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Understanding of nitrous acid (HONO) production is crucial to photochemical studies, especially in polluted environments like eastern China. In-situ measurements of gaseous and particulate compositions were conducted at a rural coastal site during the 2018 spring Ozone Photochemistry and Export from China Experiment (OPECE). This data set was applied to investigate the recycling of reactive nitrogen through daytime heterogeneous HONO production. Although HONO levels increase during agricultural burning, analysis of the observation data does not indicate more efficient HONO production by agricultural burning aerosols than other anthropogenic aerosols. Box and 1-D modeling analyses reveal the intrinsic relationships between nitrogen dioxide (NO2), particulate nitrate (pNO3), and nitric acid (HNO3), resulting in comparable agreement between observed and simulated HONO concentrations with any one of the three heterogeneous HONO production mechanisms, photosensitized NO2 conversion on aerosols, photolysis of pNO3, and conversion from HNO3. This finding underscores the uncertainties in the mechanistic understanding and quantitative parametrizations of daytime heterogeneous HONO production pathways. Furthermore, the implications for reactive nitrogen recycling, ozone (O3) production, and O3 control strategies vary greatly depending on the HONO production mechanism. On a regional scale, the conversion of HONO from pNO3 can drastically enhance O3 production, while the conversion from NO2 can reduce O3 sensitivity to NOx changes in polluted eastern China.
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Ácido Nitroso , Ozono , China , Nitrógeno , Contaminantes Atmosféricos , Aerosoles , Dióxido de NitrógenoRESUMEN
With the replacement of perfluorooctanoic acid (PFOA) with perfluorinated ether carboxylic acids (PFECAs), residents living near fluorochemical industrial parks (FIPs) are exposed to various novel PFECAs. Despite expectations of low accumulation, short-chain PFECAs, such as perfluoro-2-methoxyacetic acid (PFMOAA), previously displayed a considerably high body burden, although the main exposure routes and health risks remain uncertain. Here, we explored the distribution of perfluoroalkyl and polyfluoroalkyl substances (PFASs) in diverse environmental media surrounding a FIP in Shandong Province, China. PFECAs were found at elevated concentrations in all tested matrices, including vegetables, cereals, air, and dust. Among residents, 99.3% of the ∑36PFAS exposure, with a 43.9% contribution from PFECAs, was due to gastrointestinal uptake. Dermal and respiratory exposures were negligible at 0.1 and 0.6%, respectively. The estimated daily intake (EDI) of PFMOAA reached 114.0 ng/kg body weight (bw)/day, ranking first among all detected PFECAs. Cereals emerged as the dominant contributor to PFMOAA body burden, representing over 80% of the overall EDI. The median EDI of hexafluoropropylene oxide dimer acid (HFPO-DA) was 17.9 ng/kg bw/day, markedly higher than the USEPA reference doses (3.0 ng/kg bw/day). The absence of established threshold values for other PFECAs constrains a comprehensive risk assessment.
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Ácidos Alcanesulfónicos , Fluorocarburos , Contaminantes Químicos del Agua , Monitoreo del Ambiente , Grano Comestible/química , Éter , Ácidos Carboxílicos/análisis , Fluorocarburos/análisis , Éteres , Éteres de Etila , China , Contaminantes Químicos del Agua/análisisRESUMEN
Only a few dozens of the several thousand existing per- and polyfluoroalkyl substances (PFAS) are monitored using conventional target analysis. This study employed suspect screening to examine patterns of emerging and novel PFAS in German and Chinese river water affected by industrial point sources. In total, 86 PFAS were (tentatively) identified and grouped into 18 structure categories. Homologue patterns revealed distinct differences between fluoropolymer production sites of the two countries. In the Chinese Xiaoqing River Basin, the C8 homologue was the most prevalent compound of the emerging series of chlorinated perfluoroalkyl carboxylic acids (Cl-PFCAs) and perfluoroalkylether carboxylic acids (PFECAs). In contrast, C6 and shorter homologues were dominant in the German Alz River. This indicates that the phaseout of long-chain compounds in Europe and their ongoing production in Asian countries also apply to unregulated emerging PFAS classes. Additional characteristics to differentiate the point sources were the peak area ratio of perfluorobutane sulfonic acid (PFBS) versus the emerging compound hydro-substituted PFBS (H-PFBS) as well as the occurrence of byproducts of the sulfonated tetrafluoroethylene-based polymer Nafion. The large number of identified unregulated PFAS underlines the importance of a grouping approach on a regulatory level, whereas the revealed contamination patterns can be used to estimate, prioritize, and minimize contributions of specific sources.
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Fluorocarburos , Contaminantes Químicos del Agua , Ácidos Carboxílicos , China , Fluorocarburos/análisis , Ríos , Ácidos Sulfónicos/análisis , Contaminantes Químicos del Agua/análisisRESUMEN
As novel alternatives to legacy poly- and perfluoroalkyl substances (PFAS), perfluoroalkyl ether carboxylic acids (PFECAs) have been widely detected in the environment; however, there is limited information and knowledge regarding their bioaccumulation and trophic transfer behavior along the food chain. This research presents the first known published data on the bioaccumulation and trophic transfer characteristics of PFECAs in a source-impacted estuary. Elevated PFECA concentrations were observed in organisms (for instance, conch, with perfluoro-2-methoxyacetic acid (PFMOAA) concentration reaches up to 16â¯700 ng/g dry weight (dw)), indicating exposure risks to the consumers. Conch can be acted as a potential environmental bioindicator of PFMOAA. PFMOAA, hexafluoropropylene oxide trimer acid (HFPO-TrA) and PFOA were predominant detected in biotas. On the basis of trophic magnification factors (TMFs), PFECAs with ≥6 perfluorinated carbons (HFPO-TrA, hexafluoropropylene oxide tetramer acid (HFPO-TeA) and perfluoro (3, 5, 7, 9, 11-pentaoxadodecanoic) acid (PFO5DoA)) could be biomagnified along the food chain (TMF > 1), while PFMOAA with the least perfluorinated carbons undergone biodilution (TMF < 1). As seafood is an important dietary source of protein to human, there is a potential health risk related to the consuming polluted aquatic products.
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Ácidos Alcanesulfónicos , Fluorocarburos , Contaminantes Químicos del Agua , Ácidos Alcanesulfónicos/análisis , Bioacumulación , Ácidos Carboxílicos , China , Monitoreo del Ambiente , Éter , Éteres , Fluorocarburos/análisis , Cadena Alimentaria , Humanos , Óxidos , Contaminantes Químicos del Agua/análisisRESUMEN
The passive sampling technique, diffusive gradients in thin films (DGT) has attracted increasing interests as an in-situ sampler for organic contaminants including per- and polyfluoroalkyl substances (PFAS). However, its effectiveness has been questioned because of the small effective sampling area (3.1 cm2). In this study, we developed a DGT probe for rapid sampling of eight PFAS in waters and applied it to a water-sediment system. It has a much larger sampling area (27 cm2) and as a result lower method quantification limits (0.15 - 0.21 ng/L for one-day deployment and 0.02 - 0.03 ng/L for one-week deployment) and much higher (by > 10 factors) sampling rate (100 mL/day) compared to the standard DGT (piston configuration). The sampler could linearly accumulate PFAS from wastewater, was sensitive enough even for a 24 hr deployment with performance comparable to grab sampling (500 mL). The DGT probe provided homogeneous sampling performance along the large exposure area. The use of the probe to investigate distributions of dissolved PFAS around the sediment-water interface was demonstrated. This work, for the first time, demonstrated that the DGT probe is a promising monitoring tool for trace levels of PFAS and a research tool for studying their distribution, migration, and fate in aquatic environments including the sediment-water interface.
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Fluorocarburos , Contaminantes Químicos del Agua , Monitoreo del Ambiente/métodos , Aguas Residuales/análisis , Agua , Contaminantes Químicos del Agua/análisisRESUMEN
Both decabromodiphenyl ether (BDE 209) and decabromodiphenyl ethane (DBDPE) are still produced in large quantities in China, especially in the Shandong Province closed to the Bohai Sea (BS). This study conducted a comprehensive investigation of the distribution and budget of brominated flame retardants (BFRs) in the BS. BDE 209 was the predominant BFR in most of the investigated rivers flowing into the BS, although DBDPE exceeded BDE 209 in certain rivers as a result of the replacement of BDE 209 with DBDPE in North China. The spatial distributions of BFRs in the rivers were controlled by the proximity of the BFR manufacturing base and the extent of urbanization. BFRs' spatial distribution in the BS was influenced by a combination of land-based pollution sources, environmental parameters (e.g., suspended particulate matter, particulate organic carbon, and particulate black carbon), and hydrodynamic conditions. The spatial variation trend of BDE 209/DBDPE ratios in various environmental media provided useful information. Vertically, the BDE 209/DBDPE ratio decreased from the seawater surface layer to the sediment, indicating their differential transport in the BS. A multi-box mass balance model and analysis of BDE 209 showed that degradation was the primary sink of BFRs in seawater (â¼68%) and surface sediment (â¼72%) in the BS.
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Monitoreo del Ambiente , Retardadores de Llama , Bromobencenos/análisis , China , Retardadores de Llama/análisis , Éteres Difenilos Halogenados/análisisRESUMEN
Due to the prohibition of polybrominated diphenyl ethers, organophosphate flame retardants (OPFRs) and tetrabromobisphenol A (TBBPA) have become emerging flame retardants. However, knowledge about their occurrence, especially their transformation products, is still limited. This study collected sediment samples from two rivers, i.e., Lianjiang River (located at an e-waste dismantling area) and Xiaoqing River (situated at a flame retardant production base), to investigate the occurrence, composition, and spatiality distribution of OPFRs, TBBPA, and their transformation products. Both targets were detected in the Lianjiang River in the range of 220-1.4 × 104 and 108-3.1 × 103 ng/g dw (dry weight) for OPFRs and TBBPA, and 0.11-2.35 and 4.8-414 ng/g dw for their respective transformation products, respectively. The concentrations of OPFRs and TBBPA in the Xiaoqing River ranged from 4.15 to 31.5 and 0.76-2.51 ng/g dw, respectively, and no transformation products were detected. Different compositional characteristics of OPFRs and distinct spatial distribution from mainstream and tributary observed between the two rivers are attributed to the difference in the local industries. Spatial distribution and principal component analysis indicated that e-waste dismantling activities could be a vital source of local pollution. Besides, the confluence of tributaries seemed to determine the contaminant levels in the Xiaoqing River. Also, concentration ratios and Spearman's correlation between metabolites and parent chemicals were analyzed. Low concentration ratios (3.6 ×10-4 to 0.16) indicated a low transformation degree, and Spearman's correlation analysis suggested transformation products were partly stemming from commercial products. Considering the limited study of these transformation products, more studies on their sources, transform mechanism, and toxicity are required.
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Residuos Electrónicos , Retardadores de Llama , Monitoreo del Ambiente , Retardadores de Llama/análisis , Éteres Difenilos Halogenados/análisis , Organofosfatos , Bifenilos PolibrominadosRESUMEN
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/m3. 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-n-butyl phosphate (TnBP). Particle-bound OPEs accounted for 51 ± 21% of the total OPEs. On NHI, the median ΣOPE concentration was 210 pg/m3, 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/T (T: temperature (K)) (except TDCP, TPeP, and TCP). Among the 79 investigated samples, significant correlations between the measured OPE gas/particle partitioning coefficients (Kp,m) and subcooled liquid pressure (PLâ¦) (p < 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.
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Ésteres , Retardadores de Llama , China , Monitoreo del Ambiente , Asia Oriental , Océanos y Mares , Organofosfatos , Estaciones del AñoRESUMEN
The manufacturing of high-performance fabrics requires numerous chemical treatment steps that involve the use of per- and polyfluoroalkyl substances (PFASs) to protect apparel against water, stain, and oil penetration. However, air and wastewater emissions of PFASs generated during this manufacturing are a potential threat to both factory workers and the environment. We investigated the occurrence and distribution of PFASs in wastewater, air, airborne particles, and settled dust in a textile manufacturing plant in China. PFOA and PFDA or their precursor compounds 8:2 FTOH and 10:2 FTOH were the dominant compounds in all environmental media tested, revealing that long-chain PFASs were preferably used for the manufacturing of functional garments. Besides, PFASs were detected along the textile manufacturing chain, indicating that they were used as durable water repellents and as surfactants in, for example, coating agents. The workers' exposure to FTOHs via air inhalation was up to 5 orders of magnitude higher than the background exposure of the general western population. To the best of our knowledge, this is the first study providing information regarding the emission of PFASs during the manufacturing of textiles via various environmental media.
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Fluorocarburos , Instalaciones Industriales y de Fabricación , China , Polvo , Humanos , TextilesRESUMEN
The production and use of long-chain perfluoroalkyl substances (PFASs) must comply with national and international regulations. Driven by increasingly stringent regulations, their production has been outsourced to less regulated countries in Asia. In addition, the fluoropolymer industry started to use fluorinated alternatives, such as 2,3,3,3-tetrafluoro-2-(1,1,2,2,3,3,3-heptafluoropropoxy)propanoic acid (HFPO-DA). Between August 2013 and September 2014, we investigated the occurrence and distribution of HFPO-DA and legacy PFASs in surface waters of the following river/estuary systems: the Elbe and Rhine Rivers in Germany, the Rhine-Meuse delta in The Netherlands, and the Xiaoqing River in China. Distinct differences were revealed among the study areas; notably, the Chinese samples were highly polluted by an industrial point source discharging mainly perfluorooctanoic acid (PFOA). This particular point source resulted in concentrations more than 6000 times higher than an industrial point source observed in the Scheur River, where HFPO-DA was the dominant compound with a concentration of 73.1 ng/L. Moreover, HFPO-DA was detected in all samples along the coastline of the North Sea, indicating that the compound may be transported from the Rhine-Meuse delta into the German Bight via the water current. To the best of our knowledge, the fluorinated alternative, HFPO-DA, was detected for the first time in surface waters of Germany and China.
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Hidrocarburos Fluorados/análisis , Contaminantes Químicos del Agua/análisis , Caprilatos/análisis , Caprilatos/química , China , Monitoreo del Ambiente , Estuarios , Fluorocarburos/análisis , Fluorocarburos/química , Alemania , Hidrocarburos Fluorados/química , Países Bajos , Mar del Norte , Ríos/químicaRESUMEN
China has the world's largest population of smokers with serious health consequences, yet we know a very limited spectrum of hazardous chemicals in cigarette smoke even for carcinogenic polycyclic aromatic hydrocarbons (PAHs). Here, we chose 13 popular cigarette brands sold in China markets, collected particulate matters in mainstream smoke using filter pads and an automatic smoking machine, and analyzed 56 PAHs, including 31 parent, 18 alkylated, and 7 sulfur/oxygen-containing PAHs (S/O PAHs). The 56 PAHs in mainstream smoke totaled from 244.2 ± 28.5 to 10254.8 ± 481.5 ng cig(-1); parent, alkylated, and S/O PAHs shared 16-23%, 64-74%, and 6-18%, respectively. Benzo[a]pyrene (BaP) ranged 1.1-41.6 ng cig(-1), while BaP equivalent concentrations (BaPeq) ranged 3.6-120.2 ng cig(-1), but contributions to BaPeq by individual carcinogenic PAH species varied with cigarette brands. When these cigarette smoke source profiles were pooled together with those of other combustion ones available in the literature, we found that widely used diagnostic ratios of parent PAHs failed to distinguish cigarette smoke from other combustion sources, except that the ratio indeno[1,2,3-cd]pyrene/(indeno[1,2,3-cd]pyrene + benzo[g,h,i]perylene) can largely separate cigarette smoke from vehicular emissions and that the ratio of Retene/(Retene + chrysene) can further discriminate cigarette smoke from coal combustion when alkylated PAHs are involved.
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Álcalis/química , Oxígeno/química , Hidrocarburos Policíclicos Aromáticos/análisis , Humo/análisis , Fumar , Azufre/química , Carcinógenos/análisis , China , NicotianaRESUMEN
To assign fossil and nonfossil contributions to carbonaceous particles, radiocarbon ((14)C) measurements were performed on organic carbon (OC), elemental carbon (EC), and water-insoluble OC (WINSOC) of aerosol samples from a regional background site in South China under different seasonal conditions. The average contributions of fossil sources to EC, OC and WINSOC were 38 ± 11%, 19 ± 10%, and 17 ± 10%, respectively, indicating generally a dominance of nonfossil emissions. A higher contribution from fossil sources to EC (â¼51%) and OC (â¼30%) was observed for air-masses transported from Southeast China in fall, associated with large fossil-fuel combustion and vehicle emissions in highly urbanized regions of China. In contrast, an increase of the nonfossil contribution by 5-10% was observed during the periods with enhanced open biomass-burning activities in Southeast Asia or Southeast China. A modified EC tracer method was used to estimate the secondary organic carbon from fossil emissions by determining (14)C-derived fossil WINSOC and fossil EC. This approach indicates a dominating secondary component (70 ± 7%) of fossil OC. Furthermore, contributions of biogenic and biomass-burning emissions to contemporary OC were estimated to be 56 ± 16% and 44 ± 14%, respectively.
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Aerosoles/análisis , Contaminantes Atmosféricos/análisis , Carbono/análisis , Monitoreo del Ambiente/métodos , Material Particulado/análisis , Movimientos del Aire , Biomasa , China , Combustibles Fósiles/análisis , Islas , Estaciones del AñoRESUMEN
Halogenated flame retardants (HFRs) have attracted global attention owing to their adverse effects on ecosystems and humans. The Shandong Peninsula is the largest manufacturing base for HFRs in East Asia, yet its impacts on marine ecosystems are unclear. Seventeen HFRs were analyzed in organisms captured from the Xiaoqing River estuary, Bohai Sea (BS), Yellow Sea and Northern East China Sea to investigate the distribution and bioaccumulation of HFRs on a broad scale. The results showed a downward trend in ΣHFR concentrations from the estuary (37.7 ng/g lw on average) to Laizhou Bay (192 ng/g lw) and to coastal seas (3.13 ng/g lw). The concentrations of ΣHFRs were significantly higher in demersal fish (0.71-198 ng/g lw) and benthic invertebrates (0.81-3340 ng/g lw) than in pelagic fish (0.30-27.6 ng/g lw), reflecting a habitat dependence. The concentrations of higher-brominated homologs were greater in benthic invertebrates, whereas a greater level of lower-brominated PBDE congeners was observed in fish, suggesting different profiles between species. Furthermore, the analogue composition of HFRs in fish was similar to that in the dissolved phase of seawater, whereas the HFR pattern in benthic invertebrates was consistent with the profile in sediment. The concentrations of HFRs in organisms vary widely depending on emissions from anthropogenic activities, whereas bioaccumulation patterns are strongly influenced by species and habitat.
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Organismos Acuáticos , Ecosistema , Estuarios , Retardadores de Llama , Contaminantes Químicos del Agua , Retardadores de Llama/metabolismo , Retardadores de Llama/análisis , Animales , Contaminantes Químicos del Agua/metabolismo , Contaminantes Químicos del Agua/análisis , Organismos Acuáticos/metabolismo , Océanos y Mares , Peces/metabolismo , Bioacumulación , Especificidad de la Especie , Monitoreo del Ambiente , China , Invertebrados/metabolismoRESUMEN
The passive sampling technique of diffusive gradients in thin-films (DGT) is promising for monitoring emerging contaminants such as per- and polyfluoroalkyl substances (PFAS). It is urgent to evaluate the impacts of salinity and exposure time on DGT sampling before it can be set as a standard method. Herein, DGT sampler based on the binding gel of weak anion exchanger (WAX) resin was deployed in a representative water system of the Xiaoqing river-estuary-sea for representative sampling windows (<1 day to 28 days) with high pH (8.18 ± 0.04 to 8.51 ± 0.17) and wide ranges of salinity (0.95 ± 0.07 to 14.37 ± 3.92), total dissolved solids (1.20 ± 0.09 g/L to 15.29 ± 3.91 g/L) and dissolved organic matter (2.8-32 mg/L). The results showed that the WAX-DGT sampler exhibited good performance for most target PFAS except for short-chain perfluorocarboxylates (C ≤ 5) in 14 days. When the exposure time was over 14 days, biofouling of the sampler may deflect the mass accumulation of the PFAS in the sampler. Salinity played an important role in the mass binding of PFAS by DGT. The shorter the carbon chain of the compound, the greater the influence of the salinity. PFAS with carboxyl groups had greater affinities for the biofouled membrane filter than those with sulfonic groups. In the river-estuary-sea system, where PFAS concentrations changed dynamically, the temporal resolution of the monitoring strategy has been demonstrated to be more important than spatial resolution. DGT provided a better integral of PFAS exposure than grab sampling in the dynamic water system and offered equivalent sensitivity of grab sampling with exposure time <10 d and greater sensitivity with exposure time ≥10 d. Thus, DGT has the advantage of providing high temporal resolution monitoring. This study provided support for the standardization of the DGT technique.
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Coastal seas are important pools of persistent organic pollutants (POPs) discharged from land. Considering the complex conditions in coastal seas and various biochemical features of POPs, special temporal-spatial variations in POPs have been reported. To understand these variations, we developed a three-dimensional hydrodynamic-ecosystem-POP coupled model and applied it to the Yellow Sea. We selected two POP species (polychlorinated biphenyl congener 153 (PCB-153) and decabromodiphenyl ether (BDE-209)), which have different biochemical properties, as target materials. The dissolved PCB-153 simulated concentration was high in late spring and low in autumn, whereas that of BDE-209 was high in summer and low in winter. Both PCB-153 and BDE-209 showed high particle-bound concentrations in early spring. In summer, dissolved PCB-153 accumulated at the sea bottom, whereas dissolved BDE-209 accumulated at the sea surface. Seasonal and spatial variation differences in the two POPs are likely caused by greater Henry's Law Constant (H') and bioconcentration factor (BCF) of PCB-153 than that of BDE-209, which leads to higher volatilization and stronger absorption by the particles for PCB-153 than BDE-209. As a component of such differences, the "biological pump" of PCB-153 in the central Yellow Sea is more apparent than that of BDE-209.
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This study investigated the spatial distributions and seasonal variations of 19 CUPs in the coastal areas of the Shandong Peninsula and its surrounding rivers and assessed their ecological risk. In freshwater and seawater, insecticides (chlorpyrifos, methoxychlor, and pyridaben), as well as fungicides (fenarimol) and herbicides (dichlobenil) were the main pollutants (Detection Frequency: 100 %). Spatially, during winter, the regional pollution levels of Σ19CUPs in seawater showed a trend of Laizhou Bay (LZB, mean:4.13 ng L-1) > Yellow River Estuary (YRE, mean:2.57 ngL-1) > Bohai Bay (BHB, mean:2.21 ng L-1) > Yanwei Area (YWA, mean:1.94 ng L-1). The similarities of major substances between rivers and the marine environment suggest that river discharge is the main source of CUPs pollution in coastal areas. In summer, CUPs in rivers posed a high risk. In winter, the risk significantly decreased, indicating a moderate overall risk. Seawater exhibited a low risk in winter.
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Cloropirifos , Plaguicidas , Contaminantes Químicos del Agua , Plaguicidas/análisis , Contaminantes Químicos del Agua/análisis , Agua de Mar , Estuarios , China , Monitoreo del Ambiente , RíosRESUMEN
Excitation-emission matrix (EEM) fluorescence spectroscopy is a widely-used method for characterizing the chemical components of brown carbon (BrC). However, the molecular basics and formation mechanisms of chromophores, which are decomposed by parallel factor (PARAFAC) analysis, are not yet fully understood. In this study, we characterized the water-soluble organic carbon (WSOC) in aerosols collected from Karachi, Pakistan, using EEM spectroscopy and Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS). We identified three PARAFAC components, including two humic-like components (C1 and C2) and one phenolic-like species (C3). We determined the molecular families associated with each component by performing Spearman correlation analysis between FT-ICR MS peaks and PARAFAC component intensities. We found that the C1 and C2 components were associated with nitrogen-enriched compounds, where C2 with the longest emission wavelength exhibited a higher level of aromaticity, N content, and oxygenation than C1. The C3 associated formulas have fewer nitrogen-containing species, a lower unsaturation degree, and a lower oxidation state. An oxidation pathway was identified as an important process in the formation of C1 and C2 components at the molecular level, particularly for the assigned CHON compounds associated with the gas-phase oxidation process, despite their diverse precursor types. Numerous C2 formulas were found in the "potential BrC" region and overlapped with the BrC-associated formulas. It can be inferred that the compounds that fluoresce C2 contributed considerably to the light absorption of BrC. These findings are essential for future studies utilizing the EEM-PARAFAC method to explore the sources, processes, and compositions of atmospheric BrC.
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Three models, including an atmospheric transport model, a multimedia exposure model, and a risk assessment model, were used to assess cancer risk in China caused by γ-HCH (gamma-hexachlorocyclohexane) emitted from Chinese and Indian sources. Extensive model investigations revealed the contribution of different sources to the cancer risk in China. Cancer risk in Eastern China was primarily attributable to γ-HCH contamination from Chinese sources, whereas cancer risk in Western China was caused mostly by Indian emissions. The contribution of fresh use of lindane in India to the cancer risk in China was almost 1 order of magnitude higher than that of the reemission of γ-HCH from Indian soils. Of total population, 58% (about 0.79 billion) residents in China were found to live in the environment with high levels of cancer risk exceeding the acceptable cancer risk of 10(-6), recommended by the United States Environmental Protection Agency (U.S. EPA). The cancer risk in China was mostly induced by the local contamination of γ-HCH emitted from Chinese sources, whereas fresh use of lindane in India will become a significant source of the cancer risk in China if Indian emissions maintain their current levels.
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Contaminantes Ambientales/toxicidad , Hexaclorociclohexano/toxicidad , Insecticidas/toxicidad , Modelos Teóricos , Neoplasias/inducido químicamente , Movimientos del Aire , China , Exposición a Riesgos Ambientales/efectos adversos , India , Medición de RiesgoRESUMEN
The impact of perfluoroalkyl and polyfluoroalkyl substances on microbial communities is challenging to investigate in situ because of the complexity and dynamics of natural ecosystems. In the present study, four microcosms were established to explore the impact of perfluorooctanoate (PFOA) on bacterial communities in riverine and marine settings. PFOA distribution between the aqueous and sedimentary phases fluctuated in both PFOA-amended and unamended control systems. PFOA was more rapidly partitioned into the sediment in marine than in riverine microcosms. Differences in iron concentration and salinity may influence PFOA exchange between water and sediment. In marine microcosms, the alpha diversity of bacterial communities was significantly correlated to PFOA concentration. PFOA tended to correlate more strongly with bacterial community composition in water than in sediment. At the whole system level, Lefse's analysis indicated Algoriphagus halophilus as biomarkers for PFOA exposure in both riverine and marine systems, and the family Flavobacteriaceae were also more abundant in the exposed systems. In terms of temporal variation (comparison between three time points in the systems), metastat analysis showed great variability of potential PFOA-sensitive bacteria at the genus level. As such, most PFOA-sensitive genera were transitory and variable and existed for a short term in different systems (river, sea, blank, and experiment) and phases. Compared with other PFOA-sensitive genera, we suggest that further research is carried out to explore the use of Limnobacter as a bioindicator for temporal monitoring of PFOA pollution.
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Fluorocarburos , Contaminantes Químicos del Agua , Fluorocarburos/toxicidad , Fluorocarburos/análisis , Ecosistema , Contaminantes Químicos del Agua/toxicidad , Contaminantes Químicos del Agua/análisis , Ríos , Bacterias , Agua/análisis , Sedimentos Geológicos/análisisRESUMEN
The Bohai Sea is one of the most polluted marine areas in China with polycyclic aromatic hydrocarbons (PAHs) due to its unique hydrological and geographical environment. To investigate differences in PAH concentrations, composition, and particle-water partitioning before and after the rainy reason, water samples were collected during two surveying voyages covering most of the area of the Bohai Sea. Total and dissolved PAH concentrations were higher during the June voyage (total PAHs: 32.29 ± 15.18 ng/L, dissolved PAHs: 31.25 ± 15.26 ng/L) than the August voyage (total PAHs: 15.98 ± 6.39 ng/L, dissolved PAHs: 11.21 ± 5.59 ng/L). The opposite trend was observed for particulate PAHs (June: 1.04 ± 1.01 ng/L, August: 4.78 ± 2.96 ng/L). Among particulate PAHs, an unusually high proportion (65.07%) of low-molecular-weight (LMW) PAHs was observed during the August voyage, which was significantly higher than the proportion during the June voyage (21.86%). This high proportion was inconsistent with the general distribution of PAHs in the aquatic environment according to their physicochemical properties. The excess LMW PAHs adsorbed on suspended particulate matter arose mainly from soil affected by the petrochemical industry of the Bohai Economic Rim, and were carried with particles on runoff into the Bohai Sea during the rainy season. An estimated 5.49 t of LMW PAHs transitioned from the particulate phase to the dissolved phase during the rainy season. This transfer of LMW PAHs from coastal soil to the water column may be an important source of PAHs in the Bohai Sea.