Role of mineral aerosol as a reactive surface in the global troposphere

Abstract

A global three‐dimensional model of the troposphere is used to simulate the sources, abundances, and sinks of mineral aerosol and the species involved in the photochemical oxidant, nitrogen, and sulfur cycles. Although the calculated heterogeneous removal rates on mineral aerosol are highly uncertain, mainly due to poorly known heterogeneous reaction rates, the reaction of SO 2 on calcium‐rich mineral aerosol is likely to play an important role downwind of arid source regions. This is especially important for regions in Asia, which are important and increasing emitters of sulfur compounds. Our results indicate that the assumption that sulfate aerosol follows an accumulation mode size distribution, is particularly in Asia likely to overestimate the sulfate aerosol climate‐cooling effect. An even larger fraction of gas phase nitric acid may be associated with and neutralized by mineral aerosol. Interactions of N 2 O 5, O 3, and HO 2‐radicals with dust are calculated to affect the photochemical oxidant cycle, causing ozone decreases up to 10% in and nearby the dust source areas. Comparison of these results with limited available measurements indicates that the proposed reactions can indeed take place, although due to a lack of measurements a rigorous evaluation is not possible at this time.