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Iv Geochemical and Isotopic Characterization of Coal

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Iv Geochemical and Isotopic Characterization of Coal Geochemical and Isotopic Characterization of Coal Combustion Residuals: Implications for Potential Environmental Impacts by Laura Suzanne Ruhl Earth and Ocean Sciences Duke University Date:_______________________ Approved: ___________________________ Avner Vengosh, Supervisor ___________________________ Gary Dwyer ___________________________ Heileen Hsu-Kim ___________________________ Paul Baker ___________________________ James Hower Dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Earth and Ocean Sciences in the Graduate School of Duke University 2012 i v ABSTRACT Geochemical and Isotopic Characterization of Coal Combustion Residuals: Implications for Potential Environmental Impacts by Laura Suzanne Ruhl Earth and Ocean Sciences Duke University Date:_______________________ Approved: ___________________________ Avner Vengosh, Supervisor ___________________________ Gary Dwyer ___________________________ Heileen Hsu-Kim ___________________________ Paul Baker ___________________________ James Hower An abstract of a dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy in Earth and Ocean Sciences in the Graduate School of Duke University 2012 Copyright by Laura Suzanne Ruhl 2012 Abstract Coal fired power plants are widespread in the United States and most developed countries around the world, providing affordable electricity to consumers. In the US, approximately 600 power plants generate 136 million tons of Coal Combustion Residuals (CCRs) annually, encompassing fly ash, bottom ash, and flue gas desulfurization materials. The range and blends of CCRs vary substantially across coal-fired plants and depend on a unique set of circumstances for each plant and coal source. Current U.S. regulations mandate the installation of advanced capture technologies to reduce atmospheric pollution, but do not address the transfer and storage, or the potential impacts to water resources. Thus, improved air quality is traded for significant enrichments of contaminants in the solid waste and effluent discharged from power plants. This work examines the geochemical and isotopic characteristics of CCRs, as well as potential environmental impacts from CCRs. This investigation looks at several different aspects of CCR and environmental interactions from 1) the immediate impacts of the 2008 TVA coal ash spill in Kingston, TN, 2) the long-term (18-month) exposure of the spilled ash in the Emory and Clinch rivers, 3) impacts on waterways in North Carolina that receive CCR effluent from coal fired power plants, and 4) examination of boron and strontium isotopes of CCRs from leaching experiments and their application as tracers in the environment of the TVA spill and NC waterways. These investigations have lead to the conclusion that 1) contact of surface water with CCRs brings about leaching of high concentrations of certain CCR contaminants, such as As, Se, B, Sr, Mo, and V in the surface waters; 2) the dilution effect is critical in determining the concentration of contaminants from the CCRs in surface water (both at the spill and in waterways receiving CCR effluent); 3) recycling of trace elements (such as As) through adsorption/desorption can impact water quality; and 4) elevated boron and strontium concentrations, in addition to their distinctive isotopic ratios, can trace CCR effluent in the iv environment. Combining the geochemical behavior and isotopic characteristics provides a novel tool for the identification of CCR effluents in the environment. v Dedication I dedicate this work in honor of my grandfather, Dan H. Ruhl, a great man and one of my favorite gators. vi Contents Abstract ...........................................................................................................................................iv List of Tables.................................................................................................................................... x List of Figures .................................................................................................................................xi Acknowledgements .......................................................................................................................xiv 1. Introduction .................................................................................................................................. 1 1.1 Background.......................................................................................................................... 1 1.2 Geochemistry and Isotopic Signature.................................................................................. 3 1.3 Dissertation Research and Objectives ................................................................................. 6 1.4.1 Chapter 2 Synopsis: A Survey of the Potential Environmental and Health Impacts in the Immediate Aftermath of the Coal Ash Spill in Kingston, Tennessee ....................................... 8 1.4.2 Chapter 3 Synopsis: The Environmental Impacts of the Coal Ash Spill in Kingston, Tennessee: An Eighteen-Month Survey .................................................................................... 9 1.4.3 Chapter 4 Synopsis: The Impact of Coal Combustion Residual Effluent on Water Resources: A North Carolina Case Study.................................................................................. 9 1.4.4 Chapter 5 Synopsis: Boron and Strontium Isotopic Characterization of Coal Combustion Residuals ............................................................................................................. 10 2. A Survey of the Potential Environmental and Health Impacts in the Immediate Aftermath of the Coal Ash Spill in Kingston, Tennessee ......................................................................... 12 2.1 Introduction ....................................................................................................................... 12 2.2 Analytical Methods............................................................................................................ 13 2.3 Results and Discussion ...................................................................................................... 14 2.3.1 Coal ash and sediments ................................................................................................ 14 2.3.2 Water Contamination.................................................................................................... 17 2.3.3 Potential Environmental Impacts ................................................................................. 19 2.3.4 Potential Health Impacts............................................................................................... 22 vii 3. The Environmental Impacts of the Coal Ash Spill in Kingston, Tennessee: An Eighteen-Month Survey ............................................................................................................................................ 26 3.1 Introduction ....................................................................................................................... 26 3.2 Analytical Methods............................................................................................................ 28 3.3 Results and Discussion ...................................................................................................... 29 3.3.1 Laboratory TVA coal ash leaching............................................................................... 29 3.3.2 Surface Water ............................................................................................................... 32 3.3.3 Sediment Acid Volatile Sulfide [101] .......................................................................... 33 3.3.4 Pore Water .................................................................................................................... 33 3.3.5 The Control of pH, redox state, and ash/water ratio on contaminant mobilization...... 38 3.3.6 Implications for tracing and prediction of CCR contaminants..................................... 41 4. The Impact of Coal Combustion Residual Effluent on Water Resources: A North Carolina Case Study .............................................................................................................................................. 43 4.1 Introduction ....................................................................................................................... 43 4.2 Analytical Methods............................................................................................................ 47 4.3 Results and Discussion ...................................................................................................... 48 5. Boron and Strontium Isotopic Characterization of Coal Combustion Residuals: Validation of New Environmental Tracers .......................................................................................................... 61 5.1 Introduction ....................................................................................................................... 61 5.2 Analytical Methods............................................................................................................ 64 5.2.1 Field Sampling and Leaching Experiments.................................................................. 64 5.2.2 Boron Isotopes.............................................................................................................. 65 5.2.3 Strontium
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