Degradation of PAHs during long range transport based on simultaneous measurements at Tuoji Island, China, and at Fukue Island and Cape Hedo, Japan.

We investigated the degradation of polycyclic aromatic hydrocarbons (PAHs) during long-range transport. Aerosols were collected simultaneously at remote sites on Tuoji Island, China; Fukue Island, Japan; and the Cape Hedo Atmosphere and Aerosol Measurement Station (CHAAMS), Okinawa, Japan in April, October, and December from 2012 to 2013. These remote sites were convenient for investigating the degradation of PAHs during long-range transport. PAHs were analyzed via gas chromatography/mass spectrometry. We identified air masses that passed over all sites and combined our measurements with a chemical transport model. We estimated the relative contributions of the PAHs at the three sites by normalizing the PAH concentrations to elemental carbon. Benzo[a]pyrene persisted in 5-16% of samples. The results of this study are consistent with laboratory studies in which secondary organic aerosol (SOA) coatings protected PAHs from degradation by ozone. We detected an inhibition of the degradation PAHs by SOA coatings by collecting PAHs simultaneously at the three sites. To elucidate the major sources of the SOAs, we carried out a positive matrix factorization analysis to identify the major sources of SOA coating, which controls the lifetime of PAHs. In spring and winter, the contribution of vehicle emissions was higher (46%) at Tuoji Island than at CHAAMS (13%). In contrast, the contribution of coal combustion was higher at CHAAMS (59%) than at Tuoji Island (28%). This result implies that during long-range transport, PAHs derived from coal combustion are more slowly degraded than PAHs derived from vehicle emissions. We found that the viscosity of SOA coatings derived from vehicle emissions in China was low, and the corresponding PAHs were rapidly degraded. In contrast, the viscosity of SOA coatings derived from coal combustion was high, and degradation of the corresponding PAHs was relatively slow. These results imply that PAHs derived from coal combustion have long lifetime.