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Geochemical and Isotopic Characterization of Shallow Basinal Brines from the Makgadikgadi Pans Complex, Northeastern Botswana

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Geochemical and Isotopic Characterization of Shallow Basinal Brines from the Makgadikgadi Pans Complex, Northeastern Botswana Western Michigan University ScholarWorks at WMU Dissertations Graduate College 12-2003 Geochemical and Isotopic Characterization of Shallow Basinal Brines from the Makgadikgadi Pans Complex, Northeastern Botswana: Determination of the Sources of Salinity Loago N. Molwalefhe Western Michigan University Follow this and additional works at: https://scholarworks.wmich.edu/dissertations Part of the Geochemistry Commons Recommended Citation Molwalefhe, Loago N., "Geochemical and Isotopic Characterization of Shallow Basinal Brines from the Makgadikgadi Pans Complex, Northeastern Botswana: Determination of the Sources of Salinity" (2003). Dissertations. 3379. https://scholarworks.wmich.edu/dissertations/3379 This Dissertation-Open Access is brought to you for free and open access by the Graduate College at ScholarWorks at WMU. It has been accepted for inclusion in Dissertations by an authorized administrator of ScholarWorks at WMU. For more information, please contact [email protected]. GEOCHEMICAL AND ISOTOPIC CHARACTERIZATION OF SHALLOW BASINAL BRINES FROM THE MAKGADIKGADI PANS COMPLEX, NORTHEASTERN BOTSWANA: DETERMINATIONOF THE SOURCES OF SALINITY by Loago N. Molwalefhe A Dissertation Submitted to the Faculty of The Graduate College in partial fulfillmentof the requirements forthe Degree of Doctor of Philosophy Department of Geosciences WesternMichigan University Kalamazoo, Michigan December 2003 Copyright by Loago N. Molwalefhe 2003 ACKNOWLEDGMENTS This work was conceived and completed because of the support of several individuals and organizations that deserve recognition. To the committee members, Dr. R.V. Krishanamurthy deserves special recognition for providing guidance at every stage of the project. Dr Eliot Atekwana spent endless hours of enthusiastic discussions on the subject matter. Appreciation is extended to Dr. Carla Korestky who revised the manuscript and frequently helped with re-arrangement of thoughts and technical presentation. Dr. A. Kehew deserves recognition as program advisor. Dr Estella Atekwana is gratefully acknowledged for inviting me to pursue a doctorate at Western Michigan University, and for the support she has offered throughout the years of my research. I met Mr Ahmed Murad as a colleague and friend and together we have gone through hands-on experiences on experimental designs and laboratory techniques. The author is thankful to Botswana Ash (Pty) Ltd and Mr. Godfrey Nkala for logistical support during field data collection. The project was fullyfunded by the University of Botswana. This dissertation is dedicated to my family, and to my fiancee of many years Ms. Tebogo Mmesi for being supportive, patient and loving during the endless years of my career development. The work is an achievement by all of us. Loago N. Molwalefhe 11 GEOCHEMICAL AND ISOTOPIC CHARACTERISATION OF SHALLOW BASINAL BRINE FR OM THE MAKGADIKGADI PANS COMPLEX, NORTHEASTERN BOTSWANA: DETERMINATION OFTHESOURCES OFSALINITY Loago N. Molwalefhe, Ph.D. WesternMichigan University, 2003 Isotopes and chemical tracers have been used to constrain the sources and causes of salinity in shallow groundwater brine from the Makgadikgadi Basin, northeastern Botswana. The brine is massively rich in chloride and sodium, and moderately rich in carbonates, sulphate and potassium, and is distinctively poor in divalent cationic species. Various models that have been advanced to explain the origin of the brines include evaporative enrichment at the surface and density-induced infiltration, dissolution of evaporites, and trapped connate water. This study presents the compositional variability and behaviors of ·the stable isotopes of carbon (8 13C) and oxygen (8 180), dissolved inorganic carbon (DIC) content, chloride, bromide and sodium in the brine from the northern part of Sua Pan, one of the Makgadikgadi Pans Complex. DIC concentrations in the brine reach 5grams of carbon per liter and 8 13Crnc compositions average -1.6±0.2%0. The values are compatible with dissolution and accumulation of carbon dioxide of geothermal origin. The halogen content of the brine (Cl/Br ratio) is consistent with studies of fluid-inclusion brines from magmatic rocks, and suggests significant magmatic influence in the formation of the brine. The sodium and chloride inventory on the other hand suggests additional sodium comes from intense weathering of silicate rocks. Spatial patterns in DIC concentrations and fluid conductivity show a linear anomaly of higher conductivity and DIC to the northeast of the study area. The anomaly may correlate with subsurface structural terminus in the bedrock where saline magmatic fluids are forced towards the surface along faults. Stable hydrogen · and oxygen isotope relationships show that the brine is a mixture of local meteoric water and magmatic water from below. The conclusion of a deeper source is consistent with the geology and recent seismic evidence that indicates the area is structurally dynamic. Isotope results are also consistent with a climate-driven scenario, in which water is affectedby evaporation at the surfaceprior to infiltration. TABLE OF CONTENTS ACKNOWLEDGMENTS............................................................ ................ :......... 11 LI ST OF TAB'LES ....... ····································.......................... ... ... ....................... V LIST OF FIGURES ..... ........................... .................. ...... .................. ...................... Vl CHAPTER I. INTRODUCTION................................................................................ 1 1.1 Statement of the Problem.............................................................. 1 1.2 Objectives of the Study................................................................. 3 1.3 Significanceof the Study.............................................................. 4 II. THE STUDY SI TE..................................................................................... 5 2.1 Site Location and Site Description................................................ 5 2.2 Regional Geology and Structural Framework............................... 8 2.3 Site Geology2.4 Hydrogeology .............................. ....................... 9 2.4 Hydrogeology ................... ................... ....................................... ... 10 2.5 Previous Studies............................................................................ 12 III. INVESTIGATIVE METHODS .............................................................. 14 3.1 Overview....................................................................................... 14 3.2 Field Sampling and Experimental Procedures.............................. 25 3 .3 Chemical Analyses........................................................................ 26 3.4 Stable Carbon Isotope Analyses (o13 C, DIC)................................ 27 3.5 Stable Oxygen (8 180) and Hydrogen (o2H) Analyses................... 27 111 Table of Contents-continued 3.6 Procedure forthe Distillation of Micro-liter Quantities Water From Brine Samples............................................................................ 29 IV. RESULTS AND DISCUSSIONS......................................................... 33 4.1 DIC and Stable Carbon Isotope...... _.................................. ............. 33 4.2 DIC and Fluid Conductivity Measurements.................................. 37 4.3 Cl-Br-Na Systematics.................................................................... 39 4.4 Na/Cl Ratios.................................................................................. 40 4.5 Stable Oxygen and Hydrogen Isotopes ......................................... 43 4.6 Stable Oxygen and Chloride Concentrations................................ 46 V. SYNTHESIS AND CONCLUSIONS INTRODUCTION................... 50 APPENDICES........................................................................................................ 52 A. Summary of Field Data forNorthern Part of Sua Pan..................... 52 B. Chemical and Isotopic Data for Brines From the NorthernPart of Sua Pan........................................................................................ 54 REFERENCES ... ... .......... .............. ... .......................................... ............................ 56 lV LIST OF TABLES 1. Experimental Test Data on the Efficiency of the Brine Distillation Cell...... 32 2. Comparisons of DIC Concentrations and Water Chemistries From Other Alkaline Saline Lakes and the Makgadikgadi System. All Concentrations are in mg/L. 2=Jones et al. (1977), 3=Jankowski and Jacobson (1989), 4=Gould (1986) and Current Study................................... 35 V LIST OF FIGURES 1. Locality Map of the Makgadikgadi Pans Complex and Study Area, Botswana ....................................................................................................... 6 2. Hydrogeological Cross-section of the NorthernPart of Sua Pan Showing the Various Hydro-stratigraphic Units Beneath the Pan; the Upper ConfiningClays, Sand-hosted Brine Aquifer, and Lower ConfiningSandstone/Basalt Unit .................................................................. 10 3. Map of the NorthernPart of Showing Sample Locations and Principal Groundwater Flow Paths in the Aquifer........................................................ 12 4. Schematic Diagram Showing how Various Processes Would Affect Cl/Br Ratio in Natural Waters .. .. ... .. ... ... .. .. .. ... .. .. ... .. ..... .. .... .. .. .. ... .. 22 5. Relationship �:i2Hand 8180
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