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Black Carbon Concentrations, Sources, and Fluxes in the Tropical Atlantic Ocean

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Black Carbon Concentrations, Sources, and Fluxes in the Tropical Atlantic Ocean University of Rhode Island DigitalCommons@URI Open Access Dissertations 2014 BLACK CARBON CONCENTRATIONS, SOURCES, AND FLUXES IN THE TROPICAL ATLANTIC OCEAN Kari Ann Pohl University of Rhode Island, [email protected] Follow this and additional works at: https://digitalcommons.uri.edu/oa_diss Recommended Citation Pohl, Kari Ann, "BLACK CARBON CONCENTRATIONS, SOURCES, AND FLUXES IN THE TROPICAL ATLANTIC OCEAN" (2014). Open Access Dissertations. Paper 278. https://digitalcommons.uri.edu/oa_diss/278 This Dissertation is brought to you for free and open access by DigitalCommons@URI. It has been accepted for inclusion in Open Access Dissertations by an authorized administrator of DigitalCommons@URI. For more information, please contact [email protected]. BLACK CARBON CONCENTRATIONS, SOURCES, AND FLUXES IN THE TROPICAL ATLANTIC OCEAN BY KARI ANN POHL A DISSERTATION SUBMITTED IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY IN OCEANOGRAPHY UNIVERSITY OF RHODE ISLAND 2014 DOCTOR OF PHILOSOPHY DISSERTATION OF KARI ANN POHL APPROVED: Dissertation Committee: Major Professor Rainer Lohmann S. Bradley Moran Dawn Cardace Nasser H. Zawia DEAN OF THE GRADUATE SCHOOL UNIVERSITY OF RHODE ISLAND 2014 ABSTRACT Black carbon (BC) is the highly graphitized byproduct of incomplete combustion that could be a sink for fixed carbon. Little data is currently available for BC concentrations and fluxes to remote marine environments and there are often great discrepancies between model simulations and actual field measurements. This research analyzed BC concentrations in the mixed boundary layer, surface water, and deep pelagic sediments of the Tropical Atlantic Ocean in order to understand the fate and transport of BC to the marine environment. It also aimed to assess the importance of aeolian versus fluvial BC deposition. Black carbon concentrations were elevated in regions directly influenced by fluvial and atmospheric deposition in all environmental matrices compared to regions with minimal terrestrial inputs (such as the Sargasso Sea). Black carbon concentrations and fluxes to deep pelagic sediments were approximately 5 times greater in the Sierra Leone Rise (within an atmospheric emission plume) than the remote South Atlantic (minimal terrestrial inputs). Elevated BC fluxes at the Sierra Leone Rise were most likely due to biomass burning from the African continent, as evidence by biomarkers, enriched stable carbon isotopes, and a modern radiocarbon age. Atmospheric deposition composed 4-28% of the soot-like BC and at least 43% of the total BC in the fluvial region of the Niger Delta, suggesting that atmospheric BC deposition to remote sediments can be significant in areas with elevated biomass burning. Atmospheric BC concentrations were also enhanced within the African biomass burning emission plume. Charcoal composed up to 66% of the BC, suggesting that measurements which only quantify soot-like BC forms may be underestimating this carbonaceous fraction. Additionally, surface mixed layer BC was found to compose an average of 17% of bulk total organic carbon. This implies that terrigenous organic carbon composes a larger fraction of the pelagic organic pool than previously estimated. Overall, BC was detected in all samples regardless of environmental matrix, demonstrating its stability and persistence in the marine environment. Fluvial deposition appeared to be the greatest transport mechanism of BC to the marine environment; however atmospheric transport is quantitatively important and should be included in mass balance estimates of both black carbon and terrigenous organic carbon, especially in areas with significant inputs of biomass burning. ACKNOWLEDGMENTS Funding for this work came from a Nation Science Foundation grant (OCE- 0851044) to Rainer Lohmann. Additional funding for travel came from a Graduate School of Oceanography alumni scholarship. Support for elemental analysis came from a U.S. EPA student grantee contract with Mark Cantwell. First and foremost, I would like to thank my husband Michael St.Laurent for the continued support and encouragement throughout this entire graduate school experience. Without your support, and additional support from my cat Sahara, finishing this project would have been almost impossible. I would also like to express my gratitude and appreciation for the support from my adviser Rainer Lohmann. Rainer has spent countless hours (probably closer to days) working out problems and editing earlier drafts of this work. Without the creative freedom but well-set deadlines Rainer provided, this research would not have become as inter-disciplinary or quantitative. I have truly appreciated the opportunity Rainer has given me, as well as the foundational knowledge to complete my academic and educational goals. I also appreciate the numerous diversions Rainer has allowed me to take, including the outreach opportunities within Rhode Island and the numerous conferences he has funded. I would also like to thank my committee members, Mark Cantwell, S. Bradley Moran, Dawn Cardace, and Tom Boving, for all input, advise, constructive criticism, and flexibility with meeting. The combined knowledge of my committee has been inspirational and extremely helpful for my professional and academic growth. I also would like to acknowledge the captain and crew of the R/V Endeavor for helping to iv keep me sane and fed during the summer of 2010. I also would like to profusely thank Ann McNichol and Mary Laudie (WHOI), Rick McKinney and Julia Sullivan (U.S. EPA), Bertrand Ligouis (University of Tübingen), A.D.A Hanson (Magee Scientific), Pierre Herckes (Arizona State University), Pat Kelley (GSO-URI), and Matthias Zabel (Bremen University). I also appreciate the help and support by my past and present lab mates, Carey Friedman, Pam Luey, Matt Lambert, Victoria Sacks, Lin Zhang, Shifra Yonis, Mohammed Khairy, Dave Adelman, Zoe Ruge, Carrie McDonough, Erin Markham, Caoxin Sun, Torey Hart, Hilary Hamer, and Bridget Murphy, for help with analyses, procedures, instrumentation, and listening to me practice for everything. Lastly, I would like to thank my friends, family, the Boston Bruins and Red Sox organizations, and everyone else who supported me along the way. v PREFACE This dissertation is written and organized in the manuscript format as described by the URI Graduate school guidelines for dissertation preparation. The body of the text is divdided into four sections which correspond to the format of journal articles. The first manuscript (Chapter 2) will be submitted to Global Biogeochemical Cycles with authors K. Pohl, M. Cantwell, M. Zabel, and R. Lohmann. The second manuscript (Chapter 3) is under review in Geophysical Research Letters with the authors K. Pohl and R. Lohmann. The third manuscript (Chapter 4) has been accepted for publication in the journal Atmospheric Chemsitry and Physics with the authors K. Pohl, M. Cantwell, P. Herckes, and R. Lohmann. The fourth manuscript (Chapter 5) has been submitted to the journal Geochimica et Cosmochimica Acta with the authors K. Pohl, M. Cantwell, and R. Lohmann. vi TABLE OF CONTENTS ABSTRACT .................................................................................................................. ii ACKNOWLEDGMENTS .......................................................................................... iv PREFACE .................................................................................................................. vvi TABLE OF CONTENTS ......................................................................................... vvii LIST OF TABLES ...................................................................................................... ix LIST OF FIGURES ................................................................................................... xv CHAPTER 1 ................................................................................................................. 1 INTRODUCTION ................................................................................................ 1 CHAPTER 2 ............................................................................................................... 11 AN ASSESSMENT OF FLUVIAL VERSUS ATMOSPHERIC FLUXES OF BLACK CARBON TO SUBTROPICAL ATLANTIC SEDIMENTS .............. 11 CHAPTER 3 ............................................................................................................... 61 SIGNIFICANT CONCENTRATIONS OF TERRESTRIAL ORGANIC CARBON IN TROPICAL ATLANTIC OCEAN SEDIMENTS ....................... 61 CHAPTER 4 ............................................................................................................... 91 BLACK CARBON CONCENTRATIONS AND SOURCES IN THE MARINE BOUNDARY LAYER OF THE TROPICAL ATLANTIC OCEAN USING FOUR METHODOLOGIES ............................................................................... 91 CHAPTER 5 ............................................................................................................. 139 PARTICULATE BLACK CARBON CONCENTRATIONS IN THE SURFACE MIXED LAYER ACROSS THE SUBTROPICAL ATLANTIC OCEAN ..... 139 CHAPTER 6 ............................................................................................................. 180 vii CONCLUSION ................................................................................................. 180 viii LIST OF TABLES TABLE PAGE Ch. 2, Table 1. Global comparison of black carbon (BC) concentrations and fluxes to marine sediments from selected studies.
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