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Carbothermal Reduction of Bauxite

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Carbothermal Reduction of Bauxite SCHOOL OF MATERIALS SCIENCE AND ENGINEERING Carbothermal Reduction of Bauxite A thesis in Materials Science and Engineering by Chun-Hung Yeh Submitted in partial fulfillment of the requirements for the Degree of Master of Philosophy 2012 Certificate of Originality I hereby declare that this submission is my own work and to the best of my knowledge it contains no materials previously published or written by another person, nor material which to a substantial extent has been accepted for the award of any other degree or diploma at UNSW or any other educational institution, except where due acknowledgement is made in the thesis. Any contribution made to research by others, with whom I have worked at UNSW or elsewhere, is explicitly acknowledged in the thesis. I also declare that the intellectual content of this thesis is the product of my own work, except to the extent that assistance from others in the project design and conception, or in style, presentation and linguistic expression is acknowledged. ------------------------------------------------ Chun-Hung Yeh UNSW Materials Science and Engineering School I Acknowledgements Many people assisted me both in the laboratory work and with the written aspects of this project. To these people I express deep appreciation. Oleg Ostrovski, my supervisor, who always gave me constant encouragement and generous support; Guangqing Zhang, my co-supervisor, who sparked my interest in this thesis project and who always shared his wealth of knowledge as well as his time; Yan Li, who assisted with continual guidance and critical assessment of my work; Xing Xing and Emily Wan for help with X-ray diffraction and LECO analysers, always without delay and with enthusiasm. Emily Wan, who assisted with electron microscopy and made a good time table with me. Maggie Zhang, appreciated for all things practical. I also thank those people whose names have been omitted from this list. UNSW Materials Science and Engineering School II Abstract The commercial technologies for aluminium production include production of alumina from bauxite by the Bayer process and smelting of alumina to produce aluminium by Hall-Heroult process. The current technology is energy intensive, a major source of greenhouse gas emissions and harmful fluoride emissions. These issues have stimulated the interests in search for alternative technologies of aluminium production. Carbothermal reduction of alumina is considered a promising alternative technology for aluminium production. However, the carbothermal process in investigation still needs pure alumina which does not solve the problems related to Bayer process, such as generation of harmful red mud, requires very high temperatures, and is overall still an energy intensive process. This thesis is concerned with the development of an environmentally sustainable technology for aluminium production that will avoid the generation of environmentally negative red mud sludge. It is to investigate the feasibility of stepwise carbothermal reduction of bauxite at different temperatures with emphasis on the examination of the mechanisms and kinetics of reduction of different metal oxides in bauxite, and also on the deportment of impurities among the various phases formed. It is expected that, if successful, this technology will significantly decrease energy consumption and CO2 emissions compared to conventional carbothermal reduction for aluminium production without generation of red mud waste. Understanding the kinetics and mechanisms of reduction of the different metal oxides in bauxite and the effects of operational parameters is essential for the achievement of the UNSW Materials Science and Engineering School III optimal conditions for the production of metallic aluminium and by-products such as ferroalloys and possibly titanium and silicon carbides. This project investigated the carbothermal reduction of Western Australian and Queensland bauxites in argon, carbon monoxide and hydrogen atmospheres. Experiments were performed in a high temperature vertical tube furnace and the off-gas composition was monitored using an infra-red gas analyser. The phase composition of reduced samples was characterized by X-ray diffraction (XRD). Oxygen and carbon contents in reduced samples were determined by LECO analysers. The morphology of the surface and intersections was observed by Scanning Electron Microscopy (SEM). The chemical compositions of the phases in the reduced samples were also detected by Energy-dispersive X-ray spectroscopy (EDS). The results of this study have proved the concept of stepwise reduction of bauxite ores in solid state by appropriate controlling reduction temperature. The products in reduced bauxites by temperature programmed reduction to 1600oC include ferroalloy of silicon and aluminium, carbides of titanium, silicon and aluminium, and unreacted alumina. It also showed that temperatures and the gas environment affected the extent of reduction. These results are of importance to an explanation of the stepwise carbothermal reaction of bauxites, as well as providing aluminium industry with a better understanding of alternative ways to produce aluminium. UNSW Materials Science and Engineering School IV Table of Contents Section Page Certificate of Originality .......................................................................................... I Acknowledgements .................................................................................................. II Abstract .................................................................................................................. III 1 Introduction ...................................................................................................... I 1.1 Importance of Aluminium ................................................................................. 1 1.2 Current Aluminium Production Technologies................................................... 3 1.3 Environmental Issues Associated with Current Production Technologies ........ 4 1.4 Alternative Routes for Aluminium Production ................................................. 6 2 Literature Review ............................................................................................ 8 2.1 Introduction to Bauxite, Alumina and Aluminium ............................................ 8 2.1.1 Bauxite....................................................................................................... 8 2.1.2 Alumina ................................................................................................... 10 2.1.3 Aluminium ............................................................................................... 17 2.2 Aluminium Alloy ............................................................................................ 19 2.3 Metal Oxides Impurities in Bauxite Ores ....................................................... 21 2.4 Carbothermal Reduction of Bauxite................................................................ 22 2.4.1 Carbothermal Reduction of Alumina ...................................................... 23 2.4.2 Carbothermal Reduction of Titania ........................................................ 25 2.4.3 Carbothermal Reduction of Silica ........................................................... 27 2.4.4 Carbothermal Reduction of Iron Oxides ................................................. 29 2.5 Thermodynamics and Kinetics of Carbothermal Reduction ........................... 30 UNSW Materials Science and Engineering School V 2.5.1 Thermodynamics ..................................................................................... 31 2.5.2 Kinetics .................................................................................................... 35 2.6 Summary and Scope of the Thesis .................................................................. 38 3 Experimental.................................................................................................. 40 3.1 Materials .......................................................................................................... 43 3.2 Gases ............................................................................................................... 44 3.3 Sample Preparation ......................................................................................... 44 3.4 Experimental Set Up ....................................................................................... 45 3.4.1 Experimental Furnace ............................................................................. 45 3.4.2 Reactor Set Up ........................................................................................ 45 3.4.3 Gas System .............................................................................................. 46 3.5 Experimental Procedure .................................................................................. 48 3.6 Sample Characterisation.................................................................................. 49 3.6.1 X-ray Diffraction Analysis ...................................................................... 49 3.6.2 LECO Analyses ....................................................................................... 50 3.6.3 Scanning Electron Microscopic (SEM) and Energy Dispersive X-ray Spectroscopy (EDS) ................................................................................................. 51 3.7 Calculation of Extent of Reduction ................................................................. 51 3.7.1 Calculation
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