期刊
ACS EARTH AND SPACE CHEMISTRY
卷 3, 期 3, 页码 424-431出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsearthspacechem.8b00178
关键词
organosulfates; photochemistry; mineral dust; road dust; methacrolein; secondary organic aerosol
资金
- Faculty of Science at the University of Alberta
- Natural Sciences and Engineering Research Council of Canada (NSERC)
- Canada Foundation for Innovation (CFI)
- Alberta Ministry of Economic Development and Trade
- Department of Chemistry
Although organosulfates (ROSO3-) comprise a significant component of secondary organic aerosol (SOA) mass, their atmospheric formation mechanisms are not fully understood. Here, using methacrolein as a model organosulfate precursor, we present a new, mineral-mediated photochemical pathway for organosulfate formation. First, we describe studies of TiO2-rcatalyzed formation of the atmospherically important organosulfate hydroxyacetone sulfate from methacrolein as a function of illumination time, catalyst loading, sulfate concentration, counterion identity, and methacrolein concentration. Then, we propose a sulfate radical-mediated mechanism for organosulfate formation consistent with these observations. Finally, we show that natural Ti-containing minerals and road dust not only catalyze the formation of comparable amounts of hydroxyacetone sulfate to those formed in the presence of commercial TiO2 but also facilitate the production of additional organosulfate species. These results highlight the complex nature of photochemistry at the surface of natural mineral samples and underscore the need for further study of the role of mineral-organic interactions in atmospheric organosulfate formation.
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