Natural versus anthropogenic inhalable aerosol chemistry of transboundary East Asian atmospheric outflows into western Japan

The eastward transport of aerosols exported from mainland Asia strongly influences air quality in the Japanese archipelago. The bulk of the inhalable particulate matter (PM10) in these intrusions comprises either natural, desert-derived minerals (mostly supermicron silicates) or anthropogenic pollutants (mostly submicron sulphates), in various states of mixing. We analyse PM10 collected in Kumamoto, SW Japan, during three contrasting types of aerosol intrusions, the first being dominated by desert PM which became increasingly mixed with anthropogenic components as time progressed, the second being a relatively minor event mixing fine, distal desert PM with anthropogenic materials, and the third being dominated by anthropogenic pollutants. Whereas the chemistry of the natural mineral component is characterised by crustal elements (Si, Al, Fe, Mg, K, Li, P. Sc, V. Rb, Sr, Zr, Th, lanthanoids), the anthropogenic component is rich in secondary inorganic compounds and more toxic metallic elements (NH4+. SO42-, As, Pb, Cd, Cu, Zn, Sn, Bi, Sb, and Ge). Some desert-dust (Kosa) intrusions are more calcareous than others, implicating geologically different source areas, and contain enhanced levels of NO;, probably as supermicron Ca(NO3)(2) particles produced by chemical reaction between NOx pollutants (mostly from industry and traffic) and carbonate during atmospheric transport. The overall trace element chemistry of aerosol intrusions into Kumamoto shows low V/Rb, low NO3-/SO42-, enhanced As levels, and unfractionated La/Ce values, which are all consistent with anthropogenic sources including coal emissions rather than those derived from the refining and combustion of oil fractionates. Geographically dispersed, residual sulphatic plumes of this nature mix with local traffic (revealed by OC and EC concentrations) and industrial emissions and dissipate only slowly, due to the dominance of submicron accumulation mode PM which is atmospherically persistent, and raise questions over the chronic health effects of breathing finely respirable sulphatic aerosol containing enhanced amounts of toxic metals. (c) 2012 Elsevier B.V. All rights reserved.