Gaseous exchange fluxes of organochlorine pesticides (OCPs) across the air-water interface of the coastal East China Sea were determined in order to assess whether the contaminated plume of the Yangtze River could be an important regional source of OCPs to the atmosphere. Hexachlorocyclohexanes (HCHs), chlordane compounds (CHLs), and dichlorodiphenyltrichloroethanes (DDTs) were the most frequently detected OCPs in air and water. Air-water exchange was mainly characterized by net volatilization for all measured OCPs. The net gaseous exchange flux ranged 10-240 ng/(m2·day) for γ-HCH, 60-370 ng/(m2·day) for trans-CHL, 97-410 ng/(m2·day) for cis-CHL, and ∼0 (e.g., equilibrium) to 490 ng/(m2·day) for p,p'-DDE. We found that the plume of the large contaminated river can serve as a significant regional secondary atmospheric source of legacy contaminants released in the catchment. In particular, the sediment plume represented the relevant source of DDT compounds (especially p,p'-DDE) sustaining net degassing when clean air masses from the open ocean reached the plume area. In contrast, a mass balance showed that, for HCHs, contaminated river discharge (water and sediment) plumes were capable of sustaining volatilization throughout the year. These results demonstrate the inconsistencies in the fate of HCHs and DDTs in this large estuarine system with declining primary sources.

§Research Centre for Toxic Compounds in the Environment Masaryk University Brno 62500 Czech Republic

†State Key Laboratory of Environmental Geochemistry Institute of Geochemistry Chinese Academy of Sciences Guiyang 550002 China

‡Shanghai Key Laboratory of Atmospheric Particle Pollution and Prevention Department of Environmental Science and Engineering Fudan University Shanghai 200433 China

∥Norwegian Institute for Water Research Oslo 0349 Norway

⊥Key Laboratory of Coastal Environmental Processes and Ecological Remediation Yantai Institute of Coastal Zone Research Chinese Academy of Sciences Yantai 264003 China

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