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Volume 18, issue 21 | Copyright
Atmos. Chem. Phys., 18, 16081-16097, 2018
© Author(s) 2018. This work is distributed under
the Creative Commons Attribution 4.0 License.

Research article 08 Nov 2018

Research article | 08 Nov 2018

Drivers of atmospheric deposition of polycyclic aromatic hydrocarbons at European high-altitude sites

Lourdes Arellano1, Pilar Fernández1, Barend L. van Drooge1, Neil L. Rose2, Ulrike Nickus3, Hansjoerg Thies4, Evzen Stuchlík5, Lluís Camarero6, Jordi Catalan7, and Joan O. Grimalt1 Lourdes Arellano et al.
  • 1Institute of Environmental Assessment and Water Research (IDÆA-CSIC), Jordi Girona 18, 08034 Barcelona, Catalonia, Spain
  • 2Environmental Change Research Centre, University College London, Gower Street, London, WC1E 6BT, UK
  • 3Department of Atmospheric and Cryospheric Sciences, University of Innsbruck, Innrain 52, 6020 Innsbruck, Austria
  • 4Institute of Interdisciplinary Mountain Research, Austrian Academy of Sciences, Technikerstrasse 21a, 6020 Innsbruck, Austria
  • 5Biology Centre, Czech Academy of Science, Institute of Hydrobiology, Na Sadkach 7, 37005 Ceske Budejovice, Czech Republic
  • 6Centre for Advanced Studies of Blanes (CEAB-CSIC), Accés a la Cala St. Francesc 14, 17300 Blanes, Catalonia, Spain
  • 7Centre for Ecological Research and Forestry Applications (CREAF), Campus UAB, Edifici C, 08193 Cerdanyola, Catalonia, Spain

Abstract. Polycyclic aromatic hydrocarbons (PAHs) were analysed in bulk atmospheric deposition samples 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. Sample collection was performed monthly in the first three sites and biweekly in Lochnagar. The number of sites, period of study and sampling frequency provide the most comprehensive description of PAH fallout in high mountain areas addressed so far.

The average PAH deposition fluxes in Gossenköllesee, Redon and Lochnagar ranged between 0.8 and 2.1µgm−2month−1, and in Skalnate Pleso it was 9.7µgm−2month−1, showing the influence of substantial inputs from regional emission sources. The deposited distributions of PAHs were dominated by parent phenanthrene, fluoranthene and pyrene, representing 32%–60% of the total. The proportion of phenanthrene, the most abundant compound, was higher at the sites of lower temperature, Gossenköllesee and Skalnate Pleso, showing higher transfer from gas phase to particles of the more volatile PAHs. The sites with lower insolation, e.g. those located at lower altitude, were those with a higher proportion of photooxidable compounds such as benz[a]anthracene.

According to the data analysed, precipitation is the main driver of PAH fallout. However, when rain and snow deposition were low, particle settling also constituted an efficient driver for PAH deposition. Redon and Lochnagar were the two sites receiving the highest amounts of rain and snow and the fallout of PAH fluxes was related to this precipitation. No significant association was observed between long-range backward air trajectories and PAH deposition in Lochnagar, but in Redon PAH fallout at higher precipitation was essentially related to air masses originating from the North Atlantic, which were dominant between November and May (cold season). In these cases, particle-normalised PAH fallout was also associated with higher precipitation as these air masses were concurrent with lower temperatures, which enhanced gas to particle partitioning transfer. In the warm season (June–October), most of the air masses arriving at Redon originated from the south and particle deposition was enhanced as consequence of Saharan inputs. In these cases, particle settling was also a driver of PAH deposition despite the low overall PAH content of the Saharan particles.

In Gossenköllesee, the site receiving lowest precipitation, PAH fallout was also related to particle deposition. The particle-normalised PAH fluxes were significantly negatively correlated to temperature, e.g. for air masses originating from central and eastern Europe, showing a dominant transfer from gas phase to particles at lower temperatures, which enhanced PAH fallout, mainly of the most volatile hydrocarbons.

Comparison of PAH atmospheric deposition and lacustrine sedimentary fluxes showed much higher values in the latter case of 24–100µgm−2yr−1 vs. 120–3000µgm−2yr−1. A strong significant correlation was observed between these two fluxes, which is consistent with a dominant origin related to atmospheric deposition at each site.

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Short summary
Mountain areas are key for studying the impact of diffuse pollution due to human activities on the continental areas. Polycyclic aromatic hydrocarbons (PAHs), human carcinogens with increased levels since the 1950s, are significant constituents of this pollution. We determined PAHs in monthly atmospheric deposition collected in European high mountain areas. The number of sites, period of study and sampling frequency provide the most comprehensive description of PAH fallout at remote sites.
Mountain areas are key for studying the impact of diffuse pollution due to human activities on...