A clear north-to-south spatial gradience of chloride in marine aerosol in Chinese seas under the influence of East Asian Winter Monsoon

Particulate chloride is a major component of sea salt particles and plays a key role in atmospheric chemistry. Anthropogenic pollutants over the northeastern Asia can be transported to the adjacent seas through the northwest monsoon, which profoundly influences the chloride chemistry over the seas. In this study, spatial distribution of particulate chloride and its sources over the Chinese seas were investigated based on shipboard particle samplings especially online Single Particle Aerosol Mass Spectrometer (SPAMS) over Bohai Sea, North Yellow Sea, and South Yellow Sea (SYS) during a cruise in November 2012. A strong north-to-south (N-S) gradience in marine aerosol composition was found. The Cl-/Na+ ratios in PM2.5 and single particle composition by SPAMS indicated remarkable chloride enrichment in marine aerosol in the north (Bohai Sea), while depletion in southern SYS. The results of size distribution showed that particulate chloride had higher concentration in coarse particles, while the Cl-/Na+ ratio was much higher in submicron particles. In the north (38-40 degrees N), biomass burning, carbonaceous, and Pb-rich type particles had high fractions in all chloride-containing particles identified by SPAMS (on average 66%). Combining chemical composition with back trajectory, it was found that fine mode chloride enrichment in the north was mainly due to anthropogenic emission especially coal combustion and biomass burning from northern China. However, the high fine-mode chloride depletion in the south (32-34 degrees N) was probably due to acid replacement by sulfate in aged aerosol during atmospheric transport. Our new findings reveal that marine aerosol in Chinese seas would show a clear N-S pattern of more fresh and anthropogenic enriched particles in the north, but more aged aerosol in the south during the East Asia Winter Monsoon, which provides new insights for the quantitative assessment of anthropogenic impact on marine aerosol and future modeling study.