Observational Constraints on Air Quality and Greenhouse Gases in the Greater Toronto Area

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Observational Constraints on Air Quality and Greenhouse Gases in the Greater Toronto Area Observational constraints on air quality and greenhouse gases in the Greater Toronto Area by Stephanie C. Pugliese A thesis submitted in conformity with the requirements for the degree of Doctor of Philosophy Graduate Department of Chemistry University of Toronto © Copyright by Stephanie C. Pugliese (2017) Observational constraints on air quality and greenhouse gases in the Greater Toronto Area Stephanie C. Pugliese Doctor of Philosophy Graduate Department of Chemistry University of Toronto 2017 Abstract Urban areas are highly complex environments that are large sources of a variety of atmospheric pollutants. To better understand the spatial and temporal variability of carbon dioxide (CO2) emissions in the GTA, we developed the Southern Ontario CO2 Emissions (SOCE) inventory, a fine resolution inventory based on emissions from seven source sectors for the year 2010. When the SOCE inventory was used in combination with a chemistry transport model, agreement with mixing ratios measured in southern Ontario was strong. We found that contributions from area sources (primarily natural gas combustion) played a dominant role overnight (contributing >80 %) while on-road sources played a significant role during the day (contributing >70 %). 13 When a fine-resolution CO2 inventory is not available, stable carbon isotopes (δ CO2) are often used as tools to source apportion CO2. We combined model output CO2 mixing ratios with GTA- 13 specific δ CO2 signatures of the dominant anthropogenic sources of CO2, determined as part of 13 13 this work, to simulate hourly δ CO2. When the simulated δ CO2 was compared to measurements at the Downsview site, the agreement was generally good. To evaluate the use of Keeling and 13 chemical mass balance (CMB) analyses, we estimated the δ CO2 signature of the local ii enhancement from both model output and measurements and found that it was heavier (~3 per mil) than that calculated by the SOCE inventory. The emission of primary pollutants in urban areas (e.g. nitrogen oxides (NOx) and carbon monoxide (CO)) can also contribute to the production of secondary pollutants such as ozone (O3). Data from a governmental monitoring network in the GTA from 2000-2012 were used to explore the impact of O3 precursors on local O3 levels. Non-linear chemistry and influence of meteorology explained why reductions in precursor levels did not lead to improvements in O3, particularly for 2012. iii Acknowledgments This degree has been such an incredible experience for me. I grew immensely as an individual during these past five years and have learned and achieved more than I ever thought possible. There are numerous people who have given me a great deal of support along the way. The first person I would like to thank is my supervisor, Jennifer Murphy. Jen, you have been such an incredible role model for me, particularly as a young female in chemistry. For the past five years, you have allowed me to take my research in a unique direction, continually challenging me and teaching both inside and outside the walls of the Murphy group. You are an exceptional scientist and mentor, and I am extremely grateful to have had you as my supervisor. I would also like to express my gratitude to Jon Abbatt and James Donaldson, my internal committee members, for following my progress throughout my PhD and offering advice and encouragement along the way. I would like to thank all the members of the Murphy group, past and present, for all their collaboration and good times over the past five years. To all the Murphsters that I have shared an office with, thank you for making every day fun and positive and, of course, full of weird conversations. Thank you to Jeffery Geddes who originally taught me to code in IGOR. Finally, I would like to give a very large thank you specifically to Amy Hrdina and Pegah Baratzadeh, two incredible colleagues who have taught me so much and given me so many reasons to smile over the past few years. I would like to thank the Laboratoire des Sciences du Climat et l’Environnement (LSCE) in Paris, France for facilitating my exchanges. Specifically, I would like to thank my host supervisor Felix Vogel for sparking my interest in isotope chemistry. Felix, you have been an incredible teacher and mentor for the past 3 years, thank you for all that you have taught me. I would like to acknowledge all the various funding sources (NSERC, OGS, QEII-GSST, CGCS, SGS, University of Toronto, and Department of Chemistry) without which, all of the exchanges and conferences would not have been possible. Lastly, I would like to acknowledge the support of my family. To my parents, you have always provided me with every opportunity to follow my academic dreams. Your unconditional support and love has provided me with the drive to push forward these past five years. I cannot truly iv express my gratitude for all that you have done. To my two brothers, our need to compete against each other surely contributed to my pursuit of a PhD – thank you for all the support you have given. Specifically to Anthony, for all of our chats about atmospheric research on the drive into campus and your invaluable help with Octave, I cannot thank you enough. To my grandparents, thank you for always being so proud to have a granddaughter who is a scientist, and continually asking me to explain exactly what I do. To my aunts and uncles and cousins, thank you for all your support and for making every little award and publication a big deal. And finally, to my fiancé Angelo, thank you for being an incredible partner during this crazy period of my life. You have helped me through all the disappointments and accomplishments that come with graduate school. For all your love and support over these past years, I am truly grateful. v Table of Contents Acknowledgments.................................................................................................................... iv Table of ContentsList of Tables ............................................................................................... vi List of Tables ........................................................................................................................... xi List of Figures ......................................................................................................................... xii List of Appendices ................................................................................................................. xvi Chapter 1 Introduction............................................................................................................1 1.1 Introduction to primary and secondary pollutants in urban environments ....................1 1.2 Sources of CO2 in urban environments ..........................................................................2 1.3 Bottom-up estimates of urban emissions .......................................................................3 1.3.1 The EDGAR v4.2 CO2 Inventory ......................................................................4 1.3.2 The FFDAS v2 CO2 Inventory ..........................................................................5 1.3.3 Environment and Climate Change Canada’s CO Inventory ..............................6 1.4 Measurements of CO2 ....................................................................................................8 1.4.1 High precision, low-density measurements .......................................................9 1.4.2 Low precision, high-density measurements .....................................................12 1.4.3 Column measurements .....................................................................................14 1.5 Use of tracers to source apportion CO2........................................................................16 12 13 1.5.1 Stable carbon isotopes, CO2 and CO2 .........................................................16 1.5.2 Combustion products, CO and NOx .................................................................21 1.6 Urban NOx – VOC – O3 chemistry and trends ............................................................22 1.6.1 Urban NOx – VOC – O3 chemistry ..................................................................22 1.6.2 Trends in CO and NOx emissions in Ontario ...................................................22 1.6.3 Role of meteorology and transport ..................................................................23 1.6.4 Observed trends in ground-level O3 concentrations through time ...................25 1.7 Synthesis and Research Objectives ..............................................................................27 vi 1.8 References ....................................................................................................................29 Chapter 2 High-resolution quantification of atmospheric CO2 mixing ratios in the Greater Toronto Area, Canada .......................................................................................42 2.1 Abstract ........................................................................................................................42 2.2 Introduction ..................................................................................................................43 2.3 Methods........................................................................................................................45 2.3.1 Study region .....................................................................................................45 2.3.2 The Southern Ontario Greenhouse Gas Network ............................................46
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