Part IX – September 1969 – Papers - High-Speed Directional Solidification of Sn-Pb Eutectic Alloys

The lamellar-dendritic transition in Sn-Pb alloys near the eutectic composition has been studied at high growth rates. Lamellar structures were found over a substantial range of tin-rich compositions, and this range extended to increasingly tin-rich concentrations as growth rate increased. These results are discussed in terms of stability and competitive-growth arguments. Various experimental and structural limitations to the rate of directional solidification are discussed. The rate of heat removal at the heat sink is the major experimental limitation. ReCENT interet1,2 in the use of fine composite structures produced by directional solidification of eutectic alloys makes it important to determine the range of composition and growth conditions that yield such microstructures. Because increasing growth velocities produce increasingly finer microstructures, it is particularly significant to determine the factors limiting the rate of solidification. Mollard and Flemings3 have shown that composite structures, free of primary dendrites, can be obtained in Sn-Pb alloys of off-eutectic composition. The composition range of composite structures was found to increase with increasing values of G/V, where G is the temperature gradient and V is the growth velocity. These results are in good quantitative agreement with an analysis of the stability of a planar eutectic interface.4 This analysis specifically predicts that over a small range of compositions stable lamellar structures will be obtained even for G/V = 0, hence, even at very high growth rates. The lamellar-dendritic transition in Sn-Pb alloys has also been analyzed with a model based on competitive growth between dendrites and the composite structure.576 This treatment, based on earlier work on organic eutetics,7 predicts that the composition range yielding composite structures in Sn-Pb will increase rapidly at high growth rates. An increase in the composition range of composite structures at high growth rates was recently observed in Cu-Pb alloys near the monotectic composition.8 In view of these results, and the predictions of the stability and competitivegrowth analyses, it was decided to study the lamellar-dendritic transition in Sn-Pb alloys at high growth rates. EXPERIMENTAL Using 99.999 pct pure materials, a series of Sn-Pb alloys were prepared containing 16.8 at. pct to 27.6 at. pct lead. (Eutectic composition is 26.1 at. pct Pb.) Ingots were extruded to 0.175 in. rod, and some rod was drawn to 0.070-in. wire. Directional solidification was accomplished in two different ways, Fig. 1. For growth rates up to 2 x 10-1 cm per sec, a 0.175 in. diam sample was placed in a graphite crucible 5 in. long with 0.250 in. OD and 0.035 in. walls. Samples were melted under flowing argon in a vertical, platinum-wound furnace, and solidified by driving the crucible downwards through a \ in. hole in a water-cooled copper toroid, Fig. l(a). An insulated chromel-alumel thermocouple was imbedded in the center of a representative sample, and moved with the sample during solidification. The local temperature is plotted against the distance travelled by the sample in Fig. 2. As the growth rate increased, the solid-liquid interface moved closer to the water-cooled toroid and the temperature gradient increased. At growth rates above 10-1' cm per sec, heat was not removed fast enough and the sample moved into the toroid in the liquid state. The curve for V = 2 x 10-1 cm per sec shows a plateau caused by incomplete removal of latent heat from the interface, a problem which will be discussed later. To improve the heat removal, the toroid was cooled by nitrogen gas precooled in liquid nitrogen. This allowed successful solidification at rates up to 2 x 10-1cm per sec. Higher solidification rates required still more effective heat removal. Samples 0.070 in. in diam were placed in graphite tubes 0.125 in. in diam with 0.020 in. walls. Instead of cooling by sliding contact with a cooled toroid, these thinner samples were sprayed or directly immersed into water, Fig. l(b). After solidification, samples were stored in liquid nitrogen until they could be examined metallographic-ally. The surface was prepared with a diamond-knife microtome, followed by a light etch. The presence or absence of tin dendrites, Fig. 3, or lead dendrites, Fig. 4, was noted by optical microscopy, usually of a transverse section near the center of the sample. Replicas of the surface were prepared and examined in an electron microscope to resolve the fine lamellar structures, Fig. 5. The structures observed at various compositions and growth rates are summarized in Fig. 6. Composite structures were observed at increasingly cin-rich compositions as growth rate increased. This transition from dendritic to composite structure with increasing growth rate was also demonstrated by solidifying half a sample at a slow rate and then suddenly increasing the growth rate by lifting the furnace and quenching the sample with a water spray. A longitudinal section of this sample, Fig. 7, shows that the tin dendrites, which extended ahead of the slow-moving composite interface, were bypassed by the composite when the growth rate was increased. The range of composite structures at high growth rates was limited by the appearance of primary lead dendrites on the tin-rich side of the eutectic composition. Observation of representative longitudinal