Download as pdf or txt
Download as pdf or txt
You are on page 1of 8

This is an open access article published under an ACS AuthorChoice License, which permits

copying and redistribution of the article or any adaptations for non-commercial purposes.

Article

http://pubs.acs.org/journal/acsodf

Characterization of Coalescence-Induced Droplet Jumping Height on


Hierarchical Superhydrophobic Surfaces
Xuemei Chen, Justin A. Weibel, and Suresh V. Garimella*
School of Mechanical Engineering and Birck Nanotechnology Center, Purdue University, 585 Purdue Mall, West Lafayette, Indiana
47907-2088, United States
*
S Supporting Information

ABSTRACT: Coalescence-induced condensate droplet jump-


See https://pubs.acs.org/sharingguidelines for options on how to legitimately share published articles.

ing from superhydrophobic surfaces can be exploited in


condensation heat-transfer enhancement, imparting self-
Downloaded via INDIAN INST OF TECH ROPAR on January 5, 2021 at 12:19:16 (UTC).

cleaning behavior to surfaces, anti-icing coatings, and other


industrial uses. An intriguing application would exploit this
phenomenon to achieve thermal rectification using a sealed
vapor chamber with opposing superhydrophilic and super-
hydrophobic surfaces. During forward operation, continuous
evaporation occurs from the heated superhydrophilic evapo-
rator surface; self-propelled jumping returns the condensate droplets from the cooler superhydrophobic surface to the
evaporator, allowing passive recirculation of the working fluid without a reliance on gravity or capillary wicking for fluid return. In
reverse operation, when the superhydrophobic surface is heated, the absence of a mechanism for fluid return from the cooler
superhydrophilic side to the evaporator restricts heat transport across the (low conductivity) vapor gap. The effectiveness of this
jumping-droplet thermal diode can be enhanced by maximizing the distance between the opposing superhydrophobic and
superhydrophilic surfaces. It is, therefore, important to investigate the height to which the condensate droplets jump from the
superhydrophobic surfaces such that replenishment of liquid to the superhydrophilic surface is maintained. In this study, we
systematically investigate the height to which the condensate droplets jump from the hierarchical superhydrophobic surfaces
having truncated microcones coated with nanostructures. The condensate droplet jumping height increases with a decrease in
microcone pitch. A general theoretical model that accounts for surface adhesion, line tension, and initial wetting states of multiple
coalescing droplets of different radii is used to predict and explain the experimentally observed trend of droplet jumping height
with surface roughness. The insights provided regarding the effect of surface topography on droplet jumping height are critical to
the design of high-performance thermal diode devices.

1. INTRODUCTION transport occurs when the superhydrophilic surface side is


When vapor condenses on an ultralow-adhesion nanostruc- heated; self-propelled jumping droplets return condensed
tured superhydrophobic surface, the resulting condensate working fluid from the superhydrophobic condenser to the
droplets can jump away from the surface upon coalescence. superhydrophilic evaporator. In the reverse operating direction,
This “coalescence-induced droplet jumping” is self-propelled by when the superhydrophobic surface is heated, the fluid
excess surface energy released upon coalescence.1−8 The condensed on the superhydrophilic surface has no mechanism
jumping of condensate droplets has been observed on naturally to return to the heated superhydrophobic side; heat transport
occurring superhydrophobic surfaces, including lotus leaves,9 must occur through conduction/convection across the vapor
cicada wings,10 water strider legs,11 and gecko skin.12 Inspired space. The effectiveness of this thermal diode can be enhanced
by the structure of these surfaces, various nanostructured13−15 by maximizing the spacing between the superhydrophobic
or hierarchical micro-/nanostructured3,16−22 surfaces have been condenser and superhydrophilic evaporator surfaces.32 How-
fabricated to achieve condensate droplet jumping behavior. The ever, there exists an upper limit of spacing beyond which the
jumping of condensate droplets is of significant interest owing jumping condensate droplets cannot reach the superhydrophilic
to their potential for enhancing the performance of a variety of surface. Therefore, it is important to investigate the jumping
functional surfaces for applications including self-cleaning height of condensate droplets from the superhydrophobic
surfaces,10−12 condensation heat transfer,10,13−25 anti-icing surfaces so that the surfaces may be designed for operation at
surfaces,26−28 energy harvesting,29 and power generation.30 large spacings. Although there has been a great interest in
Beyond these demonstrated applications, the self-propelled exploiting superhydrophobic surfaces for enhanced dropwise
condensate droplet jumping from superhydrophobic surfaces
also has the potential for applications in thermal diode devices Received: February 26, 2017
comprising a sealed vapor chamber with opposing super- Accepted: June 8, 2017
hydrophobic and superhydrophilic plates.31,32 Evaporative heat Published: June 21, 2017

© 2017 American Chemical Society 2883 DOI: 10.1021/acsomega.7b00225


ACS Omega 2017, 2, 2883−2890
ACS Omega Article

condensation,13−25 none have characterized this jumping height the truncated microcones are ∼16 and ∼32 μm, respectively;
that is of critical importance to thermal diodes. the microcone height (H) and the slant height (L) are ∼11 and
We developed a new experimental approach to characterize ∼13.6 μm, respectively. The nanowires are ∼150 nm in
the condensate droplet jumping height on hierarchical diameter (Dn) and ∼1.5 μm in height (Hn), at a pitch (Pn) of
superhydrophobic surfaces featuring nanostructured truncated ∼500 nm. For comparison purposes, a baseline nanostructured
microcones. The effect of surface roughness (namely, micro- sample (Nano) without microcones was fabricated using a
structure pitch) on the condensate droplet jumping height was single-step metal-assisted chemical etching process. All sample
systematically investigated. A general theoretical model that surfaces were silanized to render them superhydrophobic;3
takes into account the surface adhesion, line tension, and water contact angles of ∼165° and contact angle hysteresis
droplet wetting states of multiple coalescing droplets of values of less than 1° were measured.
different radii was developed to explain the underlying 2.2. Measurement of Condensate Droplet Jumping
mechanisms that lead to the observed jumping height Height. Condensation experiments were carried out in an
dependence on surface roughness. ambient environment at a temperature of ∼20 °C and a relative
humidity of ∼40%. The condensation setup developed to
2. RESULTS AND DISCUSSION measure the condensate droplet jumping height on the sample
2.1. Characteristics of the Superhydrophobic Surfa- surface is shown in Figure 2. The sample was attached to a
ces. Figure 1 shows the scanning electron microscopy (SEM) temperature-controlled cooling stage (CP-031, TE Technology,
Inc.) set at 0 °C. The condensation process is visualized for 30
min using a camera (EO-5023M, Edmund Optics) and a high-
magnification zoom lens (VH-Z100R, Keyence) with in-line
illumination provided by a 300 W Xe arc lamp (Titan 300,
Sunoptic Technologies). To observe the distribution of
condensate droplets during dropwise condensation, the lens
was focused on each sample surface with a 0.3 mm × 0.23 mm
field of view. To measure the jumping height of the condensate
droplet, separate experiments were performed under the same
conditions with a glass slide inserted between the camera and
the surface; the lens was focused on the underside of the glass
slide (facing the sample) with a larger field of view of 1.53 mm
× 1.14 mm. Condensate droplets that coalesce and jump a
sufficient distance from the surface can be observed to impact
the glass slide. The image on the left of Figure 2 shows a
representative snapshot of condensate droplets attached to the
glass slide after they have jumped from sample P40. The
spacing between the glass slide and the sample surface (S) was
varied from 0.3 to 6.5 mm to investigate the number of
coalesced droplets that jump to these different heights. Testing
at a spacing smaller than 0.3 mm resulted in condensation on
the glass slide. It should be noted that the number of droplets
Figure 1. SEM images of the nanostructured truncated microcone
surfaces with pitches of (a) 40, (b) 50, (c) and 60 μm and (d) a impacting the glass slide is comparable when the sample is
nanostructured surface without microcones (denoted as P40, P50, placed vertically (as shown in Figure 2) and horizontally (facing
P60, and Nano, respectively). An enlarged view of nanostructures on upward against gravity), indicating that jumping height is
the hierarchical and flat nanostructured surfaces is shown in the inset orientation-independent (section S1). In this experiment, the
of panel (d). vertical orientation is used to eliminate the influence of falling
droplets on the droplet jumping.
images of the hierarchical superhydrophobic surfaces, which 2.3. Condensate Droplet Jumping from the Surfaces.
consist of nanostructured truncated microcones on a silicon To determine the total number of condensate droplets jumping
substrate, and these are denoted as P40, P50, and P60 based on from each surface, the condensation process on the sample
the microcone pitches, P, of 40, 50, and 60 μm, respectively. surface was visualized. Figure 3 shows selected snapshots of
For all of the surfaces, the top (D1) and base (D2) diameters of dropwise condensation on the four surfaces. The images on

Figure 2. Schematic drawing of the experimental setup used to measure the condensate droplet jumping height (right). The image on the left shows
a representative snapshot of condensate droplets impacting the glass slide after they have jumped from surface P40.

2884 DOI: 10.1021/acsomega.7b00225


ACS Omega 2017, 2, 2883−2890
ACS Omega Article

Figure 3. Selected snapshots of dropwise condensation on surfaces (a) P40, (b) P50, (c) P60, and (d) Nano. The images on the left in each pair
show the moment before the outlined group of droplets coalesced, and the images on the right show the moment just after departure by coalescence-
induced jumping. The scale bars are 100 μm.

each panel show the moment before droplet coalescence (left)


and after departure by jumping (right), as indicated by the solid
and dashed lines, respectively. Such a coalescence-induced
departure is counted as one coalesced jumping droplet; the
total number of coalesced jumping droplets per square
millimeter (the areal density of condensate droplets) occurring
on each surface within the field of view (0.3 mm × 0.23 mm)
over 30 min is counted (see Table 1). Note that the
coalescence events for droplets smaller than ∼3 μm were not
counted owing to measurement uncertainties.

Table 1. Areal Density of Coalesced Droplets Jumping Figure 4. Areal density of coalesced jumping droplets that impact the
within Specific Height Ranges for Each Surface over 30 min glass slide for different spacings from each sample over 30 min; the
(the Mean Values Are Given, with a Variation of ∼10%) inset shows an enlarged view for the larger spacings. The error bars
represent the variation in the measured areal density across the
areal density of coalesced droplets repeated experimental trials for each corresponding sample.
droplet jumping height (mm) P40 P50 P60 Nano
0−0.3 3149 3226 3342 2028 droplets impacting the glass slide at a spacing of 3.5 mm and
0.3−1 828 564 345 202 larger.
1−2.5 319 209 177 87 2.4. Droplet Jumping Height. The data shown in Figure 4
2.5−3.5 82 78 59 35 are the areal densities of the droplets that jump to or higher
3.5−5 73 63 46 25 than a given height (i.e., spacing between the camera and the
5−6.5 71 51 37 12 glass slide, S) for each sample. To assess the average droplet
>6.5 28 11 8 3 jumping height, we calculated the areal density of droplets that
total 4551 4203 4014 2391 jump to specific height ranges. For instance, the areal density of
droplets jumping in the range of 0−0.3 mm can be deduced by
subtracting the areal density of droplets that impact the glass
slide at a spacing of 0.3 mm from the total areal density of
To assess the height to which the droplets jump, the glass droplets that jump from the surface. The droplet counts for the
slide is visualized during condensation, and the areal density of rest of the jumping height ranges can be calculated similarly
droplets impacting the slide within the field of view (1.53 mm based on the data shown in Figure 4, taking the difference in
× 1.14 mm) over the testing period (30 min) is counted. Each the number of impacting droplets at each spacing increment.
sample surface at each spacing between the glass slide and the The areal densities of droplets jumping to specific height ranges
surface (S) was tested at least three times, observing the glass (0−0.3 mm, 0.3−1 mm, 1−2.5 mm, 2.5−3.5 mm, 3.5−5 mm,
slide at different locations to ensure that the number of droplets 5−6.5 mm, and >6.5 mm) for all samples are calculated, as
counted among all tests at each spacing for a given sample shown in Table 1.
varied by less than 10%, and the mean values are reported. The percentages of the total number of jumping droplets per
Figure 4 shows the areal density of condensate droplets square millimeter from any surface that reach specific height
impacting the glass slide for different spacings, S, for the four ranges are shown for each sample in Figure 5. The majority of
samples. It is observed that there are few jumping droplets that the droplets jump less than 0.3 mm for all surfaces, and the
reach the glass slide as the spacing is increased for all samples. A percentage of droplets that reach higher jumping heights
significant decrease in the number of droplets impacting the decreases for increasing heights. Here, we also observe the
glass slide is observed when the spacing S increases from 0.3 to effect of the microstructures on the jumping droplet height.
1 mm. An enlarged view of the plot area for the larger spacings Compared to the surfaces with microstructures, the distribution
(inset of Figure 4) shows that there are relatively few jumping of droplet jumping heights from the flat nanostructured sample
2885 DOI: 10.1021/acsomega.7b00225
ACS Omega 2017, 2, 2883−2890
ACS Omega Article

the gravitational resistance and comment on the suitability of


comparing the model to our experiments. The initial droplet
jumping speed is predicted using a coalescence-induced
jumping model that we developed previously, which is modified
to account for surface adhesion, line tension, and initial wetting
states of multiple coalescing droplets of different radii.3 On the
basis of the experimental visualizations of the dropwise
condensation process occurring on the sample surfaces, we
measured the number and the radius of coalescing droplets that
result in jumping events during the 30 min experiment on each
sample surface (Figures S3 and S4) and calculated the droplet
jumping height for each jumping event. The average calculated
Figure 5. Histogram showing the percentage of jumping droplets droplet jumping height of all jumping events on each sample
within specific jumping height ranges for each sample; the inset shows surface is then compared with the experimentally measured
an enlarged view of the larger jumping heights.
data to verify the model. Note that the initial wetting states of
the droplets before coalescence were considered. On the
(Nano) is shifted to smaller droplet heights (see the inset hierarchical superhydrophobic surfaces, the condensate droplets
enlarged view). Only ∼3% of all jumping droplets reach a may reside in a composite state, where the droplet is larger than
height larger than 2.5 mm for sample Nano. The shift in the microstructures and sits in contact with at least two
distribution toward larger jumping heights for the micro- truncated microcones. Alternatively, when the droplets are
structured samples also trends with the microcone pitch. For a much smaller than the microstructures, they sit in a Cassie state
decreasing pitch from sample P60 to P40 (i.e., increasing on the nanostructures; all droplets are in the Cassie state for the
microstructured surface roughness), the distribution is shifted flat nanostructured surface. Droplet coalescence can occur for
from smaller to larger droplet jumping heights. For example, various combinations of such Cassie- and composite-state
∼5.2% of all jumping droplets reach higher than 2.5 mm for droplets on the hierarchical surfaces with different microcone
sample P40 (254 droplets) versus only ∼3.7% for sample P60 pitches, which affects their initial surface energy and resulting
(150 droplets). This redistribution is also reflected in the jumping velocity.
average droplet jumping height, which is shown in Figure 6a. Previous theoretical models that predict droplet jumping
The average droplet jumping height for each sample surface is velocities are based on energetic arguments; an ad hoc form of
calculated as a weighted average of the mean heights of each bin viscous dissipation has been typically included in the energy
(note that the bin for >6.5 mm is dropped because of the balance,5−8 which may overestimate the viscous dissipation. For
unknown jumping height). The average jumping height example, some studies report that the coalescence of droplets
increases with a decrease in the microcone pitch. The flat below a critical radius (∼10−20 μm) does not lead to jumping
nanostructured sample (Nano) exhibits the lowest average on a superhydrophobic surface owing to the dominant viscous
droplet jumping height. Given that sample P40 provides the dissipation during coalescence.5−8 However, experimental and
largest average jumping height, it has the potential to enable a numerical studies have demonstrated that the coalescence of
jumping-droplet thermal diode to function with a larger vapor smaller droplets (<10 μm, even down to nanometer size) could
gap, which would increase the thermal rectification.32 cause the droplets to jump away from the surfaces.4,33−35
2.5. Theoretical Modeling of Droplet Jumping Height. Recent studies have provided strong evidence that viscous
A theoretical analysis is performed to understand the observed dissipation is not important at length scales larger than 1
experimental trend in droplet jumping height with surface μm.4,35,36 Instead, finite surface adhesion and unequal
roughness. While our experiments were conducted with the momentum flow in the vertical direction govern and limit the
surface in an orthogonal orientation with respect to gravity, in droplet jumping.4,37 The droplet jumping velocity Uj has been
the analysis, we treat the jumping droplet as an object propelled numerically simulated to be ∼0.23× the characteristic jumping
vertically upward at an initial speed Uj, with the maximum velocity U0 given by the capillary-inertial scaling for the
height determined by the air resistance and gravitational forces. coalescence of two equally sized droplets on a nonwetting
Through this analysis, we will assess the relative importance of surface with an apparent advancing contact angle of 180° and

Figure 6. Comparison between the (a) average experimental droplet jumping height and (b) theoretical predictions for each sample. Although the
vertical axis range of panel (b) is shifted, it has the same scaling as that of panel (a) for the purpose of comparing the trend in the jumping height.

2886 DOI: 10.1021/acsomega.7b00225


ACS Omega 2017, 2, 2883−2890
ACS Omega Article

Figure 7. Calculated droplet jumping velocity as a function of the jumping droplet radius on different superhydrophobic surfaces. The red curve in
each panel is the fitted value of droplet jumping velocity for all coalescence cases during 30 min of condensation; the colors of symbols in each panel
represent the jumping velocity induced by the same number of coalescing droplets.

zero adhesion.4,37 In this study, we assume that the internal expressions of Es, E′s , Eadh, and Eline for multiple Cassie-state
flow momentum generated during two-droplet coalescence is droplets (R1,C, R2,C, ......RN,C) and multiple composite-state
identical for the multiple-droplet coalescence case, with the droplets (R1,comp, R2,comp, ......RN,comp) have been derived in our
same proportionality constant of ∼0.23.4,37 Furthermore, we previous work3 and are given below.
consider the dissipation forces induced by surface adhesion and The surface energy equations of multiple Cassie-state
contact line tension between the condensate droplets and the droplets (Es,C) and multiple composite-state droplets (Es,comp)
surface. are, respectively, expressed as follows
When droplet coalescence occurs, if all of the released surface
⎧⎛ 2 ⎞
energy ΔEs (ΔEs = Es − E′s , where Es and E′s are the surface Es,C = π sin 2 θ ⎨⎜ + 1 − fn ⎟σlv
energy before and after droplet coalescence) after balancing the ⎝
⎩ 1 + cos θ ⎠
interfacial adhesion-induced dissipation energy Eadh and line- ⎫N
tension-induced dissipation energy Eline is converted to kinetic + fn (σsv − σlv cos θe) + σsv(rn − fn )⎬∑ R i ,C 2
energy Ek, then ⎭ i=1
(3)
E k = ΔEs − Eadh − E line (1)
⎧⎡ 2
where Ek = 1/2mU02, m = 2/3πρR′3(2 − 3 cos θ + cos3 θ) is the Es,comp = π sin 2 θ ⎨⎢ − 2fn rf
mass of the jumping droplet, R′ is the radius of the jumping ⎩⎣ 1 + cos θ
droplet, and U0 is the corresponding characteristic jumping ⎤ ⎫N
velocity. + rf (1 − fn cos θe)⎥σlv + rf rnσsv ⎬∑ R i ,comp2
⎦ ⎭
However, because of the incomplete conversion of the excess i=1
energy to translational kinetic energy as a result of limited (4)
momentum to provide droplet jumping, the actual droplet where f n = πDn2/4Pn2 and rn = 1 + πDnHn/Pn2 are the solid
jumping velocity Uj is estimated to be ∼0.23× the characteristic fraction and surface roughness of the nanowires, respectively; rf
jumping velocity given by eq 1, which is expressed as = 1 + [0.5πL(D1 + D2) + 0.25π(D12 − D22)]/P2 is the surface
roughness of the truncated microcones; σlv, σsl, and σsv are the
Uj ≈ 0.23U0
liquid−vapor, solid−liquid, and solid−vapor surface tensions,
⎡ 6(ΔEs − Eadh − E line) ⎤1/2 respectively; and θe ≈ 115° is the equilibrium contact angle
= 0.23⎢ ⎥ with water on the silane-coated flat and smooth surface. The
⎣ πρ(2 − 3 cos θ + cos3 θ)(R13 + R 2 3 + ···RN 3) ⎦
surface energy of multiple Cassie-state droplets coalesced with
(2) multiple composite-state droplets can be obtained by summing
where θ = 165° is the apparent contact angle of the droplet, R1, the corresponding surface energy obtained from eqs 3 and 4.
R2···RN are the radii of condensate droplets before coalescence, The surface energy of a coalesced jumping droplet (Es′) is
and N is the number of coalescing droplets. The energy expressed as
2887 DOI: 10.1021/acsomega.7b00225
ACS Omega 2017, 2, 2883−2890
ACS Omega Article

Es′ = 4πR′ 2σlv as Fa = kU(t), where k = 6πηaR′ is the air friction coefficient, ηa
N
= 1.827 × 10−5 Pa·s is the viscosity of air, and U(t) is the
= 41/3πσlv(2 − 3 cos θ + cos3 θ )2/3 (∑ R i 3)2/3 vertical jumping speed at time t.
(5) Integrating the droplet jumping speed U(t) from time 0 to tm
i=1
{the time required for the droplet to jump to the maximum
The dissipation energies during multiple-droplet coalescence height at which U(t) is zero, tm = −(m/k)ln[mg/(mg + Ujk)]},
are determined by the surface morphology, solid−liquid contact the droplet jumping height is calculated as
area, and solid−liquid contact line length. The adhesion- tm
induced energy dissipation energies for the coalescence of
multiple Cassie-state droplets (Eadh,C) and multiple composite-
h= ∫0 U (t ) d t
state droplets (Eadh,comp) are given below = (m /k)[Uj + mg /k][1 − e−ktm / m] − mgtm/k (11)
N
Eadh,C = πfn σlv sin 2 θ(1 + cos θe)∑ R i ,C 2 We calculated the droplet jumping height of each
i=1 (6) coalescence event on different sample surfaces using the
measured radius of the coalescing droplet. The average droplet
N
jumping height of all jumping events on each sample surface is
Eadh,comp = πrf fn σlv sin 2 θ(1 + cos θe)∑ R i ,C 2 then compared with the experimentally measured data, as
i=1 (7) shown in Figure 6. It should be noted that if we only consider
The line-tension-induced energy dissipation at the triple line the gravitational force on the droplet jumping behavior, the
for the coalescence of multiple Cassie-state droplets (Eline,C) respective maximum droplet jumping heights are ∼10 times
and multiple composite-state droplets (Eline,comp) is expressed, larger than the values with air friction included. This confirms
respectively, as that the influence of gravity on the droplet jumping height is
N
negligible compared with the air friction force. From Figure 6, it
π 2(sin 2 θ)σDn can be seen that the trends of the theoretical data with the
E line,C = ∑ R i ,C2 microstructured surface roughness follow the experiments. That
(Ln + Dn)2 i=1 (8)
is, the jumping height increases with the decreasing microcone
π 2rf (sin 2 θ)σDn
N pitch for the microstructured surfaces, which all yield a greater
E line,comp = ∑ R i ,comp2 jumping height than the flat nanostructured surface. The larger
(Ln + Dn)2 i=1 (9) droplet jumping height on the hierarchical surface with a
smaller microstructure pitch is likely due to the larger
On the basis of the measured coalescing droplet radius, the
percentage of composite-state droplets that the surface enables.
theoretical droplet jumping velocity Uj (eq 2) can be calculated
According to eqs 3 and 4, the surface energy before coalescence
according to eqs 3−9. The calculated droplet jumping velocity
of multiple composite-state droplets is larger than that of
Uj as a function of the jumping droplet radius for all
multiple Cassie-state droplets, which results in an increased
coalescence events on different surfaces is shown in Figure 7.
corresponding energy released upon coalescence, yielding an
The corresponding energy budget of different jumping droplet
increased droplet jumping height on the hierarchical surface
radii on each surface is given in Figure S5 to examine the
with a smaller microcone pitch.
dominant forces during the jumping process. The high scatter
We note that the theory overpredicts the jumping heights
in the droplet jumping velocity for each surface in Figure 7 is
relative to the measured values. This may be attributed to the
due to the coalescence of multiple droplets of unequal radii. By
fact that this theory assumes that the complex fluid dynamics
fitting the scatter data to the allometric function (y = axb, the
occurring during the coalescence between the two equally sized
red curve on each panel), we found that the droplet jumping
droplets on the superhydrophobic surface is identical to that in
velocity decreases with an increase in jumping droplet radius,
the multiple-droplet coalescence case. This assumption implies
and the value falls between 0.25 and 1.5 m/s for all surfaces,
that the magnitude of the internal flow momentum generated
depending on the number and size of coalescing droplets and
by the coalescence of two droplets equals that of the multiple-
the surface morphology. The trend of droplet jumping velocity
droplet coalescence cases. However, the internal flow
with the jumping droplet radius is in accordance with the
momentum necessary to enable droplet jumping should be
experimental observations by Kim et al.37 and Cha et al.,38 and
somewhat different for the cases of multiple-droplet coales-
the average droplet jumping velocity on our nanostructured
cence in the experiments because on the hierarchical super-
surface (∼0.7 m/s) is comparable to their measured values on
hydrophobic surface, droplets with uneven sizes, different
surfaces with nanostructures only (0.5−0.6 m/s),37,38 indicating
wetting states, initial positions, or arrangements are more likely
that our model can well-predict the droplet jumping velocity.
to coalesce, which could alter the droplet coalescence dynamics
To calculate the droplet jumping height, we consider the
substantially. In particular, the uneven coalescence of multiple
gravitational (Fg) and frictional (Fa) forces acting against the
droplets may create momentum in various directions away from
droplet motion in air. Note that the drag force due to vapor
the surface normal, causing the measured droplet jumping
flow toward the condensing surface can be neglected for our
height to be decreased. Such a decrease is not considered in the
experimental conditions (section S4). The equation of droplet
theoretical predictions, which would cause the theory to
motion at any time t is given by
overpredict the experiments.
Fg + Fa = −mU ′(t ) (10)
3. CONCLUSIONS
2
where Fg = mg is the gravitational force and g = 9.8 m/s is the
We systematically investigated the effect of surface topography
gravitational acceleration. According to Stokes’ law, for low
2ρa U (t )R ′
on the coalescence-induced droplet jumping height during
Reynolds number Re = ηa
, the friction force is expressed dropwise condensation on hierarchical superhydrophobic
2888 DOI: 10.1021/acsomega.7b00225
ACS Omega 2017, 2, 2883−2890
ACS Omega


Article

surfaces. The droplet jumping height exhibits dependence on ACKNOWLEDGMENTS


the microstructured surface roughness of the substrate; the
Financial support for this work provided by the Cooling
jumping height increases with a decrease in the pitch of
Technologies Research Center and the National Science
truncated microcone features on the surface. To explain the
Foundation Industry/University Cooperative Research Center
mechanisms underlying the droplet jumping height observed in
at Purdue University was gratefully acknowledged. We thank
the experiments, an energy-based model for the jumping
researchers at the Toyota Research Institute of North America,
dynamics is employed. The initial speed of the jumping droplet
specifically Drs. Feng Zhou, Ercan M. Dede, and Shailesh N.
is predicted based on the difference between the surface energy
Joshi, for their technical discussion on this topic.


released during coalescence and the dissipation energies
between the droplets and the surface, taking into account the
different initial droplet wetting states on each surface. This REFERENCES
initial droplet jumping speed is used to estimate the jumping (1) Boreyko, J. B.; Chen, C.-H. Self-propelled dropwise condensate
height. The trend in variation of the theoretically predicted on superhydrophobic surfaces. Phys. Rev. Lett. 2009, 103, 184501.
jumping droplet height as a function of the sample micro- (2) Boreyko, J. B.; Chen, C.-H. Self-propelled jumping drops on
structure pitch is consistent with the experimental data; namely, superhydrophobic surfaces. Phys. Fluids 2010, 22, 091110.
a higher surface energy for droplets in the composite state, (3) Chen, X.; Patel, R. S.; Weibel, J. A.; Garimella, S. V. Coalescence-
which are more prevalent on surfaces with a smaller Induced Jumping of Multiple Condensate Droplets on Hierarchical
Superhydrophobic Surfaces. Sci. Rep. 2016, 6, 18649.
microstructure pitch, results in an increased energy transfer
(4) Enright, R.; Miljkovic, N.; Sprittles, J.; Nolan, K.; Mitchell, R.;
to the released droplet upon coalescence, which increases the Wang, E. N. How Coalescing Droplets Jump. ACS Nano 2014, 8,
droplet jumping height. The insights provided by this study, 10352−10362.
specifically regarding the role of surface roughness in governing (5) Peng, B.; Wang, S.; Lan, Z.; Xu, W.; Wen, R.; Ma, X. Analysis of
the coalescence-induced droplet jumping height, can guide droplet jumping phenomenon with lattice Boltzmann simulation of
efforts to improve hierarchical superhydrophobic surface droplet coalescence. Appl. Phys. Lett. 2013, 102, 151601.
designs for jumping-droplet thermal diode devices and in (6) Nam, Y.; Kim, H.; Shin, S. Energy and hydrodynamic analyses of
other applications for which this behavior governs performance. coalescence-induced jumping droplets. Appl. Phys. Lett. 2013, 103,
161601.
(7) Liu, T. Q.; Sun, W.; Sun, X. Y.; Ai, H. R. Mechanism study of
4. EXPERIMENTAL METHODS condensed drops jumping on super-hydrophobic surfaces. Colloids
4.1. Fabrication of Superhydrophobic Surfaces. We Surf., A 2012, 414, 366−374.
fabricated nanostructured truncated microcones on a silicon (8) Wang, F.-C.; Yang, F.; Zhao, Y.-P. Size effect on the coalescence-
substrate using a two-step wet-etching process that we induced self-propelled droplet. Appl. Phys. Lett. 2011, 98, 053112.
developed previously.3 Briefly, the truncated microcones were (9) Lv, C.; Hao, P.; Yao, Z.; Song, Y.; Zhang, X.; He, F.
first created using photolithography and anisotropic tetrame- Condensation and jumping relay of droplets on lotus leaf. Appl.
Phys. Lett 2013, 103, 021601.
thylammonium hydroxide etching, following which the (10) Wisdom, K. M.; Watson, J. A.; Qu, X.; Liu, F.; Watson, G. S.;
nanostructures were etched across the entire surface using a Chen, C.-H. Self-cleaning of superhydrophobic surfaces by self-
metal-assisted chemical etching process. Surfaces with center- propelled jumping condensate. Proc. Natl. Acad. Sci. U.S.A. 2013, 110,
to-center microcone spacings were fabricated by varying the 7992−7997.
photolithography mask patterns. (11) Wang, Q.; Yao, X.; Liu, H.; Quéré, D.; Jiang, L. Self-removal of


condensed water on the legs of water striders. Proc. Natl. Acad. Sci.
ASSOCIATED CONTENT U.S.A. 2015, 112, 9247−9252.
(12) Watson, G. S.; Schwarzkopf, L.; Cribb, B. W.; Myhra, S.;
*
S Supporting Information Gellender, M.; Watson, J. A. Removal mechanisms of dew via self-
The Supporting Information is available free of charge on the propulsion off the gecko skin. J. R. Soc., Interface 2015, 12, 20141396.
ACS Publications website at DOI: 10.1021/acsomega.7b00225. (13) Sikarwar, B. S.; Battoo, N. K.; Khandekar, S.; Muralidhar, K.
Dropwise condensation underneath chemically textured surfaces:
Droplet numbers and sample orientation, number, and simulation and experiments. J. Heat Transfer 2011, 133, 021501.
radii of coalescing droplets during 30 min of con- (14) Miljkovic, N.; Enright, R.; Nam, Y.; Lopez, K.; Dou, N.; Sack, J.;
densation, energy budget as a function of jumping Wang, E. N. Jumping-Droplet-Enhanced Condensation on Scalable
droplet radius, and drag force on droplets owing to vapor Superhydrophobic Nanostructured Surfaces. Nano Lett. 2013, 13,
flowing toward the condensing surface (PDF) 179−187.


(15) Tian, J.; Zhu, J.; Guo, H.-Y.; Li, J.; Feng, X.-Q.; Gao, X. Efficient
Self-Propelling of Small-Scale Condensed Microdrops by Closely
AUTHOR INFORMATION Packed ZnO Nanoneedles. J. Phys. Chem. Lett. 2014, 5, 2084−2088.
(16) Hou, Y.; Yu, M.; Chen, X.; Wang, Z.; Yao, S. Recurrent
Corresponding Author Filmwise and Dropwise Condensation on a Beetle Mimetic Surface.
*E-mail: sureshg@purdue.edu (S.V.G.). ACS Nano 2015, 9, 71−81.
ORCID (17) Chu, F.; Wu, X.; Zhu, B.; Zhang, X. Self-propelled droplet
behavior during condensation on superhydrophobic surfaces. Appl.
Suresh V. Garimella: 0000-0003-1421-2912 Phys. Lett. 2016, 108, 194103.
Author Contributions (18) Chen, X.; Wu, J.; Ma, R.; Hua, M.; Koratkar, N.; Yao, S.; Wang,
The manuscript was written through contributions from all Z. Nanograssed micropyramidal architectures for continuous dropwise
authors. All authors have given approval to the final version of condensation. Adv. Funct. Mater. 2011, 21, 4617−4623.
the manuscript. (19) Rykaczewski, K.; Paxson, A. T.; Anand, S.; Chen, X.; Wang, Z.;
Varanasi, K. K. Multimode Multidrop Serial Coalescence Effects
Notes during Condensation on Hierarchical Superhydrophobic Surfaces.
The authors declare no competing financial interest. Langmuir 2013, 29, 881−891.

2889 DOI: 10.1021/acsomega.7b00225


ACS Omega 2017, 2, 2883−2890
ACS Omega Article

(20) Cheng, J.; Vandadi, A.; Chen, C.-L. Condensation heat transfer
on two-tier superhydrophobic surfaces. Appl. Phys. Lett. 2012, 101,
131909−131914.
(21) Chen, X.; Weibel, J. A.; Garimella, S. V. Exploiting Microscale
Roughness on Hierarchical Superhydrophobic Copper Surfaces for
Enhanced Dropwise Condensation. Adv. Mater. Interfaces 2015, 2,
1400480.
(22) Enright, R.; Miljkovic, N.; Alvarado, J. L.; Kim, K.; Rose, J. W.
Dropwise condensation on micro- and nanostructured surfaces.
Nanoscale Microscale Thermophys. Eng. 2014, 18, 223−250.
(23) Attinger, D.; Frankiewicz, C.; Betz, A. R.; Schutzius, T. M.;
Ganguly, R.; Das, A.; Kim, C.-J.; Megaridis, C. M. Surface engineering
for phase change heat transfer: A review. MRS Energy & Sustain. 2014,
1, No. E4.
(24) Miljkovic, N.; Wang, E. N. Condensation heat transfer on
superhydrophobic surfaces. MRS Bull. 2013, 38, 397−406.
(25) Cho, H. J.; Preston, D. J.; Zhu, Y.; Wang, E. N. Nanoengineered
materials for liquid−vapour phase-change heat transfer. Nat. Rev.
Mater. 2016, 2, 16092.
(26) Chen, X.; Ma, R.; Zhou, H.; Zhou, X.; Che, L.; Yao, S.; Wang, Z.
Activating the Microscale Edge Effect in a Hierarchical Surface for
Frosting Suppression and Defrosting Promotion. Sci. Rep. 2013, 3,
2515.
(27) Boreyko, J. B.; Collier, C. P. Delayed Frost Growth on Jumping-
Drop Superhydrophobic Surfaces. ACS Nano 2013, 7, 1618−1627.
(28) Zhao, Y.; Yang, C. Retarded condensate freezing propagation on
superhydrophobic surfaces patterned with micropillars. Appl. Phys.
Lett. 2016, 108, 061605.
(29) Miljkovic, N.; Preston, D. J.; Enright, R.; Wang, E. N. Jumping-
droplet electrostatic energy harvesting. Appl. Phys. Lett. 2014, 105,
013111.
(30) Beér, J. M. High efficiency electric power generation: The
environmental role. Prog. Energy Combust. Sci. 2007, 33, 107−134.
(31) Boreyko, J. B.; Chen, C.-H. Vapor chambers with jumping-drop
liquid return from superhydrophobic condensers. Int. J. Heat Mass
Transfer 2013, 61, 409−418.
(32) Boreyko, J. B.; Zhao, Y.; Chen, C.-H. Planar jumping-drop
thermal diodes. Appl. Phys. Lett. 2011, 99, 234105.
(33) Liang, Z.; Keblinski, P. Coalescence-induced jumping of
nanoscale droplets on super-hydrophobic surfaces. Appl. Phys. Lett.
2015, 107, 143105.
(34) Cha, H.; Xu, C.; Sotelo, J.; Chun, J. M.; Yokoyama, Y.; Enright,
R.; Miljkovic, N. Coalescence-induced nanodroplet jumping. Phys. Rev.
E 2016, 1, 064102.
(35) Liu, F.; Ghigliotti, G.; Feng, J. J.; Chen, C.-H. Numerical
simulations of self-propelled jumping upon drop coalescence on non-
wetting surfaces. J. Fluid Mech. 2014, 752, 39−65.
(36) Liu, F.; Ghigliotti, G.; Feng, J. J.; Chen, C.-H. Self-propelled
jumping upon drop coalescence on Leidenfrost surfaces. J. Fluid Mech.
2014, 752, 22−38.
(37) Kim, M.-K.; Cha, H.; Birbarah, P.; Chavan, S.; Zhong, C.; Xu,
Y.; Miljkovic, N. Enhanced Jumping-Droplet Departure. Langmuir
2015, 31, 13452−13466.
(38) Cha, H.; Chun, J. M.; Sotelo, J.; Miljkovic, N. Focal Plane Shift
Imaging for the Analysis of Dynamic Wetting Processes. ACS Nano
2016, 10, 8223−8232.

2890 DOI: 10.1021/acsomega.7b00225


ACS Omega 2017, 2, 2883−2890

You might also like