title: Potential role of sea spray generation in the atmospheric transport of perfluorocarboxylic acids.
abstract: The observed environmental concentrations of perfluorooctanoic acid (PFOA) and its conjugate base (PFO) in remote regions such as the Arctic have been primarily ascribed to the atmospheric transport and degradation of fluorotelomer alcohols (FTOHs) and to direct PFO transport in ocean currents. These mechanisms are each capable of only partially explaining observations. Transport within marine aerosols has been proposed and may explain transport over short distances but will contribute little over longer distances. However, PFO(A) has been shown to have a very short half-life in aqueous aerosols and thus sea spray was proposed as a mechanism for the generation of PFOA in the gas phase from PFO in a water body. Using the observed PFO concentrations in oceans of the Northern Hemisphere and estimated spray generation rates, this mechanism is shown to have the potential for contributing large amounts of PFOA to the atmosphere and may therefore contribute significantly to the concentrations observed in remote locations. Specifically, the rate of PFOA release into the gas phase from oceans in the Northern Hemisphere is calculated to be potentially comparable to global stack emissions to the atmosphere. The subsequent potential for atmospheric degradation of PFOA and its global warming potential are considered. Observed isomeric ratios and predicted atmospheric concentrations due to FTOH degradation are used to elucidate the likely relative importance of transport pathways. It is concluded that gas phase PFOA released from oceans may help to explain observed concentrations in remote regions. The model calculations performed in the present study strongly suggest that oceanic aerosol and gas phase field monitoring is of vital importance to obtain a complete understanding of the global dissemination of PFCAs.
authors.affiliation: Centre for Environmental Modelling and Chemistry, Trent University, 1600 West Bank Drive, Peterborough, Ontario K9J 7B8, Canada.
authors.forename: Eva
authors.initials: E
authors.lastname: Webster
authors.forename: David A
authors.initials: DA
authors.lastname: Ellis
mesh_terms: D000336:Aerosols / Q000032:analysis / Q000737:chemistry*; D000392:Air Movements; D001272:Atmosphere / Q000737:chemistry*; D002264:Carboxylic Acids / Q000032:analysis / Q000737:chemistry*; D005466:Fluorocarbons / Q000032:analysis / Q000737:chemistry*; D007700:Kinetics; D008956:Models, Chemical; D012623:Seawater / Q000737:chemistry*; D013227:Steam; D014873:Water Pollutants / Q000032:analysis / Q000737:chemistry*
chemical_list: D000336:Aerosols; D002264:Carboxylic Acids; D005466:Fluorocarbons; D013227:Steam; D014873:Water Pollutants