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Energy 30 (2005) 209–220

www.elsevier.com/locate/energy

Effect of surface wettability on boiling and evaporation


Y. Takata , S. Hidaka, J.M. Cao, T. Nakamura, H. Yamamoto,
M. Masuda, T. Ito
Department of Mechanical Engineering Science, Kyushu University, 6-10-1 Hakozaki, Higashi-ku,
Fukuoka 812-8581, Japan

Abstract

Titanium dioxide, TiO2, is one of the photocatalysts that has a very unique characteristic. The surface
coated with TiO2 exhibits extremely high affinity for water by exposing the surface to UV light and the
contact angle decreases nearly to zero. On the contrary, the contact angle increases when the surface is
shielded from UV light. We applied this superhydrophilic nature to enhancement of boiling and evapor-
ation heat transfer. Experiments of pool boiling and evaporation of single water droplet have been per-
formed to manifest the effect of high wettability on heat transfer characteristics. Both of TiO2-coated and
non-coated surfaces were used for comparison in each experiment. It is found that (1) the critical heat
flux (CHF) of TiO2-coated surface is about two times larger than that of non-coated one, and (2) Leiden-
frost temperature increases as the contact angle decreases. The superhydrophilic surface can be an ideal
heat transfer surface.
# 2004 Elsevier Ltd. All rights reserved.

1. Introduction

Titanium dioxide (TiO2) is one of the photocatalysts that has very attractive characteristics.
First, it decomposes various organic substances by its strong oxidizing power under ultraviolet
(UV) irradiation. This ability is widely used in environmental purification as anti-bacterial, anti-
pollution and deodorant materials. Another amazing nature, which was discovered quite
recently, is a superhydrophilicity [1–4]. When the surface coated with TiO2 is irradiated by UV
light, the contact angle for water decreases with time and finally reaches almost zero as illus-
trated in Fig. 1. This nature has various practical applications such as anti-fogging glass and
self-cleaning effect. When TiO2-coated glass is exposed to water steam, the droplets on the


Corresponding author. Tel.: +81-92-642-3398; fax: +81-92-642-3400.
E-mail address: takata@mech.kyushu-u.ac.jp (Y. Takata).

0360-5442/$ - see front matter # 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.energy.2004.05.004
210 Y. Takata et al. / Energy 30 (2005) 209–220

Fig. 1. Photo-induced superhydrophilicity.

surface form very thin film and the glass becomes transparent. The self-cleaning effect is used to
remove oil materials from the surface since the TiO2-coated surface has more affinity for water
than oil. These effects have already been applied to the anti-fogging side-mirror film, coating of
automobiles and various construction materials that can be self-cleaned easily by rainfall. Tech-
nologies of superhydrophilicity are now expanding rapidly its application fields.
The authors expect that heat transfer characteristics of liquid–vapor phase change phenom-
ena like boiling and condensation can be controlled and/or enhanced by UV irradiation making
use of TiO2-coated surface. It is very intriguing to know the difference between TiO2-coated sur-
face and normal surface. For example, bubble size, incipience, critical heat flux (CHF) and
minimum heat flux points (MHF) in boiling may be influenced. First, we applied it to the falling
film evaporation in which thin stable film can be realized even in extremely low flow rate region
[5]. As a result, heat transfer is enhanced tremendously in low flow rate and low heat flux
regions. Second, the experiment of immersion cooling of hot metal has been studied [6]. TiO2-
coated specimen was cooled down more rapidly than non-coated one because the film boiling
regime breaks down at higher temperature.
In the present study, we will report two different experimental results; one is pool boiling and
the other is droplet evaporation on hot surfaces. The pool boiling experiment is performed by
means of steady state measurement to reveal the effect of wettability on CHF and MHF points.
The main interest is focused on the effect of wettability on the CHF point. TiO2-coated and
non-coated surfaces are compared with each other. Effect of wettability on CHF and MHF has
been studied so far by many researchers. Chowdhury and Winterton [7] have reported that the
MHF temperature increases as the contact angle decreases. Costello and Frea [8] pointed out
that the CHF and its temperature increase as the surface wettability increases. However, the
v
smallest contact angle covered by their experiments is about 2127 and there has been no
experimental study on boiling heat transfer on superhydrophilic surfaces.
The experiment of droplet evaporation aims to make clear the effect of contact angle on the
evaporation time. Wetting limit temperature, TWL, is measured instead of Leidenfrost tempera-
ture, TLEID, by the reason described later. Usually, the different materials have been used as the
heat transfer surface to change the contact angle in the previous studies. However, when chang-
ing materials, thermal condition of the surface varies as well. In the previous works it was not
possible to conduct experiments in which the contact angle is the exclusive parameter. The
present study realized such a desirable experiment. We can manipulate the contact angle by UV
light only. To realize this, we have developed some TiO2-sputtered copper surfaces changing the
sputtering conditions and measured their contact angle, boiling and evaporation characteristics.
Y. Takata et al. / Energy 30 (2005) 209–220 211

2. Coating process and contact angle

2.1. Dipping process

We used two different coating methods; one is a dipping process and the other is a sputtering
process. In the dipping method, TiO2 suspension containing 20 wt% of SiO2 is used.
The test samples for dipping method are copper and glass plates. Prior to dipping, these sam-
ples are cleaned and dried. The copper plate is polished to mirror finish and washed by hydro-
chloric acid and then by ethanol. Glass plate is cleaned only by ethanol. When the surface
becomes dry, the samples are dipped into TiO2 suspension then extracted slowly. After this dip-
v
ping process, the samples are heated by electric furnace and maintained at about 150 C for an
hour. The thickness of the coated layer is of about 1 lm. These samples are stored in a dark
place for a week to make the surface hydrophobic state. The change in contact angle was meas-
ured in the previous study and the further detail should be referred to the literature [5].

2.2. Sputtering process

A new challenging method to create a strong TiO2 layer has been tried by making use of RF
magnetron sputtering process. The sputtering target used is a titania plate and it takes more
than 8 h to produce TiO2 layer of 250 nm in thickness on the copper heat transfer surface in the
atmosphere of dilute argon/oxygen mixture.
We have produced many sputtered samples under various sputtering conditions and measured
contact angle under UV irradiation. Figs. 2 and 3 show change in contact angle of best two
samples, denoted as No. 2 and No. 8 samples in the figures. These are produced in the same
sputtering condition.
The contact angle of each sample was measured twice under UV irradiation and each contact
angle, plotted in Figs. 2 and 3, is an average of three different locations. First measurement
designated by the symbols u and l was done in several hours after taken from a sputtering
chamber and the second one designated by the symbols v and h was done after once stored in
a dark place for several 10 h. In the first measurement, the contact angle of No. 8 sample (l)
v v v
decreased with time from 5 to 1 in 1.5 h and finally to 0 after 20 h.

Fig. 2. Contact angle of TiO2-sputtered copper surface under UV irradiation.


212 Y. Takata et al. / Energy 30 (2005) 209–220

Fig. 3. Contact angle of TiO2-sputtered copper surface after shielded from UV irradiation.

After the first measurement, the samples were stored in a dark box. As shown in Fig. 3 the
v v v
contact angle of No. 8 increased from 0 to 10 during 20 min and then finally to 20 after 4 h.
Since the sputtered surface does not contain SiO2 the recovery to the hydrophobic state is faster
than the surface that is coated by dipping process. The contact angle of No. 2 sample exhibits
the same tendency as No. 8 sample.
The second measurement in Fig. 2 was conducted after the measurement of Fig. 3. Initial
contact angle is much higher than that of the first measurement. The contact angle decreased
rapidly in 90 min after the beginning of irradiation. However, the terminal contact angle is
v
about 7 and is much larger than the first measurement. This is because the surface oxidization
changes the surface to hydrophobic state as the time elapses. At this moment, it is hard to pro-
duce a stable superhydrophilic surface.
v
In spite of the instability of the surface, the terminal contact angle of 7 in the second
measurement is by far smaller than that of normal copper surface. So we used these samples as
the heat transfer surfaces in experiments of pool boiling and droplet evaporation. However, this
surface cannot keep low contact angle for a long period as seen in Fig. 3. The contact angle
may increase during experiments. To keep the constant contact angle we have sputtered SiO2 by
120 nm on the TiO2 layer. TiO2SiO2 sputtered surface can keep the constant contact angle for
sufficiently long period. The terminal contact angles used in the experiment of droplet evapor-
v v
ation are 4 and 13 . The TiO2SiO2 sputtered surface seems promising but is under develop-
ment.

3. Pool boiling

3.1. Experimental apparatus

Fig. 4 shows a schematic diagram of experimental apparatus. The heat transfer surface is a
copper cylinder of 17 mm in diameter, facing upward. Heat flux and surface temperature are
measured by thermocouples embedded in the heat transfer block. All measurements have been
Y. Takata et al. / Energy 30 (2005) 209–220 213

Fig. 4. Experimental apparatus for pool boiling.

done in steady state that is judged by monitoring output of three thermocouples. Test liquid is
pure water at saturated temperature.
Before mounting on the apparatus, the surface is irradiated by UV lamp for long hours to
ensure low contact angle. It is also irradiated during experiments. The heat transfer surfaces
used are summarized in Table 1. No. 1 sample is a non-coated surface that is polished up as a
v
mirror surface and the contact angle is 97 in room temperature. The other samples are finished
in the same manner and then coated with TiO2 by dipping or sputtering processes.

3.2. Experimental results

Figs. 5 and 6 show boiling heat transfer characteristics. Measurements have been performed
by increasing heat flux in nucleate boiling region and by decreasing in film boiling region. The
liquid temperature is in saturated temperature. At a glance of Fig. 5, the CHF of TiO2-coated
surfaces (Nos. 3, 8 and 9) is higher than that of non-coated ones (Nos. 1 and 7). Except for the
second run of No. 9 sample, all surfaces are fresh. The No. 3 sample was coated by dipping
before each experimental run. The runs of No. 8 and No. 3 (h) were conducted only to measure
the data in high heat flux region. Only four points were measured as shown in Fig. 6. The CHF

Table 1
Type of heat transfer surfaces in pool boiling

Sample no. Coating method Coating thickness


Nos. 1,7 non –
No. 3 dipping 4 lm
Nos. 2,8,9 sputtering 250 nm
214 Y. Takata et al. / Energy 30 (2005) 209–220

Fig. 5. Boiling heat transfer characteristics.

of No. 7 is larger than that of No. 1 though both of them are non-coated surfaces that were
polished in the same manner. This discrepancy probably arises from the difference in structure
of surface surrounding. The No. 7 sample was slightly bulged out from the vessel bottom and
might have better cooling than No. 1. Anyway, among all samples, the highest value of CHF
was achieved in the second run of No. 9 sample. This is 2.2 times as large as that of No. 1 (non-
coated), 1.5 times as that of No. 7 (non-coated) and 1.7 times as that of Zuber’s theory.
Referring to nucleate boiling region, the TiO2-sputtered surface has excellent heat transfer
characteristics compared with other samples. Kutateladze’s correlation is also plotted as the
dashed line in Fig. 5. On the other hand, the No. 3 sample (l) has characteristics worse than
that of No. 1 (non-coated). The difference between No. 3 and No. 9 samples probably arises

Fig. 6. Details in high heat flux region.


Y. Takata et al. / Energy 30 (2005) 209–220 215

from the difference of coating materials and thickness. It is clear that the coating layer created
by dipping process acts as the large thermal resistance because the layer consists of material that
has low thermal conductivity. Although this coating layer is only 4 lm in thickness, it may
cause several degrees of temperature difference in higher heat flux. On the other hand, the sput-
tered surface does not have this kind of disadvantage. The layer of 250 nm is thin enough to
neglect its thermal resistance.
After the first run of No. 9 sample, the surface was covered by scale that is heavier than non-
coated surface. This is a big problem to the practical use. The second run was conducted with-
out cleaning the scale. Nevertheless, it still has a good heat transfer characteristics as shown in
Fig. 5.
The MHF temperatures of TiO2-coated surface are much higher than that of non-coated one.
It is again confirmed by the present study as seen in Fig. 5. The MHF temperature of No. 3
sample is by 100 K higher than that of No. 1.

4. Evaporation of water droplet on hot surface

4.1. Experimental apparatus

Experimental setup is shown in Fig. 7. Single water droplet is injected to the hot surface
from the syringe and observed by video camera during evaporation. The height of the nee-
dle is fixed to be 10 mm from the hot surface. The micrometer is used to assure each droplet
be of constant size. Different sizes of needles are prepared to change the size of droplets. The
droplet diameters are 2.16, 2.40, 2.66 and 2.96 mm and the corresponding Weber numbers are
v
5.18, 5.67, 6.19 and 6.72, respectively. Temperature of droplet is 20 C in all experiments.

Fig. 7. Experimental apparatus for experiment on droplet evaopration.


216 Y. Takata et al. / Energy 30 (2005) 209–220

Two types of heat transfer surfaces are used; one is a flat surface and the other is a concave
surface, which has a concavity of 0.3 mm in depth from the level of outer rim. The concave sur-
face is adopted in measurements of wide temperature range. Without concavity, the droplet
bounces out from the hot surface at higher temperatures. The flat surface is used to seek wetting
limit temperature, TWL, because of the difficulty in measuring Leidenfrost temperature, TLEID.
Heat transfer surfaces are coated by two different sputtering conditions; one is the surface sput-
tered by TiO2 only, and the other is the surface that SiO2-sputtered layer of 120 nm is added
v
on the TiO2 layer. The former surface has contact angle of 3134 under UV illumination and
v v
8284 in dark. The latter surface has contact angle of 1315 under UV illumination and it
takes very long hours to become hydrophobic state though the contact angle is still small com-
pared with the former surface. Thus the experiment for the latter surface is done only in the
hydrophilic state.

4.2. Experimental results

Fig. 8 shows evaporation curves for concave surfaces. The evaporation curve of normal sur-
face is also shown for comparison with the sputtered surfaces. The contact angles listed in Fig. 8
are those for flat surfaces but not for concave ones. TWL and TLEID in the figure are wetting
limit temperature and Leidenfrost temperature, respectively. These characteristic temperatures
for sputtered surface in hydrophobic state (u) coincide with those for normal surface (h), while
TWL and TLEID for hydrophilic surface (v) increase by 20 K. Since the evaporation curves
designated by u and v are obtained by the same heat transfer surface, the change in TWL and
TLEID is caused only by the difference in contact angle.
To examine the effect of contact angle on evaporation curves, particularly on TWL, experi-
ments using flat surfaces have been performed. The results are shown in Figs. 9–13. The TiO2-
v v
sputtered surface changes alternately between hydrophilic (31~34 ) and hydrophobic (82~84 )
states with and without UV illumination. On the other hand, TiO2SiO2-sputtered surfaces are
v v
used only in the lowest contact angle of 4 and 13~15 because they are newly developed surfa-
ces and the changes in contact angle have not yet been studied clearly.

Fig. 8. Evaporation time versus surface temperature for concave surface.


Y. Takata et al. / Energy 30 (2005) 209–220 217

v v
Fig. 9. Evaporation curve on flat surface for contact angles of 33 and 83 .

v
Fig. 10. Evaporation curve on flat surface for contact angles of 14 .

v
Fig. 11. Evaporation curve on flat surface for contact angles of 4 .
218 Y. Takata et al. / Energy 30 (2005) 209–220

Fig. 12. Evaporation time per unit volume.

As seen from Figs. 9–11, it is found that evaporation time decreases with increase in surface
temperature, decrease in contact angle and decrease in droplet diameter. Prior to each experi-
ment, the contact angle is measured in a room temperature. The angles indicated in the figures
are its ranges or nominal values. From Figs. 9 and 10, TWL increases with the decrease in con-
tact angle but is independent of droplet diameter. However, as shown in Fig. 11, TWL changes
with the droplet size. This difference is discussed below.
These data are rearranged by dividing evaporation time by droplet volume and shown in
Fig. 12. The data for 2.16, 2.40 and 2.66 mm in diameters can be expressed by common solid
lines, while the data for 2.96 mm deviates from the others and are not plotted here. This result
indicates that the evaporation time decreases with contact angle because the initial contact area
between droplet and surface at the collision increases as the contact angle decreases.
Effect of contact angle on TWL is shown in Fig. 13. As seen from the figure, TWL almost
increases with decrease in contact angle. At a glance, it is amazing that the difference between
v v v
the lowest and the highest TWL is about 40 K. The data for contact angles of 14 , 33 and 83
v
are almost independent of droplet diameter. However, TWL for contact angle of 4 depends on
the droplet diameter, namely, increases with the increase in droplet size. It is also noticed that

Fig. 13. Effect of contact angle on wetting limit temperature.


Y. Takata et al. / Energy 30 (2005) 209–220 219

TWL for D ¼ 2:66 mm and 2.96 mm agree with each other. The most interesting point is that
v
TWL for D ¼ 2:16 mm has its maximum at the contact angle of 14 . This was unexpected result
for us, but this is not an experimental error. The result was confirmed by repeated measure-
ments. At this moment, the reason is not clear why TWL has its maximum. Probably, tempera-
ture of the secondary droplet and the recovery of surface temperature relate with each other.
In superhydrophilic state, primary droplet forms extremely thin film that has a very large
contact area compared with the case for large contact angle. Its temperature may increase in a
short period and the subsequent explosive evaporation takes place soon. In this case, the tem-
perature decrease of heat transfer surface is not so large and the temperature recovery will com-
plete before the secondary droplet falls back to the surface. In case of large droplet, on the
contrary, the time for film formation may increase and the surface temperature decreases much
compared with the case of smaller droplet.

5. Concluding remarks

Superhydrophilicity has been applied to boiling and evaporation heat transfer. The contact
angles of TiO2-coated surfaces have been measured under UV irradiation first and then we per-
formed experiments of pool boiling heat transfer and evaporation of single water droplet using
superhydrophilic surfaces. Especially, the effect of contact angle on wetting limit temperature
has been studied. The results are summarized as follows:

(1) The contact angle of TiO2-coated surface gradually decreases with UV irradiation time and
reached to superhydrophilic state.
(2) The TiO2-sputtered surface exhibits excellent heat transfer characteristics in nucleate boil-
ing region and its CHF is higher than the non-coated surface. The MHF temperature is by
100 K higher than that of non-coated surface.
(3) Evaporation time decreases with the decrease in contact angle. The data except for D ¼
2:96 mm can be expressed by a common line as shown in Fig. 12.
(4) The experiments by concave surface depict that the wetting limit and the Leidenfrost tem-
peratures, TWL and TLEID increase with the decrease in contact angle.

The wetting limit temperature, TWL, for flat surfaces increases with the decrease in contact
angle for the droplet diameters of 2.40, 2.66 and 2.96 mm. However, TWL for D ¼ 2:16 mm has
v
its maximum at the contact angle of 14 .
The superhydrophilic surface can be an ideal heat transfer surface and will be applicable to
various heat transfer phenomena that are affected by surface wettability.

Acknowledgements

This study was supported partly by The Iwatani Naoji Foundation’s Research Grant and by
the Grant-in-Aid for Scientific Research (B) 12555059 from the Ministry of Education, Science,
Sports and Culture.
220 Y. Takata et al. / Energy 30 (2005) 209–220

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