Archaeological Arsenical Bronzes and Equilibrium in the As-Cu System
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Archaeological Arsenical Bronzes and Equilibrium in the As-Cu System MARIANNE MO¨DLINGER, ANDREAS CZIEGLER, DANIELE MACCIO´, HOLGER SCHNIDERITSCH, and BENJAMIN SABATINI Understanding the effects of impurities, segregation, undercooling, and solidification velocity is necessary to reconstruct prehistoric As-Cu alloy manufacturing processes and practices. Moreover, these alloys often contain a wide variety of minor and trace elements such that the binary As-Cu equilibrium phase diagram does not adequately represent arsenical bronze artifacts as-cast in ancient molds. Furthermore, the variable cooling rates present in as-cast alloys of predominantly arsenic and copper, due to the thermal properties of differing mold materials, would have had profound effects on the formation of inversely segregated arsenic. Alloys with 1 to 15 wt pct arsenic were prepared and studied using differential thermal analysis, metallography, and scanning electron microscopy with energy-dispersive X-ray spectroscopy. Equilibrium diagrams were established and the potential influence of trace elements discussed. A new liquidus curve for the equilibrium diagram in this compositional range, measuring slightly higher in temperature, was established. https://doi.org/10.1007/s11663-018-1322-8 The Minerals, Metals & Materials Society and ASM International 2018
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INTRODUCTION
ARSENIC-COPPER alloys were the first alloy intentionally produced by mankind, appearing in the archaeological record as early as c. 5000 BC on the Iranian plateau, and later in Central Europe in the fourth and early third millennium BC.[1] Although commonplace in prehistory, they were replaced by safer and more capable alloys such as tin–bronzes and brasses, and have since had few historic applications. Because of their early prehistoric origins and manufacture, the alloy is highly important to archaeologists
MARIANNE MO¨DLINGER is with the IRAMAT-CRP2A UMR 5060 CNRS, Universite´ Bordeaux Montaigne, Maison de l’arche´ologie, Esplanade des Antilles, 33607 Pessac, France. Contact e-mail: [email protected] ANDREAS CZIEGLER is with the Lehrstuhl fu¨r Gießereikunde, Montanuniversita¨t Leoben, Franz-Josef-Strasse 18, 8700 Leoben, Austria, DANIELE MACCIO` is with the Dipartimento di Chimica e Chimica Industriale, Universita` degli Studi di Genova, Via Dodecaneso, 31, 16146 Genova, Italy, HOLGER SCHNIDERITSCH is with the Lehrstuhl Nichteisenmetallurgie, Montanuniversita¨t Leoben, Franz-Josef-Strasse 18, 8700 Leoben, Austria, BENJAMIN SABATINI is with the Department of Materials Science & Engineering, Massachusetts Institute of Technology, 13-5065, 77 Massachusetts Avenue, Cambridge, MA 02139-4307 and also with the USTC Archaeometry Laboratory, University of Science and Technology of China, 96 Jinzhai Road, Hefei 230026, China. Manuscript submitted December 1, 2016.
METALLURGICAL AND MATERIALS TRANSACTIONS B
seeking to interpret the pyrotechnological past. The study of the As-Cu system is therefore essential to improve our understanding of prehistoric metallurgy
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