Secondary aerosol formation during a special dust transport event: impacts from unusually enhanced ozone and dust backflows over the ocean

Abstract

In the autumn of 2019, a 5 d long-lasting dust event was observed using a synergy of field measurement techniques in Shanghai. This particular dust event stood out from others due to its unique characteristics, including low wind speed, high relative humidity, elevated levels of gaseous precursors, and contrasting wind patterns at different altitudes. During this event, three distinct dust stages were identified. The first stage was a typical dust invasion characterized by high concentrations of particulate matters but relatively short duration. In contrast, the second stage exhibited an unusual enhancement of ozone, attributed to compound causes of a weak synoptic system, transport from the ocean, and subsidence of high-altitude ozone downdrafted by dust. Consequently, gas-phase oxidation served as the major formation pathway of sulfate and nitrate. In the third stage of dust, a noteworthy phenomenon known as dust backflow occurred. The dust plume originated from the Shandong Peninsula and slowly drifted over the Yellow Sea and the East China Sea before eventually returning to Shanghai. Evidence of this backflow was found through the enrichment of marine vessel emissions (V and Ni) and increased solubility of calcium. Under the influence of humid oceanic breezes, the formation of nitrate was dominated by aqueous processing. Additionally, parts of nitrate and sulfate were directly transported via sea salts, evidenced by their co-variation with Na+ and confirmed through thermodynamic modeling. The uptake of NH3 on particles, influenced by the contributions of alkali metal ions and aerosol pH, regulated the formation potential of secondary aerosol. By developing an upstream–receptor relationship method, the quantities of transported and secondarily formed aerosol species were separated. This study highlights that the transport pathway of dust, coupled with environmental conditions, can significantly modify the aerosol properties, especially at the complex land–sea interface.