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The Ultratrace Element Geochemistry of Tin Ores and Bronze Using Icp-Ms and the Mining and Metals Trade in Prehistoric Thailand

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The Ultratrace Element Geochemistry of Tin Ores and Bronze Using Icp-Ms and the Mining and Metals Trade in Prehistoric Thailand THE ULTRATRACE ELEMENT GEOCHEMISTRY OF TIN ORES AND BRONZE USING ICP-MS AND THE MINING AND METALS TRADE IN PREHISTORIC THAILAND Thesis submitted by VANESSA JEAN COOTE as a requirement for the degree of DOCTOR OF PHILOSOPHY at the Institute of Archaeology University college London 1991 1 ABSTRACT The geochemical variation of tin ore deposits is examined at both the genetic level and on a regional scale. The influence of tectonic, magmatic and geologic history on the distribution of tin deposits is discussed. Multielement and isotopic analysis of ultratrace elements in ores and metals, by Inductively Coupled Plasma Source Mass Spectrometry (ICP-MS), is used to determine those elements which may be used to characterise the tin component of archaeological bronzes from Thailand. The efficiency of ICP-MS for this work on tin ore provenancing is evaluated and the data analysed to provide information on the technology and trade in the early southeast asian metals industry. Documented information on the pre-industrial mining industry of Southeast Asia is examined together with the economic theory of small-scale mining and metals trade to present a scenario for the influence of an early metals industry on the culture of Thailand in the 1st millennium BC. This scenario is examined in the context of the analytical data presented and the current views of southeast asian archaeology and anthropology. 2 TABLE OF CONTENTS Abstract. 2 Table of Contents. 3 List of Figures and Tables. 8 List of Plates. 15 Acknowledgements. 17 Abbreviations. 19 1. INTRODUCTION 22 1.1 The Aims of the Project. 22 1.2 The Theory. 23 1.2.1 The Geology and Geochemistry. 23 1.2.2 The Metals. 24 1.2.3 The Analytical Method. 25 1.2.4 Mining and MetallurgicalHistory. 26 1.3 The Research Method. 26 2. GEOLOGY 28 2.1 Geology of Southeast Asia and Thailand. 28 2.1.1 Granite Provinces. 28 i) Tectonic Evolution of Southeast Asian Mineralised Granites. 33 ii) Tin Ores and Their Relationship to the Granites. 37 2.1.2 Metalliferous Regions and Zoning of Elements. 42 i) General. 42 ii) Deposits other than Tin. 57 a) Copper andLead/Zinc. 57 b) Barite. 58 c) Bismuth. 58 d) Antimony andMercury. 58 e) Chromite. 59^ f) Gold. 60 g) Zircons. 60 h) Tungsten. 61 i) Uranium. 62 2.2 Tin Geology. 62 2.2.1 Types of Tin Deposit. 62 i) Tin Provinces. 62 ii) Tectonic Environments. 65 3 iii) The Classification of Tin Deposits. 66 a) Pegmatites. 68 b) Veins and Stockworks. 70 c) Greisens. 70 d) Skarns. 71 e) Altered Primary & Secondary Deposits. 72 2.2.2 Geochemistry of Tin. 77 i) Previous Research. 77 ii) Diagnostic Elements in Cassiterite Concentrates. 8 0 a) Rare Earth Elements (Lanthanides). 80 b) Niobium and Tantalum. 82 c) Tungsten and Titanium. 83 d) Indium. 83 e) Scandium. 83 f) Zirconium. 84 g) Lithium. 84 h) Gallium. 84 i) Other Elements. 84 iii) Diagnostic Elements in the Study of Tin Bronzes. 85 iv) Elements and their Mineralogical Associations. 86 2.2.3 Tin Regions relevant to Southeast Asia. 88 i) South China. 88 a) South China Fold System. 88 b) Daxinganling and Jilin-Heilungjiang Fold System. 89 c) Sanjiang Fold System. 89 ii) India. 90 iii) South Thailand. 92 iv) North Thailand. 92 v) Central Thailand. 94 vi) West Malaysia. 95 a) Kinta Valley. 97 vii) East Malaysia. 99 3. ANALYSIS 104 3.1 Instrumentation. 104 3.1.1 ICP-MS. 104 4 i) Discussion of Methods. 104 ii) ICP-MS. 107 iii) Lead Isotopes by ICP-MS. 115 3.2 Analytical Procedure. 116 3.2.1 Basic Problems. 116 i) Contamination of Reagents. 116 ii) Preparation Methods. 118 iii) Polyatomic and Isobaric Overlap. 120 iv) Partitioning of Trace Elements. 129 v) Alloying. 129 vi) Recycling of Metals. 129 vii) Fluxes and Charcoal. 130 3.2.2 Sample Preparation. 131 i) Cassiterite and Tin. 131 3.3 Analytical Results. 132 3.3.1 Description of Samples. 132 i) Tin Samples. 132 ii) Copper Samples. 139 iii) Bronze Samples. 139 a) Non Chai. 140 b) Tham Ong Bah. 140 c) Kok Makamtao. 141 d) Ban Na Di. 141 e) Ban Don Ta Phet. 142 iv) Lead Samples. 143 3.3.2 Statistical Procedures. 145 3.3.3 The Use of Lead Isotopes. 147 3.3.4 ICP-MS Spectra. 154 3.3.5 Analytical Results. 172 i) Introduction. 176 ii) Copper Samples. 182 iii) Lead Samples. 183 iv) Tin Samples. 185 a) High Thorium Tin Sources. 186 b) High Yttrium Tin Sources. 186 c) High Tungsten Tin Sources. 186 d) High Gold Tin Sources. 186 e) Categorisation of Tin Sources. 186 v) Bronze Samples. 191 a) Notes on Some Elements. 199 5 Summary of the Bronzes. 202 4. MINERALS AND METALS INDUSTRY 211 4.1 Trade and Economics: the Present and the Past. 211 4.1.1 The Socio-Cultural Context - in brief. 211 4.1.2 Geological and Geographical Influences on Politico-Economic Structure. 222 i) The Red River Valley. 222 ii) The Southeast Asian Tin Belt. 224 iii) The Chao Phrya-Paklong Depression. 224 iv) The Tongle Sap Plains and Mekong River. 224 v) The Khorat Plateau. 224 vi) The Sichuan-Yunnan Region. 225 4.1.3 Trading Economy. 225 i) Bronze Production and Trade. 225 ii) Tin Mining in the Historical Period. 231 a) The Identification of Sites. 232 b) The Working of Different Tin Deposits.233 c) Pilok, Kanchanaburi. 233 d) Khlong Thom, Bang Saphan, Prachuap Khiri Khan. 234 e) The Peninsular Coast. 239 f) Ban Bo Kaeo, Samoeng, Chiang Mai. 241 g) Song Toh, Kanchanaburi. 244 h) Summary. 251 iii) Historical Information on Social Contexts. 251 a) Mining. 251 b) Customs. 256 c) Smelting Tin. 257 5. DISCUSSION, CONCLUSIONS AND FUTURE WORK 264 Appendix 1. Reduction Methods. 274 a) Hydrogen Reduction. 274 b) Carbon Reduction. 274 Appendix 2. ICP-MS Operating Conditions. 275 Appendix 3. Lead Mining at Song Toh, Kanchanaburi. 277 Appendix 4. Geochemical Tables. 287 Appendix 5. Mineralogical Determination of Ore 6 Sources. 293 Appendix 6. Deposit Maps. 296 a) Orientation Map. 297 b) Barite Deposits, Thailand. 298 c) Antimony Deposits, Thailand. 299 d) Tungsten Deposits, Thailand. 300 e) Tin Deposits, Thailand. 301 f) Copper/Lead/Zinc Deposits, Thailand. 302 g) Zinc Deposits, Burma. 303 h) Tin Deposits, Burma. 304 i) Barite Deposits, Burma. 305 j) Chromite Deposits, Burma. 306 k) Antimony Deposits, Burma. 307 1) Tungsten Deposits, Burma. 308 m) Lead Deposits, Burma. 309 n) Tin/Tungsten/Fluorite Deposits of Southeast Asia. 310 Appendix 7. Tin Deposit Classifications. 311 Appendix 8. Basic Heavy Mineral ProcessingMethods. 319 Appendix 9. Primitive Mining Methods Current in Thailand. 325 Appendix 10. Provinces and Regions of Thailand. 336 Appendix 11. Glossary. 339 Bibliography. 342 7 LIST OF FIGURES AND TABLES Figure 111. Orientation Map of Thailand. encl. Figure 112. Orientation Map of South China. encl. Figure 211A. Southeast Asian Metalliferous Zones. 29 Figure 211B. Southeast Asian Granite Provinces. 31 Figure 211C. Plate Tectonic Reconstruction for the Southeast Asian Tin Belt. 33 Figure 211D. Major Tectonic Events Capable of Mobilising Tin from Precambrian Continental Basement. 35 Figure 2HE. Metallogenic-Tectono-Magmatic Provinces of Southeast Asia. 36 Figure 211F. The Tin Fields of Southeast Asia in Relation to the Granites. 38 Figure 212A. Tin Occurrences Related to the Structural Zones of South China. 44 Figure 212C. Metalliferous Zones of Thailand. 46 Figure 212D. Major Southeast Asian Structural Zones. 49 Figure 212E. Sn-Nb-Ta Deposits in Relation to Malaysian Mineralised Belts. 50 Figure 212F. Mineral Zonation in Kinta Valley, Perak. 54 Figure 212G. Schematic of the Deposit Zonation in the Dachang Ore Field. 54 Figure 212H. Complex Mineral Zonation in the Herberton Tin Field, Australia. 55 Figure 2121. Vertical Zonation of Mineralisation in the Dachang Tinfield, South China. 56 Figure 221A. The Greisen Environment. 64 Figure 22IB. Environments of Placer Deposition. 77 Figure 223A. Tin Deposits in India. 91 Figure 223C. Map of the Pilok Tin-Tungsten Mineralised Field. 93 Figure 223D Major Primary Deposits of the Kinta Valley. 98 Figure 223E. Distribution of Significant Stanniferous Hydrothermal Veins, Pegmatites and Aplites in Malaysia. 101 Figure 223F. Distribution of Significant Stanniferous Skarns in Malaysia. 102 Figure 311A. System Diagram of Plasma-Source Mass Spectrometer. 108 Figure 312A. Full Range Profile of Bronze BND-1101. Ill 8 Figure 312B. Expanded Spectrum of BND-1101 Showing Tin Peaks. 112 Figure 312C. Expanded Spectrum of BND-1101 Showing Barium and Lanthanides. 112 Figure 312D. Expanded Spectrum of BND-1101 Showing Silver, Tin and Barium/REE Peaks. 113 Figure 312E. Spectrum of BND-1101, Reduced Vertical Scale to Show Tin Peaks. 113 Figure 312F. Spectrum of BND-1101 Showing Iron/Manganese Peaks. 114 Figure 312G. Expanded Spectrum of BND-1101 Showing Lead/Bismuth Peaks. 114 Figure 312H. Lead Isotopes in Bronze. 117 Figure 321A. ICP-MS Spectrum of an Aqueous Tin Solution in 500ng/ml, Illustrating the Occurrence of Tin-Related Polyatomic Interferences. 124 Figure 32IB. ICP-MS Spectrum for lug/ml Ta, Indicating the Presence of TaO+ on Au at 197 amu. 125 Figure 321C. ICP-MS Spectrum for lug/ml Nb, Indicating the Presence of NbO+ Interference on Ag at 109 amu. 126 Figure 312D. Full Range Profile of 3% HC1 Acid Blank. 127 Figure 332A. Chart Showing Copper Anomaly in Ratchaburi Cassiterite. 148 Figure 332B. Chart Showing Effect of Removal of Ratchaburi Tin Anomaly. 148 Figure 332C. Chart Showing Copper, Lead and Zinc Anomalies in Cassiterite Samples. 149 Figure 332D. Chart Showing Effect of Removal of Major Copper, Lead and Zinc Anomalies. 149 Figure 332E. Bar Chart of Lead and Zinc in Bronze. 150 Figure 332F.
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