Long range transport of polybrominated diphenyl ethers (PBDEs) and their natural analogues determined through size-resolved aerosols, and levels in Atlantic Ocean fish from Newfoundland coasts

Bautista, Joseph J. (2019) Long range transport of polybrominated diphenyl ethers (PBDEs) and their natural analogues determined through size-resolved aerosols, and levels in Atlantic Ocean fish from Newfoundland coasts. Doctoral (PhD) thesis, Memorial University of Newfoundland.

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Abstract

Conventional flame retardants of polybrominated diphenyl ethers (PBDEs) are harmful endocrine disrupters that may endure in the environment and experience long range transport (LRT) to areas far from their sources. Despite a gradual phasing out of PBDEs as flame retardants by the Stockholm Convention and other legislation, humans and the environment are still exposed. Recently, natural methoxy and hydroxyl analogues of PBDEs, MeO-BDEs and OH-BDEs, have been discovered in marine environments and are seasonally associated with phytoplankton primary production that may determine how they contribute to the general persistent organic pollutant (POP) abundance as environmental toxicants. Aerosol mechanisms may link these marine pools to the atmosphere and to the global biosphere by LRT on aerosols. Consumption of biota contaminated with PBDEs and their natural analogues may act as a pathway for human exposure. The optimization of PBDE and MeO-BDE extraction and analysis is essential to obtain accurate and precise results and improve method efficiency. Approaches to optimize several aspects of PBDE analysis are described here, along with new techniques for aerosol sampling. The efficacy of several novel internal standards for PBDE and MeO-BDE analysis by gas chromatography coupled to mass spectrometry with electron capture negative ionization (GC-ECNI-MS) is assessed. This is achieved through evaluation of standard reference material household dust and Atlantic cod liver with standard addition, internal calibration, and external calibration. A Micro Orifice Uniform Deposition Impactor (MOUDI) instrument collected aerodynamic aerosol samples in the marine boundary layer. We observe MeO-BDEs in atmospheric aerosols for the first time. We present their atmospheric levels and assessed their sources and potential for LRT based on their aerosol size distribution. We also examine PBDE and MeO-BDE levels in fish livers from Atlantic cod (Gadus Morhua) and Greenland halibut/turbot (Scophthalmus maximusfish). These are traditional Newfoundland and Labrador (NL) fishery stocks and are also known to harbor POPs. These fish samples were used to monitor PBDE and MeO-BDE distribution coastal regions of NL.

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