Hao Xu1, Chao Chang1,2, Nan Yi1, Peng Tao1, Chengyi Song1, Jianbo Wu1, Tao Deng1, Wen Shang1. 1. State Key Laboratory of Metal Matrix Composites, Advanced Energy Materials and Technology Center, School of Materials Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, P. R. China. 2. Institute of Marine Engineering and Thermal Science, Marine Engineering College, Dalian Maritime University, Dalian 116026, P. R. China.
Abstract
This paper studied the coalescence, spreading, and rebound of two droplets with different temperatures on a superhydrophobic surface. When the temperature of the impacting droplet was the same as that of the stationary droplet, there was a large deformation of both droplets before the coalescence and the energy dissipation was also large. The coalescence happened at the time close to the maximum spreading. When the temperature of the impacting droplet increased, the deformation of both droplets became smaller before the coalescence and the coalescence happened at or even before the droplets started to spread. The energy dissipation and loss in the later situation is less than those in the previous case. The rebounding characteristics of the merged droplets were also found to be dependent on the temperature. There is an optimum temperature at which the merged droplets can rebound for more times due to the balance of energy loss and also the interaction of the merged droplets with the underlying superhydrophobic substrate. These findings may help further the fundamental understanding of droplet collision on a superhydrophobic surfaces and also offer an alternative strategy to remove droplets from the underlying surfaces for different industrial applications, including condensation heat transfer in steam power plants and phase-change-based thermal management systems.
This paper studied the coalescence, spreading, and rebound of two droplets with different temperatures on a superhydrophobic surface. When the temperature of the impacting droplet was the same as that of the stationary droplet, there was a large deformation of both droplets before the coalescence and the energy dissipation was also large. The coalescence happened at the time close to the maximum spreading. When the temperature of the impacting droplet increased, the deformation of both droplets became smaller before the coalescence and the coalescence happened at or even before the droplets started to spread. The energy dissipation and loss in the later situation is less than those in the previous case. The rebounding characteristics of the merged droplets were also found to be dependent on the temperature. There is an optimum temperature at which the merged droplets can rebound for more times due to the balance of energy loss and also the interaction of the merged droplets with the underlying superhydrophobic substrate. These findings may help further the fundamental understanding of droplet collision on a superhydrophobic surfaces and also offer an alternative strategy to remove droplets from the underlying surfaces for different industrial applications, including condensation heat transfer in steam power plants and phase-change-based thermal management systems.
Droplet collision is
a complicated process that involves droplet
deformation, coalescence, spreading, rebound, and associated energy
and mass transfer. Such a phenomenon happens frequently both in the
natural processes,[1,2] such as in the rains and waterfalls,
and in many industrial processes, such as spray cooling, anti-fog,
and ink-jet printing.[3−5] This area of research attracted a large amount of
attention, and some of those studies investigated the collisions of
two droplets with different sizes to understand the droplet interaction
in the rainfall.[6,7] In the 1990s, the focus of this
research area was moved to the study of collisions involving hydrocarbon
droplets[8−11] during the fuel spray process in combustion. Qian[11] and co-workers were able to map out the two-droplet collision
states using Weber numbers and impact parameters. Their work provides
a useful methodology to study the two-droplet collisions in free space.Recently, droplet collisions on surfaces have also been studied
extensively, which involve both experimental and theoretical studies.[12−25] The early study in this topic can actually be traced back to the
19th century when Lord Rayleigh first observed the collision
of rain droplets onto the liquid surface of water pool, and he attributed
the failure of coalescence between the rain droplets and the water
pool to the trapped air layer between the interfaces of droplets and
the pool surface.[1] He hypothesized that
such an air layer prevented the contact of these droplets with the
pool surface. As the droplet collision on solid surfaces plays a critical
role in many industrial processes,[11,12,15,16] there is also an increased
research effort in studying droplet collisions on solid surfaces,[17−24] especially on superhydrophobic (SH) surfaces due to the great implication
of SH surfaces for a broad range of applications.[25−32] Li[23] experimentally studied two droplets
impacting a solid surface and identified different coalescence mechanisms
based on the comparison between the theoretical and experimental spread
lengths. Wang et al.[24] studied the impact
of nanodroplets on a solid surface and developed a new model to estimate
the maximum spreading factor. They also numerically studied a double
droplet impact on a moving liquid and analyzed the asymmetric heat
transfer characteristics.[25] For the two
droplets in free space, the collision process only involves the interaction
between two droplets. For the collision between two droplets on solid
surfaces, the process is more complicated, in which both the interaction
between the droplets and the interaction between the surfaces and
the droplets need to be considered.Most studies of the two-droplet
collision were focused on the collision
of the two droplets at the same temperature. In many industrial processes,
however, the temperatures of the colliding two droplets might not
be the same. We studied previously the collision of two droplets with
different temperatures on the SH surface. Our study revealed that
temperature had a strong impact on the ratio of collision-coalescence
to collision-separation during the two-droplet collision on SH surfaces.[32] When the temperature of one or both droplets
increased, more coalescence phenomena were observed after the collisions
between the impacting and stationary droplets. Whereas our previous
effort focused on whether the two droplets were coalesced or separated
after their collision with different temperatures of the droplets,
this present study focuses specifically on the behavior of the droplets
after their coalescence.In this work, we intend to investigate
the change of the coalescence,
spreading, and also the rebounding behaviors of the coalesced two
droplets with the impacting droplets set at different temperatures.
We used a high-speed camera to capture the images of the coalescence,
spreading, and rebounding processes on SH surface with the temperature
of the stationary droplet (TS) kept constant
and the temperature of the impacting droplet (TI) changed (Figure ). In the study, the stationary droplet was doped using a
red dye whereas the impacting droplet was not doped so the change
of the interface between two droplets during these processes can be
clearly captured. Through both the experimental investigation and
the analysis of the key factors, including the contact time, restitution
coefficient, and energy change, we hope to help reveal the details
of the collision process. The findings provide a further understanding
on the collision of two droplets with different temperatures on the
SH surface and also offer new insight in designing applications involving
droplet collisions with different temperatures.
Figure 1
Schematic of the coalescence,
spreading, and rebound of two droplets
on the SH surfaces, with TI > TS. (a) Head-on interaction between a hot impacting
droplet (top) and a cold stationary droplet (bottom). (b) Coalescence
of two droplets on the SH surface. (c) Spreading of the merged droplets
on the SH surface. (d) Rebound of the merged droplet from the surface.
Schematic of the coalescence,
spreading, and rebound of two droplets
on the SH surfaces, with TI > TS. (a) Head-on interaction between a hot impacting
droplet (top) and a cold stationary droplet (bottom). (b) Coalescence
of two droplets on the SH surface. (c) Spreading of the merged droplets
on the SH surface. (d) Rebound of the merged droplet from the surface.
Experimental Section
Materials
The
following chemicals and substrates were
used in the fabrication of superhydrophobic Si nanowire (SH Si NW)
surfaces: acetone (99.5%, Sinopharm Chemical Reagent Co. Ltd, China);
ethanol (99.7%, Changshu Hong Sheng fine chemical Co. Ltd, China);
sulfuric acid (H2SO4, 98%, Sinopharm Chemical
Reagent Co. Ltd, China); hydrogen peroxide (H2O2, 30%, Shanghai Ling Feng Chemical Reagent Co. Ltd, China); silver
nitrate (AgNO3, 99.8%, Aladdin, China); hydrofluoric acid
(HF, 40%, Sinopharm Chemical Reagent Co. Ltd, China); Perfluoro-1,1,2,2-tetrahydrooctyltrichlorosilane
(fluorinated silane, 97%, Alfa Aesar); P type silicon wafers (Zhejiang
Li Jing Photoelectric Technology Co. Ltd, China).
Fabrication
of the Superhydrophobic Surface
The SH
Si NW surface was generated via a silver-assisted etching process[33,34] followed by silanization with fluorinated silane[35] to make the surface hydrophobic. Briefly, the Si wafer
was first cleaned with acetone, ethanol, and deionized water and then
treated with a mixture of H2SO4/H2O2 (v/v = 4:1) and diluted HF solution (1 wt %) to remove
the surface contaminants and the oxide layer. The cleaned wafer was
then dipped into the solution of 0.01 mol/L AgNO3 and 4.60
mol/L HF for 1 min at room temperature to deposit silver on the surface
through electroless deposition. The wafer was then immediately transferred
into the solution containing 0.01 mol/L AgNO3, 0.44 mol/L
H2O2, and 4.60 mol/L HF. After 1 h of reaction
at 50 °C, the wafer was taken out from the solution, washed with
deionized water, and dried at room temperature. The fabricated nanostructured
wafer was further surface-modified with fluorinated silane through
vapor deposition.[36]
Droplet Collision Experiment
As shown in Figure , droplets with a diameter
of about 2.2 mm and size variance of ∼1% were generated using
a syringe pump attached with a needle that has an inner diameter of
∼0.3 mm. The temperature of the droplets was controlled through
controlling the temperature of the droplet-delivering needle using
a heating system (DIYCH401, Shanghai Hua Jian Electric Heating Appliance
Co. Ltd, China). The heating system includes a coil heater, which
was wrapping around the needle, and a thermal controller. The water
was preheated for ∼3 min in the needle before being released
as the impacting droplet. The temperature can be adjusted from room
temperature to 100 °C with the temperature resolution of 1 °C.
An IR camera (A300S, FLIR Systems Inc) was used to measure the temperature
of the released droplet. The volume of the released droplet was ∼5.6
mL, whereas the volume of the water inside the heated needle is ∼19.6
mL, all of which was preheated to the set temperature. The detachment
of the droplet from a needle observed in the experiment would induce
oscillations during the subsequent falling.[37] In this work, we assumed that the effect of the oscillations during
the falling process is the same for all impacting experiments. During
the study, a cold stationary droplet was placed on the SH Si NW substrate
first (Figure b) and
the impacting droplet was preheated inside the needle and released
down toward the stationary droplet. The position of the stationary
droplet needs to be adjusted carefully using the three-dimensional
microstage to ensure the alignment of the two droplets and therefore
a head-on collision between the two droplets (Figure c). In this work, the releasing height between
the tip of the needle and the substrate was set to 13 mm. The collision
process of the two droplets was captured by a high-speed camera (X-Stream
XS-4, IDT) with a zoom lens (XDS-0745, JANUS, China) of 3× magnification.
A planer LED light source (C-F1230, Nikon, Japan; 12 V, 100 W; 51
mm in diameter) was placed behind the droplets and used to illuminate
the droplets during the imaging acquisition process, as shown in the
optical image in Figure S1. The camera
was operated at 2000 frames per second with a resolution of 512 ×
512 pixels. All experiments were conducted with controlled humidity
of 50% to minimize the impact of humidity. The data of impacting parameter
and impacting velocity were obtained through analysis of the high-speed
video images using Motion Studio software.
Figure 2
Experimental setup: (a)
Schematic of the instruments used in the
experiment, which includes the heating system and the visualization
system. (b) Scanning electron microscopy of SH surface of Si NWs in
clusters. (c) Optical image of the impacting droplet (hot) in contact
with the stationary droplet (cold) on the SH Si NW surface.
Experimental setup: (a)
Schematic of the instruments used in the
experiment, which includes the heating system and the visualization
system. (b) Scanning electron microscopy of SH surface of Si NWs in
clusters. (c) Optical image of the impacting droplet (hot) in contact
with the stationary droplet (cold) on the SH Si NW surface.
Results and Discussion
The experimental
setup used in this study consists of a micropositioning
system, a droplet generator, a heating system, and an imaging acquisition
system. In this work, the stationary droplets were doped with 0.03
wt % Rhodamine B, which was a red dye, and were kept at room temperature
(∼27 °C). The impacting droplets had no doping, and their
temperatures were adjusted through the heater attached to the delivering
needle. Figure shows
the coalescence, spreading, and rebound of the two colliding droplets
on the SH Si NW surfaces with TI changing
from 27 °C (Figure a) to 40 °C (Figure b) and 70 °C (Figure c). The images show that the influence of temperature
is quite significant in the process of droplet coalescence. As the
temperatures of the two droplets were both set at 27 °C, the
head-on collision proceeded with a large deformation of both droplets
and a clear interface maintained during the deformation. The rapid
contact and deformation of both droplets trapped some air in the interfaces.
Due to the air layer trapped between the two droplets, both droplets
deformed as elastic balls and did not merge together.[13,19,21,22,32] During this process, the kinetic energy
was converted to the surface energy. When the droplets spread close
to the maximum spreading length (spreading length is defined as the
spreading diameter of a water droplet in contact with the substrate)
and the largest deformation, the air layer at the interface disappeared
and the two droplets started to coalesce. Many small air bubbles can
be seen inside the merging droplets due to the dissolved air (the
last image in Figure a). Previous studies showed that higher impact speeds, lowering the
pressure of the surrounding air and increasing the roughness of the
solid surface can help minimize the effect from the air layer trapped
at the interface,[18,20,38] whereas in this study, we showed that temperature may also help
reduce the amount of the air trapped at the interface.
Figure 3
Droplet coalescence,
spreading and rebound on SH Si NW surfaces
with the stationary droplet set at 27 °C and impacting droplet
set at (a) 27 °C; (b) 40 °C; and (c) 70 °C. The sizes
of both droplets were ∼2.2 mm in diameter.
Droplet coalescence,
spreading and rebound on SH Si NW surfaces
with the stationary droplet set at 27 °C and impacting droplet
set at (a) 27 °C; (b) 40 °C; and (c) 70 °C. The sizes
of both droplets were ∼2.2 mm in diameter.Compared with the collision at 27 °C, when TI increased to 40 °C, there was a change in the coalescence
process (more snapshots from 3 to 7 ms for Figure b,c are included in Figure S2). As shown in Figure b, the most obvious change was the coalescence time. The two
droplets started to merge together at around 3 ms, which was during
the spreading process rather than close to the end of the spreading
process. The increase of TI led to the
increase of water vapor around the water droplet.[39] The increased amount of water vapor at the interface between
the impacting droplet and the stationary droplet helps facilitate
the formation of water bridges between the two droplets and accelerates
the coalescence process.[40] What needs to
be pointed out is that the heating up of the stationary droplets will
help form the water bridge to shorten the coalescence time as well.
During the experiment, we found that the heating up of the stationary
droplets led to the pinning of the stationary droplet to the substrate,
which affected the spreading and rebounding of the merged droplets
and increased the complexity in analyzing the interaction between
the two droplets. In this study, we thus only focused on the heating
up of the impacting droplets. The decrease of surface tension and
viscosity with the increase of the droplet temperature will also help
the coalescence process.[13,32] The decrease in surface
tension will lead to the increase of the Weber number, which enhances
the coalescence between the two droplets.[32] The decrease in viscosity helps the formation of a large contact
area during the collision, which also will facilitate the coalescence
between the two droplets.[13] The deformation
of both droplets before the coalescence with TI at 40 °C was smaller than in the case when both droplets
were set at 27 °C. As the process moved forward, the merged droplet
deformed as an integrated droplet with the subsequent spreading and
rebounding processes similar to the processes of a single droplet
impacting on a SH surface. When the spreading area expanded to the
maximum value, the droplet was retracted for the rebound. Through
the high-speed camera we observed that after the initial deformation
of both droplets and the start of the coalescence of the droplets,
the hot impacting droplet penetrated into the middle of the stationary
droplet at the point of the head-on collision. The penetration continued
downward to the solid substrate due to the kinetic energy, which was
converted from the gravitational potential energy of the impacting
droplet. The contacting interfaces of both droplets merged together
during the penetration and the two droplets eventually coalesced into
a single droplet, with an anisotropic distribution of liquid at two
different temperatures. The kinetic energy in the impacting droplet
caused the merged droplet to deform, and the merged droplet behaved
like a single impacting droplet but with the top portion warmer than
the bottom portion. As the merging of the interface started earlier
than in the case when the impacting droplet was set at 27 °C,
there was less deformation for both droplets before the merge and
thus less air trapped at the interface, which led to less air bubble
formation inside the merged droplet (the last image in Figure b). The less air trapped at
the interface may also lead to the penetration of the impacting droplet
into the stationary droplet during the impacting process.As TI was raised further to 70 °C,
the coalescence process started even earlier due to the increase of
the amount of water vapor at the interface between the impacting droplet
and the stationary droplet. The coalescence happened almost immediately
when the two droplets started to contact and continued to the spreading
stage. The impacting droplet penetrated into the stationary droplet,
with the contact line merged outward from the initial contact center.
The two droplets merged together to form a larger anisotropic droplet.
Such a droplet went through the spreading and rebound as a single
droplet, except that there was a temperature gradient within the rebounding
droplet, with the top (transparent) at higher temperature and bottom
(red) at lower temperature through the video image analysis. With
much shorter time and much smaller contacting interface before the
coalescence of the two droplets than both previous cases, there was
much less air trapped between the merging interface and there was
almost no air bubbles observed in the merged droplet (the last image
in Figure c). Such
an observation through the high-speed camera shows that the internal
mass exchange, which was induced by the droplets mixing and internal
liquid flow, was not fast enough to heat up the interface before the
first rebound of the merged droplet from the surface. A similar trend
of accelerated coalescence with the increase of TI was observed with the change of the sizes of the droplets
and the releasing heights of the impacting droplets (Figures S3 and S4). When the size or velocity of the impacting
droplet increased, the coalescence process started as early as the
two droplets started to contact with a high impacting temperature
(TI = 70 °C).We also carried
out the study with impacting droplet at other temperatures
between 27 and 70 °C. Figure a shows the images for the impacting droplets with
different impacting temperatures at the moment when the two droplets
just started to coalescence, which was defined as the moment when
a clearly merged interface was observed in the video images. Figure shows similar trends
to what were observed in Figure . When TI was set at less
than 40 °C, the starting moment of coalescence was close to the
maximum spreading due to the existence of the trapped air layer. With
the increase of the temperature of the impacting droplet, the increasing
amount of water vapor at the interface between the impacting droplet
and the stationary droplet reduced the amount of trapped air and enhanced
the coalescence of the droplets. As shown in Figure , when the impacting droplet was set at 40
°C, the coalescence started during the early stage of spreading.
As TI increased from 40 to 60 °C,
the starting moment of coalescence moved to the beginning of the spreading,
whereas no obvious spreading was observed during the coalescence of
the droplets when TI reached 70 °C.
Figure 4
Starting
moment of coalescence and the restitution coefficient
for different TI: (a) images of the merging
moment between the two droplets. (b) The restitution coefficient of
the two droplets with different impacting temperatures.
Starting
moment of coalescence and the restitution coefficient
for different TI: (a) images of the merging
moment between the two droplets. (b) The restitution coefficient of
the two droplets with different impacting temperatures.To further understand the difference of the droplets’
interaction
when the impacting droplets are set at different temperatures, we
also calculated the restitution coefficient (ε) at different TI. The restitution coefficient is a key parameter
used to evaluate the kinetic energy loss during the coalescence process.
Conventionally, ε is defined as the ratio of impacting velocity
(v0) to rebounding velocity (vr).[41] It is quite straightforward
to calculate the velocity of the impacting droplet, which can be derived
from the initial gravitation potential energy. It is challenging,
however, to calculate the exact velocity value of the merged droplets,
which most of the time have a distorted shape. In this work, we used
gravitation potential energy at the maximum rebounding height to estimate
the rebounding velocity. What needs to be pointed out is that there
is still internal flow and kinetic energy inside the merged droplets
even at the maximum rebounding.[42] Such
an internal flow is complex and difficult to estimate, so in this
work we did not include such flow in the estimation of the restitution
coefficient. The estimated restitution coefficient can be calculated
through eqs and 2in which m is the mass of
the droplets, h1 represents the maximum
rebounding height of the merged droplet after the coalescence, h0 represents the original height of the impacting
droplet, and g is the gravitational constant. The
height (h) was measured between the center of the
droplets at the top and also the center of the droplets at the maximum
spreading length. In this study, the mass of the merged droplets doubled
and the total surface energy would reduce after coalescence. In this
study, we used the average temperature between the stationary and
the impacting droplets as the temperature for the merged droplets.
With the temperature range we studied, the average temperature for
the merged droplets was in the range of 27–48.5 °C. Within
such range, the change of surface tension is only 5%.[43] We calculated the change of the total surface energy for
the two droplets before the impact and for the merged droplets just
before rebounding (Table S1 in the supporting
information). Figure b shows that there is a large jump in the ε value between 35
and 40 °C. When TI was low, the ε
value was about 0.30–0.35 and the energy loss was large compared
with the theoretical restitution coefficient, which might be due to
the chaotic mixing process observed in the video images. When TI was higher than 40 °C, the energy loss
was small with a relatively larger coefficient of ∼0.5, which
might be due to the rather smooth merging process and relatively small
energy loss during the coalescence. Therefore, the restitution coefficients
(Figure b), which
were all smaller than the theoretical restitution coefficients (Table S1), indicate that there was loss of kinetic
energy during the droplets collision. Compared with the value of ∼0.35
at lower TI, the value of ∼0.5
at higher TI indicates the smaller energy
dissipation during the collision processes with higher TI.We also studied the contact time of the collision
process. For
droplets impacting solid surfaces, the contact time is defined as
the time duration between the time of droplets in contact with surfaces
and the time just before the droplets leaving the surfaces. It is
often a crucial parameter for the study of the interaction between
a droplet and a surface. In this study, we defined the contact time
as the time duration between the time of the contact of the two droplets
and the time of the separation of the liquid bottom interface of the
merged droplets from the SH Si NW surfaces. All contact times were
analyzed from the video images. Figure provides the contact time values before the first
rebound for the impacting droplets set at different temperatures.
The schematic inserted in the figure shows the states of the merged
droplets just before their departure from the SH Si NW surfaces for
the first rebound. As shown in Figure , the contact times stay relatively constant (within
the experimental error) for collisions at different TI. Even as the impact velocity increased with the increase
of the releasing heights of the impacting droplets (Figure S4), the contact time remained constant (∼22
ms). The relatively stable contact time was also observed during the
impact of a single droplet onto the SH substrate.[44−46] The contact
time of a single impacting droplet on a solid surface can be estimated
by balancing the inertia with the capillarity (44)where τ is the contact time,
γ
is the coefficient of surface tension of the impacting droplet, ρ
is the density of the liquid, and R is the diameter
of the droplet. Here, we also applied the same equation to explain
the realtivecontact time observed in our experiment. The R of the merged droplets for different TI is the same since there was no loss of mass during the coalescence
process. With the same ρ, eq can be simplified to eq With the average
temperature in the range
of 27–48.5 °C, the change of surface tension is only 5%[43] and the contact time thus remained relatively
constant, which was consistent with the experimental observation in Figure b,c. Certainly, here
we ignored the interaction between the droplets and the SH Si NW surface,
which was negligible during the first contact since the temperature
of the water interface interacting with the SH Si NW surface was maintained
at 27 °C.
Figure 5
Contact time of droplet collision with impacting droplets
set at
different temperatures. The schematic insets in the plot show the
merged droplets before their departure from the SH Si NW surface when
the temperature of impacting droplets was set at 27, 45, and 70 °C.
Contact time of droplet collision with impacting droplets
set at
different temperatures. The schematic insets in the plot show the
merged droplets before their departure from the SH Si NW surface when
the temperature of impacting droplets was set at 27, 45, and 70 °C.Besides the study of the interaction of the two
droplets during
their first impact, spreading, and rebound, we also investigated their
subsequent impact, spreading, and rebound processes. Figure a shows the schematic of the
1st and 2nd maximum spreading of two droplets when TI and TS are both at room
temperature, and Figure b shows the schematic of the 1st and 2nd maximum spreading of two
droplets when TI > TS. The plots in Figure c,f represent the relationship between the dimensionless
spreading
length ψ (ψ = l/D0; l is the measured spreading length of the
droplet, and D0 is the initial diameter
of the droplet) and dimensionless time t (t = tmv0/D0; v0 is the initial impact velocity of the droplet; and tm is the real time measured in the experiment, which starts
from the maximum spreading during the first impact). As the TI was set at 27 °C, the maximum spreading
length, which represented the remaining energy of the system in the
form of surface energy after coalescence, was about 1.3 (Figure c). When TI increased to 45 °C, the maximum spreading
length increased to ∼1.6 (Figure d) and then stayed close to ∼1.6 with
the increase of TI (Figure e,f). The increase in the maximum spreading
length indicated the increase of the surface energy after the coalescence
process, which also implied that there was less energy loss or less
energy dissipation during the coalescence process for TI = 45 °C than for TI = 27 °C. Another interesting observation is the number of rebounds
at each temperature. Figure c shows that the merged droplet after coalescence at TI = 27 °C only rebounded twice due to the
relatively low energy remained after coalescence. When TI increased to 45 °C (Figure d), however, the merged droplet rebounded
five times due to the reduced energy loss during the coalescence process.
With the further increase of TI, the number
of rebounds for the merged droplets decreased to four times and three
times at 60 and 70 °C. Such decrease in rebounds might be due
to the increased interaction of the merged droplets with the substrate
surface at elevated temperature.
Figure 6
Spreading and rebounding of the two droplets
with different TI. The schematics in (a)
and (b) represent the
first spreading at maximum length and the 2nd spreading at maximum
length: (a) TI = TS = 27 °C. (b) TI > TS = 27 °C. The plots represent the change
of the spreading length with the time for different TI: (c) 27 °C, (d) 45 °C, (e) 60 °C, and
(f) 70 °C.
Spreading and rebounding of the two droplets
with different TI. The schematics in (a)
and (b) represent the
first spreading at maximum length and the 2nd spreading at maximum
length: (a) TI = TS = 27 °C. (b) TI > TS = 27 °C. The plots represent the change
of the spreading length with the time for different TI: (c) 27 °C, (d) 45 °C, (e) 60 °C, and
(f) 70 °C.To understand the spreading and
rebounding behavior, we also analyzed
the change of system energy during these processes. Figure S5 showed such analysis for TI = 27 and 45 °C. Before the release of the impacting
droplet, the energy at the initial state was the sum of surface energy
of the two droplets and the gravitational potential energy of the
impacting droplet. During the falling of the impacting droplet, the
gravitational potential energy converted to kinetic energy. When the
two droplets collided, the droplets began to deform and part of the
kinetic energy was transformed to the surface energy. The surface
energy reached its maximum value at the maximum spreading and the
kinetic energy decreased to zero at that moment. During the deformation
and spreading process, a part of the kinetic energy was lost due to
the following three possible energy loss or dissipation mechanisms:
the viscous loss, the loss due to internal vibration of the droplet,
and the loss due to the interaction with the underlying surface. The
viscous dissipation is one of the most common energy dissipation mechanisms
during the droplet coalescence. The viscous dissipation varies with
the change of the droplet shape and internal liquid flow during the
coalescence process.[47,48] Reynolds number (Re = ρVR/η, ρ is the density of
the liquid, V is the velocity of the droplet, R is the radius of the droplet, and η is the viscosity of the liquid) represents the ratio between the
inertia and the energy dissipated in viscous loss. As Reynolds number
increases, the viscous dissipation tends to decrease.[47,48] Besides the viscous loss, the loss related to the internal vibration
and liquid movement is also needed to be considered in the process.
A part of the translational kinetic energy could be possibly transferred
into internal vibration during the shock of the merging process,[49,50] especially at the low temperature. As shown in Figure , the droplets went through
a large deformation before merging when the impacting droplets were
set at TI < 40 °C. The time of
their merging was usually close to the moment of maximum spreading
length of stationary droplet. At that moment, the stationary droplet
was going to bounce but the impact droplet might still have the kinetic
energy. The difference of the velocity direction between the fluid
within the two droplets produced the velocity gradient inside the
merged droplets, which resulted in the loss of kinetic energy through
internal rotation and inner mixing.[51] Compared
with the merging process at higher TI,
the merged droplet at 27 °C showed a relatively more internal
fluid movement during the rebound from the surface at first time.
The red dye within the merged droplet showed the chaotic mixing clearly.
This chaotic mixing is the main factor of energy loss when TI was low.When TI increased, the interaction
of the merged droplets with the underlying substrate surface, which
was related to the wetting property of surface, also played an important
role in the energy loss during the spreading and rebounding processes.
The stationary water droplets showed a Cassie state on the SH Si NW
surfaces in this study, with an advancing contact angle of ∼162°
and receding contact angle of ∼147° (Supporting Information). As the temperature of the water droplet
in contact with the SH surface increases, the contact angle will normally
decrease and the sliding angle will increase.[52] When the impacting droplet was set at room temperature, the merged
droplet had the same temperature as TS and the interaction with the underlying SH surface was the same
as the original stationary droplet (Figure a). Even when TI was higher than 27 °C, with the observation of the separation
of the cold water (bottom of the merged droplet) and hot water (top
of the merged droplet) and the theoretical analysis of the heat diffusion
length (Supporting Information), there
was little heat transfer from the hot impacting droplet to the cold
stationary droplet before the first rebound (Figure b). After the first rebound, however, there
were fluid mixing and also heat transfer inside the merged droplets.
Such mixing and heat transfer increased the temperature of the merged
droplet and also the water interface in contact with the SH surface,
which also resulted in the increase of the vapor pressure at the interface.
The water interface with increased temperature could transfer some
of the heat to the underlying surface (Figure b). The increased vapor pressure at the water–Si
NW interface could also lead to the condensation of water vapor on
the relatively cold SH surface. Both the heat transfer to the solid
surface and also the condensation would increase the attractive interaction
between droplets and the surface and also the pinning of the liquid
to the surfaces.[53−55] As the temperature of the merged droplet increased,
the droplet gradually transferred from the initial Cassie state to
a partial Wenzel state.[36,56] The combination of
these factors made the droplet prone to be stuck on the surface. As
shown in Figure d,
the merged droplet at TI = 45 °C
rebounded 5 times while the merged droplet stuck on the surface only
after the third rebound when TI = 70 °C
(Figure f). Besides,
as shown in Figure d,e, the contact time of the merged droplet became larger during
the subsequent rebound, which indicated a slight increasing trend
attributed to the factors mentioned above.
Conclusions
In
summary, this work studied the coalescence, spreading, and rebound
processes of two colliding droplets, with the stationary droplet sitting
on a SH surface, and the impacting droplet at elevated temperatures.
Through the use of dye and also high-speed color video imaging, the
relatively detailed observation of the change of the droplet interface,
and the internal movement of the merged droplet were observed. The
energy conversion during the coalescence, spreading and rebound was
also discussed. The increase of the impacting droplet temperature
resulted in less energy loss during the coalescence process. Optimizing
the impacting droplet temperature can lead to more rebound after the
coalescence. Such findings will help further the fundamental understanding
of the two droplets interaction at different temperatures, which will
be helpful in generating different engineering approaches for relevant
applications involving droplet interactions, such as thermal spray,
ink jet printing, and microfluidics. The efficient retaining of kinetic
energy with the high impacting temperature also provides a strategy
for the efficient separation of the merged droplets from the underlying
substrate, which could help the removal of hot droplets from solid
surfaces, such as the condensed droplets in dropwise condensation
systems.
Authors: Thomas M Schutzius; Stefan Jung; Tanmoy Maitra; Gustav Graeber; Moritz Köhme; Dimos Poulikakos Journal: Nature Date: 2015-11-05 Impact factor: 49.962