Sources Causing Long-Term and Seasonal Changes in Combustion-Derived Particulate Matter in the Urban Air of Sapporo, Japan, from 1990 to 2002

Abstract

Fifty-one samples were collected seasonally to estimate the amounts of total suspended particulate (TSP) in Sapporo, Japan, from 1990 to 2002. The atmospheric concentration of combustion-derived particulate (Pc) was calculated based on the NP method using 1-nitropyrene and pyrene. The atmospheric TSP and Pc concentration ranges were between 31–121 µg m−3 of air (Mean ± standard deviation (SD) = 58.2 ± 20.2 µg m−3) and 31–121 µg m−3 (Mean ± SD = 8.2 ± 6.0 µg m−3), respectively. First-order linear regression equations suggested that the Pc fraction decreased faster than TSP. The highest and lowest Pc concentrations were observed in winter and summer, respectively, whereas the highest and lowest TSP concentrations were observed in spring and winter, respectively. The largest and smallest Pc/TSP concentration ratios were observed in winter (0.324) and summer (0.075), respectively. The seasonal fractions of high-temperature combustion-derived particulate (Ph) in Pc ranged from 0.56 (winter) to 0.75 (summer), suggesting that the contribution of vehicle emissions to Pc was always larger than those of coal and biomass combustion. The sources of long-term and seasonal change in Pc were elucidated by analyzing organic source markers. Atmospheric concentrations of polycyclic aromatic hydrocarbons (PAHs), nitropolycyclic aromatic hydrocarbons (NPAHs) and hopanes showed long-term and seasonal changes similar to those of Pc, although biomarkers of biomass and coal combustion, such as levoglucosan, mannosan, and galactosan were not as strongly correlated. These results suggest that the change in the Pc concentration was mainly affected by vehicle emissions rather than by coal and biomass combustion or secondary pollutant formation. The decrease in the Pc over the study period was mainly a result of the Japanese particulate matter/NOx regulations on vehicle exhaust.