Occurrence, air-sea exchange, and gas-particle partitioning of atmospheric polybrominated diphenyl ethers from East Asia to the Northwest Pacific Ocean

摘要

The occurrence, air-sea exchange, and gas-particle partitioning of polybrominated diphenyl ethers (PBDEs) were analyzed during a 2015 research expedition from the East China Sea (ECS) to the open Northwest Pacific Ocean (NWP). The sum of 13 PBDEs (Sigma 13PBDEs) in air and surface seawater varied in the range of 0.54-14.5.pg m(-3) and 0.60-13.5 pg L-1, respectively, with the highest concentrations observed in the ECS. The Clausius-Clapeyron approach and air mass origin analysis indicated that continued primary emissions of PBDEs, particularly BDE-209, from East Asian sources governed the spatial variability of air PBDEs over the NWP through long-range atmospheric transport (LRAT). Net air-to-seawater gas deposition of PBDEs was evidenced based on the fugacity calculation with sum fluxes of seven selected PBDEs ranging from -45 to -582 pg m(-2) d(-1). Following the substantial advection of aerosol phase BDE-209 over the ECS, dry particle deposition dominated the input pathway of PBDEs into the ECS, whereas in the open NWP, relatively free from the influence of the land emissions, fluxes in PBDE absorption and in dry particle deposition were comparable. This suggests an impact of continental outflow on the fate of atmospheric PBDEs over the NWP. Regarding gas-particle partitioning, PBDEs over the NWP were obviously absorbed into continental organic aerosols during atmospheric transport, except for BDE-209, which tended to remain within the steady state. (C) 2019 Elsevier Ltd. All rights reserved.