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Sulfur Isotope Ratios and the Origin of the Sulfide Deposits

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Sulfur Isotope Ratios and the Origin of the Sulfide Deposits SULFUR ISOTOPE RATIOS AND THE ORIGIN OF THE SULFIDE DEPOSITS IN THE BATHURST AREA OF NORTHERN NEW BRUNSWICK by WILLIAM M. TUPPER B. Sc. Mount Allison University (1953) M. Sc. University of New Brunswick (1955) SUBMITTED IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY at the MASSACHUSETTS INSTITUTE OF TECHNOLOGY (1959) Signature of Author. ......... ..... 7 Igepartggt pf Geg6gy and Geophysics, May '7 , 1959 Certified by . -A I t) A ( ) Thesis Supervisor Certified by, -1 11.1 .1 Thesis Supervisor Accepted by. ............................. .... Chairman, Departmental Committee of Graduate Studies 11 Sulfur Isotope Ratios and the Origin of the Sulfide Deposits in the Bathurst Area of Northern New Brunswick William M. Tupper Submitted to the Department of Geology and Geophysics on May 7 , 1959 in partial fulfillment of the requirements for the degree of Doctor of Philosophy Abstract The regional geology of the Bathurst.Newcastle area is briefly outlined. There are two types of sulfide deposits in the Area; (a) epigenetic fissure deposits, and (b) massive sulfide deposits. Geological evidence can be variously interpreted to suggest a syngenetic, a source bed, or a magmatic hydrothermal origin for the massive sulfide deposits. S32 /34 ratios are presented for more than three hundred sulfide samples from the host rocks and sulfide deposits. Four granite bodies are dated by the potassiummargon method. Model lead ages are presented for five galena samples. Sulfides disseminated through the black shales and argillites of the host rocks are enriched in S 32(mean value 22. 31) relative to the meteoritic ratio, and have a broad range of values. S32/S34 ratios for the sulfide deposits fall into two distinct groups. In general one group (21. 88 - 22. 05) represents the massive sulfide deposits, while the other group (22. 18 w 22. 21) represents the fissure deposits. This suggests two separate, but probably closely related sources for the sulfur. Granites intrusive into the host rocks of the sulfide deposits have a mean age of 386 * 10 m. y. Lead minerals in the sulfide deposits have a mean model lead age of 370 * 20 m.y. Thus the lead minerals and the granite bodies were emplaced during the same major orogeneic event. The sulfide deposits of the Bathurst area have a narrow range of S32/34 values. Sulfide deposits thought to have a magmatic hydrothermal origin all have a narrow range of S32 /s 3 4 values. It therefore seems reasonable that well homogenized magmatic hydrothermal solutions are the most logical source for the sulfide deposits. The homogeneity of the lead isotope abundance data gives strong inde.. pendent evidence that the ores are of a magmatic hydrothermal origin. The problem of why the massive sulfide deposits are enriched in S34 is open for further investigation. TABLE OF CONTENTS Chapter I Introduction 1 General 1 Previous Detailed Studies on Sulfur Isotope Variations 2 Location and Accessibility 3 Acknowledgements 4 Chapter I Sample Preparation and Analytical Techniques 8 Part I - The Determination of S 32/34 Ratios 8 Preparation of Minerals 8 Preparation of Samples from Sulfide Deposits 8 Sulfide from Sedimentary Rocks 9 Sulfide from Granites 9 Preparation of Sulfide from Sulfate in Mine Waters 9 Preparation of Sulfur Dioxide 10 Sulfur Isotope Analysis 13 Description of the Mass..Spectrometer 13 Procedure of Isotope Analysis 14 Reproducibility 15 Standards 16 Calculations 17 Part II - Geological Age Measurements by the K/A Method 20 Separation of Biotite from Granites 21 Chemical Preparation of the Biotite 21 Flame Photometer Analysis 21 Argon Release System 22 Gas Purification 23 Description of the Mass-Spectrometers 23 Isotope Analysis 24 Chapter III Geology of the Bathurst-Newcastle Area 28 Intriduction 28 General Geology 28 The Central Ordovician Folded Belt 28 The Silurian Folded Belt 31 The Pennsylvanian Cover 32 The Sulfide Deposits 32 Origin of the Massive Sulfide Deposits 34 Chapter IV Theory of Isotope Fractionation Involving Geological Processes Related to the Fractionation of Sulfur Isotopes 41 Chemical Processes 41 Equilibrium Reactions 41 Isotope Effects in Unidirectional Processes 46 Physical Processes 48 Diffusion 48 Evaporation 50 Distillation 50 Biological Processes 50 Chapter V The Isotopic Distribution of Sulfur in Nature 54 Meteoritic Sulfur 55 Sulfate in Ocean Water 56 Sedimentary Sulfides 56 Sulfur in Igneous Rocks 57 Processes of Isotopic Fractionation in Nature 57 Biological Processes 57 Fractionation in Volcanic Emanations and Geothermal Bore Holes 58 Crystallization and Precipitation Processes 59 Diffusion Processes 59 Oxidation Reduction Processes 60 Relative Importance of Isotopic Fractionation Processes 60 Geochemical Cycle of Sulfur Isotopes 61 Chapter VI The Application of Sulfur Isotope Studies to Sulfide Mineral Deposits Isotope Exchange Reactions The Significance of Associated Lead Isotope Studies Chapter VII Results Chapter VIII Discussion of Results 110 Sulfur Isotope Variations in the Syngenetic Sulfides and Intrusive Igneous Rocks 110 The Age of the Granites and the Lead Minerals in the Sulfide Deposits 111 Sulfur and Lead Isotope Abundance Data from the Same Samples 112 Sulfur Isotope Variations Between Different Mineral Species 112 Statistical Analysis of the Sulfur Isotope Variations 113 The Origin of the Deposits 114 Summary and Conclusions 119 Tables 122 Figures 124 Bibliography 125 Biography 128 Appendix I Tabulation of Sulfur Isotope Abundance Data 129 INTRODUCTION General The principles of isotope fractionation are now fairly well understood. Therefore a measurement of the extent of isotopic fractionation that has occurred in any element should be indicative of the processes through which that particular element has gone. However, natural processes are commonly of a complicated character, and quantitative agreement between theory and observation may not be found. Sulfur is of particular interest in regard to isotope abundance studies in view of its many forms and its wide distribution. The S34 content of sulfur in nature is known to vary by almost ten per cent. As it is the principle non-metal in most ore deposits, an understanding of its behavior in geological processes should aid in the critical evaluation of the genesis of sulfide depos-its. Large massive sulfide bodies were discovered in the Bathurst area of northern New Brunswick in 1953. Since then exploration and develop. ment work has advanced rapidly. To date, more than twenty large sulfide bodies have been located. Many are multi..million ton massive sulfide deposits. The geological environment of these deposits is complex and varied. As a result of these variations hydrothermal, source bed, and syngenetic origins have been advocated for these deposits. Late in 1957, sulfur isotope compositions were determined for a selected suite of sulfide samples from various geological environments in the Bathurst area (Jensen 1959). These results proved to be significant as well as interpretable, and indicated that a detailed study would be rewarding. In the detailed study which followed, sulfur isotope variations were determined within twenty-five sulfide deposits, and in the sulfides disseminated throughout the sedimentary host rocks and nearby granites. It was anticipated that relations within these environments would reflect the origin of the sulfide deposits. In addition it was hoped that important statistical and geochemical data on variations within these environments would be forthcoming. Geologic ages have been determined by the potassium-argon method on four granite bodies which are intrusive into the host rocks of the sulfide deposits. The Geophysics Department of the University of Toronto supplied revised lead isotope data on a suite of lead minerals from the area. This latter study was undertaken to determine whether or not there was any genetic relation between the granite intrusions and the lead minerals. Here then, for the first time, is a detailed study of the isotopic variations of sulfur not only within a single deposit, but throughout several deposits and geologic environments in a complex geologic sub. province. Sufficient care in sampling and in analytical processing has been taken to insure the significance of the results. Over three hundred natural samples containing sulfur were subjected to isotopic analysis. Previous Detailed Studies on Sulfur Isotope Variations In 1927, Aston showed that sulfur was a mixture of isotopes contisting of S32 33 and S34 and present in abundance roughly proportional to the numbers 96,1..3 respectively. A. 0. Nier (1938) discovered S36 and determined that it made up 0. 016 per cent of all sulfur. Thode and his co,-workers at McMaster University started investigations 3 in 1949 on the variations of sulfur isotope abundances in natural materials. Their studies are still in progress. Similar studies were started by Vinogradov in Russia in 1949, by Kulp and co..workers at Columbia University in 1955, by Jensen and Bateman at Yale University in 1956, by Sakai in Japan in 1957, and by Rafter and his co...workers in New Zealand in 1957. To date, there has been two comprehensive studies on the isotopic variations of sulfur in specific mineral deposit environments. The first of these investigated the origin of the Gulf Coast salt dome sulfur deposits (Thode et al, 1954; Feely and Kulp, 1957). This study proved fairly conclusively that salt dome sulfur originated through bacterial reduction of the anhydrite in the cap rock of the salt dome to hydrogen sulfide with subsequent oxidation of the sulfide to native sulfur. The second study investigated the origin of the sandstone type uranium deposits of the Colorado Plateau and Wyoming (Jensen 1958). The isotopic variations suggest that sulfate waters were reduced by anerobic bacteria to hydrogen sulfide, which later brought about the concentration of uranium through precipitation of the soluble uranyl ions to relatively insoluble uranium dioxide. At the same time the H2S brought about the precipitation of ferrous sulfate as iron sulfide. Detailed investigations are currently underway at Yale University on the sulfur isotope variations in the Heath Steele sulfide deposits at Newcastle, New Brunswick.
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