Distribution and gas-particle partitioning of polycyclic aromatic hydrocarbons over the East China Sea and Yellow Sea in spring: Role of atmospheric transport transition

Abstract

To elucidate the variations in the East Asian monsoon system during seasonal changes and their impacts on continental outflow of polycyclic aromatic hydrocarbons (PAHs), sixteen integrated air samples were collected during a research cruise covering the Yellow Sea (YS) and East China Sea (ECS) in mid-spring of 2017. The concentrations of total suspended particle (TSP), aerosol-phase PAH fractions, ratios of organic to elemental carbon (OC/EC) and gas-particle partitioning of atmospheric PAHs exhibited clear regional differences associated with variations in the monsoon regime. The total concentrations of 16 USEPA priority PAHs (Σ16PAHs) varied from 3.11 to 13.4 ng/m3 throughout the cruise, with medium-to-high molecular weight (MW) PAHs more enriched over the YS and north ECS than the south ECS. Together with the relatively low gaseous PAH fraction over the YS and north ECS (78 ± 4%) relative to the south ECS (95 ± 13%), this result indicates the pattern of regional atmospheric transport. The ratio of organic to elemental carbon varied significantly between the south ECS (lower than 4) and the YS and north ECS (greater than 4), indicating contributions from vehicle emissions and coal combustion or biomass burning, respectively, following different atmospheric input pathways of carbonaceous aerosols, as supported by backward trajectory analysis. Considering the gas-particle partitioning of PAHs, soot adsorption was the main partitioning mechanism in the study region; while high-MW PAHs in the YS and north ECS were influenced by both absorption and adsorption. The Koa absorption model provided better predictions for high-MW PAHs when continental air masses prevailed, despite underestimating the partition coefficients (kp) of low-MW PAHs. Meanwhile, predicted kp for medium MW PAHs was better estimated over the YS and ECS when Ksa was included.