Spatial and vertical variations of perfluoroalkyl acids (PFAAs) in the Bohai and Yellow Seas: Bridging the gap between riverine sources and marine sinks.

Perfluoroalkyl acids (PFAAs) are being increasingly reported as emerging contaminants in riverine and marine settings. This study investigated the contamination level and spatial distribution of 17 PFAAs within the depth profile of the Bohai and Yellow Seas using newly detected sampling data from 49 sites (June 29 to July 14, 2016). Moreover, the riverine flux of 11 selected PFAAs in 33 rivers draining into the Bohai and Yellow Seas was estimated from previous studies (2002-2014) in order to establish the relationship between riverine sources and marine sinks. The results showed that the Bohai and Yellow Seas were commonly contaminated with PFAAs: total concentrations of PFAAs in the surface, middle, and bottom zones ranged from 4.55 to 556 ng L-1, 4.61-575 ng L-1, and 4.94-572 ng L-1, respectively. The predominant compounds were PFOA (0.55-449 ng L-1), PFBA (<LOQ-34.5 ng L-1), and PFPeA (<LOQ-54.3 ng L-1), accounting for 10.1-87.0%, 5.2-59.5%, and 0.6-68.6% of the total PFAAs, respectively. In general, the ∑PFAA concentrations showed a slightly decreasing trend with sampling depth. Contamination was particularly severe in Laizhou Bay, fed by the Xiaoqing River and an industrial park known for PFAA production. The total riverine PFAA mass flux into the Bohai and Yellow Seas was estimated to be 72.2 t y-1, of which 94.8% was carried by the Yangtze and Xiaoqing Rivers. As the concentration of short-chain PFAAs begins to rise in seawater, further studies on the occurrence and fate of short-chain PFAAs with special focus on effective control measures would be very timely, particularly in the Xiaoqing River and Laizhou Bay.