Biomonitoring airborne parent and alkylated three-ring PAHs in the Greater Cologne Conurbation II: regional distribution patterns.

The spatial distribution of an important air pollutant class, three-ring polycyclic aromatic hydrocarbons and their derivatives (PAH-3), has been monitored for the Greater Cologne Conurbation (GCC) using pine needle as passive samplers. The GCC comprises one of the most heavily populated, trafficked, and industrialized regions in Germany. Here, 71 locations covering 3600 km(2) were sampled and, for the first time, isopleths maps constructed to investigate the regional variability in PAH-3 concentration and composition. The highest PAH-3 loads on needles (1000-1500 ng g(-1)) were detected downwind of three lignite fuelled power plants, followed by Cologne City (600-700 ng g(-1)) and smaller towns (400-600 ng g(-1)), whereas rural and forest regions yielded PAH-3 loads of 60-300 ng g(-1). PAH-3 ratios facilitated source reconciliation, with high dibenzothiophene versus retene values indicating lignite combustion and high 9/(9+1)-methylphenanthrene ratios depicting traffic emissions in inner cities. PAH-3 ratios depended on topography and outlined the heavily industrialized Rhine Valley, demonstrating atmospheric dispersal of PAH-3.