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Mercury Stable Isotopes As Tracers in the Environment: Applications to Aquatic and Natural Gas Systems

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Mercury Stable Isotopes As Tracers in the Environment: Applications to Aquatic and Natural Gas Systems Mercury Stable Isotopes as Tracers in the Environment: Applications to Aquatic and Natural Gas Systems by Spencer J. Washburn A dissertation submitted in partial fulfillment of the requirements for the degree of Doctor of Philosophy (Earth and Environmental Sciences) in the University of Michigan 2018 Doctoral Committee: Professor Joel D. Blum, Chair Professor G. Allen Burton Associate Professor Rose M. Cory Professor Kyger C. Lohmann Spencer J. Washburn [email protected] ORCID iD: 0000-0002-6176-8297 © Spencer J. Washburn 2018 Acknowledgements First I would like to thank my wife Kalli for her unwavering support, keen assistance, and timely encouragement over the last five years. I would like to extend my sincere gratitude and many thanks to my advisor, Dr. Joel Blum, for his patience, guidance, and encouragement throughout my entire time at the University of Michigan. His mentorship has been an invaluable part of my PhD experience. I would like to thank all of my co-authors, who have been the source of excellent scientific discourse and support. I would also like to thank my dissertation committee members, who have provided guidance throughout this process. I would like to thank Marcus Johnson, who has been a wonderful source of technical advice and laboratory assistance. I would like to thank the other graduate students who have been members of the BEIGL lab group - Patrick Donovan, Sae Yun Kwon, Laura Motta Medina, and Aaron Kurz - for all of the discussions and friendship over the last 5 years. I would also like to thank the other members of the BEIGL lab group during my tenure, particularly Laura Sherman, Jamie Gleason, and Jason Demers. Lastly, I would like to acknowledge my cat, Tokki, who has borne witness to more poorly prepared practice presentations than anyone else over the last five years. ii Table of Contents Acknowledgements ....................................................................................................................... ii Lists of Tables ................................................................................................................................ v Lists of Figures ............................................................................................................................. vi Abstract ........................................................................................................................................ vii Chapter 1 Introduction ................................................................................................................ 1 1.1 Mercury as a Global Pollutant ........................................................................................................ 1 1.2 Mercury Stable Isotope Fundamentals ........................................................................................... 2 1.3 Applications of Mercury Stable Isotopes: Dissertation Narrative Structure .............................. 4 References ................................................................................................................................................ 7 Chapter 2 Isotopic Characterization of Mercury Downstream of Historic Industrial Contamination in the South River, Virginia ............................................................................ 11 2.1. Introduction .................................................................................................................................... 12 2.2 Materials and Methods ................................................................................................................... 13 2.2.1 Regional Setting ........................................................................................................................ 13 2.2.2 Sample Collection and Processing ............................................................................................ 14 2.2.3 Sample Preparation for Isotope Analysis and THg Concentrations .......................................... 16 2.2.4 Hg Isotope Analysis .................................................................................................................. 16 2.3. Results and Discussion .................................................................................................................. 18 2.3.1 Mercury Concentration and Isotopic Variation in Streambed Sediments and Bank Soils ........ 18 2.3.2 Mercury Concentration and Isotopic Variation in Suspended Particulates and Filtered Surface Water .................................................................................................................................................. 21 2.3.2.1 Patterns of Isotopic Variation and Mercury Concentration in Suspended Particulates and Filtered Surface Water in the Study Reach ..................................................................................................................21 2.3.2.2 Partitioning Between Dissolved and Suspended Hg ..........................................................................23 2.3.2.3 Proposed Mechanism for Observed Fractionation between Suspended and Dissolved Hg ...............24 2.3.3 Connections to the Floodplain ................................................................................................... 27 2.3.4 Identification of Unknown Hg Source Via Hg Endmember Mixing Model ............................. 30 References .............................................................................................................................................. 36 2.4 Supporting Information ................................................................................................................. 40 2.4.1. Unabridged Materials and Methods ........................................................................................ 40 2.4.1.1 Regional Setting .................................................................................................................................40 2.4.1.2 Sample Collection and Processing .....................................................................................................41 2.4.1.3 Sample Preparation for Isotope Analysis and THg Concentrations ...................................................43 2.4.1.4 Hg Isotope Analysis ...........................................................................................................................45 2.4.2. Discussion of ∆199Hg values of Hg in the dissolved load in South River surface water .......... 47 2.4.3. Alternative Explanations for the Isotopic Pattern Observed in Suspended and Dissolved Hg 49 References .......................................................................................................................................... 56 Chapter 3 Spatial and Temporal Variation in the Isotopic Composition of Mercury in the South River, VA .......................................................................................................................... 58 3.1 Introduction ..................................................................................................................................... 59 iii 3.2 Materials and Methods ................................................................................................................... 62 3.2.1 Sample Collection and Processing ............................................................................................ 62 3.2.2 Sample Preparation for Isotope Analysis and THg Concentrations .......................................... 66 3.2.3 Hg Isotope Analysis .................................................................................................................. 68 3.3 Results and Discussion ................................................................................................................... 70 3.3.1 Hg in Bank Soils and Streambed Sediments ............................................................................. 70 3.3.2 Hg in Surface Waters ................................................................................................................ 74 3.3.3 Hg in Channel Margin Hyporheic Zone Porewaters ................................................................. 77 3.3.4 Temporal Variations in Hg Isotope Composition as Observed in a Floodplain Sediment Profile ............................................................................................................................................................ 83 3.3.5 3 End-Member Isotopic Mixing Model ..................................................................................... 85 3.4 Conclusions and Future Work ...................................................................................................... 89 References .......................................................................................................................................... 96 3.5 Supporting Information ............................................................................................................... 102 References ............................................................................................................................................ 115 Chapter 4 Isotopic Characterization of Mercury in Natural Gas via Analysis of Mercury Removal Unit Catalysts ............................................................................................................ 116 4.1 Introduction ................................................................................................................................... 117 4.2 Materials
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