Abstract
A new method is presented for measuring atmospheric contents and δ34S-SO42- in airborne particulate matter using quartz wool disk passive air samplers (Pas-QW). The ability of Pas-QW samplers to provide time-integrated measurements of atmospheric SO42- was confirmed in a field calibration study. The average sampling rate of SO42- measured was 2.3±0.3m3/day, and this was not greatly affected by changes in meteorological parameters. The results of simultaneous sampling campaign showed that the average SO42- contents in Pakistan and the Indochina Peninsula (ICP) were relatively lower than that of China. The spatial distribution of SO42- concentrations was largely attributed to the development of the regional economies. The range of δ34S values observed in Pakistan (4.3±1.4‰) and the ICP (4.5±1.2‰) were relatively small, while a large range of δ34S values was observed in China (3.9±2.5‰). The regional distribution of sulfur isotope compositions was significantly affected by coal combustion. A source analysis based on a Bayesian mixing model showed that 80.4±13.1% and 19.6±13.1% of artificial sulfur dioxide (SO2) sources in China could be attributed to coal combustion and oil combustion, respectively. The two sources differed greatly between regions, and the contribution of oil combustion in cities was higher than previously reported data obtained from emission inventories. This study confirmed that the Pas-QW is a promising tool for simultaneously monitoring atmospheric δ34S-SO42- over large regions, and that the results of the isotope models can provide a reference for the compilation of SO2 emission inventories.
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