Compound class specific 14C analysis of polycyclic aromatic hydrocarbons associated with PM10 and PM1.1 aerosols from residential areas of suburban Tokyo

Compound class specific radiocarbon analysis (CCSRA) was performed for polycyclic aromatic hydrocarbons (PAHs) associated with airborne particulate matter (APM) with diameter < 10 mu m (PM10) and < 1.1 mu m (PM1.1) collected from a residential area of suburban Tokyo, Japan, and seasonal and particle-size radiocarbon variations were investigated. Source diagnostic isomer pair ratios indicated mixed contributions from petroleum combustion and from biomass and coal combustion to the PAHs in APM. The Delta C-14-PAHs in APM, ranging from-787 to-514%, indicated dominance of fossil fuel combustion. The Delta C-14 of 5-6 rings (HMW) PAHs were higher than the 3-4 rings (LMW) species in both PM10 and PM1.1 samples. The Delta C-14 of HMW-PAHs indicated greater biomass-burning contributions in summer than in winter and no apparent particle-size variation. Conversely, the Delta C-14 of LMW species showed a greater contribution from fossil sources in summer and in larger particles ( PM10). This finding could be tentatively attributed to the recondensation of fossil-PAHs vaporized from petroleum sources. A C-14 isotopic mass balance approach estimated that biomass burning contributes 17-45% of the PAH burden in suburban Tokyo, and that the increase in the biomass-PAH accounts for approximately 27% and 22% of winter-time elevation of LMW-and HMW-PAHs, respectively. These are far exceeding what is expected from the emission statistics for CO2 and combusted materials in Japan and emphasizing the importance of biomass-burning as a source of PAHs; which, in turn, demonstrates the utility and the significance of field-based source assessment by using CCSRA for an effective regulation of atmospheric pollution by PAHs.