Abstract

Sulfurous gases released by biogenic sources play a key role in the global sulfur cycle. However, the contribution of biogenic sources to sulfate aerosol in the urban atmosphere has received little attention. Emission sources and formation process of sulfate in Guangzhou, a subtropical mega-city in China, were clarified using multiple methods, including isotope tracers and chemical markers. The δ18O of sulfate suggested that secondary sulfate was the dominant component (84 %) of sulfate aerosol, which mainly formed by transition metal ion (TMI) catalyzed oxidation (31 %) and OH radical oxidation (30 %). The factors driving secondary sulfate formation were revealed using a tree boosting model, which suggested that NH3, temperature, and oxidants were the most important factors. The δ34S of sulfate indicated that biogenic sources accounted for annual average of 26.0 % of the sulfate, which increased to 30.4 % in winter monsoon period. Rice straw burning enhanced sulfate formation by promoting the release of reduced sulfur from soil, which is rapidly converted into sulfate under a subtropical urban atmosphere with high concentration of NH3 and oxidants. This study revealed the important influence of rice straw burning on biogenic sulfur emission during the rice harvest, thereby providing insight into the sulfur cycle and regional air pollution.

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