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Platinum Metals Review VOLUME 51 NUMBER 3 JULY 2007 Platinum Metals Review www.platinummetalsreview.com E-ISSN 1471–0676 E-ISSN 1471–0676 PLATINUM METALS REVIEW A Quarterly Survey of Research on the Platinum Metals and of Developments in their Application in Industry www.platinummetalsreview.com VOL. 51 JULY 2007 NO. 3 Contents Building a Thermodynamic Database for 104 Platinum-Based Superalloys: Part I By L. A. Cornish, R. Süss, A. Watson and S. N. Prins Enhancement of Industrial Hydroformylation Processes 116 by the Adoption of Rhodium-Based Catalyst: Part I By Richard Tudor and Michael Ashley The 4th Cape Organometallic Symposium: 127 Organometallics and Their Applications A conference review by David J. Robinson Vapour Pressure Equations for the Platinum Group Elements 130 By J. W. Arblaster “Nonporous Inorganic Membranes: for Chemical Processing” 136 A book review by Hugh Hamilton Platinum-Copper on Carbon Catalyst Synthesised 138 by Reduction with Hydride Anion By Hany M. AbdelDayem 2007 Fuels and Emissions Conference 145 A conference review by Andrew P. E. York Sir Geoffrey Wilkinson: New Commemorative Plaque 150 By W. P. Griffith New Autocatalyst Plant for South Korea 154 By Carlos Silva “Platinum 2007” 155 Abstracts 156 New Patents 159 Final Analysis: Why Use Platinum in Catalytic Converters? 162 By S. E. Golunski Communications should be addressed to: The Editor, Barry W. Copping, Platinum Metals Review, [email protected]; Johnson Matthey Public Limited Company, Orchard Road, Royston, Hertfordshire SG8 5HE, U.K. DOI: 10.1595/147106707X212967 Building a Thermodynamic Database for Platinum-Based Superalloys: Part I INTRODUCTION, AND INITIAL RESULTS FROM THE COMPOUND ENERGY FORMALISM MODEL By L. A. Cornish Advanced Materials Division, Mintek, Private Bag X3015, Randburg 2125, South Africa, DST/NRF Centre of Excellence in Strong Materials, Johannesburg 2050, South Africa, and School of Chemical and Materials Engineering, University of the Witwatersrand, Private Bag 3, Johannesburg 2050, South Africa R. Süss* Advanced Materials Division, Mintek, Private Bag X3015, Randburg 2125, South Africa, DST/NRF Centre of Excellence in Strong Materials, Johannesburg 2050, South Africa, and School of Chemical and Materials Engineering, University of the Witwatersrand, Private Bag 3, Johannesburg 2050, South Africa; *E-mail: [email protected] A. Watson Institute for Materials Research, University of Leeds, Leeds LS2 9JT, U.K. and S. N. Prins National Metrology Institute of South Africa, Private Bag X34, Lynwood Ridge 0040, South Africa, and Phases Research Lab, Department of Materials Science and Engineering, Pennsylvania State University, University Park, PA 16802, U.S.A. Work is being done at Mintek, the University of Leeds and the University of Bayreuth to build up a platinum-aluminium-chromium-ruthenium (Pt-Al-Cr-Ru) database for the prediction of phase diagrams for further alloy development by obtaining good thermodynamic descriptions of all of the possible phases in the system. The available databases do not cover all of the phases, and these had to be gleaned from literature, or modelled using experimental data. Similarly, not all of the experimental data were known, and where there were gaps or inconsistencies, experiments had to be undertaken. A preliminary version of the database was constructed from assessed thermodynamic data-sets for the binary systems only. The binary descriptions were combined, allowing extrapolation into the ternary systems, and experimental phase equilibrium data were compared with calculated results. Very good agreement was obtained for the Pt-Al-Ru and Pt-Cr-Ru systems, which was encouraging and confirmed that the higher-order systems could be calculated from the binary systems with confidence. Since some of the phase models in earlier databases were different, these phases had to be remodelled. However, more work is ongoing for information concerning the ternary phases present in the Al-Cr-Ru, Pt-Al-Ru (two ternary compounds in each) and Pt-Al-Cr (possibly more than three ternary compounds) systems. Later in the work, problems with the thermodynamic descriptions of the Cr-Ru and Pt-Cr binary systems were found, and a programme of experimental work to overcome these has been devised, and is being undertaken. Work has been ongoing in building a thermody- aid the design of alloys by enabling the calculation namic database for the prediction of phase of the composition and proportions of phases pre- equilibria in Pt-based superalloys (1–4). The alloys sent in alloys of different compositions. Currently, are being developed for high-temperature applica- the database contains the elements platinum, alu- tions in aggressive environments. The database will minium, chromium and ruthenium. This paper is a Platinum Metals Rev., 2007, 51, (3), 104–115 104 revised account of work presented at the confer- is a database for precious metals (7) it is not suffi- ence: Southern African Institute of Mining and ciently complete for the purposes of this Metallurgy ‘Platinum Surges Ahead’ at Sun City, investigation, and does not contain all the elements South Africa, from 8th to 12th October 2006 (4). of interest to this study, or all the phases. Ever since the possibility of basing a new series Additionally, not all the phase descriptions neces- of alloys on platinum was seen (1), work has been sary are present in Spencer’s database. The Al-Cr ongoing at Mintek, Fachhochschule Jena and system has also been independently assessed (8), Bayreuth University, Germany, with input from although some of the phases might ultimately be the National Institute for Materials Science modelled a different way by this group. (NIMS), Japan. Experimental work in this field is The phase diagram programs (e.g. Thermo- time-consuming and very expensive in terms of CalcTM, MTDATA and Pandat) comprise the equipment, materials and expertise. A number of software itself, accessed in modules through a important commercial alloy systems, such as steels, main interface, and a series of databases where the nickel-based alloys, and aluminium alloys now structural and thermodynamic data are stored. In have thermodynamic databases which have been these databases, each phase is described by a series derived from copious experimental results pub- of parameters. The SGTE database covers the lished by experts. These databases can be used phases of only the most common and well known with appropriate software to calculate phase dia- systems, and all the stable elements (5). The inter- grams, phase proportion diagrams, and Pourbaix metallic phases in the Al-Ru and Pt-Al systems are diagrams. They can be used instead of experimen- not included in the SGTE database. Providing that tation, saving both time and money. A similar the elements are available in a database (and all of database is being derived within this programme, the stable elements are in the SGTE database, or so that it will facilitate further alloy development, other available databases), a phase diagram can be and also be a tool to help designers to select alloy calculated and drawn. However, if there is no compositions and conditions in the future. description for a particular phase, then the calcu- However, steels, nickel-based and aluminium lated phase diagram cannot include it. A given alloys have been used extensively, and there are database can be modified to include new phases, or more data and accepted phase diagrams for these run in conjunction with another database. The aim systems than for Pt alloys. As inputs to the Pt- of this programme is to develop a database specif- based database, there are fewer commercial alloys, ically for the Pt-rich alloys in this investigation. experimental data, and very few accepted ternary Prior to building a database, it must be known systems. There are problems even with some of which phases need descriptions. Information on the binary systems. Thus, part of this work includ- the elements, and on any phase that is already ed the study of phase diagrams to address the lack included in the SGTE database (5), can be of data, and to use these data to compile a thermo- accessed from that database. For phases that are dynamic database. Since the basis of the alloys is not represented by the SGTE database, a number the Pt84:Al11:Cr3:Ru2 alloy, the thermodynamic of factors must be taken into consideration. Firstly, database will be built on the Pt-Al-Cr-Ru system. the structure of the phase has to be decided, The Scientific Group Thermodata Europe including the number of lattice sites for the atoms, (SGTE) database (5) includes all the elements and and which particular atoms fit on the sites. Each some of the most commonly used phases, i.e. phase is modelled with sublattices, and each sublat- those that are industrially important, but contains tice usually corresponds with a type of atom few of the required Pt phases. Additionally, the position. Elements allowed in a particular sublat- ruthenium data have been updated to capture tice are those actually found in those positions by Ansara’s modification, to obtain a better estimate crystallographic measurement. This information is of the calculated melting temperature for (hypo- usually derived from X-ray diffraction (XRD) thetical) b.c.c.-Ru (6) than hitherto. Although there structural information and composition ranges, Platinum Metals Rev., 2007, 51, (3) 105 and is usually made to be as simple as possible. ternary system must be optimised individually. Next, some values have to be obtained for the This is done using the experimental data, either interaction parameters. Initial values may be drawn from the literature, or, as was mostly the guessed, or the parameters set to zero, and the user case, derived experimentally within the pro- can decide which parameter can be varied during gramme at the University of the Witwatersrand optimisation. In preparing for optimisation, exper- and Mintek (for Al-Cr-Ru (13, 14), Pt-Cr-Ru (15, imental data are compared against the 16), Pt-Al-Cr (17, 18) and Pt-Al-Ru (19)) or the thermodynamic description, which is adjusted to CSIR and Mintek (for Pt-Al-Ru (20)).
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