Article

pubs.acs.org/Langmuir

Droplet Motion on a Shape Gradient Surface

Yanfen Zheng, Jiang Cheng,* Cailong Zhou, Haiting Xing, Xiufang Wen, Pihui Pi, and Shouping Xu
School of Chemistry and Chemical Engineering, South China University of Technology, Guangzhou 510640, People’s Republic of
China
*
S Supporting Information

ABSTRACT: We demonstrate a facile method to induce water droplet motion on an

wedge-shaped superhydrophobic copper surface combining with a poly-
(dimethylsiloxane) (PDMS) oil layer on it. The unbalanced interfacial tension from
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the shape gradient offers the actuating force. The superhydrophobicity critically
eliminates the droplet contact line pinning and the slippery PDMS oil layer lubricates
the droplet motion, which makes the droplet move easily. The maximum velocity and
furthest position of droplet motion were recorded and found to be influenced by the
gradient angle. The mechanism of droplet motion on the shape gradient surface is
systematically discussed, and the theoretical model analysis is well matched with the
experimental results.

■ INTRODUCTION
Droplet microfluidics technology continues to attract consid-
erable research interest due to many potential applications such
as DNA sequencing,1 single-cell analysis,2,3 and microchemical
reactors4 where minimal consumption of reagents can be
performed. Recent efforts have been made to induce droplet
motion onto a solid surface based on unbalanced interfacial
tension via chemical,5−7 thermal,8 thermocapillary,9 photo-
chemical,10 and electrokinetic11 methods. Popular approaches
also realize droplet motion by spatially altering surface shape
through physical texturing,12−15 chemical patterning,16−19 or a
composite interface of both.20 Commonly irregular shapes are
patterned such as wedge13,14,17,21−23 and star shapes24 which
contain interfacial tension gradients so that droplets can be
transported in a predetermined direction. Contact angle
hysteresis is the major hurdle for droplet motion which
decelerates or even stops droplet motion. Although a droplet
can wet and rapidly spread onto the crevices of structured
surfaces due to capillary force, the back end of a droplet pins at
the gradient’s start,13,14,21−23 causing surface contamination by
impurities and reagent loss.
Grafting polymer chains onto surfaces25,26 or slippery liquid-
infused porous surfaces (SLIPS)27−31 were reported for
eliminating pinning spots on the surface and obtaining a low
contact angle hysteresis. Either air or infused liquid is locked in
solid surfaces and blocks the contact of other liquids (droplets)
with the underlying solid so that discrete droplets move
smoothly. Similarly, lubricating oil film is also used in
electrowetting in microfluidic devices.32,33 The droplets are
commonly manipulated in a continuous phase of immiscible oil,
where oil has several roles including facilitating the isolation of
biomolecules, lubricating droplet motion, and eliminating cross-
contamination caused by surface interactions.
Since the irregular shape surface can provide an interfacial
tension gradient and hence induce droplet spreading, while oil
film can exhibit a low contact angle hysteresis, we propose a
simple approach to realize discrete droplet motion (without the
back end of droplet pinning) horizontally and obliquely on the
wedge-shaped copper substrate combining superhydrophobic-
ity with a poly(dimethylsiloxane) (PDMS) oil layer. Super-
hydrophobicity of the modified copper surface ensures PDMS
oil wetting the surface and the water droplet does not contact
directly with the substrate; thus the back-end pinning on the
surface in precious works is eliminated so that the droplet can
move forward maintaining the shape of a spherical crown under
the lubrication of slippery PDMS oil. Droplet deposited on the
narrow end of the shape gradient surface obtains actuation
force from boundary compressing, and its contact line moves
toward the decreasing interfacial tension direction.
The maximum velocity and furthest position from the origin
(taking the intersection of two boundary sides of the wedge as
the origin) of droplet motion are found to be influenced by the
wedge-shaped gradient head angle α. Here, we discuss the
mechanism and develop a simple formula behind the droplet
motion. Besides the single shape gradient inducing droplet
motion, we demonstrate handling droplet combination via
multiple shape gradients. The results of droplets moving and
mixing show great prospects in open microfluidic systems, lab
chips, and microchemical reactors.
■ EXPERIMENTAL SECTION
Copper foil was cut into a wedge-shaped piece (0.8 mm width of
gradient start × 23.8 mm length × 5.0 mm width of gradient end) and
Received: February 8, 2017
Revised: April 10, 2017
Published: April 11, 2017

© 2017 American Chemical Society 4172 DOI: 10.1021/acs.langmuir.7b00227

Langmuir 2017, 33, 4172−4177
Langmuir Article

Figure 1. (a) Schematic diagram of droplet on unmodified copper substrate only covered with PDMS oil and SEM image of substrate. (inset) Side
view showing droplet pinning on the substrate. (b) Schematic diagram of droplet on CuO surface only covered with PDMS oil and the SEM image
of CuO surface. (inset) Side view showing droplet pinning on the surface. (c) Schematic diagram of droplet on CuO surface modified with both
FAS-17 and PDMS oil in sequence. Side view demonstrating the low surface hysteresis with a sliding angle of 3°. (d) Top view of droplet moving
horizontally along the gradient on such surface.

Figure 2. Sequent captures of 5 μL water droplet moving on (a) a horizontal gradient surface and (b) an inclined (10°) gradient surface with the
gradient angle of both surfaces of α = 12°. (c) Experimental and predicted position evolutions of a 5 μL water droplet on horizontal surface with α =
6° and 12°. (inset) Table displays the maximum position and velocities of water droplets motion on different gradients. (d) Experimental and
predicted position evolutions of a 5 μL water droplet on an oblique surface at inclination angle of 10° with α = 12°.

cleaned several times by consecutive ultrasonication in acetone, dilute motion on the oil layer was performed by placing a 5 μL distilled water
hydrochloric acid, and distilled water for 10 min at room temperature. droplet onto the prepared sample and subsequent recording with a
The cleaned copper foil was immersed into a mixed aqueous solution high speed camera (Germany Baumer HXC20c) at 330 frames per
of 2.67 mol/L NaOH and 0.133 mol/L (NH4)2S2O8 for 2 h to form second (fps).

CuO structures.34 The reacted copper foil was then washed several
times with distilled water and dried in N2. Superhydrophobization of
the copper surface was carried out by immersing the foil into 1 wt %
1H,1H,2H,2H-perfluorodecyltrimethoxysilane (FAS-17) for 5 min and
subsequent sintering under 120 °C. Finally, an excess amount of
PDMS oil (η = 9.35 mPa·s) was applied onto the modified copper
surfaces. The liquids were maintained on the surfaces overnight to fully
saturate the microstructure. Afterward, samples were tilted vertically
for 2 h to get rid of the excess of oil lubricant before use in the
experiments. We also prepared a series of shape-gradient samples (0.8
mm width of the gradient start × 5.0 mm width of the gradient end)
with different head angles α (6, 8, 10, and 12°).
The morphology of the superhydrophobic copper surface was
characterized by scanning electron microscopy (SEM). The contact
angle was determined using a contact angle analyzer (Shanghai
Zhongchen Powereach JC2000C1) at ambient temperature. The liquid
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■
RESULTS AND DISCUSSION
Effect of Surface Modification. Droplet behaviors were
observed in succession on the unmodified naked copper
surface, CuO surface, and FAS-17 modified CuO surface on
copper substrate, all covered with PDMS oil. The droplet
adheres on the unmodified copper substrate covered with
PDMS oil layer even when the substrate is rotated 90° (Figure
1a). Since the oil phase does not wet the naked copper surface,
the droplet touches the surface directly presenting in Wenzel
state.35 Figure 1b displays the SEM image of cabbagelike CuO
structures on the copper substrate with the size of these
particles of approximately 5 μm. The droplet still pins on the
formed CuO surface covered only with PDMS oil layer due to
DOI: 10.1021/acs.langmuir.7b00227
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Langmuir
Figure 3. (a) Schematic diagram of droplet aggregation. (b)−(i) Aggregation and motion of droplets on horizontally positioned multiple shape
gradients.
Figure 4. (a) Side view schematic diagram of forces acting on advancing droplets. (b) Top view schematic diagram of the interfacial tension profile
along the shape gradient. (c) Contact angle (CA) and cosine of contact angle as a function of the radius on circular plates. The typical droplet
profiles are shown on the upper side.
the same wetting state. However, after the CuO surface is
modified with FAS-17 and further covered with PDMS oil, the
droplet moves rashly with a low sliding angle (3°) indicating
the key role of FAS-17 modification to eliminate the contact
line pinning33 (Figure 1c). Surfaces fabricated with FAS-17
became strongly hydrophobic, ensuring the oil phase wets the
hydrophobic surface and water droplet does not contact CuO
particles directly. With the combination of the super-
hydrophobicity of FAS-17 and lubrication of the oil layer, the
droplet displays high mobility on the copper substrate. The
shape gradient surface offers gradient interfacial tension to
induce droplet motion in desired directions. Due to elimination
of contact line pinning and lubrication by oil, the deposited
droplet moves horizontally along the axis of the gradient wedge
surface (Figure 1d).
Droplet Motion. Parts a and b of Figure 2 present the
displacement−time profiles of a droplet moving along a
horizontal surface and a 10° tilted substrate with α = 12°,
respectively. The droplet is deposited on the narrow end of a
wedge track, with the width of 0.8 mm significantly narrower
than the droplet diameter (∼2.7 mm). Therefore, the droplet is
constricted in the transverse direction by the shape boundary
and moves lengthwise along the wedge track from a tighter
footprint to a larger one. The droplet accelerates initially and
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gradually slows down resulting from the reducing actuating
force and the resistances along the gradient surface. The
corresponding position evolutions along the horizontal and
oblique gradients from the experimental data and model
prediction are displayed in Figure 2, parts c and d, respectively.
The point of intersection of the substrate boundary is set as the
origin. The maximum velocity on horizontal surfaces for α =
6−12° increases from 4.0 to 14.0 mm/s, whereas the furthest
position from its corresponding origin decreases from 15.8 to
12.1 mm, respectively. Experiments performed on the oblique
gradient (tilted 10°) show that the gravity affects droplet
motion where the velocity for α = 12° decreases from 14.0 to
4.1 mm/s and the position from 12.1 to 5.7 mm, compared
with the horizontal gradient. Apparently, a larger gradient angle
produces a significantly larger gradient interfacial tension in the
x-direction; as a result, the droplet presents a higher velocity
and stops at a nearer position whereas the narrower gradient
angle is the opposite.
Droplet Aggregation Using Multiple Shape Gradients.
Based on the single wedge-shaped track, a more complicated
shape was designed to drive aggregation of individual droplets
and move forward in a specified direction (Movie S1). The
substrate in the video was horizontally positioned. The shape
gradient exists on each section of track as demonstrated in
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Langmuir Article

Figure 3a. When the first probe droplet is deposited onto the α π /2 + α /2 ⎛ α⎞
narrow end of the first section of track, it moves fast toward the Fix = 4γ sin
2
∫φ r cos θr sin⎜φ − ⎟ dφ
⎝ 2⎠
1
wider transverse and can even turn a corner to the second
section of track, the width of which is slightly greater than the α⎡ α 2 ⎛ φ1 α⎞
= 4γ sin 2 ⎢ −a1 sin x ln tan⎜⎝ − ⎟
radius of a single droplet (∼1.35 mm) as shown in Figure 3b,c. 2 ⎣ 2 2 4⎠
The second probe droplet then appears, repeats the steps, and ⎛π α ⎞ ⎤
aggregates with the first droplet at the second track. The radius + a 2x ⎜ + − φ1⎟⎥
⎝2 2 ⎠⎦ (4)
of the combined droplet increases to nearly 1.71 mm, which
enables the droplet to sustain the unbalanced interfacial tension ⎡ R2 α α ⎤
and keep going as demonstrated in Figure 3d,e. The sequent 1 −1⎢ 2
φ1 = cos ⎢
(
1 − tan 2 2 − x 2 tan 2 ) 2 ⎥
combinations for three or more droplets can be followed from 2 R2 α ⎥
the other branches as displayed in Figure 3f−i. Therefore, ⎢⎣ 2
1 + tan 2 2 ( ) ⎥⎦ (5)
simultaneous or successive combination of droplets and droplet
motion in a specified direction can be operated via designing where φ1 represents the initial polar angle at the front of the
the dimension of tracks which may have potential application in droplet.
Drag Force. Considering oil flowing with a low Reynolds
open microfluidics systems.
number (<5) regime of unseparated flow, the drag force of a
Theoretial Prediction of Droplet Motion. The droplet
droplet encircled by an oil layer can be approximated as
motion on the wedge-shaped gradient surface can be explained
by a simple model such as eq 1 (Figure 4a). The temporal dx
fd = −kRη1
evolution of the total momentum P of the droplet is based on dt (6)
Newton’s equation:
where R is the droplet base radius, η1 is the viscosity of PDMS
2 oil, and k is a dimensionless constant which can be determined
dP dx
= ρV 2 = Fix + fd + fs + fg experimentally (Supporting Information).
dt dt (1) Sliding Friction. The sliding friction from the droplet
bottom touching with oil layer can be approximated by
where ρ is the liquid density and V is the droplet volume. The assuming Coulomb’s friction and described as
actuation force, Fix, is the resultant of interfacial tension
components in the lengthwise direction, while fd is the drag fs = −μρVg cos β (7)
force of a droplet encircled by an oil layer during an ongoing
process and fs is the sliding friction of the droplet base acting on where μ is the dimensionless coefficient of friction and β is the
inclination angle of the substrate. The coefficient μ can also be
the oil layer. For an oblique surface the gravitational force is
determined experimentally (Supporting Information).
fg = −ρVg sin β Defining Equation and its Solution. Inserting all the
(2) corresponding terms may result in the following second-order
nonlinear ordinary differential equation to describe the droplet
where g = 9.81 m/s2 is the acceleration due to gravity and β is moving:
the angle of orientation of the surface to the horizontal.
α
Unbalanced Interfacial Tension. The x-component of the d2x kRη1 dx 4γ sin 2 2 ⎡ α 2
interface tension force for an element of length, ds, along the + − ⎢ −a1 sin x
dt 2
ρ V dt ρV ⎣ 2
contact line is as follows:23
⎛ φ α⎞ ⎛π α ⎞⎤
ln tan⎜ 1 − ⎟ + a 2x⎜ + − φ1⎟⎥ + μg cos β
dFix = γ cos θr cos φ ds = γ cos θrr dφ (3) ⎝2 4⎠ ⎝2 2 ⎠⎦

where γ is the surface tension, θr is the contact angle at the
position of ds, r is the base radius of the droplet, and φ is the
angle that the line connecting ds with the center makes with the
x-axis. The total interface tension in a homogeneous surface is
zero due to the circular symmetry of the contact line. However,
each value of dFi is varied with constricting degree and there
will be a net force Fix in the x-direction if the droplet is placed
on a shape gradient surface (Figure 4b). The values of the
contact angle θr are determined by individually depositing each
droplet on circular plates with a series of radii (Figure 4c). The
base radius R of a droplet on the copper substrate with an oil
layer is 1.35 mm (the corresponding contact angle is 88°), and
the droplet exhibits a larger contact angle on a circular plate
with a smaller radius due to a bent contact line. Thus, the
corresponding cos θr is fitted as a linear expression of cos θr ≈
a1r + a2 ≈ 1.0140r − 1.4260 (r, mm). Therefore, the actuating
force Fix, the resultant of interfacial tension components in the
lengthwise direction within a droplet at any position of the
shape track, can be developed as
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+ g sin β = 0 (8)
Equation 8 is solved numerically using the fourth-order
Runge−Kutta method. Except for the above forces, the droplet
still sustains viscous force within the liquid, taking place during
the droplet motion. But the viscous force on the slippery oil
layer is much lower than liquid/solid friction on the unmodified
surface and approximately 1% of Fix in this work which has little
effect on droplet motion so that the viscous force is negligible
(Supporting Information). The position evolutions obtained
from eq 8, shown in Figure 2c,d, are in good agreement with
the experimental results.
■ CONCLUSIONS
In summary, we developed the wedge-shape gradient
combining PDMS oil layer and superhydrophobicity to induce
droplet motion. Both elements of PDMS oil and super-
hydrophobicity offer a very low contact angle hysteresis so that
the actuating force arising from the shape gradient, the
unbalanced interfacial tension due to boundary compressing,
DOI: 10.1021/acs.langmuir.7b00227
Langmuir 2017, 33, 4172−4177
Langmuir
can drive droplets to move on the gradient surface. The droplet
position and moving velocity are greatly related to the shape
gradient angle. With a larger gradient angle, droplets move
faster but stop at a nearer position. The theoretical model
established in this work for droplet motion is much matched
with the experimental results. Moreover, we designed a pattern
with multiple gradient branches based on the same mechanism
to operate droplet aggregation. The facile approach proposed in
this work can be a promising option for liquid transportation or
mixing in open microfluidics, microchemical reactors, and lab
chip application.
■
ASSOCIATED CONTENT
*
S Supporting Information
The Supporting Information is available free of charge on the
ACS Publications website at DOI: 10.1021/acs.lang-
muir.7b00227.
Figure S1 representing schematic diagram of forces
analysis for droplet on long stripe copper substrate;
Figure S2 showing unbalanced interfacial tension Fix and
viscous force f v as functions of position x (PDF)
Movie S1 showing aggregation of droplets on multiple
shape gradients (AVI)
■
AUTHOR INFORMATION
Corresponding Author
*E-mail: cejcheng@scut.edu.cn.
ORCID
Jiang Cheng: 0000-0002-9947-6193
Xiufang Wen: 0000-0001-5071-8940
Notes
The authors declare no competing financial interest.
■
ACKNOWLEDGMENTS
This work is supported by the National Natural Science
Foundation of China (20976055) and the Natural Science
Foundation of Guangdong Province (S2012010010417).
■
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4177 DOI: 10.1021/acs.langmuir.7b00227

Langmuir 2017, 33, 4172−4177