Scripta Materialia 53 (2005) 341345 www.actamat-journals.

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Ultrane-grained AlAl2Cu composite produced in situ by friction stir processing

C.J. Hsu, P.W. Kao *, N.J. Ho
Institute of Materials Science and Engineering, National Sun Yat-Sen University Kaohsiung, 70 Lian-Hai Road, 804 Kaohsiung, Taiwan Received 30 December 2004; received in revised form 30 March 2005; accepted 8 April 2005 Available online 29 April 2005

Abstract Ultrane-grained AlAl2Cu composite can be fabricated in situ by friction stir processing. The Al2Cu particles are distributed quite homogeneously in the composite. The composite possesses enhanced Youngs modulus, good compressive strength and reasonably good compressive ductility. 2005 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved.
Keywords: Ultrane-grained microstructure; Metal matrix composites; Friction stir welding

1. Introduction Discontinuously reinforced metal matrix composites (MMCs) have attracted considerable attention, partly due to (a) availability of various types of reinforcement at competitive costs, (b) the successful development of manufacturing processes for producing MMCs with reproducible properties, and (c) the availability of metal working methods, which can be utilized to fabricate these MMCs [1]. These MMCs are fabricated either by directly adding reinforcements into the matrix or by synthesizing the reinforcements in situ in the metal matrix [13]. The advantages of in situ MMCs are that they are more homogeneous in their microstructures and thermodynamically more stable [4]. Moreover, they also have strong interfacial bonding between the reinforcements and the matrices [1,5]. In situ aluminum matrix composites may be fabricated by various techniques such as mechanical alloying [6], conventional ingot metallurgy [7], self-propagating high-temperature synthesis
Corresponding author. Tel.: +886 752 52000x4053; fax: +886 752 54099. E-mail address: pwkao@mail.nsysu.edu.tw (P.W. Kao).
*

[8], exothermic dispersion process [9], rapid solidication processing [10], and reactive squeeze casting [11]. In this paper, we will present the microstructure and mechanical properties of an AlAl2Cu composite with ultrane-grained (UFG) structure formed in situ via the friction stir process (FSP). Friction stir welding (FSW) is a new technique for joining aluminum alloys invented in 1991 at The Welding Institute [12]. Compared with traditional fusion welding processes, FSW oers improved mechanical properties, diminished weld defect formation, and reduced distortion [1318]. Based on the principles of FSW, Mishra et al. [19] developed friction stir processing (FSP) for microstructural modication of materials. In FSP, a cylindrical rotating tool with a concentric pin and shoulder is plunged into the material to be processed. Localized heating is produced by friction between the rotating tool and the workpiece to raise the local temperature of the material to the hot working range where it can be plastically deformed easily. When the working temperature is reached, the tool is traversed along the line of interest. Metal ows to the back of the pin tool, where it is extruded/forged behind the tool, consolidated, and cooled under hydrostatic pressure conditions [20,21].

1359-6462/$ - see front matter 2005 Acta Materialia Inc. Published by Elsevier Ltd. All rights reserved. doi:10.1016/j.scriptamat.2005.04.006

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FSP has been shown to be an eective technique in many applications: (a) to form ultrane-grained structure in Al-alloys [16,2224] and Mg-alloy [25], (b) to produce a ne-grained microstructure, which exhibits superplasticity [19,2628], (c) to homogenize the microstructure of nanocomposite aluminum alloys [29], (d) to rene the microstructure of cast aluminum alloy [30,31], and (e) to fabricate a surface composite of AlSiC on an aluminum substrate [32]. The basic concept of applying FSP to the formation of in situ AlAl2Cu composite is based upon the hot working nature of FSP. In short, it can provide (a) severe deformation to promote mixing and rening of constituent phases in the composite, (b) elevated temperature to facilitate the formation of an intermetallic phase, and (c) hot consolidation to form a fully dense solid.

Fig. 1. Schematic illustration of the friction stir process.

2. Experimental The starting materials used are pure aluminum powder (99.7% purity, 325 mesh) and pure copper powder (99.5% purity, 320 mesh). The copper content of the alloy is 15 at.% (denoted as Al15Cu). The premixed Al15Cu alloy powders were cold compacted to a small billet (12 12 88 mm) in a steel die, set by using a pressure of 225 MPa. To improve the billet strength for easier handling in FSP, the green compact was sintered for 20 min in air at either 773 K or 803 K. The tool pin used is standard M1.2*6 (metrication, with pitch height and diameter of 1.2 mm and 6 mm, respectively). The tool spindle angle (angle between spindle and workpiece normal) is 3.0. A counterclockwise tool rotation speed of 700 rpm was used, and the rotating tool was traversed at a speed of 45 mm/min along the long axis of the billet. In order to obtain a fully dense solid from a powder compact, two FSP passes were applied to the billet. A schematic illustration of the FSP setup is shown in Fig. 1. X-ray diraction (XRD, CuKa, 40 kV, 30 mA) was utilized to identify the phases present in the specimens. Scanning electron microscopy (SEM, JSM-6400, and JSM-6330) was used to study the distribution of second phase particles. Thin foils for transmission electron microscopy were prepared either by twin-jet electropolishing or by ion-milling. Twin-jet electropolishing was carried out in a mixture of 25% nitric acid and 75% methanol at 233 K with an applied voltage of 20 V. Thin foils were studied by the use of an analytical electron microscope (AEM, JEOL 3010) operated at 200 kV. The Vickers microhardness was measured with 300 g load for 15 s. Mechanical properties of specimens machined from the stirred zone (SZ) were evaluated on an Instron 5582 universal testing machine with an initial strain rate of 1 103 s1. The stress direction was

aligned along the traverse direction of the FSP. Rectangular specimens with dimensions of 4 4 6 mm3 were used for compression tests. The dimensions of the gauge section of tensile specimens were 3 mm in diameter and 14 mm in gauge length.

3. Results and discussion The tangent of the tool rotation along AS is in the same direction as the traverse direction (TD), while it is opposite to TD along the retreating side. The typical onion ring type microstructure can be observed in the cross section of SZ. The distributions of Vickers microhardness across the SZ along two directions (X-, and Z-directions) are shown in Fig. 2. It reveals that the FSP resulted in signicant increase in hardness from $80 Hv in BM (the as-sintered condition) to 160 14 Hv in the SZ. In addition, the hardness distribution within the SZ is not symmetric with respect to the tool rotation axis.

Fig. 2. Vickers microhardness proles across the cross section of the FS processed specimen along two perpendicular directions (BM: base metal; SZ: stirred zone; AS: advancing side; RS: retreating side).

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Before FSP, the green compact was sintered to provide enough strength to prevent fracture as the rotating tool plunging into it. Two dierent sintering temperatures (773 K and 803 K) were investigated. Both sintering temperatures could fulll the purpose. The X-ray diraction patterns are shown in Fig. 3. After sintering at 773 K, the Cu peaks still exist, while they disappear and are replaced by Al2Cu peaks after sintering at 803 K. Irrespective of the sintering temperature, Cu had reacted completely with Al and formed Al2Cu during FSP. There were copper oxides (CuO and Cu2O) present in the as-sintered specimens, which resulted from oxidation during sintering in air. The oxides disappeared after FSP, which might be a result of the reaction between Al and copper oxides to form Al2O3 and Al2Cu [33]. The microstructure of the as-sintered material is revealed by the backscattered electron image (BEI) in Fig. 4(a). In this micrograph, the dark areas consist of almost pure Al, whereas the brighter areas contain Cu or Al2Cu. Some eutectic structures were also observed. Fig. 4(b) is a typical micrograph of FS processed specimens. It indicates that Cu-rich particles are homogenously distributed in the aluminum matrix after FSP. Fig. 4(c) is a micrograph at higher magnication, which shows that the particles have irregular shape. The cross section of SZ in specimens produced by FSP was also examined by the use of TEM. Typical microstructures are shown in Fig. 5. As shown in Fig. 5(a), the grain sizes of both phases were rened to below 12 lm. Some of the dispersed particles were found to be smaller than 100 nm. Based upon the selected area electron diraction (SAD) patterns, ne grains of Al2Cu were identied as shown in Fig. 5(b). The Al2Cu grains were also conrmed by EDX analysis, which showed that the Cu-rich grains contained 32 6 at.% Cu. In
Fig. 4. (a) Backscattered electron image (BEI) of specimen sintered at 803 K, (b) BEI of specimen sintered at 803 K followed by FSP, and (c) SEM image to reveal the morphology of Cu-rich particles in specimen sintered at 803 K followed by FSP.

Fig. 3. X-ray diraction patterns for as-sintered specimens and specimens after two FSP passes.

addition, the Al2Cu grains were often found to be connected as shown in Fig. 5(b). The interconnected Al2Cu grains shown by TEM are consistent with irregular particle shape revealed by SEM, Fig. 4(c). By assuming that all the Cu has reacted to form Al2Cu, the calculated volume fraction of Al2Cu particles is about 0.42. From image analyses of the SEM images, the volume fraction of Al2Cu particles was determined to be 0.42 0.03, which is close to the calculated value. Based upon the content of Al2Cu, the theoretical density was calculated to be 3.4 g/cm3. The measured density of the composite was also 3.4 g/cm3. It may suggest that the FS processed sample is fully dense. In addition, the microscopic observations also showed that the SZ is pore free.

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Fig. 6. Compressive stressstrain curves for FS processed specimens machined from SZ.

Fig. 5. The microstructure of FS processed specimens revealed by TEM. (a) The grain sizes of both phases were rened to below 12 lm after FSP. (b) Bright eld image and SAD pattern in [0 1 1] zone axis of the Al2Cu grain which is marked by an arrow. All the Al2Cu grains in this micrograph are marked by asterisks.

The microstructure observations indicated that Cu nearly completely reacted with Al to form ne Al2Cu particles in a short FSP time. In the literature, the range of peak temperatures for friction stir welding (FSW) of aluminum alloys with similar tool rotation speeds and traversing speeds was reported to be 673723 K [14]. Because the sintered AlCu powder compact may have a lower thermal conductivity than that of a solid aluminum alloy and there may be considerable heat release due to the formation of Al2Cu particles, the peak temperature during the FSP in the AlCu powder compact may be well above 663 K. In addition to high temperature, the material ow patterns in FSW were observed to be complex spirals and vortex-like [21,14]. Therefore, it is suggested that FSP can provide: (a) severe deformation, which not only promotes mixing and rening of constituent phases in the sample, but also increases the diusion rate of elements, thereby accelerating the reaction between Al and Cu, (b) elevated temperature to accelerate the reaction of Al and Cu to form Al2Cu particles, and (c) hot consolidation to form fully dense

solid. FSP has been shown in the literature to be an eective technique to fabricate metal matrix composites or two-phase alloys with ne and homogeneous microstructure [2932]. This work further demonstrates that FSP could be a potential solid-state method to produce in situ metal matrix composites with ne microstructure and free of porosity. The compressive stressstrain curves of FS processed specimens are shown in Fig. 6, which shows quite consistent results for two tested specimens. Fig. 6 shows that the AlAl2Cu composite has an average 0.2% yield stress of 440 MPa, an average ultimate strength about 660 MPa, and a failure strain greater than 0.15. From tensile tests of three FS processed specimens, the average Youngs modulus was determined to be 88 8 GPa. Recently, FSP has been shown to be a feasible technique to produce large-area thin sheet of ultranegrained 7075 aluminum alloy by running multiple overlapping passes [24]. Due to the severe deformation and short time at elevated temperature in FSP as well as the presence of a considerable amount of second phase, grain growth could be limited eectively in the composite studied here. Therefore, it is possible to further rene and homogenize the structure and to produce large volume of materials by applying multiple passes of FSP.

4. Summary This work has demonstrated that Al2Cu intermetallic reinforced aluminum matrix composites with ultranegrained structure can be fabricated in situ by FSP. The AlAl2Cu composites thus formed are fully dense, and the Al2Cu particles are distributed quite homogeneously. The composite possesses enhanced Youngs modulus (88 8 GPa), good compressive strength

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(450 MPa yield strength and 650 MPa ultimate strength) with reasonable good compressive ductility (0.15 failure strain). Based upon this study, FSP may be a potential technique for fabricating metal matrix composite in situ; it is also possible to fabricate a large volume of materials with multi-pass FSP.

Acknowledgment This research was supported by National Science Council of ROC (NSC93-2216-E-110-020).

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