Abstract

A four-season sampling of speciated atmospheric mercury (SAM) was employed in East Asia. Three mercury species including gaseous elemental mercury (GEM), gaseous oxidized mercury (GOM), and particulate mercury (PHg) were measured at three background sites. This study explored the temporal variation, spatial distribution, gas-solid partition, transport routes, and source resolution of SAM. The yearly average concentrations of GEM, GOM, and PHg were 2.76 ± 0.36 ng/m3, 23.14 ± 8.67 pg/m3, and 0.23 ± 0.058 ng/m3. The highest GEM and PHg concentrations occurred at Laoag (northern Philippines) in spring, while that of GOM was observed at Laoag but in summer. The lowest GEM and PHg concentrations always occurred at Dongsha Islands (northern South China Sea) in summer, while that of GOM was also observed at Dongsha Islands but in fall. SAM was partition as showed 92.64–96.72% of total gas-phase mercury (TGM) and 3.28–7.36% of solid phase mercury. Eight clustered transport routes were resolved by a HYSPLIT model with polluted air parcels originating from Central/North China. Routes from Indochina Peninsula and South China showed the highest GEM concentration. Moreover, air parcels transported from West Pacific Ocean and South China Sea (SCS) had the lowest concentration of GEM. High concentrations of SAM in the region were mainly attributed to long-range transport (LRT) from Asian continental outflows (ACOs). We further revealed that GEM was positively correlated to SO2, CO, NOx, and PM2.5, but negatively correlated to O3. GOM was positively correlated to SO2, O3, NOx, and PM2.5, but negatively correlated to CO, While, PHg was positively correlated to SO2, CO, O3, NOx, and PM2.5.

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