechanism for the synthesis of PUMC
shell with the thickness ranging from tens of nanometers to
several micrometers.
Huang et al[82] introduced a robust and easily assembled
capillary microfluidic device to produce double emulsions
while utilizing fluid flows from the dripping to the jetting
regime, generating a variety of drop sizes and encapsulation
Fig.6 Synthesis of monodisperse dual magnetic and thermo-responsive microcapsule using microfluidic technology[83]. (a) Schematic illustration
of the fabrication process; (b) Schematic illustration of magnetic PNIPAM core-shell microcapsules; (c) Thermo-responsive characteristics
of magnetic PNIPAM core-shell microcapsules in deionized water
combinations. They also investigated the relationship of relative
drop size with standard parameters such as the Weber, capillary,
and Reynolds numbers. An important advantage offered by this
device was the utilization of a robust ultra-high molecular
weight polyethylene (UHMWPE) scaffold, eliminating the need
for glues or expensive fittings. Furthermore, the use of glass
capillaries enhanced the solvent- resistance and impermeability
of microchannels, meanwhile, allowed for easy replacement of
broken or clogged capillaries and rapid change of the tip sizes.
This device could reliably and reproducibly generate nearly
monodisperse polymersomes in large amounts, with potential
applications in disease management, drug delivery, protein
storage, flavor protection, and so on.
Liu et al[83] introduced a glassy capillary device to prepare a
novel type of monodisperse dual magnetic and thermo-
responsive microcapsule with microfluidic-prepared quadruple-
component (O1 + O2)/W/O double emulsions as templates.
The microcapsule was composed of a thermo-responsive
microgel shell and an eccentric magnetic core as well as an
eccentric oil core. As shown in Fig.6, the microcapsule was
developed for site-specific targeted delivery and direction-
specific controlled release of hydrophobic substances. The
results showed that the poly(N-isopropylacrylamide)
(PNIPAM) microgel shell of the microcapsule could protect
the encapsulated hydrophobic drugs at temperatures lower
than the lower critical solution temperature (LCST), and
achieved the burst release of drugs when the environmental
temperature was increased higher than LCST. The eccentric
oil core provided a large inner volume for encapsulation of
hydrophobic drug molecules, while the eccentric magnetic core
made the microcapsule able to achieve not only magnetically-
guided translational movement for site-specific targeting but
also magnetically-guided rotational motion for direction-
specific controlled release.
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
Droplet-based microfluidic was widely used to prepare
monodisperse core-shell microparticles and multi-chamber
microcapsules. Moreover, the particle size, morphology,
monodispersity and shell thickness could be precisely
regulated by altering the flow rate, physical parameters and
channel geometry, etc. However, the types of synthetic
microparticles using microfluidic are still relatively limited, so
far, researchers mainly focus on partial inorganic
microspheres, all kinds of hydrogels and inorganic-organic
composite particles, which greatly limited its applications,
thus the structure types and application fields of synthetic
microparticles using microfluidic need to be further expanded.
3.2 Applications of droplet microfluidic in biomedical
analysis
With the development of droplet microfluidic, droplet-
based microfluidic also play an irreplaceable role in
applications of life sciences, biomedical analysis and other
fields, owing to the excellent operating characteristics of
microfluidic and flexible installation structure of microfluidic
systems. In particular, this technology shows significant
advantages in the application of biological screening, segment
labelling, cell packaging, virus detection and specific proteins
or tissue remodeling, etc.
3.2.1 Biological screening and segment labelling
Visaveliya et al[84] demonstrated a high throughput
approach for one-step synthesis of size and color-tuned
polytripropylene glycol diacrylate (poly-TPGDA) microparticles
with a broad size range down to the micron using
droplet-based microfluidic synthesis, as shown in Fig. 7a. The
size of the particles was strongly dependent upon the
concentration of surfactants and flow rate ratios of both
immiscible liquids. The synthetic polymer microparticles not
only had a broad library of size-tuned spectrum, but also
realized precisely adjustment of the type and concentration of
multi-fluorophore embedded with tuned composition. Figure
7b shows fluorescence poly-TPGDA microparticles of
different colors under the fluorescence microscope. The tracer
Fig.7 Simultaneous size and color tuning of fluorescence labeling polymer microparticles in a single-step microfluidic synthesis[84]. (a)
Schematic of the microfluidic set-up for the synthesis of poly-TPGDA microparticles; (b) Fluorescence microscopy images of different
dye-doped fluorescent poly-TPGDA microparticles at different emission wavelengths
dye fluorescent particles provided an effective approach for
the detection of many analytes in clinical diagnostic, drug
screening, gene expression studies, and drug discovery etc.
Therefore, amounts of microparticles were prepared for
applications in biological screening and segment labelling
through multi-fluorescence.
3.2.2 Specific proteins and tissue remodeling
Takimoto et al[85] prepared monodispersed submillimeter
microgels (100 μm–1 mm in size) by inverse suspension
polymerization in W/O droplets and molecular imprinting
strategy using a microchannel for the removal of specific
proteins. The synthesized microgels exhibited high affinity
and selective binding toward human serum albumin (HSA).
Furthermore, the microgels had several important advantages,
such as ease of synthesis, high stability, and long shelf life
compared with conventional affinity beads using antibodies,
which allowed for the use of these novel artificial affinity
microgels without any antibodies. Wu et al[86] combined
microfluidic technique and biosilicification strategy to prepare
monodisperse hybrid microcapsules with an ultrathin alginate/
protamine/silica (APSi) shell of about 420-nm thickness as
efficient carriers to encapsulate enzymes for rapid reaction.
The ultrathin-shelled APSi microcapsules showed excellent
reusability, storage stability and highly-efficient encapsulation
of model actives bovine serum albumin (about 99%) during
the fabrication process.
Yamada et al[87] demonstrated the production of cell-sized
collagen microparticles by means of droplet microfluidic
(Fig.8a). The synthesized microparticles would potentially be
useful as solid particulate scaffolds that were incorporated into
3D cellular constructs to achieve the reconstitution of
extracellular matrix (ECM) components, because of its ability
to preserve cellular functions, simplicity of operation, and
high versatility. They also found that the ratio of the cells to
particles was critical in terms of the improvement of hepatic
functions in the composite spheroids, and hepatocyte-specific
functions were obviously upregulated when the ratios of the
particles and cells were equal. Griffin et al[88] produced
uniform microsphere scaffold building blocks by microfluidic
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
Fig.8 Microfluidic technology to achieve tissue remodeling[87]. (a) Schematic illustration showing the microfluidic process for producing
collagen microparticles[87] ; (b) Microfluidic generation of microsphere hydrogel building blocks for the creation of microporous annealed
particle (MAP) scaffolds[88]
technique to improve tissue regeneration, organ-on-a-chip
methods, as well as stimulating clinical research and
applications in wound healing (Fig.8b). In their experiment,
the chemical and physical properties of the scaffold were
tailored through microfluidic fabrication, and the
microporosity of the scaffold was modulated by the size of
building blocks, which were precisely controlled by the flow
rate and geometry of the microfluidic device.
3.2.3 Cell encapsulation and virus detection
Akbari et al[89] developed an improved internal gelation
approach combined microfluidic method to encapsulate single
mammalian cells in monodisperse alginate microbeads as
small as 26 µm in diameter and at rates of up to 1 kHz with
high cell viability. Moreover, the cells were functional and
continued to grow inside the microparticles. The cell damage
resulting from contact with calcium carbonate nanoparticles as
gelation reagents was eliminated by employing a co-flow
microfluidic device, and the cell exposure to low pH was
minimized by a chemically balanced off-chip gelation step.
Hu et al[90] developed an approach by which different cell
types were stained with different fluorescent dyes. Subsequent
to encapsulation into droplets, the resulting emulsion was
injected into a very compact sorting device allowing for
analysis at high magnification and fixation of the cells close to
the focal plane. By applying dual-color sorting, this technique
not only enabled the specific collection and analysis of
droplets with exactly two different cells, but also paved the
way for a variety of cell-based assays in droplets.
As shown in Fig.9, Tao et al[91] developed a drop-based
culture-free microfluidic method for rapid, low-cost and highly
accurate targeted detection of viral infectivity by combining the
advantages of plaque-based assay and real-time quantitative
polymerase chain reaction (qPCR). Both replication and
detection of single infectious viruses were undergone in
microdroplets to ensure the reliability of a single infection event.
They coencapsulated single infectious viruses with host cells
into a large number of picoliter-sized drops and incubated them
for the duration of one viral replication cycle. The drops were
then combined with a gene-specific PCR cocktail that
fluoresced in the presence of replicated target viruses, and
quantified using a custom-built high-throughput drop reader to
determine the number of viral infections. They also compared
their results with the conventional plaque- based infectivity
assay and further demonstrated the utility of this technique by
determining the effectiveness of a viral neutralizing antibody.
Moreover, this technique was also adapted to measuring the
infectivity of other pathogens, such as bacteria and fungi.
Compared with traditional bioanalytical method,
microfluidic technology is easy to integrate design, by which
microfluidic is not only build a better simulation environment
for the growth of liver cells in vitro platform, complete
quantitative detection and analysis, but also provides a new
approach for the positioning, handling and observing of living
cells. However, most of the research works were directed
against a single microchannel structure at this stage, which
cause lower utilization rate and more inefficiency of
microfluidic devices for preparing microdroplets/
microparticles. To complete mass production of morphology
and size-controlled microdroplets/microparticles, which are
widely used in bioscience and disease treatment, more about
cutting manufacturing costs, improving synthetic efficiency
need further in-depth research.
3.3 Applications of droplet microfluidic in food
processing
By means of droplet-based microfluidic, more elaborated
food structures were designed including microemulsions,
microparticles, self-assemblies and microcapsules with one or
more cores inside. They were not only used to fabricate low-
fat foods, modify the texture and flavor perception in a food
product and avoid oxidation of bioactive compounds, but also
played a significant role in effective encapsulation and
controlled releasing of the active/functional compounds to
prevent from interference of internal enzymes and other
gastrointestinal adverse conditions (such as ions concentration
and pH, etc.)[92]. Therefore, in food industry, this technology
provides an effective method for synthesizing complex
microemulsions/microparticles at well-defined morphology
and dimensions which can be precisely adjusted.
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296

Fig.9 Workflow of drop-based viral infectivity assay[91]. (a) Schematic description of the assay; (b) viruses (V) and host cells (C) are
co-encapsulated in oil (O) using a microfluidic drop-making device; (c) an image of the resulting drops showing that each contain about
1‒2 cells; (d) after incubation, drops are re-injected into the“split and inject” device; (e) after off-chip in-drop amplification the drops
remain monodisperse (left), those containing viral amplicons fluoresce at 520 nm (middle) and those containing tracer Rhodamine
fluorescence at 586 nm (right); (f) the drops are re-injected into a microfluidic drop reader device. All scale bars are 100 μm

3.3.1 Microemulsion droplets production of a double emulsion with two different

Microemulsion droplets play an important role in food
industry[92–94], such as mayonnaise and dressings produced in
the form of oil-in-water (O/W) emulsions, or butter, margarine
and yogurts etc. synthesized with water-in-oil (W/O)
emulsions. Currently, conventional methods of emulsification,
such as highpressure homogenizers, high-speed mixers, etc,
do not allow a precise control in the particle size distribution,
resulting in highly polydisperse emulsions. Furthermore, in
order to accelerate the breakup of droplets, high shear stress is
applied in the system, which can cause proteins denaturation,
degradation or loss of activity in thermo- or shear-sensible
compounds. However, microfluidic, as an alternative
technology, not only can be applied to the production of
highly monodisperse microemulsion droplets or microparticles
in the range from tens to hundreds of micrometers, but also be
employed in vehicles for bioactive compounds.
Okushima et al[96] demonstrated a novel method for
preparing monodisperse W/O/W double emulsions using a
two-step method of droplet formation with two successive
T-junctions (Fig.10a). The desired number of internal
droplets in larger drops was adjusted by altering the breakup
rates of internal and external droplets. Moreover, the
compositions in the internal phase was performed using a
cross-junction geometry in the first step. Abate et al[97]
presented a simple system to form monodisperse high-order
double, triple and up to indefinitely order emulsions in
sequential cross-junction along a microchannel by alternating
wettability between the junctions (Fig.10b), they also
adjusted the morphology and structure of emulsions by
controlling the flow pattern. This method was especially
useful in breaking up viscoelastic fluids, which normally did
not detach droplets easily, however, the precise modification
of junctions’ wettability to ensure the efficient packaging of
hydrophilic/hydrophobic phases would obviously increase the
difficulty of microfluidic system’s processing. Therefore,
glassy capillary microfluidic system was more widely used to
produce core-shell emulsions with controlled thickness and
multiple emulsions with different numbers or compositions of
internal droplets[98,99].
3.3.2 Microparticles
Microparticles of several to hundreds of micrometers can be
generated based on the solidification of droplets of single or
multiple emulsions through microfluidic[100]. Generally, the

Fig.10 Synthesis of microemulsion droplets using microfluidic technology. (a) Basic concept for preparing double emulsions (W/O/W) using
T-shaped microchannels[96]; (b) Drop maker arrays used to produce multiple emulsions with controlled order[97]
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
microparticles have more narrow particle size distribution and
more uniform mechanical properties[101]. The solidification of
the droplets increases the system stability and protects the
compound from external agents (oxygen, light and reacting
environment, etc.). Moreover, the release of the compound in
the target site can be achieved by the exposition of the
microparticle in a specific condition (temperature, pH and
presence of enzymes, etc.).
Shintaku et al[102] developed a novel microfluidic device for
the cell encapsulation and the hydrogel-beads production
using W/O (water in oil) in a microchannel (Fig.11a). The
gelation was completed through the droplets coalescence
based on the collision of a droplet containing the biopolymer
solution with another droplet containing the cross-linking ion.
In this method, the continuous oil phase did not use any
surfactant, because the coalescence of the droplets was
desirable. One of the disadvantages of this method was the
difficulty in producing well-defined and homogeneous
microbeads if the gelation occurred before the stabilization of
the droplet after the coalescence, resulting in higher particle
size polydispersity and larger deformation coefficient. Ren et
al[103] prepared O/W/O double emulsion templates with
microfluidic technology, and then added a crosslinking agent
aqueous solution to the downstream after the droplets
formation, so the biopolymers reacted with the crosslinking
ion at the interface of the oil and aqueous stream to obtain
monodisperse alginate microcapsules with oil cores (Fig.11b).
When droplet-based microfluidic is used in food processing,
the whole operation is under strict laminar flow conditions, so
it’s very suitable for precise regulation of the whole flow
process. However, the current study mainly focuses on the
design and regulation of the synthetic particle size,
morphology, monodispersity and internal chamber structure,
etc. While the mechanics theory, flow regularity, reaction
mechanism of two-phase interface and mass-transport and
heat-transport properties, etc, involved in the preparation
process of microemlsions/microparticles still need to be
further studied. In addition, further in-depth research about
droplet-based microfluidic technology need to be developed to
meet the applications for designing structures in the food
industry, controlled encapsulating and releasing of biological
Fig.11 Synthesis of microparticles using microfluidic technology. (a) Schematic of microfluidic device to produce hydrogel-beads containing
living cells[102]; (b) Schematic illustration of the capillary microfluidic device for fabricating monodisperse alginate microcapsules with
oil core[103]
active ingredients, as well as preparing structure-sensitive
food material, and so on.
4 Conclusions
This review provided a comprehensive droplet-based
microfluidic fundamentals, droplet generation and droplet
manipulations. The similarities and differences of droplets’
conventional preparation methods and droplet-based
microfluidic technology were compared and analyzed. The
applications of droplet-based microfluidic for the synthesis of
functional materials, bio-medicine and design of food structure
were also discussed as a showcase of their wide rang
applications. The main conclusions are as follows: (1)
Droplet-based microfluidic technology has dimensional scaling
benefits that have enabled precise control, easy operation and
rapid extension of fluids in the droplet reactors. The advantages
of droplet microfluidic systems effectively overcome the
shortcomings of the conventional methods, and have been
widely used to produce microdroplets with excellent control of
size, composition, and morphology, as well as size distribution.
In addition, this technology makes it possible to synthesis
multi-emulsion droplets or composite microparticles with
specific structure morphology and functional properties. (2)
Droplet-based microfluidic technology exhibits great
application prospects in the fields of functional materials
synthesis, biomedical engineering, food processing, and so on.
To further promote the technological innovation and industrial
applications in drug delivery, cell encapsulation, to chemical
analysis, disease treatment, etc., the detailed mechanics, flow
characteristics and other theories of droplets’ formation and
solidification need to be deeply studied. (3) Droplet-based
microfluidic technology is still in an infantile stage, the
adjustable range of synthesized microdroplets/microparticles
with various sizes, shapes, compositions, size distributions and
functional characteristics still cannot fully meet the needs of
practical applications. Therefore, further research is also needed
to find novel methods that are more economical, environmental
and suitable to be industrialized to achieve continuous or batch
preparation of multi-emulsion droplets or microparticles with
complex structures and functions at lower prices.
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
References
[1] Whitesides G M. Nature, 2006, 442(7101): 368–373
[2] Lin B C, Qin J H. Graphic Laboratory on a Microfluidic Chip.
Beijing: Science Press, 2008: 2–86
[3] Shen F, Li Y, Liu Z M, Cao R T, Wang G R. Chinese J. Anal.
Chem., 2015, 43(12): 1942–1954
[4] Chen X D, Hu G Q. Advances in Mechanics, 2015, 45: 55–110
[5] Li Z H, Wu J K, Hu G Q, Hu G H. Fluid Flow in Microfluidic
Chips. Science Press, 2012: 12–58
[6] Lin B C, Qin J H. Micro-nano Fluidic Laboratory. Beijing:
Science Press, 2013: 153–175
[7] Teh S Y, Lin R, Hung L H, Lee A P. Lab Chip, 2008, 8(2):
198–220
[8] Belder D. Angewandte Chemie International Edition, 2005,
44(23): 3521–3522
[9] Cunha A G, Mougel J B, Cathala B, Berglund L A, Capron I.
Langmuir the Acs Journal of Surfaces & Colloids, 2014, 30(31):
9327–9335
[10] Williams M, Warren N J, Fielding L A, Armes S P, Verstraete P,
Smets J. Acs Applied Materials & Interfaces, 2014, 6(23):
20919-20927
[11] Ohno K I, Tachikawa K, Manz A. Electrophoresis, 2008,
29(22): 4443–4453
[12] Vincent M E, Liu W, Haney E B, Ismagilov R F. Chemical
Society Reviews, 2010, 39(39): 974–984
[13] Deng N N, Wang W, Ju X J, Xie R, Liu Z, Chu L Y. Scientia
Sinica Chimica, 2015, 45(1): 7–15
[14] Xu Q, Nakajima M, Ichikawa S, Nakamura N, Shiina T.
Innovative Food Science & Emerging Technologies, 2008, 9(4):
489–494
[15] De Geest B G, Sanders N N, Sukhorukov G B, Demeester J, De
Smedt S C. Chemical Society Reviews, 2007, 36(4): 636–649
[16] Pechenkin M A, Möhwald H, Volodkin D V. Soft Matter, 2012,
8(33): 8659–8665
[17] Kukizaki M, Wada T. Colloids & Surfaces A Physicochemical
& Engineering Aspects, 2008, 317(1-3): 146–154
[18] Tian R, Wang L Y, Wu J, Zhang J, Zeng Y J, Ma G H. The
Chinese Journal of Process Engineering, 2009, 9(4): 754–762
[19] Ma G H, Omi S. Macromolecular Symposia, 2002, 179(1):
223–240
[20] Freger V. Langmuir, 2003, 19(11): 4791–4797
[21] Zhu H, Szymczyk A, Balannec B. Journal of Membrane
Science, 2011, 379(1-2): 215–223
[22] Esserkahn A P, Odom S A, Sottos N R, White S R, Moore J S.
Macromolecules, 2011, 44(14): 5539–5553
[23] Wang W, Xie R, Ju X J, Chu L Y. Journal of Chemical Industry
and Engineering, 2014, 65(7): 2555–2562
[24] Farook U, Zhang H B, Edirisinghe M J, Stride E, Saffari N.
Medical Engineering & Physics, 2007, 29(7): 749–754
[25] Brugarolas T, Tu F, Lee D. Soft Matter, 2013, 9(38):
9046–9058
[26] Lee M, Lee E Y, Lee D, Park B J. Soft Matter, 2015, 11(11):
2067–2079
[27] Kooiman K, Vos H J, Versluis M, Jong N D. Advanced Drug
Delivery Reviews, 2014, 72(22): 28–48
[28] Jang W, Nikolov A, Wasan D T. Journal of Food Engineering,
2006, 76(2): 256–260
[29] Zhao C X, He L, Qiao S Z, Middelberg A P J. Chemical
Engineering Science, 2011, 66(7): 1463–1479
[30] Guo S, Yin S N, Pan Y C, Chen S, Zhang L X. Scientia Sinica
Chimica, 2015, 45(1): 24–33
[31] Wang W, Xie R, Ju X J, Luo T, Liu L, Weitz D A, Chu L Y. Lab
Chip, 2011, 11(9): 1587–1592
[32] Chu L Y, Utada A S, Shah R K, Kim J W, Weitz D A. Angewandte
Chemie International Edition, 2007, 46(47): 8970–8974
[33] Zhou J, Khodakov D A, Ellis A V, Voelcker N H.
Electrophoresis, 2012, 33(1): 89–104
[34] Mcdonald J C, Whitesides G M. Cheminform, 2002, 33(38):
491–499
[35] Qin D, Xia Y, Whitesides G M. Nature Protocol, 2010, 5(3):
491–502
[36] Abate A R, Krummel A T, Lee D, Marquez M, Holtze C, Weitz
DA. Lab on Chip, 2008, 8(12): 2157–2160
[37] Baah D, Tigner J, Bean K, Walker N, Britton B, Floyd-Smith T.
Microfluidic & Nanofluidics, 2011, 12(1-4): 657–662
[38] Ying D, Helgeson M E, Myerson A S, Hatton T A, Doyle P S,
Trout B L. Journal of the American Chemical Society, 2011,
133(11): 3756–3759
[39] Si T, Yin X Z. Science China Press, 2011, 56(8): 537–546
[40] Thorsen T, Roberts R W, Arnold F H, Quake S R. Physical
Review Letters, 2001, 86(18): 4163–4166
[41] Fu T, Wu Y, Ma Y, Li H Z. Chemical Engineering Science,
2012, 84(52): 207–217
[42] Liu Z M, Liu L K, Shen F. Journal of Mechanical Engineering,
2014, 50(8): 189–196
[43] Dreyfus R, Tabeling P, Willaime H. Physical Review Letters,
2003, 90(14): 144505–144509
[44] Gañán A M. Journal of Aerosol Science, 1999, 30(1): 117–125
[45] Utada A S, Chu L Y, Fernandez-Nieves A, Link D R, Holtze C,
Weitz D A. Mrs Bulletin, 2007, 32(9): 702–708
[46] Utada A S, Fernandez-Nieves A, Gordillo J M, Weitz D A.
Physical Review Letters, 2008, 100(1): 145–150
[47] Chen X, Glawdel T, Cui N, Ren C L. Microfluidic &
Nanofluidics, 2014, 18(5-6): 1341–1353
[48] Tarchichi N, Chollet F, Manceau J F. Microfluidic &
Nanofluidics, 2013, 14(1-2): 45–51
[49] Castro-Hernández E, García-Sánchez P, Tan S H, Gañán-Calvo
A M, Baret J C, Ramos A. Microfluidic & Nanofluidics, 2015,
19(4): 1–8
[50] Kunstmann-Olsen C, Hoyland J D, Rubahn H G. Microfluidic
& Nanofluidics, 2012, 12(12): 795–803
[51] Luo G S, Lan W J, Li S W, Xu J H, Lü Y C. Petrochemical
Technology, 2010, 39(1): 1–6
[52] Bremond N, Thiam A R, Bibette J. Physical Review Letters,
2008, 100(2): 024501–024504
 LIU Zhao-Miao et al. / Chinese Journal of Analytical Chemistry, 2017, 45(2): 282–296
[53] Niu X, Gulati S, Edel J B, Demello A J. Lab Chip, 2008, 8(11):
1837–1841
[54] Abate A R, Weitz D A. Lab Chip, 2011, 11(11): 1911–1915
[55] Liau A, Karnik R, Majumdar A, Cate J H. Anal. Chem. 2005,
77(23): 7618–7625
[56] Edgar J S, Milne G, Zhao Y, Pabbati C P, Lim D S W, Chiu D T.
Angewandte Chemie InternationalEdition, 2009, 48(15):
2719–2722
[57] Huebner A, Bratton D, Whyte G, Yang M, Demello A J, Abell C,
Hollfelder F. Lab Chip, 2009, 9(5): 692–698
[58] Wang J Y, Wang Y J, Luo G S. Chinese Journal of Chemical
Engineering, 2014, 22(11-12): 1352–1356
[59] Ding X Q, Zhang C, Dong L M, Wang C, Liang T X. Journal of
Inorganic Materials, 2015, 30(6): 605–609
[60] Wacker J B, Lignos I, Parashar V K, Gijs M A M. Lab Chip,
2012, 12(17): 3111–3116
[61] Yang Y, Zhu J, Wang X, Wang J, Li Z, Luo X, Zhang L.
Journal of Materials Science, 2015, 50(10): 3638–3645
[62] Teshima M, Seki T, Kawano R, Takeuchi S, Yoshioka S,
Takeoka Y. J. Mater. Chem. C, 2015, 3(4): 769–777
[63] Zhao H, Xu J H, Wang T, Luo G S. Lab Chip, 2014, 14(11):
1901–1906
[64] Wang W T, Chen R, Xu J H, Wang Y D, Luo G S. Rsc
Advances, 2014, 4(32): 16444–16448
[65] Liu Y M, Ju X J, Xin Y, Zheng W C, Wang W, Wei J, Xie R,
Liu Z, Chu L Y. Acs Applied Materials & Interfaces, 2014,
6(12): 9530–9542
[66] Seo M, Matsuura N. Langmuir, 2014, 30(42): 12465–12473
[67] Yang S, Guo F, Kiraly B, Mao X, Lu M, Leong K W, Huang T I.
Lab Chip, 2012, 12(12): 2097–2102
[68] Nisisako T, Torii T. Advanced Materials, 2007, 19(11):
1489–1493
[69] Prasad N, Perumal J, Choi C, Lee C, Kim D. Advanced
Functional Materials, 2009, 19(10): 1656–1662
[70] Kai P Y, Hwang D K, Haghgooie R, Doyle P S. Langmuir the
Acs Journal of Surfaces & Colloids, 2010, 26(6): 4281–4287
[71] Lee K J, Yoon J, Lahann J. Current Opinion in Colloid &
Interface Science, 2011, 16(3): 195–202
[72] Seiffert S, Romanowsky M B, Weitz D A. Langmuir the Acs
Journal of Surfaces & Colloids, 2010, 26(18): 14842‒14847
[73] Lone S, Cheong I W. Rsc Advances, 2014, 4(26): 13322–13333
[74] Lone S, Kim S H, Nam S W, Park S, Joo J, Cheong I W. Chem.
Commun., 2011, 47(9): 2634–2636
[75] Skelhon T S, Chen Y, Bon S A. Soft Matter., 2014, 10(39):
7730–7735
[76] Dendukuri D, Pregibon D C, Collins J, Hatton T A, Doyle P S.
Nature Materials, 2006, 5(5): 365–369
[77] Xu S, Nie Z, Seo M, Lewis P, Kumacheva E, Stone H A,
Garstecki P, Weibel D B, Gitlin I, Whitesides G M. Angewandte
Chemie, 2005, 44(5): 724–728
[78] Yang C H, Wang C Y, Huang K S, Kung C P, Chang Y C, Shaw
J F. International Journal of Pharmaceutics, 2014, 463(2):
155–160
[79] Lin Y S, Yang C H, Hsu Y Y, Hsieh C L. Electrophoresis, 2013,
34(3):425‒431
[80] Goran T V, Shum H C, Weitz D A. Progress in Colloid &
Polymer Science, 2011, 139: 115–118
[81] Polenz I, Datta S S, Weitz D A. Langmuir the Acs Journal of
Surfaces & Colloids, 2014, 30(44): 13405–13410
[82] Huang Y S, Bento J L, Stredney M A, Napoli O J, Adamson D
H. Microfluidic & Nanofluidics, 2014, 18(1): 149‒157
[83] Liu Y M, Wu W, Ju X J, Wang W, Xie R, Mou C L, Zheng W C,
Liu Z, Chu L Y. Rsc Advances, 2014, 4(87): 46568–46575
[84] Visaveliya N, Kohler J M. Journal of Materials Chemistry C,
2014, 3(4): 844–853
[85] Takimoto K, Takano E, Kitayama Y, Takeuchi T. Langmuir,
2015, 31(17): 4981–4987
[86] Wu F, Wang W, Liu L, Ju X J, Xie R, Liu Z, Chu L Y. Journal
of Materials Chemistry B, 2014, 3(5): 796–803
[87] Yamada M, Hori A, Sugaya S, Yajima Y, Utoh R, Yamato M,
Seki M. Lab on A Chip, 2015, 15(19): 3941–3951
[88] Griffin D R, Weaver W M, Scumpia P O, Di C D, Segura T.
Nature Materials, 2015, 14(7): 1–25
[89] Akbari S, Pirbodaghi T. Microfluidic & Nanofluidics, 2014,
16(4): 773–777
[90] Hu H, Eustace D, Merten C A. Lab Chip, 2015, 15(20): 3989–3993
[91] Tao Y, Rotem A, Zhang H, Chang C B, Basu A, Kolawole A O,
Koehler S A, Ren Y, Lin J S, Pipas J M, Feldman A B, Wobus C
E, Weitz D A. Lab Chip, 2015, 15(19): 3934–3940
[92] Neethirajan S, Kobayashi I, Nakajima M, Wu D, Nandagopal S,
Lin F. Lab Chip, 2011, 11(9): 1574–1586
[93] Capretto L, Carugo D, Mazzitelli S, Nastruzzi C, Zhang X.
Advanced Drug Delivery Reviews, 2013, 65(11-12): 1496–1532
[94] Duncanson W J, Lin T, Abate A R, Seiffert S, Shah R K, Weitz
D A. Lab Chip, 2012, 12(12): 2135–2145
[95] Lo C T, Jahn A, Locascio L E, Vreeland W N. Langmuir the
Acs Journal of Surfaces & Colloids, 2010, 26(11): 8559–8566
[96] Okushima S, Nisisako T, Torii T, Higuchi T. Langmuir the Acs
Journal of Surfaces & Colloids, 2004, 20(23): 9905–9908
[97] Abate A R, Weitz D A. Small, 2009, 5(18): 2030–2032
[98] Lyu S R, Chen W J, Hsieh W H. Sensors & Actuators B
Chemical, 2014, 197(3): 28–34
[99] Utada A S, Lorenceau E, Link D R, Kaplan P D, Stone H A,
Weitz D A. Science, 2005, 308(5721): 537–541
[100] Kim S C, Sukovich D J, Abate A R. Lab Chip, 2015, 15(15):
3163–3169
[101] Ushikubo F Y, Oliveira D R B, Michelon M, Cunha R L. Food
Engineering Reviews, 2015, 7(4): 393–416
[102] Shintaku H, Kuwabara T, Kawano S, Suzuki T, Kanno I, Kotera
H. Microsystem Technologies, 2007, 13(8-10): 951–958
[103] Ren P W, Ju X J, Xie R, Chu L Y. Journal of Colloid &
Interface Science, 2010, 343(1): 392–395