Your browser doesn't support javascript.
loading
Mostrar: 20 | 50 | 100
Resultados 1 - 20 de 211
Filtrar
Mais filtros

Base de dados
País/Região como assunto
Tipo de documento
Intervalo de ano de publicação
1.
Environ Sci Technol ; 56(14): 10239-10248, 2022 07 19.
Artigo em Inglês | MEDLINE | ID: mdl-35790344

RESUMO

Extremely high levels of decabromodiphenyl ether (BDE-209) are frequently found in the serum of occupationally exposed groups, such as e-waste dismantlers and firefighters. However, the metabolism of BDE-209 in the human body is not adequately studied. In this study, 24 serum samples were collected from workers at a typical e-waste recycling workshop in Taizhou, Eastern China, and the occurrence and fate of these higher brominated diphenyl ethers (PBDEs) were investigated. The median concentration of the total PBDEs in the serum was 199 ng/g lipid weight (lw), ranging from 125 to 622 ng/g lw. Higher brominated octa- to deca-BDEs accounted for more than 80% of the total PBDEs. Three ortho-hydroxylated metabolites of PBDEs─6-OH-BDE196, 6-OH-BDE199, and 6'-OH-BDE206─were widely detected with a total concentration (median) of 92.7 ng/g lw. The concentrations of the three OH-PBDEs were significantly higher than their octa- and nona-PBDE homologues, even exceeding those of the total PBDEs in several samples, indicating that the formation of OH-PBDEs was a major metabolic pathway of the higher brominated PBDEs in occupationally exposed workers. An almost linear correlation between 6-OH-BDE196 and 6-OH-BDE199 (R = 0.971, P < 0.001) indicates that they might undergo a similar biotransformation pathway in the human body or may be derived from the same precursor. In addition, the occurrence of a series of penta- to hepta- ortho-substituted OH-PBDEs was preliminarily identified according to their unique "predioxin" mass spectral profiles by GC-ECNI-MS. Taken together, the tentative metabolic pathway for BDE-209 in e-waste dismantlers was proposed. The oxidative metabolism of BDE-209 was mainly observed at the ortho positions to form 6'-OH-BDE-206, which later underwent a consecutive loss of bromine atoms at the meta or para positions to generate other ortho-OH-PBDEs. Further studies are urgently needed to identify the chemical structures of these ortho-OH-PBDE metabolites, and perhaps more importantly to clarify the potentially toxic effects, along with their underlying molecular mechanisms.


Assuntos
Resíduo Eletrônico , Éteres Difenil Halogenados , Biotransformação , Resíduo Eletrônico/análise , Monitoramento Ambiental , Éteres Difenil Halogenados/análise , Humanos
2.
Environ Res ; 212(Pt A): 113212, 2022 09.
Artigo em Inglês | MEDLINE | ID: mdl-35367230

RESUMO

Nine amine species in atmospheric particles during haze and low-pollution days with low and high relative humidity (RH) were analyzed in urban Guangzhou, China. The mean concentrations of total measured amines (Æ©amines) in fine particles were 208 ± 127, 63.7 ± 21.3, and 120 ± 20.1 ng m-3 during haze, low pollution-low RH (LP-LRH), and low pollution-high RH (LP-HRH) episodes, respectively. The dominant amine species were methylamine (MA), dimethylamine (DMA), diethylamine (DEA) and dibutylamine (DBA), which in total accounted for 82-91% of the Æ©amines during different pollution episodes. The contributions of Æ©amines-C to water-soluble organic carbon (WSOC) and Æ©amines-N to water-soluble organic nitrogen (WSON) were 1.52% and 2.49% during haze, 1.24% and 1.96% during LP-LRH, and 2.00 and 2.98% during LP-HRH days, respectively. The mass proportion of Æ©amines in fine particles was higher during LP-HRH periods (0.19%) than during haze and LP-LRH periods (0.16%). The mass proportion of DBA in Æ©amines increased from 7% during haze and LP-LRH episodes to 25% during LP-HRH episodes. Compared with other amines, DBA showed a stronger linear relationship with RH (r = 0.867, p < 0.01), which demonstrates its high sensitivity to high RH conditions. Meteorological parameters (including RH, the mixed layer depth, wind speed and temperature), the oxidizing capacity (ozone concentration), and gaseous pollutants (NOx and SO2) correlated with amines under different pollution conditions. Under high RH, acid-base reactions were the dominant pathway for the gas-to-particle distribution of amines in urban areas, while direct dissolution dominated in the background site. To our knowledge, this study is the first attempt to conduct in situ measurements of particulate amines during different pollution conditions in China, and further research is needed to in-depth understanding of the influence of amines on haze formation.


Assuntos
Poluentes Atmosféricos , Poluição do Ar , Aminas , Aerossóis/análise , Poluentes Atmosféricos/análise , Poluição do Ar/análise , Aminas/análise , China , Poeira , Monitoramento Ambiental , Umidade , Oxirredução , Material Particulado/análise , Rios , Água
3.
Ecotoxicol Environ Saf ; 241: 113730, 2022 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-35691194

RESUMO

Severe pollution of polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) and their brominated analogues (PBDD/Fs) was frequently reported for the waters located near unregulated e-waste recycling areas. However, the migrations of these high-level dioxins via waterways and their potential threats to the lower reaches were seldom investigated. In this study, we analyzed PCDD/Fs and PBDD/Fs in 27 surficial sediments collected from the Lian River encompassing the Guiyu, China e-waste recycling zone, and investigated their distributions, sources, migration behaviors and risks. Both PCDD/Fs and PBDD/Fs in these sediments exhibited a spatial trend of Guiyu > Guiyu downriver > Guiyu upriver, illustrating that the Guiyu e-waste recycling activities were the uppermost dioxin contributors in this watershed. Sediments from different Guiyu villages demonstrated big gaps in PCDD/F concentrations and congener compositions, and the reason was attributed to the diverse e-waste recycling activities practiced in these villages. Sediments near the e-waste open-burning areas demonstrated extremely high PCDD/F concentrations and unique PCDD/F profiles featured by low-chlorinated PCDFs (tetra- to hexa-), which is quite different from the OCDD-dominant PCDD/F profile found in most of the Lian River sediments. The geographical distributions of PCDD/F concentrations and profiles illustrate that the substantial amount of PCDD/Fs in Guiyu sediments were mainly retained in local and vicinal water bodies. The principal component analysis (PCA) results further confirm that the high-level PCDD/Fs in Guiyu sediments exhibited quite limited translocations downstream and therefore exerted little influences on the lower reaches. Pentachlorophenol use in history, ceramic industry and vehicle exhaust were diagnosed as the major PCDD/F sources for most sediments of the Lian River. Total toxicity equivalent quantities (TEQs) of 70% of the Lian River sediments surpassed the high-risk limit specified for mammalian life by the U.S.EPA (25 pg TEQ g-1), and most of these sediments were from Guiyu and its near downstream, which merit continuous attention and necessary remediation measures.


Assuntos
Benzofuranos , Dioxinas , Resíduo Eletrônico , Dibenzodioxinas Policloradas , Benzofuranos/análise , China , Dibenzofuranos/análise , Dibenzofuranos Policlorados/análise , Dioxinas/análise , Resíduo Eletrônico/análise , Monitoramento Ambiental , Dibenzodioxinas Policloradas/análise
4.
Environ Sci Technol ; 53(7): 3782-3790, 2019 04 02.
Artigo em Inglês | MEDLINE | ID: mdl-30831022

RESUMO

Spatiotemporal trends in pro-inflammatory (interleukin (IL)-6 and IL-8) release after exposure to the water-soluble fractions of PM2.5 sampled in 10 large Chinese cities over 1 year were investigated. Chemical components (water-soluble ions, metal(loid) elements, water-soluble organic carbon (WSOC), humic-like substances (HULIS), and endotoxins) in PM2.5 samples were measured, and the molecular structure of WSOC was also analyzed by nuclear magnetic resonance. Changes in DNA methylation and gene expression of candidate genes were also evaluated to explore the potential mechanisms. PM2.5 from southern cities induced lower pro-inflammatory responses compared to those from northern cities. Seasonal differences in toxicity were noted among the cities. IL-6 was significantly correlated with HULIS (as the main fraction of WSOC with oxygenated carbohydrate structures characteristic), Pb, and endotoxin. Furthermore, DNA methylation and gene expression changes in RASSF2 and CYP1B1 were related to pro-inflammatory secretion. Certain components of PM2.5, rather than PM2.5 mass itself, determine the pro-inflammatory release. In particular, HULIS, which originated from primary biomass burning and residual coal combustion, and secondary organic aerosols, appear to be the key component in PM2.5 to induce human health risk.


Assuntos
Poluentes Atmosféricos , Material Particulado , Cidades , Carvão Mineral , Monitoramento Ambiental , Humanos , Inflamação , Estações do Ano , Água
5.
Environ Sci Technol ; 53(3): 1269-1277, 2019 02 05.
Artigo em Inglês | MEDLINE | ID: mdl-30354091

RESUMO

We used a single particle mass spectrometry to online detect chemical compositions of individual particles over four seasons in Guangzhou. Number fractions (Nfs) of all the measured particles that contained oxalate were 1.9%, 5.2%, 25.1%, and 15.5%, whereas the Nfs of Fe-containing particles that were internally mixed with oxalate were 8.7%, 23.1%, 45.2%, and 31.2% from spring to winter, respectively. The results provided the first direct field measurements for the enhanced formation of oxalate associated with Fe-containing particles. Other oxidized organic compounds including formate, acetate, methylglyoxal, glyoxylate, purivate, malonate, and succinate were also detected in the Fe-containing particles. It is likely that reactive oxidant species (ROS) via Fenton reactions enhanced the formation of these organic compounds and their oxidation product oxalate. Gas-particle partitioning of oxalic acid followed by coordination with Fe might also partly contribute to the enhanced oxalate. Aerosol water content likely played an important role in the enhanced oxalate formation when the relative humidity is >60%. Interactions with Fe drove the diurnal variation of oxalate in the Fe-containing particles. The study could provide a reference for model simulation to improve understanding on the formation and fate of oxalate, and the evolution and climate impacts of particulate Fe.


Assuntos
Poeira , Compostos Orgânicos , Aerossóis , Carvão Mineral , Estações do Ano
6.
Ecotoxicol Environ Saf ; 153: 40-44, 2018 May 30.
Artigo em Inglês | MEDLINE | ID: mdl-29407736

RESUMO

To evaluate contamination by polybrominated diphenyl ethers (PBDEs) in market hens and human PBDE exposure via hen consumption in Guangzhou, hens were collected and their muscle, liver, fat, blood, yolk, and ingluvies tissues were analyzed for 13 PBDE congeners. The median highest concentration of ∑PBDEs was found in the ingluvies (5.30 ng/g lw), followed by the muscle (2.53 ng/g lw), with the lowest located in the yolk (0.09 ng/g lw). The concentrations of PBDEs in the muscle tissue of market hens in Guangzhou were at medium levels compared to others reported around the world. BDE-47, -153, -99, and -183 were the predominant congeners. The daily intake concentrations of PBDEs from hen muscle were estimated to range from 0.08 to 0.31 ng/kg/day in this study, with a Hazard Quotient (HQ) below 1.0. These results suggest that the health risk of PBDEs for the general population, through the consumption of market hens in Guangzhou, was generally low. However, the intake of PBDEs via food consumption may be one major exposure pathway for the general population of Guangzhou.


Assuntos
Exposição Dietética/análise , Poluentes Ambientais/análise , Contaminação de Alimentos/análise , Éteres Difenil Halogenados/análise , Hidrocarbonetos Bromados/análise , Carne/análise , Animais , Galinhas , China , Feminino , Humanos , Análise de Componente Principal
7.
Environ Geochem Health ; 40(5): 1931-1940, 2018 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-28477162

RESUMO

A number of studies have reported on the exposure of e-waste dismantling workers to significantly high concentrations of halogenated organic pollutants such as polychlorinated biphenyls (PCBs) and polybrominated diphenyl ethers. Such exposure can have adverse health effects. However, little information on the metabolites of these contaminants exists. In this study, we investigated PCBs levels and their hydroxylated metabolites (OH-PCB) in the serum of e-waste workers in Taizhou in eastern China. Our results indicate elevated PCB and OH-PCB levels in the serum of the workers, with medians of 443.7 and 133.9 ng/g lw, respectively. Tri- to hexachlorinated PCB congeners were the dominant homologue groups in all of the samples. 4-OH-CB107 was the predominant homologue among the hydroxylated metabolites, accounting for 88.9% of the total OH-PCB concentrations. While dietary sources (e.g., fish) appear to be an important route for PCB accumulation in non-occupational exposure groups, exposure via ingestion of house dust and inhalation of pollutants derived from the recycling of PCB-containing e-wastes may primarily contribute to the high body burden observed in the occupational groups. Since we found concentrations of metabolites higher than those of their parent compounds, further studies need to pay more attention to their bioaccumulation and toxicity.


Assuntos
Resíduo Eletrônico/análise , Poluentes Ambientais/análise , Éteres Difenil Halogenados/análise , Bifenilos Policlorados/análise , Animais , China , Dieta , Poeira/análise , Poluentes Ambientais/metabolismo , Peixes/metabolismo , Humanos , Masculino , Reciclagem , Alimentos Marinhos
8.
J Sep Sci ; 40(3): 813-818, 2017 02.
Artigo em Inglês | MEDLINE | ID: mdl-27925402

RESUMO

Two biomarkers, 5,9-dimethyl-6-isopropyl-2-decanone (1) and 4,9,11-trimethyl-6-isopropyl-2-dodecanone (2), were isolated from Chinese Maoming oil shale by silica gel column chromatography and preparative gas chromatography. Their structures were elucidated by using spectroscopic techniques.


Assuntos
Biomarcadores/química , Técnicas de Química Analítica/métodos , Cromatografia Gasosa , Biomarcadores/análise , Técnicas de Química Analítica/instrumentação , Medicamentos de Ervas Chinesas , Oxigênio/química , Sílica Gel/química
9.
Artigo em Inglês | MEDLINE | ID: mdl-26181085

RESUMO

As ubiquitous organic contaminants, polybrominated diphenyl ethers (PBDEs) were evaluated to explore the impacts of the water level fluctuating zone (WLFZ) on organic pollutant behavior and the retention mechanism of organic pollutants in the bank-WLFZ-water system of Hanfeng Lake in the Three Gorges region of China. The mean concentrations of total PBDEs were 103, 75.2, and 568 ng g(-1) dry wt for bank soils, WLFZ soils, and sediment samples, respectively. Except for sampling sites S1 and S2, the levels of PBDEs decreased in the order of sediment>WLFZ soil > bank soil, suggesting that PBDEs were transferred from bank soil to WLFZ soil and finally deposited in the sediment. Decabromodiphenyl ethers (deca-BDEs) were the predominant congener in the study area, comprising 93.8% to 98.3% of the total PBDEs. Greater photolytic degradation of deca-BDEs was suggested in bank soils based on a higher relative abundance of octa- and nona-BDEs than in WLFZ soils and sediment. This may have occurred because deca-BDEs in bank soils have relatively longer sunlight exposure than in WLFZ soils and sediment due to the annual alternation of water storage and drainage in the catchments of the Three Gorges Reservoir. More in-depth investigations of contaminants in bank-WLFZ-water systems are needed due to the large areas of WLFZ created by the construction of the Three Gorges Dam and their importance to the balance of aquatic ecosystems.


Assuntos
Sedimentos Geológicos/química , Éteres Difenil Halogenados/análise , Solo/química , China , Lagos/química , Fotólise , Poluentes do Solo/análise
10.
Artigo em Inglês | MEDLINE | ID: mdl-26301856

RESUMO

The occurrence, distribution and main removal pathway of seven widely used organophosphate esters (OPs) in a municipal wastewater treatment plant (WWTP) located in the Pearl River Delta were investigated. Their daily discharge load into the Pearl River via effluent was also estimated. All the target analytes were detected in wastewater, suspended particle and dewatered sludge, with tri-n-butyl phosphate (TBP) and tris(2-butoxyethyl) phosphate (TBEP) as the main components. The total concentrations of TBP and TBEP were 21271.8 ng L(-1) and 4349.4 ng L(-1), 3105.1 ng L(-1) and 494.5 ng L(-1) in influent wastewater and final effluent, respectively. These results indicated that non-chlorinated OPs were removed efficiently in the WWTP, while chlorinated OPs passed through the WWTP unchanged due to their resistance to current wastewater treatment technology. Approximate 91.4 g of non-chlorinated OPs and 23.4 g of chlorinated OPs per day were discharged into the Pearl River via effluent, 2.4 g of non-chlorinated OPs and 0.6 g of chlorinated OPs entered the environment following sludge disposal.


Assuntos
Monitoramento Ambiental , Retardadores de Chama/isolamento & purificação , Plastificantes/isolamento & purificação , Águas Residuárias/química , Poluentes Químicos da Água/isolamento & purificação , Purificação da Água , China , Monitoramento Ambiental/métodos , Retardadores de Chama/análise , Humanos , Governo Local , Organofosfatos/química , Compostos Organofosforados/química , Plastificantes/análise , Rios/química , Eliminação de Resíduos Líquidos , Poluentes Químicos da Água/análise , Purificação da Água/métodos
11.
Rapid Commun Mass Spectrom ; 28(13): 1473-8, 2014 Jul 15.
Artigo em Inglês | MEDLINE | ID: mdl-24861597

RESUMO

RATIONALE: Hexabromocyclododecanes (HBCDs) are raising concern due to their potential persistence, bioaccumulation and toxicity. Apart from the widely reported isomers α-, ß-, γ-HBCD, other HBCD diastereoisomers such as δ-HBCD have been also recently found in environmental media and biota. These newly reported diastereoisomers might give more insight into the degradation and biotransformation of HBCDs. METHODS: A reversed-phase C18 column coupled to a C8 column was used to improve the chromatographic resolution. A gradient mobile phase consisting of methanol, acetonitrile, and water, as well as tandem mass spectrometry parameters, were optimized. Ten HBCD diastereoisomers were finally determined by liquid chromatography/tandem mass spectrometry in multiple reaction monitoring mode with negative electrospray ionization. RESULTS: Eight of the ten HBCDs could be chromatographically separated by using the coupled reversed-phase columns. Results of the method validation indicate high reproducibility and good sensitivity. The limit of detection ranged from 0.4 to 0.8 pg, and the relative standard deviations of intra- and inter-day injections ranged from 1.8 to 5.1% and from 2.7 to 9.5%, respectively. The developed method was further applied to the analysis of HBCDs in HBCD commercial products and soil samples. δ-, η-, θ-, and ε-HBCD were detected in commercial products and soil samples. CONCLUSIONS: The present study revealed that δ-, η-, θ-, and ε-HBCD might occur ubiquitously in environmental media and biota. These newly reported diastereoisomers may help us to better understand the fate and transformation of HBCDs in the environment.


Assuntos
Cromatografia de Fase Reversa/métodos , Hidrocarbonetos Bromados/análise , Hidrocarbonetos Bromados/química , Espectrometria de Massas em Tandem/métodos , Cromatografia Líquida de Alta Pressão , Limite de Detecção , Reprodutibilidade dos Testes , Solo/química , Estereoisomerismo
12.
Environ Toxicol ; 29(1): 108-16, 2014 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-21953684

RESUMO

Benzene is an important industrial chemical that is also widely present in cigarette smoke, automobile exhaust, and gasoline. It is reported that benzene can cause hematopoietic disorders and has been recognized as a human carcinogen. However, the mechanisms by which it increases the risk of carcinogenesis are only partially understood. Aberrant DNA methylation is a major epigenetic mechanism associated with the toxicity of carcinogens. To understand the carcinogenic capacity of benzene, experiments were designed to investigate whether exposure to benzene and its metabolites would change the global DNA methylation status in human normal hepatic L02 cells and then to evaluate whether the changes would be induced by variation of DNA methyltransferase (DNMT) activity in HaeIII DNMT-mediated methylation assay in vitro. Our results showed that hydroquinone and 1,4-benzoquinone could induce global DNA hypomethylation with statistically significant difference from control (p < 0.05), but no significant global DNA methylation changes were observed in L02 cells with benzene, phenol, and 1,2,4-trihydroxybenzene exposure. Benzene metabolites could not influence HaeIII DNMT activity except that 1,4-benzoquinone shows significantly inhibiting effect on enzymatic methylation reaction at concentrations of 5 µM (p < 0.05). These results suggest that benzene metabolites, hydroquinone, and 1,4-benzoquinone can disrupt global DNA methylation, and the potential epigenetic mechanism by which that global DNA hypomethylation induced by 1,4-benzoquinone may work through the inhibiting effects of DNMT activity at 10 µM (p < 0.05).


Assuntos
Derivados de Benzeno/toxicidade , Benzeno/toxicidade , Carcinogênese/induzido quimicamente , Metilação de DNA/efeitos dos fármacos , Hepatócitos/efeitos dos fármacos , Benzeno/metabolismo , Carcinógenos/toxicidade , Linhagem Celular , Desoxirribonucleases de Sítio Específico do Tipo II/metabolismo , Epigênese Genética/efeitos dos fármacos , Humanos
13.
Environ Monit Assess ; 186(10): 6097-106, 2014 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-24898519

RESUMO

Studies specifically addressing the elemental carbon (EC)/black carbon (BC) relationship during the transition from clean-normal (CN) air quality to heavy haze (HH) are rare but have important health and climate implications. The present study, in which EC levels are measured using a thermal-optical method and BC levels are measured using an optical method (aethalometer), provides a preliminary insight into this issue. The average daily EC concentration was 3.08 ± 1.10 µg/m(3) during the CN stage but climbed to 11.77 ± 2.01 µg/m(3) during the HH stage. More importantly, the BC/EC ratio averaged 0.92 ± 0.14 during the CN state and increased to 1.88 ± 0.30 during the HH state. This significant increase in BC/EC ratio has been confirmed to result partially from an increase in the in situ light absorption efficiency (σap) due to an enhanced internal mixing of the EC with other species. However, the exact enhancement of σap was unavailable because our monitoring scheme could not acquire the in situ absorption (bap) essential for σap calculation. This reveals a need to perform simultaneous measurement of EC and bap over a time period that includes both the CN and HH stages. In addition, the sensitivity of EC to both anthropogenic emissions and HH conditions implies a need to systematically study how to include EC complex (EC concentration, OC/EC ratio, and σap) as an indicator in air quality observations, in alert systems that assess air quality, and in the governance of emissions and human behaviors.


Assuntos
Poluentes Atmosféricos/análise , Monitoramento Ambiental , Material Particulado/análise , Fuligem/análise
14.
Environ Technol ; 35(21-24): 2973-81, 2014.
Artigo em Inglês | MEDLINE | ID: mdl-25189845

RESUMO

Urinary 2-hydroxynaphthalene, 2-hydoxyfluorene, 9-hydroxyphenanthrene, 1-hydroxypyrene and 3-hydroxybenz[a]pyrene concentrations in 179 randomly selected voluntary students were determined in the Southern China, aged 14-16 and living in four areas with different levels of polycyclic aromatic hydrocarbons (PAHs) in soil, water and ambient air. The excretion of 1-hydroxypyrene is significantly higher in students of the urban than in students of the rural, while there are no significant differences of urinary 2-hydroxynaphthalene, 2-hydoxyfluorene and 9-hydroxyphenanthrene between urban and rural children. Mean concentrations of 1-hydroxypyrene (0.54-0.80 µmol/mol creatinine) in the study are much higher than those in the children of Denmark, Germany, Spain, USA, Korea, Japan and Taiwan, and a little higher than those in the children of Ukraine and Thailand. Urinary 2-hydroxynaphthalene concentrations in the study are a little higher than those in the children of USA, and similar to that in non-occupational exposure residences in Korea. Urinary 9-hydroxyphenanthrene concentrations in China are much higher than those in the children of USA. Differences between children with smoking parents and non-smoking parents are not significant in the study.


Assuntos
Poluentes Ambientais/urina , Hidrocarbonetos Policíclicos Aromáticos/urina , Adolescente , China , Cidades , Monitoramento Ambiental , Poluentes Ambientais/metabolismo , Feminino , Humanos , Masculino , Hidrocarbonetos Policíclicos Aromáticos/metabolismo , População Rural , População Urbana
15.
Rapid Commun Mass Spectrom ; 27(15): 1690-6, 2013 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-23821562

RESUMO

RATIONALE: Both chiral analysis and compound-specific stable carbon isotope analysis have limitations when applied to environmental research. However, the combination of these two techniques might overcome their respective limitation and give more insight into the enantioselective fate and source apportionment of chiral organic contaminants. METHODS: After Soxhlet extraction and clean-up, sediment extracts were further pre-concentrated using normal-phase preparative high-performance liquid chromatography to isolate sufficient quantities of highly purified galaxolide (1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta(g)-2-benzopyran; HHCB). The enantiomeric fractions and stable carbon isotopes of the HHCB were determined using gas chromatography/mass spectrometry (GC/MS) and GC/isotope ratio mass spectrometry (IRMS). RESULTS: The method was validated by analysis of the enantiomeric fractions and the stable carbon isotope ratios of the HHCB standard at each step of the pre-concentration procedure, and no significant enantiomeric and isotopic fractionation was found. The sediment sample was further used to test the developed method, and it was shown that the HHCB enantiomers in the sediment sample exhibited significantly different δ(13) C values (-33.03 to -24.57‰) and a slight enantiomeric fractionation (0.507 and 0.490) from a HHCB standard reference compound (-26.50 to -26.21‰ for δ(13) C values, and 0.519 and 0.497 for enantiomeric fractions). CONCLUSIONS: This work offers a novel approach to elucidating the sources and the abiotic or biological transformation processes of HHCB in the environment and will offer a perspective for assessing the environment fate of any chiral organic compound.


Assuntos
Benzopiranos/química , Poluentes Ambientais/química , Sedimentos Geológicos/química , Isótopos de Carbono/análise , Cromatografia Gasosa/métodos , Espectrometria de Massas/métodos , Estereoisomerismo
16.
Environ Pollut ; 316(Pt 1): 120489, 2023 Jan 01.
Artigo em Inglês | MEDLINE | ID: mdl-36273686

RESUMO

Polybrominated dibenzo-p-dioxin/furans (PBDD/Fs) and polychlorinated dibenzo-p-dioxin/furans (PCDD/Fs) in the environment are closely related to their precursors, brominated flame retardants (BFRs) and organochlorine pesticides (OCPs). However, their change trends following the regulation of BFRs and OCPs remain incompletely characterized. Here, we examined PBDD/Fs and PCDD/Fs in sediments from a historical hotspot for both BFRs and OCPs, namely the Pearl River Delta (PRD), China. PBDD/Fs showed ubiquity in these samples but significantly lower concentrations than PCDD/Fs. Spatially, the occurrence of PBDD/Fs was positively correlated with local development levels and sediments from highly urbanized/industrialized areas showed higher and increasing PBDD/F concentrations. Polybrominated diphenyl ether (PBDE)-related products/industries were the greatest PBDD/F contributors to the PRD, followed by bromo-phenol/benzene-related products/industries. PCDD/Fs in PRD sediments showed significant positive correlations with local grain planting area, yield, and pesticide consumption. The historical use of pentachlorophenol (PCP)/PCP-Na and biomass open-burning were the leading PCDD/F sources of the PRD agricultural/rural areas, where the concentrations and toxic equivalent quantities (TEQs) of PCDD/Fs in sediments changed very little over the past decade. Anthropogenic thermal processes involved in metallurgy, waste incineration, and vehicles were the greatest PCDD/F contributors in the PRD urban/industrial areas, where the PCDD/F concentrations in sediments almost doubled over the last decade. This finding indicates the increasing PCDD/F contributions of industrial and municipal activities in the PRD, despite the implementation of strict emission standards. Over sixty percent of the samples showed TEQs that surpassed the low-risk threshold specified for mammalian life by the U.S. EPA (2.5 pg TEQ g-1) and warrant continuous attention.


Assuntos
Dioxinas , Retardadores de Chama , Hidrocarbonetos Clorados , Praguicidas , Dibenzodioxinas Policloradas , Dibenzofuranos/análise , Dibenzofuranos Policlorados , Dioxinas/análise , Monitoramento Ambiental , Retardadores de Chama/análise , Furanos/análise , Mamíferos , Dibenzodioxinas Policloradas/análise
17.
Ecotoxicol Environ Saf ; 84: 325-33, 2012 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-22921253

RESUMO

The concentrations of musks (polycyclic musks and nitro musks) and traditional organochlorine pesticides (OCPs), including dichlorodiphenyltrichloroethane and its metabolites (DDT, DDE, DDD, and total DDTs), hexachlorobenzene (HCB), and hexachlorocyclohexanes (HCHs) in breast milk collected in Shanghai, China during the period 2006-2010, were determined. The total concentrations ranged from 4.7 to 276.2 (median: 58.4) ng/glipid weight (lw) for musks and from 88.3 to 2532.9 (median: 1003.8) ng/glw for OCPs. 4,4'-DDE (median: 655.4 ng/glw) was the predominant OCP, followed by ß-HCH (median: 172.5 ng/g lw), and HHCB (1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta[γ]-2-benzopyran) (median: 17.7 ng/g lw) was the dominant musk. There was no statistical correlation between total musk concentrations, and HCB, HCHs, DDTs or total OCP concentrations, indicating their different exposure routes and metabolism in humans (p=0.182-0.325). Clear reductions in temporal trends in the levels of DDTs and HCB, especially HCHs (p<0.01) were observed during the sampling period, and the high DDE/DDT ratios in the samples indicated past exposure to DDTs. The relatively high median concentrations of HHCB and HHCB-lactone in 2010 suggested a probably increasing tendency. There were statistically significant influences regarding maternal age and parity on OCP accumulation (p=0.001-0.002), but no significant effect on musks was found (p=0.542-0.919). Musk exposure in neonates via breast milk was 2-3 orders of magnitude lower than suggested provisional tolerable daily intakes (PTDI). The estimated daily intakes for HCB and DDTs were below the PTDI in Canada, however, 56% of those for HCHs exceeded the Canadian PTDI. OCP contamination of breast milk requires further attention.


Assuntos
Poluentes Ambientais/análise , Hidrocarbonetos Clorados/análise , Exposição Materna , Leite Humano/química , Praguicidas/análise , Adulto , China , Monitoramento Ambiental , Poluentes Ambientais/química , Feminino , Humanos , Hidrocarbonetos Clorados/química , Fatores de Tempo , Adulto Jovem
18.
J Environ Monit ; 14(7): 1935-42, 2012 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-22641387

RESUMO

Polychlorinated dibenzo-p-dioxins and dibenzofurans (PCDD/Fs) and polybrominated dibenzo-p-dioxins and dibenzofurans (PBDD/Fs) in surface sediment samples from Taihu Lake--an important water supply of the Yangtze River Delta, China--were investigated in the present study. Concentrations of PCDD/Fs ranged from 0.91 to 4.8 pg TEQ g(-1) dw (mean: 2.9 pg TEQ g(-1) dw, TEQ: Toxic Equivalent), which were all higher than the threshold effect level established by interim sediment quality guidelines in Canada (0.85 pg TEQ g(-1) dw). The levels of PBDD/Fs ranged from 0.16 to 1.6 pg TEQ g(-1) dw (mean: 0.52 pg TEQ g(-1) dw) and accounted for 5-33% (mean: 14%) of the total PCDD/Fs and PBDD/Fs TEQ. Comparatively, the abundance of sedimentary PCDD/Fs in the three regions (Meiliang Bay, Gonghu Bay, and Xukou Bay) showed a decreasing trend from the inflow region to the outflow region, while no significant difference was observed among their 2,3,7,8-PBDD/Fs levels, which suggested that the sources of PCDD/Fs and PBDD/Fs differed in this area. Principal component analysis suggested that the historical production/usage of pentachlorophenol and sodium pentachlorophenate was the dominant source of PCDD/Fs in the sediment of these regions. Although the specific sources of PBDD/Fs in the sediment of Taihu Lake were unclear, it was suspected to be due to atmospheric deposition; however, an additional study is needed to confirm this.


Assuntos
Benzofuranos/análise , Compostos de Bromo/análise , Compostos Clorados/análise , Dioxinas/análise , Sedimentos Geológicos/química , Poluentes Químicos da Água/análise , China , Monitoramento Ambiental , Lagos/química , Poluição Química da Água/estatística & dados numéricos
19.
Artigo em Inglês | MEDLINE | ID: mdl-22320691

RESUMO

The levels and distribution of six polycyclic musks, three nitromusks and 15 polycyclic aromatic hydrocarbons (PAHs) were investigated in sludge collected from 19 municipal wastewater treatment plants (WWTPs) in six cities in Guangdong Province, China. PAHs were detected in all of the sludge samples, and the levels of the total 15 PAHs ranged from 177.2-4421.8 µg/kg dry weight (dw). Four polycyclic musks, 4-acetyl-1,1-dimethyl-6-tert-butylindan (ADBI), 6-acetyl-1,1,2,3,3,5-hexamethylindan (AHMI), 1,3,4,6,7,8-hexahydro-4,6,6,7,8,8-hexamethylcyclopenta (g) -2-benzopyran (HHCB) and 7-acetyl -1,1,3,4,4,6-hexamethyl-1,2,3,4-tetrahydro naphthalene (AHTN), were found in these samples. The total concentrations of polycyclic musks varied from 794.4-12960.3 µg/kg dw, with HHCB and AHTN being the main components. Of the three nitromusks, 2,6-dinitro-3-methoxy-4-tert- butyl - toluene (MA) was only found in one sludge sample at the limit of detection (LOD) level, while 1-tert-butyl-3,5-dimethyl-2,4,6-trinitrobenzene (Musk xylene, MX) and 4-acetyl-1-tert-butyl-3,5-dimethyl-2,6-dinitrobenzene (Musk ketone, MK) were found at levels ranging from the LOD to 65.8 µg/kg dw and LOD to 172.7 µg/kg dw, respectively, in most of the sludge samples. The PAHs, polycyclic musks and nitro musks were also shown to have various distribution patterns, possibly due to their different wastewater sources and wastewater treatment technology.


Assuntos
Ácidos Graxos Monoinsaturados/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Esgotos/análise , Poluentes Químicos da Água/análise , China , Monitoramento Ambiental , Análise de Componente Principal
20.
Environ Pollut ; 293: 118563, 2022 Jan 15.
Artigo em Inglês | MEDLINE | ID: mdl-34838709

RESUMO

Polybrominated dibenzo-p-dioxins/furans (PBDD/Fs) and polychlorinated dibenzo-p-dioxins/furans (PCDD/Fs) share similar toxicities and thermal origins, e.g., municipal solid waste incinerator (MSWI). Recently, PBDD/Fs from MSWI attracted rising concern because their important precursors, i.e., brominated flame retardants (BFRs), were frequently found in various wastes for landfill or MSWI feedstock. So far, however, little is known about PBDD/Fs and their associated risks in the vicinal environments of MSWI. Here we analyzed PBDD/Fs and PCDD/Fs in 29 soil samples collected around a multiyear large-scale MSWI, and compared their spatial distributions, sources and risks. PBDD/Fs demonstrated comparable concentrations and toxic equivalent quantities (TEQs) to PCDD/Fs in these samples. Spatially, both the concentrations of PBDD/Fs and PCDD/Fs decreased outwards from the MSWI, and exhibited significant linear correlations with the distances from the MSWI in the southeast downwind soil, suggesting the influence of the MSWI on its vicinal soil environment. However, the existence of other dioxin sources concealed its influence beyond 6 km. PBDD/Fs in the soils were characterized by highly-brominated PBDFs, especially Octa-BDF, and their sources were diagnosed as the MSWI and diesel exhaust; PCDD/Fs, however, were dominated by highly-chlorinated PCDDs, particularly Octa-CDD, and were contributed individually or jointly by the MSWI, automobile exhaust and pentachlorophenol (PCP)/Na-PCP. The non-carcinogenic risks of dioxins in all the soil samples were acceptable, but their carcinogenic risks in 17% of the samples were unacceptable. These samples were all located close to the MSWI and highways, therefore, the land use of these two high-risk zones should be cautiously planed.


Assuntos
Dioxinas , Dibenzodioxinas Policloradas , Dibenzofuranos/análise , Dioxinas/análise , Monitoramento Ambiental , Furanos , Dibenzodioxinas Policloradas/análise , Solo , Resíduos Sólidos
SELEÇÃO DE REFERÊNCIAS
DETALHE DA PESQUISA