RESUMO
Organic aerosol (OA) is a dominant component of PM2.5, and accurate knowledge of its sources is critical for identification of cost-effective measures to reduce PM2.5. For accurate source apportionment of OA, we conducted field measurements of organic tracers at three sites (one urban, one suburban, and one forest) in the Tokyo Metropolitan Area and numerical simulations of forward and receptor models. We estimated the source contributions of OA by calculating three receptor models (positive matrix factorization, chemical mass balance, and secondary organic aerosol (SOA)-tracer method) using the ambient concentrations, source profiles, and production yields of OA tracers. Sensitivity simulations of the forward model (chemical transport model) for precursor emissions and SOA formation pathways were conducted. Cross-validation between the receptor and forward models demonstrated that biogenic and anthropogenic SOA were better reproduced by the forward model with updated modules for emissions of biogenic volatile organic compounds (VOC) and for SOA formation from biogenic VOC and intermediate-volatility organic compounds than by the default setup. The source contributions estimated by the forward model generally agreed with those of the receptor models for the major OA sources: mobile sources, biomass combustion, biogenic SOA, and anthropogenic SOA. The contributions of anthropogenic SOA, which are the main focus of this study, were estimated by the forward and receptor models to have been between 9 % and 15 % in summer 2019. The observed percent modern carbon data indicate that the amounts of anthropogenic SOA produced during daytime have substantially declined from 2007 to 2019. This trend is consistent with the decreasing trend of anthropogenic VOC, suggesting that reduction of anthropogenic VOC has been effective in reducing anthropogenic SOA in the atmosphere.
RESUMO
Airborne particulate matter, suspected to induce adverse effects on human health, have been one of the most important concerns regarding recent air pollution issues in Japan. To characterize regional and seasonal variations in emission sources of fine airborne particulate matter (d < 2 microm), monthly samples (n = 36 for each site) were collected at urban (Tokyo), suburban (Maebashi), and mountainous (Akagi) sites in Japan from April 2003 to March 2006. Multielement analysis of chemical species (Na, Al, K, Ca, V, Cr, Mn, Fe, Ni, Cu, Zn, As, Sb, and Pb) was performed by inductively coupled plasma-atomic emission spectrometry and inductively coupled plasma-mass spectrometry. The combined source receptor model, which consists of positive matrix factorization and chemical mass balance, determined the contributions of nine emission sources (local and continental soils, road dust, coal and oil combustion, waste incineration, steel industry, brake wear, and diesel exhaust) to the observed elemental concentrations. Large regional differences were identified in the source contributions among the observational sites. Diesel exhaust was identified as the most significant source (70% of identified contributions) at the urban site. Local and continental soils, coal combustion, and diesel exhaust were intricately assigned (20-30% each) to the suburban site. Continental soil was the predominant source (65%) at the mountainous site. Respective significant source contributions dominated the seasonal variations of total elemental concentrations at each site. These results suggest that a better understanding of the regional and seasonal characteristics of impacting emission sources will be important for improving regional environments.
