Increasing and decreasing trends of the atmospheric deposition of organochlorine compounds in European remote areas during the last decade

Bulk atmospheric deposition samples were collected between 2004 and 2007 at four high-altitude European sites encompassing east (Skalnate Pleso), west (Lochnagar), central (Gossenkollesee) and south (Redon) regions, and analysed for legacy and current-use organochlorine compounds (OCs). Polychlorobiphenyls (PCBs) generally showed the highest deposition fluxes in the four sites, between 112 and 488 ng m(-2) mo(-1), and hexachlorobenzene (HCB) the lowest, a few ng m(-2) mo(-1). Among pesticides, endosulfans were found at higher deposition fluxes (11-177 ng m(-2) m(-1)) than hexachlorocyclohexanes (HCHs) (17-66 ng m(-2) mo(-1)) in all sites except Lochnagar that was characterized by very low fluxes of this insecticide. Comparison of the present measurements with previous determinations in Redon (1997-1998 and 2001-2002) and Gossenkollesee (1996-1998) provided for the first time an assessment of the long-term temporal trends in OC atmospheric deposition in the European background areas. PCBs showed increasing deposition trends while HCB deposition fluxes remained nearly constant. Re-emission of PCBs from soils or as a consequence of glacier melting and subsequent precipitation and trapping of the volatilized compounds may explain the observed PCB trends. This process does not occur for HCB due to its high volatility which keeps most of this pollutant in the gas phase. A significant decline of pesticide deposition was observed during this studied decade (1996-2006) which is consistent with the restriction in the use of these compounds in most of the European countries. In any case, degassing of HCHs or endosulfans from ice melting to the atmosphere should be limited because of the low Henry's law constants of these compounds that will retain them dissolved in the melted water. Investigation of the relationship between air mass trajectories arriving at each site and OC deposition fluxes showed no correlation for PCBs, which is consistent with diffuse pollution from unspecific sources as the predominant origin of these compounds in these remote sites. In contrast, significant correlations between current-use pesticides and air masses flowing from the south were observed in Gossenkollesee, Lochnagar and Redon. In the case of Redon, the higher proportion of air masses from the south occurred in parallel to higher temperatures, which did not allow us to discriminate between these two determinant factors of pesticide deposition. However, in Gossenkollesee and Lochnagar, the relationship between pesticide concentration and southern air masses was univocal, reflecting the impact of regions with intensive agricultural activities.