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Characterization of Coalescence-Induced Droplet Jumping Height On Hierarchical Superhydrophobic Surfaces
Characterization of Coalescence-Induced Droplet Jumping Height On Hierarchical Superhydrophobic Surfaces
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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.
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.
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
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.
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
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Article
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released during coalescence and the dissipation energies
between the droplets and the surface, taking into account the
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