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1.
Int J Hyg Environ Health ; 242: 113971, 2022 05.
Artigo em Inglês | MEDLINE | ID: mdl-35472749

RESUMO

BACKGROUND: Refined coal tar sealant (RCTS) emulsions are used to seal the surface of asphalt pavement. Nine of the 22 polycyclic aromatic hydrocarbons (PAHs) evaluated in this study are classified as known, probable, or possible human carcinogens. Exposure assessment research for RCTS workers has not been published previously. OBJECTIVES: The overall objective of this study was to develop a representative occupational exposure assessment of PAH exposure for RCTS workers based on worksite surveys. The specific aims were to: 1) quantify full-shift airborne occupational exposures to PAHs among RCTS workers; 2) quantify workers' dermal exposures to PAHs; 3) quantify biomarkers of PAH exposure in workers' urine; 4) identify specific job titles associated with RCTS exposure; and 5) apply these results to a biological exposure index to assess risk of potential genotoxicity from occupational exposures. METHODS: A total of twenty-one RCTS workers were recruited from three companies. Personal and area air samples were collected using a modification of NIOSH Method 5515. Dermal exposure was assessed by hand and neck wipes before and after shifts. Twenty-two PAHs were quantified via gas chromatography-mass spectrometry selected ion monitoring. Internal dose was estimated by quantifying select PAH metabolites in pre- and post-shift urine samples using on-line solid phase extraction-high performance liquid chromatography-tandem mass spectrometry. RESULTS: PAH levels in the worker breathing zones were highest for naphthalene, acenaphthene, and phenanthrene, with geometric means of 52.1, 11.4, and 9.8 µg/m3, respectively. Hand wipe levels of phenanthrene, fluoranthene and pyrene were the highest among the 22 PAHs with geometric means of 7.9, 7.7, and 5.5 µg/cm2, respectively. Urinary PAH biomarkers for naphthalene, fluorene, phenanthrene, and pyrene were detected in all workers and were higher for post-shift samples than those collected pre-shift. Urinary concentrations of the metabolite 1-hydroxypyrene were greater than the American Conference of Governmental Industrial Hygienists (ACGIH) Biological Exposure Index (BEI) for this metabolite in 89 percent of post-shift samples collected on the final day of the work week or field survey. Statistically significances were found between concentrations of fluorene, naphthalene, and phenanthrene in the breathing zone of workers and their corresponding urinary PAH biomarkers. Workers were placed in two work place exposure groups: applicators and non-applicators. Applicators had higher total PAH concentrations in personal breathing zone (PBZ) air samples than non-applicators and were more likely to have post-shift hand wipe concentrations significantly higher than pre-shift concentrations. Concentrations of post-shift urinary biomarkers were higher, albeit not significantly, for applicators than non-applicators. CONCLUSIONS: The exposure results from RCTS worker samples cannot be explained by proximal factors such as nearby restaurants or construction. Air and skin concentration levels were substantially higher for RCTS workers than previously published levels among asphalt workers for all PAHs. PAH profiles on skin wipes were more consistent with RCTS sealant product than air samples. Last day post-shift urinary concentrations of 1-hydroxypyrene greatly exceeded the ACGIH BEI benchmark of 2.5 µg/L in 25 of 26 samples, which suggests occupational exposure and risk of genotoxicity. When pyrene and benzo[a]pyrene were both detected, concentration ratios from personal exposure samples were used to calculate the adjusted BEI. Concentrations of 1-hydroxypyrene exceeded the adjusted BEIs for air, hand wipes, and neck wipes in most cases. These results indicate the need to increase safety controls and exposure mitigation for RCTS workers.


Assuntos
Poluentes Ocupacionais do Ar , Alcatrão , Exposição Ocupacional , Fenantrenos , Hidrocarbonetos Policíclicos Aromáticos , Poluentes Ocupacionais do Ar/análise , Biomarcadores/urina , Alcatrão/análise , Monitoramento Ambiental/métodos , Fluorenos/análise , Humanos , Hidrocarbonetos/análise , Hidrocarbonetos/química , Naftalenos/análise , Exposição Ocupacional/análise , Fenantrenos/urina , Hidrocarbonetos Policíclicos Aromáticos/urina , Pirenos
2.
Artigo em Inglês | MEDLINE | ID: mdl-35457657

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) have been a problem in the environment for an extended period. They are mostly derived from petroleum, coal tar and oil spills that travel and are immobilized in wastewater/water sources. Their presence in the environment causes a hazard to humans due to their toxicity and carcinogenic properties. In the study, coal tar was analyzed using Gas Chromatography-Mass Spectrometry (GC-MS) and a concentration of 787.97 mg/L of naphthalene, followed by 632.15 mg/L of phenanthrene were found to be in the highest concentrations in the various water sources such as sewage, alkaline and acid mine drainage. A design column was used to investigate the leaching process and assessments were conducted on 300 mL of the various water sources mentioned, with 5 g of coal tar added and with monitoring for 4 weeks. The influence of the physiochemical properties of the receiving water sources, such as sewage, and acid and alkaline mine drainage, on the release of PAHs from the coal tar was assessed. The acidic media was proven to have the highest release of PAHs, with a total concentration of 7.1 mg/L of released PAHs, followed by 1.2 mg/L for the sewage, and lastly, 0.32 mg/L for the alkaline mine drainage at room temperature.


Assuntos
Alcatrão , Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Carvão Mineral/análise , Alcatrão/análise , Monitoramento Ambiental/métodos , Humanos , Hidrocarbonetos Policíclicos Aromáticos/análise , Esgotos/análise , Águas Residuárias/análise , Água/análise , Poluentes Químicos da Água/análise
3.
Environ Sci Technol ; 56(3): 1615-1626, 2022 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-35045246

RESUMO

Metals and polycyclic aromatic hydrocarbons (PAHs) are common pollutants in urban streambed sediment, yet their occurrence is highly variable and difficult to predict. To investigate sources of PAHs and metals to streambed sediment, we sampled pavement dust, soil, and streambed sediment in 10 urban watersheds in three regions of the United States and applied a fallout-radionuclide-based sediment-source analysis to quantify the pavement dust contribution to stream sediment (%dust). We also mapped the area of sealcoated pavement in each watershed (%sealed) to investigate the role of coal-tar pavement sealant (CTS) as a PAH source. Median total and carbon-normalized total PAH concentrations were significantly higher in streambed sediment in the Northeast (54.3 mg/kg and 2.71 mg/gOC) and Southeast (5.37 mg/kg and 1.36 mg/gOC), where CTS is commonly used, than in the Northwest (2.11 mg/kg and 0.071 mg/gOC), where CTS is rarely used. Generalized additive models indicated that %sealed and in some cases %dust significantly affected total PAH concentrations in streambed sediments. The %dust was a significant variable for common urban metals: Cu, Pb, and Zn. These findings advance our quantitative understanding of the role of pavement dust as a source and a vector of contaminants to urban streams.


Assuntos
Alcatrão , Poluentes Ambientais , Hidrocarbonetos Policíclicos Aromáticos , Poluentes Químicos da Água , Alcatrão/análise , Poeira/análise , Monitoramento Ambiental , Poluentes Ambientais/análise , Sedimentos Geológicos , Metais/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Rios , Poluentes Químicos da Água/análise
4.
J Chromatogr A ; 1651: 462317, 2021 Aug 16.
Artigo em Inglês | MEDLINE | ID: mdl-34161836

RESUMO

Unlike native polycyclic aromatic hydrocarbons (PAHs), quantitation of substituted polycyclic aromatic compounds (PACs) has been a challenge in the environmental industry. The challenge can be attributed in part to the large number of theoretically possible isomers and the lack of authentic standards for quantitation. In addition, the lack of a unified approach to the quantitation of these compounds has led to poor interlaboratory accuracy. Because these compounds are often used for toxicology studies or to delineate sources and fingerprinting, it is vital that a standardized approach to quantify them is established. This study evaluated different quantitation approaches to quantify both 16 individual PACs and 32 groups/clusters of substituted PACs in three standard reference materials (SRM 1944 - New York / New Jersey waterway sediments, SRM 1597 - a coal tar sample and SRM 2779 - Gulf of Mexico crude oil). The methods employed include: (1) external calibration taking into account recovery correction factor for each analyte, (2) an average relative response factor (ARRF) of PACs obtained with a recovery correction, (3) ARRF of PACs obtained using uncorrected peak areas (i.e., no recovery correction), (4) ARRF of PACs calculated by normalization to deuterated PAHs and (5) ARRF of native PAHs to quantify substituted PACs. The evaluation of concentrations of individually substituted PACs from the different quantitative approaches compared to the certified/reference values showed that methods 1, 2 and 3 performed best. The average percentage of compounds that fell within our acceptable limit (±30%) using methods 1, 2 and 3 for SRM-1944, -1597a and -2779 was 87, 75 and 100%, respectively. Using native PAHs to quantify their substituted analogs resulted in data of the poorest quality. Irrespective of the approach used, there were significant systematic errors in measurements on clusters/groups PACs most notably C1 and C2-benzanthracenes/ chrysenes/triplenylenes, and C2- and C3-dibenzothiophenes being consistently greater than 100% of the stated value. Commerical availability of more substituted PACs will mitigate the biases associated with the quanititation of PAC clusters/groups.


Assuntos
Monitoramento Ambiental/métodos , Hidrocarbonetos Policíclicos Aromáticos/análise , Alcatrão/análise , Petróleo/análise
5.
J Hazard Mater ; 410: 124648, 2021 05 15.
Artigo em Inglês | MEDLINE | ID: mdl-33257128

RESUMO

Although coal tar pitch (CTP) has a large yield in China, its large-scale and effective utilization is significantly hindered because of existing and possibly releasing polycyclic aromatic hydrocarbons (PAHs). Therefore, it is an imminent problem how to prepare an environmentally friendly CTP by detoxification modification. In the investigation, a typical CTP was subjected to structural characterization via solid-state 13C NMR and gas chromatograph/mass spectrometer, which confirmed the existence of dominant PAHs such as fluoranthene, pyrene, as well as benzo[a]pyrene, and few heterocyclic compounds. Subsequently, the CTP was modified using 10-undecenal via alkylation reaction enhanced by ultraviolet & microwave radiation. Compared with the original CTP, the total content of 16 toxic PAHs in the modified CTP decreased with a reduction efficiency of above 90%. According to different environmental standards, toxic equivalent quotient of CTP after modification was reduced by above 90%. In order to veritably and fully evaluate the toxicity of CTP, a living vascular smooth muscle cell (A-10 cell) in vitro was used in the cell counting kit-8 assay. The viability of A-10 cell was always higher when exposed to modified CTP than the original CTP. These results powerfully indicated that the enhanced modification was actually effective and efficient for reducing the toxicity of CTP.


Assuntos
Alcatrão , Hidrocarbonetos Policíclicos Aromáticos , China , Carvão Mineral/toxicidade , Alcatrão/análise , Alcatrão/toxicidade , Micro-Ondas , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/toxicidade
6.
Environ Pollut ; 254(Pt B): 113103, 2019 Nov.
Artigo em Inglês | MEDLINE | ID: mdl-31479809

RESUMO

Sealcoat is an emulsified coating product applied to asphalt to protect against surface weathering. Sealcoat products contain coal-tar (CT) or petroleum-derived residues and are a recognized source of polycyclic aromatic hydrocarbons (PAHs) in urban areas. Although the toxicity of urban runoff from CT-sealed asphalt is established, chemical characterization has focused more on PAHs and alkylated derivatives and less on polar transformation products. In this study, solid-phase extraction (SPE) was used to concentrate dissolved (<0.2 µm) species in runoff collected from asphalt surfaces sealed with CT pitch or steam-cracked petroleum (SCP) residues. CT-sealed surfaces released a 20-fold greater concentration of SPE-extractable compounds in runoff compared to SCP-sealed surfaces. Representative compounds were sorted into four groups: nitrogen heterocycles (azaarenes) and other oxygen- and sulfur-containing species (N HET); hydroxylated N heterocycles (hydroxylated N HET); the nonionic surfactant 2,4,7,9-tetramethyl-5-decyne-4,7-diol (TMDD); and styrene-acrylonitrile polymer byproducts (SAN Trimer). Species concentrations and weathering-related disappearance behavior differed among the four subgroups. While hydroxylated N HET concentrations decreased by 94% in runoff from CT-sealed surfaces 60 h after sealcoat application, SAN Trimer concentrations in CT and SCP runoff increased over time as polymerization progressed, illustrating the complex changes the chemicals in sealcoat undergo as it cures under environmentally-relevant conditions. Overall, this study shows that urban runoff collected from CT-sealed and SCP-sealed asphalt surfaces is a potential source of water-soluble contaminants with unknown long-term ecotoxicological effects to aquatic systems.


Assuntos
Alcatrão/análise , Monitoramento Ambiental , Hidrocarbonetos/química , Hidrocarbonetos Policíclicos Aromáticos/análise , Poluentes Químicos da Água/análise , Pennsylvania , Hidrocarbonetos Policíclicos Aromáticos/química , Poluentes Químicos da Água/química , Poluição da Água/análise
7.
Environ Sci Pollut Res Int ; 25(28): 28642-28653, 2018 Oct.
Artigo em Inglês | MEDLINE | ID: mdl-30094671

RESUMO

Tar oil is a complex mixture of hydrocarbon compounds obtained from high-temperature distillation of coal tar. It has been used for over 100 years from now to protect wood and has been applied to wood products, primary utility poles, and railroad ties by pressure methods. Composition of the tar oil depends on the source and typically consists of 85% polycyclic aromatic hydrocarbons (PAHs), 10% phenolic compounds, and 5% heterocyclic compounds. In this research, we performed the laboratory experiment to compare two types of tar oil: C and GX-Plus, and their effects on P-cycling enzymes (phosphatases) in sandy loam and loamy sand. Tar oil was applied to soil samples at the following doses: 2, 10, and 50 g kg-1. Soil without tar oil was used as a control sample. The experiment showed that the contamination of soil with tar oil affects the enzyme activities measured and with this most probably the P-cycle in soil. Phosphomonoesterases were the most sensitive to the contamination of soil with both type of tar oil: typeC and type GX-Plus. Greater changes in the enzymatic activity were observed in the loamy sand. Moreover, the type C tar oil demonstrated higher toxicity for phosphatases than type GX-Plus.


Assuntos
Alcatrão/química , Hidrocarbonetos/química , Monoéster Fosfórico Hidrolases/metabolismo , Poluentes do Solo/química , Solo/química , Alcatrão/análise , Hidrocarbonetos/análise , Monoéster Fosfórico Hidrolases/química , Polônia , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/química , Poluentes do Solo/análise
8.
Mar Pollut Bull ; 129(2): 494-502, 2018 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-29106939

RESUMO

Marine debris accumulation was analyzed from three exposed beaches of the Canary Islands (Lambra, Famara and Las Canteras). Large microplastics (1-5mm), mesoplastics (5-25mm) and tar pollution were assessed twice a month for a year. There was great spatial and temporal variability in the Canary Island coastal pollution. Seasonal patterns differed at each location, marine debris concentration depended mainly of local-scale wind and wave conditions. The most polluted beach was Lambra, a remote beach infrequently visited. The types of debris found were mainly preproduction resin pellets, plastic fragments and tar, evidencing that pollution was not of local origin, but it cames from the open sea. The levels of pollution were similar to those of highly industrialized and contaminated regions. This study corroborates that the Canary Islands are an area of accumulation of microplastics and tar rafted from the North Atlantic Ocean by the southward flowing Canary Current.


Assuntos
Praias/normas , Alcatrão/análise , Monitoramento Ambiental/métodos , Plásticos/análise , Resíduos/análise , Oceano Atlântico , Estações do Ano , Espanha , Vento
9.
Environ Pollut ; 212: 166-177, 2016 May.
Artigo em Inglês | MEDLINE | ID: mdl-26845364

RESUMO

Polycyclic aromatic hydrocarbons (PAHs) were assessed spatially and temporally within and adjacent to a former coking and steel manufacturing facility in Sydney, Nova Scotia, Canada. Concentrations of PAHs were measured in surface soils, marine and estuary sediments prior to and during remediation of the Sydney Tar Ponds (STPs) site which was contaminated by nearly a century of coking and steel production. Previous studies identified PAHs in surficial marine sediments within Sydney Harbour, which were considered to be derived from STP discharges. Numerous PAH fingerprint techniques (diagnostic ratios, principal component analysis, quantitative and qualitative analysis) were applied to soil and sediment samples from the STPs and surrounding area to identify common source apportionment of PAHs. Results indicate coal combustion (from historical residential, commercial and industrial uses) and coal handling (from historic on-site stockpiling and current coal transfer and shipment facilities) are likely the principal source of PAHs found in urban soils and marine sediments, consistent with current and historical activities near these sites. However, PAH fingerprints associated with STP sediments correlated poorly with those of urban soils and marine sediments, but were similar to coal tar, historically consistent with by-products produced by the former coking operations. This study suggests PAH contamination of Sydney Harbour sediments and urban soils is largely unrelated to historic coking operations or recent remediation of the STPs site, but rather a legacy of extensive use of coal for a variety of activities.


Assuntos
Alcatrão/análise , Monitoramento Ambiental/métodos , Poluentes Ambientais/química , Hidrocarbonetos Policíclicos Aromáticos/química , Carvão Mineral/análise , Coque , Estuários , Resíduos Industriais/análise , Nova Escócia , Solo/química
10.
Sci Total Environ ; 563-564: 741-54, 2016 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-26610368

RESUMO

Naturally occurring distribution and attenuation processes can keep hydrocarbon emissions from dense non aqueous phase liquids (DNAPL) into the adjacent groundwater at a minimum. In a historically coal tar DNAPL-impacted site, the de facto absence of a plume sparked investigations regarding the character of natural attenuation and DNAPL resolubilization processes at the site. Steep vertical gradients of polycyclic aromatic hydrocarbons, microbial community composition, secondary water quality and redox-parameters were found to occur between the DNAPL-proximal and shallow waters. While methanogenic and mixed-electron acceptor conditions prevailed close to the DNAPL, aerobic conditions and very low dissolved contaminant concentrations were identified in three meters vertical distance from the phase. Comprehensive two-dimensional gas chromatography-mass spectrometry (GC×GC-MS) proved to be an efficient tool to characterize the behavior of the present complex contaminant mixture. Medium to low bioavailability of ferric iron and manganese oxides of aquifer samples was detected via incubation with Shewanella alga and evidence for iron and manganese reduction was collected. In contrast, 16S rDNA phylogenetic analysis revealed the absence of common iron reducing bacteria. Aerobic hydrocarbon degraders were abundant in shallow horizons, while nitrate reducers were dominating in deeper aquifer regions, in addition to a low relative abundance of methanogenic archaea. Partial Least Squares - Canonical Correspondence Analysis (PLS-CCA) suggested that nitrate and oxygen concentrations had the greatest impact on aquifer community structure in on- and offsite wells, which had a similarly high biodiversity (H' and Chao1). Overall, slow hydrocarbon dissolution from the DNAPL appears to dominate natural attenuation processes. This site may serve as a model for developing legal and technical strategies for the treatment of DNAPL-impacted sites where contaminant plumes are absent or shrinking.


Assuntos
Bactérias/classificação , Alcatrão/análise , Água Subterrânea/análise , Água Subterrânea/microbiologia , Microbiota , Qualidade da Água , Áustria , RNA Bacteriano/análise , RNA Ribossômico 16S/análise
11.
Environ Pollut ; 207: 329-40, 2015 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-26444225

RESUMO

During the 20th century, the local economy of the Upper Loire Basin (ULB) was essentially based on industrial coal mining extraction. One of the major French coal districts with associated urban/industrial activities and numerous coking/gas plants were developed in the Ondaine-Furan subbasins, two tributaries of the upper Loire main stream. To determine the compositional assemblage, the level and the potential sources of contamination, the historical sedimentary chronicle of the 16 US EPA priority polycyclic aromatic hydrocarbons (PAHs) has been investigated. PAH concentrations were determined using gas chromatography/mass spectrometry (GC/MS) in a dated core, sampled in the Villerest flood-control reservoir located downstream of the Ondaine-Furan corridor (OFC). The most contaminated sediments were deposited prior to 1983 (Σ16PAHs ca. 4429-13,348 ng/g) and during flood events (Σ16PAHs ca. 6380 ng/g - 1996 flood; 5360 ng/g - 2003 flood; 6075 ng/g - 2008 flood), especially in medium and high molecular weight PAHs. Among them, typical pyrogenic PAHs such as FLT, PYR, BbF and BaP were prevalent in most of the core samples. In addition, some PAHs last decade data is available from the Loire Bretagne Water Agency and were analyzed using high-performance liquid chromatography with postcolumn fluorescence derivatization (HPLC/FLD). These results confirm that the most highly contaminated sediments were found downstream of OFC (Σ16PAHs ca. 2264-7460 ng/g). According to the observed molecular distribution, PAHs are originated largely from high-temperature pyrolytic processes. Major sources of pyrogenic PAHs have been emphasized by calculation of specific ratios and by comparison to reported data. Atmospheric deposition of urban and industrial areas, wood combustion and degraded coal tar derived from former factories of coking/gas plants seem to be the major pyrogenic sources. Specifically, particular solid transport conditions that can occur during major flood events lead us to emphasize weathering of former contamination sources, such as more preserved coal tar.


Assuntos
Poluição Ambiental/análise , Sedimentos Geológicos/química , Hidrocarbonetos Policíclicos Aromáticos/análise , Poluentes Químicos da Água/análise , Minas de Carvão , Alcatrão/análise , Coque , Monitoramento Ambiental/métodos , Inundações , França , Cromatografia Gasosa-Espectrometria de Massas , Hidrocarbonetos Policíclicos Aromáticos/toxicidade , Rios
12.
Sci Total Environ ; 520: 73-80, 2015 Jul 01.
Artigo em Inglês | MEDLINE | ID: mdl-25795989

RESUMO

Coal-tar-based (CTB) sealcoat, frequently applied to parking lots and driveways in North America, contains elevated concentrations of polycyclic aromatic hydrocarbons (PAHs) and related compounds. The RTL-W1 fish liver cell line was used to investigate two endpoints (genotoxicity and DNA-repair-capacity impairment) associated with exposure to runoff from asphalt pavement with CTB sealcoat or with an asphalt-based sealcoat hypothesized to contain about 7% CTB sealcoat (AS-blend). Genotoxic potential was assessed by the Formamido pyrimidine glycosylase (Fpg)-modified comet assay for 1:10 and 1:100 dilutions of runoff samples collected from 5 h to 36 d following sealcoat application. DNA-repair capacity was assessed by the base excision repair comet assay for 1:10 dilution of samples collected 26 h and 36 d following application. Both assays were run with and without co-exposure to ultraviolet-A radiation (UVA). With co-exposure to UVA, genotoxic effects were significant for both dilutions of CTB runoff for three of four sample times, and for some samples of AS-blend runoff. Base excision repair was significantly impaired for CTB runoff both with and without UVA exposure, and for AS-blend runoff only in the absence of UVA. This study is the first to investigate the effects of exposure to the complex mixture of chemicals in coal tar on DNA repair capacity. The results indicate that co-exposure to runoff from CT-sealcoated pavement and UVA as much as a month after sealcoat application has the potential to cause genotoxicity and impair DNA repair capacity.


Assuntos
Alcatrão/toxicidade , Reparo do DNA , Peixes/fisiologia , Mutagênicos/toxicidade , Poluentes Químicos da Água/toxicidade , Animais , Alcatrão/análise , Materiais de Construção , Dano ao DNA , Monitoramento Ambiental , Hidrocarbonetos/toxicidade , América do Norte , Hidrocarbonetos Policíclicos Aromáticos/análise , Hidrocarbonetos Policíclicos Aromáticos/toxicidade
15.
Environ Pollut ; 185: 59-68, 2014 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-24215941

RESUMO

We used land-use analysis, PAH concentrations and assemblages, and multivariate statistics to identify sediment PAH sources in a small (~1303 km(2)) urbanizing watershed located in South-Central, Pennsylvania, USA. A geographic information system (GIS) was employed to quantify land-use features that may serve as PAH sources. Urban PAH concentrations were three times higher than rural levels, and were significantly and highly correlated with combined residential/commercial/industrial land use. Principal components analysis (PCA) was used to group sediments with similar PAH assemblages, and correlation analysis compared PAH sediment assemblages to common PAH sources. The strongest correlations were observed between rural sediments (n = 7) and coke-oven emissions sources (r = 0.69-0.78, n = 5), and between urban sediments (n = 22) and coal-tar-based sealcoat dust (r = 0.94, n = 47) suggesting that coal-tar-based sealcoat is an important urban PAH source in this watershed linked to residential and commercial/industrial land use.


Assuntos
Alcatrão/análise , Monitoramento Ambiental , Hidrocarbonetos Policíclicos Aromáticos/análise , Rios/química , Poluentes Químicos da Água/análise , Cidades , Alcatrão/química , Pennsylvania , Urbanização
16.
Environ Pollut ; 191: 260-1, 2014 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-24373812

RESUMO

The claim made in the title of Witter et al. (2014) "Coal-tar-based sealcoated pavement: A major PAH source to urban stream sediments" is not supported by the data presented. The author's use of Pearson correlation coefficients is insufficient to indicate causation. The application of spatial analysis and principle component analysis did not include sealer specific inputs, so provides no basis for the claim. To test the hypothesis that sealers are a source of PAHs in the stream studied, EPA's Chemical Mass Balance (CMB) source evaluation model was applied to Witter's sediment data. CMB found an excellent fit (R(2) > 0.999) between measured and modeled PAH concentrations when sealers were not included as a potential source. This finding does not support Witter et al. (2014) claim that sealers are a major source of PAHs.


Assuntos
Alcatrão/análise , Monitoramento Ambiental , Hidrocarbonetos Policíclicos Aromáticos/análise , Rios/química , Poluentes Químicos da Água/análise
17.
Environ Pollut ; 179: 315-25, 2013 Aug.
Artigo em Inglês | MEDLINE | ID: mdl-23631939

RESUMO

Mass transfer processes of pollutants from non-aqueous phase liquids (NAPL) may control groundwater pollution at abandoned industrial sites. We studied release kinetics of polycyclic aromatic hydrocarbons (PAHs) from fresh and aged tar phases using a dialysis tubing technique. Time for equilibration ranged from several days to more than three years. For fresh tar materials the release seems to be limited by retarded pore diffusion, while for two of three aged tars diffusion limited release influenced by dissolved organic matter (DOM) was assumed. The equilibration process was driven by solubilization thermodynamics expressed by Raoult's law. Yet, solubility enhancement was observed potentially due to the presence of organic mobile sorbents. The results show that the release of PAHs from tar phases is generally rate limited and partitioning according to Raoult's law is the driving mechanism of the exchanges process.


Assuntos
Alcatrão/análise , Modelos Químicos , Hidrocarbonetos Policíclicos Aromáticos/análise , Poluentes Químicos da Água/análise , Difusão , Monitoramento Ambiental , Cinética , Termodinâmica
18.
Anal Chem ; 84(5): 2245-52, 2012 Mar 06.
Artigo em Inglês | MEDLINE | ID: mdl-22339202

RESUMO

Polycyclic aromatic sulfur heterocycles (PASH) are sulfur analogues of polycyclic aromatic hydrocarbons (PAH). Alkylated PAH attract much attention as carcinogens, mutagens, and as diagnostics for environmental forensics. PASH, in contrast, are mostly ignored in the same studies due to the conspicuous absence of gas chromatography/mass spectrometry (GC/MS) retention times and fragmentation patterns. To obtain these data, eight coal tar and crude oils were analyzed by automated sequential GC-GC. Sample components separated based on their interactions with two different stationary phases. Newly developed algorithms deconvolved combinatorially selected ions to identify and quantify PASH in these samples. Simultaneous detection by MS and pulsed flame photometric detectors (PFPD) provided additional selectivity to differentiate PASH from PAH when coelution occurred. A comprehensive library of spectra and retention indices is reported for the C(1)-C(4) two-, three-, and four-ring PASH. Results demonstrate the importance of using multiple fragmentation patterns per homologue (MFPPH) compared to selected ion monitoring (SIM) or extraction (SIE) to identify isomers. Since SIM/SIE analyses dramatically overestimate homologue concentrations, MFPPH should be used to correctly quantify PASH for bioavailability, weathering, and liability studies.


Assuntos
Cromatografia Gasosa-Espectrometria de Massas , Hidrocarbonetos Policíclicos Aromáticos/química , Enxofre/química , Algoritmos , Alcatrão/análise , Isomerismo , Petróleo/análise , Tiofenos/análise
19.
J Contam Hydrol ; 126(3-4): 181-94, 2011 Nov 01.
Artigo em Inglês | MEDLINE | ID: mdl-22115084

RESUMO

NSO heterocycles (HET) are typical constituents of coal tars. However, HET are not yet routinely monitored, although HET are relatively toxic coal tar constituents. The main objectives of the study is therefore to review previous studies and to analyse HET at coal tar polluted sites in order to assess the relevance of HET as part of monitored natural attenuation (MNA) or any other long-term monitoring programme. Hence, natural attenuation of typical HET (indole, quinoline, carbazole, acridine, methylquinolines, thiophene, benzothiophene, dibenzothiophene, benzofuran, dibenzofuran, methylbenzofurans, dimethylbenzofurans and xanthene) were studied at three different field sites in Germany. Compound-specific plume lengths were determined for all main contaminant groups (BTEX, PAH and HET). The results show that the observed plume lengths are site-specific and are above 250m, but less than 1000m. The latter, i.e. the upper limit, however mainly depends on the level of investigation, the considered compound, the lowest measured concentration and/or the achieved compound-specific detection limit and therefore cannot be unequivocally defined. All downstream contaminant plumes exhibited HET concentrations above typical PAH concentrations indicating that some HET are generally persistent towards biodegradation compared to other coal tar constituents, which results in comparatively increased field-derived half-lives of HET. Additionally, this study provides a review on physicochemical and toxicological parameters of HET. For three well investigated sites in Germany, the biodegradation of HET is quantified using the centre line method (CLM) for the evaluation of bulk attenuation rate constants. The results of the present and previous studies suggest that implementation of a comprehensive monitoring programme for heterocyclic aromatic compounds is relevant at sites, if MNA is considered in risk assessment and for remediation.


Assuntos
Alcatrão/química , Água Subterrânea/química , Compostos Heterocíclicos/química , Poluentes Químicos da Água/química , Biodegradação Ambiental , Alcatrão/análise , Alcatrão/toxicidade , Alemanha , Compostos Heterocíclicos/toxicidade , Poluentes Químicos da Água/toxicidade
20.
J Hazard Mater ; 192(3): 1219-25, 2011 Sep 15.
Artigo em Inglês | MEDLINE | ID: mdl-21742434

RESUMO

A comparison was made between the dissipation of polycyclic aromatic hydrocarbons (PAHs) in soil freshly spiked with pure PAHs, soil spiked with a coal tar mixture and a contaminated soil from a former coking works where the PAHs had been present for more than a century. The potential of five selected plant species for phytoremediation was investigated. The levels of all 7 PAHs in chemically amended soil, both planted and unplanted, fell significantly (>80% reduction) over the 12 weeks of the growing trial. In the coal tar treated soils all PAHs were significantly reduced. In both the planted and unplanted soils the 2-3 ringed compounds demonstrated much greater loss (>77%) than the 4-6 ringed (16-39%). The 3-4 ringed compounds demonstrated strong evidence of phytoremediation but not the 5-6 ringed. The coking soil showed limited reduction (7-24%) of all 12 PAHs present. There was little difference in dissipation between the PAHs and little evidence of a phytoremediation effect in coking soil. The results demonstrated that the form in which PAHs were added to soil influenced their susceptibility to dissipation. Therefore, predictions of PAH dissipation from laboratory amended soil do not reflect the true situation in the field.


Assuntos
Biodegradação Ambiental , Alcatrão/análise , Hidrocarbonetos Policíclicos Aromáticos/análise , Poluentes do Solo/análise , Solo/análise , Crisenos/química , Coque , Poluição Ambiental , Fluorenos/química , Gases , Resíduos Industriais , Modelos Estatísticos , Fatores de Tempo , Tempo (Meteorologia)
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