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Historical Metallurgy Interests

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The following is adapted from Wadsley (2001)

Contents


Beginnings of Metallurgy


Carbon has been the metallurgist's reductant of choice since the Stone Age. Carbon, in the form of charcoal, is readily derived from wood by pyrolysis, or partial combustion. The naturally occurring minerals of most metals, when outcropping at the earth's surface, are their oxides. Some of these oxide minerals, such as some of those of copper and iron, are brightly coloured and hence attract the eye. Probably by chance, over six thousand years ago, humans learned that these oxide minerals could be converted to metals by their interaction with charcoal at the high temperature found in fires, possibly in the kilns used to fire pottery. Those persons also learned of the beneficial properties of the metals. By observation and by trial and error people improved their ability to recognise the various minerals of metals and improved their ability to convert those minerals into metals.

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Sixteenth Century Metallurgy


A fortunate combination of events has given us a record of the production of metals and chemicals towards the end of the era when metals were produced only by the renewable or sustainable resources of water, wind, animal and human energy plus carbon, mainly as wood charcoal. These events were the invention and development of the moveable type printing press by Johann Gutenburg and Laurens Koster about the year 1445 and the commitment of their metallurgical knowledge to paper by the authors of "Bergbuchlein", and "Probierbuchlein", by Vannoccio Biringuccio in 1540, by Georgius Agricola in 1556 and by Lazarus Erckerr in 1580. Soon after this time, an acute shortage of wood in Europe in general, and in Britain in particular, caused this region to substitute coal for wood in the production of heat and in the smelting of metals. Biringuccio recognised that coal could replace charcoal in the smelting of metals but indicated that its use was restricted to certain localities and was not general.

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Further Developments


In England iron makers began in 1589 to patent methods for using coal at different stages of the manufacturing process although none of these early methods seemed to have replaced charcoal in the actual smelting. Hugo Platt, in 1603 discovered coke produced by heating coal. Simon Sturtevant obtained in 1611 the first British patent for a process in which coal was used instead of charcoal for smelting iron. The significant use of fossil fuels as reductants in extractive metallurgy had begun.

During the seventeenth century, the ability of steam under pressure to do useful work was recognised by Giambattista in 1604, by Salomon de Caus in 1615, by Giovanni Branca in 1629, by the Marquis of Worcester in 1663 and by Isaac Newton in 1680. During the eighteenth century, industrial steam engines were widely employed and the mechanical age had begun. An early use of steam power was in pumps used in mines.

In the late eighteenth century electricity, Alessandro Volta generated direct-current electricity through a pile consisting of alternating zinc and silver metal discs. In 1807 Humphrey Davy used a similar devise to electrolyse potash and form metallic potassium. Michael Faraday demonstrated rotary electromagnetic motion in 1820. In 1833, Faraday produced metallic aluminium by electrolysis. An alternate metallurgical reductant to carbon was available.

H. St.-C. Deville commenced the commercial production of aluminium by reduction of aluminium chloride with sodium metal in 1854. The sodium metal was produced by reduction of sodium carbonate with carbon. The aluminium chloride was produced by carbo-chlorination of alumina. This is an early example of achieving a desired result by multiple steps where the direct process (here the carbon reduction of alumina) is not feasible.

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Thermochemistry


It is instructive to note the metals produced prior to 1580 and those produced in modern times. Biringuccio, Agricola and Erckerr describe in detail the production of the metals gold, silver, copper, tin, lead, iron, arsenic, antimony, bismuth and mercury and of the alloys bronze, steel and brass. Zinc metal was known and small quantities were produced in Europe as a by-product in some lead smelters but it was not considered to be useful. Some other metals were probably produced in near pure or in alloy form but were not recognised because of their chemical and physical similarity with the known metals. Modern metals include aluminium, magnesium, titanium, zirconium, silicon, manganese and chromium. It is apparent from an examination of physical properties, such as melting point and boiling point, that these were not the reason why modern metals were not known to the older metallurgists. The reason lies in the relative thermochemical stability of the oxides of carbon and of the oxides of the metals. At the temperatures generated by the combustion of charcoal with air supplied at ambient temperatures, the oxides of the older metals are less stable and the oxides of the modern metals are more stable than the oxides of carbon. This information is often expressed as the oxide free energy diagram or Ellingham diagram.

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Heat Production at High Temperature


Smelting may produce condensed phase metals as either solids or liquids. The advantages of producing metal in the molten state and casting directly into useful shapes from the molten state were well known to the older metallurgists. Ancient copper smelting furnaces were able to attain temperatures in the range 1180 to 1350 C, the melting point of copper being 1085 C. However the advantages of bronze, the copper-tin alloy, which with a composition of 10 % wt tin melts at about 950 C, which could be more readily cast (and which is harder than pure copper) were well known to the older metallurgists. Although copper ores existed in many locations, tin ores were rare and tin oxide concentrates were an important traded commodity.

Iron was first smelted in ancient times in the solid state. The maximum temperature obtained in old metallurgy was apparently less than that required to melt pure iron, that is 1536 C. Slag was removed from the iron and it was shaped both by hammering. Steel was manufactured by carburising the iron with charcoal. It was learned that iron-carbon alloys could be melted and cast, the eutectic temperature being about 1153 C. China was the first region to obtain liquid iron-carbon alloys by direct smelting around 2000 years ago. Steel was manufactured by oxidising carbon from the melt. This technology was being introduced into Europe during the sixteenth century.

In pyrometallurgy, heat energy is required under reducing conditions both to heat the reactants to the desired reaction temperature and to supply the endothermic heat of reaction for most metals. In practice this usually means combustion in the presence of an excess of carbon. The combustion chemistry of carbon under these conditions is concerned both with the relative stability and the heat of formation from the elements of carbon monoxide and carbon dioxide. The thermodynamic stability of carbon monoxide relative to that of carbon dioxide increases with increasing temperature. The heat of formation from the elements of carbon dioxide (-197 kJ/g-atom O at 25 C) is significantly greater than that of carbon monoxide (-111 kJ/g-atom O at 25 C). Consequently as it is attempted to attain higher temperatures, the proportion of carbon monoxide in the gas phase increases but the heat generated by oxidation of a unit mass of carbon decreases. In addition, more heat is required to raise the temperature of the air, with its high concentration of inert nitrogen, to the reaction temperature. Smelting temperatures were thus quite limited in the simple charcoal-air system.

Modern smelting utilises air preheating and oxygen enrichment to attain higher temperatures but, with these methods, the limitations imposed by natural carbon-oxygen chemistry are still present. Electric heating is used to overcome these limitations.

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Evolution of Metallurgy


Before the time of Antoine Lavoisier's combustion experiments, around 1780, the concepts of quantitative mass and energy balances were not recognised, yet these principles form the basis of modern process design and analysis. The concept of assaying was well known to the older metallurgists who used standard procedures to determine whether the metal content of an ore was worth the effort to extract it or whether the metal product or coins were of the desired purity. In general, advancement in the ancient process industries was made predominantly by observation and experience. Much of modern industry has a similar basis. It is rare for a new plant to be designed from first principles. In many cases, the design of a new plant is based on the designs of older plants, with minor modifications being made for the different location and recent experience.

Those involved in the computer simulation of processes will be aware that many aspects of many unit operations have yet to be described in detail in terms of mathematical functions. The physical and chemical properties of many complex materials, in particular of metallurgical solutions, are still the subject of active mathematical modelling research. Many mathematical models for both operations and properties are based mainly on empirical relationships rather than fundamental properties.

The ancestry of many metallurgical processes, particularly those involving the blast furnace, may be directly traced back to ancient technology. In the lead, zinc and copper blast furnaces, sulfide minerals from beneath the earth's surface are converted to oxides before being smelted with carbon. The continued use of carbon in extractive metallurgy is partly based on its useful natural properties and partly on over six thousand years of history.

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Austherm's Courses


Austherm has collected a number of publications concerning ancient mineralogy, metallurgy and applied chemistry. Some of these are listed below. Austherm personnel have visited sites of ancient mining and metallurgy in Mediterranean Europe. Austherm are able to use their interest, resources, experiences and teaching expertise to provide tailored courses at under-graduate, graduate and community level in aspects of ancient mineralogy, metallurgy and applied chemistry.

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Bibliography


"Bergwerk und Probierbuchlein", A translation from the German of the "Bergbuchlein", a sixteenth century book on mining geology by Anneliese Grunhaldt Sisco and of the "Probierbuchlein", a sixteenth century work on assaying, by Anneliese Grunhaldt Sisco and Cyril Stanley Smith. Published by The American Institute of Mining and Metallurgical Engineers, New York, 1949

Georgius Agricola, "De Re Metallica", translated into English from the first Latin edition of 1556 by Herbert Clark Hoover and Lou Henry Hoover. Published by the Mining Magazine, London, 1912 Reprint published by Dover Publications, New York, 1950.

Georgius Agricola, "De Natura Fossilium", translated into English from the first Latin edition of 1546 by M.C.Bandy and J.A.Bandy in Geological Society of America. Special Paper 63, New York, 1995
Reprint published as Dover Phoenix Edition, New York, 2004

Vannoccio Biringuccio, "The Pirotechnia", translated from the first Italian edition of 1540 by Cyril Stanley Smith and Martha Teach Gnudi. Published by The American Institute of Mining and Metallurgical Engineers, New York,1942

Lazarus Erckerr, "Treatise on Ores and Assaying", translated from thr German Edition of 1580 by Anneliese Grunhaldt Sisco and Cyril Stanley Smith. Published by the University of Chicago Press, Chicago Illinois. 1951

Barba,A.A. "Arte De Los Metales", Coleccion de la Cultura Bolivia. A 1967 "Potosi" reprint of the original Madrid edition of 1640.

Bern Dibner, "Agricola on Metals", Burndy Library, Norwalk, 1958

Kuhner,D. and Rizzo,T. (1980). "The Herbert Hoover Collection", Claremont

Healy,J.F., (1978). "Mining and Metallurgy in the Greek and Roman World"", Thames and Hudson

Checkland,S.G., (1967). "The Mines of Tharsis", Allen & Unwin, London

Avery,D. (1974). "Not on Queen Victoria's Birthday: the Story of the Rio Tinto Mines", Collins, London

Rothenberg,B. and Blanco-Freijeiro,A., (1981). "Studies in Ancient Mining and Metallurgy in South-West Spain", Institute for Archeo-Metallurgical Studies, London

Robert Raymond "Out of the Fiery Furnace", MacMillan, South Melbourne, 1984

Bryan Bunch and Alexander Hellemans, "The Timetables of Technology", Touchstone, New York, 1993

J.R.Partington, "A Short History of Chemistry", 3rd Ed., Dover, New York, 1989

P. J. Golas, "Science and Civilisation in China ", Cambridge University Press, Cambridge, 1999

D. P. Agrawal, "Ancient Metal Technology and Archaeology of South Asia: a Pan-Asian Perspective", Aryan; India, 1999

Wadsley,M.W., (1979). "Metals and Energy Options", pp.167-169 in M.Diesendorf Ed., "Energy and People", SSRS, Canberra, 1979

Wadsley,M.W., (2001). "Greenhouse Gases and Extractive Metallurgy" pp.1-14 in Pickles,C.A. Ed. " Greenhouse Gases in the Metallurgical Industries: Policies, Abatement and Treatment " , Aug. 2001, CIM., Montreal, ISBN: 1-894475-15-1


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