Seasonal variation of gypsum in aerosol and its effect on the acidity of wet precipitation on the Japan sea side of Japan

Variations of mineral concentrations in aerosols collected weekly for a 1 yr period (from October 1992 to September 1993) on Matsue, Shimane Prefecture, Japan, were investigated by X-ray powder diffraction (XRD) analysis. Major elemental concentrations were measured by energy dispersive X-ray analysis (EDX). Sulfate minerals in aerosol include gypsum, ferricopiapite, metavoltine and glauberite. Gypsum showed two high concentration peaks during spring and early winter, which was consistent with that of clay minerals and quartz. The ratios of gypsum to clay minerals, quartz and calcite, respectively, showed an increase of gypsum in spring. A non-agreement of concentration distribution between calcite and other soil minerals during spring implies a conversion of calcite to gypsum during transport. Individual particle analyses by EDX revealed large amounts of S-rich submicrometer particles coated on the surface of minerals. A sequence favorable to be attached by S constituents was calcite (83%) > clay minerals (68%) > fly ash (55) > quartz and feldspars (36%) The reaction between calcite and simulated acid rain solution with pHs of 3, 4 and 5 showed a formation of gypsum in 12 h, indicating that the conversion of calcite to gypsum is possible in the presence of sulfuric acid or (NH4)2 SO4 aerosols during transport from the Asian continent to the Japan Islands.