Professional Documents
Culture Documents
KAERI (Korea Atomic Energy Research Institute), 989-111 Daedeok-daero, Yuseong-gu, Daejeon 305-353, Republic of Korea
Low Carbon Green Technology Laboratory, Department of Mechanical Engineering (MS312), University of Nevada Reno, Reno, NV 89557, USA
a r t i c l e
i n f o
Article history:
Received 10 October 2010
Received in revised form 30 December 2011
Accepted 24 February 2012
Available online 3 March 2012
Keywords:
Nucleate pool boiling heat transfer
Surface morphology
Aluminum hydroxide
a b s t r a c t
In order to investigate nucleate pool boiling heat transfer characteristics in saturated water, a plain aluminum alloy surface (6061, untreated) and a uniquely fabricated aluminum oxide Nano-Porous Surface
(NPS) sample were prepared. Generally, the NPS exhibited a lower wall superheat at the onset of nucleate
boiling and a higher nucleate boiling heat transfer coefcient than the plain surface. It was also noted that
the nucleate boiling heat transfer coefcient decreased by 30% on the plain surface and by 37% on the NPS
after ve repeated boiling tests. It was found that such performance-degradation in both of the test samples was due primarily to the formation of aluminum hydroxide on the boiling surfaces. It is our belief
that the aluminum hydroxide, formed on both boiling surfaces, signicantly altered the surface morphologies as shown in the microscopic images of the post-boiling surfaces, which resulted in the decrease of
the active nucleation sites. Although NPS is an excellent tool to enhance the nucleate pool boiling heat
transfer coefcient, its life span and usefulness can be impeded by undesirable surface reactions with
working uids.
2012 Elsevier Inc. All rights reserved.
1. Introduction
The development of special surface geometries/structures is a
critical issue for the performance-enhancement of the pool boiling heat transfer. Numerous studies and experiments on nucleate
pool boiling, an effective way to remove high heat ux from a
heated surface, have focused on enhancing the boiling heat transfer coefcient by fabricating micro-scaled surface geometries/
structures [18]. One approach that has success is to create a
number of small micro-porous cavities on the boiling surfaces
to increase the vapor/gas entrapment and the number of active
nucleation sites. These cavities reduce the incipient and nucleate
boiling wall superheats and increase the pool boiling heat transfer
coefcient [9].
While many of the previous studies [18] on the surface structure focused on improving the heat transfer coefcient of pool
boiling in micro-sized dimensions; however, with the evolution
of nanotechnology and nano-materials, our study focused on
well-dened nano-materials suitable for use in pool boiling.
Currently, research of nano-materials used in pool boiling heat
transfer is limited. Vemuri and Kim [9] carried out a brief experimental study on the pool boiling heat transfer of a Nano-Porous
Corresponding author. Tel.: +1 775 784 6931; fax: +1 775 784 1701.
E-mail address: kwangkim@unr.edu (K.J. Kim).
0894-1777/$ - see front matter 2012 Elsevier Inc. All rights reserved.
doi:10.1016/j.expthermusci.2012.02.011
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
151
Nomenclature
A
C1
C2
h
I
i
P
Q
r
T
DT
V
y
Greek Letters
d
thermal boundary layer thickness (m)
h
contact angle ()
q
density (kg/m3)
r
surface tension (N/m)
Subscripts
ave
average value
b
bubble
bottom at the bottom of test section
c
cavity
f
liquid
fg
liquidgas
left
at the left of test section
max
maximum
min
minimum
right
at the right of test section
sat
saturation
sub
subcooling
t
thermal boundary layer
top
at the top of test section
v
vapor
w
wall
further studies on the heat transfer coefcient and long-term performance of the surface in the nucleate pool boiling are needed.
The objective of the present study is to investigate the morphological change of NPS and plain (non-structured) aluminum alloy
(6061) surfaces in a saturated water pool boiling condition, and
the surfaces inuence on the nucleate boiling heat transfer. The
NPS was fabricated utilizing an anodizing technique. Through a
series of repeated tests, the nucleate boiling heat transfers on the
NPS and plain surfaces were monitored. The relationship between
the change of the nucleate boiling heat transfer and the transformation of the surface morphology by the chemical reaction between such surfaces and water were also observed.
2. Experiment
2.1. Sample preparation
Fig. 2 shows the schematic diagram and a photo of the boiling
test section. An aluminum alloy rod (6061, 19.1 mm in diameter
and 101.6 mm in length), with a center hole (9.5 mm wide and
99.1 mm long), was used. Four holes, each 2.4 mm in diameter
and 70.0 mm in depth, were drilled at the top, middle, and the bottom 90 apart along the periphery of the test section. In order to
heat the test section, a cartridge heater (diameter of 9.5 mm and
a length of 76.2 mm) was inserted into the center hole with a high
thermal conductive paste (Omega 201). T-type thermocouples
(Omega) were inserted into the small exterior holes with the high
thermal conductive paste to measure the surface temperatures.
Fig. 1. Typical anodizing process to make nano-porous structure on aluminum alloy (6061).
152
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
Fig. 3. Images of fabricated NPS: (a) FESEM and (b) optical microscope.
The two kinds of boiling surfaces on the test sections were prepared by electro-polishing (plain surface) and multi-step anodizing
(NPS) techniques, respectively. The fabrication process for the
nano-porous coating on aluminum alloy test section was performed in two steps; electro-polishing and subsequent anodizing.
The aluminum alloy specimens were annealed at 400 C for four
hours and then cooled to room temperature. The heat-treated
specimens were electro-polished in perchloric acid and ethanol
(1:4 by vol) at 12 V for ve minutes at 0 C. The nished specimens
were thoroughly rinsed with ethanol and distilled water several
times to remove any organic residues. In order to obtain a uniform
nano-porous growth, multi-step anodizing was carried out in 0.3 M
sulfuric acid. In the pre-anodizing step, the specimen was submerged and anodized in 0.3 M sulfuric acid at 25 V at near 0 C,
and vigorously stirred for 15 h. Then, the sample was placed in a
mixture of 5 wt.% phosphoric acid and 18 wt.% chromic acid (1:1
by vol) at 50 C for an hour. The patterned specimen was thoroughly rinsed with distilled water several times. Under the same
experimental conditions, anodizing was carried out for an additional hour. Then, pore-widening was accomplished using 5 wt.%
phosphoric acid at room temperature for 15 min. The specimen
was again thoroughly washed with distilled water.
In Fig. 3a, the FESEM (Field Emission Scanning Electron
Microscopy, Hitachi S-4700) image of the NPS created by the
multi-step anodizing fabrication process is shown. The wellordered nano-pores, which are approximately 30 nm in diameter,
appeared on the surface. In Fig. 3b, the micro-scale image of the
NPS by digital microscope (VHX-100, KEYENCE Inc.) is also
provided. The dent-like morphology appeared on the top of the
surface in the test section, which could be caused by the pitting
corrosion under the acidic conditions used.
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
Q =A
h
T w T sat
Where Q, A, Tw, and Tsat are power input to the cartridge heater, heat
transfer surface area, wall temperature, and saturation temperature,
respectively. The input power, Q, supplied to the cartridge heater of
test section was estimated utilizing Eq. (2).
Q VI
have
153
In this study, in order to evaluate the average heat transfer coefcients, the temperatures measured at each thermocouple location
were used as the wall temperatures in Eq. (1).
2.4. Experimental details
The experimental procedure, in detail, is described below:
Distilled water was heated to the pre-determined saturation
temperature and boiled to remove dissolved gases.
The auxiliary cartridge heaters were turned off, and the power
to the cartridge heater of the test section was initiated.
The voltage of power supply was increased gradually from 20 to
136 V in intervals of 4 V.
At each increase of voltage, the experimental data was obtained
under the steady state at the atmospheric pressure condition.
The pool temperature for all experiments was maintained within 0.8 C of the saturation temperature. The nominal uncertainty of
the T-type thermocouple was 0.5 C, and the voltage and current
measurements uncertainties were 0.5 V and 0.04 A, respectively.
Based on the method proposed by Kline [14], the estimated
T T sat
2rT sat
r b qv ifg
Where r, rib, qv, and ifg are surface tension, bubble radius, vapor
density, and latent heat of vaporization, respectively. If the temperature change in the thermal boundary layer with thickness, dt, is assumed to be linear, the temperature prole can be expressed as
below:
y
T T f T w T f 1
dt
Fig. 5. (a) Pool boiling curve and (b) heat transfer coefcient of rst test for plain surface and NPS.
154
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
Fig. 7, two points intersected by both Eqs. (4) and (5) indicate the
minimum, rc,min, and maximum, rc,max, values of the mouth cavity
radius, rc. Eq. (6) is then used to predict the size-range of active
nucleation cavities for a given wall superheat.
dt C 2
DT w
fr c;min ; r c;max g
2C 1 DT w DT sub
"
s#
8C 1 rT sat Pf DT w DT sub
1 1
qv ifg dt DT w 2
Where, C1, C2, DTw and DTsub indicate 1 + cos h, sin h, Tw Tsat and
Tsat Tf, respectively. It should be noted that the minus and plus
signs on the right side in Eq. (6) correspond to rc,min and rc,max,
respectively.
In Fig. 8, the prediction of the active cavity size range, employing Eq. (6), is shown. This prediction utilized cavities with microsize dimensions, instead of nano-sized dimensions. These results
suggest, according to Hsus analysis, that bubble nucleation may
not occur in a nano-pore of 30 nm within the present experimental
parameters.
During the anodizing NPS fabrication, the dent-like morphology
appeared on the top of the surface of the test section, as shown in
Fig. 3b. This could be caused by the pitting corrosion under the
acidic conditions used: Acids, such as sulfuric acids, can cause such
morphological changes. It is known that aluminum alloy is vulnerable to pitting corrosion, which is due to a lack of oxygen around a
small area. These oxygen-deprived areas become anodes, while
areas with excess of oxygen become cathodes, leading to localized,
galvanic corrosion. The corrosion penetrates the mass of metal and
leads to the creation of small holes (pitting) on the surface.
Although the passive layer is formed on the surface during the
anodizing fabrication, the metal is still porous and can be susceptible to corrosion in harsh environments (e.g., pH less than 4 or
pH greater than 9). Since most commercial alloys contain several
types of inter-metallic phases, the corrosion on aluminum alloys
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
155
Fig. 9. Boiling curves of (a) plain surface and (b) NPS with repeated tests.
Fig. 10. Heat transfer coefcients of (a) plain surface and (b) NPS with repeated tests.
Fig. 11. FESEM image of plain surface: (a) after Test 1 and (b) after Test 5.
All these reactions are thermodynamically favorable and are exothermic. They also reported that aluminum hydroxide could appear on the surface because of the reaction between the
aluminum oxide and water. Vedder and Vermilyea [22] identied
the three essential steps of growth mechanism of aluminum
hydroxide caused by the chemical reaction between the aluminum
and water: (i) The amorphous oxide formation, (ii) the dissolution
of the amorphous oxide, and (iii) precipitation of the aluminum
hydroxide. Alwitt [23] rened this model and concluded that steps
(i) and (ii) were probably limited by the diffusion of H2O (potentially acting as OH and H+) into the oxide surface. The outer layer
of the aluminum oxide developed under these conditions is typi-
156
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
Fig. 12. FESEM image of NPS: (a) after Test 1 and (b) after Test 5.
dered nano-pore structure (in Fig. 3a) to a blunt, ower-like structure (in Fig. 12a). As the number of repeated tests was increased,
the structures became more densely populated; the pores between
the nano-structures were lled and smoothed. (in Fig. 12b).
Based on previous research on the chemical reactions of aluminum and aluminum oxide with water and the surface images
(Figs. 11 and 12), the change of the boiling heat transfer performance on the plain surface and NPS is most likely caused by the
formation of the aluminum hydroxide on both surfaces. The possible reasons are the following: (i) An increase in the thermal resistance due to the aluminum hydroxide and (ii) the transformation
of the boiling surface morphology caused by the phase changes
of aluminum and aluminum oxide.
In order to estimate the thickness of the aluminum hydroxide
formed on the surface, at specimens of the NPS were prepared.
The specimens were then boiled in saturated water for 8 h and
observed using FESEM. The specimens were then boiled for an
additional 42 h and observed again using FESEM. In Fig. 13, the
cross-sectional FESEM images of the NPS at the different conditions, before boiling, after boiling for 8 h and 50 h, are shown.
The before-boiling NPS had a number of vertical columnar
nano-structures, shown in Fig. 13a, and the thickness of the aluminum oxide layer (i.e., nano-porous layer) was approximately
1.5 lm. After the two sets of pool boiling sessions, the aluminum
hydroxide (phase change of aluminum oxide) propagated to
approximately 0.5 lm (in Fig. 13b) and 1.5 lm (in Fig. 13c),
respectively. The growth rate of the aluminum hydroxide on the
NPS was approximately 30 nm per hour. The growth height of
the aluminum hydroxide after 50 h of boiling in a plain surface
was similar to that on the NPS. Based on these observations,
the thermal resistance caused by the formation of the aluminum
hydroxide appears to have little inuence on the nucleate boiling
heat transfer coefcient, since the thickness of the aluminum
hydroxide lm produced would be negligible. Therefore, the
change of the nucleate boiling heat transfer performance in
the plain surface and NPS is attributed to the transformation of
the boiling surface morphology caused by the phase changes of
the aluminum and aluminum oxide. This transformation contributes to the decrease of the active nucleation site density by ooding the cavities.
Fig. 14a and b shows the visualization-results of the pool boiling
using a NPS for Test 1 and Test 5 at q00 = 36.2 kW/m2. It can be
clearly seen that the pool boiling during Test 1 was more vigorous
than Test 5. This nding implies that the NPS of Test 5 had less active nucleation sites at the same heat ux condition. The visualization result of the plain surface was not shown, but was similar to
that of the NPS.
In summary, the aluminum hydroxide, which can be formed on
both surfaces at the water boiling condition, made the active
Fig. 13. Cross-sectional FESEM image of NPS: (a) before boiling, (b) after 8 h boiling
and (c) after 50 h boiling.
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
157
Fig. 14. Visualization of pool boiling with NPS for (a) Test 1 and (b) Test 5 at q00 = 36.2 kW/m2.
crease in the wall superheat at the ONB. At the early stage of the
pool boiling experiment for both surfaces (below q00 = 60 kW/m2
for Test 1), the aluminum hydroxide may be formed on the test
sections. Therefore, the slope of the boiling curve for Test 1 in both
surfaces appeared lower than those for the other tests in the nucleate boiling regime (Fig. 9), and the degradation of the heat transfer
coefcient between Test 1 and Test 2 was greater (Fig. 10). Based
on observations, in the rst boiling test results in Fig. 5, the inuence of transformation occurred in a part of heated surface during
degassing process before main boiling test may be included. However, the difference of boiling performance between plain surface
and NPS is attributed to the effect of nano-structure, because in
this work, all experiments were carried out at the same conditions
of degassing time and time interval between tests for plain surface
and NPS.
It is important to note that the morphologies of the aluminum
hydroxide formed on the surfaces during the pool boiling were
the ower-like nano-structures as shown in Figs. 11a and 12a.
The boiling curves of both surfaces consistently shifted to the right
(at the higher wall superheat condition) with the increase of the
number of repeated tests. This nding could imply that solely utilizing the nano-porous structure is insufcient to improve the
nucleate pool boiling heat transfer, and some passages, such as micro-cavities, that are formed inside the porous structure are instrumental in aiding in the escape of vapor [20]. Also, the nucleate pool
boiling heat transfer could potentially be inuenced by the surface
material (e.g., surface wettability), inside structure of the nanoporous layer, the cavities conguration, shape, and size. The
open-connected transformed structure in Figs. 11a and 12a may
not play a role as the active nucleate sites, because they may be
easy to be ooded due to a combination effect of the hydrophilic
surface of aluminum hydroxide and the open-connected structure.
The relationship between nano-structure and nucleate boiling heat
transfer is still not unclear. Therefore, further studies are required
to investigate the effect of the nano-structure on the nucleate boiling heat transfer.
4. Conclusion
In the present experimental study, the change of surface
morphologydue to chemical reactions occurring on the heated
aluminum alloy/aluminum oxide surfaces in a saturated water
pool boiling conditionwas investigated to determine its inuence
on the nucleate boiling heat transfer. Of particular interest are
aluminum alloy (6061) plain surface and the aluminum oxide
NPS surface that was chemically fabricated. The NPS showed a
lower wall superheat at the ONB as well as a higher nucleate
boiling heat transfer coefcient than the plain surface. Through a
Acknowledgments
This material is based upon work supported by the National
Science Foundation under Grant No. (#0923869) via a STTR Phase
II program of Advanced Materials and Devices Inc. (AMAD), Reno,
NV. Special thank goes to Dr. Y. Liu of AMAD.
References
[1] N.H. Kim, K.K. Choi, Nucleate pool boiling on structured enhanced tubes having
pores with connecting gaps, Int. J. Heat Mass Transfer 44 (1) (2001) 1728.
[2] B.J. Jones, J.P. McHale, S.V. Garimella, The inuence of surface roughness on
nucleate pool boiling heat transfer, J. Heat Transfer 131 (2009) 121009-1121009-14.
[3] A.K. Das, P.K. Das, P. Saha, Nucleate boiling of water from plain and structured
surfaces, Exp. Therm. Fluid Sci. 31 (8) (2007) 967977.
[4] W. Nakayama, T. Daikoku, H. Kuwahara, T. Nakajima, Dynamic model of
enhanced boiling heat transfer on porous surfacespart I: experimental
investigation, J. Heat Transfer 102 (3) (1980) 445450.
[5] A. Sloan, S. Penley, R.A. Wirtz, Sub-atmospheric pressure pool boiling of water
on a screen-laminate enhanced surface, in: Proceedings Semi-Therm 2009,
IEEE CFP09SEM-PRT, 2009. pp. 246253.
[6] M.G. Kang, Effect of surface roughness on pool boiling heat transfer, Int. J. Heat
Mass Transfer 43 (22) (2000) 40734085.
[7] A.E. Bergles, Some perspectives on enhanced heat transfer-second generation
heat transfer technology, J. Heat Transfer 110 (4b) (1988) 10821096.
[8] G. Guglielmini, M. Misale, C. Schenone, Boiling of saturated FC-72 on square
pin n arrays, Int. J. Therm. Sci. 41 (7) (2002) 599608.
[9] S. Vemuri, K.J. Kim, Pool boiling of saturated FC-72 on nano-porous surface, Int.
Commun. Heat Mass Transfer 32 (12) (2005) 2731.
[10] S. Launay, A. Fedorov, Y. Joshi, A. Cao, P. Ajayan, Hybrid micro-nano structured
thermal interface for pool boiling heat transfer enhancement, Microelectron. J.
37 (11) (2006) 11581164.
[11] H.S. Ahn, N. Sinha, M. Zhang, D. Banerjee, S. Fang, R.H. Baughman, Pool boiling
experiments on multiwalled carbon nanotube (mwcnt) forests, J. Heat Transfer
128 (12) (2006) 13351342.
[12] I.H. Chaudhri, I.R. McDougall, Ageing studies in nucleate pool boiling of
isopropyl acetate and perchloroethylene, Int. J. Heat Mass Transfer 12 (6)
(1969) 681688.
158
C.Y. Lee et al. / Experimental Thermal and Fluid Science 40 (2012) 150158
[13] C.Y. Lee, M.M.H. Bhuiya, K.J. Kim, Pool boiling heat transfer with nano-porous
surface, Int. J. Heat Mass Transfer 53 (1920) (2010) 42744279.
[14] S.J. Kline, The purposes of uncertainty analysis, J. Fluids Eng. 107 (1985) 153
160.
[15] Y.Y. Hsu, On the size range of active nucleation cavities on a heating surface, J.
Heat Transfer 84 (1962) 207216.
[16] V.P. Carey, LiquidVapor Phase-Change Phenomena, Hemisphere Publishing
Corporation, New York, NY, 1992.
[17] M. Pourbaix, Atlas of Electrochemical Equilibria in Aqueous Solutions, NACE
Cebelcor, Huston, 1974.
[18] K. Nisancioglu, Corrosion of aluminium alloys. in: Proceedings of 3rd
International Conference on Aluminum Alloys, vol. 3, 1992. pp. 239259.
[19] G.M. Scamans, J.A. Hunter, N.J.H. Holroyd, Corrosion of aluminum a new approach,
in: Proceedings of 8th International Light Metals Congress, 1987. pp. 699705.
[20] S. Li, R. Furberg, M.S. Toprak, B. Palm, M. Muhammed, Nature-inspired boiling
enhancement by novel nanostructured macroporous surfaces, Adv. Funct.
Mater. 18 (15) (2008) 22152220.
[21] J. Petrovic, G. Thomas, Reaction of aluminum with water to produce hydrogen:
a study of issues related to the use of aluminum for on-board vehicular
hydrogen storage, DOE (US Department of Energy), 2008.
[22] W. Vedder, D.A. Vermilyea, Aluminum + water reaction, Trans. Farady Soc. 65
(1969) 561584.
[23] R.S. Alwitt, Growth of hydrous oxide lms on aluminum, J. Electrochem. Soc.
121 (1974) 13221328.