Spatial variability and temporal changes of POPs in European background air

Concentration data on POPs in air is necessary to assess the effectiveness of international regulations aiming to reduce the emissions of persistent organic pollutants (POPs) into the environment. POPs in European background air are continuously monitored using active- and passive air sampling techniques at a limited number of atmospheric monitoring stations. As a result of the low spatial resolution of such continuous monitoring, there is limited understanding of the main sources controlling the atmospheric burdens of POPs across Europe. The key objectives of this study were to measure the spatial and temporal variability of concentrations of POPs in background air with a high spatial resolution (n = 101) across 33 countries within Europe, and to use observations and models in concert to assess if the measured concentrations are mainly governed by secondary emissions or continuing primary emissions. Hexachlorobenzene (HCB) was not only the POP detected in highest concentrations (median: 67 pg/m3), but also the only POP that had significantly increased over the last decade. HCB was also the only POP that was positively correlated to latitude. For the other targeted POPs, the highest concentrations were observed in the southern part of Europe, and a declining temporal trend was observed. Spatial differences in temporal changes were observed. For example, γ-HCH (hexachlorocyclohexane) had the largest decrease in the south of Europe, while α-HCH had declined the most in central-east Europe. High occurrence of degradation products of the organochlorine pesticides and isomeric ratios indicated past usage. Model predictions of PCB-153 (2,2’,4,4’,5,5’-hexachlorobiphenyl) by the Global EMEP Multi-media Modelling System suggest that secondary emissions are more important than primary emissions in controlling atmospheric burdens, and that the relative importance of primary emissions are more influential in southern Europe compared to northern Europe. Our study highlights the major advantages of combining high spatial resolution observations with mechanistic modelling approaches to provide insights on the relative importance of primary- and secondary emission sources in Europe. Such knowledge is considered vital for policy makers aiming to assess the potential for further emission reduction strategies of legacy POPs.