Water-Soluble Ionic Characteristics of Aerosols in the Marine Boundary Layer over the Yellow Sea during the KORUS-AQ Campaign

摘要

Major compositions of water-soluble ionic species in particulate matter less than 10 and 2.5 μm in diameter (PM_(10) and PM_(2.5), respectively) over the Yellow Sea were collected during the Korea-United States Air Quality (KORUS-AQ) campaign in 2016 onboard the research vessel Gisang 1. The secondary ionic species (NH_4~+, nss-SO_4~(2-), and NO_3~-) in PM_(10) and PM_(2.5) accounted for 84% and 89% of the total analyzed species. NH_4~+ was strongly correlated with non-sea salt (nss) SO_4~(2-) (nss-SO_4~(2-)) in PM_(10) and PM_(2.5); NO_3~- was closely correlated with Na~+, Mg~(2+), and nss-Ca~(2+) in PM_(10) and NH_4~+ in PM_(2.5). High mass concentrations of methane sulfonic acid (MSA, CH_3SO_3~-), the main source of natural sulfates over the Yellow Sea, were observed. The concentrations of MSA were found to show an increasing trend over the Yellow Sea in recent years. Biogenic sulfur contributions to the total nss-SO_4~(2-) (MSAss-SO_4~(2-) ratio) over the Yellow Sea ranged from 1.4% to 9.2% in PM_(10) and from 0.68% to 9.5% in PM_(2.5) during the cruise. Thus, biogenic nss-SO_4~(2-) must be included, especially in the spring and early summer seasons, when biological activities are elevated in Northeast Asia. We classified the high aerosol mass concentration cases such as Asian dust and haze cases. In Asian dust cases, the ratio of NO_3~- to nss-SO_4~(2-) in the aerosols showed that mobile (stationary) sources mainly affected PM_(10) (PM_(2.5)). The major chemical species for Asian dust cases over the Yellow sea were CaCO_3, Ca(NO_3)_2, Mg(NO_3)_2, Na(NO_3)_2, and sea salt. In haze cases over the Yellow sea, the contributions from stationary sources are high and the major species were (NH_4)_2SO_4 and NH_4NO_3 in PM_(10) and PM_(2.5), respectively.