September 1998

Materials Letters 37 1998. 2734

Solidification of aluminium alloys under ultrasonic irradiation using water-cooled resonator

V. Abramov
a b

a,)

, O. Abramov b, V. Bulgakov b, F. Sommer

Max-Planck-Institut fur Werkstoffwissenschaft, Seestr. 75, D-70174 Stuttgart, Germany Institute of General and Inorganic Chemistry, Russian Academy of Sciences, Leninsky prospect 31, 117907 Moscow, Russian Federation Accepted 23 February 1998

Abstract The present investigation attempts to evaluate the effect of ultrasonic treatment using water-cooled resonator on the microstructure and properties of different commercial Al-based alloys. The effect of ultrasonic treatment on the as-cast alloy microstructure can be summarized as follows: reduction of mean grain size, variation of phase distribution and better material homogeneity and segregation control. Ultrasonically treated samples have elongation values much higher than those obtainable with control processes. Our investigations confirm great advantages of ultrasonically treated ingots of hypereutectic AlSi alloys upon deformation in semisolid state. q 1998 Elsevier Science B.V. All rights reserved.
Keywords: Aluminium alloy; Ultrasonic irradiation; Water-cooled resonator; Solidification

1. Introduction The final quality of a cast is broadly dependent upon many factors which will have an effect on the solidification of the metal. Any structural defect occurring in the cast products may be transferred to the final product. Thus, any process which would reduce defects and improve the metal structure of the cast product could clearly be of benefit to the foundry industry. The major problem associated with aluminium alloy casting is an inability to completely eliminate the various production defects in their structure, such as dendrite structure, gas cavities, segregation and rough intermetallic inclusions. The

Corresponding author.

improvement in the structure of aluminium alloys can be produced mainly by two routes which are: i. mechanical or magneto-hydrodynamic stirring, ii. intensive ultrasonic treatment during solidification w1,2x. Introduction of high-power ultrasonic vibration into a liquid alloy leads to cavitation and acoustic streaming. Cavitation involves the formation, growth, pulsating and collapsing of tiny bubbles in the melt. The compression rate of these unsteady states can be so high that their collapses generate hydraulic shock waves. Primary crystallites are broken up by hydraulic shock waves, thus producing artificial sources of nuclei. The propagation of high-intensity ultrasonic wave also involves the initiation of steady-state acoustic streamings in the melt. The total effect of various kinds of streams is to vigorously mix and so homogenize the melt.

00167-577Xr98r$19.00 q 1998 Elsevier Science B.V. All rights reserved. PII: S 0 1 6 7 - 5 7 7 X 9 8 . 0 0 0 6 4 - 0

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V. Abramo et al.r Materials Letters 37 (1998) 2734

In the present work, we studied the possibility of using a water-cooled resonator for ultrasonic treatment of different types of aluminium alloys. It should be noted that the water-cooled resonator placed in the melt acts as cooler and has also an effect on the solidification kinetics. Varying the water rate, resonator shape and immersion, and the ultrasound intensity, one can better control the temperature distribution in the melt and thus the microstructure of the material. In this case the most effective crystallization will take place not at the walls of the crucible, but in the neighbourhood of the cooling element. Thus, the region of intensive crystallization will be positioned in the cavitation region and the region of the most intensive mixing. Therefore, hydraulic shock waves generated by the collapse of cavitation bubbles effectively break particles of the already solidified alloys and acoustic streams generated by ultrasonic treatment will homogeneously distribute these fine solid particles. When ultrasonic vibrations are coupled to the solidifying metal, structural changes occur including grain refinement, suppression of columnar grain structure, increased homogeneity and reduced segregation.

Fig. 2. Ultrasonic oscillations a. in rod waveguide system and b. in MTS.

ator UG., magnetostrictive transducer EMT., the waveguide system WGS. for transmission the ultrasonic vibration from EMT to technological load TL. technological block TB. and control system CS..

2. Calculation and design of waveguide system for treatment of aluminium alloys The transmission of ultrasonic vibration to the solidifying melt is not an easy problem because a resonator can rapidly fail under the effect of temperature and cyclic stresses. For these purposes, special ultrasonic equipment and technologies were developed. Ultrasonic units as a rule include at least five blocks Fig. 1., namely, the electric ultrasonic gener-

Fig. 1. Schematic diagram of the ultrasonic unit. UG s the electric ultrasonic generator, MT s magnetostrictive transducer, WGSs the waveguide system, TL s technological load, CSs control system.

Fig. 3. Pattern of deformation during the ultrasonic vibration with frequency of 25 kHz for MTS with c. plane top and d. spherical top.

V. Abramo et al.r Materials Letters 37 (1998) 2734 Table 2 Chemical composition of wrought alloy wt.%. Zn 8.54 Mg 2.73 Cu 2.35 Zr 1.5 Al balance

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Fig. 4. Schematic diagram of experimental set-up: 1. water-cooled MTS, 2. magnetostrictive transducer, 3. ultrasonic generator.

To achieve a high level of technological efficiency of ultrasonic units, two conditions must be fulfilled w1,3x: 1. The system UGEMTWGS is operated at or in the vicinity of their electric and mechanical resonance the frequency of electric current of the UG s frequency of the natural resonance of the EMT s frequency of the natural resonance of the WGS.. 2. The matching of EMT and WSG must
Table 1 Chemical composition of the AlSi alloys wt.%. Alloy AlSi9 AlSi12 AlSi17 Si 9.5 12.9 17.1 Cu 0.9 3.1 4.5 Mn 0.17 0.3 0.55 Al balance balance balance

ensure an effective transmission of the vibrations through the contact area. In order to improve the matching effect using a larger radiating surface, it has been recently proposed w4x to convert the longitudinal vibrations of EMT into vibration emitted radially from IR. In this case not only the top of the resonator but all its surface will effectively irradiate ultrasonic energy. Therefore, for increasing the efficiency of the system, longitudinal vibrations shall be converted to radial ones. For transmission of radial vibration into a load, the geometric size of IR must be calculated in such way that the resonance of longitudinal and radial modes of vibrations have been correctly adjusted. This Mode Transformation System MTS. has been developed and recently filed as a patent w4x. MTS is a tubular waveguide system which transfers the longitudinal mode oscillations to those directed perpendicular to the surface Fig. 2. of the tube and irradiated to the liquid metal. Experimental search of dimensions of waveguide system is complicated and expensive. The use of analytical methods of calculation of MTS is very restricted because of complexity of the entire task. They can be used only for obtaining a first guess of searching parameters to solve the entire problem numerically. In order to simplify and speed up the procedure of determination of waveguide system parameters together with or instead of experimental work, computation of these parameters was carried out. The waveguide system model is always three-dimensional. In this case, the appropriate accuracy in the frequency analysis can be usually achieved if the large number of finite elements is used. Numerical
Table 3 Chemical composition of the antifriction aluminium alloy wt.%. Sn 7.1 Sb - 0.3 Cu 2.6 Si 1.2 Fe - 0.15 Al balance

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Fig. 5. AlSi17 alloy cooling curves: a. control, b. solidified with ultrasonic treatment.

treatment of this problem is complicated because only a restricted number of the lowest resonance frequencies and corresponding modes can be computed whichever numerical approach is employed w5x. The finite element package COSMOS together with graphical visualisation was used for the calculations. In order to design the most effective waveguide system, we examined two possibilities: a. the tube with plane top; b. the tube with spherical top. Distribution of radial amplitude at 25 kHz for both possibilities according to finite element calculation is shown in Fig. 3. Our calculations show that in comparison with the pipe with spherical top in case of plane top, a large contribution into vibration energy is made by the top itself and vibration of the top strongly dominates over the vibration of the pipe. And what is more, in case of the plane top, it is

possible that vibration is exhibited only by the top with small displacement of the pipe. with frequency close to 25 kHz. Therefore, for construction of our waveguide system, we used the tube with spherical top. The scheme of the ultrasonic system provided with a water-cooled resonator is shown in Fig. 4. The problem of construction and the choice of materials for the waveguide system, which could run during a long time in an aluminium melt, is also very important and actual. Dobatkin and Eskin w3x used ultrasound intensities in the range of 720 W cmy2 and found that carbon steel resonators were dissolved quickly in liquid aluminium whereas 18 wt.% Cr9 wt.% Ti steel resonators have a live time of only 12 min. Niobium alloys proved to be more resistant w6x. Laboratory tests were based on the use of special benches, where ultrasonic vibrations were

Fig. 6. Microstructure of AlSi9 alloys: a. control, b. solidified with ultrasonic treatment.

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fed to the solidifying mold-held melt by top transmission method. A 10 kW ultrasonic generator and magnetostictive transducer were used in those tests.

3. Experimental procedure The ultrasonic treatment was carried out in a cylindrical ceramic crucible of approximate dimensions 80 mm diameter and 160 mm height. The thermocouple was positioned to record temperature of the melt at a position between centre of the charge and crucible wall, i.e., 30 mm from the crucible wall. In our experiments we used hypoeutectical, eutectical and hypereutectical AlSi alloys, high-strength wrought AlZnMgCu alloy, antifriction AlSn alloy and technically pure aluminium. The chemical compositions of the alloys are shown in Tables 13. The antifriction behaviour of the AlSn based alloys was tested using dry friction testing without lubrication. These experiments are easier to perform than the experiments with lubrication. Antifriction testing was carried out using a friction machine type SNTs-2 with axle-insert arrangement, sliding velocity of 2 m sy1 and pressure of 1.4 MPa. The specimens used for testing the antifriction properties were manufactured in the form of a disk with a diameter of 45 mm, on which five grooves for antifriction properties were made. During the tests the roller slides on the surface of the groove. The roller with diameter of 35 mm was made from 0.45% carbon steel not heat-treated and having the hardness HB 196200. The loss in weight of the sample and

the roller during the test is a measure of the wear loss. To study the thixotropic behaviour, control and treated specimens were upset in electro-hydraulic press under semisolid conditions. The specimens measuring 20 mm = 20 mm = 10 mm were deformed at 5808C after heating and holding for 15 min. During the deformation, the height of the specimens was twice decreased to 5 mm. The variation of the deformation load during the upsetting was measured. Tensile tests were done with an Instrone machine, at a loading rate of 0.5 mm miny1 . Tensile specimens had working length-to-diameter ratio equal to 10.

4. Results and discussion It was revealed that the use of the water-cooled waveguide system for ultrasonic treatment increases twice the solidification rate in comparison with the control process. As an example, the cooling curves of AlSi7 alloys are shown in Fig. 5. The structure changes in solidifying metal are generally due to the processes in the melt and the two-phase liquidsolid zone, i.e., crystal nucleation, dispersion and mixing. These processes depend on cavitation and streaming as well as process factors and material properties. The shock waves appeared during the collapse of the cavitation bubbles near the surface of the watercooled waveguide system, causing some crystals at the solidification front to break down and move

Fig. 7. Microstructure of AlSi12 alloys: a. control, b. solidified with ultrasonic treatment.

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Table 4 Effect of cast structure on mechanical properties of specimens of AlSi alloys Alloy AlSi9 AlSi9 AlSi12 AlSi12 AlSi17 AlSi17 Casting technique Conventional casting Casting with UST Conventional casting Casting with UST Conventional casting Casting with UST UTS MPa. 200 220 190 230 160 180 El %. 2 3 0.5 2.0 0.5 1.8 HB 91 90 97 94 102 98

toward the liquid bulk. In addition to breaking down growing crystals, the ultrasound has also an effect on the nucleation rate. There are two mechanisms of cavitation effect on the nucleation rate. Cavitation activates insoluble particles e.g., oxides, ultrafine particles of some intermetallics. that exist in the melt, and turns them into solidification sites. Fragments of destroyed dendrites also act as solidification sites. Another mechanism is described by Kapustina w7x. During the expansion half-period, the bubble rapidly increases in size, and the liquid evaporates inside the bubble. The evaporation and expansion tend to reduce the bubble temperature. A decrease of bubble temperature below equilibrium temperature results in melt undercooling at the bubble surface, and hence in the probability that a nucleus will be formed on a bubble. As a result of all these effects, ultrasonic treatment of the melt reduced liquidus undercooling from 2.18C to 0.98C. This changes in the cooling curves shows that nucleation takes place more easily. Hypoeutectical, eutectical alloys prepared at conventional casting have dendritic structure and silicon

Fig. 9. Variation of deformation load upon upsetting of AlSi17 alloy specimens at 5808C: a. conventional casting, b. casting with ultrasonic treatment.

inclusions crystallise as hexagonal plates joined together at a centre into star-shaped pattern as they appear in cross-section. Figs. 6 and 7.. By contrast, ultrasonic irradiation refined the silicon crystals and distribute them uniformly over the section. Most of the silicon plates were dissembled and broken during the ultrasonic treatment and forming spheroidized crystals. The ultrasonically induced refinement of silicon inclusions and dendrite-to-subdendrite structure change improves the mechanical properties. Table 4 lists some mechanical characteristics as strength, ductility and hardness of the alloys in both conditions. Various microstructure of hypereutectic Al17 wt.% Si alloys are shown in Fig. 8. It is clear that prior to ultrasonic treatment, the primary Si crystals within the alloy have the faceted morphologies. However, ultrasonic treatment results in morphologi-

Fig. 8. Microstructure of AlSi17 alloys: a. control, b. solidified with ultrasonic treatment.

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Fig. 10. Microstructure of AlZnMgCu alloys: a. control, b. solidified with ultrasonic treatment.

cal changes of primary Si crystals from faceted to spherical. Fragmentation of large primary crystals followed by aggregation of the fragmented Si is considered to be responsible for spheroidization of primary Si crystals. As shown in Table 4 as-cast hypereutectic AlSi alloys demonstrated modest increase of strength and decrease of hardness. Typically, the ultrasonic treatment results also in an increase of the plasticity 3.5 times. The increase in ductility makes hot cracking during casting less probable. Changes in microstructure of AlSi17 alloy facilitated the deformation of such material in semisolid conditions. The variation of deformation load during the upsetting of specimens by 50% at temperature 5808C is shown in Fig. 9. The maximum stress of upsetting is 30% lower for ultrasonically treated alloys. Probably, in this case similar to the sliding of ultrafine grains during superplastic deformation in the solid state, one can observe the thixotropic sliding of nondendritic grains in

the semisolid conditions. Therefore, ultrasonic treatment is promising for the preparation of thixocastible hypereutectic AlSi alloys. For high-strength wrought AlZnMgCu alloys, microstructure analysis suggests that ultrasound firstly increases the nucleation rate of solidification sites and secondly, suppress segregation and homogenise chemical composition of as-cast material. Ultrasonic treatment during the casting results in dendrite-free grain structure Fig. 10.. This type of the structure can only arise if the grain size is smaller than or equal to the dendrite cell size produced at a given solidification velocity. Simultaneously, ultrasonic treatment leads to refinement of inclusions of the Mg 2 Zn and MgAlCu phases. Ascast high-strength wrought AlZnMgCu alloy shows an increase of strength from 220 MPa to 250 MPa after ultrasonic treatment. Typically, the ultrasonic treatment results also in an increase of the plasticity from 12 to 16%.

Fig. 11. Microstructure of pure aluminium: a. control, b. solidified with ultrasonic treatment.

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Pure metals have poorer ultrasonic tractability than alloys. According to Ref. w1x pure aluminium cannot be effectively treated using rod-type not water-cooled waveguide system. But also here the structure changes during the solidification in an ultrasonic field. Fig. 11 demonstrates that ultrasonic treatment of high-purity Al substantially refine the microstructure, which results in better mechanical properties. The tensile strength improves by 35% from 52 MPa to 72 MPa in ultrasonically treated material and the hardness increases by 14% from HB 17.2 to HB 19.7. The hardening is paralleled by an increase of the elongation from 48 to 52%.

Acknowledgements The authors wish to thank the VW Foundation Contract No. Ir70871. and the INCO-COPERNICUS Programme Contract No. IC15-CT96-0740. for financial support.

References
w1x O.V. Abramov, Ultrasound in Liquid and Solid Metals, CRC Press, Boca Raton, FL, 1994. w2x W. Kahl, Neuere Herstellungsverfahren und Verarbeitungstechnologien fur Aluminium Werkstoffe, Metall. 1994. 4. 295301. w3x V.I. Dobatkin, G.I. Eskin, Vozdeystvie Moschnogo Ultrazvuka na Mezhfaznuyu Poverkhnost Metallov The Effect of High-Intensity Ultrasound on the Phase Interface in Metals., Nauka, Moscow, 1986. w4x V.O. Abramov, O.V. Abramov, V.E. Bulgakov, O.M. Gradov, L.O. Makarov, Apparatus for the feeding of ultrasonic into a liquid medium, Submitted to the Patent Office in Munich, 1997. w5x D.H. Norrie, G. Vries, An Introduction to Finite Element Analysis, Academic Press, New York, 1988. w6x A. Sterritt, M. Bacon, F. Bell, T.J. Mason, Proceedings of the Ultrasonic World Congress, Part 2, Berlin, 1995, pp. 725729. w7 x O.A. Kapustina, Fizicheskie Osnovy Ultrazvukovoy Tekhnologii The Physical Principles of Ultrasonic Manufacturing., Nauka, Moscow, 1970 in Russian..

5. Conclusions Our experiments demonstrated that practically all the aluminium alloys of major commercial interest can be ultrasonically treated using water-cooled waveguide system. In conclusion, as regards the ductility characteristics, it must be outlined that ultrasonically treated samples have elongation values much higher than those obtainable with control processes. Our investigations confirm great advantages of ultrasonically treated ingots of hypereutectic AlSi alloys upon deformation in semisolid state.