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Air-sea exchange of gaseous mercury in the East China Sea
2016
Wang, Chunjie | Ci, Zhijia | Wang, Zhangwei | Zhang, Xiaoshan
Two oceanographic cruises were carried out in the East China Sea (ECS) during the summer and fall of 2013. The main objectives of this study are to identify the spatial-temporal distributions of gaseous elemental mercury (GEM) in air and dissolved gaseous mercury (DGM) in surface seawater, and then to estimate the Hg0 flux. The GEM concentration was lower in summer (1.61 ± 0.32 ng m−3) than in fall (2.20 ± 0.58 ng m−3). The back-trajectory analysis revealed that the air masses with high GEM levels during fall largely originated from the land, while the air masses with low GEM levels during summer primarily originated from ocean. The spatial distribution patterns of total Hg (THg), fluorescence, and turbidity were consistent with the pattern of DGM with high levels in the nearshore area and low levels in the open sea. Additionally, the levels of percentage of DGM to THg (%DGM) were higher in the open sea than in the nearshore area, which was consistent with the previous studies. The THg concentration in fall was higher (1.47 ± 0.51 ng l−1) than those of other open oceans. The DGM concentration (60.1 ± 17.6 pg l−1) and Hg0 flux (4.6 ± 3.6 ng m−2 h−1) in summer were higher than those in fall (DGM: 49.6 ± 12.5 pg l−1 and Hg0 flux: 3.6 ± 2.8 ng m−2 h−1). The emission flux of Hg0 from the ECS was estimated to be 27.6 tons yr−1, accounting for ∼0.98% of the global Hg oceanic evasion though the ECS only accounts for ∼0.21% of global ocean area, indicating that the ECS plays an important role in the oceanic Hg cycle.
Показать больше [+] Меньше [-]Characterization and source apportionment of PM2.5-bound polycyclic aromatic hydrocarbons from Shanghai city, China
2016
Wang, Qing | Liu, Min | Yu, Yingpeng | Li, Ye
Polycyclic aromatic hydrocarbons (PAHs) were studied in 230 daily fine particulate matter (PM2.5) samples collected in four seasons at urban and suburban sites of Shanghai, China. This study focused on the emission sources of PAHs and its dynamic results under different weather conditions and pollution levels and also emphasized on the spatial sources of PM2.5 and PAHs at a regional level. Annual concentrations of PM2.5 and 16 EPA priority PAHs were 53 μg/m3 and 6.9 ng/m3, respectively, with highest levels in winter. Positive matrix factorization (PMF) modeling identified four sources of PAHs: coal combustion, traffic, volatilization and biomass combustion, and coking, with contributions of 34.9%, 27.5%, 21.1% and 16.5%, respectively. The contribution of traffic, a local-indicative source, increased from 17.4% to 28.7% when wind speed changed from >2m/s to <2m/s, and increased from 18.3% to 31.3% when daily PAH concentrations changed from below to above the annual mean values. This indicated that local sources may have larger contributions under stagnant weather when poorer dispersion conditions and lower wind speed led to the accumulation of local-emitted pollutants. The trajectory clustering and potential source contribution function (PSCF) and concentration weighted trajectory (CWT) models showed clearly that air parcels moved from west had highest concentrations of PM2.5, total PAHs and high molecular weight (HMW) PAHs. While small differences were found among all five clusters in low molecular weight (LMW) PAHs. Sector analyses determined that regional transport source contributed 39.8% to annual PM2.5 and 52.5% to PAHs, mainly from western regions and varying with seasons. This work may make contribution to a better understanding and control of the increasingly severe air pollution in China as well as other developing Asian countries.
Показать больше [+] Меньше [-]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.
Показать больше [+] Меньше [-]Spatial distribution, transport dynamics, and health risks of endosulfan at a contaminated site
2016
Fang, Yanyan | Nie, Zhiqiang | Die, Qingqi | Tian, Yajun | Liu, Feng | He, Jie | Huang, Qifei
We analyzed concentrations, distribution characteristics, and health risks of endosulfan (α and β isomers, and endosulfan sulfate) in soils (top soils and soil profiles) and air, at and around a typical endosulfan production site in Jiangsu, China. The air–soil surface exchange flux is calculated to investigate transport dynamics of endosulfan. Concentrations at the production site ranged from 0.01 to 114 mg/kg d.w. in soil and 4.81–289 ng/m3 in air, with very high concentrations occurring at the location of endosulfan emulsion workshop. In the surrounding area, endosulfan was detected in all samples, with concentrations ranging from 1.37–415 ng/g d.w. in soil and 0.89–10.4 ng/m3 in air. In the contaminated site, endosulfan concentrations fluctuated with depth in the upper soil layers, then decreased below 120 cm. Soil and air within a distance of 2.0 km appear to be affected by endosulfan originating from the site. Even the health risk at the location of the endosulfan emulsifiable solution workshop was over seven times the acceptable value, the risk to nearby adults and children was low.
Показать больше [+] Меньше [-]Fine particulate matter (PM2.5) in Edmonton, Canada: Source apportionment and potential risk for human health
2016
Bari, Md Aynul | Kindzierski, Warren B.
To design effective PM2.5 control strategies in urban centers, there is a need to better understand local and remote sources influencing PM2.5 levels and associated risk to public health. An investigation of PM2.5 levels, sources and potential human health risk associated with trace elements in the PM2.5 was undertaken in Edmonton over a 6-year period (September 2009–August 2015). The geometric mean PM2.5 concentration of was 7.11 μg/m3 (interquartile range, IQR = 4.83–10.08 μg/m3). Positive matrix factorization (PMF) receptor modeling identified secondary organic aerosol (SOA) as the major contributor (2.2 μg/m3, 27%), followed by secondary nitrate (1.3 μg/m3, 17%) and secondary sulfate (1.2 μg/m3, 15%). Other local sources included transportation (1.1 μg/m3, 14%) and industry-related emissions (0.26 μg/m3, 3.4%), biomass burning (1.0 μg/m3, 13%) and soil (0.54 μg/m3, 6.8%). Five factors (i.e., SOA, secondary nitrate, secondary sulfate, transportation and biomass burning) contributed more than 85% to PM2.5 for the 2009–2015 period. Geometric (arithmetic) mean and maximum ambient air concentrations for hazardous trace elements of public health concern in PM2.5 during the study period were below United States regulatory agency chronic and acute health risk screening criteria. Carcinogenic and non-carcinogenic risk of trace elements and source-specific risk values were well below acceptable and safe levels of risks recommended by regulatory agencies. More work is needed to understand the origin of potential SOA and wintertime wood burning sources in Edmonton and the surrounding region and to apply source-risk apportionment using all available hazardous air pollutants (HAPs) including organic compounds to better interpret the potential health risk posed by various sources in urban areas.
Показать больше [+] Меньше [-]Assessment of polycyclic aromatic hydrocarbons in indoor and outdoor air of preschool environments (3–5 years old children)
2016
Oliveira, Marta | Slezakova, Klara | Delerue-Matos, Cristina | Pereira, Maria do Carmo | Morais, Simone
This work characterizes levels of polycyclic aromatic hydrocarbons (PAHs) in indoor and outdoor air of preschool environments, and assesses the respective risks for 3–5-years old children. Eighteen gaseous and particulate (PM1 and PM2.5) PAHs were collected indoors and outdoors during 63 days at preschools in Portugal. Gaseous PAHs accounted for 94–98% of total concentration (ΣPAHs). PAHs with 5–6 rings were predominantly found in PM1 (54–74% particulate ΣPAHs). Lighter PAHs originated mainly from indoor sources whereas congeners with 4–6 rings resulted mostly from outdoor emissions penetration (motor vehicle, fuel burning). Total cancer risks of children were negligible according to USEPA, but exceeded (8–13 times) WHO health-based guideline. Carcinogenic risks due to indoor exposure were higher than for outdoors (4–18 times).
Показать больше [+] Меньше [-]In situ determination of multiple polycyclic aromatic hydrocarbons uptake by crop leaf surfaces using multi-way models
2016
Sun, Haifeng | Guo, Shuai | Zhu, Na | Sang, Nan | Chen, Zhang
Polycyclic aromatic hydrocarbons (PAHs) in the atmosphere can partition into agricultural crops, which poses a potential risk to human health through the food chain. In this study, controlled chamber experiments were conducted to investigate the kinetic uptake of anthracene (Ant), phenanthrene (Phe), fluoranthene (Fla) and pyrene (Pyr), individually or as a mixture, by the leaf surfaces of living soybean and corn seedlings using the excitation-emission matrix (EEM) coupled with three-way parallel factor analysis (PARAFAC) and n-way partial least squares (n-PLS). The four selected PAHs achieved equilibrium between the air and the two living crop leaf surfaces over the 15-day monitoring period. Inter-species and inter-chemical variability existed in terms of the time required to achieve equilibrium, mass transfer coefficients (kAL) and the equilibrated adsorption capacity (EAC), which was mainly attributed to the different lg KOA values among the four PAHs and the variable leaf-wax content between the soybean and corn species. Compared with when the PAHs existed singly, the time required to achieve adsorption equilibrium was longer while the EAC was reduced for each of the four PAHs in a mixture, which was attributed to competitive adsorption among the coexisting components. These findings prove that the novel analytical method provides a novel platform for the in situ characterization of the environmental behaviors of multiple PAHs, with their spectra overlapping, between the air and plant skin. The coexistence of multiple PAHs in the air inhibits their individual uptake capacity by crop leaf skin, but increases the total adsorption of PAHs, potentially reducing crop security and increasing human health risk via the terrestrial food web.
Показать больше [+] Меньше [-]Differential responses of healthy and chronic obstructive pulmonary diseased human bronchial epithelial cells repeatedly exposed to air pollution-derived PM4
2016
Leclercq, B. | Happillon, M. | Antherieu, S. | Hardy, E.M. | Alleman, L.Y. | Grova, N. | Perdrix, E. | Appenzeller, B.M. | Lo Guidice, J.-M. | Coddeville, P. | Garçon, G.
While the knowledge of the underlying mechanisms by which air pollution-derived particulate matter (PM) exerts its harmful health effects is still incomplete, detailed in vitro studies are highly needed. With the aim of getting closer to the human in vivo conditions and better integrating a number of factors related to pre-existing chronic pulmonary inflammatory, we sought to develop primary cultures of normal human bronchial epithelial (NHBE) cells and chronic obstructive pulmonary disease (COPD)-diseased human bronchial epithelial (DHBE) cells, grown at the air-liquid interface. Pan-cytokeratin and MUC5AC immunostaining confirmed the specific cell-types of both these healthy and diseased cell models and showed they are closed to human bronchial epithelia. Thereafter, healthy and diseased cells were repeatedly exposed to air pollution-derived PM4 at the non-cytotoxic concentration of 5 μg/cm2. The differences between the oxidative and inflammatory states in non-exposed NHBE and COPD-DHBE cells indicated that diseased cells conserved their specific physiopathological characteristics. Increases in both oxidative damage and cytokine secretion were reported in repeatedly exposed NHBE cells and particularly in COPD-DHBE cells. Diseased cells repeatedly exposed had lower capacities to metabolize the organic chemicals-coated onto the air-pollution-derived PM4, such as benzo[a]pyrene (B[a]P), but showed higher sensibility to the formation of OH-B[a]P DNA adducts, because their diseased state possibly affected their defenses. Differential profiles of epigenetic hallmarks (i.e., global DNA hypomethylation, P16 promoter hypermethylation, telomere length shortening, telomerase activation, and histone H3 modifications) occurred in repeatedly exposed NHBE and particularly in COPD-DHBE cells. Taken together, these results closely supported the highest responsiveness of COPD-DHBE cells to a repeated exposure to air pollution-derived PM4. The use of these innovative in vitro exposure systems such as NHBE and COPD-DHBE cells could therefore be consider as a very useful and powerful promising tool in the field of the respiratory toxicology, taking into account sensitive individuals.
Показать больше [+] Меньше [-]Levels, sources and chemical fate of persistent organic pollutants in the atmosphere and snow along the western Antarctic Peninsula
2016
Khairy, Mohammed A. | Luek, Jenna L. | Dickhut, Rebecca | Lohmann, Rainer
The Antarctic continent is among the most pristine regions; yet various organic contaminants have been measured there routinely. Air and snow samples were collected during the austral spring (October–November, 2010) along the western Antarctic Peninsula and analyzed for organochlorine pesticides (OCPs), polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers (PBDEs) to assess the relative importance of long-range transport versus local primary or secondary emissions. Highest concentrations of PCBs, PBDEs and DDTs were observed in the glacier’s snow sample, highlighting the importance of melting glaciers as a possible secondary source of legacy pollutants to the Antarctic. In the atmosphere, contaminants were mainly found in the vapor phase (>65%). Hexachlorobenzene (33.6 pg/m3), PCBs (11.6 pg/m3), heptachlor (5.64 pg/m3), PBDEs (4.22 pg/m3) and cis-chlordane (2.43 pg/m3) were the most abundant contaminants. In contrast to other compounds, PBDEs seem to have originated from local sources, possibly the research station itself. Gas-particle partitioning for analytes were better predicted using the adsorption partitioning model than an octanol-based absorption approach. Diffusive flux calculations indicated that net deposition is the dominant pathway for PBDEs and chlordanes, whereas re-volatilization from snow (during melting or metamorphosis) was observed for PCBs and some OCPs.
Показать больше [+] Меньше [-]Characterization and source apportionment of volatile organic compounds based on 1-year of observational data in Tianjin, China
2016
Liu, Baoshuang | Liang, Danni | Yang, Jiamei | Dai, Qili | Bi, Xiaohui | Feng, Yinchang | Yuan, Jie | Xiao, Zhimei | Zhang, Yufen | Xu, Hong
From November 2014 to October 2015, the concentrations of volatile organic compounds (VOCs), O3 and NOx were simultaneously monitored by using online instruments at the air monitoring station belonged to Tianjin Environmental Protection Bureau (TEPB). The results indicated that VOCs concentrations were higher in autumn and lower in spring, while O3 concentrations were higher in summer, and lower in winter. The diurnal variations of VOCs and NOx (NO2 plus NO) showed opposite tendency comparing to that of O3. The concentrations of alkanes were higher (the average of 18.2 ppbv) than that of aromatics (5.3 ppbv) and alkenes (5.2 ppbv), however, the alkenes and aromatics made larger contributions to ozone because of their high reactivity. Tianjin belonged to the VOC-limited region during most of seasons (except summer) according to the VOC/NOx ratios (the 8:1 threshold). The automobile exhaust, industrial emission, liquefied petroleum gas/natural gas (LPG/NG), combustion, gasoline evaporation, internal combustion engine emission and solvent usage were identified as major sources of VOCs by Positive Matrix Factorization (PMF) model in Tianjin, and the contributions to VOCs for the entire year were 23.1%, 19.9%, 18.6%, 10.6%, 8.7%, 5.4% and 4.7%, respectively. The conditional probability function (CPF) analysis indicated that the contributing directions of automobile exhaust and industrial emission were mainly affected by source distributions, and that of other sources might be mainly affected by wind direction. The backward trajectory analysis indicated that the trajectory of air mass originated from Mongolia, which reflected the features of large-scale and long-distance air transport, and that of beginning in Jiangsu, Shandong and Tianjin, which showed the features of small-scale and short-distance. Tianjin, Beijing, Hebei and Northwest of Shandong were identified as major potential source-areas of VOCs by using potential source contribution function (PSCF) and concentration-weighted trajectory (CWT) models.
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