Contributions of Long-Range Transported and Locally Emitted Nitrate in Size-Segregated Aerosols in Japan at Kyushu and Okinawa

We observed the size distributions of mass concentration, ionic composition, and trace metal concentration in aerosols collected at an urban site in Kumamoto Prefecture (KM) and a rural site at Cape Hedo in Okinawa Prefecture (HD) between 2012 and 2015. To evaluate the contribution of transboundary nitrate and locally emitted nitrate in the aerosols at Kumamoto, we distinguished between days of transboundary air pollution from East Asia and days of local air pollution on the basis of a threshold for Pb concentration and the ratio Pb (in 0.5 < projected area diameter (Dp) < 1.0 mu m)/Cu (in 2.5 < Dp < 10 mu m). Fine nitrate (particulate NH4NO3) did not arrive at HD from the Asian continent even under long-range transport conditions. Fine nitrate emitted in Kumamoto and its vicinity also was not transported to HD, even in an air mass that passed over KM and reached HD within one day. Almost all fine nitrate was converted to coarse nitrate during transport by dissociation of fine nitrate and adsorption of HNO3 on larger aerosol particles. Transboundary nitrate existed largely in the particle size range of 0.5 < Dp < 10 mu m, and the contribution of transboundary nitrate in the particle size range of 0.1 < Dp < 0.5 mu m was about 20% even under long-range transport conditions. The contribution of transboundary nitrate in particles with Dp < 2.5 mu m at KM was approximately 50%, 50%, and 80% in spring, autumn, and winter, respectively.