X-ray absorption near-edge structure (XANES) at sulfur K-edge was used to determine the sulfate species present in size-fractionated aerosol particles based on the postedge structure after the main absorption peak in the XANES region. A comparison of the XANES spectra of reference sulfate materials and aerosol samples collected in Tsukuba in Japan clearly showed that (NH4)2SO4 was the main sulfur species in particles with a smaller diameter and CaSO4 x 2H2O (gypsum) was the main sulfur species in particles with a larger diameter. A simulation of the XANES spectra by reference materials allows us to obtain the quantitative mixing ratios of the different sulfate species present in the aerosol samples. The presence of minor sulfur species other than (NH4)2SO4 and gypsum at the surface of mineral aerosols is suggested in our simulations and by a surface-sensitive conversion electron/He-ion yield XANES. In the absence of a contribution from a large dust event, the mole concentration of gypsum in the mineral aerosol fraction (particle diameter > 1 microm) determined by XANES is similar to that of Ca which is determined independently using ion chromatography. This shows that the Ca and sulfate in the mineral aerosols are present only as gypsum. Considering that calcite is the main Ca mineral in the original material arising from an arid and semiarid area in China, it is strongly suggested that gypsum is formed in aerosol during its long-range transportation by a reaction between calcite and sulfate ions.
Calcium species in mineral aerosols collected simultaneously in Aksu (near the Taklimakan Desert), Qingdao (eastern China), and Tsukuba (Japan) during dust and nondust periods were determined using Ca K-edge X-ray absorption near-edge structure (XANES). From the fitting of XANES spectra, it was found that (i) calcite and gypsum were the main Ca species in the aerosol samples, and (ii) the gypsum fraction versus total Ca minerals [Gyp]/[Ca2+]t increased progressively in the order Aksu < Qingdao < Tsukuba. Surface-sensitive XANES in the conversion electron yield mode (CEY) showed that the gypsum is formed selectively at the surface of mineral aerosols for all the samples except for that taken in Aksu during the dust period. The decrease of the [Gyp]/[Ca2+]t ratio with an increase in particle size showed that the neutralization effect proceeds from the particle surface. For the Aksu sample in the dust period, however, (i) the [Gyp]/[Ca2+]t ratios obtained by XANES measured in the fluorescence (FL; regarded as bulk analysis) and CEY modes were similar and (ii) size dependence was not found, showing that neutralization is not important for the sample because of the large supply of mineral aerosol with little neutralization effect in Aksu. It was also found that the pH of the aerosol and the ratio of (NH4)2SO4 to gypsum were positively and negatively correlated with the Ca (or calcite) content, respectively. The speciation of Ca by XANES revealed the neutralization processes of acidic sulfur species by calcite during the long-range transport of mineral aerosols.
In order to elucidate the variation and characterization of dust particles that originate in the arid and semi-arid regions of inland Asia and are transported to Japan, we established a sampling network system in east China and Japan and collected aeolian dust under the Japan-China joint project ''ADEC''. Monitoring of the total suspended particle (TSP) and size-segregated dust concentrations were carried out in Beijing, Qingdao and Hefei in China, and Fukuoka, Nagoya, Tsukuba and Naha in Japan. The seasonal variations showed the general trend that the aerosol concentration was high in spring and low in summer, though it sometimes became high in winter in Qingdao. The aerosol size distribution was
Analytical data for fourteen rare‐earth elements, scandium, yttrium, zirconium and hafnium, received by May 1992, have been compiled on twenty‐six GSJ (Geological Survey of Japan) reference samples. Seventeen of them are ‘Igneous rock series’ and nine are “Sedimentary rock series”. The reported data including personal communication were evaluated under the consideration on analytical methods and geochemical evidences. No significant difference has been observed between the values obtained by the different analytical methods. Based on the selected available data, 1992 compilation values were tabulated.
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