7 research outputs found

    Correction to Alternative and Legacy Perfluoroalkyl Substances: Differences between European and Chinese River/Estuary Systems

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    Correction to Alternative and Legacy Perfluoroalkyl Substances: Differences between European and Chinese River/Estuary System

    Brominated Flame Retardants and Dechlorane Plus in the Marine Atmosphere from Southeast Asia toward Antarctica

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    The occurrence, distribution, and temperature dependence in the marine atmosphere of several alternative brominated flame retardants (BFRs), Dechlorane Plus (DP) and polybrominated diphenyl ethers (PBDEs) were investigated during a sampling cruise from the East Indian Archipelago toward the Indian Ocean and further to the Southern Ocean. Elevated concentrations were observed over the East Indian Archipelago, especially of the non-PBDE BFR hexabromobenzene (HBB) with concentrations up to 26 pg m<sup>–3</sup> which were found to be related to continental air masses from the East Indian Archipelago. Other alternative BFRs pentabromotoulene (PBT), pentabromobenzene (PBBz), and 2,3-dibromopropyl-2,4,6-tribromophenyl ether (DPTE)were elevated, too, with concentrations up to 2.8, 4.3, and 2.3 pg m<sup>–3</sup>, respectively. DP was detected from 0.26 to 11 pg m<sup>–3</sup> and bis-(2-ethylhexyl)-tetrabromophthalate (TBPH) ranged from not detected (nd) to 2.8 pg m<sup>–3</sup>, respectively. PBDEs ranged from nd to 6.6 pg m<sup>–3</sup> (Σ<sub>10</sub>PBDEs) with the highest individual concentrations for BDE-209. The approach of Clausius–Clapeyron (CC) plots indicates that HBB is dominated by long-range atmospheric transport at lower temperatures over the Indian and Southern Ocean, while volatilization processes and additional atmospheric emissions dominate at higher temperatures. In contrast, BDE-28 and -47 are dominated by long-range transport without fresh emissions over the entire cruise transect and temperature range, indicating limited fresh emissions of the meanwhile classic PBDEs

    Organophosphorus Flame Retardants and Plasticizers in Airborne Particles over the Northern Pacific and Indian Ocean toward the Polar Regions: Evidence for Global Occurrence

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    Organophosphorus compounds (OPs) being applied as flame retardants and plasticizers were investigated in airborne particles over the Pacific, Indian, Arctic, and Southern Ocean. Samples taken during two polar expeditions in 2010/11, one from East Asia to the high Arctic (CHINARE 4) and another from East Asia toward the Indian Ocean to the Antarctic (CHINARE 27), were analyzed for three halogenated OPs (tris­(2-chloroethyl) phosphate (TCEP), tris­(2-chloroisopropyl) phosphate (TCPP) and tris­(1,3-dichloro-2-isopropyl) phosphate (TDCP)), four alkylated OPs (tri-<i>n</i>-butyl phosphate (T<i>n</i>BP), tri-<i>iso</i>-butyl phosphate (T<i>i</i>BP), tris­(2-butoxyethyl)­phosphate (TBEP), and tris­(2-ethylhexyl) phosphate (TEHP)), and triphenyl phosphate (TPhP). The sum of the eight investigated OPs ranged from 230 to 2900 pg m<sup>–3</sup> and from 120 to 1700 pg m<sup>–3</sup> during CHINARE 4 and CHINARE 27, respectively. TCEP and TCPP were the predominating compounds, both over the Asian seas as well as in the polar regions, with concentrations from 19 to 2000 pg m<sup>–3</sup> and 22 to 620 pg m<sup>–3</sup>, respectively. Elevated concentrations were observed in proximity to the Asian continent enhanced by continental air masses. They decreased sharply toward the open oceans where they remained relatively stable. This paper shows the first occurrence of OPs over the global oceans proving that they undergo long-range atmospheric transport over the global oceans toward the Arctic and Antarctica

    Spatial Distribution and Seasonal Variation of Organophosphate Esters in Air above the Bohai and Yellow Seas, China

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    Nine organophosphate esters (OPEs) were investigated in air samples collected over the Bohai and Yellow Seas (East Asia) during a research cruise between June 28 and July 13, 2016. These same OPEs were quantified at a research site (North Huangcheng Island, NHI) in the middle of the Bohai Strait from May 16, 2015, to March 21, 2016. The median total OPE (ΣOPE) concentration over the Bohai and Yellow Seas was 280 pg/m<sup>3</sup>. Tris­(1-chloro-2-propyl) (TCPP) was the most abundant OPE, followed by tris­(2-chloroethyl) phosphate (TCEP), tri-iso-butyl phosphate (TiBP), and tri-<i>n</i>-butyl phosphate (TnBP). Particle-bound OPEs accounted for 51 ± 21% of the total OPEs. On NHI, the median ΣOPE concentration was 210 pg/m<sup>3</sup>, and the average particle-bound fraction was 82 ± 17%. For samples collected on NHI, significant negative linear correlations were found between the gaseous OPEs and 1/<i>T</i> (<i>T</i>: temperature (K)) (except TDCP, TPeP, and TCP). Among the 79 investigated samples, significant correlations between the measured OPE gas/particle partitioning coefficients (<i>K</i><sub>p,m</sub>) and subcooled liquid pressure (<i>P</i><sub>L</sub><sup>◦</sup>) (<i>p</i> < 0.05) were found for only 14 samples, suggesting that OPEs have low potential to achieve equilibrium or ascribe to the artificial sampling. The annual dry deposition input of OPEs into the Bohai and Yellow Seas is estimated to be 12 tons/year

    Distribution and Air–Sea Exchange of Current-Use Pesticides (CUPs) from East Asia to the High Arctic Ocean

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    Surface seawater and marine boundary layer air samples were collected on the ice-breaker R/V <i>Xuelong </i> (<i>Snow Dragon</i>) from the East China Sea to the high Arctic (33.23–84.5° N) in July to September 2010 and have been analyzed for six current-use pesticides (CUPs): trifluralin, endosulfan, chlorothalonil, chlorpyrifos, dacthal, and dicofol. In all oceanic air samples, the six CUPs were detected, showing highest level (>100 pg/m<sup>3</sup>) in the Sea of Japan. Gaseous CUPs basically decreased from East Asia (between 36.6 and 45.1° N) toward Bering and Chukchi Seas. The dissolved CUPs in ocean water ranged widely from 2/day) than in the North Pacific (–241 ± 158 pg/m<sup>2</sup>/day). Air–sea gas exchange of chlorpyrifos varied from net volatilizaiton in East Asia (<40° N) to equilibrium or net deposition in the North Pacific and the Arctic

    Occurrence of Perfluoroalkyl Compounds in Surface Waters from the North Pacific to the Arctic Ocean

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    Perfluoroalkyl compounds (PFCs) were determined in 22 surface water samples (39–76°N) and three sea ice core and snow samples (77–87°N) collected from North Pacific to the Arctic Ocean during the fourth Chinese Arctic Expedition in 2010. Geographically, the average concentration of ∑PFC in surface water samples were 560 ± 170 pg L<sup>–1</sup> for the Northwest Pacific Ocean, 500 ± 170 pg L<sup>–1</sup> for the Arctic Ocean, and 340 ± 130 pg L<sup>–1</sup> for the Bering Sea, respectively. The perfluoroalkyl carboxylates (PFCAs) were the dominant PFC class in the water samples, however, the spatial pattern of PFCs varied. The C<sub>5</sub>, C<sub>7</sub> and C<sub>8</sub> PFCAs (i.e., perfluoropentanoate (PFPA), perfluoroheptanoate (PFHpA), and perfluorooctanoate (PFOA)) were the dominant PFCs in the Northwest Pacific Ocean while in the Bering Sea the PFPA dominated. The changing in the pattern and concentrations in Pacific Ocean indicate that the PFCs in surface water were influenced by sources from the East-Asian (such as Japan and China) and North American coast, and dilution effect during their transport to the Arctic. The presence of PFCs in the snow and ice core samples indicates an atmospheric deposition of PFCs in the Arctic. The elevated PFC concentration in the Arctic Ocean shows that the ice melting had an impact on the PFC levels and distribution. In addition, the C<sub>4</sub> and C<sub>5</sub> PFCAs (i.e., perfluorobutanoate (PFBA), PFPA) became the dominant PFCs in the Arctic Ocean indicating that PFBA is a marker for sea ice melting as the source of exposure

    Evidence for High Concentrations and Maternal Transfer of Substituted Diphenylamines in European Eels Analyzed by Two-Dimensional Gas Chromatography–Time-of-Flight Mass Spectrometry and Gas Chromatography–Fourier Transform Ion Cyclotron Resonance Mass Spectrometry

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    Chemical pollution is hypothesized to be one of the factors driving the strong decline of the critically endangered European eel population. Specifically, the impact of contaminants on the quality of spawning eels and subsequent embryo survival and development has been discussed as crucial investigation point. However, so far, only very limited information on potential negative effects of contaminants on the reproduction of eels is available. Through the combination of nontargeted ultrahigh-resolution mass spectrometry and multidimensional gas chromatography, combined with more-conventional targeted analytical approaches and multimedia mass-balance modeling, compounds of particular relevance, and their maternal transfer in artificially matured European eels from the German river Ems have been identified. Substituted diphenylamines were, unexpectedly, found to be the primary organic contaminants in the eel samples, with concentrations in the μg g<sup>–1</sup> wet weight range. Furthermore, it could be shown that these contaminants, as well as polychlorinated biphenyls (PCBs), organochlorine pesticides, and polyaromatic hydrocarbons (PAHs), are not merely stored in lipid rich tissue of eels but maternally transferred into gonads and eggs. The results of this study provide unique information on both the fate and behavior of substituted diphenylamines in the environment as well as their relevance as contaminants in European eels
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