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THESIS Entitled the GEOCHEMISTRY of FLUORINE

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THESIS Entitled the GEOCHEMISTRY of FLUORINE A THESIS entitled THE GEOCHEMISTRY OF FLUORINE AND ITS APPLICATIONS IN MINERAL EXPLORATION Submitted for the degree of DOCTOR OF PHILOSOPHY in the Faculty of Science of the University of London . by DANIEL ROBERT BOYLE Royal School of Mines •Imperial College of Science and Technology June 1976 (i) ABSTRACT A detailed description of the geochemistry of fluorine is given, followed by investigations on the analytical geochemistry of the element and its applications in mineral exploration. The role of fluorine in the formation of rocks and minerals and its concentration in these media has been described. Fluorine is concentrated in those minerals in which it is an essential element (e. g. fluorite, topaz, bastnaesite, amblygonite, humites) or in which it can easily substitute for the OH ion (e. g. micas, amphiboles, apatite, tourmaline) or 02° ion (e. g. pyrochiore). In igneous rocks, fluorine is concentrated in the more acidic and/or alkalic members; ultrabasic rocks exhibiting the lowest concentrations of fluorine and alkali granites the highest. In sedimentary rocks, the element is concentrated in phosphatic and/or highly micaceous rocks. During regional metamorphism, fluorine is remobilized and rocks formed as a result of this process contain much less fluorine than their original igneous and sedimentary counterparts. Rocks formed as a result of pneumatolytic-hydrothermal alteration, such as greisens, skarns, fenites, serpentinized basics and kaolini.zed granites are invariably fluoriferous. The role of fluorine in the formation of mineral deposits has been discussed with emphasis being placed on elemental associations, controls to mineralization (chiefly chemical) and alteration. In the pedosphere fluorine is concentrated in rocks having a high phosphate and/or micaceous content. Calcium, phosphate, humic matter and clay composition all have a controlling effect on the fixation of fluorine in soils.. In natural waters, fluorine is present largely in the ionic state but may form complexes with elements such as Al and Fe under certain conditions. Calcium and sodium greatly affect the concentration of fluorine in natural waters; the former supressing it and the latter enhancing it. On a dry weight basis, fluorine exhibits a large concentration range in vegetation ( 10 to 8, 000 ppm) but there appears to be no plants which specifically seek out areas of high fluorine concentration in their substrate. Factors affecting the concentration of fluorine in atmospheric and soil air are discussed. Cold extractable (0. 01M HC1), acid diffusible and total methods of fluorine analysis have been developed for use in mineral exploration. The procedure for each of these methods, based on the use of the fluorine ion electrode, are described together with discussions of the factors affecting determination. An understanding of the ability of these methods to extract fluorine from various fluoriferous minerals, as well as colloid and adsorbed phases, was found to be essential for their effective application in geochemical exploration. Fluorine is concentrated in a large variety of mineral deposits: namely, carbonatites; kimberli.tes; pegmatites; greisen (Sn, W, Be, Mo, Bi) deposits; skarn deposits; many types of hypo-, meso- and epithermal mineral deposits containing tourmaline, topaz and fluorite; disseminated deposits (Sn, Nb, Ta, fluorite) in granitic, syenitic and rhyo-dacitic intrusions the alteration haloes of certain. volcanogenic sulphide deposits in rhyo-dacitic intrusions; serpentinized ultrabasic and basic bodies possibly containing Ni, Cu, Cr, and Co mineralization; sedimentary phosphate deposits; and many types of placer deposits (e. g. Nb, Ta, Sn). The element is therefore an ideal pathfinder in all types and stages of geochemical exploration aimed at the detection of these deposits. Detailed descriptions of the application of fluorine in prospecting for the mineral deposits mentioned above are given. These include lithogeochemical methods for detecting primary haloes, favourable mineral environments and fault zones; hydrogeochemical methods utilizing groundwaters and drainage sediments; and pedogeochemical surveys for detailed follow-up. Results of preliminary studies on the use of fluorine in vapour geochemical surveys indicate the need for more sensitive instrumentation before this technique can be fully assessed. Finally, conclusions are drawn concerning the efficacy of fluorine in geochemical exploration. ACKNOWLEDGMENTS The author would like to thank the following people and institutions for assisting him in this research. Dr. W. T. Meyer - for supervising the author during the early stages of the research. Professor J. S. Webb - for supervising the author during the final stages of the research and also for allowing the writer to use samples from the extensive reference collection of the Applied Geochemistry Research Group. Dr. M. Thompson - for his helpful advice on aspects of the analytical geochemistry of fluorine. Rio Tinto Zinc Educational Trust - whose financial support in the form of a bursary for part of the duration of this work is greatly acknowledged. Mrs. M. Smit - who skilfully typed the manuscript. (iv) TABLE OF CONTENTS Page ABSTRACT (1) ACKNOWLEDGMENTS (iii) TABLE OF CONTENTS (iv) LIST OF TABLES (ix) LIST OF FIGURES INTRODUCTION 1 CHAPTER I THE GEOCHEMISTRY OF FLUORINE 3 1.1 INTRODUCTION 3 1.2 LITHOGEOCHEMISTRY 8 1.2.1 Fluorine in Minerals 8 1.2.2 Fluorine in the Igneous Intrusive Environment 22 1.2.3 Fluorine in the Volcanic Extrusive Environment 31 1.2.4 Fluorine in the Sedimentary Environment 34 1.2.5 Fluorine in the Metamorphic Environment 39 1.2.6 Fluoriferous Deposits 44 1.2.7 The Role of Fluorine in the Formation of Ore Deposits 43 1.2.7.1 Introduction 48 1.2.7.2 Elemental Associations and Controls of Mineralization 51 1.2.7.3 Alteration and Primary Haloes 59 1.3 HYDROGEOCHEMISTRY 65 1.4 PEDOGEOCHEMISTRY 87 1.5 BIOGEOCHEMISTRY 95 1.6 ATMOGEOCHEMISTRY 99 ( v ) CHAPTER II ANALYTICAL RESEARCH AND DEVELOPMENT •102 2.1 INTRODUCTION 102 2. 2 INSTRUMENTATION AND ELECTRODE PROPERTIES 104 2. 3 WATER ANALYSIS 113 2.4 COLD-EXTRACTABLE FLUORINE (cxF) METHODS 116 2. 5 ACID DIFFUSIBLE FLUORINE ANALYSIS 126 2. 6 TOTAL FLUORINE ANALYSIS 140 CHAPTER III APPLICATION OF FLUORINE GEOCHEMISTRY TO 156 MINERAL EXPLORATION 3. 1 REVIEW OF PREVIOUS APPLICATIONS 156 3.1. 1 Introduction 156 3.1. 2 Lithogeochemical Prospecting 157 3.1.3. Hydrogeochemical Prospecting 160 3.1.4 Pedogeochemical Prospecting 169 3.1. 5 Biogeochemical Prospecting 174 3.1.6 Atmogeochemical Prospecting 175 3. 2 PROSPECTING FOR MINERAL DEPOSITS OF 176 MAGMATIC ORIGIN 3. 2.1 Introduction 176 3. 2. 2 Prospecting for Carbonatites and Kimberlites 177 3. 2.2.1 Introduction 177 3.2. 2.2 Geology and Mineralization of Carbonatites and 177 Kimberlites 3.2.2.2.1 Introduction 177 3.2.2.2.2 Carbonatites 178 3.2. 2.2.3 Kimberlites 179 3. 2. 2. 3 Geochemistry of Carbonatites and Kimberlites 181 3. 2. 2.3.1 Introduction 181 3. 2. 2.3.2 Fluorine in Carbonatites 185 3. 2. 2. 3. 3 Fluorine in Kimberlites 186 3.2.2.4 Methods of Prospecting for Carbonatites 192 3.2.2.4.1 Introduction 192 3.2.2.4.2 Kaluwe Carbonatite Area, Zambia 193 3.2.2.4.2.1 Introduction 193 3.2.2.4.2.2 Dispersion of Fluorine in Stream Sediments 196 3.2.2.4,2.3 Dispersion of Fluorine in Soils 203 3.2.2.5 Methods of Prospecting for Kimberlites 216 3.2.2.5.1 Introduction 216 3. 2. 2.5.2 Arkansas Kimberlite Area, USA 218 3.2.2.5.2.1 Introduction 218 3.2.2.5.2.2 Dispersion of Fluorine in Stream Sediments 222 3.2.2.5.2.3 Dispersion of Fluorine in Soils 224 3.2.2.6 Conclusions on Prospecting for Carbonatites and 228 Kimberlites 3.2.3 Prospecting for Disseminated Deposits in Granitic 230 Syenitic and Rhyo-Dacitic Intrusions 3.2.4 Prospecting for Sulphide Deposits in Serpentinized 231 Basic Intrusions 3.2.5 Prospecting for Pegmatites 232 3.2.5.1 Introduction 232 3.2.5.2 Bepe 2 Beryl Pegmatite, Rhodesia 237 3.2.5.2.1 Introduction 237 3,2.5.2.2 Dispersion of Fluorine in Wallrocks 240 3.2.5.2.3 Dispersion of Fluorine in Soils 242 3.2.5.3 Richardson Uraninite-Fluorite Pegmatite, Bancroft Area, Canada 3.2.5.3.1 Introduction 250 3.2.5.3.2 Dispersion of Fluorine in Soils 253 3.2.5.4 Conclusions on Prospecting for Pegmatites 259 3.3 PROSPECTING FOR MINERAL DEPOSITS OF 260 PNEUMATOLYTIC -HYDOR THERMAL ORIGIN 3.3.1 Introduction 260 3.3.2 Prospecting for Greisen Deposits 261 (vii) 3. 3. 2. 1 Introduction 261 3. 3. 2. 2 Tin Province, S W. England 262 3. 3.2.2.1 Introduction 262 3. 3. 2. 2. 2 Primary Dispersion of Fluorine 265 3. 3. 2. 2. 3 Dispersion of Fluorine in Stream Sediments 271 3. 3. 2. 2. 4 Dispersion of Fluorine in Soils 272 3. 3. 3 Prospecting for Hypothermal Mineral Deposits 284 3. 3. 3. 1 Introduction 284 3. 3. 3. 2 Gold-Quartz Veins, Sierre Leone . 284 3. 3. 4 Prospecting for Mesothermal and Epithermal 287 Mineral Deposits 3. 3. 4. 1 Introduction 287 3. 3. 4. 2 Tynagh Pb-Zn-Cu Deposit, Eire 288 3. 3. 4. 2. 1 Introduction 288 3. 3.4. 2. 2 Dispersion of Fluorine in Soils 291 3. 3. 4. 3 Halikoy Mercury Deposit, Turkey 294 3. 3. 4. 3. 1 Introduction 294 3. 3. 4. 3. 2 Primary Dispersion of Fluorine 297 3. 3. 4. 3. 3 Dispersion of Fluorine in Soils 299 3. 3. 4. 4 Ivrindi Antimony Deposit, Turkey 302 3. 3. 4. 4. 1 Introduction 302 3. 3. 4. 4. 2 Dispersion of Fluorine in Soils 302 3. 3. 5 Prospecting for Kaolin Deposits in Granitic Intrusions 304 3. 3. 6 Prospecting for Contact Skarn Deposits 304 3.
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