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The Influence of Surface Tension and Equilibrium Contact Angle on the Spreading and Receding of

Water Droplets Impacting a Solid Surface

Philip A. Lin, Alfonso Ortega


Villanova University
800 W. Lancaster Ave.
Villanova, PA, US, 19085
Phone: (215) 798-0110, 6lO-519-7440
Email: plin02@villanova.edu, alfonso.ortega@villanova.edu
Web: www.villanova.edu/latfs

e equilibrium
ABSTRACT
o initial
An experimental investigation was performed to study the max at maximum spreading diamater
effect of surfactant on the spreading and receding of water
droplets on a flat, isothermal surface. Sodium dodecyl sulfate Superscripts
* dimensionless
(SDS) was added to water to lower both the surface tension
and the equilibrium contact angle. Two parameters, initial INTRODUCTION
velocity and initial droplet diameter, were varied. A high­
One of the endemic problems with spray cooling as a high
speed camera recorded the droplet deformation process,
heat flux cooling technology is that the coolant flow is used
including both the spreading and receding phases. Adding the
inefficiently due to the lack of understanding of the basic
surfactant had two primary effects on the spreading phase; it
mechanisms of droplet impact and subsequent evaporation
increased duration of the spreading phase and increased the
and/or boiling. In order to ensure satisfactory reliability
spreading rate of the droplet. Both of these effects ultimately
margins, excessive flow rates are used even though the
resulted in an increased maximum spreading diameter. In the
subsequent liquid flooding significantly decreases
receding phase, the surfactant decreased the rate of receding.
performance. Ideally the flow delivered in the liquid phase
In the initial deformation process, it was found that the droplet
should just balance the amount of fluid that leaves the system
collapsed at nearly a constant rate, regardless of surfactant
in the vapor phase after evaporation and/or boiling has
concentration. Maximum spreading diameter was found to
occurred on the target surface. The research reported in this
agree with several analytical models from different sources
paper is part of a program aimed at improving our
within 10%. Instantaneous spreading diameter was compared
understanding and increasing the efficiency of droplet
to an energy balance model, which also showed good
impingement followed by thin film evaporation from a heated
agreement.
surface.
KEY WORDS: spray cooling, droplet impingement, One way to increase droplet spreading and promote thin
surfactant film evaporation is to add surfactant to the water to lower
surface tension and the equilibrium contact angel, Be.
NOMENCLATURE
Several authors have studied the effect of surface tension and
D diameter of droplet, mm
contact angle modification by surfactant addition on droplet
V velocity, m/s
impingement and spreading [1-4]. Stone and Leal [1] did
h droplet height, mm
analytical and computational work on the effects of dynamic
r droplet radius, mm
surface tension on the droplet impingement process. Their
s fitting parameter
results showed an effect of surface tension on droplet
time, s
spreading and even asymmetrical spreading.
Ediss energy dissipated through viscous forces, J
Stoebe et el. [2] experimentally studied the effect of
KE2 kinetic energy of droplet during spreading, J surfactant on droplet spreading rate. In this study, surface
SE2 surface energy of droplet during spreading, J characteristics were modified by gold deposition and the
authors found surface energy had a strong effect on spreading
Re Renolds number(pDoVo I JI)
2 rates. They showed that SDS solutions do not spread on
We Weber number (pDoVo I () ) Parafilm and polyethylene, which are hydrophobic surfaces,
spread effectively on hydrophilic surfaces. Both SDS and
Greek sym bois
trisiloxane lower surface tension but only trisiloxane increases
e contact angle, degrees
3 spreading on Parafilm.
p mass density, kg/m
Zhang and Basaran [3] performed experiments with
(J surface tension, N/m
droplets varying from 1 mm to 3 mm. Their results clearly
fJ viscosity, kg/s*m
show that adding SDS increased maximum spreading.
� spreading factor ( D I Do ) Furthermore, large concentrations of Triton were shown to
impede spreading at velocities greater than 3 m/s.
Subscripts
a advancing

978-1-4244-9532-0/12/$3l.00 ©2012 IEEE 1379 13th IEEE ITHERM Conference


Mourougou-Candoni et el. [4] experimentally created 2 EXPERIMENTAL RESULTS
mm to 3 mm droplets from a height of 70 cm using one needle
size and ten different surfactants. They found water had the Effect of Surfactant on Maximum Spreading

largest maximum spreading factor. This is explained by the Adding surfactant had a noticeable effect on contact angle
increasing droplet diameter increases Re number which has a and surface tension. Without surfactant, Be was measured to
positive effect on (max so it is important to compare droplets be approximately 40 degrees. Once surfactant was added, Be
with the same Re to study the effects of surfactant on (max . decreased to about 20 degrees. At maximum spreading, the
The present research sought to contribute to the droplet lamella was so thin that Ba could not be measured. As
experimental data by a parametric study. The effect of adding suggested by others [6, 7], there is a large degree of
surfactant on the droplet impingement process was studied at uncertainty in these measurements as only the macroscopic
various different velocities and diameters. This data was then contact angle was visible in this experiment. Coupled with
compared to several theoretical models that were developed, hysteresis effects also documented in previous studies [8], the
in order to gage the different models' validity in predicting uncertainty in the Be may be as high as +1- 20 degrees.
droplet spreading and receding when surfactant is added.
Figures 1 and 2 show the effect of surfactant on ';max and
Additionally, the effects of surfactant on the important
the increase of the maximum surface area, respectively, at
parameters surface tension and equilibrium contact angle, Be
various droplet velocities and diameters. Figure 1 summarizes
and subsequently, droplet spreading and receding, were
sixty-five trials, thus each column represents the average of
studied.
about five data points. Figure 2 not only makes clear that
EXPERIMENTAL METHOD adding surfactant increases spreading, but also shows two sub­
trends: 1) the effect of surfactant decreases with decreasing
Droplets were manually formed one at a time using a
diameter and 2) the effect of surfactant decreases with
Hamilton glass syringe suspended over a three inch silicon
increasing velocity.
wafer by a ring stand. Droplets were accelerated by gravity
and initial impact velocities, Vo, were varied by varying the
5.0 ,------,
free fall distance. The liquid used was distilled water or a 1000 _OPPIII
ppm by weight sodium dodecyl sulfate (SDS) solution with _1000PI'III

water. Different diameter droplets, Do, were generated by


4.5
using different gage Hamilton needles. 22 gage and 33 gage
needles were used to created 3 mm and 2 mm pure water
droplets, respectively. 18 gage and 30 gage needles were used
4.0
to create 3 mm and 2 mm 1000 ppm SDS water droplets due
to the decreased surface tension of the SDS solution. The
surface tension of the surfactant solution was measured to be
n.5
."po
0.045 N/m using the method described by Fordham [5].
Images were captured at 20,000 frames per second using a
Phantom v7.l high speed camera. A Zeiss Makro­
3.0
Planar T* 100mm F/2 ZF.2 Lens provided a 1:2 magnification
ratio. Images were post processed using imaging software
provided and calibrated using a common standard.
2.5
After each trial, the surface was cleaned with distilled
water and dried with a lint free paper. All properties and
measurements were taken at room temperature, which was 0.0 ..-_-._______L-II__"---__I-J__OU
1.0 m/s I. 7 m/s 2.8 IIl/s 1.0 IIl/s I. 7 Ill/s 2.8 IlI/s
constant at 22°C (±2 0c) for this experiment.
Table 1 lists the values tested for each parameter in the 3111111 2111111

experiments. The values chosen enabled twelve unique


combinations of the parameters to be tested. This allowed the
effect of surfactant at various velocities and diameters to be
Fig. 1 Effect of surfactant on ';max at various droplet velocities
studied. Of the droplets tested, the Re numbers ranged from and diameters
2090 to 8790 and the We numbers ranged from 27 to 522

Table 1 Values tested for each parameter in experiments

Velocities, Diameters, Surfactant


(m/s) (rum) Concentrations (ppm)
1 2.1 o
1.7 3.0 1000
2.8
35 value. Several studies have investigated the effect of dynamic
surface tension on droplet impingement ([9-11D.
Pasandideh-Fard et el. [9] found that using two different
'" 30
..
... values for surface tension, 0.073 N/m and 0.045 N/m, in their
'"
�� computational models made little difference in their
"
:a 25 computational results. Using a value of 0.073 N/m actually
'"
...
... gave slightly better fit to their experimental results,in fact.
=-
"' .. In later work, Mourougou-Candoni et el. [10] studied the
== .5 20
"
" <.J effect of dynamic surface tension on the droplet impingement
;: ..5
" ... process with large (2 to 3 mm) and small (0.7 to 0.8 mm
" "
'" 15 droplets) using two surfactants, neither of which were SDS.
"

. : .. They determined the dynamic surface tension value at the time
.. "
"' "::0 of maximum spreading for each droplet using the maximum
'"
... 10
...
....
bubble pressure method [12] and developed a theoretical
.: model that improves on a previous model [9] by including
0:; 5 dynamic surface tension values.
OJ
...
... Crooks et el.'s [11] experimental work found that the

surface material and surface tension had a negligible influence
1.0 IlIls 1.7 IlIls 2.8 Illls 1.0 IIIls 1.7 IIIls 2.8 IlIls on the maximum spreading diameter, although the droplet

3mm 2111111 height and receding were significantly affected. They dropped
different solutions on surfaces that were both hydrophobic and
V._ D.
hydrophilic (Parafilm M and quartz glass surfaces treated
Fig. 2 Effect of surfactant on the maximum surface area separately with dichlorosilane and polysysytrene). The authors
covered by the droplet at Dmax stated that below critical micelle concentration (CMC), the
accumulation of surfactant in the drop is driven by the fluid
dynamics and is not comparable to dynamic surface tension
+10%
data obtained from the bubble pressure method. At above
CMC however, the response of dynamic surface tension
-111% matched between the maximum bubble pressure method and
the droplet experiments.
In the current work, no adjustments were made for
dynamic surface tension in comparing experimental results to
six different models [9,10,13-17]. The models predicted both
the experimental results for pure water and water with
surfactant equally well (Fig. 3). It was thus assumed that the
difference between dynamic surface tension and static surface
tension effects were negligible.

Droplet Spreading Dynamics


Figure. 4 and 5 depict the experimental behavior of
droplet spreading factor with respect to dimensionless time
*
t =tVo I D o . As presented in Fig. 1, surfactant has a much

more noticeable effect on the larger 3 mm droplets (higher Re


number). Yet the maximum spreading factor results in Fig. 1
fail to capture the effects of surfactant in the later receding
5 6
regime of the droplet. Figures 4 and 5 show that the droplet
Experimental �"'"' recedes at a much slower rate with the addition of surfactant.
This is especially noticeable at the higher velocity for both
Fig. 3 Comparison of Experimental ';max to Theoretical ';max
droplet diameter cases. This effect of surfactant on droplet
from Various Models [9,10,13-17]
receding is important when heat transfer occurs and will be
Dynamic Surface Tension investigated in future research.
A potential concern with surface tension measurements is Figure 4 conveys the importance of studying the impact
the dynamic nature of surface tension. It is well known of surfactant on the receding phase,and not just the maximum
phenomenon that the surface tension of a liquid will vary in spreading factor. Figure 4 shows that the difference between
time as the surfactant diffuses to the free liquid surface. As the the maximum spreading factor and rate of spreading up to the
surface area of the free liquid surface changes during the time of maximum spreading for cases with and without
droplet impingement process,the surface tension changes. The surfactant are negligible. After the instant of maximum
value for surface tension used in calculation Weber number, spreading however, the surfactant plays an important role on
We, for the models was the measured static surface tension the receding phase of these droplets.
Figure 4 shows that for smaller droplets, surfactant Figure 6 compares the previously shown experimental
decreases the recession of the droplet. For the larger droplets, data with model predictions developed by Attane et el. [18].
Fig. 5, surfactant significantly increase the maximum Attane used the energy equation in differential form,
spreading and decreases the droplet recession. d
- ( KE2+SE2+Ed'ss ) = 0 (1)
dt
5
where, as before, KE2 , SE2, and Ediss are the kinetic energy
• 1.0 OIls

of the droplet, surface energy of the droplet, and energy loss
1.7 OIls
... 2.8 OIls due to viscous dissipation, respectively, during the spreading
4 • o ppm and receding regimes. Attane et el. proposed an improved
• 1000 ppm rimmed disk I-D model over the spherical cap model
proposed by Bechtel et el. [19] and the cylinder model used by

[ ( )]
• Kim and Chun [20] for deriving the energy terms in Eq.
3
• (3.26). The [mal form of the Attane et el. model was
• . 2 [ ]
Id 1 dr Id . 1
u.J' .. . .. �
••• • • -- 1+ --
. - +--- r l-cosBe +-* ( ) +

18dt 30r 6 dt Wedt 3r
2
. 2

(2)
4
- 3r
*4
+-*-
2
)( )
dr
-
2 +sr

=0
Re ( 3r dt

with initial conditions

*2
1= ro
[ I-COSBe +
( ) :]
3 0
* for Be <lO9°,

0.1 10 ro' = 0.39 for Be > lO9°, and (3)


-1/2
dr' 1 =
(2+ 1 )
Fig. 4 Effect of Surfactant on Experimental Spreading Factor dt 0 l 3 45ro'6
where s was determined by fitting the following power-law
Behavior with Respect to Dimensionless Time for a 2
mm Droplet at Various Velocities
variation of s with Oh (Oh = JWe / Re ) with experimental
data,
2
• 1.0 mls .......
. .... s = l.41 h - / 3
0 • (4)
• 1.7 OIls For Figs. 6 and 7, a coefficient of l.6 instead of lAI was used
... 2.8 mls
because it provided a better general fit to the experimental
4 •

0 ppm
1000 ppm .
.... data.

.... In Fig. 6, the Attane et el. model follows the general trend
... of the droplet behavior over time and performs especially well

.. .. ... for the higher Re number droplets with no surfactant. With


3
... surfactant, Be was set to 20 degrees and without surfactant, Be
...

....
was set to 40 degrees, based on experimental measurements.
When droplets with surfactant were modeled, the spreading
2 factor was generally over predicted, but the results for 3 mm
droplets at l.7 mls and 2.8 mls were excellent.
Early time scales do not match because the model
assumes the droplet to have a cylindrical shape with an outer
rim that is compressed and spreads out as the droplet
impinges. While this is true in the later stages of droplet
impingement, in the earlier stages, the droplet assumes the
shape of a truncated sphere.
0.1 10

Fig. 5 Effect of Surfactant on Experimental Spreading Factor


Behavior with Respect to Dimensionless Time for a 3
mm Droplet at Various Velocities
• Experimental. 0 I>pm
• E�I)eril1lentltl. 0 ppm
• Exprrimenlal. 100011Pl1l
• Experill1ental. IOOOppm
--Theoretical. 0 ppm
--Theorelical, 0 ppm
4 Theorelical. 1000 Pilln 4 --Theoretical. 1000 ppm



2

0.1 10 0.1 10

a) 2mm, 1.0 m/s d) 3mm, 1.0 m/s

• Experimenlal.O ppm
• Expcrimcntnl.O ppm
• Experi",enlal. 100011Pl1l
• Expe.-ill.ll'ntnl. IOOOppm
--:rheorClical.O ppm
--Theoretical. 0 ppm
4 Theorelical. 1000 ppm 4 --Theoretical. 1000 ppm

......

3 3 •

2 2

0 0
0.1 10 0.1 10

b) 2mm, 1.7 m/s e) 3mm, 1.7 m/s


5 5
.. .. Experimental. 0 ppm
E�pcrilUentltl. 0 I>pm
.. .. Exprrimenl3l. 100011Pl1l
Expe.-illll'ntni. IOOOppm
Theoretical, 0 ppm
--Theoreticlll. 0 ppm
4 --Theorelic"l. 1000 ppm 4 --Theorelical, 1000 ppm

,. ..... ..
..
..
3 3
..

u.1' .. u.1'

2 2

f
.. ..
.. ..

0 0
0.1 10 0.1 10

C) 2mm, 2.3 m/s t) 3mm, 2.3 m/s

Fig. 6a-fComparison of Experimental and Theoretical Spreading Behavior for


both 2 mm and 3 mm Droplets and Various Velocities
• -----2111111,OPPII1
The Attane et el. model can also be used to determine the
... -----2111111 , l000ppll1
• -- 3m 111 , 0PPII1
effects of Be and surface tension (We number) on the
• -- 3mll1,IOOOppm spreading behavior. Figure 8 shows that decreasing Be mainly
3 affected the long term behavior of the droplet as it comes to
rest,increasing its equilibrium diameter,while having a small
increase on the maximum spreading diameter. At the lowest
.. . . . .. Be' 10 degrees,the droplet barely receded and remained at a
».1' 2 constant diameter equal to its maximum spreading diameter.
At the highest Be' 110 degrees, the droplet receded a
.... �.-.: . • considerable amount and even showed a relaxation phase as it
came to rest, which matches experimental observations on
hydrophobic surfaces.
Figure 9 shows that according to the Attane et el. model
We number has a greater effect on the maximum spreading
diameter,but no effect on the equilibrium spreading factor. A
droplet with more surfactant will only take longer to reach its
equilibrium diameter.
O L-������L-��
0.01 0.1 10 100 1000 These predictions by the Attane et el. model are important
'" in that the effects of Be and We number are somewhat
t
independent. Generally,it can be concluded from the Attane et
Fig. 7 Effect of Surfactant on Long Term Experimental
el. model that Be affects the equilibrium spreading factor
(Points) and Attane et el. Model (Lines) Spreading
Factor Behavior with Respect to Dimensionless Time while We number affects the maximum spreading factor and
for Droplets at 1 mls time needed to reach equilibrium.

Figure 7 shows the same data in Fig. 4 for droplets falling


at 1 mls at longer time scales but the time scale is extended to
show when the droplet comes to rest in its equilibrium state.
Each set of data was pieced together with two droplet runs as
4
the high speed camera only had enough memory to capture the
initial spreading behavior at high frame rates or the long term
behavior at slower frame rates. More importantly, in Fig. 7,
the Attane et el. model correctly captures the long term 3
trending differences in droplets with and without surfactant,
although there is a large discrepancy between the model and
the data for droplets with surfactant. This implies that the
effect of surfactant on inhibiting droplet receding is partially 2
explained by modifications in surface tension and contact
angle as a result of adding surfactant.
These experimental results paired with the model,
validates the model's ability to predict the trend in both
spreading and receding in the ranges of the parameters tested
for droplets with and without surfactant. The model is more
accurate when compared to experimental trials without
O '--��-----'-�--J._�---".-�---L-�--'
surfactant and significantly off for trials with surfactant, o 20 40 60 80 100
especially at the lower velocities (Figs. 6a and 6d),implying ..
there is a parameter in addition to surface tension and contact t
angle that is not being accounted for. Fig. 8 Effect of Be on the instantaneous spreading factor
In summary, Figs. 6 and 7 show that surfactant has the predicted by the Attane et el. model for a 3 mm droplet
primary effect of decreasing the droplet receding phase and in at 2.8 mls. Be was varied from 10 degrees to 110
some cases eliminating droplet recession. Thus the
degrees in 10 degree increments. The blue and red lines
equilibrium droplet spreading factor remained roughly
are provided for reference and correspond to the same
constant after achieving its maximum value. Surfactant did not
color lines in Fig. 5.
significantly change the rate of spreading during the spreading
phase, but in the case of 3 mm droplets, it did prolong the
spreading phase so that the maximum spreading factor was
increased.
response time to equilibrium. This means that an increase in
equilibrium spreading may be achieved by merely modifying
5
the contact angle, such as coating the surface with a chemical
or mechanically etching the surface. In a commercial or
industrial cooling process, this would avoid surfactant buildup
4 on the surface over time as the water evaporates. Lastly, it was
found that all droplets tested in this study collapsed at the
same rate during the length of time it took each droplet to
move a distance equal to its initial diameter. This fmding
3
could be used to improve the accuracy of the Attane et el.
model at early times.

2 I
0.9
0.8
0.7
·
-- We= 100-1000 0.6 h '= 1.264e(-t /I·066J_0.263
-- Oppm
-- IOOOppm 0.5

O ��--�--��--�--L-�-�
o 20 40 60 80 100 0.4

t
'.Q 0.3
Fig. 9 Effect of We on the instantaneous spreading factor
predicted by the Attane et el. model for a 3 mm droplet
at 2.8 m/s. The blue and red lines are provided for
reference and correspond to the same color lines in Fig. 0.2

5.
Dimensionless Height with Respect to Dimensionless Time

One last observation made is on the response of


dimensionless height with respect to dimensionless time. 0.1 L _�__ ----L__ ���:J
2
Figure 10 plots the instantaneous height with respect to
dimensionless time for thirteen different runs at various Re t
and We numbers. Interestingly, all the plots collapsed onto the
Fig. 10 Dimensionless Droplet Height with Respect to
same line before leveling off once maximum spreading was
* * Dimensionless Time for Thirteen Different Droplets at
reached. Up until t = 1, h (h I Do) follows the form of an
Various Re and We Numbers
*
exponential decay with respect to t . This data suggests
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during the initial length of time it takes the droplet to move a
distance equal to its initial diameter, all droplets collapse at the
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