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Influence of Human Activities, Volcanic Eruptions and Bolide Events Kari Peterson South Dakota State University, [email protected]

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Influence of Human Activities, Volcanic Eruptions and Bolide Events Kari Peterson South Dakota State University, Kari.Peterson@Sdstate.Edu South Dakota State University Open PRAIRIE: Open Public Research Access Institutional Repository and Information Exchange Theses and Dissertations 2016 Perchlorate Variations Over 300 Years: Influence of Human Activities, Volcanic Eruptions and Bolide Events Kari Peterson South Dakota State University, [email protected] Follow this and additional works at: http://openprairie.sdstate.edu/etd Part of the Biogeochemistry Commons, and the Environmental Chemistry Commons Recommended Citation Peterson, Kari, "Perchlorate Variations Over 300 Years: Influence of Human Activities, Volcanic Eruptions and Bolide Events" (2016). Theses and Dissertations. Paper 681. This Thesis - Open Access is brought to you for free and open access by Open PRAIRIE: Open Public Research Access Institutional Repository and Information Exchange. It has been accepted for inclusion in Theses and Dissertations by an authorized administrator of Open PRAIRIE: Open Public Research Access Institutional Repository and Information Exchange. For more information, please contact [email protected]. PERCHLORATE VARIATIONS OVER 300 YEARS: INFLUENCE OF HUMAN ACTIVITIES, VOLCANIC ERUPTIONS, AND BOLIDE EVENTS BY KARI PETERSON A dissertation submitted in partial fulfillment of the requirements for the Doctor of Philosophy Major in Chemistry South Dakota State University 2016 iii ACKNOWLEDGEMENTS There have been many people who have assisted in the completion of this project, and I would like to take a moment to thank these individuals. First, I would like to thank my advisor, Dr. Jihong Cole-Dai, for his support and guidance. Dr. Cole-Dai has provided me with the opportunity to explore new ideas, while still providing insight and clarity when it was needed. He has always challenged me to seek a greater understanding of the ideas and concepts I have studied. Without his support and insight, the completion of this project would not have been possible. I would also like to thank the members of my advisory committee, Dr. James Rice, Dr. Brian Logue, Dr. Douglas Raynie, and Dr. Todd Trooien for their support and guidance. I would like to thank the Campus Core Mass Spectrometry Facility for access to and maintenance of the QTRAP 5500 tandem mass spectrometer. I would like to thank all past and present members of the ICECL lab. So many people have contributed to this project in one way or another, and without their assistance completion of this project would not have been possible. Finally, I would like to thank my family. Their love and support has been invaluable as I have undertook the pursuit of this degree. iv TABLE OF CONTENTS Page ABBREVIATIONS ........................................................................................................... ix LIST OF FIGURES ........................................................................................................... xi LIST OF TABLES ........................................................................................................... xiii ABSTRACT ..................................................................................................................... xiv 1 Introduction ................................................................................................................. 1 1.1 Chemistry of Perchlorate ...................................................................................... 1 1.2 Perchlorate in the Environment ............................................................................ 1 1.3 Sources of Perchlorate .......................................................................................... 2 1.3.1 Anthropogenic Sources ................................................................................. 2 1.3.2 Natural Perchlorate ....................................................................................... 4 1.4 Environmental Stability of Perchlorate ................................................................ 5 1.5 Health Concerns over Perchlorate ........................................................................ 6 1.6 Regulation of Perchlorate ..................................................................................... 7 1.7 Ice Core Records .................................................................................................. 8 1.8 Objectives of Research ......................................................................................... 9 2 Analytical Method Development ............................................................................... 13 2.1 Techniques for Measuring Perchlorate .............................................................. 13 2.2 Overview of IC-ESI-MS/MS ............................................................................. 14 v 2.3 Analytical Figures of Merit ................................................................................ 15 2.3.1 Selectivity ................................................................................................... 15 2.3.2 Limit of Detection and Lower Limit of Quantification .............................. 16 2.3.3 Accuracy and Precision............................................................................... 17 2.3.4 Inter-laboratory Comparison ....................................................................... 18 3 Sample Preparation and Analysis .............................................................................. 20 3.1 Ice Core Collection............................................................................................. 20 3.2 Ion Chromatography Eluent Preparation............................................................ 21 3.3 Calibration .......................................................................................................... 22 3.4 Sample Preparation ............................................................................................ 22 4 Ice Core Dating .......................................................................................................... 25 4.1 Importance .......................................................................................................... 25 4.2 Dating Methods .................................................................................................. 25 4.2.1 Annual Layer Counting............................................................................... 25 4.2.2 Constant Accumulation Method ................................................................. 27 4.3 Dating SM07C2.................................................................................................. 27 4.4 Dating the TUNU and Basin 4 Cores ................................................................. 29 5 Long Term Trends in Perchlorate .............................................................................. 31 5.1 Pre-Industrial Revolution vs. Modern Concentrations ....................................... 31 5.2 Perchlorate Concentrations across the Arctic..................................................... 33 vi 5.3 Possible Anthropogenic Sources ........................................................................ 36 5.3.1 Perchlorate as an Oxidizer .......................................................................... 36 5.3.2 Perchlorate as an Impurity .......................................................................... 39 5.4 Conclusions ........................................................................................................ 41 6 Stratospheric Chlorine ............................................................................................... 43 6.1 Evidence of Stratospheric Production of Perchlorate ........................................ 43 6.2 Overview of Chlorine Chemistry in the Stratosphere ........................................ 43 6.3 Trends in Stratospheric Chlorine and Perchlorate Concentrations .................... 46 6.3.1 Enhanced Chlorine Activation over Antarctica .......................................... 50 6.4 Mechanisms for Stratospheric Perchlorate Production ...................................... 52 6.4.1 Chlorine Activation ..................................................................................... 52 6.4.2 Oxidation..................................................................................................... 54 6.4.2.1 Ozone-Mediated Oxidation …………………………….………………..54 6.4.2.2 Photochemical Oxidation …………………………………………..……62 6.4.3 Hydrolysis ................................................................................................... 64 6.5 Conclusions ........................................................................................................ 64 7 Impact of Volcanic Eruptions .................................................................................... 66 7.1 Identification of Volcanic Eruptions in Ice Cores .............................................. 67 7.2 Elevated Perchlorate Concentrations ................................................................. 68 7.2.1 Correlation between Perchlorate and Sulfate .............................................. 69 vii 7.3 Volcanoes as a Direct Source ............................................................................. 70 7.4 Volcanic Aerosols .............................................................................................. 71 7.5 Possible Explanations for Increased Perchlorate Concentrations ...................... 72 7.5.1 Input of Chlorine to the Stratosphere .......................................................... 73 7.5.2 H2SO4 Aerosols
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