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Polybrominated Diphenyl Ether Flame Retardants

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Polybrominated Diphenyl Ether Flame Retardants POLYBROMINATED DIPHENYL ETHER FLAME RETARDANTS IN THE ANTARCTIC ENVIRONMENT A Dissertation by GILVAN TAKESHI YOGUI Submitted to the Office of Graduate Studies of Texas A&M University in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY August 2008 Major Subject: Oceanography POLYBROMINATED DIPHENYL ETHER FLAME RETARDANTS IN THE ANTARCTIC ENVIRONMENT A Dissertation by GILVAN TAKESHI YOGUI Submitted to the Office of Graduate Studies of Texas A&M University in partial fulfillment of the requirements for the degree of DOCTOR OF PHILOSOPHY Approved by: Co-Chairs of Committee, Jose L. Sericano Mahlon C. Kennicutt, II Committee Members, Terry L. Wade Miguel A. Mora Head of Department, Piers Chapman August 2008 Major Subject: Oceanography iii ABSTRACT Polybrominated Diphenyl Ether Flame Retardants in the Antarctic Environment. (August 2008) Gilvan Takeshi Yogui, B.S., University of Rio Grande Foundation (FURG – Brazil); M.S., University of Sao Paulo (USP – Brazil) Co-Chairs of Advisory Committee: Dr. Jose L. Sericano Dr. Mahlon C. Kennicutt, II Polybrominated diphenyl ethers (PBDEs) are anthropogenic chemicals whose environmental behavior is similar to the well-known polychlorinated biphenyls (PCBs). Few studies have quantified the amount and distribution of PBDEs in the southern hemisphere and Antarctica. The analyses reported in this dissertation document the levels of PBDEs in lichens, mosses and seabird eggs collected at King George Island, Antarctic Peninsula. The analyses were carried out using Gas Chromatography/Electron Impact-Mass Spectrometry (GC/EI-MS). Employing the ion stacking technique lowered detection limits and ensured instrument selectivity and sensitivity to the compounds of interest. Lichens and mosses absorb PBDEs directly from the atmosphere and their contamination indicates that long-range transport is the primary source of these chemicals to King George Island. The congener patterns of PBDEs in plants indicate that commercial mixtures of Penta-BDE and Octa-BDE have reached Antarctica. Differences in the levels of PBDEs observed in lichens and mosses are probably due to factors that iv govern the uptake of PBDEs from the atmosphere. Contamination in lichens showed a positive correlation with local precipitation. Conversely, absorption of PBDEs in mosses appears to be controlled by other plant-specific factors. Marine phytoplankton-derived aerosols are hypothesized to play an important role in the atmospheric transport of PBDEs to the Antarctic environment. PBDEs in south polar skua eggs revealed much higher concentration than in penguin eggs. This is likely associated with the northward migration of these seabirds during the non-breeding season. While penguins reside year-round in Antarctica, south polar skuas migrate northward and can be seen in boreal oceans during the austral winter. Distribution of PBDEs in penguin eggs matches the pattern found in local vegetation suggesting a common source for the chemicals. In contrast, the congener pattern of south polar skuas suggests that birds breeding at King George Island are wintering in the northwestern Pacific Ocean. A potential metabolism of PBDEs in penguin eggs during the incubation period seems to be limited. Most congeners were unaltered from source material in the eggs of chinstrap and gentoo penguins. Low levels of PBDEs, short incubation periods and energy constraints may explain these observations. v DEDICATION To my beloved mother Izilda, father Gilberto and sister Gilvana. vi ACKNOWLEDGEMENTS First of all I thank God for giving me perseverance, peace and health to finish this important step of my professional and academic education. My deepest appreciation goes to my family in Brazil for their infinite and unconditional love, encouragement, support and prayers. I LOVE YOU! I would like to acknowledge my committee co-chairs, Dr. Jose Sericano and Dr. Chuck Kennicutt, and my committee members, Dr. Terry Wade and Dr. Miguel Mora, for their contribution to this dissertation. A special recognition should be given to Dr. Sericano for his support, friendship and guidance throughout this research. I also want to extend my gratitude to CAPES (Ministry of Education, Brazil) for sponsoring the first four years of my studies at Texas A&M University, and to Dr. Wade and Dr. Sericano for giving me the opportunity to work at GERG. These earnings, along with the university International Education Fee Scholarship, were essential to support my fifth year as a graduate student. I greatly appreciate Dr. Rosalinda Montone for the opportunity to participate in the Antarctic expeditions. My two field trips to collect samples in Antarctica were financially supported by the Brazilian Antarctic Program and the College of Geosciences (through the Pipes Endowed Fellowship). Chemical analyses were financially supported by GERG funds. I wish to thank EACF scientists and staff for their friendship during my field trips to Antarctica. Mr. Filipe Victoria and Mr. Adriano Spielmann deserve credit for the vii identification of plant species in this study. Many thanks also go to GERG scientists and staff for making my time at Texas A&M University a great experience. Particular acknowledgment should be paid to the staff of the library electronic document delivery system (aka deliverEdocs). The quality of my research would not be the same without this outstanding library service. Finally, I would like to commend all my teachers and professors with admiration (from my first teacher, Tia Graça, to my last professor, Dr. Sericano). My academic achievements are the product of your brilliant minds that shaped my intellectual skills. Last but not least, a special appreciation is reserved for my Brazilian friends who emotionally supported my 5-year stay in College Station. I would not have made it without that cheerful and warm Brazilian spirit. You are my Aggie family! viii NOMENCLATURE critical value of a statistical test used to reject the null hypothesis ANOVA Analysis of Variance BDE Brominated Diphenyl Ether BFR Brominated Flame Retardant DC Direct Current DDE Dichlorodiphenyldichloroethylene DDT Dichlorodiphenyltrichloroethane df degrees of freedom DMS Dimethylsulfide dw dry weight GC Gas Chromatography (or Gas Chromatograph) GERG Geochemical and Environmental Research Group GPC Gel Permeation Chromatography ECNI Electron Capture Negative Ionization EI Electron Ionization (or Electron Impact) F F-test Statistic H Kruskal-Wallis Test Statistic HBCD Hexabromocyclododecane HCB Hexachlorobenzene HCH Hexachlorocyclohexane ix HPLC High Performance Liquid Chromatography id inner diameter IUPAC International Union of Pure and Applied Chemistry KOA octanol-air partition coefficient KOW octanol-water partition coefficient LOEL Low-Observed-Effect-Level LOQ Limit of Quantification m/z mass-to-charge ratio MDL Method Detection Limit MS Mass Spectrometry (or Mass Spectrometer) MSA Methanesulfonic Acid n number of samples nd not detected NIST National Institute of Standards and Technology NOAA National Oceanic and Atmospheric Administration p level of significance of the statistical test (aka p-value) PBB Polybrominated Biphenyl PBDE Polybrominated Diphenyl Ether PCB Polychlorinated Biphenyl PCDD Polychlorinated Dibenzo-p-dioxin PCDF Polychlorinated Dibenzofuran POP Persistent Organic Pollutant x QA Quality Assurance QC Quality Control r Pearson’s product-moment correlation coefficient rs Spearman’s rank order correlation coefficient RPD Relative Percent Difference SD Standard Deviation SIM Selected Ion Monitoring S/N Signal-to-Noise Ratio SOC Semivolatile Organic Compound SRM Standard Reference Material TEQ 2,3,7,8-tetrachlorodibenzo-p-dioxin Toxic Equivalent TBBPA Tetrabromobisphenol A TIC Total Ion Chromatogram ww wet weight xi TABLE OF CONTENTS Page ABSTRACT.............................................................................................................. iii DEDICATION .......................................................................................................... v ACKNOWLEDGEMENTS ...................................................................................... vi NOMENCLATURE.................................................................................................. viii TABLE OF CONTENTS .......................................................................................... xi LIST OF FIGURES................................................................................................... xiii LIST OF TABLES .................................................................................................... xv CHAPTER I INTRODUCTION AND LITERATURE REVIEW............................ 1 1.1. Brominated flame retardants ................................................. 1 1.2. PBDEs in the environment.................................................... 5 1.3. PBDEs in the U.S. marine environment................................ 7 1.4. PBDEs in Antarctica ............................................................. 27 1.5. Summary ............................................................................... 30 II RATIONALE AND OBJECTIVES..................................................... 34 2.1. Study area.............................................................................. 34 2.2. Transport of POPs to Antarctica ........................................... 36 2.3. Vegetation as pollution monitors .......................................... 37 2.4. Antarctic vegetation .............................................................
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