Polycyclic aromatic hydrocarbons (PAHs), organochlorine compounds (OCs) and polybromodiphenyl ethers (PBDEs) were analyzed in bulk atmospheric deposition collected at four European high mountain areas, Gossenköllesee (Tyrolean Alps), Redon (Central Pyrenees), Skalnate Pleso (High Tatra Mountains) and Lochnagar (Grampian Mountains) between 2004 and 2006. The samples were collected monthly in the first three sites and biweekly in Lochnagar, providing the most comprehensive fallout description of these compounds in high mountains. The average PAH deposition fluxes were highest in Skalnate Pleso, 9700 ng m-2 mo-1. In Gossenköllesee, Redon and Lochnagar they ranged between 800 and 2100 ng m-2 mo-1. Parent phenanthrene, fluoranthene and pyrene were the dominant compounds (32-60% of total). Polychlorobiphenyls (PCBs) generally showed the highest OC deposition fluxes in the four sites, 112-488 ng m-2 mo-1, and hexachlorobenzene the lowest, a few ng m-2 mo-1. Endosulfans were found at higher deposition fluxes, 11-177 ng m-2 mo-1, than hexachlorocyclohexanes, 17-66 ng m-2 mo-1, in all sites except Lochnagar that was characterized by very low fluxes of this insecticide. The total PBDE fluxes ranged between 100 ng m-2 mo-1 (Alps) and 190 ng m-2 mo-1 (Tatras). These distributions were dominated by BDE209. Significant correlations between PBDE deposition and percent of North Atlantic backwards air mass trajectories were observed in the westernmost sites, Lochnagar and Redon, suggesting a transcontinental transfer of these pollutants from North American sources into Europe. Skalnate and, to a lower extent Redon, also recorded secondary emissions of the pentaBDE mixture from central Europe. A specific PBDE source was observed in United Kingdom and recorded in Lochnagar. Significant correlations between current-use OC pesticides and air masses flowing from the south were observed in Gossenköllesee, Lochnagar and Redon. No relationship between PCB deposition fluxes and air mass trajectories were observed. Photolytic degradation during transport decreased the relative abundance of BDE209 and modified the emitted pentaBDE technical mixtures by depletion of the relative composition of BDE99 and, to a lower extent, BDE47. The transformations were more intense in the sites located above 2000 m, Redon and Gossenköllesee, and particularly during the warm periods. These sites were also those with lowest relative fluxes of photooxidable PAH such as benz[a]anthracene.

Atmospheric deposition of polycyclic aromatic hydrocarbons and organohalogen compounds in high mountain areas of Europe

Macromolecular Chemistry: The Second Century

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