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Received 28 June 2006; received in revised form 12 March 2007; accepted 5 April 2007
Abstract
In order to investigate the effects of ultrasonic vibration on degassing of aluminum alloys, three experimental systems have been designed and
built: one for ultrasonic degassing in open air, one for ultrasonic degassing under reduced pressure, and one for ultrasonic degassing with a purging
gas. Experiments were first carried out in air to test degassing using ultrasonic vibration alone. The limitations with ultrasonic degassing were
outlined. Further experiments were then performed under reduced pressures and in combination with purging argon gas. Experimental results
suggest that ultrasonic vibration alone is efficient for degassing a small volume of melt. Ultrasonic vibration can be used for assisting vacuum
degassing, making vacuum degassing much faster than that without using ultrasonic vibration. Ultrasonically assisted argon degassing is the fastest
method for degassing among the three methods tested in this research. More importantly, dross formation during ultrasonically assisted argon
degassing is much less than that during argon degassing. The mechanisms of ultrasonic degassing are discussed.
© 2007 Elsevier B.V. All rights reserved.
0921-5093/$ – see front matter © 2007 Elsevier B.V. All rights reserved.
doi:10.1016/j.msea.2007.04.040
H. Xu et al. / Materials Science and Engineering A 473 (2008) 96–104 97
Three experimental systems have been designed and built: An experimental apparatus was designed and fabricated in
one for ultrasonic degassing in air, one for ultrasonic degassing order to investigate the possibility of combining ultrasonic vibra-
under reduced pressure, and one for ultrasonic degassing with tion with argon degassing. Apart from the usual components
a purging gas. These systems were successfully used to test used for the ultrasonic system in air, an acoustic probe with gas
ultrasonic degassing under various conditions. The aluminum purging capability was fabricated. Tests were carried out in an
alloy used was A356 alloy and its composition is listed in A356 melt. The furnace used to melt the A356 alloy holds up to
Table 1. 6 kg of melt. A flowmeter was used to control and monitor the
flow rate of argon. Ultrasonic vibration was injected from the
top of the melt. Argon was introduced into the melt through the
2.1. Ultrasonic degassing in open air
center of the ultrasonic probe.
The experimental system for ultrasonic degassing under 2.4. Experimental methods
normal atmospheric pressure consisted of a 20 kHz ultrasonic
generator, an air-cooled converter made of piezoelectric lead Ultrasonic degassing was first carried out in aluminum A356
zirconate titanate (PZT) crystals, a booster, a probe, an acoustic melt in air. The alloy was melted and then held at predetermined
radiator to transmit ultrasonic vibration into aluminum melt, temperatures for a half of an hour before degassing. Parameters
and a furnace in which the aluminum melt was held. The that affect ultrasonic degassing were then studied. These param-
transducer was capable of converting up to 1.5 kW of electric eters included the humidity of air, the temperature of the melt,
energy at a resonant frequency of 20 kHz. The amplitude of the and the volume/size of the melt.
ultrasonic vibration could be continuously adjusted from 30% Vacuum degassing was then carried out in the ultrasonic
to 100% of 81 m, which is the maximum amplitude of the system under reduced pressure. The chamber was evacuated
unit. after the molten aluminum was held at the targeted temperature
During experiments, ultrasound was injected into the alu- for 30 min. The process parameters studied under vacuum
minum melt by using a cylindrical radiator made of titanium degassing were the remnant pressure and degassing time.
alloy Ti–6Al–4V. The aluminum alloy was held in a graphite cru- Having determined the vacuum degassing characteristics,
cible and melted in the electric furnace. The temperature of the ultrasonic degassing under the reduced pressure was carried
melt was controlled within an accuracy of ±10 ◦ C. After the melt out to compare the degassing rates.
was heated to a predetermined temperature, a preheated ultra- Ultrasonic degassing combined with argon degassing was
sonic radiator was inserted in molten metal. Ultrasonic vibration also carried out in air. Argon was blown through the center of an
was then applied in the molten metal for certain amount of time ultrasonic radiator. For comparison, the argon degassing without
before samples were solidified and prepared for either density ultrasonic vibration was first carried out in the melt with a fixed
or hydrogen concentration measurements. argon flow rate.
The molten metal that had been processed using these
2.2. Ultrasonic degassing under reduced pressure degassing systems was then analyzed. Reduced pressure test
(RTP) was used to determine the porosity level of the melt. The
A steel vacuum chamber was built for vacuum degassing porosity level thus measured was then correlated to the hydrogen
with the assistance of ultrasonic vibrations. The crucible inside concentration using a calculated curve obtained using LecoTM
the electric furnace could hold molten aluminum alloys weigh- hydrogen analysis. Details of these two methods are discussed
ing up to 800 g. The minimum remnant pressure of this in the following sections.
vacuum chamber was 50 mTorr. The evacuation time was a
few seconds for the vacuum chamber to reach 100 Torr and 2.4.1. Density measurement
10 Torr, around 1 min to reach 1 Torr, and 20–30 min to reach The reduced pressure test (RPT) was used to determine the
0.1 Torr. porosity levels of the melts. Molten alloy (∼120 g) was poured
into a preheated thin-walled iron cup and allowed to solidify
under a reduced pressure of 50 mm Hg. Pressures of 50–100 mm
Table 1 Hg are usually used for RPT [17,18]. The RPT specimens were
Chemical composition of A356 alloy
sectioned vertically in the middle and were polished to reveal
Element wt.% the extent of the hydrogen porosity. The densities of the RPT
Al 92.5 specimens were measured using the apparent density measure-
Cu 0.1 ment method [4]. Specimens were weighed in air and water. The
Fe 0.1 density, D, of the specimen is given by the following equation:
Mg 0.35
Wa
Mn 0.05 D= (3)
Si 7.2 Wa − W w
Ti 0.1
Zn 0.05
where Wa and Ww are the weights of the specimen measured in
air and water, respectively.
98 H. Xu et al. / Materials Science and Engineering A 473 (2008) 96–104
ume/size of the melt. The humidity was varied from 40% to 60%.
Four melt temperatures, 620 ◦ C, 660 ◦ C, 700 ◦ C and 740 ◦ C
were tested. The weight of the melt was 0.2 kg, 0.6 kg and 2 kg,
respectively.
creates a large number of small cavities in the liquid. In the rar- high viscosity hampers the pulsation of the cavitation bubbles,
efaction phase, the surface area of a pulsating bubble is many their coagulation and floating. In the mean time, the diffusion
times greater than its area in the compression phase. Therefore, coefficient of hydrogen in liquid metals decreases with decreas-
the gas diffusion flow toward the bubble during rarefaction phase ing temperature thus decreasing the rate of one-way diffusion
exceeds the gas diffusion flow from the bubble during the com- rate of hydrogen from solution to bubbles. These two effects
pression phase. Because of the one-way gas diffusion toward the contribute to the decreased efficiency of ultrasonic degassing at
cavity, the pulsating cavity enlarges, resulting in degassing in the low temperatures.
melt. Since the cavitation bubbles are quite small and their num- The data plotted in Fig. 3 also indicates that the plateau hydro-
ber is large, the early stage of ultrasonic degassing is extremely gen content is not sensitive to the processing temperature within
fast. the range of 620 ◦ C and 740 ◦ C. It takes longer processing time
The kinetics of ultrasonic degassing suggests that as the gas is to reach the plateau hydrogen content when the processing tem-
being removed from the liquid, the rate of ultrasonic degassing perature is low but once the plateau hydrogen content is reached,
slows down. In the meantime, hydrogen is still being absorbed the porosity levels in the specimens are identical. The plateau
and dissolved into the melt at the melt surface according to hydrogen concentration is in the range of 0.1–0.2 ppm.
Eq. (4). When the hydrogen removal rate equals the hydro-
gen absorption rate, a steady-state hydrogen concentration is 3.1.3. Effect of melt volume on ultrasonic degassing
established in the melt. This steady-state hydrogen concentra- In order to obtain a quantitative evaluation of the degassing
tion should not be affected by the initial hydrogen concentration speed in molten aluminum, the weight (volume) of the melt was
in the melt. varied. The experiments were carried out in melt at 700 ◦ C under
a humidity of 60%. The weights of the melts were 0.2 kg, 0.6 kg
3.1.2. Effect of melt temperature on ultrasonic degassing and 2.0 kg, respectively. As illustrated in Fig. 4, the ultrasonic
Fig. 3 shows the efficiency of ultrasonic degassing in A356 processing time required for reaching the steady-state plateau
alloy melts under various melt temperatures. The results were hydrogen content increases with increasing weight (or volume)
obtained in a crucible containing 0.2 kg aluminum alloy. As illus- of the melt. Degassing times were as follows: 0.2-kg melt, 1 min;
trated in Fig. 3, it took about 1 min of ultrasonic vibration for the 0.6-kg melt, 4 min; 2.0-kg melt, almost 7 min. Degassing speed
melt to reach a steady-state hydrogen content plateau when the in a larger volume melt is much slower than that in a smaller
melt was ultrasonically processed at a temperature of 700 ◦ C or melt. However it is still encouraging that the steady-state plateau
740 ◦ C. The processing time required to degas the melt (the time hydrogen content is not sensitive to the volume of the melt. Fast
to reach the steady-state hydrogen content plateau) increased degassing of a large-volume melt can be obtained by use of
with decreasing melt temperature in the temperature range of multiple ultrasonic radiators to inject ultrasonic vibrations into
620 ◦ C to 700 ◦ C. It took almost 10 min to degas the melt held at the melt.
620 ◦ C, much longer than the melt held at temperatures higher
than 700 ◦ C. 3.2. Ultrasonic degassing under reduced pressures
There are various reasons why the degassing efficiency
decreases with decreasing temperature. The temperature of the Ultrasonic degassing under reduced pressure was also eval-
melt has a significant effect on the efficiency of ultrasonic uated. The vacuum degassing data was used as a baseline for
degassing. The lower the melt temperature, the higher the viscos- evaluating ultrasonic degassing under reduced pressures. Vac-
ity of the melt. When the melt temperature is below 700 ◦ C, the uum degassing was carried out in 0.6-kg aluminum samples. The
process parameters studied under vacuum degassing included
Fig. 3. The hydrogen content as a function of ultrasonic processing time in melt Fig. 4. The hydrogen content as a function of ultrasonic processing time in melt
degassed at different processing temperatures. of different sizes.
100 H. Xu et al. / Materials Science and Engineering A 473 (2008) 96–104
the remnant pressure and degassing time. The remnant pres- to a decrease of the bulk hydrogen concentration in the melt.
sure was varied from 760 Torr to 0.1 Torr and the degassing Since hydrogen evaporation occurs only at the melt/air inter-
time was varied from 1 min to 45 min. For the remnant pressure face, the hydrogen atoms in the melt have to diffuse to the melt
of 100–10 Torr, the experiments were conducted at temperature surface before evaporating into the atmosphere. Thus vacuum
of 720 ◦ C with a humidity of ∼60%. For remnant pressures of degassing is a diffusion-controlled, slow process. This explains
0.1 Torr and 1 Torr, the humidity was maintained at ∼50%. the 20–30 min needed to reach the steady-state plateau hydrogen
Vacuum degassing with the assistance of ultrasonic vibration content during vacuum degassing. Also, since the equilibrium
was performed under two different remnant pressures: 100 Torr hydrogen content is proportional to the partial pressure of hydro-
and 1 Torr, respectively. The experiments were carried out with gen in the atmosphere, the steady-state plateau hydrogen content
0.6-kg melts at 720 ◦ C with a humidity of 50%. should decrease with decreasing remnant pressure. These trends
are clearly shown in Fig. 5.
3.2.1. Vacuum degassing Assuming that the equilibrium hydrogen concentration in the
The hydrogen level in the melt can be decreased by creating melt was maintained for 45 min during vacuum degassing, the
a vacuum above the melt surface. Even a partial vacuum has equilibrium hydrogen concentration can be plotted in Fig. 6
been found to be effective in reducing the hydrogen level in the under the remnant pressure of 0.1 Torr, 1 Torr, 10 Torr, 100 Torr
melt. Fig. 5 shows the hydrogen content as a function of treat- and 760 Torr, respectively. As shown in Fig. 6, the hydrogen
ment time under different remnant pressures. As is indicated content of the specimen decreases with decreasing remnant
in Fig. 5, the hydrogen content of a specimen decreased with pressure.
increasing hold (vacuum degassing) time. The degassing rates at
lower remnant pressures (0.1 Torr and 1 Torr) were much higher 3.2.2. Ultrasonic degassing under reduced pressure
than that at higher remnant pressures (100 Torr and 10 Torr). It Having established the baseline of vacuum degassing, ultra-
was evident that the degassing rates were slow using unassisted sonic degassing of aluminum melt under reduced pressure was
vacuum degassing. For instance, 20–30 min were required for investigated. During the experiments of ultrasonic degassing
a 0.6-kg melt to reach the steady-state plateau hydrogen con- under reduced pressure, the ultrasonic vibration was induced into
tent with the vacuum degassing technique, while the ultrasonic the melt after the remnant pressure reached 100 Torr and 1 Torr,
vibration technique required <4 min to achieve the same result, respectively. It took several seconds for the remnant pressure to
as shown in Fig. 4. reach 100 Torr and around 1 min to reach 1 Torr.
The data points plotted in Fig. 5 indicate that the steady-state The hydrogen contents as a function of processing time
plateau hydrogen content is strongly affected by the remnant under various conditions are shown in Fig. 7(a) and (b). Data
pressure. The plateau hydrogen content at the steady-state is points marked by filled squares indicate the efficiency of ultra-
much lower at lower remnant pressures than that at higher rem- sonic degassing under two remnant pressure levels (100 Torr and
nant pressures. 1 Torr). As the figure indicates, the plateau hydrogen content
The results shown in Fig. 5 can be explained by consider- was attained much faster through the use of the combination of
ing the hydrogen/water vapor partial pressure in the degassing ultrasonic degassing and vacuum degassing than by use of either
chamber. The equilibrium hydrogen content in the melt is pro- ultrasonic degassing or vacuum degassing alone. For compari-
portional to the partial hydrogen pressure in the atmosphere son, Fig. 7 also displays data obtained using ultrasonic vibration
above the melt. When the pressure in the chamber is reduced, the under atmosphere pressure (marked on the figure with trian-
partial pressure of hydrogen is also reduced. As a result, hydro- gles) and data obtained using vacuum degassing (marked with
gen dissolved in the melt evaporates at the melt surface, leading filled circles). Clearly, the most efficient degassing method is
Table 2
Processing time for steady-state plateau hydrogen content using various
degassing methods
Degassing method Processing time required (min)
Ultrasonic 4
Vacuum 20
Ultrasonic under reduced pressure 1 Fig. 8. A comparison of hydrogen content as a function of processing time for
argon degassing and ultrasonically assisted argon degassing in a 5 kg melt.
102 H. Xu et al. / Materials Science and Engineering A 473 (2008) 96–104
Table 3
Amount (g) of dross formed at various degassing times using argon degassing and ultrasonically assisted argon degassing
Degassing method Degassing time (min)
2 5 10 15 20 25
a melt containing dissolved gases, the gaseous elements diffuse melt. As the purging gas bubbles travel from the radiator to the
into the cavitation bubbles through the bubble/melt interfaces bulk melt, they collect the cavitation bubbles which contains
during the nucleation and growth stage of the cavitation bubbles. dissolved gases. On the other hand, acoustic streaming helps to
Some of the dissolved gases escape when cavitation bubbles at distribute the small purging gas bubbles uniformly throughout
the molten surface collapse, thereby resulting in degassing. the melt, improving the degassing efficiency further. The exper-
Generally ultrasonic degassing can be divided into three imental results show that the new degassing method is more
stages: (1) nucleation of cavitation bubbles on nuclei (usually efficient than the traditional purging gas methods.
solid inclusions containing cavities) and growth of the bubbles
due to the diffusion of hydrogen atoms from the surrounding
melt to the bubbles, (2) coalescence of bubbles to form large 4. Conclusions
bubbles, and (3) float of large bubbles to the surface of the molten
metal and escape of the bubbles at the top melt surface. (1) Ultrasonic degassing is an efficient way of degassing a
The first stage of ultrasonic degassing, nucleation and growth small volume melt. The early stage of ultrasonic degassing
of cavitation bubbles, can be easily achieved using high inten- is extremely fast. It takes only a few minutes to degas a
sity ultrasonic vibration. The ultrasonic unit used in this project small volume melt and to reach a steady-state plateau hydro-
has a power density much higher than the critical power den- gen content. The humidity/initial hydrogen concentration
sity for creating cavitation. As a result, cavitation can be readily has little effect on the degassing efficiency using ultrasonic
achieved when the unit is operated at amplitudes higher than vibrations. The melt temperature has a significant effect on
30% of the maximum amplitude. Due to the high attenuation the efficiency of ultrasonic degassing. The degassing rate
of ultrasonic vibration in the liquid, cavitation mainly forms in the temperature range between 700 ◦ C and 740 ◦ C is
near the ultrasonic radiator and the cavitation bubbles are trans- faster than that in the temperature range between 620 ◦ C
ported through the bulk liquid by ultrasonic streaming. Since the and 660 ◦ C. These results clearly suggest that ultrasonic
cavitation bubbles are small (in the range of microns) and the vibration alone is efficient for degassing a small volume
interfacial area of the bubble/melt interfaces is large, degassing of melt. The applications would be degassing a shallow
is extremely fast if most of the cavitation bubbles escape from aluminum trough for transporting aluminum from a melt-
the melt. This is what happens when ultrasonic vibration is used ing furnace to a casting machine. Often multiple radiators
for degassing a small volume of melt. Due to flow produced have to be used for degassing a large volume of molten
by acoustic streaming, the cavitation bubbles formed near the aluminum.
ultrasonic radiator are quickly transported to the melt surface, (2) The combination of ultrasonic degassing and vacuum
bringing with them the dissolved gases, which then escape the degassing results in a much faster degassing than does
melt. Use of the reduced pressure of a vacuum facilitates the the use of ultrasonic degassing alone. Even under a par-
escape of the gasses at the melt surfaces. This accounts for tial vacuum condition such as 100 Torr, the efficiency of
the result that ultrasonic degassing and the ultrasonic degassing ultrasonic degassing could be increased by using ultrasonic
under a reduced pressure are two methods which enable fast degassing under a reduced pressure. Nevertheless, ultra-
degassing of small volume melts. sonic degassing under reduced pressure has the inherent
One critical issue of ultrasonic degassing is the survival of limitations of ultrasonic degassing. The method can only
the cavitation bubbles in the melt, affecting the degassing effi- be used for degassing a small-volume melt. Other methods
ciency. During the initial stages of the nucleation and growth of need to be explored for the degassing of a large volume of
the cavitation bubbles, the dissolved gases diffuse into the bub- molten aluminum.
ble and form gas molecules. As these bubbles travel away from (3) Ultrasonically assisted argon degassing is a more efficient
the ultrasonic radiator (the stress becomes more compressive), method than argon degassing alone. For a 5-kg aluminum
the gas molecules can decompose at the bubble/melt interfaces, melt, a steady-state hydrogen content plateau was reached
dissolving back into the melt. The gases in the cavitation bub- in only 5 min using ultrasonically assisted degassing, com-
bles will also dissolve into the melt when the cavitation bubbles pared to more than 10 min using argon degassing. More
collapse. In fact, most of the cavitation bubbles cannot survive importantly, dross formation during ultrasonically assisted
longer enough to reach the melt surface. Based on the ultrasonic argon degassing is much less than that during argon
degassing principles, a novel approach for ultrasonic degassing degassing.
has been developed. The new approach involves the use of a
small amount of purging gas (argon) for ultrasonic degassing. Acknowledgements
The idea is to use this small amount of purging gas to extend
the survival time of the cavitation bubbles which contain dis- This research was supported by the United States Depart-
solved gas as the bubbles nucleate and grow. In practice, the ment of Energy, Assistant Secretary for Energy Efficiency and
purging gas is introduced through the ultrasonic radiator. High Renewable Energy, Industrial Technologies Program, Indus-
intensity ultrasonic vibration is fed through the radiator to break trial Materials for the Future (IMF), Aluminum Industry of
up the purging gas bubbles as well as to create a large amount the Future, under contract No. DE-FC36-02ID14399 with UT-
of cavitation bubbles. The small purging gas bubbles can sur- Battelle, LLC. The authors would like to thank Ohio Valley
vive in the melt forever because argon will not dissolve into the Aluminum Co. and Secat Inc. for providing industrial support.
104 H. Xu et al. / Materials Science and Engineering A 473 (2008) 96–104
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