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Atmospheric particulate represents a source of C8–C12 perfluoroalkyl carboxylates and 10:2 fluorotelomer alcohol in tree bark
2021
Zhao, Nan | Zhao, Meirong | Liu, Weiping | Jin, Hangbiao
In this study, we analyzed 30 legacy and emerging poly- and perfluoroalkyl substances (PFASs) in paired atmospheric particulate and bark samples collected around a Chinese fluorochemical manufacturing park (FMP), with the aim to explore the sources of PFASs in tree bark. The results showed that PFASs in atmospheric particulate and tree bark samples were consistently dominated by perfluorooctanoate (mean 73 ng/g; 44 pg/m³), perfluorohexanoate (47 ng/g; 36 pg/m³), perfluorononanoate (9.1 ng/g; 8.8 pg/m³), and 10:2 fluorotelomer alcohol (10:2 FTOH; 5.6 ng/g; 12 pg/m³). Spatially, concentrations of C₈–C₁₂ perfluoroalkyl carboxylates (PFCAs) and 10:2 FTOH all showed a similar and exponentially decreased trend in both bark and atmospheric particulate samples with the increasing distance from the FMP. For the first time, we observed strongly significant (Spearman’s correlation coefficient = 0.53–0.79, p < 0.01) correlations between bark and atmospheric particulate concentrations for C₈–C₁₂ PFCAs and 10:2 FTOH over 1–2 orders of magnitude, suggesting that the continues trapping of atmospheric particulates resulted in the accumulation of these compounds in bark. Overall, this study provides the first evidence that atmospheric particulate is an obvious source of C₈–C₁₂ PFCAs and 10:2 FTOH in tree bark. This result may further contribute to the application of tree bark as an indicator of certain PFASs in atmospheric particulate.
Mostrar más [+] Menos [-]Emerging and legacy per- and polyfluoroalkyl substances in water, sediment, and air of the Bohai Sea and its surrounding rivers
2020
Zhao, Zhen | Cheng, Xianghui | Hua, Xia | Jiang, Bin | Tian, Chongguo | Tang, Jianhui | Li, Qilu | Sun, Hongwen | Lin, Tian | Liao, Yuhong | Zhang, Gan
Per- and polyfluoroalkyl substances (PFASs) contamination in the Bohai Sea and its surrounding rivers has attracted considerable attention in recent years. However, few studies have been conducted regarding the distribution of PFASs in multiple environmental media and their distributions between the suspended particles and dissolved phases. In this study, surface water, surface sediment, and air samples were collected at the Bohai Sea to investigate the concentration and distribution of 39 targeted PFASs. Moreover, river water samples from 35 river estuaries were collected to estimate PFAS discharge fluxes to the Bohai Sea. The results showed that total ionic compound (Σi-PFASs) concentrations ranged from 19.3 to 967 ng/L (mean 125 ± 152 ng/L) in the water and 0.70–4.13 ng/g dw (1.78 ± 0.76 ng/g) in surface sediment of the Bohai Sea, respectively. In the estuaries, Σi-PFAS concentrations were ranged from 10.5 to 13500 ng/L (882 ± 2410 ng/L). In the air, ΣPFAS (Σi-PFASs + Σn-PFASs) concentrations ranged from 199 to 678 pg/m³ (462 ± 166 pg/m³). Perfluorooctanoic acid (PFOA) was the predominant compound in the seawater, sediment, and river water; in the air, 8:2 fluorotelomer alcohol was predominant. Xiaoqing River discharged the largest Σi-PFAS flux to the Bohai Sea, which was estimated as 12,100 kg/y. Some alternatives, i.e., 6:2 fluorotelomer sulfonate acid (6:2 FTSA), hexafluoropropylene oxide dimer acid (HFPO-DA), and chlorinated 6:2 polyfluorinated ether sulfonic acid (Cl-6:2 PFESA), showed higher levels than or comparable concentrations to those of the C8 legacy PFASs in some sampling sites. The particle-derived distribution coefficient in seawater was higher than that in the river water. Using high resolution mass spectrometry, 29 nontarget emerging PFASs were found in 3 river water and 3 seawater samples. Further studies should be conducted to clarify the sources and ecotoxicological effects of these emerging PFASs in the Bohai Sea area.
Mostrar más [+] Menos [-]Photochemical degradation kinetics and mechanism of short-chain chlorinated paraffins in aqueous solution: A case of 1-chlorodecane
2019
Zhang, Wanlan | Gao, Yanpeng | Qin, Yaxin | Wang, Mei | Wu, Junji | Li, Guiying | An, Taicheng
Short chain chlorinated paraffins (SCCPs) have attracted worldwide attention in recent years, due to their high production volume, persistent, bioaccumulative and toxic properties. In this study, 1-chlorodecane (CD) was selected as a model of SCCPs to explore its photochemical degradation behavior under UV irradiation. The results found that CD could be completely photochemical degradation within 120 min, and the •OH was found to be the main reactive species from both quenching experiments and electron paramagnetic resonance (EPR) results. However, the contribution of triple excited state of CD (³CD*) was still nonnegligible from the results with the absorption peak at 480 nm obtained by laser flash photolysis. Based on the identified intermediates as well as the data from theoretical chemical calculation, the detailed photochemical degradation mechanism of CD was tentatively proposed that CD firstly was excited and photo-ionized under UV irradiation, and the released Cl• in water could result in generating •OH. Then •OH initiates CD degradation mainly through the H-abstraction pathway, leading to the generation of several dehydrogenation radicals, which further generated alcohols or long chain intermediates through radical-radical reactions. The results will provide a comprehensive understanding of the degradation mechanism and environmental fates of SCCPs in water under UV irradiation.
Mostrar más [+] Menos [-]Social microbial inocula confer functional stability in a methyl tert-butyl ether extractive membrane biofilm bioreactor
2019
Purswani, Jessica | Guisado, Isabel M. | Coello-Cabezas, Julio | Gonzalez-López, Jesús | Pozo, Clementina
Methyl tert-butyl ether (MTBE) degradation technologies based on two-phase partitioning systems such as extractive membrane biofilm reactors (EMBFR) permit separation of biological and contaminant compartments, thus allowing optimization of the biological section. In this study, we set-up an EMBFR with three MTBE-degrading and cooperating strains (termed social biofilm: Agrobacterium sp. MS2, Paenibacillus etheri SH7ᵀ and Rhodococcus ruber EE6). The removal efficiency of the social-biofilm EMBFR was 80%, and functional stability was observed in the reactor, i.e. more efficient than previous studies (single-strain inoculated EMBFR, <50% removal efficiency and unstable function). Metabolite tert-butyl alcohol was not observed, and the EC₅₀ values were higher than those observed in single-strain EMBFRs. Comparative analysis of the MTBE enzymatic pathway and the social-biofilm was performed, where the mechanism of cooperation observed within the social-biofilm is likely due to enzymatic redundancy. Functional outcomes were equal to previous batch tests, hence 100% scalability was obtained. Overall, higher functional and stability outcomes are obtained with the use of the social-biofilm in an MTBE-EMBFR.
Mostrar más [+] Menos [-]Atmospheric concentrations and trends of poly- and perfluoroalkyl substances (PFAS) and volatile methyl siloxanes (VMS) over 7 years of sampling in the Global Atmospheric Passive Sampling (GAPS) network
2018
Rauert, Cassandra | Shoieb, Mahiba | Schuster, Jasmin K. | Eng, Anita | Harner, Tom
Poly- and per-fluoroalkyl substances (PFAS) and volatile methyl siloxanes (VMS) were monitored at 21 sites in the Global Atmospheric Passive Sampling (GAPS) Network. Atmospheric concentrations previously reported from 2009 were compared to concentrations measured at these sites in 2013 and 2015, to assess trends over 7 years of monitoring. Concentrations of the fluorotelomer alcohols (FTOHs) and fluorinated sulfonamides and sulfonamidoethanols (FOSAs and FOSEs) were stable at these sites from 2009 to 2015 with no significant difference (p > 0.05) in concentrations. Elevated concentrations of all the neutral PFAS were detected at the urban sites as compared to the polar/background sites. The perfluorosulfonic acids (PFSAs), meanwhile, saw a significant increase (p < 0.001) in concentrations from 2009 to 2015. The perfluorocarboxylic acids (PFCAs) had elevated concentrations in 2015, however, the difference was not statistically significant (p > 0.05). Concentrations of the PFSAs and the PFCAs were similar at all location types, showing the global reach of these persistent compounds. Concentrations of the cyclic VMS (cVMS) were at least an order of magnitude higher than the linear VMS (lVMS) and the PFAS. Octamethylcyclotetrasiloxane (D4), decamethylcyclopentasiloxane (D5) and dodecamethylcyclohexasiloxane (D6) saw a weak significant increase in concentrations from 2009 to 2013 (p < 0.05), however, hexamethylcyclotrisiloxane (D3) had a strong significant decrease in concentrations from 2009 to 2015 (p < 0.01).
Mostrar más [+] Menos [-]Associations between residential traffic noise exposure and smoking habits and alcohol consumption–A population-based study
2018
Roswall, Nina | Christensen, Jeppe Schultz | Bidstrup, Pernille Envold | Raaschou-Nielsen, Ole | Jensen, Steen Solvang | Tjønneland, Anne | Sørensen, Mette
Traffic noise stresses and disturbs sleep. It has been associated with various diseases, and has recently also been associated with lifestyle. Hence, the association between traffic noise and disease could partly operate via a pathway of lifestyle habits, including smoking and alcohol intake.We investigated associations between modelled residential traffic noise and smoking habits and alcohol consumption.In a cohort of 57,053 participants, we performed cross-sectional analyses using data from a baseline questionnaire (1993-97), and longitudinal analyses of change between baseline and follow-up (2000-02). Smoking status (never, former, current) and intensity (tobacco, g/day) and alcohol consumption (g/day) was self-reported at baseline and follow-up. Address history from 1987-2002 for all participants were found in national registries, and road traffic and railway noise was modelled 1 and 5 years before enrolment, and from baseline to follow-up. Analyses were performed using logistic and linear regression, and adjusted for demographics, socioeconomic variables, leisure-time sports, and noise from the opposite source (road/railway).Road traffic noise exposure 5 years before baseline was positively associated with alcohol consumption (adjusted difference per 10 dB: 1.38 g/day, 95% confidence interval (CI): 1.10–1.65), smoking intensity (adjusted difference per 10 dB: 0.40 g/day, 95% CI: 0.19–0.61), and odds for being a current vs. never/former smoker at baseline (odds ratio (OR): 1.14; 95% CI: 1.10–1.17). In longitudinal analyses, we found no association between road traffic noise and change in smoking and alcohol habits. Railway noise was not associated with smoking habits and alcohol consumption, neither in cross-sectional nor in longitudinal analyses.The study suggests that long-term exposure to residential road traffic is associated with smoking habits and alcohol consumption, albeit only in cross-sectional, but not in longitudinal analyses.
Mostrar más [+] Menos [-]Neutral and ionic per- and polyfluoroalkyl substances (PFASs) in atmospheric and dry deposition samples over a source region (Tianjin, China)
2016
Yao, Yiming | Chang, Shuai | Sun, Hongwen | Gan, Zhiwei | Hu, Hongwei | Zhao, Yangyang | Zhang, Yufen
Per- and polyfluoroalkyl substances (PFASs) were detected in the atmosphere of a source region in Tianjin, China. Fluorotelomer alcohols (FTOHs) were the dominant neutral PFASs in the atmosphere with total concentrations of 93.6-131 pg/m3 and 8:2 FTOH contributing the most, whereas perfluorooctane sulfonamide derivatives (PFOSAs) were two magnitudes lower or undetected. In comparison, ionic PFASs (perfluoroalkyl carboxyl acids (PFCAs)) in the atmosphere were detected at similar or even higher levels. At wastewater treatment plants (WWTPs), the air over influent was found with higher levels of FTOHs than over aeration tank and effluent; whereas in the air over the aeration tank, the concentrations of PFOSAs and nonvolatile ionic PFASs substantially increased, suggesting a possible direct release of ionic PFASs to the atmosphere besides the atmospheric conversion from volatile precursors. In the air phase, a low proportion (1-5%) of PFCAs was subjected to dry deposition in the source region. Interestingly, the dry-deposition-to-bulk-air ratios of PFCA analogues were the lowest at medium chain lengths (C8 and C9) and increased with either shorter or longer chain length. The extraordinary affinity of shorter-chain PFCAs (C6-C7) to particles was presumed to be due to their smaller molecular size favoring the interactions between the carboxyl head groups and specific sorption sites on particulate matter.
Mostrar más [+] Menos [-]Measurements of major VOCs released into the closed cabin environment of different automobiles under various engine and ventilation scenarios
2016
Kim, Ki Hyun | Szulejko, Jan E. | Jo, Hyo-Jae | Lee, Min-Hee | Kim, Yong-Hyun | Kwon, Eilhann | Ma, Chang-Jin | Kumar, Pawan
Volatile organic compounds (VOCs) in automobile cabins were measured quantitatively to describe their emission characteristics in relation to various idling scenarios using three used automobiles (compact, intermediate sedan, and large sedan) under three different idling conditions ([1] cold engine off and ventilation off, [2] exterior air ventilation with idling warm engine, and [3] internal air recirculation with idling warm engine). The ambient air outside the vehicle was also analyzed as a reference. A total of 24 VOCs (with six functional groups) were selected as target compounds. Accordingly, the concentration of 24 VOC quantified as key target compounds averaged 4.58 ± 3.62 ppb (range: 0.05 (isobutyl alcohol) ∼ 38.2 ppb (formaldehyde)). Moreover, if their concentrations are compared between different automobile operational modes: the ‘idling engine’ levels (5.24 ± 4.07) was 1.3–5 times higher than the ‘engine off’ levels (4.09 ± 3.23) across all 3 automobile classes. In summary, automobile in-cabin VOC emissions are highly contingent on changes in engine and ventilation modes.
Mostrar más [+] Menos [-]Seasonal variation and source estimation of organic compounds in urban aerosol of Augsburg, Germany
2011
Pietrogrande, Maria Chiara | Abbaszade, Gülcin | Schnelle-Kreis, Jürgen | Bacco, Dimitri | Mercuriali, Mattia | Zimmermann, Ralf
This study reports a general assessment of the organic composition of the PM₂.₅ samples collected in the city of Augsburg, Germany in a summer (August–September 2007) and a winter (February–March 2008) campaign of 36 and 30 days, respectively. The samples were directly submitted to in-situ derivatisation thermal desorption gas chromatography coupled with time of flight mass spectrometry (IDTD–GC–TOFMS) to simultaneously determine the concentrations of many classes of molecular markers, such as n-alkanes, iso- and anteiso-alkanes, polycyclic aromatic hydrocarbons (PAHs), oxidized PAHs, n-alkanoic acids, alcohols, saccharides and others. The PCA analysis of the data identified the contributions of three emission sources, i.e., combustion sources, including fossil fuel emissions and biomass burning, vegetative detritus, and oxidized PAHs. The PM chemical composition shows seasonal trend: winter is characterized by high contribution of petroleum/wood combustion while the vegetative component and atmospheric photochemical reactions are predominant in the hot season.
Mostrar más [+] Menos [-]Perfluorochemicals in wastewater treatment plants and sediments in Hong Kong
2010
Ma, Ruowei | Shih, Kaimin
The study reported in this paper examined the concentrations of nineteen perfluorochemicals (PFCs), including perfluoroalkyl sulfonates, carboxylates, and sulfonamides in samples collected from Hong Kong wastewater treatment plants (WWTPs) and sediments. The study was the first to use an external isolator column to assist in the quantification of PFCs in environmental samples without having to make internal modifications to a liquid chromatography system. Perfluorooctanesulfonate was found to be the dominant PFC pollutant in Hong Kong, and the WWTP sludge was the major sink of PFCs discharged from the urban areas. Compared to discharge influenced by industrial activities, much less perfluorooctanoate was found in waste streams. The significantly lower level of perfluorodecanesulfonate in WWTP sludge reflects the important influence of consumer products on PFC distribution. The dominance of even-chain length perfluoroalkyl carboxylates in all of the WWTP sludge samples investigated further suggests the strong aerobic degradation of fluorotelomer alcohols in WWTPs.
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