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Perfluoroalkyl substances (PFASs) have become an important class of global environmental contaminants, yet their vertical profile in the marine water column is still less understood, especially for the semi-closed seas. In this study, the contamination level and spatial distribution of 8 PFASs were investigated in both surface and vertical water samples from two semi-closed seas, the Japan Sea and the Mediterranean Sea. Similar levels and compositions of PFASs were found between these two seas. The vertical profile of PFASs in the Mediterranean Sea was variable while that was relatively steady in the Japan Sea, probably due to their different pollution sources. The accumulation rate of PFASs from the East China Sea to the Japan Sea was calculated, for which perfluorooctanesulfonic acid and perfluorooctanoic acid were found to have high accumulation potency in both surface and deep water; most of the investigated PFASs were accumulated in the deep water due to the long residence time while they were more likely to escape to the Pacific Ocean in the surface water. This work aimed (i) to study the distribution of PFASs in both surface and vertical water samples in two semi-closed seas, namely the Japan Sea and for the first time the Mediterranean Sea, (ii) to assess the temporal trend in the Japan Sea, and (iii) to firstly investigate the potential transport of PFASs from the East China Sea and Taiwan Strait in order to estimate the inventory of PFASs in whole water mass in the Japan Sea. Image 1 • A remarkable increase in PFASs levels was found in the Japan Sea from 2005 to 2010. • The inventory of PFASs in whole water mass was firstly assessed in semi-closed sea. • The annual ΣPFASs inflow from the East China Sea to the Japan Sea was around 70.8 t. • The PFASs vertical profile in the Mediterranean Sea implied a few pollution sources. • PFOA predominated in the Japan Sea, the Mediterranean Sea, and the East China Sea. [ABSTRACT FROM AUTHOR]

As typical chemical indicators of the Anthropocene, polycyclic aromatic hydrocarbons (PAHs) and their environmental behavior in urban estuaries can reveal the influence of anthropogenic activities on coastal zones worldwide. In contrast to conventional approaches based on concentration datasets, we provide a compound-specific radiocarbon ( 14 C) perspective to quantitatively evaluate the sources and land‒sea transport of PAHs in an estuarine‒coastal surficial sedimentary system impacted by anthropogenic activities and coastal currents. Compound-specific 14 C of PAHs and their 14 C end-member mixing models showed that 67-73% of fluoranthene and pyrene and 76-80% of five- and six-ring PAHs in the Jiulong River Estuary (JRE, China) originated from fossil fuels (e.g., coal, oil spill, and petroleum-related emissions). In the adjacent Western Taiwan Strait (WTS), the contributions of fossil fuel to these PAH groups were higher at 74-79% and 84-87%, respectively. Furthermore, as a significant biomarker for source allocation of terrigenous organic matter, perylene, a typical five-ring PAH, and its land‒sea transport from the basin through the JRE and finally to the WTS was quantitatively evaluated based on the 14 C transport models. In the JRE, fluvial erosions and anthropogenic emissions affected the 14 C signature of perylene (Δ 14 C perylene , -535 ± 5‰) with contributions of > 38% and < 62%, respectively. From the JRE to the WTS, the decreased Δ 14 C perylene (-735 ± 4‰) could be attributed to the long‒range transport of "ocean current-driven" perylene (-919 ± 53‰) with a contribution of 53 ± 8%. This compound-specific 14 C approach and PAH transport model help provide a valuable reference for accurately quantifying land‒sea transport and burial of organic pollutants in estuarine‒coastal sedimentary systems., Competing Interests: Declaration of Competing Interest The authors declare no competing financial interest., (Copyright © 2021. Published by Elsevier Ltd.)

A simultaneous sampling of atmospheric and seawater samples was performed in the Taiwan Western Strait, western Arctic Ocean, and the Antarctic Ocean. Analysis of both particle and gas phase PFAS in oceanic air was conducted using cascade impactor particle fractionator, cryogenic air sampler and activated charcoal fiber sorbent for the first time with application in the Taiwan Western Strait. Mean concentration of Σ 12 PFAS in surface seawater and atmospheric samples were 1178 pg/L and 24 pg/m 3 in the Taiwan Western Strait, 430 pg/L and 6 pg/m 3 in the western Arctic Ocean, and 456 pg/L and 3 pg/m 3 in the Antarctic Ocean. In oceanic air from the Taiwan Western Strait, fluorotelomer alcohol (FTOH) and the ionic PFAS [perfluoroalkyl sulfonic acid (PFSA) and perfluoroalkyl carboxylic acid (PFCA)] were found in 76% and 7% respectively. Regional comparison of air/water exchange (K AW ) and gas-particle (K p ) partition coefficients of PFAS in the oceanic environment indicated potential partitioning of ionic PFAS between surface seawater and oceanic air. These findings highlight the advancement in atmospheric PFAS measurements through combined novel technologies, namely size-fractionated particle sampling with cryogenic air trapping and/or activated charcoal sorption. Correlation between K p and carbon chain length of PFAS was observed using both hyphenated techniques., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2021 Elsevier Ltd. All rights reserved.)

On the basis of the application of compound-specific radiocarbon analysis (CSRA) and air-water exchange models, the contributions of fossil fuel and biomass burning derived polycyclic aromatic hydrocarbons (PAHs) as well as their air-water transport were elucidated. The results showed that fossil fuel-derived PAHs (an average contribution of 89%) presented the net volatilization process at the air-water interface of the Taiwan Strait in summer. Net volatile fluxes of the dominant fluorene and phenanthrene (>58% of the total PAHs) were 27 ± 2.8 μg m -2 day -1 , significantly higher than the dry deposition fluxes (average 0.43 μg m -2 day -1 ). The Δ 14 C contents of selected PAHs (fluorene, phenanthrene plus anthracene, fluoranthene, and pyrene) determined by CSRA in the dissolved seawater ranged from -997 ± 4‰ to -873 ± 6‰, indicating that 89-100% (95 ± 4%) of PAHs were supplied by fossil fuels. The South China Sea warm current originating from the southwest China in summer (98%) and the Min-Zhe coastal current originating from the north China in winter (97%) input more fossil fuel PAHs than the Jiulong River estuary (90%) and Xiamen harbor water (93%). The more radioactive decayed 14 C of fluoranthene (a 4-ring PAH) than that of phenanthrene and anthracene (3-ring PAHs) represented a greater fossil fuel contribution to the former in dissolved seawater.