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Free keywords:
Polycyclic aromatic hydrocarbons; Global fate; Long-range transport potential; Gas–particle partitioning; Multicompartmental model
Abstract:
The long-range atmospheric transport (LRT) of polycyclic aromatic hydrocarbons (PAHs) is not fully understood and has hardly been addressed by model studies. By model experiments the LRT of PAH emissions into air from Europe and Russia is studied testing several scenarios of gas–particle partitioning and degradability by reaction with ozone and
the hydroxyl and nitrate radicals for two PAHs, benzo[a]pyrene (BAP) and fluoranthene (FLT). The model used is the atmosphere general circulation model ECHAM5 with a dynamic modal aerosol sub-model, HAM, ozone and sulfur
species chemistry and bidirectional mass exchange on 2D marine (ocean surface mixed layer) and terrestrial surfaces (top soil layer and vegetation surfaces). After 5 years the substances are found to be mostly distributed to the soil compartment (64–97% as the global mean, varying with substance and season), which after 10 years is still filling; 1–5% are found in air and 2–33% in ocean. It is found that the lifetime and vertical distribution of the substances in the atmosphere and the LRT potential are all significantly influenced by the partitioning and degradation scenario. The total environmental burden is higher when sorption to organic matter and black carbon are considered to determine gas–particle partitioning rather than adsorption to the surface of particulate matter. The effect is þ20% for BAP but sevenfold for FLT. Concentrations in
Arctic air are mostly underestimated by the model, which is partly explained by emissions not considered in the simulation. The comparison shows, however, that degradation of the sorbed BAP and FLT molecules should be significantly slower than the respective gaseous molecules and that absorptive partitioning is necessary to explain the LRT potential of FLT.
